In recent years,reducing carbon emissions to achieve carbon neutrality has become an urgent issue for environmental protection and sustainable development.Converting CO_(2) into valuable chemical products through elec...In recent years,reducing carbon emissions to achieve carbon neutrality has become an urgent issue for environmental protection and sustainable development.Converting CO_(2) into valuable chemical products through electrocatalysis powered by renewable electricity exhibits great potential.However,the electroreduction of CO_(2) heavily relies on efficient catalysts to overcome the required energy barrier due to the high stability of CO_(2).p-block metal-based MOFs and MOF-derived catalysts have been proven to be efficient catalysts for electrochemical CO_(2) reduction reaction(CO_(2)RR)due to their unique electronic structure and clear active sites.However,factors such as conductivity and stability limit the practical application of p-block metal-based MOFs and MOF-derived catalysts.In this review,we summarize the latest progress of MOFs and MOF-derived catalysts based on typical p-block metals in the field of CO_(2)RR.Then the modification strategies for MOFs-based catalysts and the related catalytic mechanism are briefly introduced.Furthermore,we offer the challenges and prospects of p-block metal-based MOFs and MOF-derived catalysts in the hope of providing guidance for potential applications.展开更多
Metal-Organic Frameworks(MOFs)have emerged as promising materials for gas adsorption and separation due to their exceptional surface area,tunable porosity,and versatility in functionalization.This paper explores the m...Metal-Organic Frameworks(MOFs)have emerged as promising materials for gas adsorption and separation due to their exceptional surface area,tunable porosity,and versatility in functionalization.This paper explores the mechanisms of gas adsorption in MOFs,including physical adsorption,chemisorption,and synergistic effects,which contribute to their efficiency in capturing and separating gases.The applications of MOFs in key areas such as carbon dioxide capture,hydrogen storage,natural gas separation,and air purification are discussed,highlighting their potential to address pressing environmental and energy challenges.Additionally,the use of MOFs in selective gas separation,membranes,and adsorption-based technologies like Pressure Swing Adsorption(PSA)and Vacuum Swing Adsorption(VSA)is explored,emphasizing their advantages over traditional materials.Despite challenges related to scalability,stability,and cost,MOFs hold great promise for advancing gas separation technologies in the near future,offering more efficient,sustainable,and environmentally friendly solutions.展开更多
The reaction of Mg^(2+)and 5-{1,3-dioxo-1H-benzo[de]isoquinolin-2(3H)-yl}terephthalic acid(H_(2)L)leads to two metal-organic frameworks,[Mg(L)(DMF)_(2)(H_(2)O)_(2)]_(2)·5DMF·2H_(2)O(1)with a 1D structure and...The reaction of Mg^(2+)and 5-{1,3-dioxo-1H-benzo[de]isoquinolin-2(3H)-yl}terephthalic acid(H_(2)L)leads to two metal-organic frameworks,[Mg(L)(DMF)_(2)(H_(2)O)_(2)]_(2)·5DMF·2H_(2)O(1)with a 1D structure and[Mg_(2)(L)_(2)(DMSO)_(3)(H_(2)O)](2)with a 2D(4,4)-net structure.Interestingly,the two compounds exhibit distinct luminescent responses to external mechanical stimuli.1 exhibited exceptional resistance mechanical chromic luminescence(RMCL),which can be attributed to the predominant hydrogen bonds and the presence of high-boiling-point solvent molecules within its structure.2 had a reversible MCL property,which can be attributed to the dominantπ-πweak interactions,coupled with the reversible destruction/restoration of its crystallinity under grinding/fumigation.CCDC:2410963,1;2410964,2.展开更多
Cancer is one of the most complex diseases and the second leading cause of mortality worldwide.Due to its poor prognosis and challenges in diagnosis,eradicating cancer remains highly difficult.The limitations associat...Cancer is one of the most complex diseases and the second leading cause of mortality worldwide.Due to its poor prognosis and challenges in diagnosis,eradicating cancer remains highly difficult.The limitations associated with conventional therapies have led to the emergence of copious therapeutic strategies such as chemotherapy,phototherapy,starvation therapy,radiotherapy and immunotherapy;however,limited therapeutic efficacy,poor tumor cell selectivity and substantial adverse effects remain significant concern.Attributed to the expeditious advancement of nanotechnology,the amalgamation of nanomaterials with therapeutic approaches provides an opportunity to address the shortcomings of conventional chemotherapy.Metal-organic frameworks(MOFs),which consist of bridging ligands and ions/clusters connected by coordination bonds,have been widely used in cancer therapy to address the limitations of currently therapeutic interventions,such as poor efficacy,low stability and severe side effects.This potential arises from their tuneable porosities,high specific surface area-to-volume ratio,tailorable diameters,tractable morphologies,variegated compositions,biocompatibility and facile functionalization.We summarized the role of MOF-based nanoplatforms along with mechanistic insights into emerging avenues-such as cuproptosis,ferroptosis,cell-penetrating and biomimetic MOFs,and tumor microenvironment-responsive MOFs-alongside recent advancements in mono-and multifunctional cancer therapeutics.Theragnostic and imaging functionalities,as well as regulatory considerations and future prospects of MOF-based nanoplatforms utilized in cancer treatment,are also discussed.展开更多
Constructing hierarchical nanostructures with highly exposed surfaces is a promising strategy for developing advanced cathode materials in aqueous batteries.Herein,we employed a competitive coordination strategy to op...Constructing hierarchical nanostructures with highly exposed surfaces is a promising strategy for developing advanced cathode materials in aqueous batteries.Herein,we employed a competitive coordination strategy to optimize the characteristics of nickel metal-organic framework(Ni-MOF).Specifically,the acetate ions were employed as precise regulators,exerting a distinct influence on the morphology of the Ni-MOF and leading to a structural transition from a block structure to a two-dimensional(2D)layered structure.The optimized Ni-MOF exhibits a unique superstructure composed of hierarchical 2D layers assembled into flower-like architectures.This distinctive superstructure increases the electrochemically active surface area of Ni-MOF(N-2)and provides abundant pathways for electron/ion transfer,thereby facilitating efficient electrochemical reactions.Remarkably,the assembled aqueous alkaline N-2//Zn battery demonstrated enhanced specific capacity(0.446 mAh·cm^(-2)at 1 mA·cm^(-2))and excellent maximum energy/power density(0.789 mWh·cm^(-2)/17.262 mW·cm^(-2)).This work not only offers valuable insights into regulating MOF morphology,but also makes a contribution toward enhancing the application potential of MOFs in aqueous batteries.展开更多
