Visible-light-driven selective oxidation of alcohols using a dye-sensitized TiO2-polyoxometalate catalyst
Visible-light-driven selective oxidation of alcohols using a dye-sensitized TiO2-polyoxometalate catalyst
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使用染料敏化 TiO2-多金属氧酸盐催化剂进行可见光驱动的醇选择性氧化
DOI：
10.1016/j.jcat.2017.03.017
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发表时间：
2017-07
影响因子：
7.3
通讯作者：
Cao Rong
中科院分区：
文献类型：
--
作者：
Yang Xue;Zhao Hui;Feng Jifei;Chen Yanning;Gao Shuiying;Cao Rong
本研究展示了染料敏化的TiO 2-聚氧乙烯酸盐体系（表示为TiO 2-（PW 12-TH）8，其中PW 12 = PW 12 O 403-，TH =噻托溴铵）在可见光下选择性氧化醇类。结果表明，各种取代醇都能高选择性地转化为相应的醛。TiO 2-（PW 12-TH）8光催化剂具有电子转移效率高、比表面积大、可见光吸收增强等优点，其光催化活性上级优于其他染料敏化体系。在几个开/关周期的间歇照射的光电流-时间曲线的响应表现出良好的再现性。结果表明，TiO 2-（PW 12-TH）8的光电流响应远高于TiO 2/TH、SiO2-（PW 12-TH）8和P25-（PW 12-TH）8（P25 = Degussa P25），这是由于光激发电子的转移效率和寿命更高。该光催化过程证实了光催化氧化过程中有效的电子转移在决定反应转化率和获得良好的选择性方面起着至关重要的作用。电子顺磁共振（EPR）谱和自由基清除实验证明，超氧自由基和电子是该体系的主要反应物种，羟基自由基和空穴的不存在是高反应选择性的关键。
This study demonstrated a dye-sensitized TiO2-polyoxometalate system (denoted TiO2-(PW12-TH)8, where PW12= PW12O403−and TH = thionine) for selective oxidation of alcohols under visible light. The results showed that various substituted alcohols were transformed into their corresponding aldehydes with high selectivity. Due to more efficient electrons transfer, large surface area, and enhanced visible light absorption, the photocatalytic activity of TiO2-(PW12-TH)8was superior to any other dye-sensitized system reported to date. The response in the photocurrent-time curves over several on/off cycles of intermittent irradiation showed good reproducibility. The photocurrent response of TiO2-(PW12-TH)8was much higher than that of TiO2/TH (physical mixture of TiO2and TH), SiO2-(PW12-TH)8or P25-(PW12-TH)8(P25 = Degussa P25), attributed to the more efficient transfer and longer lifetime of photoexcited electrons. This photocatalytic process confirmed that efficient electron transfer during photocatalytic oxidation plays a vital role in determining the reaction conversion and obtaining good selectivity. Electron paramagnetic resonance (EPR) spectra and radical scavenging experiments proved that superoxide radicals and electrons were the main reactive species in the proposed system, the absence of hydroxyl radicals and holes is demonstrated to be the key of high reaction selectivity.
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影响因子：
11.4
作者：
Cho, YM;Choi, WY;Lee, HI
通讯作者：
Lee, HI
影响因子：
--
作者：
Tao Wang;Xianguang Meng;Guigao Liu;Kun Chang;Peng Li;Qing Kang;Lequan Liu;Mu Li;S. Ouyang-
通讯作者：
Tao Wang;Xianguang Meng;Guigao Liu;Kun Chang;Peng Li;Qing Kang;Lequan Liu;Mu Li;S. Ouyang-
影响因子：
4.9
作者：
Palmisano, Giovanni;Garcia-Lopez, Elisa;Palmisano, Leonardo
通讯作者：
Palmisano, Leonardo
影响因子：
10.8
作者：
Wang, Daoai;Liu, Lifeng;Domen, Kazunari
通讯作者：
Domen, Kazunari
具有优异可见光光催化活性的核壳结构CdS@SnO2纳米棒用于苯甲醇选择性氧化为苯甲醛
影响因子：
9.5
作者：
Liu, Ya;Zhang, Ping;Zhang, Jinlong
通讯作者：
Zhang, Jinlong