@article{f32cde65c78a409fbc2f0e1b124e5d52,
title = "Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction",
abstract = "Copper electrocatalysts have been shown to selectively reduce carbon dioxide to hydrocarbons. Nevertheless, the absence of a systematic study based on time-resolved spectroscopy renders the functional agent—either metallic or oxidative Copper—for the selectivity still undecidable. Herein, we develop an operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts. An oxide-derived Copper electrocatalyst is employed as a model catalyst to offer scientific insights into the roles metal states serve in carbon dioxide reduction reaction (CO2RR). Using a potential switching approach, the model catalyst can achieve a steady chemical state of half-Cu(0)-and-half-Cu(I) and selectively produce asymmetric C2 products - C2H5OH. Furthermore, a theoretical analysis reveals that a surface composed of Cu-Cu(I) ensembles can have dual carbon monoxide molecules coupled asymmetrically, which potentially enhances the catalyst{\textquoteright}s CO2RR product selectivity toward C2 products. Our results offer understandings of the fundamental chemical states and insights to the establishment of selective CO2RR.",
author = "Lin, {Sheng Chih} and Chang, {Chun Chih} and Chiu, {Shih Yun} and Pai, {Hsiao Tien} and Liao, {Tzu Yu} and Hsu, {Chia Shuo} and Chiang, {Wei Hung} and Tsai, {Ming Kang} and Chen, {Hao Ming}",
note = "Funding Information: This study is supported by the Ministry of Science and Technology of Taiwan (108-2628-M-002-004 -RSP, 107-2113-M-003-007, 107-2811-M-003-528, and 108-2113-M-003-003). We also thank the innovation-oriented trilateral research fund for young investigators of NTU system (108PNTUS01), thanks to Ms. C.-Y. Chien and Ms. S.-J. Ji of Ministry of Science and Technology (National Taiwan University) for the assistance in SEM and TEM experiments. The technical support from the Advanced nano/micro-Fabrication and Characterization lab at Academia Sinica is acknowledged. We are grateful to the computational resources provided by National Center for High-Performance Computing of Taiwan and Center for Cloud Computing in National Taiwan Normal University. Publisher Copyright: {\textcopyright} 2020, The Author(s).",
year = "2020",
month = dec,
day = "1",
doi = "10.1038/s41467-020-17231-3",
language = "English",
volume = "11",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",
number = "1",
}