Integrated electrocatalysts(IECs)containing well-defined functional materials directly grown on the current collector have sparked increasing interest in the fields of electrocatalysis owing to efficient activity,high...Integrated electrocatalysts(IECs)containing well-defined functional materials directly grown on the current collector have sparked increasing interest in the fields of electrocatalysis owing to efficient activity,high stability and the fact that they are easily assembled into devices.Recently,metal organic frameworks(MOFs)provide a promising platform for constructing advanced IECs because of their properties of low cost,large surface area and efficient structural tunability.In this review,the design principles of state-of-the-art IECs based on MOFs are presented,including by hydrothermal/solvothermal,template-directed,electrospinning,electrodeposition and other methods.The high performance of MOF-derived IECs has also been demonstrated in electrocatalytic gasinvolved reactions.This is promising for green energy storage and conversion.The structure-activity relationship and performance improvement mechanism of IECs are uncovered by discussing some in situ technologies for IECs.Finally,we provide an outlook on the challenges and prospects in this booming field.展开更多
The aim of this study is a present of a simple solvothermal synthesis approach to preparation of Cu-based magnetic metal organic framework(MMOF)and subsequently its application as sorbent for ultrasound assisted magne...The aim of this study is a present of a simple solvothermal synthesis approach to preparation of Cu-based magnetic metal organic framework(MMOF)and subsequently its application as sorbent for ultrasound assisted magnetic solid phase extraction(UAMSPE)of ampicillin(AMP)from cow milk samples prior to high performance liquid chromatography-Ultraviolet(HPLC-UV)determination.Characteristics of prepared MMOF were fully investigated by different techniques which showed the exclusive properties of proposed sorbent in terms of proper functionality,desirable magnetic property and also high specific surface area.Different influential factors on extraction recovery including sorbent dosage,ultrasonic time,washing solvent volume and eluent solvent volume were assessed using central composite design(CCD)based response surface methodology(RSM)as an operative and powerful optimization tool.This is the first report for determination of AMP using MMOF.The proposed method addressed some drawbacks of other methods and sorbents for determination of AMP.The presented method decreases the extraction time(4 min)and also enhances adsorption capacity(250 mg/g).Moreover,the magnetic property of presented sorbent(15 emu/g)accelerates the extraction process which does not need filtration,centrifuge and precipitation procedures.Under the optimized conditions,the proposed method is applicable for linear range of 1.0-5000.0 μg/L with detection limit of 0.29 μg/L,satisfactory recoveries(≥95.0%)and acceptable repeatability(RSD less than 4.0%).The present study indicates highly promising perspectives of MMOF for highly effective analysis of AMP in complicated matrices.展开更多
The highly selective catalytic transfer hydrogenation(CTH)of furfural(FF)to furfuryl alcohol(FOL)is a significant route of biomass valorization.Herein,a series microporous Zr-metal organic framework(ZrMOF)functionaliz...The highly selective catalytic transfer hydrogenation(CTH)of furfural(FF)to furfuryl alcohol(FOL)is a significant route of biomass valorization.Herein,a series microporous Zr-metal organic framework(ZrMOF)functionalized by sulfonic groups are prepared.Based on the comprehensive structural characterizations by means of X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),N2 physisorption,Thermogravimetric(TG)and Fourier transformed infrared spectroscopy(FTIR),we find that sulfonic acid(–SO_(3)H)functional groups are tethered on the UIO-66 without affecting the structure of the framework.Systematic characterizations(NH_(3)-TPD,CO_(2)-TPD,and in-situ FTIR)demonstrate that modifying of sulfonic groups on UIO-66 results in the formation of stronger Lewis acidic-basic and Brnsted acidis sites.The cooperative role of the versatile Lewis acidic-basic and Brnsted acidic sites in 60%mol fraction of sulfonic acid-containing UIO-66(UIO-S_(0.6))retain high surface area and exhibit excellent catalytic performance of 94.7%FOL yield and 16.9 h^(-1).turnover number(TOF)under mild conditions.Kinetic experiments reveal that the activation energy of the CTH of furfural(FF)over UIO-S_(0.6) catalyst is as low as 50.8 k J mol^(-1).Besides,the hydrogen transfer mechanism is investigated through isotope labeling experiments,exhibiting that theβ-H in isopropanol is transferred to the a-C of FF by forming six-membered intermediates on the Lewis acidic-basic and Brnsted acidic sites of the UIO-S_(0.6),which is the rate-determining step in the formation of FOL.展开更多
Aqueous zinc ion hybrid capacitors(ZIHCs)hold great potential for large-scale energy storage applications owing to their high safety and low cost,but suffer from low capacity and energy density.Herein,pyridinic nitrog...Aqueous zinc ion hybrid capacitors(ZIHCs)hold great potential for large-scale energy storage applications owing to their high safety and low cost,but suffer from low capacity and energy density.Herein,pyridinic nitrogen enriched porous carbon(nPC)was successfully synthesized via the growth,subsequent annealing and acid etching of bimetal organic frameworks for high capacity and safe ZIHCs with exceptional rate capability.Benefiting from the mesopores for easy ion diffusion,high electrical conductivity enabled by in-situ grown carbon nanotubes matrix and residual metal Co nanoparticles for fast electron transfer,sufficient micropores and high N content(8.9 at%)with dominated pyridinic N(54%)for enhanced zinc ion storage,the resulting nPC cathodes for ZIHCs achieved high capacities of 302 and137 m Ah g^(-1) at 1 and 18 A g^(-1),outperforming most reported carbon based cathodes.Theoretical results further disclosed that pyridinic N possessed larger binding energy of-4.99 eV to chemically coordinate with Zn2+than other N species.Moreover,quasi-solid-state ZIHCs with gelatin based gel electrolytes exhibited high energy density of 157.6 Wh kg^(-1) at 0.69 kW kg^(-1),high safety and mechanical flexibility to withstand mechanical deformation and drilling.This strategy of developing pyridinic nitrogen enriched porous carbon will pave a new avenue to construct safe ZIHCs with high energy densities.展开更多
