摘要
Nitrate is a crucial environmental pollutant,and its risk on ecosystem keeps increasing.Photocatalytic conversion of nitrate to ammonia can simultaneously achieve the commercialization of environmental hazards and recovery of valuable ammonia,which is green and sustainable for the planet.However,due to the thermodynamic and kinetic energy barriers,photocatalytic nitrate reduction usually involves a higher selectivity of the formation of nitrogen that largely limits the ammonia synthesis activity.In this work,we reported a green and facile synthesis of novel metallic ruthenium particle modified graphitic carbon nitride photocatalysts.Compare with bulk graphitic carbon nitride,the optimal sample had 2.93-fold photocatalytic nitrate reduction to ammonia activity(2.627 mg/h/gcat),and the NH3 selectivity increased from 50.77%to 77.9%.According to the experimental and calculated results,the enhanced photocatalytic performance is attributed to the stronger light absorption,nitrate adsorption,and lower energy barrier for the generation of ammonia.This work may provide a facile way to prepare metal modified photocatalysts to achieve highly efficient nitrate reduction to ammonia.
基金
an Australian Research Council(ARC)Future Fellowship(FT160100195)
the National Key Research and Development Program of China(2016YFA0602900)
the National Natural Science Foundation of China(21673220)
Department of Science and Technology of Sichuan Province(2017GZ0051)
Jilin Province Science and Technology Development Program(20190201270JC,20180101030JC)
Part of the computational time is supported by the High Performance Computing Center of Jilin University and Jilin Province,as well as Network and Computing Center of Changchun Institute of Applied Chemistry
Derek Hao acknowledges the technical support of Beijing NBET Technology Co.,Ltd.The authors also acknowledge the Sydney Analytical(USYD),CTWW,MAU,and Chem Lab of UTS for the lab supports.
