bluuebunny/crossref_metadata_2025_split huggingface dataset:
Creating Clinically-Relevant Biosensors-Integrating Hierarchically Structured Transducers with Dynamic Signal Recognition Elements
Authors: Soleymani Leyla , Chan Yuting , Hosseini Amin 
Published: February 2020

Biosensors combine biorecognition and signal transduction to analyze biologically-relevant species that are markers of disease or indicators of health. The performance metrics of biosensors, such as limit-of-detection and speed, are strongly influenced by the structure of the transducer. Designing material architectures that increase the sensor sensitivity, decrease background signals, and reduce analysis time is critical for entering biosensors into clinical decision making and health monitoring. Additionally, the specificity of biosensors are controlled by introducing biorecognition elements into the biosensing system. Developing biorecognition elements that specifically capture analytes of interest and effectively translate this capture to a detectible signal is the other critical piece of biosensor development. We have developed strategies for creating three-dimensional transducer architectures, combining them with dynamic biorecognition elements, and translating biorecognition into electrochemical signals.
All-solution-processing is used to create three-dimensional biosensing electrodes. This method combines self-assembly, electroless deposition, electrodeposition, and shape memory polymer substrates to create porous and wrinkled hierarchical electrodes. Biorecognition is achieved using molecular machines that release an electroactive DNA barcode in response to a target analyte, which is analyzed at the electrode surface using electrochemical readout.
Three-dimensional electrodes, biorecognition elements, and signal transduction components are integrated into microfluidic networks for sensing small molecules, nucleic acids, and proteins. This integrated biosensing platform is used for analyzing clinical samples, and a test with a clinically-relevant limit-of-detection is achieved.
A Real-Time Wearable Sensor to Monitor Alcohol Consumption through Ethyl Glucuronide Detection
Authors: Lin Kai-Chun , Sankhala Devangsingh , Muthukumar Sriram , Prasad Shalini 
Published: February 2020

Here we demonstrate for the first time a wearable sensor that can differentiate Ethyl Glucuronide (EtG) concentrations in synthetic human sweat correlating to the predicted alcohol consumption profiles of moderate drinkers. Alcohol consumption monitoring devices typically report blood alcohol content (BAC) through correlation with breath alcohol content (BrAC). However, the rapid decay of expressed ethanol can limit the application space of these devices. Alcohol is metabolized and excreted from the body by different processes or pathways, ethyl Glucuronide (EtG) is one of them and is produced in the liver. EtG is readily expressed and detectable in transdermal human sweat making it a promising candidate for wearable alcohol consumption monitoring.
A wearable biosensor device capable of reporting EtG levels in sweat both continuously via low power impedance spectroscopy is reported. The device was not only able to detect and respond to EtG present in the samples, but also able to differentiate each test scenario from one another. The three distinct EtG concentrations was designed as simulated drinking scenarios estimated to be 1, 2, and 3 standard U.S. drinks consumed over a duration of 60 minutes. It shows the ability for this device to act as an accurate reporter of EtG levels in low volume sweat (less than 5 microliter). The device will serve as a candidate tool for researchers to better understand and characterize the relationship between sweat EtG and consumed alcohol in real-time.
Facile Mn Surface Doping of Ni-Rich Layered Cathode Materials for Lithium Ion Batteries
Authors: Kim Jong Hwa , Cho Woosuk , Park Min-Sik 
Published: February 2020

As the electric vehicles (EVs) market is growing rapidly, lithium ion batteries (LIBs) have received great attention as a suitable power source owing to its high-energy density and excellent power characteristic. To extend a driving mileage of the EVs, it is crucial to further improve the energy density of LIBs. Since the specific capacity and operating voltage of cathode materials are important factors for determining the energy density of LIBs, many researches focus on the development of advanced cathode materials with high specific capacity and high operating voltage. Among various cathode materials, layered cathode materials (e.g., LiMO2, M = transition metal) have been one of the most popular cathode materials in LIBs. The electrochemical properties of these cathode materials are tunable by the choice of transition metals in the host structure; i) Mn secures structural stability, ii) Co increases power characteristic, and iii) Ni contributes to a specific capacity of the materials. In order to increase the achievable specific capacity, researchers have designed the layered cathode materials with a high Ni content (>80%) and they offer a high reversible capacity more than 190 mA h g-1. Unfortunately, Ni-rich layered cathode materials suffer from poor thermal and structural stabilities arising from the high Ni content in the structure. To overcome these limitations, therefore, structural modifications on the Ni-rich cathode materials is highly required to suppress undesirable side reactions and formations of impurities (e.g., NiO).
Herein, we prepare Mn surface-doped NCM811 (Mn-NCM811) with a core-shell structure via a simple wet-coating process using lithium ethoxide and Mn acetate precursors. Various structural and electrochemical investigations support that Mn-rich shell can effectively improve the structural and thermal stabilities of Ni-rich core, leading to the significant improvement in electrochemical performance of Ni-rich layered cathode materials even at a high operating temperature of 60 °C. From the results, we emphasize the importance of material design and this study will provide practical guidelines for development of Ni-rich layered cathode materials for LIBs.

