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Review

Advancements in Metal–Organic Framework Materials for Photocatalytic CO2 Reduction

by
Jilong Zheng
1,†,
Xueli Yan
2,*,†,
Xiaojuan Guo
3,*,
Xinyi Wang
2,
Shanfa Tang
1,* and
Maochang Liu
2
1
College of Petroleum Engineering, Yangtze University, Wuhan 430100, China
2
International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
3
Guangdong Provincial Key Laboratory of Multi-Energy Complementary Distributed Energy Systems, Dongguan University of Technology, Dongguan 523808, China
*
Authors to whom correspondence should be addressed.
†
These authors contributed equally to this work.
Catalysts 2025, 15(3), 208; https://doi.org/10.3390/catal15030208
Submission received: 31 January 2025 / Revised: 18 February 2025 / Accepted: 19 February 2025 / Published: 21 February 2025
(This article belongs to the Special Issue Recent Advances in Metal-Organic Framework Catalysts)
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Abstract

:
In recent years, metal–organic frameworks (MOFs) have garnered significant attention as highly efficient catalysts for CO2 photoreduction, owing to their unique electronic configurations and exceptional CO2 adsorption properties. This review provides a comprehensive analysis of recent advancements in the design, synthesis, and application of MOF-based photocatalysts for CO2 reduction. Following a concise overview of the fundamental properties of MOF materials, the review focuses on pure MOFs, highlighting the structural and functional roles of metal clusters and organic ligands. Subsequently, it explores into MOF-based composites, analyzing their compositional design, CO2 uptake capabilities, and photocatalytic efficiency. This review concludes by discussing the current challenges, future opportunities, and potential research directions for MOF photocatalysts in the field of CO2 conversion, offering valuable insights to advance this rapidly progressing field.

1. Introduction

The continuous expansion of human activities and industrialization has led to a substantial increase in CO2 emissions. This rise has significantly exacerbated the greenhouse effect and contributed to global warming [1]. Currently, two primary strategies exist for addressing this issue. The first strategy involves the physical capture and storage of CO2. However, the underground storage component of this process is highly energy-intensive and costly, thereby limiting its current practicality [2,3]. Another approach is to convert CO2 into organic compounds that can serve as raw materials for chemical manufacturing [4,5,6,7,8]. One promising solution to address energy and environmental challenges is the use of clean and renewable solar energy to convert CO2 into valuable chemicals through photocatalysis [9,10,11]. The main challenge associated with CO2 utilization is the strong stability of the C=O bond, which necessitates a significant amount of energy for bond formation and CO2 conversion [12]. Solar energy represents a modern energy source that employs photochemical processes to reduce CO2 emissions. It transforms solar energy into chemical energy, which can be harnessed to produce high-calorific-value chemicals, such as organic acids, alcohols, and olefins [13].
Metal–organic frameworks (MOFs) are porous materials composed of metal nodes and organic ligands that are formed through self-assembly. They are renowned for their unique porosity, synthetic tunability, and the resulting chemical and structural diversity. MOFs are particularly effective in regulating the kinetics and thermodynamics of CO2 adsorption, as well as in photocatalytic reduction [14,15]. There are several reasons why MOFs are employed for photocatalytic CO2 reduction. First, the energy levels of the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) of MOFs are influenced by the selection of organic ligands and metal centers. Notably, there is a significant overlap between the empty d orbitals of the metal center and the LUMO of the organic ligand. When exposed to light, the organic ligand can function as an “antenna” to capture light and generate electrons. These generated electrons are subsequently transferred to the metal center via the ligand. The well-defined coordination structure of MOFs facilitates efficient electron transfer from photoexcited ligands to metal clusters via orbital hybridization, thereby enhancing charge separation. Additionally, the metal nodes play a crucial role in the photocatalytic process [16,17]. MOFs exhibit photocatalytic activity due to their molecular structure, which includes unsaturated metal atoms or organic ligands with catalytic properties. Furthermore, additional active sites can be introduced by functionalizing the MOF structure. The porous architecture of MOFs can accommodate highly active photoreactive metal complexes or dyes, making them an ideal platform for absorption homogenization, catalysis, and heterogeneous catalysis, which facilitates easy separation and recycling [18,19,20]. Finally, the photocatalytic efficiency of MOFs can be enhanced by modifying their organic ligands, metal centers, or morphology [21,22,23,24,25]. Given the diversity of organic ligands and coordination structures at the metal center, an almost limitless variety of MOF structures can be designed.
In this review, we systematically analyze the latest research advancements in MOFs as photocatalysts for the reduction of CO2. To provide a comprehensive understanding of the structural characteristics of MOFs, we present a detailed introduction to the metal clusters and organic linkers that constitute MOF photocatalysts. Additionally, we discuss MOF-based composite photocatalysts, focusing on their composition, CO2 adsorption capabilities, and photocatalytic performance. This analysis offers essential guidance for the development of CO2 reduction photocatalysts utilizing MOFs. Finally, we highlight the challenges and potential areas for further research regarding MOF-based photocatalysts in the context of photocatalytic CO2 reduction.

2. Metal Clusters and Organic Ligands in MOFs

MOFs have the potential to serve as effective, durable, and tunable photocatalysts for the photoreduction of CO2. The properties of MOF photocatalysts are determined by their composition, which significantly influences their photocatalytic performance. Since MOFs are structured as 3D porous materials, the selection of metal clusters and organic linkers is crucial [26,27].

