Chen Xiaofei, Zhang Guohua, Li Bao, Wu Lixin
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, China.
Sci Adv. 2021 Jul 23;7(30). doi: 10.1126/sciadv.abf8413. Print 2021 Jul.
A strategy integrating near infrared (NIR) photothermal and catalytic effects within one active center beyond ultraviolet and visible light is proposed without the combination of separated photothermal transformation components. A giant polyoxomolybdate, which has high NIR photothermal conversion efficiency, is selected as the model catalyst, while a cationic β-cyclodextrin is used to cover its negatively charged surface electrostatically. Under NIR light radiation, the designed catalyst increases catalytic activity of cyclohexene oxidation under O atmosphere in water. The conversion reaches about pentaploid of the reaction without NIR radiation. By excluding heating effect from the external heater at the same temperature, about twice as much enhancement, which can be attributed to the sole photothermal action, is still observed. While the catalytic center is shielded by the organic porous layer, the surface cavity allows the integrated catalyst to conduct a selective catalysis by screening the molecules in size over the surface channel.
提出了一种在一个活性中心内整合近红外(NIR)光热和催化效应的策略,该活性中心超越了紫外线和可见光,且无需结合分离的光热转换组件。选择具有高近红外光热转换效率的巨型多金属氧酸盐作为模型催化剂,同时使用阳离子β-环糊精通过静电作用覆盖其带负电荷的表面。在近红外光辐射下,所设计的催化剂在水中氧气氛围下提高了环己烯氧化的催化活性。转化率达到无近红外辐射反应的约五倍。通过在相同温度下排除外部加热器的加热效应,仍观察到约两倍的增强,这可归因于唯一的光热作用。当催化中心被有机多孔层屏蔽时,表面空腔允许整合催化剂通过筛选表面通道上尺寸过大的分子进行选择性催化。