Metal-organic Frameworks Research Articles

Gas adsorption meets geometric deep learning: points, set and match

Thanks to their unique properties such as ultra high porosity and surface area, metal-organic frameworks (MOFs) are highly regarded materials for gas adsorption applications. However, their combinatorial nature results in a vast chemical space, precluding its exploration with traditional techniques. Recently, machine learning (ML) pipelines have been established as the go-to method for large scale screening by means of predictive models. These are typically built in a descriptor-based manner, meaning that the structure must be first coarse-grained into a 1D fingerprint before it is fed to the ML algorithm. As such, the latter can not fully exploit the 3D structural information, potentially resulting in a model of lower quality. In this work, we propose a descriptor-free framework called “AIdsorb”, which can directly process raw structural information for predicting gas adsorption properties. To accomplish that, the structure is first treated as a point cloud and then passed to a deep learning algorithm suitable for point cloud analysis. As a proof of concept, AIdsorb is applied for predicting CO2\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\ ext {CO}_{2}$$\\end{document} uptake in MOFs, outperforming a conventional pipeline that uses geometric descriptors as input. Additionally, to evaluate the transferability of the proposed framework to different host-guest systems, CH4\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\ ext {CH}_{4}$$\\end{document} uptake in COFs is examined. Since AIdsorb bases its roots on raw structural information, its applicability extends to all fields of material science.

In situ synthesis of metal-organic frameworks on sulfonated cellulose nanofibrils

The intrinsic fragility and inferior processibility of metal-organic frameworks (MOFs) particles often restrict their functional application despite their high surface area and porous structure. We investigated the feasibility of sulfonated cellulose nanofibrils (SCNF) as a biopolymer template to hybridize MOFs. SCNF was synthesized through periodate oxidation followed by bisulfite sulfonation. The sulfonate groups increased electronegativity and enhanced the dispersibility of the cellulose fibers. More importantly, the negatively charged sulfonates could serve as anchors for metal ions to initiate the in situ growth of MOFs along the surface of cellulose fibers. We have achieved the synthesis of three types of SCNF/MOF hybrids, namely, SCNF/ZIF-8, SCNF/ZIF-67, and SCNF/HKUST-1. These hybrids can be formed as free-standing aerogels, exhibiting remarkably high surface areas and flexibility for applications. The assessment of the adsorptive efficiency of the SCNF/ZIF-8 hybrid indicates that the hybrid material exhibited a notably higher adsorption capacity for methylene blue versus the SCNF control. DFT calculation provides further insights into the underlying adsorption mechanisms, revealing that the sulfonates on the SCNF and the nitrogen atoms in the ZIF-8 ligands primarily contributed to the affinity for methylene blue. SCNF offers a versatile and robust biopolymer substrate for templating a wide array of MOFs with promising applications as adsorbents and beyond.

Bifunctional Metal–Organic Framework Synergistically Enhances Radiotherapy and Activates STING for Potent Cancer Radio‐Immunotherapy

AbstractThe activation of the stimulator of interferon genes (STING) protein by cyclic dinucleotide metabolites plays a critical role in antitumor immunity. However, synthetic STING agonists like 4‐(5,6‐dimethoxybenzo[b]thiophen‐2‐yl)‐4‐oxobutanoic acid (MSA‐2) exhibit suboptimal pharmacokinetics and fail to sustain STING activation in tumors for effective antitumor responses. Here, we report the design of MOF/MSA‐2, a bifunctional MSA‐2 conjugated nanoscale metal–organic framework (MOF) based on Hf6 secondary building units (SBUs) and hexakis(4′‐carboxy[1,1′‐biphenyl]‐4‐yl)benzene bridging ligands, for potent cancer radio‐immunotherapy. By leveraging the high‐Z properties of the Hf6 SBUs, the MOF enhances the therapeutic effect of X‐ray radiation and elicits potent immune stimulation in the tumor microenvironment. MOF/MSA‐2 further enhances radiotherapeutic effects of X‐rays by enabling sustained STING activation and promoting the infiltration and activation of immune cells in the tumors. MOF/MSA‐2 plus low‐dose X‐ray irradiation elicits strong STING activation and potent tumor regression, and when combined with an immune checkpoint inhibitor, effectively suppresses both primary and distant tumors through systemic immune activation.

