谭静静,高宽,苏以豪,崔静磊,张静,赵永祥.Ru/磺化石墨烯催化木糖直接转化制备糠醇[J].分子催化编辑部,2021,35(2):103-112
Ru/磺化石墨烯催化木糖直接转化制备糠醇
Direct Conversion of Xylose to Furfuryl Alcohol over Ru/Sulfonated Graphene Catalyst
投稿时间:2021-02-08  修订日期:2021-03-11
DOI:10.16084/j.issn1001-3555.2021.02.001
中文关键词:  木糖  糠醛  糠醇  Ru/磺化石墨烯  金属-酸双中心
英文关键词:xylose  furfural  furfuryl alcohol  Ru/sulfonated graphene  metal-acid double center
基金项目:国家自然科学基金项目(No.22005182,21703275,21972081,U1710221);山西省高等学校科技创新项目(No.2020L0012)和山西省面上青年基金项目(No.201701D221030)
作者单位E-mail
谭静静 山西大学 精细化学品教育部工程研究中心, 山西 太原 030006 tanjingjing@sxu.edu.cn 
高宽 山西大学 精细化学品教育部工程研究中心, 山西 太原 030006
山西大学 化学化工学院, 山西 太原 030006 
 
苏以豪 山西大学 精细化学品教育部工程研究中心, 山西 太原 030006
山西大学 化学化工学院, 山西 太原 030006 
 
崔静磊 山西大学 资源与环境工程研究所, 山西 太原 030006  
张静 山西大学 应用化学研究所, 山西 太原 030006  
赵永祥 山西大学 精细化学品教育部工程研究中心, 山西 太原 030006 yxzhao@sxu.edu.cn 
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中文摘要:
      以氧化石墨烯为载体,在其表面引入酸性位-SO3H和金属位Ru,制备了Ru/磺化石墨烯金属-酸双中心催化剂(Ru/SRGO).采用X-射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、激光拉曼光谱(Raman)、X-射线光电子能谱(XPS)、透射电子显微镜(TEM)和酸-碱滴定等技术对催化剂的结构和性质进行了表征.相对氧化石墨烯,磺化改性后石墨烯的特征衍射峰向低角度偏移(XRD),在Raman光谱中其D峰发生红移,G峰发生蓝移,结合ID/IG的比值证实其表面产生更多有利于活性金属Ru负载及其稳定的缺陷位.酸性表征显示催化剂表面-SO3H密度随磺化过程中添加磺化试剂含量的增加而增加.在催化木糖直接制备糠醇的反应过程中,催化剂的活性与其表面的酸量呈正相关,而产物糠醇的选择性则随酸量的增加呈现“火焰山形态”分布,在金属和酸双中心量的匹配及其协同催化下,在150℃,1 MPa H2条件下,实现了木糖高效转化制备糠醇,其收率达70.4%.
英文摘要:
      A Ru/sulfonated graphene (Ru/SRGO) metal-acid double center catalyst was prepared using oxide graphene as a support and -SO3H as an acid site. The composition, structure and properties of the catalyst were characterized by X-ray diffraction(XRD), Fourier transform infrared(FTIR), Laser raman spectroscopy(Raman), X-ray photoelectron spectroscopy(XPS), Transmission electron microscope(TEM), acid-base titration and so on. The acidic functional group -SO3H and metal active sites were successfully introduced into the surface of graphene, which were proved by FTIR, Raman, XPS and TEM. Compared with graphene oxide, the characteristic diffraction peak of sulfonated graphene shifts to a low angle (XRD), and in the Raman spectrum, the peak of D occurred red-shift, while the peak of G appeared blue-shift, combing with the value of ID/IG, indicating thatmore defects which are conducive to the loading and stabilization of active metal Ru was presented. The acid characterization confirmed that the surface acid density of the catalyst increased linearly with the increase of the sulfonated reagent content during the modification process. The activity of the Ru/SRGO catalyst is positively correlated with the amount of acid on the surface, while the selectivity of furfuryl alcohol is distributed in a "flame-like" shape with the increase of the density of acid for direct conversion of xylose to furfuryl alcohol. Under the matching of the amount of metal and acid and their synergistic catalysis, the conversion of xylose was achieved 100% with a yield of 70.4% for furfuryl alcohol under the conditions of 150℃ and 1 MPa H2.
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