Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few importa...Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.展开更多
Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the back...Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.展开更多
A series of dual-extended-polyhedral metal-organic frameworks(MOFs)was constructed based on the 14-coordinated Cu_(24)-MOP-1(MOP=metal-organic polyhedron)supermolecular building blocks(SBBs)with enhanced stability and...A series of dual-extended-polyhedral metal-organic frameworks(MOFs)was constructed based on the 14-coordinated Cu_(24)-MOP-1(MOP=metal-organic polyhedron)supermolecular building blocks(SBBs)with enhanced stability and tunable functionality for high water uptake efficiency and capacity.Exceptional water stability was demonstrated by the retention of chemical integrity and crystallinity of USC-CP-5(where USC-CP stands for University of South China coordination polymer)after exposure to boiling water for 24 h.Functionalization with-Cl,-OCH_(3),-OH,and-NH_(2)groups of USC-CP-5 resulted in water uptake capacities of 450,460,490,and 590 cm^(3)·g^(-1) at relative pressure(P/P_(0))=0.9,respectively.This performance is ascribed to both the increased hydrophilicity of the ligands and stronger hydrogen bonding.Intriguingly,high-temperature activated USC-5-NH_(2)exhibits a significant water uptake of 38.5 wt.%at P/P_(0)=0.3 and releases 0.44 L·kg^(-1) water between 25 and 65℃.This water release process is reversible for at least 100 cycles with minimal weight loss of only 1.6 wt.%.Consequently,USC-5-NH_(2)holds considerable potential for harvesting and releasing atmospheric water in arid desert regions,powered by solar energy.展开更多
Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly depen...Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly dependent on the thickness of the photoactive layer,which is typically around 100 nm.This sensitivity poses a challenge for industrial-scale fabrication.Achieving high PCEs in thick-film OPVs is therefore essential.This review systematically examines recent advancements in thick-film OPVs,focusing on the fundamental mechanisms that lead to efficiency loss and strategies to enhance performance.We provide a comprehensive analysis spanning the complete photovoltaic process chain:from initial exciton generation and diffusion dynamics,through dissociation mechanisms,to subsequent charge-carrier transport,balance optimization,and final collection efficiency.Particular emphasis is placed on cutting-edge solutions in molecular engineering and device architecture optimization.By synthesizing these interdisciplinary approaches and investigating the potential contributions in stability,cost,and machine learning aspects,this work establishes comprehensive guidelines for designing high-performance OPVs devices with minimal thickness dependence,ultimately aiming to bridge the gap between laboratory achievements and industrial manufacturing requirements.展开更多
Enhancing the activity of fragile enzymes is greatly useful for various purposes,including fabrication of enzyme-based immunosensors.Herein,we report a defect-engineering strategy for encapsulating enzymes within cova...Enhancing the activity of fragile enzymes is greatly useful for various purposes,including fabrication of enzyme-based immunosensors.Herein,we report a defect-engineering strategy for encapsulating enzymes within covalent organic frameworks(COFs),enabling the resulting immobilized enzymes with excellent catalytic activity and stability to construct high performance immunosensors.In this design,by consciously introducing monoaldehyde ligands into the imine-linked COFs structure,we have precisely customized the structural defects to improve enzyme loading capacity and conformational stability.Defect-engineering interaction modulation between enzymes and COFs drives the enhancement of catalytic performance.Compared to the pristine COFs,the enzyme@defective COFs composites with optimally tuned catalytic performance exhibit a 4.49-fold enhancement in enzymatic activity.Furthermore,it is demonstrated that the stable skeletons of COFs provide exceptional protection for the enzymes against external perturbations.Thereafter,the optimized enzyme@defective COFs are employed to fabricate immunosensor.We have successfully established a detection method for prostate-specific antigen(PSA),achieving a low detection limit of 0.09 ng/mL.More importantly,the developed immunosensor has successfully distinguished the prostate cancer patients from healthy individuals.This work establishes a novel paradigm for enzyme immobilization,ultimately empowering the construction of a PSA immunosensor with high sensitivity,remarkable operational stability,and great clinical application potential.展开更多
A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 pol...A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.展开更多
Constructing catalysts featuring an ordered structure,stable performance,and uniformly dispersed catalytic sites is vital for the epoxidation of small-molecular olefins.Here,we design catalysts by tracing the oxidatio...Constructing catalysts featuring an ordered structure,stable performance,and uniformly dispersed catalytic sites is vital for the epoxidation of small-molecular olefins.Here,we design catalysts by tracing the oxidationprocess origin and synthesize a series of highly dispersed metal porphyrin-based covalent organic frameworks(COFs)materials.The aim is to efficiently oxidize the C-H bonds of cumene by air to in-situ generate organic peroxides at a safe concentration,and integrate the multi-step oxidation method of cumene in industry into a one-step method for olefins’epoxidation.The carbonyl-ruthenium COF(Ru-COF-1)exhibits excellent performance,with 98% epoxide selectivity,1221.77 h^(-1) productivity,and over 95% selectivity after 9 cycles for 1-hexene.Analysis of structure-properties-catalytic relationships of Ru-COF-1 shows that,compared with Ru-porphyrins and metal-free COFs,the enhanced reaction performance mainly results from Ru metal introduction,which promotes benzylic proton transfer in cumene.Besides,Ru-COF-1’s porous,ordered structure aids oxygen enrichment,forming active peroxy radicals with the cumene carboncentered radicals formed on the catalyst surface.Ru-H sites then accelerate active oxygen transfer from peroxy radicals,enabling olefin tandem epoxidation.Density functional theory(DFT)calculations verify the reaction mechanism,and this work offers a reference for the design of catalysts for the green,safe,and efficient oxidation of olefins.展开更多
Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving e...Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving efficient volatile organic compounds and CO emission control.The subnano cluster catalyst can not only provide catalytic sites with multiple metal atoms,but also maintain full utilization efficiency.Almost all metal atoms in highly dispersed clusters can be used for adsorption and conversion of reactants.Recently,various types of sub-nano clusters,including subnano cluster oxides,have been developed and demonstrated excellent performance in low-temperature gas-phase pollutants combustion.In this mini review,we systematically summarize the structure,physicochemical properties,characterization,and applications of sub-nano cluster catalysts in catalytic oxidation of CO,methane,propane,propylene,toluene and its derivatives,formaldehyde and chlorinated volatile organic compounds.Finally,we have analyzed and discussed the problems and challenges faced by sub-nano cluster catalysts in both basic research and practical applications,providing a scientific basis for the design,synthesis,and application of efficient heterogeneous catalysts for CO and VOCs oxidation.展开更多
Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.Th...Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.The published version showed“Hongzhen Chen”,whereas the correct spelling should be“Hongzheng Chen”.The correct author name has been provided in this Correction,and the original article[1]has been corrected.展开更多
A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamin...A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamino side groups,TT-Ph-C6 demonstrates excellent solubility and its crystal structure exhibits compact packing structures with a three-dimensional molecular stacking network.These structural attributes markedly promote exciton diffusion and charge carrier mobility,particularly advantageous for the fabrication of thick-film devices.TT-Ph-C6-based devices have attained a PCE of 18.01%at a film thickness of 100 nm,and even at a film thickness of 300 nm,the PCE remains at 14.64%,surpassing that of devices based on 2BTh-2F.These remarkable properties position TT-Ph-C6 as a highly promising NFREA material for boosting the efficiency of OSCs.展开更多
To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both me...To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both mechanical stretchability and high capacitance in SC still faces great challenges,and the crucial factors lie in creating superior electrode materials that exhibit high electrochemical performance as well as excellent mechanical stretchability.Covalent organic frameworks(COFs)possess considerable potential as electrode materials for SCs by virtue of stable organic frameworks,open channels and designable functional groups.Nevertheless,their applications in flexible SCs are greatly hindered by their rigid characteristics.Here a novel COFs@conductive polymer hydrogels(CPHs)@poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)complexes,which integrate the pseudocapacitance of PDITAPA COF,mechanical stretchability of hydrogels and high conductivity of PEDOT:PSS,has been developed as stretchable electrode of SCs.Physically cross-linked PEDOT nanofibers,with their interlinked and entangled architecture,collectively boost mechanical,electrical,and electrochemical performance.The COFs@CPHs@PEDOT:PSS simultaneously demonstrates outstanding mechanical stretchability,high electrical behaviors,and superior swelling characteristics.The resulting SC exhibits advantages of simple structures,facile assembly processes,high specific capacitance,excellent cycling stability,and arbitrary deformation,which holds great application prospects for wearable electronic products.Owing to its uncomplicated structure,ease of production,high energy storage capacity,robust cycling performance,and adaptability to deformation,this fabricated SC is well-suited for next-generation wearable technologies.展开更多
Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-org...Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-organic frameworks(MOFs),characterized by their highly porous structure,exceptional CO_(2)adsorption capacity,and tunable architecture,have emerged as promising candidates for photocatalytic CO_(2)reduction.This review systematically examines the recent advancement in MOFs-based photocatalysts for CO_(2)reduction to CO.It begins with the overview of the fundamental mechanisms and processes of MOFs towards photocatalytic CO_(2)reduction.Subsequently,common strategies for the modulation of MOFs-based photocatalysts are summarized,including metallic site modification,functionalized ligand incorporation,morphological control,defect engineering,and heterostructure construction.Notably,the review analyzes the critical factors contributing to the high selectivity of CO_(2)photoreduction to CO from both thermodynamic and kinetic perspectives.The conclusion addresses current challenges and future perspectives in designing highly efficient photocatalysts with abundant active sites,providing valuable insights for their continued development.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.展开更多
Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibite...Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.展开更多
Poly(vinylidene-trifluoroethylene) [P(VDF-TrFE)] copolymer films generally demonstrate limited compatibility with organic semiconductors. The material is frequently compromised by exposure to organic semiconductor sol...Poly(vinylidene-trifluoroethylene) [P(VDF-TrFE)] copolymer films generally demonstrate limited compatibility with organic semiconductors. The material is frequently compromised by exposure to organic semiconductor solutions and other fabrication processes utilized in the production of organic ferroelectric transistors. In this study, an organic ferroelectric field effect transistor(OFeFET) with the 6,13-Bis(triisopropylsilylethynyl) pentacene(TIPS-pentacene) channel is fabricated, in which the aluminum oxide(Al_(2)O_(3)) interlayer is used to improve compatibility. The device displays polymorphic memory and synaptic plasticity of long-term potentiation and depression. Furthermore, an artificial neural network constructed using our devices is simulated to succeed in recognizing the MNIST handwritten digit database with a high accuracy of 92.8%. This research offers a viable approach to enhance the compatibility of the organic ferroelectric polymer P(VDF-TrFE) with organic semiconductors.展开更多
Lower Paleozoic black shales are important source rocks worldwide.The Upper Ordovician-Lower Silurian Renheqiao Formation of the Baoshan Block is a low-maturity equivalent of the Wufeng-Longmaxi(WF-LMX)Shale of the Si...Lower Paleozoic black shales are important source rocks worldwide.The Upper Ordovician-Lower Silurian Renheqiao Formation of the Baoshan Block is a low-maturity equivalent of the Wufeng-Longmaxi(WF-LMX)Shale of the Sichuan Basin.However,organic matter(OM)characteristics in these low-maturity Lower Paleozoic shales are not well understood.In this study,50 Renheqiao Formation shale samples collected from seven outcrop sections and one drill core were investigated with organic petrology,organic geochemistry,R_(o)ck-Eval pyrolysis,N_(2) and CO_(2) adsorption,and scanning electron microscope(SEM)analyses to study the OM content,type,thermal maturity,and the development of OM-hosted pores in these Lower Paleozoic shales.The total organic carbon(TOC)content of the Renheqiao Formation shales varies,with the maximum content of 10.07 wt%.R_(o)ck-Eval pyrolysis results show that present OM in the Renheqiao Formation shales is Type IV kerogen,a result of advanced thermal maturation.Graptolite reflectance(GR_(o))ranges from 1.26%to 1.85%,and equivalent vitrinite reflectance(EqR_(o))converted from GR_(o) ranges from 1.08%to 1.51%,indicating that the studied Renheqiao Formation shales are dominantly within the late-mature stage.EqR_(o) based on R_(o)ck-Eval T_(max) shows large variations,which indicates that R_(o)ck-Eval T_(max) is not a reliable thermal maturity indicator for the Lower Paleozoic Renheqiao Formation shales.Caution should be applied when assessing the thermal maturity of high-maturity black shales based on T_(max) when the S2 values are too low.Organic petrographic observations show that OM in these shales is dominated by solid bitumen(>70 vol%of total OM),with minor contributions by graptolites and chitinozoans.The specific surface area and pore volume of shales are controlled by TOC content.Organic pores are hosted by solid bitumen and were not observed in graptolites when examined under the SEM.Although the Renheqiao Formation has a lower thermal maturity than the over-mature WF-LMX Shale,it is mature enough that primary oil-prone macerals have been thermally transformed and could not be identified under the microscope.展开更多
Covalent organic frameworks(COFs)are two-(2D)or threedimensional(3D)crystalline,porous networks generated by reversible polymerization of organic building blocks[1,2].The structures and functionalities of COFs are pre...Covalent organic frameworks(COFs)are two-(2D)or threedimensional(3D)crystalline,porous networks generated by reversible polymerization of organic building blocks[1,2].The structures and functionalities of COFs are precisely controlled via appropriately selected organic building blocks.This design imparts unique properties to COFs,including exceptional structural stability,tunable pore structure,and surface chemical activity,making them promising for gas separation,catalysis,optoelectronics,and sensing applications.Since Yaghi et al.'s seminal report on COFs in 2005[2],these frameworks have swiftly emerged as a hotspot in the field of materials.Originally,the focus was on fabricating rigid frameworks with static structures and optoelectronic properties.However,the inherently static nature of these frameworks hinders their responsiveness to external stimuli,potentially constraining their functionality in specific applications.Hence,an increasing number of researchers are now directing their attention toward the development of dynamic COFs capable of modifying their structures in response to external stimuli[3].Specifically,dynamic 2D COFs exhibiting enhanced structural responsiveness are of particular interest due to their capability to integrate switchable geometries and porosities with semiconductor building blocks,as well as electron conjugation across COF layers and π-stacked columns,which may enable stimuli-responsive electronic and spin properties[4].展开更多
As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 n...As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.展开更多
Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA ...Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA process by integrating the OA and associated ions previously misidentified as inorganic aerosol in high-resolution aerosol mass spectrometry data.The mass spectra and time series of primary OA(POA)and less oxidized oxygenated OA(OOA)identified by this new method resembled those resolved by traditional PMF.However,more oxidized OOA(MO-OOA)identified by traditional PMF can be further subdivided into multiple OA factors,including nitrogen-enriched OA(ON-OA)and sulfur-enriched OA(OS-OA)in summer,and ON-OA,OS-OA,and OOA in winter.Our findings highlight the significant role of photochemical processes in the formation of OS-OA compared to ON-OA.The compositions of reconstructed MO-OOA varied under different Ox(=O_(3)+NO_(2))and relative humidity conditions,emphasizing the limitations of using a constant mass spectrum.Aged biomass burning OA(BBOA)and coal combustion OA(CCOA),previously misattributed as POA,contributed 9.2%(0.43μg m^(−3))and 7.0%(0.33μg m^(−3))to SOA,respectively.Aged BBOA was more prone to forming OS-OA,whereas ON-OA showed higher correlations with aged CCOA,indicating distinct molecular compositions of SOA from different aged POA sources.Compared to aged BBOA,aged CCOA was more subject to conversion during aqueous phase processing.These results suggest that the variations in mass spectra and compositions need to be considered when simulating SOA processes.展开更多
Metal-organic frameworks(MOFs),assembled periodically by coordinating inorganic metal ions and organic motifs,have arisen widespread curiosity and intensive investigation owing to their tailorable electronic propertie...Metal-organic frameworks(MOFs),assembled periodically by coordinating inorganic metal ions and organic motifs,have arisen widespread curiosity and intensive investigation owing to their tailorable electronic properties and well-defined topological structure.However,the majority of MOFs are intrinsically dielectric or insulative[1]and typically form as 3D bulk or powder crystals,making them incompatible with complementary metal-oxide semiconductor(CMOS)techniques.In recent years,layer-stacked two-dimensional conjugated MOFs(2D c-MOFs),composed of planar conjugated ligands and linkages[2],have demonstrated high in-plane π conjugation and weak out-of-plane van der Waals interactions,due to their long-range electron delocalization over metal ions and ligands[3].As a result,highly tunable band gaps from semiconductor to conductor,modulable porosity from micropore to macropore and versatile processability into conductive 2D thin films with controllable lateral thickness and domain size are presented,rendering charming potential for applications in(opto-)electronics compared with classic 2D metal oxide,chalcogenide and crystalline polymer materials.To improve interfacial charge-transport and precisely tune the charge extraction and band alignment of 2D c-MOFs in(opto-)electronic devices[4],developing highly efficient synthetic methods of 2D c-MOFs is of utmost importance.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22361162668 and 42021004)the National Key Research and Development Program of China(No.2023YFC3706203).
文摘Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.
基金supported by the National Key R&D Program of China(No.2024YFC3714200)Guangxi Key Research and Development Program,China(No.Guike AB24010074)+2 种基金the National Natural Science Foundation of China(Nos.22276099,U24A20515 and 22361162668)the Natural Science Foundation of Jiangsu Province(No.BK20240036)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_1529).
文摘Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.
基金supported by the National Natural Science Foundation of China(Nos.11375082,22271189,12405385,92356301,and 21522105)the Hunan Provincial Natural Science Foundation of China(No.2021JJ30565)+5 种基金the Science and Technology Commission of Shanghai Municipality(Nos.21XD1402300,21JC1401700,and 21DZ2260400)the supports by the Double First-Class Initiative Fund of ShanghaiTech University(No.SYLDX0052022)the Analytical Instrumentation Center(No.SPST-AIC10112914)for adsorption measurementthe staff at BL17B1 beamline of the National Facility for Protein Science in Shanghai(NFPS),Shanghai Advanced Research Institute,CAS,for providing beamtime for single-crystal X-ray diffraction data collectionthe project CICECO-Aveiro Institute of Materials,Grants(Nos.UIDB/50011/2020,UIDP/50011/2020,and LA/P/0006/2020)financed by national funds through the FCT/MEC(PIDDAC).
文摘A series of dual-extended-polyhedral metal-organic frameworks(MOFs)was constructed based on the 14-coordinated Cu_(24)-MOP-1(MOP=metal-organic polyhedron)supermolecular building blocks(SBBs)with enhanced stability and tunable functionality for high water uptake efficiency and capacity.Exceptional water stability was demonstrated by the retention of chemical integrity and crystallinity of USC-CP-5(where USC-CP stands for University of South China coordination polymer)after exposure to boiling water for 24 h.Functionalization with-Cl,-OCH_(3),-OH,and-NH_(2)groups of USC-CP-5 resulted in water uptake capacities of 450,460,490,and 590 cm^(3)·g^(-1) at relative pressure(P/P_(0))=0.9,respectively.This performance is ascribed to both the increased hydrophilicity of the ligands and stronger hydrogen bonding.Intriguingly,high-temperature activated USC-5-NH_(2)exhibits a significant water uptake of 38.5 wt.%at P/P_(0)=0.3 and releases 0.44 L·kg^(-1) water between 25 and 65℃.This water release process is reversible for at least 100 cycles with minimal weight loss of only 1.6 wt.%.Consequently,USC-5-NH_(2)holds considerable potential for harvesting and releasing atmospheric water in arid desert regions,powered by solar energy.
基金supported by Natural Science Foundation of Zhejiang Province(Nos.LQ23E030002,LZ23B040001)the National Natural Science Foundation of China(Nos.52303226,21971049)L.Zhan acknowledges the research start-up fund from Hangzhou Normal University(4095C50222204002).
