Article
Chemistry, Physical
Fu Yuan, Yu Lei, Huwei Wang, Xiaojing Li, Junyang Hu, Yaojie Wei, Rongyi Zhao, Baohua Li, Feiyu Kang, Dengyun Zhai
Summary: Modified graphite (MG) with enlarged graphitic space and unique porous microstructure exhibits outstanding potassium ion storage performance. The optimized MG anode shows high specific capacity and excellent cycling stability at high current densities.
Article
Chemistry, Physical
Austin G. Paul-Orecchio, Lucas Stockton, Jason A. Weeks, Andrei Dolocan, Yixian Wang, C. Buddie Mullins
Summary: This study investigates the synergistic combination of a Li-In alloy and a nitrate-derived protective layer in lithium metal batteries, which effectively prevents dendritic lithium plating and achieves stable cycling with high Coulombic efficiency.
ACS ENERGY LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Yangyang Liu, Haodong Shi, Zhong-Shuai Wu
Summary: This review summarizes the current advancements, challenges, and key strategies for achieving fast-charging lithium-ion batteries with graphite anodes, providing inspiration for further commercialization.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Multidisciplinary Sciences
Minsung Baek, Jinyoung Kim, Jaegyu Jin, Jang Wook Choi
Summary: The current lithium-ion battery technology requires extremely fast charging, such as achieving 80% of storage capacity within 15 minutes. A major obstacle in boosting charging rate is accelerating lithium ion transport through the solid-electrolyte interphase (SEI) layer, which negatively affects cycle life and battery safety. This study demonstrates the potential of non-electrochemical approaches in adjusting SEI composition to improve fast charging and long-term stability simultaneously.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Yanbing Mo, Gaopan Liu, Yue Yin, Mingming Tao, Jiawei Chen, Yu Peng, Yonggang Wang, Yong Yang, Congxiao Wang, Xiaoli Dong, Yongyao Xia
Summary: Popular fluorination methods can weaken Li+-solvent interaction, facilitating the desolvation process at low temperature. However, highly fluorinated compounds sacrifice salt dissociation and ionic conductivity. In this study, functional fluorinations with different degrees of fluorination are used to balance Li+-solvent interactions and ion movement. The moderately-fluorinated ethyl difluoroacetate (EDFA) exhibits a trade-off between weak affinity and sufficient ionic conductivity, enabling excellent fast-charging capability and low-temperature performance in lithium-ion batteries. The wide electrochemical potential window of EDFA-based electrolyte also allows high reversible capacity retention and discharge capacity under harsh conditions.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Meng Xia, Tianpeng Jiao, Gaopan Liu, Yuhui Chen, Jian Gao, Yong Cheng, Yong Yang, Mingsheng Wang, Jianming Zheng
Summary: The study focuses on a DME-based high-concentration electrolyte that enhances the stability and capacity retention of lithium metal batteries.
JOURNAL OF POWER SOURCES
(2022)
Article
Chemistry, Multidisciplinary
Junhua Zhou, Keni Ma, Xueyu Lian, Qitao Shi, Jiaqi Wang, Zhujie Chen, Lingli Guo, Yu Liu, Alicja Bachmatiuk, Jingyu Sun, Ruizhi Yang, Jin-Ho Choi, Mark H. Ruemmeli
Summary: Although graphite materials dominate the anode market of commercial lithium-ion batteries, they suffer from low capacity during fast charging and charge failure after many cycles. This study proposes an ultrathin artificial solid electrolyte interphase (SEI) modification strategy, which effectively addresses these issues and improves the stability and capacity retention of the graphite anode.
