bluuebunny/crossref_metadata_2025_split huggingface dataset:
Highly Sensitive Acetylcholine Biosensing Via Chemical Amplification of Enzymatic Processes in Single Track-Etched Nanochannels
Authors: Cayón Vanina M. , Toum Terrones Yamili , Laucirica Gregorio , Fenoy Gonzalo , Cortez M. Lorena , Toimil Molares Maria Eugenia , Trautmann Christina , Marmisolle Waldemar , Azzaroni Omar 
Published: February 2024

Neurotransmitters are endogenous chemical messengers that play crucial roles in the transmission, enhancement and conversion of specific signals between neurons and other cells and are considered biomarkers of neurodegenerative diseases.[1] Neurodegenerative diseases cause progressive loss of cognitive and/or motor function and, as life expectancy rises, they imply major challenges for societies with rapidly aging populations.[2] As a result, monitoring neurotransmitters is becoming increasingly relevant in clinical environments. Acetylcholine (Ach) is a neurotransmitter that plays a key role in the communication between neurons in the spinal cord and nerve skeletal junctions in vertebrates. [3] Since an abnormal concentration of Ach has proven to be related to neurodegenerative diseases, novel strategies for highly sensitive and specific Ach (bio)sensing are in great demand.
In this work we present the construction of Ach enzymatic biosensors with remarkable sensitivity by acetylcholinesterase immobilization on polyamine-modified single nanochannels via electrostatic self-assembly. [4] To fabricate bullet-shaped single nanochannels in polyethylene terephthalate (PET), 12 µm thick PET foils are irradiated with a single swift heavy ion. The resulting ion track consists of highly localized damaged material along the ion trajectory and is selectively dissolved in a highly basic aqueous solution under asymmetric conditions to obtain a bullet-shaped channel. The controlled PET hydrolysis exposes carboxylic groups at the channel surface (negative charge at pH < 4), which allows the immobilization of further functional groups to design and construct the biosensor.
Here, we will discuss in detail the sensor design, the applied functionalization strategy, and the performance of the sensor. In short, changes in the surface charge of the nanochannel lead to measurable changes in the transmembrane current in a steady-state configuration. We will show experimental results that evidence that the designed sensor successfully transduces the presence of acetylcholine into measurable ionic signals with a 16 nM low limit of detection.
[1] World Health Organization, Neurological Disorders: Public Health Challenges, World Health Organization Press, Geneva, Switzerland,2007.
[2] L. Gan, M. R. Cookson, L. Petrucelli and A. R. La Spada,Nat. Neurosci., 2018, 21, 1300–1309.
[3] M. Hasanzadeh, N. Shadjou and M. de la Guardia, TrAC, Trends Anal. Chem., 2017, 86, 107–121.
[4] Yamili Toum Terrones, Gregorio Laucirica, Vanina M. Cayón, Gonzalo E. Fenoy, M. Lorena Cortez, María Eugenia Toimil-Molares, Christina Trautmann, Waldemar A. Mamisollé and Omar Azzaroni, Chem. Commun., 2022, 58, 10166
Sensitive Recognition of Acetamiprid with a Unique Electrochromic Molecular Imprinted Polymer Sensor
Authors: Mutlu Esma , Şenocak Ahmet , Demirbaş Erhan , Koca Atif , Akyuz Duygu 
Published: February 2024

The development of molecularly imprinted polymers (MIPs) and the applications for them have attracted a great deal of interest during the last two decades. MIPs are generally used in different fields, specially molecularly imprinted electrochemical sensors (MIECS), due to their particular design and specific detection abilities [1]. The advantages of an electrochemical MIP sensor include low cost, easy operation, rapid response time and excellent potential for miniaturization and construction for portable equipment applications [2]. In the scope of this work, we performed that electropolymerization of IrO2 as an electrochromic material on an indium tin oxide (ITO) glass substrate and electrosynthesis on this electrode using pyrrole as a functional monomer in the presence of acetamiprid as template were used to create the electrochromic molecular imprinted polymer sensor (MIP/IrO2/ITO). With the created electrochromic MIP sensor, it is intended to create a selective pesticide sensor by utilizing molecular imprinted polymer (MIP) technology, and to detect with the naked eye by color change depending on the acetamiprid concentration by using electrochromic material. The IrO2/ITO electrochromic film demonstrated magnificent cycle stability (100 cycles), high coloration efficiency (400 cm2 C-1 at 450 nm), and quick coloring/bleaching reaction time (8.60s/7.10s, respectively). By using in-situ spectroelectrochemical measurements, these optical properties of MIP/IrO2/ITO were obtained at various acetamiprid concentrations for quantitative analysis. By using differential pulse voltammetry between -0.2 V and +0.8 V (versus Ag/AgCl in 0.1 M PBS), the sensor performance of MIP/IrO2/ITO was assessed. In an acetamiprid concentration range of 4.29–38.6 nM, the MIP/IrO2/ITO electrode demonstrated linear response with a detection limit of 2.72 nM, sensitivity of 47.2 µA nM-1, and repeatability of 0.87%.

