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Laminar Composite Solid Electrolyte with Poly(Ethylene Oxide)-Threaded Metal-Organic Framework Nanosheets for High-Performance All-Solid-State Lithium Battery

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Energy & Environmental Materials 2023年第1期6卷 264-273页

作者： Na Peng Weijie Kou Wenjia Wu Shiyuan Guo Yan Wang Jingtao Wang School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450003China

Developing laminar composite solid electrolyte with ultrathin thickness and continuous conduction channels in vertical direction holds great promise for all-solid-state lithium batteries.Herein,a thin,laminar solid electrolyte is synthesized by filtrating–NH 2 functionalized metal-organic framework nanosheets and then being threaded with poly(ethylene oxide)chains induced by the hydrogen-bonding interaction from–NH_(2) groups.It is demonstrated that the threaded poly(ethylene oxide)chains lock the adjacent metal-organic framework nanosheets,giving highly enhanced structural stability(Young’s modulus,1.3 GPa)to 7.5-μm-thick laminar composite solid electrolyte.Importantly,these poly(ethylene oxide)chains with stretching structure serve as continuous conduction pathways along the chains in pores.It makes the non-conduction laminar metal-organic framework electrolyte highly conductive:3.97×10^(−5) S cm^(−1) at 25℃,which is even over 25 times higher than that of pure poly(ethylene oxide)electrolyte.The assembled lithium cell,thus,acquires superior cycling stability,initial discharge capacity(148 mAh g^(−1) at 0.5 C and 60℃),and retention(94% after 150 cycles).Besides,the pore size of nanosheet is tailored(24.5–40.9˚A)to evaluate the mechanisms of chain conformation and ion transport in confined space.It shows that the confined pore only with proper size could facilitate the stretching of poly(ethylene oxide)chains,and meanwhile inhibit their disorder degree.Specifically,the pore size of 33.8˚A shows optimized confinement effect with trans-poly(ethylene oxide)and cis-poly(ethylene oxide)conformation,which offers great significance in ion conduction.Our design of poly(ethylene oxide)-threaded architecture provides a platform and paves a way to the rational design of next-generation high-performance porous electrolytes.

关键词： all-solid-state lithium battery ion conduction laminar composite solid electrolyte poly(ethylene oxide)-threaded metal-organic framework nanosheet structural stability

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Molecular dynamics simulations of ovalbumin adsorption at squalene/water interface

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Chinese Journal of Chemical Engineering 2022年第10期50卷 369-378页

作者： Qingxia Xiong Ying Ren Yufei Xia Guanghui Ma Reiji Noda Wei Ge State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Division of Environmental Engineering Science Graduate School of Science and TechnologyGunma University1-5-1 Tenjin-choKiryuGunma 376-8515Japan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China

The adsorption of protein molecules to oil/water(O/W)interface is of critical importance for the product design in a wide range of technologies and industries such as biotechnology,food industry and pharmaceutical industry.In this work,with ovalbumin(OVA)as the model protein,the adsorption conformations at the O/W interface and the adsorption stability have been systematically studied via multiple simulation methods,including all-atom molecular dynamic(AAMD)simulations,coarse-grained molecular dynamic(CGMD)simulations and enhanced sampling methods.The computational results of AAMD and CGMD show that the hydrophobic tail of OVA tends to be folded under long time relaxation in aqueous phase,and multiple adsorption conformations can exist at the interface due to heterogeneous interactions raising from oil and water respectively.To further study the adsorption sites of the protein,the adsorption kinetics of OVA at the O/W interface is simulated using metadynamics method combined with CGMD simulations,and the result suggests the existence of multiple adsorption conformations of OVA at interface with the head-on conformation as the most stable one.In all,this work focuses on the adsorption behaviors of OVA at squalene/water interface,and provides a theoretical basis for further functionalization of the proteins in emulsion-based products and engineering.

