基于煤层气甲烷富集的固体多孔材料研究进展

doi:10.16085/j.issn.1000-6613.2023-1763

化工进展 ›› 2024, Vol. 43 ›› Issue (11): 6215-6232.DOI: 10.16085/j.issn.1000-6613.2023-1763

• 材料科学与技术 • 上一篇

基于煤层气甲烷富集的固体多孔材料研究进展

程春晖¹(), 明淑君², 庞磊³, 田士东⁴, 李克伦⁴, 李涛¹()

^1.华中科技大学化学与化工学院，能量转换与存储材料化学教育部重点实验室，材料化学与服役失效湖北省重点实验室，湖北武汉 430074
^2.黄冈师范学院化学化工学院，湖北黄冈 438000
^3.东风商用车有限公司技术中心，湖北武汉 430056
^4.陕西煤业化工技术研究院有限责任公司，陕西西安 710100

收稿日期:2023-10-09 修回日期:2023-12-18 出版日期:2024-11-15 发布日期:2024-12-07
通讯作者: 李涛
作者简介:程春晖（1995—），男，博士研究生，研究方向为固体多孔吸附剂材料的合成与改性。E-mail：chunhuicheng@hust.edu.cn。
基金资助:
国家重点研发计划(2020YFB1711200)

Developments in solid porous materials for methane enrichment in coalbed gas

CHENG Chunhui¹(), MING Shujun², PANG Lei³, TIAN Shidong⁴, LI Kelun⁴, LI Tao¹()

^1.School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, MOE Key Laboratory of Material Chemistry for Energy Conversion and Storage, Hubei Key Laboratory of Material Chemistry and Service Failure, Wuhan 430074, Hubei, China
^2.School of Chemistry and Chemical Engineering, Huanggang Normal University, Huanggang 438000, Hubei, China
^3.Technical Center, Dongfeng Commercial Vehicle Co. , Ltd. , Wuhan 430056, Hubei, China
Shaanxi Coal Chemical Industry Technology Research Institute Co. , Ltd. , Xi’an 710100, Shaanxi, China

Received:2023-10-09 Revised:2023-12-18 Online:2024-11-15 Published:2024-12-07
Contact: LI Tao

摘要/Abstract

摘要：

煤层气（CMM）中的甲烷不仅是一种重要的绿色可持续的低碳清洁能源，亦是一种令人担忧的爆炸和温室气体污染物。因此寻找一种稳定且高效的甲烷富集技术，对于增加目前煤炭开采业的安全系数及克服常规天然气短缺问题具有重要意义。然而煤层气中存在大量杂质已成为其工业化大规模利用的关键技术障碍，尤其是对二氧化碳和氮气污染物的高效分离。本文综述了在煤层气甲烷富集真空变压吸附工艺（VPSA）过程中的两个主要方向：二氧化碳捕集（CO₂/CH₄分离）和天然气净化（CH₄/N₂分离），其中制备高效分离甲烷气体混合物的固体吸附剂是VPSA技术的核心突破点。进而重点分析和比较了碳基吸附材料、沸石分子筛和金属有机骨架这三种典型的固体吸附剂在上述两个方向上分离或吸附甲烷的差异性与相似性，其中在吸附剂表面耦合不同功能的官能团或在纳米尺度上微调其孔隙结构将是不断提高煤层气甲烷富集吸附分离效率的有效途径。此外还讨论了固体多孔材料未来发展面临的挑战和发展方向，希望在帮助研究人员了解CMM甲烷富集吸附剂的技术前提下，理解并设计出新型吸附剂以期满足工业上多重苛刻的甲烷分离要求。

关键词: 煤层气, 甲烷富集, 固体吸附剂, 二氧化碳捕集, 天然气净化

Abstract:

