Interfacial coupling induced direct Z-scheme water splitting in metal-free photocatalyst: C3N/g-C3N4 heterojunctions

被引:46
作者
Wang, Jiajun [1 ]
Li, Xiaoting [1 ]
You, Ya [1 ]
Yang, Xintong [1 ]
Wang, Ying [1 ]
Li, Qunxiang [2 ,3 ]
机构
[1] Tianjin Normal Univ, Coll Chem, Tianjin Key Lab Struct & Performance Funct Mol, Minist Educ,Key Lab Inorgan Organ Hybrid Funct Ma, Tianjin 300387, Peoples R China
[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
基金
中国国家自然科学基金;
关键词
C3N/g-C3N4; band bending; direct Z-scheme heterojunction; water splitting; GRAPHITIC CARBON NITRIDE; HYDROGEN-PRODUCTION; CHARGE-TRANSFER; ANATASE TIO2; HETEROSTRUCTURE; GRAPHENE; C3N; PERFORMANCE; COMPOSITES; ADSORPTION;
D O I
10.1088/1361-6528/aace20
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
Mimicking the natural photosynthesis in green plants, artificial Z-scheme photocatalysis enables more efficient utilization of solar energy for photocatalytic water splitting. Most currently designed g-C3N4-based Z-scheme heterojunctions are usually based on metal-containing semiconductor photocatalysts, thus exploiting metal-free photocatalysts for Z-scheme water splitting is of huge interest. Herein, we propose two metal-free C3N/g-C3N4 heterojunctions with the C3N monolayer covering g-C3N4 sheet (monolayer or bilayer) and systematically explore their electronic structures, charge distributions and photocatalytic properties by performing extensive hybrid density functional calculations. We clearly reveal that the relative strong built-in electric fields around their respective interface regions, caused by the charge transfer from C3N monolayer to g-C3N4 monolayer or bilayer, result in the bands bending, renders the transfer of photogenerated carriers in these two heterojunctions following the Z-scheme instead of the type-II pathway. Moreover, the photogenerated electrons and holes in these two C3N/g-C3N4 heterojunctions can not only be efficiently separated, but also have strong redox abilities for water oxidation and reduction. Compared with the isolated g-C(3)N(4 )sheets, the light absorption in visible to near-infrared region are significantly enhanced in these proposed heterojunctions. These theoretical findings suggest that these proposed metal-free C3N/g-C3N4 heterojunctions are promising direct Z-scheme photocatalysts for solar water splitting.
引用
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页数:9
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