Alkaline phosphatase(ALP) activity assay is not only significant to the clinical diagnosis of some related disease, but also momentous to the construction of ALP-based enzyme-linked immunosorbent assay(ELISA). Herein,...Alkaline phosphatase(ALP) activity assay is not only significant to the clinical diagnosis of some related disease, but also momentous to the construction of ALP-based enzyme-linked immunosorbent assay(ELISA). Herein, for the first time, we have discovered that ascorbic acid(AA) can specially react with N-methylethylenediamine(N-MEDA) to generate fluorescent non-conjugated polymer dots(NCPDs) under mild conditions. On the basis of the AA-responsive emission and ALP-catalyzed hydrolysis of ascorbic acid 2-phosphate(AA2P) to AA, we have exploited a fluorometric ALP activity assay with high sensitivity and selectivity. Furthermore, by means of conventional ALP-based ELISA platform, a conceptual fluorescent ELISA has been constructed and applied in the potential clinical diagnosis, during which cardiac troponin I(cTnI), a well-established biomarker of acute myocardial infarction, has been chosen as the model target. We envision that such original fluorescent NCPDs generation-enabled ELISA could become a versatile tool in biochemical sensing and medical diagnosis in the future.展开更多
Polymer dielectrics capable of operating efficiently at high electric fields and elevated temperatures are urgently demanded by next-generation electronics and electrical power systems.While inorganic fillers have bee...Polymer dielectrics capable of operating efficiently at high electric fields and elevated temperatures are urgently demanded by next-generation electronics and electrical power systems.While inorganic fillers have been extensively utilized to improved high-temperature capacitive performance of dielectric polymers,the presence of thermodynamically incompatible organic and inorganic components may lead to concern about the long-term stability and also complicate film processing.Herein,zero-dimensional polymer dots with high electron affinity are introduced into photoactive allyl-containing poly(aryl ether sulfone)to form the all-organic polymer composites for hightemperature capacitive energy storage.Upon ultraviolet irradiation,the crosslinked polymer composites with polymer dots are efficient in suppressing electrical conduction at high electric fields and elevated temperatures,which significantly reduces the high-field energy loss of the composites at 200℃.Accordingly,the ultraviolet-irradiated composite film exhibits a discharged energy density of 4.2 J cm^(−3)at 200℃.Along with outstanding cyclic stability of capacitive performance at 200℃,this work provides a promising class of dielectric materials for robust high-performance all-organic dielectric nanocomposites.展开更多
For efficient colloidal quantum dot(CQD)solar cells(CQD-SCs),thiol-passivated p-type CQDs are generally used as a hole-transporting material(HTM);however,there are issues with the control of optoelectrical properties,...For efficient colloidal quantum dot(CQD)solar cells(CQD-SCs),thiol-passivated p-type CQDs are generally used as a hole-transporting material(HTM);however,there are issues with the control of optoelectrical properties,low thiol passivation rate,and poor morphology with a power conversion efficiency(PCE)of approximately 11%.Although polymeric HTMs have been introduced to address these issues,maximizing efficiency and achieving green-solvent processability and thermal stability for commercialization is necessary.Here,we synthesize a novel benzodifuran(BDF)-based HTM(asy-ranPBTBDF)showing an electron-deficient state,low steric hindrance,and low planarity compared to those of a typical benzodithiophene(BDT)-based HTM(asy-ranPBTBDT).BDF properties lead to deep high occupied molecular orbital(HOMO)levels,closeπ-πstacking,excellent solubility,and amorphous properties related to efficiency,green-solvent processability,and thermal stability.With these benefits,the asy-ranPBTBDF-based CQD-SC showed enhanced open-circuit voltage(Voc)(0.65 V)and PCE(13.29%)compared to those of the asy-ranPBTBDT-based device(0.63 V and 12.22%)in toxic processes with chlorobenzene.The asy-ranPBTBDF-based CQD-SC showed a PCE of 12.51%in a green-solvent process with 2-methylanisole and improved thermal stability at 80℃(83.8%retaining after 24 h)owing to less lateral crystallization than the asy-ranPBTBDT-based device(60.8%retaining after 24 h).展开更多
Two non-conjugated polymers PEIE-DBO and PEIE-DCO, prepared by quaternization of polyethyleneimine ethoxylate by 1,8-dibromooctane and 1,8-dichlorooctane respectively, are developed as electron transport layer(ETL) in...Two non-conjugated polymers PEIE-DBO and PEIE-DCO, prepared by quaternization of polyethyleneimine ethoxylate by 1,8-dibromooctane and 1,8-dichlorooctane respectively, are developed as electron transport layer(ETL) in high-performance inverted organic solar cells(OSCs), and the effects of halide ions on polymeric photoelectric performance are fully investigated. PEIE-DBO possesses higher electron mobility(3.68×10-4 cm2 V-1s-1), higher conductivity and more efficient exciton dissociation and electron extraction, attributed to its lower work function(3.94 eV) than that of PEIE-DCO, which results in better photovoltaic performance in OSCs. The inverted OSCs with PTB7-Th: PC71BM as photoactive layer and PEIE-DBO as ETL exhibit higher PCE of 10.52%, 9.45% and 9.09% at the thickness of 9, 35 and 50 nm,respectively. To our knowledge, PEIE-DBO possesses the best thickness-insensitive performance in polymeric ETLs of inverted fullerene-based OSCs. Furthermore, PEIE-DBO was used to fabricate the inverted non-fullerene OSCs(PM6:Y6) and obtained a high PCE of 15.74%, which indicates that PEIE-DBO is effective both in fullerene-based OSCs and fullerene-free OSCs.展开更多
Herein, two nanoparticles with different dimensions, spherical carbon dots (C-dots) and sheetlike hectorite clay, were used as physical crosslinkers to fabricate C-dots-clay-poly(N-isopropylacrylamide)nanocompositehyd...Herein, two nanoparticles with different dimensions, spherical carbon dots (C-dots) and sheetlike hectorite clay, were used as physical crosslinkers to fabricate C-dots-clay-poly(N-isopropylacrylamide)nanocompositehydrogels (coded as C-dots-clay-PNIPAm hydrogels). The mechanical properties, fluorescence features and thermal-responsive properties of the C-dots-clay-PNIPAm hydrogels were evaluated. The experimental results indicate that synergistic effects of C-dots and hectorite clay nanoparticles are able to significantly enhance mechanical properties of the hydrogels. The hydrogels can be stretched up to 1730%with strength as high as 250 kPa when the C-dots concentration is 0.1wt%and the clay concentration is 6wt%. The hydrogels exhibit complete self-healing through autonomic reconstruction of crosslinked network a damaged interface. The hydrogels show favorable thermal-responsive properties with the volume phase transition around 34℃. In addition, the hydrogels are endowed with fluorescence features that are associated with C-dots in the hydrogels. It can be expected that the as-fabricated C-dots-clay-PNIPAm hydrogels are promising for applications in sensors, biomedical carriers and tissue engineering.展开更多
