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pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
by
Chan, Karen
, Sandberg, Robert B.
, Ringe, Stefan
, Jaramillo, Thomas F.
, Hahn, Christopher
, Peng, Hongjie
, Brown, Kristopher S.
, Tang, Michael
, Liu, Xinyan
, Wang, Lei
, Schlexer, Philomena
, Xiao, Jianping
, Ji, Yongfei
, Nørskov, Jens K.
in
119/118
/ 639/301/299/886
/ 639/638/563/606
/ 639/638/563/934
/ 639/638/77/886
/ Carbon dioxide
/ Catalysis
/ Chemical engineering
/ Chemical reduction
/ Copper
/ Dependence
/ Depletion
/ Electrochemistry
/ Humanities and Social Sciences
/ Hydrocarbons
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Kinetics
/ multidisciplinary
/ pH effects
/ Reaction kinetics
/ Science
/ Science (multidisciplinary)
/ Selectivity
/ Solvents
/ Tafel slopes
2019
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pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
by
Chan, Karen
, Sandberg, Robert B.
, Ringe, Stefan
, Jaramillo, Thomas F.
, Hahn, Christopher
, Peng, Hongjie
, Brown, Kristopher S.
, Tang, Michael
, Liu, Xinyan
, Wang, Lei
, Schlexer, Philomena
, Xiao, Jianping
, Ji, Yongfei
, Nørskov, Jens K.
in
119/118
/ 639/301/299/886
/ 639/638/563/606
/ 639/638/563/934
/ 639/638/77/886
/ Carbon dioxide
/ Catalysis
/ Chemical engineering
/ Chemical reduction
/ Copper
/ Dependence
/ Depletion
/ Electrochemistry
/ Humanities and Social Sciences
/ Hydrocarbons
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Kinetics
/ multidisciplinary
/ pH effects
/ Reaction kinetics
/ Science
/ Science (multidisciplinary)
/ Selectivity
/ Solvents
/ Tafel slopes
2019
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While trying to remove the title from your shelf something went wrong :( Kindly try again later!
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pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
by
Chan, Karen
, Sandberg, Robert B.
, Ringe, Stefan
, Jaramillo, Thomas F.
, Hahn, Christopher
, Peng, Hongjie
, Brown, Kristopher S.
, Tang, Michael
, Liu, Xinyan
, Wang, Lei
, Schlexer, Philomena
, Xiao, Jianping
, Ji, Yongfei
, Nørskov, Jens K.
in
119/118
/ 639/301/299/886
/ 639/638/563/606
/ 639/638/563/934
/ 639/638/77/886
/ Carbon dioxide
/ Catalysis
/ Chemical engineering
/ Chemical reduction
/ Copper
/ Dependence
/ Depletion
/ Electrochemistry
/ Humanities and Social Sciences
/ Hydrocarbons
/ INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
/ Kinetics
/ multidisciplinary
/ pH effects
/ Reaction kinetics
/ Science
/ Science (multidisciplinary)
/ Selectivity
/ Solvents
/ Tafel slopes
2019
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pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
Journal Article
pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper
2019
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Overview
We present a microkinetic model for CO
(2)
reduction (CO
(2)
R) on Cu(211) towards C
2
products, based on energetics estimated from an explicit solvent model. We show that the differences in both Tafel slopes and pH dependence for C
1
vs C
2
activity arise from differences in their multi-step mechanisms. We find the depletion in C
2
products observed at high overpotential and high pH to arise from the 2
nd
order dependence of C-C coupling on CO coverage, which decreases due to competition from the C
1
pathway. We further demonstrate that CO
(2)
reduction at a fixed pH yield similar activities, due to the facile kinetics for CO
2
reduction to CO on Cu, which suggests C
2
products to be favored for CO
2
R under alkaline conditions. The mechanistic insights of this work elucidate how reaction conditions can lead to significant enhancements in selectivity and activity towards higher value C
2
products.
CO
2
conversion to reduced products provides a use for greenhouse gases, but reaction complexity stymies mechanistic studies. Here, authors present a microkinetic model for CO
2
and CO reduction on copper, based on ab initio simulations, to elucidate pH’s impact on competitive reaction pathways.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
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