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Electrocatalytic reduction of nitrate to ammonia has been considered a promising and sustainable pathway for pollutant treatment and ammonia has significant potential as a clean energy. Therefore, the method has received much attention. In this work, Cu/Fe 2D bimetallic metal-organic frameworks were synthesized by a facile method applied as cathode materials without high-temperature carbonization. Bimetallic centers (Cu, Fe) with enhanced intrinsic activity demonstrated higher removal efficiency. Meanwhile, the 2D nanosheet reduced the mass transfer barrier between the catalyst and nitrate and increased the reaction kinetics. Therefore, the catalysts with a 2D structure showed much better removal efficiency than other structures (3D MOFs and Bulk MOFs). Under optimal conditions, Cu/Fe-2D MOF exhibited high nitrate removal efficiency (87.8%) and ammonium selectivity (89.3%) simultaneously. The ammonium yielded up to significantly 907.2 µg/(hr·mgcat) (7793.8 µg/(hr·mgmetal)) with Faradaic efficiency of 62.8% at an initial 100 mg N/L. The catalyst was proved to have good stability and was recycled 15 times with excellent effect. DFT simulations confirm the reduced Gibbs free energy of Cu/Fe-2D MOF. This study demonstrates the promising application of Cu/Fe-2D MOF in nitrate reduction to ammonia and provides new insights for the design of efficient electrode materials.

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Two isostructural, three-dimensional, interpenetrated amino-functionalized Metal-Organic Frameworks (Co-2AIN-MOF and Cd-2AIN-MOF) based on 2-aminoisonicotinic acid (2AIN) were synthesized, structurally characterized and determined. Based on the PXRD analysis, the solvent exchange hardly changed their framework structure, and the samples fully activated by methanol can be achieved and examined by infrared spectroscopy. Due to the presence of the carbonyl group and free amino groups in the pore of the framework, the NH3 uptakes of Co-2AIN-MOF and Cd-2AIN-MOF are 11.70 and 13.81 mmol/g and at 1 bar, respectively. In-situ Infrared spectroscopy and DFT calculations revealed the different adsorption sites and processes between Co-2AIN-MOF and Cd-2AIN-MOF.

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Copper-catalyzed click chemistry offers creative strategies for activation of therapeutics without disrupting biological processes. Despite tremendous efforts, current copper catalysts face fundamental challenges in achieving high efficiency, atom economy, and tissue-specific selectivity. Herein, we develop a facile "mix-and-match synthetic strategy" to fabricate a biomimetic single-site copper-bipyridine-based cerium metal-organic framework (Cu/Ce-MOF@M) for efficient and tumor cell-specific bioorthogonal catalysis. This elegant methodology achieves isolated single-Cu-site within the MOF architecture, resulting in exceptionally high catalytic performance. Cu/Ce-MOF@M favors a 32.1-fold higher catalytic activity than the widely used MOF-supported copper nanoparticles at single-particle level, as first evidenced by single-molecule fluorescence microscopy. Furthermore, with cancer cell-membrane camouflage, Cu/Ce-MOF@M demonstrates preferential tropism for its parent cells. Simultaneously, the single-site CuII species within Cu/Ce-MOF@M are reduced by upregulated glutathione in cancerous cells to CuI for catalyzing the click reaction, enabling homotypic cancer cell-activated in situ drug synthesis. Additionally, Cu/Ce-MOF@M exhibits oxidase and peroxidase mimicking activities, further enhancing catalytic cancer therapy. This study guides the reasonable design of highly active heterogeneous transition-metal catalysts for targeted bioorthogonal reactions.

