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Revealing the solid electrolyte interface on calcium metal anodes

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Journal of Energy Chemistry 2022年第7期31卷 174-190,I0005页

作者： Yumeng Zhao Aoxuan Wang Libin Ren Xingjiang Liu Jiayan Luo Key Laboratory for Green Chemical Technology of Ministry of Education State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin UniversityTianjin 300072China Shanghai Key Lab of Advanced High-Temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China National Key Laboratory of Science and Technology on Power Sources Tianjin Institute of Power SourcesTianjin 300384China

Owing to its low potential, crustal abundances and environmental friendliness, calcium metal anode(CMA) is emerging as a powerful contender in post-lithium era. However, the passivation of CMA fatally hinders its development. Recently, several feasible electrolytes have been developed. Nevertheless, as a pivotal part, the solid electrolyte interface(SEI) formed on CMA has not been paid enough attention to. In this review, based on the passivation mechanism of CMA, the favorable composition of SEI is emphasized with the corresponding electrolytes. It is considered that boron-containing and organic–inorganic hybrid SEI might be preferred. By comparing electrolytes and SEI on CMA with lithium and magnesium metal anodes, the root causes of CMA passivation are further elaborated, enlightening rational design rules of suitable SEI. Furthermore, some noteworthy details when assembling secondary calcium metal batteries(CMBs) are put forward. It is expected that deeper understanding of SEI on CMA will promote the development of CMBs.

关键词： solid electrolyte interface Calcium metal anode Reversible deposition Passivation mechanism

Unraveling the stabilization mechanism of solid electrolyte interface on ZnSe by rGO in sodium ion battery

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Journal of Energy Chemistry 2021年第3期30卷 124-130页

作者： Shuang Men Hui Zheng Dejun Ma Xiaolian Huang Xiongwu Kang School of Environment and Energy South China University of TechnologyGuangzhou 510006GuangdongChina Department of Chemical Engineering Northwest UniversityXi'an 710069ShaanxiChina School ofPhamacy Guangdong Pharmaceutical UniversityGuangzhou 510006GuangdongChina College of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina

Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its infancy.Here in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged states.It is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode structure.However,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was formed.ZnSe@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/g.This study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.

关键词： ZIF-8 Zinc selenide Transition metal selenide Reduced graphene oxide XPS solid electrolyte interface Sodium ion batteries

Postmortem ^(7)Li NMR analysis for assessing the reversibility of lithium metal electrodes in lithium metal batteries

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Journal of Energy Chemistry 2024年第7期94卷 430-440页

作者： Jaewon Baek Sunha Kim Hee-Tak Kim Oc Hee Han Department of Chemical&Biomolecular Engineering KAISTDaejeon 34141Republic of Korea Metropolitan Seoul Center Korea Basic Science InstituteSeoul 03759Republic of Korea Graduate School of Analytical Science&Technology Chungnam National UniversityDaejeon 34134Republic of Korea

Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,we conducted a comprehensive postmortem analysis utilizing ^(7)Li NMR,employing a stan-dard magic angle spinning probe to examine protective-layer coated Li metal electrodes and LiAg alloy electrodes against bare Li metal electrodes within Li metal batteries(LMBs).Our investigation explores the effects of sample burrs,alignment with the magnetic field,the existence of liquid electrolytes,and precycling on the ^(7)Li NMR signals.Through contrasting NMR spectra before and after cycling,we identi-fied alterations in Li^(0) and Li^(+) signals attributable to the degradation of the Li metal electrode.Our NMR analyses decisively demonstrate the efficacy of the protective layer in mitigating dendrite and solid elec-trolyte interphase formation.Moreover,we noted that Li*ions near the Li metal surface exhibit magnetic susceptibility anisotropy,revealing a novel approach to studying diamagnetic species on Li metal elec-trodes in LMBs.This study provides valuable insights and practical guidelines for characterizing distinct lithium states within LMBs.

