To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and ...To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).展开更多
In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesize...In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesized by hydrothermal method.The structure and properties were systematically characterized and tested by techniques such as single‑crystal X‑ray diffraction,powder X‑ray diffraction,thermogravimetric analysis,infrared spectroscopy,and fluorescence spectroscopy.The results indicate that this complex has a unique 3D structure,excellent thermal stability,and outstanding luminescent performance.Based on its luminescent properties,a polymer‑embedding method was employed to fabricate the Gd‑Na‑MOF into a flexible,washable composite fluorescent film,Gd‑Na‑MOF@PMMA/BMA(PMMA=polymethyl methacrylate,BMA=butyl methacrylate).This fluorescent film exhibited highly sensitive recognition capability for tyramine,with a low detection limit of 1.66μmol·L^(-1).It was used for the detection of tyramine in bananas,with a recovery rate of 96.92%‑100.26%.CCDC:2466949.展开更多
CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organ...CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.展开更多
A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescenc...A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.展开更多
Glucose,ascorbic acid(AA),uric acid(UA),and dopamine(DA)are vital biomarkers whose dynamic concentrations correlate with critical diseases;however,multiplexed detection remains challenging for conventional electrochem...Glucose,ascorbic acid(AA),uric acid(UA),and dopamine(DA)are vital biomarkers whose dynamic concentrations correlate with critical diseases;however,multiplexed detection remains challenging for conventional electrochemical sensors because of their limited sensitivity and selectivity.Here,we present a millimeter-scale all-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS)organic electrochemical transistor(OECT)platform that integrates dual-mode sensing with enzyme/metal-free operation for ultrasensitive biomarker monitoring.By engineering polycrystalline PEDOT:PSS channels via H_2 SO_4 post-treatment,the device achieves record-high conductivity(about(2312.0±29.9)S·cm^(–1)),maximum transconductance(about(2.82±0.12)mS),and on/off ratio(about 210.0±7.8),enabling signal amplification at low gate voltages.The dual-mode strategy combines the selectivity of electrochemistry with the sensitivity of OECTs,realizing simultaneous detection of glucose,AA,UA,and DA with clinical-level sensitivity:detection limits down to 8 nmol·L^(–1)(glucose),0.5 nmol·L^(–1)(AA),5 nmol·L^(–1)(DA),and 0.5 nmol·L^(–1)(UA).Validation using human urine samples yielded recovery rates of 94%–114%.This flexible sensing platform provides a new pathway for the development of wearable biosensors for precision diagnostics.展开更多
Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.Th...Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.They feature well-defined pore structure,high specific surface area,and tunable physicochemical properties,endowing them with broad application prospects in gas storage,molecular separation.展开更多
Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through...Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through covalent bonds exhibits excellent structural stability.It has been shown that the stationary phases prepared by combining MOF and COF can make up for the poor stability of MOF@SiO_(2),and the MOF/COF composites have superior chromatographic separation performance.However,the traditional methods for preparing COF/MOF based stationary phases are generally solvent thermal synthesis.In this study,a green and low-cost synthesis method was proposed for the preparation of MOF/COF@SiO_(2) stationary phase.Firstly,COF@SiO_(2) was prepared in a choline chloride/ethylene glycol based deep eutectic solvent(DES).Secondly,another acid-base tunable DES prepared by mixing p-toluenesulfonic acid(PTSA)and 2-methylimidazole in different proportions was introduced as the reaction solvent and reactant for rapid synthesis of MOF/COF@SiO_(2).Compared with the toxic transition metal-based MOFs selected in most previous studies,a lightweight and non-toxic S-zone metal(calcium) based MOF was employed in this study.PTSA and calcium will form the calcium/oxygen-containing organic acid framework in acidic DES,which assembles with terephthalic acid dissolved in basic DES to form MOF.The strong hydrogen bonding effect of DES can facilitate rapid assembly of Ca-MOF.The obtained Ca-MOF/COF@SiO_(2) can be used for multi-mode chromatography to efficiently separate multiple isomeric/hydrophilic/hydrophobic analytes.The synthesis method of Ca-MOF/COF@SiO_(2) is green and mild,especially the use of acid-base tunable DES promotes the rapid synthesis of non-toxic Ca-MOF/COF@silica composites,which offers an innovative approach of greenly synthesizing novel MOF/COF stationary phases and extends their applications in the field of chromatography.展开更多
In natural aquatic ecosystems,algal-derived organic carbon(AOC)often coexists with exogenous organic carbon(EOC).Microbial utilization of these distinct carbon sources affects carbon flux and transformation in water c...In natural aquatic ecosystems,algal-derived organic carbon(AOC)often coexists with exogenous organic carbon(EOC).Microbial utilization of these distinct carbon sources affects carbon flux and transformation in water column and algal growth.Microcystis blooms significantly increase AOC levels in water,but the microbial transformation process of Microcystis-derived AOC in the presence of EOC remain poorly understood.We conducted a simulated experiment by introducing^(13)C-sodium bicarbonate and^(13)C-glucose as substrates for indoor simulation of non-axenic Microcystis aeruginosa(M.aeruginosa)populations in a sealed system.The microbial transformation processes of AOC and EOC and their effects on M.aeruginosa growth were investigated.Results demonstrated that the addition of glucose accelerated M.aeruginosa growth and significantly increased their biomass.During the experiment,as the particulate organic carbon and nitrogen content increased,the concentrations of CO_(2)and N_(2)O were gradually decreased,while the concentration of CH4 were gradually increased.Significant differences were observed in the microbial processes involved in the uptake of AOC and EOC.Bacteria involved in AOC transformation throughout the growth period were dominated by Proteobacteria,Gemmatimonadota,Actinobacteriota,Bacteroidota,Acidobacteriota,and Firmicutes.The bacteria involved in EOC transformation were dominated by Proteobacteria,Actinobacteriota,Firmicutes,Cyanobacteria,Armatimonadota,and Bacteroidota.Linear discriminant analysis Effect Size(LEfSe)analysis revealed Massilia and Akkermansia as biomarkers involved in AOC transformation,while Ligilactobacillus was associated with EOC transformation.These findings provide valuable insights into the effects of EOC on algae-bacteria interaction,and on the dynamics of carbon and nitrogen cycling among M.aeruginosa and its associated bacteria.展开更多
