Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO2 Reduction★

doi:10.6023/A26020053

Acta Chimica Sinica ›› 2026, Vol. 84 ›› Issue (5): 755-774.DOI: 10.6023/A26020053 Previous Articles Next Articles

Review

基于含氮杂环配体的金属有机框架材料在电催化CO₂还原中的应用与前景展望^★

张亚^a^,^*(), 周功兵^a, 孙为银^b^,^*()

^a 重庆师范大学化学与材料科学学院绿色催化材料与技术重庆市重点实验室重庆 401331
^b 南京大学化学学院配位化学全国重点实验室南京 210023

投稿日期:2026-02-10 发布日期:2026-05-06
通讯作者: 张亚, 孙为银

作者简介:

张亚, 重庆师范大学化学与材料科学学院讲师, 2024年于南京大学化学化工学院获博士学位, 主要从事金属有机框架及其复合材料、过渡金属纳米材料的可控合成及其在电催化小分子(CO₂/H₂O/N₂)转化领域的应用.

周功兵, 重庆师范大学化学与材料科学学院教授, 2009年于华南理工大学获学士学位(应用化学专业), 2014年于复旦大学获博士学位(物理化学专业). 目前研究方向为金属纳米催化剂的结构调控及其在生物质小分子催化转化、电催化水分解中的应用.

孙为银, 南京大学化学学院教授, 1986年上海华东师范大学化学系本科毕业, 1990年和1993年在日本大阪大学分别获得硕士和理学博士学位. 近期的研究重点是利用金属有机框架及其衍生材料光/电催化CO₂还原. 已发表超过400篇研究论文, 担任J. Coord. Chem. 编委, CrystEngComm顾问编委, 并自2014年起成为英国皇家化学学会会士(FRSC).

★ 框架材料化学专辑.

基金资助:
国家自然科学基金(22231006); 国家自然科学基金(21703024); 重庆市自然科学基金(CSTB2025NSCQ-GPX0259); 重庆市教委科技项目(KJZD-K202200514); 重庆师范大学基金(24XLB028)

Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction^★

Ya Zhang^a^,^*(), Gongbing Zhou^a, Wei-Yin Sun^b^,^*()

^a Chongqing Key Laboratory of Green Catalysis Materials and Technology, College of Chemistry and Materials Science, Chongqing Normal University, Chongqing 401331, China
^b State Key Laboratory of Coordination Chemistry, School of Chemistry, Nanjing University, Nanjing 210023, China

Received:2026-02-10 Published:2026-05-06
Contact: Ya Zhang, Wei-Yin Sun
About author:
★ For the VSI “Chemistry of Framework Materials”.
Supported by:
National Natural Science Foundation of China(22231006); National Natural Science Foundation of China(21703024); Natural Science Foundation of Chongqing, China(CSTB2025NSCQ-GPX0259); Science and Technology Research Program of Chongqing Municipal Education Commission of China(KJZD-K202200514); Chongqing Normal University Foundation(24XLB028)

Achieving carbon neutrality through reducing amounts of atmospheric carbon dioxide (CO₂) has emerged as an urgent global challenge in the fields of environmental science and sustainable development. Among the emerging mitigation strategies, electrocatalytic CO₂ reduction reaction (ECRR) stands out for its capacity to convert CO₂ into high-valued chemicals or energy-dense fuels, providing a promising approach for reducing CO₂ emissions and converting renewable electric energy into chemical energy. Metal-organic frameworks (MOFs) represent a promising class of catalysts for ECRR, owing to their intrinsic structural advantages—including well-defined porosity and atomic-level structural tunability—which collectively enhance CO₂ mass transport and adsorption, and enable systematic investigation of structure-activity relationship as well as reaction mechanism. In particular, MOFs constructed from nitrogen-containing heterocyclic ligands have garnered remarkable research interest, attributed to their superior features such as structural flexibility, abundant catalytic active sites and suitable stability. This review outlines the fundamental physicochemical properties and advanced characterization techniques for the nitrogen-containing heterocyclic ligand-based MOFs. Then recent advances in the application of such MOFs to ECRR were summarized categorizing by the nitrogen-containing moieties, namely imidazolyl-, pyrazolyl-, triazolyl- and tetrazolyl-based ligands. Finally, this review analyzed the critical challenges impeding the practical application of nitrogen-containing heterocyclic ligand-based MOFs in ECRR, including intrinsic electronic conductivity limitations, structural and electrochemical stability under prolonged operational conditions, integration of electrolyzer systems and mechanistic ambiguities arising from dynamic structural evolution during the ECRR. On this basis, prospects for future research directions are presented.

