提高金属有机骨架材料在二氧化碳热催化转化中的性能: 策略及前景展望

doi:10.1016/S1872-2067(21)63841-X

催化学报 ›› 2021, Vol. 42 ›› Issue (11): 1903-1920.DOI: 10.1016/S1872-2067(21)63841-X

提高金属有机骨架材料在二氧化碳热催化转化中的性能: 策略及前景展望

郝磊端^a, 夏启能^b^,^$(), 张强^c^,^#(), Justus Masa^d, 孙振宇^a^,^*()

^a北京化工大学化学工程学院, 有机-无机复合材料国家重点实验室, 北京100029, 中国
^b嘉兴学院生物与化学工程学院, 浙江嘉兴314001, 中国
^c华盛顿州立大学化学系, 普尔曼, 美国
^d克雅博格大学化学系, 坎帕拉, 乌干达

收稿日期:2021-04-15 修回日期:2021-04-15 出版日期:2021-11-18 发布日期:2021-05-20
通讯作者: 夏启能,张强,孙振宇
基金资助:
国家自然科学基金(21972010);国家自然科学基金(21972056);北京市自然科学基金面上项目(2192039);有机-无机复合材料国家重点实验室基金(oic-201901001)

Improving the performance of metal-organic frameworks for thermo-catalytic CO₂ conversion: Strategies and perspectives

Leiduan Hao^a, Qineng Xia^b^,^$(), Qiang Zhang^c^,^#(), Justus Masa^d, Zhenyu Sun^a^,^*()

^aState Key Laboratory of Organic-Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^bCollege of Biological, Chemical Science and Engineering, Jiaxing University, Jiaxing 314001, Zhejiang, China
^cDepartment of Chemistry, Washington State University, Pullman 99164, United States
^dDepartment of Chemistry, Kyambogo University, P. O. Box 1, Kyambogo, Kampala, Uganda

Received:2021-04-15 Revised:2021-04-15 Online:2021-11-18 Published:2021-05-20
Contact: Qineng Xia,Qiang Zhang,Zhenyu Sun
About author:^#Tel: +1-509-335-1269; E-mail: q.zhang@wsu.edu
^$Tel: +86-13736870651; E-mail: xiaqineng@mail.zjxu.edu.cn;
^*Tel: +86-13301308339; E-mail: sunzy@mail.buct.edu.cn;
Supported by:
National Natural Science Foundation of China(21972010);National Natural Science Foundation of China(21972056);Beijing Natural Science Foundation(2192039);State Key Laboratory of Organic-Inorganic Composites(oic-201901001)

摘要/Abstract

摘要：

近年来, 大气中CO₂的浓度不断增加, 带来全球变暖等一系列严重后果, 成为国际社会共同关注的环境问题. 将CO₂催化转化为高附加值化学品可有效降低其向大气中的排放, 同时可实现其资源化利用, 符合低碳社会的发展目标. 目前, 已有多种催化体系实现了CO₂向不同化学品的转化. 然而, 由于CO₂自身的热力学稳定性和动力学惰性, 这些转化通常需要在苛刻的反应条件和较高能耗下进行. 设计开发高效催化体系、实现温和条件下CO₂的转化利用引起了工业界和学术界的广泛兴趣.
金属有机骨架材料(MOFs)是一类由有机配体和金属中心通过配位键组装而成的有机-无机杂化材料, 在很多方面展现出良好的应用性能. 由于其结构的多样性、可设计性、高比表面积和多孔性等独特性质, MOFs在催化领域吸引了很多研究者的关注. 其中, MOFs作为非均相催化剂在CO₂热催化转化中表现出良好的应用前景, 已实现多种CO₂向高值化学品的转化路径. 但这些催化体系也存在一些缺点, 如有些MOFs材料在催化反应中稳定性差以及其微孔性对反应中的传质造成限制等. 因此, 设计稳定的MOFs和MOF-基材料并对其结构进行优化改性, 从而在温和条件下实现高效的CO₂转化具有重要意义.
本文综述了提高MOFs在CO₂热催化转化反应中性能的几种策略: (1)对MOFs结构中的配体进行设计, 包括具有活性官能团的配体、活性配合物作为配体和引入混合配体设计多元MOF; (2)调节MOFs结构中的金属中心, 设计混合金属中心和包含活性金属团簇的金属中心; (3)构筑多级孔MOFs; (4)设计MOF-基的复合材料, 包括MOFs作为载体与金属纳米颗粒、活性配合物和聚合物构建复合材料; (5)利用MOFs作为前驱体制备MOF-基衍生物材料, 重点阐述了如何增加MOFs作为非均相催化剂的催化活性位点以及在CO₂转化反应中各位点之间的协同作用. 此外, 介绍了原位表征技术在MOF-基材料用于CO₂固定和转化中的应用. 最后, 分析了MOF-基非均相催化材料在CO₂热催化转化领域目前面临的问题和挑战, 包括MOFs材料结构优化、催化机理研究和规模化制备等方面, 并对未来的发展趋势进行了展望.

