化工学报 ›› 2020, Vol. 71 ›› Issue (2): 660-668.DOI: 10.11949/0438-1157.20190998

• 催化、动力学与反应器 • 上一篇    下一篇

煤基富氮层级多孔碳制备及其催化脱硫性能

孙明慧1,2(),陈静圆2,肖南1,2,陈奥博2,王旭珍1,2(),邱介山1,2,3()   

  1. 1.精细化工国家重点实验室,辽宁 大连 116024
    2.大连理工大学化工学院,辽宁省功能材料化工重点实验室,辽宁 大连 116024
    3.北京化工大学化学工程学院,北京 100029
  • 收稿日期:2019-09-03 修回日期:2019-11-08 出版日期:2020-02-05 发布日期:2020-02-05
  • 通讯作者: 王旭珍,邱介山
  • 作者简介:孙明慧(1993—),女,硕士研究生,smh1105@mail.dlut.edu.cn
  • 基金资助:
    国家自然科学基金项目(U1610105)

Preparation of hierarchical nitrogen-rich porous carbon from coal tar for catalytic desulfurization

Minghui SUN1,2(),Jingyuan CHEN2,Nan XIAO1,2,Aobo CHEN2,Xuzhen WANG1,2(),Jieshan QIU1,2,3()   

  1. 1.State Key Laboratory of Fine Chemical Engineering, Dalian 116024, Liaoning, China
    2.School of Chemical Engineering & Liaoning Key Laboratory for Energy Materials and Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China
    3.School of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
  • Received:2019-09-03 Revised:2019-11-08 Online:2020-02-05 Published:2020-02-05
  • Contact: Xuzhen WANG,Jieshan QIU

摘要:

以煤加工副产物煤焦油中蒽油馏分为碳源、多巴胺为氮源,基于纳米碳酸钙球模板在碳化过程中发生的诱导自活化作用,一步共碳化制得氮掺杂多孔碳(NPCs)材料。通过元素分析、低温氮气吸附-脱附测试、扫描及透射电镜表征,结果表明,NPCs材料的氮元素掺杂量高,且具有发达的微孔-介孔梯级孔道结构。结合室温下催化硫化氢选择性氧化为单质硫的反应性能评价,发现改变模板剂用量、碳/氮源投料比和碳化温度,可调控NPCs材料的氮掺杂量(质量分数6.4%~21.3%)、比表面积、孔道结构发达程度及相应的定向转化硫容,最佳工艺条件下合成样品的饱和硫容高达5.8 g H2S/(g催化剂)。

关键词: 碳材料, 煤焦油, 氮掺杂, 纳米结构, 催化, 氧化脱硫

Abstract:

Nitrogen-doped porous carbon (NPCs) were prepared by one-step co-carbonization used the anthracene oil fraction form coal taras the carbon source and dopamine as the nitrogen source, based on the induced self-activation of the nano-calcium carbonate template in the carbonization process. The results from element analyses, cryogenic nitrogen adsorption-desorption test, scanning and transmission electron microscopy characterization show that NPCs have a high level of doping nitrogen and the developed micro-mesoporous hierarchical structure. Combined with the evaluation for catalytic oxidation of hydrogen sulfide to elemental sulfur at room temperature, it is found that the doped-nitrogen amount (6.4%-21.3%,mass fraction), the specific surface area, the channel texture and the corresponding desulfurization performance of NPCs can be controlled by changing the dosage of template agent, the feeding ratio of carbon/nitrogen source and the carbonization temperature. And the saturated sulfur capacity of NPCs can be up to 5.8 g H2S/(g cat.) when synthesized under the optimal process conditions.

Key words: carbon material, coal tar, nitrogen doped, nanoscale structure, catalysis, oxidative desulfurization

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