Themetal-organic frameworks(MOFs)MIL-100 andNH2-MIL-125 have hierarchical structure pores with high adsorption capacities and have therefore been suggested for drug delivery,gas storage,catalysis and chemical sensing....Themetal-organic frameworks(MOFs)MIL-100 andNH2-MIL-125 have hierarchical structure pores with high adsorption capacities and have therefore been suggested for drug delivery,gas storage,catalysis and chemical sensing.The widespread applications of these MOFs raise concerns about the possible release into the environment and subsequent human exposure.Yet,the available knowledge of the toxicity of these MOFs is rather scarce despite the encouraging applications.Here,we investigated the hematopoietic effects in different organs induced by MIL-100 and NH_(2)-MIL-125 in mice after intratracheal instillation.The hematopoietic cells in the bonemarrow(BM),lungs,and spleen were analyzed through flow cytometry method.Compared to NH2-MIL-125,MIL-100 triggered changes in more types of hematopoietic cells in the BM and spleen,but comparable changes in the lungs.In the BM and lungs,both the twoMOFs suppressedmyelopoiesis on day 1,but promotedmyelopoiesis on day 7.In the spleen,by contrast,continuous suppressedmyelopoiesis were found on day 1 and day 7.Moreover,changes in megakaryocyte progenitors(MkPs)were only detected in the lungs.These results unveil the potential disruption of hematopoietic homeostasis during inhalation of the two MOFs,which provided in vivo biological effect data for further evaluation of the biosafety of MOFs for future medical applications.展开更多
Energy conversion and environmental pollution present significant challenges that necessitate the development of materials with optimal characteristics for effective applications in solar energy-driven photocatalysis....Energy conversion and environmental pollution present significant challenges that necessitate the development of materials with optimal characteristics for effective applications in solar energy-driven photocatalysis.Metal-organic frameworks(MOFs)serve as excellent platforms for the development of various MOF-derived materials,which have garnered extensive attention due to their unique structural features,high crystallinity,large surface areas,diverse morphologies,adjustable dimensions,tunable textural characteristics,and inherent catalytic activity.However,the sluggish charge kinetics and poor stability of MOFs and MOF-derived photocatalysts restrict their photocatalytic activity,thereby limiting their applications in the field of photocatalysis.Consequently,substantial research efforts have been directed toward maximizing the advantages of these intriguing materials while addressing their shortcomings.This review provides a comprehensive summary and analysis of various synthesis strategies of MOFs and their derivatives.Effective modification strategies to enhance the performance of these novel materials are also summarized.This review systematically explores the current advancements in the application of MOFs and their derivatives for photocatalytic water splitting,photocatalytic CO_(2)reduction,and environmental water pollution treatment.Finally,it discusses the challenges and future prospects of MOFs and MOF-derived materials in photocatalytic applications.Researchers should systematically optimize synthetic strategies and functionalize MOFs and their derivatives to enhance their application in energy conversion and environmental pollution control,thereby underscoring their extensive potential.Future research will increasingly concentrate on the intelligent design and functionalization of MOFs to attain superior catalytic performance and tackle the urgent energy and environmental challenges confronting the world.展开更多
The effi ciency of photocatalytic ammonia(NH_(3))synthesis is severely limited by the extremely diffi cult activation of N_(2) owing to its high N≡N triple bond energy.To address this challenge,we propose an N-doping...The effi ciency of photocatalytic ammonia(NH_(3))synthesis is severely limited by the extremely diffi cult activation of N_(2) owing to its high N≡N triple bond energy.To address this challenge,we propose an N-doping strategy to facilitate the N_(2) activation.Our strategy involves optimizing the electronic structure of the metal active sites by modulating the coordination element.First,we introduce fi ve diff erent N-coordination ligands with distinct steric hindrances and N electron densities(2-methyl-imidazole(MI),isoindolin-1-one(II),1,2-benzisothiazolin-3-one(BIT),benzo[d]isoxazol-3-ol(BIX),and terephthalamide(TA))into an amino-functionalized metal-organic framework(MOF),NH_(2)-MIL-68(NM),to construct the N-coordination via the partial replacement of the O-coordination in the metal clusters.Electrochemical impedance spectroscopy and photocur-rent analysis demonstrate that N-doping enhances electron transfer and carrier separation.Moreover,incorporating ligands with moderate sizes and steric hindrances(II,BIT,and BIX)more eff ectively boosts the carrier separation efficiency than incorporating small(MI)or large(TA)ligands.Furthermore,the N-doped MOF modifi ed with BIT(in which N exhibits a moderate electron density)exhibits the strongest carrier separation capability.Concurrently,the X-ray photoelectron spec-troscopy,density functional theory,and N_(2) temperature-programmed desorption results confi rm that the established low-electronegativity N-coordination elevates the electron density of the metal active sites,which consequently enhances the N_(2) activation process.The systematic optimization of the N-coordinating ligand species and doping concentrations allows the optimal NM-0.5BIT to achieve a NH 3 production rate of 175.5μmol/(g·h).The proposed N-doping strategy off ers several insights into the activation of inert molecules and the development of organic framework photocatalysts.展开更多
A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+)...A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+).Characterization of the materials was carried out using techniques such as X-ray diffraction(XRD),Fourier transform infrared(FTIR),scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS),thermogravimetric analysis(TGA)and Brunauer-Emmett-Teller(BET).The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and mo rphology of MIL-101(Cr).Adsorption experiments were conducted to explore parameters including equilibrium pH,initial Eu3+concentration,and duration,with comprehensive analyses of adsorption kinetics,isotherms,and mechanisms.Findings reveal that Poly(IL1-AA)@MIL-101(Cr),Poly(IL3-AA)@MIL-101(Cr),and Poly(IL5-AA)@MIL-101(Cr)achieve adsorption equilibrium for Eu3+at approximately 9 h with an equilibrium pH of 6.2.The adso rption of Eu^(3+)predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model.Moreover,the prepared composite material exhibits superior adsorption selectivity for Eu^(3+)over other metal ions in the mixture(K^(+),Mg^(2+),Ni^(2+),Co^(2+),Zn^(2+),La^(3+),and Nd^(3+)).Even after five adsorption-desorption cycles,the composite material maintains satis factory adsorption performance.展开更多