We synthesized C60 quantum dots(QDs) with a uniform size by a modified ultrasonic process and studied its polymerization under high pressure and high temperature(HPHT).Raman spectra showed that a phase assemblage of a...We synthesized C60 quantum dots(QDs) with a uniform size by a modified ultrasonic process and studied its polymerization under high pressure and high temperature(HPHT).Raman spectra showed that a phase assemblage of a dimer(D) phase(62 vol%) and a one-dimensional chain orthorhombic(O) phase(38 vol%) was obtained at 1.5 GPa and 300℃.At 2.0 GPa and 430℃,the proportion of the O phase increased to 46 vol%,while the corresponding D phase decreased to 54 vol%.Compared with bulk and nanosized C60,C60 QDs cannot easily form a high-dimensional polymeric structure.This fact is probably caused by the small particle size,orientation of the disordered structure of C60 QDs,and the barrier of oxide function groups between C60 molecules.Our studies enhance the understanding of the polymerization behavior of low-dimension C60 nanomaterials under HPHT conditions.展开更多
Photodynamic therapy(PDT)is a new and rapidly developing treatment modality for dinical cancer therapy.Semiconductor polymer dots(Pdots)doped with photosensitizers have been successfully applied to PDT,and have made p...Photodynamic therapy(PDT)is a new and rapidly developing treatment modality for dinical cancer therapy.Semiconductor polymer dots(Pdots)doped with photosensitizers have been successfully applied to PDT,and have made progress in the field of tumor therapy.However,the problems of severe photosensitivity and limited tisue penetration depth are needed to be solved during the implementation process of PDT.Here we developed the Pdots doped with photosensitizer molecule Chlorin e6(Ce6)and photochromic molecule 1,2-bis(2,4-dimethy1-5 phenyl-3-thiophene)-3,3,4,5-hexafuoro-1-cyclopentene(BTE)to construct a photoswitchable nanoplatform for PDT.The Ce6-BTE-doped Pdots were in the green region,and the tissue penetration depth was increased compared with most Pdots in the blue region.The reversible conversion of BTE under different light irradiation was utilized to regulate the photodynamic effect and solve the problem of photosensitivity.The prepared Ce6-BTE-doped Pdots had small size,excellent optical property,efficient ROS generation and good photoswitchable ability.The cellular uptake,cytotoxicity,and photodynamic effect of the Pdots were detected in human colon tumor cells.The experiments in vitro indicated that Ce6-BTE-doped Pdots could exert excellent photodynamic effect in ON state and reduce photosensitivity in OFF state.These results demonstrated that this nanoplatform holds the potential to be used in clinical PDT.展开更多
Thermochromic smart windows have gained increasing popularity in light modulation and energy management in buildings.However,the fabrication of flexible thermochromic smart windows with high luminous transmittance(Tlu...Thermochromic smart windows have gained increasing popularity in light modulation and energy management in buildings.However,the fabrication of flexible thermochromic smart windows with high luminous transmittance(Tlum),tailorable critical temperature(τc),strong solar modulation ability(ΔTsol),and long-term durability remains a huge challenge.In this study,hydrogel-based thermochromic smart windows are fabricated by sandwiching thermochromic hydrogels of polyallylamine hydrochloride,polyacrylic acid,and carbonized polymer dots(CPDs)complexes between two pieces of transparent substrates.Benefiting from the incorporation of nanosized CPDs,the thermochromic hydrogel has an ultrahigh Tlum of~98.7%,a desirableτc of~24.2℃,aΔTsol of~89.3%and a rapid transition time of~3 s from opaque state to transparent state.Moreover,the thermochromic hydrogel exhibits excellent anti-freezing ability,tight adhesion toward various substrates,and excellent self-healing capability.The self-healing capability enables the fabrication of large-area smart windows by welding multiple hydrogel pieces.The smart windows retain their original thermochromic properties after being stored under ambient conditions for at least 147 days or undergoing 10,000 uninterrupted heating/cooling cycles.The model houses with smart windows can achieve a temperature reduction of 9.2℃,demonstrating the excellent indoor temperature modulation performance of the smart windows.展开更多
Carbonized polymer dots(CPDs)as one type of carbon dots have attracted widespread attention in recent years.The proposal of the“shell–core”structure of CPDs leads to further thinking about the association between t...Carbonized polymer dots(CPDs)as one type of carbon dots have attracted widespread attention in recent years.The proposal of the“shell–core”structure of CPDs leads to further thinking about the association between their special structures and luminescent properties.In recent years,great progress has been made in the field of CPD-based room-temperature phosphorescent materials.This review pays particular attention to how the special“core–shell”structure of CPDs influences the activation of roomtemperature phosphorescence(RTP).The strategies and vital factors to activate RTP for CPD-based materials in both solid state and water were reviewed in detail to elaborate on the effect of the special structure on RTP generation.Furthermore,some perspectives on the current challenges were also provided to guide the further development of CPD-based room-temperature phosphorescent materials.展开更多
