Article
Materials Science, Multidisciplinary
Shaojie Chen, Xiangchen Hu, Lu Nie, Yi Yu, Wei Liu
Summary: Solid-state lithium metal batteries (SSLMBs) have potential for high safety and energy density, but the growth of lithium dendrite in solid electrolytes limits their practical applications. This study develops a simple heat treatment method to revive and recycle garnet oxide electrolytes with Li dendrite penetration. The recovered garnet electrolyte shows higher relative density, enhanced ionic conductivity, and improved critical current density compared to the pristine one. Thermal healing is attributed to the reaction products between dendritic Li metal and air, contributing to further densification of garnet electrolytes during heat treatment.
SCIENCE CHINA-MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Pengbo Zhai, Lixuan Liu, Yi Wei, Jinghan Zuo, Zhilin Yang, Qian Chen, Feifei Zhao, Xiaokun Zhang, Yongji Gong
Summary: Utilizing liquid gallium-indium (GaIn) nanoparticles with structural self-healing properties to guide uniform metallic lithium nucleation and deposition effectively addresses the issue of Li dendrite growth during charge/discharge processes. The self-healing design of nucleation seeds provides important insights for achieving high-performance lithium metal anodes.
Article
Chemistry, Physical
Yuxiao Zhang, Yunfan Li, Weijia Shen, Ke Li, Yixin Lin
Summary: A phase-field model with atom diffusion and heat transfer modules is developed to investigate the role of atom diffusion in dendrite growth and thermally induced dendrite self-healing. The results show that atom diffusion can induce surface self-healing and bulk self-healing, optimizing the dendritic profile. The model precisely predicts the threshold temperature for thermal self-healing of dendrites, consistent with experimental observations.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Caiyun Chang, Yuan Yao, Rongrong Li, Zi Hao Guo, Longwei Li, Chongxiang Pan, Weiguo Hu, Xiong Pu
Summary: In this study, a self-healing and single-ion conductive artificial SEI layer was developed to stabilize Li metal batteries. By optimizing the polymeric SS-ASEI layer, extremely stable cycling performance and rate capability were achieved.
Review
Chemistry, Multidisciplinary
Xiao-Ru Chen, Bo-Chen Zhao, Chong Yan, Qiang Zhang
Summary: Lithium metal as a promising alternative anode material for high-energy-density batteries is crucial in the new era of advanced energy storage. Understanding the deposition mechanism from nucleation to early growth is essential for improving battery performance and dendrite-free deposition behavior. Various models have been proposed to enhance the insight into the lithium deposition process, opening up new possibilities for practical lithium metal batteries.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
Linhai Pan, Haiyong He, Hualong He
Summary: Constructing a fast cation conductor layer on a commercial separator to form a vermiculite composite separator (VCS) can improve the electrochemical performance and thermal stability of lithium metal batteries, enhancing the Coulombic efficiency and reducing voltage polarization.
MATERIALS TODAY ENERGY
(2022)
Article
Chemistry, Physical
Wenhao Ren, Chenfeng Ding, Xuewei Fu, Yun Huang
Summary: Lithium metal batteries (LMBs) are gaining attention for their high energy density, but safety concerns and performance degradation have hindered their practical use. Gel polymer electrolytes (GPEs) are seen as a promising alternative to liquid electrolytes, with advancements in design and fabrication enabling the development of safe and durable LMBs. This review highlights the progress in GPEs with specific functionalities and outlines future directions and challenges for large-scale production and application in new energy storage systems.
ENERGY STORAGE MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Min Cao, Xianli Huang, Datuan Li, Xingxu Gao, Lei Sheng, Xingyu Yu, Xin Xie, Lu Wang, Tao Wang, Jianping He
Summary: To address the issues of volume expansion and lithium dendrite growth in lithium metal anodes, researchers have developed a CuO-loaded composite anode with a 3D polyethersulfone nanofiber frame, which effectively mitigates volume expansion. The reaction between lithium and CuO in the composite nanofiber, as well as Cu2O in the substrate, forms Li2O, strengthening the solid electrolyte interface (SEI) layer and ensuring uniform lithium deposition. The combination of heat treatment and electrospinning resolves the adhesion problem between the fiber film and the substrate. This study provides a low-cost and highly effective strategy for stabilizing lithium metal anodes.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Qingyuan Dong, Bo Hong, XinJing Huang, Maohui Bai, Yanqing Lai
Summary: The growth of lithium dendrites on graphite negative electrodes during high charging rates can be suppressed by using expansion graphite as inducing sites, allowing for stable plating and stripping of lithium metal.
