bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Paper-Based Surface-Enhanced Raman Scattering (SERS) Biosensor for Label-Free Detection of Serum Bilirubin for Diagnosis of Jaundice
Authors: Li Ming 
Published: July 2021

Jaundice continues to be a serious health concern and is among the leading causes of deaths during the first days of newborn babies’ lives. Serum bilirubin is currently being exploited in the clinic as a key biomarker for the diagnosis and management of neonatal jaundice. The commonly used methods for serum bilirubin determination in clinical settings are direct spectroscopic measurement and the diazo reaction method. These methods have drawbacks such as low sensitivity, matrix interference, poor stability, high-cost, professional training, less specificity and tedious sample preparation. Thus, it is very urgent to develop a rapid and economical route for sensitive and specific detection of free bilirubin directly in human serum.
Surface-enhanced Raman scattering (SERS) has emerged as a powerful analytical technique for biosensing applications with high sensitivity, molecular specificity, powerful multiplex detection capability, and excellent photostability. This talk will present our recent study on the development of a paper-based SERS biosensor for label-free detection of bilirubin in serum. This biosensor comprises multifunctional graphene oxide-gold nanostar (GO-GNS) hybrids decorated on the filter paper. This biosensor combines the enrichment for serum bilirubin and plasmonic enhancement for Raman signals of bilirubin for boosting the label-free detection sensitivity directly in blood serum without the need for additional sample preparation. Our results demonstrated the excellent detection performance for detection of bilirubin directly in serum in a label-free manner, and the detection results were compared with the commercial diazo reaction method, which justifies the clinical effectiveness and suitability of the present paper-based SERS biosensor. We believe that the present paper-based SERS biosensor has great potential for clinical translation in accurate diagnosis of jaundice and other related diseases.

Reference:

Xiang Pan, Linhu Li, Hangduo Lin, Jiayi Tan, Haitao Wang, Mengling Liao, Caiju Chen, Beibei Shan, Yingfan Chen, Ming Li, A graphene oxide-gold nanostar hybrid based-paper biosensor for label-free SERS detection of serum bilirubin for diagnosis of jaundice, Biosensors and Bioelectronics, 2019, 145, 111713.
(Invited) Electrochemiluminescence Biosensing: From Bead-Based Immunoassays to Cell Microscopy
Authors: Sojic Neso 
Published: July 2021

Electrogenerated chemiluminescence (ECL) is the process of light emission by the excited state of a luminophore upon electrochemical stimulation[1-2]. To increase the sensitivity and the multiplexing performances of ECL, many efforts have been focused on the development of novel analytical strategies and original imaging applications. In this lecture, we will present a few recent works on biosensing[3-5] and cell microscopy[6-7], which exploit the remarkable characteristics of ECL.
Bead-based ECL assays have been the object of numerous works and they are currently commercialized for more than 150 immunoassays. In a first part, new ECL approaches based either on the light polarisation or on semi-conductors will be presented to extend the performances of ECL[3-4]. In a second part, the development of coreactant-based ECL as a surface-confined microscopy to image single cells and their membrane proteins will be discussed[5-7].
References

A. J. Bard. Electrogenerated Chemiluminescence. M. Dekker. 2004.

N. Sojic. Analytical Electrogenerated Chemiluminescence: from Fundamentals to Bioassays. Royal Society of Chemistry. 2019.

F. Zinna, S. Voci, L. Arrico, E. Brun, A. Homberg, L. Bouffier, T. Funaioli, J. Lacour, N. Sojic, L. Di Bari. Angew. Chem. Int. Ed., 58, 6952 (2019).

Y. Zhao, J. Yu, G. Xu, N. Sojic, G. Loget. J. Am. Chem. Soc., 141, 13013 (2019).

M. Sentic, M. Milutinovic, F. Kanoufi, D. Manojlovic, S. Arbault, N. Sojic Chem. Sci., 5, 2568 (2014)

G. Valenti, S. Scarabino, B. Goudeau, A. Lesch, M. Jović, E. Villani, M. Sentic, S. Rapino, S. Arbault, F. Paolucci, N. Sojic. J. Am.
Chem. Soc., 139, 16830 (2017).

