To elucidate the variations in volatile organic compounds(VOCs)among widely cultivated japonica rice varieties in China and offer novel perspectives on flavor formation during rice-based beer brewing,nine prevalent Ch...To elucidate the variations in volatile organic compounds(VOCs)among widely cultivated japonica rice varieties in China and offer novel perspectives on flavor formation during rice-based beer brewing,nine prevalent Chinese japonica rice variaties were selected as experimental materials.Comprehensive analyses were conducted to investigate three key aspects:differences in VOCs among the selected japonica rice varieties,the retention of rice VOCs after beer brewing,and the influence of rice additives on beer sensory characteristics.Results showed that the total contents of VOCs in Wuyoudao 4(WYD4)and Nangeng 9108(NG9108)were significantly higher than those in the other varieties(P<0.05).The popcorn-flavor compound 2-acetyl-1-pyrroline(2-AP)was detected in Suigeng 27(SG27,26.80 ng/g),WYD4(25.25 ng/g),NG9108(21.18 ng/g),and Suigeng 18(SG18,11.62 ng/g),with the levels in the first three varieties significantly higher than those in SG18.Circular heatmap analysis classified the nine japonica varieties into three major categories:fragrant japonica from North China(WYD4),fragrant japonica from South China(NG9108),and others.Ten characteristic VOCs across the japonica varieties were identified by headspace solid-phase microextraction gas chromatography-mass spectrometry(HS-SPME-GC-MS).Using beer brewed with whole wheat as the control,we analyzed the VOCs and sensory characteristics of beer brewed with fragrant japonica rice as an additive.We found that rice VOCs were not detected in beer brewed with fragrant japonica rice as an additive.Adding rice promoted the formation of banana-like flavors and reduced the beer’s richness and mellowness.展开更多
Soil organic matter(SOM)is crucial for ecosystem carbon cycling,soil fertility,and environmental quality.As the main component of SOM,humic substances(HS)are considered a unique category of nonuniformly assembled subs...Soil organic matter(SOM)is crucial for ecosystem carbon cycling,soil fertility,and environmental quality.As the main component of SOM,humic substances(HS)are considered a unique category of nonuniformly assembled substances.展开更多
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
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
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
Although the concentration of fine particulate matter(PM_(2.5))is reducing continuously,the proportion of secondary organic aerosols(SOA)in PM_(2.5) and the O_(3) levels are increasing.This is causing severe complex a...Although the concentration of fine particulate matter(PM_(2.5))is reducing continuously,the proportion of secondary organic aerosols(SOA)in PM_(2.5) and the O_(3) levels are increasing.This is causing severe complex atmospheric pollution in North China.It is essential to identify and quantify the driving factors of SOA and O_(3),including the various pollution sources and meteorological factors.PM_(2.5) and volatile organic compounds(VOCs)samples were collected simultaneously in three cities in Shandong Province during different pollution scenarios from 2021 to 2023.Then,the carbonaceous aerosol and 99 VOC species were analyzed.Random forest(RF)combined with positive matrix factorization and an observation-based model(OBM)were used to quantify the key drivers of SOA and O_(3).Aromatic hydrocarbons were the main contributors to secondary organic aerosol potential(74.3%-89.9%),whereas alkenes contributed the most to the ozone formation potential(27.0%-62.3%).The RF modeling identified temperature and NOx as the dominant drivers of ozone formation.These accounted for 47.8%and 17.4%,respectively.Temperature showed a positive correlation with O_(3) because an increase in temperature can promote ozone formation.NOx had a significant negative correlation with O_(3),which was consistent with the conclusions from the sensitivity analysis of the OBM.The dominant contributors to SOA were vehicle emissions,solvent use,and industrial emissions.These accounted for 43.9%,18.2%,and 10.5%,respectively.An evident positive correlation existed between these emission sources and SOA.展开更多
