Atomically Dispersed Cu Catalysts on Sulfide-Derived Defective Ag Nanowires for Electrochemical CO₂ Reduction
Date
2023
Authors
Ma, Z.
Wan, T.
Zhang, D.
Yuwono, J.A.
Tsounis, C.
Jiang, J.
Chou, Y.-H.
Lu, X.
Kumar, P.V.
Ng, Y.H.
Editors
Advisors
Journal Title
Journal ISSN
Volume Title
Type:
Journal article
Citation
ACS Nano, 2023; 17(3):2387-2398
Statement of Responsibility
Zhipeng 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
Conference Name
Abstract
Single-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.
School/Discipline
Dissertation Note
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Description
Published: February 2, 2023
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© 2023 American Chemical Society