关键词: 二氧化碳转化, 金属有机骨架材料, 催化活性位点, 协同作用, 催化性能

Abstract:

Climate change caused by the increasing emission of CO₂ to the atmosphere has become a global concern. To ameliorate this issue, converting CO₂ into valuable chemicals is highly desirable, enabling a sustainable low-carbon future. To this end, developing efficient catalytic systems for CO₂ conversion has sparked intense interests from both academia and industry. Taking advantage of their highly porous structures and unique properties, metal-organic frameworks (MOFs) have shown great potential as heterogeneous catalysts for CO₂ conversion. Various transformations involving CO₂ have been accomplished over MOFs-based materials. Here we provide a comprehensive and up-to-date review on recent advances of heterogeneous CO₂ thermocatalysis using MOFs, highlighting relationships between structures and properties. Special attention is given to the design strategies for improving the catalytic performance of MOFs. Avenues available to enrich the catalytic active sites in MOF structures are stressed and their respective impacts on CO₂ conversion efficiency are presented. The synergistic effects between each active site within the structure of MOFs and derivatives are discussed. In the end, future perspectives and challenges in CO₂ conversion by heterogeneous catalysis with MOFs are described.

Key words: CO₂ conversion, Metal-organic frameworks, Catalytic active sites, Synergy, Catalytic performance

郝磊端, 夏启能, 张强, Justus Masa, 孙振宇. 提高金属有机骨架材料在二氧化碳热催化转化中的性能: 策略及前景展望[J]. 催化学报, 2021, 42(11): 1903-1920.

Leiduan Hao, Qineng Xia, Qiang Zhang, Justus Masa, Zhenyu Sun. Improving the performance of metal-organic frameworks for thermo-catalytic CO₂ conversion: Strategies and perspectives[J]. Chinese Journal of Catalysis, 2021, 42(11): 1903-1920.

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图/表 17

Scheme 1. Proposed mechanism for cycloaddition of CO2 with epoxides catalyzed by MOFs with a cocatalyst.

Fig. 1. (a) The structure of the H8L1 ligand; (b) perspective view of 3D porous framework of NTU-180 (yellow and blue balls represent two kinds of pores). Adapted with permission from Ref. [64]. Copyright 2016, American Chemical Society. (c) The structure of the acylamide-containing ligand.

Fig. 3. (a-c) Schematic illustration of the synthesis of ZnTCPP?(Br-)Etim-UiO-66: Sequential mixed-ligands of different geometry, post-synthetic ionization, and post-synthetic metalation strategy (a); one-pot synthesis based on [(Br-)(Etim-H2BDC)+] ligand (b, c). Im-Zr6, imidazole functionalized Zr6 cluster; (Br-)Etim-Zr6, imidazolium functionalized Zr6 cluster. The yellow sphere represents the pore cavity. (d) Proposed mechanism of the catalytic process. Adapted with permission from Ref. [85]. Copyright 2018, American Chemical Society.

