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CO2甲烷化反应路径的研究进展

付豪 廉红蕾

付豪, 廉红蕾. CO2甲烷化反应路径的研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022063
引用本文: 付豪, 廉红蕾. CO2甲烷化反应路径的研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022063
FU Hao, LIAN Hong-lei. Research progress on the reaction pathway of CO2 methanation[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022063
Citation: FU Hao, LIAN Hong-lei. Research progress on the reaction pathway of CO2 methanation[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022063

CO2甲烷化反应路径的研究进展

doi: 10.19906/j.cnki.JFCT.2022063
基金项目: 煤基生态精细化工河南省工程实验室开放课题(C202003)
详细信息
    作者简介:

    付豪(1997−),男,硕士研究生。E-mail:fuhao0416@163.com

    通讯作者:

    廉红蕾(1977−),女,博士,硕导,研究方向为多相催化材料合成及原位光谱表征技术。TEL: 13663002080,E-mail: hongleilian@zzu.edu.cn

  • 中图分类号: O643.3

Research progress on the reaction pathway of CO2 methanation

Funds: Opening Foundation of Henan Provincial Engineering Laboratory of Coal-based Ecological Fine Chemicals (C202003)
  • 摘要: CO2甲烷化反应是一个十分复杂的多相催化过程,在反应过程中会产生各种各样的中间体,其反应路径目前还存在许多争议和矛盾。深入系统地研究CO2甲烷化反应中催化剂表面中间体的演变过程,可以进一步从机理的角度优化催化剂的设计方案,提高催化性能。本文主要基于原位红外光谱表征技术,总结梳理了最近关于CO2甲烷化反应路径研究的相关工作,着重探讨了负载型催化剂的活性金属、载体、助剂、合成方法等因素对CO2甲烷化反应路径的影响以及由此对催化剂性能所产生的积极效果。同时针对现阶段所面临的争论点,即反应气CO2与H2的活化位点、催化剂的活性位点以及未来可行的研究方法进行了详细论述。
  • 图  1  CO2甲烷化反应过程中的各种中间体

    Figure  1  Various intermediates during the CO2 methanation reaction

    图  2  催化剂Rh(1%)/γ-Al2O3上CO2吸附30秒,15分钟,30分钟的原位红外谱图(常压,125 ℃) [13]

    Figure  2  DRIFTS results after adsorption of CO2 on Rh(1%)/γ-Al2O3 at 125 ℃ and atmospheric pressure, after 30 s, 15 min and 30 min [13]

    图  3  金属K, Ni改性的催化剂Rh/Al2O3表面CO2加氢反应物种与反应机理[18]

    Figure  3  Identified species and proposed mechanism for CO2 hydrogenation over K and Ni modified Rh/Al2O3 catalyst [18]

    图  4  红外吸收光谱法表征催化剂的常用模式[19]

    Figure  4  Common setups used for the characterization of catalytic samples using infrared absorption spectroscopy[19]

    图  5  不同Ni负载量的Ni-Al催化剂的CO2-TPD谱图[35]

    Figure  5  CO2-TPD plot of Ni-Al catalysts with different Ni loading amounts[35]

    图  6  Rh/ZrO2催化剂上的CO2甲烷化路径示意图[24]

    Figure  6  Schematic representation of the proposed routes for CO2 methanation catalyzed by ZrO2-supported Rh [24]

    图  7  在CO2与H2混合气体下升温处理时(A)Ni/ZrO2和(B)纯载体ZrO2的红外光谱表征 [12]

    Figure  7  IR spectra characterizing (A) the ZrO2-supported Ni sample and (B) the bare support as they were treated in a flowing mixture of CO2 and H2 at increasing temperature [12]

    图  8  (A)流动反应器/DRIFT池流出气体质谱中CH4和H2O质量碎片信号强度和甲酸盐(1570−1590 cm−1)、甲氧基(1160 cm−1)的红外吸收峰强度变化曲线,甲酸加氢过程红外采样(左),甲醇加氢过程红外采样(右)(B)甲酸加氢过程中催化剂Ni/ZrO2的红外谱图(左);甲醇加氢过程中催化剂Ni/ZrO2的红外谱图(右)[12]

    Figure  8  (A) Correlation between the signal intensities of the mass fragments of CH4 and H2O in mass spectra of the effluent gases from the flow reactor/DRIFT cell,Infrared absorption peak intensity change curve of formate (1570−1590 cm−1), methoxy (1160 cm−1), infrared sampling during formic acid hydrogenation process (left), infrared sampling during methanol hydrogenation process (right) (B) Infrared spectra of catalyst Ni/ZrO2 during hydrogenation of formic acid (left) Infrared spectrogram of catalyst Ni/ZrO2 during hydrogenation of methanol (right) [12]

    图  9  513 K下,原料气CO2 + H2与CO2交替切换时催化剂5%Pd/Al2O3上随时间变化的(a)红外谱图(b)在DRIFT池出口处收集的相应质谱信号曲线图(左)513 K下,原料气CO2 + H2与CO2交替切换时还原的催化剂0.5%Pd/Al2O3上随时间变化的(a)红外谱图(b)在DRIFT池出口处收集的相应质谱信号曲线图(右)[43]

    Figure  9  (a) DRIFT spectra and (b) the corresponding MS signals collected at the exit of the DRIFT cell as a function of time when the feed gas was switched alternately between CO2 + H2 and CO2 over 5% Pd/Al2O3 at 513 K (left) (a) DRIFT spectra and (b) the corresponding MS signals at the exit of the DRIFT cell collected at 513 K as a function of time when the feed gas was switched alternately between CO2 + H2 and CO2 over a reduced 0.5% Pd/Al2O3 sample [43]

    图  10  CH4和CO的形成机理[44]

    Figure  10  CH4 and CO formation mechanism. [44]

    图  11  催化剂Ni/ZrO2-P(a)与Ni/ZrO2-C(b)在2.5%H2,0.5%CO2和Ar作为载体组成的混合气体(40 ml min−1)下进行程序升温反应时的原位红外光谱[69]双齿碳酸氢盐(♣), 单齿碳酸盐(♦), 双齿甲酸盐( + )、单齿甲酸盐(*)、线性CO或桥连CO (△) 以及气态CH4 (●)

    Figure  11  Operando DRIFT spectra during temperature-programmed reaction of a gas mixture (40 ml min−1) containing 2.5% H2, 0.5% CO2 with Ar as carrier gas over Ni/ZrO2-P (a) and Ni/ZrO2-C (b) [69] bidentate bicarbonate (♣), monodentate carbonates (♦), bidentate formate ( + ), monodentate formate (*), linear CO or bridge CO (△) and gaseous CH4 (●)

    图  12  中间体碳酸盐的生成路径 (ⅰ.碳酸氢盐解离生成碳酸盐;ⅱ.CO2吸附直接生成碳酸盐)

    Figure  12  Formation path of intermediate carbonate (i. bicarbonate dissociation to form carbonate; ii. CO2 adsorption directly generates carbonates)

    图  13  氢气的活化解离

    Figure  13  Activation and dissolution of hydrogen

    图  14  M/MSN上CO2甲烷化的反应机制[15]

    Figure  14  Reaction path mechanism of CO2 methanation on M/MSN[15]

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  • 收稿日期:  2022-05-20
  • 录用日期:  2022-07-18
  • 修回日期:  2022-07-11
  • 网络出版日期:  2022-07-28

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