关键词： NMR spectroscopy Lithium-7 Lithium metal battery electrolyte Electrode-protective layer solid electrolyte interface Magnetic susceptibility anisotropy Lithium-metal NMR signal Diamagnetic^(7)Li NMR signal

Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries

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能源化学:英文版 2023年第8期83卷 239-246,I0008页

作者： Qing-Song Liu Yi-Zhou Quan Mei-Chen Liu Guo-Rui Zhu Xiu-Li Wang Gang Wu Yu-Zhong Wang The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu 610064SichuanChina

The rapid development and widespread application of lithium-ion batteries(LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on LIBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate(BMOP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity,high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for LIBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance LIBs.

关键词： Multifunctional additives Electrode compatibility solid electrolyte interface Solvation structure Lithium-ion batteries

Engineering homotype heterojunctions in hard carbon to induce stable solid electrolyte interfaces for sodium-ion batteries

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Carbon Energy 2023年第1期5卷 181-193页

作者： Chengxin Yu Yu Li Haixia Ren Ji Qian Shuo Wang Xin Feng Mingquan Liu Ying Bai Chuan Wu Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science and EngineeringBeijing Institute of TechnologyBeijingPeople's Republic of China Yangtze Delta Region Academy of Beijing Institute of Technology JiaxingPeople's Republic of China Department of Materials Science and Engineering Peking UniversityBeijingPeople's Republic of China

Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.

关键词： hard carbon anodes homotype heterojunctions sodium-ion batteries solid electrolyte interface surface engineering

electrolyte and current collector designs for stable lithium metal anodes

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International Journal of Minerals,Metallurgy and Materials 2022年第5期29卷 953-964页

作者： Simeng Zhang Gaojing Yang Xiaoyun Li Yejing Li Zhaoxiang Wang Liquan Chen Key Laboratory for Renewable Energy Chinese Academy of SciencesBeijing Key Laboratory for New Energy Materials and DevicesInstitute of PhysicsChinese Academy of SciencesBeijing 100190China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100190China

With the increasing demand for high energy-density batteries for portable electronics and large-scale energy storage systems,the lithium metal anode(LMA)has received tremendous attention because of its high theoretical capacity and low redox potential.However,the commercial application of LMAs is impeded by the uncontrolled growth of lithium dendrites.Such dendrite growth may result in internal short circuits,detrimental side reactions,and the formation of dead lithium.Therefore,the growth of lithium metal must be controlled.This article summarizes our recent efforts in inhibiting such dendrite growth,decreasing the detrimental side reactions,and elongating the LMA lifespan by optimizing the electrolyte structure and by designing appropriate current collectors.After identifying that the unstable solid electrolyte inter-face(SEI)film is responsible for the potential dropping in carbonate electrolytes,we developed LiPF_(6)-LiNO_(3) dual-salt electrolyte and lithium bis(fluorosulfonyl)imide(LiFSI)-carbonate electrolyte to stabilize the SEI film of LMAs.In addition,we achieved controlled lithium depos-ition by designing the structure and material of the current collectors,including selective lithium deposition in porous current collectors,lithio-philic metal guided lithium deposition,and iron carbide induced underpotential lithium deposition in nano-cavities.The limitations of the cur-rent strategies and prospects for future research are also presented.

关键词： lithium metal anode electrolyte current collector lithium dendrite solid electrolyte interface

Boosting high initial coulombic efficiency of hard carbon by in-situ electrochemical presodiation

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Journal of Energy Chemistry 2023年第2期77卷 310-316,I0008页

作者： Nannan Qin Yanyan Sun Chao Hu Sainan Liu Zhigao Luo Xinxin Cao Shuquan Liang Guozhao Fang School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083HunanChina College of Chemistry Xiangtan UniversityXiangtan 411105HunanChina Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083HunanChina

