Xuan Zhou1,2,3, Yurong Liu2,3, Zhengyuan Jin1, Meina Huang1, Feifan Zhou1, Jun Song1, Junle Qu1, Yu-Jia Zeng1, Peng-Cheng Qian4, Wai-Yeung Wong2,3. 1. College of Physics and Optoelectronic Engineering, Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province Shenzhen University Shenzhen 518060 P. R. China. 2. Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University (PolyU) Hung Hom Hong Kong P. R. China. 3. PolyU Shenzhen Research Institute Shenzhen 518057 P. R. China. 4. Key Laboratory of Environmental Functional Materials Technology and Application of Wenzhou City Institute of New Materials and Industry College of Chemistry and Materials Engineering Wenzhou University Wenzhou 325035 P. R. China.
Abstract
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 H2 generation rate of 1.38 µmol h-1 under simulated sunlight irradiation (AM1.5G, filter), which is sixfold higher than that of the pristine g-C3N4.
A metal-compn>lex-modified n>an class="Chemical">graphiticcarbon 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 H2 generation rate of 1.38 µmol h-1 under simulated sunlight irradiation (AM1.5G, filter), which is sixfold higher than that of the pristine g-C3N4.
Authors: Wai-Yeung Wong; Xing-Zhu Wang; Ze He; Aleksandra B Djurisić; Cho-Tung Yip; Kai-Yin Cheung; Hai Wang; Chris S K Mak; Wai-Kin Chan Journal: Nat Mater Date: 2007-05-13 Impact factor: 43.841