bluuebunny/crossref_metadata_2025 huggingface dataset:
A Dual-Channel Biosensor Enables Concurrent Detection of Pathogens and Antibiotic Resistance
Authors: Vernick Sefi , Gunasekaran Dharanivasan
Published: August 2024

Diarrhoeagenic infections, commonly treated with β-lactam antibiotics, contribute to antibiotic resistance - a pressing public health concern. Rapid monitoring of pathogen antibiotic resistance is vital to combat antimicrobial spread. Current bacterial diagnosis methods identify pathogens or determine antibiotic resistance separately, necessitating multiple assays. There is an urgent need for tools that simultaneously identify infectious agents and their antibiotic resistance at the point of care (POC). We developed an integrated electrochemical chip-based biosensor for detecting enteropathogenic E. coli. Leveraging an antibody against the virulence marker EspB, the dual-channel chip facilitated electrochemical impedance spectroscopy-based detection of EspB antigen (sensitivity of 10 ng/mL) and EspB-expressing bacteria. For β-lactam resistance profiling, a second channel enabled differential-pulse voltammetric measurement of hydrolyzed nitrocefin, a β-lactam analogue, demonstrating sensitive detection of the antibiotic resistance marker, β-lactamase at concentrations as low as 1 ng/mL. The integrated electrochemical biosensor successfully achieved simultaneous, rapid detection of double positive EspB- and β-lactamase-expressing bacteria, promoting advancements in POC clinical diagnosis.
Astrosense – a Printed Wearalbe Electrochemical Sensor for Monitoring Cortisol in Sweat during Human Spaceflight
Authors: Cordeiro Milton , Koehne Jessica E.
Published: August 2024

The In Space Manufacturing of sensors and electronics can directly addresses the logistic challenge for long-duration human spaceflight missions by reducing mission logistics mass, increase reliability, mitigate risk, while also offering a high degree of customization and tailorability. This manufacturing approach relies on additive manufacturing technologies, due to its versatility, low power consumption, automation, fast manufacturing time with low waste generation, and ability to print a variety of materials. To ensure the health and safety of crew members, developing human health portable diagnostic tools that can be manufactured during long duration missions is necessary to ensure that the crew members are monitored in real time so that countermeasures can be deployed as soon as possible. Here we report the development of Astrosense (Figure 1), a wearable wireless and fully printed platform that integrates several sensors, including, electrochemical sensor for the detection of cortisol in sweat, temperature, CO2 and humidity sensors, as well as, the required hardware required to control each individual sensor.Astrosense consists of two sections, a reusable, and a disposable section. The reusable section contains the CO2,temperature, humidity sensor, the potentiostat that controls the cortisol sensor and the printed antennas for data transmission. The cortisol sensor, sweat harvest component and printed batteries will be located on the disposable section of Astrosense, so that they can be easily replaced once the sensor is either saturated, degraded or when the batteries need to be replaced. The disposable section will interfase with the reusable section of Astrosense through several medical grade adhesives and pogo pins. This allows for the easy replacement of the cortisol sensor as well as mounting and dismounting of the device on the human skin.

Figure 1
Solutions to Overcome Competitive Displacement of Oligonucleotides from Nucleic Acid-Based Electrochemical Sensors in Biofluids
Authors: Clark Vincent , Arroyo Netz
Published: August 2024

Nucleic acid-based electrochemical sensors (NBEs) can support continuous and highly selective molecular monitoring in biological fluids, both in vitro and in vivo, via affinity-based interactions. Such interactions afford a sensing versatility that is not supported by strategies that depend on target-specific reactivity. Thus, NBEs have significantly expanded the scope of molecules that can be monitored continuously in biological systems. Although sufficiently robust for continuous, multihour sensing of small molecules, peptides, and proteins in biological fluids both in vitro and in vivo, NBEs decay over periods longer than 12 hours of continuous operation if unprotected. Previous work has sought to deeply understand the mechanisms underlaying NBE sensor decay in biofluids, as a framework to later develop solutions that eliminate such degradation pathways. Here I present a biofluid mimetic that can be leveraged to specifically study competitive displacement of oligonucleotides from NBEs, a critical degradation pathway, and varying solutions to circumvent this degradation pathway.
Ion Conduction Mechanism and Interfacial Stability in Fluorine Containing Lithium Argyrodite Electrolytes for Solid-State Lithium-Sulfur Batteries
Authors: Shreyas Varun , Gupta Saransh , Narayanan Badri
Published: August 2024

Solid-state lithium-sulfur batteries (SSLSBs) hold great potential as a safe and energy-dense storage technology for wide variety of applications. Among solid-state electrolytes, halogen-doped lithium argyrodites have become an attractive category. This is attributed to their notable features, including high lithium-ion conductivity (~10-3 S/cm), favorable elastic stiffness (~ 30 GPa), and low flammability, making them promising candidates for enhancing the performance of SSLSBs.Despite their potential, SSLSBs based on sulfide faces challenges due to a limited atomic-scale understanding of ion-conduction, charge transport, structural evolution, and interfacial reactions such as dendrite growth, electrolyte decomposition. Here we employ a combination of density functional theory calculations, and ab initio molecular dynamics simulations to address this challenge for fluorinated argyrodites. Specifically, using accurate materials modeling, we design fluorine-containing argyrodite electrolytes that simultaneously offer enhanced (a) Li-ion conduction facilitated by unique Li-disorder induced by fluorine and other halogen co-dopants, and (b) stability against Li-anode owing to formation of a stable solid-electrolyte interface containing conductive species (Li3P), alongside LiCl and LiF. We will discuss these results in the context of accelerating design of novel solid-state electrolytes for long-lived, stable, and high-energy density SSLSBs.
Investigation of Plasmon-Mediated Oxygen Evolution Reaction
Authors: Zhen Janet , Forbes Tucker , Lin Timothy , Tao Jinhui , Engelhard Mark H. , Qiu Jingjing
Published: August 2024

