CIESC Journal ›› 2020, Vol. 71 ›› Issue (10): 4800-4807.DOI: 10.11949/0438-1157.20200680

• Material science and engineering, nanotechnology • Previous Articles     Next Articles

Synthesis of ruthenium-embedded nitrogen-doped graphene for carbon dioxide hydrogenation

Lu LI1,2(),Linghui LIU1,3(),Jinming XU1(),Yanqiang HUANG1,Tao ZHANG1   

  1. 1.Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
    2.College of Chemistry and Chemical Engineering, Yantai University, Yantai 264005, Shandong, China
    3.School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
  • Received:2020-06-02 Revised:2020-07-20 Online:2020-10-05 Published:2020-10-05
  • Contact: Jinming XU

负载钌的氮掺杂石墨烯催化剂的制备及应用

李路1,2(),刘灵惠1,3(),徐金铭1(),黄延强1,张涛1   

  1. 1.中国科学院大连化学物理研究所,辽宁 大连 116023
    2.烟台大学化学与化工学院,山东 烟台 264005
    3.重庆大学化学与化工学院,重庆 400044
  • 通讯作者: 徐金铭
  • 作者简介:李路(1990—),女,硕士研究生,1562607571@qq.com|刘灵惠(1991—),女,博士研究生,lhliu@dicp.ac.cn
  • 基金资助:
    科技部国家重点研发计划项目(2016YFB0600902);国家自然科学基金项目(21925803)

Abstract:

Two-dimensional (2D) layered materials have attracted great interest in the energy storage and catalysis field due to their graphene-like structure and excellent performance. Ruthenium-embedded nitrogen-doped graphene (Ru-NG) have been obtained by a novel method, using montmorillonite as hard template and Ru-phenanthroline chelate as precursor. After calcination in N2 atmosphere at 800℃, Ru-NG were obtained and further characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and nitrogen sorption. Ru-NG have 2D layered structure just like the montmorillonite template, and C, N, O and Ru are homogeneously distributed on them. The average sizes of Ru nanoparticles do not change much with the increasing of Ru content, and they keep at about 1.2 to 1.4 nm. The XPS results indicate that phenanthroline has been successfully transformed to nitrogen-doped carbon during pyrolysis, and the peaks at 398.5, 400.1 and 401.5 eV suggest the presence of pyridine-like, pyrrole-like and quaternary nitrogen atoms, respectively. Compared with the Ru catalyst supported on activated carbon prepared by the traditional impregnation-reduction method, Ru-NG exhibits excellent catalytic activity in the reaction of hydrogenation of carbon dioxide to formic acid.

Key words: catalyst, carbon dioxide, hydrogenation, hard template method, composites, graphene

摘要:

利用人工合成的蒙脱石做硬模板,以插层的邻菲罗啉-钌络合物为前体,在惰性气氛下热解后用氢氟酸和盐酸刻蚀除去蒙脱石模板制备出负载钌纳米粒子的氮掺杂石墨烯催化剂(Ru-NG)。Ru-NG具有与模板蒙脱石类似的层状石墨烯结构,C、N、O及Ru元素在其上分布均匀。Ru-NG中钌的含量随钌前体的加入量的增加而增加,但受蒙脱石片层的物理限域作用及与含氮物种的配位作用,钌纳米粒子的粒径却无显著变化,且粒径均一,平均粒径在1.2~1.4 nm范围内。与传统浸渍-还原法制备的活性炭负载的Ru催化剂相比,Ru-NG在二氧化碳加氢生成甲酸反应中表现出优异的催化活性。

关键词: 催化剂, 二氧化碳, 加氢, 硬模板法, 复合材料, 石墨烯

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