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Deciphering the oxygen Absorption Pre-edge: A Caveat on its Application for Probing oxygen redox Reactions in Batteries

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Energy & Environmental Materials 2021年第2期4卷 246-254页

作者： Subhayan Roychoudhury Ruimin Qiao Zengqing Zhuo Qinghao Li Yingchun Lyu Jung-Hyun Kim Jun Liu Eungje Lee Bryant J.Polzin Jinghua Guo Shishen Yan Yongsheng Hu Hong Li David Prendergast Wanli Yang Advanced Light Source Lawrence Berkeley National Laboratory1 Cyclotron RoadBerkeley CA 94720USA School of Advanced Materials Shenzhen Graduate SchoolPeking UniversityShenzhen 518055China School of Physics National Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Mechanical and Aerospace Engineering The Ohio State UniversityColumbus OH 43210USA R&D department 2M LLC193 Thompson DrHockessin DE 19707USA Chemical Science and Engineering Division Argonne National LaboratoryArgonne IL 60439 USA The Molecular Foundry Lawrence Berkeley National Laboratory1 Cyclotron Road Berkeley CA 94720 USA

The pre-edges of oxygen-K X-ray absorption spectra have been ubiquitous in transition metal(TM)oxide studies in various fields,especially on the fervent topic of oxygen redox states in battery ***,critical debates remain on the use of the O-K pre-edge variations upon electrochemical cycling as evidences of oxygen redox reactions,which has been a popular practice in the battery *** study presents an investigation of the O-K pre-edge of 55 oxides covering all 3d TMs with different elements,structures,and electrochemical states through combined experimental and theoretical *** is shown unambiguously that the O-K pre-edge variation in battery cathodes is dominated by changing TM-d ***,the pre-edge enables a unique opportunity to project the lowest unoccupied TM-d states onto one common energy window,leading to a summary map of the relative energy positions of the low-lying TM states,with higher TM oxidation states at lower energies,corresponding to higher electrochemical *** results naturally clarify some unusual redox reactions,such as Cr^(3+/6+).This work provides a critical clarification on O-K pre-edge interpretation and more importantly a benchmark database of O-K pre-edge for characterizing redox reactions in batteries and other energy materials.

关键词： battery oxygen redox x-ray absorption spectroscopy cathode material redox reaction

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Cationic ordering transition in oxygen-redox layered oxide cathodes

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Carbon Energy 2024年第1期6卷 197-206页

作者： Xinyan Li Ang Gao Qinghua Zhang Hao Yu Pengxiang Ji Dongdong Xiao Xuefeng Wang Dong Su Xiaohui Rong Xiqian Yu Hong Li Yong-Sheng Hu Lin Gu Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijingChina College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijingChina Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials School of Materials Science and EngineeringTsinghua UniversityBeijingChina Beijing Advanced Innovation Center for Materials Genome Engineering Huairou DivisionInstitute of PhysicsChinese Academy of SciencesBeijingChina

Understanding the structural origin of the competition between oxygen 2p and transition-metal 3d orbitals in oxygen-redox(OR)layered oxides is eminently desirable for exploring reversible and high-energy-density Li/Na-ion ***,we reveal the correlation between cationic ordering transition and OR degradation in ribbon-ordered P3-Na_(0.6)Li_(0.2)Mn_(0.8)O_(2) via in situ structural *** two different voltage windows,the OR capacity can be improved approximately twofold when suppressing the in-plane cationic ordering *** find that the intralayer cationic migration is promoted by electrochemical reduction from Mn^(4+)to Jahn–Teller Mn^(3+)and the concomitant NaO_(6) stacking transformation from triangular prisms to octahedra,resulting in the loss of ribbon ordering and electrochemical ***-principles calculations reveal that Mn^(4+)/Mn^(3+)charge ordering and alignment of the degenerate eg orbital induce lattice-level collective Jahn–Teller distortion,which favors intralayer Mn-ion migration and thereby accelerates OR *** findings unravel the relationship between in-plane cationic ordering and OR reversibility and highlight the importance of superstructure protection for the rational design of reversible OR-active layered oxide cathodes.

