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Cite this: DOI: 10.1039/d1an01096d

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Nanowire-based sensor electronics for chemicaland biological applications
Guozhu Zhang, a Hao Zeng, a Jiangyang Liu, a Kazuki Nagashima,
Tsunaki Takahashi, a,b Takuro Hosomi,a,b Wataru Tanakaa andTakeshi Yanagida *a,ca,bDetection and recognition of chemical and biological species via sensor electronics are important not
only for various sensing applications but also for fundamental scientiﬁc understanding. In the past two
decades, sensor devices using one-dimensional (1D) nanowires have emerged as promising and powerfulplatforms for electrical detection of chemical species and biologically relevant molecules due to theirsuperior sensing performance, long-term stability, and ultra-low power consumption. This paper presents
a comprehensive overview of the recent progress and achievements in 1D nanowire synthesis, working
principles of nanowire-based sensors, and the applications of nanowire-based sensor electronics in
Received 21st June 2021,
Accepted 12th September 2021
DOI: 10.1039/d1an01096d
rsc.li/analyst

1.

chemical and biological analytes detection and recognition. In addition, some critical issues that hinder
the practical applications of 1D nanowire-based sensor electronics, including device reproducibility andselectivity, stability, and power consumption, will be highlighted. Finally, challenges, perspectives, andopportunities for developing advanced and innovative nanowire-based sensor electronics in chemicaland biological applications are featured.

Introduction

For the upcoming “trillion sensor electronics” era, molecularsensor and electronic recognition devices, which collect enormous
information as big data from various chemical species (e.g., volatile organic molecules, small molecules, and ions) and biologically-relevant molecules (e.g., DNA and mRNA, proteins, metabolites, drugs, etc.), have attracted considerable attention due totheir promising applications in environment monitoring,1–5
industrial production,6–10 food security,11,12 health, andbiomedicine.13–16 The key to realizing molecular detection andrecognition is the transduction of chemical and biologicalbinding events into electronic and digital signals with selective
merit.17 To significantly and selectively amplify the moleculebinding events, several sensing approaches have been discovered
for the detection of chemical and biological molecules, mainly
including chemiresistive,18–23 electrochemical,24–28 and field-eﬀect
transistors (FETs)29–31 types of molecular sensing mechanisms. In
particular, with the advancement of nanomaterial fabrication
technology, a large number of functional nanostructures, such asa

Department of Applied Chemistry, Graduate School of Engineering, The Universityof Tokyo, 7-3-1, Hongo, Bunkyo-ku, Tokyo, 113-8654, Japan.
E-mail: yanagida@g.ecc.u-tokyo.ac.jpbJST-PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japanc
Institute for Materials Chemistry and Engineering, Kyushu University, 6-1 KasugaKoen, Kasuga, Fukuoka, 816-8580, Japan

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nanodots,32–36 nanowires,37–40 nanosheets,41,42 and hierarchicalnanostructures,43–45 have been synthesized as building blocks forthe fabrication of sensor electronics.
Among the recent nanostructured forms, one-dimensional(1D) nanowires oﬀer lots of advantages for molecular sensing
compared with other nanostructures, which can be summarized as superior sensing performance, long-term stability, andlow power consumption. Due to nanoscale diameter and highsurface to volume ratio, very few molecules binding on the
nanowire surface can trigger the fluctuation of its electricalproperties.46,47 This allows the nanowire-based sensor electronics to detect molecules with high sensitivity and fast
response/recovery dynamics,48–50 and further enables thesensors to work at room temperature, thereby reducing power
consumption.48,51,52 In addition, the high crystallinity of the
nanowire structure would improve thermal stability, and therefore, the long-term working stability of the sensor device.53
Especially, as the sensor devices are manufactured by single
nanowires, it would significantly eliminate the sensing performance degradation originating from the interaction andmass transfer on the sintering necks and grain boundaries
during the high temperature operation.54,55 Besides, a single
nanowire device structure enables the utilization of self-Jouleheating possible, which would significantly reduce the power
consumed by the sensor electronics.56–58
Ever since the first report of using 1D metallic nanowires as
the molecular sensor by Tao and co-workers in 2000,59 signifi-

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cant progress has been achieved in the past two decades.60–66
To date, thousands of papers have been published on sensor
integration based on 1D nanowires, including metallic, semiconductor, and conducting polymer compositions, for chemicaland biological analytes detection, as shown in Fig. 1. Moreover,to fulfill the rising demands of versatile molecule detection andmonitoring, many innovative sensor designs have been introduced for nanowire sensor fabrication and platform integration.
For example, chemiresistive sensors integrated by metallic
nanowire networks are fabricated for the detection of hydrogengas and biological molecules (e.g., enzymes, glucose, etc.).67–69
Semiconductor nanowires are used to fabricate single nanowire
chemiresistive/FET sensor devices for the detection of gas molecules and charged species (e.g., toxic heavy metal cations, DNA,
RNA, virus, etc.).70–74 Electrochemical analysis methods, inwhich the 1D nanowire structures are integrated as the transduction element (working electrode), also have attracted greatinterest in the detection of chemical analytes (such as heavyions) and biological molecules in the liquid phase.39,75–79 In
addition, some on-chip sensing systems are designed and fabricated by Si nanowires for protein separation and recognition.80
Electronically conducting polymer nanowires also attracted theattention of analytical chemists for the fascinating gas sensor
and biosensor discovery.63,81–83 Therefore, the design and fabrication of molecular sensors and electronic recognition devices
derived from 1D nanowires have a bright future in the Internetof Things (IoT) applications.
Here, in this review, we firstly give a comprehensive overview of the recent studies and achievements in 1D nanowire
synthesis, working principles of nanowire-based sensors, andthe applications of nanowire-based sensor electronics inchemical and biological molecule detection and recognition.
Then, some critical issues that hinder the practical applications of 1D nanowire-based sensor electronics, including
selectivity, long-term stability, and low power consumption,
will be pointed out. Finally, we give an outlook of the remaining issues towards the lab-to-market transfer of 1D nanostructure-based sensor electronics.

Fig. 1 Number of publications in the area of nanowires and nanowire
sensors from 2001 to 2021 (internet search of the Web of Science on
Apr. 15, 2021). Keywords for search: nanowire + chemical sensor; nanowire + bio/biological sensor.

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2. Synthesis of 1D nanowire
structures
Nanowire-based electronics oﬀer an excellent possibility for
future systems beyond the limitation of Moore’s law andprovide a promising platform to explore the physical origin
and intrinsic properties. In recent decades, significant eﬀorts
and progress have been made, and many methods have beendeveloped to synthesize 1D metallic, semiconductor, and electrically conducting polymer nanowires.22,84–89 Generally, theformation of 1D nanowires can be categorized into two paradigms, the top-down and bottom-up approaches (Fig. 2). In
the case of top-down approach (Fig. 2(a)), nanowires areusually fabricated in well-defined locations with a homogeneous diameter and length, which are realized via a combination of patterning lithography, etching, and deposition
processes.90–94 On the contrary, the bottom-up approach(Fig. 2(b)) starts with single atoms or molecules and selfassemble to 1D nanostructures with a high aspect ratio.93,95–97
Additionally, this nanowire synthesis strategy can realize nanowire controlling with tunable size, composition, heterostructure, and electronic properties, which directly benefits a
lot of distinct nanowire sensor device integration.98–101 In thepast two decades, significant eﬀorts have been devoted to thediscovery and growth of 1D nanowires based on the bottom-up
approach.22,58,99,102–126 In this section, we review the recent
progress in the 1D nanowire synthesis in terms of these twoparadigms, including homogeneous nanowires and nanowire
heterostructures within axial and lateral dimensions.
2.1.

Metallic nanowire (MNWs) synthesis

MNWs have been explored as sensing elements because they
possess an apparent electrical signal fluctuation as analytes
bind on their surface.127,128 To date, various kinds of MNWs,
such as single metals (Ag, Au, Pt, Pd, Ni),60,64,66,74,129–152 bimetallic alloys (NiCo),153,154 and trimetallic alloys (PtPdCu),154
have been successfully synthesized for molecular sensing.
Their synthesis methods can be classified into three categories: template-assisted electrodeposition,155 self-assembled
growth in solution-phase and vapour-phase,156 and lithographically patterned deposition via top-down approach.157,158
Specifically, the synthetic methods and molecular sensing
applications of MNWs in the past two decades have been summarized in Table 1.
Template-assisted synthesis coupled with electrodeposition
is a facile and eﬃcient strategy to fabricate MNWs structureswith uniform diameter and length on arbitrary
substrates.205–208 Recently, anodic aluminum oxides (AAO) areusually applied as a hard template for the MNWs growth. For
example, Choi et al. fabricated high density and uniform Pdnanowire arrays utilizing AAO template and integrated such astructure as a sensor for H2 detection (Fig. 3(a)).209 Gu et al.
also used the AAO template to successfully fabricate threedimensional (3D) Pt nanowire arrays and applied them aselectrochemical sensors for glucose detection.136 Besides, poly-This journal is © The Royal Society of Chemistry 2021

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Fig. 2 (a) Top-down method of nanowire synthesis. SEM image is reproduced from ref. 94 with permission from BioMed Central, copyright 2021.
(b) Bottom-up method of nanowire synthesis. SEM image is reproduced from ref. 97 with permission from Springer Nature, copyright 2016.

Table 1

Summary of metallic nanowire (MNW) synthesis and their molecular sensing applications

Class
Single metals

Materials

Synthetic method
160,161160

162–165

Pb
Mo
Pt
Pd

H2 184–190

Cu
NiPt
AuCu
NiCo
AgCu
AgAu
PtAg
PbPt
Pt Au
PtCoIr
AuCdTeNitrite191
H2O2 192
H2O2 193
Glucose153
H2O2 194
HNO3;66 rhodamine 6G195
H2 197
H2;198 glucose199,200
H2O2 201,202
Procalcitonin203
DNA Molecules204

Ni

Trimetallic
alloys159,160

NO2;
H2O; H2O2;
NH3;
4-nitrophenol;166,167 phosphate;168 heavy ions169
pH;170,171 Na+;170 K+;170 heavy ions;74
H2O2;149,172–174 dopamine;175 cholesterol;147,176
thrombin;177 telomerase178
Glucose;148 glutamate;152 salmonella
typhimurium179
H2 180H2 181
H2;150 glucose;182 H2O2 183

Ag
Au

Bimetallic
alloysAnalytescarbonates, which served as a soft template, are also favorable
in metallic nanowire formation.210 Hasan et al. demonstrated aconvenient way to fabricate Pd nanoparticle modified Au nanowire array electrodes using polycarbonate membrane templatesfor H2O2 detection.211 Escarpa et al. also utilized polycarbonate
templates for the fabrication of Ni and Co metallic nanowires
and applied them for the electrochemical detection of carbohydrates involved in rare metabolic diseases.212 However, template-assisted electrodeposition methods sometimes suﬀer fromthe diﬃculty in template removal for some systems.213

