Hydrogenation of CO2 to Methanol on a Auδ+–In2O3–x Catalyst,ACS Catalysis

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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 Au^δ+–In₂O_3–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 Au^δ+–In₂O_3–x catalyst. It is even 67.8% with a space time yield of methanol of 0.47 g_MeOH/(h·g_cat) at 300 °C, 5 MPa, and 21,000 cm³ h^–1 g_cat^–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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