Article
Nanoscience & Nanotechnology
Pan Zhou, Yingchun Xia, Yuhao Wu, Wen -hui Hou, Yang Lu, Shuai Shuai Yan, Hang-yu Zhou, Weili Zhang, Kai Liu
Summary: This study proposes a novel urea-based molecule, 1,3-dimethyl-2-imidazolidinone (DMI), as an additive in carbonate-based electrolytes for lithium metal batteries. The addition of DMI enhances the solubility of LiNO3 and forms a stable solid electrolyte interphase, inhibiting electrolyte decomposition and dendrite growth. Experimental results show that the system can achieve stable operation and excellent capacity retention under high-rate and high-temperature conditions.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Zeyu Wu, Zhenhua Wang, Jing Zhang, Zhe Bai, Lina Zhao, Ruilong Li, Zhanfeng Yang, Yu Bai, Kening Sun
Summary: This study reveals the importance of hysteresis and mixed-phase state of graphite during deintercalation in the degradation of hybrid battery through in situ X-ray diffraction and in situ Raman analysis. By introducing an inorganic-rich solid electrolyte interface, the degradation of graphite was successfully mitigated and the reversible capacity of the hybrid anode was increased. This work contributes to the advancement of high-specific-energy lithium secondary batteries.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Le Anh Ma, Andrew J. Naylor, Leif Nyholm, Reza Younesi
Summary: This study investigates the impact of electrolyte chemistry on the dissolution of the solid electrolyte interphase (SEI) in sodium-ion batteries, using beta-alumina as a sodium-conductive membrane to prevent crosstalk. The research found that the solubility of SEI species in the electrolyte can reach up to 30% after a 50-hour pause, and saturation of the electrolyte with these SEI species can counteract aging due to SEI dissolution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Gaojing Yang, Simeng Zhang, Suting Weng, Xiaoyun Li, Xuefeng Wang, Zhaoxiang Wang, Liquan Chen
Summary: Research has enhanced the stability of SEI film on the graphite substrate for lithium deposition, improving the efficiency of lithium plating/stripping cycle. The FSI- anion was found to play a key role in the formation of SEI film and protecting the graphite substrate.
Editorial Material
Materials Science, Multidisciplinary
Sheng Shui Zhang
Summary: Fast charging of Li-ion cells faces challenges including accelerated capacity fade and inferior charging capability. Apart from the well-known issues of Li plating and voltage polarization, there are hidden factors such as failure of the solid electrolyte interphase, structural degradation of cathode materials, and high activation energies of Li+ ions in the electrolyte. Understanding these factors can help propose solutions to the fast-charging problems.
ENERGY & ENVIRONMENTAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Caiyun Chang, Sanlue Hu, Titi Li, Fanbin Zeng, Dun Wang, Songde Guo, Minwei Xu, Guojin Liang, Yongbing Tang, Hongfei Li, Cuiping Han, Hui-Ming Cheng
Summary: The construction of a stable solid-electrolyte interphase (SEI) on the zinc anode using a ternary aqueous electrolyte with DMTFA and DMF has been developed in this study. The gradient SEI layer formed provides excellent structural integrity, prevents direct contact between water and the zinc anode, and exhibits high compression modulus and electron-insulating feature. AZIBs with the gradient SEI demonstrate ultra-long cycling stability and high utilization rate under harsh conditions.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Jiahang Chen, Huichao Lu, Xuan Zhang, Yang Zhang, Jun Yang, Yanna Nuli, Yudai Huang, Jiulin Wang
Summary: This study proposed an in-situ electrochemical polymerization approach to create a nonflammable polyether electrolyte for lithium-sulfur batteries, which enhanced the kinetics of the electrode interface and achieved high energy density and stability.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Wurigumula Bao, Chengcheng Fang, Diyi Cheng, Yihui Zhang, Bingyu Lu, Darren H. S. Tan, Ryosuke Shimizu, Bhagath Sreenarayanan, Shuang Bai, Weikang Li, Minghao Zhang, Ying Shirley Meng
Summary: The continuous growth of the SEI is found to be the dominant factor for lithium inventory loss during cycling, with only a marginal increase in trapped Li-Si alloy. This study offers a quantitative approach to differentiate Li in the SEI from trapped Li in Li-Si alloy, providing unique insights into identifying critical bottlenecks for developing Si anodes.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Article
Chemistry, Physical
Eric J. McShane, Peter Benedek, Valerie A. Niemann, Sarah J. Blair, Gaurav A. Kamat, Adam C. Nielander, Thomas F. Jaramillo, Matteo Cargnello
Summary: This study demonstrates the utility of a Li0.5FePO4 (LFP) reference electrode in nonaqueous electrochemical systems, showing remarkable voltage stability and flexibility.
