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Construction of Indium Oxide/N-Doped Titanium Dioxide Hybrid Photocatalysts for Efficient and Selective Oxidation of Cyclohexane to Cyclohexanone
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-09-01 , DOI: 10.1021/acs.jpcc.1c05730
Kuan Wang 1 , Bing Xue 1 , Jun-Lei Wang 1 , Zhen-Hong He 1 , Song-Song Li 1 , Dan Wang 1 , Wei-Tao Wang 1 , Yang Yang 1 , Zhao-Tie Liu 1, 2
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Photocatalytic oxidation of cyclohexane (CHA) to generate cyclohexanone (CHA-one) is one of the most important strategic links for the production of nylon-6 and nylon-66. Herein, an indium oxide/N-doped titanium dioxide (In2O3/N-TiO2) hybrid photocatalyst with a p–n heterointerface was successfully constructed by a two-step strategy of the hydrothermal N-doped method and impregnation method with structural reconstruction. Under green and mild reaction conditions (room temperature, atmospheric pressure, and solvent-free), the In2O3/N-TiO2 hybrid catalyst achieved the desired photocatalytic performance for the production of CHA-one at simulated solar light. Compared with bare TiO2, the 5% In2O3/N-TiO2 composite achieved a 4-fold increase for producing CHA-one in catalytic activity and an increase in selectivity to the CHA-one of approximately 90%. Moreover, the In2O3/N-TiO2 composites exhibited a desirable cycling durability and recoverability. According to the photoelectrochemical tests and density functional theory (DFT) calculations, the enhanced photocatalytic performance of In2O3/N-TiO2 can be attributed to high visible-light absorption derived from N-doping and fast separation of photoformed electron–hole pairs caused by the p–n heterointerface. A possible photo-oxidation mechanism of CHA over the In2O3/N-TiO2 catalyst was proposed and verified by the trapping detection of active species. Thereby, the present approach provides a green and prospective strategy for extending the application of the TiO2-based photocatalyst for selective photo-oxidation.

中文翻译:

氧化铟/氮掺杂二氧化钛杂化光催化剂的构建,用于环己烷高效选择性氧化成环己酮

环己烷(CHA)光催化氧化生成环己酮(CHA-one)是尼龙6和尼龙66生产的重要战略环节之一。在此,通过水热 N 掺杂法和浸渍法两步策略,成功构建了具有 ap-n 异质界面的氧化铟/N 掺杂二氧化钛(In 2 O 3 /N-TiO 2)杂化光催化剂。重建。在绿色温和的反应条件下(室温、常压和无溶剂),In 2 O 3 /N-TiO 2杂化催化剂在模拟太阳光下实现了生产CHA-one所需的光催化性能。与裸二氧化钛相比如图2所示,5%的In 2 O 3 /N-TiO 2复合物实现了生产CHA-one的4倍催化活性增加和对CHA-one的选择性增加约90%。此外,In 2 O 3 /N-TiO 2复合材料表现出理想的循环耐久性和可恢复性。根据光电化学测试和密度泛函理论(DFT)计算,In 2 O 3 /N-TiO 2 的光催化性能增强可以归因于 N 掺杂产生的高可见光吸收和由 p-n 异质界面引起的光形成电子 - 空穴对的快速分离。提出了CHA在In 2 O 3 /N-TiO 2催化剂上可能的光氧化机制,并通过活性物种的捕获检测进行了验证。因此,本方法为扩展基于TiO 2的光催化剂用于选择性光氧化的应用提供了一种绿色且有前景的策略。
更新日期:2021-09-16
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