Fe oxide nanoparticles/Ti-modified mesoporous silica as a photo-catalyst for efficient and selective cyclohexane conversion with O2 and solar light
Fe oxide nanoparticles/Ti-modified mesoporous silica as a photo-catalyst for efficient and selective cyclohexane conversion with O2 and solar light
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DOI：
10.1039/c6ta04222h
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发表时间：
2016-10
影响因子：
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通讯作者：
Y. Ide;M. Iwata;Yuya Yagenji;Nao Tsunoji;Minoru Sohmiya;K. Komaguchi;T. Sano;Y. Sugahara
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文献类型：
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作者：
Y. Ide;M. Iwata;Yuya Yagenji;Nao Tsunoji;Minoru Sohmiya;K. Komaguchi;T. Sano;Y. Sugahara
我们报告了一种新的、环境友好且经济的光催化工艺，具有前所未有的高环己烷部分氧化活性。通过SBA-15依次与乙酰丙酮钛(IV)和乙酰丙酮铁(III)反应合成了孔表面固定有分离的四面体配位Ti和Fe氧化物纳米颗粒的介孔二氧化硅。各种表征表明，接枝的四面体配位钛物种通过 Ti-O-Fe 键与 Fe 氧化物纳米颗粒偶联。 SBA-15光催化剂在太阳光下用分子O2生产环己醇和环己酮时表现出高产率（高达亚毫摩尔）和接近100%的选择性。前所未有的高活性可以通过Ti-O-Fe键上的电子离域延长活性Ti物质的寿命以及与Ti物质偶联的Fe氧化物纳米粒子赋予的可见光（λ> 420 nm）诱导的活性来解释。
We report a new, environmentally and economically friendly photocatalytic process with unprecedentedly high activity for partial cyclohexane oxidation. Mesoporous silicas containing isolated tetrahedrally 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 O2 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 (λ > 420 nm)-induced activity endowed by Fe oxide nanoparticles coupled to the Ti species.