2.1. Metal Clusters

The metal center within the structure of MOFs is regarded as the primary site for their catalytic activity. Transition metal ions are frequently utilized as inorganic clusters in MOFs due to their varied coordination numbers and geometries, which lead to a wide range of MOF structures. One effective strategy to enhance the visible-light absorption capacity and photocatalytic performance of MOFs is to functionalize their metal centers. Metal cluster MOFs not only provide a greater diversity of structural types but also enhance the stability of the material through an increased number of connections [28,29].
The Fe-O clusters facilitate the rapid separation of photogenerated electrons and holes by providing electron-trapping Fe3+ sites. This mechanism suppresses recombination and ensures that a higher proportion of charge carriers participates in CO2 reduction, rather than being lost to recombination. The Fe3+ ions in the Fe-O clusters can trap photogenerated electrons, prolonging their lifespan and enhancing the photocatalytic reaction [16,30]. Wang et al. synthesized NH2-MIL-101(Fe) using a solvothermal method, employing triethanolamine (TEOA) as a sacrificial agent to reduce CO2 to HCOO− [31]. One terminal water molecule coordinated with the Fe center in MIL-101(Fe) can be easily removed, resulting in unsaturated Fe metal sites. These sites can directly adsorb CO2 onto the Fe center, leading to a high CO2 adsorption capacity. As illustrated in Figure 1a, during the photocatalytic reduction of CO2 by MIL-101(Fe), the Fe-O cluster absorbs visible light, generating photogenerated electrons and holes. The electrons then transfer from O2− to Fe3+, subsequently reducing CO2 to HCOO−. Thus, the metal active center serves as the photocatalytic active site that drives the reaction. Furthermore, the dual-channel reaction and the synergistic effect between NH2 and the Fe-O cluster significantly enhance the catalytic performance of NH2-MIL-101(Fe). The new peak at 1253 cm−1 observed in situ via Fourier Transform Infrared Spectroscopy (FTIR) indicates that CO2 was directly adsorbed onto the Fe center (Figure 1b). Sun et al. prepared two Fe-based MOFs with single trinuclear metal clusters but different organic ligands to investigate the structural effects on photocatalytic CO2 reduction performance [32]. The results showed that the CH4 yield of MIL-100(Fe) was 16.5 times higher than that of MIL-101(Fe) under visible-light irradiation. Figure 1c presents a schematic illustration of MIL-100(Fe) and MIL-101(Fe), featuring Fe3O clusters along with BTC and BDC ligands. It was found that modifications to the ligands can influence the electron density surrounding the metal nodes, which serve as the fundamental building blocks of the frameworks. Additionally, a high concentration of Fe3O clusters within MIL-100(Fe) could enhance the migration of photogenerated carriers, thereby improving the efficiency of photocatalytic CO2 reduction. Moreover, density functional theory (DFT) calculations confirmed the most effective reaction pathway for the conversion of CO2 to CH4 catalyzed by MIL-100(Fe). They also revealed the critical role of bridging ligands and Fe3O clusters in modulating charge transfer dynamics and CO2 activation barriers, as illustrated in Figure 1d. Feng et al. synthesized a novel Fe-based MOF composed of Fe3 and carboxyl-functionalized photosensitizers [33]. Figure 2a presents a schematic illustration of the synthesis of Fe3 and Fe2Mn. As depicted in Figure 2b,c, the synthesized catalyst exhibits large pore structures and excellent crystallinity. Notably, the [Ru(bpy)3].2+ photosensitizer (Ru-PS) shown in Figure 2b has a smaller molecular size compared to the MOF pores (PCN-333: ~2.7 nm; PCN-600: ~3.1 nm), ensuring its successful encapsulation within the frameworks. The sharp PXRD peaks of PCN-333 and PCN-600 (Figure 2c) match well with their simulated patterns, confirming minimal structural distortion after Ru-PS loading. The researchers found that the Fe2Mn cluster demonstrated the highest catalytic performance, achieving an average rate of 140.9 μmol h−1 over 6 h (Figure 2d). Furthermore, the photocatalytic performance of the MOFs was inferior to that of the Fe3 clusters, as the structure of the MOFs impeded the mass transfer process.
Zirconium (Zr) clusters are recognized for their unique structures, which are ideal for photocatalytic reactions. The coordination bonds of Zr-carboxylate facilitate the formation of MOFs with a large surface area, improved electronic structure, and adaptable reaction environments. Consequently, Zr-based MOFs have garnered significant attention in the field of photocatalysis [34,35,36]. Li et al. prepared BUT-110 with varying porphyrin contents by utilizing different ligands [37]. Figure 3a illustrates the schematic diagram of ligand selection and the synthesis route for BUT-110 and BUT-109(Zr)-P. The results indicated that BUT-110 exhibited greater chemical stability compared to BUT-109(Zr) (Figure 3b). Specifically, BUT-110-50%-Co demonstrated broad pH tolerance and exceptional performance in photocatalytic CO2 reduction (Figure 3c). This work presents a novel approach to modifying MOFs by adjusting the synthesis method. Mellot-Draznieks et al. synthesized a Zr-based porphyritic MOF-545 by metalating the porphyrin linkers under microwave conditions [38]. In comparison to conventional micron-sized crystals, the photocatalytic performance of MOF-545 (TM) derived nanocrystals (150 nm) was significantly revised enhanced. This improvement was attributed to the higher concentration of catalytic sites available in the solvents.
