通过调制激发 X 射线吸收光谱研究铜的电极-电解质界面

IF 32.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Energy & Environmental Science Pub Date : 2025-04-09 DOI:10.1039/d5ee01068c

Angel T. Garcia-Esparza, Xiang Li, Finn Babbe, Jinkyu Lim, K. Dean Skoien, Philipp Stefan Simon, Junko Yano, Dimosthenis Sokaras

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引用次数: 0

摘要

在操作条件下访问电极-电解质界面并捕获时间分辨动力学是电化学研究的挑战。尽管进行了广泛的研究，铜的界面氧化动力学仍不清楚。调制激发x射线吸收光谱（ME-XAS）以亚秒灵敏度探测100 mM KHCO₃中的Cu，在开路条件下，在正电位（0至0.5 V RHE）下，比Cu₂O早30±10 ms形成氢氧化物。在-0.4 ~ 0.8 V RHE范围内，Cu(I)和Cu（II）氧化物平衡，氢氧化物含量达到49%。这些对间歇性可再生能源操作下Cu界面氧化还原的见解（与CO₂电解槽的耐久性相关）增强了我们对电化学界面的基本理解。

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The electrode-electrolyte interface of Cu via modulation excitation X-ray absorption spectroscopy

Accessing the electrode-electrolyte interface under operating conditions and capturing time-resolved kinetics challenge electrochemical studies. Copper’s interfacial oxidation dynamics remain unclear despite extensive research. Modulation excitation X-ray absorption spectroscopy (ME-XAS) probes Cu in 100 mM KHCO₃ with sub-second sensitivity, revealing hydroxide forming 30±10 ms before Cu₂O at positive potentials (0 to 0.5 V RHE) near open-circuit conditions. From -0.4 to 0.8 V RHE, hydroxide reaches 49% with balanced Cu(I) and Cu(II) oxides. These insights into Cu interfacial redox under intermittent renewable energy operation—relevant to CO₂ electrolyzer durability—enhance our fundamental understanding of electrochemical interfaces.

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来源期刊

Energy & Environmental Science 化学-工程：化工

CiteScore

50.50

自引率

2.20%

发文量

349

审稿时长

2.2 months

期刊介绍： Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).