Cu−Bi Bimetallic Catalysts Derived from Metal–Organic Framework Arrays on Copper Foam for Efficient Glycine Electrosynthesis

AbstractGlycine as one of the most abundant amino acids in human proteins, with extensive applications in both life and industry, is conventionally synthesized through complex procedures or toxic feedstocks. In this study, we present a facile and benign electrochemical pathway for synthesis of glycine through reductive coupling of glyoxylic acid and nitrate over a copper‐bismuth bimetal catalyst derived from a metal–organic framework (MOF) array on copper foam (Cu/Bi−C@CF). Remarkably, Cu/Bi−C@CF achieves a fantastic selectivity of 89 %, corresponding a high Faraday efficiency of 65.9 %. From control experiments, the introduction of Bi caused the binding energy of Cu shift to a lower state, which leads to a high selectivity towards the formation of key intermediate hydroxylamine rather than ammonia product, facilitating the formation of oxime and providing additional sites for subsequent hydrogenation reaction on the way to glycine. Moreover, the derivation of MOF arrays ensures the effective dispersion of Bi and enhances the stability of Cu/Bi−C@CF. This innovative approach not only presents sustainable pathways for the production of value‐added organonitrogen compounds utilizing readily available carbon and nitrogen sources, but also provides novel insights into the design of multistage structural catalysts for sequential reactions.

Catalytically Active Site Mapping Realized through Energy Transfer Modeling

AbstractThe demands of a sustainable chemical industry are a driving force for the development of heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous‐to‐heterogeneous catalyst transitions can be realized through the integration of efficient homogeneous catalysts within porous matrices. Herein, we offer a versatile approach to understanding how guest distribution and evolution impact the catalytic performance of heterogeneous host–guest catalytic platforms by implementing the resonance energy transfer (RET) concept using fluorescent model systems mimicking the steric constraints of targeted catalysts. Using the RET‐based methodology, we mapped condition‐dependent guest (re)distribution within a porous support on the example of modular matrices such as metal–organic frameworks (MOFs). Furthermore, we correlate RET results performed on the model systems with the catalytic performance of two MOF‐encapsulated catalysts used to promote CO2 hydrogenation and ring‐closing metathesis. Guests are incorporated using aperture‐opening encapsulation, and catalyst redistribution is not observed under practical reaction conditions, showcasing a pathway to advance catalyst recyclability in the case of host–guest platforms. These studies represent the first generalizable approach for mapping the guest distribution in heterogeneous host–guest catalytic systems, providing a foundation for predicting and tailoring the performance of catalysts integrated into various porous supports.

Low Temperature and Rapid Synthesis of Li‐Rich Li(Li0.17Mn0.83)2O4 Spinel Cathodes Derived from Metal‐Organic Frameworks for Lithium‐Ion Batteries

AbstractLi‐rich spinel materials (Li1+xMn2−xO4) have shown promise for lithium‐ion batteries. Nevertheless, the preparation of Li1+xMn2−xO4 faces significant challenges due to the difficulty in achieving a balance between well‐crystallized phases and stoichiometric chemistry. Moreover, the synthesis process is highly sensitive to calcination temperature and time, making it susceptible to phase transformations. Therefore, the rational selection of precursors and corresponding calcination procedures is absolutely essential. Herein, we make full use of the nature of metal‐organic frameworks (MOFs) to achieve phase‐controlled synthesis of Li(Li0.17Mn0.83)2O4 (LMO−F) spinel cathodes in 8 minutes at 500 °C. The composition and structural evolution during the pyrolysis process were systematically investigated to clarify the relationship between precursors and derivatives. Notably, the LMO−F achieved good electrochemical performance with 100.4 mAh g−1 at 50 mA g−1 after 100 cycles.

Bifunctional Metal-Organic Framework Synergistically Enhances Radiotherapy and Activates STING for Potent Cancer Radio-Immunotherapy.