Doping metal cations into the metal nodes can significantly enhance the catalytic performance of MOFs when optimized for metal selection and doping concentration. Specifically, the metal cations are partially substituted within the MOFs without altering the original backbone structure, thereby introducing catalytically active sites. However, improper doping (e.g., excessive substitution or the selection of incompatible metal choice) can create charge recombination centers or disrupt structural stability, ultimately diminishing photocatalytic activity. Sun et al. prepared NH2-UiO-66 (Zr/Ti) using the post-synthetic exchange method, where controlled Ti doping preserved the MOF framework while minimizing recombination risks. This strategy markedly improved the CO2 reduction capability under visible light. By utilizing TEOA as the electron donor, the system effectively converted CO2 to HCOO− (5.8 mmol mol−1) under visible light, which is 1.7 times higher than that of NH2-UiO-66(Zr) under the same conditions [39]. Its exceptional photocatalytic performance arises from two synergistic effects. The absorption edge of the MOF was redshifted from 265 nm (UV-C) to 365 nm (UV-A) due to the influence of Ti-O clusters. While UV-C (200–280 nm) accounts for less than 1% of solar irradiance, the extended absorption into the UV-A range (315–400 nm, approximately 5% of sunlight) represents a critical advancement toward practical solar-driven applications. Additionally, Ti³+ serves as an electronic intermediate, facilitating electron transfer from the organic ligand 2-amino terephthalic acid (ATA) to the Zr-O clusters for interfacial charge transfer. Upon light activation of ATA, photogenerated electrons transition to the excited state of (Ti3+/Zr4+)6O4(OH)4, where Ti3+ functions as an electron donor, leading to the formation of Ti4+-O-Zr3+. This mechanism highlights the importance of balanced doping—excessive Ti substitution could destabilize the charge transfer pathway, while insufficient doping limits the formation of active sites. To bridge the gap between laboratory studies and real-world applications, future research should focus on further extending light absorption into the visible range (>400 nm). Strategies such as ligand functionalization (e.g., incorporating conjugated moieties) or co-doping with narrow-bandgap metals (e.g., Fe, Cu) could enhance solar energy utilization, as demonstrated in recent studies [40,41].
In addition to Fe and Zr, numerous other metallic elements can be utilized to prepare MOFs for photocatalytic CO2 reduction [42,43,44]. NH2-MIL-125(Ti) is a representative Ti-based MOF that is widely employed as a photocatalyst for CO2 reduction due to its abundant active sites, large surface area, and excellent porosity [45]. Utilizing the covalent strategy of imine condensation, Pang et al. designed a novel type of Ti-MOF by carefully selecting aldehyde ligands, as illustrated in Figure 4a [46]. They discovered that the incorporation of the aldehyde ligand narrowed the band gap of the Ti-MOF and shifted the conduction band negatively, thereby enhancing its photocatalytic performance (Figure 4b–e). Consequently, the Ti-MOF exhibited significantly higher photocatalytic CO2 reduction efficiency compared to that of MOF-902 (Figure 4f,g). Wang et al. employed an in situ covalent bonding strategy to incorporate single-point Ru-N2 into a conjugated covalent triazine framework, achieving an impressive selectivity of 98.5% for the photoreduction of CO2 to formic acid [47]. They discovered that the single-point Ru-N2 unit could effectively activate CO2, while the Ru-N2 unit with H2O substitution served as an efficient active center for photocatalysis. Li et al. reported that dimethyl sulfide (DMSP) in the single-site forms of Cu and Ni was integrated into a MOF within a flexible microenvironment, resulting in the formation of MOF-808-CuNi. This integration enhanced the selectivity for CH4 production to as high as 99.4% [48]. The flexible adaptive DMSPs stabilized various C1 intermediates during multi-step basic reactions, thereby facilitating a highly selective conversion of CO2 to CH4. Additionally, Li et al. developed a novel two-dimensional NiZrCu-BDC nanosheet photocatalyst with an average thickness of approximately 4 nm [49]. The NiZrCu-BDC nanosheet demonstrated the ability to reduce CO2 to methanol (41.05 μmol h−1 g−1) and ethanol (36.62 μmol h−1 g−1) under solar light irradiation. The incorporation of Zr and Cu into Ni enhanced the surface charge of Ni, thereby accelerating the chemical adsorption of CO2. The ultra-thin structure reduced the electron transfer distance. Furthermore, the presence of Cu and Zr increased the electron density at the Ni catalytic sites in NiZrCu-BDC, promoting the formation of COOH* and CHO, which are considered key intermediates for the generation of liquid products in the CO2 reduction reaction.