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Solvothermal method;161–163,165–168 electrodeposition;164 dropcasted;159 LPNE technique160
Hydrothermal method;172 solvothermal method;149,170,173,174
electrodeposition;171,177 electroplating;147,176 CVD;178 vapor
transport method;74 LPNE technique175
Electrodeposition;148,152 solvothermal method179
Template-assisted method180
Electrodeposition181
LPNE technique;150 template-assisted method;182
electrodeposition183
LPNE technique;184,185,188–190 vapor transport method;186 template-assisted method187
Template galvanic deposition191
Mild dealloying192
Solvothermal method193
CVD153Co-precipitation194
Template-assisted method;66 thermal deposition196
LPNE technique197
LPNE technique;198 template-assisted method199,200
Template-assisted method;201 chemical deposition202
Solvothermal method203
Electrochemical deposition204

Self-assembled growth in the solution phase, especially inthe polyol process, is a preferred method for large-scale MNWs
synthesis.214,215 The solution-phase synthesis of MNWs issimilar in growth recipes, which usually contain two important
reactants, a reducing agent, and a capping agent,216 as shownin Fig. 3(b). The reducing agent is an indispensable component during the growth because it would promote thereduction of metal ions to metal. The capping agent has astructure-directing feature, which preferentially caps a specificcrystal face to obtain the selectivity of crystal growth direc-

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AnalystFig. 3 (a) Template-assisted method of metal nanowire synthesis. SEM image is reproduced from ref. 209 with permission from American Chemical
Society, copyright 2003. (b) Metal nanowire self-assembling in solution phase. SEM image is reproduced from ref. 216 with permission from WileyVCH, copyright 2016. (c) Lithographically patterned nanowire electrodeposition (LPNE) method of metal nanowire synthesis. SEM image reproduced
from ref. 197 with permission from American Chemical Society, copyright 2017.

tion.215 This type of synthesis generally yields MNWs with atypical diameter ranging from 20 to 150 nm and lengths fromfew to several tens of micrometers.156 For instance, Huang
et al. synthesized graphene/Au nanowire composites via a
solvothermal method and applied them as electrochemical
gene sensors for tulobuterol detection.217 Herein, the triisopropylsilane was used as a reducing agent, and oleylamine
served as a structure-directing agent. Pu et al. also realized
Pt@Pd nanowire synthesis in a mixed solution of ethylene
glycol and N,N-dimethylformamide. It is indicated that Pt@Pd
nanowires modified with horseradish peroxidase show excellent sensing properties toward Mycoplasma pneumonia DNA.218
In addition, Du et al. have demonstrated a bimetallic PtNi
nanowire synthesis via a facile solvothermal method for caﬀeic
acid electrochemical detection.219 Besides, reduction of metalsalts in the vapor phase is another feasible way to self-assemble single crystalline metal and metal alloy nanowires.220,221
Scott et al. have demonstrated a facile method to synthesize
Co, Ni, NiCo, CoFe, and NiFe nanowires in nitrogen atmo-

Analystsphere via directly reducing their metal nitride precursors at
550–600 °C.220
The significant advancements in the field of lithography
have promoted the wide application of these techniques in patterned nanowire fabrication with well-controlled placement
and feature-size.222–224 In contrast to the template-assisted
MNWs synthesis, in which the metal components are electrodeposited into the nanopores along the axis of the template
membrane and the as-fabricated MNWs are oriented perpendicular to the plane of the membrane after their removal, the
MNWs are commonly obtained horizontally onto the substratesurface,197 as shown in Fig. 3(c). Over the past two decades,
several types of pattern synthesis techniques, including opticaland X-ray lithography, electron-beam and ion-beam lithography, and printing, imprinting, and scanning probe lithography, have been proposed for MNWs deposition.138,184,197,225–229
Prajapati et al. successfully realized an individual Pt nanowire
device fabrication with suspended structure through the combination of electron-beam lithography (EBL) and reactive ion

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Analystetching (RIE) techniques, and this kind of sensor device
enables the sub-ppm H2 detection with a 500 ppb limit ofdetection (LOD).138 Penner et al. demonstrated nanocrystalline
Pd nanowire (with a diameter of 5 nm) synthesis through alithographically patterned nanowire electrodeposition (LPNE),
and successfully integrated them as a chemiresistive sensor forH2 detection.184 Although advanced lithography techniques
enable nanowire fabrication with the desired regime in micro/
nanoscale dimensions, high equipment costs and complex
fabrication processes impede their wide applications in large
scale nanowire formation.
2.2.

Semiconductor nanowires (SNWs) synthesis

Among various nanowire sensing components, 1D SNWs are
the most successful and promising candidates for the electrical detection of molecules due to their high sensitivity and fast
response.230,231 Ever since the first report of using 1D borondoped silicon nanowires (SiNWs) as molecule sensors for biological and chemical species detection by Cui et al.,232 significant progress both on the SNWs synthesis and sensor applications has been achieved in the past two decades.37,233–235
Till date, the synthesis of SNWs nanowire is generally categorized as vapor-phase growth, solution-phase growth, and template synthesis.236,237 Here, we will focus the discussion of
nanowire synthesis on several important SNWs corresponding
to group IV, group III–V, group II–VI, and metal oxide compounds. Similar to the MNWs, the synthetic methods andmolecular sensing applications of SNWs in the past two
decades have been summarized in Table 2.
2.2.1. Group IV SNWs synthesis. Si nanowire is one of themost important semiconductor nanostructures in group IV,
and extensive eﬀorts have been devoted to the synthesis of Si
nanowires with controlled structure, doping, and electronic
structures.238–240 Recently, numerous methods have beendeveloped to fabricate Si nanowires, which can be generallyclassified as vapor–liquid–solid (VLS) processed bottom-up
approaches and chemical etching assisted top-down
approaches.239–246 Si nanowire VLS growth is a nanoclustermediated crystal self-assembly process.240,241,247 The specificgrowth mechanisms are depicted in Fig. 4(a). Metallic catalyst
nanoclusters, such as Au, are firstly ablated by laser or hightemperature. As the Si vapor sources (e.g., SiH4 and Si2H6) are
fed to the metallic catalyst at an elevated temperature, a liquid
metal/Si eutectic alloy is formed. Subsequently, with thefurther accumulation and decomposition of Si vapor source atthe vapor–liquid interface, the alloy reaches a supersaturated
state, and silicon starts to precipitate, forming a liquid–solidinterface. Furthermore, with the continuous process of Sivapor source adsorbing at the vapor–liquid interface and thentransferring to the liquid–solid interface, the Si nanowires areanisotropically grown below the metal nanoclusters.247
Germanium (Ge) and silicon carbide (SiC) nanowires are two
promising semiconductor nanowires in group IV.248–251 They
can also be well grown via the nanocluster-catalyzed VLS
process. Based on the VLS growth mechanism, well-definedp-type and n-type Si nanowires are obtained and successfully

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Critical Review
integrated as electronic sensor devices for the detection of biological and chemical species.252–256 Lieber’s group firstly
demonstrated that the boron-doped silicon nanowire ( p-type)
integrated FET device can be used for ions (H+, Ca2+) andprotein (streptavidin) detection.232 In addition, Lieber’s groupfurther confirmed that Si nanowire FET devices also can serveas high performance sensor electronics to electrically detect
single virus particles.257 Apart from the detection of ions andbiological molecules, Haick et al. have proved that molecularly
modified SiNW FET device allows the highly accurate detectionof volatile organic compounds (VOCs) in both single-component and multicomponent mixtures.258
In contrast to the harsh conditions for the VLS growth of Si
nanowires, chemical etching is a simple and low-cost method tofabricate highly crystalline Si nanowires within the Si
wafer.243–246 Currently, various etching techniques, including
reactive ion etching (RIE), electrochemical etching, and metalassisted etching, are developed to obtain high density Si
nanowires.244,259,260 Among these approaches, metal-assisted
etching has attracted considerable interest since it enables theSi nanowire fabrication with controllable morphology (e.g.,cross-sectional shape, diameter, length, orientation, doping
type, and doping level), as shown in Fig. 4(b). In a typical metalassisted chemical etching procedure, a selected area of the Si
wafer is firstly covered by noble metals after film deposition.
Then, the Si wafer is subjected to an etchant composed ofhydrofluoric acid (HF) and oxidative reagent (H2O2). Since the
Si beneath the noble metal presents a faster etching rate thanthat of Si without noble metal coverage, the noble metals sink
into the Si substrate vertically and generate orientated pores on
the Si wafer. As a result, single crystalline and highly oriented Si
nanowires are formed. For example, Kim et al. used Au layer asa catalyst and successfully realized wafer-scale graphene/Si
nanowire array fabrication, and this heterostructure integrated
molecular sensor showed huge (1280%) resistance changes andfast response/recovery (12/0.15 s) times toward H2.261
In addition, high regularity of Si nanowire array can beobtained as the electron-beam or nanoimprint lithography
techniques are utilized to design dot array pattern on the Si
wafer.262–264
2.2.2. Group III–V and II–VI SNWs synthesis. Similarly,
VLS-catalyzed growth is also a promising approach for the synthesis of group III–V (e.g., GaN, GaSb, GaAs, InAs, and InP)
and II–VI (e.g., ZnS, CdS, ZnSe, and CdTe) semiconductor
nanowires.265–276 For example, Duan et al. reported a laserablation technique to synthesize high-quality, single-crystal
GaAs, GaP, GaAsP, InAs, InP, InAsP, ZnS, ZnSe, CdS, and CdSe
semiconductor nanowires using Au as a catalyst.277 Chen et al.
have demonstrated that high-purity and -quality GaN nanowires can be obtained using metals (In, Co, Ni, Fe) and alloys(Ni/Co and Fe/Co) as catalysts via controlled VLS growth.278
Furthermore, such kinds of nanowires can also be synthesized
via a catalyst-free molecular beam epitaxy (MBE) growthmethod, which avoids unintentional catalyst doping during
the nanowire VLS growth.279 The MBE growth has stringent
requirements for the growth parameter (e.g., ultrahigh vacuum

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Ternary
semiconductor
Quaternary
semiconductor

Solution deposition440

InAs

InN
SiC

TCVD;428 metal organic chemical vapor deposition (MOCVD);429,432 low-pressure
metalorganic vapor-phase epitaxy (LP-MOVPE);430,431 MBE433–435

CVD;417,418,420 MBE419
Carbothermal reduction;421,425 CVD;422,423,427 electrospinning;424 VLS426

VLS;387 CVD;388 Ge-condensation technology389
Oxidative chemical vapor deposition (oCVD)390
VLS;405 CVD;396–401,406,413–416 thermal chemical vapor deposition (TCVD);394,395,404 plasma
enhanced chemical vapor deposition (PECVD);391–393,408 molecular beam epitaxy (MBE);410–412
hydrothermal;409 top-down microfabrication technique402,403,407

