Donor-Acceptor structural polymeric carbon nitride with in-plane electric field accelerating charge separation for efficient photocatalytic hydrogen evolution

被引:54
作者
Liu, Zengjian [1 ]
Zhang, Jin [1 ]
Wan, Yingfei [1 ]
Chen, Jinwei [1 ,2 ]
Zhou, Yufeng [1 ]
Zhang, Jie [1 ]
Wang, Gang [1 ,2 ]
Wang, Ruilin [1 ,2 ]
机构
[1] Sichuan Univ, Coll Mat Sci & Engn, Chengdu 610065, Peoples R China
[2] Minist Educ, Engn Res Ctr Alternat Energy Mat & Devices, Chengdu 610065, Peoples R China
基金
国家重点研发计划;
关键词
Carbon nitride; Photocatalytic hydrogen evolution; Donor-acceptor structure; In-plane electric field; Charge separation; TOTAL-ENERGY CALCULATIONS; H-2; EVOLUTION; G-C3N4; WATER; COPOLYMERS;
D O I
10.1016/j.cej.2021.132725
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The realization of efficient photocatalytic hydrogen evolution based on polymeric carbon nitride (PCN) is severely hampered by the insufficient separation of photogenerated electrons and holes. Herein, we successfully introduced Benzo[b]thiophene-2-carboxylic acid (BTH) as donor parts through supramolecular self-assembly into the framework of PCN to form D-A structure to promote the photoexciton separation efficiency. The SCNBTH structure shows the improved separation efficiency of charge carriers and shorter diffusion path resulting in hydrogen evolution rate up to 3950 mu mol/g/h, which is 13.3 times higher than that of bulk carbon nitride (BCN) under visible light irradiation (lambda > 420 nm). Further density functional theory (DFT) calculation reveals that SCN-BTH structure exhibits strong spatial separation of lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) compared to that of BCN with the even distribution. In addition, electrostatic potential diagram indicates the in-plane polarized electric field in SCN-BTH embedded with the D-A structure can drive the photo-generated electrons and holes toward reverse direction, thereby accelerating the separation of carriers. All those factors synergistically facilitated the charge separation and transport process which are responsible for the improved photocatalytic performance.
引用
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页数:11
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