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Journal of Energy Chemistry 2023年第4期79卷 110-117页

作者： Zhuangzhuang Cui Shunqiang Chen Qingshun Nian Yecheng Li Yawei Chen Bing-Qing Xiong Zihong Wang Zixu He Shuhong Jiao Xiaodi Ren School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026AnhuiChina

Ethers are promising electrolyte solvents for secondary Li metal batteries because of their excellent reduction stability.However,their oxidation stability has been mostly relying on the high concentration approach,and limited progress has been made on building effective interphase to protect the cathode from the corrosion of the electrolyte.In this work,we construct a semi-crystalline interfacial layer on the surface of Li(Ni_(0.8)Co_(0.1)Mn_(0.1))O_(2)cathode that can achieve improved electrochemical stability in the highly corrosive chemical environment formed by the decomposition of ether molecules.Different from traditional brittle crystalline interphases,the optimized semi-crystalline layer with low modulus and high ionic conductivity can effectively relieve electrode strain and maintain the integrity of the interface layer.Due to this design,the continuous oxidation decomposition of ether-based electrolytes could be significantly suppressed and the battery shows outstanding cycling stability(84%capacity retention after 300 cycles).This article provides a solution to address the oxidation instability issue of ether-based electrolytes.

关键词： cathode/electrolyte interphase Semi-crystalline Ether electrolyte high-voltage cathode Li-metal batteries

One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi_(0.5)Mn_(1.5)O_(4) for high-voltage lithium-ion battery

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Nano Research 2024年第5期17卷 4192-4202页

作者： Min Xu Bifu Sheng Yong Cheng Junjie Lu Minfeng Chen Peng Wang Bo Liu Jizhang Chen Xiang Han Ming-Sheng Wang Siqi Shi College of Materials Science and Engineering Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesNanjing Forestry UniversityNanjing 210037China State Key Laboratory of Physical Chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamen 361005China College of Mathematics and Physics Jinggangshan UniversityJi’an 343009China School of Materials Science and Engineering Shanghai UniversityShanghai 200444China Western Digital Corporation 951 Sandisk DrMilpitasCA 95035USA

LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)with a spinel crystal structure presents a compelling avenue towards the development of economic cobalt-free and high voltage(~5 V)lithium-ion batteries.Nevertheless,the elevated operational voltage of LNMO gives rise to pronounced interfacial interactions between the distorted surface lattices characterized by Jahn-Teller(J-T)distortions and the electrolyte constituents.Herein,a localized crystallized coherent LaNiO_(3) and surface passivated Li_(3)PO_(4) layer is deposited on LNMO via a one-step calcination process.As evidenced by transmission electron microscopy(TEM),time-of-flight secondary ion mass spectrometry(ToF-SIMS)and density functional theory(DFT)calculation,the epitaxial growth of LaNiO_(3) along the LNMO lattice can effectively stabilize the structure and inhibit irreversible phase transitions,and the Li_(3)PO_(4) surface coating can prevent the chemical reaction between HF and transition metals without sacrificing the electrochemical activity.In addition,the ionic conductive Li_(3)PO_(4) and atomic wetting inter-layer enables fast charge transfer transport property.Consequently,the LNMO material enabled by the lattice bonding and surface passivating features,demonstrates high performance at high current densities and good capacity retention during long-term test.The rational design of interface coherent engineering and surface coating layers of the LNMO cathode material offers a new perspective for the practical application of high-voltage lithium-ion batteries.

关键词： high-voltage cathode interface-coherent surface passivating electrochemical performance

Facile synthesis of hierarchical Na2Fe(SO4)2@rGO/C as high-voltage cathode for energy density-enhanced sodium-ion batteries

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Journal of Energy Chemistry 2020年第11期29卷 387-394页

作者： Ge Yao Xixue Zhang Yongliang Yan Jiyu Zhang Keming Song Juan Shi Liwei Mi Jinyun Zheng Xiangming Feng Weihua Chen Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina Center for Advanced Materials Research Zhongyuan University of TechnologyZhengzhou 450007HenanChina

