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混合胺溶液耦合CaO吸收-矿化CO2特性及矿化过程关键影响因素研究

王中辉 苏胜 马智伟 宋亚伟 陈逸峰 刘涛 江龙 汪一 胡松 向军

王中辉, 苏胜, 马智伟, 宋亚伟, 陈逸峰, 刘涛, 江龙, 汪一, 胡松, 向军. 混合胺溶液耦合CaO吸收-矿化CO2特性及矿化过程关键影响因素研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60020-3
引用本文: 王中辉, 苏胜, 马智伟, 宋亚伟, 陈逸峰, 刘涛, 江龙, 汪一, 胡松, 向军. 混合胺溶液耦合CaO吸收-矿化CO2特性及矿化过程关键影响因素研究[J]. 燃料化学学报. doi: 10.1016/S1872-5813(22)60020-3
WANG Zhong-hui, SU Sheng, MA Zhi-wei, SONG Ya-wei, CHEN Yi-feng, LIU Tao, JIANG Long, WANG Yi, HU Song, XIANG Jun. Study on CO2 absorption-mineralization characteristics of mixed amine solution coupled with CaO and key influencing factors of mineralization process[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60020-3
Citation: WANG Zhong-hui, SU Sheng, MA Zhi-wei, SONG Ya-wei, CHEN Yi-feng, LIU Tao, JIANG Long, WANG Yi, HU Song, XIANG Jun. Study on CO2 absorption-mineralization characteristics of mixed amine solution coupled with CaO and key influencing factors of mineralization process[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(22)60020-3

混合胺溶液耦合CaO吸收-矿化CO2特性及矿化过程关键影响因素研究

doi: 10.1016/S1872-5813(22)60020-3
基金项目: 国家自然科学基金(U20A20302)资助
详细信息
    通讯作者:

    Tel: 13317181417, E-mail: susheng@mail.hust.edu.cn

  • 中图分类号: TQ127.1+3

Study on CO2 absorption-mineralization characteristics of mixed amine solution coupled with CaO and key influencing factors of mineralization process

Funds: The project was supported by National Natural Science Foundation of China(U20A20302).
  • 摘要: 有机胺捕集CO2是一种有效的燃烧后碳捕集(PCC)技术,同时CO2矿物碳酸化是一种安全和稳定封存CO2的方法。本研究通过将两种方式结合,以MEA/MDEA混合胺溶液作为CO2吸收剂,以CaO作为CO2矿化原料,研究了不同混合胺溶液配比、温度、反应时间和CaO添加比例等条件下混合胺溶液耦合CaO吸收-矿化CO2性能。结果表明,在常温常压下CaO可对MEA/MDEA溶液中吸收的CO2进行有效矿化并同时实现MEA/MDEA溶液的再生;并且经过五次循环吸收-矿化实验后,MEA/MDEA溶液仍保持了较高的CO2转化率(77.4%)和CO2循环负荷(1.03 mol/L)。FT-IR和XRD表征分析表明,CaO的添加向MEA/MDEA溶液中提供了大量Ca2+和OH,可分别与溶液中的CO32-/HCO3、质子化胺反应生成碳酸钙沉淀和游离胺,从而同时完成对CO2的矿化和MEA/MDEA溶液的化学再生;并且得到的固体产物主要成分为碳酸钙,方解石是其主要晶型。
  • 图  1  CO2吸收和矿化反应系统示意图

    Figure  1  (a) System of CO2 absorption, (b) The system of CO2 mineralization

    1: gas cylinder; 2: pressure reducing valve; 3: mass flowmeter; 4: mixing tank; 5: buffer bottle; 6: CO2 bubbling absorption device; 7: thermostatic heating magnetic stirrer; 8: pH meter; 9: serpentine condenser; 10: drying tube; 11: flue gas analyzer; 12: slurry reaction device; 13: filter unit

    图  2  不同混合胺溶液配比条件下CO2吸收速率(a),不同混合胺溶液配比条件下CO2吸收负荷(b)

    Figure  2  (a) CO2 absorption rate under different ratios of mixed amine solutions, (b) CO2 absorption loading under different ratios of mixed amine solutions(40 ℃, 180 min)