Antibiotics are a category of chemical compounds used to treat bacterial infections and are widely applied in cultivation,animal husbandry,aquaculture,and pharmacy.Currently,residual antibiotics and their metabolites ...Antibiotics are a category of chemical compounds used to treat bacterial infections and are widely applied in cultivation,animal husbandry,aquaculture,and pharmacy.Currently,residual antibiotics and their metabolites pose a potential risk of allergic reactions,bacterial resistance,and increased cancer incidence.Residual antibiotics and the resulting bacterial antibiotic resistance have been recognized as a global challenge that has attracted increasing attention.Therefore,monitoring antibiotics is a critical way to limit the ecological risks from antibiotic pollution.Accordingly,it is desirable to devise new analytical platforms to achieve efficient antibiotic detection with excellent sensitivity and specificity.Quantum dots(QDs)are regarded as an ideal material for use in the development of antibiotic detection biosensors.In this review,we characterize different types of QDs,such as silicon,chalcogenide,carbon,and other doped QDs,and summarize the trends in QD-based antibiotic detection.QD-based sensing applications are classified according to their recognition strategies,including molecularly imprinted polymers(MIPs),aptamers,and immunosensors.We discuss the advantages of QD-derived antibiotic sensors,including low cost,good sensitivity,excellent stability,and fast response,and illustrate the current challenges in this field.展开更多
In this work the enhanced molecularly imprinted optosensing material based on graphene oxide-quantum dots ( GO- QDs) was synthesized for highly selective and sensitive specific recognition of the target protein, bov...In this work the enhanced molecularly imprinted optosensing material based on graphene oxide-quantum dots ( GO- QDs) was synthesized for highly selective and sensitive specific recognition of the target protein, bovine serum albumin (BSA). Here, GO was introduced to enhance the efficiency of mass-transfer in recognition of target protein. Molecularly imprinted polymer coated GO-QDs using BSA as template (BMIP-coated GO-QDs ) exhibited a fast mass-transfer speed, which could be ascribed to the high volume of efficient surface area and high target recognition efficiency of the synthesized nanoscale device. Under optimal conditions, it was found that the BSA as target protein could remarkably quench the relative fluorescence intensity of BMIP- coated GO-QDs linearly in a concentration-dependent manner that was best described by a Stern-Volmer equation. The Ksv (Stern- Volmer constant) for template BSA was much higher than bovine hemoglobin (BHb) and lysozyme (Lyz), implying a highly selective recognition ability of the BMIP-coated GO-QDs to BSA. This enhanced fluorescent nanoscale device may provide opportunities to develop a system that is efficient and effective and has potential in the design of highly effective fluorescent receptor for recognition of target protein in Droteomics studies.展开更多
In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting m...In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting materials(HTMs) is still desired and meaningful. One simple and efficient way to achieve high performance dopant-free HTMs is to synthesize novel non-conjugated side-chain polymers via rational molecular design. In this work, N-(4-methoxyphenyl)-9,9-dimethyl-9H-fluoren-2-amine(FMeNPh) groups are introduced into the poly(N-vinylcarbazole)(PVK) side chains to afford two nonconjugated polymers PVCz-DFMeNPh and PVCz-FMeNPh as dopant-free HTMs in inverted quasi-2D PSCs. Benefited from the flexible properties of polyethylene backbone and excellent optoelectronic natures of FMeNPh side-chain groups, PVCz-DFMeNPh with more FMeNPh units exhibited excellent thermal stability, well-matched energy levels and improved charge mobility as compared to PTAA and PVCzFMeNPh. Moreover, the morphologies investigation of quasi-2D perovskite on PVCz-DFMeNPh shows more compact and homogeneous perovskite films than those on PTAA and PVCz-FMeNPh. As a result,the dopant-free PVCz-DFMeNPh based inverted quasi-2D PSCs deliver power conversion efficiency(PCE) up to 18.44% as well as negligible hysteresis and favorable long-term stability, which represents as excellent performance reported to date for inverted quasi-2D PSCs. The results demonstrate the great potentials of constructing non-conjugated side-chain polymer HTMs based on phenylfluorenamine-func tionalized PVK for the development of high efficient and stable inverted 3D or quasi-2D PSCs.展开更多
High-temperature polymer dielectrics with high energy density are urgently needed for capacitive energy storage fields.However,the huge conduction loss at elevated temperatures makes the capacitive performance of poly...High-temperature polymer dielectrics with high energy density are urgently needed for capacitive energy storage fields.However,the huge conduction loss at elevated temperatures makes the capacitive performance of polymers degrade sharply,limiting the application of them.Herein,the polymer dots(PDs)with high-electron-affinity were introduced into high-temperature polymers to prepare all-organic nanocomposite dielectrics by solution casting.It is found that polymer dots capture injected electrons via strong electrostatic attraction and impede charges transport and accumulation inside composites,thus reducing leakage current density and improving high-temperature energy storage performance.Consequently,the high-temperature capacitance performance of nanocomposites was improved significantly and reached over 2.5 times that of the pristine polymers,e.g.,the energy density of polyetherimide(PEI)/PD reached 3.24 J·cm^(-3)with excellent electrical fatigue reliability over 20,000 times.This work addresses the current problem of poor discharged energy density of polymer dielectrics at high temperatures with a simple and universal method.展开更多
Comprehensive Summary Currently,solid-state fluorescent carbonized polymer dots(CPDs)have attracted attention increasingly due to their applications for optoelectronic display.However,designing CPDs possessing solid-s...Comprehensive Summary Currently,solid-state fluorescent carbonized polymer dots(CPDs)have attracted attention increasingly due to their applications for optoelectronic display.However,designing CPDs possessing solid-state fluorescence and clarifying the fluorescence mechanism remain challenging.Herein,we initially synthesized a novel type of polythiophene derivatives CPDs,poly-4,4’-(thiophene-3,4-diyl)dibenzoic acid carbonized polymer dots(PDBA-CPDs)with solid-state fluorescence.Subsequently,the structural and optical characterization revealed that the solid-state fluorescence originated from the aggregation induced emission of the CPDs.In brief,in aggregation state,the remaining polymer structure groups on the surface of the CPDs overlapped and weakened the non-radiative transition,enhancing solid-state fluorescence emission.Thirdly,three polythiophene-derived CPDs were designed to further demonstrate the aggregation induced solid-state fluorescence mechanism.Finally,owing to their unique properties of solid-state fluorescence,the white LEDs(light emitting diodes)were fabricated with high color rendering index(CRI)of 82.7 and CIE coordinates of(0.37,0.39)using commercial 460 nm chip.展开更多
