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A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
by
Lee, Geonhui
, Li, Yuhang
, Peng, Tao
, Yan, Yu
, Cervantes, Eduardo González
, Wang, Ning
, Hung, Sung-Fu
, Wicks, Joshua
, Hsu, Shao-Hui
, Luo, Mingchuan
, Xu, Aoni
, Wang, Xue
, Li, Yuguang C.
, Nam, Dae-Hyun
, Sargent, Edward H.
, Rasouli, Armin Sedighian
, Li, Fengwang
in
119/118
/ 140/133
/ 147/135
/ 147/143
/ 147/3
/ 639/301/299/886
/ 639/638/675
/ 639/638/77/886
/ Absorption spectroscopy
/ Adsorption
/ Carbon dioxide
/ Carbon monoxide
/ Carbon neutrality
/ Catalysts
/ Catalytic converters
/ Chemical reduction
/ Copper
/ Copper converters
/ Density functional theory
/ Electrocatalysis
/ Energy
/ Graphene
/ Humanities and Social Sciences
/ Hydrogenation
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ Iron
/ Metal phthalocyanines
/ Methane
/ multidisciplinary
/ Nitrogen
/ Raman spectroscopy
/ Science
/ Science (multidisciplinary)
/ Single atom catalysts
/ Spectrum analysis
/ X ray absorption
/ X-ray absorption spectroscopy
2022
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A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
by
Lee, Geonhui
, Li, Yuhang
, Peng, Tao
, Yan, Yu
, Cervantes, Eduardo González
, Wang, Ning
, Hung, Sung-Fu
, Wicks, Joshua
, Hsu, Shao-Hui
, Luo, Mingchuan
, Xu, Aoni
, Wang, Xue
, Li, Yuguang C.
, Nam, Dae-Hyun
, Sargent, Edward H.
, Rasouli, Armin Sedighian
, Li, Fengwang
in
119/118
/ 140/133
/ 147/135
/ 147/143
/ 147/3
/ 639/301/299/886
/ 639/638/675
/ 639/638/77/886
/ Absorption spectroscopy
/ Adsorption
/ Carbon dioxide
/ Carbon monoxide
/ Carbon neutrality
/ Catalysts
/ Catalytic converters
/ Chemical reduction
/ Copper
/ Copper converters
/ Density functional theory
/ Electrocatalysis
/ Energy
/ Graphene
/ Humanities and Social Sciences
/ Hydrogenation
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ Iron
/ Metal phthalocyanines
/ Methane
/ multidisciplinary
/ Nitrogen
/ Raman spectroscopy
/ Science
/ Science (multidisciplinary)
/ Single atom catalysts
/ Spectrum analysis
/ X ray absorption
/ X-ray absorption spectroscopy
2022
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A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
by
Lee, Geonhui
, Li, Yuhang
, Peng, Tao
, Yan, Yu
, Cervantes, Eduardo González
, Wang, Ning
, Hung, Sung-Fu
, Wicks, Joshua
, Hsu, Shao-Hui
, Luo, Mingchuan
, Xu, Aoni
, Wang, Xue
, Li, Yuguang C.
, Nam, Dae-Hyun
, Sargent, Edward H.
, Rasouli, Armin Sedighian
, Li, Fengwang
in
119/118
/ 140/133
/ 147/135
/ 147/143
/ 147/3
/ 639/301/299/886
/ 639/638/675
/ 639/638/77/886
/ Absorption spectroscopy
/ Adsorption
/ Carbon dioxide
/ Carbon monoxide
/ Carbon neutrality
/ Catalysts
/ Catalytic converters
/ Chemical reduction
/ Copper
/ Copper converters
/ Density functional theory
/ Electrocatalysis
/ Energy
/ Graphene
/ Humanities and Social Sciences
/ Hydrogenation
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Intermediates
/ Iron
/ Metal phthalocyanines
/ Methane
/ multidisciplinary
/ Nitrogen
/ Raman spectroscopy
/ Science
/ Science (multidisciplinary)
/ Single atom catalysts
/ Spectrum analysis
/ X ray absorption
/ X-ray absorption spectroscopy
2022
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A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
Journal Article
A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
2022
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Overview
Nitrogen-doped graphene-supported single atoms convert CO
2
to CO, but fail to provide further hydrogenation to methane – a finding attributable to the weak adsorption of CO intermediates. To regulate the adsorption energy, here we investigate the metal-supported single atoms to enable CO
2
hydrogenation. We find a copper-supported iron-single-atom catalyst producing a high-rate methane. Density functional theory calculations and in-situ Raman spectroscopy show that the iron atoms attract surrounding intermediates and carry out hydrogenation to generate methane. The catalyst is realized by assembling iron phthalocyanine on the copper surface, followed by in-situ formation of single iron atoms during electrocatalysis, identified using operando X-ray absorption spectroscopy. The copper-supported iron-single-atom catalyst exhibits a CO
2
-to-methane Faradaic efficiency of 64% and a partial current density of 128 mA cm
−2
, while the nitrogen-doped graphene-supported one produces only CO. The activity is 32 times higher than a pristine copper under the same conditions of electrolyte and bias.
Converting CO2 and H2O into value-added chemical feedstocks and fuels offers a carbon neutral approach to tackling global energy and climate concerns. Here the authors report a metal supported single-atom catalytic site enabling the electrocatalytic reduction of CO2 to methane.
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