期刊
JOURNAL OF CATALYSIS
卷 380, 期 -, 页码 153-160出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.10.013
关键词
CO2 hydrogenation; Ag; Lewis acidic supports; Formates; Operando DRIFTS
资金
- Swiss National Science Foundation (SNF), Switzerland [CRSII2-154448]
- Generalitat de Catalunya through the CERCA Programme
- MINECO, Spain [CTQ2016-75499-R]
- SCCER Heat and Energy Storage
- Swiss National Science Foundation (SNF) [CRSII2_154448] Funding Source: Swiss National Science Foundation (SNF)
Silica-supported silver nanoparticles exhibit outstanding efficiency in the CO2 hydrogenation to methyl formate in the presence of methanol under high pressure. Here, we show that ZrO2 and Al2O3 supports significantly increase the catalyst activity, in line with their higher Lewis acidity. The weight time yield of methyl formate over Ag/ZrO2 is up to 16.2 g(MF)g(Ag) h(-1) without detectable side-products, 25 times higher compared to Ag/SiO2 at the same temperature. Transient in situ and operando DRIFTS studies uncover spillover processes of formate species from Ag onto the acidic support materials and show that the surface formates can further react with adsorbed methanol at the sites near the perimeter between Ag and the support to yield methyl formate. (C) 2019 The Author(s). Published by Elsevier Inc.
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