The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8...The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8PBPy)based on cycloparaphenylenes(CPPs)grafted with eight pyrene-functionalized units was reported.This structurally well-defined nanohoop not only acts as a segment of armchair-type CNTs but also achieves enhanced longitudinal π-extension.The structure of[12]CPP-8PBPy was confirmed by high-resolution mass spectrometry(HRMS)and nuclear magnetic resonance(NMR).The photophysical properties were studied by UV/Vis and photoluminescence spectroscopy.The potential applications of[12]CPP-8PBPy in electron-transport devices were further investigated.展开更多
Cancer is the second leading cause of death globally.Its treatment remains a major challenge due to the disease's complexity,heterogeneity,and adaptive nature.Among the array of available treatments,targeted thera...Cancer is the second leading cause of death globally.Its treatment remains a major challenge due to the disease's complexity,heterogeneity,and adaptive nature.Among the array of available treatments,targeted therapy emerges as a paramount approach to address this substantial unmet clinical need,owing to its precise tumor targeting capabilities and potential for mitigating tumor progression risks.Drug conjugates are in high demand for targeted therapy due to their unique ligand specificity and potent cytotoxicity,thereby significantly enhancing therapeutic efficacy and reducing the incidence of adverse effects.Therefore,as a burgeoning field in biomedical research,it is timely to outline the latest advances in drug conjugates-driven cancer treatment.Herein,we aim to present the emerging breakthroughs in this exciting field at the intersection of target ligands,linkers,payloads,and cancer treatments.This review focuses on several drug conjugates-related strategies,including antibody-drug conjugates(ADCs),peptide-drug conjugates(PDCs),small molecule-drug conjugates(SMDCs),aptamer-drug conjugates(ApDCs)and radionuclide-drug conjugates(RDCs).Finally,we discuss the fundamentals behind drug conjugate-based anticancer therapeutics,along with their inherent advantages and associated challenges,as well as recent research advances.展开更多
The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water ev...The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.展开更多
The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by th...The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials.In response,we propose a prototypal hybridization strategy to design a novel series of aminated conjugated microporous polymer(CMPN)@collagen fiber membrane(COLM).These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90%of the uranium in just 30 min from 50 ppm with a high selectivity of Kd>105 mL·g^(−1).They also afford a robustly reusable adsorption capacity as high as 345 mg·g^(−1)that could harvest 1.61 mg·g^(−1)of uranium in a short 7-day real marine engineering in Fujian Province,even though suffered from very low uranium concentration of 3.29μg·L^(−1)and tough influence of salts such as 10.77 g·L^(−1)of Na^(+),1.75μg·L^(−1)of VO_(3)^(−)etc.in the rough seas.The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN-COLM,and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.展开更多
Conjugated microporous polymers(CMPs)are a unique class of organic porous materials characterized byπ-conjugated structures and permanent micropores,distinguishing them from non-porous polymers and conventionalπ-con...Conjugated microporous polymers(CMPs)are a unique class of organic porous materials characterized byπ-conjugated structures and permanent micropores,distinguishing them from non-porous polymers and conventionalπ-conjugated polymers.CMPs offer extensive versatility in synthetic approaches,enabling the synthesis of cross-linked and mesoporous structures.Advances in chemical processes,structural design,and synthesis methodologies have been developed,resulting in a diverse range of CMPs with unique configurations and properties,contributing to the fast expansion of the field.CMPs are particularly notable for their ability to enable the competitive utilization ofπ-conjugated structures within mesoporous configurations,making them valuable for investigations across various domains.They have shown considerable promise in addressing fuel and environmental challenges,demonstrated by their exceptional performance in applications such as vapor adsorption,heterogeneous catalysis,light emission,light harvesting,and energy generation.This review examines the chemical engineering principles underlying CMPs,including synthesis approaches,systemic research advancements,multifunctional investigations boundaries,potential applications,and progress in synthesis,dimensionality,and morphology studies.Specifically,it offers a comparative analysis of CMPs and linear polymeric materials,aiding in the development of functional polymers.Furthermore,this review explores the primary fundamental limitations of CMPs in fuel-related domains and discusses alternative strategies,including novel synthesis methods incorporating interactions and morphologies,to address these challenges.Ultimately,this assessment aims to provide a valuable and inspiring resource for professionals in the field of fuel management,guiding future research and development efforts.展开更多
