煤基富氮层级多孔碳制备及其催化脱硫性能

孙明慧; 陈静圆; 肖南; 陈奥博; 王旭珍; 邱介山

doi:10.11949/0438-1157.20190998

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煤基富氮层级多孔碳制备及其催化脱硫性能

催化、动力学与反应器 | 更新时间：2026-07-24

- 煤基富氮层级多孔碳制备及其催化脱硫性能
- Preparation of hierarchical nitrogen-rich porous carbon from coal tar for catalytic desulfurization
- 化工学报 2020年71卷第2期页码：660-668
- 作者机构：
  
  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
- 作者简介：
  
  孙明慧（1993—），女，硕士研究生，smh1105@mail.dlut.edu.cn
  王旭珍（1968—），女，博士，教授，xzwang@dlut.edu.cn
  邱介山（1964—），男，博士，教授，jqiu@dlut.edu.cn
- 基金信息：
  
  国家自然科学基金项目(U1610105)
- DOI：10.11949/0438-1157.20190998
  中图分类号： TQ 127.1
- 收稿：2019-09-03，
  
  修回：2019-11-08，
  
  网络首发：2020-08-14，
  
  纸质出版：2020-02-05
- 稿件说明：
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孙明慧, 陈静圆, 肖南, 陈奥博, 王旭珍, 邱介山. 煤基富氮层级多孔碳制备及其催化脱硫性能[J]. 化工学报, 2020, 71(2): 660-668

SUN Minghui, CHEN Jingyuan, XIAO Nan, CHEN Aobo, WANG Xuzhen, QIU Jieshan. Preparation of hierarchical nitrogen-rich porous carbon from coal tar for catalytic desulfurization[J]. CIESC Journal, 2020, 71(2): 660-668
孙明慧, 陈静圆, 肖南, 陈奥博, 王旭珍, 邱介山. 煤基富氮层级多孔碳制备及其催化脱硫性能[J]. 化工学报, 2020, 71(2): 660-668 DOI： 10.11949/0438-1157.20190998.

SUN Minghui, CHEN Jingyuan, XIAO Nan, CHEN Aobo, WANG Xuzhen, QIU Jieshan. Preparation of hierarchical nitrogen-rich porous carbon from coal tar for catalytic desulfurization[J]. CIESC Journal, 2020, 71(2): 660-668 DOI： 10.11949/0438-1157.20190998.

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 H

S/(g催化剂)。

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 H

S/(g cat.) when synthesized under the optimal process conditions.

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references

Sun F G , Liu J , Chen H C , et al . Nitrogen-rich mesoporous carbons: highly efficient, regenerable metal-free catalysts for low-temperature oxidation of H 2 S [J ] . ACS Catal ., 2013 , 3 : 862 - 870 .

Adib F , Bagreev A , Bandosz T J . Analysis of the relationship between H 2 S removal capacity and surface properties of unimpregnated activated carbons [J ] . Environ. Sci. Technol ., 2000 , 34 : 686 - 692 .

Yuan W X , Bandosz T J . Removal of hydrogen sulfide from biogas on sludge-derived adsorbents [J ] . Fuel , 2007 , 86 : 2736 - 2746 .

Bandosz T J , Bagreev A , Adib F , et al . Unmodified versus caustics-impregnated carbons for control of hydrogen sulfide emissions from sewage treatment plants [J ] . Environ. Sci. Technol ., 2000 , 34 : 1069 - 1074 .

Long D H , Chen Q J , Qiao W M , et al . Three-dimension al mesoporous carbon aerogels: ideal catalyst supports for enhanced H 2 S oxidation [J ] . Chem. Commun ., 2009 , 26 : 3898 - 3900 .

Yu Z F , Wang X Z , Song X D , et al . Molten salt synthesis of nitrogen-doped porous carbons for hydrogen sulfide adsorptive removal [J ] . Carbon , 2015 , 95 : 852 - 860 .

Seredych M , Bandosz T J . Desulfurization of digester gas on wood-based activated carbons modified with nitrogen: importance of surface chemistry [J ] . Energy & Fuels , 2008 , 22 : 850 - 859 .

Seredych M , Bandosz T J . Role of microporosity and nitrogen functionality on the surface of activated carbon in the process of desulfurization of digester gas [J ] . J . Phys. Chem. C ., 2008 , 112 : 4704 - 4711 .

Xing W , Liu C , Zhou Z Y , et al . Superior CO 2 uptake of N-doped activated carbon through hydrogen-bonding interaction [J ] . Energy Environ . Sci ., 2012 , 5 : 7323 - 7327 .

Bing X F , Wei Y J , Wang M , et al . Template-free synthesis of nitrogen-doped hierarchical porous carbons for CO 2 adsorption and supercapacitor electrodes [J ] . J. Colloid Inter. Sci ., 2017 , 488 : 207 - 217 .

Shen W Z , Fan W B . Nitrogen-containing porous carbons: synthesis and application [J ] . J. Mater. Chem ., 2013 , 1 : 999 - 1013 .