Zero-dimensional(0D)organic-inorganic metal halide perovskite is one of the hot research topics in the field of optoelectronic materials.Their structure generally consists of discrete metal halide octahedra entirely i...Zero-dimensional(0D)organic-inorganic metal halide perovskite is one of the hot research topics in the field of optoelectronic materials.Their structure generally consists of discrete metal halide octahedra entirely isolated by surrounding organic cations,forming independent luminescent centers[1,2].Such a configuration results in high exciton binding energy and exceptional luminescence efficiency,due to strong quantum confinement[3,4].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
This study employed integrated metabolomic and transcriptomic analyses to investigate the impacts of moderate withering(approximately 30%weight loss)on organic acid and flavonoid accumulation in blueberries and the re...This study employed integrated metabolomic and transcriptomic analyses to investigate the impacts of moderate withering(approximately 30%weight loss)on organic acid and flavonoid accumulation in blueberries and the resultant blueberry wines.Moderate withering led to decreases in aliphatic organic acids but increases in phenolic acids and flavonoids in blueberries.The decrease in malate could be linked to the downregulated VcMDH and VcDTC,and the decrease in citrate and 2-oxoglutarate could be a consequence of y-aminobutyric acid shunt activation.The increases of phenolic acids were associated with upregulated VcCAD and VcPOD in withered blueberries.Additionally,moderate withering upregulated the expression of VcLAR and VcUFGT,promoting flavonoid accumulation.In blueberry wines,moderate withering decreased total aliphatic organic acid content but increased anthocyanin content,consistent with the findings in blueberries.Overall,this study provided references for applying moderate withering in blueberry winemaking,contributing to modulating acidity and enriching phenolic substances.展开更多
In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry bet...In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed.Herein,two novel imide-linked 1D COFs with phthalocyanine building blocks,namely NiPc-CZDM-COF and NiPc-CZDL-COF,were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II)(NiPc(COOH)_(8))with 9H-carbazole-3,6-diamine(CZDM)and 4,4′-(9H-carbazole-3,6-diyl)dianiline(CZDL),respectively.Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Due to their high ratio of exposed active centers on the edge sites of porous ribbons,both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0%and 7.5% according to the electrochemical measurement,resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%.In particular,NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH3 partial current density of−246 mA/cm^(2),ammonia yield rate of 19.5 mg cm^(−2) h^(−1),and turnover frequency of 5.8 s^(−1) at−1.2 V in an H-type cell associated with its higher conductivity.This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.展开更多
High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carb...High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody(Ab1)and ferrocene(Fc),and used for electrochemical detection of AFP.Due to the small,homogeneous pore size of the COF,Ab1 with a big size was immobilized on the surface of the COF,while Fc with a small size was covalently modified both on the surface and in the pores of COF.The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers.Meanwhile,the enriched Fc molecules not only improved the conductivity of the COF,but also effectively transferred and amplified the electrochemical signal.This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL(S/N of 3:1)and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations.Furthermore,this immunosensor showed excellent selectivity,stability and reproducibility in the testing of real samples.This study presents an innovative prototype for construction of a precious metal-free,antibody-directly-immobilized,simple and stable electrochemical immunoprobe.展开更多
In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation pro...In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation processes(AOPs).Results indicated that the silicon and oxygen elements from the montmorillonite were incorporated into the catalyst matrix to form the Si-O-C structure.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array,achieving over 90 % removal rate of most pollutants within 60 min.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array.The salt bridge system confirmed that pollutants can provide electrons to the Si-O-C/PMS system,and we verified that the electron transfer process(ETP) mechanism was the main pathway for the degradation of pollutants in the Si-O-C/PMS system via the open-circuit potential analysis.In combination with the structural properties of different pollutants,we discovered that electron-donating pollutants can supply more electrons to the Si-O-C/PMS system,thereby enhancing the ETP process.The findings of this study are anticipated to advance the development and practical application of layered carbonaceous materials-based catalysts and support the design and implementation of nanoconfined catalysts in the field of AOPs.展开更多