The scalable fabrication of stretchable conjugated polymer films via solution printing is essential for their practical application in largearea wearable electronics.However,the printed conjugated polymer films typica...The scalable fabrication of stretchable conjugated polymer films via solution printing is essential for their practical application in largearea wearable electronics.However,the printed conjugated polymer films typically exhibit high crystallinity,limiting their mechanical deformability.Herein,we propose a plasticizer-assisted printing strategy to simultaneously enhance the stretchability and electrical performance of films based on the conjugated polymer poly(3-(5-(5-methylselenophen-2-yl)thiophen-2-yl)-6-(5-methylthiophen-2-yl)-2,5-bis(4-octyltetradecyl)-2,5-dihydropyrrolo[3,4-c]pyrrole-1,4-dione)(P(TDPP-Se)).The incorporation of a plasticizer trioctyl trimellitate(TOTM)promotes P(TDPP-Se)aggregation in initial solution,facilitates chain alignment under flow field,and shorten solidification process,thereby restricting randomly polymer crystallization.Consequently,a low-crystallinity film with favorable edge-on orientation,strong chain alignment and improved chain dynamics is realized,which effectively alleviates crystallites fragmentation and crack propagation under large strain.The TOTM-plasticized film exhibits approximately 2-fold improvements in fracture strain and charge mobility,along with superior mobility retention under 100%strain in comparison to the neat film.This study provides a feasible approach for microstructure control in printed stretchable conjugated polymer film.展开更多
Pure organic room-temperature phosphorescent(RTP)polymers possess good processability and flexibility over small molecular crystals.However,most of RTP polymers reported so far are based on non-conjugated polymers,and...Pure organic room-temperature phosphorescent(RTP)polymers possess good processability and flexibility over small molecular crystals.However,most of RTP polymers reported so far are based on non-conjugated polymers,and achieving efficient phosphorescent emission in RTP conjugated polymers(CPs)remains a significant challenge.Herein,we developed two RTP CPs(P(PSe ZPh-p-Ph)and P(PSe ZPh-m-Ph))by linking the phenoselenazine units with the para-and meta-phenylene units,respectively,to form the conjugated main chains.The phenylene linker with different lingking mode manipulates the effictiveπ-conjugation of the polymer backbones.Comparing with the para-linked P(PSe ZPh-pPh),meta-linked P(PSe ZPh-m-Ph)exhibit the decreased effectiveπ-conjugation and the enhanced contribution of selenium atoms to the frontier orbitals,leading to the larger spin-orbit coupling(SOC)constants and the accelerated phosphorescence radiative decay process.The P(PSe ZPhm-Ph)achieves a phosphorescence quantum yield of 21.4%in doped polystyrene films,which is among the highest efficiencies reported to date for pure organic RTP CPs.These CPs are applied to construct phosphorescent film sensors for oxygen detection with the high quenching constants(K_(sv))up to 14.80 kPa^(-1)and low detection of limit of 0.84 ppm,demostrating the potential for application in oxygen film sensors.展开更多
The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial reg...The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial regulation of the state transition between photosystem I(PSI)and photosystem II(PSII)represents a strategic and promising approach for improving the efficiency of natural photosynthesis.In this study,we demonstrate that poly(benzimidazolium-phenylthiophene)(CP4)featuring a flexible cationic backbone exhibits superior ultraviolet light-harvesting capability.The polymer CP4 enhanced PSI activity in Chlorella pyrenoidosa(C.pyrenoidosa),subsequently promoting PSII activity and augmenting overall photosynthetic performance.During light-dependent reactions,CP4 significantly accelerated photosynthetic electron transfer,resulting in a 330%increase in the production of oxygen and 93%and 96%increases in the ATP and NADPH contents,respectively.In the context of dark reactions,CP4 facilitated the conversion and utilization of light energy,leading to a 6%increase in both carbohydrate and protein contents.These findings indicate that synthetic light-harvesting polymer materials exhibit considerable application potential in the field of biomass production through enhancement of natural photosynthetic efficiency.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
Breast cancer is a heterogeneous disease stratified by hormone receptors(HRs)and human epidermal growth factor receptor 2(HER2)status and each subtype has divergent therapeutic needs.Despite the current therapeutic ad...Breast cancer is a heterogeneous disease stratified by hormone receptors(HRs)and human epidermal growth factor receptor 2(HER2)status and each subtype has divergent therapeutic needs.Despite the current therapeutic advances,resistance to standard therapies remains pervasive,underscoring the demand for novel strategies.Antibody-drug conjugates(ADCs)offer a powerful strategy by combining tumor-specific antibodies to potent cytotoxins,enabling selective delivery and minimizing off-target toxicity1.TROP2,a transmembrane glycoprotein broadly overexpressed in breast cancer,has emerged as a promising ADC target.The approval of datopotamab deruxtecan(Dato-DXd)with sacituzumab govitecan(SG)and the incorporation of these ADCs into the National Comprehensive Cancer Network(NCCN)guidelines(v2.2025)highlight the fast penetration of TROP2 ADCs into clinical practice2.This editorial provides timely insights into optimizing TROP2-targeted strategies to improve outcomes across breast cancer subtypes.展开更多