    图  3  不同混合胺溶液配比条件下CO2吸收富液FT-IR谱图

    Figure  3  FT-IR spectrum of CO2 absorption rich solution under different ratios of mixed amine solutions A: 1 mol/L MEA + 2 mol/L MDEA; B: 1.5 mol/L MEA + 1.5 mol/L MDEA; C: 2 mol /L MEA + 1 mol/L MDEA; D: 3 mol/L MEA; E: 3 mol/L MDEA

    图  4  不同混合胺溶液配比条件下CO2矿化性能

    Figure  4  CO2 mineralization performance under different ratios of mixed amine solutions A: 1 mol/L MEA + 2 mol/L MDEA; B: 1.5 mol/L MEA + 1.5 mol/L MDEA; C: 2 mol/L MEA + 1 mol/L MDEA; D: 3 mol/L MEA;E: 3 mol/L MDEA (40 ℃, 90 min, 500 r/min, CaO addition ratio = 1∶1)

    图  5  不同温度条件下CO2矿化性能

    Figure  5  CO2 mineralization performance under different temperature(ratios of mixed amine solution: 2 mol/L MEA + 1 mol/L MDEA, 60 min, 500 r/min, CaO addition ratio = 1:1)

    图  6  不同反应时间下CO2矿化性能

    Figure  6  CO2 mineralization performance under different reaction time(ratios of mixed amine solution: 2 mol/L MEA + 1 mol/L MDEA, 40 ℃, 500 r/min, CaO addition ratio = 1∶1)

    图  7  不同CaO添加比例条件下CO2矿化性能

    Figure  7  CO2 mineralization performance under different CaO addition(ratios of mixed amine solution: 2 mol/L MEA + 1 mol/L MDEA, 40 ℃, 60 min, 500 r/min)

    图  8  2 mol/L MEA + 1 mol/L MDEA混合胺溶液经五次吸收-矿化实验后的循环性能

    Figure  8  Cyclic performance of 2 mol/L MEA + 1 mol/L MDEA mixed amine solution after 5 absorption-mineralization experiments(40 ℃, 60 min, 500 r/min, CaO addition ratio = 1∶1)

    图  9  不同反应条件下MEA/MDEA贫液FT-IR谱图

    Figure  9  FT-IR spectra of MEA/MDEA lean solution at different reaction conditions (a) temperature; (b) reaction time; (c) CaO addition ratio

    图  10  不同反应条件下得到的固体产物XRD谱图

    Figure  10  XRD patterns of solid products obtained under different reaction conditions (a) temperature; (b) reaction time; (c) CaO addition ratio

    表  1  MEA/MDEA混合胺溶液耦合CaO吸收-矿化CO2反应过程

    Table  1  MEA/MDEA mixed amine solution coupling CaO absorption-mineralization CO2 reaction process

    CO2 absorption processMEARNH2 + CO2 (aq) ↔ RNH2+COO(Zwitterion)(1)
    RNH2+COO + RNH2 ↔ RNHCOO +RNH3+ (Protonated amine)(2)
    RNHCOO + H2O ↔ RNH2 + HCO$_3^{{\rm{ - }}} $(3)
    MDEACO2 (aq) + H2O ↔ H2CO3 ↔ H+ + HCO$_3^{{\rm{ - }}} $(4)
    R1R2R3N + H+ → R1R2R3NH+(Protonated amine)(5)
    CO2 mineralization processCaO(s) + H2O → Ca2+ + 2OH(6)
    Ca2+ + HCO$_3^{{\rm{ - }}} $ → CaCO3↓+ H+(7)
    HCO$_3^{{\rm{ - }}} $ + OH ↔ CO$_3^{2{\rm{ - }}} $ + H2O(8)
    Ca2++ CO$_3^{2{\rm{ - }}} $→CaCO3(9)
    Mixed amine chemical
    regeneration process
    MEARNH3+ + OH ↔ RNH2 + H2O(10)
    MDEAR1R2R3NH+ + OH ↔ R1R2R3N + H2O(11)
    Note: In the table, RNH2 represents MEA, R1R2R3N represents MDEA, and R, R1, R2 and R3 represent different alkyl side chains
    下载: 导出CSV
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  • 收稿日期:  2022-02-22
  • 录用日期:  2022-04-07
  • 修回日期:  2022-04-02
  • 网络出版日期:  2022-04-29

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