2.2. Organic Ligands in MOFs

The functions of organic ligands in the structure of MOFs include (i) maintaining the stability of the skeletal structure, (ii) providing catalytic sites, and (iii) capturing light. In MOF structures, organic ligands can absorb light at specific wavelengths. Consequently, the direct utilization of functionalized or photoactive organic ligands can simultaneously modify their absorption wavelength and intensity, thereby broadening the light absorption capabilities of MOF materials to include visible- and even infrared-light wavelengths [50,51,52]. The incorporation of amino modifications in organic ligands can extend the range of solar light absorption, enabling MOF materials to capture light in the visible and infrared regions, which enhances their photocatalytic activity. Numerous studies have demonstrated that NH2 modification can improve the CO2 adsorption capacity, solar light absorption, and photocatalytic CO2 reduction performance of MOFs [53].
Defect engineering is a promising strategy for enhancing the photocatalytic performance of MOFs. Fu et al. employed concentrated hydrochloric acid as a modulator to synthesize a series of defective NH2-UiO-66(Zr) by adjusting the synthesis temperature [54]. After 10 h of illumination, Zr-MOF-473K demonstrated the ability to convert CO2 into formic acid with an efficiency of 129.8 mmol gcat−1 h−1. This efficiency is attributed to HCl acting as an intermediate that mitigates the proton effect. As the temperature increases, it becomes advantageous to compete with ATA in binding metal clusters to form inherent defects. The creation of these defects can alter the environment surrounding the Zr atoms, reduce the number of vacant d orbitals, enhance carrier migration, and subsequently improve photocatalytic performance. Li et al. developed an -NH2 modified carbon framework-decorated Cu2O (NH2-C@Cu2O) photocatalyst through a low-temperature carbonization process, as illustrated in Figure 5a [55]. The amorphous carbon formed through thermal treatment with organic ligands not only accelerates electron transfer but also enhances the stability of Cu2O, thereby preventing photo-corrosion. The -NH2 component in photocatalysts interacts strongly with CO2, which increases the chemical adsorption capacity for CO2. Furthermore, compared to Cu2O, NH2-C@Cu2O exhibits higher selectivity in reducing CO2 to HCOOH, resulting in a threefold increase in HCOOH yield (Figure 5b–e). In situ FTIR analysis (Figure 5b–d) elucidated the mechanistic basis for this selectivity. For pristine Cu2O (Figure 5b), illumination generated multiple intermediates, including monodentate carbonate (m-CO32−, 1307–1520 cm−1), bidentate carbonate (b-CO32−, 1158–1589 cm−1), bicarbonate (HCO3−, 1417–1650 cm−1), and HCOO− (1748 cm−1). However, competing intermediates such as CHO (1070 cm−1) and CH3O− (1102 cm−1) were also observed, which reduced the selectivity for HCOOH. In contrast, NH2-C@Cu2O (Figure 5d) exhibited a clean pathway: adsorbed HCO3− (1329 cm−1) under dark conditions rapidly converted to HCOO− (1732–1749 cm−1) upon illumination, with no detectable side intermediates. The sharp peak for formic acid at 1716 cm−1 further confirmed efficient protonation and desorption of HCOO−. This is in contrast to C@Cu2O (Figure 5c), where residual formaldehyde intermediates (CHO−, 1462 cm−1) persisted, highlighting the critical role of the -NH2 group in suppressing parasitic pathways and directing selectivity toward HCOOH.
Transition metal bipyridine complex photosensitizers exhibit high selectivity and activity for the photoreduction of CO2; however, they are susceptible to decomposition under light conditions [56]. To enhance their stability, these photosensitizers can be integrated into MOFs. Specifically, MOF-253, which contains Al(OH)(dcbpy), incorporates 2,2′-bipyridine units that can be utilized in conjunction with metal centers to develop active porous photocatalysts. Sun et al. synthesized MOF-253-Ru(CO)2Cl2 by loading MOF-253 with a Ru complex [57]. The high activity of MOF-253-Ru(CO)2Cl2 is attributed to its efficient charge carrier separation. Upon absorbing visible light, the photogenerated electrons undergo metal-to-ligand charge transfer (RuII → bipyridine π*), which is quenched by TEOA, leading to the formation of a single-electron reduced species. Additionally, organic ligands can function as molecular catalyst carriers, facilitating the assembly of multiple active groups.
The porphyrin network is a typical electron-rich conjugated linker, consisting of four pyrrole rings connected by methine groups [58,59,60]. The pyrrole ring in porphyrins features a unique macrocyclic cavity, a large aromatic structure that facilitates strong interactions with CO2. Porphyrins can enhance the light absorption of MOFs across the entire visible spectrum. Porphyrin-based molecular materials hold significant potential for applications in the capture and conversion of CO2. Metal ions can be introduced into the porphyrin center to participate in photocatalytic reactions. For example, copper porphyrins based MOFs can be utilized for CO2 reduction. Sadeghi et al. employed 4-carboxyphenyl porphyrin (TCPP) as an organic ligand to synthesize Zn/PMOF with a particle size exceeding 200 nm through a solvothermal method [61]. This type of MOFs can reduce CO2 to CH4 under UV-Vis light irradiation. Due to the high polarity of H2O, it competes with CO2 for adsorption. Upon adsorption and under UV-Vis light irradiation, electrons are initially excited from the HOMO of Zn/PMOF molecules to LUMO, creating an excited intermediate and generating electrons and holes, thereby initiating the reaction. Photogenerated holes oxidize H2O to produce H+, OH−, and O2, while the electrons interact with the adsorbed CO2, reducing it to anionic radicals to form CH4. Lu et al. prepared a porphyrin-modified porous x-TA/C-ZCF photocatalyst (TA—meso-tetra (4-carboxyphenyl) porphyrin aminated with (3-aminopropyl) triethoxysilane; C-ZCF—carbonized ZnCo-ZIF-L/CN Foam) for CO2 photocatalytic reduction, as shown in Figure 6a [62]. The prepared photocatalysts also demonstrated a strong CO2 adsorption capacity (Figure 6b,c). The TCPP porphyrin molecules grafted onto the photocatalyst not only broadened the light absorption range of the photocatalyst but also promoted the separation and migration of photogenerated carriers, leading to excellent CO2 photocatalytic reduction performance.
Incorporating metals into the organic chains of MOFs can significantly enhance CO2 adsorption capacity and facilitate efficient carrier separation. Fei et al. embedded a manganese bipyridine complex Mn(bpydc)-(CO)3Br (where bpydc refers to 5,5-dicarboxylate-2,2-dipyridine) into a Zr-MOF to prepare UiO-67-Mn(bpy)(CO)3Br using the thermal solvent method. This approach achieved the metallization of organic chains, enabling the framework to function as a CO2 reduction photocatalyst [63]. The roles of MOFs include the following: (i) the structural pillars provide independent active sites that inhibit the mono-reduced Mn complex, (ii) they offer a large cavity for CO2 storage, and (iii) upon excitation by visible light, the photogenerated Ru(II) electrons are transferred to Mn, with the large cavity (1–2.3 nm) of UiO-67 enhancing carrier separation efficiency. Duan et al. prepared a Cu-MOF photocatalyst by introducing Cu2+ into the defective UiO-66-NH2 framework, which was utilized to reduce CO2 to acetone, as illustrated in Figure 7a,b [64]. The Cu-MOF photocatalyst achieved a CO2 conversion rate of 70.9 μmol gcat−1 h−1, with an overall rate efficiency of 97.1% (Figure 7c). DFT theoretical calculations indicated that the coupling process of *CO*CH3 was easier than *CO*CO coupling, ultimately leading to the formation of CH3COCH3 (Figure 7d).

