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Manipulation of plasmon-induced hot electron transport in Pd/MoO3-x@ZIF-8: Boosting the activity of Pd-catalyzed nitroaromatic hydrogenation under visible-light irradiation
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2020-09-06 , DOI: 10.1016/j.apcatb.2020.119511
Meicheng Wen , Shengnan Song , Qiuxia Liu , Haibo Yin , Kohsuke Mori , Yasutaka Kuwahara , Guiying Li , Taicheng An , Hiromi Yamashit

Controlling the charge carrier transfer pathway in a plasmonic catalyst is the key to developing efficient catalyst. Herein, a visible-light responsive plasmonic catalyst is prepared by depositing Pd nanoparticles on ZIF-8 (zeolitic imidazolate framework) coated plasmonic MoO3-x composites (Pd/MoO3-x@ZIF-8). The as-prepared catalyst allows effective plasmon-induced electron transfer from plasmonic MoO3-x to Pd active site by taking advantages of the Schottky junction formed between Pd metal nanoparticles and MoO3-x@ZIF-8 composite as well as heterojunction formed between ZIF-8 and MoO3-x, effectively retarding the recombination of the plasmonic induced hot electron-hole pairs in MoO3-x. As a result, the Pd/MoO3-x@ZIF-8 presents exceptionally higher catalytic activities for the hydrogenation of nitroaromatics under visible-light irradiation than that under dark conditions, which are far superior to those of Pd/MoO3-x and Pd/ZIF-8. The enhanced activity can be attributed to the cooperative promoting effects between Pd nanoparticles and plasmonic MoO3-x@ZIF-8 on facilitating the plasmon-induce electron transfer, and the possible reaction mechanism is proposed. This study expands the scope of reductive organic chemical transformation catalyzed by plasmonic catalysts and sheds light on design of efficient plasmonic catalysts by steering an electron flow to promote the photogenerated electron transfer from plasmonic semiconductor to catalytic active site.



中文翻译:

在Pd / MoO 3-x @ ZIF-8中操纵等离激元诱导的热电子传输:在可见光照射下提高Pd催化的硝基芳族氢化的活性

控制等离激元催化剂中的电荷载流子转移途径是开发高效催化剂的关键。本文中,通过将Pd纳米颗粒沉积在ZIF-8(沸石咪唑酸酯骨架)涂覆的等离子MoO 3-x复合材料(Pd / MoO 3-x ZIF-8)上来制备可见光响应型等离激元催化剂。通过利用Pd金属纳米颗粒与MoO 3-x @ ZIF-8复合材料之间形成的肖特基结以及在Pd金属纳米颗粒与MoO 3-x @ ZIF-8复合材料之间形成的异质结,所制备的催化剂可以使等离激元诱导的电子有效地从等离激元MoO 3-x转移到Pd活性位点。 ZIF-8和的MoO 3-X 有效延缓等离子体振子诱生热电子-空穴对的再结合中的MoO 3-x。结果,Pd / MoO 3-x @ ZIF-8在可见光照射下表现出比在黑暗条件下更高的催化硝基芳烃氢化的催化活性,远远优于Pd / MoO 3-x和Xd -8。钯/ ZIF-8。增强的活性可以归因于Pd纳米颗粒与等离子体MoO 3-x的协同促进作用@ ZIF-8对促进等离子体激元诱导电子转移,并提出了可能的反应机理。这项研究扩大了等离子体催化剂催化的还原性有机化学转化的范围,并通过控制电子流以促进光生电子从等离子体半导体转移到催化活性位,为高效等离子体催化剂的设计提供了启示。

更新日期:2020-09-20
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