文摘Organic photovoltaics(OPVs)have achieved remarkable progress,with laboratory-scale single-junction devices now demonstrating power conversion efficiencies(PCEs)exceeding 20%.However,these efficiencies are highly dependent on the thickness of the photoactive layer,which is typically around 100 nm.This sensitivity poses a challenge for industrial-scale fabrication.Achieving high PCEs in thick-film OPVs is therefore essential.This review systematically examines recent advancements in thick-film OPVs,focusing on the fundamental mechanisms that lead to efficiency loss and strategies to enhance performance.We provide a comprehensive analysis spanning the complete photovoltaic process chain:from initial exciton generation and diffusion dynamics,through dissociation mechanisms,to subsequent charge-carrier transport,balance optimization,and final collection efficiency.Particular emphasis is placed on cutting-edge solutions in molecular engineering and device architecture optimization.By synthesizing these interdisciplinary approaches and investigating the potential contributions in stability,cost,and machine learning aspects,this work establishes comprehensive guidelines for designing high-performance OPVs devices with minimal thickness dependence,ultimately aiming to bridge the gap between laboratory achievements and industrial manufacturing requirements.
基金supported by the Nanjing Second Hospital talent lifting project(No.RCZD23001)the Jiangsu Province traditional Chinese medicine science and technology development general program(No.MS2023063)+1 种基金Medical Science and Technology Development Foundation,Nanjing Department of Health(No.ZKX20033)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX25_0240).
文摘Enhancing the activity of fragile enzymes is greatly useful for various purposes,including fabrication of enzyme-based immunosensors.Herein,we report a defect-engineering strategy for encapsulating enzymes within covalent organic frameworks(COFs),enabling the resulting immobilized enzymes with excellent catalytic activity and stability to construct high performance immunosensors.In this design,by consciously introducing monoaldehyde ligands into the imine-linked COFs structure,we have precisely customized the structural defects to improve enzyme loading capacity and conformational stability.Defect-engineering interaction modulation between enzymes and COFs drives the enhancement of catalytic performance.Compared to the pristine COFs,the enzyme@defective COFs composites with optimally tuned catalytic performance exhibit a 4.49-fold enhancement in enzymatic activity.Furthermore,it is demonstrated that the stable skeletons of COFs provide exceptional protection for the enzymes against external perturbations.Thereafter,the optimized enzyme@defective COFs are employed to fabricate immunosensor.We have successfully established a detection method for prostate-specific antigen(PSA),achieving a low detection limit of 0.09 ng/mL.More importantly,the developed immunosensor has successfully distinguished the prostate cancer patients from healthy individuals.This work establishes a novel paradigm for enzyme immobilization,ultimately empowering the construction of a PSA immunosensor with high sensitivity,remarkable operational stability,and great clinical application potential.
基金supported by the National Natural Science Foundation of China(No.51939009)Shenzhen Science and Technology Program(Nos.JCYJ20241202125905008 and GXWD20201231165807007-20200810165349001).
文摘A trace analytical method based on solid-phase extraction gas chromatography-tandem mass spectrometry(SPE–GC–MS/MS)was developed for the rapid detection of 256 semi-volatile organic compounds(SVOCs),including 25 polycyclic aromatic hydrocarbons(PAHs),70 polychlorinated biphenyls(PCBs),123 pesticides,20 phthalate esters(PAEs),4 organophosphate esters(OPEs),9 synthetic musks(SMs),and 5 UV filters(UVs)in water.No-tably,this method provided a decent linearity of calibration standards(R^(2)>0.999),excellent method limits of quantification(MLOQs)(0.12–11.41 ng/L),satisfactory matrix spiking recovery rates(60.4%–126%),and high precision(intra-day relative standard deviations(RSDs):1.0%–10.0%,inter-day RSDs:3.0%–15.0%,and inter-week RSDs:3.4%–15.7%),making it suitable for trace-level studies.Statistical analysis revealed that SVOCs with higher volatility exhibited enhanced recovery rates.Validation of the methodology involved analyzing SVOCs in real spring water and river water samples.Twenty-seven SVOCs were detected in spring water and 58 in river water,with an average concentration of 631.73 and 16,095 ng/L,respectively.Among the detected SVOCs,PAEs constituted the predominant proportion.This study underscored the presence of SVOCs contamination specifi-cally within the spring water,although SVOCs concentrations in river water were significantly greater than those found in spring water.In summary,this sensitive method based on SPE–GC–MS/MS was successfully developed and validated for the rapid analysis of a diverse array of 256 SVOCs at trace levels in water,including not only the traditional highly valued PAHs,PCBs,pesticides,and PAEs,but also the emerging OPEs,UVs,and SMs.
基金financially supported by the National Natural Science Foundation of China(No.22508360)Zhejiang Provincial Natural Science Foundation of China(No.QN26B060028)+1 种基金the National Key Research and Development Program Nanotechnology Specific Project(No.2020YFA0210900)Innovative Team Project of Guang-dong Ordinary University(No.2019KCXTD002).