ELECTROCHIMICA ACTA
(2022)
Review
Engineering, Chemical
Jia-Xin Guo, Wen-Bo Tang, Xiaosong Xiong, He Liu, Tao Wang, Yuping Wu, Xin-Bing Cheng
Summary: With the increasing demand for high energy-density rechargeable batteries, lithium metal is considered an ideal candidate for next-generation battery systems due to its ultrahigh specific capacity and low electrode potential. However, the practical applications of lithium metal batteries are severely hindered by limited Coulombic efficiency and safety risks caused by the growth of lithium dendrites and poor interface stability. This paper provides an overview of the recent developments of localized high-concentration electrolytes in lithium metal batteries, analyzing their solvation structures, physicochemical properties, and discussing their potential to address these challenges and enable practical applications.
FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Junyu Jiao, Genming Lai, Liang Zhao, Jiaze Lu, Qidong Li, Xianqi Xu, Yao Jiang, Yan-Bing He, Chuying Ouyang, Feng Pan, Hong Li, Jiaxin Zheng
Summary: Li is an ideal anode material for advanced batteries, but dendrite growth limits its commercial application. By using machine learning to construct a Li potential model, research shows that self-healing mechanisms can effectively promote dendrite-free Li formation.
Article
Chemistry, Physical
Chaobo Zhang, Zefang Li, Yi Sun, Jie Gao, Yanan Zhou, Zhanbin Qin, Ran Tian, Yun Gao
Summary: With the rapid development of technology, improving the utilization and conversion rate of sustainable energy has become crucial for ecological and sustainable development. However, the limited capacity and poor electrochemical property of current electrode materials hinder this progress. In this study, a lithium metal composite anode was developed through an excessive alloying process, effectively solving the issues of dendrite formation and poor electrochemical stability. The results showed that the lithium metal deposition on silver and silicon electrodes significantly enhanced coulombic efficiency and electrochemical stability, with the silver-lithium composite electrodes exhibiting twice the cycling capability of bare Cu electrodes. This new anode structure and excessive alloying process provide a promising approach for extending the application of commercial anodes.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Kang Wang, Weijie Wang, Jianlin Deng, Xiaoping Jiang, Guanchen Xu, Hongyu Gong, Na Zhang, Dongwei Li
Summary: The article introduces a stable 3D host made of highly lithiophilic ZnO nanosheets array decorated Ni foam (ZnO-NF) fabricated by thermal infusion method to inhibit dendrite growth in lithium metal anodes and improve the uniformity of Li stripping/plating behavior.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Engineering, Environmental
Tiansheng Mu, Hongfu Lu, Yang Ren, Xin Wan, Xing Xu, Siping Tan, Yulin Ma, Geping Yin
Summary: An artificial protective layer with interface defects is proposed to improve the cycling stability and rate performance of lithium metal anodes. The study focuses on titanium oxide (TiO2) and demonstrates that the interfacial oxygen-deficient TiO2 coating (H-TiO2) promotes lithium ion diffusion kinetics and prevents lithium dendrite formation. The H-TiO2 protective layer enables lithium metal anodes to have ultra-long cycling stability and improves the performance of full cells paired with LiFePO4 cathode.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Hee Jae Kim, Nurzhan Umirov, Jae-Sang Park, Jae-Hong Lim, Jiefang Zhu, Sung-Soo Kim, Seung-Taek Myung
Summary: In this study, the addition of phosphorous pentoxide (P2O5) to carbonate-based electrolytes was found to effectively suppress the dendritic growth on the surface of a lithium-metal anode, leading to improved lifespan and coulombic efficiency. The reduction mechanism of the P2O5-induced solid-electrolyte interphase (SEI) formation on Li metal was also elucidated, providing insights into the inhibitory effect on dendritic growth.