S. Voci, B. Goudeau, G. Valenti, A. Lesch, M. Jović, S. Rapino, F. Paolucci, S. Arbault, N. Sojic. J. Am.
Chem. Soc., 140, 14753 (2018).
Investigation of Calcium Alloying with Sb, Sn and Bi As Negative Electrode Materials for Rechargeable Calcium Battery in Non-Aqueous Electrolytes
Authors: Baltruschat Helmut , Xing Da 
Published: July 2021

Alloys were suggested as alternative anode materials for Ca metal anode because they have a high specific capacity and low overpotential. [1] A DFT study of CaxM has suggested a variety of alloy-type anode materials and considered the alloying voltage, volume expansion, and specific capacity. The metals such as Si, Sb, Bi, Al, Pt, Pb, and so on were predicted to be promising inexpensive anode candidates. [1] An Sn Nano-particular with a thickness of 25 μm was investigated for both the anode and current collector using 0.8 M Ca(PF6)2 in EC:PC:DMC:EMC (2:2:3:3) electrolytes. [2] It’s showed a high and wide voltage window (up to 4.8 V) and the cell could be cycled more than 300 cycles. The alloying compounds were found to be different phases with finally Ca7Sn6.
In this work, we study the fundamentals of the alloying process alloying of Ca thin film of bulk Sb, Sn, and Bi on polycrystalline Au using non-aqueous electrolyte (1.5 M Ca(BH4)2 in THF) at room temperature. Calcium stripping and plating using a Ca(BH4)2 in THF electrolyte shows high Coulombic efficiency (95 %) at room temperature on an Au substrate. [3] The cycling reversibility of alloying/de-alloying with Sb, Sn, and Bi have been demonstrated. The cyclic voltammogram for Ca insertion/de-insertion into Sb, Sn, and Bi-modified electrode shows a positive shift of the onset potential of Ca deposition compared to that at bare Au electrode. The ratio of moles of Ca to Sb, Sn, and Bi agrees with the stoichiometry of CaSb2, CaSn2, and CaBi3 alloy. Potential step were used to study the kinetics of insertion. The diffusion coefficient of Ca into the Sb, Sn, and Bi layers is calculated to be 10−14 𝑡𝑜 10−15 cm2s-1.

Acknowledgments: The authors acknowledge funding by the Federal Ministry of Education and Research of Germany (BMBF, FKZ; 03EK3027A).
[1] Z. Yao, V. I. Hegde, A. Aspuru-Guzik, and C. Wolverton, Advanced Energy Materials 9:1802994 (2019).
[2] N. Z. Wu, W. J. Yao, X. H. Song, G. Zhang, B. J. Chen, J. H. Yang, and Y. B. Tang, Advanced Energy Materials 9:7 (2019).
[3] D. Wang, X. Gao, Y. Chen, L. Jin, C. Kuss, and P. G. Bruce, Nature Materials 17:16 (2017).
Host-Guest Complex for Heparin Binding and Sensing
Authors: Välimäki Salla , Beyeh Ngong Kodiah , Linko Veikko , Ras Robin , Kostiainen Mauri 
Published: July 2021

Heparin is a naturally occurring highly charged polyanion and a well-known anticoagulant widely used in surgical practice.[1] More specifically, it is a negatively charged sulfated polysaccharide belonging to the group of glycosaminoglycans. The anticoagulant effect of heparin is based on its ability to activate antithrombin-III, which, subsequently, inactivates vital coagulation cascade substance such as thrombin and factor Xa consequently preventing fibrin and clot formation.[2] To balance and neutralize heparin dosing, a heparin inhibitor is needed, and commonly, arginine-rich protein protamine sulfate (PS) is used for this purpose.[3] However, in recent years there has been an interest to investigate alternatives for protamine due to its adverse effects like hypotension and serious allergic reactions.[4]
In this study, a host-guest complex capable of selective heparin binding and sensing is presented.[5] Heparin binding affinity was studied in solution with a variety of polycationic macrocyclic hosts, a pillar[5]arene and multiple resorcin[4]arenes, by dynamic light scattering, dye displacement assay, isothermal titration calorimetry, and anti-Xa assay. The measurements reveal the significant importance of multivalency in the electrostatic host-heparin binding in competitive, application-relevant media. Additionally, to monitor heparin concentration, a host-guest indicator displacement assay was performed by following the free and bound state of methyl orange dye in UV-Vis spectroscopic experiments. Furthermore, this colorimetric sensing based on the tertiary host-guest-heparin supramolecular assembly was utilized in the construction of a calibration curve in a range of blood plasma concentrations.