DNA440

VLS;232,288,293,294,299,311,318,319,322,347,353,378,385 chemical
etching;254,261,286,287,290,296,298,303–310,312–314,326–329,331,332,334,349,352,366 in-planesolid–liquid–solid (IPSLS);289 top-down microfabrication
technique;263,291,297,300–302,315–317,323,335–338,340,341,343–346,350,354–357,359–361,363,364,368–372,374–377,381–384,386
oxide-assisted growth;292,295,325,330,333,348,351 CVD;9,257,320–322,342,358,362,365,367,373,379,380 electrospinning339

Synthetic method

Cu2CdSnS4

261

CVD;436 chemical beam epitaxy437
CVD438
Solvothermal method439

Ge
GaAs
GaN

Binarysemiconductor

261,298–304

InP
InSb
Zn1−xCdxSSi

Singlesemiconductor

232,286–297

Analytes

NH3;
H2;
O2; NO/
NO2;263,305–308 H2O;309–311 H2S;312
ethanol;313 formaldehyde;314 2,4,6-trinitrotoluene (TNT);9,315 nerve agent;316,317
VOCs;318–324 H2O2;325–329 glucose;325,330–333
pH;334–346 K+;347 heavy ions;254,348–351 hydrazine;352 exhaled breath VOCs;353 DNA/
RNA;354–361 virus;257,360,362–369
protein;370–383 tumor cell;384 action potentials (APs)385,386
H2O;387 pH;388 DNA389
Methanol, toluene390
Ar, N2, methane;391–393 H2;392,394–400
H2O;401 SO2;402,403 NO/NO2;402,404–409 CO/
CO2;392 alchohol;410 aromatic compounds;411 TNT;412 DNA413–416
H2;417 NO2;418–420 NH3 420
H2;421 H2O;422,423 NH3;424 nitrite;425
DNA;426 reactive oxygen and nitrogenspecies427
H2O;428,429 NO/NO2;429–432 ethanol;428
acetone;428 isopropanol;428 acetic acid;433
pH;434 proteins;434 cell435
CO, CH4;436 DNA437
NO2 438
Ethanol439

Materials

Summary of Si nanowire, group III–V and II–VI semiconductor nanowires (SNWs) synthesis and their molecular sensing applications

Class

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AnalystFig. 4 (a) Typical vapor–liquid–solid (VLS) growth mechanism of nanowire. SEM image is reproduced from ref. 243 with permission from AIP
publication, copyright 2007. (b) Metal-assisted chemical etching
methods of silicon nanowire synthesis. SEM image is reproduced fromref. 326 with permission from American Chemical Society, copyright2014.

and lattice matched growth substrate), which impede its wide
applications in the versatile SNWs growth.280,281
As another important approach to synthesize nanowires interms of bottom-up strategy, solution synthesis has been
widely used for the group III–V and II–VI semiconductor nanowire growth.282 Korgel et al. proposed a Bi nanocrystal seedsolution–liquid–solid (SLS) growth of crystalline high aspectratio GaP, GaAs, InP, and InAs nanowires in conventional solvents, such as trioctylphosphine (TOP), trioctylphosphineoxide (TOPO), and trioctylamine (TOA), at 320–340 °C.283 Yanet al. demonstrated a hydrothermal synthesis route for the
wurtzite ZnS nanowire preparation with a low temperature(180 °C) in the presence of ethylenediamine (en).284 Li et al.
presented a simple synthetic route for the production of highquality CdS, CdSe, and CdTe nanowires in diﬀerent organic
solvents.285 However, because inevitable contamination or
doping usually occurred during the growth of nanowires in solvents, the electronic properties of solution-grown nanowires
are far from that of nanowires grown via the vapor phase. In
addition, the synthetic methods and molecular sensing applications of group III–V and II–VI SNWs in the past two decades
have been summarized in Table 2.
2.2.3. Metal oxide SNWs synthesis. Metal oxide semiconductor nanowires, such as ZnO, SnO2, and WO3, areanother promising class of nanostructures that have been
widely studied for molecular sensor electronics.441–443 In
recent decades, significant eﬀorts and progress have been
made, and many methods have been developed to synthesize
1D metal oxide SNWs, including PVD, CVD, PLD, thermal oxi-

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Critical Review
dization and solution-based growth for single-crystalline nanowires, and template growth and electrospinning for polycrystalline/amorphous nanowires. The synthetic methods and molecular sensing applications of SNWs have been summarized inTable 3. Following the VLS-catalyzed Si SNWs growth by the
Lieber group in 1998,444 VLS based growth concept has been
intensively applied for the metal oxide nanowire growth. In
recent years, Yanagida et al. has made great eﬀorts in the VLS
growth of metal–oxide nanowires.102,103,105,107,112,115,122,445,446
They have pointed out that material flux is an important variable, which has been underestimated in VLS nanowire growth.
In terms of the proposed “material flux window” concept(Fig. 5(a)), numerous single crystalline nanowires, such as SnO2,
In2O3, ITO, ZnO, NiO, MnO, CaO, Sm2O3, Eu2O3, and MgO,
have been successfully synthesized.103,115 Meanwhile, nanowire
heterostructures, which include core/shell heterostructures,axial/radial heterostructures, and other irregular heterostructures, can be properly achieved by rationally controlling the
growth parameters during the VLS process.116,447 For example,
via precisely controlling the material flux within an order ofmagnitude, the structure and composition of VLS growth ITO
nanowires can be altered from Rutile structure (Sn 100%, In0%) to Fluorite structure (Sn 28%, In 72%) and Bixbyite structure (Sn 21%, In 79%),112,122 as shown in Fig. 5(b).
Owing to the metal oxide SNWs that are grown via VLS
mechanism having a high surface to volume ratio, single crystallinity, and well-defined crystal orientations, they oﬀer an
ideal platform for nanoscale sensor integration due to theirhigh surface to volume ratio, Debye length comparable size,
excellent surface chemical reaction, and low power
consumption.58,448,449 For example, Morante et al. successfully
realized the growth of single crystalline SnO2 nanowires by
CVD method based on VLS mechanism, and it is indicatedthat the single SnO2 nanowire integrated sensor device showsa high sensing response and stability toward CO and humidity.450 Ho et al. demonstrated a monoclinic β-Ga2O3 nanowire
growth using the VLS technique along with the Au catalyst,
and the single nanowire gas sensor fabricated by the proposed
Au decorated β-Ga2O3 nanowire achieved remarkable sensitivity for 100 ppm CO gas at room temperature.451
1D metal oxide SNWs can also be directly formed from thevapor phase into the solid phase, that is, the vapor–solid (VS)growth in the absence of a metal catalyst. Recently, various
metal oxide nanowires, such as Ga2O3, ZnO, SnO2, TiO2, andWO3,452–459 have been successfully synthesized via VS growth.
In view of the current studies, VS growth mechanisms are generally concluded as three types: (1) the anisotropic growthmechanism: nanowires can be synthesized via the preferential
reactivity and binding of gas reactants on a specific surface tominimize the total surface energy;460–462 (2) the defect-induced
growth (or screw dislocations) mechanism: the growth of thecrystal proceeds by adding atoms at the kink sites of a surface
step;463–466 (3) the self-catalytic growth mechanism: metaloxide can be decomposed into metal and oxygen by heating
under vacuum condition, then the metal vapors are condensed, forming liquid droplets on a lower temperature sub-AnalystView Article Online

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Table 3Class

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SingleMOS

Summary of metal oxide semiconductor (MOS) nanowire synthesis and their molecular sensing applications

Materials
ZnO

SnO2

TiO2

WO3/
W18O49In2O3

CuO/Cu2O

NiO/Ni
(OH)2

Co3O4
Fe2O3
Ga2O3
TeO2

BinaryMOS
Ternary
MOS

AnalystVO2/VOx
CeO2
MnO2
ZnCo2O4
ZnWO4
ZnFe2O4
Na2Ti3O7
CuNiCoO4

Analytes
48,496–500

Synthetic method
501

502

498,499,503–506

O2; O3; CO;
H2;
NH3;507–510 NO/NO2;108,498,511–515 H2S;516,517
SO2;518 acetone;519 ethanol;441,520–522
benzene;523,524 toluene;523,524
formaldehyde;525,526 nonanal;527 K+;528
streptavidin;529 uric acid;530–532 dopamine;530 ascorbic acid;530 ammonium;533
levodopa;534 glucose;535,536 hydrazine;537,538
protein;539 DNA540
H2;49,234,541–547 O2;448,548 O3;502 H2O;443,549
CO2;34,448,450,541,543,550–553 NH3;234,547,554,555
NO2;58,234,548,556–567 H2S;547,568–571 SO2;548
Cl2;572 ethanol;234,547,550,552,564,573–575
acetone;234,576 isopropanol;54,550
benzene;234 toluene;577 formaldehyde;578,579
liquefied petroleum gas;555 cyclodextrin;580
methane;551 heavy ions;581 protein;582
DNA583
H2;584,585 H2O;586 CO;587 NH3;588
ethanol;589–593 methanol;589 isopropanol;589
toluene;594 xylene;594 pH;595 H2O2;596
glucose;597 phospholipid/phosphopeptide;598 listeria monocytogenes;599
protein;600 glutathione;601 DNA602
H2;442,603–607 O3;608 CO;609 NH3;610–615 NO/
NO2;609,616–619 H2S;608,620,621 ethanol;622–624
acetone;479,625,626 n-butanol;627,628 exhaled
breath VOCs;620 formaldehyde;622 triethylamine;629 nonanal;99,100,106 pH;630 rhodamine B;631 rhodamine 6G;632 methyl red632
H2;633,634 O2;635 O3;502 CO;636,637 NO2;471,638
H2S;639 ethanol;640–642 acetone;643–645 formaldehyde;646 SARS virus;647 RNA;648
DNA649H2;650,651 H2O;652 CO;493,653–656 NH3;657,658
NO2;659,660 H2S;661 ethanol;662,663
glucose;657,664–671 H2O2;672,673 DNA674
H2;675 NO/NO2;676,677 NH3;678 methanol;679
ethanol;476,679–682 formaldehyde;683
acetone;679,680 trimethylamine;679
toluene;679 acetaldehyde;681 acetylcholine;681 glucose684
Acetone;685 trimethylamine;686 glucose;687
H2O2;688 dopamine689
CO;690 H2S;691 ethanol;690,692,693 acetone;694
glucose695
H2;696,697 O2;698 CO;451,698–701 NO;404
acetone;404 isopropanol;702 nitromethane;703 trimethylamine703,704
H2;705 NO2;706–709 NH3;709 H2S;709
ethanol;710,711 isopropanol;712 H2O2 713
H2;714 NH3 715
H2O;716 CO;717 H2S;478 H2O2 718
Glucose719
Formaldehyde;720 glucose721
Chloramphenicol722
H2S;723 acetone724
H2O;725 H2O2 726
Glucose727

strate, and such droplets are the ideal catalysts for metal oxide
nanowire growth, as shown in Fig. 6. Compared with the VLS
growth, VS growth nanowires suﬀer from insuﬃcient ability tocontrol uniformity, which usually results in a tapered morphology of nanowires.

