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Artificial intelligence for the understanding of electrolyte chemistry and electrode interface in lithium battery

National Science Open 2024年第2期3卷 74-97页

作者： Yawei Chen Yue Liu Zixu He Liang Xu Peiping Yu Qintao Sun Wanxia Li Yulin Jie ruiguo cao Tao Cheng Shuhong Jiao Hefei National Laboratory for Physical Science at Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China

Recognizing the critical role of electrolyte chemistry and electrode interfaces in the performance and safety of lithium batteries,along with the urgent need for more sophisticated methods of analysis,this comprehensive review underscores the promise of machine learning(ML)models in this research field.It explores the application of these innovative methods to studying battery interfaces,particularly focusing on lithium metal anodes.Amid the limitations of traditional experimental techniques,the review supports a hybrid approach that couples experimental and simulation methods,enabling granular insights into the formation process and characteristics of battery interfaces at the molecular level and harnessing AI to extract patterns from voluminous data sets.It showcases the utility of such techniques in electrolyte design and battery life prediction and introduces a novel perspective on battery interface mechanisms.The review concludes by asserting the potential of artificial intelligence(AI)or ML models as invaluable tools in the future of battery research and highlights the importance of fostering confidence in these technologies within the scientific community.

关键词： lithium batteries battery interfaces artificial intelligence machine learning electrolyte chemistry

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Tuning electrochemical transformation process of zeolitic imidazolate framework for efficient water oxidation activity

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Journal of Energy Chemistry 2022年第2期31卷 505-513页

作者： Zhanwu Lei Xu Jin Jianming Li Yang Liu Jian Liu Shuhong Jiao ruiguo cao Hefei National Laboratory for Physical Science at Microscale Department of Materials Science and EngineeringUniversity of Science and Technology of Chin1Hefei 230026AnhuiChina b Research Center of New Energy Research Institute of Petroleum Exploration and Development(RIPED)PetroChin1Beijing 100083China School of Engineering Faculty of Applied ScienceUniversity of British Columbi1Kelown1BC V1V1V7Canada

Metal-organic frameworks(MOFs)have been widely studied as efficient electrocatalysts for water oxidation due to their tunable structure and easy preparation.However,the rational design of MOFs-based electrocatalysts and fundamental understanding of their structural evolution during oxygen evolution reaction(OER)remain critical challenges.Here,we report a facile approach to tune the structural transformation process of the Co-based zeolitic imidazolate framework(ZIF)during the OER process by using water molecules as a vacancy promoter.The modified ZIF catalyst accelerates the structural transformation from MOF precursor to electrochemical active species and simultaneously enhances the vacancy density during the electrochemical activation process.The optimized electrocatalyst exhibits an extremely low overpotential 175 mV to deliver 10 mA cm^(-2) and superior durability(100 h)at 100 mA cm^(-2).The comprehensive characterization results reveal the structural transformation from the initial tetrahedral Co sites to cobalt oxyhydroxide(CoOOH)and the formation process of oxygen vacancies(CoOOH-Vo)at a high anodic potential.These findings represent a promising way to achieve highly active MOF-based electrocatalysts for water oxidation.

关键词： Metal-organic framework Structural transformation Electrocatalyst Water splitting

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Regulating surface chemistry of separator with LiF for advanced Li-S batteries

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Frontiers in Energy 2022年第4期16卷 601-606页

作者： Shuai WANG Fanyang HUANG Shuhong JIAO Yulin JIE Yawei CHEN Shiyang WANG ruiguo cao Hefei National Laboratory for Physical Science at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Lithium-sulfur(Li-S)batteries have attracted intensive attention owing to their ultrahigh theoretical energy density.Nevertheless,the practical application of Li-S batteries is prevented by uncontrollable shuttle effect and retarded reaction kinetics.To address the above issues,lithium fluoride(LiF)was employed to regulate the surface chemistry of routine separator.The functional separator demonstrates a great ability to suppress active S loss and protect lithium anode.This work provides a facile strategy for the development of advanced Li-S batteries.

