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Article Dans Une Revue Angewandte Chemie International Edition Année : 2023

Hydride-containing 2-Electron Pd/Cu Superatoms as Catalysts for Efficient Electrochemical Hydrogen Evolution

Résumé

The first hydride-containing 2-electron palladium/copper alloys, [PdHCu11{S2P(O i Pr)2}6(C≡CPh)4] (PdHCu11) and [PdHCu12{S2P(O i Pr)2}5{S2PO(O i Pr)} (C≡CPh)4] (PdHCu12), are synthesized from the reaction of [PdH2Cu14{S2P(O i Pr)2}6(C≡CPh)6] (PdH2Cu14) with trifluoroacetic acid (TFA). X-ray diffraction reveals that the PdHCu11 and PdHCu12 kernels consist of a central PdH unit encapsulated within a vertex-missing Cu11 cuboctahedron and complete Cu12 cuboctahedron, respectively. DFT calculations indicate that both PdHCu11 and PdHCu12can be considered as axially-distorted 2-electron superatoms. PdHCu11 shows excellent HER activity, unprecedented within metal nanoclusters, with an onset potential of -0.05 V (at 10 mA cm-2), a Tafel slope of 40 mV dec-1, and consistent HER activity during 1000 cycles. Our study suggests that the accessible central Pd site is the key to HER activity and may provide guidelines for correlating catalyst structures and HER activity.

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hal-04013808 , version 1 (30-03-2023)

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Paternité - Pas d'utilisation commerciale

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Rhone P. Brocha Silalahi, Yongsung Jo, Jian-Hong Liao, Tzu-Hao Chiu, Eunsaem Park, et al.. Hydride-containing 2-Electron Pd/Cu Superatoms as Catalysts for Efficient Electrochemical Hydrogen Evolution. Angewandte Chemie International Edition, 2023, pp.e202301272. ⟨10.1002/anie.202301272⟩. ⟨hal-04013808⟩
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