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Published on: April 27, 2018
Asymmetrically Doping a Platinum Atom into a Au38 Nanocluster for Changing the Electron Configuration and Reactivity
Xu Liu1, Endong Wang2, Meng Zhou3
1Key Lab of Mesoscopic Chemistry of MOE and Jiangsu Key Lab of Vehicle Emissions Control, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210093, China.
Abstract:
It is an obstacle to precisely manipulate a doped heteroatom into a desired position in a metal nanocluster. Herein, we overcome this difficulty to obtain Pt1 Au37 (SCH2 Pht Bu)24 and Pt2 Au36 (SCH2 Pht Bu)24 nanoclusters via controllably doping Pt atoms into the kernels of Au38 (SCH2 Pht Bu)24 . We reveal that asymmetrical doping of one Pt atom into either of the cores of Au38 (SCH2 Pht Bu)24 elevates the relative energy of the HOMO (highest occupied molecular orbital) accompanied by one valence electron loss of Pt1 Au37 (SCH2 Pht Bu)24 , compared to Au38 (SCH2 Pht Bu)24 with 14 electrons, while symmetrical doping of two Pt atoms into the cores of Au38 (SCH2 Pht Bu)24 narrows the HOMO-LUMO gap (LUMO: lowest unoccupied molecular orbital) of Pt2 Au36 (SCH2 Pht Bu)24 with two valence electrons less. Consequently, Pt1 Au37 (SCH2 Pht Bu)24 shows an electron-spin-induced high activity for CO2 electroreduction, whereas Pt2 Au36 (SCH2 Pht Bu)24 is least efficient and Au38 (SCH2 Pht Bu)24 has a decent performance.