Table 1 CO2 conversion reactions catalyzed by MOFs with designed metal centers.

Catalyst/Active sites	Optimal reaction conditions and performance	Ref.
1-Zn/Lewis acidic Zn²⁺	r.t., 1.2 MPa, 60 h, 3.75 mol% TBAB; propylene carbonate yield: 99%	[87]
Yb-DDIA/Lewis acidic Yb³⁺	60 °C, 1.0 MPa, 12 h, 0.5 mol% TBAB; 5 substrates, yield: up to 93%	[88]
RE-BDC (RE = Y or Tb or Er)/Y³⁺ or Tb³⁺ or Er³⁺	60 °C, 1.0 MPa, 12 h, 1.05 mol% TBAB; 5 substrates, yield: up to 95%	[89]
Sm-BTB/Sm³⁺	80 °C, 0.1 MPa, 15 h, 1.0 mol% TBAB; 5 substrates, yield: up to 100%	[90]
CZ-BDO/Co-Zn and Lewis basic N	100 °C, 3.0 MPa, 5 h; 4 substrates, yield: up to 97.05%	[53]
ErCo-1/Er³⁺	70 °C, 1.0 MPa, 10 h, 5.0 mol% TBAB; 5 substrates, yield: up to 94%	[52]
CuGd-I or CuGd-II/ [Cu₁₂I₁₂] or [Cu₃I₂]	80 °C, 0.1 MPa, 4 h, 1.2 equiv. Cs₂CO₃, 1.2 equiv. nBuI, ethylene carbonate; 14 substrates, yield: up to 86%	[51]
CuIn-1/[Cu₄I₄] and In³⁺	50 °C, 0.5 MPa, 10 h, TEA; 8 substrates, yield: up to 99%	[102]
Ag27-MOF/Ag	25 °C, 0.1 MPa, 6 h, 0.1 equiv. DBU, acetonitrile; 12 substrates, yield: up to 99%	[108]

Fig. 5. (a) Schematic illustration of the synthesis of hierarchically porous mesoCu@Al-bpydc; (b) catalytic performance of microCu@Al-bpydc and mesoCu@Al-bpydc with different epoxides. Adapted with permission from Ref. [115]. Copyright 2019, WILEY-VCH.

Fig. 6. (a) The building blocks of mesoporous JLU-MOF58 (simplified as linear rod and cube); (b) two types of mesoporous cages in JLU-MOF58. Adapted with permission from Ref. [54]. Copyright 2019, American Chemical Society.

Table 2 CO2 conversion reactions catalyzed by MNPs@MOFs.

