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Efficient Photocatalytic Nitrogen Fixation: Enhanced Polarization, Activation, and Cleavage by Asymmetrical Electron Donation to NN Bond
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2019-10-31 , DOI: 10.1002/adfm.201906983
Jili Yuan 1 , Xuanying Yi 2 , Yanhong Tang 1 , Meijun Liu 2 , Chengbin Liu 2
Affiliation  

Photocatalytic nitrogen (N2) fixation suffers from low efficiency due to the difficult activation of the strongly nonpolar NN bond. In this study, a Ru–Co bimetal center is constructed at the interface of Ru/CoSx with S‐vacancy on graphitic carbon nitride nanosheets (Ru‐Vs‐CoS/CN). Upon adsorption, the two N atoms in N2 are bridged to the Ru–Co center, and the asymmetrical electron donation from Ru and Co atoms to N2 adsorbate highly polarized NN bond to double bond order. The plasmonic electric‐field‐enhancement effect enables the Ru/CoSx interface to boost the generation of energetic electrons. The Schottky barrier between Ru and CoSx endows the interface with electron transfer from CoSx 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 NH3 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.

中文翻译:

高效的光催化固氮:通过不对称电子给NN键增强极化,活化和裂解

由于强非极性NN键难以激活,光催化氮(N 2)固定效率低下。在本研究中,在石墨氮化碳纳米片(Ru-Vs-CoS / CN)上,Ru / CoS x与S-空位的界面处构建了Ru-Co双金属中心。吸附后,N 2中的两个N原子桥接至Ru-Co中心,并且Ru和Co原子向N 2的不对称电子给体吸附高度极化的NN键成双键顺序。等离子体电场增强效应使Ru / CoS x界面能够促进高能电子的产生。Ru和CoS x之间的肖特基势垒使界面具有从CoS x到Ru的电子转移。Ru-Co中心的Ru-end结合N优先被氢化。结果,Ru-Vs-CoS / CN光催化剂显示NH 3的生产速率高达0.438 mmol g -1 h -1,在400 nm时达到1.28%的高表观量子效率和日照-氨气效率在AM1.5G光照射下纯水中的0.042%的污染物。
更新日期:2020-01-24
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