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This work introduces a novel method of recovering bioactive berry natural products (BNPs) using solid phase extraction with metal-organic frameworks (MOF-SPE). Two pyrene-based MOFs with different structural topologies, Al-PyrMOF and Zr-NU-1000, were evaluated for their ability to capture and desorb BNPs, including ellagic acid, quercetin, gallic acid, and p-coumaric acid. Time-dependent BNP uptake via dispersive SPE revealed that NU-1000 outperformed Al-PyrMOF in capturing all BNPs. Our findings show NU-1000 demonstrated a higher and more consistent BNP capture profile, achieving over 90% capture of all BNPs within 36 hours, with only a 9% variation between the most and least effectively captured BNPs. In contrast, Al-PyrMOF, displayed a staggered uptake profile, with a significant 53% difference in capture efficiency between the most and least effectively captured BNP. However, when a BNP mixture was used at a loading concentration of 50 µg/mL, Al-PyrMOF outperformed NU-1000, capturing over 70% of all BNPs. Al-PyrMOF also exhibited improved BNP recovery, with a minimum of two-fold greater amount recovered for all BNPs. Further testing with a BNP mixture at a concentration of 15 µg/mL demonstrated that Al-PyrMOF efficiently concentrated all BNPs, achieving a maximum extraction factor of 2.71 observed for quercetin.

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Due to the heterogeneity of the tumor microenvironment, the clinical efficacy of tumor treatment is not satisfied, highlighting the necessity for new strategies to tackle this issue. To effectively treat breast tumors by tumor-targeted chemo/chemodynamic therapy, herein, the Fe3+-rich MIL-88B nanobullets (MNs) covered with hyaluronic acid (HA) were fabricated as vehicles of zoledronic acid (ZA). The attained ZA@HMNs showed a high ZA payload (ca 29.6 %), outstanding colloidal stability in the serum-containing milieu, and accelerated ZA as well as Fe3+ release under weakly acidic and glutathione (GSH)-rich conditions. Also, the ZA@HMNs consumed GSH by GSH-mediated Fe3+ reduction and converted H2O2 into OH via Fenton or Fenton-like reaction with pH reduction. After being internalized by 4T1 cells upon CD44-mediated endocytosis, the ZA@HMNs depleted intracellular GSH and degraded H2O2 into OH, thus eliciting lipid peroxidation and mitochondria damage to suppress cell proliferation. Also, the ZA@HMNs remarkably killed macrophage-like RAW 264.7 cells. Importantly, the in vivo studies and ki67 and GPX4 staining of tumor sections demonstrated that the ZA@HMNs efficiently accumulated in 4T1 tumors to hinder tumor growth via ZA chemotherapy combined with OH-mediated ferroptosis. This work presents a practicable strategy to fabricate ZA@HMNs for breast tumor-targeted chemo/chemodynamic therapy with potential clinical translation.

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An aggregation-induced emission (AIE)-based strategy was proposed for fluorescence immunoassays of protein biomarkers using Cu-based metal-organic frameworks (Cu-MOFs) to load recombinant targets and enzymes for dual signal amplification. The immunosensing platform was built based on the sequestration and consumption of the substrates of pyrophosphate (PPi) ions by Cu-MOFs and enzymatic catalysis. The negatively charged PPi could trigger the aggregation of positively charged tetraphenylethene (TPE)-substituted pyridinium salt nanoparticles (TPE-Py NPs) by electrostatic interactions, lighting up the fluorescence due to the AIE phenomenon. The consumption of PPi by the captured Cu-MOFs through the Cu2+-PPi chelation interaction and ALP-enzymatic hydrolysis depressed the aggregation of TPE-Py NPs. Capture of the tested targets in samples by the antibodies on the plate surface could prevent the attachment of target/ALP-loaded Cu-MOFs due to the competitive immunoreactions. The "signal-on" competitive immunoassay was applied for the detection of procalcitonin (PCT) as the model analyte with a linear range of 0.01-10 pg/mL and a detection limit down to 8 pg/mL. The conceptual integration of AIE with enzymatic and MOFs-based dual signal amplification endowed fluorescence immunoassays with high sensitivity and selectivity. The surface modification of Cu-MOFs with hexahistine (His6)-tagged recombinant proteins through metal coordination interactions should be evaluable for the design of novel biosensors.

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Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca1/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal-organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca1/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.