To achieve a carbon-neutral future, sustainable energy is needed through storing energy through its chemical bond. Water electrolysis, an exemplary form of electrocatalysis, presents an example of storing energy within chemical bonds of the high-energy hydrogen gas. Nevertheless, the anodic reaction involved in the oxygen evolution reaction (OER) poses limitations on the overall rate of the process. Plasmonic gold nanoparticles (Au NPs) have been added to enhance the charge transfer at the interface of the OER electrocatalysts and electrolyte under light illumination.1-3 However, the mechanistic understanding of how the Au NPs on the photo-assisted electrochemical process is still lacking. We applied a model system of plasmonic Au electrode with nickel (Ni) and cobalt (Co)-based OER electrocatalyst to investigate the plasmon-mediated OER process. The composite system has been characterized with XPS, AFM, (photo)electrochemical and spectroscopic characterizations. Our preliminary data shows that the electrodeposited plasmonic Au electrode is free of surfactant and the resonant light illumination could modulate the electrochemical properties of the Au electrode and the Ni- and Co-based electrocatalysts in the alkaline electrolytes.

Liu, G.; Li, P.; Zhao, G.; Wang, X.; Kong, J.; Liu, H.; Zhang, H.; Chang, K.; Meng, X.; Kako, T.; Ye, J. Promoting Active Species Generation by Plasmon-Induced Hot-Electron Excitation for Efficient Electrocatalytic Oxygen Evolution. Am. Chem. Soc.
2016, 138(29), 9128–9136.

Wang, M.; Wang, P.; Li, C.; Li, H.; Jin, Y. Boosting Electrocatalytic Oxygen Evolution Performance of Ultrathin Co/Ni-MOF Nanosheets via Plasmon-Induced Hot Carriers. ACS Appl. Mater. Interfaces
2018, 10(43), 37095–37102.

Zeng, X.; Choi, S. M.; Bai, Y.; Jang, M. J.; Yu, R.; Cho, H.-S.; Kim, C.-H.; Myung, N. V.; Yin, Y. Plasmon-Enhanced Oxygen Evolution Catalyzed by Fe2N-Embedded TiOxNy
ACS Appl. Energy Mater.
2020, 3(1), 146–151.
Averaged Cell Expansion As a Predictor of State of Health of Lithium-Ion Pouch Cell
Authors: Kajiura Yuichi , Scott Logan M , Zhang Dong
Published: August 2024

The rise of electric vehicles on the road and associated supply chain concerns draw researchers' attention to batteries' second life. For this purpose, non-destructive and economical methodologies for battery state of health (SoH) have been sought. Although it is known that LiB pouch cells expand as they degrade, how the expansion evolves over their lifecycle and how the location of measurement affects the discussion, are not well studied. Consequently, the method to accurately determine SoH from cell thickness is yet to be reported. This study uses digital image correlation to obtain cell expansion at every surface point and observe its non-uniformity. The evolution of the non-uniform expansion is observed during extended cycling until cells reach their end of life. We further find that the expansion averaged over the cell surface has a strong linear correlation with SoH, and develop a machine-learning-based method to estimate cell SoH accurately from the averaged expansion. Lastly, we verify that this methodology is effective when using the averaged expansion approximated only from several points of measurement, which can practically and economically be obtained by lining up displacement sensors, for example, at the battery repurposing factory.

Figure 1
Joint Time-Frequency Signal Analysis of Li-Ion Batteries
Authors: Allagui Anis , Miao Kepei , Wang Chunlei
Published: August 2024

Measurements acquired from batteries, such as voltage-time and capacity-time signals, offer valuable insights into their cyclability performance. While analyzing these signals in the time domain provides an understanding of global characteristics, scrutinizing local behavior is crucial for detecting issues like battery fading. In this context, we delve into the application of short-time Fourier transform for time-frequency deconstruction of galvanostatic charge/discharge signals, using lithium-sulfur batteries as an illustrative example. Spectrograms resulting from this analysis unveil the evolving frequency content of signals throughout the battery's lifespan, facilitating the identification of critical changes in the response and early detection of issues leading to fading and potential default. Simultaneously, the stability analysis of the dynamic response of red phosphorus and sulfide polyacrylonitrile (RP-SPAN) composite, a promising anode material for lithium batteries, can also be studied using Fourier transform analysis. Our study employs transfer function stability analysis, Kramers-Kronig integral relations, and differential capacity analysis to assess the cell's behavior in both frequency and time domains. Parameters such as stationarity, stability, linearity, dissipation, and degradation are scrutinized over extended charge/discharge cycles. Results reveal a highly nonlinear and time-variant system at low frequencies, aligning with the observed 0.21% average capacity loss per cycle. Our results indicate that short-time Fourier transform could provide insightful information for analyzing battery health.
Engineering a High Stable and Active RuO2 on Ti Sheet for Kolbe Electrolysis of Acetic Acid: An Investigation to Valorize the Pyroligneous Acid
Authors: Jin Yangxin , Jin Yangxin
Published: August 2024