AnalystHydrothermal
method;108,499,500,503,508,515,517,518,521,524,525,527,528,531,533,535,538,539 VLS
method;523,529,540 CVD;48,441,497,498,501,504–506,511,519,520,522,530,532,534,537
PECVD;526 carbothermal reduction;509,510,512,514,516 thermaloxidation;513,536 evaporation–condensation technique;502 templateassisted method;507 nanoscale spacer lithography496

Hydrothermal method;569,570 polyol method;552,581 precipitation
method;541 spray pyrolysis process;551,566,568 VLS
method;58,546,548,549,556,576,579,580 VS method;54,450,543,550
CVD;234,443,547,571,572,574,582 thermal
evaporation;49,542,544,545,553–555,557–562,564,565,573,575,583 evaporation–condensation technique;502,567 template-assisted method;448
electrospinning;577,578 LPNE technique563
Hydrothermal method;586,588,589,594–598,600,601 thermal evaporation;584,585
sol–gel method;602 spray pyrolysis process;590 electrospinning;587,592 LPNE
technique591,593

Hydrothermal method;99,100,106,479,604,606,610,611,615,619,622,623,625,627,629
solvothermal method;605,612–614,628,631 electrochemical etching;632 VLS
method;608 aerosol-assisted chemical vapor deposition (AACVD);620
thermal evaporation;442,607,609,620,621,624 thermal oxidation;603,616,618
electrospinning;626,630 nanocasting method617
Hydrothermal method;471 VLS method;635,636,638,640,644,645,649
CVD;633,634,636,637,647 thermal evaporation;641,643 evaporation–condensation technique;502 template-assisted method;646 LPNE technique;648
electrospinning639,642
Hydrothermal method;662 precipitation method;657 liquid–solid (LS)growth method;665,668 thermaloxidation;493,650,651,653,654,656,658–661,663,664,666,672,674 CVD;652
anodization667,669–671,673
Hydrothermal method;476,676,679,683 chemical reduction;678 VLS;675,677,680
electrodeposition;681 nanocasting method;682 electrospinning684

Hydrothermal method; solvothermal method689
Hydrothermal method;690,692 solvothermal method;695 thermal oxidation;694 nanocasting method;693 electrospinning691
Hydrothermal method;699 thermal evaporation;696,698,700–702
VLS404,451,697,703,704
Thermal evaporation;705,706,708–713 VLS707
CVD;714 solvothermal method715
Hydrothermal method478,716–718
Hydrothermal method719
Hydrothermal method720,721
Hydrothermal method722
Solvothermal;724 electrospinning723
Hydrothermal method725,726
Hydrothermal727

The solution-phase growth, for example, the hydrothermal
growth, is extensively used for the synthesis of metal oxide
nanowires.99,100,106,123,467 Compared with the vapor phasegrowth (both VLS and VS), a much lower temperature isrequired for the solution growth, which allows the nanowires

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Fig. 5 (a) The concept of “material ﬂux window” for nanowire growth (VLS, vapor–liquid–solid; VS, vapor–solid). Reproduced from ref. 103 withpermission from American Chemical Society, copyright 2016. (b) VLS growth of SnO2 nanowire under the guidance of ‘material ﬂux window’.
Reproduced from ref. 103 with permission from American Chemical Society, copyright 2016. (c) VLS growth of TiO2 nanowire. Reproduced from ref.
445 with permission from American Chemical Society, copyright 2012. (d) VLS growth of ITO nanowires. Reproduced from ref. 122 with permission
from American Chemical Society, copyright 2013.

Fig. 6 A typical vapor–solid (VS) growth mechanism in nanowire fabrication. SEM image is reproduced from ref. 459 with permission from
American Chemical Society, copyright 2015.

to be directly integrated on flexible organic substrates formodern wearable devices. In addition, the morphology andproperties of the solution phase growth nanowires can be conveniently manipulated by tuning the concentration of the composition, introducing additional composition, or adding additives to the solvent. Currently, many kinds of nanowires, suchas SnO2, ZnO, TiO2, In2O3, MnO2, and WO3, have been successfully synthesized via solution-phase growth with/without
the assistance of the seed layer.106,468–478 Their growth can beclassified as seed-assistant and seed-free growth, as shown in
Fig. 7. Owing to the low cost, less hazardous, no metal catalysts, the eﬀectively controllable morphology and properties,

This journal is © The Royal Society of Chemistry 2021

the solution phase growth strategy has been successfully integrated into a well-developed micro-electro-mechanical system(MEMS).69,479,480 For example, in terms of the “material flux
window” strategy proposed for nanowire VLS growth, theYanagida research group intensively investigated the seedassistant ZnO nanowire growth, and they also demonstrated
that there existed a “concentration window” in the ZnO nanowire growth. By carefully controlling the concentration of Zn
ionic species within a specific concentration range, selective
growth on the (0001) plane can be realized.481 Meanwhile,with the guidance of the “concentration window” concept,
Sakai et al. achieved a significant improvement in the growthrate of ZnO nanowires (up to 2000 nm h−1) with the assistanceof ammonia.482 Taking WO3 nanowire growth as an example
for the seed-free method, Zhang et al. have successfully fabricated ultra-long h-WO3 nanowires up to the millimeter range(1.2 mm) for a wider range of precursor concentrations
through the hydrothermal method.106 They also demonstrated
the feasibility of these millimeter-long h-WO3 nanowires forthe electrical sensing of molecules (lung cancer biomarker:
nonanal) on flexible substrates, which can be operated atroom temperature with mechanical flexibility with bending
cycles up to 104 times due to the enhanced textile eﬀect.
Besides, thermal oxidation, template-assisted deposition,and electro-spinning methods have been developed to syn-AnalystView Article Online

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AnalystFig. 7 Hydrothermal/solvothermal growth of metal–oxide semiconductor nanowire (a) with and (b) without the seed layer. SEM images of ZnO
nanowire is reproduced from ref. 527 with permission from Royal Society of Chemistry, copyright 2021. SEM image of WO3 nanowire is reproduced
from ref. 99 with permission from Royal Society of Chemistry, copyright 2021.

thesize functional metal oxide SNWs,483–495 as shown in Fig. 8.
For instance, Steinhauer et al. demonstrated a facile method togrow CuO nanowires via direct thermal oxidization of Cu foil,
and it is shown that the CuO nanowire integrated sensor
device presented a high sensing performance to 30–100 ppm
CO molecules.493 Hussain et al. reported a template-assisted

sol–gel method to fabricate well-aligned 1D ZnO nanowires forCO2 molecular sensing.495 Nikfarjam et al. proposed a novel
electro-spinning procedure to fabricate single-aligned TiO2
nanofibers and integrate them into a sensor to electricallydetect CO.485 Furthermore, the electro-spinning technique has
attracted increasing attention in the commercial field of mole-Fig. 8 (a) Thermal oxidization method of metal–oxide semiconductor nanowires. SEM images of ZnO nanowires is reproduced from ref. 491 withpermission from American Chemical Society, copyright 2013. (b) Electrospinning method of metal–oxide semiconductor nanowires. Reproduced
from ref. 494 with permission from American Chemical Society, copyright 2014.

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cular sensor fabrication due to its simple and inexpensive fabrication process.

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2.3. Electrically conducting polymer nanowire (PNWs)
synthesis
Since the discovery of polyacetylene in the 1970s by Hideki
Shirakawa, Alan Heeger, and Alan MacDiarmid and coworkers,84,85 significant eﬀorts have been devoted to the development and synthesis of electrically conducting PNWs for themonitoring and detection of chemical and biological analytes,
and the preparation approaches can be mainly divided into
the template-assisted method and the template-freemethod.728 The synthetic methods and molecular sensing
applications of SNWs have been summarized in Table 4.
The template-assisted method was firstly explored byMartin and Parthasarathy by employing aluminum oxide(AAO), commercial track-etch membranes (PTM), and porous
diblock copolymer films as “hard” templates to synthesize conducting polymer nanowires, such as polyacetylene, polypyrrole,
polythiophene, and polyaniline.729–731 The specific nanowire
synthesis processes are shown in Fig. 9(a). Within the pores ofthese templates, electrically conducting PNWs can be obtainedby oxidative polymerization of the corresponding monomer via
a simple chemical oxidization method or electrochemical
polymerization.732–734 Chemical oxidization synthesis is generally accomplished by simply immersing a template membrane
in a solution with the desired monomer, oxidant, dopant andthen allowing monomer polymerization within the pores.735
By controlling the polymerization time, diﬀerent types ofnanostructures can be produced.734–737 For the electrochemical synthesis, a metal film is usually coated on thesurface of the template membrane, and then electrochemical

polymerization of the desired polymer within the pores of thetemplate is carried out.738–740 As compared to the chemical
oxidization method, the electrochemical polymerization
method is more complex and has a high cost, but it is more
controllable by tailoring the current density, applied potential,
and polymerization time. Polypyrrole was one of the first conducting polymers to be applied for gas sensing materials.741
Using FeCl3 as the oxidizing agent, Hernandez et al. realized
the chemical polymerization of pyrrole in SiO2 coated alumina
membrane.742 It is shown that hundreds of nanometers inlength and 50 to 60 mm of polypyrrole nanowires can beachieved, and the single polypyrrole nanowire integrated
sensor device exhibits good sensitivity to 40 ppm of ammonia.
Ramanathan et al. demonstrated a simple, one-step method
for fabricating a single biologically functionalized conductingpolymer ( polypyrrole, polyaniline) nanowire on pre-patterned
electrodes by electrochemical polymerization route in alumina
template.743 The as-fabricated nanowire sensor generated a
rapid change in resistance upon the introduction of biotinDNA, and the limit of detection can be as low as 1 nm.
The template-free method, which is also called as the softtemplate or self-assembly method, is another relatively simple,
cheap, and powerful approach to synthesize electrically conducting PNWs since it requires no template and no post-treatment
for template removal.744 The specific nanowire synthesis processes are as shown in Fig. 9(b). To date, chemical oxidative
polymerization, interfacial polymerization, and electrochemical
deposition have been employed as general template-freemethods to assemble conducting PNWs. For example, Pal et al.
applied a standard chemical oxidization method to synthesize
polyaniline nanowires in the presence of ammonium persulfate
as oxidizing agent for the detection of foodborne pathogen,

Table 4 Summary of electrically conducting polymer nanowire (PNWs) synthesis and their molecular sensing applications

Class
Singlepolymer

Materials
Polyaniline (PANI)

Polypyrrole (PPy)Copolymer

Polythiophene (PT)
Poly(3-hexylthiophene)(P3HT)
Poly(3,4ethylenedioxythiophene)(PEDOT)PEDOT-PSS

Analytes
753,754

Synthetic method
755

749

H2O; CO;H2;
NH3;746,747,753,756–759 NO2;760 H2S;761
volatile sulfur compounds (VSCs);748
cigarette smoke;762 pH;763–765 heavy
ions;766,767 chloramphenicol;768
H2O2;764 carcinoembryonic antigen;769
cardiac biomarkers;770 protein;771
Bacillus cereus;745 DNA772,773
H2;774 NH3;742,775–777 pH;190,765,778
Cu2+;779,780 nitrite;781–784
glucose;785–787 H2O2;788,789 CA 125 biomarker;790 protein;791 mRNA;789,792
DNA793Chlorpromazine;794 protein795
NH3 796
H2O;797 methanol;797,798 ethanol;797
acetone;797 Fe3+;799 DNA;800 antibody;751 nitrite;801 protein802
NH3;63 NO/NO2;63,752 p-xylene;62,803
acetone;62,803,804 methanol;804
ethanol;62,804 hexane;62 isopropamide;62 streptavidin;81 prostate
specific antigen (PSA);81 Escherichia
coli (E. coli)81

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Lithographically patterned growth;753,758 interfacial
polymerization;746,747,760,769 electrochemical
polymerization;748,749,761,763,765,767,768,770–773 template-freemethod;745,762,764 template-assisted method;754,756 galvanostatic method;766 electrospinning755,757,759

Electrochemical polymerization;81,190,774,776,780–790,792,793
chemical oxidative polymerization;779,791 template-assisted
method742,765,775,777,778
Electrochemical polymerization794,795
Liquid-bridge-mediated nanotransfer molding (LB-nTM)
process796
Electrochemical polymerization;797,798,800–802 LPNE
technique751,799
Electrochemical polymerization;804 soft lithography;62,63,803
dip pen nanolithography (DPN)752

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AnalystFig. 9 (a) Template-assisted method of PNWs growth. SEM image is reproduced from ref. 730 with permission from American Chemical Society,copyright 2015. (b) Template-free method of PNWs growth. Reproduced from ref. 744 with permission from American Chemical Society, copyright2018.

