催化作用
氧化还原
纳米颗粒
水煤气变换反应
氢
氧化物
介电谱
吸收光谱法
材料科学
氧气
光谱学
化学
无机化学
光化学
化学工程
物理化学
纳米技术
电化学
电极
有机化学
物理
量子力学
工程类
作者
Marc Ziemba,Mariusz Radtke,Leon Schumacher,Christian Heß
标识
DOI:10.1002/anie.202209388
摘要
Abstract In 2 O 3 has emerged as a promising catalyst for CO 2 activation, but a fundamental understanding of its mode of operation in CO 2 hydrogenation is still missing, as the application of operando vibrational spectroscopy is challenging due to absorption effects. In this mechanistic study, we systematically address the redox processes related to the reverse water‐gas shift reaction (rWGSR) over In 2 O 3 nanoparticles, both at the surface and in the bulk. Based on temperature‐dependent operando UV/Vis spectra and a novel operando impedance approach for thermal powder catalysts, we propose oxidation by CO 2 as the rate‐determining step for the rWGSR. The results are consistent with redox processes, whereby hydrogen‐containing surface species are shown to exhibit a promoting effect. Our findings demonstrate that oxygen/hydrogen dynamics, in addition to surface processes, are important for the activity, which is expected to be of relevance not only for In 2 O 3 but also for other reducible oxide catalysts.
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