Three kinds of carbonized polymer dots(CPDs) synthesized via a one-pot process from ophenylenediamine(OPD), m-phenylenediamine(MPD) and p-phenylenediamine(PPD) exhibit excitationwavelength independent yellow, green an...Three kinds of carbonized polymer dots(CPDs) synthesized via a one-pot process from ophenylenediamine(OPD), m-phenylenediamine(MPD) and p-phenylenediamine(PPD) exhibit excitationwavelength independent yellow, green and red emissions, respectively. In sharp contrast, two kinds of CPDs prepared via a hydrothermal process from citric acid(CA) and diethylenetriamine(DETA) exhibit obvious excitation-wavelength dependent emissions. Through the characterization and comparison of the two types of CPDs, it is concretely revealed that the polymer structure types during the formation of CPDs can effectively control the fluorescence excitation-wavelength independence/dependence. The homogeneous polymer structures contained in CPDs contribute to excitation-wavelength independence, whereas random copolymer structures contribute to excitation-wavelength dependence. These studies are of great significance for further understanding the polymer structures and designing unique optical properties of CPDs.展开更多
Identification of lymph nodes(LNs)is critical for studies of the structure,the role in disease development,and the efficacy of disease treatment.Carbonized polymer dots(CPDs)are expected to be potential LNs-targeted i...Identification of lymph nodes(LNs)is critical for studies of the structure,the role in disease development,and the efficacy of disease treatment.Carbonized polymer dots(CPDs)are expected to be potential LNs-targeted imaging agents due to their excellent properties with special structure,better photoluminescence(PL)and great biocompatibility.Herein,a red/near infrared(NIR)emission CPDs(RCPDs)with one and two-photon bioimaging based on citric acid(CA)and benzoylurea(BU)are prepared.Notably,the RCPDs are capable of targeting LNs for imaging.Lymphocyte homing has been demonstrated to be the cellular mechanism of RCPDs target LNs imaging.This work has developed a new nanomaterial for targeted imaging of LNs,while the biological applications of CPDs have been expanded and deepened.展开更多
It is highly desired to accurately and selectively detect and image intracellular L-lysine and pH in biological systems because they could act as the biomarkers in certain abnormal conditions and may give us a warning...It is highly desired to accurately and selectively detect and image intracellular L-lysine and pH in biological systems because they could act as the biomarkers in certain abnormal conditions and may give us a warning of the occurrence of diseases.It has been attracted more focuses to design new ratiometric fluorescent probe for monitoring L-lysine and pH to improve detection accuracy.Carbonized polymer dots(CPDs),which possess carbon/polymer hybrid structure rather than pure carbon structure and constitute of a carbon core and large amounts of functional groups/polymer chains on the surface,rise up as a new type of fluorescent nanomaterials and especially display many advantages for bioanalysis.In this study,o-phenylenediamine(o-PD)and poly(styrene-co-maleic anhydride)(PSMA)are used as the precursors to synthesize the desired CPDs through one-step hydrothermal amide method.The prepared CPDs display two well-resolved fluorescence emission bands,i.e.,a very weak emission centered at 470 nm in blue region and a strong emission centered at 558 nm in yellow region.It is found that the two emissions are both responsive to L-lysine based on the surface passivation mechanism,whereas,only the yellow emission is responsive to pH due to the protonation/deprotonation process of the amino groups.Based on the different responsive behaviors,ratiometric detection and imaging of L-lysine and pH are achieved.The prepared ratiometric CPDs probe is successfully applied for L-lysine and pH sensing and imaging at two emission channels in live cell and zebrafish with satisfactory results.展开更多
Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ...Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ABT-TSA-CPDs)with an absolute photoluminescence quantum yield(PLQY)of 76%in solid state without matrix were synthesized.Through adjusting the reaction temperature and time,the PL centers were proved to be carbon core state and surface state associated to carbonyl group which was the source of strong fluorescence emission in solid state.The mechanism of the unique phenomenon of enhanced emission from ethanol solution(PLQY=7%)to powder(PLQY=76%)was investigated by analyzing the chemical properties and structures of o ABT-TSA-CPDs at different temperatures and o ABT-TSACPDs/PVC composites,and was confirmed as fixation of PL centers.展开更多
基金financial supports of the National Natural Science Foundation of China(Nos.22034006,21974132 and 21721003)the Youth Innovation Promotion Association,CAS(No.2018258)the Development Project of Science and Technology of Jilin Province,China(No.20200201091JC)。
文摘Alkaline phosphatase(ALP) activity assay is not only significant to the clinical diagnosis of some related disease, but also momentous to the construction of ALP-based enzyme-linked immunosorbent assay(ELISA). Herein, for the first time, we have discovered that ascorbic acid(AA) can specially react with N-methylethylenediamine(N-MEDA) to generate fluorescent non-conjugated polymer dots(NCPDs) under mild conditions. On the basis of the AA-responsive emission and ALP-catalyzed hydrolysis of ascorbic acid 2-phosphate(AA2P) to AA, we have exploited a fluorometric ALP activity assay with high sensitivity and selectivity. Furthermore, by means of conventional ALP-based ELISA platform, a conceptual fluorescent ELISA has been constructed and applied in the potential clinical diagnosis, during which cardiac troponin I(cTnI), a well-established biomarker of acute myocardial infarction, has been chosen as the model target. We envision that such original fluorescent NCPDs generation-enabled ELISA could become a versatile tool in biochemical sensing and medical diagnosis in the future.
