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Residual alkali-evoked cross-linked polymer layer for anti-air-sensitivity LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)cathode

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Journal of Energy Chemistry 2024年第5期92卷 450-458页

作者： Chao Zhao Xuebao Li Yun Zhao Jingjing He Yuanpeng Cao Wei Luo Ding Wang Jianguo Duan Xianshu Wang Baohua Li National and Local Joint Engineering Research Center of lithium-ion batteries and materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina School of materials Science and Engineering Central South UniversityChangsha 410083HunanChina Institute of materials Research Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055Guangdong China City College Kunming University of Science and TechnologyKunming 650051YunnanChina

High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.

关键词： lithium-ion batteries Nickel-rich layered cathode Residual alkalis Cross-linked polyme rmodification Airsensitivity

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Regulating the inner Helmholtz plane structure at the electrolyte-electrode interface for highly reversible aqueous Zn batteries

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Journal of Energy Chemistry 2024年第8期95卷 57-67页

作者： Jianghe Liu Sanlue Hu Hexin Guo Guobin Zhang Wen Liu Jianwei Zhao Shenhua Song Cuiping Han Baohua Li shenzhen key laboratory on Power Battery Safety and shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate School Tsinghua University shenzhen key laboratory of Advanced materials School of Materials Science and Engineering Harbin Institute of Technology Faculty of materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences shenzhen HUASUAN Technology Co. Ltd.

The development of aqueous Zn batteries is limited by parasitic water reactions,corrosion,and dendrite growth.To address these challenges,an inner Helmholtz plane（IHP） regulation method is proposed by employing low-cost,non-toxic maltitol as the electrolyte additive.The preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane,and thus hinder the immediate contact between Zn metal and H2O.Meanwhile,strong interaction between maltitol and H2O molecules can restrain the activity of H2O.Besides,the "IHP adsorption effect" along with the low LUMO energy level of maltitol-CF3SO3-can promote the in-situ formation of an organic-inorganic complex solid electrolyte interface（SEI） layer.As a result,the hydrogen/oxygen evolution side reaction,corrosion,and dendrites issues are effectively suppressed,thereby leading to highly reversible and dendrite-free Zn plating/stripping.The Zn‖I2battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability,showing a capacity retention of 75% over 20000 charge-discharge cycles at a large current density of 5 A g-1.In addition,the capacity of the device has almost no obvious decay over20000 cycles even at-30℃.This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.

关键词： Adsorption effect Dendrite suppression Inner Helmholtz plane SEI layer Zn||I2 battery

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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

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Macroporous Directed and Interconnected Carbon Architectures Endow Amorphous Silicon Nanodots as Low‑Strain and Fast‑Charging Anode for lithium‑ion batteries

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Nano-Micro Letters 2024年第5期16卷 333-351页

作者： Zhenwei Li Meisheng Han Peilun Yu Junsheng Lin Jie Yu Guangdong Provincial key laboratory of Semiconductor Optoelectronic materials and Intelligent Photonic Systems Shenzhen Engineering Lab for Supercapacitor MaterialsSchool of Material Science and EngineeringHarbin Institute of TechnologyShenzhenUniversity TownShenzhen 518055People’s Republic of China Songshan Lake materials laboratory Dongguan Dongguan 523808GuangdongPeople’s Republic of China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055People’s Republic of China

Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries.Herein,we report a unique silicon-carbon composite fabricated by uniformly dis-persing amorphous Si nanodots(SiNDs)in carbon nanospheres(SiNDs/C)that are welded on the wall of the macroporous carbon framework(MPCF)by vertical graphene(VG),labeled as MPCF@VG@SiNDs/C.The high dispersity and amor-phous features of ultrasmall SiNDs(~0.7 nm),the flexible and directed electron/Li+transport channels of VG,and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites,rapid Li+transport path,and unique low-strain property during Li+storage.Consequently,the MPCF@VG@SiNDs/C exhibits high cycle stability(1301.4 mAh g^(-1) at 1 A g^(-1) after 1000 cycles without apparent decay)and high rate capacity(910.3 mAh g^(-1),20 A g^(-1))in half cells based on industrial electrode standards.The assembled pouch full cell delivers a high energy density(1694.0 Wh L^(-1);602.8 Wh kg^(-1))and an excellent fast-charging capability(498.5 Wh kg^(-1),charging for 16.8 min at 3 C).This study opens new possibilities for preparing advanced silicon-carbon com-posite anodes for practical applications.

