Limbic Inducted and Delocalized Effects of Diazole in Carbon Nitride Skeleton for Propelling Photocatalytic Hydrogen Evolution

被引:45
作者
Dong, Hongjun [1 ]
Zuo, Yan [1 ]
Xiao, Mengya [1 ]
Zhou, Tingxu [1 ]
Cheng, Shasha [1 ]
Chen, Gang [2 ]
Sun, Jingxue [2 ]
Yan, Ming [1 ]
Li, Chunmei [1 ]
机构
[1] Jiangsu Univ, Inst Green Chem & Chem Technol, Sch Chem & Chem Engn, Zhenjiang 212013, Jiangsu, Peoples R China
[2] Harbin Inst Technol, Sch Chem & Chem Engn, MIIT Key Lab Crit Mat Technol New Energy Convers, Harbin 150001, Peoples R China
基金
中国国家自然科学基金;
关键词
carbon nitride; diazole; limbic inducted and delocalized effects; photocatalytic hydrogen evolution; charge separation behavior; HIGHLY EFFICIENT; POROUS G-C3N4; WATER; 2,4,6-TRIAMINOPYRIMIDINE; HETEROJUNCTION; ACIDIFICATION; DEGRADATION; SEPARATION; NANOSHEETS;
D O I
10.1021/acsami.1c18450
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Skeleton modification on carbon nitride (g-C3N4) via organic molecules is a recognized effective strategy to improve photocatalytic performance because it can powerfully improve charge separation in the skeleton plane. Herein, a diazole with a unique conjugated structure is bonded on edge of the g-C3N4 skeleton through a moderate polymerization of urea with 4-aminoantipyrine (4AAP). Meanwhile, the Pt nanoparticles selectively deposit on edge of the g-C3N4-4AAP(15) nanosheet. It reveals that the robust limbic inducted and delocalized effects of diazole not only facilitate photogenerated electrons aggregation toward skeleton edge to promote in-plane carrier separation but also effectively stabilize and delocalize photogenerated electrons to improve carrier lifetime for propelling the photocatalytic hydrogen evolution (PHE) reaction. Specifically, the PHE rate over optimal g-C3N4-4AAP(15) (284.2 mu mol h(-1)) is 10 times that of pure g-C3N4 (27.6 mu mol h(-1)) and the apparent quantum efficiency (AQE) at 420 nm reaches up to 24.2%. Through insights into the functionalized effect of small nitrogenous heterocycles introduced into the skeleton edge of g-C3N4, this work opens a new design thought for exploiting high-efficiency g-C3N4-based photocatalysts for photocatalytic application.
引用
收藏
页码:56273 / 56284
页数:12
相关论文
共 51 条
[1]   Extending the π-electron conjugation in 2D planar graphitic carbon nitride: efficient charge separation for overall water splitting [J].
Bellamkonda, Sankeerthana ;
Shanmugam, Ramasamy ;
Gangavarapu, Ranga Rao .
JOURNAL OF MATERIALS CHEMISTRY A, 2019, 7 (08) :3757-3771
[2]   Dendritic Tip-on Polytriazine-Based Carbon Nitride Photocatalyst with High Hydrogen Evolution Activity [J].
Bhunia, Manas K. ;
Melissen, Sigismund ;
Parida, Manas R. ;
Sarawade, Pradip ;
Basset, Jean-Marie ;
Anjum, Dalaver H. ;
Mohammed, Omar F. ;
Sautet, Philippe ;
Le Bahers, Tangui ;
Takanabe, Kazuhiro .
CHEMISTRY OF MATERIALS, 2015, 27 (24) :8237-8247
[3]   Preparation of Hollow Cobalt-Iron Phosphides Nanospheres by Controllable Atom Migration for Enhanced Water Oxidation and Splitting [J].
Chen, Qiming ;
Zhang, Qicheng ;
Liu, Huibin ;
Liang, Junmei ;
Peng, Wenchao ;
Li, Yang ;
Zhang, Fengbao ;
Fan, Xiaobin .
SMALL, 2021, 17 (13)
[4]   Three-dimensional porous g-C3N4 for highly efficient photocatalytic overall water splitting [J].
Chen, Xianjie ;
Shi, Run ;
Chen, Qian ;
Zhang, Zijian ;
Jiang, Wenjun ;
Zhu, Yongfa ;
Zhang, Tierui .
NANO ENERGY, 2019, 59 :644-650
[5]   Molecular and textural engineering of conjugated carbon nitride catalysts for selective oxidation of alcohols with visible light [J].
Chen, Yan ;
Zhang, Jinshui ;
Zhang, Mingwen ;
Wang, Xinchen .
CHEMICAL SCIENCE, 2013, 4 (08) :3244-3248
[6]   First principles methods using CASTEP [J].
Clark, SJ ;
Segall, MD ;
Pickard, CJ ;
Hasnip, PJ ;
Probert, MJ ;
Refson, K ;
Payne, MC .
ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2005, 220 (5-6) :567-570
[7]   Metal-free Z-scheme 2D/2D VdW heterojunction for high-efficiency and durable photocatalytic H2 production [J].
Dong, Hongjun ;
Hong, Shihuan ;
Zhang, Pingfan ;
Yu, Siyu ;
Wang, Yun ;
Yuan, Shouqi ;
Li, Hong ;
Sun, Jingxue ;
Chen, Gang ;
Li, Chunmei .
CHEMICAL ENGINEERING JOURNAL, 2020, 395
[8]   Construction of morphology-controlled nonmetal 2D/3D homojunction towards enhancing photocatalytic activity and mechanism insight [J].
Dong, Hongjun ;
Zhang, Xiaoxu ;
Li, Jiaming ;
Zhou, Pengjie ;
Yu, Siyu ;
Song, Ning ;
Liu, Chunbo ;
Che, Guangbo ;
Li, Chunmei .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 263
[9]   Insight into the Activity and Stability of RhXP Nano-Species Supported on g-C3N4 for Photocatalytic H2 Production [J].
Dong, Hongjun ;
Xiao, Mengya ;
Yu, Siyu ;
Wu, Huihui ;
Wang, Yun ;
Sung, Jingxue ;
Chen, Gang ;
Li, Chunmei .
ACS CATALYSIS, 2020, 10 (01) :458-462
[10]   Boron/oxygen-codoped graphitic carbon nitride nanomesh for efficient photocatalytic hydrogen evolution [J].
Du, Juan ;
Li, Songmei ;
Du, Zhiguo ;
Meng, Shiming ;
Li, Bin .
CHEMICAL ENGINEERING JOURNAL, 2021, 407