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氧化硅载体对Ir-Re双金属的结构及其催化甘油氢解的影响
  • ISSN号:0438-1157
  • 期刊名称:《化工学报》
  • 时间:0
  • 分类:TQ203.2[化学工程—有机化工]
  • 作者机构:华东理工大学化学工程联合国家重点实验室,上海200237
  • 相关基金:国家自然科学基金项目(21106047)~~
中文摘要:

采用3种氧化硅载体KIT-6、G-6和FS制备了Ir-Re双金属催化剂,并应用于甘油选择性氢解制备1,3-丙二醇,采用TEM、XRD、H2-TPR、CO-DRIFTS和NH3-TPD等手段详细表征了催化剂结构,并探讨其构效关系。研究结果表明:3种催化剂表面的Ir-Re双金属催化剂均形成了Ir-Re合金结构,合金化程度为Ir-Re/KIT-6〉Ir-Re/FS〉Ir-Re/G-6;载体表面羟基含量显著影响Ir-Re纳米粒子的分散度及其与载体的相互作用。Ir-Re/FS的金属分散度最高,甘油氢解的初始活性最高但稳定性最差;而具有良好合金结构的Ir-Re/KIT-6在甘油氢解中表现出良好的氢解活性和最高的1,3-丙二醇选择性。

英文摘要:

As an alternative process to petroleum based processes, hydrogenolysis of biomass-derived glycerol to 1, 3-propanediol(1, 3-PD) can be effectively catalyzed by bimetallic Ir-Re catalyst. However it still suffers from low selectivity of 1, 3-PD and low reaction rate. With extension of our previous study, silica was selected as a promising catalyst support to investigate the role of silica chemistry in the Ir-Re catalyst for glycerol hydrogenolysis. Bimetallic Ir-Re catalysts supported on three kinds of silica supports of KIT-6, G-6 and FS were prepared for glycerol hydrogenolysis to produce desired 1, 3-PD. The structure of catalysts were characterized by varied techniques of N2 adsorption-desorption, transmission electron microscopy(TEM), X-ray diffraction(XRD), H2 temperature-programmed reduction(H2-TPR), in-situ CO adsorption diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) and temperature-programmed desorption(TPD) of ammonia. Also, the structure-activity relationship of the catalysts was discussed. It showed that the bimetallic catalysts on three silica supports possessed alloy structure of Ir-Re on surface, of which the order of alloy degree follows Ir-Re/KIT-6Ir-Re/FSIr-Re/G-6. Hydroxyl groups on support surfaces significantly affected the degree of metal dispersion and the interaction between active metallic components and support. The Ir-Re/FS catalyst possessed the highest degree of metal dispersion and exhibited the best initial activity but the worst stability for glycerol hydrogenolysis, while the Ir-Re/KIT-6 catalyst featured the highest degree of alloy thus showed excellent catalytic performance and the highest selectivity to 1, 3-PD of desired product.

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期刊信息
  • 《化工学报》
  • 中国科技核心期刊
  • 主管单位:中国科学技术协会
  • 主办单位:中国化工学会 化学工业出版社
  • 主编:李静海
  • 地址:北京市东城区青年湖南街13号
  • 邮编:100011
  • 邮箱:hgxb126@126.com
  • 电话:010-64519485
  • 国际标准刊号:ISSN:0438-1157
  • 国内统一刊号:ISSN:11-1946/TQ
  • 邮发代号:2-370
  • 获奖情况:
  • 中国科协优秀期刊二等奖,化工部科技进步二等奖,北京全优期刊奖,中国期刊方阵“双效”期刊,第三届中国出版政府奖
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),中国北大核心期刊(2000版)
  • 被引量:35185