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过程工程学报 ›› 2024, Vol. 24 ›› Issue (12): 1425-1434.DOI: 10.12034/j.issn.1009-606X.224094CSTR: 32067.14.jproeng.224094

• 研究论文 • 上一篇    下一篇

含硫烟气对MFM-136捕集CO2的影响及烟气组分共吸附机理研究

许丽1,2,3， 耿娜3， 刘文1,2,3， 田京雷4， 朱廷钰3， 姚明水3*， 郭旸旸3*   

  1. 1. 中国科学技术大学稀土学院，安徽 合肥 230026 2. 中国科学院赣江创新研究院，江西 赣州 341000 3. 中国科学院过程工程研究所，介科学与工程全国重点实验室，中国科学院绿色过程与工程重点实验室，北京 100190 4. 河钢集团有限公司，河北 石家庄 050023
  • 收稿日期:2024-03-13 修回日期:2024-04-30 出版日期:2024-12-28 发布日期:2024-12-27
  • 通讯作者: 郭旸旸 yyguo@ipe.ac.cn
  • 基金资助:
    国家自然科学基金;国家自然科学基金;中国科学院青年创新促进会;全国重点实验室科研基金;全国重点实验室科研基金

Effect of sulfur-containing flue gas on CO2 capture of MFM-136 and co-adsorption mechanism of flue gas components

Li XU1,2,3,  Na GENG3,  Wen LIU1,2,3,  Jinglei TIAN4,  Tingyu ZHU3,  Mingshui YAO3*,  #br# Yangyang GUO3*   

  1. 1. School of Rare Earths, University of Science and Technology of China, Hefei, Anhui 230026, China 2. Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou, Jiangxi 341000, China 3. Key Laboratory of Green Process and Engineering, State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China 4. HBIS Group Co., Ltd., Shijiazhuang, Hebei 050023, China
  • Received:2024-03-13 Revised:2024-04-30 Online:2024-12-28 Published:2024-12-27

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摘要： 在全球向可持续低碳经济过渡的过程中，实现吸附剂高吸附容量和长久稳定性之间的平衡至关重要。本研究以具有Kagome构型的MFM-136为研究对象。采用XRD, BET, FT-IR, TG和SEM分析了MFM-136的结构和性质，考察了MFM-136的CO2吸附性能，进一步通过CO2穿透实验和原位红外光谱(in situ DRIFTS)实验明确了杂质气体与CO2之间的竞争吸附关系，揭示了烟气组分在MFM-136表面的共吸附机理。吸附实验结果表明，MFM-136在298 K下的CO2和H2O吸附容量分别为3.0和11.94 mmol/g，MFM-136的微孔(0.59 nm)及其骨架中的多重吸附位点使其可以在室温下选择性吸附CO2，298 K下CO2/N2吸附选择性达24，气体的等量吸附热达23 kJ/mol，在120℃脱气30 min即可实现吸附能力的完全再生。穿透实验和in situ DRIFTS实验表明，O2的存在促进了CO2的化学吸附。SO2在吸附剂上主要发生化学吸附，形成硫酸盐和亚硫酸盐。含氧条件下NO与O2反应生成NO2，与吸附剂之间形成强烈的化学吸附，生成硝酸盐和亚硝酸盐物种。水蒸气的存在不仅促进了CO2的化学吸附和碳酸氢盐的产生，同时也促进了CO2与SO2, NO之间的竞争吸附。

关键词: 金属有机框架材料, CO2捕获, 杂质气体影响, 原位红外光谱, 竞争吸附

Abstract: In the global transition towards a sustainable low-carbon economy, achieving a balance between high adsorption capacity and long-term stability of the adsorbent is crucial. In this study, MFM-136 with Kagome configuration was selected as the research object. The structure of MFM-136 was analyzed by XRD, BET, FT-IR, TG and SEM. The CO2 adsorption performance of MFM-136 was investigated by a series of gas adsorption experiments. The competitive adsorption relationship between impurity gas and CO2 was further identified by CO2 breakthrough experiment and in situ DRIFTS experiment, and revealed the co-adsorption mechanism of impurity gas and CO2 on MFM-136 surface. The adsorption experiment results showed that the adsorption capacity of MFM-136 for CO2 and H2O at 298 K was 3.0 and 11.94 mmol/g, respectively. The micro pore size (0.59 nm) of MFM-136 and the multiple adsorption sites in its skeleton enabled MFM-136 to selectively adsorption CO2 at room temperature. The adsorption selectivity of CO2/N2 reached 24 at 298 K, the Qst reached 23 kJ/mol, and the adsorption capacity was completely regenerated after degassing at 120℃ for 30 min. The results of breakthrough experiment and in situ DRIFTS experiment showed that the O2 promoted the chemisorption of CO2. The chemisorption of SO2 mainly occurs on the surface of the adsorbent to form sulfate and sulfite. Under O2-containing conditions, NO will react with O2 to form NO2, which will generate strong chemisorption on the surface of the adsorbent and generate corresponding nitrate and nitrite species. The water vapor not only promotes the chemical adsorption of CO2 and the production of bicarbonate, but also promotes the competitive adsorption between CO2 and SO2, NO.

Key words: metal organic frameworks, CO2 capture, impurity gas influence, in situ DRIFTS experiment, competitive adsorption