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Visible-Light-Driven Methane Conversion with Oxygen Enabled by Atomically Precise Nickel Catalyst
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DOI：10.31635/ccschem.020.202000521.png)
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摘要
En 中文
It remains an extreme challenge to activate thermodynamically unfavorable, chemically inert methane molecules under mild conditions. Herein, we report a molecular-like nickel-thiolate hexameric cluster [Ni-6(PET)(12); PET = SC2H4Ph] catalyst that resembles a double crown, comprising of a hexagonal Ni-6 kernel encapsulated by an exterior shell of 12 thiolates capable of efficient conversion of methane plus O-2 to methanol and formic acid under visible light irradiation. Exclusive photocatalysis by Ni-6(PET)(12) is related to its suitable molecular orbital gap, energy alignment, and the unique atomic-packing structure able to harvest solar energy to activate O-2 with the subsequent accomplishment of H-atom abstraction from sluggish methane. This work is a major step toward promising practical applications of atomically precise metal catalysts in arduous bond cleavages and construction of low-carbon alkanes, with the potential to further facilitate fossil energy conversions.
Keyword:
CH4
O-2
atomic level
nanocluster
chemicals
