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

Lu LI; Linghui LIU; Jinming XU; Yanqiang HUANG; Tao ZHANG

doi:10.11949/0438-1157.20200680

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

Material science and engineering, nanotechnology | 更新时间：2025-11-25

- Synthesis of ruthenium-embedded nitrogen-doped graphene for carbon dioxide hydrogenation
- CIESC Journal Vol. 71, Issue 10, Pages: 4800-4807(2020)
- 作者机构：
  
  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
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20200680
  CLC： TQ 032.4
- Received：02 June 2020，
  
  Revised：2020-07-20，
  
  Published：05 October 2020
- 稿件说明：
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李路, 刘灵惠, 徐金铭, 黄延强, 张涛. 负载钌的氮掺杂石墨烯催化剂的制备及应用[J]. 化工学报, 2020, 71(10): 4800-4807

LI Lu, LIU Linghui, XU Jinming, HUANG Yanqiang, ZHANG Tao. Synthesis of ruthenium-embedded nitrogen-doped graphene for carbon dioxide hydrogenation[J]. CIESC Journal, 2020, 71(10): 4800-4807
李路, 刘灵惠, 徐金铭, 黄延强, 张涛. 负载钌的氮掺杂石墨烯催化剂的制备及应用[J]. 化工学报, 2020, 71(10): 4800-4807 DOI： 10.11949/0438-1157.20200680.

LI Lu, LIU Linghui, XU Jinming, HUANG Yanqiang, ZHANG Tao. Synthesis of ruthenium-embedded nitrogen-doped graphene for carbon dioxide hydrogenation[J]. CIESC Journal, 2020, 71(10): 4800-4807 DOI： 10.11949/0438-1157.20200680.

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。

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 N

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

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.

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references

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