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Revisiting the Role of Physical Confinement and Chemical Regulation of 3D Hosts for Dendrite-Free Li Metal Anode

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Nano-Micro Letters 2022年第11期14卷 290-306页

作者： Shufen Ye Xingjia Chen Rui Zhang Yu Jiang fanyang huang Huijuan huang Yu Yao Shuhong Jiao Xiang Chen Qiang Zhang Yan Yu Hefei National Center for Physical Sciences at the Microscale Department of Materials Science and EngineeringiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)CAS Key Laboratory of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei 230026AnhuiPeople’s Republic of China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081People’s Republic of China School of Materials Science and Engineering Anhui UniversityHefei 230601AnhuiPeople’s Republic of China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084People’s Republic of China National Synchrotron Radiation Laboratory Hefei 230026AnhuiPeople’s Republic of China

Lithium metal anode has been demonstrated as the most promising anode for lithium batteries because of its high theoretical capacity,but infinite volume change and dendritic growth during Li electrodeposition have prevented its practical *** physical morphology confinement and chemical adsorption/diffusion regulation are two crucial approaches to designing lithiophilic materials to alleviate dendrite of Li metal ***,their roles in suppressing dendrite growth for long-life Li anode are not fully understood ***,three different Ni-based nanosheet arrays(NiO-NS,Ni_(3)N-NS,and Ni_(5)P_(4)-NS)on carbon cloth as proof-of-concept lithiophilic frame-works are proposed for Li metal *** two-dimensional nanoarray is more promising to facilitate uniform Li^(+)flow and electric *** with the NiO-NS and the Ni_(5)P_(4)-NS,the Ni_(3)N-NS on carbon cloth after reacting with molten Li(Li-Ni/Li_(3)N-NS@CC)can afford the strongest adsorption to Li+and the most rapid Li+diffusion ***,the Li-Ni/Li_(3)N-NS@CC electrode realizes the lowest overpotential and the most excellent electrochemical performance(60 mA cm^(−2)and 60 mAh cm^(−2)for 1000 h).Furthermore,a remarkable full battery(LiFePO_(4)||Li-Ni/Li_(3)N-NS@CC)reaches 300 cycles at *** research provides valuable insight into designing dendrite-free alkali metal batteries.

关键词： Li metal anodes 3D carbon framework Ni-based nanosheets Physical morphology confinement Chemical adsorption/diffusion regulation

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 ***,their working mechanisms are still mysterious,especially in practical high-voltage LiCoO_(2)pouch lithium-ion ***,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 *** 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 *** 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 *** 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

Regulating Pd‐catalysis for electrocatalytic CO_(2) reduction to formate via intermetallic PdBi nanosheets

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Chinese Journal of Catalysis 2022年第7期43卷 1680-1686页

作者： Linfeng Xie Xuan Liu fanyang huang Jiashun Liang Jianyun Liu Tanyuan Wang Liming Yang Ruiguo Cao Qing Li State Key Laboratory of Material Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina Key Laboratory of Materials for Energy Conversion Chinese Academy of Science(CAS) Department of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026AnhuiChina School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074HubeiChina

Electrocatalytic CO_(2) reduction plays an important role in the reduction of the CO_(2) concentration in atmosphere and consequently the mitigation of greenhouse *** has been extensively inves‐tigated as an electrocatalyst for the CO_(2) reduction to formate,which is an important raw material in the production of organic ***,the low selectivity and competitive reaction(hydro‐gen evolution reaction(HER))have hindered the performance of monometallic Pd *** this paper,intermetallic PdBi nanosheets(NSs)are prepared for efficient CO_(2) reduction to *** highest Faradaic efficiency(FE)of formate on fully ordered PdBi NSs reaches 91.9%at−1.0 V ***,which outperforms that of the disordered PdBi and pure Pd *** functional theo‐ry calculations suggest that compared to disordered PdBi NSs,the ordered structure can decrease the free energy barrier of*OCHO(a key intermediate of formate formation)and inhibit H_(2) evolution as well,thereby enhancing the activity and selectivity for formate production.

关键词： CO_(2)reduction Electrocatalysis Formate Palladium Intermetallic compound Nanosheet

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 ***,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 *** 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 *** 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 ***,L1_(0)-Mo-PdZn NSs is extremely stable for ORR,with only 2.3% activity loss after 10000 potential *** 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

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

Deciphering pitting behavior of lithium metal anodes in lithium sulfur batteries

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Journal of Energy Chemistry 2020年第10期29卷 257-261页

作者： fanyang huang Shuai Wang Yulin Jie Evan Hansen Shiyang Wang Zhanwu Lei Jian Liu Ruiguo Cao Genqiang Zhang 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 230026AnhuiChina School of Engineering Faculty of Applied ScienceUniversity of British ColumbiaKelownaBCV1V1V7Canada

Unambiguous understanding in lithium anode failure mechanism calls for a comprehensive methodology to investigate the coupled morphological,electrochemical and mechanical behaviors during the stripping *** this work,a mechanistic investigation of the pitting behavior of lithium metal in an electrolyte containing lithium polysulfides in lithium sulfur batteries was *** is found that lithium polysulfides could aggravate the nonuniform stripping of lithium electrodes.