The efficient utilization of renewable sources based on the simultaneous production of energy fuels and value-added chemicals is an essential to enable a biobased circular economy that benefits carbon neutrality. As an abundant by-product during the pyrolysis of biomass, pyroligneous acid is rich in acetic acid (CH3COOH) that is difficult to handle due to its highly acidic content. However, it is essential made up of renewable carbon that can be converted into valuable chemicals and fuels (e.g. methane, ethane, propane). Herein, we fabricate a highly stable and effective ruthenium oxide electrocatalyst (RuO2/TiOx) via using available titanium sheet as the substrate, to highly selectively transform AA to ethane by electrochemical conversion with ~82 (±5)% selectivity. The obtained results demonstrate that RuO2/TiOx exhibits an efficient electrochemical performance at low temperatures (5℃), and can convert AA at various pH, current density, and different concentrations. Moreover, we mimicked the complex chemical environment of the pyroligneous acid by adding diverse hydrocarbons (e.g., phenols, aldehydes) in acid solution to evaluate the stability of RuO2/TiOx. The electrolysis was also conducted in original pyroligneous acid solution, in which the RuO2/TiOx exhibits a considerable performance to convert AA to ethane. This work, based on the selective production of ethane from AA by a RuO2/TiOx electrode as an alternative to bulk metals as anodes for oxidative upgrading of carboxylic acids, making it promise to directly turn biomass residual into fuel thus improve the biomass utilization.
Getting Everyone Jazzed about Electrochemistry: How Education in Electrochemistry Jump-Starts Citizen Science
Authors: Dick Jeffrey E
Published: August 2024

As a science, electrochemistry (and methods therein) is one of the oldest methods of probing the world around us. Electrochemistry has witnessed tremendous growth in the past half-century. The science continues to be central to several areas of study, from materials science to biology to chemistry and beyond. Critical to the growth of electrochemistry as a field are robust pedagogical tools that introduce students to the joys of seeing the world through the goggles of an electrochemist. This talk will detail our group's strategy at developing pedagogical tools ranging from rather simple ways of building instrumentation to teaching our colleagues important historical insights. Electrochemistry must also be accessible to young students and senior citizens to cement its bright future as a foundational science, and we will discuss our activities to reach such groups to forge a foundation for citizen science.
Influence of Catalyst Surface Structure on the Electrochemical Hydrogenation of Cis,Cis-Muconic Acid
Authors: Prabhu Prathamesh Tushar , Patel Deep M. , Kling Samantha , Nguyen Huy , Roling Luke T. , Tessonnier Jean-Philippe
Published: August 2024

Adipic acid (AA) production from petroleum-based cyclohexane is one of the largest chemical processes in terms of annual volumetric turnover accounting for 3 million tons as of 2022. The current commercial approach to synthesize AA is through the oxidation of petroleum-derived cyclohexane using nitric acid. The release of N2O in stoichiometric amounts makes it one of the most significant greenhouse gas (GhG) emitting processes. The abundance of biomass in the Midwestern United States has driven significant research efforts to synthesize bio-derived and sustainable commodity products and lower the chemical industry’s carbon footprint.1
cis,cis-Muconic acid (ccMA), a biobased C6 diunsaturated diacid platform molecule can be transformed to commodity chemicals like caprolactam, adipic acid, and terephthalic acid, with AA being of particular interest for the synthesis of nylon 6,6.2

For the first time in literature, we demonstrate appreciable production of AA (conversion: 91%, selectivity: >95%) through electrochemical hydrogenation (ECH) of ccMA on PGM catalysts. Carbon-supported palladium (Pd/C) and platinum (Pt/C) selectively produced AA while bulk Pd and Pt yielded the monounsaturated trans-3-hexenedioic acid (t3HDA) intermediate and H2 under all tested conditions. Such an influence of surface structure on the electrochemistry of organics is not unprecedented. Koper et. al3 studied Pt single crystals for the electrochemical hydrogenation of acetone and showed how activity, selectivity, and extent of catalytic poisoning are highly sensitive to the Pt surface structure. Similarly, we used density functional calculations to elucidate the structure-sensitive nature of ccMA ECH and its intermediates by identifying thermodynamically preferred reaction pathways as a function of surface geometry (terrace vs steps). The energetics coupled with experimental observations suggest that the reduction of ccMA to t3HDA occurs through an outer sphere proton-coupled electron transfer mechanism, while the reduction of HDA to AA preferentially occurs on Pd and Pt (111), the most abundant facet in Pd/C and Pt/C. Our calculations also explain the exceptional performance of Pd/C compared to Pt/C by the weaker binding of Pd terrace sites compared to Pt. Overall, combining renewable electricity, in-situ hydrogen generation from water, and a biologically-produced intermediate enabled us to open a sustainable route for bio-adipic acid production. This allows us to further design and optimize the catalyst for the selective production of biobased AA.

References:

(1) Dell’Anna, M. N. et al. Green Chem.
23, 6456–6468 (2021).

(2) Matthiesen, J. E. et al. ACS Sustain. Chem. Eng. 4, 3575–3585 (2016).

