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

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
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Pd/MoO3-x@ZIF-8 中等离激元诱导的热电子传输的操控:提高可见光照射下 Pd 催化硝基芳香族氢化的活性

DOI:
10.1016/j.apcatb.2020.119511
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发表时间:
2021-03
期刊:
Applied Catalysis B: Environmental
影响因子:
--
通讯作者:
Hiromi Yamashit
Hiromi Yamashit
中科院分区:
其他
文献类型:
--
作者:
Meicheng Wen;Shengnan Song;Qiuxia Liu;Haibo Yin;Kohsuke Mori;Yasutaka Kuwahara;Guiying Li;Taicheng An;Hiromi Yamashit

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控制等离子体催化剂中载流子的转移途径是开发高效催化剂的关键。本文通过将Pd纳米颗粒沉积在ZIF-8(沸石咪唑酸框架)涂层的等离子体moo3 - x复合材料(Pd/MoO3-x@ZIF-8)上,制备了一种可见光响应等离子体催化剂。所制备的催化剂利用Pd金属纳米颗粒与MoO3-x@ZIF-8复合材料之间形成的肖特基结以及ZIF-8与MoO3-x之间形成的异质结,使等离子体诱导的电子从MoO3-x有效地转移到Pd活性位点,有效地阻碍了MoO3-x中等离子体诱导的热电子-空穴对的重组。结果表明,Pd/MoO3-x@ZIF-8在可见光下对硝基芳烃加氢反应的催化活性明显高于黑暗条件下,远远优于Pd/MoO3-xand Pd/ZIF-8。活性的增强可归因于钯纳米粒子与等离子体MoO3-x@ZIF-8协同促进等离子体诱导的电子转移,并提出了可能的反应机理。本研究扩大了等离子体催化剂催化还原性有机化学转化的范围,并通过引导电子流促进光生电子从等离子体半导体转移到催化活性位点,为高效等离子体催化剂的设计提供了思路。
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-xcomposites (Pd/MoO3-x@ZIF-8). The as-prepared catalyst allows effective plasmon-induced electron transfer from plasmonic MoO3-xto 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-xand 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.
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