Preparation of coal tar pitch-based porous carbon from K2CO3-KCl molten salt for CH4/N2 adsorption and separation

WANG Jiawei; ZHANG Chujie; JING Jiaxin; YANG Xu; WANG Yugao; YANG Jiangfeng

doi:10.12434/j.issn.2097-2547.20260019

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Preparation of coal tar pitch-based porous carbon from K₂CO₃-KCl molten salt for CH₄/N₂ adsorption and separation

更新时间：2026-07-21

- Preparation of coal tar pitch-based porous carbon from K₂CO₃-KCl molten salt for CH₄/N₂ adsorption and separation
- Pages: 1-10(2026)
- 作者机构：
  
  太原理工大学化学与化工学院，山西太原 030024
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20260019
  CLC： TQ028.1
- Received：12 January 2026，
  
  Revised：2026-03-04，
  
  Online First：20 July 2026，
- 稿件说明：
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王佳玮,张楚杰,景佳鑫等.K₂CO₃-KCl熔盐制备煤沥青基多孔炭用于CH₄/N₂吸附分离[J].低碳化学与化工,DOI:10.12434/j.issn.2097-2547.20260019.

WANG Jiawei,ZHANG Chujie,JING Jiaxin,et al.Preparation of coal tar pitch-based porous carbon from K₂CO₃-KCl molten salt for CH₄/N₂ adsorption and separation[J].Low-Carbon Chemistry and Chemical Engineering,DOI:10.12434/j.issn.2097-2547.20260019.
王佳玮,张楚杰,景佳鑫等.K₂CO₃-KCl熔盐制备煤沥青基多孔炭用于CH₄/N₂吸附分离[J].低碳化学与化工,DOI:10.12434/j.issn.2097-2547.20260019. DOI：

WANG Jiawei,ZHANG Chujie,JING Jiaxin,et al.Preparation of coal tar pitch-based porous carbon from K₂CO₃-KCl molten salt for CH₄/N₂ adsorption and separation[J].Low-Carbon Chemistry and Chemical Engineering,DOI:10.12434/j.issn.2097-2547.20260019. DOI：

摘要

高效分离是低浓度煤层气资源化利用的关键。为开发高性能吸附剂，以中温煤沥青（CTP）为炭前驱体，采用兼具活化、阻燃与模板功能的K

-KCl混合熔盐体系，在空气氛围下通过一步炭化工艺制备了煤沥青基多孔炭（CTP-

，

为炭化温度）。系统探究了炭化温度对CTP-

织构性质、表面化学性质及20%CH

/80%N

（以下简写为“CH

”）吸附分离性能的影响。结果表明，CTP-

富含微孔结构与含氧官能团，其中CTP-700 CH

吸附分离性能最优，其比表面积达863.04 m

/g，微孔孔隙率为96%，298 K下CH

吸附量为25.09 cm

/g，基于理想吸附溶液理论（IAST）计算的CH

吸附分离选择性为6.27。动态穿透测试和变压吸附模拟证实，CTP-700对CH

混合气具有良好分离效果，为低浓度煤层气高效利用提供了良好吸附材料与技术支撑。

Abstract

Efficient CH

separation is crucial for the resource utilization of low-concentration coalbed methane. To develop high-performance adsorbents

medium-temperature coal tar pitch (CTP) was used as the carbon precursor and a K

-KCl mixed molten salt system with activation activation

flame-retardant and template functions

was used to prepare coal tar pitch-based porous carbon (CTP-

where

represents carbonization temperatures) via a one-step carbonization process under air atmosphere. The effects of carbonization temperatures on textural properties

surface chemical properties

and 20%CH

/80%N

(abbreviated as “CH

” below) adsorption and separation performances of CTP-

were

investigated. The results show that CTP-

is rich in micropores structures and oxygen-containing functional groups. The CTP-700 shows the best CH

adsorption and separation performance with the specific surface area of 863.04 m

/g and micropore porosity of 96%. Its CH

adsorption capacity is 25.09 cm

/g at 298 K and CH

adsorption and separation selectivity calculated based on ideal adsorption solution theory (IAST) is 6.27. Dynamic breakthrough tests and pressure swing adsorption simulations confirm that CTP-700 shows a good separation effect on CH

mixed gas

providing good adsorbent materials and technical supports for efficient utilization of low-concentration coalbed methane.

关键词

Keywords

references

CHANG M , ZHAO Y J , LIU D H , et al . Methane-trapping metal-organic frameworks with an aliphatic ligand for efficient CH 4 /N 2 separation [J ] . Sustainable Energy & Fuels , 2020 , 4 : 138 - 142 .

