Journal
CHEMPHYSCHEM
Volume 18, Issue 22, Pages 3266-3273Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201700736
Keywords
classification; CO2 reduction; electrochemistry; formaldehyde reduction; scaling relation
Funding
- Climate-KIC under the EnCO2re project
- Carlsberg Foundation [CF15-0165]
- Innovation Fund Denmark [ProActivE 5124-00003A]
- German Federal Ministry for Education and Research (BMBF) under project CO2EKAT [03SF0523]
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In this work, we propose four non-coupled binding energies of intermediates as descriptors, or genes, for predicting the product distribution in CO2 electroreduction. Simple reactions can be understood by the Sabatier principle (catalytic activity vs. one descriptor), while more complex reactions tend to give multiple very different products and consequently the product selectivity is a more complex property to understand. We approach this, as a logistical classification problem, by grouping metals according to their major experimental product from CO2 electroreduction: H-2, CO, formic acid and beyond CO* (hydrocarbons or alcohols). We compare the groups in terms of multiple binding energies of intermediates calculated by density functional theory. Here, we find three descriptors to explain the grouping: the adsorption energies of H*, COOH*, and CO*. To further classify products beyond CO*, we carry out formaldehyde experiments on Cu, Ag, and Au and combine these results with the literature to group and differentiate alcohol or hydrocarbon products. We find that the oxygen binding (adsorption energy of CH3O*) is an additional descriptor to explain the alcohol formation in reduction processes. Finally, the adsorption energy of the four intermediates, H*, COOH*, CO*, and CH3O*, can be used to differentiate, group, and explain products in electrochemical reduction processes involving CO2, CO, and carbon-oxygen compounds.
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