Objectives:B-cell maturation antigen(BCMA)-targeted antibody–drug conjugates(ADCs)have emerged as promising therapies for relapsed/refractory multiple myeloma(RRMM),but the overall efficacy and safety profile is uncl...Objectives:B-cell maturation antigen(BCMA)-targeted antibody–drug conjugates(ADCs)have emerged as promising therapies for relapsed/refractory multiple myeloma(RRMM),but the overall efficacy and safety profile is unclear.This study aimed to synthesize the available evidence on the safety and efficacy of BCMA-ADCs in development for RRMM.Methods:A systematic search was conducted using six bibliographic databases and ClinicalTrials.gov up to November 2024.Studies were eligible if they were human clinical trials or animal studies evaluating BCMA-ADCs and reported efficacy and safety outcomes.Data extraction and quality assessments were conducted using validated tools,including ROBINS-I and SYRCLE’s risk of bias tool.Results:A total of 21 studies were included:16 clinical trials and five animal studies.Key findings included that belantamab mafodotin demonstrated variable but generally durable response rates(32%–85%)and a broad range of progression-free survival(PFS)(2.8–36.6 months),albeit with ocular toxicities in 51%–96%.Among newer candidates,MEDI2228 showed median PFS 5.1–6.6 months with 14%discontinuation for ocular symptoms,while AMG 224 had an overall response rate(ORR)of 23%(9/40)with anemia 21%,thrombocytopenia 24%,and ocular adverse events(AEs)21%.Animal studies supported the tumor-eradicating potential of all BCMA-ADC candidates,although safety signals such as hepatic and renal toxicity were noted with HDP-101.The risk of bias assessment revealed generally moderate to serious concerns in human trials,while the overall quality of the animal studies was acceptable.Conclusions:BCMA-targeted ADC candidates show encouraging efficacy in RRMM,particularly belantamab mafodotin.However,frequent AEs,especially ocular and hematologic toxicities,underscore the need for optimization in ADC design.Further research should prioritize enhancing safety while maintaining clinical benefit.展开更多
Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended...Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended conjugation is designed and synthesized,named NaPh-4PACz.Compared to Ph-4PACz,NaPh-4PACz exhibits a larger adsorption energy with the ITO substrate,enabling the formation of a more uniform and dense film,thereby preventing direct contact between the perovskite and ITO.Additionally,NaPh-4PACz also has a stronger interaction with the perovskite,which can reduce buried interface defects and suppress non-radiative recombination.Consequently,NaPh-4PACz-based devices achieved a power conversion efficiency of 25.48%due to their interfacial“adhesive”ability.Importantly,the stability of the NaPh-4PACz-based devices was significantly improved.展开更多
Formamidinium lead iodide(FAPbI_(3))perovskite exhibits an impressive X-ray absorption coefficient and a large carrier mobility-lifetime product(μτ),making it as a highly promising candidate for X-ray detection appl...Formamidinium lead iodide(FAPbI_(3))perovskite exhibits an impressive X-ray absorption coefficient and a large carrier mobility-lifetime product(μτ),making it as a highly promising candidate for X-ray detection application.However,the presence of larger FA^(+)cation induces to an expansion of the Pb-I octahedral framework,which unfortunately affects both the stability and charge carrier mobility of the corresponding devices.To address this challenge,we develop a novel low-dimensional(HtrzT)PbI_(3) perovskite featuring a conjugated organic cation(1H-1,2,4-Triazole-3-thiol,HtrzT^(+))which matches well with theα-FAPbI_(3) lattices in two-dimensional plane.Benefiting from the matched lattice between(HtrzT)PbI_(3) andα-FAPbI_(3),the anchored lattice enhances the Pb-I bond strength and effectively mitigates the inherent tensile strain of theα-FAPbI_(3) crystal lattice.The X-ray detector based on(HtrzT)PbI_(3)(1.0)/FAPbI_(3) device achieves a remarkable sensitivity up to 1.83×10^(5)μC Gy_(air)^(−1) cm^(−2),along with a low detection limit of 27.6 nGy_(air) s^(−1),attributed to the release of residual stress,and the enhancement in carrier mobility-lifetime product.Furthermore,the detector exhibits outstanding stability under X-ray irradiation with tolerating doses equivalent to nearly 1.17×10^(6) chest imaging doses.展开更多
In this paper,we propose a three-term conjugate gradient method for solving unconstrained optimization problems based on the Hestenes-Stiefel(HS)conjugate gradient method and Polak-Ribiere-Polyak(PRP)conjugate gradien...In this paper,we propose a three-term conjugate gradient method for solving unconstrained optimization problems based on the Hestenes-Stiefel(HS)conjugate gradient method and Polak-Ribiere-Polyak(PRP)conjugate gradient method.Under the condition of standard Wolfe line search,the proposed search direction is the descent direction.For general nonlinear functions,the method is globally convergent.Finally,numerical results show that the proposed method is efficient.展开更多
The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Cova...The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.展开更多
π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviolo...π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviologen 3c was modified with a methylnaphthalene group,while 3a and 3b were modified with methyl and benzyl groups,respectively,for comparison.These pyrenoviologens exhibit reversible redox properties and strong fluorescence emission.Electrochromic devices(ECDs)were prepared using pyrenoviologens as the active materials.Notably,naphthalene-containing pyrenoviologen 3c,with its DA-D-A-D conjugated structure,possesses more stable free radicals,enabling it to maintain the radical color for a longer duration after power loss.A series of color-changing devices were successfully assembled.Due to the strong fluorescence of pyrenoviologens and the unique electron transfer effect between them and picric acid(PA),a sensor film with good selectivity and high sensitivity for PA in aqueous solution was prepared using pyrenoviologens as the fluorescent probe.Specifically,3c exhibited the highest sensitivity to PA due to its lowest energy gap.The introduction of the D-A-D-A-D structure is a strategic approach to enhancing photoelectric performance and broadening the application of viologens.展开更多