Organic electrochemical transistors(OECTs)are promising for next-generation bioelectronics due to their high performance and biocompatibility.Nevertheless,they still face tremendous operational stability challenges du...Organic electrochemical transistors(OECTs)are promising for next-generation bioelectronics due to their high performance and biocompatibility.Nevertheless,they still face tremendous operational stability challenges due to the limited robustness of the organic mixed ionic-electronic conductor(OMIEC)channel.Here,by modulating the molecular weight(MW)of OMiEC,enhanced OECT and relevant circuit operation stabilities are demonstrated,showing more than 3,000,0o0 full cycles(~42 h)with less than 15%current variation in an OECT,and 150,000 cycles(~4 h)with less than 5%voltage variation in an OECT-based inverter,which are among the highest of reported OECT-based electronics.Specifically,p(g2T-T),a typical p-type OMIEC,with varying MW(7-43 kDa),is synthesized,where lower-MW p(g2T-T)(~9 kDa)exhibits superior device performance and cycling stability in OECTs,outperforming those in high-MW counterparts(>30 kDa).It is indicated that low-MW p(g2T-T)maintains higher volumetric capacitance,ordered orientation,and reduced swelling.Therefore,irreversible microstructural degradation is effectively avoided,along with better performance yield.Furthermore,MW regulation enables physiological signal sensing with high tolerance to body fluid environments for 7 days.These findings highlight MW modulation as a versatile approach to suppress excessive swelling,advancing the design of durable OECT-based electronics.展开更多
The development of non-corrosive and efficient anode interlayers(AILs)is pivotal for advancing highperformance organic optoelectronic devices.Conventional materials such as PEDOT:PSS,though widely adopted,suffer from ...The development of non-corrosive and efficient anode interlayers(AILs)is pivotal for advancing highperformance organic optoelectronic devices.Conventional materials such as PEDOT:PSS,though widely adopted,suffer from significant limitations including acidity,corrosion,and poor device stability.Herein,we propose a novel molecular design strategy by introducing p-πconjugation into a p Hneutral conjugated polyelectrolyte(CPE)(PIDT-T)to simultaneously enhance work function(WF)and electrical conductivity.Through doping with polyoxometalate(POM),the optimized PIDT-T:POM achieves a high WF of 4.85 e V,conductivity of 7.25×10^(-3)S cm^(-1),and>98%optical transmittance.In organic solar cells(OSCs),PIDT-T:POM delivers a power conversion efficiency(PCE)of 19.04%,outperforming PEDOT:PSS-based counterparts(18.52%)and representing one of the highest PCEs reported for devices utilizing non-acidic AILs.Moreover,organic light-emitting diodes(OLEDs)incorporating PIDTT:POM exhibit a remarkable reduction in turn-on voltage(from 5.8 to 3.0 V)and enhanced luminous efficiency,demonstrating its dual functionality for both OSCs and OLEDs.These findings establish p-πconjugated polyelectrolytes as a powerful molecular platform for next-generation,high-efficiency,and corrosion-free organic optoelectronic applications.展开更多
Redox-active covalent organic polymers(COPs)have emerged as appealing renewable electrode materials for next-generation Li-ion batteries,but their performance is limited by insufficient redox sites and inadequate Li-i...Redox-active covalent organic polymers(COPs)have emerged as appealing renewable electrode materials for next-generation Li-ion batteries,but their performance is limited by insufficient redox sites and inadequate Li-ion diffusion.Here,we develop a novel class of mesoporous covalent organic polymer(namely TF-Azo-COP)bearing multiple redox sites and explore its first use as efficient 18-electron-redox anodes for superior Li-ion storage in both coin-type and fiber-type batteries.The newly produced TF-Azo-COP involves three types of active sites including C=N in triazines and imines,N=N in azo,and C6-ring aromatics to enable 18-Li-ion storage on one repeatable segment,while affording extendedπ-conjugation for fast electron transfer and a pore size of~2.5 nm for facilitated ion diffusion with a high coefficient up to~10^(-10)cm^(2)s^(-1)—superior to some reported organic electrodes.Meriting from the above,pairing TF-Azo-COP with metal Li endows a coin cell with good cycling stability and a large reversible capacity of 795.4 mAh g^(-1)at 0.1 A g^(-1)—representing one of the best performances among reported organic electrodes.When coupled with fiber-shaped LiFePO_(4)cathodes,the assembled fiber cell delivers an excellent combination of linear capacity(0.23 mAh cm^(-1)),energy density(0.55 mWh cm^(-1)),cycling stability(250 cycles),and good flexibility.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
