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arXiv · 2511.16382

Quantifying Phase Transformations in Alloying Anodes via In-Situ Liquid Cell Hard X-ray Spectroscopy and Cryogenic Microscopy

Neil Mulcahy·Syeda Ramin Jannat·Yaqi Li·Tigran Simonian·Mariana Palos·James O. Douglas·Jessica M. Walker·Baptiste Gault·Mary P. Ryan·Michele Shelly Conroy
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Abstract

Understanding electrochemical phenomena at complex liquid solid interfaces requires linking real time structural dynamics with atomic scale interfacial chemistry. Here, we integrate operando synchrotron X-ray fluorescence and diffraction with high resolution cryogenic electron and ion multi model microscopy to provide a mechanistic understanding of Pt based alloying anodes across length scales. We directly observe the initial lithiation driven formation of Li2Pt and its evolution to a stable LiPt intermetallic phase during extended cycling via a solid solution type reaction mechanism. Simultaneously, the solid electrolyte interphase transitions from an unstable carbonate rich to a stable LiF dominated composition, confirmed by cryogenic scanning transmission electron microscopy and electron energy loss spectroscopy. Crucially, cryogenic atom probe tomography reveals spatially distinct compositional regimes within the alloy anode, including lithium flux limited, heterogeneous interfacial zone and a diffusion controlled, homogeneous LiPt alloy bulk. This nanoscale compositional gradient rationalises the emergent solid solution reaction mechanism and highlights how kinetic limitations and interface dynamics govern alloy formation and electrochemical stability. Our findings demonstrate a broadly applicable correlative framework bridging operando structural dynamics with near atomic resolution interfacial chemistry, advancing the rational design of durable alloy electrodes for next generation energy storage.

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Neil Mulcahy, Syeda Ramin Jannat, Yaqi Li, Tigran Simonian, Mariana Palos, James O. Douglas, Jessica M. Walker, Baptiste Gault, Mary P. Ryan, Michele Shelly Conroy. 2025-11-20. Quantifying Phase Transformations in Alloying Anodes via In-Situ Liquid Cell Hard X-ray Spectroscopy and Cryogenic Microscopy. https://arxiv.org/abs/2511.16382

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