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Although metal-organic frameworks (MOFs) and metalo hydrogen-bonded organic frameworks (MHOFs) are designed as promising solid-state proton conductors by incorporating various protonic species intrinsically or extrinsically, design and development of such materials by employing the concept of proton conduction through coordinated polar protic solvent is largely unexplored. Herein, we have constructed two proton-conducting materials having different solvent coordinated metal cationic species: In-H2O-MOF, ({[In(H2O)6][In3(Pzdc)6]·15H2O}n; H2Pzdc: pyrazine-2,3-dicarboxylic acid) with coordinated water molecules from hexaaquaindium cationic species, and MHOF-4, ([{Co(NH3)6}2(2,6-NDS)2(H2O)2]n; 2,6-H2NDS: 2,6-naphthalenedisulfonic acid) with coordinated ammonia from hexaammoniacobalt cationic species. Interestingly, higher proton conductivity was achieved for In-H2O-MOF (1.5 × 10-5 S cm-1) than MHOF-4 (6.3 × 10-6 S cm-1) under the extreme conditions (80 ºC and 95% RH), which could be attributed to enhanced acidity of coordinated water molecules having much lower pKa value than that of coordinated ammonia. Greater charge polarization on hydrogen atoms of In3+-coordinated water molecules than that of Co2+-coordinated ammonia led to the high conductivity of In-H2O-MOF, as evident by quantum chemical studies. Such a comparative study on metal-coordinated protic polar solvents in achieving proton conduction in crystalline solids is yet to be made.

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Rare-earth elements (REEs) play a crucial role in state-of-the-art technologies and sustainable energy generation. However, conventional production methods of REE often instigate detrimental impacts on environment. Hence, the development of efficient and sustainable hydrometallurgical methods for REE recovery from complex solution has become a crucial research focus. This study investigates a mixed-matrix membrane composed of a highly europium selective metal-organic framework-based adsorbent, Cr-MIL-PMIDA, embedded in sulfonated poly(ether ketone) (SPEK) polymer membrane matrix to preferentially concentrate europium (Eu3+) ions in the presence of other competing cations. The activated membrane notably reduced ionic conductivity for Eu3+ compared to other multivalent ions. Membrane extraction experiments further confirmed the selective behavior, demonstrating slower diffusion for Eu3+ compared to Mg2+ and Zn2+ cations. Especially, at pH 5, Mg2⁺ and Zn2⁺ recovery was greater than 30%, whereas Eu³âº recovery remained lower than 4%. We propose that the strong chemical affinity between the phosphate group and Eu3+ help partition of the Eu3+ ions in the membrane phase and inhibit the diffusion and further partitioning of the Eu3+ ion from bulk solution. Furthermore, we demonstrate the stability of the composite membrane and the embedded MOF particles in aqueous solution for up to 12 days without degradation, attributing it to the robust chemical stability of the MOF structure.

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Organic linker-based luminescent metal-organic frameworks (LMOFs) have received extensive studies due to the unlimited species of emissive organic linkers and tunable structure of MOFs. However, the multiple-step organic synthesis is always a great challenge for the development of LMOFs. As an alternative strategy, in situ "one-pot" strategy, in which the generation of emissive organic linkers and sequential construction of LMOFs happen in one reaction condition, can avoid time-consuming pre-synthesis of organic linkers. In the present work, we demonstrate the successful utilization of in situ "one-pot" strategy to construct a series of LMOFs via the single-site modification between the reaction of aldehydes and o-phenylenediamine-based tetratopic carboxylic acid. The resultant MOFs possess csq topology with emission covering blue to near-infrared. The nanosized LMOFs exhibit excellent sensitivity and selectivity for tryptophan detection. In addition, two component-based LMOFs can also be prepared via the in situ "one-pot" strategy and used to study energy transfer. This work not only reports the construction of LMOFs with full-color emissions, which can be utilized for various applications, but also indicates that in situ "one-pot" strategy indeed is a useful and powerful method to complement the traditional MOFs construction method for preparing porous materials with tunable functionalities and properties.