关键词： Lithium anode Pitting behavior Failure mechanism Lithium sulfur batteries

各向同性模量的分级多孔隔膜促进锌离子均匀扩散及水系锌离子电池循环稳定性

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Science China Materials 2023年第3期66卷 982-991页

作者：张丰麟黄凡洋黄仁智董宁焦淑红曹瑞国潘慧霖 Department of Chemistry Zhejiang UniversityHangzhou 310027China Department of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027China

水系锌离子电池具有低成本、高安全的特点,有望应用于大规模储能.然而,锌负极的循环稳定性仍不理想,且水系电池缺少合适的亲水隔膜,这限制了水系锌离子电池的实际应用.在本文中,我们报道了一种可用于水系电池的分级多孔的聚偏二氟乙烯-... 详细信息

水系锌离子电池具有低成本、高安全的特点,有望应用于大规模储能.然而,锌负极的循环稳定性仍不理想,且水系电池缺少合适的亲水隔膜,这限制了水系锌离子电池的实际应用.在本文中,我们报道了一种可用于水系电池的分级多孔的聚偏二氟乙烯-双三氟甲磺酰亚胺锂(PVDF-LiTFSI)(PVDF-Li)隔膜.均匀混合的LiTFSI盐降低了PVDF的结晶性,使隔膜具有优异的机械强度,并形成分级的孔隙结构.这种LiTFSI诱导的分级多孔结构有助于实现Zn2+的快速传输和锌的均匀沉积,同时保证隔膜在水系电解液中具有优异的润湿性.这种先进的PVDF-Li隔膜能显著抑制锌枝晶的生长,提高水系锌离子电池的循环寿命.因此,使用PVDF-Li隔膜的Zn||V2O5电池的初始容量达324 mA h g-1,比传统玻璃纤维隔膜高27%,且容量保持率也得到大幅提升.该研究设计了一种功能隔膜来调控正负极反应的均匀性,这为高性能水系电池的开发提供了新的思路.

关键词：锌离子电池循环寿命水系电解液初始容量聚偏二氟乙烯锌负极循环稳定性均匀扩散

AI for organic and polymer synthesis

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Science China Chemistry 2024年第8期67卷 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You Center of Chemistry for Frontier Technologies Department of ChemistryZhejiang UniversityHangzhou 310027China Center of Basic Molecular Science Department of ChemistryTsinghua UniversityBeijing 100084China Guangzhou National Laboratory Guangzhou 510005China Center for Quantitative Biology Academy for Advanced Interdisciplinary StudiesPeking UniversityBeijing 100871China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China School of Materials Science and Engineering Peking UniversityBeijing 100871China Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China AI for Science(AI4S)-Preferred Program Shenzhen Graduate SchoolPeking UniversityShenzhen 518055China State Key Laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Department of Chemical Sciences National Natural Science Foundation of ChinaBeijing 100085China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

关键词： organic synthesis polymer synthesis machine learning prediction chemical database automated synthesis

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氟代溶剂在锂金属电池中的应用

物理化学学报 2022年第11期38卷 72-88页

作者：何子旭陈亚威黄凡洋揭育林李新鹏曹瑞国焦淑红中国科学技术大学中国科学院能量转换材料重点实验室材料科学与工程系合肥微尺度物质科学国家研究中心合肥230026

近年来,锂金属电池由于具有较高的能量密度而成为储能领域的研究热点。电解液作为锂金属电池的“血液”发挥着至关重要的作用。在传统锂离子电池电解液中,锂金属负极与电解液之间的界面副反应严重并伴随着锂枝晶生长,从而导致安全隐患... 详细信息

近年来,锂金属电池由于具有较高的能量密度而成为储能领域的研究热点。电解液作为锂金属电池的“血液”发挥着至关重要的作用。在传统锂离子电池电解液中,锂金属负极与电解液之间的界面副反应严重并伴随着锂枝晶生长,从而导致安全隐患以及循环寿命缩短等问题。在解决锂金属负极问题上,电解液调控策略具有易操作性和有效性,因而在推动锂金属电池发展方面具有举足轻重的地位。氟代电解液是目前重要的研究方向,氟代电解液在循环过程中能够在电极表面形成富含LiF的固体电解质界面膜(SEI);该界面膜不仅可以有效抑制负极锂枝晶的形成,并且在正极方面能够大幅提高电解液的氧化稳定性,从而提升高电压正极的适配性和锂金属电池的循环稳定性。氟代电解液中氟代溶剂/氟代锂盐的分子结构对电解液的溶剂化结构有重要影响。当氟代溶剂分子中氟原子的位置与数量不同时,氟代溶剂的物理化学性质也会随之发生变化,进而改变了电解液与电极的界面反应性。因此,氟代溶剂能够起到调制SEI膜成分和结构的作用,是决定电池性能的关键因素。本文总结了应用于锂金属电池的主要氟代溶剂,尤其是近几年来发展的新型氟代溶剂;着重介绍了高度氟代的溶剂分子作为局域超浓电解液的稀释剂,以及对溶剂进行精准分子设计得到的部分氟代溶剂等。此外,本文还分析探讨了氟代溶剂分子与电池性能之间的构效关系,展望了构建新型氟代溶剂分子的策略,希望能对电解液溶剂分子的结构设计以及构效关系的评估有一定的启发意义。

关键词：锂金属电池氟代电解液氟代溶剂溶剂化结构固体电解质界面膜

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