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

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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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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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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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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Three‐dimensional(3D)‐printed MXene high‐voltage aqueous micro‐supercapacitors with ultrahigh areal energy density and low‐temperature tolerance

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Carbon Energy 2024年第8期6卷 36-48页

作者： Yuanyuan Zhu Qingxiao Zhang Jiaxin Ma Pratteek Das Liangzhu Zhang Hanqing Liu Sen Wang Hui Li zhong‐shuai wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhouChina Shanghai Key Laboratory of Rare Earth Functional Materials and Education Ministry Key Laboratory of Resource Chemistry Shanghai Normal UniversityShanghaiChina University of Chinese Academy of Sciences BeijingChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalianChina

The rapid advancement in the miniaturization,integration,and intelligence of electronic devices has escalated the demand for customizable microsupercapacitors(MSCs)with high energy ***,efficient microfabrication of safe and high‐energy MXene MSCs for integrating microelectronics remains a significant challenge due to the low voltage window in aqueous electrolytes(typically≤0.6 V)and limited areal mass loading of MXene ***,we tackle these challenges by developing a highconcentration(18mol kg^(−1))“water‐in‐LiBr”(WiB)gel electrolyte for MXene symmetric MSCs(M‐SMSCs),demonstrating a record high voltage window of 1.8 ***,additive‐free aqueous MXene ink with excellent rheological behavior is developed for three‐dimensional(3D)printing customizable all‐MXene microelectrodes on various *** the synergy of a highvoltage WiB gel electrolyte and 3D‐printed microelectrodes,quasi‐solid‐state MSMSCs operating stably at 1.8 V are constructed,and achieve an ultrahigh areal energy density of 1772μWhcm^(−2)and excellent low‐temperature tolerance,with a long‐term operation at−40℃.Finally,by extending the 3D printing protocol,M‐SMSCs are integrated with humidity sensors on a single planar substrate,demonstrating their reliability in miniaturized integrated microsystems.

关键词： 3D printing aqueous electrolyte high voltage micro‐supercapacitors MXene

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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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2.4 V ultrahigh-voltage aqueous MXene-based asymmetric micro-supercapacitors with high volumetric energy density toward a self-sufficient integrated microsystem

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Fundamental Research 2024年第2期4卷 307-314页

作者： Yuanyuan Zhu Shuanghao Zheng Jieqiong Qin Jiaxin Ma Pratteek Das Feng Zhou zhong-shuai wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China College of Science Henan Agricultural UniversityZhengzhou 450002China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China Key Laboratory of Spin Electron and Nanomaterials of Anhui Higher Education Institutes Suzhou UniversitySuzhou 234000China

Two-dimensional MXenes are key high-capacitance electrode materials for micro-supercapacitors(MSCs)catering to integrated ***,the narrow electrochemical voltage windows of conventional aqueous electrolytes(≤1.23 V)and symmetric MXene MSCs(typically≤0.6 V)substantially limit their output voltage and energy *** concentrated aqueous electrolytes exhibit lower water molecule activity,which inhibits water splitting and consequently widens the operating voltage ***,we report ultrahigh-voltage aqueous planar asymmetric MSCs(AMSCs)based on a highly concentrated LiCl-gel quasi-solid-state electrolyte with MXene(Ti3C2Tx)as the negative electrode and MnO_(2) nanosheets as the positive electrode(MXene//MnO_(2)-AMSCs).The MXene//MnO_(2)-AMSCs exhibit a high voltage of up to 2.4 V,attaining an ultrahigh volumetric energy density of 53 mWh cm−***,the in-plane geometry and the quasi-solid-state electrolyte enabled excellent mechanical flexibility and performance uniformity in the serially/parallel connected packs of our ***,the MXene//MnO_(2)-AMSC-based integrated microsystem,in conjunction with solar cells and consumer electronics,could efficiently realize simultaneous energy harvesting,storage,and *** findings of this study provide insights for constructing high-voltage aqueous MXene-based AMSCs as safe and self-sufficient micropower sources in smart integrated microsystems.

关键词： Asymmetric micro-supercapacitors MXene MnO_(2) Aqueous electrolyte High voltage Integrated microsystem

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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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高能量密度的微型储能器件的展望

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Science Bulletin 2024年第6期69卷 714-717页

作者：王森 Pratteek Das 吴忠帅 State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

The pursuit for Internet of Things(IoT)-enabled microelectronic devices has taken the scientific community by storm,and to power them,microscale electrochemical energy storage devices(MESDs),including microsupercapacitors(MSCs)and microbatteries(MBs)are considered ideal on-chip power sources[1].This is not surprising,given the inherent advantages of MESDs like facile microfabrication with an ultra-compact footprint,easy achievement of high areal capacity,and compatible integration with various functional microelectronic devices while providing smaller current drains.

关键词：高能量密度 pursuit drain

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A perspective on graphene for supercapacitors: Current status and future challenges

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Journal of Energy Chemistry 2021年第2期30卷 354-357,I0012页

作者： Feng Su zhong-shuai wu Dalian National Laboratory for Clean Energy.Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Supercapacitors,also known as ultracapacitors or electrochemical capacitors,possess intriguing merits of high power density(10-100 times higher than that of batteries),long life expectancy(millions of cycles),wide ope... 详细信息

关键词： Graphene Supercapacitors Energy storage Electric double layer capacitors Pseudocapacitors Hybrid supercapacitors

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