基金the National Natural Science Foundation of China(No.51973080,92066104).
文摘Polymer dielectrics capable of operating efficiently at high electric fields and elevated temperatures are urgently demanded by next-generation electronics and electrical power systems.While inorganic fillers have been extensively utilized to improved high-temperature capacitive performance of dielectric polymers,the presence of thermodynamically incompatible organic and inorganic components may lead to concern about the long-term stability and also complicate film processing.Herein,zero-dimensional polymer dots with high electron affinity are introduced into photoactive allyl-containing poly(aryl ether sulfone)to form the all-organic polymer composites for hightemperature capacitive energy storage.Upon ultraviolet irradiation,the crosslinked polymer composites with polymer dots are efficient in suppressing electrical conduction at high electric fields and elevated temperatures,which significantly reduces the high-field energy loss of the composites at 200℃.Accordingly,the ultraviolet-irradiated composite film exhibits a discharged energy density of 4.2 J cm^(−3)at 200℃.Along with outstanding cyclic stability of capacitive performance at 200℃,this work provides a promising class of dielectric materials for robust high-performance all-organic dielectric nanocomposites.
基金supported by National Research Foundation of Korea(NRF)grant funded by Ministry of Science and ICT(MSIT)(2021R1A2C3004420,2021M3H4A1A02055684,and 2020R1C1C1012256)the DGIST R&D Program of the Ministry of Science and ICT(21-CoE-ET-01)Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(2021R1A6A3A14038599).
文摘For efficient colloidal quantum dot(CQD)solar cells(CQD-SCs),thiol-passivated p-type CQDs are generally used as a hole-transporting material(HTM);however,there are issues with the control of optoelectrical properties,low thiol passivation rate,and poor morphology with a power conversion efficiency(PCE)of approximately 11%.Although polymeric HTMs have been introduced to address these issues,maximizing efficiency and achieving green-solvent processability and thermal stability for commercialization is necessary.Here,we synthesize a novel benzodifuran(BDF)-based HTM(asy-ranPBTBDF)showing an electron-deficient state,low steric hindrance,and low planarity compared to those of a typical benzodithiophene(BDT)-based HTM(asy-ranPBTBDT).BDF properties lead to deep high occupied molecular orbital(HOMO)levels,closeπ-πstacking,excellent solubility,and amorphous properties related to efficiency,green-solvent processability,and thermal stability.With these benefits,the asy-ranPBTBDF-based CQD-SC showed enhanced open-circuit voltage(Voc)(0.65 V)and PCE(13.29%)compared to those of the asy-ranPBTBDT-based device(0.63 V and 12.22%)in toxic processes with chlorobenzene.The asy-ranPBTBDF-based CQD-SC showed a PCE of 12.51%in a green-solvent process with 2-methylanisole and improved thermal stability at 80℃(83.8%retaining after 24 h)owing to less lateral crystallization than the asy-ranPBTBDT-based device(60.8%retaining after 24 h).
基金the support from the National Natural Science Foundation of China (51873177, 51573153, 61564003 and 21875204)the group of Advanced Photoelectricity and Supermolecule Function Materials of Ministry of Education (IRT-17R90)+1 种基金the Hunan 2011 Collaborative Innovation Center of Chemical Engineering & Technology with Environmental Benignity and Effective Resource Utilizationsupport from Guangxi Bagui Scholar Program and Guangxi Natural Science Foundation (2015GXNSFGA139002)。
文摘Two non-conjugated polymers PEIE-DBO and PEIE-DCO, prepared by quaternization of polyethyleneimine ethoxylate by 1,8-dibromooctane and 1,8-dichlorooctane respectively, are developed as electron transport layer(ETL) in high-performance inverted organic solar cells(OSCs), and the effects of halide ions on polymeric photoelectric performance are fully investigated. PEIE-DBO possesses higher electron mobility(3.68×10-4 cm2 V-1s-1), higher conductivity and more efficient exciton dissociation and electron extraction, attributed to its lower work function(3.94 eV) than that of PEIE-DCO, which results in better photovoltaic performance in OSCs. The inverted OSCs with PTB7-Th: PC71BM as photoactive layer and PEIE-DBO as ETL exhibit higher PCE of 10.52%, 9.45% and 9.09% at the thickness of 9, 35 and 50 nm,respectively. To our knowledge, PEIE-DBO possesses the best thickness-insensitive performance in polymeric ETLs of inverted fullerene-based OSCs. Furthermore, PEIE-DBO was used to fabricate the inverted non-fullerene OSCs(PM6:Y6) and obtained a high PCE of 15.74%, which indicates that PEIE-DBO is effective both in fullerene-based OSCs and fullerene-free OSCs.
