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金属有机骨架材料在二氧化碳加氢中的应用

周程 南永永 查飞 田海锋 唐小华 常玥

周程, 南永永, 查飞, 田海锋, 唐小华, 常玥. 金属有机骨架材料在二氧化碳加氢中的应用[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60097-X
引用本文: 周程, 南永永, 查飞, 田海锋, 唐小华, 常玥. 金属有机骨架材料在二氧化碳加氢中的应用[J]. 燃料化学学报. doi: 10.1016/S1872-5813(21)60097-X
ZHOU Cheng, NAN Yong-yong, ZHA Fei, TIAN Hai-feng, TANG Xiao-hua, CHANG Yue. Application of metal-organic frameworks in CO2 hydrogenation[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60097-X
Citation: ZHOU Cheng, NAN Yong-yong, ZHA Fei, TIAN Hai-feng, TANG Xiao-hua, CHANG Yue. Application of metal-organic frameworks in CO2 hydrogenation[J]. Journal of Fuel Chemistry and Technology. doi: 10.1016/S1872-5813(21)60097-X

金属有机骨架材料在二氧化碳加氢中的应用

doi: 10.1016/S1872-5813(21)60097-X
基金项目: 国家自然科学基金(21865031)资助
详细信息
    通讯作者:

    E-mail: zhafei@nwnu.edu.cn

  • 中图分类号: TQ 426.94

Application of metal-organic frameworks in CO2 hydrogenation

Funds: The project was supported by National Natural Science Foundation of China (21865031)
  • 摘要: 大气中二氧化碳(CO2)浓度的急剧增加引起了人们的关注,并提出了许多将CO2转化为高价值化学品的策略。金属有机框架材料(MOFs)由于其独特的孔隙率、大的比表面积、丰富的孔结构、多活性中心、良好的稳定性和可回收性,可用于二氧化碳的捕获和催化转化。基于晶体多孔材料的金属有机骨架(MOF)设计和合成的各种功能纳米材料可以作为多相催化剂或载体/前体来应对这些挑战。在本文中,笔者将主要关注MOFs在催化二氧化碳加氢领域的最新研究进展,包括催化加氢制备一氧化碳、甲烷、甲酸、甲醇和烯烃,分析了基于MOFs的催化剂的合成方法和提高催化活性的原因。介绍了提高新型MOF材料的催化活性和探索新的CO2转化可行的策略。讨论了MOF型催化剂在CO2化学转化中的主要挑战和机遇,对本研究领域中进一步的发展进行了简要的展望。
  • 图  1  ZIF-8热解合成Cu/Zn@C示意图[29]

    Figure  1  Pyrolysis of ZIF-8 to produce hierarchical Cu/Zn@C[29]

    图  2  (a)Pt/Au@Pd@UiO-66纳米复合材料的合成过程;(b)Pt/Au@Pd@UiO-66在不同温度下催化CO2还原;(c)Au@Pd@UiO-66和Pt/Au@Pd@UiO-66的CO选择性[30]

    Figure  2  (a): Synthesis process of Pt/Au@Pd@UiO-66 nanocomposites; (b): CO2-reduction catalyzed by Pt/Au@Pd@UiO-66 at different temperatures; (c): CO product selectivity of Au@Pd@UiO-66 and Pt/Au@Pd@UiO-66[30]

    图  3  (a)M/ZIF-8-C的CO2转化率;(b)CO、CH4的选择性[31]

    Figure  3  (a): CO2 conversion; (b): selectivity of CO, and CH4 on M/ZIF-8-C[31]

    图  4  (a)xNi@MIL-101(DSM)合成示意图;(b)CO2甲烷化在20Ni@MIL-101(DSM)催化剂上的反应机理[39]

    Figure  4  (a): Schematic illustration on the synthesis of xNi@MIL-101(DSM) catalysts; (b): The proposed possible reaction mechanism of CO2 methanation over 20Ni@MIL-101(DSM) catalyst[39]

    图  5  Ru/UiO-66合成和原位转化为MOF衍生催化剂的示意图[40]

    Figure  5  Scheme of synthesis and in situ transformation Ru/UiO-66 to MOF derived catalyst[40]

    图  6  添加不同含量十六烷基三甲基溴化铵的催化剂的CO2转化率[41]

    Figure  6  CO2 conversion on catalysts with different content of CATB[41] (with permission from ACS)

    图  7  协同和逐步机理的CO2加氢能谱[44]

    Figure  7  Energy profile of the CO2 hydrogenation for concerted and stepwise systems[44]

    图  8  (a)LPs功能化UiO-66的八面体笼的BDC配体(b)UiO-66-X中CO2加氢的反应能垒与H2在UiO-66-X中的吸附能的关系[45]

    Figure  8  (a): LPs functionalized BDC ligand of the octahedral cage of UiO-66; (b): Calculated reaction energy barriers for CO2 hydrogenation in UiO-66-X as a function of the adsorption energies of H2 in UiO-66-X[45]

    图  9  以ZIF-8为牺牲模板制备CuZn-BTC的形成机理示意图[49]

    Figure  9  Schematic diagram of the formation mechanism of CuZn-BTC prepared with ZIF-8 as a sacrificial template[49]

    图  10  (a)Cu NC-UiO-6活性位点的图示;(b)${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66 $和Cu/ZnO/Al2O3在各不同反应温度下产物的TOFs;(c)在${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66 $上和Cu在UiO-66上甲醇的初始TOFs;(d)${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66 $(UiO-66内部的单个CuNC)的TEM;(e)UiO-66上Cu的TEM[50]

    Figure  10  (a) Illustration of active site of Cu NC-UiO-66 catalyst; (b) TOFs of product formation over ${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66$ catalyst and Cu/ZnO/Al2O3 catalyst as various reaction temperatures; (c) Initial TOFs of methanol formation over ${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66$ and Cu on UiO-66 ; (d) TEM images of ${\rm{Cu}} \subset {\rm{UiO}} {\text{-}} 66$(single Cu NC inside UiO-66); (e) TEM images of Cu on UiO-66[50]

    图  11  (a)合成后金属化的UiO-bpy原位还原制备CuZn@UiO-bpy示意图;(b)CH3OH的时空产率随在反应时间的变化;(c)产物的选择性随反应时间的变化;(d)MOF中封装的活性位点以及各种表面位点在催化CO2加氢中的功能[51]

    Figure  11  (a): Preparation of CuZn@UiO-bpy via in situ reduction of post-synthetically metalized UiO-bpy; (b): STY of CH3OH vs reaction time on stream; (c) Selectivity of product vs reaction time; (d) Schematic showing the encapsulated active sites in MOF and the functions of the various surface sites in catalytic CO2 hydrogenation [51] (with permission from ACS)

    图  12  PZ8-t催化剂的制备和Pd-ZnO@ZIF-8催化CO2加氢制甲醇的示意图[54]

    Figure  12  Schematic illustration of the preparation process of the PZ8-T and the preparation procedure of Pd-ZnO@ZIF-8 for CO2 hydrogenation to methanol [54]

    图  13  在不同催化剂上的二氧化碳转化率和产物选择性[58]

    Figure  13  CO2 conversion rate and selectivity on different catalysts[58] (with permission from Elsevier)

    图  14  Fe基Basolite F300催化剂合成机理与形态表征[59]

    Figure  14  Synthesis mechanism and morphology of Fe-based Basolite F300[59] (with permission from ACS)

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  • 收稿日期:  2021-03-16
  • 修回日期:  2021-04-21
  • 网络出版日期:  2021-05-18

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