Lyulyukin Mikhail, Filippov Tikhon, Cherepanova Svetlana, Solovyeva Maria, Prosvirin Igor, Bukhtiyarov Andrey, Kozlov Denis, Selishchev Dmitry
Department of Unconventional Catalytic Processes, Boreskov Institute of Catalysis, 630090 Novosibirsk, Russia.
Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel.
Nanomaterials (Basel). 2021 Apr 19;11(4):1036. doi: 10.3390/nano11041036.
In this study, various solid uranium oxycompounds and TiO-supported materials based on nanocrystalline anatase TiO are synthesized using uranyl nitrate hexahydrate as a precursor. All uranium-contained samples are characterized using N adsorption, XRD, UV-vis, Raman, TEM, XPS and tested in the oxidation of a volatile organic compound under visible light of the blue region to find correlations between their physicochemical characteristics and photocatalytic activity. Both uranium oxycompounds and TiO-supported materials are photocatalytically active and are able to completely oxidize gaseous organic compounds under visible light. If compared to the commercial visible-light TiO KRONOS vlp 7000 photocatalyst used as a benchmark, solid uranium oxycompounds exhibit lower or comparable photocatalytic activity under blue light. At the same time, uranium compounds contained uranyl ion with a uranium charge state of 6+, exhibiting much higher activity than other compounds with a lower charge state of uranium. Immobilization of uranyl ions on the surface of nanocrystalline anatase TiO allows for substantial increase in visible-light activity. The photonic efficiency of reaction over uranyl-grafted TiO, 12.2%, is 17 times higher than the efficiency for commercial vlp 7000 photocatalyst. Uranyl-grafted TiO has the potential as a visible-light photocatalyst for special areas of application where there is no strict control for use of uranium compounds (e.g., in spaceships or submarines).
在本研究中,以六水合硝酸铀酰为前驱体,合成了各种固态铀氧基化合物以及基于纳米晶锐钛矿型TiO₂的负载型材料。所有含铀样品均通过N₂吸附、XRD、UV-vis、拉曼光谱、TEM、XPS进行表征,并在蓝色区域可见光下对挥发性有机化合物的氧化反应中进行测试,以找出其物理化学特性与光催化活性之间的相关性。铀氧基化合物和负载型TiO₂材料均具有光催化活性,且能够在可见光下将气态有机化合物完全氧化。与用作基准的商用可见光TiO₂(KRONOS vlp 7000)光催化剂相比,固态铀氧基化合物在蓝光下表现出较低或相当的光催化活性。同时,含铀化合物中铀酰离子的铀电荷态为6+,其活性远高于其他铀电荷态较低的化合物。将铀酰离子固定在纳米晶锐钛矿型TiO₂表面可大幅提高可见光活性。铀酰接枝TiO₂的反应光子效率为12.2%,比商用vlp 7000光催化剂的效率高17倍。铀酰接枝TiO₂有潜力作为可见光光催化剂应用于对铀化合物使用无严格管控的特殊领域(如宇宙飞船或潜艇中)。