3. MOF-Based Composites for Photocatalysts

Accelerating the separation and transfer of photogenerated carriers is crucial for improving the efficiency of photocatalytic CO2 reduction. When MOFs are combined with other photocatalysts, they can form heterojunctions or electron capture sites within the composites. These structures facilitate the transfer of photogenerated electrons between different photocatalysts, leading to more efficient charge separation and enhanced selectivity. The photocatalytic performance of MOF-based composite photocatalysts can be significantly improved by incorporating semiconductors, metals, or photosensitizers into the MOFs. Combining semiconductor photocatalysts with CO2 reduction capabilities with MOF materials that exhibit exceptional CO2 capture properties is an effective strategy for creating composite photocatalysts that leverage the strengths of both materials [65,66,67].

3.1. Metal Oxides

Metal oxides have rapidly advanced in the field of CO2 reduction due to their exceptional redox capabilities and chemical stability [68,69,70]. Recently, Petit et al. synthesized titanium dioxide nanofibers and subsequently grew MOF particles on the surface of these fibers in situ to optimize effective charge transfer, as illustrated in Figure 8a,b [71]. The detailed analysis of the structure, light absorption, and charge carrier dynamics in the composites confirmed the interfacial charge transfer across the heterojunction. Furthermore, it was demonstrated that the MOF induces significant band bending in anatase TiO2, leading to enhanced charge separation as electrons migrate from TiO2 to the MOF (Figure 8c). MOFs with 2D structures have attracted considerable interest for photocatalytic applications due to the abundance of active sites on their surfaces. Tian et al. synthesized ultra-thin MIL-125(Ti) nanosheets with a thickness of 1.3 nm and assembled zinc phthalocyanine tetra-carboxylic acid (ZnTcPc) molecules onto these nanosheets, forming a MIL-125(Ti)NS/ZnTcPc S-type heterojunction through strong interactions [72]. The introduction of ZnTcPc significantly broadened the light absorption spectrum and enhanced charge separation. Experiments, combined with DFT calculations, confirmed that the heterojunction promoted CO2 adsorption and reduced the formation energy of intermediates, resulting in a high CO evolution rate of 450.8 µmol g−1 h−1. Jing et al. prepared a Ni@MOF/BiVO4 (BVO) 2D heterojunction via a hydrogen-bonding-induced assembly process [73]. The heterojunction exhibited remarkable efficiency, achieving approximately 66 times greater CO2 conversion compared to BVO nanoparticles, with nearly 100% selectivity for CO. The remarkable photoactivity was attributed to the advantageous S-scheme, which facilitated charge transfer from BVO to the MOF and subsequently to the Ni(II) sites. In particular, the hydroxyl groups in carboxylic compounds could form hydrogen bonds with CO2 to enhance its adsorption on the Ni(II) sites and could also provide protons to facilitate the reduction of CO2. Peng et al. synthesized a novel single-atom CoN cluster–decorated TiO2 (CoNx/TiO2) composite photocatalyst by immersing MIL-125 in a solution of cobalt (4-pyridyl) porphyrin (CoPy), followed by calcination, as illustrated in Figure 9a [74]. This composite demonstrated a high photocatalytic performance for CO2 reduction, achieving CO yields of 24.4 μmol g−1 h−1, which is more than 10 times higher than that of TiO2 (Figure 9b,c). The study revealed that CoPy molecules infiltrated the micropores of MIL-125, facilitating the thermal decomposition of CoPy into single-atom CoN clusters, which formed strong interactions with TiO2 nanoparticles. Consequently, the CoN/TiO2 photocatalyst exhibited efficient charge carrier separation, enhanced chemical adsorption of reactants, and high atomic utilization efficiency.

