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High-Voltage and Fast-Charging Lithium Cobalt Oxide Cathodes: From Key Challenges and Strategies to Future Perspectives

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Engineering 2024年第6期37卷 105-127页

作者： Gongrui Wang Zhihong Bi Anping Zhang Pratteek Das Hu Lin Zhong-Shuai Wu State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China dalian national laboratory for clean energy Chinese Academy of SciencesDalian 116023China

Lithium-ion batteries(LIBs)with the“double-high”characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable ***,the lithium ion(Li+)-storage performance of the most commercialized lithium cobalt oxide(LiCoO_(2),LCO)cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high ***,we systematically summarize and discuss high-voltage and fast-charging LCO cathodes,covering in depth the key fundamental challenges,latest advancements in modification strategies,and future perspectives in this *** and elaborated discussions are first presented on key fundamental challenges related to structural degradation,interfacial instability,the inhomogeneity reactions,and sluggish interfacial *** provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms,categorized into element doping(Li-site,cobalt-/oxygen-site,and multi-site doping)for improved Li+diffusivity and bulkstructure stability;surface coating(dielectrics,ionic/electronic conductors,and their combination)for surface stability and conductivity;nanosizing;combinations of these strategies;and other strategies(i.e.,optimization of the electrolyte,binder,tortuosity of electrodes,charging protocols,and prelithiation methods).Finally,forward-looking perspectives and promising directions are sketched out and insightfully elucidated,providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.

关键词： Lithium cobalt oxide High energy/power density Fast-charging High-voltage Lithium-ion battery

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Hierarchically Structured Nb_(2)O_5 Microflowers with Enhanced Capacity and Fast-Charging Capability for Flexible Planar Sodium Ion Micro-Supercapacitors

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Nano-Micro Letters 2024年第4期16卷 97-109页

作者： Jiaxin Ma Jieqiong Qin Shuanghao Zheng Yinghua Fu Liping Chi Yaguang Li Cong Dong Bin Li Feifei Xing Haodong Shi Zhong‑Shuai Wu State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China College of Science Henan Agricultural UniversityNo.63 Agricultural RoadZhengzhou 450002People’s Republic of China dalian national laboratory for clean energy Chinese Academy of Sciences457 Zhongshan RoadDalian 116023People’s Republic of China University of Chinese Academy of Sciences 19A Yuquan RoadShijingshan DistrictBeijing 100049People’s Republic of China Hebei Key Lab of Optic‑Electronic Information and Materials The College of Physics Science and TechnologyInstitute of Life Science and Green DevelopmentHebei UniversityBaoding 071002People’s Republic of China

Planar Na ion micro-supercapacitors(NIMSCs) that offer both high energy density and power density are deemed to a promising class of miniaturized power sources for wearable and portable microelectron-ics. Nevertheless, the development of NIMSCs are hugely impeded by the low capacity and sluggish Na ion kinetics in the negative ***, we demonstrate a novel carbon-coated Nb_(2)O_5 microflower with a hierarchical structure composed of vertically intercrossed and porous nanosheets, boosting Na ion storage performance. The unique structural merits, including uniform carbon coating, ultrathin nanosheets and abun-dant pores, endow the Nb_(2)O_5 microflower with highly reversible Na ion storage capacity of 245 mAh g^(-1) at 0.25 C and excellent rate *** from high capacity and fast charging of Nb_(2)O_5 microflower, the planar NIMSCs consisted of Nb_(2)O_5 negative electrode and activated car-bon positive electrode deliver high areal energy density of 60.7 μWh cm^(-2),considerable voltage window of 3.5 V and extraordinary cyclability. Therefore, this work exploits a structural design strategy towards electrode materials for application in NIMSCs, holding great promise for flexible microelectronics.

关键词： Nb_(2)O_5 nanosheets Microflowers Sodium ion micro-supercapacitors Flexibility energy storage

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Regulating surface electron structure of PtNi nanoalloy via boron doping for high‐current‐density Li‐O2 batteries with low overpotential and long‐life cyclability

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SmartMat 2024年第1期5卷 110-120页

作者： Yajun Ding Yuanchao Huang Yuejiao Li Tao Zhang Zhong‐Shuai Wu State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina State Key laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang UniversityHangzhouChina Institute of Advanced Semiconductors Hangzhou Innovation CenterZhejiang UniversityHangzhouChina University of Chinese Academy of Sciences BeijingChina State Key laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghaiChina dalian national laboratory for clean energy Chinese Academy of SciencesDalianChina

