当前位置：
X-MOL 学术
›
J. Am. Chem. Soc.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Light-Induced Selective Hydrogenation over PdAg Nanocages in Hollow MOF Microenvironment
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-09-07 , DOI: 10.1021/jacs.2c06720 Luyan Li 1, 2 , Yanxiao Li 2 , Long Jiao 2 , Xiaoshuo Liu 3 , Zhentao Ma 4 , Yu-Jia Zeng 1 , Xusheng Zheng 4 , Hai-Long Jiang 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-09-07 , DOI: 10.1021/jacs.2c06720 Luyan Li 1, 2 , Yanxiao Li 2 , Long Jiao 2 , Xiaoshuo Liu 3 , Zhentao Ma 4 , Yu-Jia Zeng 1 , Xusheng Zheng 4 , Hai-Long Jiang 2
Affiliation
|
Selective hydrogenation with high efficiency under ambient conditions remains a long-standing challenge. Here, a yolk–shell nanostructured catalyst, PdAg@ZIF-8, featuring plasmonic PdAg nanocages encompassed by a metal–organic framework (MOF, namely, ZIF-8) shell, has been rationally fabricated. PdAg@ZIF-8 achieves selective (97.5%) hydrogenation of nitrostyrene to vinylaniline with complete conversion at ambient temperature under visible light irradiation. The photothermal effect of Ag, together with the substrate enrichment effect of the catalyst, improves the Pd activity. The near-field enhancement effect from plasmonic Ag and optimized Pd electronic state by Ag alloying promote selective adsorption of the −NO2 group and therefore catalytic selectivity. Remarkably, the unique yolk–shell nanostructure not only facilitates access to PdAg cores and protects them from aggregation but also benefits substrate enrichment and preferential −NO2 adsorption under light irradiation, the latter two of which surpass the core–shell counterpart, giving rise to enhanced activity, selectivity, and recyclability.
中文翻译：
中空 MOF 微环境中 PdAg 纳米笼的光诱导选择性氢化
在环境条件下高效选择性加氢仍然是一个长期存在的挑战。在这里，合理地制造了一种蛋黄壳纳米结构催化剂 PdAg@ZIF-8，该催化剂具有由金属有机框架（MOF，即 ZIF-8）壳包围的等离子体 PdAg 纳米笼。PdAg@ZIF-8 实现了硝基苯乙烯选择性 (97.5%) 氢化为乙烯基苯胺，并在环境温度下在可见光照射下完全转化。Ag的光热效应以及催化剂的底物富集效应提高了Pd的活性。等离子体Ag的近场增强效应和Ag合金化优化的Pd电子态促进-NO 2的选择性吸附基团，因此催化选择性。值得注意的是，独特的蛋黄壳纳米结构不仅有利于接触 PdAg 核并保护它们免于聚集，而且有利于底物富集和光照射下优先吸附 -NO 2，后两者超过核壳对应物，从而产生增强的活性、选择性和可回收性。
更新日期：2022-09-07
中文翻译：
中空 MOF 微环境中 PdAg 纳米笼的光诱导选择性氢化
在环境条件下高效选择性加氢仍然是一个长期存在的挑战。在这里，合理地制造了一种蛋黄壳纳米结构催化剂 PdAg@ZIF-8，该催化剂具有由金属有机框架（MOF，即 ZIF-8）壳包围的等离子体 PdAg 纳米笼。PdAg@ZIF-8 实现了硝基苯乙烯选择性 (97.5%) 氢化为乙烯基苯胺，并在环境温度下在可见光照射下完全转化。Ag的光热效应以及催化剂的底物富集效应提高了Pd的活性。等离子体Ag的近场增强效应和Ag合金化优化的Pd电子态促进-NO 2的选择性吸附基团，因此催化选择性。值得注意的是，独特的蛋黄壳纳米结构不仅有利于接触 PdAg 核并保护它们免于聚集，而且有利于底物富集和光照射下优先吸附 -NO 2，后两者超过核壳对应物，从而产生增强的活性、选择性和可回收性。
京公网安备 11010802027423号