A magnetic metal organic framework（MMOF） was synthesized and used to separate Sr^2＋ in aqueous solution. The shape and structure of prepared Fe3O4@UiO-66-NH2 were characterized, and the absorbed concentration of st...A magnetic metal organic framework（MMOF） was synthesized and used to separate Sr^2＋ in aqueous solution. The shape and structure of prepared Fe3O4@UiO-66-NH2 were characterized, and the absorbed concentration of strontium was determined through inductively coupled plasma mass spectrometry. The results indicated that Fe3O4 and UiO-66-NH2 combined through chemical bonding. The experimental adsorption results for separation of Sr^2＋ in aqueous solution indicated that the adsorption of Sr^2＋ to Fe3O4@UiO-66-NH2 increased drastically from pH 11 to pH 13. The adsorption isotherm model indicated that the adsorption of Sr^2＋ conformed to the Freundlich isotherm model（R2 = 0.9919）. The MMOF thus inherited the superior qualities of magnetic composites and metal organic frameworks, and can easily be separated under an external magnetic field. This MMOF thus has potential applications as a magnetic adsorbent for low level radionuclide （90）Sr.展开更多
A novel adsorbent(MTZ-MOFs)was synthesized by a one-step reaction of zinc nitrate hexahydrate and 1-(2-dimethylaminoethyl)-1H-5-mercaptotetrazole to remove mercury from waste water.The results showed that MTZ-MOFs had...A novel adsorbent(MTZ-MOFs)was synthesized by a one-step reaction of zinc nitrate hexahydrate and 1-(2-dimethylaminoethyl)-1H-5-mercaptotetrazole to remove mercury from waste water.The results showed that MTZ-MOFs had excellent selectivity and repeatability for Hg(Ⅱ),the optimum pH was 3.0,the maximum adsorption capacity was 872.8 mg/g,and the process was a spontaneous exothermic reaction.The adsorption behavior was chemisorption,which conformed to the pseudo-second-order kinetic and Freundlich isothermal model.Moreover,the adsorption mechanism showed that the adsorption process mainly depended on ion exchange and chelation,and the synergistic action of S and N atoms played a key role.So,MTZ-MOFs were an efficient adsorbent for mercury ion removal.展开更多
Exploring efficient and cost-saving electrocatalysts is essential to the renewable energy storage and utilization,which is still in its embryonic period.MOFs have drawn tremendous attention due to their adjustability,...Exploring efficient and cost-saving electrocatalysts is essential to the renewable energy storage and utilization,which is still in its embryonic period.MOFs have drawn tremendous attention due to their adjustability,abundant active sites,and plentiful pores.Notably,satisfactory electrocatalytic performance has been achieved by MOFs-based electrocatalysts comparable to traditional electrocatalysts.State-of-the-art works about the MOFs-based electrocatalysts for hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and ORR were summarized in this review.This review comprises a series of modifying strategies of MOFs and their derivatives,from aspects of structure,composition,and morphology.Furthermore,the active sites and functional mechanisms’recognition are involved in this review expecting to provide reference for rationally designing efficient electrocatalysts.At last,the current status,challenges,and perspectives of MOFs-based electrocatalysts are also discussed.展开更多
The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current C...The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current CO_(2) electrolyzers remain impractical on a large scale due to the low current densities and faradaic efficiencies(FE)on various electrocatalysts.In this study,hybrid HKUST‐1 metal‐organic framework‒fluorinated imidazolium‐based room temperature ionic liquid(RTIL)electrocatalysts are designed to selectively reduce CO_(2) to CH_(4).An impressive FE of 65.5%towards CH_(4) at-1.13 V is achieved for the HKUST‐1/[BMIM][PF_(6)]hybrid,with a stable FE greater than 50%maintained for at least 9 h in an H‐cell.The observed improvements are attributed to the increased local CO_(2) concentration and the improved CO_(2)‐to‐CH_(4) thermodynamics in the presence of the RTIL molecules adsorbed on the HKUST‐1‐derived Cu clusters.These findings offer a novel approach of immobilizing RTIL co‐catalysts within porous frameworks for CO_(2) electroreduction applications.展开更多
Solid-state fiber dye-sensitized solar cells(SS-FDSSCs) have been the subject of intensive attention and development in recent years. Although this field is only in its infancy, metal–organic frameworks(MOFs) are one...Solid-state fiber dye-sensitized solar cells(SS-FDSSCs) have been the subject of intensive attention and development in recent years. Although this field is only in its infancy, metal–organic frameworks(MOFs) are one such material that has been utilized to further improve the power conversion efficiency of solar cells. In this study, MOF-integrated DSSCs were shown to have potential in the development of solar cell devices with efficiency comparable to or better than that of conventional solar cells. The power conversion efficiency(PCE) of SS-FDSSCs was improved by embedding MOF-801 into a mesoporous-TiO_(2)(mp-TiO_(2)) layer, which was used as a photoanode in SS-FDSSCs, which are inherently flexible. The PCE of the MOF-integrated SS-FDSSCs was 6.50%, which is comparable to that of the reference devices(4.19%).The MOF-801 enhanced SS-FDSSCs decreased the series resistance(R_(s)) value, resulting in effective electron extraction with improved short-circuit current density(J_(SC)), while also increasing the shunt resistance(R_(sh)) value to prevent the recombination of photo-induced electrons. The result is an improved fill factor and, consequently, a higher value for the PCE.展开更多
Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor hi...Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor high rate performance still constitute great challenges.Metal organic framework-derived carbon has been widely researched because of its high porosity,tunable structure,and good conductivity.In this work,N/S codoped hierarchical porous carbon microspheres were prepared by a high-temperature heat treatment and atomic doping process using a zinc-based organic framework as the precursor.When used as a potassium-ion battery anode,it has a high reversible specific capacity(435.7 mAh g^(-1)),good rate performance(133.5 mAh g^(-1)at 10,000 m A g^(-1)),and long-term cycling stability(73.2%capacity retention after the 2500th cycle).The potassium storage mechanism of the derived carbon was explained by various electrochemical analysis methods and microstructure characterization techniques,and the relationship between the structural characteristics and electrochemical properties was researched.In a supercapacitor,the porous carbon material exhibits a specific capacitance of 307.2 F g^(-1)at a current density of 0.2 A g^(-1)in a KOH aqueous solution and achieves a retention rate of 99.88%after 10,000 cycles.The assembled symmetric supercapacitor device delivers a high energy density of 6.69 Wh kg^(-1),with a corresponding power density of 2500 W kg^(-1).In addition,density functional theory calculations further confirmed that N/S codoping can improve the adsorption capacities of potassium and hydroxyl ions in the derived carbon.展开更多
