CO2‐to‐Methanol Hydrogenation on Zirconia‐Supported Copper Nanoparticles: Reaction Intermediates and the Role of the Metal–Support Interface,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

CO2‐to‐Methanol Hydrogenation on Zirconia‐Supported Copper Nanoparticles: Reaction Intermediates and the Role of the Metal–Support Interface
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2017-01-23 , DOI: 10.1002/anie.201610166
Kim Larmier ₁ , Wei-Chih Liao ₁ , Shohei Tada ₁ , Erwin Lam ₁ , René Verel ₁ , Atul Bansode ₂ , Atsushi Urakawa ₂ , Aleix Comas-Vives ₁ , Christophe Copéret ₁

Affiliation

Methanol synthesis by CO₂ hydrogenation is a key process in a methanol‐based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO₂ to methanol still remain unknown. A mechanistic study of the hydrogenation of CO₂ on Cu/ZrO₂ is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO₂ hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.

中文翻译：

氧化锆负载的铜纳米粒子上的CO2到甲醇的加氢：反应中间体和金属-支持界面的作用

通过CO ₂加氢合成甲醇是基于甲醇的经济中的关键过程。该反应被负载的铜纳米颗粒催化，并显示出强的载体或助催化剂作用。众所周知，氧化锆既可以提高甲醇的生产速度，又可以提高选择性。然而，该观察的起源以及与CO ₂转化为甲醇相关的反应机理仍然未知。提出了在Cu / ZrO ₂上CO ₂加氢的机理研究。使用动力学，原位IR和NMR光谱学以及同位素标记策略，在CO ₂期间形成了表面中间体在不同压力下观察到氢化。结合DFT计算，表明甲酸盐是反应中间体，氧化锆/铜界面对于该中间体向甲醇的转化至关重要。

更新日期：2017-01-23

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南