References

[1] Y. –K. Sun, S. –T. Myung, B. –C. Park, J. Prakash, I. Belharouak, K. Amine, Nat. Mater.
8, 320-324 (2009).
[2] J. Lu, C. Zhan, T. Wu, J. Wen, Y. Lei, A. J. Kropf, H. Wu, D. J. Miller, J. W. Elam, Y. –K. Sun, X. Qiu, K. Amine, Nat. Commun.
5, 5693 (2014).

Figure 1
A Study on the Decontamination Possibility of Simulated Radioactive Inconel 600 – Co Alloy Using Electrorefining in LiCl-KCl Electrolyte
Authors: Choi Woo-Seok , Lee Young-Jun , Lee Seong-Hun , Lee Jong-Hyeon 
Published: February 2020

As the operating period of a nuclear power plant increases, the demand for dismantling of nuclear facilities has been rising, and the dismantling market is expected to continue to expand steadily. The Inconel 600, which was used as a material for the steam generator, has problem with crack and corrosion, and it is currently replaced with a steam generator of Inconel 690. It has been reported that if this steam generator is corroded or cracked, the cooling water contaminated with radioactive elements such as cobalt, strontium, may penetrate into the cracks. Therefore, development of decontamination technology for radioactive metal waste is essential to minimize waste during dismantling process.
This study investigates the decontamination possibility of Inconel 600 in LiCl-KCl-CoCl2-NiCl2 molten salt electrolyte. Inconel 600 – cobalt alloy was used for anode as a simulated radioactive metal waste. After electrorefining process, the cobalt remains in the molten salt. Therefore, CoCl2 was added to the electrolyte to imitate the case when the radioactive metal waste was dissolved and concentrated in the electrolyte. Electrochemical analysis was performed by cyclic voltammetry (CV) to confirm the redox behavior of Ni ions in molten salt electrolytes. Decontamination experiments were performed by chrono potentiometry (CP) to analyze the oxidation behavior of Inconel 600 – cobalt alloy (anode) and the reduction behavior of Ni on Ni plate electrodes (cathode). Decontamination factor(DF) of the deposits produced by electrorefining was analyzed by ICP.
Simultaneous SECM-AFM-Ters Mapping of Electrocatalytic Reactions on a Nanometric Scale
Authors: Schechter Alex , Subramanian Palaniappan , Kolagatla Srikanth 
Published: February 2020

We have developed and used Scanning Electrochemical Microscopy-Atomic Force Microscopy (SECM-AFM) imaging technique that can provide high resolution detailed electrochemical and spectral information of oxygen reduction reaction (ORR) reaction at a lateral resolution of less than 50 nm. The ORR activity of an individual unsupported Pt nanoparticle, carbon-supported Pt aggregates and Fe, N surface modified graphitic carbon was mapped under selected reduction conditions. This newly developed method utilizes a gold coated SiO2 tip imbedding a 50 nm diameter Pt electrode. positioned at a constant working distance of ~4-8 nm above the catalyst surface using force feedback control. A 532 nm Raman laser directed to the apex of the tip was applied to collect tip enhanced Raman spectral (TERS) signal of the reaction byproduct (H2O2). Thus, we simultaneously mapped the electrochemical oxygen reduction by the Pt tip electrode and measured the H2O2 oxidation currents on the gold coating secondary electrode and at the same time reordered the peroxide tip enhanced Raman signal under the same scanned area. A direct evidence was seen, showing for the first time that the same active ORR sites are also responsible for peroxide formation (figure 1). Moreover, on a nanometric level ORR proceed mostly via 2 electron reaction to hydrogen peroxide rather than the literature reported 4 electrons reduction of O2 to water, as widely accepted from other electrochemical techniques.
Fig. 1. Nanoscale Mapping of Catalytic Hotspots on Fe, N -modified HOPG by Scanning Electrochemical Microscopy-Atomic Force Microscopy [1].
[1] Srikanth Kolagatla, Palaniappan Subramanian and Alex Schechter*, Nanoscale, 2018, 10, 6962