In this study,Co/Zr-metal organic framework(MOF)precursors were obtained by a roomtemperature liquid-phase precipitation method and the equivalent-volume impregnation method,respectively,using a Zr-MOF as the support,...In this study,Co/Zr-metal organic framework(MOF)precursors were obtained by a roomtemperature liquid-phase precipitation method and the equivalent-volume impregnation method,respectively,using a Zr-MOF as the support,and Co/Zr-MOF-M and Co/Zr-MOF-N catalysts were prepared after calcination in a hydrogen-argon mixture gases(VAr:V_(H_(2))=9:1)at 350℃for 2 h.The catalytic activities of the prepared samples for CO_(2)methanation under atmosphericpressure cold plasma were studied.The results showed that Co/Zr-MOF-M had a good synergistic effect with cold plasma.At a discharge power of 13.0 W,V_(H_(2)):VCO_(2)=4:1 and a gas flow rate of 30 ml·min^(-1),the CO_(2)conversion was 58.9%and the CH4 selectivity reached 94.7%,which was higher than for Co/Zr-MOF-N under plasma(CO_(2)conversion 24.8%,CH4 selectivity 9.8%).X-ray diffraction,scanning electron microscopy,transmission electron microscopy,N_(2)adsorption and desorption(Brunauer-Emmett-Teller)and x-ray photoelectron spectroscopy analysis results showed that Co/Zr-MOF-M and Co/Zr-MOF-N retained a good Zr-MOF framework structure,and the Co oxide was uniformly dispersed on the surface of the Zr-MOF.Compared with Co/Zr-MOF-N,the Co/Zr-MOF-M catalyst has a larger specific surface area and higher Co^(2+)/Cototaland Co/Zr ratios.Additionally,the Co oxide in Co/ZrMOF-M is distributed on the surface of the Zr-MOF in the form of porous particles,which may be the main reason why the catalytic activity of Co/Zr-MOF-M is higher than that of Co/ZrMOF-N.展开更多
The need for a net zero carbon emission future is imperative forenvironmental sustainability hence, intensive carbon fuels would need tobe replaced with less carbon emitting energy sources such as natural gastill clea...The need for a net zero carbon emission future is imperative forenvironmental sustainability hence, intensive carbon fuels would need tobe replaced with less carbon emitting energy sources such as natural gastill clean energy source such as hydrogen becomes commercialized. Asa result, this mini review discusses the use of metal organic framework(MOF) for adsorption of methane and hydrogen in specially designed tanksfor improved performance so as to increase their applicability. Herein,adsorption (delivery) capacity of selected high performing MOFs formethane and hydrogen storage were highlighted in reference to the targetsset by United States Department of Energy’s Advanced Research ProjectsAgency-Energy (ARPA-E) and Fuel Cells Technology Office. In thisregard, specific design and chemistry of MOFs for improved methane andhydrogen adsorption were highlighted accordingly. In addition, an overviewof computational and molecular studies of hypothetical MOFs was done- the various approaches used and their proficiency for construction ofspecific of crystalline structures and topologies were herewith discussed.展开更多
Two isomeric metal-organic frameworks(MOFs) with 2-dimensional(2D) and 3-dimensional(3D) topologies both comprised of Cu(Ⅱ) and OTf(OTf = trifluoromethanesulfonate) ions were synthesized and characterized.The CO_2,CH...Two isomeric metal-organic frameworks(MOFs) with 2-dimensional(2D) and 3-dimensional(3D) topologies both comprised of Cu(Ⅱ) and OTf(OTf = trifluoromethanesulfonate) ions were synthesized and characterized.The CO_2,CH_4 and N_2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at0.1 MPa.The results showed that the 2D MOF exhibited a higher selectivity for CO_2 from CO_2/CH_4 and CH_4from CH_4/N_2 compared to the 3D MOF,even though it possessed a lower surface area and pore volume.The higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered MOFs.Dynamic separation experiments using CO_2/CH_4 and CH_4/N_2 mixtures on the two MOFs proved that the2 D MOF had a longer elution time than the 3D MOF as well as better separation abilities.展开更多
Li-S batteries(LSBs)have been considering as new and promising energy storage systems because of the high theoretical energy density and low price.Nevertheless,their practical application is inhibited by several facto...Li-S batteries(LSBs)have been considering as new and promising energy storage systems because of the high theoretical energy density and low price.Nevertheless,their practical application is inhibited by several factors,including poor electrical conductivity of electrode materials,greatly volumetric variation,as well as the polysulfide formation upon the cycling.To address these problems,it is imperative to develop and design effective and suitable sulfur host anode materials.Metal organic frameworks(MOFs)-based cathode materials,possessing their good conductivity and easy morphology design,have been extensively studied and exhibited enormously potential in LSBs.In this review,a comprehensive overview of MOFs-based sulfur host materials is provided,including their electrochemical reaction mechanisms,related evaluation parameters,and their performances used in LSBs in the past few years.In particular,the recent advances using in-situ characterization technologies for investigating the electrochemical reaction mechanism in LSBs are presented and highlighted.Additionally,the challenges and prospects associated with future research on MOF-related sulfur host materials are discussed.It is anticipated to offer the guidance for the identification of suitable MOFs-based sulfur cathode materials for high-performance LSBs,thereby contributing for the achievement of a sustainable and renewable society.展开更多
Sodium dentrite formed by uneven plating/stripping can reduce the utilization of active sodium with poor cyclic stability and,more importantly,cause internal short circuit and lead to thermal runaway and fire.Therefor...Sodium dentrite formed by uneven plating/stripping can reduce the utilization of active sodium with poor cyclic stability and,more importantly,cause internal short circuit and lead to thermal runaway and fire.Therefore,sodium dendrites and their related problems seriously hinder the practical application of sodium metal batteries(SMBs).Herein,a design concept for the incorporation of metal-organic framework(MOF)in polymer matrix(polyvinylidene fluoride-hexafluoropropylene)is practiced to prepare a novel gel polymer electrolyte(PH@MOF polymer-based electrolyte[GPE])and thus to achieve high-performance SMBs.The addition of the MOF particles can not only reduce the movement hindrance of polymer chains to promote the transfer of Na^(+)but also anchor anions by virtue of their negative charge to reduce polarization during electrochemical reaction.A stable cycling performance with tiny overpotential for over 800 h at a current density of 5 mA cm^(-2)with areal capacity of 5 mA h cm^(-2)is achieved by symmetric cells based on the resulted GPE while the Na_(3)V_(2)O_(2)(PO_(4))_(2)F@rGO(NVOPF)|PH@MOF|Nacell also displays impressive specific cycling capacity(113.3 mA h g^(-1)at 1 C)and rate capability with considerable capacity retention.展开更多