Methane in coal mine methane (CMM) serves not merely as a pivotal and sustainable low-carbon energy source, but equally as a disconcerting explosive and greenhouse gas pollutant. Finding a consistent, efficient technique for methane enrichment is of paramount importance in enhancing safety measures within the current coal mining industry and addressing natural gas shortages. Industrial scale application has, however, been impeded by significant impurities present in coal-bed methane, specifically the efficient separation of carbon dioxide and nitrogen contaminants. This paper aimed to encapsulate two major focus areas in the process of coal-bed methane enrichment via vacuum pressure swing adsorption (VPSA): carbon dioxide capture (CO₂/CH₄ separation) and purification of natural gas (CH₄/N₂ separation). Here, effective adsorbents for segregating methane gas mixtures denoted the crux of VPSA technology advancements. Furthermore, it was further focused on analyzing and comparing the differences and similarities of three typical solid adsorbents, namely carbon-based adsorbents, zeolite molecular sieves and metal-organic frameworks, in separating or adsorbing methane in the above two directions. Among them, coupling different functional groups on the adsorbent surface or fine-tuning their pore structure at the nanoscale would be an effective way to continuously improve the adsorption separation efficiency of coalbed methane enrichment. In addition, the challenges and development directions faced by solid porous materials in the future were also discussed, hoping to help researchers understand the technical premise of CMM methane enrichment adsorbents and design novel adsorbents to meet the multiple stringent industrial requirements for methane separation.

Key words: coal mine methane, methane enrichment, solid adsorbents, carbon dioxide capture, natural gas purification

中图分类号:

O647.3

程春晖, 明淑君, 庞磊, 田士东, 李克伦, 李涛. 基于煤层气甲烷富集的固体多孔材料研究进展[J]. 化工进展, 2024, 43(11): 6215-6232.

CHENG Chunhui, MING Shujun, PANG Lei, TIAN Shidong, LI Kelun, LI Tao. Developments in solid porous materials for methane enrichment in coalbed gas[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6215-6232.

图/表 17

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技术	变压吸附分离	低温深冷分离	膜分离	水合物基分离
机理	吸附选择性	沸点不同	渗透率差异	甲烷水合物结晶
相变	无	有	无	有
压力	PSA需要高压；VPSA仅需常压	高压	高压	高压
优点	高安全性、长寿命、高操作灵活性、低能耗	富集性能好	操作灵活性高、能耗低	富集性能好
缺点	一次操作的富集性能有限	能耗高、工艺复杂、爆炸风险高	选择性低、膜寿命短	能耗高、水合物形成速率低、爆炸风险大
发展现状	商业化应用	局部试验阶段	实验室开发阶段	实验室开发阶段
潜在问题	低产出投入比	高成本和爆炸风险	放大问题、膜耐久性	放大问题、技术不成熟

技术	变压吸附分离	低温深冷分离	膜分离	水合物基分离
机理	吸附选择性	沸点不同	渗透率差异	甲烷水合物结晶
相变	无	有	无	有
压力	PSA需要高压；VPSA仅需常压	高压	高压	高压
优点	高安全性、长寿命、高操作灵活性、低能耗	富集性能好	操作灵活性高、能耗低	富集性能好
缺点	一次操作的富集性能有限	能耗高、工艺复杂、爆炸风险高	选择性低、膜寿命短	能耗高、水合物形成速率低、爆炸风险大
发展现状	商业化应用	局部试验阶段	实验室开发阶段	实验室开发阶段
潜在问题	低产出投入比	高成本和爆炸风险	放大问题、膜耐久性	放大问题、技术不成熟

吸附剂类型	优点	缺点
活性炭	成本低廉、比表面积大、易于修饰	孔隙分布杂乱、选择性低、机械稳定性差
沸石分子筛	良好的热和机械稳定性、高的表面积	再生能耗高、对水敏感
有机聚合物	可定制化孔隙结构和化学性质	热和机械稳定性差、合成复杂、再生性弱
金属有机框架	极高的表面积、可定制化孔隙结构和化学性质	制造成本高、对水敏感、热和机械稳定性差
二氧化硅	良好的热稳定性和机械强度	吸附量和选择性低
碳纳米管	高表面积、可调节的化学性质和孔结构	制造成本高、分散性和加工性能需优化

吸附剂类型	优点	缺点
活性炭	成本低廉、比表面积大、易于修饰	孔隙分布杂乱、选择性低、机械稳定性差
沸石分子筛	良好的热和机械稳定性、高的表面积	再生能耗高、对水敏感
有机聚合物	可定制化孔隙结构和化学性质	热和机械稳定性差、合成复杂、再生性弱
金属有机框架	极高的表面积、可定制化孔隙结构和化学性质	制造成本高、对水敏感、热和机械稳定性差
二氧化硅	良好的热稳定性和机械强度	吸附量和选择性低
碳纳米管	高表面积、可调节的化学性质和孔结构	制造成本高、分散性和加工性能需优化

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基于煤层气甲烷富集的固体多孔材料研究进展

Developments in solid porous materials for methane enrichment in coalbed gas

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