期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 7, 页码 2911-2915出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b13786
关键词
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资金
- National Key R&D Program of China [2016YFB0600901]
- National Natural Science Foundation of China [U1463205, 21525626, 21606169]
- Program of Introducing Talents of Discipline to Universities [B06006]
The role of surface hydroxyls is significant for understanding catalytic performance of metallic oxides for CO2 electroreduction reaction (CO2ER). This Communication describes, employing SnOx as a model system, how to moderate coverage of hydroxyl to derive a stable Sn branches catalyst for CO2ER with a 93.1% Faradaic efficiency (FE) of carbonaceous products. With use of in situ attenuated total reflection surface enhanced infrared adsorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations, we found that a proper amount of surface hydroxyls offered effective sites to boost CO2 adsorption via hydrogen bond. However, a higher surface coverage of hydroxyls leads to self-reduction of Sn-OH. We also explained the competition between self-reduction and CO2 reduction over Sn-based catalysts. The findings revealed the quantitative correlation between surface coverage of hydroxyl and CO2ER activity and suggested a logical extension to other metal oxide catalysts for CO2ER.
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