期刊
ACS CATALYSIS
卷 11, 期 19, 页码 12208-12219出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c00591
关键词
CO2 reduction reaction; capped-gold nanoparticles; dithiocarbamate; online DEMS; CO selectivity
资金
- Sao Paulo Research Foundation (FAPESP) [2016/13323-0, 2013/16930-7, 2019/22183-6, 2018/10415-7]
- CNPq (Conselho Nacional de Desenvolvimento Cientifico e Tecnologico) [309465/2019-2]
- CAPES (Coordenacao de Aperfeicoamento de Pessoal de Nivel Superior)
- FAPESP, Brazil [2013/07296-2]
- Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP) [16/13323-0] Funding Source: FAPESP
Gold nanoparticles functionalized with dibenzyldithiocarbamate (DBDTC-Au NPs) were synthesized in the lab, displaying excellent electrocatalytic activity for the reduction of CO2 to CO. The strong bonding and stability of the DBDTC ligand on the Au nanoparticles played a crucial role in enhancing CO formation efficiency. Through online differential electrochemical mass spectrometry (DEMS) experiments and gas chromatography (GC) analysis, it was demonstrated that the DBDTC-Au catalyst achieved high faradaic efficiency and selectivity for CO production.
Dibenzyldithiocarbamate-functionalized gold nanoparticles (DBDTC-Au NPs) were synthesized in the laboratory, and the effects of the DBDTC ligand on the Au electrocatalytic activity for CO2 reduction reaction to CO were investigated in CO2-saturated KHCO3 electrolyte. Our synthesis route produced sub-2.0 nm Au particles, with the number of gold atoms in the range of 67-120, and with strongly bonded and stable DBDTC ligands on the surface. Online differential electrochemical mass spectrometry (DEMS) experiments on the DBDTC-Au nanoparticles showed higher faradic current and higher CO/H-2 ratio of their ionic signals compared to those for citrate-capped Au NPs. Quantitative analyses via gas chromatography (GC) showed that our DBDTC-Au catalyst converts CO2 into CO with a faradic efficiency of approximately 100 +/- 1% at -0.8 V and 93 +/- 0.5% at -1.0 V vs RHE. The higher activity of the synthesized DBDTC-Au electrocatalyst was attributed to the following important functionalities of the DBDTC ligand: (i) the strong bonding to the surface stabilizes the Au NPs, inhibiting the formation of large agglomerates, and (ii) the hydrophobic character of the dibenzyl moieties allows the permeation of CO2, but repels water from the Au surface, minimizing the electrochemical reduction of water and, therefore, enhancing the faradic efficiency for CO formation.
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