Fe-based sulfates are ideal cathode candidates for sodium-ion batteries(SIBs) owing to their high operating voltage and low cost but suffer from the nature of poor power performance. Herein, a hierarchical porous Na2Fe(SO4)2@reduced graphene oxide/carbon dot(Na2Fe(SO4)2@rGO/C) with low carbon content(4.12 wt%) was synthesized via a facile homogeneous strategy benefiting for engineering application,which delivers excellent sodium storage performance(high voltage plateau of 3.75 V, 85 m Ah g-1 and330 Wh kg-1 at 0.05 C;5805 W kg-1 at 10 C) and high Na+diffusion coefficient(1.19 × 10-12 cm2 s-1).Moreover, the midpoint voltage of assembled full cell could reach 3.0 V. The electron transfer and reaction kinetics are effectively boosted since the nanoscale Na2Fe(SO4)2 is supported by a robust crosslinked carbon matrix with rGO sheets and carbon dots. The slight rGO sheets sufficiently enhance the electron transfer like a current collecter and restrain the aggregation, as well as ensure smooth ion channels. Meanwhile, the carbon dots in the whole space connect with Na2Fe(SO4)2 and help rGO to promote the conductivity of the electrode. Ex-situ X-ray powder diffraction and X-ray photoelectron spectrometry analysis confirm the high reversibility of this sodiation/desodiation process.

关键词： Sodium ion batteries high-voltage cathode Fe-based sulfates Full cell Hierarchical structure

Sodium-based dual-ion batteries via coupling high-capacity selenium/graphene anode with high-voltage graphite cathode

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Chinese Chemical Letters 2020年第9期31卷 2314-2318页

作者： Xiankun Hou Wenhao Li Yingying Wang Shaofang Li Yunfeng Meng Haiyue Yu Baokuan Chen Xinglong Wu National&Local United Engineering Lab for Power Battery Department of ChemistryNortheast Normal UniversityChangchun 130024China Key Laboratory for UV Light-Emitting Materials and Technology of Ministry of Education Northeast Normal UniversityChangchun 130024China College of Chemistry Chemical Engineering and Environmental EngineeringLiaoning Shihua UniversityFushun 113001China

Dual ion batteries(DIBs) exhibit broad application prospects in the field of electrical energy storage(EES)devices with excellent properties,such as high voltage,high energy density,and low cost.In the graphitebased DIBs,high voltage is needed to store enough anions with the formation of anion intercalation compound XCn(X=AlCl4-,PF6-,TFSI-,etc.).Hence,it is difficult for graphite-based DIBs to match proper anodes and electrolytes.Here,an Se/graphene composite is prepared via a convenient method,and assembled into a dual-ion full battery(DIFB) as anode with graphite cathode and 1 mol/L NaPF6 in EC:EMC(1:1,v:v).This DIFB has achieved a high discharge capacity of 75.9 mAh/g and high medium output voltage of 3.5 V at 0.1 A/g.Actually,the suitable anode materials,such as the present Se/graphene composite,are extremely important for the development and application of graphite-based DIBs.This study is enlightening for the design of future low-cost EES devices including graphite-based DIBs.

关键词： Dual ion batteries high-capacity anode Se/grapheme high-voltage cathode Graphite

Research Progress in Improving the Cycling Stability of high-voltage LiNi0.5Mn1.5O4 cathode in Lithium-Ion Battery

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Nano-Micro Letters 2017年第2期9卷 97-115页

作者： XiaoLong Xu SiXu Deng Hao Wang JingBing Liu Hui Yan The College of Materials Science and Engineering Beijing University of TechnologyBeijing 100124People’s Republic of China

high-voltage lithium-ion batteries(HVLIBs) are considered as promising devices of energy storage for electric vehicle, hybrid electric vehicle, and other high-power equipment. HVLIBs require their own platform voltages to be higher than 4.5 V on charge. Lithium nickel manganese spinel LiNi_(0.5)Mn_(1.5)O_4(LNMO) cathode is the most promising candidate among the 5 V cathode materials for HVLIBs due to its flat plateau at 4.7 V. However, the degradation of cyclic performance is very serious when LNMO cathode operates over 4.2 V. In this review, we summarize some methods for enhancing the cycling stability of LNMO cathodes in lithium-ion batteries, including doping, cathode surface coating,electrolyte modifying, and other methods. We also discuss the advantages and disadvantages of different methods.