The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic...The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic N(UIN)additions neglect canopy processes and the impacts of organic N,potentially misevaluating N deposition effects.This study was conducted in a long-term N addition experiment established in a Moso bamboo forest,which included six treatments combining canopy and understory N additions with organic(urea glycine)and inorganic(NH_(4)NO_(3))forms at a rate of 50 kg N·ha^(-1)·yr^(-1).Litterbags were installed for a two-year decomposition experiment and collected at quarterly intervals,together with concurrent soil sampling under litterbags at 0–10 cm depth.We aimed to examine the effects of canopy vs.understory N addition and organic vs.inorganic N form on soil POC and MAOC concentrations.Our results showed that canopy N additions significantly reduced POC(ased POC-15.9%)but did not affect MAOC(P>0.05).Conversely,understory N additions significantly incre(30.9%)and decreased MAOC(and fungal diversity(FuD),-28.9%).Canopy N additions decreased POC by enhancing peroxidase activity while understory N additions promoted POC by inhibiting litter decomposition.Additionally,understory N addition-induced soil acidification decreased soil Ca^(2+)concentration,microbial carbon use efficiency,and bacterial necromass C,as well as the release of litter water-soluble compounds,thereby inhibiting MAOC.Moreover,nitrogen forms(organic vs.inorganic)had no effect on SOC fractions.Our findings underscore that canopy and understory N addition approaches differentially regulate SOC fractions by altering litter decomposition–microbial–mineral interactions,and the understory approach may overestimate soil POC gain and MAOC loss driven by atmospheric N deposition.展开更多
As an essential component of terrestrial carbon sinks,lake sediments store vast quantities of both organic carbon(OC)and inorganic carbon(IC).However,the spatiotemporal relationship between the OC and IC in sediments ...As an essential component of terrestrial carbon sinks,lake sediments store vast quantities of both organic carbon(OC)and inorganic carbon(IC).However,the spatiotemporal relationship between the OC and IC in sediments and their responses to climate change remains unclear,which hinders the comprehensive understanding of carbon dynamics in lake ecosystems.This study systematically analyzes the spatiotemporal dynamics of carbon burial across the Tibetan Plateau using surface sediments from 119 lakes and sediment cores from four representative lakes.Results show that OC burial dominates in humid and dry sub-humid zones,whereas IC burial prevails in arid and semi-arid regions.This distribution reflects the influences of lake and catchment productivity and water chemistry on OC and IC patterns.Sediment cores confirm that these factors have consistently affected lake carbon burial over the past century.Specifically,in humid and dry sub-humid zones,increased precipitation enhances watershed productivity and sedimentation,promoting coupled OC and IC burial.In arid and semi-arid regions,wind-driven dust supplies nutrients and alters water chemistry,also driving coupled OC and IC burial.Based on these findings,the carbon sink capacity of lake sediments on the Tibetan Plateau is projected to increase under the“warming and wetting”trend.展开更多
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
The efficient extraction and separation of valuable metal elements from coal gasification fine slag(CGFS)are crucial for the comprehensive high-value utilization of its constituents.This study focused on the carbon-ri...The efficient extraction and separation of valuable metal elements from coal gasification fine slag(CGFS)are crucial for the comprehensive high-value utilization of its constituents.This study focused on the carbon-rich components of CGFS(CGFS-H)and systematically investigates the selective leaching behavior of Fe^(3+),Al^(3+)and Ca^(2+)using three organic acid extractants,i.e.,citric acid,tartaric acid,and tetrasodium iminodisuccinate.Additionally,the stepwise leaching of iron,aluminum and calcium from CGFS-H is explored.The selective dissolution mechanisms of these metals by different organic acids are elucidated through X-ray diffraction(XRD),X-ray fluorescence(XRF),and scanning electron microscopy(SEM)analyses.The results indicate that tetrasodium iminodisuccinate exhibits the highest leaching selectivity for Fe^(3+),while tartaric acid demonstrateds a comparable affinity for both Fe^(3+)and Al^(3+).In contrast citric acid shows superior selectivity toward Ca^(2+).The leaching yield of Fe^(3+),Al^(3+)and Ca^(2+)after sequential leaching with the three organic acids were 79.8%,65.08%and 78.6%,respectively.These findings confirm that effective and selective separation of Fe^(3+),Al^(3+)and Ca^(2+)from CGFS-H can be achieved via optimized organic acid-based leaching strategies.This advancement provides a critical foundation for developing Ca/Fe/Al hydrotalcite materials using CGFS-H as a sustainable feedstock,thereby facilitating the transformation of waste residue into high-value functional materials and promoting resourceefficient utilization of coal gasification fine slag.展开更多
