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Asymmetrically Doping a Platium Atom into a Au38 Nanocluster for Changing the Electron Configuration and Reactivity in Electrocatalysis.

It becomes an obstacle to precisely manipulate a doped heteroatom into a desired position of a metal nanocluster. Here, we overcome such a difficulty to obtain Pt1Au37(SCH2PhtBu)24 and Pt2Au36(SCH2PhtBu)24 nanoclusters via controllably doping Pt atoms into the kernels of Au38(SCH2PhtBu)24. We reveal that asymmetrical doping of one Pt atom into either core of Au38(SCH2PhtBu)24 elevates relative energy of the HOMO (highest occupied molecular orbital) accompanied by one free valence electron loss of Pt1Au37(SCH2PhtBu)24, compared to Au38(SCH2PhtBu)24 with 14 electrons, while symmetrical doping of two Pt atoms into the cores of Au38(SCH2PhtBu)24 narrows the HOMO-LUMO gap (LUMO: lowest unoccupied molecular orbital) of Pt2Au36(SCH2PhtBu)24 with two valence electrons less. Consequently, Pt1Au37(SCH2PhtBu)24 shows an electron-spin-induced high activity for CO2 electroreduction, whereas Pt2Au36(SCH2PhtBu)24 is least efficient and Au38(SCH2PhtBu)24 has a decent performance.