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An in situ three-dimensional fluorescence computed tomography–X-ray absorption fine structure (CT–XAFS) imaging technique and an in situ same-view nano-XAFS–scanning electron microscopy (SEM)/energy-dispersive spectrometry (EDS) combination technique were applied for the first time to perform operando spatial visualization and depth-profiling analysis of Ce radical scavengers in a practical PEFC of Toyota MIRAI FCV under PEFC operating conditions. Using these in situ techniques, we successfully visualized and analyzed the domain, density, valence, and migration of Ce scavengers that were heterogeneously distributed in the components of PEFC, such as anode microporous layer, anode catalyst layer, polymer electrolyte membrane (PEM), cathode catalyst layer, and cathode microporous layer. 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Operando Imaging of Ce Radical Scavengers in a Practical Polymer Electrolyte Fuel Cell by 3D Fluorescence CT–XAFS and Depth-Profiling Nano-XAFS–SEM/EDS Techniques
https://uec.repo.nii.ac.jp/records/10306
https://uec.repo.nii.ac.jp/records/1030651f2486f-516c-4c18-9c4d-a3ed52f2747d
名前 / ファイル | ライセンス | アクション |
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ACS Appl. Mater. Interfaces_submitted_r1.pdf (2.7 MB)
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Item type | 学術雑誌論文 / Journal Article(1) | |||||
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公開日 | 2023-03-03 | |||||
タイトル | ||||||
言語 | en | |||||
タイトル | Operando Imaging of Ce Radical Scavengers in a Practical Polymer Electrolyte Fuel Cell by 3D Fluorescence CT–XAFS and Depth-Profiling Nano-XAFS–SEM/EDS Techniques | |||||
言語 | ||||||
言語 | eng | |||||
キーワード | ||||||
言語 | en | |||||
主題 | operando imaging of Ce scavengers in practical PEFCs | |||||
キーワード | ||||||
言語 | en | |||||
主題 | distribution and migration of Ce³⁺ radical scavengers | |||||
キーワード | ||||||
言語 | en | |||||
主題 | Ce³⁺/Ce⁴⁺ fraction | |||||
キーワード | ||||||
言語 | en | |||||
主題 | 3D fluorescence CT−XAFS imaging | |||||
キーワード | ||||||
言語 | en | |||||
主題 | same-view nano-XAFS−SEM/EDS imaging | |||||
資源タイプ | ||||||
資源タイプ識別子 | http://purl.org/coar/resource_type/c_6501 | |||||
資源タイプ | journal article | |||||
著者 |
Matsui, Hirosuke
× Matsui, Hirosuke× Takao, Shinobu× Higashi, Kotaro× Kaneko, Takuma× Samjeské, Gabor× Uruga, Tomoya× Tada, Mizuki× Iwasawa, Yasuhiro |
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抄録 | ||||||
内容記述タイプ | Abstract | |||||
内容記述 | There is little information on the spatial distribution, migration, and valence of Ce species doped as an efficient radical scavenger in a practical polymer electrolyte fuel cell (PEFC) for commercial fuel cell vehicles (FCVs) closely related to a severe reliability issue for long-term PEFC operation. An in situ three-dimensional fluorescence computed tomography–X-ray absorption fine structure (CT–XAFS) imaging technique and an in situ same-view nano-XAFS–scanning electron microscopy (SEM)/energy-dispersive spectrometry (EDS) combination technique were applied for the first time to perform operando spatial visualization and depth-profiling analysis of Ce radical scavengers in a practical PEFC of Toyota MIRAI FCV under PEFC operating conditions. Using these in situ techniques, we successfully visualized and analyzed the domain, density, valence, and migration of Ce scavengers that were heterogeneously distributed in the components of PEFC, such as anode microporous layer, anode catalyst layer, polymer electrolyte membrane (PEM), cathode catalyst layer, and cathode microporous layer. The average Ce valence states in the whole PEFC and PEM were 3.9+ and 3.4+, respectively, and the Ce³⁺/Ce⁴⁺ ratios in the PEM under H₂ (anode)–N₂ (cathode) at an open-circuit voltage (OCV), H₂–air at 0.2 A cm⁻², and H₂–air at 0.0 A cm⁻² were 70 ± 5:30 ± 5%, as estimated by both in situ fluorescence CT–X-ray absorption near-edge spectroscopy (XANES) and nano-XANES–SEM/EDS techniques. The Ce³⁺ migration rates in the electrolyte membrane toward the anode and cathode electrodes ranged from 0.3 to 3.8 μm h⁻¹, depending on the PEFC operating conditions. Faster Ce³⁺ migration was not observed with voltage transient response processes by highly time-resolved (100 ms) and spatially resolved (200 nm) nano-XANES imaging. Ce³⁺ ions were suggested to be coordinated with both Nafion sulfonate (Nf_sul) groups and water to form [Ce(Nf_sul)_x(H₂O)_y]³⁺. The Ce migration behavior may also be affected by the spatial density of Ce, interactions of Ce with Nafion, thickness and states of the PEM, and H₂O convection, in addition to the PEFC operating conditions. The unprecedented operando imaging of Ce radical scavengers in the practical PEFCs by both in situ three-dimensional (3D) fluorescence CT–XAFS imaging and in situ depth-profiling nano-XAFS–SEM/EDS techniques yields intriguing insights into the spatial distribution, chemical states, and behavior of Ce scavengers under the working conditions for the development of next-generation PEFCs with high long-term reliability and durability. | |||||
書誌情報 |
en : ACS Applied Materials & Interfaces 巻 14, 号 5, p. 6762-6776, 発行日 2022-02-09 |
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出版者 | ||||||
出版者 | American Chemical Society | |||||
ISSN | ||||||
収録物識別子タイプ | ISSN | |||||
収録物識別子 | 19448244 | |||||
DOI | ||||||
関連タイプ | isVersionOf | |||||
識別子タイプ | DOI | |||||
関連識別子 | 10.1021/acsami.1c22336 | |||||
権利 | ||||||
権利情報 | This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © 2022 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see (https://doi.org/10.1021/acsami.1c22336). | |||||
関連サイト | ||||||
識別子タイプ | DOI | |||||
関連識別子 | https://doi.org/10.1021/acsami.1c22336 | |||||
著者版フラグ | ||||||
出版タイプ | AM | |||||
出版タイプResource | http://purl.org/coar/version/c_ab4af688f83e57aa |