Figure 1
Potentiometric Tip Electrodes for Improved Visualization of Galvanic Corrosion Processes Using SECM
Authors: Filotás Dániel , Fernández-Pérez Bibiana M. , Nagy Lívia , Nagy Géza , Souto Ricardo M. 
Published: February 2020

Galvanic corrosion of magnesium is one of the main reasons of the limited usage of this metal. Therefore the galvanic corrosion of magnesium is of great scientific and industrial interest. Among many analytical methods being used, Scanning Electrochemical Microscopy (SECM) has the advantage of chemical surface imaging with high spatial and temporal resolution. When it comes to Mg corrosion, the amperometric mode of SECM is an attractive option although Mg ions cannot be measured directly due to the high negative overvoltage of Mg2+ reduction. Instead, the feedback mode and hydrogen detection in sample generator – tip collector mode are employed [1]. However, H2 oxidation is not a diffusion controlled process and local ion concentrations may affect the oxidation current.
Alternately, SECM can be employed in potentiometric mode. In this case, the sensing probe is an ion selective microelectrode (ISME) which potential is measured against a reference electrode using an operational amplifier-based voltage follower. In this way, direct measurement of Mg2+ distribution has been achieved [2]. However, the occurrence of electric field effects for Mg corroding under galvanic coupling has been demonstrated [3]. Electric cross-talk shifts the measured potentials with respect to the calibration completed in unbiased conditions, resulting in the determination of wrong ion activities.
The work reported here demonstrates the applicability of ion selective electrodes in multibarreled arrangement for simultaneous monitoring of pH and Mg2+ distribution above AZ63 magnesium alloy using SECM. The superior performance of multibarreled tips containing an internal reference electrode compared to “traditional’ single barreled electrodes and double barreled electrodes is shown.
References:
[1] S.S. Jamali, S.E. Moulton, D.E. Tallman, M. Forsyth, J. Weber, G.G. Wallace, Electrochim. Acta 152 (2015) 294.
[2] N.A. Chaniotakis, J.K. Tsagatakis, E.A. Moschou, S.J. West, X. Wen. Anal. Chim. Acta 356 (1997) 105.
[3] A. Kiss, D. Filotás, R. M. Souto, G. Nagy, Electrochem. Commun. 77 (2017) 138.
Characterizing the Surface Free Energy of Composite Electrodes for Li-Ion Batteries
Authors: Li Jianlin , Davoodabadi Ali , Jin Congrui , Wood David L. 
Published: February 2020

One of the crucial steps in battery manufacturing is the electrolyte wetting step which typically requires a relatively long time to be completed. It is known that the relationship between polar and dispersive components of the electrolyte surface tension and the electrode surface free energy (SFE) plays a vital role in the extent of wetting and, thus, tuning the SFE can accelerate the wetting step in battery manufacturing.
This work developed and validated a systematic approach to characterize surface free energy of composite electrodes for lithium-ion batteries, which has never been reported in literature. It’s demonstrated as shown in Figure 1 [1] that the SFE of LiNi0.5Mn0.3Co0.2O2 cathode was higher than the graphite anode. In addition, when switching manufacturing from conventional solvent based processing to aqueous processing, the polar component of SFE increases; it increases 74.1% from NMC532-NMP to NMC532-Water, and 48.2% from A12-NMP to A12-Water due to different binders. SFE decreases with reducing porosity. The results provide valuable guidance for our goal to optimize the electrolyte wetting process, helping lower costs and enable higher product quality. In addition, the method allows us to characterize the SFE of electrodes and optimize electrolyte wetting via tailored electrode manufacturing, including slurry and electrode formulation, mixing sequences, drying protocols and calendering. Figure 1 Surface energy of electrodes Reference:
[1] A. Davoodabadi, J. Li, Y. Liang, R. Wang, H. Zhou, D.L. Wood III, T. J. Singler, and C. Jin, Journal of the Electrochemical Society, 165(11) (2018) A2493-A2501

Figure 1
Battery Characterization Using Operando Optical Diagnostics
Authors: Porter Jason Morgan , Saqib Najmus 
Published: February 2020

