Hydride‐Containing Pt‐doped Cu‐rich Nanoclusters: Synthesis, Structure, and Electrocatalytic Hydrogen Evolution
Résumé
A structurally precise hydride-containing Pt-doped Cu-rich nanocluster [PtH Cu {S P(O Pr) } (CCPh) ] (1) has been synthesized. It consists of a bicapped icosahedral Cu cage that encapsulates a linear PtH unit. Upon the addition of two equivalents of CF COOH to 1, two hydrido clusters are isolated. These clusters are [PtHCu {S P(O Pr) } (CCPh) ] (2), which is a vertex-missing Cu cuboctahedron encaging a PtH moiety, and [PtH Cu {S P(O Pr) } (CCPh) ] (3), a distorted 3,3,4,4,4-pentacapped trigonal prismatic Cu cage enclosing a PtH unit. The electronic structure of 2, analyzed by Density Functional Theory, is a 2e superatom. The electrocatalytic activities of 1-3 for hydrogen evolution reaction (HER) were compared. Notably, Cluster 2 exhibited an exceptionally excellent HER activity within metal nanoclusters, with an onset potential of -0.03 V (at 10 mA cm ), a Tafel slope of 39 mV dec , and consistent HER activity throughout 3000 cycles in 0.5 M H SO . Our study suggests that the accessible central Pt site plays a crucial role in the remarkable HER activity and may provide valuable insights for establishing correlations between catalyst structure and HER activity.
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Silalahi et al. - 2024 - Hydride-Containing Pt-doped Cu-rich Nanoclusters.pdf (1.88 Mo)
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