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Efficient Photocatalytic Nitrogen Fixation: Enhanced Polarization, Activation, and Cleavage by Asymmetrical Electron Donation to NN 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
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
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Photocatalytic nitrogen (N2) 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/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 NN 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NN键增强极化,活化和裂解
由于强非极性NN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NN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
中文翻译:
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高效的光催化固氮:通过不对称电子给NN键增强极化,活化和裂解
由于强非极性NN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NN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。