Highly selective oxidation of furfuryl alcohol over monolayer titanate nanosheet under visible light irradiation
Highly selective oxidation of furfuryl alcohol over monolayer titanate nanosheet under visible light irradiation
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可见光照射下单层钛酸酯纳米片上糠醇的高选择性氧化
DOI：
10.1016/j.apcatb.2017.10.069
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发表时间：
2018-05
期刊：
影响因子：
--
通讯作者：
Wu Ling
中科院分区：
文献类型：
--
作者：
Wang Hao;Song Yujie;Xiong Jinhua;Bi Jinhong;Li Liuyi;Yu Yan;Liang Shijing;Wu Ling
制备了单层H1.4Ti1.65O4·H2O纳米片（NST），并将其用于可见光催化氧化糠醇制备糠醛. NST的光催化活性比层状NST高10倍以上。这种增强的活性可能归因于NST中暴露的刘易斯酸位点的高百分比。原位FTIR结果表明，FA通过C单键O基团有效地吸附在表面暴露的刘易斯酸中心上形成配位物种，从而活化了FA.表面配位物种将响应可见光吸收。另外，XAFS结果表明，与层状结构相比，NST中的Ti单键O和Ti-Ti键的信号明显减弱，信号位置在高R方向上移动了0.03 μ m，表明NST中暴露了更多的Ti和O缺陷。在可见光照射下，吸收在这些表面缺陷上的氧分子被光电子激活，形成自由基dotO 2 −。最后，在分子水平上提出了一种可能的机制。
Monolayer H1.4Ti1.65O4·H2O nanosheet (denoted as NST) has been prepared as a photocatalyst for the oxidation of furfuryl alcohol (denoted as FA) to furaldehyde under visible light irradiation. The photocatalytic activity of NST is over 10 times higher than that of its layered counterpart. This enhanced activity may be attributed to the high percentage of exposed Lewis acid sites in NST. The in-situ FTIR result suggests that FA are efficiently chemosorbed on the exposed Lewis acid sites forming the surface coordination species via Csingle bondO groups, resulting in the activation of FA. The surface coordination species would respond to visible light absorption. Furthermore, The XAFS result shows that the signals for Tisingle bondO and Ti–Ti in NST are weaker dramatically and the signals positions are shifted by 0.03 Å in the higher R direction as compared with those in layered counterpart, suggesting the more exposed Ti and O defects in NST. The oxygen molecules absorbed on these surface defects are activated forming radical dotO2−by photo-electrons under visible light irradiation. Finally, a possible mechanism has been proposed at a molecular level.
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