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
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
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
Microplastic contamination has emerged as a threat in transplantation,with evidence of its presence in human tissues and potential to compromise grafts.Transplant recipients,vulnerable due to immunosuppression and sur...Microplastic contamination has emerged as a threat in transplantation,with evidence of its presence in human tissues and potential to compromise grafts.Transplant recipients,vulnerable due to immunosuppression and surgical exposure,face risk from microplastics via airborne particles,surgical materials,and organ preservation systems.These particles trigger inflammation,oxidative stress,and immune dysregulation—pathways critical in rejection.Microplastics support biofilm formation,potentially facilitating antimicrobial resistance in clinical settings.Despite this risk,transplant-specific research is lacking.We urge action through environmental controls,material substitutions,and procedural modifications,alongside research targeting exposure pathways,biological impact,and mitigation strategies.Transplantation has historically led medical innovation and must do so in confronting this environmental challenge.Leadership from global transplant societies is essential to protect recipients and ensure safe procedures.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
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
Multi-organ-on-a-chip(MOOC)technology represents a pivotal direction in the organ-on-a-chip field,seeking to emulate the complex interactions of multiple human organs in vitro through microfluidic systems.This technol...Multi-organ-on-a-chip(MOOC)technology represents a pivotal direction in the organ-on-a-chip field,seeking to emulate the complex interactions of multiple human organs in vitro through microfluidic systems.This technology overcomes the limitations of traditional single-organ models,providing a novel platform for investigating complex disease mechanisms and evaluating drug efficacy and toxicity.Although it demonstrates broad application prospects,its development still faces critical bottlenecks,including inadequate physiological coupling between organs,short functional maintenance durations,and limited real-time monitoring capabilities.Contemporary research is advancing along three key directions,including functional coupling,sensor integration,and full-process automation systems,to propel the technology toward enhanced levels of physiological relevance and predictive accuracy.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
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
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
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
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
Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comp...Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes(CnBTBT,n=4,8,12)as donors and fluorinated derivatives of tetracyanoquinodimethane(F_(m)TCNQ,m=0,2,4)as acceptors,aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure-property relationships.Our calculation results,based on the Boltzmann transport equation and deformation potential theory,reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties.Notably,the CnBTBT-F_(m)TCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics,particularly C4BTBT-F4TCNQ,which achieves an excellent power factor of 671µW cm^(-1) K^(-2) at an optimal charge carrier concentration.Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.展开更多
Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystall...Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystallinity and surface area of COFs,are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation,catalysis,chemical sensing,and energy storage.Therefore,it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development.In this review,we offer a comprehensive overview of recent advancements in PI-COFs,emphasizing their synthesis methods,design principles and applications.Finally,our brief outlooks on the current challenges and future developments of PI-COFs are provided.Overall,this review aims to guide the recent and future development of PI-COFs.展开更多
In floodplain wetlands,alterations in hydrological patterns resulting from climate change and human activities could potentially diminish the carbon sequestration capacity of the soils,thereby having a negative impact...In floodplain wetlands,alterations in hydrological patterns resulting from climate change and human activities could potentially diminish the carbon sequestration capacity of the soils,thereby having a negative impact on global climate change.However,the magnitude of the influence of hydrological regime change on soil carbon remains inadequately monitored.To address this research gap,we collected 306 upper layer(0–20 cm)soil samples from the Dongting Lake floodplain between 2013 and 2022.The random forest(RF)algorithm was used to analyze the spatial distribution of soil organic carbon(SOC)in the upper soil layer of Dongting Lake floodplain and the impact of climate and hydrological changes in the past decade on surface SOC in the East Dongting Lake area was studied.In 2022,the SOC concentration of the Dongting Lake floodplain upper layer soil ranged from 3.34 to 17.67 g kg^(-1),averaging 10.43 g kg^(-1),with a corresponding SOC density of(2.65±0.49)kg m^(-2) and total SOC stock of 6.82 Tg C(2.87–13.48 Tg C).From 2013 to 2022,the SOC concentration of the upper soil layer of the East Dongting Lake area decreased from 18.37 to 10.82 g kg^(-1).This reduction could be attributed to climate and hydrological changes which reduce SOC input by reducing vegetation growth and accelerating SOC decomposition.Above 21.4 m elevation,the amount of SOC loss increased with elevation,the loss being related to the decline in Miscanthus community biomass and greater susceptibility of higher altitude areas to climate and hydrological changes.Our results highlight the need for strengthening wetland SOC management to increase SOC in the soils to help combat climate change.展开更多
Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford prod...Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford products with fixed sequences and compositions.Herein,we report the triethylborane/1,8-diazabicyclo[5.4.0]undec-7-ene(Et_3B/DBU)pair-mediated four-component switchable polymerization of propylene oxide(PO),CO_(2),phthalic anhydride(PA),and racemic lactide(rac-LA),which enables the on-demand synthesis of four different block copolymers,i.e.,poly(propylene phthalate)-b-polylactide(PPE-b-PLA),PPE-b-PLA-b-poly(propylene carbonate)(PPC),PPE-b-PPC-b-PLA,and PPE-b-PPCb-poly(propylene oxide)(PPO),through rationally modulating the Lewis pair(LP)ratio.Core to this protocol is that increasing the loading of Et_(3)B accelerates the ring-opening of PO while impeding the reactivity of rac-LA,thus allowing for fine-tuning of the thermodynamic and kinetic of the switchable polymerization.Therefore,the four polymerization cycles involving PO/PA ring-opening copolymerization(ROCOP),PO/CO_(2) ROCOP,rac-LA ring-opening polymerization(ROP),and PO ROP can be connected and discriminated in precisely programmed manners.展开更多
Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible trans...Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible transmittance(AVT)and power conversion efficiency(PCE)remains a key issue of STOPVs.Herein,we innovatively applied a surface texturization strategy by integrating with a pseudo-planar heterojunction(PPHJ)structure to fabricate ST-OPVs,which possess outstanding photoelectric conversion and light management capability.The textured active layer performs significantly improved light capture capability and reduced optical loss due to that the micro-patterned arrays can deflect incident light multiple times.Moreover,the surface texturization strategy can enhance the crystallinity of the active layer and precisely control donor/acceptor inter-penetration,which magnifies exciton dissociation interface and forms ordered carrier dynamics.Consequently,the textured opaque device via blade-coating performs a record PCE of 19.17%(certified 19.02%)and the semi-transparent device achieves one of the highest light utilization efficiency(LUE)of 5.54%with prominent PCE(14.40%)and AVT(38.43%).Most importantly,the excellent thermal insulation performance and color rendering index of ST-OPVs are fitting for the agricultural greenhouses and insulation roofing,which shows that the surface texturization strategy can provide promising application prospects for ST-OPVs in economically sustainable agricultural development.展开更多
The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result...The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result in interface defects lurking between the photovoltaic layer and the electrode,thereby causing non-radiative recombination losses of interfacial charges.To tackle this issue,we introduced 4-bromobutyric acid to co-assemble with the SAM,yielding a more compact co-assembled monolayer(co-SAM)that effectively repairs these defective zones.Confocal laser scanning microscopy and Kelvin Probe Force Microscopy show that co-SAMs successfully mitigate interface defects in the previously uncovered electrode regions.Furthermore,the work function of the electrodes is elevated to 5.6 eV,facilitating efficient hole extraction.Consequently,devices incorporating co-SAMs exhibit notably reduced non-radiative recombination losses.The power conversion efficiency(PCE)of the devices is enhanced to 20.0% in binary organic solar cells,and an even more remarkable breakthrough PCE of 25.8% is achieved in perovskite/organic tandem devices.This study introduces a straightforward strategy to improve the hole-selective contact of electrodes,ultimately boosting the overall efficiency of the devices.展开更多
Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon ...Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon storage across different soil types,and identifying effective land management practices for enhanced carbon accumulation is essential for reducing agricultural emissions and strengthening carbon sinks.This study examined SOC variations in eastern Yunnan’s subtropical highlands(2,132 sites),analyzing topsoil(0–20 cm)across five land uses(dryland,irrigated land,forestland,grassland and plantation)of five soil types(red,yellow,yellowbrown,brown,purple).The investigation explored relationships between SOC and edaphic factors(26 elements)to determine SOC influencing factors.The study area demonstrated a mean SOC content of 27.78 g kg^(–1),with distinct spatial heterogeneity characterized by lower values in the southwestern sector and higher concentrations in the northeastern region.Brown soils displayed the highest SOC content(P<0.05),followed by yellow-brown then red,yellow,and purple soils.Irrigation significantly enhanced SOC storage,particularly in brown soils where irrigated land contained 2.2-,2.4-,and 1.6-times higher SOC than forestland,grassland,and