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首页> 外文期刊>Catalysis science & technology >An efficient route to prepare highly dispersed metallic copper nanoparticles on ordered mesoporous silica with outstanding activity for hydrogenation reactions
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An efficient route to prepare highly dispersed metallic copper nanoparticles on ordered mesoporous silica with outstanding activity for hydrogenation reactions

机译：在有序的介孔二氧化硅上准备高度分散的金属铜纳米颗粒的有效途径，具有出色的氢化反应活性

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摘要

Copper nanoparticles at relatively high metal loading of 10 wt.% were successfully synthesized via incipient wetness impregnation by using polyether-functionalized ordered mesoporous silica as organic-inorganic hybrid supports. The effect of functionalized triblock copolymer Pluronic P123 (0, 25 and 50 wt.% of total triblock copolymer in gel) on the structural and catalytic properties of copper nanocomposite materials was specifically investigated. The oxide forms of materials were systematically characterized by nitrogen physisorption, SAXS, WAXS, TEM, EDXS, DR UV-vis and TPR, while the metallic forms were analysed by N2O chemisorption, WAXS and TEM. The results indicated that the use of mesoporous silica hybrids leads to highly dispersed supported copper nanoparticles (dispersions in the range of 43-57%) displaying excellent activity in the hydrogenation of cinnamaldehyde. The average particle size was shown to decrease from 2.3 to 1.7 nm with the increase in the amount of functionalized triblock copolymer from 0 to 50 wt.%. Under standard test conditions, all the nanosized copper catalysts showed high catalytic activity but selectivity towards the saturated aldehyde. Further improvements in activity and selectivity towards the unsaturated alcohol were achieved by increasing the hydrogen pressure and applying a two-step reduction-oxidation pre-treatment, respectively. The structure and controllable properties of nanoscale copper materials developed herein, both oxidic and metallic forms, make them very attractive candidates for both fundamental research and practical catalytic applications.
机译：通过使用多核官能化有序的中孔二氧化硅作为有机无机杂种载体，通过初期湿度浸渍成功合成了10 wt。％的铜纳米颗粒。专门研究了功能化的三嵌段共聚物共聚物P123（凝胶中总三嵌段共聚物的0、25和50 wt。％）对铜纳米复合材料的结构和催化性能的影响。氧化物形式的材料形式是通过氮物质，SAX，蜡，TEM，EDX，UV-VIS和TPR的，而金属形式通过N2O化学吸附，蜡和TEM分析的。结果表明，介孔二氧化硅杂种的使用导致高度分散的支持的铜纳米颗粒（分散在43-57％的分散体）在肉桂醛中表现出极好的活性。显示平均粒径从2.3降低到1.7 nm，功能化三嵌段共聚物的数量从0升至50 wt。％。在标准测试条件下，所有纳米化的铜催化剂均表现出较高的催化活性，但对饱和醛的选择性。通过增加氢压并分别应用两步减少氧化预处理，可以进一步改善对不饱和酒精的活性和选择性。本文开发的纳米级铜材料的结构和可控性能，包括氧化和金属形式，使其成为基础研究和实际催化应用的吸引力。

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