ACS ENERGY LETTERS
(2023)
Editorial Material
Chemistry, Physical
Jordi Cabana, Thomas Alaan, George W. Crabtree, Po-Wei Huang, Akash Jain, Megan Murphy, Jeanne N'Diaye, Kasinath Ojha, George Agbeworvi, Helen Bergstrom, Simon Gersib, Hassan Harb, Adrien Stejer, Genesis Quiles-Galarza, Oliver Rodriguez, Isabella Caruso, Josue M. Goncalves, Grace Y. Chen, Carlos A. Fernandez, Hanqing Pan, Kabian Ritter, Yingjie Yang, Haozhe Zhang, Ana Cristina Garcia-Alvarez, Stefan Ilic, Khagesh Kumar, Rachel Silcox, Yu Yao, Hakhyeon Song, Stoyan Stoyanov, Mohit Saraf, Celine H. Chen, S. M. Supundrika Subasinghe, Reginaldo Gomes, Shuangyan Lang, Eamonn Murphy, Arashdeep Singh Thind, Yu Zheng
ACS ENERGY LETTERS
(2023)
Editorial Material
Energy & Fuels
Eric J. McShane, Matteo Cargnello
Summary: The morphology of the solid-electrolyte interphase layer formed during N-2 reduction, mediated by Li, is revealed, providing insights into by-product formation mechanisms and NH3 selectivity improvement.
Article
Energy & Fuels
Zachary M. Konz, Brendan M. Wirtz, Ankit Verma, Tzu-Yang Huang, Helen K. Bergstrom, Matthew J. Crafton, David E. Brown, Eric J. McShane, Andrew M. Colclasure, Bryan D. McCloskey
Summary: By using simple and accessible cycling techniques, we were able to quantify irreversible lithium plating in over 200 cells and provide an empirical equation for predicting the onset state of charge. This research has significant implications for the development of rapid battery engineering.
Article
Nanoscience & Nanotechnology
Matthew J. Crafton, Tzu-Yang Huang, Yuan Yue, Raynald Giovine, Vincent C. Wu, Chaochao Dun, Jeffrey J. Urban, Raphaele J. Clement, Wei Tong, Bryan D. McCloskey
Summary: In this study, the extent of chemical reactions of a series of Mn2+/4+-based lithum-excess, cation-disordered rocksalt (DRX) oxyfluorides were quantified using a combination of differential electrochemical mass spectrometry (DEMS) and titration mass spectrometry. The results show that increasing the fluorine content can decrease redox reactions and suppress the generation of high-voltage O2 from the DRX surface.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
J. Wayne Mullinax, Charles W. Bauschlicher Jr, Kristian B. Knudsen, Pedro L. Arrechea, Rocco P. Viggiano, Donald A. Dornbusch, Justin B. Haskins, Baochau Nguyen, Bryan D. McCloskey, John W. Lawson
Summary: In this study, potential decomposition mechanisms of amide and urea solvents were investigated using density functional theory (DFT). Proton and hydrogen abstraction reactions were examined, and the preferred abstraction sites were identified. It was found that the N-H bond of secondary amides and the α-hydrogen atoms were more susceptible to proton abstraction. Additionally, hydrogen abstraction was more favorable at the N-alkyl substituents and α-hydrogen atoms, resulting in the formation of secondary and tertiary radicals. The presence of a coordinating Li+ ion affected the proton abstraction energies, but not the hydrogen abstraction energies. The study also examined the initial steps of a Baeyer-Villiger oxidation type mechanism and found that barriers for these steps were lower with HO2- as the oxidant compared to LiO2-. A comparison with previous experimental results indicated that no single reaction could be identified as the rate-limiting step for predicting the performance of these solvents in Li-O-2 batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Peter J. Weddle, Sangwook Kim, Bor-Rong Chen, Zonggen Yi, Paul Gasper, Andrew M. Colclasure, Kandler Smith, Kevin L. Gering, Tanvir R. Tanim, Eric J. Dufek
Summary: This paper presents a framework for identifying battery aging modes using fast charge/discharge voltage responses. The framework utilizes a physics-based battery model to generate synthetic high-rate responses, which are then used to train a deep-learning model for identifying real cell state-of-health. The performance of the framework is validated by comparing it with traditional methods.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Ankit Verma, Maxwell C. Schulze, Andrew Colclasure, Marco-Tulio Fonseca Rodrigues, Stephen E. Trask, Krzysztof Pupek, Christopher S. Johnson, Daniel P. Abraham