关键词： Li-S batteries LiF functional separator

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Crossover effects of transition metal ions in high-voltage lithium metal batteries

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Nano Research 2023年第6期16卷 8417-8424页

作者： Wanxia Li Yulin Jie Yunhua Chen Ming Yang Yawei Chen Xinpeng Li Youzhang Guo Xianhui Meng ruiguo cao Shuhong Jiao Hefei National Laboratory for Physical Science at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China NIO Incorporation Shanghai 201800China Science and Technology on Power Sources Laboratory Tianjin Institute of Power SourcesTianjin 300384China

Enhancing the cut-off voltage of high-nickel layered oxide cathodes is an efficient way to obtain higher energy density of lithiummetal batteries(LMBs).However,the phase transition of the cathode materials and the uncontrolled decomposition of the electrolytes at high voltage can lead to irreversible dissolution of transition metal ions,which might cause the crossover effects on the lithium metal anodes.Nonetheless,the mechanism and electrolyte dependence of the crossover effects for Li metal anodes are still unclear.Herein,we investigate the crossover effects between LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)and Li-metal anode in two electrolyte systems.For ether-based electrolyte,its poor oxidation stability results in massive dissolution of transition metal ions,leading to dendrite growth on anode and rapid cells failure.Conversely,ester-based electrolyte exhibits good electrochemical performances at 4.5 V with little crossover effect.This study provides an idea for electrolyte systems selection for high-voltage LMBs,and verifies that the crossover effect should not be neglected in LMBs.

关键词： crossover effects lithium-metal batteries high-nickel layered cathodes electrolyte systems dependence transition metals dissolution

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Stable cycling of practical high-voltage LiCoO_(2)pouch cell via electrolyte modification

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Nano Research 2023年第3期16卷 3864-3871页

作者： Chao Tang Yawei Chen Zhengfeng Zhang Wenqiang Li Junhua Jian Yulin Jie Fanyang Huang Yehu Han Wanxia Li Fuping Ai ruiguo cao Pengfei Yan Yuhao Lu Shuhong Jiao Hefei National Laboratory for Physical Science at Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Ningde Amperex Technology limited(ATL) Ningde 352100China Beijing Key Laboratory of Microstructure and Properties of Solids Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China

Nitriles as efficient electrolyte additives are widely used in high-voltage lithium-ion batteries.However,their working mechanisms are still mysterious,especially in practical high-voltage LiCoO_(2)pouch lithium-ion batteries.Herein,we adopt a tridentate ligandcontaining 1,3,6-hexanetricarbonitrile(HTCN)as an effective electrolyte additive to shed light on the mechanism of stabilizing high-voltage LiCoO_(2)cathode(4.5 V)through nitriles.The LiCoO_(2)/graphite pouch cells with the HTCN additive electrolyte possess superior cycling performance,90%retention of the initial capacity after 800 cycles at 25℃,and 72%retention after 500 cycles at 45℃,which is feasible for practical application.Such an excellent cycling performance can be attributed to the stable interface:The HTCN molecules with strong electron-donating ability participate in the construction of cathode-electrolyte interphase(CEI)through coordinating with Co ions,which suppresses the decomposition of electrolyte and improves the structural stability of LiCoO_(2)during cycling.In summary,the work recognizes a coordinating-based interphase-forming mechanism as an effective strategy to optimize the performance of high voltage LiCoO_(2)cathode with appropriate electrolyte additives for practical pouch batteries.

关键词： LiCoO_(2) high voltage nitrile additive interface adsorption pouch cell electrolyte modification

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Molybdenum-doped ordered L1_(0)-PdZn nanosheets for enhanced oxygen reduction electrocatalysis

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SusMat 2022年第3期2卷 347-356页

作者： Jiashun Liang Yu Xia Xuan Liu Fanyang Huang Jinjia Liu Shenzhou Li Tanyuan Wang Shuhong Jiao ruiguo cao Jiantao Han Hsing-Lin Wang Qing Li State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhenChina School of Physics and Astronomy University of BirminghamBirminghamUK Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS) Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Institute of Coal Chemistry Chinese Academy of SciencesTaiyuanChina National Energy Center for Coal to Clean Fuels Synfuels China Co.LtdBeijingChina

