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Nanocluster Surface Microenvironment Modulates Electrocatalytic CO2 Reduction

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Title
Nanocluster Surface Microenvironment Modulates Electrocatalytic CO2 Reduction
Author(s)
Seungwoo Yoo; Suhwan Yoo; Guocheng Deng; Sun, Fang; Kangjae Lee; Hyunsung Jang; Chan Woo Lee; Xiaolin Liu; Junghwan Jang; Tang, Qing; Yun Jeong Hwang; Taeghwan Hyeon; Megalamane S. Bootharaju
Publication Date
2024-03
Journal
Advanced Materials, v.36, no.13
Publisher
WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Abstract
The catalytic activity and product selectivity of the electrochemical CO2 reduction reaction (eCO2RR) depend strongly on the local microenvironment of mass diffusion at the nanostructured catalyst and electrolyte interface. Achieving a molecular-level understanding of the electrocatalytic reaction requires the development of tunable metal-ligand interfacial structures with atomic precision, which is highly challenging. Here, the synthesis and molecular structure of a 25-atom silver nanocluster interfaced with an organic shell comprising 18 thiolate ligands are presented. The locally induced hydrophobicity by bulky alkyl functionality near the surface of the Ag25 cluster dramatically enhances the eCO2RR activity (CO Faradaic efficiency, FECO: 90.3%) with higher CO partial current density (jCO) in an H-cell compared to Ag25 cluster (FECO: 66.6%) with confined hydrophilicity, which modulates surface interactions with water and CO2. Remarkably, the hydrophobic Ag25 cluster exhibits jCO as high as −240 mA cm−2 with FECO >90% at −3.4 V cell potential in a gas-fed membrane electrode assembly device. Furthermore, this cluster demonstrates stable eCO2RR over 120 h. Operando surface-enhanced infrared absorption spectroscopy and theoretical simulations reveal how the ligands alter the neighboring water structure and *CO intermediates, impacting the intrinsic eCO2RR activity, which provides atomistic mechanistic insights into the crucial role of confined hydrophobicity. © 2023 Wiley-VCH GmbH.
URI
https://pr.ibs.re.kr/handle/8788114/15368
DOI
10.1002/adma.202313032
ISSN
0935-9648
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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