dryland,respectively.Similar irrigation benefits occurred in purple,yellow,and yellow-brown soils,indicating moisture limitation as the primary SOC constraint.Notably,SOC exhibited strong positive correlations with nitrogen,sulfur,and selenium.Nitrogen fertilization demonstrated dual benefits:enhancing SOC sequestration and promoting Se enrichment in crops,potentially supporting specialty agriculture.Although land use impacts on SOC varied across soil types(P>0.05),irrigation consistently emerged as the optimal management for carbon sink enhancement.These findings suggest that targeted water management could effectively reduce farmland carbon emissions in moisture-limited subtropical highlands.Strategic nitrogen application offers co-benefits for soil fertility and selenium biofortification,providing practical pathways for climate-smart agriculture in similar ecoregions.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Microplastic contamination has emerged as a threat in transplantation,with evidence of its presence in human tissues and potential to compromise grafts.Transplant recipients,vulnerable due to immunosuppression and surgical exposure,face risk from microplastics via airborne particles,surgical materials,and organ preservation systems.These particles trigger inflammation,oxidative stress,and immune dysregulation—pathways critical in rejection.Microplastics support biofilm formation,potentially facilitating antimicrobial resistance in clinical settings.Despite this risk,transplant-specific research is lacking.We urge action through environmental controls,material substitutions,and procedural modifications,alongside research targeting exposure pathways,biological impact,and mitigation strategies.Transplantation has historically led medical innovation and must do so in confronting this environmental challenge.Leadership from global transplant societies is essential to protect recipients and ensure safe procedures.
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.
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 Shenzhen Medical Research Fund(Grant No.A2303049)Guangdong Basic and Applied Basic Research(Grant No.2023A1515010647)+1 种基金National Natural Science Foundation of China(Grant No.22004135)Shenzhen Science and Technology Program(Grant No.RCBS20210706092409020,GXWD20201231165807008,20200824162253002).
文摘Multi-organ-on-a-chip(MOOC)technology represents a pivotal direction in the organ-on-a-chip field,seeking to emulate the complex interactions of multiple human organs in vitro through microfluidic systems.This technology overcomes the limitations of traditional single-organ models,providing a novel platform for investigating complex disease mechanisms and evaluating drug efficacy and toxicity.Although it demonstrates broad application prospects,its development still faces critical bottlenecks,including inadequate physiological coupling between organs,short functional maintenance durations,and limited real-time monitoring capabilities.Contemporary research is advancing along three key directions,including functional coupling,sensor integration,and full-process automation systems,to propel the technology toward enhanced levels of physiological relevance and predictive accuracy.
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 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 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 Strategic Priority Research Program of the Chinese Academy of Science(No.XDB0520000)the National Natural Science Foundation of China(Nos.52273170 and 52394271)the National Key R&D Program of China(No.2022YFA1203200).
文摘Charge-transfer complexes(CTCs)have emerged as promising n-type organic thermoelectric(TE)materials due to their inherent high electrical conductivity and tunable transport polarities.In this study,we performed a comprehensive first-principles investigation on the TE properties of nine CTCs comprised of 2,7-dialkyl[1]benzothieno[3,2-b][1]benzothiophenes(CnBTBT,n=4,8,12)as donors and fluorinated derivatives of tetracyanoquinodimethane(F_(m)TCNQ,m=0,2,4)as acceptors,aiming to identify high-performance n-type organic TE materials and elucidate the underlying structure-property relationships.Our calculation results,based on the Boltzmann transport equation and deformation potential theory,reveal that the length of the alkyl side chains and the number of fluorine substitutions significantly impact their electronic structures and TE properties.Notably,the CnBTBT-F_(m)TCNQ CTCs with shorter alkyl chains and more fluorine substitution demonstrate superior n-type characteristics,particularly C4BTBT-F4TCNQ,which achieves an excellent power factor of 671µW cm^(-1) K^(-2) at an optimal charge carrier concentration.Our findings not only clarify the critical role of molecular engineering in CTC-based TE materials but also provide valuable guidance for developing high-efficiency organic TE materials with versatile practical applications.
基金supported by the National Key R&D Program of China(No.2023YFA1507204)National Natural Science Foundation ofChina(Nos.22475074,22171139,22225109,22302055)+4 种基金Natural Science Foundation of Guangdong Province(No.2023B1515020076)Key Scientific Research Project Plan of Colleges and Universities of Henan Province(No.24B150004)The Double Thousand Talents Plan of Jiangxi Province(No.jxsq2023102003)Project supported by the Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization(No.2024B121201001)Project supportedby the Major Research plan of the National Natural Science Foundation of China(No.92461310).