(3) Bondue, C. J. et al. Nat Catal. 2, 243-250 (2019)

Figure 1
Stable High-Voltage Operation of Anionic Redox on P2-Type Na-Layered Cathode at Fast Discharge through Improved Kinetics
Authors: Ku Bonyoung , Ahn Jinho , Kim Jongsoon
Published: August 2024

Sluggish kinetics and structural instability from oxygen redox can result in suboptimal electrochemical performance for cathode materials. This leads to a considerably lower operating voltage during discharge, especially at high current densities, and compromises power capability. Undesirable phase reactions during charge/discharge further hinder the electrochemical performance of oxygen-redox-based P2-type Mn-based layered oxide cathodes. Our study demonstrates the successful stabilization of oxygen redox in these cathodes through the cooperative synergy of Cu-Co. Specifically, this synergy significantly enhances the discharge operation voltage and energy density during fast charging. For instance, the discharge voltage difference for P2-type Na0.67[Cu0.2Co0.2Mn0.6]O2 between 10 and 1000 mA g−
1 is approximately ~0.18 V, contrasting sharply with P2-type Na0.67[Cu0.2Mn0.8]O2, which exhibits differences of around ~0.36 V under the same conditions. Furthermore, after 100 cycles, the discharge capacity of P2-type Na0.67[Cu0.2Co0.2Mn0.6]O2 with oxygen redox remains at ~93% of the initial capacity. This is attributed to both a minimal volume change during charge/discharge (~0.6%) and the successful suppression of undesirable phase transitions in P2-OP4. These findings highlight the feasibility of utilizing oxygen-redox-based P2-type Na-layered oxide as an effective approach for achieving outstanding high-rate and high-voltage performance.
Electrospun Nano-Porous Cellulose Acetate Membrane Casted with Chitosan for Solid-State Sodium-Ion Batteries
Authors: Hassan Md. Mehadi , Lu Qingye
Published: August 2024

Emerging as a safe and economically viable alternative to lithium-ion batteries, the solid-state sodium ion battery (ss-SIB) has captured increasing attention as a transformative technology for realizing a decarbonized economy and ensuring a sustainable energy supply. Here we report a nanoarchitecture strategy of biodegradable, biocompatible, and naturally abundant cellulose derivative (cellulose acetate, CA) and chitosan (CH) biopolymer-based nano-porous electrospun composite electrolyte (ECE) for flexible and wearable ss-SIBs. A simple combination of electrospinning and solution casting was utilized to fabricate mechanically robust (13.76 MPa), thin-film (0.067 mm), highly flexible, and high room temperature Na-ion conductive (1.04 x 10-4 S.cm-2) ECE. Lower activation energy (Ea = 0.13 eV) indicates easy charge carrier diffusion ability of as prepared ECE. The electrochemical stability window (ESW = 3.45 V) of ECE is studied by the linear sweep voltammetry (LSV) with respect to stainless steel and sodium metal electrodes. Uniform galvanostatic Na plating and stripping at room temperature is observed over 900 hrs at 0.5 mA•cm-2 current density in symmetric (Na|ECE|Na) cell performance, this underscores impressive electrochemical stability and compatibility with sodium metal. Using Na3V2(PO4)3 (NVP) as cathode, ECE, and Na metal as anode in the full cell, specific discharge capacity of 83 mA×h×g-1 at room temperature was attained at 0.1 C rate, highlighting the practical applicability of the nanostructured electrospun composite electrolyte for flexible and wearable ss-SIBs.

Keywords

Cellulose acetate, chitosan, electrospun, solid-state sodium-ion battery, specific discharge capacity.
(Invited) 3D Integration of 2D Devices for Neuromorphic Computing
Authors: Das Saptarshi
Published: August 2024

In this presentation, I will delve into the exciting realm of monolithic 3D integration, where emerging 2D FETs take center stage, empowering advanced memory, and logic devices. Furthermore, I will also discuss our work on bio-inspired neuromorphic computing. Notably, our recent breakthroughs have culminated in the successful demonstration of wafer-scale 2-tier and 3-tier 3D integration, utilizing MoS2 and WSe2 FETs as the building blocks. These achievements have paved the way for multifunctional circuits that hold immense promise for the future of electronics. Delving deeper into our research, we have harnessed the potential of 2D materials to design solid-state devices with low power consumption mimicking auditory processing in barn owl, collision avoidance in locust, and probabilistic computing in dragonfly. By combining the power of 2D materials with bio-inspired principles, our work lays a solid foundation for the creation of highly compact and functionally diverse integrated circuits in the revolutionary third dimension. The implications of this technology are far-reaching and hold the potential to shape the future of electronics and computing.
(Invited) Novel Neuromorphic Computing Paradigms Enabled By Emerging Memory Devices
Authors: Jha Rashmi , Gogi Vamshi Kiran Kiran , Barve Siddharth
Published: August 2024