The facets effect on the catalytic properties of inorganic compounds and metal-organic frameworks(MOFs)has been widely demonstrated,but the intrinsic facets effect free of interference of capping agents has not been d...The facets effect on the catalytic properties of inorganic compounds and metal-organic frameworks(MOFs)has been widely demonstrated,but the intrinsic facets effect free of interference of capping agents has not been discussed.Here we give a proof-of-concept illustration on the intrinsic facets effect by employing the popularly investigated NH2-MIL-125(Ti)MOFs with{001},{111}and{100}facets controllably exposed as model photocatalysts,which were synthesized via a simple supersaturation strategy free of any capping agents.Compared to conventional synthetic routes with capping agents employed,the NH2-MIL-125(Ti)MOFs obtained in this work exhibit remarkably different physical and chemical properties such as surface wettability,charge separation as well as trend of facets effect on photocatalytic water splitting performance.The main reason has been unraveled to originate from unavoidable residue/influence of capping agents during the conventional facets-controlled synthetic routes leading to changed local surface structural environment as well as distinct charge separation property.Our results demonstrate the importance and feasibility of facets-controllable synthesis free of capping agents in getting insight into the intrinsic facets effect of MOFs-related materials.展开更多
Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined acti...Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.展开更多
Metal-organic frameworks(MOFs)have emerged as promising materials owing to their high surface areas,tunable pore sizes,and diverse functionalities.However,their practical deployment is frequently hindered by intrinsic...Metal-organic frameworks(MOFs)have emerged as promising materials owing to their high surface areas,tunable pore sizes,and diverse functionalities.However,their practical deployment is frequently hindered by intrinsic microporosity and structural fragility.In this review,we systematically analyze recent advancements in MOF etching techniques,which strategically modify framework architectures to enhance mass transport,expose active sites,and improve stability.The discussion encompasses a range of methods―including acid,base,ion,solvent,steam,selective,in-situ,pyrolysis,and physical etching―with emphasis on the underlying mechanisms that govern the formation of hierarchical pore structures,defect engineering,and heterojunction formation.Notably,etching approaches facilitate precise control over crystal morphology and surface chemistry,thereby optimizing MOF performance in catalysis,electrocatalysis,photocatalysis,adsorption,energy storage,sensing,and biomedical applications.We also outline challenges such as etchant toxicity,over-etching risks,and scalability,while highlighting emerging strategies and computational simulations to refine the etching process.Ultimately,this review underscores the transformative impact of etching on MOF properties,paving the way for the design of next-generation multifunctional materials that address critical issues in environmental remediation,energy conversion,and beyond.展开更多
The development of solid frustrated Lewis pairs(FLPs)catalysts with porous structures is a promising strategy for advancing green hydrogenation technologies and has garnered significant attention.Leveraging the divers...The development of solid frustrated Lewis pairs(FLPs)catalysts with porous structures is a promising strategy for advancing green hydrogenation technologies and has garnered significant attention.Leveraging the diverse oxidation states and structural tunability of cerium-based metal-organic frameworks(Ce-MOFs),this study employed a competitive coordination strategy utilizing a single carboxylate functional group ligand to construct a series of MOF-808-X(X=-NH_(2),-OH,-Br,and-NO_(2))featuring rich solid-state FLPs for hydrogenation of unsaturated olefins.The-X functional group serves as a microenvironment,enhancing hydrogenation activity by modulating the electronic properties and acid-base characteristics of the FLP sites.The unique redox properties of elemental cerium facilitate the exposure of unsaturated Ce sites(Ce-CUS,Lewis acid(LA))and adjacent Ce-OH(Lewis base(LB))sites within the MOFs,generating abundant solid-state FLP(Ce-CUS/Ce-OH)sites.Experimental results demonstrate that Ce-CUS and Ce-OH interact with theσandσ^(*)orbitals of H-H,and this"push-pull"synergy promotes heterolytic cleavage of the H-H bond.The lone pair electrons of the electron-donating functional group are transmitted through the molecular backbone to the LB site,thereby increasing its strength and reducing the activation energy required for H_(2)heterolytic cleavage.Notably,at 100℃and 2 MPa H_(2),MOF-808-NH_(2)achieves complete conversion of styrene and dicyclopentadiene,significantly outperforming MOF-808.Based on in-situ analysis and density functional theory calculations,a plausible reaction mechanism is proposed.This research enriches the theoretical framework for unsaturated olefin hydrogenation catalysts and contributes to the development of efficient catalytic systems.展开更多
Baicalin,a major flavonoid compound found in Scutellariae radix,is the first SARS-CoV-23CLpro virus inhibitor.Therefore,developing an accurate and reliable strategy to detect baicalin in biological systems is vital.He...Baicalin,a major flavonoid compound found in Scutellariae radix,is the first SARS-CoV-23CLpro virus inhibitor.Therefore,developing an accurate and reliable strategy to detect baicalin in biological systems is vital.Herein,we report the first indolyl-lanthanide metal-organic framework(MOF)materials and their application as baicalin sensors.The results of this study indicate that the new crystal structure has good stability and luminous performance.The detection limits of baicalin in serum and urine are 0.05 and 0.04μmol/L,respectively,suggesting high sensitivity and selectivity.Various background substances present in practical samples,such as anions,cations,and amino acids,do not interfere with the photoluminescence analytical signal of Eu^(3+).We identified that the quenching of the Eu-MOF is due to the inner filter effect,absorption energy competition,and photoinduced electron transfer among the baicalin,ligand,and MOF through powder X-ray diffraction analysis,Fourier transform infrared spectroscopy,luminescence lifetimes,ultraviolet studies,and computational analysis.Thus,we designed a convenient,sensitive,and facile detection method using the Eu-MOF and demonstrate that Eu^(3+)-based materials are promising sensors for baicalin detection in actual serum and urine.Additionally,the prepared Eu-MOF@polyvinyl alcohol composite matrix membrane test film has considerable practical application value for the portable detection of baicalin.展开更多