基金the National Natural Science Foundation of China(Nos.51873167 and 50803048)the 2018 National College Students Innovation and Entrepreneurship Training Program Project Funding(No.20181049701035)。
文摘Herein, two nanoparticles with different dimensions, spherical carbon dots (C-dots) and sheetlike hectorite clay, were used as physical crosslinkers to fabricate C-dots-clay-poly(N-isopropylacrylamide)nanocompositehydrogels (coded as C-dots-clay-PNIPAm hydrogels). The mechanical properties, fluorescence features and thermal-responsive properties of the C-dots-clay-PNIPAm hydrogels were evaluated. The experimental results indicate that synergistic effects of C-dots and hectorite clay nanoparticles are able to significantly enhance mechanical properties of the hydrogels. The hydrogels can be stretched up to 1730%with strength as high as 250 kPa when the C-dots concentration is 0.1wt%and the clay concentration is 6wt%. The hydrogels exhibit complete self-healing through autonomic reconstruction of crosslinked network a damaged interface. The hydrogels show favorable thermal-responsive properties with the volume phase transition around 34℃. In addition, the hydrogels are endowed with fluorescence features that are associated with C-dots in the hydrogels. It can be expected that the as-fabricated C-dots-clay-PNIPAm hydrogels are promising for applications in sensors, biomedical carriers and tissue engineering.
基金Project supported by the National Key R&D Program of China(Grant No.2018YFA0305900)the National Natural Science Foundation of China(Grant Nos.11634004 and 11404036)+2 种基金“the 13th Five-year”Planning Project of Jilin Provincial Education Department Foundation,China(Grant No.20190504)JLU Science and Technology Innovative Research Team,China(Grant No.2017TD-01)Natural Science Foundation of Chang-chun Normal University,China(Grant No.2014-001).
文摘We synthesized C60 quantum dots(QDs) with a uniform size by a modified ultrasonic process and studied its polymerization under high pressure and high temperature(HPHT).Raman spectra showed that a phase assemblage of a dimer(D) phase(62 vol%) and a one-dimensional chain orthorhombic(O) phase(38 vol%) was obtained at 1.5 GPa and 300℃.At 2.0 GPa and 430℃,the proportion of the O phase increased to 46 vol%,while the corresponding D phase decreased to 54 vol%.Compared with bulk and nanosized C60,C60 QDs cannot easily form a high-dimensional polymeric structure.This fact is probably caused by the small particle size,orientation of the disordered structure of C60 QDs,and the barrier of oxide function groups between C60 molecules.Our studies enhance the understanding of the polymerization behavior of low-dimension C60 nanomaterials under HPHT conditions.
基金supported by the science and technology research project of education department of Jilin province(JJKH20211189KJ)Jilin province medical and health talents special project.
文摘Photodynamic therapy(PDT)is a new and rapidly developing treatment modality for dinical cancer therapy.Semiconductor polymer dots(Pdots)doped with photosensitizers have been successfully applied to PDT,and have made progress in the field of tumor therapy.However,the problems of severe photosensitivity and limited tisue penetration depth are needed to be solved during the implementation process of PDT.Here we developed the Pdots doped with photosensitizer molecule Chlorin e6(Ce6)and photochromic molecule 1,2-bis(2,4-dimethy1-5 phenyl-3-thiophene)-3,3,4,5-hexafuoro-1-cyclopentene(BTE)to construct a photoswitchable nanoplatform for PDT.The Ce6-BTE-doped Pdots were in the green region,and the tissue penetration depth was increased compared with most Pdots in the blue region.The reversible conversion of BTE under different light irradiation was utilized to regulate the photodynamic effect and solve the problem of photosensitivity.The prepared Ce6-BTE-doped Pdots had small size,excellent optical property,efficient ROS generation and good photoswitchable ability.The cellular uptake,cytotoxicity,and photodynamic effect of the Pdots were detected in human colon tumor cells.The experiments in vitro indicated that Ce6-BTE-doped Pdots could exert excellent photodynamic effect in ON state and reduce photosensitivity in OFF state.These results demonstrated that this nanoplatform holds the potential to be used in clinical PDT.
基金supported by the National Natural Science Foundation of China (No.21935004).
文摘Thermochromic smart windows have gained increasing popularity in light modulation and energy management in buildings.However,the fabrication of flexible thermochromic smart windows with high luminous transmittance(Tlum),tailorable critical temperature(τc),strong solar modulation ability(ΔTsol),and long-term durability remains a huge challenge.In this study,hydrogel-based thermochromic smart windows are fabricated by sandwiching thermochromic hydrogels of polyallylamine hydrochloride,polyacrylic acid,and carbonized polymer dots(CPDs)complexes between two pieces of transparent substrates.Benefiting from the incorporation of nanosized CPDs,the thermochromic hydrogel has an ultrahigh Tlum of~98.7%,a desirableτc of~24.2℃,aΔTsol of~89.3%and a rapid transition time of~3 s from opaque state to transparent state.Moreover,the thermochromic hydrogel exhibits excellent anti-freezing ability,tight adhesion toward various substrates,and excellent self-healing capability.The self-healing capability enables the fabrication of large-area smart windows by welding multiple hydrogel pieces.The smart windows retain their original thermochromic properties after being stored under ambient conditions for at least 147 days or undergoing 10,000 uninterrupted heating/cooling cycles.The model houses with smart windows can achieve a temperature reduction of 9.2℃,demonstrating the excellent indoor temperature modulation performance of the smart windows.
基金supported by the National Science Foundation of China(NSFC)under grant no.22035001.
文摘Carbonized polymer dots(CPDs)as one type of carbon dots have attracted widespread attention in recent years.The proposal of the“shell–core”structure of CPDs leads to further thinking about the association between their special structures and luminescent properties.In recent years,great progress has been made in the field of CPD-based room-temperature phosphorescent materials.This review pays particular attention to how the special“core–shell”structure of CPDs influences the activation of roomtemperature phosphorescence(RTP).The strategies and vital factors to activate RTP for CPD-based materials in both solid state and water were reviewed in detail to elaborate on the effect of the special structure on RTP generation.Furthermore,some perspectives on the current challenges were also provided to guide the further development of CPD-based room-temperature phosphorescent materials.