文摘Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystallinity and surface area of COFs,are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation,catalysis,chemical sensing,and energy storage.Therefore,it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development.In this review,we offer a comprehensive overview of recent advancements in PI-COFs,emphasizing their synthesis methods,design principles and applications.Finally,our brief outlooks on the current challenges and future developments of PI-COFs are provided.Overall,this review aims to guide the recent and future development of PI-COFs.
基金supported by the National Key Research and Development Program of China(2022YFC3204101 and 2023YFF0807202)the National Natural Science Foundation of China(U22A20570 and U2444221)+4 种基金the Youth Promotion Association of the Chinese Academy of Sciences(2021365)the Changsha Outstanding Innovative Youth Project,China(kq2305035)the Science,Technology and Innovation Platform Plan of Hunan Province,China(2022PT1010)the Major Scientific and Technological Projects of the Ministry of Water Resources,China(SKS-2022081)the Comprehensive Investigation and Potential Evaluation of Natural Resources Carbon Sink in Southern Hilly Region,China(DD20220880)。
文摘In floodplain wetlands,alterations in hydrological patterns resulting from climate change and human activities could potentially diminish the carbon sequestration capacity of the soils,thereby having a negative impact on global climate change.However,the magnitude of the influence of hydrological regime change on soil carbon remains inadequately monitored.To address this research gap,we collected 306 upper layer(0–20 cm)soil samples from the Dongting Lake floodplain between 2013 and 2022.The random forest(RF)algorithm was used to analyze the spatial distribution of soil organic carbon(SOC)in the upper soil layer of Dongting Lake floodplain and the impact of climate and hydrological changes in the past decade on surface SOC in the East Dongting Lake area was studied.In 2022,the SOC concentration of the Dongting Lake floodplain upper layer soil ranged from 3.34 to 17.67 g kg^(-1),averaging 10.43 g kg^(-1),with a corresponding SOC density of(2.65±0.49)kg m^(-2) and total SOC stock of 6.82 Tg C(2.87–13.48 Tg C).From 2013 to 2022,the SOC concentration of the upper soil layer of the East Dongting Lake area decreased from 18.37 to 10.82 g kg^(-1).This reduction could be attributed to climate and hydrological changes which reduce SOC input by reducing vegetation growth and accelerating SOC decomposition.Above 21.4 m elevation,the amount of SOC loss increased with elevation,the loss being related to the decline in Miscanthus community biomass and greater susceptibility of higher altitude areas to climate and hydrological changes.Our results highlight the need for strengthening wetland SOC management to increase SOC in the soils to help combat climate change.
基金financially supported by National Key R&D Program Young Scientists Project(No.2023YFC3903100)the National Natural Science Foundation of China(No.22322503)analytical and testing assistance from the Analysis and Testing Center of HUST。
文摘Switchable polymerization is emerging as a powerful tool to construct block copolymers directly from mixtures of monomers.However,current achievements typically iterate between two polymerization cycles to afford products with fixed sequences and compositions.Herein,we report the triethylborane/1,8-diazabicyclo[5.4.0]undec-7-ene(Et_3B/DBU)pair-mediated four-component switchable polymerization of propylene oxide(PO),CO_(2),phthalic anhydride(PA),and racemic lactide(rac-LA),which enables the on-demand synthesis of four different block copolymers,i.e.,poly(propylene phthalate)-b-polylactide(PPE-b-PLA),PPE-b-PLA-b-poly(propylene carbonate)(PPC),PPE-b-PPC-b-PLA,and PPE-b-PPCb-poly(propylene oxide)(PPO),through rationally modulating the Lewis pair(LP)ratio.Core to this protocol is that increasing the loading of Et_(3)B accelerates the ring-opening of PO while impeding the reactivity of rac-LA,thus allowing for fine-tuning of the thermodynamic and kinetic of the switchable polymerization.Therefore,the four polymerization cycles involving PO/PA ring-opening copolymerization(ROCOP),PO/CO_(2) ROCOP,rac-LA ring-opening polymerization(ROP),and PO ROP can be connected and discriminated in precisely programmed manners.
