Single Metal-organic Framework Research Articles

Recent research progress of MOFs-based heterostructures for photocatalytic hydrogen evolution

The growing serious energy crisis and environmental pollution expedite the development of green hydrogen energy. Photocatalytic water splitting technology, converting solar energy into chemical energy directly, provides a clean and economical way for hydrogen evolution. For the past few years, metal–organic frameworks (MOFs) semiconductor materials have become a research hotspot in the field of photocatalytic hydrogen evolution (PHE) due to their multiple advantages, including adjustable structure, high porosity, large specific surface area, abundant active sites, and so forth. Besides this, the construction of heterogeneous structures based on MOFs materials can further improve PHE performance through the effective internal electric field directional transfer of photogenerated electrons and the superior utilization rate of sunlight in comparison to the single MOFs photocatalyst. Herein, in this minireview, we summed up the varieties of synthesis methods of diverse types of MOFs heterojunction complex materials, discussed the H2 evolution efficiency based on this heterostructure photocatalyst in detail, and lastly proposed the advantages, limitations, and outlook of MOFs composites in the PHE field. We sincerely hope this review can provide a reference for future research based on MOFs materials for alleviating the current energy crisis.

Development of a Multiparticulate Metal-Organic Framework/Textile Fiber Swatch.

The versatility of metal-organic frameworks (MOFs) has led to groundbreaking applications in a wide variety of fields, especially in the areas of energy, environment, and sustainability. For example, MOFs can be designed for high uptake of toxic gases and pollutants, such as CO2, NH3, and SO2, but designing a single MOF that shows tangible uptake for all of these gases is challenging due to the differences in the chemical and physical properties of these molecules. To this end, integrating multiple MOFs onto textile fibers and crafting various structures have emerged as pivotal developments, enhancing framework durability and usability. MOF composites prepared on readily available textile fibers offer the flexibility essential for critical applications, including heterogeneous catalysis, chemical sensing, toxic gas adsorption, and drug delivery, while preserving the unique characteristics of MOFs. This study introduces a scalable and adaptable method for seamlessly embedding multiple high-performing MOFs onto a single textile fiber using a dip-coating method. We explored the uptake capacity of these multi-MOF composites for CO2, NH3, and SO2 and observed a performance similar to that of traditional powdered materials. Along with harmful gas adsorption, we also have evaluated the permeation and reactivity of these MOF/textile composites toward chemical warfare agents (CWAs) like GD (soman), HD (mustard gas), and VX. In combination, these results demonstrate a fundamental advancement toward establishing a consistent strategy for the hydrolysis of nerve agents in real-world scenarios. This approach can substantially increase the protection toward CWAs and enhance the effectiveness of protective equipment such as fabrics for protective garments. This dip-coating method for the integration of multiple MOFs on a single textile fiber unlocks a wealth of possibilities and paves the way for future innovations in the deployment of MOF-based composites.

Boosting capacitive performance of electrode material by facile incorporation of phthalic acid ligand-based bimetallic MOF for supercapacitors

The bimetallic approach can offer a synergistic effect and energy-efficient metal-organic frameworks (MOFs) based electrode materials for electrochemical applications. The interconnected frameworks convert themselves into a two-dimensional conducting stacked structure with the favorable entity of metal ions bonded to metal-ligand covalence. This network prioritizes charge transport within the plane, minimizing the importance of out-plane transport. To achieve this, we propose a straightforward and efficient method for integrating Ni2+ and Co2+ metal ions with 1, 2-benzene dicarboxylic acid (phthalic acid) ligands. By employing this strategy, we can fabricate a bimetallic metal-organic framework electrode using a simple aromatic ligand, thus avoiding the complex synthesis typically associated with MOFs. This specially designed MOF electrode material enhances the electrochemical activities of the selected ligands. The presence of redox-active centers and conductive structure provides excellent behavior of the material with a high performance of 1755 Fg−1 (754.82 Cg−1) at 2 Ag−1. Also, the fabricated asymmetric device delivers (58.25 Whkg−1 energy density and 1299.90 Wkg−1 power density) with only a 9 % reduction in capacitance over 22 K cycles. The strategic design of a bimetallic Ni-Co-based metal-organic framework with bidentate ligand offers the potential to increase the electrochemical activities relative to single metallic MOFs.

Controlling Triboelectric Charge of MOFs by Leveraging Ligands Chemistry.