关键词： cationic ordering layered oxide cathodes oxygen redox sodium-ion batteries

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Suppress oxygen evolution of lithium-rich manganese-based cathode materials via an integrated strategy

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Green Energy & Environment 2024年第1期9卷 138-151页

作者： Wenhua Yu Yanyan Wang Aimin Wu Aikui Li Zhiwen Qiu Xufeng Dong Chuang Dong Hao Huang Key Laboratory of Energy Materials and Devices(Liaoning Province) School of Materials Science and EngineeringDalian University of TechnologyDalian116024Liaoning ProvinceChina Dalian Engineering Research Center for New Electric Power Systerms School of Electrical EngineeringDalian University of TechnologyDalian116024Liaoning ProvinceChina

Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO_(2) surface coating is *** doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond ***_(2) nanocoating has the function of structural constraint and protection,that protecting the lattice oxygen exposed to the surface,thus avoiding irreversible *** an Li^(+) conductor,LiYO_(2) nano-coating can provide a fast Li^(+) transfer channel,which enables the sample to have excellent rate *** synergistic effect of Y doping and nano-LiYO_(2) coating integration suppresses the oxygen release from the surface,accelerates the diffusion of Li^(+)from electrolyte to electrode and decreases the interfacial side reactions,enabling the lithium ion batteries to obtain good electrochemical *** lithium-ion full cell employing the Y-1 sample(cathode)and commercial graphite(anode)exhibit an excellent specific energy density of 442.9 Wh kg^(-1) at a current density of 0.1C,with very stable safety performance,which can be used in a wide temperature range(60 to-15℃)stable *** result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.

关键词： Lithium-rich manganese-based cathodes Lithium ion batteries oxygen redox oxygen evolution Integrated strategy

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A Perspective on Studying Electronic Structure of Batteries through Soft X-ray Spectroscopy

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Chinese Journal of Structural Chemistry 2019年第12期38卷 2009-2014页

作者： ZHUO Zeng-Qing PAN Feng YANG Wan-Li School of Advanced Materials Peking UniversityShenzhen Graduate SchoolShenzhen 518055China Advanced Light Source Lawrence Berkeley National Laboratory1 Cyclotron RoadBerkeley CA 94720United States

Understanding electronic structure is crucial to enhance the battery performance. Soft X-ray spectroscopy(SXS) is one of the most effective methods to provide direct probe of electronic states. Here, spectroscopic measurements of transition metal 3 d and oxygen 2 p states are simply reviewed. Then, we mainly focus on the perspective of the development direction of modern SXS techniques. Although the true power of recently developed high efficiency mapping of resonant inelastic X-ray scattering(m RIXS) has been apparent for materials and chemistry studies, great challenges remain for mRIXS spectroscopic interpretation, and the understanding of the battery materials on novel redox activities remains elusive.

关键词： electronic structure soft X-ray spectroscopy oxygen redox O-K mRIXS

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Empowering higher energy sodium-ion battery cathode by oxygen chemistry

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Interdisciplinary Materials 2023年第3期2卷 416-422页

作者： Guangying Wan Wendi Dou Hanye Zhu Wu Zhang Tiefeng Liu Liguang Wang Jun Lu College of Materials Science and Engineering Zhejiang University of TechnologyHangzhouChina College of Civil Engineering and Architecture Zhejiang UniversityHangzhouChina College of Chemical and Biological Engineering Zhejiang UniversityHangzhouChina

Sodium(Na)ion batteries(SIBs)promise low-cost energy storage systems but are still restricted by insufficient energy *** oxygen(O)redox into the design of the Na-storage cathode is presently considered an effective avenue to generate extra capacity in solving the energy density *** succeeding issues are how to overcome the irreversible electrochemical behavior accompanied by O ***,the O redox chemistry and subsequent structural evolution remain ambiguous so ***,we deliberate on the O redox mechanism in Na-storage transition metal *** associated with the reaction irreversibility and structural collapse are summarized by virtue of the advanced characterization *** that,strategies that potentially enhance the electrochemical properties of O redox and future research perspectives on exploring useable O redox cathode materials are outlined.

关键词： anionic redox layered transition metal oxides oxygen redox sodium-ion batteries

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