基金the support from the National Natural Science Foundation of China(52333006)the support from the National Natural Science Foundation of China(52303232)+1 种基金the Natural Science Foundation of Jiangxi Province(20242BAB20184)the support from National Natural Science Foundation of China(52373186)。
文摘Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible transmittance(AVT)and power conversion efficiency(PCE)remains a key issue of STOPVs.Herein,we innovatively applied a surface texturization strategy by integrating with a pseudo-planar heterojunction(PPHJ)structure to fabricate ST-OPVs,which possess outstanding photoelectric conversion and light management capability.The textured active layer performs significantly improved light capture capability and reduced optical loss due to that the micro-patterned arrays can deflect incident light multiple times.Moreover,the surface texturization strategy can enhance the crystallinity of the active layer and precisely control donor/acceptor inter-penetration,which magnifies exciton dissociation interface and forms ordered carrier dynamics.Consequently,the textured opaque device via blade-coating performs a record PCE of 19.17%(certified 19.02%)and the semi-transparent device achieves one of the highest light utilization efficiency(LUE)of 5.54%with prominent PCE(14.40%)and AVT(38.43%).Most importantly,the excellent thermal insulation performance and color rendering index of ST-OPVs are fitting for the agricultural greenhouses and insulation roofing,which shows that the surface texturization strategy can provide promising application prospects for ST-OPVs in economically sustainable agricultural development.
基金supported by the National Natural Science Foundation of China(52303239,51933001,22475114)the Natural Science Foundation of Shandong Province(ZR2022QB141,2023HWYQ-087)+1 种基金the Shanghai Pujiang Program(23PJ1409700)the Hubei Province Key Research Program(2023BAB109)。
文摘The self-assembled monolayer(SAM),functioning as a hole transport layer,holds the potential to substantially elevate the efficiency of perovskite and organic solar cells.Nevertheless,incomplete SAM coverage may result in interface defects lurking between the photovoltaic layer and the electrode,thereby causing non-radiative recombination losses of interfacial charges.To tackle this issue,we introduced 4-bromobutyric acid to co-assemble with the SAM,yielding a more compact co-assembled monolayer(co-SAM)that effectively repairs these defective zones.Confocal laser scanning microscopy and Kelvin Probe Force Microscopy show that co-SAMs successfully mitigate interface defects in the previously uncovered electrode regions.Furthermore,the work function of the electrodes is elevated to 5.6 eV,facilitating efficient hole extraction.Consequently,devices incorporating co-SAMs exhibit notably reduced non-radiative recombination losses.The power conversion efficiency(PCE)of the devices is enhanced to 20.0% in binary organic solar cells,and an even more remarkable breakthrough PCE of 25.8% is achieved in perovskite/organic tandem devices.This study introduces a straightforward strategy to improve the hole-selective contact of electrodes,ultimately boosting the overall efficiency of the devices.
基金funded by the Yunnan Provincial Key Programs for Basic Research Project,China(202301AS070087)the Yunnan Provincial R&D Program,China(202405AF140014 and 202302AO370015)the National Natural Science Foundation of China(42307058).
文摘Soil organic carbon(SOC)dynamics significantly influence ecosystem carbon source-sink balance,particularly in agroecosystems.However,uncertainty remains regarding optimal land use types for maximizing farmland carbon storage across different soil types,and identifying effective land management practices for enhanced carbon accumulation is essential for reducing agricultural emissions and strengthening carbon sinks.This study examined SOC variations in eastern Yunnan’s subtropical highlands(2,132 sites),analyzing topsoil(0–20 cm)across five land uses(dryland,irrigated land,forestland,grassland and plantation)of five soil types(red,yellow,yellowbrown,brown,purple).The investigation explored relationships between SOC and edaphic factors(26 elements)to determine SOC influencing factors.The study area demonstrated a mean SOC content of 27.78 g kg^(–1),with distinct spatial heterogeneity characterized by lower values in the southwestern sector and higher concentrations in the northeastern region.Brown soils displayed the highest SOC content(P<0.05),followed by yellow-brown then red,yellow,and purple soils.Irrigation significantly enhanced SOC storage,particularly in brown soils where irrigated land contained 2.2-,2.4-,and 1.6-times higher SOC than forestland,grassland,and dryland,respectively.Similar irrigation benefits occurred in purple,yellow,and yellow-brown soils,indicating moisture limitation as the primary SOC constraint.Notably,SOC exhibited strong positive correlations with nitrogen,sulfur,and selenium.Nitrogen fertilization demonstrated dual benefits:enhancing SOC sequestration and promoting Se enrichment in crops,potentially supporting specialty agriculture.Although land use impacts on SOC varied across soil types(P>0.05),irrigation consistently emerged as the optimal management for carbon sink enhancement.These findings suggest that targeted water management could effectively reduce farmland carbon emissions in moisture-limited subtropical highlands.Strategic nitrogen application offers co-benefits for soil fertility and selenium biofortification,providing practical pathways for climate-smart agriculture in similar ecoregions.