文摘Constructing catalysts featuring an ordered structure,stable performance,and uniformly dispersed catalytic sites is vital for the epoxidation of small-molecular olefins.Here,we design catalysts by tracing the oxidationprocess origin and synthesize a series of highly dispersed metal porphyrin-based covalent organic frameworks(COFs)materials.The aim is to efficiently oxidize the C-H bonds of cumene by air to in-situ generate organic peroxides at a safe concentration,and integrate the multi-step oxidation method of cumene in industry into a one-step method for olefins’epoxidation.The carbonyl-ruthenium COF(Ru-COF-1)exhibits excellent performance,with 98% epoxide selectivity,1221.77 h^(-1) productivity,and over 95% selectivity after 9 cycles for 1-hexene.Analysis of structure-properties-catalytic relationships of Ru-COF-1 shows that,compared with Ru-porphyrins and metal-free COFs,the enhanced reaction performance mainly results from Ru metal introduction,which promotes benzylic proton transfer in cumene.Besides,Ru-COF-1’s porous,ordered structure aids oxygen enrichment,forming active peroxy radicals with the cumene carboncentered radicals formed on the catalyst surface.Ru-H sites then accelerate active oxygen transfer from peroxy radicals,enabling olefin tandem epoxidation.Density functional theory(DFT)calculations verify the reaction mechanism,and this work offers a reference for the design of catalysts for the green,safe,and efficient oxidation of olefins.
基金supported by the National Natural Science Foundation of China(No.22506042)the Natural Science Foundation of Henan Province(Nos.252300421710 and 252300421552)the High level Talent Research Launch Fund of Henan University of Technology(No.2024BS061).
文摘Effective control of gas-phase pollutants(volatile organic compounds(VOCs)and CO)is critical to human health and the ecological environment.Catalytic oxidation is one of the most promising technologies for achieving efficient volatile organic compounds and CO emission control.The subnano cluster catalyst can not only provide catalytic sites with multiple metal atoms,but also maintain full utilization efficiency.Almost all metal atoms in highly dispersed clusters can be used for adsorption and conversion of reactants.Recently,various types of sub-nano clusters,including subnano cluster oxides,have been developed and demonstrated excellent performance in low-temperature gas-phase pollutants combustion.In this mini review,we systematically summarize the structure,physicochemical properties,characterization,and applications of sub-nano cluster catalysts in catalytic oxidation of CO,methane,propane,propylene,toluene and its derivatives,formaldehyde and chlorinated volatile organic compounds.Finally,we have analyzed and discussed the problems and challenges faced by sub-nano cluster catalysts in both basic research and practical applications,providing a scientific basis for the design,synthesis,and application of efficient heterogeneous catalysts for CO and VOCs oxidation.
文摘Correction to:Nano-Micro Letters(2026)18:10.https://doi.org/10.1007/s40820-025-01852-8 Following publication of the original article[1],the authors reported that the last author’s name was inadvertently misspelled.The published version showed“Hongzhen Chen”,whereas the correct spelling should be“Hongzheng Chen”.The correct author name has been provided in this Correction,and the original article[1]has been corrected.
基金Financial support from the National Natural Science Foundation of China(22375024,21975031,21734009,51933001,22109080,and 52173174)the Natural Science Foundation of Shandong Province(No.ZR2022YQ45)+2 种基金the Taishan Scholars Program(Nos.tstp20221121 and tsqnz20221134)The Beijing Natural Science Foundation(No.2244073)supported by State Key Laboratory of Bio-Fibers and Eco-Textiles(Qingdao University)(RZ2200002821)is acknowledged.
文摘A nonfused ring electron acceptor(NFREA),designated as TT-Ph-C6,has been synthesized with the aim of enhancing the power conversion efficiency(PCE)of organic solar cells(OSCs).By integrating asymmetric phenylalkylamino side groups,TT-Ph-C6 demonstrates excellent solubility and its crystal structure exhibits compact packing structures with a three-dimensional molecular stacking network.These structural attributes markedly promote exciton diffusion and charge carrier mobility,particularly advantageous for the fabrication of thick-film devices.TT-Ph-C6-based devices have attained a PCE of 18.01%at a film thickness of 100 nm,and even at a film thickness of 300 nm,the PCE remains at 14.64%,surpassing that of devices based on 2BTh-2F.These remarkable properties position TT-Ph-C6 as a highly promising NFREA material for boosting the efficiency of OSCs.
基金granted by the National Natural Science Foundation of China(Nos.52533008,21835003,62274097,and 62004106)National Key Research and Development Program of China(Nos.2024YFB3612500,2024YFB3612600,and 2023YFB3608900)+2 种基金Basic Research Program of Jiangsu Province(No.BK20243057)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX25_1213)the Natural Science Foundation of Nanjing Universityof Posts and Telecommunications(No.NY225135).
文摘To meet the growing needs of flexible and wearable electronics,stretchable energy storage devices—especially supercapacitors(SCs)—have become a key focus in advanced energy storage research.However,achieving both mechanical stretchability and high capacitance in SC still faces great challenges,and the crucial factors lie in creating superior electrode materials that exhibit high electrochemical performance as well as excellent mechanical stretchability.Covalent organic frameworks(COFs)possess considerable potential as electrode materials for SCs by virtue of stable organic frameworks,open channels and designable functional groups.Nevertheless,their applications in flexible SCs are greatly hindered by their rigid characteristics.Here a novel COFs@conductive polymer hydrogels(CPHs)@poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS)complexes,which integrate the pseudocapacitance of PDITAPA COF,mechanical stretchability of hydrogels and high conductivity of PEDOT:PSS,has been developed as stretchable electrode of SCs.Physically cross-linked PEDOT nanofibers,with their interlinked and entangled architecture,collectively boost mechanical,electrical,and electrochemical performance.The COFs@CPHs@PEDOT:PSS simultaneously demonstrates outstanding mechanical stretchability,high electrical behaviors,and superior swelling characteristics.The resulting SC exhibits advantages of simple structures,facile assembly processes,high specific capacitance,excellent cycling stability,and arbitrary deformation,which holds great application prospects for wearable electronic products.Owing to its uncomplicated structure,ease of production,high energy storage capacity,robust cycling performance,and adaptability to deformation,this fabricated SC is well-suited for next-generation wearable technologies.