The fluorescence imaging (FLI) in the second near-infrared window (NIR-II, 1000–1700nm) has attracted considerable attention in the past decade. In contrast to conventional NIR-I window excitation (808nm/980nm), FLI ...The fluorescence imaging (FLI) in the second near-infrared window (NIR-II, 1000–1700nm) has attracted considerable attention in the past decade. In contrast to conventional NIR-I window excitation (808nm/980nm), FLI with NIR-II window excitation (1064nm/other wavelength beyond 1000nm) can afford deeper tissue penetration depth with high clarity due to the merits of suppressed photon scattering and diminished autofluorescence. In this review, we have summarized NIR-II window excitable/emissive organic/polymeric fluorophores recently developed. The characteristics of these fluorophores such as chemical structures and photophysical properties have also been critically discussed. Furthermore, the latest development of noninvasive in vivo FLI with NIR-II excitation was highlighted. The ideal imaging results emphasized the importance of NIR-II excitation of these fluorophores in enabling deep tissue penetration and high-resolution imaging. Finally, a perspective on the challenges and prospects of NIR-II excitable/emissive organic/polymeric fluorophores was also discussed. We expected this review will be served as a source of inspiration for researchers, stimulating the creation of novel NIR-II excitable fluorophores and fostering the development of bioimaging applications.展开更多
Urothelial carcinoma(UC)is the 9th most common and the 13th most deadly cancer worldwide1.Despite the availability of platinum-based chemotherapy and immune checkpoint inhib-itors(ICIs),the 5-year survival rate of pat...Urothelial carcinoma(UC)is the 9th most common and the 13th most deadly cancer worldwide1.Despite the availability of platinum-based chemotherapy and immune checkpoint inhib-itors(ICIs),the 5-year survival rate of patients with metastatic UC(mUC)remains poor(10-15%)2.展开更多
Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we repo...Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we report the design of four novel metal-salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO_(2)with gaseous water.Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks,they show a maximum CO_(2)adsorption capacity of 46.1 cm3 g^(−1)and adsorption selectivity for CO_(2)/N_(2)of up to 82 at 273 K.Under air atmosphere and simulated solar light(100mWcm^(−2)),TEPT-Zn shows an excellent CO yield of 304.96μmol h^(−1)g^(−1)with a selectivity of approximately 100%,which represents one of the best results in terms of organic photocatalysts for gas-phase CO_(2)photoreduction so far.Furthermore,only small degradation in the CO yield is observed even after 120-h continuous illumination.More importantly,a good CO yield of 152.52μmol g^(−1)was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h(25-28℃,52.3±7.9mWcm^(−2)).This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO_(2)from air.展开更多
A comprehensive understanding of the relevance between molecular structure and passivation ability to screen efficient modifiers is essential for enhancing the performance of perovskite solar cells(PSCs).Here,three si...A comprehensive understanding of the relevance between molecular structure and passivation ability to screen efficient modifiers is essential for enhancing the performance of perovskite solar cells(PSCs).Here,three similarπ-πstacking molecules namely benzophenone(BPN),diphenyl sulfone(DPS),and diphenyl sulfoxide(DPSO)are used as back-interface modifiers in carbon-based CsPbBr_(3)PSCs.After investigation,the results demonstrate the positive effect of the p-πconjugation characteristic inπ-πstacking molecules on maximizing their passivation ability.The p-πco njugation of DPSO enables a higher coordinative activity of oxygen atom in its S=O group than that in 0=S=O group of DPS and C=O group of BPN,which gives a superior passivation effect of DPSO on defects of perovskite films.The modification of DPSO also significantly improves the p-type behavior of perovskite films and the back-interfacial energetics matching,inducing an increase of hole extraction and a decrease of energy loss.Finally,the unencapsulated carbon-based CsPbBr_(3)PSCs with DPSO achieve a maximum power conversion efficiency of 10.60%and outstanding long-term stability in high-temperature,high-humidity(85℃,85%relative humidity)air environment.This work provides insights into the influence of the structure ofπ-πstacking molecules on their ability to improve the perovskite films quality and therefore the PSCs performance.展开更多
文摘The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8PBPy)based on cycloparaphenylenes(CPPs)grafted with eight pyrene-functionalized units was reported.This structurally well-defined nanohoop not only acts as a segment of armchair-type CNTs but also achieves enhanced longitudinal π-extension.The structure of[12]CPP-8PBPy was confirmed by high-resolution mass spectrometry(HRMS)and nuclear magnetic resonance(NMR).The photophysical properties were studied by UV/Vis and photoluminescence spectroscopy.The potential applications of[12]CPP-8PBPy in electron-transport devices were further investigated.
基金the Project of China-Japan Joint International Laboratory of Advanced Drug Delivery System Research and Translation of Liaoning Province(No.2024JH2/102100007)the open fund of National Key Laboratory of Advanced DrugFormulations for Overcoming Delivery Barriers(No.2024-KFB-003)+1 种基金the National Natural Science Foundation of China(No.82104109)Scientific Research Project of Liaoning Department of Education(No.LJ212410163045).