Keywords: Electrochromism; Molecularly imprinted polymer (MIP); Pyrrole; IrO2;Acetamiprid; Electrochemical sensor; Spectroelectrochemistry.

Acknowledgements

This work was supported by The Scientific and Technological Research Council of Türkiye, TUBITAK (Project No:121Z784) as the financial.

References

[1] Cui B., Liub P., Liub X., Liua S., Zhang Z., 2020, Journal of Materials Research and Technology, 9(6):12568–12584.
[2 ]Zaidi S. and Shin J., 2014, Int. J. Electrochem. Sci., Vol. 9.
Novel Amino Acid Based Molecularly Imprinted Polymers as Recognition Elements for Electrochemical Detection of Contaminants of Emerging Concern (CEC)
Authors: Beddok Claire , Calas-Blanchard Carole , Fuks Gad 
Published: February 2024

Water pollution is a major issue of this era and the development of new sensors and biosensors for specific detection of contaminants of emerging concern (CEC) is of growing interest. Researchers have taken advantage of different recognition systems such as antibodies or enzymes that can be very specific and sensitive toward their target1. However, those biological molecules tend to be expensive, tedious to obtain in large amount, unstable in changing environments and have a short shelf life. To overcome these issues, synthetic analogues named molecularly imprinted polymers (MIPs) have been used as recognition elements. MIPs are polymers with imprinted nanopores that are able to rebind specifically the chosen target. They have the advantage of being cheaper to prepare in large quantities and display a higher robustness, inertness and resistance than their biological counterpart 2. The library of functional monomers used by researchers to prepare MIPs is quite narrow 3 and their recognition in water can be limited 4. That is why we believe it is interesting to design new functional monomers based on amino acids. Indeed, amino acids are good candidates for recognition agent, as they display a variety of functions that can interact through hydrogen bonds, hydrophobic interaction, Π-Π stacking or cation-Π stacking. As a part of antibodies and enzymes, they are capable of recognition in aqueous environment. We believe that using amino acids could get MIP technology closer to biological selectivity and sensitivity, while keeping it cheap and robust. The preparation of a MIP consists in the polymerization of a functional monomer made from an amino acid and a polymerizable agent in the presence of a template (the target of the recognition system).Integrating the MIP in an electrochemical sensor should provide selective detection of the target.
References:

Valera, E. et al. Application of Bioassays/Biosensors for the Analysis of Pharmaceuticals in Environmental Samples. in Comprehensive Analytical Chemistry vol. 62 195–229 (Elsevier, 2013).

Baggiani, C., Anfossi, L. & Giovannoli, C. MIP-based immunoassays: State of the Art, limitations and Perspectives. Molecular Imprinting
1, 41–54 (2013).

Kadhem, A. J., Gentile, G. J. & Fidalgo de Cortalezzi, M. M. Molecularly Imprinted Polymers (MIPs) in Sensors for Environmental and Biomedical Applications: A Review. Molecules
26, 6233 (2021).

Tse Sum Bui, B., Belmont, A.-S., Witters, H. & Haupt, K. Molecular recognition of endocrine disruptors by synthetic and natural 17β-estradiol receptors: a comparative study. Anal. Bioanal. Chem 2081–2088 (2008).

Figure 1
Controlled Surface Functionalization Using Aryldiazonium Salts for the Development of Aptasensing Platforms
Authors: Florea Ciprian , Onas Andra Mihaela , Pandele Andreea Madalina , Raicopol Matei , Pilan Luisa 
Published: February 2024