Achieving simultaneous enhancement of crystallinity and optimal domain size remains a fundamental challenge in organic photovoltaics(OPVs),where conventional crystallization strategies often trigger excessive aggregat...Achieving simultaneous enhancement of crystallinity and optimal domain size remains a fundamental challenge in organic photovoltaics(OPVs),where conventional crystallization strategies often trigger excessive aggregation of small-molecule acceptors.This work pioneers a kinetic paradigm for resolving the crystallinity-domain size trade-off in organic photovoltaics through dual-additive-guided stepwise crystallization.By strategically pairing 1,2-dichlorobenzene(o-DCB,low binding energy to Y6)and 1-fluoronaphthalene(FN,high binding energy),we achieve temporally decoupled crystallization control:o-DCB first mediates donor-acceptor co-crystallization during film formation,constructing a metastable network,whereupon FN induces confined Y6 crystallization within this framework during thermal annealing,refining nanostructure without over-aggregation.Morphology studies reveal that this synergy enhances crystallinity of(100)diffraction peaks by 21%–10%versus single-additive controls(o-DCB/FN alone),while maintaining optimal domain size.These morphological advantages yield balanced carrier transport(μh/μe=1.23),near-unity exciton dissociation(98.53%),and a champion power conversion efficiency(PCE)of 18.08%for PM6:Y6,significantly surpassing single-additive devices(o-DCB:17.20%;FN:17.53%).Crucially,the dual-additive strategy demonstrates universal applicability across diverse active layer systems,achieving an outstanding PCE of 19.27%in PM6:L8-BO-based devices,thereby establishing a general framework for morphology control in high-efficiency OPVs.展开更多
Bentonite is a necessary binder in producing pellets.Its excessive use reduces the iron grade of pellets and increases production costs.Minimizing bentonite dosage is essential for producing high-quality iron ore pell...Bentonite is a necessary binder in producing pellets.Its excessive use reduces the iron grade of pellets and increases production costs.Minimizing bentonite dosage is essential for producing high-quality iron ore pellets.Addressing the gap in the application of organically-intercalated modified bentonite in the pelletizing field,this study introduces an innovative modification process for bentonite that employs the synergistic effect of mechanical force and dimethyl sulfoxide to enhance the intercalation of organic compounds within bentonite,thus significantly enhancing its binding performance.The colloid value and swell capacity of modified bentonite(98.5 m L/3g and 55.0 m L/g)were much higher than the original bentonite(90.5 m L/3g and 17.5 m L/g).With the decrease of bentonite dosage from1.5wt%to 1.0wt%,the drop number of green pellets from a height of 0.5 m and the compressive strengths of roasted pellets using the modified bentonite(6.0 times and 2916 N per pellet)were significantly higher than those of the original bentonite(4.0 times and 2739 N per pellet).This study provides a comprehensive analysis of the intercalation modification mechanism of bentonite,offering crucial technical insights for the development of high-performance modified bentonite as iron ore pellet binders.展开更多
Abstract:Graphene-Based separation membranes hold promise for water treatment.However,their practical deployment in high-salinity brines remains challenging due to structural instability.Herein,a defect-free Na^(+)-Cu...Abstract:Graphene-Based separation membranes hold promise for water treatment.However,their practical deployment in high-salinity brines remains challenging due to structural instability.Herein,a defect-free Na^(+)-Cu^(2+)/GO-PEI nanocomposite membrane was fabricated via a pH-controlled cross-linking polymerization strategy.Polyethyleneimine(PEI)serves as a critical interfacial stabilizer,enhancing the connection between the Na^(+)-GO and Cu^(2+)-GO layers through amide bond formation with GO nanosheets while facilitating Cu^(2+)chelation.The Na^(+)/GO layer modifies the pore structure of the polyether sulfone(PES)substrate,synergistically optimizing the membrane’s microstructure.Performances evaluation revealed that the as-prepared membrane achieved exceptional separation efficiency(>98%)for tributyl phosphate,sulfonated kerosene,and bis(2-ethylhexyl)phosphate in high-salinity brine,accompanied by a high flux of 160~224 L·m^(-2)·h^(-1).Notably,it exhibited robust chemical stability in corrosive environment and maintained mechanical durability after 500 folding cycles coupled with consistent separation performances over 10 recycles.This study presents a novel multi-component modification approach for constructing high-performance GObased membrane,promising practical applications in organic pollutant removal from high salt solution.展开更多
The Dongsha area,a key target for gas hydrate exploration,is influenced by multiple factors,including sedimentary processes and the paleoenvironment,which play critical roles in gas hydrate formation.To elucidate the ...The Dongsha area,a key target for gas hydrate exploration,is influenced by multiple factors,including sedimentary processes and the paleoenvironment,which play critical roles in gas hydrate formation.To elucidate the coupling among sedimentary processes,paleoenvironment,and gas hydrate accumulation,this study investigates the Site DS-W16 using particle size analysis,biological component content,and geochemistry data.Oxygen isotope data from foraminifera and biostratigraphic evidence indicate that sedimentation at the bottom of core interval from Site DS-W16 began during MIS 11(Marine isotope stage).The sedimentation dynamics of the studied layers are complex,involving gravity flows,traction currents,and suspended deposition.Organic matter shows a significant correlation with transgressive-regressive cycle.The site DS-W16 contains two distinct gas hydrate reservoirs:a shallow reservoir(10-24 mbsf)and a deep reservoir(below 182 mbsf).The paleomarine environment influences gas hydrate accumulation by altering sedimentary processes and sediment characteristics,especially the distribution of biological components.Both shallow and deep gas hydrate reservoirs formed under dynamic conditions dominated by traction currents and are characterized by a higher abundance of foraminifera.Sedimentary layers rich in foraminifera and modified by traction currents represent key intervals for preferential gas hydrate accumulation.展开更多