Ultrathin Pd-based two-dimensional(2D)nanosheets(NSs)with tunable physicochemical properties have emerged as promising candidate for oxygen reduction reaction(ORR).Unfortunately,structurally ordered Pd-based NSs can be hardly prepared as high temperature annealing(>600℃)is necessary for disorder to order phase transition,making it a considerable challenge for morphology control.Herein,a new class of ultrathin structurally ordered Mo-doped L1_(0)-PdZn NSs with curved geometry and abundant defects/lattice distortions is reported as an efficient oxygen reduction electrocatalyst in alkaline solution.It is found that Mo(CO)_(6) serves as reducing agent and Mo source to generate the unique ordered 2D morphology,which leads to the significantly modified electronic structure.The developed L1_(0)-Mo-PdZn NSs exhibit excellent ORR mass activity of 2.6 A mg_(Pd)^(−1) at 0.9 V versus reversible hydrogen electrode,31.5 and 17.6 times higher than those of Pd/C and Pt/C,respectively,outperforming most of the reported Pdbased ORR electrocatalsyts.Impressively,L1_(0)-Mo-PdZn NSs is extremely stable for ORR,with only 2.3% activity loss after 10000 potential cycles.Density functional theory study suggests that ordered L1_(0) structure and Mo doping can raise the vacancy formation energy of Pd atom and thus promote the ORR stability.

关键词： electrocatalysis fuel cell nanosheeets oxygen reduction Pd-based intermetallics

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锂金属负极固体电解质界面膜的理解与改性策略

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科学通报 2024年第10期69卷 1298-1314页

作者：李宛峡李新鹏陈亚威揭育林曹瑞国焦淑红中国科学技术大学化学与材料科学学院材料科学与工程系合肥230026

锂金属负极因具有较高的比容量和较低的电极电势,被认为是最有发展前景的电池负极材料之一.然而,不稳定的锂金属负极固体电解质界面膜和严重的锂枝晶生长问题限制了锂金属负极的实际应用.认识和理解锂金属负极固体电解质界面膜的组成与... 详细信息

锂金属负极因具有较高的比容量和较低的电极电势,被认为是最有发展前景的电池负极材料之一.然而,不稳定的锂金属负极固体电解质界面膜和严重的锂枝晶生长问题限制了锂金属负极的实际应用.认识和理解锂金属负极固体电解质界面膜的组成与结构,并将其与锂金属生长行为建立有效的关联,是解决锂金属负极不稳定问题的关键.本文综述了近年来有关锂金属负极固体电解质界面膜的表征技术和调控策略,并介绍了锂金属软包电池的界面研究现状.本文对锂金属负极的实际应用具有一定的指导意义.

关键词：锂金属负极固体电解质界面膜锂金属枝晶锂金属电池

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Pomegranate-like C_(60)@cobalt/nitrogen-codoped porous carbon for high-performance oxygen reduction reaction and lithium-sulfur battery

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Nano Research 2021年第8期14卷 2596-2605页

作者： Jianhua Wu Shiyang Wang Zhanwu Lei Runnan Guan Muqing Chen Pingwu Du Yalin Lu ruiguo cao Shangfeng Yang Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy ConversionAnhui Laboratory of Advanced Photon Science and TechnologyDepartment of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026China

Porous carbon materials play essential roles in electrocatalysis and electrochemical energy storage.It is of significant importance to rationally design and tune their porous structure and active sites for achieving high electrochemical activity and stability.Herein,we develop a novel approach to tune the morphology of porous carbon materials(PCM)by embedding fullerene C_(60),achieving improved performance of oxygen reduction reaction(ORR)and lithium-sulfur(Li-S)battery.Owing to the strong interaction between C_(60)and imidazole moieties,pomegranate-like hybrid of Ow-embedded zeolitic imidazolate framework(ZIF-67)precursor is synthesized,which is further pyrolyzed to form C_(60)-embedded cobalt/nitrogen-codoped porous carbon materials(abbreviated as C_(60)@Co-N-PCM).Remarkably,the unique structure of C_(60)@Co-N-PCM offers excellent ORR electrocatalytic activity and stability in alkaline solutions,outperforming the commercial Pt/C(20 wt.%)catalyst.Besides,C_(60)@Co-N-PCM as a novel cathode delivers a high specific capacity of-900 mAh·g^(-1) at 0.2 C rate in Li-S batteries,which is superior to the pristine ZIF-67-derived PCM without embedding C_(60).