关键词： Amorphous Si nanodots Low-strain Fast-charging lithium-ion batteries

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Tailored architecture of composite electrolyte for all-solid-state sodium batteries with superior rate performance and cycle life

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Nano Research 2024年第5期17卷 4171-4180页

作者： Xiang Guan Zhenhua Jian Xingan Liao Wenchao Liao Yanfei Huang Dazhu Chen Robert K.Y.Li Chen Liu shenzhen key laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518055China Department of materials Science and Engineering City University of Hong KongHong KongChina

Seeking for composite electrolytes reinforced all-solid-state sodium ion batteries with superior long lifespan and rate performance remains a great challenge.Here,a unique strategy to tailor the architecture of composite electrolyte via inserting polymer chains into a small quantity of sulfate sodium grafted C_(48)0H_(28)O_(32)Zr_(6)(UIOSNa)is proposed.The intimate contact between polymer segments and UIOSNa with limited pore size facilitates the anion immobilization of sodium salts and reduction of polymer crystallinity,thereby providing rapid ion conduction and reducing the adverse effect caused by the immigration of anions.The tNa+grafting of-SO_(3)Na groups on fillers allows the free movement of more sodium ions to further improve and ionic conductivity.Consequently,even with the low content of UIOSNa fillers,a high ionic conductivity of 6.62×10^(-4) S·cm^(-1) at 60℃ and a transference number of 0.67 for the special designed composite electrolyte are achieved.The assembled all-solid-state sodium cell exhibits a remarkable rate performance for 500 cycles with 95.96%capacity retention at a high current rate of 4 C.The corresponding pouch cell can stably work for 1000 cycles with 97.03%capacity retention at 1 C,which is superior to most of the reported composite electrolytes in the literature.

关键词： solid state sodium battery composite electrolyte rate performance cycle life

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Enhanced cycling stability and rate performance of Co-doped and La_(2)O_(3)-coated LiNi_(0.9)Mn_(0.1)O_(2) toward power battery

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Rare Metals 2024年第2期43卷 658-670页

作者： Jia-Qi Peng Yuan-Yuan Wei Dong-Ming Liu Yun Li Bin Hu Bin Huang Jian-Wen Yang Shun-Hua Xiao Ren-Heng Wang Guangxi key laboratory of Electrochemical and Magneto-Chemical Functional materials College of Chemistry and BioengineeringGuilin University of TechnologyGuilin541004China key laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen518060China

Ultra-high nickel layered oxide cathode material with high energy density is the most promising material to improve the electrochemical performance of lithium-ion batteries(LIBs).However,the poor structural stability and severe surface/interface side reactions of the material lead to poor rate performance and cyclic stability,which limits its application in practice.In this paper,the dual-modification strategy of Co doping and La_(2)O_(3) coating is used to meet the above challenges.Co doping can effectively widen layer spacing and reduce Li^(+)/Ni^(2+) mixing,and La_(2)O_(3) coating can effectively eliminate the residual alkali on the surface of active material,inhibit the thickening of cathode electrolyte interphase(CEI)film and reduce surface/interface side reactions.Therefore,the modified material(NM90-CL)with excellent electrochemical properties is achieved through the synergistic enhancement of Co doping and La_(2)O_(3) coating.Its capacity retention rate can reach 77.9%after 200 cycles at 1.0℃ and 75.7%after 200 cycles at 5.0℃.Its reversible capacity can up to 153.5 mAh·g^(–1) at 10.0℃.This dual-modification strategy will provide theoretical guidance and technical support for the synthesis of other high-performance electrode materials.

关键词： High nickel cathode material Co doping La_(2)O_(3) coating Electrochemical performance Electrochemical mechanism

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In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

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Journal of Energy Chemistry 2024年第1期88卷 282-292,I0007页

作者： Huanhui Chen Xing Cao Moujie Huang Xiangzhong Ren Yubin Zhao Liang Yu Ya Liu Liubiao Zhong Yejun Qiu shenzhen Engineering Lab of Flexible Transparent Conductive Films School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina Guangdong Provincial key laboratory of Semiconductor Optoelectronic materials and Intelligent Photonic Systems School of Materials Science and EngineeringHarbin Institute of TechnologyShenzhen 518055GuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina School of Resource and Environmental Sciences Wuhan UniversityWuhan 430072HubeiChina

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

关键词： Solid-state lithium batteries Composite solid electrolyte In-situ polymerization Interfacial passivation layer Self-adaptability

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Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities

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Carbon Energy 2024年第1期6卷 1-43页

作者： Munir Ahmad Jiahui Chen Jianwen Liu Yan Zhang Zhongxin Song Shahzad Afzal Waseem Raza Liaqat Zeb Andleeb Mehmood Arshad Hussain Jiujun Zhang Xian-Zhu Fu Jing-Li Luo shenzhen key laboratory of Energy Electrocatalytic materials Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhenGuangdongChina College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhenGuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Environmental Engineering China Jiliang UniversityHangzhouZhejiangChina Institute for Advanced Study Shenzhen UniversityShenzhenGuangdongChina School of Bioengineering Dalian University of TechnologyDalianLiaoningChina College of materials Science and Engineering Fuzhou UniversityFuzhouFujianChina Institute for Sustainable Energy Shanghai UniversityShanghaiChina

Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.