In this study,a multifunctional aptamer-conjugated magnetic covalent organic framework(COF)-CuO/Au nanozyme(MCOF-CuO/Au@apt)was developed as a“three-in-one”platform for dual-signal colorimetric and fluorescent detec...In this study,a multifunctional aptamer-conjugated magnetic covalent organic framework(COF)-CuO/Au nanozyme(MCOF-CuO/Au@apt)was developed as a“three-in-one”platform for dual-signal colorimetric and fluorescent detection of Vibrio parahaemolyticus.The nanozyme integrated magnetic separation,peroxidase-like catalytic activity,and specific target recognition through an aptamer-based strategy.Upon binding to V.parahaemolyticus,the catalytic oxidation of tetra-aminophenylethylene(TPE-4A)by the nanozyme was selectively inhibited,resulting in distinct colorimetric and fluorescent signals that significantly enhanced the detection accuracy and reliability.The proposed method exhibited high sensitivity,with limits of detection(LOD)of 21 and 7 CFU/mL for the colorimetric and fluorescent assays,respectively.The performance of this method was validated using real seafood samples,including Penaeus vannamei,Mytilus coruscus,and Crassostrea gigas,which showed high recovery rates(101.11%-107.30%)and excellent reproducibility.The system also demonstrated strong specificity and accuracy under various conditions,confirming its robustness and practical applicability.Collectively,this innovative platform presents a promising solution for the rapid,versatile,and sensitive detection of V.parahaemolyticus in seafood,with considerable potential to advance food safety diagnosis and on-site monitoring.展开更多
The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the effici...The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the efficiency of OSCs.Herein,two bridging polymer acceptors(PAs)—benzodithiophene-(2-ethylhexyl)oxy(BDT-C2C4)and benzodithiophene-octyloxy(BDT-C_(8))—are designed and synthesized by combining a benzodithiophene(BDT)unit as the donor moiety[poly({4,8-bis[5-(2-ethylhexyl)-4-fluorothiophen-2-yl]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}){5,8-bis[4-(2-butyloctyl)thiophen-2-yl]dithieno[3',2':3,4]},D18],and a 2,2′-((2Z,2′Z)-{[12,13-Bis(2-butyloctyl)-12,13-dihydro-3,9-dinonylthieno[2,3]thieno[3,2-b]pyrrolo[4,5-g]thieno[2,3-b]indole-2,10-diyl]bis(methanylylidene)}bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(Y6)derivative as the acceptor moiety.BDT-C2C4 and BDT-C_(8) are functionalized with(2-ethylhexyl)oxy and octyloxy side chains on the BDT unit,respectively.Both PAs show complementary absorption and cascaded energy levels with the donor D18 and the acceptor 2,2′-((2Z,2′Z)-{[12,13-bis(3-ethylheptyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″∶4′,5′]thieno[2′,3′∶4,5]pyrrolo[3,2-g]thieno[2′,3′∶4,5]thieno[3,2-b]indole-2,10-diyl]bis(meth⁃aneylylidene)}bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(N3),but BDT-C_(8) exhibits better compatibility with D18 and N3 compared to BDT-C2C4.When incorporated as a third component into the D18∶N3 blend,both PAs improve the active layer morphology.In particular,the D18∶N3∶BDT-C_(8) blend shows significantly optimized morphology,featuring reduced phase separation and a fibrous network structure.As a result,the device based on D18∶N3∶BDT-C_(8) achieves a power conversion efficiency of 18.18%,significantly higher than that of the device based on D18∶N3(ca.17.37%).This work presents a compatibilizer strategy for optimizing blend morphology towards high-performance ternary OSCs.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
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
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
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
基金supported by the Natural Science Foundation of Zhejiang Province,China(Grant No.LTGN24C020004)the Enterprise Cooperation Project,China(Grant No.HRJYH-202330)+1 种基金the Zhejiang Province Pioneer and Bellwethers Research&Development Project of Science and Technology,China(Grant No.2023C02014)the Central Public-Interest Scientific Institution Basal Research Fund,China(Grant No.CPSIBRFCNRRI-202303).