Figure 1
Towards Tailored Carbon Nanotube-Based Fluorescent Sensors
Authors: Nißler Robert , Kruss Sebastian 
Published: July 2021

Single-walled carbon nanotubes (SWCNTs) are an emerging building block for nanoscale sensors and labels because of their unique photophysical properties. Semiconducting SWCNTs fluoresce in the tissue transparency near infrared (nIR) window (840 – 1650 nm) and do not bleach. Due to their 1D nature small perturbations in their environment strongly affect their fluorescence. The major challenges in using SWCNTS for sensing is on the one side their purification and on the other side a tailored surface chemistry for molecular recognition and photophysical signal transduction.
Here, we present different approaches to tailor SWCNT surface chemistry and fluorescence emission properties for the detection of biologically important metabolites. Firstly, we tuned the sensitivity of ssDNA/SWCNTs against the neurotransmitter dopamine and different plant polyphenols by changing systematically the DNA sequence. In a more rational approach, we engineered DNA strands conjugated to small peptide sequences. In order to enable a ratio-specific linkage, we determined the amount of bound DNA on the SWCNT surface, which was further observed to play an important role in maintaining colloidal stability of the modified ssDNA/SWCNT conjugates. Finally, aptamer-based approaches were used to combine stable surface modification with target selective binding. For all these approaches we demonstrated via nIR-fluorescence spectroscopy and nIR-fluorescence stand-off imaging that tailoring these nanosensors resulted in an increased specificity against their targets, ranging from small chemical communication compounds (dopamine, H2O2) to cell wall components and secreted enzymes and metabolites. Lastly, we demonstrate that these tailored SWCNT sensors can also be transferred to purified nanotube building blocks, which enables a predictable design concept for sensor properties (emission wavelength and target specificity).
Developing Polymer Electrolytes with Balanced Thermomechanical and Conductive Properties through Incorporation of High Aromatic Content
Authors: Baroncini Elyse 
Published: July 2021

Thermomechanical and electrochemical properties of thiol-ene polymers with high aromatic content afforded by lignocellulosic biomass were evaluated to explore feasibility and advantages in polymer electrolyte applications. Polymer electrolytes have the potential to mitigate stability and safety concerns accompanying incumbent liquid electrolyte systems in lithium-ion batteries. The thermal properties associated with low glass transition temperature (T
g) polymers are thought to improve contact with electrodes and ionic flow through the membranes compared to other liquid electrolyte alternatives such as solid electrolytes. Additionally, the high aromatic content of the lignin macromolecule can impart mechanical and thermal stability, making it attractive for use in applications that require robust polymers.
Low molecular weight fractions of wheat straw/Sarkanda grass soda lignin were functionalized and prepared through thiol-ene polymerization into polymer electrolytes. In combination with previous work, it was determined that differing solubility, functionality, and aromatic content of lignin fractions vary the glass transition temperatures of the resulting polymers and the suitability for electrolyte applications. The wheat straw/Sarkanda grass soda lignin utilized in solid polymer electrolytes (SPEs) displayed room temperature conductivity values in the range of 5 – 7 x 10-5 S cm-1. The lignin-based SPEs exhibited excellent cationic transport with ion transference values up to 0.90. Voltage stability and compatibility with electrode materials were also explored. The promising conductivity and ion transference results reveal the potential for use of functionalized, low molecular weight wheat straw/Sarkanda grass soda lignin in SPE applications as a way to improve thermal stability, electrochemical performance, and incorporate an abundant, sustainable resource in a high performance application.
Evaluation of Redox Mediator’s Oxidation Stability in Lithium-Oxygen Batteries
Authors: Kim Hun , Kwak Won-Jin , Park Jiwon , Aurbach Doron , Byon Hye Ryung , Sun Yang-Kook 
Published: July 2021

Employing organic redox mediators (ORMs) as mobile catalyst into the electrolyte system has been selected as an important strategy to lower the charging overpotentials in lithium-oxygen (Li-O2) batteries. Careful choice of molecular designs of ORMs can also tailor their redox potential and rate of electron-transfer to improve the catalytic efficiency. However, the stability of ORMs in Li–O2 cells was scarcely studied. In here, catalytic efficiency and stability of several important ORMs are assessed through in situ gas analysis and reactivity tests with singlet oxygen. Some well-known ORMs are detrimentally decomposed during the first cycle in Li–O2 cells, whereas nitroxyl-radical-based ORMs bear the most stable and efficient response. Analogous nitroxyl-radical derivatives further increase round-trip energy efficiency and electron-transfer kinetics. This study also emphasizes the evaluation of chemical stability of ORMs, which are mandatory for the long-term cyclability in Li–O2 cells.
references

W.-J. Kwak, H. Kim, H.-G. Jung, D. Aurbach, Y.-K. Sun, J. Electrochem. Soc.
2018, 165, A2274–A2293.