关键词： Molecular dynamicssimulation Metadynamics Protein adsorption structural stability Ovalbumin

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Improving the stability,lithium diffusion dynamics,and specific capacity of SrLi_(2)Ti_(6)O_(14)via ZrO_(2)coating

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Green Energy & Environment 2022年第1期7卷 53-65页

作者： Hong-Li Ding Hai-Tao Yu Xiao-dong Wang Chen-Feng Guo Bing Zheng Ying Xie Ting-Feng Yi Key Laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin150080China College of Material Science and Chemical Engineering Harbin Engineering UniversityHarbin150001China School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdao066004China Institute of Advanced Electrochemical Energy&School of Materials Science and Engineering Xi'an University of TechnologyXi'anShaanxi710048China

SrLi_(2)Ti_(6)O_(14)(SLTO)coated with different amount of ZrO_(2)was successfully prepared.The as-obtained composites are stacked by a series of particles with a pure phase structure and a good crystallinity.Furthermore,ZrO_(2)coating not only enhances the structural stability of the materials but also facilitates the diffusion of lithium through the SEI film.As a result,the redox polarization was reduced,and the reversibility of the electrochemical reaction was enhanced.Particularly,SLTO-ZrO_(2)-2 sample delivers a high initial lithiation capacity of 283.6 mA h g^(-1),and the values maintain at 251.7,228.0,207.4,175.3,and 147.7 mA h g^(-1)at the current densities of 0.13,0.26,0.54,1.31,and 2.62 A g^(-1),respectively.Our experiment also confirmed that SLTO materials coated with ZrO_(2)are suitable for high power density applications,and the lithiation specific energy efficiency of SLTO-ZrO_(2)-2 is 200%as high as that of pure SLTO at a power density of 1257 W kg^(-1).

关键词： SrLi_(2)Ti_(6)O_(14) ZrO_(2)coating structural stability Anode material Electrochemical performance

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Unexpected Li displacement and suppressed phase transition enabling highly stabilized oxygen redox in P3-type Na layered oxide cathode

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Journal of Energy Chemistry 2023年第10期85卷 144-153,I0006页

作者： Myungeun Choi Hobin Ahn Hyunyoung Park Yongseok Lee Jinho Ahn Bonyoung Ku Junseong Kim Wonseok Ko Jungmin Kang Jung-Keun Yoo Duho Kim Jongsoon Kim Department of Energy Science Sungkyunkwan UniversitySuwon 16419Republic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwon 16419Republic of Korea Carbon Composites Department Korea Institute of Materials Science(KIMS)Changwon 51508Republic of Korea Department of Mechanical Engineering(Integrated Engineering Program) Kyung Hee University1732Deogyeong-daeroGiheung-guYongin-siGyeonggi-do 17104Republic of Korea Department of KHU-KIST Convergence Science and Technology Kyung Hee University23Kyunghee-daero Dongdaemun-guSeoul 02447Republic of Korea

Oxygen redox is considered a new paradigm for increasing the practical capacity and energy density of the layered oxide cathodes for Na-ion batteries. However, severe local structural changes and phase transitions during anionic redox reactions lead to poor electrochemical performance with sluggish kinetics.Here, we propose a synergy of Li-Cu cations in harnessing the full potential of oxygen redox, through Li displacement and suppressed phase transition in P3-type layered oxide cathode. P3-type Na_(0.7)[Li_(0.1)Cu_(0.2)Mn_(0.7)]O_(2) cathode delivers a large specific capacity of ~212 mA h g^(-1)at 15 mA g^(-1). The discharge capacity is maintained up to ~90% of the initial capacity after 100 cycles, with stable occurrence of the oxygen redox in the high-voltage region. Through advanced experimental analyses and first-principles calculations, it is confirmed that a stepwise redox reaction based on Cu and O ions occurs for the charge-compensation mechanism upon charging. Based on a concrete understanding of the reaction mechanism, the Li displacement by the synergy of Li-Cu cations plays a crucial role in suppressing the structural change of the P3-type layered material under the oxygen redox reaction, and it is expected to be an effective strategy for stabilizing the oxygen redox in the layered oxides of Na-ion batteries.