Implementation of Artificial Intelligence and Machine Learning algorithms on conventional Von Neumann computing architectures are crippled by the memory-wall bottleneck. To overcome these issues, novel computing architectures with high-bandwidth memories, in-memory computing, and near-memory computing capabilities are being developed. Almost all of these architectures will benefit from high-density on-chip non-volatile memories, offered by the emerging non-volatile memory devices. Additionally, emerging memory devices offer rich device physics that can be leveraged for the implementation of novel computing paradigms. This paper will talk about three such emerging memory technologies: Vertical-Thin Film Transistors-Resistive Random Access Memory (V-TFT-RRAMs), Gated-RRAMs, and Ferroelectric Field Effect transistors (FeFETs). A comparative studies of various conventional neuromorphic computing approaches that can be implemented using these devices will be discussed. Finally, materials and device requirements and pending challenges will be discussed by successful realization of the proposed computing approaches. Implementation of Artificial Intelligence and Machine Learning algorithms on conventional Von-Neumann computing architectures are crippled by the memory-wall bottleneck. To overcome these issues, novel computing architectures with high-bandwidth memories, in-memory computing, and near-memory computing capabilities are getting developed. Almost all of these architectures will benefit from high-density on-chip non-volatile memories, offered by the emerging non-volatile memory devices. Additionally, emerging memory devices offer a rich set of device physics that can be leveraged for the implementation of novel computing paradigms. This paper will talk about three such emerging memory technologies: Vertical-Thin Film Transistors-Resistive Random Access Memory (V-TFT-RRAMs), Gated-RRAMs, and Ferroelectric Field Effect Transistors (FeFETs). A comparative studies of various unconventional and brain-inspired neuromorphic computing approaches that can be implemented using these devices will be discussed. Finally, materials and device requirements and pending challenges will be discussed for these device technologies.
(Invited) Analog Computing with High Precision and Programmability Enabled by Memristors
Authors: Song Wenhao , Yang J. Joshua
Published: August 2024

While digital computing dominates the technological landscape, analog computing distinguishes itself with superior energy efficiency and high throughput. However, its historical limitation in precision and programmability has confined its application to specific and low-precision domains, notably in neural networks. The escalating challenge posed by the analog data deluge calls for versatile analog platforms. These platforms must not only exhibit exceptional efficiency but also boast reconfigurability and precision.

Recent breakthroughs in analog devices, such as memristors, have laid the groundwork for unparalleled analog computing capabilities. Leveraging the multifaceted role of memristors, we introduce memristive field-programmable analog arrays (FPAAs), mirroring the functionality of their digital counterparts, field-programmable digital arrays (FPGAs). To elevate precision, we delve into the origins of reading noise, successfully mitigating it and achieving an unparalleled 2048 conductance levels in individual memristors—equivalent to 11 bits per cell, setting a record precision among diverse memory types. Acknowledging the persistent demand for single or double precision in various applications, we propose and develop a circuit architecture and programming protocol. This innovation enables analog memories to attain arbitrarily high precision with minimal circuit overhead. Our experimental validation involves a memristor System-on-Chip fabricated in a standard foundry, demonstrating significantly improved precision and power efficiency compared to traditional digital systems.

The co-design approach presented empowers low-precision analog devices to perform high-precision computing within a programmable platform. This demonstration underscores the transformative potential of analog computing, transcending historical limitations and ushering in a new era of precision and efficiency.
Screening Conductive Mxenes for Polysulfide Adsorption in Li-S Batteries
Authors: Valurouthu Geetha , Gogotsi Yury , Harrison Kate , Wang Ruocun (John) , Kalra Vibha , Oh Il-Kwon
Published: August 2024

Lithium-sulfur batteries (LSBs) show promise as next-generation batteries due to their high charge density and natural abundance of sulfur. Nevertheless, their commercialization faces challenges due to the polysulfide shuttle effect and the insulating nature of sulfur and discharge products. MXenes have recently emerged as a solution by providing conducting pathways and polar sites to trap lithium polysulfides (LiPSs). While previous studies have explored the potential of MXenes in various passive components, a quantitative investigation of polysulfides adsorbed on MXenes, a crucial factor in enhancing LSB performance, remains lacking. In this study, we systematically investigate LiPSs adsorbed on seven MXenes: Ti2CT
x
, Ti3C2T
x
, Ti3CN
x
, Mo2TiC2T
x
, V2CT
x
, Nb2CT
x
, and Nb4C3T
x
. We explore the influence of soaking time, polysulfide concentration, and MXene composition on polysulfide adsorbed. Our spectroscopic findings reveal the formation of thiosulfate and polythionate species upon polysulfide adsorption for all MXene compositions. Furthermore, our study reveals the specific preferences of sulfur and lithium adsorbed on the MXene surface, dependent on MXene chemistry, adding a new level of understanding to the field. We expect our work can serve as a general guiding principle for the rational selection of MXenes for various passive components in the development of high-performance LSBs.
Homogenizing Interfacial Stress by Nanoporous Metal Current Collector to Enable Stable All-Solid-State Li Metal Battery
Authors: Feng Shijie , Yeerella Hemanth , Zhou Jianbin , Harpak Nimrod , Cai Shengqiang , Liu Ping
Published: August 2024

All-solid-state lithium-metal batteries are prone to shorting due to lithium penetration through the electrolyte layer. Li experiences creep during compression which creates stress in the electrolyte layer. Uneven deposition and stripping of Li further exaggerate the heterogeneity of stress distribution. To overcome this challenge, we design a current collector for Li metal. Its specific properties can homogenize interfacial stress distribution and prevent the solid electrolyte layer from developing additional defects that encourage penetration by Li metal during processes of fabrication and electrochemical cycling. Compared with a conventional current collector, our current collector effectively enhances the critical current density (1.7 vs. 0.5 mA/cm2) and extends cycle life (> 360 vs. 12 hours) for Li/Li symmetric cells. This development provides a chemistry-agnostic approach to improving the cycle life of solid-state Li batteries.
Balancing the Mechanical and Electrochemical Properties of Multifunctional Composite Electrolyte for Structural Batteries
Authors: Wang Zeru , Wang Ke
Published: August 2024