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Tuning a material's hydrophobicity is desirable in several industrial applications, such as hydrocarbon storage, separation, selective CO2 capture, oil spill cleanup, and water purification. The introduction of fluorine into rare-earth (RE) metal-organic frameworks (MOFs) can make them hydrophobic. In this work, the linker bis(trifluoromethyl)terephthalic acid (TTA) was used to make highly fluorinated MOFs. The reaction of the TTA and RE3+ (RE: Y, Gd, or Eu) ions resulted in the primitive cubic structure (pcu) exhibiting RE dimer nodes (RE-TTA-pcu). The crystal structure of the RE-TTA-pcu was obtained. The use of the 2-fluorobenzoic acid in the synthesis resulted in fluorinated hexaclusters in the face-centered cubic (fcu) framework (RE-TTA-fcu), analogous to the UiO-66 MOF. The RE-TTA-fcu has fluorine on the linker as well as in the cluster. The MOFs were characterized by powder X-ray diffraction, X-ray photoelectron spectroscopy, thermogravimetric analysis, and contact angle measurements.

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Radioactive iodine (131I) with a short half-life of ~8.02 days is one of the most commonly used nuclides in nuclear medicine. However, 131I easily poses a significant risk to human health and ecological environment. Therefore, there is an urgent need to develop a secure and efficient strategy to capture and store radioactive iodine. Metal-organic frameworks (MOFs) are a new generation of sorbents with outstanding physical and chemical properties, rendering them attractive candidates for the adsorption and immobilization of iodine. This review focuses on recent research advancements in mechanisms underlying iodine adsorption over MOFs and their derivatives, including van der Waals interactions, complexing interactions, and chemical precipitation. Furthermore, this review concludes by outlining the challenges and opportunities for the safe disposal of radioactive iodine from the perspective of the material design and system evaluation based on our knowledge. Thus, this paper aims to offer necessary information regarding the large-scale production of MOFs for iodine adsorption.

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In the present study, an acid catalyst (UiO-66-SO3H) with Brønsted and Lewis acid sites was synthesised for the preparation of highly efficient biodiesel from oleic acid and methanol using chlorosulphonic acid sulfonated metal-organic frameworks (UiO-66) prepared with acetic acid as a moderator. The prepared catalysts were characterised using XRD, SEM, FT-IR and BET. The catalytic efficiency of the sulfonated catalysts was significantly improved and successful sulfonation was demonstrated by characterisation techniques. Biodiesel was synthesised by the one-pot method and an 85.0% biodiesel yield was achieved under optimum conditions of the reaction. The esterification reaction was determined to be consistent with a proposed primary reaction and the kinetics of the reaction was investigated. A reusability study of the catalyst (UiO-66-SO3H) was also carried out with good reproducibility. In conclusion, the present study provides some ideas for the synthesis of catalysts with high catalytic activity for the application in the catalytic preparation of biodiesel.

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Achieving high-performance aqueous zinc (Zn)-ion batteries (AZIBs) requires stable and efficient cathode materials capable of reversible Zn-ion intercalation. Although layered vanadium oxides possess high Zn-ion storage capacity, their sluggish kinetics and poor conductivity present significant hurdles for further enhancing the performance of AZIBs. In response to this challenge, a dissolution-regrowth and conversion approach is formulated using metal-organic frameworks (MOFs) as a sacrificial template, which enables the in situ creation of copper vanadium oxides (CuVOx) with porous 1D channels and distinctive nanoarchitectures. Owing to their distinctive structure, the optimized CuVOx cathode experiences a reaction involving the synergistic insertion/extraction of Zn2+, resulting in rapid Zn2+ diffusion kinetics and enhanced electrochemical activity postactivation. Specifically, the activated electrode delivers a reversible capacity of 519 mAh g-1 at 0.5 A g-1 for AZIBs. It is noteworthy that the electrode exhibits a remarkable reversible rate capacity of 220 mAh g-1 at 5 A g-1 with excellent durable cycleability, retaining 88% of its capacity even after 3000 cycles. Various ex situ testing methods endorse the reversible insertion/extraction of Zn2+ in the CuVOx cathode. This study provides a novel insight into high-performance MOF-derived unique structure designs for AZIB electrodes.