3.2. Sulfides

Sulfides are well-known compounds that function as semiconductors responsive to visible light. They possess a moderate band gap, and their electrical conductivity increases with the intensity of incident light. When cross-linked with MOF components, these photocatalysts play a crucial role in the photocatalytic CO2 reduction [75,76,77,78]. Ho et al. assembled CdS quantum dots into a porous framework derived from MOFs using a ligand grafting method to achieve efficient photocatalytic CO2 reduction [79]. The combination of CdS and Co3O4-derived Prussian blue analogues facilitates the formation of high-density heterojunctions, resulting in enhanced charge separation. Consequently, the heterojunction exhibited a high photocatalytic CO2 reduction performance, with a CO production rate of 73.9 µmol g−1 h−1. Co9S8 exhibits a narrow band gap and an abundance of surface Co atoms, which provide sufficient active reaction sites for catalysis. Xu et al. prepared a composite photocatalyst (UiO-66/Co9S8) by dispersing Co9S8 onto a UiO-66 substrate, successfully achieving infrared light-driven CO2 reduction [80]. Co9S8 imparted excellent infrared light absorption capabilities to UiO-66/Co9S8, while UiO-66 significantly enhanced the CO2 adsorption capacity. As a result, UiO-66/Co9S8 achieved a CH4 yield rate of up to 25.7 µmol g−1 h−1, with a selectivity of approximately 100% under infrared light conditions. Li et al. designed a novel core–shell structured CoS/NC@ZnS/NC heterojunction using a controlled process of carbonization and sulfidation, as shown in Figure 10a [81]. In comparison to Co3S4/NC and ZnS/NC, the Co3S4/NC@ZnS/NC catalyst demonstrated superior photocatalytic activity in converting CO2 into CO and C2H4 under visible-light irradiation (Figure 10b–d). Experiments and DFT calculations confirmed that ZnS/NC in the heterojunctions provided a feasible channel for electron transport, enhancing the separation and transfer of charge carriers. Furthermore, Co and Zn acted as adsorption sites, promoting the activation of CO and reducing the energy barrier for COOH* formation (Figure 10e–g). ZnIn2S4 has exhibited excellent photocatalytic performance for CO2 reduction due to its suitable band structure and ability to respond to visible light. To prevent the recombination of photogenerated carriers, Huo et al. constructed a ZnIn2S4/MOF-808 S-scheme heterostructure by growing MOF-808 on the ZnIn2S4 surface via a simple hydrothermal method [82]. The designed heterojunction accelerated electron transport and shortened the transfer path. The CO yield of ZnIn2S4/MOF-808 reached 8.21 μmol g−1 h−1, which was 10 times and 8 times higher than that of ZnIn2S4 and MOF-808, respectively.

3.3. Perovskites

Perovskites have been recognized as effective semiconductor photocatalysts due to their exceptional photoelectronic properties, including broad absorption capabilities, tunable band structures, and extended charge diffusion distances [83,84,85]. Combining perovskites with MOFs is an effective strategy to enhance the separation of electrons and holes, thereby promoting reaction kinetics [86,87]. Previous studies have demonstrated that CsPbBr3 exhibits improved CO2 reduction performance when combined with ZIF and UiO MOFs as cocatalysts [88,89]. Bai et al. developed an Ni based MOF(NMF) cocatalyst, which not only improved the separation of electrons and holes but also facilitated the activation of CO2 molecules in the photocatalytic process [90]. Wang et al. prepared a new composite photocatalyst by integrating perovskite and MOF structures, where the Pb could be coordinated with ligands to form a bimetallic MOF, as shown in Figure 11a [91]. The ZIF-8@CsPbBr3 photocatalyst had an average particle size of approximately 40 nm and a specific surface area of 1325.8 m2 g−1, which improved the CO2 adsorption capacity and the photocatalytic efficiency (Figure 1b–d). Lu et al. encapsulated CH3NH3PbI3 (MAPbI3) quantum dots (QDs) within the pores of an iron porphyrin-based MOF through a deposition method, constructing a series of MAPbI3@PCN-221 (Fex) composite (where x = 0 to 1) for photocatalytic applications [92]. The MOF provided protection, significantly enhancing the durability of the composite photocatalyst. The QDs were strategically positioned near the Fe active sites within the MOF, facilitating rapid electron transfer from the QDs to the iron catalytic sites, which in turn improved the photocatalytic performance for CO2 reduction. Consequently, MAPbI3@PCN-221(Fe0.2) achieved a total yield of 1559 μmol g−1 for photocatalytic CO2 reduction, which is 38 times higher than that of PCN-221(Fe0.2). Su et al. designed a ternary CsPbBr3/Au/PCN-333(Al) composite photocatalyst, which has demonstrated a high loading capacity for nanocrystals, charge separation, and excellent adsorption ability [93]. The interaction between and Au nanoparticles could facilitate the transfer of electrons from CsPbBr3 to Au, effectively suppressing charge recombination and accelerating the CO generation. Therefore, the composite photocatalyst demonstrated a significantly enhanced performance in CO2 reduction, achieving 100% selectivity for CO.

4. Summary and Outlook

Recent advancements have significantly accelerated the development of MOFs as photocatalysts for CO2 reduction. Key factors influencing their photocatalytic efficiency include enhanced light absorption, increased reactive sites, improved CO2 adsorption rates, and efficient charge carrier separation. Compared to traditional photocatalysts, MOF-based alternatives offer distinct advantages. Firstly, their highly porous structure facilitates exceptional CO2 adsorption. Secondly, the catalytic sites in MOF photocatalysts can be precisely engineered by manipulating metal clusters and organic ligands. Thirdly, through the strategic design of metal clusters and organic linkers, MOF-based photocatalysts exhibit broadened light absorption spectra, thereby capturing a larger fraction of incident photons. However, the effective utilization of these photons—quantified by photonic efficiency (the ratio of the target reaction rate to the photon flux incident on the catalyst)—also requires minimizing charge recombination and optimizing interfacial electron transfer processes. Lastly, their straightforward synthesis under mild conditions makes MOF photocatalysts ideal for the production of various composite photocatalysts.
However, challenges persist. Current MOFs photocatalysts exhibit limited efficiency in CO2 reduction and face stability issues in aqueous environments, which can lead to permanent deactivation during prolonged catalytic processes. Addressing these drawbacks necessitates the development of highly stable MOFs specifically designed for sustained exposure to water. Despite significant advancements, practical applications remain elusive. To enhance efficiency, innovative strategies are essential. The incorporation of cocatalysts with single metal atoms shows promise for maximizing the utilization of active sites. Additionally, ultra-thin 2D MOF nanosheets, which feature abundant surface metal sites, present a promising avenue for CO2 photocatalysis. Furthermore, leveraging advanced simulation and in situ characterization techniques can elucidate the complex reaction mechanisms of MOF-based photocatalysts.

