The state of zinc in methanol synthesis over a Zn/ZnO/Cu(211) model catalyst

IF 44.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2022-05-05 DOI:10.1126/science.abj7747

Peter Amann, Bernhard Klötzer, David Degerman, Norbert Köpfle, Thomas Götsch, Patrick Lömker, Christoph Rameshan, Kevin Ploner, Djuro Bikaljevic, Hsin-Yi Wang, Markus Soldemo, Mikhail Shipilin, Christopher M. Goodwin, Jörgen Gladh, Joakim Halldin Stenlid, Mia Börner, Christoph Schlueter, Anders Nilsson

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引用次数: 35

Abstract

The active chemical state of zinc (Zn) in a zinc-copper (Zn-Cu) catalyst during carbon dioxide/carbon monoxide (CO₂/CO) hydrogenation has been debated to be Zn oxide (ZnO) nanoparticles, metallic Zn, or a Zn-Cu surface alloy. We used x-ray photoelectron spectroscopy at 180 to 500 millibar to probe the nature of Zn and reaction intermediates during CO₂/CO hydrogenation over Zn/ZnO/Cu(211), where the temperature is sufficiently high for the reaction to rapidly turn over, thus creating an almost adsorbate-free surface. Tuning of the grazing incidence angle makes it possible to achieve either surface or bulk sensitivity. Hydrogenation of CO₂ gives preference to ZnO in the form of clusters or nanoparticles, whereas in pure CO a surface Zn-Cu alloy becomes more prominent. The results reveal a specific role of CO in the formation of the Zn-Cu surface alloy as an active phase that facilitates efficient CO₂ methanol synthesis.

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Zn/ZnO/Cu(211) 模型催化剂合成甲醇过程中锌的状态

在二氧化碳/一氧化碳（CO2/CO）氢化过程中，锌-铜（Zn）催化剂中锌（Zn）的活性化学态是氧化锌（ZnO）纳米颗粒、金属锌还是锌-铜表面合金一直存在争议。我们使用 X 射线光电子能谱在 180 至 500 毫巴的温度下探测 Zn/ZnO/Cu(211)上 CO2/CO 加氢过程中 Zn 和反应中间产物的性质。通过调节掠入射角，可以实现表面或体液灵敏度。二氧化碳的氢化反应更倾向于采用团簇或纳米颗粒形式的氧化锌，而在纯二氧化碳中，表面的锌铜合金变得更加突出。研究结果揭示了 CO 在形成 Zn-Cu 表面合金中的特殊作用，这种合金是促进 CO2 甲醇高效合成的活性相。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

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