文摘To elucidate the variations in volatile organic compounds(VOCs)among widely cultivated japonica rice varieties in China and offer novel perspectives on flavor formation during rice-based beer brewing,nine prevalent Chinese japonica rice variaties were selected as experimental materials.Comprehensive analyses were conducted to investigate three key aspects:differences in VOCs among the selected japonica rice varieties,the retention of rice VOCs after beer brewing,and the influence of rice additives on beer sensory characteristics.Results showed that the total contents of VOCs in Wuyoudao 4(WYD4)and Nangeng 9108(NG9108)were significantly higher than those in the other varieties(P<0.05).The popcorn-flavor compound 2-acetyl-1-pyrroline(2-AP)was detected in Suigeng 27(SG27,26.80 ng/g),WYD4(25.25 ng/g),NG9108(21.18 ng/g),and Suigeng 18(SG18,11.62 ng/g),with the levels in the first three varieties significantly higher than those in SG18.Circular heatmap analysis classified the nine japonica varieties into three major categories:fragrant japonica from North China(WYD4),fragrant japonica from South China(NG9108),and others.Ten characteristic VOCs across the japonica varieties were identified by headspace solid-phase microextraction gas chromatography-mass spectrometry(HS-SPME-GC-MS).Using beer brewed with whole wheat as the control,we analyzed the VOCs and sensory characteristics of beer brewed with fragrant japonica rice as an additive.We found that rice VOCs were not detected in beer brewed with fragrant japonica rice as an additive.Adding rice promoted the formation of banana-like flavors and reduced the beer’s richness and mellowness.
基金financial support from the National Key Research and Development Program of China(No.2022YFD1500304)the Postdoctoral Fellowship Program of CPSF,China(No.GZC20232641)the Postdoctoral Science Foundation of China(No.2024M753215)。
文摘Soil organic matter(SOM)is crucial for ecosystem carbon cycling,soil fertility,and environmental quality.As the main component of SOM,humic substances(HS)are considered a unique category of nonuniformly assembled substances.
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.
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 Qingdao Natural Science Foundation(No. 23-2-1-224-zyyd-jch)。
文摘Although the concentration of fine particulate matter(PM_(2.5))is reducing continuously,the proportion of secondary organic aerosols(SOA)in PM_(2.5) and the O_(3) levels are increasing.This is causing severe complex atmospheric pollution in North China.It is essential to identify and quantify the driving factors of SOA and O_(3),including the various pollution sources and meteorological factors.PM_(2.5) and volatile organic compounds(VOCs)samples were collected simultaneously in three cities in Shandong Province during different pollution scenarios from 2021 to 2023.Then,the carbonaceous aerosol and 99 VOC species were analyzed.Random forest(RF)combined with positive matrix factorization and an observation-based model(OBM)were used to quantify the key drivers of SOA and O_(3).Aromatic hydrocarbons were the main contributors to secondary organic aerosol potential(74.3%-89.9%),whereas alkenes contributed the most to the ozone formation potential(27.0%-62.3%).The RF modeling identified temperature and NOx as the dominant drivers of ozone formation.These accounted for 47.8%and 17.4%,respectively.Temperature showed a positive correlation with O_(3) because an increase in temperature can promote ozone formation.NOx had a significant negative correlation with O_(3),which was consistent with the conclusions from the sensitivity analysis of the OBM.The dominant contributors to SOA were vehicle emissions,solvent use,and industrial emissions.These accounted for 43.9%,18.2%,and 10.5%,respectively.An evident positive correlation existed between these emission sources and SOA.
基金supported by the National Key R&D Program of China(2024YFB3211600)the National Natural Science Foundation of China(Nos.62273073,52273316)+4 种基金the National Key R&D Program of China(2023YFC2411800,2022YFE0134800)the Natural Science Foundation of Sichuan(2025ZNSFSC0515)Chengdu Science Technology Bureau(2023-YF06-00028-HZ)and the Fundamental Research Funds for the Central Universities(ZYGX2025TS009,ZYGX2024XJ029,ZYGX2024XJ031)Sci-entific Research Innovation Capability Support Project for Young Faculty(ZYGXQNJSKYCXNLZCXM-M1P).
