Dramatic differences in carbon dioxide adsorption and initial steps of reduction between silver and copper
Autor: | Jin Qian, Kyung Jae Lee, Ethan J. Crumlin, Hongyang Su, Hai Xiao, Tao Cheng, William A. Goddard, Yifan Ye, Junko Yano, Hao Yang |
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Jazyk: | angličtina |
Rok vydání: | 2019 |
Předmět: |
0301 basic medicine
Science Reaction mechanisms General Physics and Astronomy chemistry.chemical_element 02 engineering and technology General Biochemistry Genetics and Molecular Biology Article Catalysis Metal 03 medical and health sciences chemistry.chemical_compound Adsorption X-ray photoelectron spectroscopy MD Multidisciplinary lcsh:Science Multidisciplinary Catalytic mechanisms General Chemistry 021001 nanoscience & nanotechnology Copper Surface spectroscopy 030104 developmental biology chemistry visual_art Carbon dioxide visual_art.visual_art_medium Physical chemistry lcsh:Q 0210 nano-technology Syngas Ambient pressure Materials for energy and catalysis |
Zdroj: | Nature Communications, Vol 10, Iss 1, Pp 1-9 (2019) Nature communications, vol 10, iss 1 Nature Communications |
ISSN: | 2041-1723 |
Popis: | Converting carbon dioxide (CO2) into liquid fuels and synthesis gas is a world-wide priority. But there is no experimental information on the initial atomic level events for CO2 electroreduction on the metal catalysts to provide the basis for developing improved catalysts. Here we combine ambient pressure X-ray photoelectron spectroscopy with quantum mechanics to examine the processes as Ag is exposed to CO2 both alone and in the presence of H2O at 298 K. We find that CO2 reacts with surface O on Ag to form a chemisorbed species (O = CO2δ−). Adding H2O and CO2 then leads to up to four water attaching on O = CO2δ− and two water attaching on chemisorbed (b-)CO2. On Ag we find a much more favorable mechanism involving the O = CO2δ− compared to that involving b-CO2 on Cu. Each metal surface modifies the gas-catalyst interactions, providing a basis for tuning CO2 adsorption behavior to facilitate selective product formations. The recycling of CO2 into storable chemicals is critical in order to mitigate climate change, although CO2’s inert nature has limited the reduction’s mechanistic considerations. Here, authors pair in-situ spectroscopy with quantum mechanics to elucidate CO2 adsorption on copper and silver surfaces. |
Databáze: | OpenAIRE |
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