As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemmin...As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.展开更多
Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal...Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal-organic frameworks(MOFs)with tunable Lewis-base passivation sites have been constructed(Cd-Httb and Cd-Httb-BDC,Httb=5-(4-(1H-1,2,4-triazole-1-yl)benzyl)-1h-tetrazole,BDC=1,4-dicarboxybenzene)to eliminate deep-level defects and simultaneously as nanostructured heterogeneous nucleation seed to assist the growth of large-grained perovskite films.Compared with the control and Cd-Httb,Cd-Httb-BDC designed with mix-ligands strategy exhibited the enhanced inducted effect on the crystallization and nucleation of high-quality perovskite films during annealing process.Consequently,the resultant Cd-Httb-BDC-modified device achieved higher power conversion efficiency(PCE)(22.18%)than the control(20.89%)and Cd-Httb(21.56%).Meanwhile,the unencapsulated Cd-Httb-BDC-modified device still maintained 90%of initial PCE after 1500 h in ambient conditions and exhibited enhanced thermal stability(85℃ in N_(2) atmosphere).This work presented a successful example of mixligands strategy on construction of high-quality MOF-assisted perovskite films for high-efficient and stable PSCs.展开更多
The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-fun...The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-functionalized zirconium metal organic framework(Zr-MOF)was covalently modified with different functional groups via the condensation of Zr-MOF with 2-pyridinecarboxaldehyde(PA),salicylaldehyde(SA),benzaldehyde(BA),and trifluoroacetic acid(TA),named Zr-MOF-X(X=PA,SA,BA,and TA),respectively,through the post-synthesis modification.Compared with Zr-MOF and Zr-MOF-TA,the introduction of PA,SA,or BA into the framework of Zr-MOF can not only enhance the visible-light harvesting and CO_(2)capture,but also accelerate the photogenerated charge separation and transfer,thereby improving the photocatalytic ability of Zr-MOF for CO_(2)reduction.These results indicate that the modification of Zr-MOF with electron-donating groups can promote the photocatalytic CO_(2)reduction.Therefore,the current work provides an instructive approach to improve the photocatalytic efficiency of CO_(2)reduction through the covalent modification of MOFs.展开更多
Xenon and krypton are widespread useful noble gases in commercial lighting, lasers, electronics, and medical industry. At the same time, radioactive noble gases may proliferate from used nuclear fuel and diffuse in op...Xenon and krypton are widespread useful noble gases in commercial lighting, lasers, electronics, and medical industry. At the same time, radioactive noble gases may proliferate from used nuclear fuel and diffuse in open atmospheres. Metal organic frameworks as hotspot porous materials for gases uptake and separation are considered to be potential solutions. In this review, we comprehensively summarized recent researches on metal organic frameworks for selective capture and separation of xenon and krypton. Particularly, we followed the aspects of different optimal design strategies, including optimal pore/cage size and geometry, open metal sites, ions (anions and cations), and polar functional groups for enhancing the xenon adsorption and separation performances. Meanwhile, a comparison of each strategy and the mechanisms of xenon/krypton separation were pointed out. The separation of krypton from gases mixtures by dual-bed systems was further discussed. Finally, some existing challenges and opportunities for possible real applications were proclaimed.展开更多
Phosphorylation plays crucial parts in lenticular biological function.Getting knowledge of region-resolved phosphoproteome contributes to better comprehending the pathogenesis.Here,we prepared the hybrid metal organic...Phosphorylation plays crucial parts in lenticular biological function.Getting knowledge of region-resolved phosphoproteome contributes to better comprehending the pathogenesis.Here,we prepared the hybrid metal organic frameworks(HMOFs)for probing the region-resolved heterogeneity of phosphoproteome in human lens.1334 phosphosites corresponding to 564 phosphoproteins,1160 phosphosites corresponding to 316 phosphoproteins and 517 phosphosites corresponding to 205 phosphoproteins were identified in capsule,cortex and nucleus,respectively,providing the relatively extensive distribution mapping of phosphorylation in human lens for the first time.The label-free quantification experiments and principal component analysis presented differential expression of phopshoproteins in three subregions.For instance,α-crystallin,β-crystallin and fibrillin-1 closely associated with cataract and Marfan syndrome showed disparate spatial distribution.The preferential phosphoproteins in capsule,cortex and nucleus were involved in cytoskeleton organization,metabolic process and lens development in camera-type eye,respectively.This work first provided a general overview of region-resolved phosphoproteome of human lens.展开更多
基金supported by National Natural Science Foundation of China(22090031,21922501,22109004)China Postdoctoral Science Foundation(2021M690319)。
文摘Integrated electrocatalysts(IECs)containing well-defined functional materials directly grown on the current collector have sparked increasing interest in the fields of electrocatalysis owing to efficient activity,high stability and the fact that they are easily assembled into devices.Recently,metal organic frameworks(MOFs)provide a promising platform for constructing advanced IECs because of their properties of low cost,large surface area and efficient structural tunability.In this review,the design principles of state-of-the-art IECs based on MOFs are presented,including by hydrothermal/solvothermal,template-directed,electrospinning,electrodeposition and other methods.The high performance of MOF-derived IECs has also been demonstrated in electrocatalytic gasinvolved reactions.This is promising for green energy storage and conversion.The structure-activity relationship and performance improvement mechanism of IECs are uncovered by discussing some in situ technologies for IECs.Finally,we provide an outlook on the challenges and prospects in this booming field.
基金This work was financially supported by Graduate School and Research Council of Yasouj University.