Metal-organic frameworks (MOFs) have emerged as promising materials for triboelectric nanogenerators (TENGs), but the effects of ligand choice on triboelectric charge remain underexplored. Hence, this paper demonstrates the effect of single, binary, and ternary ligands on TENG performance of cobalt/cerium-based (Co─Ce) bimetallic MOFs utilizing 2-methylimidazole (2Melm), terephthalic acid (BDC), and benzene tricarboxylic acid (BTC) as ligands. The detailed structural characterization revealed that varying ligand chemistries led to distinct MOF features affecting TENG performance. Single ligand bimetallic MOFs (designated as CoCe-2MeIm, CoCe-BDC, CoCe-BTC) has lower performance than binary ligand (designated as CoCe-2MeIm-BDC, CoCe-2MeIm-BTC, CoCe-BDC-BTC) and ternary ligand MOFs (designated as CoCe-2MeIm-BDC-BTC). Among all, the binary ligand MOF, CoCe-2MeIm-BTC, shows the best results (598V, 26.7µA) due to the combined effect of imidazole ring and (─COO─) groups. This is attributed to lone pairs on nitrogen atoms and a delocalized π-electron system in imidazole system in this material. CoCe-BTC has the lowest results (31V, 3.2µA) due to the bulkier nature of the electron-withdrawing (─COO─) groups and their impact on the π-electron system of the benzene ring. This study showcases the potential of ligand chemistry manipulation to control triboelectric charge and thereby enhance MOF-based TENG performance.

Interfacial modification of recombinant protein for immunoglobulin G adsorption with spindle-shaped MOF as nano molecular containers

Development of fresh solid phase extractant is critical for selective separation and purification of special proteins. Herein, we demonstrated a recombinant Staphylococcal Protein G (rSPG) with a His-tag modified the novel single-metal organic framework (rSPG@Ni-MOF-74). The proposed solid-phase extraction material possessed a uniform spindle-shaped structure, large surface area (709.60 m2 g−1) and pore volume (0.08 m3 g−1), high metal content (22.57 wt%), which facilitated the interaction between host and guest. As results, the composite displayed outstanding selective recognition and adsorption of IgG, due to synergistic effect of the binding ability of rSPG with the Fc region of IgG, maintained through hydrogen bonding and electrostatic attraction, as well as hydrophobic interaction. The adsorption performance and mechanism of rSPG@Ni-MOF-74 have been fully investigated. Additionally, the rSPG@Ni-MOF-74 composite could effectively separate IgG from serum obtained from healthy humans, with the purity of the separated IgG verified through SDS-PAGE analysis. Furthermore, LC-MS/MS analysis identified a high content of IgG (55.3 %) in the eluate from rSPG@Ni-MOF-74, suggesting the great potential of rSPG@Ni-MOF-74 in IgG separation and enrichment from complex matrix.

Hierarchical metal–organic framework nanoarchitectures for catalysis

Metal–organic frameworks (MOFs) have garnered significant attention in the field of catalysis due to their unique advantages such as diverse coordination geometry, variable metal nodes, and organic linkers, facilitating precise structural and compositional control for achieving programmable catalytic functionalities. Although their inherent microporous structure could provide excellent shape selectivity during catalysis, it typically impedes the mass transfer process, thereby reducing the use of internal active sites and overall catalytic efficiency. Additionally, employing single MOFs as catalysts presents challenges in achieving complex catalytic reactions that require multifunctional active sites. In recent years, considerable research efforts have focused on designing and constructing hierarchical nanostructured MOFs to alleviate substrate diffusion limitations by introducing secondary nanopores, shortening diffusion distances via the construction of low-dimensional nanoarchitectures, and constructing multifunctional catalysts by integrating distinct MOFs with suitable functions. This review provides a comprehensive overview of the design, synthesis methods, and formation mechanisms of MOF-based hierarchical nanostructures in recent years. Subsequently, it further highlights their applications in thermal catalysis, electrocatalysis, and photocatalysis, along with the relationship between their hierarchical nanostructures and catalytic performances. Finally, it provides an outlook on the challenges and potential development directions of hierarchically structured MOF nanocatalysts.

