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负载在具有 FeO 核和含磺酸的周期性介孔有机硅壳的磁性蛋黄壳纳米结构上的 Ru 纳米粒子作为双功能催化剂,用于纤维素直接转化为异山梨醇。

Ru nanoparticles dispersed on magnetic yolk-shell nanoarchitectures with FeO core and sulfoacid-containing periodic mesoporous organosilica shell as bifunctional catalysts for direct conversion of cellulose to isosorbide.

机构信息

State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Changping, Beijing 102249, China.

出版信息

Nanoscale. 2018 Feb 1;10(5):2199-2206. doi: 10.1039/c7nr07875g.

Abstract

A green and sustainable approach for biorefining involves the development of bifunctional catalysts for the one-pot conversion of cellulosic biomass to isosorbide. This requires highly efficient, easily separated and versatile metal-acid catalysts for hydrolysis-hydrogenation-dehydration cascade reactions. Herein, we report a new type of metal-acid bifunctional catalyst by dispersing Ru nanoparticles (NPs) on magnetic yolk-shell nanoarchitectures comprising an FeO core and a sulfoacid (SOH)-containing periodic mesoporous organosilica shell. The resultant magnetic Ru-SOH nanoreactors are highly porous and have large surface areas (>350 m g), uniform mesopores (∼3.8 nm), well-dispersed Ru NPs (<1.5 wt%) and superior magnetization. Tailoring the size of the Ru NPs and the amount of SOH moieties produced a highly efficient Ru-SOH nanocatalyst, which delivered a high yield of isosorbide of 58.1% with almost complete conversion of cellulose in 2 h and achieved maximum productivity of 2.19 mol h g, which was one order of magnitude higher than that achieved using other Ru-containing acidic catalysts. Moreover, the elaborately fabricated Ru-SOH nanocatalyst can be easily separated by applying an external magnetic field and can be cycled four times. This work reveals new possibilities for the fabrication of highly efficient, easily separated metal-acid catalysts in virtue of the concept of nanoreactor design.

摘要

一种绿色可持续的生物炼制方法涉及开发多功能催化剂,以实现纤维素生物质到异山梨醇的一锅转化。这需要高效、易于分离和多功能的金属-酸催化剂,用于水解-加氢-脱水级联反应。在此,我们通过将 Ru 纳米颗粒 (NPs) 分散在包含 FeO 核和含磺酸基 (SOH) 的周期性介孔有机硅壳的磁性蛋黄壳纳米结构上来报告一种新型的金属-酸双功能催化剂。所得的磁性 Ru-SOH 纳米反应器具有高度多孔性和大表面积 (>350 m g)、均匀的介孔 (∼3.8nm)、分散良好的 Ru NPs(<1.5wt%)和优异的磁化强度。调整 Ru NPs 的尺寸和 SOH 部分的数量可得到高效的 Ru-SOH 纳米催化剂,在 2 小时内纤维素几乎完全转化的情况下,异山梨醇的收率高达 58.1%,最大产率为 2.19 mol h g,这比使用其他含 Ru 酸性催化剂高一个数量级。此外,精心制备的 Ru-SOH 纳米催化剂可以通过施加外部磁场轻松分离,并可以循环使用四次。这项工作通过纳米反应器设计的概念揭示了制造高效、易于分离的金属-酸催化剂的新可能性。

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