关键词： porous carbon materials fullerene zeolitic imidazolate framework(ZIF) oxygen reduction reaction(ORR) lithium-sulfur(Li-S)battery

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Conductive metal-organic frameworks promoting polysulfides transformation in lithium-sulfur batteries

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Journal of Energy Chemistry 2021年第12期30卷 336-343,I0008页

作者： Shuai Wang Fanyang Huang Zhengfeng Zhang Wenbin Cai Yulin Jie Shiyang Wang Pengfei Yan Shuhong Jiao ruiguo cao Hefei National Laboratory for Physical Science at the Microscale Department of Material Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026AnhuiChina Beijing Key Laboratory of Microstructure and Properties of Solids Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China

Metal organic frameworks(MOFs) have been extensively investigated in Li-S batteries owing to high surface area, adjustable structures and abundant catalytic sites. Nevertheless, the insulating nature of traditional MOFs render retarded kinetics of polysulfides conversion, leading to insufficient utilization of sulfur. In comparison, conductive MOFs(c-MOFs) show great potential for promoting polysulfides transformation due to superb electronic conductivity. In this work, a nickel-catecholates based c-MOF, NiHHTP(HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene), is designed to regulate surface chemistry of self-supported carbon paper for advanced Li-S batteries. Taking advantage of the porous structure and high conductivity, the as-prepared Ni-HHTP is conducive to synergising strengthening the chemisorption of polysulfides and accelerating the reaction kinetics in Li-S batteries, significantly mitigating the polysulfides diffusion from the non-encapsulated sulfur cathode, therefore promoting polysulfides transformation in Li-S batteries. This work points out a promising modification strategy for developing advanced sulfur cathode in Li-S batteries.

关键词： Li-S batteries Conductive metal-organic framework Surface modification Ni-HHTP

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Carbon materials for stable Li metal anodes: Challenges, solutions, and outlook

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Carbon Energy 2021年第6期3卷 957-975页

作者： Qiongqiong Lu Yulin Jie Xiangqi Meng Ahmad Omar Daria Mikhailova ruiguo cao Shuhong Jiao Yan Lu Yaolin Xu Leibniz Institute for Solid State and Materials Research(IFW)Dresden e.V. DresdenGermany Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiChina Department of Electrochemical Energy Storage Helmholtz-Zentrum Berlin für Materialien und Energie(HZB)BerlinGermany Institute of Chemistry University of PotsdamPotsdamGermany

Lithium(Li)metal is regarded as the ultimate anode for next-generation Li-ion batteries due to its highest specific capacity and lowest electrochemical potential.However,the Li metal anode has limitations,including virtually infinite volume change,nonuniform Li deposition,and an unstable electrode-electrolyte interface,which lead to rapid capacity degradation and poor cycling stability,significantly hindering its practical application.To address these issues,intensive efforts have been devoted toward accommodating and guiding Li deposition as well as stabilizing the interface using various carbon materials,which have demonstrated excellent effectiveness,benefiting from their vast variety and excellent tunability of the structure-property relationship.This review is intended as a guide through the fundamental challenges of Li metal anodes to the corresponding solutions utilizing carbon materials.The specific functionalities and mechanisms of carbon materials for stabilizing Li metal anodes in these solutions are discussed in detail.Apart from the stabilization of the Li metal anode in liquid electrolytes,attention has also been paid to the review of anode-free Li metal batteries and solid-state batteries enabled by strategies based on carbon materials.Furthermore,we have reviewed the unresolved challenges and presented our outlook on the implementation of carbon materials for stabilizing Li metal anodes in practical applications.

关键词： carbon materials interface engineering Li deposition regulation Li metal anode structure stabilization

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