期刊
JOURNAL OF ENERGY CHEMISTRY
卷 64, 期 -, 页码 1-7出版社
ELSEVIER
DOI: 10.1016/j.jechem.2021.04.049
关键词
Operando HERFD-XANES; Delta mu analysis; Structural evolution; Copper(II) phthalocyanine; Electrochemical CO2 reduction reaction
资金
- National Natural Science Foun-dation of China [U1732267]
Quantitatively understanding the impact of atomic-level catalyst structural changes on the reactivity of the electrochemical CO2 reduction reaction is challenging. Operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used in this study to identify the dynamic structural transformation of active sites of a model copper(II) phthalocyanine catalyst. The approach developed is a novel and powerful technique for elucidating complex catalytic mechanisms and may contribute to the rational design of highly effective catalysts.
The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO2 reduction reaction is challenging. Due to the complexity of catalytic systems, conventional in situ X-ray spectroscopy plays a limited role in tracing the underlying dynamic structural changes in catalysts active sites. Herein, operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used to precisely identify the dynamic structural transformation of well-defined active sites of a representative model copper(II) phthalocyanine catalyst which is of guiding significance in studying single-atom catalysis system. Comprehensive X-ray spectroscopy analyses, including surface sensitive Delta mu spectra which isolates the surface changes by subtracting the disturb of bulk base and X-ray absorption near-edge structure spectroscopy simulation, were used to discover that Cu species aggregated with increasing applied potential, which is responsible for the observed evolution of C2H4. The approach developed in this work, characterizing the active-site geometry and dynamic structural change, is a novel and powerful technique to elucidate complex catalytic mechanisms and is expected to contribute to the rational design of highly effective catalysts. (C) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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