The relationship between charge and structure dictates the properties of electrochemical systems. For example, reversible Na-ion intercalation - a low-cost alternative to Li-ion technology - often induces detrimental structural phase transformations coupled with charge compensation reactions. However, little is known about the underpinning charge-structure mechanisms because the reduction-oxidation (redox) reactions within coexisting structural phases have so far eluded direct operando investigation. Here, we distinguish x-ray spectra of individual crystalline phases operando during a redox-induced phase transformation in P2-Na2/3Ni1/3Mn2/3O2 - an archetypal layered oxide for sodium-ion batteries. We measure the resonant elastic scattering on the Bragg reflection corresponding to the P2-phase lattice spacing. These resonant spectra become static midway through the sodium extraction in an operando coin cell, while the overall sodium extraction proceeds as evidenced by the X-ray absorption averaging over all electrochemically active Ni atoms. The stop of redox activity in the P2-structure signifies its inability to host Ni4+ ions. The coincident emergence of the O2- structure reveals the rigid link between the local redox and the long-range order during the phase transformation. The structure-selective x-ray spectroscopy thus opens a powerful avenue for resolving the dynamic chemistry of different structural phases in multi-phase electrochemical systems.
Operando Raman probing of mode selective electron phonon coupling in two dimensional halide perovskites
Institut national de la recherche scientifique(国家科学研究学院);Eindhoven University of Technology(埃因霍温理工大学);CNR NANOTEC, c/o Department of Chemistry, University of Bari(巴里大学化学系附属意大利国家研究委员会纳米技术研究所);Faculty of Science and Technology and MESA+ Institute for Nanotechnology, University of Twente(特温特大学科学与技术学院及MESA+纳米技术研究所)
Operando Charge Carrier Dynamics by Intensity-Modulated Photoluminescence: From Perovskite Thin Films to Solar Cells
Technische Universität Chemnitz(开姆尼茨工业大学);Leibniz-Institut für Festkörper- und Werkstoffforschung Dresden (IFW)(德累斯顿莱布尼茨固体与材料研究所);Chair for Emerging Electronic Technologies, Technische Universität Dresden(德累斯顿工业大学新兴电子技术系)
Quantifying Phase Transformations in Alloying Anodes via In-Situ Liquid Cell Hard X-ray Spectroscopy and Cryogenic Microscopy
Imperial College London(帝国理工学院);Diamond Light Source(钻石光源);Max-Planck Institute for Sustainable Materials(马克斯·普朗克可持续材料研究所);Univ Rouen Normandie, CNRS, INSA Rouen Normandie, Groupe de Physique des Matériaux, UMR 6634(鲁昂诺曼底大学、法国国家科学研究中心、鲁昂诺曼底国立应用科学学院、材料物理研究组)
Spatially inhomogeneous delithiation in LiNiO2 positive electrode: the effect of X-rays dose
Synchrotron SOLEIL(Soleil 同步辐射光源);Technische Universität München(慕尼黑工业大学);Centre National de la Recherche Scientifique, CNRS UR1(法国国家科学研究中心);Réseau sur le Stockage Electrochimique de l’Energie (RS2E), CNRS FR3459(电化学储能研究网络);Sorbonne Université, CNRS, Physicochimie des Electrolytes et Nanosystèmes Interfaciaux, CNRS UMR8234(索邦大学)
Insights on the volume variation of LiCoxMn2-xO4 electrode upon cycling: a correlative operando XRD and XAS study
Sorbonne Université, CNRS, Physicochimie des Electrolytes et Nanosystèmes interfaciaux (PHENIX)(索邦大学,法国国家科学研究中心,电解质与界面纳米系统物理化学);Sorbonne Université, CNRS, Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP)(索邦大学,法国国家科学研究中心,巴黎凝聚态物质化学实验室);Réseau sur le Stockage Electrochimique de l’Energie (RS2E), FR CNRS 3459(电化学储能研究网络(RS2E),FR CNRS 3459)
Ultrafast order-selective electron imaging and spectroscopy
Georg-August-Universität Göttingen(哥廷根大学);Max Planck Institute for Multidisciplinary Sciences(马克斯·普朗克多学科科学研究所);University of Göttingen(哥廷根大学);Philipps-Universität Marburg(马尔堡菲利普大学)
Unraveling the storage mechanism of Na$_{3}$V$_{2-x}$Ni$_x$(PO$_4$)$_2$F$_3$/C cathodes for sodium-ion batteries through electrochemical, {\it operando} X-ray diffraction and microscopy studies
本研究结合 EIS、GITT、CV、operando XRD 与原位同步辐射 TXM,揭示 Ni 掺杂 Na₃V₂(PO₄)₂F₃/C 正极的储钠机制、扩散动力学及长循环稳定性。
Ultrafast electron dynamics in Au/Fe/MgO(001) analyzed by Au- and Fe-selective pumping in time-resolved two-photon photoemission spectroscopy: Separation of excitations in adjacent metallic layers
Predictive autoencoder-transformer model of Cu oxidation state from EELS and XAS spectra
Brookhaven National Lab(布鲁克海文国家实验室);Binghamton University(宾汉顿大学);Lawrence Berkeley National Laboratory(劳伦斯伯克利国家实验室);University of California, Berkeley(加州大学伯克利分校)