文摘The aim of this study is a present of a simple solvothermal synthesis approach to preparation of Cu-based magnetic metal organic framework(MMOF)and subsequently its application as sorbent for ultrasound assisted magnetic solid phase extraction(UAMSPE)of ampicillin(AMP)from cow milk samples prior to high performance liquid chromatography-Ultraviolet(HPLC-UV)determination.Characteristics of prepared MMOF were fully investigated by different techniques which showed the exclusive properties of proposed sorbent in terms of proper functionality,desirable magnetic property and also high specific surface area.Different influential factors on extraction recovery including sorbent dosage,ultrasonic time,washing solvent volume and eluent solvent volume were assessed using central composite design(CCD)based response surface methodology(RSM)as an operative and powerful optimization tool.This is the first report for determination of AMP using MMOF.The proposed method addressed some drawbacks of other methods and sorbents for determination of AMP.The presented method decreases the extraction time(4 min)and also enhances adsorption capacity(250 mg/g).Moreover,the magnetic property of presented sorbent(15 emu/g)accelerates the extraction process which does not need filtration,centrifuge and precipitation procedures.Under the optimized conditions,the proposed method is applicable for linear range of 1.0-5000.0 μg/L with detection limit of 0.29 μg/L,satisfactory recoveries(≥95.0%)and acceptable repeatability(RSD less than 4.0%).The present study indicates highly promising perspectives of MMOF for highly effective analysis of AMP in complicated matrices.
基金supported by the National Key R&D Program of China(2020YFA0710000)the National Natural Science Foundation of China(22122901,21902047)+1 种基金the Provincial Natural Science Foundation of Hunan(2020JJ5045,2021JJ20024,2021RC3054)the Shenzhen Science and Technology Program(JCYJ20210324140610028)。
文摘The highly selective catalytic transfer hydrogenation(CTH)of furfural(FF)to furfuryl alcohol(FOL)is a significant route of biomass valorization.Herein,a series microporous Zr-metal organic framework(ZrMOF)functionalized by sulfonic groups are prepared.Based on the comprehensive structural characterizations by means of X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),N2 physisorption,Thermogravimetric(TG)and Fourier transformed infrared spectroscopy(FTIR),we find that sulfonic acid(–SO_(3)H)functional groups are tethered on the UIO-66 without affecting the structure of the framework.Systematic characterizations(NH_(3)-TPD,CO_(2)-TPD,and in-situ FTIR)demonstrate that modifying of sulfonic groups on UIO-66 results in the formation of stronger Lewis acidic-basic and Brnsted acidis sites.The cooperative role of the versatile Lewis acidic-basic and Brnsted acidic sites in 60%mol fraction of sulfonic acid-containing UIO-66(UIO-S_(0.6))retain high surface area and exhibit excellent catalytic performance of 94.7%FOL yield and 16.9 h^(-1).turnover number(TOF)under mild conditions.Kinetic experiments reveal that the activation energy of the CTH of furfural(FF)over UIO-S_(0.6) catalyst is as low as 50.8 k J mol^(-1).Besides,the hydrogen transfer mechanism is investigated through isotope labeling experiments,exhibiting that theβ-H in isopropanol is transferred to the a-C of FF by forming six-membered intermediates on the Lewis acidic-basic and Brnsted acidic sites of the UIO-S_(0.6),which is the rate-determining step in the formation of FOL.
基金financially supported by the National Key R@D Program of China(Grants 2016YBF0100100 and 2016YFA0200200)National Natural Science Foundation of China(Grants 51872283,and 21805273)+8 种基金Liaoning BaiQianWan Talents Program,LiaoNing Revitalization Talents Program(Grant XLYC1807153)Natural Science Foundation of Liaoning Province(2020-MS-095)Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science(Grants 20180510038)DICP(DICP ZZBS201708,DICP ZZBS201802,and DICP I202032)DICP&QIBEBT(Grant No.DICP&QIBEBT UN201702)Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL180310,DNL180308,DNL201912,and DNL201915)the Fundamental Research Funds for the Central Universities of China(N180503012)the State Key Laboratory of Fine Chemicals(KF1911)the CAS Key Laboratory of Carbon Materials(KLCMKFJJ2004)。
文摘Aqueous zinc ion hybrid capacitors(ZIHCs)hold great potential for large-scale energy storage applications owing to their high safety and low cost,but suffer from low capacity and energy density.Herein,pyridinic nitrogen enriched porous carbon(nPC)was successfully synthesized via the growth,subsequent annealing and acid etching of bimetal organic frameworks for high capacity and safe ZIHCs with exceptional rate capability.Benefiting from the mesopores for easy ion diffusion,high electrical conductivity enabled by in-situ grown carbon nanotubes matrix and residual metal Co nanoparticles for fast electron transfer,sufficient micropores and high N content(8.9 at%)with dominated pyridinic N(54%)for enhanced zinc ion storage,the resulting nPC cathodes for ZIHCs achieved high capacities of 302 and137 m Ah g^(-1) at 1 and 18 A g^(-1),outperforming most reported carbon based cathodes.Theoretical results further disclosed that pyridinic N possessed larger binding energy of-4.99 eV to chemically coordinate with Zn2+than other N species.Moreover,quasi-solid-state ZIHCs with gelatin based gel electrolytes exhibited high energy density of 157.6 Wh kg^(-1) at 0.69 kW kg^(-1),high safety and mechanical flexibility to withstand mechanical deformation and drilling.This strategy of developing pyridinic nitrogen enriched porous carbon will pave a new avenue to construct safe ZIHCs with high energy densities.
基金financially supported by the National Natural Science Foundation of China[Grant No.20477058]by the Chinese Ministry of Science and Technology[Grant No.2014YF211000]
文摘A magnetic metal organic framework（MMOF） was synthesized and used to separate Sr^2＋ in aqueous solution. The shape and structure of prepared Fe3O4@UiO-66-NH2 were characterized, and the absorbed concentration of strontium was determined through inductively coupled plasma mass spectrometry. The results indicated that Fe3O4 and UiO-66-NH2 combined through chemical bonding. The experimental adsorption results for separation of Sr^2＋ in aqueous solution indicated that the adsorption of Sr^2＋ to Fe3O4@UiO-66-NH2 increased drastically from pH 11 to pH 13. The adsorption isotherm model indicated that the adsorption of Sr^2＋ conformed to the Freundlich isotherm model（R2 = 0.9919）. The MMOF thus inherited the superior qualities of magnetic composites and metal organic frameworks, and can easily be separated under an external magnetic field. This MMOF thus has potential applications as a magnetic adsorbent for low level radionuclide （90）Sr.
