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Hydrogenation of CO2 to Methanol on a Auδ+–In2O3–x Catalyst
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-08-07 , DOI: 10.1021/acscatal.0c02120
Ning Rui 1, 2 , Feng Zhang 3 , Kaihang Sun 1 , Zongyuan Liu 2 , Wenqian Xu 4 , Eli Stavitski 5 , Sanjaya D. Senanayake 2 , José A. Rodriguez 2, 3 , Chang-Jun Liu 1
Affiliation  

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.

中文翻译:

Auδ + –In 2 O 3– x催化剂上将CO 2加氢成甲醇

随着可再生氢的发展,CO 2加氢成甲醇已引起越来越多的关注。一个巨大的挑战是确定能够实现高转化率和选择性的催化剂。在这里,我们报告了一种In 2 O 3负载的Au催化剂,该催化剂具有出色的将CO 2选择性氢化为甲醇的性能。使用时间分辨X射线衍射,环境压力X射线光电子能谱和X射线吸收能谱法进行的原位表征证实,强金属-载体相互作用会导致反应性Auδ + –In 2 O 3– x界面用于CO 2的活化和氢化甲醇。有效的金-铟氧化物键有利于贵金属的分散并防止其在反应条件下烧结。相对于Auδ+ –In 2 O 3– x催化剂,甲醇的选择性在225°C以下的温度下达到100%,在275°C上超过70%。在300°C,5 MPa和21,000 cm 3 h –1 g cat –1的条件下,甲醇的时空收率为0.47 g MeOH /(h·g cat)甚至为67.8%。此处获得的结果代表有史以来在负载型金催化剂上报道的CO 2加氢的最高选择性和最高活性。我们的研究表明,较强的金/铟2 O 3的相互作用和In 2 O 3的固有化学活性可用于显着改善Au催化剂的催化性能,为合理设计和应用Au催化剂提供了超越CO 2加氢的可行途径。
更新日期:2020-10-02
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