The activation of the stimulator of interferon genes (STING) protein by cyclic dinucleotide metabolites plays a critical role in antitumor immunity. However, synthetic STING agonists like 4-(5,6-dimethoxybenzo[b]thiophen-2-yl)-4-oxobutanoic acid (MSA-2) exhibit suboptimal pharmacokinetics and fail to sustain STING activation in tumors for effective antitumor responses. Here, we report the design of MOF/MSA-2, a bifunctional MSA-2 conjugated nanoscale metal-organic framework (MOF) based on Hf6 secondary building units (SBUs) and hexakis(4'-carboxy[1,1'-biphenyl]-4-yl)benzene bridging ligands, for potent cancer radio-immunotherapy. By leveraging the high-Z properties of the Hf6 SBUs, the MOF enhances the therapeutic effect of X-ray radiation and elicits potent immune stimulation in the tumor microenvironment. MOF/MSA-2 further enhances radiotherapeutic effects of X-rays by enabling sustained STING activation and promoting the infiltration and activation of immune cells in the tumors. MOF/MSA-2 plus low-dose X-ray irradiation elicits strong STING activation and potent tumor regression, and when combined with an immune checkpoint inhibitor, effectively suppresses both primary and distant tumors through systemic immune activation.

Cu-Bi Bimetallic Catalysts Derived from Metal-Organic Framework Arrays on Copper Foam for Efficient Glycine Electrosynthesis.

Glycine as one of the most abundant amino acids in human proteins, with extensive applications in both life and industry, is conventionally synthesized through complex procedures or toxic feedstocks. In this study, we present a facile and benign electrochemical pathway for synthesis of glycine through reductive coupling of glyoxylic acid and nitrate over a copper-bismuth bimetal catalyst derived from a metal-organic framework (MOF) array on copper foam (Cu/Bi-C@CF). Remarkably, Cu/Bi-C@CF achieves a fantastic selectivity of 89 %, corresponding a high Faraday efficiency of 65.9 %. From control experiments, the introduction of Bi caused the binding energy of Cu shift to a lower state, which leads to a high selectivity towards the formation of key intermediate hydroxylamine rather than ammonia product, facilitating the formation of oxime and providing additional sites for subsequent hydrogenation reaction on the way to glycine. Moreover, the derivation of MOF arrays ensures the effective dispersion of Bi and enhances the stability of Cu/Bi-C@CF. This innovative approach not only presents sustainable pathways for the production of value-added organonitrogen compounds utilizing readily available carbon and nitrogen sources, but also provides novel insights into the design of multistage structural catalysts for sequential reactions.

Catalytically Active Site Mapping Realized through Energy Transfer Modeling.

The demands of a sustainable chemical industry are a driving force for the development of heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous-to-heterogeneous catalyst transitions can be realized through the integration of efficient homogeneous catalysts within porous matrices. Herein, we offer a versatile approach to understanding how guest distribution and evolution impact the catalytic performance of heterogeneous host-guest catalytic platforms by implementing the resonance energy transfer (RET) concept using fluorescent model systems mimicking the steric constraints of targeted catalysts. Using the RET-based methodology, we mapped condition-dependent guest (re)distribution within a porous support on the example of modular matrices such as metal-organic frameworks (MOFs). Furthermore, we correlate RET results performed on the model systems with the catalytic performance of two MOF-encapsulated catalysts used to promote CO2 hydrogenation and ring-closing metathesis. Guests are incorporated using aperture-opening encapsulation, and catalyst redistribution is not observed under practical reaction conditions, showcasing a pathway to advance catalyst recyclability in the case of host-guest platforms. These studies represent the first generalizable approach for mapping the guest distribution in heterogeneous host-guest catalytic systems, providing a foundation for predicting and tailoring the performance of catalysts integrated into various porous supports.

An Enzyme-Free Impedimetric Sensor Based on Flower-like NiO/Carbon Microspheres for L-Glutamic Acid Assay.

This research introduces a non-enzymatic electrochemical sensor utilizing flower-like nickel oxide/carbon (fl-NiO/C) microspheres for the precise detection of L-glutamic acid (LGA), a crucial neurotransmitter in the field of healthcare and a frequently utilized food additive and flavor enhancer. The fl-NiO/C were synthesized with controllable microstructures using metal-organic frameworks (MOFs) as precursors followed by a simple calcination process. The uniformly synthesized fl-NiO/C microspheres were further characterized using Fourier transform infrared spectroscopy (FTIR), X-ray powder diffraction (XRD), energy-dispersive X-ray spectroscopy (EDX), and field emission scanning electron microscopy (FE-SEM). The fl-NiO/C was utilized as a modifier on the surface of a glassy carbon electrode, and an impedimetric sensor based on electrochemical impedance spectroscopy (EIS) was developed for the detection of LGA. The proposed sensor demonstrated excellent catalytic activity and selectivity towards LGA across a broad concentration range of 10-800 μM with a sensitivity of 486.9 µA.mM-1.cm-2 and a detection limit of 1.28 µM (S/N = 3). The sensor was also employed to identify LGA in blood plasma samples, yielding results that align with those obtained through HPLC. This achievement highlights the potential of fl-NiO/C microspheres in advancing cutting-edge biosensing applications.