基金supported by the Hubei Provincial Department of Education Science and Technology Research Program Young Talent Project,China (No. Q20201102)the National Natural Science Foundation of China (Nos. 51864042, 51804220)
文摘A novel adsorbent(MTZ-MOFs)was synthesized by a one-step reaction of zinc nitrate hexahydrate and 1-(2-dimethylaminoethyl)-1H-5-mercaptotetrazole to remove mercury from waste water.The results showed that MTZ-MOFs had excellent selectivity and repeatability for Hg(Ⅱ),the optimum pH was 3.0,the maximum adsorption capacity was 872.8 mg/g,and the process was a spontaneous exothermic reaction.The adsorption behavior was chemisorption,which conformed to the pseudo-second-order kinetic and Freundlich isothermal model.Moreover,the adsorption mechanism showed that the adsorption process mainly depended on ion exchange and chelation,and the synergistic action of S and N atoms played a key role.So,MTZ-MOFs were an efficient adsorbent for mercury ion removal.
基金supported by the National Key R&D Program of China(No.2018YFA0108300)the Overseas High-level Talents Plan of China and Guangdong Province+3 种基金the Fundamental Research Funds for the Central Universitiesthe 100 Talents Plan Foundation of Sun Yat-sen Universitythe Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2017ZT07C069)the National Natural Science Foundation of China(Nos.22075321,21821003,21890380,and 21905315).
文摘Exploring efficient and cost-saving electrocatalysts is essential to the renewable energy storage and utilization,which is still in its embryonic period.MOFs have drawn tremendous attention due to their adjustability,abundant active sites,and plentiful pores.Notably,satisfactory electrocatalytic performance has been achieved by MOFs-based electrocatalysts comparable to traditional electrocatalysts.State-of-the-art works about the MOFs-based electrocatalysts for hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and ORR were summarized in this review.This review comprises a series of modifying strategies of MOFs and their derivatives,from aspects of structure,composition,and morphology.Furthermore,the active sites and functional mechanisms’recognition are involved in this review expecting to provide reference for rationally designing efficient electrocatalysts.At last,the current status,challenges,and perspectives of MOFs-based electrocatalysts are also discussed.
文摘The electrochemical reduction of CO_(2) towards hydrocarbons is a promising technology that can utilize CO_(2) and prevent its atmospheric accumulation while simultaneously storing renewable en‐ergy.However,current CO_(2) electrolyzers remain impractical on a large scale due to the low current densities and faradaic efficiencies(FE)on various electrocatalysts.In this study,hybrid HKUST‐1 metal‐organic framework‒fluorinated imidazolium‐based room temperature ionic liquid(RTIL)electrocatalysts are designed to selectively reduce CO_(2) to CH_(4).An impressive FE of 65.5%towards CH_(4) at-1.13 V is achieved for the HKUST‐1/[BMIM][PF_(6)]hybrid,with a stable FE greater than 50%maintained for at least 9 h in an H‐cell.The observed improvements are attributed to the increased local CO_(2) concentration and the improved CO_(2)‐to‐CH_(4) thermodynamics in the presence of the RTIL molecules adsorbed on the HKUST‐1‐derived Cu clusters.These findings offer a novel approach of immobilizing RTIL co‐catalysts within porous frameworks for CO_(2) electroreduction applications.
基金supported by the Fundamental Research Program(PNK 7350 and PNK 7340)of the Korea Institute of Materials Science(KIMS)the National Research Foundation(NRF)grant funded by the Korean government(MEST)(2021R1A2C2014192)。
文摘Solid-state fiber dye-sensitized solar cells(SS-FDSSCs) have been the subject of intensive attention and development in recent years. Although this field is only in its infancy, metal–organic frameworks(MOFs) are one such material that has been utilized to further improve the power conversion efficiency of solar cells. In this study, MOF-integrated DSSCs were shown to have potential in the development of solar cell devices with efficiency comparable to or better than that of conventional solar cells. The power conversion efficiency(PCE) of SS-FDSSCs was improved by embedding MOF-801 into a mesoporous-TiO_(2)(mp-TiO_(2)) layer, which was used as a photoanode in SS-FDSSCs, which are inherently flexible. The PCE of the MOF-integrated SS-FDSSCs was 6.50%, which is comparable to that of the reference devices(4.19%).The MOF-801 enhanced SS-FDSSCs decreased the series resistance(R_(s)) value, resulting in effective electron extraction with improved short-circuit current density(J_(SC)), while also increasing the shunt resistance(R_(sh)) value to prevent the recombination of photo-induced electrons. The result is an improved fill factor and, consequently, a higher value for the PCE.
基金supported by the National Natural Science Foundation of China (51764029, 52004116)the National Key Research and Development Program of China (2019YFC1803501)+1 种基金the Applied Basic Research Plan of Yunnan Province(202001AU070039, 2018FB087)the Science Research Foundation of Yunnan Provincial Department of Education (2020J0070)
文摘Carbon-based materials have become a research hotspot in the field of energy storage devices in recent years due to their abundant resources,low cost,and environmental friendliness.However,the low capacity and poor high rate performance still constitute great challenges.Metal organic framework-derived carbon has been widely researched because of its high porosity,tunable structure,and good conductivity.In this work,N/S codoped hierarchical porous carbon microspheres were prepared by a high-temperature heat treatment and atomic doping process using a zinc-based organic framework as the precursor.When used as a potassium-ion battery anode,it has a high reversible specific capacity(435.7 mAh g^(-1)),good rate performance(133.5 mAh g^(-1)at 10,000 m A g^(-1)),and long-term cycling stability(73.2%capacity retention after the 2500th cycle).The potassium storage mechanism of the derived carbon was explained by various electrochemical analysis methods and microstructure characterization techniques,and the relationship between the structural characteristics and electrochemical properties was researched.In a supercapacitor,the porous carbon material exhibits a specific capacitance of 307.2 F g^(-1)at a current density of 0.2 A g^(-1)in a KOH aqueous solution and achieves a retention rate of 99.88%after 10,000 cycles.The assembled symmetric supercapacitor device delivers a high energy density of 6.69 Wh kg^(-1),with a corresponding power density of 2500 W kg^(-1).In addition,density functional theory calculations further confirmed that N/S codoping can improve the adsorption capacities of potassium and hydroxyl ions in the derived carbon.