文摘Cancer is the second leading cause of death globally.Its treatment remains a major challenge due to the disease's complexity,heterogeneity,and adaptive nature.Among the array of available treatments,targeted therapy emerges as a paramount approach to address this substantial unmet clinical need,owing to its precise tumor targeting capabilities and potential for mitigating tumor progression risks.Drug conjugates are in high demand for targeted therapy due to their unique ligand specificity and potent cytotoxicity,thereby significantly enhancing therapeutic efficacy and reducing the incidence of adverse effects.Therefore,as a burgeoning field in biomedical research,it is timely to outline the latest advances in drug conjugates-driven cancer treatment.Herein,we aim to present the emerging breakthroughs in this exciting field at the intersection of target ligands,linkers,payloads,and cancer treatments.This review focuses on several drug conjugates-related strategies,including antibody-drug conjugates(ADCs),peptide-drug conjugates(PDCs),small molecule-drug conjugates(SMDCs),aptamer-drug conjugates(ApDCs)and radionuclide-drug conjugates(RDCs).Finally,we discuss the fundamentals behind drug conjugate-based anticancer therapeutics,along with their inherent advantages and associated challenges,as well as recent research advances.
基金financially supported by the Natural Science Foundation of Jiangxi Province(No.20232ACB204002)the Jiangxi Provincial Key Laboratory of Flexible Electronics(No.20242BCC32010).
文摘The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.
基金supported by National Natural Science Foundation of China(Grant No.22378066,22108040)Collaboration&Innovation Platform Project of National Independent Innovation Demonstration Zone(Fuzhou,Xiamen&Quanzhou)(Project No:3502ZCQXT2023004).
文摘The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials.In response,we propose a prototypal hybridization strategy to design a novel series of aminated conjugated microporous polymer(CMPN)@collagen fiber membrane(COLM).These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90%of the uranium in just 30 min from 50 ppm with a high selectivity of Kd>105 mL·g^(−1).They also afford a robustly reusable adsorption capacity as high as 345 mg·g^(−1)that could harvest 1.61 mg·g^(−1)of uranium in a short 7-day real marine engineering in Fujian Province,even though suffered from very low uranium concentration of 3.29μg·L^(−1)and tough influence of salts such as 10.77 g·L^(−1)of Na^(+),1.75μg·L^(−1)of VO_(3)^(−)etc.in the rough seas.The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN-COLM,and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.
基金supported by the King Khalid University,Abha,Saudi Arabiathe Deanship of Scientific Research at King Khalid University for funding this work through Large Groups Project under grant number(R.G.P.2/335/46)the Guangdong Office of Research Projects at the Provincial University(No.2024KCXTD064)。
文摘Conjugated microporous polymers(CMPs)are a unique class of organic porous materials characterized byπ-conjugated structures and permanent micropores,distinguishing them from non-porous polymers and conventionalπ-conjugated polymers.CMPs offer extensive versatility in synthetic approaches,enabling the synthesis of cross-linked and mesoporous structures.Advances in chemical processes,structural design,and synthesis methodologies have been developed,resulting in a diverse range of CMPs with unique configurations and properties,contributing to the fast expansion of the field.CMPs are particularly notable for their ability to enable the competitive utilization ofπ-conjugated structures within mesoporous configurations,making them valuable for investigations across various domains.They have shown considerable promise in addressing fuel and environmental challenges,demonstrated by their exceptional performance in applications such as vapor adsorption,heterogeneous catalysis,light emission,light harvesting,and energy generation.This review examines the chemical engineering principles underlying CMPs,including synthesis approaches,systemic research advancements,multifunctional investigations boundaries,potential applications,and progress in synthesis,dimensionality,and morphology studies.Specifically,it offers a comparative analysis of CMPs and linear polymeric materials,aiding in the development of functional polymers.Furthermore,this review explores the primary fundamental limitations of CMPs in fuel-related domains and discusses alternative strategies,including novel synthesis methods incorporating interactions and morphologies,to address these challenges.Ultimately,this assessment aims to provide a valuable and inspiring resource for professionals in the field of fuel management,guiding future research and development efforts.
基金supported by the National Natural Science Foundation of China(No.52433009)the Fundamental Research Funds for the Central Universities(No.GK202501005)the State Key Laboratory of Polymer Science and Technology(No.PST-KF2025-07)。
文摘The scalable fabrication of stretchable conjugated polymer films via solution printing is essential for their practical application in largearea wearable electronics.However,the printed conjugated polymer films typically exhibit high crystallinity,limiting their mechanical deformability.Herein,we propose a plasticizer-assisted printing strategy to simultaneously enhance the stretchability and electrical performance of films based on the conjugated polymer poly(3-(5-(5-methylselenophen-2-yl)thiophen-2-yl)-6-(5-methylthiophen-2-yl)-2,5-bis(4-octyltetradecyl)-2,5-dihydropyrrolo[3,4-c]pyrrole-1,4-dione)(P(TDPP-Se)).The incorporation of a plasticizer trioctyl trimellitate(TOTM)promotes P(TDPP-Se)aggregation in initial solution,facilitates chain alignment under flow field,and shorten solidification process,thereby restricting randomly polymer crystallization.Consequently,a low-crystallinity film with favorable edge-on orientation,strong chain alignment and improved chain dynamics is realized,which effectively alleviates crystallites fragmentation and crack propagation under large strain.The TOTM-plasticized film exhibits approximately 2-fold improvements in fracture strain and charge mobility,along with superior mobility retention under 100%strain in comparison to the neat film.This study provides a feasible approach for microstructure control in printed stretchable conjugated polymer film.