The realization of high‐efficiency,reversible,stable,and safe Li‐O2 batteries is severely hindered by the large overpotential and side reactions,especially at high rate ***,rational design of cathode catalysts with high activity and stability is crucial to overcome the terrible issues at high current ***,we report a surface engineering strategy to adjust the surface electron structure of boron(B)‐doped PtNi nanoalloy on carbon nanotubes(PtNiB@CNTs)as an efficient bifunctional cathodic catalyst for high‐rate and long‐life Li‐O2 ***,the Li‐O2 batteries assembled with as‐prepared PtNiB@CNT catalyst exhibit ultrahigh discharge capacity of 20510 mA·h/g and extremely low overpotential of 0.48 V at a high current density of 1000 mA/g,both of which outperform the most reported Pt‐based catalysts ***,our Li‐O2 batteries offer excellent rate capability and ultra‐long cycling life of up to 210 cycles at 1000 mA/g under a fixed capacity of 1000 mA·h/g,which is two times longer than those of Pt@CNTs and PtNi@***,it is revealed that surface engineering of PtNi nanoalloy via B doping can efficiently tailor the electron structure of nanoalloy and optimize the adsorption of oxygen species,consequently delivering excellent Li‐O2 battery ***,this strategy of regulating the nanoalloy by doping nonmetallic elements will pave an avenue for the design of high‐performance catalysts for metal‐oxygen batteries.

关键词： B doping bifunctional catalyst Li‐O2 battery low charge overpotential PtNi nanoalloy

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Selective cyclohexane oxidation enhancement by electronic structures regulation of metal-poly(ionic liquid)s

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Green Chemical Engineering 2024年第2期5卷 213-221页

作者： Ying Jin Shengxin Chen Ruirui Wang Yumei Liu Xinxin Li Yingwei Li Ruirui Zhang Ruixia Liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China Beijing Key laboratory of Ionic Liquids clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringInnovation Academy for Green ManufactureCASBeijing100190China

Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in *** this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of *** analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial *** with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil *** interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the ***,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.

关键词： Metal-PILs Cyclohexane oxidation C-H activation Co-N sites

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Towards rational design in electrochemical denitrification by analyzing pH dependence

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national Science Review 2024年第6期11卷 223-232页

作者： Huan Li Dong Luan Jun Long Xiaoyan Fu Jianping Xiao State Key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences

A small fraction of NOx（<1%） always exists in CO2feedstock（e.g. exhausted gas）, which can significantly reduce the efficiency of CO2electroreduction by ～30%. Hence, electrochemical denitrification is the precondition of CO2electroreduction. The pH effect is a key factor, and can be used to tune the selectivity between N2and N2O production in electrochemical denitrification. However, there has been much controversy for many years about the origin of pH dependence in electrocatalysis. To this end, we present a new scheme to accurately model the pH dependence of the electrochemical mechanism. An extremely small pH variation from pH 12.7 to pH 14 can be accurately reproduced for N2O production. More importantly,the obviously different pH dependence of N2production, compared to N2O, can be attributed to a cascade path. In other words, the N2was produced from the secondary conversion of the as-produced N2O molecule（the major product）, instead of the original reactant NO. This is further supported by more than 35 experiments over varying catalysts（Fe, Ni, Pd, Cu, Co, Pt and Ag）, partial pressures（20%, 50% and100%） and potentials（from -0.2 to 0.2 V vs. reversible hydrogen electrode）. All in all, the insights herein overturn long-lasting views in the field of NO electroreduction and suggest that rational design should steer away from catalyst engineering toward reactor optimization.

关键词： electrocatalysis denitrification pH-dependence nitric oxide reduction reaction mechanism

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Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu Beijing Key laboratory of Ionic Liquids clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of *** this work,a strategy of lanthanum manganese mixed metal oxides(LMMO)regulated via a facile ionic liquid(IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of *** 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone)selectivity was achieved over the optimal LMMO catalyst under mild *** effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional *** formation of self-assembled spherical nanoparticles followed the"dissolution-nucleation-proliferation"mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal ***,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and radical trapping *** recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： Ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

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Interfacial assembly of 2D polydopamine/graphene heterostructures with well-defined mesopore and tunable thickness for high-energy planar micro-supercapacitors

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Chinese Chemical Letters 2024年第7期35卷 439-444页

作者： Jieqiong Qin Zhi Yang Jiaxin Ma Liangzhu Zhang Feifei Xing Hongtao Zhang Shuxia Tian Shuanghao Zheng Zhong-Shuai Wu College of Science Henan Agricultural UniversityZhengzhou 450002China State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Mechanical and Electrical Engineering Institute Zhengzhou University of Light IndustryZhengzhou 450002China

Two-dimensional(2D)mesoporous pseudocapacitive polymer/graphene heterostructures combine the advanced merits of 2D materials and mesoporous materials,possessing unique nanosheet structure,large specific surface area(SSA),abundant oxygen/nitrogen-containing groups,desirable electrical conductivity and admirable electrochemical redox activity,and hold great potential for constructing high-performance planar micro-supercapacitors(MSCs).Herein,we demonstrate the interfacial assembly of 2D mesoporous polydopamine/graphene(mPDG)heterostructures with well-defined mesopore structure(12 nm)and adjustable thickness(7.5–14.1 nm)for planar high-energy pseudocapacitive *** to medium thickness,exposed mesopore of 12 nm and large SSA of 108 m^(2)/g,the m PDG with 10.8 nm thickness reveals prominent mass capacitance of 419 F/g and impressive cycling stability with~96%capacitance retention after 5000 ***,the symmetric mPDG-based MSCs with“water-in-salt”gel electrolyte present wide voltage window of 1.6 V,superior volumetric energy density of 11.5 mWh/cm^(3),outstanding flexibility and self-integration ***,this work offers a new platform of controllably synthesizing 2D mesoporous heterostructures for high-performance MSCs.