基金supported by National Natural Science Foundation of China(Nos.21673026,11605020)Innovative Training Program for College Student of Liaoning Province(No.S202011258068)。
文摘In this study,Co/Zr-metal organic framework(MOF)precursors were obtained by a roomtemperature liquid-phase precipitation method and the equivalent-volume impregnation method,respectively,using a Zr-MOF as the support,and Co/Zr-MOF-M and Co/Zr-MOF-N catalysts were prepared after calcination in a hydrogen-argon mixture gases(VAr:V_(H_(2))=9:1)at 350℃for 2 h.The catalytic activities of the prepared samples for CO_(2)methanation under atmosphericpressure cold plasma were studied.The results showed that Co/Zr-MOF-M had a good synergistic effect with cold plasma.At a discharge power of 13.0 W,V_(H_(2)):VCO_(2)=4:1 and a gas flow rate of 30 ml·min^(-1),the CO_(2)conversion was 58.9%and the CH4 selectivity reached 94.7%,which was higher than for Co/Zr-MOF-N under plasma(CO_(2)conversion 24.8%,CH4 selectivity 9.8%).X-ray diffraction,scanning electron microscopy,transmission electron microscopy,N_(2)adsorption and desorption(Brunauer-Emmett-Teller)and x-ray photoelectron spectroscopy analysis results showed that Co/Zr-MOF-M and Co/Zr-MOF-N retained a good Zr-MOF framework structure,and the Co oxide was uniformly dispersed on the surface of the Zr-MOF.Compared with Co/Zr-MOF-N,the Co/Zr-MOF-M catalyst has a larger specific surface area and higher Co^(2+)/Cototaland Co/Zr ratios.Additionally,the Co oxide in Co/ZrMOF-M is distributed on the surface of the Zr-MOF in the form of porous particles,which may be the main reason why the catalytic activity of Co/Zr-MOF-M is higher than that of Co/ZrMOF-N.
文摘The need for a net zero carbon emission future is imperative forenvironmental sustainability hence, intensive carbon fuels would need tobe replaced with less carbon emitting energy sources such as natural gastill clean energy source such as hydrogen becomes commercialized. Asa result, this mini review discusses the use of metal organic framework(MOF) for adsorption of methane and hydrogen in specially designed tanksfor improved performance so as to increase their applicability. Herein,adsorption (delivery) capacity of selected high performing MOFs formethane and hydrogen storage were highlighted in reference to the targetsset by United States Department of Energy’s Advanced Research ProjectsAgency-Energy (ARPA-E) and Fuel Cells Technology Office. In thisregard, specific design and chemistry of MOFs for improved methane andhydrogen adsorption were highlighted accordingly. In addition, an overviewof computational and molecular studies of hypothetical MOFs was done- the various approaches used and their proficiency for construction ofspecific of crystalline structures and topologies were herewith discussed.
基金Supported by National Natural Science Foundation of China(No.21136007,No.51302184)the National Research Fund for Fundamental Key Projects(No.2014CB260402)
文摘Two isomeric metal-organic frameworks(MOFs) with 2-dimensional(2D) and 3-dimensional(3D) topologies both comprised of Cu(Ⅱ) and OTf(OTf = trifluoromethanesulfonate) ions were synthesized and characterized.The CO_2,CH_4 and N_2 adsorption properties of the two isomeric MOFs were investigated from 263 K to 298 K at0.1 MPa.The results showed that the 2D MOF exhibited a higher selectivity for CO_2 from CO_2/CH_4 and CH_4from CH_4/N_2 compared to the 3D MOF,even though it possessed a lower surface area and pore volume.The higher adsorption heats of gases on the 2D MOF inferred the strong adsorption potential energy in the layered MOFs.Dynamic separation experiments using CO_2/CH_4 and CH_4/N_2 mixtures on the two MOFs proved that the2 D MOF had a longer elution time than the 3D MOF as well as better separation abilities.
基金acknowledge the National Natural Science Foundation of China(Nos.22279121 and 22209153)Key Research and Development Program of Henan Province(No.231111241400)+1 种基金Joint Fund of Scientific and Technological Research,Development Program of Henan Province(No.222301420009)the Chunhui Plan Cooperative Research Project Foundation of Ministry of Education of China(No.202200713).
文摘Li-S batteries(LSBs)have been considering as new and promising energy storage systems because of the high theoretical energy density and low price.Nevertheless,their practical application is inhibited by several factors,including poor electrical conductivity of electrode materials,greatly volumetric variation,as well as the polysulfide formation upon the cycling.To address these problems,it is imperative to develop and design effective and suitable sulfur host anode materials.Metal organic frameworks(MOFs)-based cathode materials,possessing their good conductivity and easy morphology design,have been extensively studied and exhibited enormously potential in LSBs.In this review,a comprehensive overview of MOFs-based sulfur host materials is provided,including their electrochemical reaction mechanisms,related evaluation parameters,and their performances used in LSBs in the past few years.In particular,the recent advances using in-situ characterization technologies for investigating the electrochemical reaction mechanism in LSBs are presented and highlighted.Additionally,the challenges and prospects associated with future research on MOF-related sulfur host materials are discussed.It is anticipated to offer the guidance for the identification of suitable MOFs-based sulfur cathode materials for high-performance LSBs,thereby contributing for the achievement of a sustainable and renewable society.
基金financially supported by National Natural Science Foundation of China(Grans Nos.22179109 and 22005315)Fundamental Research Funds for the Central Universities(SWU120080)Chongqing Key Laboratory of Materials Surface&Interface Science(Project No.KFJJ2002)
文摘Sodium dentrite formed by uneven plating/stripping can reduce the utilization of active sodium with poor cyclic stability and,more importantly,cause internal short circuit and lead to thermal runaway and fire.Therefore,sodium dendrites and their related problems seriously hinder the practical application of sodium metal batteries(SMBs).Herein,a design concept for the incorporation of metal-organic framework(MOF)in polymer matrix(polyvinylidene fluoride-hexafluoropropylene)is practiced to prepare a novel gel polymer electrolyte(PH@MOF polymer-based electrolyte[GPE])and thus to achieve high-performance SMBs.The addition of the MOF particles can not only reduce the movement hindrance of polymer chains to promote the transfer of Na^(+)but also anchor anions by virtue of their negative charge to reduce polarization during electrochemical reaction.A stable cycling performance with tiny overpotential for over 800 h at a current density of 5 mA cm^(-2)with areal capacity of 5 mA h cm^(-2)is achieved by symmetric cells based on the resulted GPE while the Na_(3)V_(2)O_(2)(PO_(4))_(2)F@rGO(NVOPF)|PH@MOF|Nacell also displays impressive specific cycling capacity(113.3 mA h g^(-1)at 1 C)and rate capability with considerable capacity retention.