基金supported by the National Natural Science Foundation of China(Nos.22275182,22075272,51973211,51833009,21674111 and 52261135541)the Ministry of Science and Technology of the People’s Republic of China(the National Key R&D Program of China,No.2022YFB4200400)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0520102)。
文摘Pure organic room-temperature phosphorescent(RTP)polymers possess good processability and flexibility over small molecular crystals.However,most of RTP polymers reported so far are based on non-conjugated polymers,and achieving efficient phosphorescent emission in RTP conjugated polymers(CPs)remains a significant challenge.Herein,we developed two RTP CPs(P(PSe ZPh-p-Ph)and P(PSe ZPh-m-Ph))by linking the phenoselenazine units with the para-and meta-phenylene units,respectively,to form the conjugated main chains.The phenylene linker with different lingking mode manipulates the effictiveπ-conjugation of the polymer backbones.Comparing with the para-linked P(PSe ZPh-pPh),meta-linked P(PSe ZPh-m-Ph)exhibit the decreased effectiveπ-conjugation and the enhanced contribution of selenium atoms to the frontier orbitals,leading to the larger spin-orbit coupling(SOC)constants and the accelerated phosphorescence radiative decay process.The P(PSe ZPhm-Ph)achieves a phosphorescence quantum yield of 21.4%in doped polystyrene films,which is among the highest efficiencies reported to date for pure organic RTP CPs.These CPs are applied to construct phosphorescent film sensors for oxygen detection with the high quenching constants(K_(sv))up to 14.80 kPa^(-1)and low detection of limit of 0.84 ppm,demostrating the potential for application in oxygen film sensors.
基金supported by the National Key R&D Program of China(Nos.2023YFC3404200,2023YFC34042012023YFC3404202)+1 种基金the National Natural Science Foundation of China(No.22575253)the Beijing Natural Science Foundation(No.Z220025)。
文摘The development of synthetic hybrid biological systems integrating photosynthetic organisms with organic-abiotic functional materials holds significant promise for enhancing photosynthetic processes.The artificial regulation of the state transition between photosystem I(PSI)and photosystem II(PSII)represents a strategic and promising approach for improving the efficiency of natural photosynthesis.In this study,we demonstrate that poly(benzimidazolium-phenylthiophene)(CP4)featuring a flexible cationic backbone exhibits superior ultraviolet light-harvesting capability.The polymer CP4 enhanced PSI activity in Chlorella pyrenoidosa(C.pyrenoidosa),subsequently promoting PSII activity and augmenting overall photosynthetic performance.During light-dependent reactions,CP4 significantly accelerated photosynthetic electron transfer,resulting in a 330%increase in the production of oxygen and 93%and 96%increases in the ATP and NADPH contents,respectively.In the context of dark reactions,CP4 facilitated the conversion and utilization of light energy,leading to a 6%increase in both carbohydrate and protein contents.These findings indicate that synthetic light-harvesting polymer materials exhibit considerable application potential in the field of biomass production through enhancement of natural photosynthetic efficiency.
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.
文摘Breast cancer is a heterogeneous disease stratified by hormone receptors(HRs)and human epidermal growth factor receptor 2(HER2)status and each subtype has divergent therapeutic needs.Despite the current therapeutic advances,resistance to standard therapies remains pervasive,underscoring the demand for novel strategies.Antibody-drug conjugates(ADCs)offer a powerful strategy by combining tumor-specific antibodies to potent cytotoxins,enabling selective delivery and minimizing off-target toxicity1.TROP2,a transmembrane glycoprotein broadly overexpressed in breast cancer,has emerged as a promising ADC target.The approval of datopotamab deruxtecan(Dato-DXd)with sacituzumab govitecan(SG)and the incorporation of these ADCs into the National Comprehensive Cancer Network(NCCN)guidelines(v2.2025)highlight the fast penetration of TROP2 ADCs into clinical practice2.This editorial provides timely insights into optimizing TROP2-targeted strategies to improve outcomes across breast cancer subtypes.
文摘Objectives:B-cell maturation antigen(BCMA)-targeted antibody–drug conjugates(ADCs)have emerged as promising therapies for relapsed/refractory multiple myeloma(RRMM),but the overall efficacy and safety profile is unclear.This study aimed to synthesize the available evidence on the safety and efficacy of BCMA-ADCs in development for RRMM.Methods:A systematic search was conducted using six bibliographic databases and ClinicalTrials.gov up to November 2024.Studies were eligible if they were human clinical trials or animal studies evaluating BCMA-ADCs and reported efficacy and safety outcomes.Data extraction and quality assessments were conducted using validated tools,including ROBINS-I and SYRCLE’s risk of bias tool.Results:A total of 21 studies were included:16 clinical trials and five animal studies.Key findings included that belantamab mafodotin demonstrated variable but generally durable response rates(32%–85%)and a broad range of progression-free survival(PFS)(2.8–36.6 months),albeit with ocular toxicities in 51%–96%.Among newer candidates,MEDI2228 showed median PFS 5.1–6.6 months with 14%discontinuation for ocular symptoms,while AMG 224 had an overall response rate(ORR)of 23%(9/40)with anemia 21%,thrombocytopenia 24%,and ocular adverse events(AEs)21%.Animal studies supported the tumor-eradicating potential of all BCMA-ADC candidates,although safety signals such as hepatic and renal toxicity were noted with HDP-101.The risk of bias assessment revealed generally moderate to serious concerns in human trials,while the overall quality of the animal studies was acceptable.Conclusions:BCMA-targeted ADC candidates show encouraging efficacy in RRMM,particularly belantamab mafodotin.However,frequent AEs,especially ocular and hematologic toxicities,underscore the need for optimization in ADC design.Further research should prioritize enhancing safety while maintaining clinical benefit.
