Catalyst consisting of Ag nanoparticles anchored on amine-derivatized mesoporous silica nanospheres for the selective hydrogenation of dimethyl oxalate to methyl glycolate
Catalyst consisting of Ag nanoparticles anchored on amine-derivatized mesoporous silica nanospheres for the selective hydrogenation of dimethyl oxalate to methyl glycolate
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DOI：
10.1016/j.jcat.2020.08.018
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发表时间：
2020-11-01
影响因子：
7.3
通讯作者：
Zhou, Xinggui
中科院分区：
文献类型：
--
作者：
Dong, Guilin;Cao, Yueqiang;Zhou, Xinggui
开发高效的草酸二甲酯(DMO)选择加氢催化剂对煤基生产乙醇酸甲酯(MG)具有重要意义，但该转化工艺的设计具有挑战性。在这里，我们报道了一种前所未有的催化DMO选择加氢合成MG的性能，这是通过使用固定在胺衍生物二氧化硅纳米球(NH2-MSNS)介孔内的银纳米粒子(NH2-MSNS)实现的。结果表明，胺衍生物通道表面所赋予的独特微环境有助于该银催化剂促进DMO和H-2的活化，高选择性地生成MG，并防止了烧结和结焦，从而提高了稳定性。相应地，所得到的Ag/NH2-MSNS催化剂能够促进加氢反应，其转化频率为230h(-1)，在DMO转化率接近100%的情况下，MG选择性为97%，这一性能至少持续了250h，这些结果明显好于其他文献报道的催化剂。我们的研究为开发用于煤基金属镁生产的高性能银催化剂提供了一条很有前途的途径。(C)2020 Elsevier Inc.保留所有权利。
Developing efficient catalysts for the selective hydrogenation of dimethyl oxalate (DMO) is of great significance for the coal-based production of methyl glycolate (MG), but designing processes for this conversion is challenging. Herein we report an unprecedented catalytic performance for the selective hydrogenation of DMO to MG, achieved by using a catalyst based on Ag nanoparticles anchored inside the mesopores of amine-derivatized silica nanospheres (NH2-MSNS). It was determined that the unique microenvironment endowed by the amine-derivatized channel surfaces helps this Ag catalyst promote the activation of DMO and H-2 to yield MG with high selectivity, and also prevents sintering and coking, hence improving stability. Accordingly, the resulting Ag/NH2-MSNS catalyst was shown to be capable of promoting the hydrogenation reaction with a turnover frequency of 230 h(-1) and a MG selectivity of 97% at nearly 100% of DMO conversion, a performance that was sustained for at least 250 h; these results are significantly better than those seen with other reported catalysts. Our study points to a promising route for the development of high-performing Ag catalysts to be used in the coal-based MG production. (C) 2020 Elsevier Inc. All rights reserved.