基金supported by grants from the National Key Research and Development Project(Project No.:2019YFC1605800)the National Natural Science Foundation of China(Grant Nos.:22006070 and 82103816)+2 种基金the Natural Science Foundation of Jiangsu Province(Grant Nos.:BK20200715,BK20200718,and BK20210538)the Natural Science Foundation of Jiangsu Higher Education Institutions,China(Grant No.:20KJB350010)the Natural Science Fund for Colleges and Universities in Jiangsu Province(Grant No.:19KJB530011).
文摘Antibiotics are a category of chemical compounds used to treat bacterial infections and are widely applied in cultivation,animal husbandry,aquaculture,and pharmacy.Currently,residual antibiotics and their metabolites pose a potential risk of allergic reactions,bacterial resistance,and increased cancer incidence.Residual antibiotics and the resulting bacterial antibiotic resistance have been recognized as a global challenge that has attracted increasing attention.Therefore,monitoring antibiotics is a critical way to limit the ecological risks from antibiotic pollution.Accordingly,it is desirable to devise new analytical platforms to achieve efficient antibiotic detection with excellent sensitivity and specificity.Quantum dots(QDs)are regarded as an ideal material for use in the development of antibiotic detection biosensors.In this review,we characterize different types of QDs,such as silicon,chalcogenide,carbon,and other doped QDs,and summarize the trends in QD-based antibiotic detection.QD-based sensing applications are classified according to their recognition strategies,including molecularly imprinted polymers(MIPs),aptamers,and immunosensors.We discuss the advantages of QD-derived antibiotic sensors,including low cost,good sensitivity,excellent stability,and fast response,and illustrate the current challenges in this field.
文摘In this work the enhanced molecularly imprinted optosensing material based on graphene oxide-quantum dots ( GO- QDs) was synthesized for highly selective and sensitive specific recognition of the target protein, bovine serum albumin (BSA). Here, GO was introduced to enhance the efficiency of mass-transfer in recognition of target protein. Molecularly imprinted polymer coated GO-QDs using BSA as template (BMIP-coated GO-QDs ) exhibited a fast mass-transfer speed, which could be ascribed to the high volume of efficient surface area and high target recognition efficiency of the synthesized nanoscale device. Under optimal conditions, it was found that the BSA as target protein could remarkably quench the relative fluorescence intensity of BMIP- coated GO-QDs linearly in a concentration-dependent manner that was best described by a Stern-Volmer equation. The Ksv (Stern- Volmer constant) for template BSA was much higher than bovine hemoglobin (BHb) and lysozyme (Lyz), implying a highly selective recognition ability of the BMIP-coated GO-QDs to BSA. This enhanced fluorescent nanoscale device may provide opportunities to develop a system that is efficient and effective and has potential in the design of highly effective fluorescent receptor for recognition of target protein in Droteomics studies.
基金financially supported by the National Key Research and Development Program of China (2018YFB0406704)the National Natural Science Foundation of China (61974066, 61725502, 61634001)+3 种基金the Major Research Plan of the National Natural Science Foundation of China (91733302)the fund for Talented of Nanjing Tech University (201983)the Major Program of Natural Science Research of Jiangsu Higher Education Institutions of China (18KJA510002)the Synergetic Innovation Center for Organic Electronics and Information Displays。
文摘In order to improve the efficiency and stability of inverted three-dimensional(3D) or quasi-2D perovskite solar cells(PSCs) for future commercialization, exploring high efficient dopant-free polymer holetransporting materials(HTMs) is still desired and meaningful. One simple and efficient way to achieve high performance dopant-free HTMs is to synthesize novel non-conjugated side-chain polymers via rational molecular design. In this work, N-(4-methoxyphenyl)-9,9-dimethyl-9H-fluoren-2-amine(FMeNPh) groups are introduced into the poly(N-vinylcarbazole)(PVK) side chains to afford two nonconjugated polymers PVCz-DFMeNPh and PVCz-FMeNPh as dopant-free HTMs in inverted quasi-2D PSCs. Benefited from the flexible properties of polyethylene backbone and excellent optoelectronic natures of FMeNPh side-chain groups, PVCz-DFMeNPh with more FMeNPh units exhibited excellent thermal stability, well-matched energy levels and improved charge mobility as compared to PTAA and PVCzFMeNPh. Moreover, the morphologies investigation of quasi-2D perovskite on PVCz-DFMeNPh shows more compact and homogeneous perovskite films than those on PTAA and PVCz-FMeNPh. As a result,the dopant-free PVCz-DFMeNPh based inverted quasi-2D PSCs deliver power conversion efficiency(PCE) up to 18.44% as well as negligible hysteresis and favorable long-term stability, which represents as excellent performance reported to date for inverted quasi-2D PSCs. The results demonstrate the great potentials of constructing non-conjugated side-chain polymer HTMs based on phenylfluorenamine-func tionalized PVK for the development of high efficient and stable inverted 3D or quasi-2D PSCs.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51973080,92066104,and 52003099)Natural Science Foundation of Jilin Province(No.YDZJ202101ZYTS002)Capital Construction Fund of Jilin Province(No.2021C039-1).
文摘High-temperature polymer dielectrics with high energy density are urgently needed for capacitive energy storage fields.However,the huge conduction loss at elevated temperatures makes the capacitive performance of polymers degrade sharply,limiting the application of them.Herein,the polymer dots(PDs)with high-electron-affinity were introduced into high-temperature polymers to prepare all-organic nanocomposite dielectrics by solution casting.It is found that polymer dots capture injected electrons via strong electrostatic attraction and impede charges transport and accumulation inside composites,thus reducing leakage current density and improving high-temperature energy storage performance.Consequently,the high-temperature capacitance performance of nanocomposites was improved significantly and reached over 2.5 times that of the pristine polymers,e.g.,the energy density of polyetherimide(PEI)/PD reached 3.24 J·cm^(-3)with excellent electrical fatigue reliability over 20,000 times.This work addresses the current problem of poor discharged energy density of polymer dielectrics at high temperatures with a simple and universal method.