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Self-powered biosensors with high sensitivity have garnered significant interest for their potential applications in the realm of portable sensing. Herein, a self-powered biosensor with a novel signal amplification strategy was developed by integrating target-controlled release of mediator with an enzyme biofuel cell for the ultrasensitive detection of acetamiprid (ACE). Zeolitic imidazolate framework-67 was utilized as both a nanocontainer for capturing the electron mediator 2,2'-azidobis (3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), and a precursor for the synthesis of cobalt nanoparticles/nitrogen, sulfur-codoped carbon nanotubes (Co NPs/NS-CNTs), which were employed as the electrode material for constructing both the glucose oxidase-based bioanode and the laccase-based biocathode. The target analyte ACE can specifically bind to its aptamer, leading to the release of ABTS, which cyclically participates in the catalytic reaction of the biocathode, thereby amplifying the electrochemical signal. By leveraging the benefits of ABTS cyclic catalysis and the effective electrocatalysis of bioelectrodes based on Co NPs/NS-CNTs, the self-powered biosensor has a broad detection range of 0.1-1000 fM and a low detection limit of 25 aM toward ACE. The proposed signal amplification approach presents a promising strategy for enhancing sensitivity and enabling portable analysis in applications of food safety, environmental monitoring, and medical diagnostics.

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The study investigated the performance of a novel magnetic hybrid MIL-53(Fe)/Fe3O4@TiO2 composite for removing reactive red 195 (RR195) dye from water using UVc light. Various analytical techniques were used to characterize the nanocomposite materials. X-ray diffraction analysis confirmed the presence of MIL-53(Fe) and TiO2 in the composite. FT-IR analysis identified carboxyl and Ti-O-Ti groups in the photocatalyst structure. The study evaluated the effects of pH, dye concentration, photocatalyst dosage, and temperature on RR195 photodegradation. The Langmuir-Hinshelwood kinetic model provided the best fit for the reaction rate. Optimal conditions for an 84 % dye degradation were found at a photocatalyst dose of 15 mg/100 mL, pH 3, dye concentration of 100 mg/L, and 35 °C after 120 minutes of UVc light exposure. Thermodynamic analysis indicated an endothermic reaction with positive values for Δ#H and negative values for Δ#S. The MIL-53(Fe)/Fe3O4@TiO2 composite demonstrated excellent stability and achieved over 90 % dye degradation after five cycles. Overall, the composite shows promise for treating wastewater with dyes.

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Laccases act as green catalysts for oxidative cross-coupling of phenolic antioxidnt compounds, but low stability and non-recyclability limit its application. To address that, metal-organic frameworks Cu-BTC and Cr-MOF were synthesized as supports to immobilize the efficient laccase from Cerrena sp. HYB07. The Brunauer-Emmett-Teller surface area of Cu-BTC and Cr-MOF were 1213.2 and 907.1 m2/g, respectively. The two carriers respectively presented pore diameters of 1.2-10 nm and 1.4-12 nm as octahedron, indicating nano-scale mesoporosity. These Cu-BTC and Cr-MOF carriers could adsorb laccase with enzyme loading of 1933.2 and 1564.4 U/g carrier, respectively. The stability and organic solvent tolerance of Cu-BTC-laccase and Cr-MOF-laccase were both obviously improved compared to free laccase. Thermal inactivation kinetics showed that both the two immobilized laccases displayed lower thermal inactivation rate constants. Importantly, the Cu-BTC-laccase and Cr-MOF-laccase both showed much higher activity for cross-coupling of ethyl ferulate than free laccase, which had 2.5-fold higher cross-coupling efficiency than that by free laccase. The ethyl ferulate coupling product was also analyzed by mass spectroscopy and the synthesis pathway of ethyl ferulate dimer was proposed. The cross coupling of ethyl ferulate required the formation of radical intermediates of ethyl ferulate generated by laccase mediated oxidation. This work paved the way for MOFs immobilized laccase for cross coupling of antioxidant phenols.

