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Efficient Photocatalytic Nitrogen Fixation: Enhanced Polarization, Activation, and Cleavage by Asymmetrical Electron Donation to NN Bond
Author(s) -
Yuan Jili,
Yi Xuanying,
Tang Yanhong,
Liu Meijun,
Liu Chengbin
Publication year - 2020
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201906983
Subject(s) - materials science , photocatalysis , graphitic carbon nitride , photochemistry , bond cleavage , electron , catalysis , chemistry , biochemistry , physics , quantum mechanics
Photocatalytic nitrogen (N 2 ) fixation suffers from low efficiency due to the difficult activation of the strongly nonpolar NN bond. In this study, a Ru–Co bimetal center is constructed at the interface of Ru/CoS x with S‐vacancy on graphitic carbon nitride nanosheets (Ru‐Vs‐CoS/CN). Upon adsorption, the two N atoms in N 2 are bridged to the Ru–Co center, and the asymmetrical electron donation from Ru and Co atoms to N 2 adsorbate highly polarized NN bond to double bond order. The plasmonic electric‐field‐enhancement effect enables the Ru/CoS x interface to boost the generation of energetic electrons. The Schottky barrier between Ru and CoS x endows the interface with electron transfer from CoS x to Ru. The Ru‐end bound N at the Ru–Co center is preferentially hydrogenated. As a result, the Ru‐Vs‐CoS/CN photocatalyst shows an NH 3 production rate of up to 0.438 mmol g −1 h −1 , reaching a high apparent quantum efficiency of 1.28% at 400 nm and solar‐to‐ammonia efficiency of 0.042% in pure water under AM1.5G light irradiation.