Sulfur-doped g-C3N4 nanosheets with carbon vacancies: General synthesis and improved activity for simulated solar-light photocatalytic nitrogen fixation

被引:338
作者
Cao, Shihai [1 ]
Fan, Bin [1 ]
Feng, Yanchao [1 ]
Chen, Huan [1 ]
Jiang, Fang [1 ]
Wang, Xin [2 ]
机构
[1] Nanjing Univ Sci & Technol, Key Lab Jiangsu Prov Chem Pollut Control & Resour, Sch Environm & Biol Engn, Nanjing 210094, Jiangsu, Peoples R China
[2] Nanjing Univ Sci & Technol, Minist Educ, Key Lab Soft Chem & Funct Mat, Nanjing 210094, Jiangsu, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
Sulfur-doped; g-C3N4; nanosheets; Gaseous polymerization; Nitrogen fixation; Carbon vacancies; Density functional theory; DENSITY-FUNCTIONAL THEORY; VISIBLE-LIGHT; HYDROGEN EVOLUTION; NITRIDE NANOSHEETS; PHOTOFIXATION ABILITY; REACTION-MECHANISM; AMMONIA-SYNTHESIS; OXYGEN VACANCIES; AQUEOUS-MEDIA; EFFICIENT;
D O I
10.1016/j.cej.2018.07.116
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Ultrathin sulfur-doped g-C3N4 porous nanosheets (SCNNSs) with large lateral size and carbon vacancies were obtained by directly collecting the gaseous product of thiourea under a self-generated NH3 atmosphere. The NH3 atmosphere promoted the formation of sulfur doped g-C3N4 nanosheets with a hierarchical pore structure and a high specific surface area. Carbon vacancies were also generated in the SCNNSs without notably changing the overall chemical structure. The obtained SCNNSs-550 showed a photocatalytic nitrogen fixation rate of 5.99mMh(-1) gCat(-1) under simulated sunlight irradiation within 4 h, which is 2.8 times as high as that of bulk SCN. This superior photocatalytic performance of SCNNSs was attributed to the porous sheet structure with sulfur doping and carbon vacancies, which provide many active sites for surface reactions and increase the charge-carrier separation rate. This novel synthetic method provides a simple and efficient way to dope nonmetals and form a defect structure in g-C3N4 for excellent photocatalytic performance.
引用
收藏
页码:147 / 156
页数:10
相关论文
共 54 条
[1]   Semiconductor clusters, nanocrystals, and quantum dots [J].
Alivisatos, AP .
SCIENCE, 1996, 271 (5251) :933-937
[2]  
[Anonymous], 2017, ANGEW CHEM INT EDIT, DOI DOI 10.1002/CHEM.201603407
[3]   Density functional theory-based analysis on O2 molecular interaction with the tri-s-triazine-based graphitic carbon nitride [J].
Aspera, Susan Menez ;
Kasai, Hideaki ;
Kawai, Hiroyuki .
SURFACE SCIENCE, 2012, 606 (11-12) :892-901
[4]   Nitrogen photofixation by ultrathin amine-functionalized graphitic carbon nitride nanosheets as a gaseous product from thermal polymerization of urea [J].
Cao, Shihai ;
Chen, Huan ;
Jiang, Fang ;
Wang, Xin .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 224 :222-229
[5]   All-solid-state Z-scheme 3,4-dihydroxybenzaldehyde-functionalized Ga2O3/graphitic carbon nitride photocatalyst with aromatic rings as electron mediators for visible-light photocatalytic nitrogen fixation [J].
Cao, Shihai ;
Zhou, Ning ;
Gao, Fenghua ;
Chen, Huan ;
Jiang, Fang .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 218 :600-610
[6]   One-step synthesis of sulfur-doped and nitrogen-deficient g-C3N4 photocatalyst for enhanced hydrogen evolution under visible light [J].
Chen, Jingling ;
Hong, Zhenhua ;
Chen, Yilin ;
Lin, Bizhou ;
Gao, Bifen .
MATERIALS LETTERS, 2015, 145 :129-132
[7]   Photocatalytic fixation of nitrogen to ammonia: state-of-the-art advancements and future prospects [J].
Chen, Xingzhu ;
Li, Neng ;
Kong, Zhouzhou ;
Ong, Wee-Jun ;
Zhao, Xiujian .
MATERIALS HORIZONS, 2018, 5 (01) :9-27
[8]   Steering the interlayer energy barrier and charge flow via bioriented transportation channels in g-C3N4: Enhanced photocatalysis and reaction mechanism [J].
Cui, Wen ;
Li, Jieyuan ;
Cen, Wanglai ;
Sun, Yanjuan ;
Lee, S. C. ;
Dong, Fan .
JOURNAL OF CATALYSIS, 2017, 352 :351-360
[9]   Construction of Conjugated Carbon Nitride Nanoarchitectures in Solution at Low Temperatures for Photoredox Catalysis [J].
Cui, Yanjuan ;
Ding, Zhengxin ;
Fu, Xianzhi ;
Wang, Xinchen .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (47) :11814-11818
[10]   AN ALL-ELECTRON NUMERICAL-METHOD FOR SOLVING THE LOCAL DENSITY FUNCTIONAL FOR POLYATOMIC-MOLECULES [J].
DELLEY, B .
JOURNAL OF CHEMICAL PHYSICS, 1990, 92 (01) :508-517