Atomic-Precise Active Site Surgery on Carboranylthiolate-Protected Silver Nanocluster Catalysts DOI
Jia‐Hong Huang, Han Zhang, Zhao‐Yang Wang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 30, 2025

Although significant progress has been made in precisely modulating the composition and structure of metal nanoclusters to tailor their properties, well-controlled synthesis with unsaturated coordination environments highly active sites enhance catalytic performance remains remarkably challenging. Here, we propose an atomic-level surgical strategy involving stepwise creation manipulation on nanoclusters. A newly constructed Ag17P nanocluster, costabilized by carboranethiolate phosphine ligands, features Ag13 icosahedral kernel capped four tetrahedrally symmetrical silver atoms. Taking advantage ligands readily dissociating from peripheral atoms under solvent regulation, could transform into Ag17 exposed Furthermore, site-specific substitution be accomplished these open through a judicious choice heterometal, resulting isostructural Cu-doping Ag13Cu4 nanocluster. As result, showed improved activities electrocatalytic nitrate reduction reaction (NO3RR) compared Ag17P, displayed superior optimal faradaic efficiency (FE) 90.4 ± 0.2% for NH3 production total FE 99.6 0.3%. This study not only offers pathway generating manipulating but also provides new perspectives design efficient nanocluster-based materials.

Language: Английский

Atomic-Precise Active Site Surgery on Carboranylthiolate-Protected Silver Nanocluster Catalysts DOI
Jia‐Hong Huang, Han Zhang, Zhao‐Yang Wang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 30, 2025

Although significant progress has been made in precisely modulating the composition and structure of metal nanoclusters to tailor their properties, well-controlled synthesis with unsaturated coordination environments highly active sites enhance catalytic performance remains remarkably challenging. Here, we propose an atomic-level surgical strategy involving stepwise creation manipulation on nanoclusters. A newly constructed Ag17P nanocluster, costabilized by carboranethiolate phosphine ligands, features Ag13 icosahedral kernel capped four tetrahedrally symmetrical silver atoms. Taking advantage ligands readily dissociating from peripheral atoms under solvent regulation, could transform into Ag17 exposed Furthermore, site-specific substitution be accomplished these open through a judicious choice heterometal, resulting isostructural Cu-doping Ag13Cu4 nanocluster. As result, showed improved activities electrocatalytic nitrate reduction reaction (NO3RR) compared Ag17P, displayed superior optimal faradaic efficiency (FE) 90.4 ± 0.2% for NH3 production total FE 99.6 0.3%. This study not only offers pathway generating manipulating but also provides new perspectives design efficient nanocluster-based materials.

Language: Английский

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