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Cu/ZnO-CeO催化剂的火焰合成：协同的金属-载体相互作用促进CO加氢制CHOH的选择性

Flame Synthesis of Cu/ZnO-CeO Catalysts: Synergistic Metal-Support Interactions Promote CHOH Selectivity in CO Hydrogenation.

作者信息

Zhu Jiadong, Ciolca Diana, Liu Liang, Parastaev Alexander, Kosinov Nikolay, Hensen Emiel J M

机构信息

Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.

出版信息

ACS Catal. 2021 Apr 16;11(8):4880-4892. doi: 10.1021/acscatal.1c00131. Epub 2021 Apr 6.

DOI:10.1021/acscatal.1c00131
PMID:33898079
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8057230/
Abstract

The hydrogenation of CO to CHOH is an important reaction for future renewable energy scenarios. Herein, we compare Cu/ZnO, Cu/CeO, and Cu/ZnO-CeO catalysts prepared by flame spray pyrolysis. The Cu loading and support composition were varied to understand the role of Cu-ZnO and Cu-CeO interactions. CeO addition improves Cu dispersion with respect to ZnO, owing to stronger Cu-CeO interactions. The ternary Cu/ZnO-CeO catalysts displayed a substantially higher CHOH selectivity than binary Cu/CeO and Cu/ZnO catalysts. The high CHOH selectivity in comparison with a commercial Cu-ZnO catalyst is also confirmed for Cu/ZnO-CeO catalyst prepared with high Cu loading (∼40 wt %). In situ IR spectroscopy was used to probe metal-support interactions in the reduced catalysts and to gain insight into CO hydrogenation over the Cu-Zn-Ce oxide catalysts. The higher CHOH selectivity can be explained by synergistic Cu-CeO and Cu-ZnO interactions. Cu-ZnO interactions promote CO hydrogenation to CHOH by Zn-decorated Cu active sites. Cu-CeO interactions inhibit the reverse water-gas shift reaction due to a high formate coverage of Cu and a high rate of hydrogenation of the CO intermediate to CHOH. These insights emphasize the potential of fine-tuning metal-support interactions to develop improved Cu-based catalysts for CO hydrogenation to CHOH.

摘要

将CO加氢生成CHOH对于未来的可再生能源方案来说是一个重要反应。在此，我们比较了通过火焰喷雾热解制备的Cu/ZnO、Cu/CeO和Cu/ZnO-CeO催化剂。改变Cu负载量和载体组成以了解Cu-ZnO和Cu-CeO相互作用的作用。由于更强的Cu-CeO相互作用，相对于ZnO，CeO的添加改善了Cu的分散性。三元Cu/ZnO-CeO催化剂显示出比二元Cu/CeO和Cu/ZnO催化剂高得多的CHOH选择性。对于高Cu负载量（约40 wt%）制备的Cu/ZnO-CeO催化剂，与商业Cu-ZnO催化剂相比，其高CHOH选择性也得到了证实。采用原位红外光谱法探测还原催化剂中的金属-载体相互作用，并深入了解Cu-Zn-Ce氧化物催化剂上的CO加氢反应。较高的CHOH选择性可以通过Cu-CeO和Cu-ZnO的协同相互作用来解释。Cu-ZnO相互作用通过Zn修饰的Cu活性位点促进CO加氢生成CHOH。Cu-CeO相互作用抑制了逆水煤气变换反应，这是由于Cu上的甲酸盐覆盖率高以及CO中间体加氢生成CHOH的速率高。这些见解强调了微调金属-载体相互作用以开发用于CO加氢生成CHOH的改进型Cu基催化剂的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8f16/8057230/7400373443f8/cs1c00131_0011.jpg
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