Hard carbon(HC)is a promising anode material for sodium ion batteries(SIBs),whereas inferior initial coulombic efficiency(ICE)severely limits its practical application.In the present work,we propose an in situ electrochemical presodiation approach to improve ICE by mixing sodium biphenyl(Na-Bp)dimethoxyethane(DME)solution with DME-based ether electrolyte.A solid electrolyte interface(SEI)could be formed beforehand on the HC electrode and Na^(+)was absorbed to nanopores and graphene stacks,compensating for the sodium loss and preventing electrolyte decomposition during the initial charge and discharge cycle.By this way,the ICE of half-cells was increased to nearly 100%and that of full-cells from 45%to 96%with energy density from 132.9 to 230.5 W h kg^(-1).Our work provides an efficient and facile method for improving ICE,which can potentially promote the practical application of HCbased materials.

关键词： Hard carbon In situ presodiation Initial coulombic efficiency solid electrolyte interface Sodium-ion batteries

A review on lithium-sulfur batteries:Challenge,development,and perspective

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Nano Research 2023年第6期16卷 8097-8138页

作者： Qinjun Shao Shengdong Zhu Jian Chen Advanced rechargeable battery Laboratory Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Lithium-sulfur(Li-S)battery is recognized as one of the promising candidates to break through the specific energy limitations of commercial lithium-ion batteries given the high theoretical specific energy,environmental friendliness,and low cost.Over the past decade,tremendous progress have been achieved in improving the electrochemical performance especially the lifespan by various strategies mainly concentrated on the sulfur cathodes.In this review,the fundamental electrochemistry of sulfur cathode and lithium anode is revealed to understand the current dilemmas.And the advances achieved through diverse strategies are comprehensively summarized,which involves lithium polysulfides(LiPSs)limitation,sulfur redox reaction regulation and electrocatalysis in sulfur cathode and artificial solid electrolyte interface(SEI),electrolyte design,and structured anode in lithium anode.Additionally,the differences between laboratory level coin cells and actual pouch cells need to be addressed that only few reports on practical Li-S pouch cell are available due to the unexpected problems on both sulfur cathode and lithium anode which are masked at lithium and electrolyte excess.Lastly,the challenges and perspective toward the practical Li-S batteries are also offered.

关键词： lithium-sulfur batteries shuttle effect lithium dendrite solid electrolyte interface Coulombic efficiency

Surface engineering based on in situ electro-polymerization to boost the initial Coulombic efficiency of hard carbon anode for sodium-ion battery

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Rare Metals 2022年第5期41卷 1616-1625页

作者： Cheng-Xin Yu Yu Li Zhao-Hua Wang Xin-Ran Wang Ying Bai Chuan Wu Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China Yangtze Delta Region Academy of Beijing Institute of Technology Jiaxing 314019China

Hard carbon(HC) is considered as a commercial candidate for anode materials of sodium-ion batteries due to its low cost and excellent capacity. However, the problem of low initial Coulombic efficiency is still urgently needed to be solved to promote the industrialization of HC.In this paper, 2,2-dimethylvinyl boric acid(DEBA) is used to modify the surface of HC to prepare HC-DEBA materials. During the cycling, the C = C bonds of DEBA molecules will be in situ electro-polymerized to form a polymer network, which can act as the passive protecting layer to inhibit irreversible decomposition of electrolyte,and induce a thinner solid electrolyte interface with lower interface impedance. Therefore, HC-DEBA has higher initial Coulombic efficiency and better cycling stability. In ester-based electrolyte, the initial Coulombic efficiency of the optimized HC-DEBA-3% increases from 65.2% to77.2%. After 2000 cycles at 1 A·g^(-1), the capacity retention rate is 90.92%. Moreover, it can provide a high reversible capacity of 294.7 m Ah·g^(-1) at 50 mA·g^(-1). This simple surface modification method is ingenious and versatile,which can be extended to other energy storage materials.

关键词： Sodium-ion battery Hard carbon Initial Coulombic efficiency solid electrolyte interface Surface modification Ester electrolyte