炼油厂
格式化
催化作用
甲醇
电化学
氧气
化学
化学工程
材料科学
有机化学
物理化学
电极
工程类
作者
Fanxu Meng,Qian Wu,Kamal Elouarzaki,Songzhu Luo,Yuanmiao Sun,Chencheng Dai,Shibo Xi,Yubo Chen,Xinlong Lin,Mingliang Fang,Xin Wang,Daniel Mandler,Zhichuan J. Xu
出处
期刊:Science Advances
[American Association for the Advancement of Science (AAAS)]
日期:2023-08-25
卷期号:9 (34)
标识
DOI:10.1126/sciadv.adh9487
摘要
Developing technologies based on the concept of methanol electrochemical refinery (e-refinery) is promising for carbon-neutral chemical manufacturing. However, a lack of mechanism understanding and material properties that control the methanol e-refinery catalytic performances hinders the discovery of efficient catalysts. Here, using 18 O isotope–labeled catalysts, we find that the oxygen atoms in formate generated during the methanol e-refinery reaction can originate from the catalysts’ lattice oxygen and the O-2p-band center levels can serve as an effective descriptor to predict the catalytic performance of the catalysts, namely, the formate production rates and Faradaic efficiencies. Moreover, the identified descriptor is consolidated by additional catalysts and theoretical mechanisms from density functional theory. This work provides direct experimental evidence of lattice oxygen participation and offers an efficient design principle for the methanol e-refinery reaction to formate, which may open up new research directions in understanding and designing electrified conversions of small molecules.
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