ENERGY STORAGE MATERIALS
(2022)
Article
Multidisciplinary Sciences
Venkatasubramanian Viswanathan, Alan H. Epstein, Yet-Ming Chiang, Esther Takeuchi, Marty Bradley, John Langford, Michael Winter
Summary: This Perspective explores the requirements and potential chemistries for battery-powered aircraft. The differences between flight and terrestrial needs are highlighted, with the major constraint for aviation being safe and usable specific energy.
Correction
Multidisciplinary Sciences
Venkatasubramanian Viswanathan, Alan H. Epstein, Yet-Ming Chiang, Esther Takeuchi, Marty Bradley, John Langford, Michael Winter
Article
Physics, Multidisciplinary
Pin-Wen Guan, Ying Sun, Russell J. Hemley, Hanyu Liu, Yanming Ma, Venkatasubramanian Viswanathan
Summary: Researchers evaluated the feasibility of synthesizing ternary Li-Mg superhydrides using the pressure-potential method and found that appropriate electrode potentials can stabilize Li2MgH16 and Li4MgH24 at modest pressures. Three structural forms of Li2MgH16 were observed below 300 GPa, with the highest pressure phase exhibiting superconductivity.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Physical
Nikifar Lazouski, Katherine J. Steinberg, Michal L. Gala, Dilip Krishnamurthy, Venkatasubramanian Viswanathan, Karthish Manthiram
Summary: This study investigates the influence of proton donor selection and concentration on ammonia production in lithium-mediated electrochemical nitrogen reduction reaction (LM-NRR). The research finds that alcohols can promote nitrogen reduction, with n-butanol exhibiting the highest ammonia Faradaic efficiency. Additionally, slight changes in proton donor structure significantly affect ammonia yield, and there is a thresholding behavior regarding the selectivity of ammonia depending on proton donor concentration.
Article
Chemistry, Physical
Victor Venturi, Venkatasubramanian Viswanathan
Summary: This study investigates the initial step of void formation in lithium metal batteries and suggests that faceting control during electrodeposition could be a key pathway toward preventing voids.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Venkatesh Krishnamurthy, Venkatasubramanian Viswanathan
Summary: Li-CFx batteries have the potential to electrify aviation due to their high specific energy. However, the rechargeability of these batteries is hindered by the formation of LiF. This study proposes three mechanisms to explain the transformation of lithium-intercalated CFx into LiF and graphite. By calculating the energetics, the feasibility of these mechanisms is estimated. This work could lead to targeted synthesis strategies for high specific energy rechargeable Li-CFx batteries and has broad applications in investigating phase transformations in two-dimensional heterostructures and layered materials.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Lydia Maria Tsiverioti, Lance Kavalsky, Venkatasubramanian Viswanathan
Summary: The electrochemical synthesis of hydrazine is an exciting avenue in sustainable production. This study explores the optimization of catalysts for hydrazine synthesis through the 4e(-) electrochemical nitrogen reduction reaction (NRR). The research uses first-principles calculations and uncertainty quantification to analyze various catalyst surfaces, finding that catalysts with weak binding for NH3 are more favorable for hydrazine synthesis. Additionally, single-atom alloys exhibit the same scaling relations as monometallic surfaces. The study also quantifies the uncertainty of branching points within 4e(-) NRR and highlights the challenge of overcoming the hydrogen evolution reaction (HER) for weakly binding catalysts and the dominance of 6e(-) NRR for strongly binding catalysts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Samuel M. Dull, Olga Vinogradova, Shicheng Xu, David M. Koshy, Per Erik Vullum, Jan Torgersen, Sebastian Kirsch, Venkatasubramanian Viswanathan, Thomas F. Jaramillo, Fritz B. Prinz
Summary: Better oxygen reduction catalysts are needed to improve the efficiency of proton exchange membrane fuel cells. This study prepared high-activity Pt-Zn alloy catalysts using two different synthetic approaches, and evaluated their activity. One approach introduced Zn to Pt nanoparticles via atomic layer deposition, resulting in a 30% increase in the activity per Pt mass. Density functional theory calculations were used to understand the origin of this enhancement and guide the preparation of an alloy with higher Zn content.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Yumin Zhang, Imanuel Bier, Venkatasubramanian Viswanathan
Summary: Ionic conductivity in liquid electrolytes can be predicted using a chemical physics formalism and classical molecular dynamics simulations. This approach allows for quantitative and qualitative agreements with conductivity measurements, providing a basis for high-throughput electrolyte discovery.