Key words: metal-organic frameworks, nitrogen-containing heterocyclic ligands, CO₂ reduction reaction, electrocatalytic conversion

Cite this article

Ya Zhang, Gongbing Zhou, Wei-Yin Sun. Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction^★[J]. Acta Chimica Sinica, 2026, 84(5): 755-774.

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Fig. & Tab. 14

Figure 1. (a) The EDL structure on the surface of an MOF particle; (b) ions/molecules diffusion into the MOF framework in the EDL structure; (c) cross-sectional illustration of MOF-coated electrode in neutral electrolyte; (d) structural destruction of MOFs driven by the redox reactions involving metal nodes or organic linkers; (e) EDL formation and ion diffusion on the surface or inside the pores of MOFs due to the dynamic potential sweeping[54] (Copyright 2021 American Chemical Society)

Figure 2. (a) Potentiostatic synthesis methods and performance of Cu3(DMPz)3; (b) Schematic illustration for the catalytic mechanism of CH4 and C2H4 production on Cu3(DMPz)3 with ALPS methods[57] (Copyright 2023 American Chemical Society)

Figure 3. (a) Synthesis process of ZIF-A-LD; (b) FECO of ZIF-8, ZIF-A-LD, ZIF-8/CB, and ZIF-A-LD/CB at different potentials; (c) free energy profile of ZIF-8 and ZIF-A-LD on the sp2 C atom sites[77] (Copyright 2019 Wiley-VCH GmbH); (d) schematic diagram of synthesis process for ZIF-8/Zn[79] (Copyright 2022 Wiley-VCH GmbH); (e) preparation of Cu-MOF-CF; (f) ECRR products of CF and Cu-MOF-CF; (g) FEC2H4 of CF and Cu-MOF-CF[83] (Copyright 2023 Wiley-VCH GmbH)

Figure 4. (a) Scheme for preparation of ZIF-P5/In[84] (Copyright 2024 Elsevier); (b) schematic illustration of the synthesis process of Cu2O/ZIF-8; (c) FEC2＋ of Cu/ZIF-8 and Cu NPs; (d) Cu K-edge FT-EXAFS curves of Cu/ZIF-8 and the references; (e) C—C coupling free-energy profile of Cu/ZIF-8 and Cu cluster[69] (Copyright 2024 Chinese Chemical Society)

Figure 5. (a) Scheme for preparation and structure of Cu—X; (b) FEs of different products on Cu-I at various potentials; (c) FECH4 of Cu—Cl, Cu—Br, and Cu—I catalysts; (d) free energy profiles of ECRR on Cu—Cl, Cu—Br, and Cu—I[85] (Copyright 2022 Wiley-VCH GmbH)

Figure 6. (a) Interpenetrated 3D structures of Ag-MOF1 along the c-axis; (b) 2D structure of Ag-MOF2; (c) FECO of Ag-MOFs at different potentials[86] (Copyright 2024 Royal Society of Chemistry); 2D networks of (d) [Cu(TIPE)0.5](ClO4) and (e) [Co(TIPE)(TFA)2]•2DMF; (f) FEs of ECRR products for [Cu(TIPE)0.5](ClO4) at different potentials[87] (Copyright 2024 Royal Society of Chemistry)

Figure 7. (a) Schematic diagram of the synthesis procedure for Ag@BIF-104NSs(Cu); (b) the calculated structures of CO desorption on BIF-104NSs(Cu) and the C—C coupling on Ag@BIF-104NSs(Cu)[89] (Copyright 2023 Wiley-VCH GmbH); (c) schematic illustration of the post-assembly modification of tetrahedral cages; (d) structural diagram of BIC-145; (e) the possible ECRR pathways for CO2 to C2H4 conversions on BIC-145[90] (Copyright 2025 Science China Press)

Figure 8. (a) Illustration of the difference in selectivity for Cu-PzX (where X=H, Cl, Br, I) in the ECRR[91] (Copyright 2021 Wiley-VCH GmbH); (b) synthetic route and 3D structure of CuBPZ[92] (Copyright 2022 Wiley-VCH GmbH); (c) 3D framework of NNU-50[94] (Copyright 2022 Tsinghua University Press); (d) structural model of the Cu1Ni-BDP MOF; (e) HRTEM image and (f) simulated structure model of Cu1Ni-BDP MOF; (g) FEs toward ECRR products and H2 on the Cu1Ni-BDP MOF at different potentials; (h) calculated Gibbs free energy diagrams on the Ni-BDP MOF, Cu1Ni-BDP MOF, and Cu2Ni-BDP MOF[95] (Copyright 2023 American Chemical Society)