Bacillus cereus.745 Huang et al. reported a facile chemical routeto synthesize high-quality polyaniline nanofibers underambient conditions using aqueous/organic interfacial polymerization.746 The polyaniline nanofiber integrated thin film sensor
showed superior performance in both sensitivity and time
response to hydrochloric acid (HCl) and ammonia (NH3) gas
molecules. Virji et al. also demonstrated an interfacial polymerization method for the synthesis of polyaniline nanofibers andapplied them for HCl and NH3 sensing.747 Liu et al. realized thefabrication of polyaniline (PANI) nanofibers via electrochemical
polymerization approach and used for the detection of CO contained in hydrogen fuel and volatile sulfur compounds (VSCs)of human expired breath.748,749
In addition to the above-mentioned template-assisted
method and template-free method, other approaches, such as
electro-spinning,750 lithographically patterned nanowire electrodeposition (LPNE) process,751 dip-pen nanolithography(DPN),752 and mechanical stretching732 have also been used toprepare electrically conducting PNWs for the detection ofchemical and biological molecules.

3. Working principles of 1D
nanowire-based molecular sensors
To study the intrinsic properties of nanowires and use their functionality as a sensing element, one necessary process is transfer-Analystring nanowires from the growth substrate and integrating themwith contact electrodes on a platform. To date, the molecule
sensor electronics can be classified as chemiresistive type, electrochemistry type, and field-eﬀect transistor (FET) type of sensor
devices based on their electrical measurement strategy.20,26,29
3.1.

Chemiresistive type nanowire sensor

The basic principle of chemiresistive sensors is the chemicalinteraction between the target molecules with the sensor
surface resulting in electrical conductance variation.805 In particular, a change in electrical conductance is measured as afunction of time for a known amount of exposed molecules,
and the electric conductance can be measured by a simple
ohmmeter. This type of sensor is usually applied for gas molecule detection and analysis. Chemiresistive molecular sensors
based on 1D nanowires are often realized using a single nanowire, a multiple nanowire film, or bridged nanowire structures,as shown in Fig. 10.
Currently, metal oxide semiconductors are the most extensively investigated sensing structures for gas sensing, and their
sensing mechanisms have been intensively studied.805 The
operation of metal oxide-based gas sensors is currently
described by two diﬀerent models, the ionosorption805 andoxygen vacancy theory model.806 The ionosorption model considers that the sensor electrical conductivity fluctuation originates from the space-charge eﬀects/changes of the electricsurface potential, which result from the “ionosorption” ofThis journal is © The Royal Society of Chemistry 2021

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Fig. 10 (a) Single nanowire sensor device for molecular sensing. Reproduced from ref. 99 with permission from Royal Society of Chemistry, copyright 2021. (b) Multiple nanowire ﬁlm sensor device for molecular sensing. Reproduced from ref. 108 with permission from American Chemical
Society, copyright 2019. (c) Bridged nanowire sensor device for molecular sensing. Reproduced from ref. 498 with permission from American
Chemical Society, copyright 2013.

gaseous molecules. With regard to the oxygen-vacancy model,
it explains the sensing eﬀects by changes in the oxygen stoichiometry, that is, by the amount of variation of the surface
oxygen vacancies and their redox mechanism.
3.1.1. Chemiresistive sensor based on ionosorption model.
With regard to the ionosorption model, the key in the mechanistic description of gas sensing is the ionosorbed oxygenions.805 Taking n-type semiconductor oxide as an example,
when a sensor is exposed to the atmosphere, oxygen can beadsorbed on the surface of the oxide nanowire and becomes
negatively charged ionic species (O2−, O−, and O2−). Suchoxygen charged behaviour would extract electrons and create ashell-like surface depletion layer on the nanowire surface,which can eﬀectively modulate channel conductivity. As thesensor is exposed to reducing gases (such as toluene, ethanol,
CO, NH3, H2, and methanol), the charged oxygen can reactwith these gases and release electrons back to the nanowire
bulk. As a result, the thickness of the depletion layer shrinks,
leading to an increase in conductance. In contrast, when thesensor is exposed to oxidizing gases (such as NO2, O3), theseThis journal is © The Royal Society of Chemistry 2021

gases can extract more electrons from the nanowire surface.
Then, the depletion layer thickness increases and results in a
reduction of nanowire conductance. The detailed working
mechanisms are shown in Fig. 11. Due to its convenience indata analysis, tremendous works have used the Ohmic contacted nanowire device as a platform for fundamental studies
to improve the device sensing performance.98,234,776 The gas
sensing mechanism of group IV (such as Si SNWs), group III–V
and group II–VI SNWs, and electrically conducting PNWs are
similar to the ionosorption sensing mechanism that isreported for metal oxide semiconductors.734,807–809 In the caseof n-type semiconductors, the reaction with reducing gases
decreases their conductivity, while oxidizing gases increase theconductivity (for p-type semiconductors, it is opposite).810,811
3.1.2. Chemiresistive sensor based on oxygen-vacancy
model. The oxygen-vacancy model focuses on the redox molecule on the surface oxygen vacancy sites, which are consideredas the determining factor in the chemiresistive behaviour.806
Considering an n-type semiconductor oxide, for example, theoxygen vacancies (VO) are the dominating donor defects, which

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AnalystFig. 11 The detailed working mechanism of the chemiresistive sensor based on ionosorption model. Taking single nanowire sensor device as an
example. R: reducing gas; D: oxidizing gas; CB: conduction band.

serve as active sites for the molecule redox reactions that arecontrolled by gaseous oxygen. During the alternate reduction
and reoxidation of surface oxygen vacancies between thegaseous oxygen and sensing molecules, the conductivities ofsensing materials remarkably change and therefore the overallsensing behaviour. In this model, the mechanism to the reducing gases (R) is represented as follows: (1) reducing gas molecules remove surface lattice oxygen to give oxidation products(RO), thereby producing an oxygen vacancy; (2) the vacancy
becomes ionized at a certain temperature, thereby releasing
electrons into the conduction band and increasing the conductivity; (3) at the same time, the oxygen molecules fill the vacancy
and trap one or more electrons from the conduction band,
which results in the decrease in conductivity. While for thesensing mechanism to the oxidizing gases (D), their electron
exchange process on the oxygen vacancy sites are similar to thatof gaseous oxygen: (1) introduced oxidizing gas molecules are
directly bonding to the oxygen vacancy sites and trap the electrons from the conduction band, leading to a decrease in conductivity; (2) as the oxidizing gas molecules are desorbed fromthe oxygen vacancy sites, their trapped electrons are released tothe conduction band, which increases the sensor conductivity.
The detailed working mechanisms are shown in Fig. 12.

Analyst

3.2.

Electrochemical type nanowire sensor

Due to the merits of short analytical time, low power cost, highsensitivity, and easy adaptability for in situ measurement,
electrochemical detection methods have attracted great interestin the detection of chemical analytes (such as heavy ions) andbiological molecules in the liquid phase.26,39,75–77 The electrochemical detection is normally performed with a three-electrodesystem containing a working electrode (WE), a reference electrode (RE), and a counter electrode (CE), as shown in Fig. 13.
The WE serves as the transduction element in the biochemical
reaction, while the CE establishes a connection to the electrolytic solution so that a current can be applied to the working
electrode.26 These electrodes should be both conductive andchemically stable. The WE can be modified with diﬀerent 1D
nanowire structures for specific recognition or/and concentration of metal ions.79 The binding of chemical or biologicalmolecules on the WE causes the change in current, potential,
electrochemical impedance, capacitance, or electrochemiluminescence, which can then be used for their detection. The
working mechanisms of the electrochemical sensor are clearly
depicted in Fig. 13. Based on these detection signals, theelectrochemical sensing principles can be classified into

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Fig. 12 The detailed working mechanism of the chemiresistive sensor based on oxygen vacancy model. Taking single nanowire device as an
example: reducing gas; D: oxidizing gas; VOX: oxygen vacancy; VO•: singly ionized oxygen vacancy; VO••: doubly ionized oxygen vacancy; CB: conduction band.

amperometric,28,812–814 potentiometry,25,27 electrochemical
impedance,815–817 capacitance,24 and other methods.818
3.2.1. Amperometric
type
electrochemicalsensor.
Electrochemical molecular sensing in terms of amperometricmeasurement is a type of sensor that operates under a continuously measured current resulting from the oxidation or
reduction of an electroactive species in a chemical/biochemical
reaction.28,812 Typically, the current measured under a constant potential is referred to as amperometry, and this issimilar to the chemiresistive type molecule sensing measurement. From the view of the principle, the peak intensity of themeasurement current over a linear potential range is directly
proportional to the concentration of the analyte species.812,819
When a current is measured during controlled variations of
the potential, this is referred to as voltammetry. Usually, theelectroactive species reacting on the working electrode have a
specific electrochemical cell potential, also known as redox
potential. At the redox potential, ions are adsorbed or desorbed on the working electrodes, which results in electron
exchange between the analytes and the electrodes. ElectronThis journal is © The Royal Society of Chemistry 2021

transfer induces an electrical current flow between theworking and the counter electrodes in the electrolytic cellsystem, which in turn produces an amperometric response.
This sensing response is frequently analysed with a cyclic voltammetric (CV) current peak, as shown in Fig. 14(a). Recently,
these types of electrochemical sensors are usually applied forthedetectionofgas
molecules,352,537,538,657,715
191,425,782,801
ionsand biological molecules.131,135,173,194 A
typical amperometric sensor is the Clark electrode, which is anelectrode that measures ambient oxygen concentration in aliquid using a catalytic platinum surface according to the net
reaction (O2 + 4e− + 4H+ → 2H2O), and it is demonstrated thatthe produced current is proportional to the oxygen concentration.820 Furthermore, Kurowska et al. fabricated a novel
amperometric sensor based on a silver nanowire (Ag NW) arrayfor the rapid and sensitive detection of hydrogen peroxide(H2O2) in the liquid phase, and it is shown that the detection
limit of this amperometric sensor can be close to 29.2 μM.151
Wang et al. demonstrated that the PPy nanowire modified electrode can detect NO3− at the micromolar level.782 A very impor-

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Fig. 13

AnalystGeneral setup for electrochemical detection of target molecules and their working mechanisms.

