期刊
ADVANCED SCIENCE
卷 8, 期 4, 页码 -出版社
WILEY
DOI: 10.1002/advs.202002465
关键词
carbon nitrides; hydrogen generation; cocatalysts; photocatalysis; poly(platinaynes)
资金
- Science, Technology and Innovation Committee of Shenzhen Municipality [JCYJ20180507183413211]
- National Natural Science Foundation of China [51873176, 61775145/61525503/616201060166183500921828102]
- Hong Kong Research Grants Council [PolyU 153062/18P, C5037-18G]
- Hong Kong Polytechnic University [1-ZE1C]
- Ms. Clarea Au for the Endowed Professorship in Energy [847S]
- National Key R&D Program of China [2018YFC0910602]
- China Postdoctoral Science Foundation Funded Project [2019M653007, 2020M672817]
- Key Project of Department of Education of Guangdong Province [2015KGJHZ002/2016KCXTD007]
- Guangdong Province Key Area RD Program [2019B110233004]
- Foundation of Wenzhou Science and Technology Bureau [W20170003]
- Research Grants Council, University Grants Committee of the HKSAR
A metal-complex-modified graphitic carbon nitride bulk heterostructure is proposed as a promising alternative to high-cost noble metals as artificial photocatalysts. Experimental studies show that the Pt(II) acetylide group effectively expands electron delocalization and enhances light-harvesting efficiencies. Among the tested assemblies, Pt-P@CN without any Pt metal additives exhibits significantly improved photocatalytic H-2 generation rate under simulated sunlight irradiation.
A metal-complex-modified graphitic carbon nitride (g-C3N4) bulk heterostructure is presented here as a promising alternative to high-cost noble metals as artificial photocatalysts. Theoretical and experimental studies of the spectral and physicochemical properties of three structurally similar molecules Fo-D, Pt-D, and Pt-P confirm that the Pt(II) acetylide group effectively expands the electron delocalization and adjusts the molecular orbital levels to form a relatively narrow bandgap. Using these molecules, the donor-acceptor assemblies Fo-D@CN, Pt-D@CN, and Pt-P@CN are formed with g-C3N4. Among these assemblies, the Pt(II) acetylide-based composite materials Pt-D@CN and Pt-P@CN with bulk heterojunction morphologies and extremely low Pt weight ratios of 0.19% and 0.24%, respectively, exhibit the fastest charge transfer and best light-harvesting efficiencies. Among the tested assemblies, 10 mg Pt-P@CN without any Pt metal additives exhibits a significantly improved photocatalytic H-2 generation rate of 1.38 mu mol h(-1) under simulated sunlight irradiation (AM1.5G, filter), which is sixfold higher than that of the pristine g-C3N4.
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