Supramolecular preorganization effect to access single cobalt sites for enhanced photocatalytic hydrogen evolution and nitrogen fixation

被引:46
作者
Zhang, Wenyao [1 ,2 ]
Fu, Yongsheng [1 ]
Peng, Qiong [1 ]
Yao, Qiushi [3 ]
Wang, Xin [1 ]
Yu, Aiping [2 ]
Chen, Zhongwei [2 ]
机构
[1] Nanjing Univ Sci & Technol, Key Lab Soft Chem & Funct Mat, Nanjing 210094, Peoples R China
[2] Univ Waterloo, Waterloo Inst Nanotechnol, Waterloo, ON N2L 3G1, Canada
[3] Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
基金
加拿大自然科学与工程研究理事会; 中国国家自然科学基金;
关键词
CARBON NITRIDE NANOSHEETS; IN-SITU; DOPED G-C3N4; WATER; ELECTROCATALYSTS; NANOTUBES; REDUCTION; CHEMISTRY; CATALYSIS; STRATEGY;
D O I
10.1016/j.cej.2020.124822
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Ever-increased investigation has been focused on designing photocatalysts comprising intimately interfaced photo-absorbers and co-catalysts for promoting the separation of electron-hole pairs and surface redox reaction. Herein, we present a photocatalytic system in which the single-site-cobalt-atom is firmly trapped and stabilized into the frameworks of porous crimped graphitic carbon nitride (g-C3N4), proposing as advanced photocatalysts for solar-photon-driven hydrogen production and nitrogen fixation. A single molecular source of dicyandiamide was used to partly transformed and then in-situ preorganized into supermolecular precursor, which could coordinate with cobalt ions and manipulate the interactions under elevated temperature prior to the condensation to form atomically Co dispersed g-C3N4 materials. Theoretical evaluation and experimental validation identified that the chemical integration of single-site-cobalt-atom on g-C3N4 is critical in optimizing the electron and band structures and accelerating the interfacial charge transfer process. As a result, the as-obtained Co@g-C3N4 possesses an exceptional photocatalytic hydrogen production rate (2481 μmolh−1g−1, λ > 420 nm) and conspicuous nitrogen photofixation performances under visible-light irradiation. Such concerted catalysis attributes to the negative shift of the Fermi level in Co@g-C3N4 system deriving from the induced charge-transfer effect, which effectively gains the reducibility of electrons and creates more active sites for photocatalytic reactions. © 2020
引用
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页数:9
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