基金the National Natural Science Foundation of China(Grant Nos.52272052,51972315,21873110,and 61720106014).
文摘Comprehensive Summary Currently,solid-state fluorescent carbonized polymer dots(CPDs)have attracted attention increasingly due to their applications for optoelectronic display.However,designing CPDs possessing solid-state fluorescence and clarifying the fluorescence mechanism remain challenging.Herein,we initially synthesized a novel type of polythiophene derivatives CPDs,poly-4,4’-(thiophene-3,4-diyl)dibenzoic acid carbonized polymer dots(PDBA-CPDs)with solid-state fluorescence.Subsequently,the structural and optical characterization revealed that the solid-state fluorescence originated from the aggregation induced emission of the CPDs.In brief,in aggregation state,the remaining polymer structure groups on the surface of the CPDs overlapped and weakened the non-radiative transition,enhancing solid-state fluorescence emission.Thirdly,three polythiophene-derived CPDs were designed to further demonstrate the aggregation induced solid-state fluorescence mechanism.Finally,owing to their unique properties of solid-state fluorescence,the white LEDs(light emitting diodes)were fabricated with high color rendering index(CRI)of 82.7 and CIE coordinates of(0.37,0.39)using commercial 460 nm chip.
基金the Priority Academic Program Development of Jiangsu Higher Education Institutions (No. 1107047002)the Key Research and Development Plan (Modern Agriculture) of Jiangsu Province (No. BE2018385)Innovation Platform Project supported by Jiangsu Province (No. 6907041203)。
文摘Three kinds of carbonized polymer dots(CPDs) synthesized via a one-pot process from ophenylenediamine(OPD), m-phenylenediamine(MPD) and p-phenylenediamine(PPD) exhibit excitationwavelength independent yellow, green and red emissions, respectively. In sharp contrast, two kinds of CPDs prepared via a hydrothermal process from citric acid(CA) and diethylenetriamine(DETA) exhibit obvious excitation-wavelength dependent emissions. Through the characterization and comparison of the two types of CPDs, it is concretely revealed that the polymer structure types during the formation of CPDs can effectively control the fluorescence excitation-wavelength independence/dependence. The homogeneous polymer structures contained in CPDs contribute to excitation-wavelength independence, whereas random copolymer structures contribute to excitation-wavelength dependence. These studies are of great significance for further understanding the polymer structures and designing unique optical properties of CPDs.
基金supported by National Natural Science Foundation of China(No.U21A20308)Sichuan Science and Technology Program(Nos.21ZDYF3218,2022ZYD0048)Talent Project of Sichuan Province,Sichuan Provincial College Student Innovation Training Program(Nos.S202010650073,S202210623049).
文摘Identification of lymph nodes(LNs)is critical for studies of the structure,the role in disease development,and the efficacy of disease treatment.Carbonized polymer dots(CPDs)are expected to be potential LNs-targeted imaging agents due to their excellent properties with special structure,better photoluminescence(PL)and great biocompatibility.Herein,a red/near infrared(NIR)emission CPDs(RCPDs)with one and two-photon bioimaging based on citric acid(CA)and benzoylurea(BU)are prepared.Notably,the RCPDs are capable of targeting LNs for imaging.Lymphocyte homing has been demonstrated to be the cellular mechanism of RCPDs target LNs imaging.This work has developed a new nanomaterial for targeted imaging of LNs,while the biological applications of CPDs have been expanded and deepened.
基金financially supported by the National Natural Science Foundation of China(Nos.21874001,21575004)the Foundation for Innovation Team of Bioanalytical Chemistry of Anhui Province。
文摘It is highly desired to accurately and selectively detect and image intracellular L-lysine and pH in biological systems because they could act as the biomarkers in certain abnormal conditions and may give us a warning of the occurrence of diseases.It has been attracted more focuses to design new ratiometric fluorescent probe for monitoring L-lysine and pH to improve detection accuracy.Carbonized polymer dots(CPDs),which possess carbon/polymer hybrid structure rather than pure carbon structure and constitute of a carbon core and large amounts of functional groups/polymer chains on the surface,rise up as a new type of fluorescent nanomaterials and especially display many advantages for bioanalysis.In this study,o-phenylenediamine(o-PD)and poly(styrene-co-maleic anhydride)(PSMA)are used as the precursors to synthesize the desired CPDs through one-step hydrothermal amide method.The prepared CPDs display two well-resolved fluorescence emission bands,i.e.,a very weak emission centered at 470 nm in blue region and a strong emission centered at 558 nm in yellow region.It is found that the two emissions are both responsive to L-lysine based on the surface passivation mechanism,whereas,only the yellow emission is responsive to pH due to the protonation/deprotonation process of the amino groups.Based on the different responsive behaviors,ratiometric detection and imaging of L-lysine and pH are achieved.The prepared ratiometric CPDs probe is successfully applied for L-lysine and pH sensing and imaging at two emission channels in live cell and zebrafish with satisfactory results.
基金supported financially by the National Science Foundation of China(Nos.22035001,21774041)Jilin University Science and Technology Innovative Research Team(No.2017TD-06)。
文摘Development of high-performance solid state luminescent carbon-based nanomaterials remains challenging.Here,strong blue-green fluorescent carbonized polymer dots(CPDs)from o-aminobenzenethiol and thiosalicylic acid(o ABT-TSA-CPDs)with an absolute photoluminescence quantum yield(PLQY)of 76%in solid state without matrix were synthesized.Through adjusting the reaction temperature and time,the PL centers were proved to be carbon core state and surface state associated to carbonyl group which was the source of strong fluorescence emission in solid state.The mechanism of the unique phenomenon of enhanced emission from ethanol solution(PLQY=7%)to powder(PLQY=76%)was investigated by analyzing the chemical properties and structures of o ABT-TSA-CPDs at different temperatures and o ABT-TSACPDs/PVC composites,and was confirmed as fixation of PL centers.