Fig. 14 Typical electrochemical sensor that is integrated by nanowire nanostructures. (a) Amperometric type of electrochemical sensor.
Reproduced from ref. 148 with permission from Elsevier, copyright 2009. (b) Potentiometric type of electrochemical sensor. Reproduced from ref.
170 with permission from American Chemical Society, copyright 2020. (c) Electrochemical impedance type of electrochemical sensor. Reproduced
from ref. 361 with permission from American Chemical Society, copyright 2016. (d) Capacitance type of electrochemical sensor. Reproduced fromref. 422 with permission from Elsevier, copyright 2012.

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tant application of amperometric biosensors is the detectionof glucose. Zhang et al. proposed a highly ordered Ni nanowire
array integrated electrode for the electrochemical detection of
glucose.148 It is indicated that the as-fabricated nonenzymatic
biosensor presented a very high electrochemical activity for theelectrocatalytic oxidation of glucose in an alkaline medium
and a low detection limit of 1 × 10−7 M.
3.2.2. Potentiometric
type
electrochemicalsensor.
Potentiometric molecule sensing is an important subgroup ofelectrochemical sensors, generally applied for the detection ofions, gas molecules, and biological molecules.821 The largest
group among potentiometric sensors is represented by ionselective electrodes (ISEs), and the most widely used among
them is the pH sensor electrode.171,340,342,765 Potentiometric
type of electrochemical sensor functions by measuring theaccumulation of a charge potential versus a stable and welldefined reference electrode contacting the sample solution
through a liquid junction.822 For potentiometric measurements, the relationship between the analyte concentration andthe potential is governed by the Nernst equation, where Ecell°represents the observed cell potential at zero current. ECellis aconstant potential contribution to the cell, R the universal gas
constant, T the absolute temperature in degrees Kelvin, n is
the charge number of the electrode reaction, F is the Faraday
constant, and Q is the ratio of ion concentration at the anodeto ion concentration at the cathode.25°
EMF=ECell ¼ ECell


RT
ln Q
nF

In terms of this working principle, various ion-selective
electrodes fabricated by 1D nanowires are used for the detection of ions and biological molecules in solution.170,528,531,765
Fig. 14(b) shows a gold nanowire integrated electrochemicalsensor for the potentiometric detection of pH in the solution.
Furthermore, recently many potentiometric sensor devices areintegrated by combining with various forms of field-eﬀect transistor (FET) devices to measure chemical ions and biologicalmolecules.823 A conventional ISEs is a two-terminal system
wherein the voltage between the working electrode enclosed
indicator and the reference electrode is modulated by the reaction of ions/biomolecules on the working electrode.824
However, ion-sensitive FETs (ISFETs) employ a three-terminal
configuration with an active channel whose current is modulated in the presence of charged species.823 Owing to thepotential for miniaturization, parallel sensing, fast response
time, and seamless integration with electronic manufacturing
processes, such as complementary metal–oxide semiconductors (CMOS), ISFETs integrated by 1D nanowire structures have attracted considerable attention in the detection ofchemical and biological molecules.384,532,582
3.2.3. Electrochemical impedance type electrochemicalsensor. Impedance spectroscopy is a powerful technique foranalysing the complex electrical resistance of a system, and it
is sensitive to surface phenomena and changes in bulk properties.815 Thus, impedance techniques are useful to monitorchanges in electrical properties arising from molecule binding

This journal is © The Royal Society of Chemistry 2021

and interaction events at the surfaces of modified electrodes.
Like other electrochemical sensors, an impedimetric sensor isa type of electronic device that makes use of the interactions ofmolecules with an active transducer surface.361,815,825 Fig. 14(c)shows a single Si nanowire integrated sensor for the impedimetric detection of protein in the solution. The detection
process involves the binding or interaction of the analyte at
the interface of the electronic transducer, which directly or
indirectly alters the electrical properties of the sensing surface.
Impedance spectroscopy is mainly applied in bioanalytics tomonitor the biosensor fabrication process, but it is also used
to investigate the recognition process at the biosensor. For
example, Lin et al. reported an impedance type electrochemical sensor for rapid and sensitive detection of
Salmonella typhimurium using the aptamer coated interdigitated microelectrode (nickel nanowire).179 Huang et al. proposed a novel DNA biosensor based on oxidized graphene andpolyaniline nanowire modified glassy carbon electrode.772 The
results indicated that the graphene/polyaniline nanowires
showed high selectivity and sensitivity towards complementary
DNA sequence.
3.2.4. Capacitancetypeelectrochemicalsensor.
Capacitance type electrochemical sensor is usually referred toa subcategory of impedance sensors, in which the changes incapacitance values are measured indirectly.24 Capacitive
sensor devices are operated based on the changes of the permittivity as the chemical or biological analytes are subdivided
into two categories: interdigitated electrodes (IDEs) and electrode–solution interfaces. In the first case, interdigitated electrodes are implemented on a substrate and functionalizedwith probe biomolecules. Reactions between the immobilizedprobes and target molecules may be monitored as a change incapacitance or impedance of the device. In the case of electrode–solution interfaces, the capacitance variations between afunctionalized electrode and a reference electrode into the biological solution are measured. In these systems, the signal isaﬀected not only by changes in the dielectric permittivity ofthe biological material but also by the increase of its thickness
and the displacements of ions and water molecules from thesurface. In an alternative approach, capacitance type biosensors and sensor arrays are being developed based onchanges in the distance between the capacitor plates. These
devices are made of a rigid electrode on the substrate and aflexible electrode, which is typically a membrane.826 Recently,
various 1D nanowires have been integrated as capacitive molecular sensors for the detection of gas molecules and biologicalmolecules.377,422,535,703 Fig. 14(d) shows a SiC nanowire integrated sensor for capacitive humidity sensing.
3.3.

Field-eﬀect transistor (FET) type nanowire sensor

FET type molecular sensors are based on changes in the FET
parameters due to the interaction between the channel layer(source and drain) and target molecules.827–830 Apart from thecurrent variation within the channel, changes in thresholdvoltage or sub-threshold swing could also be used for identifying the sensing performance. Recently, many kinds of semi-

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Critical Review
conductor nanowires, such as Si nanowires,254,318,346,369 metal
oxide
based
nanowires
(e.g.
SnO2,
ZnO,
and
In2O3),532,549,582,636 and electrical conductivity polymer
nanowires743,763,830 have been intensively investigated in FET
molecular sensor applications. Nanowire FET molecularsensors work on the principle that adsorption or desorption ofmolecules on the surface of the nanowire will modify the FET
parameters, such as channel conductance, which is similar tothe sensing mechanism of resistive type of sensors.29,831
Furthermore, FET-type molecular sensors can be fabricated as
chemiresistive and electrochemical type sensor devices, as wellas integrate micro-electro-mechanical systems (MEMS) with avery small size and a low cost, which have a promising futurein the future IoT applications.
Among all the nanowire based FET sensing elements, Si
nanowires have proven to be a powerful and versatile tool inbiomedical analyte analysis. In a typical Si nanowire FET
device, an electric field is applied via a capacitively coupledgate electrode to modulate the conductivity of the Si nanowire
channel, as shown in Fig. 15. To ensure device stability, a commonly used reference electrode (e.g., Ag/AgCl, Ag wire, or Pt
wire) is used as a solution gate controller and maintained at
the ground potential to reduce electrical noise.832 Unlike conventional planar FETs, the sensing performance enhancementof Si nanowire FETs is attributed to the reduced dimensionality and large surface–volume ratio of the nanowire structure,
which gives rise to a susceptible response to any perturbationof electric bias that is triggered by the molecular interaction
on the surface of the nanowire.832 Currently, Si nanowire integrated FETs have been employed to convert various bio/chemical charge variations into electrical signals for in vitro andFig. 15 Schematic illustrations of the FET sensor device for (a) chemicalmolecule sensing. Reproduced from ref. 289 with permission from
American Chemical Society, copyright 2021. (b) FET sensor device forbiological molecule sensing. Reproduced from ref. 832 with permission
from Wiley-VCH, copyright 2018.

AnalystAnalystin vivo applications based on target-receptor binding, such as
pH,334,335,337,341,342,346
DNA/RNA,354,356,357,360,833
370,373,378,380,381,833
proteins,
and action potentials (APs).385,386

4. 1D nanowire-based sensors forchemical species detection
In this section, we will comprehensively review the recent
applications of 1D nanowire based sensor devices for thedetection and recognition of chemical species.
4.1.

Indoor/outdoor pollutant gas detection

With the rapid development of a super smart society, hugeachievements have been accomplished in the past decades,
which in turn gigantically improve the daily lives of humanbeings. However, unprecedented environmental issues, suchas indoor and outdoor air quality, have accompanied this progress and have triggered public awareness and demands toimprove our living standards, especially in residential environments.834 Poor quality of indoor air may significantly lead toan increase in the incidence of various types of human respiratory and related diseases because people spend most of theirtime working and living in the building envelopes.835 Due tothe human activity and emission of building materials, matterand gas pollutants, such as particulate matter, inorganic
gases, volatile organic compounds (VOCs), semi-volatileorganic compounds (SVOCs), mold, and radioactive compounds, are easy to accumulate indoors.834 Optical instruments in terms of the detection of light scattering from particles are usually used for the monitoring and detection ofindoor particulate matter (PM2.5 and PM10).836 While for volatile gas molecules, lots of electrically conducting polymer
nanowires and numerous semiconductor nanowires, such as
Si and metal oxides (Fig. 16(a)), have been synthesized andintegrated as chemiresistive type sensors to realize their detection and monitoring.312,314,448,504,516,523,543,720,749
As compared with indoor pollutant gases, outdoor air pollution is a more serious health threat to human beings. Due tofossil fuel combustion, burning, industrial/agricultural production, urbanization, and traﬃc transportation, many pollutants, such as inorganic gases (e.g., SO2, NO2, CO, NH3, CO2,
O3) and particle matters, are emitted to the living atmosphere.834 These pollutant emissions are naturally broughtindoors, which results in the worsening of indoor air quality.
Therefore, on the one hand, much eﬀort should be devoted to
exploiting renewable energy sources for sustainable development. On the other hand, there is an urgent demand todevelop simple and reliable methods for detecting andmapping the concentration of toxic and polluting gases.837,838
Recently, many types of sensors and e-nose platforms integrated by 1D nanowire structures have been developed toacquireandprovidepollutant
data
in
real
time.58,98,286,290,291,306,403,405–407,430,438,448,508,512,514,543,557,567,749,839
Fig. 16(b) shows a typical SnO2 bridged nanowire sensor device
toward the outdoor pollutant (NO2) sensing response.