Summary: The impact of electrolyte fluorination on the calendar fade of blended silicon-graphite anodes is explored. Unfluorinated electrolyte shows higher cell resistance compared to fluorinated electrolyte, with slower rate of parasitic capacity loss for the LiBOB system. The results suggest that fluorinated electrolyte performs better in calendar life.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Instruments & Instrumentation
Sarah J. Blair, Adam C. Nielander, Kevin H. Stone, Melissa E. Kreider, Valerie A. Niemann, Peter Benedek, Eric J. McShane, Alessandro Gallo, Thomas F. Jaramillo
Summary: In situ techniques are crucial for studying the behavior of electrocatalysts. A versatile electrochemical cell has been designed for studying non-aqueous electrochemical systems, which is capable of observing the formation of relevant compounds and providing a functional method for understanding the mechanism of complex electrochemical systems.
JOURNAL OF SYNCHROTRON RADIATION
(2023)
Article
Chemistry, Physical
Zachary M. Konz, Peter J. Weddle, Paul Gasper, Bryan D. Mccloskey, Andrew M. Colclasure
Summary: Maintaining safe operating conditions is a key challenge for high-performance lithium-ion battery applications. By using pseudo-2D electrochemical modeling and data visualization methods, we can reveal the relationship between cell voltage and Li plating onset criteria, and find simple prevention strategies to reduce the risk of Li plating.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Eric J. Mcshane, Valerie A. Niemann, Peter Benedek, Xianbiao Fu, Adam C. Nielander, Ib Chorkendorff, Thomas F. Jaramillo, Matteo Cargnello
Summary: In this study, the quantitative analysis of lithium alkoxide solid-electrolyte interphase (SEI) species and its effect on the efficiency of lithium-mediated electrochemical ammonia synthesis were investigated. The results showed that the thickness of the lithium alkoxide SEI layer significantly influenced the Faradaic efficiency, with an optimal thickness of around 4 μm.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Sarah J. Blair, Mathieu Doucet, Valerie A. Niemann, Kevin H. Stone, Melissa E. Kreider, James F. Browning, Candice E. Halbert, Hanyu Wang, Peter Benedek, Eric J. McShane, Adam C. Nielander, Alessandro Gallo, Thomas F. Jaramillo
Summary: One way to improve the electrochemical synthesis of ammonia through the Li-mediated N-2 reduction reaction (Li-NRR) is by cycling the current between open-circuit conditions and periods of applied current density. In this study, the dynamics of the electrode-electrolyte interface under Li-NRR conditions during current cycling were investigated using in situ time-resolved neutron reflectometry and grazing-incidence synchrotron X-ray diffraction. The observations suggest that the benefits associated with returning to open-circuit conditions may be related to the concomitant loss of Li-containing species from a thin layer at the cathode surface into a porous SEI layer that becomes filled with electrolyte or dissolves.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Helen K. K. Bergstrom, Kara D. D. Fong, David M. M. Halat, Carl A. A. Karouta, Hasan C. C. Celik, Jeffrey A. A. Reimer, Bryan D. D. McCloskey
Summary: Polyelectrolyte solutions (PESs) have been proposed as high conductivity, high lithium transference number (t(+)) electrolytes. However, increasing the anion charge decreases t(+) due to competing effects. In this study, ion mobilities in a model non-aqueous PESs were directly measured using electrophoretic Nuclear Magnetic Resonance Spectroscopy (eNMR). It was found that below the entanglement limit, both conductivity and t(+) decrease with increasing degree of polymerization. Additionally, negative transference numbers were observed for polyanions with 10 or more repeat units, indicating ion clustering. Understanding ion correlations is important for designing concentrated electrolytes for improved battery performance.