Iron-porphyrin metal-organic frameworks(MOFs)have emerged as a remarkable class of semiconductors with adjustable photoelectrical properties and peroxidase-mimicking activities,yet their full potential remains largely...Iron-porphyrin metal-organic frameworks(MOFs)have emerged as a remarkable class of semiconductors with adjustable photoelectrical properties and peroxidase-mimicking activities,yet their full potential remains largely unexplored.The organic photoelectrochemical transistor(OPECT)has been proven to be a prominent platform for diverse applications.Herein,iron-porphyrin MOFs,as bifunctional photo-gating module and horseradish peroxidase-mimicking nanozyme,is explored for novel OPECT bioanalysis.Exemplified by alpha-fetoprotein(AFP)-dependent sandwich immunorecognition and therein glucose oxidase(GOx)-generated H_(2)O_(2)to etch CdS quantum dots on the surface of iron-porphyrin MOFs,this OPECT bioanalysis achieved high-performance AFP detection with a low detection limit of 24 fg/mL.This work featured a bifunctional iron-porphyrin MOFs gated OPECT,which is envisioned to inspire more interest in developing the diverse MOFs-nanozymes toward novel optoelectronics and beyond.展开更多
Precise regulation of the platform capacity/voltage of electrode materials contributes to the efficient operation of sodium-ion fast-charging devices.However,the design of such electrode materials is still in a blank ...Precise regulation of the platform capacity/voltage of electrode materials contributes to the efficient operation of sodium-ion fast-charging devices.However,the design of such electrode materials is still in a blank stage.Herein,based on tunable metal-organic frameworks,we have designed a novel material system-two-dimensional high-entropy metal-organic frameworks(HE-MOFs),which exhibits unique properties in sodium storage and is of vital importance for realizing fastcharging batteries.Furthermore,we have found that the highentropy effect can regulate the electronic structure,the sodiumion migration environment,and the sodium-ion storage active sites,thereby meeting the requirements of electrode materials for sodium-ion fast-charging devices.Impressively,the HE-MOFs material still maintains a reversible specific capacity of 89 mAh g^(−1)at a current density of 20 A g^(−1).It presents an ideal sodium storage voltage plateau of approximately 0.5 V,and its platform capacity is increased to 122.7 mAh g^(−1),far superior to that of Mn-MOFs(with no platform capacity).This helps to reduce safety hazards during the fastcharging process and demonstrates its great application value in the fields of fastcharging sodium-ion batteries and capacitors.Our research findings have broken the barriers to the application of non-conductive MOFs as energy storage materials,enhanced the understanding of the regulation of platform capacity and voltage,and paved the way for the realization of high-security sodium-ion fast-charging devices.展开更多
Chirality is not only a natural phenomenon but also a bridge between chemistry and life sciences.An effective way to obtain a single enantiomer is through racemates resolution.Recent literature shows that chiral metal...Chirality is not only a natural phenomenon but also a bridge between chemistry and life sciences.An effective way to obtain a single enantiomer is through racemates resolution.Recent literature shows that chiral metal-organic frameworks(CMOFs)have many applications in various fields because of their diverse topologies and functionalities.This review outlines the design idea and summarizes the latest synthesis strategies and applications of CMOFs.It highlights key advances and issues in the separation domain.In conclusion,the review provides perspectives on the challenges and prospective advancements of CMOFs materials and CMOFs-based separation technologies.展开更多
Chiral metal-organic frameworks (CMOFs), a class of highly crystalline and porous materials with tailorable chiral characteristics, have currently become an interdisciplinary between chirality chemistry, coordination ...Chiral metal-organic frameworks (CMOFs), a class of highly crystalline and porous materials with tailorable chiral characteristics, have currently become an interdisciplinary between chirality chemistry, coordination chemistry, and material chemistry, which involve in many subjects including chemistry, physics, optics, medi-cine, pharmacology, biology, crystal engineering, environmental science, etc. Their special structural features such as porosity, modularity, and chirality have endowed them with a variety of unique effects in promoting enantioselective processes, particularly asymmetric catalysis. Here, we provide a brief review of the state of CMOF field from the privileged ligand design to the heterogeneous enantioselective catalysis. We hope that this review will provide researchers a better understanding of CMOF chemistry and facilitate the future research endeavors for rationally designing privileged chiral framework materials for challenging catalytic applications.展开更多
The fabrication of bioreceptor-free method for accurate and sensitive detection of ochratoxin A(OTA) in cereal is critical, but still a significant challenge to mitigate risks to food industries and public health. In ...The fabrication of bioreceptor-free method for accurate and sensitive detection of ochratoxin A(OTA) in cereal is critical, but still a significant challenge to mitigate risks to food industries and public health. In this study, a smartphone-ratiometric fiuorescence sensor for the ultrasensitive detection of OTA is developed based on a porphyrinic metal-organic framework and silica nanoparticle composite(Zr-MOF/Si NPs)away from the use of antibodies and aptamers. Due to the excellent recognition ability of Zr-MOF and good storage stability of Si NPs, OTA is detected by Zr-MOF/Si NPs with a wide linear range of 0.05–1000 ng/m L and low detection limit of 0.016 ng/m L. Moreover, the red–blue ratio values of the fiuorescence images are extracted through the smartphone color recognizer application with a limit of detection of 1.74 ng/m L, lower than the permissible content of OTA in cereal prescribed by World Health Organization. This sensing platform has been successfully applied in maize samples with superior repeatability and satisfactory recoveries, providing a novel way for simple and label-free analysis of OTA in cereal.展开更多
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 receive...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 themass 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 BulkMOFs).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 907.2μg/(hr·mg_(cat))(7793.8μg/(hr·mg_(metal)))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.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22061019 and 22261021)the Jiangxi Provincial Natural Science Foundation(Nos.20224BAB203002,20232ACB203018,20232BAB203005,and 20224BAB213001)+5 种基金the Jiangxi Province Key Laboratory of Functional Crystalline Materials Chemistry(No.2024SSY05161)the Ganzhou Key Research and Development Program(No.2023PNS26963)the Youth Jinggang Scholars Program in Jiangxi Province(No.QNJG2019053)the Two Thousand Talents Program in Jiangxi Province(No.jxsq2019201068)the Doctor’s Starting Research Foundation of Jiangxi University of Science and Technology(No.205200100597)the Science and Technology Research Project of Jiangxi Provincial Department of Education(No.GJJ2200860).