The pursuit of energy-efficient for electric vehicles and aircraft has driven the exploration of structural batteries. In the material-level design of structural batteries, electrode and electrolyte materials act as both load-bearing structures and energy storage elements. During these developments, carbon fibers with excellent mechanical and electrical conductive properties were used as electroactive materials and current collectors. However, most of these systems are combined with electrolytes without mechanical integrity (such as liquid or gel-type electrolytes), thus limiting the load-carrying performance of the battery. Currently the development of electrolytes for structural batteries remains challenging because the parameters enhancing electrochemical properties are often in contradiction with that for mechanical properties. In response to this challenge, the present study proposes a multifunctional composite electrolyte with balanced mechanical and electrochemical properties, which uses polyvinylidene fluoride (PVDF) as the matrix and metal-organic frameworks (MOF) modified glass fabric (MOF@GF) as the reinforcement. This study systematically investigates the following factors on mechanical and electrochemical properties of the composite electrolytes. Firstly, MOF with high specific surface areas and metal open sites onto the surface of glass fibers establishes a robust ion transporting network. With 20% MOF modified glass fiber and resin content 89%, the electrolyte exhibits high ion conductivity (1.74 × 10-3 S cm−1). In addition, by carefully controlling the resin content, a key parameter for fiber-reinforced composites, a delicate balance between mechanical strength and ionic conductivity can be achieved. Furthermore, interfaces were investigated, including glass fiber-MOF and MOF-PVDF interfaces, revealing the importance of effectively transfers stress and maintains structural integrity. Finally, these findings were combined to create a structural lithium metal battery that utilizes carbon fiber (CF) as the positive electrode and lithium metal as the anode. The resulting battery exhibits ultra-high tensile strength while maintaining a moderate capacity, ensuring normal operation under high voltage stress. This breakthrough discovery not only enhances the understanding of multifunctional composite electrolytes, but is also expected to promote further research and applications in the field of structural batteries. The promise of enhanced system electrolytes opens new avenues for lightweight design, space efficiency and expanded energy storage capabilities in electric vehicles and aircraft.

Figure
1
. SEM images of (a) bare glass fiber. (b) MOF grown in-situ on glass fiber. (c) Single fiberglass within polymer matrix. (d) Cross section of the composite polymer electrolyte membrane.

Figure 1
Flexible Aluminum-Air Batteries
Authors: Pimenov Albert
Published: August 2024

Wearable and flexible electronics have a wide range of applications. Making a flexible power source for them is essential. Aluminum-air batteries are attractive for powering portable, lightweight devices due to their inexpensive, light, and powerful energy source. In this project, the Al-air battery was made using activated carbon and aluminum electrodes, chloride-based electrolytes with ionic liquid additives. Various mixtures of 1-ethyl-3-methylimidazolium chloride, aluminum chloride, sodium hydroxide, and sodium chloride were studied. Fundamental properties of room-temperature ionic liquids, such as lower conductivity and density, improved the performance of aluminum-air batteries. Cell capacity, cyclic voltammetry behavior, and cell interfacial impedance with various electrolytes were optimized using the design of experiments. The battery's electrical power output and cell capacity were lower than those obtained using an activated carbon air cathode. The cell capacity over repeated electrochemical reactions was stable. The Al-air battery had regular cyclic voltammetry behavior. Aluminum hydroxide was not found on the anode electrode when an ionic liquid electrolyte was used. The interfacial cell impedance did not decrease after electrochemical reactions over a long time.
Grain Analysis of NCM Cathode Materials by ASTAR Technique and Its Effect on Battery Performance
Authors: Jung Yongjo , Hong Kijoo , Kim Juseong , Lee Sunhwa , Nam Sangcheol
Published: August 2024

Lithium-ion batteries (LIBs) are one of the most promising energy storage systems for portable electronic devices, electric vehicles, and renewable energy systems. Among the various cathode materials for LIBs, nickel cobalt manganese (NCM) oxide has attracted considerable attention due to its high specific capacity, good cycling stability, and appropriate cost for commercialization. However, Ni-rich NCM (Ni >80%) showed poor cyclability and huge gas evolution because of surface instability.

Single crystal NCM has been suggested as a solution to these issues due to its excellent properties. However, it is difficult to quantify the degree of single crystallinity because it is so far subjective. In this study, we employed ASTAR technique (transmission electron microscopy combined with electron backscatter diffraction) to investigate the microstructural features of NCM cathode materials. Our ASTAR analysis showed that NCM cathode materials consist of complex grain and grain boundary structures with varying orientations and sizes. By analyzing the grain size and its morphology, we were able to define the single crystallinity of NCM cathode materials, including the poly NCM and single crystal NCM particles.

Furthermore, we found that the grain size and its distribution significantly affects the battery performance and lifespan of NCM cathode materials. Specifically, the poly NCM particles exhibited a larger grain boundary and surface area compared to the single crystal NCM particles. The poly NCM particles also showed a faster DC-IR increase and a shorter lifespan than the single crystal NCM particles, indicating that the grain size has a critical influence on the battery performance and lifespan of NCM cathode materials.