关键词： Layered oxide cathode Oxygen redox reaction structural stability Li displacement No phase transition

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Constructing the bonding between conductive agents and active materials/binders stabilizes silicon anode in Lithium-ion batteries

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Journal of Energy Chemistry 2023年第5期80卷 23-31,I0002页

作者： Jie Tang Jiawang Zhou Xingyu Duan Yujie Yang Xinyi Dai Fuzhong Wu Guizhou High-level Institution Key Laboratory of High-Performance Battery Materials Guizhou UniversityGuiyang 550025GuizhouChina

Silicon(Si)anode has been considered a promising candidate due to its remarkable theoretical capacity but it was plagued by severe pulverization because of the inherent huge volume variation.Enhancing electrode stability is an effective approach to improve electrochemical performance.Herein,a stable Si anode was established by an innovative construction of the bonding between conductive agents and active materials/binders.As a result,the strong interaction of electrode components not only effectively alleviates the volume expansion of Si but also achieves a stable interface by generating the beneficial solid electrolyte interphase(SEI)composition.Attributed to the deliberate scheme of the electrode,the Si anode exhibits sterling electrochemical performance.Besides,the device of the electrode is not only effective for other binders but also for other anode materials with high volume variation,thus shedding light on the rational design of electrodes for high-energy-density lithium-ion batteries.

关键词： Lithium-ion batteries Si MXene SEI structural stability

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Tuning Li-excess to optimize Ni/Li exchange and improve stability of structure in LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cathode material for lithium-ion batteries

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Nano Research 2022年第10期15卷 8962-8971页

作者： Fangya Guo Yongfan Xie Youxiang Zhang College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China

Ni/Li exchange is a detrimental effect on electrochemical performances for high-Ni cathode materials(LiNi_(x)Co_(y)Mn_(z)O_(2),x≥0.6).Adjusting Li-excess degree has been proved to be an effective way to optimize Ni/Li exchange in the materials.However,until now,how the Ni/Li exchange and thus the structural properties is affected by the Li-excess has not been understood and clearly elucidated in the literature.Herein,a feasible strategy is utilized to optimize Ni/Li exchange and the amount of anti-Li^(+)in LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) by mixing Ni_(0.8)Co_(0.1)Mn_(0.1)(OH)_(2) precursor with different amounts of lithium sources during lithiation.It was found that morphology and phase stability of the material can be tuned with moderate excessive lithium.With 10%Li-excess,LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) exhibits an initial discharge capacity of 211.5 mAh·g^(–1) at 0.1 C and maintains 93.3%of its initial capacity after 100 cycles at 1 C.Different technologies were used to characterize the materials and it shows that the formation of broader Li slab space,decreased anti-Ni^(2+)in Li layer,and gradient distribution of Ni3+in the surface is contributed to moderate Li-excess in the materials.Broader Li slab space facilitates diffusion of Li^(+),decreased antisite-Ni^(2+)and gradient distribution of Ni3+in materials surfaces optimizes the Ni/Li exchange.Based on these results,we thus believe that it is the moderate Li-excess in material that optimized the electrochemical performance of high-Ni cathode materials.

关键词： Ni-rich cathodes Ni/Li exchange Li-excess structural stability cycling stability

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Stabilizing effects of atomic Ti doping on high-voltage high-nickel layered oxide cathode for lithium-ion rechargeable batteries

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Nano Research 2022年第5期15卷 4091-4099页

作者： Yong Cheng Yan Sun Changting Chu Limin Chang Zhaomin Wang Dongyu Zhang Wanqiang Liu Zechao Zhuang Limin Wang Key Laboratory of Preparation and Applications of Environmental Friendly Materials(Ministry of Education) Jilin Normal UniversityChangchun 130103China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of materials science and engineering Changchun University of Science and TechnologyChangchun 130022China Department of Chemistry Tsinghua UniversityBeijing 100084China