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AnalystFig. 16 Nanowire based sensor devices for chemical molecule sensing and detection. (a) Indoor pollutant gas detection. Reproduced from ref. 720
with permission from American Chemical Society, copyright 2016. (b) Outdoor pollutant detection. Reproduced from ref. 567 with permission fromWiley-VCH, copyright 2014. (c) Humidity detection. Reproduced from ref. 443 with permission from American Chemical Society, copyright 2007. (d)Food quality and safety monitoring. Reproduced from ref. 83 with permission from American Chemical Society, copyright 2018. (e) Disease-related
VOCs molecule detection from exhaled breath. Reproduced from ref. 353 with permission from American Chemical Society, copyright 2016. (f ) Ion
detection in solution. Reproduced from ref. 191 with permission from Elsevier, copyright 2021.

4.2.

Humidity detection

Humidity is a natural phenomenon occurring due to the presence of moisture contents in the air. It plays a key role inhealth, manufacturing, storage, and testing processes.840
Hence, it is essential to develop simple and low-cost sensors
capable of accurately quantifying the humidity level in theliving space and various control systems for industrial andmanufacturing processes. In view of the working principles,
humidity sensors can be either capacitive or resistive

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types.310,841 The sensing mechanism of capacitive-type humidity sensors depend largely on the dielectric constant value ofsensing layers, apart from the crucial capacity of the film toenfold water clusters on its surface.840 Resistive-type humidity
sensors operate through the interaction of water moleculeswith the sensing layer, which directly aﬀects the electrical conductivity of the active sensing layer.805 Among recent sensing
elements, metal oxide semiconductor based sensors are promising due to their high sensitivity, fast response speed, longterm stability, and repeatability.842 In terms of metal oxides, aAnalystView Article Online

Critical Review
large number of metal oxide nanowire structures (e.g., ZnO,
SnO2 (Fig. 16(c)), and CeO2) have been synthesized andapplied for humidity detection.586,652,716,725,843 Besides, electrical conductivity polymer nanowires (e.g., PAN) are also considered as a good choice to integrate sensor electronics forhumidity detection.755
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4.3.

Food quality and safety monitoring

In addition to air pollution, food safety is another important
public health and challenging issue worldwide.844 Food
quality and safety are of primary importance with respect tonutrition, health, and quality of life. However, chemical andmicrobiological changes that occur during harvest, transportation, storage, and consumption aﬀect food quality and shelflife.845 As such, monitoring and detection of food pathogens,contaminants such as carcinogens, toxins, and pesticides
emitted from the food are always necessary. In response to thisconcern, nanotechnology-based molecular sensors havebecome a very eﬀective and promising tool due to their high/fast sensing response and low cost.845–849 For example, electronic nose (e-nose) instruments have been demonstrated as
an eﬀective technique to real-time and noninvasively monitor
the quality of muscle food, such as fish, meat, and poultry, interms of the emission of gas/VOCs molecules during their
spoilage,83 as shown in Fig. 16(d). Several electronic noses are
already commercially available in the market for food quality
and safety monitoring.850 Metal oxide semiconductors andelectrically conducting polymers are the most successful
sensing elements for the integration of these electronic
noses.10,83,632,745,851
4.4. Disease-related VOCs molecule detection from exhaled
breathRecently, exhaled breath test based on the detection and classification of biomarkers, namely the chemical profiles of volatileorganic compounds (VOCs) linked with disease conditions,has been considered as a promising method for early detection
due to its clinical non-invasive, direct, and real-time of
merits.852,853 At present, gas chromatography-mass spectroscopy (GC-MS) and fluorescence spectroscopy (FS) are still
the primary options for discriminative molecular analysis,
whereas they are expensive, time consuming, and too large to
be integrated.854 Therefore, developing high performancemolecular sensing and discrimination platforms, especially tomeet the demands of future portable electronic devices, areurgently needed. During the last decade, many eﬀorts havebeen devoted to exhaled breath analysis by electrically conducting molecular sensors.353,855–857 Recently, gas sensors
based on silicon nanowires, metal oxide nanowires, electricallyconducting polymer nanowires and their composites havebeen widely reported for exhaled breath analysis and applied
for early diagnosis of diseases (Fig. 16(e)).99,100,353,620,748
4.5.

Ion detection in solution

Ions, including cations and anions, play a vital role in a broad
range of environmental, technological, and physiological pro-

AnalystAnalystcesses.858 Hence, realizing the accurate detection/quantification of these ions is essential and valuable. Electrochemicalmolecular sensing, which oﬀers a strategy to detect ions withhigh selectivity/sensitivity, low-cost, portable, and real-time
analysis, has received considerable attention in the past
decades.26,859 As one of the most important applications, electrical molecular sensors have been widely applied in heavy
metal ions (e.g., As+, Cd2+, Pb2+, Hg+, and Cr3+) monitoringand detection.26,860–864 As is known, heavy metal ions are extremely toxic pollutants, which are carcinogens and non-biodegradable, and long-term exposure to them and ubiquitous
distribution would lead to a greater risk to human health andthe environment.865 Recently, metallic nanowires (e.g., Au, Ag),Si nanowires, metal oxide semiconductor nanowires (e.g. SnO2,
ZnO, WO3), electrically conducting nanowires (e.g., PAN) andtheir compositions have been successfully synthesized assensing electrodes for ion detection.74,169,254,348–351,581,766 In
addition, proton (H+) detection, a pH sensor, is highly indemand for various applications such as chemical reaction,
health monitoring, agriculture, and food safety, and water
quality monitoring.866 Up to now, a variety of proton measurement techniques, such as conductometric/capacitive,867
potentiometric,868–871 and ion sensitive field eﬀect
transistors337,872,873 are exploited for monitoring of protons insolutions. Apart from the cations, accurate monitoring of thelevel of anions, such as nitrate (NO3−)191 (Fig. 16(f )), phosphate (PO43−)168 and ammonium (NH4+),533 are also importantin environmental pollution control, food, clinical analyses,
and other industries.

5. 1D nanowire-based sensors forbiological species detection
Apart from chemical molecule analysis, nanowire integrated
sensor electronics also show promising applications in the biological species (e.g., DNA/mRA, proteins, biomarkers andvirus) detection and recognition. In this section, we will comprehensively review the recent applications of 1D nanowire
based sensor devices in the detection and recognition of biological species.
5.1.

Protein biomarker detection

Early disease diagnosis is a crucial and promising research
field in human health.874,875 Recent proteomics and genomics
research has revealed that many new protein biomarkers areformed in the bio fluids as human body encounter a specificdisease, such as cancer.874 Hence, biomarker detection andevaluation hold enormous potential for early disease diagnosis. Recently, 1D nanowire integrated biosensor electronics are
emerging as talented sensing platforms for biomarker detection due to their ultra-sensitive, low-cost, and low-power
consumption.39,61,78,876 In terms of the working principles, thebiomarker sensors can be classified into two categories: labelbased and label-free sensors.877 Label-based sensors use biomarkers that are decorated by secondary labels, such as fluo-

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Analystrescent materials, magnetic beads, or even biologicalmaterials. Their working principles are as follows: (1) the secondary antibody (Ab2) is decorated with electroactive labels,
such as biochemical materials and nanoparticles of novel 1D
materials; (2) the Ab2 is bound on the analyte through anintermediate antibody (Ab1) and then is immobilized onto theelectrode surface by specific binding; and (3) the concentrationof the analyte is obtained by measuring the current at the electrode. Compared to the label-based sensors, label-free electric
sensors operate based on the electrical property changes as thebiomarkers directly bind on the sensing materials.878 By
measuring these changes, biomarker information, such asconcentration, is obtained, which can be applied for the
related disease diagnosis. Among various electrical transduction sensor electronics, nanowire-based FET structures havebeen considered as a promising tool for biomarker detection
and reported in many studies.40,827 For example, Janissen et al.
demonstrated an ultrasensitive and highly selective disease biomarker biosensor based on surface functionalized InP nanowire
FET sensor device.437 The developed devices provide ultrahighlabel-free detection sensitivities ∼1 fM for specific DNA
sequences, measured via the net change in device electrical re-

Critical Review
sistance. Similar levels of ultrasensitive detection of ∼6 fM wereachieved for a Chagas Disease protein marker (IBMP8-1), as
shown in Fig. 17(a). Lieber et al. have reported a highly sensitiveand multiplexed detection of cancer marker proteins using Si
nanowires.909 It is shown that the cancer marker antibodies
modified Si nanowire arrays allowed the real-time multiplexed
detection of free protein specific antigen (f-PSA), PSAα-antichymotrypsin (PSA-ACT) complex, and carcinoembryonicantigen (CEA) and mucin-1 with good signal-to-noise ratios
and enabled the limit of detection down to a 50 to 100 fg mL−1
level. In addition, Si nanowire FET biosensors can also be
utilized as the label-free sensor electronics for protein detection.437 Apart from Si nanowire, other nanowire structures, suchas conductive polymer nanowire81,770,771,790,791 and semiconductor nanowires,365,370,372,376,437,530,582 are also favorable
for the sensor electronics integration for protein marker
detection.
5.2.

Virus detection

Viruses are the most common cause of human diseases,879 as
well as war crisis.880 For example, as the outbreak of highly
contagious SARS-CoV-2 at the end of 2019, 167 011 807 cases

Fig. 17 Nanowire based sensor devices for biological molecule sensing and detection. (a) Protein biomarker molecule detection. Reproduced fromref. 437 with permission from American Chemical Society, copyright 2017. (b) Virus detection. Reproduced from ref. 365 with permission from
American Chemical Society, copyright 2012. (c) DNA and RNA detection. Reproduced from ref. 886 with permission from Wiley-VCH, copyright2016. (d) Microorganisms detection. Reproduced from ref. 599 with permission from American Chemical Society, copyright 2008.

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Critical Review
have been confirmed as infected, and meanwhile, this pathogenic Coronavirus has caused 3 472 068 deaths up to now.880
Hence, accurate detection of viruses in the early stage will dramatically prevent the pandemic and save lives. Cell culturebased techniques, mainly including nucleic acid sequencebased amplification (NASBA)881 and real-time polymerase
chain reaction (real-time PCR),882 are the gold standard forviral detection.882 Meanwhile, in the past decades, biosensor
techniques have become promising tools for electrochemical
detection of infected viruses due to high sensitivity and specificity.883 Fig. 17(b) shows a high selectivity detection of influenza A viruses from clinical exhaled breath condensate (EBC)
samples (diluted by 100-fold) within minutes using silicon
nanowire (SiNW) integrated sensor devices.365 Among various
1D nanowire sensing elements, Si nanowires and metal oxide
nanowire sensors, which have excellent biocompatibility arebroadly explored as novel biological sensor electronics forhighly sensitive detection of viruses, such as Dengue,363,364,369
SARS,647 Influenza A H3N2,257,365 H5N2,362 and HIV.368

5.3.