Reaction	Catalyst/Active sites	Optimal reaction conditions and performance	Ref.
	Ag@MIL-101(Cr)/Ag Ag@MIL-101(Fe)/Ag Ag@UiO-66(Zr)/Ag	50 °C, 0.1 MPa, 15 h, 1.5 equiv. Cs₂CO₃, DMF; 5 substrates, yield: up to 98.7%	[117, 109]
	Ag@Co(II)-salicylate/Ag	80 °C, 0.1 MPa, 14 h, 1.5 equiv. Cs₂CO₃, DMF; 7 substrates, yield: up to 98%	[108]
	Pd-Cu@MIL-101(Cr)/Pd-Cu	25 °C, 0.1 MPa, 24 h, 1.5 equiv. Cs₂CO₃, DMF; 5 substrates, yield: up to 98%	[122]
	AuAg@ZIF-8/AuAg	50 °C, 0.1 MPa, 24 h, 0.24 equiv. K₂CO₃, DMF; 6 substrates, yield: up to 100%	[123]
CO₂ hydrogenation to methanol	CuZn@UiO-bpy/Cu/ZnO_x	250 °C, 4 MPa total pressure; methanol space-time yield: 2.59 g_MeOH kg_Cu^-1h^-1, selectivity: 100%	[120]
CO₂ hydrogenation to methanol	Cu@UiO-66/Cu	175 °C, 1 MPa total pressure; methanol selectivity: 100%, TOF: 3.7 × 10^-3 s^-1	[125]
CO₂ hydrogenation to light olefins	Fe₂O₃@ZIF-8/Fe₂O₃	300 °C, 3 MPa total pressure; light olefin C₂-C₄ selectivity: ~20%	[124]
CO₂ hydrogenation to methane	Ni@MIL-101(Cr)/Ni	300 °C, H₂ to CO₂ ratio = 4:1; methane selectivity: 100%, TOF: 1.63 × 10^-3 s^-1	[126]
CO₂ hydrogenation to methane	Ni@UiO-66/Ni	300 °C, 1 MPa total pressure; CO₂ conversion: 57.6%, methane selectivity: 100%	[127]
CO₂ hydrogenation to CO	Pt@UiO-67/Pt	220-280 °C, H₂ to CO₂ ratio = 6:1; CO selectivity: > 90%	[128]
	Pt@MOF-74(Zn)/Pt	400 °C, 2 MPa total pressure, H₂ to CO₂ ratio = 3:1; CO₂ conversion: 33.8%, CO selectivity: > 99%	[129]
	Pt-Au@Pd@[Co₂(oba)₄(3-bpd h)₂]·4H₂O/Pt-Au@Pd	400 °C, 2 MPa total pressure, H₂ to CO₂ ratio = 3:1; CO₂ conversion: 15.6%, CO selectivity: 87.5%	[130]

Fig. 9. Schematic illustration of the synthesis of (a) (R,R)-salen(Co(III))@IRMOF-3-AM. Adapted with permission from Ref. [132]. Copyright 2017, Royal Society of Chemistry. (b) Salen-Cu(II)@MIL-101(Cr). Adapted with permission from Ref. [133]. Copyright 2017, Elsevier.

Fig. 11. (a) Schematic illustration of the synthesis of polyILs@MIL-101; (b) Catalytic performance of different catalysts. Adapted with permission from Ref. [138]. Copyright 2018, American Chemical Society.

Fig. 12. Schematic illustration of (a) the synthesis of ZnO@NPC-Ox toward CO2 cycloaddition with epoxides. Adapted with permission from Ref. [146]. Copyright 2017, WILEY-VCH. (b) The fabrication of HPC. Adapted with permission from Ref. [147]. Copyright 2019, WILEY-VCH.

Fig. 13. Schematic illustration of the synthesis of M@CSN nanoreactor. M represents monometallic or bimetallic nanoparticles; mSiO2 = mesoporous SiO2; R-NBH4 = tetrabutylammonium borohydride; CTAC = cetyltrimethylammonium chloride; TEOS = tetraethylorthosilicate. Adapted with permission from Ref. [151]. Copyright 2017, American Chemical Society.

Fig. 14. In situ FT-IR spectra of the reaction between CO2 and epichlorohydrin catalyzed by (I-)Meim-UiO-66, whose spectrum was subtracted for clarity. Adapted with permission from Ref. [159]. Copyright 2017, Royal Society of Chemistry.

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提高金属有机骨架材料在二氧化碳热催化转化中的性能: 策略及前景展望

Improving the performance of metal-organic frameworks for thermo-catalytic CO₂ conversion: Strategies and perspectives

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提高金属有机骨架材料在二氧化碳热催化转化中的性能: 策略及前景展望

Improving the performance of metal-organic frameworks for thermo-catalytic CO2 conversion: Strategies and perspectives

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Improving the performance of metal-organic frameworks for thermo-catalytic CO₂ conversion: Strategies and perspectives