文摘In recent years,reducing carbon emissions to achieve carbon neutrality has become an urgent issue for environmental protection and sustainable development.Converting CO_(2) into valuable chemical products through electrocatalysis powered by renewable electricity exhibits great potential.However,the electroreduction of CO_(2) heavily relies on efficient catalysts to overcome the required energy barrier due to the high stability of CO_(2).p-block metal-based MOFs and MOF-derived catalysts have been proven to be efficient catalysts for electrochemical CO_(2) reduction reaction(CO_(2)RR)due to their unique electronic structure and clear active sites.However,factors such as conductivity and stability limit the practical application of p-block metal-based MOFs and MOF-derived catalysts.In this review,we summarize the latest progress of MOFs and MOF-derived catalysts based on typical p-block metals in the field of CO_(2)RR.Then the modification strategies for MOFs-based catalysts and the related catalytic mechanism are briefly introduced.Furthermore,we offer the challenges and prospects of p-block metal-based MOFs and MOF-derived catalysts in the hope of providing guidance for potential applications.
文摘Metal-Organic Frameworks(MOFs)have emerged as promising materials for gas adsorption and separation due to their exceptional surface area,tunable porosity,and versatility in functionalization.This paper explores the mechanisms of gas adsorption in MOFs,including physical adsorption,chemisorption,and synergistic effects,which contribute to their efficiency in capturing and separating gases.The applications of MOFs in key areas such as carbon dioxide capture,hydrogen storage,natural gas separation,and air purification are discussed,highlighting their potential to address pressing environmental and energy challenges.Additionally,the use of MOFs in selective gas separation,membranes,and adsorption-based technologies like Pressure Swing Adsorption(PSA)and Vacuum Swing Adsorption(VSA)is explored,emphasizing their advantages over traditional materials.Despite challenges related to scalability,stability,and cost,MOFs hold great promise for advancing gas separation technologies in the near future,offering more efficient,sustainable,and environmentally friendly solutions.
文摘The reaction of Mg^(2+)and 5-{1,3-dioxo-1H-benzo[de]isoquinolin-2(3H)-yl}terephthalic acid(H_(2)L)leads to two metal-organic frameworks,[Mg(L)(DMF)_(2)(H_(2)O)_(2)]_(2)·5DMF·2H_(2)O(1)with a 1D structure and[Mg_(2)(L)_(2)(DMSO)_(3)(H_(2)O)](2)with a 2D(4,4)-net structure.Interestingly,the two compounds exhibit distinct luminescent responses to external mechanical stimuli.1 exhibited exceptional resistance mechanical chromic luminescence(RMCL),which can be attributed to the predominant hydrogen bonds and the presence of high-boiling-point solvent molecules within its structure.2 had a reversible MCL property,which can be attributed to the dominantπ-πweak interactions,coupled with the reversible destruction/restoration of its crystallinity under grinding/fumigation.CCDC:2410963,1;2410964,2.
基金funding support by the Department of Pharmaceuticals(DoP),Ministry of Chemicals and Fertilizers,Govt.of India to“Pharmaceutical Innovation and Translational Research Lab”(PITRL),National Institute of Pharmaceutical Education and Research(NIPER),Hyderabad,INDIA.
文摘Cancer is one of the most complex diseases and the second leading cause of mortality worldwide.Due to its poor prognosis and challenges in diagnosis,eradicating cancer remains highly difficult.The limitations associated with conventional therapies have led to the emergence of copious therapeutic strategies such as chemotherapy,phototherapy,starvation therapy,radiotherapy and immunotherapy;however,limited therapeutic efficacy,poor tumor cell selectivity and substantial adverse effects remain significant concern.Attributed to the expeditious advancement of nanotechnology,the amalgamation of nanomaterials with therapeutic approaches provides an opportunity to address the shortcomings of conventional chemotherapy.Metal-organic frameworks(MOFs),which consist of bridging ligands and ions/clusters connected by coordination bonds,have been widely used in cancer therapy to address the limitations of currently therapeutic interventions,such as poor efficacy,low stability and severe side effects.This potential arises from their tuneable porosities,high specific surface area-to-volume ratio,tailorable diameters,tractable morphologies,variegated compositions,biocompatibility and facile functionalization.We summarized the role of MOF-based nanoplatforms along with mechanistic insights into emerging avenues-such as cuproptosis,ferroptosis,cell-penetrating and biomimetic MOFs,and tumor microenvironment-responsive MOFs-alongside recent advancements in mono-and multifunctional cancer therapeutics.Theragnostic and imaging functionalities,as well as regulatory considerations and future prospects of MOF-based nanoplatforms utilized in cancer treatment,are also discussed.
基金supported by the National Natural Science Foundation of China(No.52371240)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_3510).
文摘Constructing hierarchical nanostructures with highly exposed surfaces is a promising strategy for developing advanced cathode materials in aqueous batteries.Herein,we employed a competitive coordination strategy to optimize the characteristics of nickel metal-organic framework(Ni-MOF).Specifically,the acetate ions were employed as precise regulators,exerting a distinct influence on the morphology of the Ni-MOF and leading to a structural transition from a block structure to a two-dimensional(2D)layered structure.The optimized Ni-MOF exhibits a unique superstructure composed of hierarchical 2D layers assembled into flower-like architectures.This distinctive superstructure increases the electrochemically active surface area of Ni-MOF(N-2)and provides abundant pathways for electron/ion transfer,thereby facilitating efficient electrochemical reactions.Remarkably,the assembled aqueous alkaline N-2//Zn battery demonstrated enhanced specific capacity(0.446 mAh·cm^(-2)at 1 mA·cm^(-2))and excellent maximum energy/power density(0.789 mWh·cm^(-2)/17.262 mW·cm^(-2)).This work not only offers valuable insights into regulating MOF morphology,but also makes a contribution toward enhancing the application potential of MOFs in aqueous batteries.
基金supported by the National Natural Science Foundation of China(Nos.22193053,42377386,and 22325606)the National Key Research and Development Programof China(No.2023YFA0915101)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0750000).
文摘Themetal-organic frameworks(MOFs)MIL-100 andNH2-MIL-125 have hierarchical structure pores with high adsorption capacities and have therefore been suggested for drug delivery,gas storage,catalysis and chemical sensing.The widespread applications of these MOFs raise concerns about the possible release into the environment and subsequent human exposure.Yet,the available knowledge of the toxicity of these MOFs is rather scarce despite the encouraging applications.Here,we investigated the hematopoietic effects in different organs induced by MIL-100 and NH_(2)-MIL-125 in mice after intratracheal instillation.The hematopoietic cells in the bonemarrow(BM),lungs,and spleen were analyzed through flow cytometry method.Compared to NH2-MIL-125,MIL-100 triggered changes in more types of hematopoietic cells in the BM and spleen,but comparable changes in the lungs.In the BM and lungs,both the twoMOFs suppressedmyelopoiesis on day 1,but promotedmyelopoiesis on day 7.In the spleen,by contrast,continuous suppressedmyelopoiesis were found on day 1 and day 7.Moreover,changes in megakaryocyte progenitors(MkPs)were only detected in the lungs.These results unveil the potential disruption of hematopoietic homeostasis during inhalation of the two MOFs,which provided in vivo biological effect data for further evaluation of the biosafety of MOFs for future medical applications.