High-voltage high-nickel lithium layered oxide cathodes show great application prospects to meet the ever-increasing demand for further improvement of the energy density of rechargeable lithium-ion batteries(LIBs)mainly due to their high output capacity.However,severe bulk structural degradation and undesired electrode-electrolyte interface reactions seriously endanger the cycle life and safety of the battery.Here,2 mol%Ti atom is used as modified material doping into LiNi_(0.8)Co_(0.2)Mn_(0.2O2)(NCM)to reform LiNi_(0.6)Co_(0.2)Mn_(0.18)Ti_(0.02)O_(2)(NCM-Ti)and address the long-standing inherent problem.At a high cut-off voltage of 4.5 V,NCM-Ti delivers a higher capacity retention ratio(91.8%vs.82.9%)after 150 cycles and a superior rate capacity(118 vs.105 mAh·g^(-1))at the high current density of 10 C than the pristine NCM.The designed high-voltage full battery with graphite as anode and NCM-Ti as cathode also exhibits high energy density(240 Wh·kg^(-1))and excellent electrochemical performance.The superior electrochemical behavior can be attributed to the improved stability of the bulk structure and the electrode-electrolyte interface owing to the strong Ti-O bond and no unpaired electrons.The in-situ X-ray diffraction analysis demonstrates that Ti-doping inhibits the undesired H2-H3 phase transition,minimizing the mechanical degradation.The ex-situ TEM and X-ray photoelectron spectroscopy reveal that Ti-doping suppresses the release of interfacial oxygen,reducing undesired interfacial reactions.This work provides a valuable strategic guideline for the application of high-voltage high-nickel cathodes in LIBs.

关键词： lithium-ion battery high-voltage high-nickel cathode Ti-doping structural stability interface stability

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Complementary two-phase anode improving stability and conductivity for lithium storage performance

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Rare Metals 2023年第1期42卷 85-99页

作者： Xue-Fang Xie Guo-Zhao Fang Ying-Zhu Hu Xin-Xin Cao Ting Zhu An-Qiang Pan School of Materials Science&Engineering Central South UniversityChangsha410083China

Metal chalcogenides with multiple lithium ions storage capability have received extensive attentions in recent years;however,their practical application is restricted by the structural instability and poor reversibility.Herein,a unique structure of N and S co-doped C/TiO_(2)nanofibers is reported to support SnS nanosheets for fast and ultra-stable lithium storage.The incorporation of TiO_(2)can notably suppress the excessive uncontrollable growth of SnS and improve the structural stability of the electrode material.The effects of the ratios between Ti and Sn and the corresponding synthesis temperatures on the structure and electrochemical properties of the electrodes have been systematically studied.The interface charge transfer behavior of SnS and TiO_(2)composite heterostructure was clarified by density functional theory(DFT)calculation.The electronic interaction SnS and TiO_(2)can effectively reduce the energy band gap and form a built-in electric field at the interface of the two phases.This is beneficial for the adsorption of lithium ion and consequently accelerate the reaction kinetics of the electrode material.After the two phases are combined,the agglomeration of SnS is effectively suppressed,and the overall conductivity of the composite is greatly improved.Furthermore,the synergistic effect induced by SnS and TiO_(2)enables the good stability of the electrode in both lithium-ion half-cells and full cells.This work can provide new insights toward improving the performance of alloy-type anodes.