The crystallization and aggregation characteristics of the active layer components in organic solar cells(OSCs)are one of the core factors determining photovoltaic performance,influencing the entire process from light...The crystallization and aggregation characteristics of the active layer components in organic solar cells(OSCs)are one of the core factors determining photovoltaic performance,influencing the entire process from light absorption to charge separation,transport,and ultimately charge collection.Dynamic changes in crystallization and aggregation states can also disrupt the microstructure of the active layer,thus shortening the lifetime of the cell.In this study,a morphology modulation strategy is proposed to regulate the crystallization kinetics of non-fullerene acceptors by employing the polymer molecule PYIT as a nucleating agent.An appropriate amount of PYIT was first completely dissolved with the non-fullerene acceptor Y6 and left to stand for 24 h,followed by the fabrication of layer-by-layer processed OSCs.Experiments demonstrated that high crystallinity of PYIT allows it to act as a crystallization nucleus,promoting the crystallization,orientation consistency,and ordered stacking of the acceptor.These nanoscale structural optimizations facilitate efficient charge transport,enhance exciton dissociation efficiency,and suppress unfavorable energetic disorder.Consequently,not only was the power conversion efficiency(PCE)of D18-Cl/Y6-based layer-by-layer processed OSC increased from 18.08%to 19.13%,but the atmospheric stability and long-term lifetime of the OSCs were also significantly improved.Notably,this strategy is also applicable to indoor OSCs,and the PYIT-optimized device can achieve a PCE of 27.0%under 1000 lux light-emitting diode(LED,3200K)irradiation,which is superior to that of the control device(24.2%).This work develops a crystal engineering strategy that is able to simultaneously optimize the microscopic morphology and charge dynamics properties in OSCs,thereby achieving simultaneous improvement in efficiency and stability.展开更多
This research explores the influence of crystallinity on gas chromatographic(GC) separation using covalent organic frameworks(COFs) as stationary phases.Three COF materials(CTF-DCBs) with varying crystallinity were sy...This research explores the influence of crystallinity on gas chromatographic(GC) separation using covalent organic frameworks(COFs) as stationary phases.Three COF materials(CTF-DCBs) with varying crystallinity were synthesized and characterized.CTF-DCB-1,with superior crystallinity,demonstrated highselectivity GC separation of benzene isomers as well as styrene/phenylacetylene mixtures,while CTFDCB-2 and CTF-DCB-3 exhibited lower crystallinity and worse separation performance.Thermodynamic and kinetic tests showed that CTF-DCB-1 had the worst thermodynamic adsorption but low diffusion mass transfer resistance,which resulted in the best separation.Therefore,optimizing the crystallinity of COFs is necessary for balancing the kinetic diffusion and thermodynamic interactions towards the analytes,achieving high-performance GC stationary phases.展开更多
基金Supported by National Natural Science Foundation of China(22378180,22078141)Education Department Foundation of Liaoning Province(JYTMS20230960)。
文摘To deepen understanding of the evolution of coal char microstructural properties of coal char during the co-pyrolysis of coking coal with additives,this study incorporated two typical additives,coal tar pitch(CTP)and waste plastic(HDPE),into a blended coal sample and carried out pyrolysis experiments.The pyrolysis process and the microstructure of char were systematically characterized using various analytical techniques,including thermogravimetric analysis(TGA),X-ray diffraction(XRD)and Raman spectroscopy.Data correlation analysis was performed to reveal the mechanism of carbon structural ordering evolution within the critical temperature range(350−600℃)from colloidal layer formation to semi-coke conversion in coking coal,and to elucidate the regulatory effects of different additives on coal pyrolysis pathways.The results indicate that HDPE releases free radicals during high-temperature pyrolysis,accelerating the pyrolysis reaction and increase the yield of volatile components.Conversely,CTP facilitates pyrolysis at low temperatures through its light components,thereby delaying high-temperature reactions due to the colloidal layer’s effect.XRD results indicate that during the process of pyrolysis,there is a progressive decrease in the interlayer spacing of aromatic layers(d002),while the aromatic ring stacking height(L_(c))and lateral size(L_(a))undergo significant of carbon skeleton ordering.Further comparative reveals that CTP partially suppresses structural ordering at low temperatures,whereas HDPE promotes the condensation and alignment of aromatic clusters via a free radical mechanism.Raman spectroscopy reveals a two-stage reorganization mechanism in the microstructure of the coal char:the decrease in the I_(D)/I_(G)ratio between 350 and 550℃is primarily attributed to the cleavage of aliphatic side chains and cross-linking bonds,leading to a reduction in defective structures;whereas the increase in ID/IG between 550 and 600℃is closely associated with enhanced condensation reactions of aromatic structures.Correlation analysis further demonstrates progressive graphitization during pyrolysis,with a significant positive correlation(R^(2)>0.85)observed between d002 and the full width at half maximum of the G-band(FWHM-G).
文摘In this study,using 3,5‑di(3′,5′‑dicarboxylphenyl)‑1H‑1,2,4‑triazole(H4L)as ligands,a gadolinia‑based organic framework complex{[GdNa(L)(H_(2)O)3]·2H_(2)O}_(n)(Gd‑Na‑MOF)was successfully designed and synthesized by hydrothermal method.The structure and properties were systematically characterized and tested by techniques such as single‑crystal X‑ray diffraction,powder X‑ray diffraction,thermogravimetric analysis,infrared spectroscopy,and fluorescence spectroscopy.The results indicate that this complex has a unique 3D structure,excellent thermal stability,and outstanding luminescent performance.Based on its luminescent properties,a polymer‑embedding method was employed to fabricate the Gd‑Na‑MOF into a flexible,washable composite fluorescent film,Gd‑Na‑MOF@PMMA/BMA(PMMA=polymethyl methacrylate,BMA=butyl methacrylate).This fluorescent film exhibited highly sensitive recognition capability for tyramine,with a low detection limit of 1.66μmol·L^(-1).It was used for the detection of tyramine in bananas,with a recovery rate of 96.92%‑100.26%.CCDC:2466949.
