4 years ago

Site-Selective Growth of AgPd Nanodendrite-Modified Au Nanoprisms: High Electrocatalytic Performance for CO2 Reduction

Site-Selective Growth of AgPd Nanodendrite-Modified Au Nanoprisms: High Electrocatalytic Performance for CO2 Reduction
Jeffrey M. Zaleski, Erin T. Martin, Changsheng Shan, Dennis G. Peters
Environmental impacts of continued CO2 production have led to an increased need for new methods of CO2 removal and energy development. Nanomaterials are of special interest for these applications, because of their unique chemical and physical properties that allow for highly active surfaces. Here, we successfully synthesize AgPd nanodendrite-modified Au nanoprisms in various shapes (nanoprisms, hexagonal nanoplates, and octahedral nanoparticles) by selective metal deposition. This strategy involves coupling galvanic replacement between Ag layers in Au@Ag core–shell nanoprisms and H2PdCl4 with a coreduction process of silver and palladium ions. Synthesis of AgPd nanodendrite-tipped (4.14–11.47 wt % Pd) and -edged (25.25–31.01 wt % Pd) Au nanoparticles can be controlled simply by tuning the concentration of H2PdCl4. More importantly, these multicomponent AgPd nanodendrite-modified Au nanoparticles show exceptional electrocatalytic performance for CO2 reduction. AgPd nanodendrite-edged Au nanoprisms show more favorable potentials (−0.18 V vs RHE) than previously reported nanocatalysts for the reduction of CO2 to formate, and exhibit higher faradaic efficiencies (49%) than Au, Au@Ag, and AgPd nanodendrite-tipped Au nanoprisms in aqueous electrolytes. Moreover, AgPd nanodendrite-modified Au nanoprisms show much higher selectivity and faradaic efficiency for CO2 reduction to CO (85–87%) than Au and Au@Ag nanoprisms (43–64%) in organic electrolytes. The high performance of these particles for CO2 reduction is attributed to the unique structure of AgPd nanodendrite-modified Au nanoprisms and the synergistic effect of Ag having an affinity for CO2, efficient binding of hydrogen at Pd, and Au as a stable, conductive support. In addition, AgPd nanodendrite-edged Au nanoprisms show highly stable catalytic activity during long-term electrolyses (up to 12 h) and repetitive use. These exciting results indicate that AgPd nanodendrite-modified Au nanoparticles are promising for application in CO2 conversion into useful fuels.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b01813

DOI: 10.1021/acs.chemmater.7b01813

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