关键词： SnS TiO_(2) structural stability Battery

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Improvement of multi-functional properties by fabricating micro-pillar arrays structures on zirconium alloy surface

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Science China(Technological Sciences) 2022年第6期65卷 1243-1252页

作者： WANG XiaoLiang WANG HaoYu LIU YongDa QI Min REN QuanYao XU Jie SHAN DeBin GUO Bin Key Laboratory of Micro-systems and Micro-structures Manufacturing of Ministry of Education Harbin Institute of TechnologyHarbin 150080China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001China Science and Technology on Reactor System Design Technology Laboratory Chengdu 610041China

Although using the microstructure of a surface to enhance specific functions has immense applicability in numerous fields,few studies have been conducted on the multi-functional properties of nuclear fuel elements in harsh environments.In this study,surfaces with zirconium alloy micro-pillar arrays were prepared using micro-milling and ultraviolet nanosecond laser technology,and their functional properties such as the wettability,structural stability,and corrosion resistance were investigated.It was found that the geometric dimension of the micro-pillar arrays prepared using these two methods could meet the design requirements,but the micro-milling process had the best dimensional accuracy.Micro-nano multi-scale structures were obtained by laser ablation.However,these multi-scale structures exhibited weak structural stability,and the nanostructures were easily corroded.By contrast,the micro-pillar arrays manufactured using micro-milling were confirmed to have better structural stability and corrosion resistance.On one hand,the area mass loss of the micro-milled structure was lower than that of a flat surface after experiencing high-pressure fluid scouring at 8 and 38 m/s.On the other hand,the oxidation weight gain of the surface with the micro-milled structure was lower than that of a flat surface,and the oxide film was 22.5% thinner after 100 days of deionized water corrosion at 360℃ and 18.7 MPa.

关键词： zirconium alloy micro-pillar arrays wettability structural stability corrosion

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Surface Doping vs.Bulk Doping of Cathode Materials for Lithium-Ion Batteries:A Review

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Electrochemical Energy Reviews 2022年第4期5卷 254-285页

作者： Huaming Qian Haoqi Ren Ying Zhang Xianfeng He Wenbin Li Jingjing Wang Junhua Hu Hong Yang Hirbod Maleki Kheimeh Sari Yu Chen Xifei Li Xi’an Key Laboratory of New Energy Materials and Devices Institute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi’an University of TechnologyXi’an 710048ShaanxiChina Shaanxi International Joint Research Center of Surface Technology for Energy Storage Materials Xi’an 710048ShaanxiChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntario N6A 5B9Canada State Center for International Cooperation On Designer Low‑Carbon and Environmental Materials(CDLCEM) Zhengzhou University100 Kexue AvenueZhengzhou 450001China Xi’an Safty Energy Technology Co. LtdXi’an 710005ShaanxiChina

To address the capacity degradation,voltage fading,structural instability and adverse interface reactions in cathode materi-als of lithium-ion batteries(LIBs),numerous modification strategies have been developed,mainly including coating and doping.In particular,the important strategy of doping(surface doping and bulk doping)has been considered an effective strategy to modulate the crystal lattice structure of cathode materials.However,special insights into the mechanisms and effectiveness of the doping strategy,especially comparisons between surface doping and bulk doping in cathode materials,are still lacking.In this review,recent significant progress in surface doping and bulk doping strategies is demonstrated in detail by focusing on their inherent differences as well as effects on the structural stability,lithium-ion(Li-ion)diffusion and electrochemical properties of cathode materials from the following mechanistic insights:preventing the exposure of reactive Ni on the surface,stabilizing the Li slabs,mitigating the migration of transition metal(TM)ions,alleviating unde-sired structural transformations and adverse interface issues,enlarging the Li interslab spacing,forming three-dimensional(3D)Li-ion diffusion channels,and providing more active sites for the charge-transfer process.Moreover,insights into the correlation between the mechanisms of hybrid surface engineering strategies(doping and coating)and their influences on the electrochemical performance of cathode materials are provided by emphasizing the stabilization of the Li slabs,the enhancement of the surface chemical stability,and the alleviation of TM ion migration.Furthermore,the existing challenges and future perspectives in this promising field are indicated.

关键词： Lithium-ion batteries Cathode materials Surface doping Bulk doping Hybrid surface engineering structural stability Lithium-ion diffusion

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