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Nanocluster Surface Microenvironment Modulates Electrocatalytic CO<sub>2</sub> Reduction
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- Citation
- Advanced Materials, Vol.36 No.13
- Abstract
- The catalytic activity and product selectivity of the electrochemical CO2 reduction reaction (eCO(2)RR) 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 Ag-25 cluster dramatically enhances the eCO(2)RR activity (CO Faradaic efficiency, FECO: 90.3%) with higher CO partial current density (j(CO)) in an H-cell compared to Ag-25 cluster (FECO: 66.6%) with confined hydrophilicity, which modulates surface interactions with water and CO2. Remarkably, the hydrophobic Ag-25 cluster exhibits j(CO) 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 eCO(2)RR 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 eCO(2)RR activity, which provides atomistic mechanistic insights into the crucial role of confined hydrophobicity.
- ISSN
- 0935-9648
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