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

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

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63841-X

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

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