文摘CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.
文摘A series of blue and blue‑green Ir(Ⅲ)complexes has been investigated theoretically to explore their electronic structures,photophysical properties,efficiency roll‑off effect,and thermal activation delayed fluorescence(TADF)properties.All calculations were performed using density functional theory(DFT)and time‑dependent density functional theory(TDDFT).Calculations for electronic structures,frontier molecular orbital characteristics(which determine the efficiency roll‑off effect of the complexes),and photophysical properties were conducted using the Gaussian 09 software package.The calculation of spin‑orbit coupling matrix elements<T|HSOC|S>,which determine the TADF properties of the complexes,was performed using the ORCA software package.The calculation results show that the auxiliary ligand tetraphenylimidodiphosphinate(tpip),a strong electron‑withdrawing group,can mitigate the efficiency roll‑off effect of the complex.Furthermore,TADF is observed in one of the designed complexes,(F_(3)Phppy)_(2)Ir(tpip),where F_(3)Phppy=2‑[4‑(2,4,6‑trifluorophenyl)phenyl]pyridine.
基金financially supported by the National Natural Science Foundation of China(Nos.52272214,52372082,52466013,52373184,and U24A20660)Jiangxi Provincial Natural Science Foundation(Nos.20242BAB26059,20232BAB204032,20252BAC200290,20252BEJ730349,and 20252BAC240326)Doctoral Start-Up Fund of Jiangxi Science&Technology Normal University(No.2024BSQD16)。
文摘Glucose,ascorbic acid(AA),uric acid(UA),and dopamine(DA)are vital biomarkers whose dynamic concentrations correlate with critical diseases;however,multiplexed detection remains challenging for conventional electrochemical sensors because of their limited sensitivity and selectivity.Here,we present a millimeter-scale all-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS)organic electrochemical transistor(OECT)platform that integrates dual-mode sensing with enzyme/metal-free operation for ultrasensitive biomarker monitoring.By engineering polycrystalline PEDOT:PSS channels via H_2 SO_4 post-treatment,the device achieves record-high conductivity(about(2312.0±29.9)S·cm^(–1)),maximum transconductance(about(2.82±0.12)mS),and on/off ratio(about 210.0±7.8),enabling signal amplification at low gate voltages.The dual-mode strategy combines the selectivity of electrochemistry with the sensitivity of OECTs,realizing simultaneous detection of glucose,AA,UA,and DA with clinical-level sensitivity:detection limits down to 8 nmol·L^(–1)(glucose),0.5 nmol·L^(–1)(AA),5 nmol·L^(–1)(DA),and 0.5 nmol·L^(–1)(UA).Validation using human urine samples yielded recovery rates of 94%–114%.This flexible sensing platform provides a new pathway for the development of wearable biosensors for precision diagnostics.
文摘Covalent organic frameworks(COFs)are an emerging class of porous crystalline materials formed by the precise assembly of organic molecular building blocks into extended periodic structures via strong covalent bonds.They feature well-defined pore structure,high specific surface area,and tunable physicochemical properties,endowing them with broad application prospects in gas storage,molecular separation.
基金supported by National Natural Science Foundation of China (Nos.21906124,32302202)Natural Science Foundation of Hubei Province (No.2017CFB220)Natural Science Foundation of Shandong Province (No.ZR2023MH278)。
文摘Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through covalent bonds exhibits excellent structural stability.It has been shown that the stationary phases prepared by combining MOF and COF can make up for the poor stability of MOF@SiO_(2),and the MOF/COF composites have superior chromatographic separation performance.However,the traditional methods for preparing COF/MOF based stationary phases are generally solvent thermal synthesis.In this study,a green and low-cost synthesis method was proposed for the preparation of MOF/COF@SiO_(2) stationary phase.Firstly,COF@SiO_(2) was prepared in a choline chloride/ethylene glycol based deep eutectic solvent(DES).Secondly,another acid-base tunable DES prepared by mixing p-toluenesulfonic acid(PTSA)and 2-methylimidazole in different proportions was introduced as the reaction solvent and reactant for rapid synthesis of MOF/COF@SiO_(2).Compared with the toxic transition metal-based MOFs selected in most previous studies,a lightweight and non-toxic S-zone metal(calcium) based MOF was employed in this study.PTSA and calcium will form the calcium/oxygen-containing organic acid framework in acidic DES,which assembles with terephthalic acid dissolved in basic DES to form MOF.The strong hydrogen bonding effect of DES can facilitate rapid assembly of Ca-MOF.The obtained Ca-MOF/COF@SiO_(2) can be used for multi-mode chromatography to efficiently separate multiple isomeric/hydrophilic/hydrophobic analytes.The synthesis method of Ca-MOF/COF@SiO_(2) is green and mild,especially the use of acid-base tunable DES promotes the rapid synthesis of non-toxic Ca-MOF/COF@silica composites,which offers an innovative approach of greenly synthesizing novel MOF/COF stationary phases and extends their applications in the field of chromatography.