基金The financial support for this study by the Technology Project of Qingdao(22-3-7-cspz-9-nsh)the National Key Research and Development Program(2021YFB3500102)。
文摘Energy conversion and environmental pollution present significant challenges that necessitate the development of materials with optimal characteristics for effective applications in solar energy-driven photocatalysis.Metal-organic frameworks(MOFs)serve as excellent platforms for the development of various MOF-derived materials,which have garnered extensive attention due to their unique structural features,high crystallinity,large surface areas,diverse morphologies,adjustable dimensions,tunable textural characteristics,and inherent catalytic activity.However,the sluggish charge kinetics and poor stability of MOFs and MOF-derived photocatalysts restrict their photocatalytic activity,thereby limiting their applications in the field of photocatalysis.Consequently,substantial research efforts have been directed toward maximizing the advantages of these intriguing materials while addressing their shortcomings.This review provides a comprehensive summary and analysis of various synthesis strategies of MOFs and their derivatives.Effective modification strategies to enhance the performance of these novel materials are also summarized.This review systematically explores the current advancements in the application of MOFs and their derivatives for photocatalytic water splitting,photocatalytic CO_(2)reduction,and environmental water pollution treatment.Finally,it discusses the challenges and future prospects of MOFs and MOF-derived materials in photocatalytic applications.Researchers should systematically optimize synthetic strategies and functionalize MOFs and their derivatives to enhance their application in energy conversion and environmental pollution control,thereby underscoring their extensive potential.Future research will increasingly concentrate on the intelligent design and functionalization of MOFs to attain superior catalytic performance and tackle the urgent energy and environmental challenges confronting the world.
基金the National Natural Science Foundation of China(Nos.21621004,22478295,and 22122809)the National Key Research and Development Program of China(Nos.2022YFC2105902 and 2024YFB4206301)+2 种基金Young Scientifi c and Technological Talents(Level One)in Tianjin(No.QN20230103)Program of Introducing Talents of Discipline to Universities(No.BP0618007)Haihe Laboratory of Sustainable Chemical Transformations.
文摘The effi ciency of photocatalytic ammonia(NH_(3))synthesis is severely limited by the extremely diffi cult activation of N_(2) owing to its high N≡N triple bond energy.To address this challenge,we propose an N-doping strategy to facilitate the N_(2) activation.Our strategy involves optimizing the electronic structure of the metal active sites by modulating the coordination element.First,we introduce fi ve diff erent N-coordination ligands with distinct steric hindrances and N electron densities(2-methyl-imidazole(MI),isoindolin-1-one(II),1,2-benzisothiazolin-3-one(BIT),benzo[d]isoxazol-3-ol(BIX),and terephthalamide(TA))into an amino-functionalized metal-organic framework(MOF),NH_(2)-MIL-68(NM),to construct the N-coordination via the partial replacement of the O-coordination in the metal clusters.Electrochemical impedance spectroscopy and photocur-rent analysis demonstrate that N-doping enhances electron transfer and carrier separation.Moreover,incorporating ligands with moderate sizes and steric hindrances(II,BIT,and BIX)more eff ectively boosts the carrier separation efficiency than incorporating small(MI)or large(TA)ligands.Furthermore,the N-doped MOF modifi ed with BIT(in which N exhibits a moderate electron density)exhibits the strongest carrier separation capability.Concurrently,the X-ray photoelectron spec-troscopy,density functional theory,and N_(2) temperature-programmed desorption results confi rm that the established low-electronegativity N-coordination elevates the electron density of the metal active sites,which consequently enhances the N_(2) activation process.The systematic optimization of the N-coordinating ligand species and doping concentrations allows the optimal NM-0.5BIT to achieve a NH 3 production rate of 175.5μmol/(g·h).The proposed N-doping strategy off ers several insights into the activation of inert molecules and the development of organic framework photocatalysts.
基金Project supported by the State Key Laboratory of Geohazard Prevention and Geoenvironment Protection(SKLGP2020Z003)。
文摘A novel composite material,Poly(IL-AA)@MIL-101(Cr),combining metal-organic framework,polymeric ionic liquid and acrylic acid,was synthesized for the selective and efficient adsorption of rare earths europium(Ⅲ)(Eu3+).Characterization of the materials was carried out using techniques such as X-ray diffraction(XRD),Fourier transform infrared(FTIR),scanning electron microscopy-energy dispersive X-ray spectroscopy(SEM-EDS),thermogravimetric analysis(TGA)and Brunauer-Emmett-Teller(BET).The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and mo rphology of MIL-101(Cr).Adsorption experiments were conducted to explore parameters including equilibrium pH,initial Eu3+concentration,and duration,with comprehensive analyses of adsorption kinetics,isotherms,and mechanisms.Findings reveal that Poly(IL1-AA)@MIL-101(Cr),Poly(IL3-AA)@MIL-101(Cr),and Poly(IL5-AA)@MIL-101(Cr)achieve adsorption equilibrium for Eu3+at approximately 9 h with an equilibrium pH of 6.2.The adso rption of Eu^(3+)predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model.Moreover,the prepared composite material exhibits superior adsorption selectivity for Eu^(3+)over other metal ions in the mixture(K^(+),Mg^(2+),Ni^(2+),Co^(2+),Zn^(2+),La^(3+),and Nd^(3+)).Even after five adsorption-desorption cycles,the composite material maintains satis factory adsorption performance.
文摘The facets effect on the catalytic properties of inorganic compounds and metal-organic frameworks(MOFs)has been widely demonstrated,but the intrinsic facets effect free of interference of capping agents has not been discussed.Here we give a proof-of-concept illustration on the intrinsic facets effect by employing the popularly investigated NH2-MIL-125(Ti)MOFs with{001},{111}and{100}facets controllably exposed as model photocatalysts,which were synthesized via a simple supersaturation strategy free of any capping agents.Compared to conventional synthetic routes with capping agents employed,the NH2-MIL-125(Ti)MOFs obtained in this work exhibit remarkably different physical and chemical properties such as surface wettability,charge separation as well as trend of facets effect on photocatalytic water splitting performance.The main reason has been unraveled to originate from unavoidable residue/influence of capping agents during the conventional facets-controlled synthetic routes leading to changed local surface structural environment as well as distinct charge separation property.Our results demonstrate the importance and feasibility of facets-controllable synthesis free of capping agents in getting insight into the intrinsic facets effect of MOFs-related materials.
