Construction of indium oxide/N-doped titanium dioxide hybrid photocatalysts for efficient and selective oxidation of cyclohexane to cyclohexanone
Construction of indium oxide/N-doped titanium dioxide hybrid photocatalysts for efficient and selective oxidation of cyclohexane to cyclohexanone
复制标题
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为环己酮
DOI：
10.1021/acs.jpcc.1c05730
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发表时间：
2021
影响因子：
3.7
通讯作者：
Liu Zhao-Tie
中科院分区：
文献类型：
--
作者：
Wang Kuan;Xue Bing;Wang Jun-Lei;He Zhen-Hong;Li Song-Song;Wang Dan;Wang Wei-Tao;Yang Yang;Liu Zhao-Tie
光催化氧化环己烷（CHA）生成环己酮（CHA- 1）是生产尼龙6和尼龙66的重要环节之一。本文采用水热n掺杂法和浸渍法两步策略，成功构建了具有p-n异质界面的氧化铟/掺n的二氧化钛（In2O3/N-TiO2）杂化光催化剂。在绿色和温和的反应条件下（室温、常压和无溶剂），In2O3/ n - tio2杂化催化剂在模拟太阳光下获得了理想的光催化性能。与裸TiO2相比，5% In2O3/ n -TiO2复合材料对cha - 1的催化活性提高了4倍，对cha - 1的选择性提高了约90%。此外，In2O3/ n - tio2复合材料表现出良好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，In2O3/ n - tio2的光催化性能增强可归因于n掺杂引起的高可见光吸收和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In2O3/ n - tio2催化剂上的一种可能的光氧化机理，并通过捕获活性物质的检测进行了验证。因此，本方法为扩大二氧化钛基光催化剂在选择性光氧化中的应用提供了绿色和前瞻性的策略。
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-TiO2hybrid catalyst achieved the desired photocatalytic performance for the production of CHA-one at simulated solar light. Compared with bare TiO2, the 5% In2O3/N-TiO2composite 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-TiO2composites 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-TiO2can 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-TiO2catalyst 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.