Our results provide insights into the design and optimization of NCM cathode materials for next-generation LIBs. By controlling the grain size and its distribution of NCM cathode materials, it is possible to enhance the battery performance and lifespan. Therefore, our study highlights the importance of understanding the microstructural features of NCM cathode materials for developing high-performance and stable LIBs.
Design and Characterization of Porous Electrodes for Redox Flow Batteries
Authors: Murali Advaith , Patil Sairaj Chandrakant , Yang Bo , Narayan Sri , Prakash G. K. Surya G. K.
Published: August 2024

The commercialization of redox flow batteries as large-scale energy storage systems depends on lowering the capital and operating costs which depend on achieving maximum power density. Optimizing electrode design parameters and flow field-electrode combinations is critical to minimize losses and maximize active material utilization. Modeling the current drawn from an electrode offers a means to interpret electrode structure based on the electrolyte distribution driven by internal design. However, direct imaging methods (such as in-situ fluorescence microscopy and X-ray tomography) and numerical methods for current to potential prediction (3D Lattice Boltzmann modeling) are specific to individual electrode structures and possess limited predictable value to obtain an ideal electrode design. In this work, we present an electrode impedance spectroscopy (EIS)-based approach for determining electrode design parameters and devise a general method for determination of effective diffusion layer thickness. Using COMSOL modeling we verified the development of slug flow behavior in highly randomized porous electrode systems, indicating that the mass transport properties are dictated by inter-fiber distance. An analytical model to predict current as a function of applied overpotential is presented which allows us to vary structural parameters of the porous electrodes to study the influence of surface area, inter-fiber distances and diffusion layer thickness on the RFB performance. This model is a highly flexible tool applicable to any electrochemical system using a porous electrode and identifies critical variables affecting electrode design to characterize optimal electrode structure to minimize mass transport losses and optimize operational parameters.
Interfacial Stability and Dry Room Compatibility of Na3PS4 Solid-State Electrolyte Dry Films
Authors: Tang Wei , Xu Dapeng , Wu Junlin , Li Feng , Lee Dong Ju , Tao Andrea , Liu Ping , Chen Zheng
Published: August 2024

Sodium solid-state batteries (NaSSBs) employing nonflammable sulfide solid-state electrolytes (SSEs) are a promising solution for large-scale energy storage due to their safety, low cost, and high volumetric energy density. However, the state-of-the-art pellet type NaSSBs face challenges such as inadequate humidity stability and poor mechanical properties, resulting in nonnegligible ohmic losses, limited crucial current density, and low energy density. Reducing the thickness of the SSE layer and improving the anti-moisture stability is crucial to realize the scalable production and practical applications of NaSSBs. To address these challenges, a dry process was developed to fabricate Na3PS4 (NPS) solid electrolyte film with high retention of intrinsic ionic conductivity, and increased flexibility by incorporating only 0.2wt% of polytetrafluoroethylene (PTFE) binders. Notably, it is found that PTFE with hydrophobic groups improves moisture stability by reducing the available adsorption sites for H2O on the surface. After 24 hours exposure in a dry room condition (RH 0.1%), the NPS film exhibits more than 90% conductivity retention and stable cycling for up to 100 cycles, representing a significant step towards the scalable production and practical use of low-cost NaSSBs. Our findings may also guide the development of robust lithium-based sulfide electrolyte films, such as Li6PS5Cl.
Carbon Quantum Dots with Highly Efficient Bandgap Emission for Electroluminescent Light-Emitting Diodes
Authors: Fan Louzhen , Yuan Ting
Published: August 2024

Carbon quantum dots (CQDs) feature bright and tunable photoluminescence, solution processability, and low toxicity, showing great potential in optoelectronics. The multicolor fluorescent CQDs were first fabricated as active layers in our lab, and then the high-performance electroluminescent warm white light-emitting diodes (LEDs) were obtained with the synthesized bright red CQDs. More significantly, through designing the triangular structure of the carbon core, fluorescent CQDs first achieved the narrow-bandwidth (∼30 nm) electroluminescent LEDs with appreciable stability, high color purity, and high luminescence performance. These results lay the foundation for the development of next-generation high performance displays based on CQDs. Here, we will report the large-scale synthesis of CQDs with near-unity photoluminescence quantum yield and the synthesis of red (625 nm) phosphorescent carbon quantum dot organic frameworks (CDOFs) with a quantum yield of up to 42.3% and realization of high-efficiency red phosphorescent electroluminescent LEDs. The LEDs based on the CDOFs exhibited a red emission with a maximum luminance of 1818 cd m−2 and an EQE of 5.6%. This work explores the possibility of a new perspective for developing high-performance CQD-based electroluminescent LEDs.

References

Yuxin Shi, Louzhen Fan, et al., Red Phosphorescent Carbon Quantum Dot Organic Framework-Based Electroluminescent Light-Emitting Diodes Exceeding 5% External Quantum Efficiency, Am. Chem. Soc. 2021, 143, 45, 18941–18951

Ting Yuan, Louzhen Fan, et al., Carbon Quantum Dots with Near-Unity Quantum Yield Bandgap Emission for Electroluminescent Light-Emitting Diodes, Angew. Chem. Int. Ed. 2023, e202218568.

