期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 18, 页码 7672-7678出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c02011
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资金
- European Integrated Center for the Development of New Metallic Alloys and Compounds
- COMETE project (COnception in silico de Materiaux pour l'EnvironnemenT et l'Energie)
- European Union under the program FEDER-FSE Lorraine et Massif des Vosges 2014-2020
- EXPLOR centre by the University de Lorraine [2017M4XXX0108]
The tunability offered by alloying different elements is useful to design catalysts with greater activity, selectivity, and stability than single metals. By comparing the Pd(111) and PdZn(111) model catalysts for CO2 hydrogenation to methanol, we show that intermetallic alloying is a possible strategy to control the reaction pathway from the tuning of adsorbate binding energies. In comparison to Pd, the strong electron-donor character of PdZn weakens the adsorption of carbon-bound species and strengthens the binding of oxygen-bound species. As a consequence, the first step of CO2 hydrogenation more likely leads to the formate intermediate on PdZn, while the carboxyl intermediate is preferentially formed on Pd. This results in the opening of a pathway from carbon dioxide to methanol on PdZn similar to that previously proposed on Cu. These findings rationalize the superiority of PdZn over Pd for CO2 conversion into methanol and suggest guidance for designing more efficient catalysts by promoting the proper reaction intermediates.
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