Active site-tuned high peroxidase-like activity nanozyme for on-the-spot detection of saliva total antioxidant capacity using smartphone devices

Metal-Organic Framework (MOF) based nanozymes with clear structure are beneficial for exploration of structural-performance and exhibit broad prospects in improving activity. In this study, the prepared bimetallic Fe3Ni-MOF nanozyme was superior to single metal MOF in the peroxidase-like activity. Subsequently, a derivative nanozyme (Fe3Ni-MOF-Ar) was prepared by pyrolysis using Fe3Ni-MOF as the precursor in argon atomoshere with controlled temperature. The investigated of Fe3Ni-MOF-Ar revealed that the irregular macroporous state and the presence of heterovalent FeIII/FeII sites of Fe3Ni-MOF-Ar enable the retention, exposure, and electronic structure regulation of active sites, promoting the dual mechanism (the generation of •OH and electron transfer mechanism) and significantly increasing the peroxidase-like activity. Fe3Ni-MOF-Ar exhibited a strong affinity for substrate H2O2, which is higher than horseradish peroxidase. Ascorbic acid and cysteine are typical substances of antioxidants. Fe3Ni-MOF-Ar was used for sensitive colorimetric detection of ascorbic acid and cysteine, and the detection limit was as low as 150 and 60 nM. In addition, the smartphone devices was used to detection of antioxidant equivalent ascorbic acid, with a detection range of 0.5–120 μM. Fe3Ni-MOF-Ar nanozyme is feasible for sensitive detection of saliva total antioxidant capacity.

Copper/cobalt metal-organic framework composites for advanced anode material of lithium-ion battery

In this paper, two new types of metal-organic frameworks (MOFs) materials, namely Cu-IM and Co-MOF, have been successfully applied to the anode of lithium-ion batteries with LiPF6 (EC: DMC = 1:1, volume) electrolyte additive. Cu-IM and Co-MOF employed imidazole (IM) and 2-methylimidazole (2-MeIM) as organic ligands, respectively. The results revealed the synthesized MOFs exhibited high initial discharge specific capacities (Cu-IM: 1964.5 mAh g−1, Co-MOF: 1423.3 mAh g−1) as well as low internal resistances (Cu-IM: 146 Ω; Co-MOF: 236 Ω). To alleviate the issue of capacity decay in single MOFs, we attempted the dual-MOFs materials through the rational design of interfacial/surface properties and microstructure. Compared to Cu-IM, the prepared Cu-IM/Co-MOF composites have a higher specific surface area and pore volume. Furthermore, the charge transfer resistance of Cu-IM/Co-MOF composites (141 Ω) was lower than that of Cu-IM and Co-MOF respectively. After a heat treatment to Cu-IM/Co-MOF composites, the electrochemical performance of obtained Cu-IM/Co-MOF 250 dual-MOFs composites have been significantly improved. The Cu-IM/Co-MOF 250 dual-MOFs composites demonstrated excellent cycling stability and high discharge specific capacities at various current densities. The composites displayed stable discharge specific capacity retention of 834 mAh g−1 (50 mA g−1, 75 cycles), 710.5 mAh g−1 (200 mA g−1, 50 cycles), and 392.5 mAh g−1 (500 mA g−1, 50 cycles), highlighting their promising performance for energy storage applications. The synthesized Cu-IM/Co-MOF 250 dual-MOFs composites demonstrates exceptional cycling performance and rate capability, implying that it has the promising prospects as anode material for lithium-ion batteries.

The reconstruction of equal-mole bimetal organic framework to heterostructure for effective oxygen evolution reaction

Oxygen evolution reaction (OER) is one of the most important issues for hydrogen production from water splitting. During the OER process, electrochemical reconstruction is widely observed for the majority of electrocatalysts, which is strongly related to the formation and evolution of real active species. Herein, bimetal metal-organic framework (MOF) with an equal ratio of Co and Fe sites is screened to exhibit the superior OER property. An obvious reconstruction is observed to transform single MOF phase into the heterostructure composed of active CoOOH and FeOOH. Meanwhile, the generation of Co3+ species is more reliant on the blessing of electricity and electrolyte than that of Fe3+ species. As a result, the optimal electrocatalyst shows the overpotential of 267 mV at 10 mA/cm2 and ultra-low Tafel slope of 24.7 mV/dec with a stable OER performance.

Three-Dimensional Visualization of Adsorption Distribution in a Single Crystalline Particle of a Metal-Organic Framework.