基金supported by the National Natural Science Foundation of China(61904053,22279033)the National Key Research and Development Program of China(2023YFB4204502)+2 种基金the 111 Project(B16016)the Fundamental Research Funds for the Central Universities(2025MS043)the Special Foundation for Carbon Peak Carbon Neutralization Technology Innovation Program of Jiangsu Province(BE2022026).
文摘Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended conjugation is designed and synthesized,named NaPh-4PACz.Compared to Ph-4PACz,NaPh-4PACz exhibits a larger adsorption energy with the ITO substrate,enabling the formation of a more uniform and dense film,thereby preventing direct contact between the perovskite and ITO.Additionally,NaPh-4PACz also has a stronger interaction with the perovskite,which can reduce buried interface defects and suppress non-radiative recombination.Consequently,NaPh-4PACz-based devices achieved a power conversion efficiency of 25.48%due to their interfacial“adhesive”ability.Importantly,the stability of the NaPh-4PACz-based devices was significantly improved.
基金supports from the National Natural Science Foundation of China(22375220,U2001214,22471302)the Guangdong Basic and Applied Basic Research Foundation(2024B1515020101)Open Project Fund from State Key Laboratory of Optoelectronic Materials and Technologies(OEMT-2024-KF-08).
文摘Formamidinium lead iodide(FAPbI_(3))perovskite exhibits an impressive X-ray absorption coefficient and a large carrier mobility-lifetime product(μτ),making it as a highly promising candidate for X-ray detection application.However,the presence of larger FA^(+)cation induces to an expansion of the Pb-I octahedral framework,which unfortunately affects both the stability and charge carrier mobility of the corresponding devices.To address this challenge,we develop a novel low-dimensional(HtrzT)PbI_(3) perovskite featuring a conjugated organic cation(1H-1,2,4-Triazole-3-thiol,HtrzT^(+))which matches well with theα-FAPbI_(3) lattices in two-dimensional plane.Benefiting from the matched lattice between(HtrzT)PbI_(3) andα-FAPbI_(3),the anchored lattice enhances the Pb-I bond strength and effectively mitigates the inherent tensile strain of theα-FAPbI_(3) crystal lattice.The X-ray detector based on(HtrzT)PbI_(3)(1.0)/FAPbI_(3) device achieves a remarkable sensitivity up to 1.83×10^(5)μC Gy_(air)^(−1) cm^(−2),along with a low detection limit of 27.6 nGy_(air) s^(−1),attributed to the release of residual stress,and the enhancement in carrier mobility-lifetime product.Furthermore,the detector exhibits outstanding stability under X-ray irradiation with tolerating doses equivalent to nearly 1.17×10^(6) chest imaging doses.
基金Supported by the Science and Technology Project of Guangxi(Guike AD23023002)。
文摘In this paper,we propose a three-term conjugate gradient method for solving unconstrained optimization problems based on the Hestenes-Stiefel(HS)conjugate gradient method and Polak-Ribiere-Polyak(PRP)conjugate gradient method.Under the condition of standard Wolfe line search,the proposed search direction is the descent direction.For general nonlinear functions,the method is globally convergent.Finally,numerical results show that the proposed method is efficient.
基金supported by the National Natural Science Foundation of China(Nos.22375031,22202037,22472023)the Fundamental Research Funds for the Central Universities(Nos.2412023YQ001,2412023QD019,2412024QD014)+1 种基金supported by grants from the seventh batch of Jilin Province Youth Science and Technology Talent Lifting Project(No.QT202305)Science and Technology Development Plan Project of Jilin Province,China(No.20240101192JC)。
文摘The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.
基金supported by the Shaanxi Province Technological Innovation Guidance Special(No.2022QFY08-01)the National Key Research and Development Program of China(No.2021YFB3200702)+5 种基金Natural Science Foundation of China(Nos.22201228,22205172,52203240 and 22175138)China Postdoctoral Science Foundation(Nos.2022M712530,2023T160506,and 2022M712497)Fundamental Research Funds for the Central Universities(No.xzy012022017)Young Talent Fund of Association for Science and Technology in Shaanxi(No.20230624)Shaanxi Province Postdoctoral Science Foundation(No.2023b SHTBZZ04)the Youth Innovation Team of Shaanxi Universities。
文摘π-Conjugated donor-acceptor-donor-acceptor-donor(D-A-D-A-D)type pyrenoviologens(PyV^(2+)),with the 2,7 positions of pyrene serving as connection bridges,were synthesized through SN2 reactions.Specifically,pyrenoviologen 3c was modified with a methylnaphthalene group,while 3a and 3b were modified with methyl and benzyl groups,respectively,for comparison.These pyrenoviologens exhibit reversible redox properties and strong fluorescence emission.Electrochromic devices(ECDs)were prepared using pyrenoviologens as the active materials.Notably,naphthalene-containing pyrenoviologen 3c,with its DA-D-A-D conjugated structure,possesses more stable free radicals,enabling it to maintain the radical color for a longer duration after power loss.A series of color-changing devices were successfully assembled.Due to the strong fluorescence of pyrenoviologens and the unique electron transfer effect between them and picric acid(PA),a sensor film with good selectivity and high sensitivity for PA in aqueous solution was prepared using pyrenoviologens as the fluorescent probe.Specifically,3c exhibited the highest sensitivity to PA due to its lowest energy gap.The introduction of the D-A-D-A-D structure is a strategic approach to enhancing photoelectric performance and broadening the application of viologens.