Oriented Growth of Highly Emissive Manganese Halide Microrods for Dual-Mode Low-Loss Optical Waveguides.

Zero-dimensional (0D) structured lead-free metal halides have recently attracted widespread attention due to their high photoluminescence quantum yield (PLQY) and negligible self-absorption, showing enormous potential as optical waveguides towards miniaturized photonic devices. However, due to the great difficulty in growth of rod-like nano/micro-sized morphologies, such applications have been less explored. Herein, a new-type emissive organic-inorganic manganese (II) halide crystal (TPS2MnCl4, TPS=C18H15S, triphenylsulfonium) in the form of microrods is synthesized via a facile chloride ion (Cl-) induced oriented growth method. Due to a combination of attractive features such as a high PLQY of 86 %, negligible self-absorption and smooth crystal surface, TPS2MnCl4 microrods are well suited for use in optical waveguide with an ultra-low optical loss coefficient of 1.20 ⋅ 10-4 dB μm-1, superior to that of most organic-inorganic metal halide hybrids, organic materials, polymers and metal nanoclusters to the best of our knowledge. Importantly, TPS2MnCl4 microrods can further work as dual-mode optical waveguides, combining active and passive light transmission functionalities in one single crystal. In addition, TPS2MnCl4 microrods also display remarkable performance in lighting and anti-counterfeiting due to their distinct optical properties and commendable stability.

Enhanced C(sp3)–H Selective Oxidation Using Efficient Polyoxometalate-Based Metal–Organic Framework Photocatalysts Synergized with Ir Metalloligands and Polyoxometalates

Enhanced C(sp³)–H Selective Oxidation Using Efficient Polyoxometalate-Based Metal–Organic Framework Photocatalysts Synergized with Ir Metalloligands and Polyoxometalates

A Scorpion–Type Dopant‐Free Hole Transport Material for n‐i‐p Organic–Inorganic Hybrid Perovskite Solar Cells

AbstractIt is significant to develop dopant‐free hole transport materials (HTMs) to improve the long‐term stability of n‐i‐p organic–inorganic hybrid perovskite solar cells (PSCs). In this work, two HTMs (DTTP‐T and DTTP‐D) based on dithienothiopyrrole (DTTP) core were synthesized to explore the effects of different substituents on the nitrogen atom on the properties of HTMs. Compared with anisole‐substituted DTTP‐D, triarylamine‐substituted scorpion‐type DTTP‐T shows better matching energy level, stronger charge transfer and defect passivation ability. Therefore, the power conversion efficiency (PCE) of dopant‐free DTTP‐T‐based n‐i‐p PSCs reaches 18.67 %, which is comparable to that of doped Spiro‐OMeTAD (19.51 %). More encouragingly, the efficiency of DTTP‐T‐based devices remains above 80 % of its initial efficiency after 1728 h of storage in air, while the Spiro‐OMeTAD‐based devices could only maintain 600 h. This work provides a good reference for the development of dopant‐free small molecular HTMs for efficient and stable PSCs.

Single‐Component White Emissive Organic–Inorganic Hybrid Copper Halide Composite Films for Remote UV‐pumped White Light‐Emitting Diodes with High Color Rendering Index

AbstractLead‐free organic–inorganic metal halides (OIMHs) are highly desirable owing to their remarkable properties including low toxicity, structural diversity, high stability, and solution processability. Nevertheless, the development of their single‐component white emissive films remains a formidable challenge for remote white light‐emitting diodes (WLEDs) application. In this work, (C16H36N)2Cu2I4/polyvinylidene fluoride (PVDF) white emissive composite film is successfully fabricated through an in situ solvent evaporation crystallization process at room temperature. The elemental analysis and bonding between (C16H36N)2Cu2I4 and PVDF are demonstrated by X‐ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FTIR) measurements. In addition, this composite film exhibits a broadband white emission with two peaks. Notably, the best photoluminescence quantum yields (PLQYs) of the PVDF based composite film reaches an impressive 96.7%. A (C16H36N)2Cu2I4/PVDF based remote UV‐pumped WLEDs with an impressive color rendering index of 95.5 is realized. Finally, the in situ fabrication method is expanded to fabricate (C16H36N)2Cu2I4/polyacrylonitrile (PAN) composite films, and we further realized their single component remote WLEDs.