基金Supported by the Jiangsu Provincial Science and Technology Planning Project(No.BK20231516)the National Natural Science Foundation of China(Nos.42293264,32371606,31971449)。
文摘In natural aquatic ecosystems,algal-derived organic carbon(AOC)often coexists with exogenous organic carbon(EOC).Microbial utilization of these distinct carbon sources affects carbon flux and transformation in water column and algal growth.Microcystis blooms significantly increase AOC levels in water,but the microbial transformation process of Microcystis-derived AOC in the presence of EOC remain poorly understood.We conducted a simulated experiment by introducing^(13)C-sodium bicarbonate and^(13)C-glucose as substrates for indoor simulation of non-axenic Microcystis aeruginosa(M.aeruginosa)populations in a sealed system.The microbial transformation processes of AOC and EOC and their effects on M.aeruginosa growth were investigated.Results demonstrated that the addition of glucose accelerated M.aeruginosa growth and significantly increased their biomass.During the experiment,as the particulate organic carbon and nitrogen content increased,the concentrations of CO_(2)and N_(2)O were gradually decreased,while the concentration of CH4 were gradually increased.Significant differences were observed in the microbial processes involved in the uptake of AOC and EOC.Bacteria involved in AOC transformation throughout the growth period were dominated by Proteobacteria,Gemmatimonadota,Actinobacteriota,Bacteroidota,Acidobacteriota,and Firmicutes.The bacteria involved in EOC transformation were dominated by Proteobacteria,Actinobacteriota,Firmicutes,Cyanobacteria,Armatimonadota,and Bacteroidota.Linear discriminant analysis Effect Size(LEfSe)analysis revealed Massilia and Akkermansia as biomarkers involved in AOC transformation,while Ligilactobacillus was associated with EOC transformation.These findings provide valuable insights into the effects of EOC on algae-bacteria interaction,and on the dynamics of carbon and nitrogen cycling among M.aeruginosa and its associated bacteria.
文摘Zero-dimensional(0D)organic-inorganic metal halide perovskite is one of the hot research topics in the field of optoelectronic materials.Their structure generally consists of discrete metal halide octahedra entirely isolated by surrounding organic cations,forming independent luminescent centers[1,2].Such a configuration results in high exciton binding energy and exceptional luminescence efficiency,due to strong quantum confinement[3,4].
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 Anhui Agricultural University Foundation for Stability and Introduction of Talent(rc352111)the Natural Science Research Project in Anhui Universities(2023AH051046)+2 种基金the Anhui Provincial Natural Science Foundation(2108085MC118)the Special Fund for Anhui Provincial Academic and Technological Leader(2021D297)the Special Fund for Anhui Agriculture Research System(AHCYJSTX-NCPJG)。
文摘This study employed integrated metabolomic and transcriptomic analyses to investigate the impacts of moderate withering(approximately 30%weight loss)on organic acid and flavonoid accumulation in blueberries and the resultant blueberry wines.Moderate withering led to decreases in aliphatic organic acids but increases in phenolic acids and flavonoids in blueberries.The decrease in malate could be linked to the downregulated VcMDH and VcDTC,and the decrease in citrate and 2-oxoglutarate could be a consequence of y-aminobutyric acid shunt activation.The increases of phenolic acids were associated with upregulated VcCAD and VcPOD in withered blueberries.Additionally,moderate withering upregulated the expression of VcLAR and VcUFGT,promoting flavonoid accumulation.In blueberry wines,moderate withering decreased total aliphatic organic acid content but increased anthocyanin content,consistent with the findings in blueberries.Overall,this study provided references for applying moderate withering in blueberry winemaking,contributing to modulating acidity and enriching phenolic substances.
基金supported by the Natural Science Foundation(NSF)of China(Nos.22205015,22175020,and 22235001)the National Postdoctoral Program for Innovative Talents(No.BX20220032)+2 种基金the China Postdoctoral Science Foundation Funded Project(No.2022BG013)the Fundamental Research Funds for the Central Universities(Nos.00007709,00007770,and FRFBR-23-02B)University of Science and Technology Beijing is gratefully acknowledged.
文摘In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed.Herein,two novel imide-linked 1D COFs with phthalocyanine building blocks,namely NiPc-CZDM-COF and NiPc-CZDL-COF,were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II)(NiPc(COOH)_(8))with 9H-carbazole-3,6-diamine(CZDM)and 4,4′-(9H-carbazole-3,6-diyl)dianiline(CZDL),respectively.Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Due to their high ratio of exposed active centers on the edge sites of porous ribbons,both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0%and 7.5% according to the electrochemical measurement,resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%.In particular,NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH3 partial current density of−246 mA/cm^(2),ammonia yield rate of 19.5 mg cm^(−2) h^(−1),and turnover frequency of 5.8 s^(−1) at−1.2 V in an H-type cell associated with its higher conductivity.This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.
基金the Natural Science Foundation of ZhejiangProvince(No.LZ24B020005)the National Natural Science Foundation of China(No.22071040)for financial support.
文摘High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody(Ab1)and ferrocene(Fc),and used for electrochemical detection of AFP.Due to the small,homogeneous pore size of the COF,Ab1 with a big size was immobilized on the surface of the COF,while Fc with a small size was covalently modified both on the surface and in the pores of COF.The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers.Meanwhile,the enriched Fc molecules not only improved the conductivity of the COF,but also effectively transferred and amplified the electrochemical signal.This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL(S/N of 3:1)and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations.Furthermore,this immunosensor showed excellent selectivity,stability and reproducibility in the testing of real samples.This study presents an innovative prototype for construction of a precious metal-free,antibody-directly-immobilized,simple and stable electrochemical immunoprobe.