It is well known that both the aptamer surface density and surface chemistry can have a strong influence on the analytical performance of aptasensors based on target-induced conformational changes1. In this context, we report here an improved protocol for obtaining aptasensing platforms which allows fine-tuning the DNA aptamer surface coverage. First, glassy carbon substrates were functionalized with ethynylphenyl groups through the electrochemical reduction of silyl-protected ethynylphenyl diazonium tetrafluoroborates followed by deprotection with tetrabutylammonium fluoride2. The successful removal of the protecting groups (triisopropylsilyl-, triphenylsilyl- and tris(biphen-4-yl)silyl-) was confirmed by X-ray photoelectron spectroscopy and cyclic voltammetry in the presence of Fe(CN)6
3-/4- as soluble redox probe. Following “click” post-modification with suitable derivatization reagents, the surface coverage with ethynylphenyl groups was assessed using complementary techniques such as XPS, cyclic voltammetry and chronocoulometry. For example, the F/C surface ratio of substrates derivatized with 1-(2,2,2-trifluoroethoxy)-6-azidohexane provided an indication of the functionalization degree, and the integration of Fc/Fc+ voltammetric peaks for substrates modified with N-(6-azidohexyl)ferrocenecarboxamide allowed a quantitative determination of the surface coverage. Both techniques showed a good correlation between the protective group size and the surface coverage with alkyne groups. Likewise, we observed a similar trend for substrates derivatized with azide-modified oligonucleotides, where the surface packing density was determined based on the chronocoulometric response of Ru(NH3)6
3+, a cationic redox probe which binds with the negatively charged phosphate groups from the oligonucleotide backbone. As proof of concept, we further developed an electrochemical molecular beacon aptasensor employing a ferrocene-labeled quinine aptamer. We demonstrate that the aptamer surface density, and ultimately the analytical performance of molecular beacon aptasensors, can be effectively fine-tuned by employing silyl protecting groups of different sizes.
Acknowledgements

This work was supported by a grant from the Romanian Ministry of Education and Research, CNCS-UEFISCDI, project number PN-III-P4-ID-PCE-2020-2474, within PNCDI III.

References

Onaş, A. M., Dascălu, C., Raicopol, M. D. & Pilan, L. Critical Design Factors for Electrochemical Aptasensors Based on Target-Induced Conformational Changes: The Case of Small-Molecule Targets. Biosensors 12, (2022).

Leroux, Y. R., Fei, H., Noël, J.-M. M., Roux, C. & Hapiot, P. Efficient covalent modification of a carbon surface: Use of a silyl protecting group to form an active monolayer. J. Am. Chem. Soc. 132, 14039–14041 (2010).
(Invited) All-3D-Printed Devices for Electrochemical Sensing
Authors: Kokkinos Christos 
Published: February 2024

Three-dimensional (3D) printing has gained significant attention in research laboratories, since it provides the end user with the freedom and ability to produce in-house and on-demand specific electrochemical platforms in a fast and affordable way. The most applied 3D-printing technology in the manufacturing of electrochemical sensors is fused deposition modeling (FDM) which is based on the e-printing of the device by thermoplastic filaments. In particular, the use of FDM for the printing of sensors offers noteworthy advantages compared to conventional fabrication technologies, such as desktop-sized equipment, very low capital, operational, and materials costs, easy fabrication process, design transferability (as the respective file format can be transferred through e-mail and printed on every dual extruder 3D printer), and ecofriendliness (since no waste is produced) [1,2].
This presentation will discuss our recent developments of all-3D-printed integrated mini devices and their applications to electrochemical sensing [3-6]. The devices are printed from specific filaments (conductive and non-conductive) at different sizes and shapes, by a dual extruder 3D-printer, in order to fit to the demands of numerous applications. More specifically, all-3D-printed electrochemical microtitration wells for the in-situ and micro-volume quantum dot-based bioassays, as well as a 3D-printed wearable glucose monitoring device in the form of an electrochemical ring will be described. Besides, a 3D-printed wearable device in the form of an electrochemical finger for date rape drugs screening and a 3D-printed microfluidic device modified with metallic film for the trace determination of heavy metals will be presented.
Acknowledgements:I thank the Special Account for Research Grants of National and Kapodistrian University of Athens for the financial support.
References

A. Abdalla and B. A. Patel, Curr. Opin. Electrochem., 20 (2020) 78–81.

E. J. Carrasco-Correa, E. F. Simó-Alfonso, J. M. Herrero-Martínez, M. Miró, TrAC - Trends Anal. Chem., 136 (2021) 116177.

A Baltima, H. Panagopoulou, A. Economou, C. Kokkinos, Anal. Chim. Acta 1159 (2021) 338426.