Metal-organic frameworks for atmospheric water extraction: Kinetic analysis and stochastic programming under climate variability

Increasing demands for sustainable and distributed freshwater sources drive the exploration of water extraction from ambient air. This study presents a comprehensive computational approach for optimizing unit harvesting cost of the adsorption-based atmospheric water extraction (AWE) systems. There are three objectives (i) assessing the impact of climate variability: utilizing k-means clustering, utilizing climate data in different regions to explore the effects of ambient conditions in dry-hot (California), humid-hot (Florida), and dry-cold (Wyoming) regions, resulting in a preference for harvesting under humid-hot conditions. (ii) performing kinetic analysis: The derived kinetic model connects climate variability to operational time and regeneration temperature, critical process design variables. (iii) assessing adsorption materials: three materials (MIL-100 (Fe), MOF-303, and ZJNU-30) were assessed revealing the impact of variations in maximum capacity and isotherm shape on performance and cost. The optimization algorithm uses a two stage stochastic programming approach to account for climate variability and enables an optimization that balances the capital and operating costs across a range of temperature and humidity conditions.

Twinned Metal-Organic Framework Nanoplates for Hydrocarbon Separation Membranes.

Filler morphology control is critical for enhancing the gas separation performance of mixed matrix membranes (MMMs). A vertical transport channel using the crystal twinning phenomenon is designed on the zeolitic imidazolate framework (ZIF) nanoplate. Twinned ZIF-8 (TZIF-8) nanoplate is prepared by controlling the shape of ZIF-L from nanosheet to twinned flake, followed by conversion into the ZIF-8 phase. With the addition of TZIF-8 in 6FDA-DAM polymer, propylene/propane selectivity is dramatically enhanced, showing propylene permeability of 40 Barrer and propylene/propane selectivity of 82. The separation performance surpasses the performance of MMMs reported so far, and the selectivity is comparable to that of polycrystalline ZIF-8 membranes. A transport mechanism study using mathematical models implies that the percolated twin fillers create rapid and selective gas channels for desired molecules and substantial tortuous pathways for undesired molecules.

Tailoring of electrocatalytic oxygen evolution reaction performance of 2D conductive Co-catecholate metal-organic frameworks

Herein, we report the microwave hydrothermal synthesis of highly porous and conductive 2D Co-catecholate MOFs (Co-CATs) in the absence (Co-CAT-WO) and presence (Co-CAT-W) of N-methyl-2-pyrrolidone (NMP) polar solvent, and the study of these Co-CATs as electrocatalysts for oxygen evolution reaction (OER). The OER performance of Co-CAT-WO and Co-CAT-W is compared. The as-synthesized Co-CATs exhibit a 2D layered hexagonal structure. The electrical conductivity of Co-CAT-WO and Co-CAT-W is 6.9 and 5.8 S/m, respectively. The good conductivity and porous structure can initiate charge transport to achieve better OER performance under the 4e--transfer process. The as-prepared Co-CAT-WO and Co-CAT-W, respectively, show an overpotential of 455 and 424 mV at 10 mA/cm2 after performing the durability and chronoamperometry experiments for 13 h in 1 M KOH. From the electrochemical studies, it is apparent that the Co-CAT-W exhibits better OER performance with low overpotential, high current density, and excellent stability over extended cycling. Moreover, the lower HOMO-LUMO gap for Co-CAT-W than that of the Co-CAT-WO endorses its better electrocatalytic activity. The post-OER results show that the Co-CAT-W electrocatalyst acts as a "precatalyst" rather than the original catalyst, and it undergoes electrochemical transformation to metal hydroxide and metal oxyhydroxide after the OER studies, promoting the OER kinetics. The findings of this work offer valuable insights into the synthetic strategies for developing 2D conducting metal-catecholate MOF catalysts for efficient and sustainable OER processes, which is crucial in water splitting for sustainable energy production.