基金supported by National Natural Science Foundation of China (Nos.52170086,22476116,52074176)Natural Science Foundation of Shandong Province (Nos.ZR2021ME013,ZR2024ME156,ZR2022QB250)。
文摘In this study,we meticulously designed a layered carbon-based catalytic material to induce the degradation of a series of organic pollutants by activating peroxymonosulfate(PMS) in the PMS-based advanced oxidation processes(AOPs).Results indicated that the silicon and oxygen elements from the montmorillonite were incorporated into the catalyst matrix to form the Si-O-C structure.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array,achieving over 90 % removal rate of most pollutants within 60 min.It was notable that the layered carbonaceous material with Si-O-C structure exhibited an outstanding catalytic effect on the synthesized layered catalytic material array.The salt bridge system confirmed that pollutants can provide electrons to the Si-O-C/PMS system,and we verified that the electron transfer process(ETP) mechanism was the main pathway for the degradation of pollutants in the Si-O-C/PMS system via the open-circuit potential analysis.In combination with the structural properties of different pollutants,we discovered that electron-donating pollutants can supply more electrons to the Si-O-C/PMS system,thereby enhancing the ETP process.The findings of this study are anticipated to advance the development and practical application of layered carbonaceous materials-based catalysts and support the design and implementation of nanoconfined catalysts in the field of AOPs.
基金supported by the Shaanxi Provincial High level Talent Introduction Project(5113220044)the Shaanxi Outstanding Youth Project(2023-JC-JQ-33)+8 种基金the Youth Science and Technology Talent Promotion Project of Jiangsu Association for Science and Technology(TJ-2022-088)the Project funded by China Postdoctoral Science Foundation(2023TQ0273,2023TQ0274,2023M742833)the NationalNatural Science Foundation of China(62304181)the Natural Science Basic Research Program of Shaanxi(2023-JC-QN-0726,2025JC-YBQN-469)the GuangdongBasic and Applied Basic Research Foundation(2022A1515110286,2024A1515012538)the Basic Research Programs of Taicang(TC2024JC04)the Suzhou Science and Technology Development Plan Innovation Leading Talent Project(ZXL2023183)the Fundamental Research Funds for the Central Universities(G2022KY05108,G2024KY0605,G2023KY0601)and the Aeronautical Science Foundation of China(2018ZD53047).
文摘Achieving simultaneous enhancement of crystallinity and optimal domain size remains a fundamental challenge in organic photovoltaics(OPVs),where conventional crystallization strategies often trigger excessive aggregation of small-molecule acceptors.This work pioneers a kinetic paradigm for resolving the crystallinity-domain size trade-off in organic photovoltaics through dual-additive-guided stepwise crystallization.By strategically pairing 1,2-dichlorobenzene(o-DCB,low binding energy to Y6)and 1-fluoronaphthalene(FN,high binding energy),we achieve temporally decoupled crystallization control:o-DCB first mediates donor-acceptor co-crystallization during film formation,constructing a metastable network,whereupon FN induces confined Y6 crystallization within this framework during thermal annealing,refining nanostructure without over-aggregation.Morphology studies reveal that this synergy enhances crystallinity of(100)diffraction peaks by 21%–10%versus single-additive controls(o-DCB/FN alone),while maintaining optimal domain size.These morphological advantages yield balanced carrier transport(μh/μe=1.23),near-unity exciton dissociation(98.53%),and a champion power conversion efficiency(PCE)of 18.08%for PM6:Y6,significantly surpassing single-additive devices(o-DCB:17.20%;FN:17.53%).Crucially,the dual-additive strategy demonstrates universal applicability across diverse active layer systems,achieving an outstanding PCE of 19.27%in PM6:L8-BO-based devices,thereby establishing a general framework for morphology control in high-efficiency OPVs.
基金financial support by the National Key Research and Development Program of China(No.2023YFC2907801)the Hunan Provincial Natural Science Foundation of China(No.2023JJ40760)the Scientific and Technological Project of Yunnan Precious Metals Laboratory,China(No.YPML-2023050276)。
文摘Bentonite is a necessary binder in producing pellets.Its excessive use reduces the iron grade of pellets and increases production costs.Minimizing bentonite dosage is essential for producing high-quality iron ore pellets.Addressing the gap in the application of organically-intercalated modified bentonite in the pelletizing field,this study introduces an innovative modification process for bentonite that employs the synergistic effect of mechanical force and dimethyl sulfoxide to enhance the intercalation of organic compounds within bentonite,thus significantly enhancing its binding performance.The colloid value and swell capacity of modified bentonite(98.5 m L/3g and 55.0 m L/g)were much higher than the original bentonite(90.5 m L/3g and 17.5 m L/g).With the decrease of bentonite dosage from1.5wt%to 1.0wt%,the drop number of green pellets from a height of 0.5 m and the compressive strengths of roasted pellets using the modified bentonite(6.0 times and 2916 N per pellet)were significantly higher than those of the original bentonite(4.0 times and 2739 N per pellet).This study provides a comprehensive analysis of the intercalation modification mechanism of bentonite,offering crucial technical insights for the development of high-performance modified bentonite as iron ore pellet binders.
基金Special Research Assistant Program,China(2024000020)the Science and Technology Department of Qinghai Province,China(2024-ZJ-918)the“Kunlun Talents”Program of Qinghai(2024000075)。
文摘Abstract:Graphene-Based separation membranes hold promise for water treatment.However,their practical deployment in high-salinity brines remains challenging due to structural instability.Herein,a defect-free Na^(+)-Cu^(2+)/GO-PEI nanocomposite membrane was fabricated via a pH-controlled cross-linking polymerization strategy.Polyethyleneimine(PEI)serves as a critical interfacial stabilizer,enhancing the connection between the Na^(+)-GO and Cu^(2+)-GO layers through amide bond formation with GO nanosheets while facilitating Cu^(2+)chelation.The Na^(+)/GO layer modifies the pore structure of the polyether sulfone(PES)substrate,synergistically optimizing the membrane’s microstructure.Performances evaluation revealed that the as-prepared membrane achieved exceptional separation efficiency(>98%)for tributyl phosphate,sulfonated kerosene,and bis(2-ethylhexyl)phosphate in high-salinity brine,accompanied by a high flux of 160~224 L·m^(-2)·h^(-1).Notably,it exhibited robust chemical stability in corrosive environment and maintained mechanical durability after 500 folding cycles coupled with consistent separation performances over 10 recycles.This study presents a novel multi-component modification approach for constructing high-performance GObased membrane,promising practical applications in organic pollutant removal from high salt solution.