关键词： high-voltage cathode LiNi0.5Mn1.5O4 Lithium-ion battery Cycling stability Platform voltage

Fluorine-substituted O3-type NaNi_(0.4)Mn_(0.25)Ti_(0.3)Co_(0.05)O_(2-x)F_(x) cathode with improved rate capability and cyclic stability for sodium-ion storage at high voltage

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Journal of Energy Chemistry 2021年第9期30卷 341-350页

作者： Chaojin Zhou Lichun Yang Chaogang Zhou Jiangwen Liu Renzong Hu Jun Liu Min Zhu School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510641GuangdongChina College of Metallurgy and Energy Key Laboratory of the Ministry of Education for Modern Metallurgy TechnologyNorth China University of Science and TechnologyTangshan 063210HebeiChina

O3-type Na NiO_(2)-based cathode materials undergo irreversible phase transition and serious capacity decay at high voltage above 4.0 V in sodium-ion batteries. To address these challenges, effects of Fsubstitution on the structure and electrochemical performance of Na Ni_(0.4)Mn_(0.25)Ti_(0.3)Co_(0.05)O_(2) are investigated in this article. The F-substitution leads to expanding of interlayer, which can enhance the mobility of Na+. NaNi_(0.4)Mn_(0.25)Ti_(0.3)Co_(0.05)O_(1.92)F_(0.08)(NMTC-F_(0.08)) with the optimal F-substitution degree exhibits much improved rate capability and cyclic stability. It delivers reversible capacities of 177 and 97 m Ah g^(-1) at 0.05 and 5 C within 2.0–4.4 V, respectively. Galvanostatic intermittent titration technique verifies faster kinetics of Na+diffusion in NMTC-F_(0.08). And in-situ XRD investigation reveals the phase evolution of NMTC-F_(0.08), indicating enhanced structural stability results from F-substitution. This study may shed light on the development of high performance cathode materials for sodium-ion storage at high voltage.

关键词： F-substitution Sol-gel method O3-type cathode Sodium-ion battery high-voltage cathode

Insights Into the Interfacial Degradation of high-voltage All-Solid-State Lithium Batteries

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Nano-Micro Letters 2022年第12期14卷 1-13页

作者： Jiawen Li Yuchen Ji Haoran Song Shiming Chen Shouxiang Ding Bingkai Zhang Luyi Yang Yongli Song Feng Pan School of Advanced Material Peking University Shenzhen Graduate SchoolShenzhen 518055People’s Republic of China Guangzhou Key Laboratory of Clean Transportation Energy Chemistry School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 51006People’s Republic of China

Poly(ethylene oxide)(PEO)-based solid polymer electrolyte(SPE)is considered as a promising solid-state electrolyte for all-solid-state lithium batteries(ASSLBs).Nevertheless,the poor interfacial stability with high-voltage cathode materials(e.g.,LiCoO_(2))restricts its application in high energy density solid-state batteries.Herein,high-voltage stable Li_(3)AlF_(6) protective layer is coated on the surface of LiCoO_(2) particle to improve the performance and investigate the failure mechanism of PEO-based ASSLBs.The phase transition unveils that chemical redox reaction occurs between the highly reactive LiCoO_(2) surface and PEO-based SPE,resulting in structure collapse of LiCoO_(2),hence the poor cycle performance of PEO-based ASSLBs with LiCoO_(2) at charging voltage of 4.2 V vs Li/Li+.By sharp contrast,no obvious structure change can be found at the surface of Li_(3)AlF_(6)-coated LiCoO_(2),and the original layered phase was well retained.When the charging voltage reaches up to 4.5 V vs Li/Li+,the intensive electrochemical decomposition of PEO-based SPE occurs,leading to the constant increase of cell impedance and directly causing the poor performance.This work not only provides important supplement to the failure mechanism of PEO-based batter-ies with LiCoO_(2),but also presents a universal strategy to retain structure stability of cathode-electrolyte interface in high-voltage ASSLBs.