关键词： carbon energy generation MOF-derived-supported MOF-supported single atoms

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Two-dimensional silica enhanced solid polymer electrolyte for lithium metal batteries

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Particuology 2024年第2期85卷 146-154页

作者： Zhihong Luo Weiyong Li Chong Guo Ya Song Mingxia Zhou Yan Shi Jing Xu Long Li Bin Shi Quansheng Ouyang Jiao-jing Shao Guangmin Zhou School of materials and Metallurgy Guizhou UniversityGuiyang550025China State key laboratory of Advanced Chemical Power Sources Zunyi563003China Graphene materials Engineering Research Center of Guizhou Colleges and Universities Guiyang550025China Tsinghua-Berkeley shenzhen Institute&Tsinghua shenzhen International Graduate Schoo Tsinghua UniversityShenzhen518055China

Solid polymer electrolytes(SPEs)are promising substitutes for current flammable liquid electrolytes to achieve high-safety and high-energy-density lithium metal batteries.Polyethylene oxide(PEO)based solid polymer electrolytes have attracted increasing attention because of their excellent flexibility,manufacturability,light weight,and low-cost processing,while they often suffer from low ionic con-ductivity at room temperature,low lithium transference number and unsatisfactory interfacial resis-tance,which largely restrain their practical application.Herein,two-dimensional holey silica nanosheets(2D-HSN)as the fillers,together with LiNO_(3) as the electrolyte additive,are introduced in a PEO/poly(-vinylidene fiuoride-co-hexafluoropropylene)(PVDF-HFP)blended polymer matrix to obtain a SPE.The incorporation of HSN filler creates supplementary channels for lithium ion migration and lowers the crystallinity of the polymer,thereby facilitating the movement of lithium ions.The HSN-based SPE demonstrates higher ionic conductivity up to 3.7 x 10-4 S cm-1 at 30℃,larger Li+transference number close to 0.34,and more stable lithium plating/stripping than that without the fillers,and HSN can promote the formation of more stable solid electrolyte interphase(SEI)layer.The as-assembled LiFePO4||Li batteries deliver a high specific capacity of 159 mA h g-1 with the capacity retention of 95.5%after 200 cycles at 30℃,as well as superior rate performance and cycling stability compared to that using the blank SPE.

关键词： Vermiculite nanosheets Two-dimensional silica Solid polymer electrolytes Fillerslithium metal batteries

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lithium-induced graphene layer containing Li_(3)P alloy phase to achieve ultra-stable electrode interface for lithium metal anode

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Rare Metals 2024年第2期43卷 562-574页

作者： Jia-Xin Chen Guo-Qiang Zhang Xian-Ying Qin Kui Lin Zi-Jin Yang Ge-Meng Liang Yue Xia Guo-Bin Zhang Hai-Kun Wu Qiu-Chan Cai Hai Lin Bao-Hua Li shenzhen key laboratory on Power Battery Safety Research and shenzhen Geim Graphene Center Tsinghua Shenzhen International Graduate SchoolShenzhen518055China shenzhen Graphene Innovation Center Co. Ltd.Shenzhen518107China School of Chemical Engineering and Advanced materials The University of AdelaideAdelaideSA5005Australia Department of Chemistry City University of Hong KongHong Kong990077China

Uncontrolled growth of lithium dendrite will lead to low Coulombic efficiency and poor cycle stability,which hinders the commercialization of lithium metal batteries.Herein,a novel modified lithium anode with reduced graphene oxide conductive network containing trace lithiophilic phosphorus(P-rGO/Cu)is prepared by electrospraying technique combined with heat treatment process.The rGO layer has a concave and undulating conductive structure,which can significantly improve the effective electrical contact between lithium metal and the current collector,speed up the kinetics of interfacial electron transport and reaction,and improve the resistance of the negative electrode to the internal stress caused by volume change of the lithium,which is advantageous for the stability of the SEI film.The extremely small and uniformly distributed red phosphorus element avoids the volume change caused by lithiation to the maximum extent.Lithiophilic two-phase compound Li_(3)P obtained by alloying P with Li can directionally induce the homogeneous nucleation and dense deposition of lithium metal,address the issue of lithium dendrites and extend the cycle life of the batteries.The obtained P-rGO/Cu exhibits excellent electrochemical performance with an average Coulombic efficiency(CE)of 98%at a current density of 1 mA·cm^(−2) for 400 cycles,and the capacity retention rate of the full cell matched with lithium iron phosphate(LFP)is 83%after 400 cycles at 1C.

关键词： lithium anode Dendrite-free Lithiophilicity Induced nucleation deposition

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