基金supported by National Natural Science Foundation of China(No.42376217)Fundamental Research Funds for the Central Universities of China(No.3-7-10-2025-03)National Key Research and Development Program of China(No.2024YFC2814702).
文摘The Dongsha area,a key target for gas hydrate exploration,is influenced by multiple factors,including sedimentary processes and the paleoenvironment,which play critical roles in gas hydrate formation.To elucidate the coupling among sedimentary processes,paleoenvironment,and gas hydrate accumulation,this study investigates the Site DS-W16 using particle size analysis,biological component content,and geochemistry data.Oxygen isotope data from foraminifera and biostratigraphic evidence indicate that sedimentation at the bottom of core interval from Site DS-W16 began during MIS 11(Marine isotope stage).The sedimentation dynamics of the studied layers are complex,involving gravity flows,traction currents,and suspended deposition.Organic matter shows a significant correlation with transgressive-regressive cycle.The site DS-W16 contains two distinct gas hydrate reservoirs:a shallow reservoir(10-24 mbsf)and a deep reservoir(below 182 mbsf).The paleomarine environment influences gas hydrate accumulation by altering sedimentary processes and sediment characteristics,especially the distribution of biological components.Both shallow and deep gas hydrate reservoirs formed under dynamic conditions dominated by traction currents and are characterized by a higher abundance of foraminifera.Sedimentary layers rich in foraminifera and modified by traction currents represent key intervals for preferential gas hydrate accumulation.
基金supported by the National Natural Science Foundation of China (NSFC grant no. 62474028, 52130304, and62222503)the Natural Science Foundation of Sichuan Province(2025ZNSFSC0037, 2025ZNSFSC1460, and 2024NSFSC1447)+1 种基金the National Key R and D Program of China (2023YFB2604101)sponsored by the Sichuan Province Key Laboratory of Display Science and Technology
文摘The crystallization and aggregation characteristics of the active layer components in organic solar cells(OSCs)are one of the core factors determining photovoltaic performance,influencing the entire process from light absorption to charge separation,transport,and ultimately charge collection.Dynamic changes in crystallization and aggregation states can also disrupt the microstructure of the active layer,thus shortening the lifetime of the cell.In this study,a morphology modulation strategy is proposed to regulate the crystallization kinetics of non-fullerene acceptors by employing the polymer molecule PYIT as a nucleating agent.An appropriate amount of PYIT was first completely dissolved with the non-fullerene acceptor Y6 and left to stand for 24 h,followed by the fabrication of layer-by-layer processed OSCs.Experiments demonstrated that high crystallinity of PYIT allows it to act as a crystallization nucleus,promoting the crystallization,orientation consistency,and ordered stacking of the acceptor.These nanoscale structural optimizations facilitate efficient charge transport,enhance exciton dissociation efficiency,and suppress unfavorable energetic disorder.Consequently,not only was the power conversion efficiency(PCE)of D18-Cl/Y6-based layer-by-layer processed OSC increased from 18.08%to 19.13%,but the atmospheric stability and long-term lifetime of the OSCs were also significantly improved.Notably,this strategy is also applicable to indoor OSCs,and the PYIT-optimized device can achieve a PCE of 27.0%under 1000 lux light-emitting diode(LED,3200K)irradiation,which is superior to that of the control device(24.2%).This work develops a crystal engineering strategy that is able to simultaneously optimize the microscopic morphology and charge dynamics properties in OSCs,thereby achieving simultaneous improvement in efficiency and stability.
基金supported by the National Natural Science Foundation of China (Nos.22174067,22204078,and 22374077)the Natural Science Foundation of Jiangsu Province of China (No.BK20220370)+3 种基金Jiangsu Provincial Department of Education (No.22KJB150009)State Key Laboratory of Analytical Chemistry for Life Science (No.SKLACLS2218)the Priority Academic Program Development of Jiangsu Higher Education Institutions,Jiangsu Association for Science and Technology (No.TJ-2023-076)Shanghai Synchrotron Radiation Facility Beamline BL17B1 (No.2021-NFPSPT-006657)。
文摘This research explores the influence of crystallinity on gas chromatographic(GC) separation using covalent organic frameworks(COFs) as stationary phases.Three COF materials(CTF-DCBs) with varying crystallinity were synthesized and characterized.CTF-DCB-1,with superior crystallinity,demonstrated highselectivity GC separation of benzene isomers as well as styrene/phenylacetylene mixtures,while CTFDCB-2 and CTF-DCB-3 exhibited lower crystallinity and worse separation performance.Thermodynamic and kinetic tests showed that CTF-DCB-1 had the worst thermodynamic adsorption but low diffusion mass transfer resistance,which resulted in the best separation.Therefore,optimizing the crystallinity of COFs is necessary for balancing the kinetic diffusion and thermodynamic interactions towards the analytes,achieving high-performance GC stationary phases.