ACS ENERGY LETTERS
(2022)
Article
Nanoscience & Nanotechnology
Shang Zhu, Zijian Hong, Zeeshan Ahmad, Venkatasubramanian Viswanathan
Summary: With a phase-field model, we computationally characterize the morphological evolution dynamics during the plating and stripping steps at the lithium-metal-electrolyte interface. This recrystallization phenomenon mitigates the overall reaction rate heterogeneity and provides a potential approach to improving the morphological stability. Furthermore, we systematically investigate the correlation between the recrystallization phenomenon and lithium-ion activity and draw a simplified phase diagram for the overpotential-dependent recrystallization.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Multidisciplinary Sciences
Alexander Bills, Shashank Sripad, Leif Fredericks, Matthew Guttenberg, Devin Charles, Evan Frank, Venkatasubramanian Viswanathan
Summary: Electric vertical takeoff and landing aircraft have a unique duty cycle with high discharge currents during takeoff and landing, and moderate power requirements in between. A dataset of battery duty profiles was generated for such aircraft, consisting of 22 cells with a total of 21,392 charge and discharge cycles. This dataset is valuable for training machine learning models, fitting battery performance models, and various other applications.
Article
Computer Science, Artificial Intelligence
Varun Shankar, Vedant Puri, Ramesh Balakrishnan, Romit Maulik, Venkatasubramanian Viswanathan
Summary: Data-driven turbulence modeling is gaining attention with advancements in the data sciences. By combining known physics with machine learning, we present an approach using differentiable physics paradigm to develop closure models for Burgers' turbulence. Our study focuses on the one-dimensional Burgers system as a test case for modeling unresolved terms in advection-dominated turbulence problems. Through training models with various physical assumptions and evaluating their performance across different system parameters, we demonstrate that models constrained with inductive biases and partial differential equations outperform existing baselines in terms of efficiency, accuracy, and generalizability. Adding physics information also enhances interpretability and holds potential for the future of closure modeling.
MACHINE LEARNING-SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Physical
Alexander Bills, Leif Fredericks, Valentin Sulzer, Venkatasubramanian Viswanathan
Summary: This study uses a fast electrochemical model and high-throughput computing to analyze the degradation modes of an EVTOL aircraft battery dataset. The research identifies the causes of battery degradation and finds that depth of discharge, temperature, and charging current have significant impacts. A protocol for early identification of active degradation mechanisms is proposed.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Shang Zhu, Bichlien H. Nguyen, Yingce Xia, Kali Frost, Shufang Xie, Venkatasubramanian Viswanathan, Jake A. Smith
Summary: Rapid prediction of environmental chemistry properties is essential for the green and sustainable development of the chemical industry and drug discovery. Graph machine learning, which learns representations directly from molecular graphs, shows great potential in predicting these properties with high accuracy and outperforming conventional feature-based models. This study leveraged graph neural networks to accurately predict the environmental chemistry properties of molecules and compared their performance to commonly used methods. The results demonstrated the power of graph machine learning in representation learning for environmental chemistry and provided guidance for model selection based on data efficiency and feature requirements.
Article
Chemistry, Physical
Rituja B. Patil, Manjodh Kaur, Stephen D. House, Lance Kavalsky, Keda Hu, Shirley Zhong, Dilip Krishnamurthy, Venkatasubramanian Viswanathan, Judith Yang, Yushan Yan, Judith Lattimer, James R. Mckone
Summary: Coupling water electrolysis and fuel cell energy conversion is an attractive strategy for long-duration energy storage. This study reports the synthesis of Ni-Mo catalyst composites supported on oxidized Vulcan carbon and demonstrates their ability to catalyze reversible hydrogen evolution and oxidation.