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The synthesis of bioinspired metal-organic frameworks (MOFs) performed in mild conditions with a high quality is greatly demanded. Moreover, the influence of the morphology and structure of bio-MOFs on the cell interaction and toxicity is important to determine. In this work, we developed an ultrasound (US)-assisted synthesis of HKUST-1 MOFs under mild conditions and investigated the influence of the parameters of synthesis on the morphology, structure, and biological properties of the developed MOFs. It was found that the US power, reaction time, temperature, and type of solvent composition would affect the morphology, size, and yield of the obtained crystals. Employing the optimal synthetic conditions, five types of HKUST-1 MOFs were prepared, achieving highest yields (67.8-96.2%) and different morphologies (octahedral, dodecahedral, icosahedral). The relationship between the morphological features and biological properties of developed bio-MOFs was evaluated and discussed. The cellular association and cytotoxicity of MOF@US and MOF@US-PARG were studied on various cell cultures, i.e. normal mouse embryonic fibroblasts (MEF NF2), chronic myeloid leukemia (K562), and mouse melanoma (B16-F10). The experimental results showed that MOF@US-PARG has a higher percentage of association compared to MOF@US. It has also been shown that the cytotoxicity depends on the concentration and surface modification of the developed MOFs.

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In this work, a horseradish peroxidase (HRP)-encapsulated metal organic framework (MOF)@MOF nanocomposite is developed for detecting H2O2 converted by dismutation of superoxide anions released from live HeLa mitochondria. Initially, an HRP-polyacrylic acid cluster is incorporated on a mesoporous, peroxidase-like Cu/Co-1,4-benzenedicarboxylate (BDC) MOF platform to avoid structural change and deactivation of HRP through its interactions with MOF metal ions. Additionally, a Cu/Co-BDC(HRP)@1,3,5-benzenetricarboxyate (BTC) core-shell MOF/MOF structure, also with peroxide-like properties, serves as a protective matrix for HRP. Then, ultrathin porous carbon shells (UPCS) are adopted to improve the electrical conductivity of the MOF@MOF. The Cu/Co-BDC(HRP)@BTC|UPCS sensing platform exhibits two linear ranges of 0.05-1 µM and 1-1000 µM with a sensitivity of 172 mA mM-1 cm-2 and 1.63 mA mM-1 cm-2, respectively. A limit of detection of 0.057 µM, good selectivity and stability over 35 days for H2O2 detection are also achieved. After treating the mitochondrial complex with specific inhibitors, amperometric results at the sensing platform confirmed complex I and III within mitochondria as the main electron leakage sites in the electron transfer chains. Therefore, this sensing platform provides a tool that may aid in predicting and even developing treatments for some oxidative stress diseases caused by mitochondrial abnormalities.

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This study introduces a high-performance Ce-Co MOFs/Ti3C2Tx nanocomposite, synthesized via hydrothermal methods, designed to advance supercapacitor technology. The integration of Ce-Co metal-organic frameworks (MOFs) with Ti3C2Tx (Mxene) yields a composite that exhibits superior electrochemical properties. Structural analyses, including X-ray Diffraction (XRD) and Scanning Electron Microscopy (SEM), confirm the successful formation of the composite, featuring well-defined rod-like Ce-Co MOFs and layered Ti3C2Tx sheets. Electrochemical evaluation highlights the exceptional performance of the Ce-Co MOFs/Ti3C2Tx nanocomposite, achieving a specific capacitance of 483.3 Fg⁻1 at 10 mVs⁻1, a notable enhancement over the 200 Fg⁻1 of Ce-Co MOFs. It also delivers a high energy density of 78.48 Whkg⁻1 compared to 19 Whkg⁻1 for Ce-Co MOFs. Remarkably, the nanocomposite shows outstanding cyclic stability with a capacitance retention of 109 % after 4000 cycles and electrochemical surface area (ECSA) of 845 cm2, coupled with a reduced charge transfer resistance (Rct) of 2.601 Ω and an equivalent series resistance (ESR) of 0.8 Ω. These findings demonstrate that the Ce-Co MOFs/Ti3C2Tx nanocomposite is a groundbreaking material, offering enhanced energy storage, conductivity, and durability, positioning it as a leading candidate for next-generation supercapacitors.