Understanding Support Effects of ZnO-Promoted Co Catalysts for Syngas Conversion to Alcohols Using Atomic Layer Deposition

被引:5
作者
Nathan, Sindhu S. [1 ]
Asundi, Arun S. [1 ]
Singh, Joseph A. [2 ]
Hoffman, Adam S. [3 ]
Boubnov, Alexey [3 ,4 ]
Hong, Jiyun [3 ]
Bare, Simon R. [3 ]
Bent, Stacey F. [1 ]
机构
[1] Stanford Univ, Dept Chem Engn, 443 Via Ortega, Stanford, CA 94305 USA
[2] Stanford Univ, Dept Chem, 443 Via Ortega, Stanford, CA 94305 USA
[3] SLAC Natl Accelerator Lab, SSRL, 2575 Sand Hill Rd, Menlo Pk, CA 94025 USA
[4] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem, D-76131 Karlsruhe, Germany
基金
美国国家科学基金会;
关键词
cobalt carbide; support effects; oxygenate synthesis; in  situ XANES; syngas; SYNTHESIS GAS CONVERSION; FISCHER-TROPSCH SYNTHESIS; COPPER-COBALT CATALYSTS; SELECTIVITY; HYDROGENATION; CARBON; CARBIDE; TRANSITION; INTERFACE; RHODIUM;
D O I
10.1002/cctc.202001630
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Co2C, an emerging catalyst for the conversion of syngas to oxygenates, shows support-sensitive behavior that has not yet been fully explained. Here, we characterize Co catalysts modified with ZnO atomic layer deposition on SiO2, carbon, CeO2, and Al2O3 supports. We find that under syngas conditions, ZnO-promoted Co transforms into Co2C on SiO2, carbon, and CeO2, but not on Al2O3. Moreover, the support affects the extent of carburization: while the SiO2-supported catalyst carburizes completely, carbon- and CeO2-supported catalysts show incomplete conversion of Co to Co2C. These three catalysts also exhibit different oxygenate selectivities. In contrast, the modified Al2O3-supported catalyst retains the Fischer-Tropsch catalytic properties of metallic Co. By depositing increasing amounts of Al2O3 by ALD on the SiO2 support, decreasing Co2C formation and oxygenate selectivity occurs. In-situ XANES reveals that Al2O3 prevents Co2C formation by enabling the ZnO to restructure into ZnAl2O4 during reduction. Thus, in addition to modifying the active catalyst phase, the promoter can also strongly interact with the support, significantly impacting catalyst performance.
引用
收藏
页码:770 / 781
页数:12
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