期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 9, 页码 2318-2323出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201610166
关键词
CO2 hydrogenation; copper; density functional theory; solid-state NMR; zirconia
资金
- SCCER-Heat and Energy Storage program
- SNF [200020_149704, PZ00P2_148059]
- ETH Career Seed Grant [SEED-21 16-2]
- Japan Society for the Promotion of Science for a fellowship (JSPS) [15J10157]
- Generalitat de Catalunya
- MINECO, Spain [CTQ2012-34153]
- Severo Ochoa Excellence Accreditation [SEV-2013-0319]
- [IZK0Z2_160957]
- Grants-in-Aid for Scientific Research [15J10157] Funding Source: KAKEN
Methanol synthesis by CO2 hydrogenation is a key process in a methanol-based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO2 to methanol still remain unknown. A mechanistic study of the hydrogenation of CO2 on Cu/ZrO2 is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO2 hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.
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