Fe oxide nanoparticles/Ti-modified mesoporous silica as a photo-catalyst for efficient and selective cyclohexane conversion with O2 and solar light

被引:31
作者
Ide, Y. [1 ,2 ]
Iwata, M. [2 ]
Yagenji, Y. [3 ]
Tsunoji, N. [3 ]
Sohmiya, M. [4 ]
Komaguchi, K. [3 ]
Sano, T. [3 ]
Sugahara, Y. [2 ,5 ,6 ]
机构
[1] Natl Inst Mat Sci, Int Ctr Mat Nanoarchitecton MANA, 1-1 Namiki, Tsukuba, Ibaraki 3050044, Japan
[2] Waseda Univ, Grad Sch Creat Sci & Engn, Shinjuku Ku, 1-6-1 Nishiwaseda, Tokyo 1698050, Japan
[3] Hiroshima Univ, Grad Sch Engn, Dept Appl Chem, 1-4-1 Kagamiyama, Higashihiroshima 7398527, Japan
[4] Waseda Univ, Dept Earth Sci, Shinjuku Ku, 1-6-1 Nishiwaseda, Tokyo 1698050, Japan
[5] Waseda Univ, Sch Adv Sci & Engn, Dept Appl Chem, Shinjuku Ku, 3-4-1 Ohkubo, Tokyo 1698555, Japan
[6] Waseda Univ, Kagami Mem Res Inst Mat Sci & Technol, Shinjuku Ku, 2-8-26 Nishiwaseda, Tokyo 1690054, Japan
关键词
VISIBLE-LIGHT; ACTIVATION; DIOXIDE; PHOTOOXIDATION; PERFORMANCE; REDUCTION; OXIDATION; CENTERS; DESIGN;
D O I
10.1039/c6ta04222h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We report a new, environmentally and economically friendly photocatalytic process with unprecedentedly high activity for partial cyclohexane oxidation. Mesoporous silicas containing isolated tetra-hedrally coordinated Ti and Fe oxide nanoparticles immobilized on the pore surface were synthesized by reacting SBA-15 with Ti(IV) acetylacetonate and Fe(III) acetylacetonate successively. A variety of characterizations suggested that the grafted tetrahedrally coordinated Ti species were coupled with Fe oxide nanoparticles via Ti-O-Fe bonds. The SBA-15 photocatalysts showed a high yield (up to sub-mmol) and nearly 100% selectivity for the production of cyclohexanol and cyclohexanone with molecular O-2 under solar light. The unprecedentedly high activity could be explained by the lengthened lifetime of the active Ti species by electron delocalization over Ti-O-Fe bonds and the visible light (lambda > 420 nm)-induced activity endowed by Fe oxide nanoparticles coupled to the Ti species.
引用
收藏
页码:15829 / 15835
页数:7
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