W.-J. Kwak, H. Kim, Y. K. Petit, C. Leypold, T. T. Nguyen, N. Mahne, P. Redfern, L. A. Curtiss, H.-G. Jung, S. M. Borisov, S. A. Freunberger and Y.-K. Sun, Nat. Commun., 2019, 10, 1380.
Non-Confinement Approach Towards Employing Carbonate-Based Electrolytes in Li-S Battery
Authors: Pai Rahul , Kalra Vibha 
Published: July 2021

Rechargeable lithium-sulfur (Li-S) batteries have received increasing attention due to the high theoretical capacity of sulfur cathodes (1675 mAh.g-1), abundance, environmental friendliness, low toxicity and low cost of elemental sulfur. The commercialization of this technology, however, relies heavily on tackling yet unsolved operational issues that hinder the practical energy density delivered by Li-S batteries, such as (i) low electrical conductivity of sulfur and lithium sulfide (Li2S), (ii) severe capacity fade due to shuttling of long-chain lithium polysulfides, and (iii) lithium dendrite growth. In addition, another major obstacle towards commercialization is use of ether-based electrolytes owing towards its high flammability slightly above room temperature.
Carbonate-based electrolytes demonstrate safe and stable electrochemical performance in lithium ion batteries. Literature reports have demonstrated that sulfur can trigger substantial electrolyte decomposition due to formation of polysulfides to exhibit sudden battery failure. However, few types of cathodes with confinement of sulfur and cross-linking with polymer can be employed. However, higher sulfur loading, and improved conductivity of cathode still remains a prominent challenge in carbonate-based electrolyte. In this work, we have developed free-standing carbon nanofiber/S cathodes for achieving long-term cycling in Li-S batteries. The as-prepared CNF/S (1 – 5 mg.cm-2, ~50 wt% S) cathodes were used directly in 2032 type coin cells. The electrochemical tests were performed in EC:DEC based electrolyte against Li/Li+anode. The cyclic voltammetry and charge discharge results showed a single potential for conversion of sulfur to Li2S. The CNF/S cathodes delivered capacity of ~1300 mAh.g-1 during the first cycle with ~93% coulombic efficiency. The capacity of Li-S cells was stabilized at ~800 mAh.g-1 after Ist cycle and sustained up to 4000 cycles with only ~.01% decay rate per cycle. The postmortem XRD results confirmed the conversion of sulfur to Li2S and vice versa. Further, postmortem XPS analysis was conducted to understand the underlaying conversion mechanism. The preliminary results showed that the observed single plateau and long-term cycling of Li-S cells were the convoluted effect of deposited sulfur and digression from typical polysulfide formation route.
Understanding Sodium Ion Transport in Cathode Materials for Na-Ion Batteries Using MD Simulations
Authors: Seth Deepak , Haider M. Ali , Agarwal Manish , Anjum Uzma , Wani M. Shaharyar , Khan Tuhin S 
Published: July 2021

Classical molecular dynamics (MD) simulations are applied to study the transport of Na-ions in cathode materials for Na-ion batteries (SIB). Two different materials (NaxV4O10 [1] and in NaxTi2(PO4)3) are studied to access and compare the level of Na-ion diffusion in electrode structure. Sodium constitute a potential alternative of Lithium in alkali metal batteries, since sources of Li are limited, and Na is readily available. The diffusion coefficient of Na-ions in SIB materials is reported in a wide range of experimental methods (potentiostatic titration, impedance measurements etc.). However, reported values differ from 2 to 4 orders of magnitude based on the experimental method used, since diffusivity estimates specifically from impedance curves are often measured away from the equilibrium and fitting parameters are prone to produce large errors. MD simulations using universal force field have provided a direct assessment of self-diffusion coefficient of Na-ions in the structure of NaxV4O10 with varying concentrations of Na-ions (0.33 < x < 1.33), calculating a diffusion coefficient of 5.75 x 10-8 cm2/s for x=0.66 at 300 K, which is in good agreement with experiments. Mean square displacement (MSD) and Na-ion density plots are further providing a mechanistic insight on the route of Na-ion transport.[2]
As a next generation material, NASICON structured type (NaTi2(PO4) SIB materials, are investigated for Na-ion transport. Inter-atomic based partial charge potential model is applied, and concentration of Na-ion is varied (from 0.82 <x < 0.98) in the supercell (total of 9000 atoms) of NaxTi2(PO4)3 at 323 K. Na+ transport of five different runs at varying concentration of Na+ are calculated and MD trajectory are visualized. MSD of Na+ as a function of time is shown as Figure. Self-diffusion coefficient of Na+ is calculated from the slope of MSD vs time plot for the three-dimensional transport, following Einstein’s relation. Calculated diffusivities are in the range of ~10-8-10-9 cm2/s and corresponding ionic conductivity is estimated to be (~10-4 S/cm). These values are in agreement with experimentally measured values of Na-ions in the similar structure.