基金supported by the National Nature Science Foundation of China(Nos.62075079,62305127,61975200)the Natural Science Foundation of Jilin Province(20230508135RC)the Science and Technology Development Foundation of Changchun City(23GZZ15).
文摘The fluorescence imaging (FLI) in the second near-infrared window (NIR-II, 1000–1700nm) has attracted considerable attention in the past decade. In contrast to conventional NIR-I window excitation (808nm/980nm), FLI with NIR-II window excitation (1064nm/other wavelength beyond 1000nm) can afford deeper tissue penetration depth with high clarity due to the merits of suppressed photon scattering and diminished autofluorescence. In this review, we have summarized NIR-II window excitable/emissive organic/polymeric fluorophores recently developed. The characteristics of these fluorophores such as chemical structures and photophysical properties have also been critically discussed. Furthermore, the latest development of noninvasive in vivo FLI with NIR-II excitation was highlighted. The ideal imaging results emphasized the importance of NIR-II excitation of these fluorophores in enabling deep tissue penetration and high-resolution imaging. Finally, a perspective on the challenges and prospects of NIR-II excitable/emissive organic/polymeric fluorophores was also discussed. We expected this review will be served as a source of inspiration for researchers, stimulating the creation of novel NIR-II excitable fluorophores and fostering the development of bioimaging applications.
基金supported by the Beijing Natural Science Foundation(Grant No.L244024)National Natural Science Foundation of China(Grant Nos.82172604 and 82473199)CSCO Clinical Oncology Research Foundation(Grant No.Y-2022HER2AZMS-0258).
文摘Urothelial carcinoma(UC)is the 9th most common and the 13th most deadly cancer worldwide1.Despite the availability of platinum-based chemotherapy and immune checkpoint inhib-itors(ICIs),the 5-year survival rate of patients with metastatic UC(mUC)remains poor(10-15%)2.
基金Research Foundation for Advanced Talents of East China University of Technology,Grant/Award Number:DHBK201927Excellent Youth Foundation of Jiangxi Scientific Committee,Grant/Award Number:20232ACB213012+2 种基金National Science Foundation for Young Scientists of China,Grant/Award Number:21905122National Science Foundation for Young Scientists,Grant/Award Number:21905147Jiangxi Talent Program,Grant/Award Number:DHSQT32022005.
文摘Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we report the design of four novel metal-salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO_(2)with gaseous water.Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks,they show a maximum CO_(2)adsorption capacity of 46.1 cm3 g^(−1)and adsorption selectivity for CO_(2)/N_(2)of up to 82 at 273 K.Under air atmosphere and simulated solar light(100mWcm^(−2)),TEPT-Zn shows an excellent CO yield of 304.96μmol h^(−1)g^(−1)with a selectivity of approximately 100%,which represents one of the best results in terms of organic photocatalysts for gas-phase CO_(2)photoreduction so far.Furthermore,only small degradation in the CO yield is observed even after 120-h continuous illumination.More importantly,a good CO yield of 152.52μmol g^(−1)was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h(25-28℃,52.3±7.9mWcm^(−2)).This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO_(2)from air.
基金financial supports from the Natural Science Foundation of Shandong Province(ZR2021ME037)the National Natural Science Foundation of China(52472259,22179051 and 61604143)+2 种基金the National Key Research and Development Program of China(2021YFE0111000)the Special Fund of Taishan Scholar Program of Shandong Province(tsqnz20221141)the Foundation of Key Laboratory of Advanced Technique&Preparation for Renewable Energy Materials,Ministry of Education,Yunnan Normal University(OF2022-02)。
文摘A comprehensive understanding of the relevance between molecular structure and passivation ability to screen efficient modifiers is essential for enhancing the performance of perovskite solar cells(PSCs).Here,three similarπ-πstacking molecules namely benzophenone(BPN),diphenyl sulfone(DPS),and diphenyl sulfoxide(DPSO)are used as back-interface modifiers in carbon-based CsPbBr_(3)PSCs.After investigation,the results demonstrate the positive effect of the p-πconjugation characteristic inπ-πstacking molecules on maximizing their passivation ability.The p-πco njugation of DPSO enables a higher coordinative activity of oxygen atom in its S=O group than that in 0=S=O group of DPS and C=O group of BPN,which gives a superior passivation effect of DPSO on defects of perovskite films.The modification of DPSO also significantly improves the p-type behavior of perovskite films and the back-interfacial energetics matching,inducing an increase of hole extraction and a decrease of energy loss.Finally,the unencapsulated carbon-based CsPbBr_(3)PSCs with DPSO achieve a maximum power conversion efficiency of 10.60%and outstanding long-term stability in high-temperature,high-humidity(85℃,85%relative humidity)air environment.This work provides insights into the influence of the structure ofπ-πstacking molecules on their ability to improve the perovskite films quality and therefore the PSCs performance.
