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In order to solve the current energy and environmental issues, photolysis of hydrogen in aquatic products has important research significance. However, there are still many problems in the photoresponse range, photo-carrier separation efficiency, stability, and hydrogen production activity of currently developed catalysts. For example, the commonly used titanium dioxide material only acts in the ultraviolet region, which limits the efficiency of solar energy utilization; and the visible light-responsive cadmium sulfide material has low efficiency and poor stability. Therefore, the preparation of a highly efficient and stable visible light driven hydrogen production catalytic system is still a very big challenge.
Based on the reaction mechanism, inorganic synthetic chemistry team led by Zhang Jian and Zhang Lei, researchers of the State Key Laboratory of Structural Chemistry of the Fujian Institute of Materials Structure, Chinese Academy of Sciences, purposefully designed a series of composite photocatalytic material systems based on titanium-oxygen clusters. Through solvothermal reaction, cadmium sulfide nano-particles and titanium-oxygen clusters were assembled in-situ into porous framework material MIL-101 in step-by-step manner to obtain a ternary composite material with good visible light absorption. At the same time, thanks to the synergistic effect among the three components, the hydrogen production efficiency of photolysis of water has been greatly improved compared to CdS/MIL-101 binary materials without the use of precious metals as promoters. More interestingly, the catalytic activity of the ternary material system can be further optimized by changing the conjugation properties of the modified organic ligands on the titanium oxygen clusters, and eventually the hydrogen production rate can be increased by nearly 50 times. Spectroscopic and electrochemical analyses indicate that in this composite system, the titanium-oxygen clusters can act as electron transfer media, dispersing photogenerated electrons from the cadmium sulfide particles onto the surface of the porous material, thereby promoting charge-hole separation and improving catalytic activity. The research results not only established a highly efficient visible light driven hydrogen production catalytic system based on titanium-oxygen clusters, but also provided an effective tool for controlling and optimizing its catalytic activity from the molecular level. Relevant results have been published in "Adv. Mater. 2017, 29, 1603369".
The study was awarded the "973" plan of the Ministry of Science and Technology, an innovative group of "inorganic-organic hybrid functional materials" of the State Development Fund, the "emerging and cross-domain" project of the Chinese Academy of Sciences, the China National Academy of Sciences' strategic pilot technology project (category B) and the National Outstanding Youth Fund. . The research team previously synthesized the world’s first fullerene-type titanium oxygen cluster (J. Am. Chem. Soc. 2016, 138, 2556) and the world’s highest nuclear Ti52 cluster (J. Am. Chem. Soc. (2016, 138, 7480), systematically investigated the energy band regulation of titanium-oxygen clusters (Angew. Chem. Int. Ed. 2016, 55, 5160), and achieved the preparation of titanium oxygen cluster supported metal-organic framework films ( ACS Nano 2016, 10, 977).
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