V. Katseli, M. Angelopoulou, C. Kokkinos, Adv. Funct. Mater., 31 (2021) 2102459.

V. Katseli, A. Economou, C. Kokkinos, Anal. Chem. 93 (2021) 3331−3336.

G. Poulladofonou, C. Freris, A. Economou, C. Kokkinos, Anal. Chem. 94 (2022) 4087−4094.
(Invited) Metal and Nonmetal Plasmonic Nanostructures for Surface-Enhanced Raman Spectroscopy Detection
Authors: Tang Haibin , Meng Guowen 
Published: February 2024

Toxic small molecules such as pesticides, food additives, plasticizers and dyes have been posing increasing threat to human health. Surface-enhanced Raman scattering spectroscopy (SERS) is a powerful sensing strategy for these small molecules with advantages including fast response, high sensitivity and fingerprint identification.
Based on the surface plasmon effect, gold and silver nanostructures are the typical plasmonic sensing materials for rapid detection with SERS. However, the crucial challenges for realizing on-site real detection application is to fabricate reproducible and highly sensitive SERS substrates and portable instrument. We fabricated several long-range ordered sensitive nanostructure arrays based on anodic aluminum oxide templates which could provide reproducible structural patterns. Then, we developed a portable instrument integrated with database of the standard Raman spectra of common contaminants and a software for automatic identification and comparison of the test spectrum with the standard database, which can identify the specific analytes. Combined with the sensitive and reproducible SERS substrates, we realized the on-site and rapid detection of various toxic contaminants.
Recently, as an inexpensive candidate, nonmetal plasmonic materials like oxide semiconductors have attracted increasing interests, which induced by the increase of free charge carriers via introducing oxygen vacancies. We synthesized oxygen-deficient WO3-x and NayWO3-x nanosheets and realized the localized surface plasmon resonance (LSPR) band in visible range (~530 nm) as same as the gold nanoparticles, which is the bluest. Then, SERS detection of dyes has also been realized on nonmetal substrate. Moreover, the plasmonic oxygen-deficient oxides showed wide LSPR tuning window from visible to infrared range and plasmon-driven photocatalysis, which may open potentials for biological applications.
(Invited) Advanced Scanning Probe Microscopy for Studying Biofilm Formation and Single Cell Entities at Electrified Interfaces
Authors: Caniglia Giada , Hellmann Andreas , Daboss Sven , Kranz Christine 
Published: February 2024

Advanced scanning probe microscopy techniques such as atomic force – scanning electrochemical microscopy (AFM-SECM) und scanning electrochemical microscopy (SECM) are highly attractive hybrid techniques for studying biomedically relevant samples down to the single entity level. Our group introduced a new type of AFM-SECM probe having a conductive colloid instead of a sharp AFM tip. As this spherical microelectrode, which is located at the end of an electrically insulated AFM cantilever can be easily modified by electrodeposition with e.g., conductive polymers and electrocatalytic layers, single cell force spectroscopy under potential control allows studying adhesion properties [1,2]. Cell adhesion is a crucial parameter not only for developing new materials serving as substrates for neural scaffolds, electrodes, and biomedical devices but also in biofilm formation. Biofilms are well-organized aggregates of bacteria able to attach to and proliferate at almost every type of solid surface resulting in increased resistance to conventional antimicrobial and antibiofouling agents [3].The first attachment of bacterials is a process highly influenced by the nature of the surface, such as hydrophobicity, chemical structure, surface charge, and presence of antimicrobials [4].
In this contribution, we present the potential of various scanning probe microscopy techniques, as suitable tools to locally investigate the early stages of biofilm formation and the effects of various antibiofouling and antimicrobial systems against Escherichia coli and Pseudomonas fluorescens. For example, the properties of polydopamine, a bio-compatible polymer, are studied in respect to early stages of bacterial adhesion in dependence of surface charge density and applied potential [5]. Colloidal conductive AFM probes can also be modified electrocatalytic layers, suitable for detecting signaling molecules and at the same time allow electrochemical force spectroscopy at soft samples like biomedically relevant single entities.

References

[1] P. Knittel, H. Zhang, C. Kranz, G. Wallace and M. Higgins, Nanoscale 8, 4475 (2016).

[2] S. Daboss, J. Lin M. Godejohan, C. Kranz, Anal. Chem. 92, 8404 (2020).
[3] O. Ciofu, C. Moser, P. Østrup Jensen, N. Høiby Nat.
Rev. Microbiol. 20, 621 (2022).
[4] A. Viljoen, et al. J
.
Bacteriology, 202, e00125 (2020).
[5] G. Caniglia, A. Teuber, B. Mizaikoff, C. Kranz Anal.
Bioanal. Chem. 415, 2059 (2023).
Electrochemical Synthesis of Self-Doped Poly(3,4-ethylenedioxythiophene) and Application to Flexible Biosensors
Authors: Jing Yuxin , Miyai Fumika , Okuzaki Hidenori 
Published: February 2024

