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Abstract
Tuning surface structures by bottom-up synthesis has been demonstrated as an effective strategy to improve the catalytic performances of nanoparticle catalysts. Nevertheless, the surface modification of three-dimensional nanoporous metals, fabricated by a top-down dealloying approach, has not been achieved despite great efforts devoted to improving the catalytic performance of three-dimensional nanoporous catalysts. Here we report a surfactant-modified dealloying method to tailor the surface structure of nanoporous gold for amplified electrocatalysis toward methanol oxidation and oxygen reduction reactions. With the assistance of surfactants, {111} or {100} faceted internal surfaces of nanoporous gold can be realized in a controllable manner by optimizing dealloying conditions. The surface modified nanoporous gold exhibits significantly enhanced electrocatalytic activities in comparison with conventional nanoporous gold. This study paves the way to develop high-performance three-dimensional nanoporous catalysts with a tunable surface structure by top-down dealloying for efficient chemical and electrochemical reactions.
Highlights
Tuning surface structures by bottom-up synthesis has been demonstrated as an effective strategy to improve the catalytic performances of nanoparticle catalysts
Unlike low-dimensional nanostructured materials, which are usually synthesized by bottom-up chemical approaches, 3D nanoporous metals, such as nanoporous gold (NPG), are fabricated by a top-down dealloying method
Different from nanoparticle catalysts, the selection of terminal surfaces of nanopore channels is determined by the surface/interface energy of crystalline ligaments and involves surface stresses, from the confinement of precursor substrates and complicated kinetic factors during top-down dealloying. It is important in basic research and technical applications, tailoring the surface structure of nanoporous catalysts has not been fulfilled at the crystallographic level and it remains unknown whether the surface structure of 3D nanoporous catalysts can be controlled by the top-down dealloying to optimize their catalytic performances
Summary
Tuning surface structures by bottom-up synthesis has been demonstrated as an effective strategy to improve the catalytic performances of nanoparticle catalysts. Different from nanoparticle catalysts, the selection of terminal surfaces of nanopore channels is determined by the surface/interface energy of crystalline ligaments and involves surface stresses, from the confinement of precursor substrates and complicated kinetic factors during top-down dealloying It is important in basic research and technical applications, tailoring the surface structure of nanoporous catalysts has not been fulfilled at the crystallographic level and it remains unknown whether the surface structure of 3D nanoporous catalysts can be controlled by the top-down dealloying to optimize their catalytic performances. Na3CA-NPG) with an abundance of {100} facets and step/kink sites have been successfully realized These surface-engineered NPG catalysts with preferred surface structures show a significant improvement in catalytic activities toward methanol oxidation reaction (MOR) and ORR in comparison with conventional NPG (C-NPG)
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