基金supported by Henan Province Key Research and Development and Promotion of Science and Technology Project(No.25A150001)the National Natural Science Foundation of China(Nos.22409171,22125303,92361302,and 92061203).
文摘Single-atom catalysts(SACs),as the rising stars in the field of catalytic science,are leading catalytic technology into an un-precedented new era.However,the synthe-sis of high-performance SACs with well-de-fined active sites and high loadings under precise control has become a hotly debated topic in scientific research.Metal-organic frameworks(MOFs),with their exceptional properties such as ultrahigh specific surface areas,precisely controllable structural de-signs,and highly flexible functional cus-tomization capabilities,are regarded as one of the ideal matrices for supporting and sta-bilizing SACs.This review provides an in-sightful overview of the diverse preparation strategies for MOFs-derived SACs.It comprehen-sively analyzes the unique advantages and challenges of each method in achieving efficient synthesis of SACs,emphasizing the crucial role of optimized processes in unlocking the antici-pated performance of SACs.Furthermore,this review delves into a series of advanced charac-terization techniques,including aberration-corrected scanning transmission electron mi-croscopy(AC-STEM),electron energy loss spectroscopy(EELS),X-ray absorption spec-troscopy(XAS),and infrared absorption spectroscopy(IRAS),offering valuable insights into the atomic-scale fine structures and properties of SACs,significantly advancing the under-standing of SAC mechanisms.Moreover,this review focuses on exploring the potential appli-cations of MOFs-derived SACs in electrocatalysis frontier fields.This comprehensive exami-nation lays a solid theoretical foundation and provides a directional guidance for the rational design and controllable synthesis of high-performance MOFs-derived SACs.
基金the financial support of the National Natural Science Foundation of China(Nos.22308296)。
文摘Metal-organic frameworks(MOFs)have emerged as promising materials owing to their high surface areas,tunable pore sizes,and diverse functionalities.However,their practical deployment is frequently hindered by intrinsic microporosity and structural fragility.In this review,we systematically analyze recent advancements in MOF etching techniques,which strategically modify framework architectures to enhance mass transport,expose active sites,and improve stability.The discussion encompasses a range of methods―including acid,base,ion,solvent,steam,selective,in-situ,pyrolysis,and physical etching―with emphasis on the underlying mechanisms that govern the formation of hierarchical pore structures,defect engineering,and heterojunction formation.Notably,etching approaches facilitate precise control over crystal morphology and surface chemistry,thereby optimizing MOF performance in catalysis,electrocatalysis,photocatalysis,adsorption,energy storage,sensing,and biomedical applications.We also outline challenges such as etchant toxicity,over-etching risks,and scalability,while highlighting emerging strategies and computational simulations to refine the etching process.Ultimately,this review underscores the transformative impact of etching on MOF properties,paving the way for the design of next-generation multifunctional materials that address critical issues in environmental remediation,energy conversion,and beyond.
文摘The development of solid frustrated Lewis pairs(FLPs)catalysts with porous structures is a promising strategy for advancing green hydrogenation technologies and has garnered significant attention.Leveraging the diverse oxidation states and structural tunability of cerium-based metal-organic frameworks(Ce-MOFs),this study employed a competitive coordination strategy utilizing a single carboxylate functional group ligand to construct a series of MOF-808-X(X=-NH_(2),-OH,-Br,and-NO_(2))featuring rich solid-state FLPs for hydrogenation of unsaturated olefins.The-X functional group serves as a microenvironment,enhancing hydrogenation activity by modulating the electronic properties and acid-base characteristics of the FLP sites.The unique redox properties of elemental cerium facilitate the exposure of unsaturated Ce sites(Ce-CUS,Lewis acid(LA))and adjacent Ce-OH(Lewis base(LB))sites within the MOFs,generating abundant solid-state FLP(Ce-CUS/Ce-OH)sites.Experimental results demonstrate that Ce-CUS and Ce-OH interact with theσandσ^(*)orbitals of H-H,and this"push-pull"synergy promotes heterolytic cleavage of the H-H bond.The lone pair electrons of the electron-donating functional group are transmitted through the molecular backbone to the LB site,thereby increasing its strength and reducing the activation energy required for H_(2)heterolytic cleavage.Notably,at 100℃and 2 MPa H_(2),MOF-808-NH_(2)achieves complete conversion of styrene and dicyclopentadiene,significantly outperforming MOF-808.Based on in-situ analysis and density functional theory calculations,a plausible reaction mechanism is proposed.This research enriches the theoretical framework for unsaturated olefin hydrogenation catalysts and contributes to the development of efficient catalytic systems.
基金Project supported by Jilin Province Science and Technology Development Plan Project(20210201061GX)。
文摘Baicalin,a major flavonoid compound found in Scutellariae radix,is the first SARS-CoV-23CLpro virus inhibitor.Therefore,developing an accurate and reliable strategy to detect baicalin in biological systems is vital.Herein,we report the first indolyl-lanthanide metal-organic framework(MOF)materials and their application as baicalin sensors.The results of this study indicate that the new crystal structure has good stability and luminous performance.The detection limits of baicalin in serum and urine are 0.05 and 0.04μmol/L,respectively,suggesting high sensitivity and selectivity.Various background substances present in practical samples,such as anions,cations,and amino acids,do not interfere with the photoluminescence analytical signal of Eu^(3+).We identified that the quenching of the Eu-MOF is due to the inner filter effect,absorption energy competition,and photoinduced electron transfer among the baicalin,ligand,and MOF through powder X-ray diffraction analysis,Fourier transform infrared spectroscopy,luminescence lifetimes,ultraviolet studies,and computational analysis.Thus,we designed a convenient,sensitive,and facile detection method using the Eu-MOF and demonstrate that Eu^(3+)-based materials are promising sensors for baicalin detection in actual serum and urine.Additionally,the prepared Eu-MOF@polyvinyl alcohol composite matrix membrane test film has considerable practical application value for the portable detection of baicalin.
