期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 248, 期 -, 页码 44-53出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2019.02.007
关键词
Biological template; Mo-doped g-C3N4; Chelation; Receptor-donor built-in electric field; Photocatalytic hydrogen evolution
资金
- National Natural Science Foundation of China [21878047, 21676056, 51673040]
- Six Talents Pinnacle Program of Jiangsu Province of China [JNHB-006]
- Qing Lan Project of Jiangsu Province [1107040167]
- Graduate student scientific research innovation program of Jiangsu Province [KYCX18_0132]
- Scientific Research Foundation of Graduate School of Southeast University [YBPY1880]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) [1107047002]
Herein, a novel strategy is established to synthesize Mo-doped graphitic carbon nitride (g-C3N4) with excellent photocatalytic activity through a green approach of biological template. The addition of biotemplates provides a microenvironment for the formation of hydrogen bonds in which the flower-like g-C3N4 is formed by self-assembly between precursors, which not only increases the specific surface area of the material but also exposes more catalytic activity edge. Benefiting from the non-localized of Mo(VI) 4d orbital, Mo-doped g-C(3)N(4 )constructs a suitable band structure and a built-in electric field that promotes electron delocalization, which improves the absorption range of visible light and separation efficiency of photo-generated electron-hole pairs. Subsequently, a possible chelation-hydrogen bond coordination mechanism was proposed based on the characterization results of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) and N-15 solid-state NMR (N-15 NMR). As a result, the pi-conjugated system of g-C3N4 was extended by forming a chelate centered on Mo(VI). Photocatalytic hydrogen evolution (PHE) showed that the optimal hydrogen evolution rate of Mo-doped g-C3N4 was as high as 2008.9 umol/g.h, which was 9.6 times than that of bulk g-C3N4.
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