Many unique adsorption properties of metal-organic frameworks (MOFs) have been revealed by diffraction crystallography, visualizing their vacant and guest-loaded crystal structures at the molecular scale. However, it has been challenging to see the spatial distribution of the adsorption behaviors throughout a single MOF particle in a transient equilibrium state. Here, we report three-dimensional (3D) visualization of molecular adsorption behaviors in a single crystalline particle of a MOF by in situ X-ray absorption fine structure spectroscopy combined with computed tomography for the first time. The 3D maps of water-coordinated Co sites in a 100 μm-scale MOF-74-Co crystal were obtained with 1 μm spatial resolution under several water vapor pressures. Through the visualization of the water vapor adsorption process, 3D spectroimaging revealed the mechanism and spatial heterogeneity of guest adsorption inside a single particle of a crystalline MOF.

Synergistic Boosting Capture Ability of Thiophene Sulfur with a Novel Dual-Amino-Functionalized MOF-on-MOF Adsorbent.

A single metal-organic framework (MOF) exhibits some drawbacks in deep adsorptive desulfurization such as insufficient functional active sites, water instability, low surface area, etc. Herein, a dual-amino-functionalized (ZIF-8-NH2)-PVP-(Cu-BTC-NH2) core-shell dual MOF adsorbent was first synthesized by the hydrothermal growth method. The adsorption performance of thiophene sulfur (ThS) is systematically investigated and evaluated at mild temperatures through batch tests. The (ZIF-8-NH2)-PVP-(Cu-BTC-NH2) exhibits good adsorption ability toward ThS, which is attributed to the associative effects of dual MOFs with structure features such as hydrogen bond, open metal active sites, suitable pore sizes and π-π conjugation, etc. Meanwhile, the (ZIF-8-NH2)-PVP-(Cu-BTC-NH2) embedded 25 wt % water still remains crystal intact and good adsorption desulfurization performance, which is attributed to the NH2- functional groups. After five recycles, more than 90% ThS uptake onto (ZIF-8-NH2)-PVP-(Cu-BTC-NH2) could be recovered, exhibiting good reuse performance. This study presents a new strategy for grafting MOF-on-MOF with specific functional groups to improve the abilities of desulfurization and water resistance.

TpBD/UiO-66-NH2 micro-mesoporous hybrid material as a stationary phase for open tubular capillary electrochromatography.

The excellent stability of covalent organic frameworks (COFs) and the diversity of metal organic frameworks (MOFs) make MOF/COF hybrid materials promising candidates for chromatographic stationary phases. In this paper, a TpBD/UiO-66-NH2 hybrid material was synthesized through a Schiff-base reaction between TpBD COFs and UiO-66-NH2 MOFs; characterized using Fourier-transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy; and bonded to a capillary to prepare a TpBD/UiO-66-NH2-bonded open tubular capillary electrochromatography (OT-CEC) column. Results suggested that the hybrid material had the crystal morphology of a single COF and MOF, a micro-mesoporous structure, and good thermal stability. The inner surface of the OT-CEC column was tightly and uniformly distributed with the stationary phase (∼1.5 μm). The baseline separation of 13 amino acids and three families (4 acidic antibiotics, 4 preservatives and 6 sulfonamides) of emerging pollutant mixtures was achieved due to the synergistic effect of TpBD and UiO-66-NH2 in the stationary phase. The OT-CEC column showed good reproducibility and stability with relative standard deviations of migration time and resolutions in the range of 1.17-3.93% and 1.79-4.31%, respectively.

Mitochondria-targeting nanozyme alleviating temporomandibular joint pain by inhibiting the TNFα/NF-κB/NEAT1 pathway.

Inflammatory cytokines that are secreted into the spinal trigeminal nucleus caudalis (Sp5C) may augment inflammation and cause pain associated with temporomandibular joint disorders (TMD). In a two-step process, we attached triphenylphosphonium (TPP) to the surface of a cubic liposome metal-organic framework (MOF) loaded with ruthenium (Ru) nanozyme. The design targeted mitochondria and was designated Mito-Ru MOF. This structure scavenges free radicals and reactive oxygen species (ROS) and alleviates oxidative stress. The present study aimed to investigate the effects and mechanisms by which Mito-Ru MOF ameliorates TMD pain. Intra-temporomandibular joint (TMJ) injections of complete Freund's adjuvant (CFA) induced inflammatory pain for ≥10 d in the skin areas innervated by the trigeminal nerve. Tumor necrosis factor-alpha (TNF-α), nuclear factor kappa-light-chain-enhancer of activated B cells (NF-κB), long non-coding RNA nuclear paraspeckle assembly transcript 1 (lncRNA NEAT1), and ROS also have been proved to be significantly upregulated in the Sp5C of TMD mice. Moreover, a single Mito-Ru MOF treatment alleviated TMD pain for 3 d and downregulated TNF-α, NF-κB, lncRNA NEAT1, and ROS. NF-κB knockdown downregulated NEAT1 in the TMD mice. Hence, Mito-Ru MOF inhibited the production of ROS and alleviated CFA-induced TMD pain via the TNF-α/NF-κB/NEAT1 pathway. Therefore, Mito-Ru MOF could effectively treat the pain related to TMD and other conditions associated with severe acute inflammatory activation.

