期刊
NANO RESEARCH
卷 16, 期 4, 页码 4723-4728出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-022-5159-8
关键词
molecular surface functionalization; Au nanoparticles; macrocyclic molecule; tunable CO2 enrichment; electrochemical CO2 reduction reaction
By modifying gold nanoparticles (Au NPs) with the macrocyclic molecule cucurbit[6]uril (Au@CB[6]), we report a hybrid nanomaterial based on Au. Au@CB[6] exhibits the optimal selectivity for CO, with the highest CO Faraday efficiency (FECO) reaching 99.50% at -0.6 V vs. reversible hydrogen electrode (RHE). The partial current density of CO formed by Au@CB[6] increases dramatically to 3.18 mA/cm(2) at -0.6 V, which is more than ten times greater than that of oleylamine-coated Au NPs (Au@OAm, 0.31 mA/cm(2)). Operando electrochemical measurement combined with density functional theory (DFT) calculations reveals that CB[6] can gather CO2 and increase the localized CO2 concentration near the metal interface, resulting in significantly enhanced electrochemical CO2 reduction reaction (CO2RR) performance.
Electrochemical conversion of carbon dioxide (CO2) to higher-value products provides a forward-looking way to solve the problems of environmental pollution and energy shortage. However, the low solubility of CO2 in aqueous electrolytes, sluggish kinetics, and low selectivity hamper the efficient conversion of CO2. Here, we report a Au-based hybrid nanomaterial by modifying Au nanoparticles (NPs) with the macrocyclic molecule cucurbit[6]uril (Au@CB[6]). Au@CB[6] displays the optimal selectivity of CO, with the highest CO Faraday efficiency (FECO) reaching 99.50% at -0.6 V vs. reversible hydrogen electrode (RHE). The partial current density of CO formed by Au@CB[6] increases dramatically, as 3.18 mA/cm(2) at -0.6 V, which is more than ten times as that of oleylamine-coated Au NPs (Au@OAm, 0.31 mA/cm(2)). Operando electrochemical measurement combined with density functional theory (DFT) calculations reveals that CB[6] can gather CO2 and lead the increased local CO2 concentration near metal interface, which realizes significantly enhanced electrochemical CO2 reduction reaction (CO2RR) performance.
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