文摘Organic electrochemical transistors(OECTs)are promising for next-generation bioelectronics due to their high performance and biocompatibility.Nevertheless,they still face tremendous operational stability challenges due to the limited robustness of the organic mixed ionic-electronic conductor(OMIEC)channel.Here,by modulating the molecular weight(MW)of OMiEC,enhanced OECT and relevant circuit operation stabilities are demonstrated,showing more than 3,000,0o0 full cycles(~42 h)with less than 15%current variation in an OECT,and 150,000 cycles(~4 h)with less than 5%voltage variation in an OECT-based inverter,which are among the highest of reported OECT-based electronics.Specifically,p(g2T-T),a typical p-type OMIEC,with varying MW(7-43 kDa),is synthesized,where lower-MW p(g2T-T)(~9 kDa)exhibits superior device performance and cycling stability in OECTs,outperforming those in high-MW counterparts(>30 kDa).It is indicated that low-MW p(g2T-T)maintains higher volumetric capacitance,ordered orientation,and reduced swelling.Therefore,irreversible microstructural degradation is effectively avoided,along with better performance yield.Furthermore,MW regulation enables physiological signal sensing with high tolerance to body fluid environments for 7 days.These findings highlight MW modulation as a versatile approach to suppress excessive swelling,advancing the design of durable OECT-based electronics.
基金the financial support from the Beijing Municipal Science&Technology Commission(2242013)。
文摘The development of non-corrosive and efficient anode interlayers(AILs)is pivotal for advancing highperformance organic optoelectronic devices.Conventional materials such as PEDOT:PSS,though widely adopted,suffer from significant limitations including acidity,corrosion,and poor device stability.Herein,we propose a novel molecular design strategy by introducing p-πconjugation into a p Hneutral conjugated polyelectrolyte(CPE)(PIDT-T)to simultaneously enhance work function(WF)and electrical conductivity.Through doping with polyoxometalate(POM),the optimized PIDT-T:POM achieves a high WF of 4.85 e V,conductivity of 7.25×10^(-3)S cm^(-1),and>98%optical transmittance.In organic solar cells(OSCs),PIDT-T:POM delivers a power conversion efficiency(PCE)of 19.04%,outperforming PEDOT:PSS-based counterparts(18.52%)and representing one of the highest PCEs reported for devices utilizing non-acidic AILs.Moreover,organic light-emitting diodes(OLEDs)incorporating PIDTT:POM exhibit a remarkable reduction in turn-on voltage(from 5.8 to 3.0 V)and enhanced luminous efficiency,demonstrating its dual functionality for both OSCs and OLEDs.These findings establish p-πconjugated polyelectrolytes as a powerful molecular platform for next-generation,high-efficiency,and corrosion-free organic optoelectronic applications.
基金support from Guangdong Basic and Applied Basic Research Foundation(2020B1515420001 and 2023B1515040027)Fundamental Research Funds for the Central Universities,Sun Yat-sen University(23yxqntd002)the Postdoctoral Fellowship Program of CPSF(GZC20242066).
文摘Redox-active covalent organic polymers(COPs)have emerged as appealing renewable electrode materials for next-generation Li-ion batteries,but their performance is limited by insufficient redox sites and inadequate Li-ion diffusion.Here,we develop a novel class of mesoporous covalent organic polymer(namely TF-Azo-COP)bearing multiple redox sites and explore its first use as efficient 18-electron-redox anodes for superior Li-ion storage in both coin-type and fiber-type batteries.The newly produced TF-Azo-COP involves three types of active sites including C=N in triazines and imines,N=N in azo,and C6-ring aromatics to enable 18-Li-ion storage on one repeatable segment,while affording extendedπ-conjugation for fast electron transfer and a pore size of~2.5 nm for facilitated ion diffusion with a high coefficient up to~10^(-10)cm^(2)s^(-1)—superior to some reported organic electrodes.Meriting from the above,pairing TF-Azo-COP with metal Li endows a coin cell with good cycling stability and a large reversible capacity of 795.4 mAh g^(-1)at 0.1 A g^(-1)—representing one of the best performances among reported organic electrodes.When coupled with fiber-shaped LiFePO_(4)cathodes,the assembled fiber cell delivers an excellent combination of linear capacity(0.23 mAh cm^(-1)),energy density(0.55 mWh cm^(-1)),cycling stability(250 cycles),and good flexibility.