Fanglong Yuan，Louzhen Fan, et al., Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs, Nat. Commun., 2018, 9, 2249.

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Δ-MnO2 / Carbon Material Nanocomposites for Aqueous Metal-Ion Electrochemical Energy Storage Devices
Authors: Lin Jeng-Yu
Published: August 2024

In this study, we successfully synthesized δ-MnO2/reduced graphene oxide (rGO) and K-doped MnO₂/graphite nanofibers (GNF) nanocomposite cathode materials for Mg/Zn-ion electrochemical energy storage applications. The device based on the δ-MnO2/rGO nanocomposite cathode showed a high operating voltage of 2V. At a power density of 823 W kg−1, it delivered a maximum energy density of 29.8 Wh kg−1. The device displayed impressive discharge capacity and excellent cycling stability even at a low temperature of −20 °C. Additionally, the K-doped MnO₂/GNF electrode exhibited a high specific capacitance of 410.31 F g⁻¹ at a current density of 0.5 A g⁻¹, while also demonstrating superior cycle stability under high current density, retaining 57.0% of the charge/discharge efficiency at 4 A g⁻¹. Furthermore, the device based on the K-doped MnO₂/GNF electrode delivered a high specific capacitance of 32.51 F g⁻¹ at 0.5 A g⁻¹ and maintained 88.2% of the initial capacitance after 20000 cycles.
Electrospun Polyacrylonitrile (PAN) Derived One Dimensional Carbon Nanofibers for Na-Ion Batteries
Authors: Anshu Satvik , Priya Surbhi , Chandra Amreesh
Published: August 2024

The desire for high performance storage devices is driven by energy demand, security and sustainability. Metal oxide based nanomaterials have limitations of high cost, poor cycle life, low yeild and structural stability. In comparison, carbon materials exhibit porous structure, work well in a wide potential window, and are highly conductive. Hence, they show enhanced rate capability and cycle life. In this work, one dimensional (1D) carbon nanofibers are synthesized with the help of electrospun PAN nanofibers as precursors. These electrospun carbonaceous nanostructures can be employed as electrodes as well as substrates, leading to structural stability after cycling and increased electrode conductivity. The morphologies and structures of as-spun nanofibers were investigated in order to develop a fundamental understanding of the nucleation and growth mechanism of carbon nanofibers. These high surface area carbon nanofibers were used as anode material for sodium (Na)-ion batteries. The electrochemical performance was first optimized in a half cell configuration. These batteries can deliver a capacity of 300 mAh g-1 at 0.1 A g-1, with cycling stability of 82% for more than >500 cycles. Thus, these electrodes can become useful in batteries beyond lithium.
Nature-Derived Sulfur Carbons for Highly-Efficient Room Temperature Sodium-Sulfur Energy Storage
Authors: Senokos Evgeny
Published: August 2024

In recent years, a growing interest in “beyond-Li-ion“ batteries has caused a speedy development of alternative battery technologies based on other alkali metals. Room temperature sodium sulfur (RT Na-S) batteries are potential candidate for sustainable large-scale energy storage systems. They offer low cost, nontoxicity and natural abundance of both cathode and anode materials combined with high theoretical energy density. However, rapid capacity fading related to the irreversible shuttling of soluble polysulfides, poor reaction kinetics and low sulfur utilisation in the cathode materials significantly limit their practical application.

In this work, a microporous sulfur-carbon complex is produced from sustainable natural precursors in a one-pot synthesis via stepwise thermally-induced inverse vulcanisation and condensation. The material exhibits a unique structure, with sulfur chains covalently anchored to the conductive carbon matrix and physically confined in ultra-micropores. An increase in sulfur content in the sulfur-copolymer alters the morphology and chemical composition of the final sulfur-carbon material, enhancing the amount of long-chain sulfur. The combination of optimal microstructure, good electrical conductivity and high content of electrochemically active sulfur translates to an unprecedented ~99% utilisation of sulfur and the highest reported capacity for a room temperature Na-S cathode, along with high rate capability, coulombic efficiency and long-term stability. This study offers an innovative approach towards the understanding of the key chemico-physical properties of the sulfur-carbon composite materials for the development of high-performance cathodes in RT Na-S batteries with an atom-efficient utilisation of sulfur.
(Invited) Tailoring the Surface Chemistry and Assembling Structure of 2D Materials for Supercapacitors and Batteries
Authors: Sun Jinhua
Published: August 2024

Energy storage devices are important components in portable electronics, electric vehicles, and the electrical distribution grid. Batteries and supercapacitors have achieved great success as the spearhead of electrochemical energy storage devices, but need to be further developed in order to meet the ever-increasing energy demands, especially attaining higher power and energy density, and longer cycling life. Rational design of electrode materials plays a critical role in developing energy storage systems with higher performance. Starting from the classical 2D material - graphene to the other new 2D materials for example MXene, I will introduce some of our recent works about how to design and tune the surface chemistry of 2D materials and how to tailor the structure of 2D materials. Specifically, the interlayer structure and the self-assembled unique structure will be discussed, and the use of various advanced characterization techniques (in situ/operando) to understand the materials and their energy storage mechanisms will be covered in my talk as well. Most importantly, I will also introduce how can we strategically use 2D materials in different applications from battery, supercapacitors to sensors.