Atomically Dispersed Cu Catalysts on Sulfide-Derived Defective Ag Nanowires for Electrochemical CO₂ Reduction

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dc.contributor.authorMa, Z.
dc.contributor.authorWan, T.
dc.contributor.authorZhang, D.
dc.contributor.authorYuwono, J.A.
dc.contributor.authorTsounis, C.
dc.contributor.authorJiang, J.
dc.contributor.authorChou, Y.-H.
dc.contributor.authorLu, X.
dc.contributor.authorKumar, P.V.
dc.contributor.authorNg, Y.H.
dc.contributor.authorChu, D.
dc.contributor.authorToe, C.Y.
dc.contributor.authorHan, Z.
dc.contributor.authorAmal, R.
dc.date.issued2023
dc.descriptionPublished: February 2, 2023
dc.description.abstractSingle-atom catalysts (SACs) have shown potential for achieving an efficient electrochemical CO2 reduction reaction (CO2RR) despite challenges in their synthesis. Here, Ag2S/Ag nanowires provide initial anchoring sites for Cu SACs (Cu/Ag2S/Ag), then Cu/Ag(S) was synthesized by an electrochemical treatment resulting in complete sulfur removal, i.e., Cu SACs on a defective Ag surface. The CO2RR Faradaic efficiency (FECO2RR) of Cu/Ag(S) reaches 93.0% at a CO2RR partial current density (jCO2RR) of 2.9 mA/cm2 under −1.0 V vs RHE, which outperforms sulfur-removed Ag2S/Ag without Cu SACs (Ag(S), 78.5% FECO2RR with 1.8 mA/cm2jCO2RR). At −1.4 V vs RHE, both FECO2RR and jCO2RR over Cu/Ag(S) reached 78.6% and 6.1 mA/cm2, which tripled those over Ag(S), respectively. As revealed by in situ and ex situ characterizations together with theoretical calculations, the interacted Cu SACs and their neighboring defective Ag surface increase microstrain and downshift the d-band center of Cu/Ag(S), thus lowering the energy barrier by ∼0.5 eV for *CO formation, which accounts for the improved CO2RR activity and selectivity toward related products such as CO and C2+ products.
dc.description.statementofresponsibilityZhipeng Ma, Tao Wan, Ding Zhang, Jodie A. Yuwono, Constantine Tsounis, Junjie Jiang, Yu-Hsiang Chou, Xunyu Lu, Priyank V. Kumar, Yun Hau Ng, Dewei Chu, Cui Ying Toe, Zhaojun Han, and Rose Amal
dc.identifier.citationACS Nano, 2023; 17(3):2387-2398
dc.identifier.doi10.1021/acsnano.2c09473
dc.identifier.issn1936-0851
dc.identifier.issn1936-086X
dc.identifier.orcidYuwono, J.A. [0000-0002-0915-0756]
dc.identifier.urihttps://hdl.handle.net/2440/137620
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.granthttp://purl.org/au-research/grants/arc/IC200100023
dc.relation.granthttp://purl.org/au-research/grants/arc/DE190100131
dc.rights© 2023 American Chemical Society
dc.source.urihttps://doi.org/10.1021/acsnano.2c09473
dc.subjectCu single atom catalysts; defective Ag nanowire; underpotential electrochemical deposition; synergistic effects; electrochemical CO₂ reduction
dc.titleAtomically Dispersed Cu Catalysts on Sulfide-Derived Defective Ag Nanowires for Electrochemical CO₂ Reduction
dc.title.alternativeAtomically Dispersed Cu Catalysts on Sulfide-Derived Defective Ag Nanowires for Electrochemical CO2 Reduction
dc.typeJournal article
pubs.publication-statusPublished

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