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The effects of nitrogen(N)deposition on forest soil organic carbon(SOC)are largely unclear,likely due to the divergent responses of particulate(POC)and mineral-associated carbon(MAOC).Conventional understory inorganic N(UIN)additions neglect canopy processes and the impacts of organic N,potentially misevaluating N deposition effects.This study was conducted in a long-term N addition experiment established in a Moso bamboo forest,which included six treatments combining canopy and understory N additions with organic(urea glycine)and inorganic(NH_(4)NO_(3))forms at a rate of 50 kg N·ha^(-1)·yr^(-1).Litterbags were installed for a two-year decomposition experiment and collected at quarterly intervals,together with concurrent soil sampling under litterbags at 0–10 cm depth.We aimed to examine the effects of canopy vs.understory N addition and organic vs.inorganic N form on soil POC and MAOC concentrations.Our results showed that canopy N additions significantly reduced POC(ased POC-15.9%)but did not affect MAOC(P>0.05).Conversely,understory N additions significantly incre(30.9%)and decreased MAOC(and fungal diversity(FuD),-28.9%).Canopy N additions decreased POC by enhancing peroxidase activity while understory N additions promoted POC by inhibiting litter decomposition.Additionally,understory N addition-induced soil acidification decreased soil Ca^(2+)concentration,microbial carbon use efficiency,and bacterial necromass C,as well as the release of litter water-soluble compounds,thereby inhibiting MAOC.Moreover,nitrogen forms(organic vs.inorganic)had no effect on SOC fractions.Our findings underscore that canopy and understory N addition approaches differentially regulate SOC fractions by altering litter decomposition–microbial–mineral interactions,and the understory approach may overestimate soil POC gain and MAOC loss driven by atmospheric N deposition.
基金National Natural Science Foundation of China,No.42225105,No.42201175The China Postdoctoral Science Foundation,No.2023M733605。
文摘As an essential component of terrestrial carbon sinks,lake sediments store vast quantities of both organic carbon(OC)and inorganic carbon(IC).However,the spatiotemporal relationship between the OC and IC in sediments and their responses to climate change remains unclear,which hinders the comprehensive understanding of carbon dynamics in lake ecosystems.This study systematically analyzes the spatiotemporal dynamics of carbon burial across the Tibetan Plateau using surface sediments from 119 lakes and sediment cores from four representative lakes.Results show that OC burial dominates in humid and dry sub-humid zones,whereas IC burial prevails in arid and semi-arid regions.This distribution reflects the influences of lake and catchment productivity and water chemistry on OC and IC patterns.Sediment cores confirm that these factors have consistently affected lake carbon burial over the past century.Specifically,in humid and dry sub-humid zones,increased precipitation enhances watershed productivity and sedimentation,promoting coupled OC and IC burial.In arid and semi-arid regions,wind-driven dust supplies nutrients and alters water chemistry,also driving coupled OC and IC burial.Based on these findings,the carbon sink capacity of lake sediments on the Tibetan Plateau is projected to increase under the“warming and wetting”trend.
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).
基金Supported by National Natural Science Foundation(52374279)。
文摘The efficient extraction and separation of valuable metal elements from coal gasification fine slag(CGFS)are crucial for the comprehensive high-value utilization of its constituents.This study focused on the carbon-rich components of CGFS(CGFS-H)and systematically investigates the selective leaching behavior of Fe^(3+),Al^(3+)and Ca^(2+)using three organic acid extractants,i.e.,citric acid,tartaric acid,and tetrasodium iminodisuccinate.Additionally,the stepwise leaching of iron,aluminum and calcium from CGFS-H is explored.The selective dissolution mechanisms of these metals by different organic acids are elucidated through X-ray diffraction(XRD),X-ray fluorescence(XRF),and scanning electron microscopy(SEM)analyses.The results indicate that tetrasodium iminodisuccinate exhibits the highest leaching selectivity for Fe^(3+),while tartaric acid demonstrateds a comparable affinity for both Fe^(3+)and Al^(3+).In contrast citric acid shows superior selectivity toward Ca^(2+).The leaching yield of Fe^(3+),Al^(3+)and Ca^(2+)after sequential leaching with the three organic acids were 79.8%,65.08%and 78.6%,respectively.These findings confirm that effective and selective separation of Fe^(3+),Al^(3+)and Ca^(2+)from CGFS-H can be achieved via optimized organic acid-based leaching strategies.This advancement provides a critical foundation for developing Ca/Fe/Al hydrotalcite materials using CGFS-H as a sustainable feedstock,thereby facilitating the transformation of waste residue into high-value functional materials and promoting resourceefficient utilization of coal gasification fine slag.
