高OER活性铱阳极中电子缺氧体的x射线吸收和发射光谱特征

IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL
Lorena Alzate-Vargas, Lorenz J. Falling, Sourav Laha, Bettina Lotsch, Jau-Wern Chiou, Ting-Shan Chan, Way-Faung Pong, Cheng-Hao Chuang, J. J. Velasco Vélez and T. E. Jones
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引用次数: 0

摘要

近年来,水裂解已成为一种很有前途的可再生能源存储技术,但由于缺乏稳定的阳极材料来克服析氧反应(OER)的缓慢性,其发展受到限制。铱氧化物是最活跃和最稳定的OER催化剂之一,然而这些材料如何达到它们的性能仍在讨论中。铱基材料的活性归因于高金属氧化态和o2p空穴的出现。在这里,我们采用了一种技术组合- Ir - LII, iii -边缘的x射线吸收,O - k边缘的x射线吸收和发射,以及从头算方法-来识别和表征存在于高oer活性x射线非晶氧化物中的配体空穴。我们发现,与基于ok边缘x射线吸收测量的原始命题一致,o2p空穴存在于这些材料中,并且可能与OER期间活性的增加有关。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Electron deficient oxygen species in highly OER active iridium anodes characterized by X-ray absorption and emission spectroscopy†

Electron deficient oxygen species in highly OER active iridium anodes characterized by X-ray absorption and emission spectroscopy†

Water splitting is a promising technology for storing energy, yet it is challenged by the lack of stable anode materials that can overcome the sluggishness of the oxygen evolution reaction (OER). Iridium oxides are among the most active and stable OER catalysts, however how these materials achieve their performance remains under discussion. The activity of iridium based materials has been attributed to both high metal oxidation states and the appearance of O 2p holes. Herein we employ a combination of techniques—X-ray absorption at the Ir LII,III-edge, X-ray absorption and emission at the O K-edge, along with ab initio methods—to identify and characterize ligand holes present in highly OER-active X-ray amorphous oxides. We find, in agreement with the original proposition based on X-ray absorption measurement at the O K-edge, that O 2p holes are present in these materials and can be associated with the increased activity during OER.

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来源期刊
Physical Chemistry Chemical Physics
Physical Chemistry Chemical Physics 化学-物理:原子、分子和化学物理
CiteScore
5.50
自引率
9.10%
发文量
2675
审稿时长
2.0 months
期刊介绍: Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.
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