催化作用
甲醇
选择性
X射线光电子能谱
氧化物
无机化学
空间速度
贵金属
金属
化学
烧结
材料科学
化学工程
有机化学
工程类
作者
Ning Rui,Feng Zhang,Kaihang Sun,Zongyuan Liu,Wenqian Xu,Eli Stavitski,Sanjaya D. Senanayake,José A. Rodríguez,Changjun Liu
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2020-08-07
卷期号:10 (19): 11307-11317
被引量:197
标识
DOI:10.1021/acscatal.0c02120
摘要
CO2 hydrogenation to methanol has attracted increasing attention with the development of renewable hydrogen. A big challenge is to identify catalysts able to achieve high conversion and selectivity. Here, we report an In2O3-supported Au catalyst that exhibits excellent performance for hydrogenation of CO2 selectively to methanol. In situ characterizations using time-resolved X-ray diffraction, ambient-pressure X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy confirm that a strong metal–support interaction leads to a reactive Auδ+–In2O3–x interface for activation and hydrogenation of CO2 to methanol. An effective gold-indium oxide bonding favors the dispersion of the noble metal and prevents its sintering under reaction conditions. The methanol selectivity reaches 100% at temperatures below 225 °C and is more than 70% at 275 °C over the Auδ+–In2O3–x catalyst. It is even 67.8% with a space time yield of methanol of 0.47 gMeOH/(h·gcat) at 300 °C, 5 MPa, and 21,000 cm3 h–1 gcat–1. The results obtained here represent the highest selectivity and activity ever reported for CO2 hydrogenation over supported gold catalysts. Our study shows that the strong Au/In2O3 interaction and the intrinsic chemical activity of In2O3 can be used to significantly improve the catalytic performance of Au catalysts, providing promising routes for the rational design and application of Au catalysts beyond CO2 hydrogenation.
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