文摘In this study,a multifunctional aptamer-conjugated magnetic covalent organic framework(COF)-CuO/Au nanozyme(MCOF-CuO/Au@apt)was developed as a“three-in-one”platform for dual-signal colorimetric and fluorescent detection of Vibrio parahaemolyticus.The nanozyme integrated magnetic separation,peroxidase-like catalytic activity,and specific target recognition through an aptamer-based strategy.Upon binding to V.parahaemolyticus,the catalytic oxidation of tetra-aminophenylethylene(TPE-4A)by the nanozyme was selectively inhibited,resulting in distinct colorimetric and fluorescent signals that significantly enhanced the detection accuracy and reliability.The proposed method exhibited high sensitivity,with limits of detection(LOD)of 21 and 7 CFU/mL for the colorimetric and fluorescent assays,respectively.The performance of this method was validated using real seafood samples,including Penaeus vannamei,Mytilus coruscus,and Crassostrea gigas,which showed high recovery rates(101.11%-107.30%)and excellent reproducibility.The system also demonstrated strong specificity and accuracy under various conditions,confirming its robustness and practical applicability.Collectively,this innovative platform presents a promising solution for the rapid,versatile,and sensitive detection of V.parahaemolyticus in seafood,with considerable potential to advance food safety diagnosis and on-site monitoring.
文摘The morphology of active layer plays a critical role in determining the photovoltaic performance of organic solar cells(OSCs).However,binary blends often suffer from suboptimal phase separation,which limits the efficiency of OSCs.Herein,two bridging polymer acceptors(PAs)—benzodithiophene-(2-ethylhexyl)oxy(BDT-C2C4)and benzodithiophene-octyloxy(BDT-C_(8))—are designed and synthesized by combining a benzodithiophene(BDT)unit as the donor moiety[poly({4,8-bis[5-(2-ethylhexyl)-4-fluorothiophen-2-yl]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl}){5,8-bis[4-(2-butyloctyl)thiophen-2-yl]dithieno[3',2':3,4]},D18],and a 2,2′-((2Z,2′Z)-{[12,13-Bis(2-butyloctyl)-12,13-dihydro-3,9-dinonylthieno[2,3]thieno[3,2-b]pyrrolo[4,5-g]thieno[2,3-b]indole-2,10-diyl]bis(methanylylidene)}bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(Y6)derivative as the acceptor moiety.BDT-C2C4 and BDT-C_(8) are functionalized with(2-ethylhexyl)oxy and octyloxy side chains on the BDT unit,respectively.Both PAs show complementary absorption and cascaded energy levels with the donor D18 and the acceptor 2,2′-((2Z,2′Z)-{[12,13-bis(3-ethylheptyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2″,3″∶4′,5′]thieno[2′,3′∶4,5]pyrrolo[3,2-g]thieno[2′,3′∶4,5]thieno[3,2-b]indole-2,10-diyl]bis(meth⁃aneylylidene)}bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile(N3),but BDT-C_(8) exhibits better compatibility with D18 and N3 compared to BDT-C2C4.When incorporated as a third component into the D18∶N3 blend,both PAs improve the active layer morphology.In particular,the D18∶N3∶BDT-C_(8) blend shows significantly optimized morphology,featuring reduced phase separation and a fibrous network structure.As a result,the device based on D18∶N3∶BDT-C_(8) achieves a power conversion efficiency of 18.18%,significantly higher than that of the device based on D18∶N3(ca.17.37%).This work presents a compatibilizer strategy for optimizing blend morphology towards high-performance ternary OSCs.
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.
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 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.