Figure 9. (a) Schematic synthesis of Pd-Cu@CuPz2; (b) the FEC2＋ over the different catalysts at various potentials; (c) the Gibbs free energy diagrams of CO2 to *OCCO on Cu2O-CuPz2 and Cu2O-PdO-CuPz2 surface; (d) the Gibbs free energy diagrams of *CH2CHO to EtOH on Cu2O-PdO-CuPz2 (Cu) and Cu2O-PdO-CuPz2 (Pd) surface[58] (Copyright 2024 Wiley-VCH GmbH)

Figure 10. (a) Synthetic route of CuTrz nanostructures with different sizes as well as the chemical structure of the CuTrz; (b) FE of C2H4 and (c) FE of C2＋ products on CuTrz-53 nm, CuTrz-109 nm, CuTrz-307 nm, and CuTrz-1335 nm at different potentials, respectively[98] (Copyright 2023 American Chemical Society); (d) chemical structure of ligand molecules; (e) the structure of Ln-Cu, X represents the substituents and is on the right frame, * indicates the position connecting with triazole rings; (f) ηC—C coupling of Ln-Cu at －(0.930±0.008) V[67] (Copyright 2024 Springer Nature)

Figure 11. (a) Schematic synthesis of Cu-N-S and Cu-I-S and the different products of ECRR on Cu-N-S and Cu-I-S, respectively; (b) The FE of C2H4 and C2＋ products on Cu-N-S and Cu-I-S at different potentials[101] (Copyright 2024 American Chemical Society); 3D frameworks of (c) MAF-2Fa and (d) MAF-2Fb; (e) Comparison of typical performances at －1.2 V for MAF-2Fa and MAF-2Fb; (f) Coordination modes change as *CO/*CO-*CO intermediate binding for PD-Cu, BD-Cu, LM-Cu, and TM-Cu sites[56] (Copyright 2024 Wiley-VCH GmbH)

Figure 12. (a) Diagram of the phase transformation from Cu-btca-c; ECRR product distributions on (b) Cu-btca-s and (c) Cu NPs at different current densities[109] (Copyright 2024 American Chemical Society); (d) channels in the framework and the 3D framework of compound 1; The products selectivity of ECRR for compound 1 (e) in 0.5 mol/L NaCl electrolyte and (f) in treated natural seawater[110] (Copyright 2025 Wiley-VCH GmbH)

Figure 13. Perspective drawings of the structures for (a) 1 and (b) 2[111] (Copyright 2025 American Chemical Society); (c) schematic representation of the intralayer structure for Cu(4-pt); (d) interlayer stacking pattern of Cu(4-pt)[113] (Copyright 2025 Elsevier); (e) schematic illustration of the synthesis for Cu-MMT nanostructures with different exposed facets; Product distributions of (f) Cu-MMT-H2O and (g) Cu-MMT-IPA at different potentials[115] (Copyright 2024 American Chemical Society)

Figure 14. (a) Schematic diagram of the synthesis of Cu-N2O2 and Cu-N2O3; (b) schematic pathway of CO2 to C2 products on Cu-N2O2[116] (Copyright 2025 Wiley-VCH GmbH); (c) crystal construction strategy of 2D AgCe-MOF and 3D AgCe-MOF; (d) distance between the parallel pyridine rings and the distance between the centers of mass of six-membered rings of 2D AgCe-MOF; (e) intralayer π-π interactions of 2D AgCe-MOF; (f) nyquist plots and (g) charging current density at different rates of the 2D AgCe-MOF nanosheet and 3D AgCe-MOF; (h) the product of C1 distribution for 2D AgCe-MOF and 3D AgCe-MOF at different potentials[117] (Copyright 2024 American Chemical Society)

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基于含氮杂环配体的金属有机框架材料在电催化CO₂还原中的应用与前景展望^★

Recent Advance and Perspective of Metal-Organic Frameworks Based on Nitrogen-Containing Heterocyclic Ligands for Electrocatalytic CO₂ Reduction^★

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基于含氮杂环配体的金属有机框架材料在电催化CO2还原中的应用与前景展望★