TANG R L , DAI Q B , LIANG W W , et al . Synthesis of novel particle rice-based carbon materials and its excellent CH 4 /N 2 adsorption selectivity for methane enrichment from low-rank natural gas [J ] . Chemical Engineering Journal , 2020 , 384 : 123388 .

YANG Z X , HUSSAIN M Z , MARÍN P , et al . Enrichment of low concentration methane: An overview of ventilation air methane [J ] . Journal of Materials Chemistry A , 2022 , 10 : 6397 - 6413 .

WANG S M , SHIVANNA M , YANG Q Y . Nickel-based metal-organic frameworks for coal‐bed methane purification with record CH 4 /N 2 selectivity [J ] . Angewandte Chemie International Edition , 2022 , 61 : e202201017 .

杨江峰 , 赵强 , 于秋红 , 等 . 煤层气回收及CH 4 /N 2 分离PSA材料的研究进展 [J ] . 化工进展 , 2011 , 30 ( 4 ): 793 - 801 .

YANG J F , ZHAO Q , YU Q H , et al . Progress of recovery of coal bed methane and adsorption materials for separation of CH 4 /N 2 by pressure swing adsorption [J ] . Chemical Industry and Engineering Progress , 2011 , 30 ( 4 ): 793 - 801 .

WEI M N , TANG X , WANG Y T , et al . Significant improvement in CH 4 /N 2 selectivity achieved through ammonium exchange in mordenite [J ] . Separation and Purification Technology , 2024 , 340 : 126799 .

YANG J F , BAI H H , SHANG H , et al . Experimental and simulation study on efficient CH 4 /N 2 separation by pressure swing adsorption on silicalite-1 pellets [J ] . Chemical Engineering Journal , 2020 , 388 : 124222 .

SUN W N , SHEN Y H , ZHANG D H , et al . A systematic simulation and proposed optimization of the pressure swing adsorption process for CH 4 /N 2 separation under external disturbances [J ] . Industrial & Engineering Chemistry Research , 2015 , 54 ( 30 ): 7489 - 7501 .

SANTOS K M C , MENEZES T R , OLIVEIRA M R , et al . Natural gas dehydration by adsorption using MOFs and silicas: A review [J ] . Separation and Purification Technology , 2021 , 276 : 119409 .

HEDLUND J , GARCIA G , BALSAMO M . Microchannel zeolite 13X adsorbent with high CO 2 separation performance [J ] . Separation and Purification Technology , 2021 , 277 : 119483 .

LI Y , WANG Y T , LI X M , et al . Grafting of functional organic ligand on zeolite Y for efficient CH 4 /N 2 separation [J ] . Separation and Purification Technology , 2025 , 354 : 128719 .

WANG L , LI Y , WANG Y , et al . Research on CO 2 -N 2 O separation using flexible metal organic frameworks [J ] . Separation and Purification Technology , 2020 , 251 : 117311 .

ZHANG F F , TANG Y H , ZHAO Z W , et al . Construction of a novel nickel-based MOF with accessible oxygen sites for efficient CH 4 /N 2 separation [J ] . Inorganic Chemistry Frontiers , 2024 , 11 : 3889 - 3896 .

马蕾 , 张飞飞 , 宋志强 , 等 . 金属有机骨架材料用于吸附分离CH 4 和N 2 的研究进展 [J ] . 化工进展 , 2021 , 40 ( 9 ): 5107 - 5117 .

MA L , ZHANG F F , SONG Z Q , et al . Development of metal-organic frameworks in adsorptive separation of CH 4 -N 2 [J ] . Chemical Industry and Engineering Progress , 2021 , 40 ( 9 ): 5107 - 5117 .

PARK D , JU Y , KIM J H , et al . Equilibrium and kinetics of nitrous oxide, oxygen and nitrogen adsorption on activated carbon and carbon molecular sieve [J ] . Separation and Purification Technology , 2019 , 223 : 63 - 80 .

WANG Q , YU Y X , LI Y H , et al . Methane separation and capture from nitrogen rich gases by selective adsorption in microporous materials: A review [J ] . Separation and Purification Technology , 2022 , 283 : 120206 .

孟宇 , 朱仕元 , 彭娜 , 等 . 煤沥青基多孔碳材料研究进展 [J ] . 化工科技， 2020 , 28 ( 4 ): 73 - 76 .

MENG Y , ZHU S Y , PENG N , et al . Research progress and prospect of coal asphaltene-based porous carbon materials [J ] . Chemical Science and Technology , 2020 , 28 ( 4 ): 73 - 76 .

