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钌催化一氧化碳加氢反应催化途径的实时阐释

Real-Time Elucidation of Catalytic Pathways in CO Hydrogenation on Ru.

作者信息

LaRue J, Krejčí O, Yu L, Beye M, Ng M L, Öberg H, Xin H, Mercurio G, Moeller S, Turner J J, Nordlund D, Coffee R, Minitti M P, Wurth W, Pettersson L G M, Öström H, Nilsson A, Abild-Pedersen F, Ogasawara H

机构信息

SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.

Department of Physics, AlbaNova University Center, Stockholm University , SE-10691 Stockholm, Sweden.

出版信息

J Phys Chem Lett. 2017 Aug 17;8(16):3820-3825. doi: 10.1021/acs.jpclett.7b01549. Epub 2017 Aug 3.

Abstract

The direct elucidation of the reaction pathways in heterogeneous catalysis has been challenging due to the short-lived nature of reaction intermediates. Here, we directly measured on ultrafast time scales the initial hydrogenation steps of adsorbed CO on a Ru catalyst surface, which is known as the bottleneck reaction in syngas and CO reforming processes. We initiated the hydrogenation of CO with an ultrafast laser temperature jump and probed transient changes in the electronic structure using real-time X-ray spectroscopy. In combination with theoretical simulations, we verified the formation of CHO during CO hydrogenation.

摘要

由于反应中间体的寿命较短,直接阐明多相催化中的反应途径具有挑战性。在这里,我们在超快时间尺度上直接测量了钌催化剂表面吸附的一氧化碳的初始氢化步骤,这是合成气和一氧化碳重整过程中的瓶颈反应。我们用超快激光温度跃升启动了一氧化碳的氢化反应,并使用实时X射线光谱探测电子结构的瞬态变化。结合理论模拟,我们验证了一氧化碳氢化过程中CHO的形成。

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