Engineering Ion Affinity of Zr-MOF Hybrid PDMS Membranes for the Selective Separation of Na+/Ca2.

Ion-selective separation, especially Na+/Ca2+ separation, is of significant importance in the realms of biomimetic research and the fabrication of biomimetic devices, underscoring the pivotal role that sodium and calcium ions play in cellular metabolism. However, the analogous ionic radii and charge densities shared by sodium and calcium ions significantly impede their effective discrimination, presenting formidable challenges for the precise engineering of ion separation materials, such as separation membranes. In this study, a polydimethylsiloxane (PDMS) separation membrane hybridized with zirconium-based metal-organic frameworks (UiO-66, UiO-66-NO2 and UiO-66-NH2) was constructed. Through the meticulous design of the MOF functional groups, the material's affinity for specific ions was modulated, thereby achieving efficient Na+/Ca2+ separation. Notably, the PDMS integrated with amino-modified Zr-MOF exhibited an efficacious selective separation of Na+ and Ca2+ ions. The interaction between the amino group of UiO-66-NH2 and Ca2+ gave rise to the observed superior selectivity toward Ca2+ cations and enhanced separation efficiencies of up to 64% compared to pristine PDMS for UiO-66-NH2-embedded membranes.

Optimizing Aqueous Zinc-Sulfur Battery Performance via Regulating Acetonitrile Co-Solvents and Carbon Nanotube Carriers.

Rechargeable aqueous zinc-sulfur batteries (AZSBs) are gaining attention due to their high energy density, ultra-stable discharge platform, and safety. However, poor liquid/solid reaction processes at the anode and cathode reduce reaction kinetics, and the severe dissolution of polysulfides causes shuttle effects during discharge/charge cycles, hindering practical applications. Improving performance requires optimizing both the cathode and electrolyte. Herein, we design an organic-inorganic hybrid electrolyte (zinc trifluoromethanesulfonate and trace iodine monomer dissolved in an acetonitrile/water co-solvent (AN-X)) and a partially exfoliated multi-walled carbon nanotube (PECNT) hosted sulfur (S@PECNTs) cathode for AZSBs. The sulfur is highly dispersed along the PECNTs with appropriate wettability at the electrode/electrolyte interface using AN-3 as the electrolyte. Meanwhile, this electrolyte inhibits hydrogen evolution at negative potentials and promotes uniform Zn ion stripping/plating. Expressively, the AN-3-based AZSB exhibits a high discharge capacity of 1370 mAh g-1 with excellent Coulombic efficiency (79.9 %), outstanding rate capability, and cycling performance. These improvements are attributed to the synergistic effect between the S@PECNTs and the AN-3 electrolyte, which reduces Rct to enhance reaction kinetics and blocks the dissolution and shuttle effect of polysulfides, ensuring a reversible reaction between zinc and sulfur.

A tripartite synergistic optimization strategy for zinc-iodine batteries

The energy industry has taken notice of zinc-iodine (Zn-I2) batteries for their high safety, low cost, and attractive energy density. However, the shuttling of I3− by-products at cathode electrode and dendrite issues at Zn metal anode result in short cycle lifespan. Here, a tripartite synergistic optimization strategy is proposed, involving a MXene cathode host, a n-butanol electrolyte additive, and the in-situ solid electrolyte interface (SEI) protection. The MXene possesses catalytic ability to enhance the reaction kinetics and reduce I3− by-products. Meanwhile, the partially dissolved n-butanol additive can work synergistically with MXene to inhibit the shuttling of I3−. Besides, the n-butanol and I− in the electrolyte can synergistically improve the solvation structure of Zn2+. Moreover, an organic-inorganic hybrid SEI is in situ generated on the surface of the Zn anode, which induces stable non-dendritic zinc deposition. As a result, the fabricated batteries exhibit a high capacity of 0.30 mAh cm−2 and a superior energy density of 0.34 mWh cm−2 at a high specific current of 5 A g−1 across 30,000 cycles, with a minimal capacity decay of 0.0004% per cycle. This work offers a promising strategy for the subsequent research to comprehensively improve battery performance.