关键词： Solid-state battery Poly(ethylene oxide) Surface modification Interface stability high-voltage cathode

LiF and LiNO_(3) as synergistic additives for PEO-PVDF/LLZTO-based composite electrolyte towards high-voltage lithium batteries with dualinterfaces stability

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Journal of Energy Chemistry 2022年第2期31卷 319-328页

作者： Liansheng Li Yuanfu Deng Huanhuan Duan Yunxian Qian Guohua Chen The Key Laboratory of Fuel Cell for Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640GuangdongChina Electrochemical Energy Engineering Research Center of Guangdong Province South China University of TechnologyGuangzhou 510640GuangdongChina Shenzhen CAPCHEM Technol Co Ltd. Shenzhen 518118GuangdongChina Department of Mechanical Engineering The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina

Solid electrolytes with desirable properties such as high ionic conductivity,wide electrochemical stable window,and suitable mechanical strength,and stable electrode-electrolyte interfaces on both cathode and anode side are essential for high-voltage all-solid-state lithium batteries(ASSLBs)to achieve excellent cycle stability.In this work,a novel strategy of using LiF and LiNO_(3) as synergistic additives to boost the performance of PEO-PVDF/LLZTO-based composite solid electrolytes(CSEs)is developed,which also promotes the assembled high-voltage ASSLBs with dual-interfaces stability characteristic.Specifically,LiF as an inactive additive can increase the electrochemical stability of the CSE under high cut-off voltage,and improve the high-voltage compatibility between cathode and CSE,thus leading to a stable cathode/CSE interface.LiNO_(3) as an active additive can lead to an enhanced ionic conductivity of CSE due to the increased free-mobile Li+and ensure a stable CSE/Li interface by forming stable solid electrolyte interphase(SEI)on Li anode surface.Benefiting from the improved performance of CSE and stable dualinterfaces,the assembled NCM622/9[PEO_(15)-LiTFSI]-PVDF-15 LLZTO-2 LiF-3 LiNO_(3)/Li cell delivers a high rate capacity of 102.1 mAh g^(-1) at 1.0 C and a high capacity retention of 77.4%after 200 cycles at 0.5 C,which are much higher than those of the ASSLB assembled with additive-free CSE,with only 60.0 mAh g^(-1) and 52.0%,respectively.Furthermore,novel cycle test modes of resting for 5 h at different charge states after every 5 cycles are designed to investigate the high-voltage compatibility between cathode and CSE,and the results suggest that LiF additive can actually improve the high-voltage compatibility of cathode and CSE.All the obtained results confirm that the strategy of using synergistic additives in CSE is an effective way to achieve high-voltage ASSLBs with dual-interfaces stability.

关键词： Synergistic additives Composite solid electrolyte Dual-interfaces stability high-voltage cathode Lithium metal battery

A cerium-doped NASICON chemically coupled poly(vinylidene fluoride-hexafluoropropylene)-based polymer electrolyte for high-rate and high-voltage quasi-solid-state lithium metal batteries

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Journal of Energy Chemistry 2022年第10期31卷 311-321,I0007页

作者： Tao Huang Wei Xiong Xue Ye Zhencheng Huang Yuqing Feng Jianneng Liang Shenghua Ye Jishou Piao Xinzhong Wang Yongliang Li Xiangzhong Ren Chao Chen Shaoluan Huang Xiaoping Ouyang Qianling Zhang Jianhong Liu Graphene Composite Research Center College of Chemistry and Environmental Engineering.Shenzhen UniversityShenzhen 518060GuangdongChina Institute of information Technology Shenzhen Institute of Information TechnologyShenzhen 518060.GuangdongChina henzhen Eigen-Equation Graphene Technology Co.Ltd Shenzhen 518060Guangdong.China School of Materials Science and Engineering Xiangtan UniversityXiangtan 41105HunanChina

The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors(NASICON)Na_(1.3+x)Al_(0.3)Ce_(x)Ti_(1.7-x)(PO_(4))_(3)(NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide(LiTFSI) matrix.A strong interaction between Ce^(3+)from NCATP and TFSI-anion from the polymer matrix contributes to the fast Li+transportation at the interface.The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0^(-3) S cm^(-1) and a Li^(+) transference number of 0.88.A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm^(-2) presents outstanding cycling stability over 2000 h at 25℃.The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO_(4) at 2 C after 400 cycles and Li/CPEs/LiCoO_(2) at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g^(-1) at 25℃,respectively.

关键词： Quasi-solid-state batteries Composite polymer electrolytes high conductivity high-voltage cathode Oxygen vacancies