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金属氢化物在 CO2 还原中催化活性的起源。

The Origin of the Catalytic Activity of a Metal Hydride in CO2 Reduction.

机构信息

École Polytechnique Fédérale de Lausanne (EPFL), 1951, Sion, Switzerland.

Empa, Swiss Federal Laboratories for Materials Science and Technology, 8600, Dübendorf, Switzerland.

出版信息

Angew Chem Int Ed Engl. 2016 May 10;55(20):6028-32. doi: 10.1002/anie.201601402. Epub 2016 Apr 9.

Abstract

Atomic hydrogen on the surface of a metal with high hydrogen solubility is of particular interest for the hydrogenation of carbon dioxide. In a mixture of hydrogen and carbon dioxide, methane was markedly formed on the metal hydride ZrCoHx in the course of the hydrogen desorption and not on the pristine intermetallic. The surface analysis was performed by means of time-of-flight secondary ion mass spectroscopy and near-ambient pressure X-ray photoelectron spectroscopy, for the in situ analysis. The aim was to elucidate the origin of the catalytic activity of the metal hydride. Since at the initial stage the dissociation of impinging hydrogen molecules is hindered by a high activation barrier of the oxidised surface, the atomic hydrogen flux from the metal hydride is crucial for the reduction of carbon dioxide and surface oxides at interfacial sites.

摘要

对于二氧化碳的加氢反应,具有高氢溶解度的金属表面上的原子氢特别有趣。在氢气和二氧化碳的混合物中,在氢化锆钴 ZrCoHx 金属氢化物的氢气解吸过程中明显形成了甲烷,而不是在原始的金属间化合物上形成。通过飞行时间二次离子质谱和近常压 X 射线光电子能谱进行了表面分析,用于原位分析。目的是阐明金属氢化物催化活性的起源。由于在初始阶段,撞击氢分子的离解受到氧化表面的高活化能垒的阻碍,因此来自金属氢化物的原子氢通量对于界面处二氧化碳和表面氧化物的还原至关重要。

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