Author Contributions

The project was conceived and supervised by X.Y., X.G., S.T. and M.L. Manuscript writing and revisions were managed by J.Z., X.Y., X.G., X.W. and M.L. All authors contributed to the discussion of results and the development of manuscript. All authors have read and agreed to the published version of the manuscript.

Funding

The authors are grateful for the generous financial support by the China Fundamental Research Funds for the Central Universities.

Conflicts of Interest

The authors declare no conflicts of interest.

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Figure 1. (a) Schematic diagram of the photocatalytic process for Fe-Based MOF photocatalysts. (b) In situ infrared spectrum of MIL-101(Fe). Reproduced with permission [31]. Copyright 2014, American Chemical Society. (c) Structural diagram of MIL-100(Fe) and MIL-101(Fe). (d) Relative energy of MIL-100(Fe) and MIL-101(Fe) for photocatalytic reduction CO2-to-CH4. * The active surface sites for adsorption and reaction. Reproduced with permission [32]. Copyright 2020, The Royal Society of Chemistry.
Figure 1. (a) Schematic diagram of the photocatalytic process for Fe-Based MOF photocatalysts. (b) In situ infrared spectrum of MIL-101(Fe). Reproduced with permission [31]. Copyright 2014, American Chemical Society. (c) Structural diagram of MIL-100(Fe) and MIL-101(Fe). (d) Relative energy of MIL-100(Fe) and MIL-101(Fe) for photocatalytic reduction CO2-to-CH4. * The active surface sites for adsorption and reaction. Reproduced with permission [32]. Copyright 2020, The Royal Society of Chemistry.
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Figure 2. (a) Synthesis process diagram of Fe3. (b) Chemical structures of PCN-333, PCN-600, and Ru PS. (c) XRD patterns of PCN-333 and PCN-600. (d) Photocatalytic activity of different photocatalysts for CO2 reduction. Reproduced with permission [33]. Copyright 2023, American Chemical Society.
Figure 2. (a) Synthesis process diagram of Fe3. (b) Chemical structures of PCN-333, PCN-600, and Ru PS. (c) XRD patterns of PCN-333 and PCN-600. (d) Photocatalytic activity of different photocatalysts for CO2 reduction. Reproduced with permission [33]. Copyright 2023, American Chemical Society.
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Figure 3. (a) Schematic diagram of ligand selection and synthesis route for BUT-110 and BUT-109(Zr)-P. (b) Photocatalytic CO2 reduction performance of BUT-110-50%-Ni, BUT-110-50%-Fe, BUT-110-50%-Cu, and BUT-110-50%-Co. (c) Productions of CO and CH4 obtained from CO2 photoreduction over BUT-110-50%-Co catalyst in five cycles. Reproduced with permission [37]. Copyright 2021, Wiley-VCH.
Figure 3. (a) Schematic diagram of ligand selection and synthesis route for BUT-110 and BUT-109(Zr)-P. (b) Photocatalytic CO2 reduction performance of BUT-110-50%-Ni, BUT-110-50%-Fe, BUT-110-50%-Cu, and BUT-110-50%-Co. (c) Productions of CO and CH4 obtained from CO2 photoreduction over BUT-110-50%-Co catalyst in five cycles. Reproduced with permission [37]. Copyright 2021, Wiley-VCH.
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Figure 4. (a) Synthesis route schematic diagram of Ti-MOFs. Mott–Schottky curve of (b) Tc, (c) Ti-MOF, and (d) MOF-902. (e) Band structures of Ti-MOF and MOF-902. (f,g) Photocatalytic performance of different photocatalysts. Reproduced with permission [46]. Copyright 2019, Elsevier.
Figure 4. (a) Synthesis route schematic diagram of Ti-MOFs. Mott–Schottky curve of (b) Tc, (c) Ti-MOF, and (d) MOF-902. (e) Band structures of Ti-MOF and MOF-902. (f,g) Photocatalytic performance of different photocatalysts. Reproduced with permission [46]. Copyright 2019, Elsevier.
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Figure 5. (a) Synthesis route diagram of NH2-C@Cu2O photocatalyst. (b) In situ FTIR spectra of Cu2O. (c) C@Cu2O and (d) NH2-C@Cu2O. (e) Photocatalytic performance of different photocatalysts. Reproduced with permission [55]. Copyright 2021, Elsevier.
Figure 5. (a) Synthesis route diagram of NH2-C@Cu2O photocatalyst. (b) In situ FTIR spectra of Cu2O. (c) C@Cu2O and (d) NH2-C@Cu2O. (e) Photocatalytic performance of different photocatalysts. Reproduced with permission [55]. Copyright 2021, Elsevier.
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Figure 6. (a) Schematic diagram of the CO2 adsorption process on photocatalysts. (b) Thermal conductivity signals and (c) CO2 adsorption isotherms of different photocatalysts. (d–f) Photocatalytic performance of different photocatalysts. Reproduced with permission [62]. Copyright 2023, Elsevier.