关键词： 2D materials Mesopores Heterostructures Polydopamine High energy density Micro-supercapacitors

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Recent advances and key perspectives of in-situ studies for oxygen evolution reaction in water electrolysis

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Green energy & Environment 2024年第10期9卷 1497-1517页

作者： Yi Wang Zichen Xu Xianhong Wu Zhong-Shuai Wu State Key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Shijingshan District dalian national laboratory for clean energy Chinese Academy of Sciences

Electricity-driven water splitting to produce hydrogen is one of the most efficient ways to alleviate energy crisis and environmental pollution problems, in which the anodic oxygen evolution reaction(OER) is the key half-reaction of performance-limiting in water splitting. Given the complicated reaction process and surface reconstruction of the involved catalysts under actual working conditions, unraveling the real active sites, probing multiple reaction intermediates and clarifying catalytic pathways through in-situ characterization techniques and theoretical calculations are essential. In this review, we summarize the recent advancements in understanding the catalytic process, unlocking the water oxidation active phase and elucidating catalytic mechanism of water oxidation by various in-situ characterization techniques. Firstly, we introduce conventionally proposed traditional catalytic mechanisms and novel evolutionary mechanisms of OER, and highlight the significance of optimal catalytic pathways and intrinsic stability. Next, we provide a comprehensive overview of the fundamental working principles,different detection modes, applicable scenarios, and limitations associated with the in-situ characterization techniques. Further, we exemplified the in-situ studies and discussed phase transition detection, visualization of speciation evolution, electronic structure tracking, observation of reaction active intermediates, and monitoring of catalytic products, as well as establishing catalytic structure–activity relationships and catalytic mechanism. Finally, the key challenges and future perspectives for demystifying the water oxidation process are briefly proposed.

关键词： In-situ studies Water splitting Oxygen evolution reaction Catalytic mechanism

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Biomass-based production of trimellitic and trimesic acids

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Green energy & Environment 2024年第8期9卷 1267-1278页

作者： Lin Yuan Yancheng Hu Guangyi Li Fengan Han Aiqin Wang Yu Cong Tao Zhang Feng Wang Ning Li CAS Key laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences University of Chinese Academy of Sciences 19 A Yuquan RoadShijingshan District School of Chemical Engineering and Technology China University of Mining and Technology State Key laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences

The production of industrial chemicals with renewable biomass feedstock holds potential to aid the world in pursuing a carbon-neutral *** and trimesic acids are important commodity chemicals in industry that are prepared by the oxidation of petroleum-derived *** reduce the dependence on the limited oil source,we develop a potential sustainable alternative towards trimellitic and trimesic acids using biomass-based 2-methyl-2,4-pentandiol （MPD）,acrylate and crotonaldehyde as starting *** process for trimellitic acid includes dehydration/D-A reaction of MPD and acrylate,flow aromatization over Pd/C catalyst,hydrolysis and catalytic aerobic oxidation （60%overall yield）.The challenging regioselectivity issue of D-A reaction is tackled by a matched combination of temperature and deep eutectic solvent ChCl/*** can also participate in the reaction,followed by Pd/C-catalyzed decarbonylation/dehydrogenation and oxidation to provide trimesic acid in 54%overall *** cycle assessment implies that compared to conventional fossil process,our biomass-based routes present a potential in reducing carbon emissions.

关键词： Biomass Trimellitic acid Trimesic acid Deep eutectic solvent Dehydration/D-A reaction

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Hybrid ion/electron interfacial regulation stabilizes the cobalt/oxygen redox of ultrahigh-voltage lithium cobalt oxide for fast-charging cyclability

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Science Bulletin 2024年第13期69卷 2071-2079页

作者： Zhihong Bi Anping Zhang Gongrui Wang Cong Dong Pratteek Das Xiaoyu Shi Zhong-Shuai Wu State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China dalian national laboratory of clean energy Chinese Academy of SciencesDalian 116023China

High-voltage and fast-charging LiCoO_(2)(LCO)is key to high-energy/power-density Li-ion ***,unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging ***,we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling ***,the resulting artificial hybrid conductive network enhances the reversible conversion of Co^(3+)/^(4+)/O_(2)/nredox by the interfacial ion–electron cooperation and suppresses interface side reactions,inducing an ultrathin yet compact cathode electrolyte ***,the derived near-surface Na+/Mg2+/Si^(4+)-pillared local intercalation structure greatly promotes the Li^(+)diffusion around the 4.55 V phase transition and stabilizes the cathode ***,excellent 3 C(1 C=274 mA g1)fast charging performance is demonstrated with 73.8%capacity retention over 1000 *** findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.

关键词： High-voltage Fast-charging LiCoO_(2) Interfacial ion-electron cooperation Local intercalation

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