Heterostructures of NiFe-MOF/PBAs with high-performance supercapacitors obtained by compounding Prussian blue analogues on bimetallic organic frames

Metal organic framework (MOF) is considered as an excellent electrode material for supercapacitors due to its low cost and homogeneous nanostructure, but the drawbacks of single MOF, such as low specific capacity and stability, limit its development, so the design of bimetallic MOF structural composites is a challenging but favourable strategy for the development of supercapacitors. In this paper, NiFe-MOF/PBAs heterostructure, a bimetallic MOF material with a granular rod-like structure, is successfully prepared by using bimetallic MOF as a precursor and introducing [Co(CN)6]3− ions to further convert it into PBAs (Prussian blue analogs). Due to the special macroporous structure of PBAs, the composite combines the advantages of the two MOF materials, and the specific capacity is as high as 4270.19 C g−1 at 1 A g−1. The composite still has excellent electrochemical properties when assembled into devices. The specific capacity is 1996.01 C g−1 at 1 A g−1, the energy density reached 749.99 W h kg−1 at a power density of 415.85 W kg−1, and the decay rate is only 1.14 % after 20,000 cycles at 10 A g−1. These results indicate that the designed dual MOFs composite electrodes have good application prospects in the field of electrochemical energy storage.

Fabrication of Single Metal–Organic Framework Crystal Devices to Inform Energy Conversion Platforms

Fabrication of Single Metal–Organic Framework Crystal Devices to Inform Energy Conversion Platforms

Enhanced Photoinduced Carrier Separation in Fe-MOF-525/CdS for Photocatalytic Hydrogen Evolution: Improved Catalytic Dynamics with Specific Active Sites.

Single-atom metal-anchored porphyrin-based metal-organic frameworks (MOFs) have shown excellent light absorption, catalytic sites, and high stability during photocatalytic reactions, while there are still challenges for facile assembly with quantum dots to enhance catalytic dynamics. Herein, a kind of Fe single atom-doped MOF material (Fe-MOF-525) was ball milled with CdS in a proper ratio through Fe-N4 and Fe-N-C bonding, which showed the enhanced photoinduced carrier separation ability. As a result, extended light absorption ranges of CdS/Fe-MOF-5252.3 induced the promotion of the photocatalytic hydrogen (H2) value (3638.6 μmol g-1 h-1), which was 7.2 and 2.3 times higher than those of Fe-MOF-525 and CdS. In this work, the facile synthetic technique, specific active sites, and enhanced catalytic dynamics in the composite highlight the future research on MOF-based heterojunctions and their potential photocatalysis applications..

Integrating Bi-containing metal–organic frameworks for enhancing their LED visible-light-driven photocatalytic activities towards Rhodamine dye

Tuning metal–organic framework (MOF) properties to enhance their catalytic activities has recently gained considerable attention. In this work, Bi(III) MOFs, including UU-200, CAU-17, and their integrated architecture, namely MIX-UCAU, were effectively prepared and characterized by various techniques, including FE-SEM, XRD, XPS, FT-IR, Raman, TGA, and EIS analyses. Results revealed that the UU-200 and CAU-17 frameworks were effectively integrated into a heterojunction MOF using a mixture of DMF and MeOH. The MIX-UCAU exhibited increased crystallinity, higher oxygen defect concentration and improved light absorption. The combined UU-200-CAU-17 framework also showed enhanced photo-generated electron-hole pairs separation and immigration performance compared to single MOFs. The photodegradation experiments of Rhodamine B dye (RhB) in an aqueous solution showed that the MIX-UCAU had a high photodegradation efficiency of ca. ∼ 99 % within 90 min under energy-saving visible LED light irradiation, surpassing the bare UU-200 (∼81 %) and CAU-17 (∼89 %). In addition, the catalyst showed good photostability under successive cyclic experiments. The LC/MS and radical quenching tests revealed the degradation of RhB, including several steps, including the N-dealkylation, decarboxylation, deamination, and ring cleavages to tiny fragmentation products, and these procedures were predominantly controlled by the active species of O2•– and h+. The study provides a facile and efficient strategy for developing photocatalysts for treating organic pollutants in wastewater.

