A Heteroleptic Gold Hydride Nanocluster for Efficient and Selective Electrocatalytic Reduction of CO₂ to CO
2022
Gao, Ze-Hua | Wei, Kecheng | Wu, Tao | Dong, Jia | Jiang, De'en | Sun, Shouheng | Wang, Lai-Sheng
It has been a long-standing challenge to create and identify the active sites of heterogeneous catalysts, because it is difficult to precisely control the interfacial chemistry at the molecular level. Here we report the synthesis and catalysis of a heteroleptic gold trihydride nanocluster, [Au₂₂H₃(dppe)₃(PPh₃)₈]³⁺ [dppe = 1,2-bis(diphenylphosphino)ethane, PPh₃ = triphenylphosphine]. The Au₂₂H₃ core consists of two Au₁₁ units bonded via six uncoordinated Au sites. The three H atoms bridge the six uncoordinated Au atoms and are found to play a key role in catalyzing electrochemical reduction of CO₂ to CO with a 92.7% Faradaic efficiency (FE) at −0.6 V (vs RHE) and high reaction activity (134 A/gAᵤ mass activity). The CO current density and FECO remained nearly constant for the CO₂ reduction reaction for more than 10 h, indicating remarkable stability of the Au₂₂H₃ catalyst. The Au₂₂H₃ catalytic performance is among the best Au-based catalysts reported thus far for electrochemical reduction of CO₂. Density functional theory (DFT) calculations suggest that the hydride coordinated Au sites are the active centers, which facilitate the formation of the key *COOH intermediate.
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