Strategy of constructing D-A structure and accurate active sites over graphitic carbon nitride nanowires for high efficient photocatalytic nitrogen fixation

被引:3
|
作者
Cui, Donghui [1 ]
Yang, Xue [1 ]
Liu, Yu [1 ]
Ou, Ting [2 ,3 ]
Kong, Xiangyi [3 ]
Zhang, Yali [4 ]
Zhang, Jiangwei [3 ,5 ]
Li, Fengyan [1 ]
机构
[1] Northeast Normal Univ, Coll Chem, Minist Educ, Key Lab Polyoxometalate & Reticular Mat Chem, Changchun 130024, Peoples R China
[2] Shaanxi Univ Technol, Sch Chem & Environm Sci, Inst Theoret & Computat Chem, Shaanxi Key Lab Catalysis, Hanzhong 723001, Shaanxi, Peoples R China
[3] Inner Mongolia Univ, Coll Energy Mat & Chem, Hohhot 010021, Peoples R China
[4] Inner Mongolia Univ, Sch Econ & Management, Hohhot 010021, Peoples R China
[5] Ordos Lab, Ordos 017000, Peoples R China
关键词
Graphitic carbon nitride; Phenanthroline; Donor-acceptor; Intramolecular charge transfer; Nitrogen fixation; DOPED G-C3N4; AMMONIA; DONOR;
D O I
10.1016/j.jcis.2024.09.052
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Constructing photocatalysts for the stable and efficient production of NH3 is of excellent research significance and challenging. In this paper, the electron acceptor 5-amino-1,10-phenanthroline (AP) is introduced into the electron-donor graphitic carbon nitride (CN) framework by a simple heated copolymerization method to construct a donor-acceptor (D-A) structure. Subsequently, the phenanthroline unit is coordinated with transition metal Fe3+ ions to obtain the photocatalyst Fe(III)-0.5-AP-CN with better nitrogen fixation performance, and the average NH3 yield can reach 825.3 mu mol g(-1) h(-1). Comprehensive experimental results and theoretical calculations show that the presence of the D-A structure can induce intramolecular charge transfer, effectively separating photogenerated electrons and holes. The Fe active sites can improve the chemisorption energy for N-2, enhance the N-Fe bonding, and better activate the N-2 molecule. Therefore, the synergistic effect between the construction of the D-A structure and the stably dispersed Fe active sites can enable CN to achieve high-performance N-2 reduction to produce NH3.
引用
收藏
页码:955 / 969
页数:15
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