Insights into the synergistic promotion of spin polarization over C_(3)N_(5.4) for enhancing cooperative hydrogen evolution and benzylamine oxidation coupling  

作　　者：Qiuchen Wang Xiaoxu Deng Haiyan Pen Fei Liu Meiyang Song Peng Chen Shuang-Feng Yin 

机构地区：[1]Provincial Guizhou Key Laboratory of Green Chemical and Clean Energy Technology,School of Chemistry and Chemical Engineering,Guizhou University,Guiyang 550025,China [2]College of Big Data and Information Engineering,Guizhou University,Guiyang 550025,China [3]College of Chemistry and Chemical Engineering,Advanced Catalytic Engineering Research Center of the Ministry of Education,State Key Laboratory of Chemo/Biosensing and Chemometrics,Hunan University,Changsha 410082,China

出　　处：《Nano Research》2023年第4期4225-4232,共8页纳米研究（英文版）

基　　金：financially supported by Guizhou Provincial Science and Technology Foundation(No.ZK2021069);Young Science and Technology Talents Development Project of Education Department in Guizhou Province(No.KY2022144);National Natural Science Foundation of China(No.22268015).

摘　　要：Polymers are usually restricted on the high exciton binding energies and sluggish electron transfer because of the low dielectric constants.Regulating spin-polarized electrons is regarded as an attractive strategy,but often confined to the d-orbital elements.Here,the nonmetal P and N elements co-mediated the spin polarization of carbon nitrides(PCN)have been elaborately designed.The optimized PCN-3 shows an outstanding hydrogen production(22.2 mmol·g^(-1)·h^(-1))coupled with selective benzylamine oxidation without using any solvent and cocatalysts,which is 200 times of original C_(3)N_(4)and superior to the photocatalysts has been reported to date.Experimental and theoretical results verified that the spin-orbital coupling of N 2p and P 2p remarkably increased the parallel spin states of charge and reduced the formation of singlet excitons to accelerate exciton dissociation in carbon nitride.In addition,charge separation and surface catalysis can be significantly enhanced by the electron spin polarization of carbon nitride with the parallel arrangement,huge built-in electric field and disturbed electronic structure.Our finding deepens the insight into the charge separation and exciton dissociation in spin polarization,and offers new tactics to develop high-efficiency catalysts.

关 键 词：spin polarization photocatalysis amine oxidative coupling hydrogen production C_(3)N_(5.4) 

分 类 号：O57[理学—粒子物理与原子核物理]