AMIN M N , HABIBI M Z , SAEED S . Preparation and optimization of activated nano-carbon production using physical activation by water steam from agricultural wastes [J ] . RSC Advances , 2020 , 10 ( 3 ): 1463 - 1475 .

CARROTT P , CARROTT R M , MOURÃO P , et al . Preparation of activated carbons from cork by physical activation in carbon dioxide [J ] . Adsorption Science & Technology , 2003 , 21 ( 7 ): 669 - 681 .

辛冉冉 , 缪杭锦 , 姜伟 , 等 . 氮掺杂高比表面多孔碳的一步化学活化法制备及其超电容性能 [J ] . 无机化学学报 , 2019 , 35 ( 10 ): 1781 - 1790 .

XIN R R , MIAO H J , JIANG W , et al . N-doped porous carbons with high surface areas prepared through one-step chemical activation and their application for supercapacitors [J ] . Chinese Journal of Inorganic Chemistry , 2019 , 35 ( 10 ): 1781 - 1790 .

刘慧文 . 水热炭化法制备生物质基活性炭及其CH 4 /N 2 吸附分离性能研究 [D ] . 太原 : 太原理工大学 , 2021 .

LIU H W . Preparation of bi omass based activated carbons byhydrothermal carbonization and its adsorption andseparation performance of CH 4 /N 2 [D ] . Taiyuan : Taiyuan University of Technology , 2021 .

戴琼斌 , 刘宏斌 , 夏启斌 , 等 . 一种新的颗粒炭材料的制备及其高效分离甲烷氮气性能 [J ] . 化工学报 , 2021 , 72 ( 8 ): 4196 - 4203 .

DAI Q B , LIU H B , XIA Q B , et al . Preparation of new granular carbon material and its efficient separation of methane and nitrogen [J ] . CIESC Journal , 2021 , 72 ( 8 ): 4196 - 4203 .

LI H P , SONG X Y , WANG X J , et al . One-step construction of hierarchically porous carbon nanorods with extraordinary capacitive behavior [J ] . Carbon , 2020 , 160 : 176 - 187 .

GAO S , GE L , RUFFORD T E , et al . The preparation of activated carbon discs from tar pitch and coal powder for adsorption of CO 2 , CH 4 and N 2 [J ] . Microporous and Mesoporous Materials , 2017 , 238 : 19 - 26 .

DÍEZ N , FUERTES A B , SEVILLA M . Molten salt strategies towards carbon materials for energy storage and conversion [J ] . Energy Storage Materials , 2021 , 38 : 50 - 69 .

宋瑞珍 , 陈云霄 , 杨晓阳 , 等 . K 2 CO 3 活化低阶煤和污泥共水热炭制备多孔炭及其对CO 2 和SO 2 吸附性能 [J ] . 洁净煤技术 , 2024 , 30 ( 7 ): 47 - 59 .

SONG R Z , CHEN Y X , YANG X Y , et al . Preparation of porous carbon by co-hydrothermal carbonization of low-rank coal and sludge activated with K 2 CO 3 and its adsorption performance for CO 2 and SO 2 [J ] . Clean Coal Technology , 2024 , 30 ( 7 ): 47 - 59 .

CHENG Z , LIU X H , DIAO R , et al . Structural regulation of ultra-microporous biomass-derived carbon materials induced by molten salt synergistic activation and its application in CO 2 capture [J ] . Chemical Engineering Journal , 2024 , 486 : 150227 .

BANDANI M , NAJAFI M , KHALILI S , et al . Preparation and characterization of low-cost chemically activated carbons using H 3 PO 4 , ZnCl 2 and KOH for CO 2 adsorption applications [J ] . Scientific Reports , 2026 , 16 : 6288 .

ZHANG Y , XU X , GENG Q , et al . Redefining the roles of alkali activators for porous carbon [J ] . Chemical Science , 2024 , 16 : 2034 - 2043 .

LIU Q , WANG T , JIA D Z , et al . A refined stepwise carbonation strategy for controllable synthesis of porous carbon for high-performance zinc-ion hybrid capacitors [J ] . Advanced Functional Materials , 2025 , 35 : 2500016 .

REN P X , WU D L , WANG T , et al . K 2 CO 3 -KCl acts as a molten salt flame retardant to prepare N and O doped honeycomb-like carbon in air for supercapacitors [J ] . Journal of Power Sources , 2022 , 532 : 231072 .

TU S , YU L , LIN D X , et al . Robust nickel-based metal-organic framework for highly efficient methane purification and capture [J ] . ACS Applied Materials & Interfaces , 2022 , 14 ( 3 ): 3444 - 3452 .