基金financially supported by the National Natural Science Foundation of China(Nos.22034003,22374066)the Fundamental Research Funds for the Central Universities(No.2022300285)+1 种基金the Excellent Research Program of Nanjing University(No.ZYJH004)State Key Laboratory of Analytical Chemistry for Life Science(No.5431ZZXM2203).
文摘Iron-porphyrin metal-organic frameworks(MOFs)have emerged as a remarkable class of semiconductors with adjustable photoelectrical properties and peroxidase-mimicking activities,yet their full potential remains largely unexplored.The organic photoelectrochemical transistor(OPECT)has been proven to be a prominent platform for diverse applications.Herein,iron-porphyrin MOFs,as bifunctional photo-gating module and horseradish peroxidase-mimicking nanozyme,is explored for novel OPECT bioanalysis.Exemplified by alpha-fetoprotein(AFP)-dependent sandwich immunorecognition and therein glucose oxidase(GOx)-generated H_(2)O_(2)to etch CdS quantum dots on the surface of iron-porphyrin MOFs,this OPECT bioanalysis achieved high-performance AFP detection with a low detection limit of 24 fg/mL.This work featured a bifunctional iron-porphyrin MOFs gated OPECT,which is envisioned to inspire more interest in developing the diverse MOFs-nanozymes toward novel optoelectronics and beyond.
基金supported by the National Natural Science Foundation of China(22378431,52004338,51622406,and 21673298)Hunan Provincial Natural Science Foundation(2022JJ20075 and 2023JJ40704)+2 种基金the Science and Technology Innovation Program of Hunan Province(2023RC3259)the Key R&D plan of Hunan Province(2024JK2096)Central South University Innovation-Driven Research Programme(2023CXQD008).
文摘Precise regulation of the platform capacity/voltage of electrode materials contributes to the efficient operation of sodium-ion fast-charging devices.However,the design of such electrode materials is still in a blank stage.Herein,based on tunable metal-organic frameworks,we have designed a novel material system-two-dimensional high-entropy metal-organic frameworks(HE-MOFs),which exhibits unique properties in sodium storage and is of vital importance for realizing fastcharging batteries.Furthermore,we have found that the highentropy effect can regulate the electronic structure,the sodiumion migration environment,and the sodium-ion storage active sites,thereby meeting the requirements of electrode materials for sodium-ion fast-charging devices.Impressively,the HE-MOFs material still maintains a reversible specific capacity of 89 mAh g^(−1)at a current density of 20 A g^(−1).It presents an ideal sodium storage voltage plateau of approximately 0.5 V,and its platform capacity is increased to 122.7 mAh g^(−1),far superior to that of Mn-MOFs(with no platform capacity).This helps to reduce safety hazards during the fastcharging process and demonstrates its great application value in the fields of fastcharging sodium-ion batteries and capacitors.Our research findings have broken the barriers to the application of non-conductive MOFs as energy storage materials,enhanced the understanding of the regulation of platform capacity and voltage,and paved the way for the realization of high-security sodium-ion fast-charging devices.
基金fund by the National Natural Science Foundation of China(Grant Nos.:82473880 and 82003705)the Shanghai Science and Technology Innovation Foundation(Grant Nos.:23010500200 and 23ZR1422700)the Postdoctoral Fellowship Program of CPSF(Program No.:GZC20231528).
文摘Chirality is not only a natural phenomenon but also a bridge between chemistry and life sciences.An effective way to obtain a single enantiomer is through racemates resolution.Recent literature shows that chiral metal-organic frameworks(CMOFs)have many applications in various fields because of their diverse topologies and functionalities.This review outlines the design idea and summarizes the latest synthesis strategies and applications of CMOFs.It highlights key advances and issues in the separation domain.In conclusion,the review provides perspectives on the challenges and prospective advancements of CMOFs materials and CMOFs-based separation technologies.
基金the National Key R&D Program of China(2023YFA1507601)the National Natural Science Foundation of China(22522108,52373213,22301176).
文摘Chiral metal-organic frameworks (CMOFs), a class of highly crystalline and porous materials with tailorable chiral characteristics, have currently become an interdisciplinary between chirality chemistry, coordination chemistry, and material chemistry, which involve in many subjects including chemistry, physics, optics, medi-cine, pharmacology, biology, crystal engineering, environmental science, etc. Their special structural features such as porosity, modularity, and chirality have endowed them with a variety of unique effects in promoting enantioselective processes, particularly asymmetric catalysis. Here, we provide a brief review of the state of CMOF field from the privileged ligand design to the heterogeneous enantioselective catalysis. We hope that this review will provide researchers a better understanding of CMOF chemistry and facilitate the future research endeavors for rationally designing privileged chiral framework materials for challenging catalytic applications.
基金funding from the National Natural Science Foundation of China (No. 31871877)the National Key Research and Development Program of China (No. 2019YFC1606303)。
文摘The fabrication of bioreceptor-free method for accurate and sensitive detection of ochratoxin A(OTA) in cereal is critical, but still a significant challenge to mitigate risks to food industries and public health. In this study, a smartphone-ratiometric fiuorescence sensor for the ultrasensitive detection of OTA is developed based on a porphyrinic metal-organic framework and silica nanoparticle composite(Zr-MOF/Si NPs)away from the use of antibodies and aptamers. Due to the excellent recognition ability of Zr-MOF and good storage stability of Si NPs, OTA is detected by Zr-MOF/Si NPs with a wide linear range of 0.05–1000 ng/m L and low detection limit of 0.016 ng/m L. Moreover, the red–blue ratio values of the fiuorescence images are extracted through the smartphone color recognizer application with a limit of detection of 1.74 ng/m L, lower than the permissible content of OTA in cereal prescribed by World Health Organization. This sensing platform has been successfully applied in maize samples with superior repeatability and satisfactory recoveries, providing a novel way for simple and label-free analysis of OTA in cereal.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.52370044 and 21976134)the State Key Laboratory of Pollution Control and Resource Reuse Foundation(Nos.PCRRK21003 and PCRRK21001)+1 种基金Shanghai Scientific Research Plan Project(No.23ZR1467000)the State Key Laboratory of Treatments and Recycling for Organic Effluents by Adsorption in Petroleum and Chemical Industry(No.SDHY2206).
文摘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 themass 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 BulkMOFs).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 907.2μg/(hr·mg_(cat))(7793.8μg/(hr·mg_(metal)))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.