基金supported by the National Key Research and Development Program of China(No.2021YFC2901100)the National Natural Science Foundation of China(No.22478425).
文摘Photocatalytic carbon dioxide(CO_(2))reduction offers an alternative strategy for converting CO_(2)into high-value added gaseous fuels,thereby paving the way for the development of clean and renewable energy.Metal-organic frameworks(MOFs),characterized by their highly porous structure,exceptional CO_(2)adsorption capacity,and tunable architecture,have emerged as promising candidates for photocatalytic CO_(2)reduction.This review systematically examines the recent advancement in MOFs-based photocatalysts for CO_(2)reduction to CO.It begins with the overview of the fundamental mechanisms and processes of MOFs towards photocatalytic CO_(2)reduction.Subsequently,common strategies for the modulation of MOFs-based photocatalysts are summarized,including metallic site modification,functionalized ligand incorporation,morphological control,defect engineering,and heterostructure construction.Notably,the review analyzes the critical factors contributing to the high selectivity of CO_(2)photoreduction to CO from both thermodynamic and kinetic perspectives.The conclusion addresses current challenges and future perspectives in designing highly efficient photocatalysts with abundant active sites,providing valuable insights for their continued development.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
基金supported by the National Natural Science Foundation of China(Nos.22406081,22276086,22306086)the Natural Science Foundation of Jiangxi Province(No.20232BAB213029),all of which are greatly acknowledged by the authors.
文摘Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.
基金supported by the National Key Research and Development program of China (Nos. 2024YFA1410700 and 2021YFA1200700)the National Natural Science Foundation of China (Nos. T2222025, 62174053, 62474065 and 52372120)+3 种基金the Natural Science Foundation of Chongqing (CSTB2024NSCQ-JQX0005)the Shanghai Science and Technology Innovation Action Plan (Nos. 24QA2702300 and 24YF2710400)the National Postdoctoral Program (GZB20240225)the Fundamental Research Funds for the Central Universities。
文摘Poly(vinylidene-trifluoroethylene) [P(VDF-TrFE)] copolymer films generally demonstrate limited compatibility with organic semiconductors. The material is frequently compromised by exposure to organic semiconductor solutions and other fabrication processes utilized in the production of organic ferroelectric transistors. In this study, an organic ferroelectric field effect transistor(OFeFET) with the 6,13-Bis(triisopropylsilylethynyl) pentacene(TIPS-pentacene) channel is fabricated, in which the aluminum oxide(Al_(2)O_(3)) interlayer is used to improve compatibility. The device displays polymorphic memory and synaptic plasticity of long-term potentiation and depression. Furthermore, an artificial neural network constructed using our devices is simulated to succeed in recognizing the MNIST handwritten digit database with a high accuracy of 92.8%. This research offers a viable approach to enhance the compatibility of the organic ferroelectric polymer P(VDF-TrFE) with organic semiconductors.
基金supported by the project of“Shale Gas Resources Investigation and Evaluation in the Baoshan Block”from Sinopec Exploration Company and the National Natural Science Foundation of China(41925014 and 42172192)。
文摘Lower Paleozoic black shales are important source rocks worldwide.The Upper Ordovician-Lower Silurian Renheqiao Formation of the Baoshan Block is a low-maturity equivalent of the Wufeng-Longmaxi(WF-LMX)Shale of the Sichuan Basin.However,organic matter(OM)characteristics in these low-maturity Lower Paleozoic shales are not well understood.In this study,50 Renheqiao Formation shale samples collected from seven outcrop sections and one drill core were investigated with organic petrology,organic geochemistry,R_(o)ck-Eval pyrolysis,N_(2) and CO_(2) adsorption,and scanning electron microscope(SEM)analyses to study the OM content,type,thermal maturity,and the development of OM-hosted pores in these Lower Paleozoic shales.The total organic carbon(TOC)content of the Renheqiao Formation shales varies,with the maximum content of 10.07 wt%.R_(o)ck-Eval pyrolysis results show that present OM in the Renheqiao Formation shales is Type IV kerogen,a result of advanced thermal maturation.Graptolite reflectance(GR_(o))ranges from 1.26%to 1.85%,and equivalent vitrinite reflectance(EqR_(o))converted from GR_(o) ranges from 1.08%to 1.51%,indicating that the studied Renheqiao Formation shales are dominantly within the late-mature stage.EqR_(o) based on R_(o)ck-Eval T_(max) shows large variations,which indicates that R_(o)ck-Eval T_(max) is not a reliable thermal maturity indicator for the Lower Paleozoic Renheqiao Formation shales.Caution should be applied when assessing the thermal maturity of high-maturity black shales based on T_(max) when the S2 values are too low.Organic petrographic observations show that OM in these shales is dominated by solid bitumen(>70 vol%of total OM),with minor contributions by graptolites and chitinozoans.The specific surface area and pore volume of shales are controlled by TOC content.Organic pores are hosted by solid bitumen and were not observed in graptolites when examined under the SEM.Although the Renheqiao Formation has a lower thermal maturity than the over-mature WF-LMX Shale,it is mature enough that primary oil-prone macerals have been thermally transformed and could not be identified under the microscope.
