Kim, Cheonghee Eom, Taedaehyeong Jee, Michael Shincheon Jung, Hyejin Kim, Hyungjun Min, Byoung Koun Hwang, Yun Jeong 2024-01-20T02:32:40Z 2024-01-20T02:32:40Z 2021-09-05 2017-01 2155-5435 https://pubs.kist.re.kr/handle/201004/123263 The electrochemical CO2 reduction reaction to form valued hydrocarbon molecules is an attractive process, because it can be coupled with renewable energy resources for carbon recycling. For an efficient CO2 conversion, designing a catalyst with high activity and selectivity is crucial, because the CO2 reduction reaction in aqueous media competes with the hydrogen evolution reaction (HER) intensely. We have developed a strategy to tune CO2 reduction activity by modulating the binding energies of the intermediates on the electrocatalyst surfaces with the assistance of molecules that contain the functional group. We discovered that the amine functional group on Ag nanoparticle is highly effective in improving selective CO production (Faradaic efficiency to 94.2%) by selectively suppressing HER, while the thiol group rather increases HER activity. A density functional theory (DFT) calculation supports the theory that attaching amine molecules to Ag nanoparticles destabilizes the hydrogen binding, which effectively suppresses HER selectively, while an opposite tendency is found with thiol molecules. In addition, changes in the product selectivity, depending on the functional group, are also observed when the organic molecules are added after nanoparticle synthesis or nanoparticles are immobilized with an amine (or thiol)-containing anchoring agent. CO Faradaic efficiencies were consistently improved when the Ag nanoparticle was modified with amine groups, compared with that of its thiol counterpart. English AMER CHEMICAL SOC CARBON-DIOXIDE SILVER NANOPARTICLES ELECTROCATALYTIC REDUCTION SELECTIVE CONVERSION AU NANOPARTICLES RENEWABLE ENERGY CATALYSTS CAPTURE Insight into Electrochemical CO2 Reduction on Surface-Molecule Mediated Ag Nanoparticles Article 10.1021/acscatal.6b01862 1 ACS CATALYSIS, v.7, no.1, pp.779 - 785 ACS CATALYSIS 7 1 779 785 scie scopus 000391783200084 2-s2.0-85019974391 Chemistry, Physical Chemistry Article CARBON-DIOXIDE SILVER NANOPARTICLES ELECTROCATALYTIC REDUCTION SELECTIVE CONVERSION AU NANOPARTICLES RENEWABLE ENERGY CATALYSTS CAPTURE silver nanoparticle electrocatalyst CO2 reduction reaction selectivity