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核壳等离子体分级结构硫化铜微球@沸石咪唑框架-8中的光热增强催化作用

Photothermal-enhanced catalysis in core-shell plasmonic hierarchical CuS microsphere@zeolitic imidazole framework-8.

作者信息

Wang Feifan, Huang Yanjie, Chai Zhigang, Zeng Min, Li Qi, Wang Yuan, Xu Dongsheng

机构信息

Beijing National Laboratory for Molecular Sciences , State Key Laboratory for Structural Chemistry of Unstable and Stable Species , College of Chemistry and Molecular Engineering , Peking University , Beijing 100871 , P. R. China . Email:

Academy for Advanced Interdisciplinary Studies , Peking University , Beijing 100871 , P. R. China.

出版信息

Chem Sci. 2016 Dec 1;7(12):6887-6893. doi: 10.1039/c6sc03239g. Epub 2016 Aug 11.

Abstract

Conventional semiconductor photocatalysis based on band-edge absorption remains inefficient due to the limited harvesting of solar irradiation and the complicated surface/interface chemistry. Herein, novel photothermal-enhanced catalysis was achieved in a core-shell hierarchical CuS nano-heater@ZIF-8 heterostructures near-infrared localized surface plasmon resonance. Our results demonstrated that both the high surface temperature of the photothermal CuS core and the close-adjacency of catalytic ZIF-8 shell contributed to the extremely enhanced catalytic activity. Under laser irradiation (1450 nm, 500 mW), the cyclocondensation reaction rate increased 4.5-5.4 fold compared to that of the process at room temperature, in which the 1.6-1.8 fold enhancement was due to the localized heating effect. The simulated sunlight experiments showed a photothermal activation efficiency (PTAE) of 0.07%, further indicating the validity of photothermal catalysis based on the plasmonic semiconductor nanomaterials. More generally, this approach provides a platform to improve reaction activity with efficient utilization of solar energy, which can be readily extended to other green-chemistry processes.

摘要

基于带边吸收的传统半导体光催化由于对太阳辐射的有限捕获以及复杂的表面/界面化学而仍然效率低下。在此,通过核壳分级CuS纳米加热器@ZIF-8异质结构中的近红外局域表面等离子体共振实现了新型光热增强催化。我们的结果表明,光热CuS核的高表面温度和催化ZIF-8壳的紧密相邻都有助于极大地增强催化活性。在激光照射(1450 nm,500 mW)下,环缩合反应速率比室温下的过程提高了4.5至5.4倍,其中1.6至1.8倍的提高归因于局部加热效应。模拟太阳光实验显示光热活化效率(PTAE)为0.07%,进一步表明基于等离子体半导体纳米材料的光热催化的有效性。更普遍地说,这种方法提供了一个通过有效利用太阳能来提高反应活性的平台,并且可以很容易地扩展到其他绿色化学过程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/fdd1/5450595/b05ddecde942/c6sc03239g-s1.jpg

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