基金supported by the National Natural Science Foundation of China(Nos.51902121 and 22372067)。
文摘Covalent organic frameworks(COFs)are two-(2D)or threedimensional(3D)crystalline,porous networks generated by reversible polymerization of organic building blocks[1,2].The structures and functionalities of COFs are precisely controlled via appropriately selected organic building blocks.This design imparts unique properties to COFs,including exceptional structural stability,tunable pore structure,and surface chemical activity,making them promising for gas separation,catalysis,optoelectronics,and sensing applications.Since Yaghi et al.'s seminal report on COFs in 2005[2],these frameworks have swiftly emerged as a hotspot in the field of materials.Originally,the focus was on fabricating rigid frameworks with static structures and optoelectronic properties.However,the inherently static nature of these frameworks hinders their responsiveness to external stimuli,potentially constraining their functionality in specific applications.Hence,an increasing number of researchers are now directing their attention toward the development of dynamic COFs capable of modifying their structures in response to external stimuli[3].Specifically,dynamic 2D COFs exhibiting enhanced structural responsiveness are of particular interest due to their capability to integrate switchable geometries and porosities with semiconductor building blocks,as well as electron conjugation across COF layers and π-stacked columns,which may enable stimuli-responsive electronic and spin properties[4].
基金support from the National Natural Science Foundation of China(22088101,21733003,22365021,22305132)the Inner Mongolia Autonomous Region“Grassland Talents”Project(2024098)+3 种基金the Inner Mongolia Natural Science Foundation Youth Fund(2023QN02014)The Local Talent Project of Inner Mongolia(12000-15042222)the Basic Research Expenses Supported under 45 Years Old of Inner Mongolia(10000-23112101/036)the“Young Academic Talents”Program of Inner Mongolia University 23600-5233706.
文摘As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0760200)the National Natural Science Foundation of China(Grant No.42377101,91744207).
文摘Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA process by integrating the OA and associated ions previously misidentified as inorganic aerosol in high-resolution aerosol mass spectrometry data.The mass spectra and time series of primary OA(POA)and less oxidized oxygenated OA(OOA)identified by this new method resembled those resolved by traditional PMF.However,more oxidized OOA(MO-OOA)identified by traditional PMF can be further subdivided into multiple OA factors,including nitrogen-enriched OA(ON-OA)and sulfur-enriched OA(OS-OA)in summer,and ON-OA,OS-OA,and OOA in winter.Our findings highlight the significant role of photochemical processes in the formation of OS-OA compared to ON-OA.The compositions of reconstructed MO-OOA varied under different Ox(=O_(3)+NO_(2))and relative humidity conditions,emphasizing the limitations of using a constant mass spectrum.Aged biomass burning OA(BBOA)and coal combustion OA(CCOA),previously misattributed as POA,contributed 9.2%(0.43μg m^(−3))and 7.0%(0.33μg m^(−3))to SOA,respectively.Aged BBOA was more prone to forming OS-OA,whereas ON-OA showed higher correlations with aged CCOA,indicating distinct molecular compositions of SOA from different aged POA sources.Compared to aged BBOA,aged CCOA was more subject to conversion during aqueous phase processing.These results suggest that the variations in mass spectra and compositions need to be considered when simulating SOA processes.
基金supported by the National Natural Science Foundation of China(Nos.22201086,22471084,92261204,21925104,and 22431005).
文摘Metal-organic frameworks(MOFs),assembled periodically by coordinating inorganic metal ions and organic motifs,have arisen widespread curiosity and intensive investigation owing to their tailorable electronic properties and well-defined topological structure.However,the majority of MOFs are intrinsically dielectric or insulative[1]and typically form as 3D bulk or powder crystals,making them incompatible with complementary metal-oxide semiconductor(CMOS)techniques.In recent years,layer-stacked two-dimensional conjugated MOFs(2D c-MOFs),composed of planar conjugated ligands and linkages[2],have demonstrated high in-plane π conjugation and weak out-of-plane van der Waals interactions,due to their long-range electron delocalization over metal ions and ligands[3].As a result,highly tunable band gaps from semiconductor to conductor,modulable porosity from micropore to macropore and versatile processability into conductive 2D thin films with controllable lateral thickness and domain size are presented,rendering charming potential for applications in(opto-)electronics compared with classic 2D metal oxide,chalcogenide and crystalline polymer materials.To improve interfacial charge-transport and precisely tune the charge extraction and band alignment of 2D c-MOFs in(opto-)electronic devices[4],developing highly efficient synthetic methods of 2D c-MOFs is of utmost importance.