基金funded by the Natural Science Foundation of Fujian Province(2023J05180)the President's Foundation of Minnan Normal University(KJ2021011).
文摘As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery nature.Engineering macroscopic structures from pulverous MOF is thus of great importance for broadening their practical applications.In this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature calcination.The FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 min.Compared to the GA/PMS system,there was over a 300-fold increase in the reaction rate constant.Remarkably,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water matrices.Radical trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was dominant.Furthermore,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.
基金supported by the National Natural Science Foundation of China(22072034,22001050,and 21873025)the China Postdoctoral Science Foundation(2020T130147,2020M681084,and 2022M710949)+1 种基金the Postdoctoral Foundation of Heilongjiang Province(LBH-Z19059)the Natural Science Foundation of Heilongjiang Youth Fund(YQ2021B002).
文摘Deep-level defects and random oriented configuration in perovskite crystallization process would cause the nonradiative recombination and further affect the performance of perovskite solar cells(PSCs).Herein,two metal-organic frameworks(MOFs)with tunable Lewis-base passivation sites have been constructed(Cd-Httb and Cd-Httb-BDC,Httb=5-(4-(1H-1,2,4-triazole-1-yl)benzyl)-1h-tetrazole,BDC=1,4-dicarboxybenzene)to eliminate deep-level defects and simultaneously as nanostructured heterogeneous nucleation seed to assist the growth of large-grained perovskite films.Compared with the control and Cd-Httb,Cd-Httb-BDC designed with mix-ligands strategy exhibited the enhanced inducted effect on the crystallization and nucleation of high-quality perovskite films during annealing process.Consequently,the resultant Cd-Httb-BDC-modified device achieved higher power conversion efficiency(PCE)(22.18%)than the control(20.89%)and Cd-Httb(21.56%).Meanwhile,the unencapsulated Cd-Httb-BDC-modified device still maintained 90%of initial PCE after 1500 h in ambient conditions and exhibited enhanced thermal stability(85℃ in N_(2) atmosphere).This work presented a successful example of mixligands strategy on construction of high-quality MOF-assisted perovskite films for high-efficient and stable PSCs.
基金We gratefully acknowledge financial support from the Zhejiang Provincial Key R&D Project(No.2019C03118)the Programme of Introducing Talents of Discipline to Universities(No.D17008).
文摘The reduction of CO_(2)into high value-added chemicals and fuels by a photocatalytic technology can relieve energy shortages and the environmental problems caused by greenhouse effects.In the current work,an amino-functionalized zirconium metal organic framework(Zr-MOF)was covalently modified with different functional groups via the condensation of Zr-MOF with 2-pyridinecarboxaldehyde(PA),salicylaldehyde(SA),benzaldehyde(BA),and trifluoroacetic acid(TA),named Zr-MOF-X(X=PA,SA,BA,and TA),respectively,through the post-synthesis modification.Compared with Zr-MOF and Zr-MOF-TA,the introduction of PA,SA,or BA into the framework of Zr-MOF can not only enhance the visible-light harvesting and CO_(2)capture,but also accelerate the photogenerated charge separation and transfer,thereby improving the photocatalytic ability of Zr-MOF for CO_(2)reduction.These results indicate that the modification of Zr-MOF with electron-donating groups can promote the photocatalytic CO_(2)reduction.Therefore,the current work provides an instructive approach to improve the photocatalytic efficiency of CO_(2)reduction through the covalent modification of MOFs.
基金funding support from the National Science Foundation of China(Grants Nos.22276054,U2167218,and 22006036)the Beijing Outstanding Young Scientist Program.
文摘Xenon and krypton are widespread useful noble gases in commercial lighting, lasers, electronics, and medical industry. At the same time, radioactive noble gases may proliferate from used nuclear fuel and diffuse in open atmospheres. Metal organic frameworks as hotspot porous materials for gases uptake and separation are considered to be potential solutions. In this review, we comprehensively summarized recent researches on metal organic frameworks for selective capture and separation of xenon and krypton. Particularly, we followed the aspects of different optimal design strategies, including optimal pore/cage size and geometry, open metal sites, ions (anions and cations), and polar functional groups for enhancing the xenon adsorption and separation performances. Meanwhile, a comparison of each strategy and the mechanisms of xenon/krypton separation were pointed out. The separation of krypton from gases mixtures by dual-bed systems was further discussed. Finally, some existing challenges and opportunities for possible real applications were proclaimed.
基金financially supported by National Key R&D Program of China(No.2018YFA0507501)the National Natural Science Foundation of China(Nos.22074019,21425518 and 22004017)Shanghai Sailing Program(No.20YF1405300)。
文摘Phosphorylation plays crucial parts in lenticular biological function.Getting knowledge of region-resolved phosphoproteome contributes to better comprehending the pathogenesis.Here,we prepared the hybrid metal organic frameworks(HMOFs)for probing the region-resolved heterogeneity of phosphoproteome in human lens.1334 phosphosites corresponding to 564 phosphoproteins,1160 phosphosites corresponding to 316 phosphoproteins and 517 phosphosites corresponding to 205 phosphoproteins were identified in capsule,cortex and nucleus,respectively,providing the relatively extensive distribution mapping of phosphorylation in human lens for the first time.The label-free quantification experiments and principal component analysis presented differential expression of phopshoproteins in three subregions.For instance,α-crystallin,β-crystallin and fibrillin-1 closely associated with cataract and Marfan syndrome showed disparate spatial distribution.The preferential phosphoproteins in capsule,cortex and nucleus were involved in cytoskeleton organization,metabolic process and lens development in camera-type eye,respectively.This work first provided a general overview of region-resolved phosphoproteome of human lens.
