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arXiv · 2108.05913

Structure-selective operando x-ray spectroscopy

Daniel Weinstock·Hayley S. Hirsh·Oleg Yu. Gorobtsov·Minghao Zhang·Jason Huang·Ryan Bouck·Jacob P. C. Ruff·Y. Shirley Meng·Andrej Singer
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Abstract

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.

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Daniel Weinstock, Hayley S. Hirsh, Oleg Yu. Gorobtsov, Minghao Zhang, Jason Huang, Ryan Bouck, Jacob P. C. Ruff, Y. Shirley Meng, Andrej Singer. 2021-08-12. Structure-selective operando x-ray spectroscopy. https://doi.org/10.1021/acsenergylett.1c02371

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