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关于W-Ni双金属催化剂上生物质高效催化转化为乙二醇和1,2-丙二醇的见解。

Insight into the efficient catalytic conversion of biomass to EG and 1,2-PG over W-Ni bimetallic catalyst.

作者信息

Li Meng-Qing, Ma Yu-Long, Ma Xiao-Xia, Sun Yong-Gang, Song Zhi

机构信息

State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University Yinchuan 750021 China

出版信息

RSC Adv. 2018 Mar 19;8(20):10907-10913. doi: 10.1039/c8ra00584b. eCollection 2018 Mar 16.

Abstract

In this work, a mesoporous silica microsphere (MSM) was selected as a support to prepare a bimetallic supported catalyst (15% W-5% Ni/MSM) by a co-impregnation method that was simple and easy to conduct. We wished to improve the capability of catalytic conversion of biomass into ethylene glycol (EG) and 1,2-propylene glycol (1,2-PG). 15% W-5% Ni/MSM was examined on microcrystalline cellulose (cellulose) and corn stalks in a one-pot catalytic process, and total yields of EG and 1,2-PG reached up to 82.40 wt% and 62.60 wt%, respectively. This remarkable catalytic performance of W-Ni/MSM catalyst could be attributed to the synergistic effect between the active sites of Ni and W and the unique structure of MSM, which was suitable for mass transfer and metal loading. Based on physicochemical characterizations, the metal component was well-distributed on the surface of the MSM, and the metallic Ni, W and WO of the fresh catalyst were converted mainly into NiWO during the catalytic conversion of cellulose. To shed light on the reaction mechanism of the catalyzed hydrogenation of biomass, a possible process involving the formation of H WO homogeneous catalysts, cellulose hydrolysis, C-C cleavage and hydrogenation conversion to 1,2-PG and EG was illustrated. Furthermore, the reusability of W-Ni/MSM catalyst was tested and we explored the cause of decreased diols yields. In summary, this work provides important guidance to rationally design effective catalysts for biomass conversion.

摘要

在本工作中,选用介孔二氧化硅微球(MSM)作为载体,通过简单易行的共浸渍法制备了双金属负载型催化剂(15%W-5%Ni/MSM)。我们希望提高生物质催化转化为乙二醇(EG)和1,2-丙二醇(1,2-PG)的能力。在微晶纤维素(纤维素)和玉米秸秆的一锅法催化过程中对15%W-5%Ni/MSM进行了考察,EG和1,2-PG的总产率分别达到了82.40 wt%和62.60 wt%。W-Ni/MSM催化剂的这种卓越催化性能可归因于Ni和W活性位点之间的协同效应以及MSM的独特结构,该结构适合传质和金属负载。基于物理化学表征,金属组分在MSM表面分布良好,新鲜催化剂中的金属Ni、W和WO在纤维素催化转化过程中主要转化为NiWO。为了阐明生物质催化加氢的反应机理,阐述了一个可能的过程,包括形成H WO均相催化剂、纤维素水解、C-C键断裂以及加氢转化为1,2-PG和EG。此外,测试了W-Ni/MSM催化剂的可重复使用性,并探究了二醇产率降低的原因。总之,这项工作为合理设计用于生物质转化的有效催化剂提供了重要指导。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7d1d/9078988/803c0a32df0a/c8ra00584b-f1.jpg

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