References

Saroha, R., Khan, T.S., Chandra, M., Shukla, R., Panwar, A.K., Gupta, A., Haider, M.A., Basu, S. and Dhaka, R.S., 2019. Electrochemical properties of Na66V4O10 nanostructures as cathode material in rechargeable batteries for energy storage applications. ACS omega, 4(6), pp.9878-9888.

Wani, M.S., Anjum, U., Khan, T.S., Dhaka, R.S. and Haider, M.A., 2020. Understanding Na-Ion Transport in NaxV4O10 Electrode Material for Sodium-Ion Batteries. Journal of Electronic Materials, pp.1-6.

Figure 1
“Na Redistribution” Induced By K Intercalation during Na/K Ion Exchange in a Layered Oxide Cathode
Authors: Kim Haegyeom , Kwon Deok-Hwang , Kim Jae Chul , Ouyang Bin , Kim Hyunchul , Yang Julia , Ceder Gerbrand 
Published: July 2021

An ion exchange reaction that can stabilize potassium transition metal oxides was proposed as a new approach to develop cathode materials for K-ion batteries (KIBs).1-4 Such ion exchange method indeed has frequently used for the development of novel Li-layered oxides to attain structural features of Na layered oxides.5-7 Although the ion exchange reaction has the potential to discover novel layered cathode materials by accessing the metastable states that cannot be achieved by conventional high-temperature solid-state reaction, the solid-state ion-exchange mechanism and the resulting phase evolution are barely understood.
In this study, we systematically investigate electrochemical Na+/K+ ion exchange in layered oxides. 8 Here, O3-type Na3Ni2SbO cathode is used as a model system.8 We found intriguing phase evolutions according to the relative Na/K content upon K intercalation by in-situ X-ray diffraction study. First, we observe that K-rich and Na-rich phases coexist during charging and discharging. Second, Na-rich phase goes through phase transformation upon K intercalation. Strong electrostatic repulsion between Na and K ions that have radically different bond lengths to coordinating oxygen ions can result in this complex phase evolutions. We uncovered that the intercalating K ions pushes away Na ions remaining in the desodiated Na
x
Ni2SbO6 phase, thereby separating Na-rich and K-rich phases in a particle. Interestingly, this phenomenon creates complex, three-phase equilibrium during the desodiation and potassiation processes in Na
x
K
y
Ni2SbO6: phase equilibrium between one K-rich and two Na-rich phases or two K-rich and one Na-rich phase is observed, as dictated by the Gibbs phase rule. Our computational study further demonstrated that this phase separation originates from the large lattice mismatch along the c-axis between the K-rich and Na-rich phases. Our observations and interpretations demonstrate that “ion-exchanged” systems may be more complex to interpret than the previously understood. Our analysis should be applicable to other ion-exchange systems where the exchanged ions are not well miscible in the host structure.

References

[1] S. Baskar et al. ECS Transactions
2017, 80, 357.
[2] N. Naveen et al. Chem. Mater.
2018, 30, 2049.
[3] J. Y. Hwang et al. Energy Environ. Sci.
2018, 11, 2821.
[4] H. Zhang et al. Chem. Commun.
2019, 55, 7910.
[5] C, Delmas et al. Mater. Res. Bull.
1982, 17, 117.
[6] A. R. Armstrong et al. Nature
1996, 381, 499.
[7] F. Capitaine et al. Solid State Ionc.
1996, 89, 197.
[8] H. Kim et al. Chem. Mater.
2020, 32, 4312.