journal article·2023-07Open access

Emergence of Dynamically‐Disordered Phases During Fast Oxygen Deintercalation Reaction of Layered Perovskite

Takafumi Yamamoto, Shogo Kawaguchi, Taiki Kosuge, Akira Sugai, Naoki Tsunoda, Yu Kumagai, Kosuke Beppu, Takuya Ohmi, Teppei Nagase, Kotaro Higashi, Kazuo Kato, Kiyofumi Nitta, Tomoya Uruga, Seiji Yamazoe, Fumiyasu Oba, Tsunehiro Tanaka, Masaki Azuma, Saburo Hosokawa

Advanced Science· Volume 10· Issue 19

Abstract

Abstract Determination of a reaction pathway is an important issue for the optimization of reactions. However, reactions in solid‐state compounds have remained poorly understood because of their complexity and technical limitations. Here, using state‐of‐the‐art high‐speed time‐resolved synchrotron X‐ray techniques, the topochemical solid‐gas reduction mechanisms in layered perovskite Sr3Fe2O7−δ (from δ ∼ 0.4 to δ = 1.0), which is promising for an environmental catalyst material is revealed. Pristine Sr3Fe2O7−δ shows a gradual single‐phase structural evolution during reduction, indicating that the reaction continuously proceeds through thermodynamically stable phases. In contrast, a nonequilibrium dynamically‐disordered phase emerges a few seconds before a first‐order transition during the reduction of a Pd‐loaded sample. This drastic change in the reaction pathway can be explained by a change in the rate‐determining step. The synchrotron X‐ray technique can be applied to various solid‐gas reactions and provides an opportunity for gaining a better understanding and optimizing reactions in solid‐state compounds.
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Research context

OpenAlex topics: Advanced Condensed Matter Physics · Magnetic and transport properties of perovskites and related materials · Layered Double Hydroxides Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Laboratory for Materials and Structures Institute of Innovative Research Tokyo Institute of Technology Yokohama 2268503 Japan

Japan Synchrotron Radiation Research Institute (JASRI) SPring‐8, 1‐1‐1 Kouto Sayo‐gun Hyogo 6795198 Japan

Institute for Materials Research Tohoku University 2‐1‐1 Katahira, Aoba‐ku Sendai 9808577 Japan

Department of Applied Chemistry for Environment Graduate School of Urban Environmental Sciences Tokyo Metropolitan University 1‐1 Minami‐Osawa Hachioji Tokyo 1920397 Japan

Department of Chemistry Graduate School of Science Tokyo Metropolitan University 1‐1 Minami‐Osawa Hachioji Tokyo 1920397 Japan

Elements Strategy Initiative for Catalysts & Batteries (ESICB) Kyoto University Katsura, Nishikyo‐ku Kyoto 6158245 Japan

Department of Molecular Engineering Graduate school of Engineering Kyoto University Nishikyo‐ku Kyoto 6158510 Japan

Living Systems Materialogy (LiSM) Research Group International Research Frontiers Initiative (IRFI) Tokyo Institute of Technology Yokohama 2268501 Japan

Kanagawa Institute of Industrial Science and Technology (KISTEC) 705‐1 Shimoimaizumi Ebina Kanagawa 2430435 Japan

Faculty of Materials Science and Engineering Kyoto Institute of Technology Matsugasaki Sakyo‐ku Kyoto 6068585 Japan

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