Porous S-doped carbon nitride foam with accelerated charge dynamics for synchronous photocatalytic hydrogen production and highly selective oxidation of amines  

作　　者：Yu He Aiping Wu Nan Wang Ying Xie Chungui Tian Honggang Fu 

机构地区：[1]Key Laboratory of Functional Inorganic Material Chemistry(Ministry of Education of the People’s Republic of China),Heilongjiang University,Harbin 150080,China

出　　处：《Nano Research》2024年第8期6860-6869,共10页纳米研究（英文版）

基　　金：the National Key Research and Development Program of China(No.2022YFA1503003);the National Natural Science Foundation of China(Nos.U20A20250 and 22271081);the Natural Science Foundation of Heilongjiang Province(No.ZD2021B003);the University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2020004).

摘　　要：Photocatalytic hydrogen evolution coupled with organic oxidation holds great promise for converting solar energy into high-valueadded chemicals,but it is hampered by sluggish charge dynamics and limited redox potential.Herein,a porous S-doped carbon nitride(S-C_(3)N_(4−y))foam assembled from ultrathin nanosheets with rich nitrogen vacancies was synthesized using a molecular selfassembly strategy.The S dopants and N vacancies synergistically adjusted the band structure,facilitating light absorption and enhancing the oxidation ability.Moreover,the ultrathin nanosheets and porous structure provided more exposed active sites and facilitated mass and charge transfer.Consequently,S-C_(3)N_(4−y) foam exhibited enhanced photocatalytic activities for synchronous hydrogen evolution(4960μmol/(h·g))and benzylamine oxidation to N-benzylidenebenzylamine(4885μmol/(h·g))with high selectivity of>99%,which were approximately 17.6 and 72.9 times higher than those of bulk CN,respectively.The photocatalytic coupling pairing reaction promotes the water splitting by consuming H2O2,thereby improving the hydrogen evolution efficiency and achieving the production of high value-added imines.This study provides an effective route for regulating the morphology and band structure of carbon nitride for synthesizing highly valuable chemicals.

关 键 词：photocatalysis S-doped carbon nitride band structure regulation hydrogen evolution coupled with benzylamine oxidation reaction mechanism 

分 类 号：O64[理学—物理化学]