Battery development is being accelerated by the use of operando characterization tools, which provide real-time measurements of chemistry and transport during battery operation. While much attention has focused on recent advancements in diagnostic tools, such as x-ray spectroscopy and tomography or neutron reflectometry, optical diagnostics continue to provide new insights into battery chemistry and transport. Optical diagnostics, including ultraviolet and infrared absorption spectroscopy, Raman spectroscopy, optical microscopy, and fluorescence, are being used to study complex battery phenomena from dendrite growth and solid electrolyte interface formation to electrolyte stability.
Optical access is a fundamental challenge to using optical characterization in batteries, as electrochemistry necessarily occurs between two conductors, which are opaque to electromagnetic radiation in the UV, visible, and infrared. While transparent conductors have been used in select cases, most optical characterization studies employ custom electrochemical cells with modified battery geometries to allow for optical access (so called “spectro-electrochemical” cells). Spectro-electrochemical cells create unique challenges for operando battery characterization, as the observed trends are necessarily impacted by modifications to battery geometry and materials. The recent commercialization of spectro-electrochemical cells is accelerating adoption of these techniques.
In this work, we review operando optical characterization tools applied to battery research. A recently developed diagnostic using attenuated total reflection infrared spectroscopy is also presented, including applications in lithium sulfur and lithium ion batteries. Operando measurements of the polysulfide shuttle mechanism in a Li-S battery is presented, including the impact of additives on the shuttle mechanism. Electrolyte decomposition in Li-ion batteries during SEI formation is also reported. Finally, operando measurements of electrolyte chemical stability during battery operation at elevated temperature is presented. An optical thermometry technique is also demonstrated for internal battery temperature measurements.
Pressure Evolution in Constrained Li Metal Pouch Cells
Authors: Raj Abhi , Dickerson Charles C , Niu Chaojiang , Xiao Jie , Steingart Daniel A. , Dufek Eric J. , Liaw Boryann 
Published: February 2020

Increased research in lithium metal anodes has been motivated by a rising need for high energy density batteries for transportation and portable electronics applications. While promising a low redox potential and high specific capacity, lithium is hindered by nonuniform deposition on the anode surface, as well as unwanted side reactions with the electrolyte as fresh lithium is exposed during discharge. The majority of research in this area has been done with coin cells [1, 2], which are unsuitable for scaling towards practical applications and mask variations across an electrode as well as gas evolution during cycling.
In this work, we demonstrate the use of a fixed-gap fixture to monitor pressure evolution across a 7-layer Li metal/NMC 622 pouch cell. While initial cycles exhibit a linear and reversible change in pressure as a function of state of charge, the baseline pressure steadily increases at the end of discharge with continued cycling, indicating lost inventory of lithium. Moreover, towards the end of cycling as the cell approaches sudden failure, large increases in baseline pressure are correlated to gas evolution within the cell. These correlations are further supported by electrochemical data, specifically through changes in polarization at the beginning of a charge or discharge step, or through peaks in dQ/dV curves at later stages during charge.

References:

[1] Xu, W. et al., “Lithium metal anodes for rechargeable batteries,” Energy Environ. Sci., 2014, 7, 513-537. DOI: 10.1039/C3EE40795K
[2] Liu, Y. et al., “An Artificial Solid Electrolyte Interphase with High Li-Ion Conductivity, Mechanical Strength, and Flexibility for Stable Lithium Metal Anodes,” Adv. Mater., 2017, 1605531. DOI: 10.1002/adma.201605531
Four-Electrode Setup for Electrochemical Impedance Spectroscopy Study of Lithium–Sulfur Batteries
Authors: Fang Jie , Ghashghaie Sasan , Shahzad Hafiz Khurram , Chung Chi Yuen 
Published: February 2020