Figure 6. (a) Schematic diagram of the CO2 adsorption process on photocatalysts. (b) Thermal conductivity signals and (c) CO2 adsorption isotherms of different photocatalysts. (d–f) Photocatalytic performance of different photocatalysts. Reproduced with permission [62]. Copyright 2023, Elsevier.
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Figure 7. (a) Synthesis process schematic diagram of Cu-MOF photocatalyst. (b) Photocatalytic performance of different photocatalysts. (c) Schematic diagram of CuN2O2 active sites reducing CO2 to acetone. (d) Free energy diagram of Cu-MOF photocatalyst for photocatalytic CO2 reduction. * The intermediate and active species. Reproduced with permission [64]. Copyright 2024, Wiley-VCH.
Figure 7. (a) Synthesis process schematic diagram of Cu-MOF photocatalyst. (b) Photocatalytic performance of different photocatalysts. (c) Schematic diagram of CuN2O2 active sites reducing CO2 to acetone. (d) Free energy diagram of Cu-MOF photocatalyst for photocatalytic CO2 reduction. * The intermediate and active species. Reproduced with permission [64]. Copyright 2024, Wiley-VCH.
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Figure 8. (a) Synthesis process schematic diagram of TiO2/NH2–UiO-66 photocatalyst. (b) Photocatalytic performance of different photocatalysts. (c) Electron transfer pathway of MOF/TiO2 photocatalyst. Reproduced with permission [71]. Copyright 2019, Wiley-VCH.
Figure 8. (a) Synthesis process schematic diagram of TiO2/NH2–UiO-66 photocatalyst. (b) Photocatalytic performance of different photocatalysts. (c) Electron transfer pathway of MOF/TiO2 photocatalyst. Reproduced with permission [71]. Copyright 2019, Wiley-VCH.
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Figure 9. (a) Schematic diagram of Synthesis route for CoNx/TiO2. (b) CO/CH4 yields and (c) total consumed electron number of different photocatalysts. Reproduced with permission [74]. Copyright 2024, Elsevier.
Figure 9. (a) Schematic diagram of Synthesis route for CoNx/TiO2. (b) CO/CH4 yields and (c) total consumed electron number of different photocatalysts. Reproduced with permission [74]. Copyright 2024, Elsevier.
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Figure 10. (a) Schematic diagram of synthesis route for Co3S4/NC@ZnS/NC. (b) Photocatalytic rates and (c) product selectivity of different photocatalysts. (d) Gas chromatography–mass spectrometry analysis of products for Co3S4/NC@ZnS/NC. DFT calculations of the energy barrier for COOH* of (e) Co3S4/NC, (f) ZnS/NC, and (g) Co3S4/NC@ZnS/NC. Reproduced with permission [81]. Copyright 2024, Elsevier.
Figure 10. (a) Schematic diagram of synthesis route for Co3S4/NC@ZnS/NC. (b) Photocatalytic rates and (c) product selectivity of different photocatalysts. (d) Gas chromatography–mass spectrometry analysis of products for Co3S4/NC@ZnS/NC. DFT calculations of the energy barrier for COOH* of (e) Co3S4/NC, (f) ZnS/NC, and (g) Co3S4/NC@ZnS/NC. Reproduced with permission [81]. Copyright 2024, Elsevier.
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Figure 11. (a) Schematic diagram of synthesis route for ZIF-8@CsPbBr3. (b) Transmission electron microscope images of ZIF-8-Pb and ZIF-8@CsPbBr3. (c) Photocatalytic rates of CsPbBr3 and ZIF-8@CsPbBr3. (d) Stability of the ZIF-8@CsPbBr3. Reproduced with permission [91]. Copyright 2024, Wiley-VCH.
Figure 11. (a) Schematic diagram of synthesis route for ZIF-8@CsPbBr3. (b) Transmission electron microscope images of ZIF-8-Pb and ZIF-8@CsPbBr3. (c) Photocatalytic rates of CsPbBr3 and ZIF-8@CsPbBr3. (d) Stability of the ZIF-8@CsPbBr3. Reproduced with permission [91]. Copyright 2024, Wiley-VCH.
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MDPI and ACS Style

Zheng, J.; Yan, X.; Guo, X.; Wang, X.; Tang, S.; Liu, M. Advancements in Metal–Organic Framework Materials for Photocatalytic CO2 Reduction. Catalysts 2025, 15, 208. https://doi.org/10.3390/catal15030208

AMA Style

Zheng J, Yan X, Guo X, Wang X, Tang S, Liu M. Advancements in Metal–Organic Framework Materials for Photocatalytic CO2 Reduction. Catalysts. 2025; 15(3):208. https://doi.org/10.3390/catal15030208

Chicago/Turabian Style

Zheng, Jilong, Xueli Yan, Xiaojuan Guo, Xinyi Wang, Shanfa Tang, and Maochang Liu. 2025. "Advancements in Metal–Organic Framework Materials for Photocatalytic CO2 Reduction" Catalysts 15, no. 3: 208. https://doi.org/10.3390/catal15030208

APA Style

Zheng, J., Yan, X., Guo, X., Wang, X., Tang, S., & Liu, M. (2025). Advancements in Metal–Organic Framework Materials for Photocatalytic CO2 Reduction. Catalysts, 15(3), 208. https://doi.org/10.3390/catal15030208

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