Wet-processable and highly conductive polymers are promising candidates for key materials in organic electronics. Poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS), commercially available as a water dispersion of colloidal particles, has potential applications to organic electronics because of its high electrical conductivity, transparency and thermal stability 1). However, the PEDOT:PSS has some technical issues owing to the PSS: The ultra-thin layers thinner than the colloidal particle size is difficult; The PEDOT:PSS colloids aggregate and precipitate when stored for an extended period; The pristine PEDOT:PSS exhibits poor electrical conductivity without secondary dopants such as ethylene glycol and DMSO. Recently, we have developed a novel fully soluble self-doped PEDOT (S-PEDOT) by chemical oxidative polymerization having a high conductivity without secondary dopants 2).
This presentation deals with the first study on synthesis of the S-PEDOT by a facile electrochemical polymerization and characterization by means of cyclic voltammetry (CV), reflection spectroscopy, X-ray diffraction analysis (XRD), and the four-point technique.
The S-PEDOT was electrochemically synthesized at different current densities ranging from 0.5 to 5 mA/cm2. It was found that the electrical conductivity increased with increasing current density and attained as high as 427 S/cm at 5 mA/cm2 which was one order of magnitude higher than those so far reported in the literature. Further investigation has been made to clarify the role and effect of current density on molecular weight, crystallinity, and carrier transport properties in more detail.
For the application to biosensors, flexible organic electronic circuits consisting of working, counter, and reference electrodes were fabricated by line-patterning 3) the S-PEDOT water solution as a conductive ink on a Kapton film as a flexible substrate. The flexible glucose sensor was then fabricated by coating the bioink containing glucose oxidase, ferrocene, and chitosan on the working electrode. It was found that the flexible biosensor successfully worked where the electric current during the CV measurement increased with increasing the glucose concentration.
1) H. Okuzaki ed., PEDOT: Materials Properties and Device Applications, S&T (2012).
2) H. Yano, K. Kudo, K. Marumo, H. Okuzaki, Sci. Adv., 5, eaav9492 (2019).
3) D. Hohnholz, H. Okuzaki, and A. G. MacDiarmid, Adv. Funct. Mater., 15, 51 (2005).
Lithiophilic Nanowire Architectures as Hosts for Lithium Metal Anodes
Authors: Abdul Ahad Syed , Bhattacharya Shayon , Ottaviani Michela , Ryan Kevin M , Kennedy Tadhg , Thompson Damien , Geaney Hugh 
Published: February 2024

Lithium (Li) metal is considered the ‘holy grail’ of battery anodes and has attracted enormous interest due to its low density (0.59 g cm-3), high theoretical capacity (3860 mAh g-1) and lowest electrochemical potential (-3.07 V vs. standard hydrogen electrode - SHE) [1-2]. However, several issues during its cycling in a Li-metal battery (LMB) have hindered its commercialization. Some notable problems include the formation of an unstable solid electrolyte interphase (SEI), excessive dendrite growth and subsequent short-circuiting during the Li stripping/plating process [3-4].
In our poster presentation, we will detail the design of a hierarchical nanowire (NW) – Carbon paper (CP) host for dendrite-free and stable cycling in LMBs. These NWs were grown on high surface area carbon paper substrate via a modified Vapour-Liquid-Solid (VLS) approach. The lithiophilic NWs enabled quick Li infusion (< 10 sec) in the NW-CP substrate whereas no Li infusion was possible in lithiophobic bare CP substrate (without the presence of NWs). Additionally, the NW morphology helped in reducing the localized current density on the surface of the NW-CP host, thereby promoting uniform Li deposition during plating/stripping process. With careful design of the NW-CP host, symmetric cell performance with high current density (3 mA cm-2) and areal capacity (3 mAh cm-2) was achieved for up to 500 h while a typical Li metal anode failed within 200 h. High loading NMC811 and high specific capacity Sulfur (S) cathodes demonstrated superior performance using NW-CP host as compared to pristine Li anodes.
In addition, we will also present some new concepts of NW decorated lithiophilic interlayers, which can be integrated with pristine Li metal anodes for uniform Li deposition. These lithiophilic interlayers can promote ‘bottom-up’ Li infilling between the Li-interlayer interface such that dendrite formation near the separator and eventual short-circuit is avoided. Detailed electrochemical as well as density functional theory (DFT) analysis shedding light on the improved lithiophilic properties of NW use in stabilizing Li metal anodes will also be presented. Overall, our work is aimed to develop high energy density (ED) Li metal anodes to meet the rising ED demands of electric vehicle (EV) industry.

References

[1] Nat. Nanotechnol.
2017, 12, 194.
[2] Chem. Rev.
2017, 117, 10403.
[3] Chem. Soc. Rev.
2013, 42, 9011.
[4] Chem. Rev.
2004, 104, 4303.