Cu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO

Handle URI:
http://hdl.handle.net/10754/603956
Title:
Cu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO
Authors:
Sarfraz, Saad; Garcia Esparza, Angel T. ( 0000-0002-4884-171X ) ; Jedidi, Abdesslem ( 0000-0003-4070-3299 ) ; Cavallo, Luigi ( 0000-0002-1398-338X ) ; Takanabe, Kazuhiro ( 0000-0001-5374-9451 )
Abstract:
We report a selective and stable electrocatalyst utilizing non-noble metals consisting of Cu and Sn for the efficient and selective reduction of CO2 to CO over a wide potential range. The bimetallic electrode was prepared through the electrodeposition of Sn species on the surface of oxide-derived copper (OD-Cu). The Cu surface, when decorated with an optimal amount of Sn, resulted in a Faradaic efficiency (FE) for CO greater than 90% and a current density of −1.0 mA cm−2 at −0.6 V vs. RHE, compared to the CO FE of 63% and −2.1 mA cm−2 for OD-Cu. Excess Sn on the surface caused H2 evolution with a decreased current density. X-ray diffraction (XRD) suggests the formation of Cu-Sn alloy. Auger electron spectroscopy of the sample surface exhibits zero-valent Cu and Sn after the electrodeposition step. Density functional theory (DFT) calculations show that replacing a single Cu atom with a Sn atom leaves the d-band orbitals mostly unperturbed, signifying no dramatic shifts in the bulk electronic structure. However, the Sn atom discomposes the multi-fold sites on pure Cu, disfavoring the adsorption of H and leaving the adsorption of CO relatively unperturbed. Our catalytic results along with DFT calculations indicate that the presence of Sn on reduced OD-Cu diminishes the hydrogenation capability—i.e., the selectivity towards H2 and HCOOH—while hardly affecting the CO productivity. While the pristine monometallic surfaces (both Cu and Sn) fail to selectively reduce CO2, the Cu-Sn bimetallic electrocatalyst generates a surface that inhibits adsorbed H*, resulting in improved CO FE. This study presents a strategy to provide a low-cost non-noble metals that can be utilized as a highly selective electrocatalyst for the efficient aqueous reduction of CO2.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division
Citation:
Cu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO 2016 ACS Catalysis
Publisher:
American Chemical Society (ACS)
Journal:
ACS Catalysis
Issue Date:
23-Mar-2016
DOI:
10.1021/acscatal.6b00269
Type:
Article
ISSN:
2155-5435; 2155-5435
Sponsors:
The research reported in this publication was supported by King Abdullah University of Science and Technology (KAUST). Furthermore, we are also thankful to Dr. Shahid Rasul at KAUST for the helpful discussions. We are also grateful for the computational resources acquired from KAUST Supercomputing Laboratory using the supercomputer Shaheen II under the project k1016.
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/acscatal.6b00269
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorSarfraz, Saaden
dc.contributor.authorGarcia Esparza, Angel T.en
dc.contributor.authorJedidi, Abdesslemen
dc.contributor.authorCavallo, Luigien
dc.contributor.authorTakanabe, Kazuhiroen
dc.date.accessioned2016-03-30T07:20:18Zen
dc.date.available2016-03-30T07:20:18Zen
dc.date.issued2016-03-23en
dc.identifier.citationCu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to CO 2016 ACS Catalysisen
dc.identifier.issn2155-5435en
dc.identifier.issn2155-5435en
dc.identifier.doi10.1021/acscatal.6b00269en
dc.identifier.urihttp://hdl.handle.net/10754/603956en
dc.description.abstractWe report a selective and stable electrocatalyst utilizing non-noble metals consisting of Cu and Sn for the efficient and selective reduction of CO2 to CO over a wide potential range. The bimetallic electrode was prepared through the electrodeposition of Sn species on the surface of oxide-derived copper (OD-Cu). The Cu surface, when decorated with an optimal amount of Sn, resulted in a Faradaic efficiency (FE) for CO greater than 90% and a current density of −1.0 mA cm−2 at −0.6 V vs. RHE, compared to the CO FE of 63% and −2.1 mA cm−2 for OD-Cu. Excess Sn on the surface caused H2 evolution with a decreased current density. X-ray diffraction (XRD) suggests the formation of Cu-Sn alloy. Auger electron spectroscopy of the sample surface exhibits zero-valent Cu and Sn after the electrodeposition step. Density functional theory (DFT) calculations show that replacing a single Cu atom with a Sn atom leaves the d-band orbitals mostly unperturbed, signifying no dramatic shifts in the bulk electronic structure. However, the Sn atom discomposes the multi-fold sites on pure Cu, disfavoring the adsorption of H and leaving the adsorption of CO relatively unperturbed. Our catalytic results along with DFT calculations indicate that the presence of Sn on reduced OD-Cu diminishes the hydrogenation capability—i.e., the selectivity towards H2 and HCOOH—while hardly affecting the CO productivity. While the pristine monometallic surfaces (both Cu and Sn) fail to selectively reduce CO2, the Cu-Sn bimetallic electrocatalyst generates a surface that inhibits adsorbed H*, resulting in improved CO FE. This study presents a strategy to provide a low-cost non-noble metals that can be utilized as a highly selective electrocatalyst for the efficient aqueous reduction of CO2.en
dc.description.sponsorshipThe research reported in this publication was supported by King Abdullah University of Science and Technology (KAUST). Furthermore, we are also thankful to Dr. Shahid Rasul at KAUST for the helpful discussions. We are also grateful for the computational resources acquired from KAUST Supercomputing Laboratory using the supercomputer Shaheen II under the project k1016.en
dc.language.isoenen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/acscatal.6b00269en
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/acscatal.6b00269.en
dc.titleCu-Sn Bimetallic Catalyst for Selective Aqueous Electroreduction of CO2 to COen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalACS Catalysisen
dc.eprint.versionPost-printen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorSarfraz, Saaden
kaust.authorGarcia Esparza, Angel T.en
kaust.authorJedidi, Abdesslemen
kaust.authorCavallo, Luigien
kaust.authorTakanabe, Kazuhiroen
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