HE W T , MA R G , ZHU Y F , et al . Study on the preparation of renewable porous carbon activated by potassium hydroxide and its electrocatalytic performance for oxygen reduction reaction [J ] . Journal of Inorganic Materials , 2019 , 34 ( 10 ): 1115 - 1122 .

DONG Z , LI B , SHANG H , et al . Ultra microporous carbon granules with narrow pore size distribution for efficient CH 4 separation from coal-bed gases [J ] . AIChE Journal , 2021 , 67 ( 9 ): e17281 .

夏笑虹 . 酚醛树脂基多孔炭材料的可控制备与电容性能研究 [D ] . 长沙 : 湖南大学 , 2012 .

XIA X H . Controllable preparation and electrochemical performance ofphenolic resin based porous carbon for electric double layercapacitors [D ] . Changsha : Hunan University , 2012 .

JAGTOYEN M , DERBYSHIRE F . Activated carbons from yellow poplar and white oak by H 3 PO 4 activation [J ] . Carbon , 1998 , 36 ( 7/8 ): 1085 - 1097 .

LIU F , ZHANG Y , ZHANG P X , et al . Facile preparation of N and O-rich porous carbon from palm sheath for highly selective separation of CO 2 /CH 4 /N 2 gas-mixture [J ] . Chemical Engineering Journal , 2020 , 399 : 125812 .

SHI M , XIN Y F , CHEN X X , et al . Coal-derived porous activated carbon with ultrahigh specific surface area and excellent electrochemical performance for supercapacitors [J ] . Journal of Alloys and Compounds , 2020 , 847 : 157856 .

ZHONG D L , WANG W C , ZOU Z L , et al . Investigation on methane recovery from lo w-concentration coal mine gas by tetra- n -butyl ammonium chloride semiclathrate hydrate formation [J ] . Applied Energy , 2017 , 227 : 686 - 693 .

FERRARI C A . Raman spectroscopy of graphene and graphite: Disorder, electron-phonon coupling, doping and nonadiabatic effects [J ] . Solid State Communications , 2007 , 143 ( 1/2 ): 47 - 57 .

ARAMI-NIYA A , RUFFORD T E , ZHU Z . Activated carbon monoliths with hierarchical pore structure from tar pitch and coal powder for the adsorption of CO 2 , CH 4 and N 2 [J ] . Carbon , 2016 , 103 : 115 - 124 .

LI S H , FU S G , GONG Y Q , et al . New insight into efficient CH 4 /N 2 separation based on Ni-decorated porous carbon functional composites [J ] . Fuel , 2023 , 347 : 128480 .

LI Y , XU R , WANG B B , et al . Enhanced N-doped porous carbon derived from KOH-activated waste wool: A promising material for selective adsorption of CO 2 /CH 4 and CH 4 /N 2 [J ] . Nanomaterials , 2019 , 9 ( 2 ): 266 .

ZHANG Y , LIU L , ZHANG P X , et al . Ultra-high surface area and nitrogen-rich porous carbons prepared by a low-temperature activation method with superior gas selective adsorption and outstanding supercapacitance performance [J ] . Chemical Engineering Journal , 2019 , 355 : 309 - 319 .

YI H H , LI F R , NING P , et al . Adsorption separation of CO 2 , CH 4 , and N 2 on microwave activated carbon [J ] . Chemical Engineering Journal , 2013 , 215/216 : 635 - 642 .

YANG X , LI Z Y , ZHANG C Z , et al . Practical separation performance evaluation of coal mine methane upgrading with carbon molecular sieves [J ] . Chemical Engineering Journal , 2019 , 367 : 295 - 303 .

LI T Y , WANG Y S , ZHANG M Y , et al . Carbon nanofibers with gas selective layer containing rich and accessible ultramicropores for methane/nitrogen separation [J ] . Chemical Engineering Journal , 2023 , 462 : 142118 .

RUFFORD T E , WATSON G C Y , SALEMAN T L , et al . Adsorption equilibria and kinetics of methane + nitrogen mixtures on the activated carbon Norit RB3 [J ] . Industrial & Engineering Chemistry Research , 2013 , 52 ( 41 ): 14270 - 14281 .

MUJMULE R B , RAJPURE M M , KIM U , et al . Tailored microporous graphitic carbon adsorbents from the urea-assisted method for efficient selective gas adsorption and separation of CH 4 /N 2 and CH 4 /H 2 [J ] . Separation and Purification Technology , 2025 , 358 : 130249 .

GUO Y , HU J L , LIU X W , et al . Scalable solvent-free preparation of [Ni 3 (HCOO) 6 ] frameworks for highly efficient separation of CH 4 from N 2 [J ] . Chemical Engineering Journal , 2017 , 327 : 564 - 572 .

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