DNA and RNA detection

Deoxyribonucleic acid (DNA) and ribonucleic acid (RNA) detection via advanced biological sensor electronics has enabledmany opportunities in modern health for disease diagnosis/
treatment.358,884,885 Recently, nanowire sensor electronics havebeen demonstrated as a successful platform for the detectionof specific sequences of DNA and RNA.358,886–888 For example,
Ingebrandt et al. used a long-channel, ion-sensitive silicon
nanowire field-eﬀect transistor device (ISFETs) fabricated in a
top-down approach for DNA capture and detection,886 as
shown in Fig. 17(c). Lieber et al. demonstrated a p-type Si
nanowire resistive sensor for ultrasensitive and selective realtime DNA sensing.358 It is shown that Si nanowire sensors
functionalized with peptide nucleic acid (PNA) receptors candistinguish wild-type from the ΔF508 mutation site in thecystic fibrosis transmembrane receptor (CFTR) gene, and theirdetection limit can be down to tens of femtomolar range.
Wang et al. reported a FET biosensor based on uniformly sizedhigh-response silicon nanowire (SiNW) array for real-time,label-free, super-sensitive detection of PIK3CA E542K
ctDNA.889 In order to recognize the target ctDNA, the Si nanowires were modified with the probe DNA through silanization
and acted as a molecular gate, and it is indicated that the asfabricated biosensor had significant superiority in ctDNA
detection, achieving an ultralow detection limit of 10 aM andgood linearity under the ctDNA concentration range from 0.1
fM to 100 pM. In addition, Si nanowire devices also served as
excellent RNA sensor electronics.354,355 For instance, Chenet al. reported an ultra-sensitive Si nanowire FET biosensor forthe detection of GC-rich RNA.354 Specifically, Si nanowire FET
device was surface functionalized by hepatitis C virus (HCV)
genotype 3b chimeric neutralized DNA (nDNA) probe, and it isindicated the HCV-3b chimeric neutralized DNA (nDNA) probe
exhibited better performance for SNP discrimination in
10 mM bis–tris propane buﬀer.

AnalystAnalyst5.4.

Microorganism detection

Every year, millions of people worldwide are infected by foodor waterborne pathogens (e.g., bacteria, viruses, and parasites)
via the consumption of contaminated water and food.354,355
Hence, rapid and accurate detection of hazardous microorganisms in water and food is also of high importance for publichealth and environmental protection. Current methods ofdiagnosing these pathogens are based on conventional microbiological culturing techniques followed by biochemical
identification.890 Although accurate infections can be concluded by these techniques, time consuming and labor-intensive processes have impeded the early diagnosing and treatment of these pathogenic diseases.891 In recent years, nanowire integrated biosensor electronics have emerged as a successful tool for the detection of whole bacteria, bacterial byproducts and metabolites, as well as enzymes.82,179,599,745,892,893
For example, Alocilja et al. developed a direct-charge-transfer(DCT) biosensor integrated by polyaniline nanowires for thedetection of the foodborne pathogen Bacillus cereus.745 The
biosensor was fabricated using antibodies as the sensing
element and polyaniline nanowire as the molecular electricaltransducer. The sensing signal was recorded as the resistancechange upon the antigen–antibody interaction. Testing of thebiosensor showed that it had the ability to detect the presenceof the target microorganism, B. cereus, at concentrations as
low as 10 CFU ml−1, the detection time is only 6 min. Li et al.
reported a TiO2 nanowire bundle-based immunosensor connected with an Au microelectrode for the impedimetric detection of Listeria monocytogenes, a foodborne bacterial pathogen,599 as shown in Fig. 17(d). This platform exhibited highsensitivity, high selectivity ( poor response to other foodborne
pathogens such as Escherichia coli O157:H7, Salmonella
Typhimurium, and Staphylococcus aureus), and rapid (1 h assaytime) detection to the target pathogens, and oﬀered the limit
of detection as low as 500 CFU mL−1.
5.5.

OthersIn addition to the detection of various biological macromolecules, nanowire-based sensor electronics have potential
applications in drug discovery894 and electrophysiologicalsignal generation and measurements, such as the measurements of intracellular action potentials generated by beating
cardiomyocytes385,895,896 and extracellular action potentials
from brain tissues and cells,897,898 the development of 3D
macroporous tissues,899 and the study of the metabolism ofcells.900

6. Critical issues and perspectives ofnanowire-based sensor electronics
Despite the extraordinary achievements of 1D nanowire-based
sensor electronics, there still exist several challenges that need
to be overcome to make these devices commercially available
for analytes monitoring and recognition of chemical and bio-

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Analystlogical analytes. Here, we mainly discuss four remaining critical issues, including reproducibility, selectivity, stability,
energy consumption, and the perspectives against thesechallenges.

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6.1.

Reproducibility of devices

Integrating nanowire devices allow us to study the intrinsic
properties of the nanowire, as well as to explore the potential
sensing applications. However, a tiny variation in the size or
shape of nanostructures will powerfully alter their physical/
chemical properties and functionalities. Thus, we should carefully consider how to synthesize nanowires with high uniformity. Template-assisted nanowire growth has been considered as
an alternative approach to achieve a highly ordered nanowire
array. However, the complexity of template fabrication, lowdensity of nanowires, and the extensive distribution of nanowire diameter have limited the wide application of suchmethods.901 Recently, Zhao et al. reported a two-step method
to fabricate ZnO nanowires with uniformly shaped structures.113 Firstly, ZnO nanowires of random size are etched by
NH4+ as the seed layer, and then, a very similar diameter(average about 17 nm with σ 1.3 nm) of ZnO nanowires aregrown in the second step. Such a high uniformity in nanowire
diameter would significantly increase the performance reproducibility of nanowire based sensor devices. This uniquefinding paves the way for the fabrication of nanowires-integrated nanodevices with reliable performance.
6.2.

Selectivity of devices

Another critical issue is the selectivity of the sensor device. 1D
nanowire sensors generally have high sensitivity to gas analytes, but they also suﬀer from poor selectivity. To enhance theselectivity of gas sensors, a widely accepted method is introducing recognition elements on the sensing materials, forexample, impurity element doping, nanoparticle surface decorating, and core/shell heterostructure construction. In
addition, operational temperature modulation and nanowire
architecture altering also serve as eﬀective methods to improve
the selectivity of nanowire-based molecular sensors toward thetarget molecules. However, the results are usually far from prospects due to the low operational stability. Inspired by catalytical chemistry, it is worth considering combining porous
materials such as zeolites, metal–organic frameworks, andmesostructured oxides with a nanowire.902–904 Canlas et al.
reported a novel method to fabricate molecule imprinted oxide
catalysts.905 Using this structure, the nanocavities can preferentially react with nitrobenzene rather than nitroxylene in thephotoreduction model and react with benzyl alcohol rather
than 2,4,6-trimethylbenzyl alcohol in the photo-oxidation
model. This technique can be applied to nanowire based gas
sensor and biological sensor to gigantically improve selectivity
due to their preferential interactions with specific VOC molecules and biological macromolecules, even with a chemicallysimilar structure. In addition, biological receptors, e.g.,
peptide nucleic acid (PNA),358,906 aptamers907 andantibodies,908,909 are usually functionalized on the nanowire

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Critical Review
surface to realize the biological analyte or cell specific binding
and sensing.
6.3.

Long-term stability of devices

Stability, including chemical stability and physical stability, isthe essential key to open the gates for practical applications of
sensors. However, although numerous eﬀorts are devoted to
improving the long-term stability of nanowire sensors, theinfluence of humidity, poisoning, and contact issues still exist,
preventing such kinds of sensors from practical applications.
Thus, preventing the degradation of nanowire bulk, nanowire/
electrode contact, and electrodes is the only way to achieve thelong-term stability of nanowire devices. Recently, Nakamura
et al. also demonstrated a strategy for achieving atmosphericelectrical stability of ZnO nanowire devices via a sequentiallythermal annealing treatment in vacuum/air.121 This simple
and low-cost method can enhance nanowire atmosphericstability for at least 40 days with stable electrical properties.
Meanwhile, Zeng et al. oﬀered a way to overcome the degradation of device contact by deposition of antimony doped tinoxide (ATO) instead of conventional contact metal (Ti).120 It is
indicated that the nanowire sensor device can work stably over2000 h. Besides, Zhou et al. recently introduced a simple
method to improve the long-term stability of Si nanowire FET
biosensor devices through surface deposition of Al2O3 shell.910
It is observed that the diameter of the Si nanowire remained
almost the same after 100 days of storage in phosphatebuﬀered saline ( pH 7.4) and neurobasal solvent, respectively,
while the Si nanowire without the shell disappeared. These
strategies propose some ideas to significantly improve thelong-term stability of nanowires in complex environments,
opening up further investigations of using nanowires as theplatform for the harsh environment applications.
6.4.

Power consumption

An external heater or power supply is usually needed to drive
the eﬃcient operation of nanowire-based gas and biologicalsensors, which inevitably increases the power consumption
and sensor size. To eﬀectively decrease the power consumptionof nanowire sensor electronics, several options are proposed,such as (1) developing room temperature sensing materials, (2)using the self-Joule-heat technique, and (3) harvesting energy
via the piezoelectric eﬀect. Meng et al. recently reported an
excellent thermal management approach in metal oxide nanowire sensors via a pulsed self-Joule-heating technique.58 It isfound that the thermal conductivity of the device was reduced
due to the prohibition of heat dissipation from the nanowire
to surroundings, and its thermal relaxation times can be
decreased down to a microsecond range, while several tens ofseconds are needed for conventional MEMS gas sensors. Thismethod enables the reduction in energy consumption down to∼102 pJ s−1 and the enhancement of sensitivity for electricalsensing of NO2 (100 ppb). This proposed thermal management
concept of nanowires in both spatial and time domains oﬀers
a strategy for exploring novel functionalities of nanowire-based
sensors with high performance.

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With improved 1D nanowire synthesis and device fabrication processes with high uniformity, the integrated nanowire
sensor electronics would have high reproducibility, selectivity,and long-term stability. This would promote the wide usage of
nanowire sensor electronics in IoT applications, such as medicine, food industry, security, and environment protection.

Author contributions
G. Z. and T. Y. wrote this manuscript. All the authors contributed to improving the manuscript, manuscript preparation, andapproved the final version of the manuscript.

Conﬂicts of interest
There are no conflicts to declare.

Acknowledgements
This work was supported by KAKENHI (Grant No. JP17H04927,
JP18H01831, JP18H05243, and JP18KK0112). T. H., K. N., T. T.,
and T. Y. were supported by JST CREST, Japan (Grant No.
JPJSBP120187207). This work was performed under the
Cooperative Research Program of “Network Joint ResearchCenter for Materials and Devices”, “Dynamic Alliance for Open
Innovation Bridging Human, Environment and Materials”,
and the MEXT Project of “Integrated Research Consortium on
Chemical Sciences”.

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