Direct White-Light Emitting From a Single Metal-Organic Framework with Dual Phosphorescence Peaks.

Single component white-light-emitting (SCWLE) materials are extremely desired in the field of solid-state lighting. However, pure-phosphorescent SCWLE has rarely been reported. Herein, one halogen-bonding-containing MOF [Cd(5-BIPA)(phen)] (1) has been synthesized, which shows efficient white-light emission originating from dual phosphorescence bands with different wavelengths and lifetimes. The fabrication of a phosphor-converted white-light-emitting diode device driven by pulsing current enables this MOF to be a promising phosphor.

Plasma-catalytic removal of toluene over bimetallic M/Mn-BTC catalysts in dielectric barrier discharge reactor

In this study, novel bimetallic metal–organic frameworks (MOFs) catalysts were synthesized using a simple solvothermal method. These catalysts involved the incorporation of transitional metals such as Co, Cu, Ce, and Fe into Mn-BTC, which served as the precursor substrate. This approach was undertaken to address the limitations of catalytic degradation of toluene observed in both plasma-based and traditional catalytic materials. The physicochemical characterization confirmed successful synthesis of the bimetallic MOFs with well-defined crystal shape and structure. In toluene degradation experiments, the DBD-coupled bimetallic MOFs (M/Mn-BTC) presented higher toluene removal efficiency, CO2 selectivity, mineralization degree, and fewer by-products when compared to both DBD-coupled single metal MOFs and the DBD-alone system. Besides, the catalytic activity of the DBD-coupled M/Mn-BTC followed the order: Co/Mn-BTC > Cu/Mn-BTC > Ce/Mn-BTC > Fe/Mn-BTC. Furthermore, it was observed that the Co/Mn molar ratio played a significant role in influencing the properties of MOFs catalysts and subsequently had an impact on their performance. The highest catalytic activity was observed at a Co/Mn molar ratio of 1:1. Under conditions of an energy density of 808.99 J‧L-1 and an oxygen fraction of 4% (v/v), Co/Mn-BTC exhibited a CO2 selectivity of 54.1%, a mineralization degree of 93.9%, and a toluene abatement efficiency of 96.2%. Additionally, an energy efficiency of 8.32 g·kWh−1 was achieved. The mechanism of toluene degradation was analyzed, uncovering a synergistic effect between DBD and Co/Mn-BTC. High-energy electron and adsorbed oxygen (denoted as Oads), along with active oxygen species (O*) from O3 decomposition, played crucial roles in the catalytic oxidation reaction. The interactions between Mn and Co enhanced electron mobility and accelerated the formation of Oads and O*, thereby facilitating toluene oxidation within the hybrid catalytic system.

Orbital Coupling of PbO7 Node in Single-Crystal Metal-Organic Framework Enhances Li-O2 Battery Electrocatalysis.

Optimizing the local coordination environment of metal centers in metal-organic frameworks (MOFs) is crucial yet challenging for regulating the overpotential of lithium-oxygen (Li-O2) batteries. Herein, we report the synthesis of a class of PbO7 nodes in a single crystal MOF (naphthalene-lead-MOF, known as Na-Pb-MOF) to significantly enhance the kinetics of both discharge and charge processes. Compared to the PbO6 node in the single-crystal tetramethoxy-lead-MOF (4OMe-Pb-MOF), the bond length between Pb and O in the PbO7 node of Na-Pb-MOF increases, resulting in weaker Pb 5d-O 2p orbital coupling, which optimizes the adsorption interaction toward intermediates, and thereby promotes the rate-determining steps of both the reduction of LiO2 to Li2O2 and the oxidation of LiO2 to O2 for reducing the activation energy of the overall reaction. Consequently, Li-O2 batteries based on Na-Pb-MOF electrocatalysts exhibit a low total charge-discharge overpotential of 0.52 V and an excellent cycle life of 140 cycles.