Machnikowski J , Grzyb B , Machnikowska H , et al . Surface chemistry of porous carbons from N-polymers and their blends with pitch [J ] . Micropor. Mesopor. Mater ., 2005 , 82 : 113 - 120 .

Guo H S , Ding B , Wang J , et al . Template-induced self-activation route for nitrogen-doped hierarchically porous carbon spheres for electric double layer capacitors [J ] . Carbon , 2018 , 136 : 204 - 210 .

Gu Y , Wu H , Xiong Z G , et al . The electrocapacitive properties of hierarchical porous reduced graphene oxide templated by hydrophobic CaCO 3 spheres [J ] . J. Mater. Chem. A , 2014 , 2 : 451 - 459 .

Kim Y K , Park J H , Lee J W . Facile nano-templated CO 2 conversion into highly interconnected hierarchical porous carbon for high-performance supercapacitor electrodes [J ] . Carbon , 2018 , 126 : 215 - 224 .

Li S , Jiang T , Xu Z H , et al . The Mn-promoted double-shelled CaCO 3 hollow microspheres as high efficient CO 2 adsorbents [J ] . Chem. Eng. J ., 2019 , 372 : 53 - 64 .

徐春霞 . 煤焦油的性质与加工利用 [J ] . 洁净煤技术 , 2013 , 5 : 63 - 67 .

Xu C X . Properties, processing and utilization of coal tar [J ] . Clean Coal Technology , 2013 , 5 : 63 - 67 .

史晓斐 , 杨思宇 , 钱宇 . 化学链技术在煤炭清洁高效利用中的研究进展 [J ] . 化工学报 , 2018 , 69 ( 12 ): 4931 - 4946 .

Shi X F , Yang S Y , Qian Y . Research progress of chemical chain technology in clean and efficient utilization of coal [J ] . CIESC Journal , 2018 , 69 ( 12 ): 4931 - 4946 .

程炎 , 颜彬航 , 李天阳 , 等 . 煤/煤焦油/沥青质的热等离子体裂解特性比较分析 [J ] . 化工学报 , 2015 , 66 ( 8 ): 3210 - 3217 .

Cheng Y , Yan B H , Li T Y , et al . Comparative analysis of thermal plasma cracking characteristics of coal/coal tar/asphaltene [J ] . CIESC Journal , 2015 , 66 ( 8 ): 3210 - 3217 .

Cui M J , Ren S M , Zhao H C , et al . Polydopamine coated graphene oxide for anticorrosive reinforcement of water-borne epoxy coating [J ] . Chem. Eng. J ., 2018 , 335 : 255 - 266 .

Jiang H , Ren D Y , Hu H F , et al . 2D Monolayer MoS 2 -carbon interoverlapped superstructure: engineering ideal atomic interface for lithium ion storage [J ] . Adv. Mater ., 2015 , 27 : 3687 - 3695 .

Wang J , Tang J , Xu Y , et al . Interface miscibility induced double-capillary carbon nanofibers for flexible electric double layer capacitors [J ] . Nano Energy , 2016 , 28 : 232 - 240 .

Lin T , Chen I W , Liu F , Y et al . Nitrogen-doped mesoporous carbon of extraordinary capacitance for electrochemical energy storage [J ] . Science , 2015 , 350 ( 6267 ): 1508 - 1513 .

Guang P H , Wen C L , Dan Q , et al . Rapid synthesis of nitrogen-doped porous carbon monolith for CO 2 capture [J ] . Adv. Mater ., 2010 , 22 : 853 - 857 .

Shen F H , Liu J , Zhang Z , et al . Density functional study of hydrogen sulfide adsorption mechanism on activated carbon [J ] . Fuel Process . Technol ., 2018 , 171 : 258 - 264 .

Mochizuki T , Kubota M , Matsuda H , et al . Adsorption behaviors of ammonia and hydrogen sulfide on activated carbon prepared from petroleum coke by KOH chemical activation [J ] . Fuel Process . Technol ., 2016 , 144 : 164 - 169 .

Ozekmekci M , Salkic G , Fellah M F . Use of zeolites for the removal of H 2 S: a mini-review [J ] . Fuel Process . Technol ., 2015 , 139 : 49 - 60 .

Liu H , Jia M , Sun N , et al . Nitrogen-rich mesoporous carbon as anode material for high-performance sodium-ion batteries [J ] . ACS Appl . Mater . Interfaces , 2015 , 7 ( 49 ): 27124 - 27130 .

Zhao C , Wang W , Yu Z , et al . Nano-CaCO 3 as template for preparation of disordered large mesoporous carbon with hierarchical porosities [J ] . J. Mater. Chem ., 2010 , 20 ( 5 ): 976 - 980 .

Yu C , Fan X M , Yu L M , et al . Adsorptive removal of thiophenic compounds from oils by activated carbon modified with concentrated nitric acid [J ] . Energy & Fuels , 2013 , 27 : 1499 - 1505 .

Zhang Z , Wang J , Li W , et al . Millimeter-sized mesoporous carbon spheres for highly efficient catalytic oxidation of hydrogen sulfide at room temperature [J ] . Carbon , 2016 , 96 : 608 - 615 .

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