The practical lithium-sulfur batteries (LSBs) show less capacity and energy density than the theoretical values (1675 mAh/g and 2570 Wh/kg) [1]. The insulated Li2S (the end-product of discharge) and dissolved polysulfide intermediates lead to a growth of internal resistance, which reduces the output voltage, rate performance, and efficiency of energy storage. Although the internal resistance of LSBs has been investigated by the EIS method for studying fading mechanism, polysulfides reactivity, and diffusivity, it is still a challenge to in situ monitor the impedance of cathode and anode [2,3]. We have compared cells with two and three-electrode setups for EIS measurements and demonstrated the influence of electrochemical asymmetric in three-electrode setup. To overcome the drawback of the three-electrode cell, a novel four-electrode symmetric cell was proposed. The resistance of the anode solid electrolyte interphase (SEI), the interface between the porous current collector and the case of the coin cell, the electrolyte in the separator, porous structure, and the charge transfer process of active materials were evaluated at a different state of dis/charge. The change of polysulfides concentration induced a mountain in the resistance maps of anode SEI and the electrolyte in the separator. The liquid state polysulfides and solid phase Li2S came together to produce two resistance peaks in the map of the porous structure. For charge transfer resistance, there were two local minima which were caused by the reactions of different polysulfide species. Moreover, the passivation of the cathode by Li2S gave a high charge transfer resistance and limited the complete use of active materials. The increase of electrolyte resistance in the separator indicated a continued consumption of electrolyte.
References
[1] B.D. McCloskey, Attainable gravimetric and volumetric energy density of Li–S and Li Ion battery cells with solid separator-protected Li metal anodes, J. Phys. Chem. Lett. 6 (2015) 4581–4588. doi:10.1021/acs.jpclett.5b01814.
[2] Z. Deng, Z. Zhang, Y. Lai, J. Liu, J. Li, Y. Liu, Electrochemical impedance spectroscopy study of a lithium/sulfur battery: Modeling and analysis of capacity fading, J. Electrochem. Soc. 160 (2013) A553–A558. doi:10.1149/2.026304jes.
[3] S. Drvarič Talian, J. Moškon, R. Dominko, M. Gaberšček, Reactivity and Diffusivity of Li Polysulfides: A Fundamental Study Using Impedance Spectroscopy, ACS Appl. Mater. Interfaces. 9 (2017) 29760–29770. doi:10.1021/acsami.7b08317.
(Invited) Unravelling Solvation Phenomena in Glyme-Based Electrolytes for Na-O2 Batteries
Authors: Ortiz Vitoriano Nagore , Sacci Robert L , Bridges Craig A. , Arcelus Oier , Enterria Marina , Carrasco Javier , Veith Gabriel M. 
Published: February 2020

Research into new energy storage technologies, for both portable and stationary applications, has become an urgent necessity. Rechargeable metal-air (oxygen) batteries are receiving intense interest as possible alternatives to lithium-ion batteries, because of their potential to provide higher gravimetric energies. While much attention has been focused on aprotic Li-O2 batteries, substantial challenges must be addressed before widespread commercialization is possible. Recently, a metal-air battery in which lithium has been replaced by sodium has received increasing attention.1 Although Na-O2 batteries (NABs) present lower gravimetric energies on a cell basis (1605 or 1108 Wh/kg based on Na2O2 or NaO2 discharge products, respectively)2 than Li-O2 batteries (3505 Wh/kgLi2O2),3 much lower charge overpotentials (~100 mV) than those in typical Li-O2 batteries (~1000 mV) have been reported based on reversible sodium superoxide (NaO2) formation.
At present, Na systems have mostly been designed according to strategies developed for Li-O2 research which, though a useful initial approach, may have led to the use of suboptimal materials due to the current lack of exploration in this area. The vast majority of the work has been devoted to electrode materials, with little or negligible work on electrolytes which – as the component responsible for ion transportation between the electrodes - are key of any optimized NAB system.
Glyme-based solvents have been widely used in NABs but their selection seems arbitrary and most of the studies do not consider the differences these glymes might have. In this work, we demonstrate that the selection of the solvent plays an important role on the cell chemistry and performance. The coordination number of different glymes measured by infrared spectroscopy and coupled with density functional theory revealed different solvation behavior. Moreover, the enthalpy of dissolution measured using isothermal microcalorimetry varies significantly as a function of solvent selection. In addition, the rechargeable nature of Na-O2 batteries is governed by the formation and oxidation of NaO2, making it vital to study the effect of the electrolyte in the presence of NaO2, and also to prevent the formation of irreversible side products.

References

1 I. Landa-Medrano, C. Li, N. Ortiz-Vitoriano, I. Ruiz de Larramendi, J. Carrasco and T. Rojo, J. Phys. Chem. Lett., 2016, 7(7), 1161–1166.
2 P. Hartmann, C. L. Bender, M. Vračar, A. K. Dürr, A. Garsuch, J. Janek and P. Adelhelm, Nat. Mater., 2013, 12, 228–32.
3 D. G. Kwabi, N. Ortiz-Vitoriano, S. A. Freunberger, Y. Chen, N. Imanishi, P. G. Bruce and Y. Shao-Horn, MRS Bull., 2014, 39, 443–452.