To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoin...To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoinduced electron transfer reversible addition-fragmentation chain-transfer(PET-RAFT)polymerization is a precise methodology for constructing polymers with well-defined structures.However,conventional semiconductor-mediated PET-RAFT polymerization still has considerable limitations in terms of efficiency as well as the polymerization environment.Herein,sulfur-doped carbonized polymer dots(CPDs)were hydrothermally synthesized for catalysis of aqueous PET-RAFT polymerization at unprecedented efficiency with a highest propagation rate of 5.05 h-1.The resulting polymers have well-controlled molecular weight and narrow molecular weight dispersion(Ð<1.10).Based on the optoelectronic characterizations,we obtained insights into the photoinduced electron transfer process and proposed the mechanism for CPD-mediated PET-RAFT polymerization.In addition,as-synthesized CPDs for PET-RAFT polymerization were also demonstrated to be suitable for a wide range of light sources(blue/green/solar irradiation),numerous monomers,low catalyst loading(low as 0.01 mg mL^(-1)),and multiple polar solvent environments,all of which allowed to achieve efficiencies much higher than those of existing semiconductor-mediated methods.Finally,the CPDs were confirmed to be non-cytotoxic and catalyzed PET-RAFT polymerization successfully in cell culture media,indicating broad prospects in biomedical fields.展开更多
Designing efficient and stable electrocatalysts for the oxygen evolution reaction(OER)is of paramount importance for many energy-related technologies and devices.Herein,we propose a controlled oxidation pyrolysis stra...Designing efficient and stable electrocatalysts for the oxygen evolution reaction(OER)is of paramount importance for many energy-related technologies and devices.Herein,we propose a controlled oxidation pyrolysis strategy to develop carbonized polymer dots(CPDs)-modified Rh-doped RuO_(2)electrocatalyst(Rh-RuO_(2)/CPDs).CPDs act as structure-directing agents,facilitating the formation of small-sized RhRuO_(2)/CPDs nanoparticles and engineering them with abundant defective structures and stable Ru-O sites.The experimental results and theoretical simulation unravel that the modulation effect of CPDs and Rh doping can effectively regulate the electronic structure,valence state and morphology of active Ru-O sites,thereby enhancing the electron transfer at the active site interface and optimizing the chemisorption behavior of oxygen intermediates.The resultant Rh-RuO_(2)/CPDs demonstrates overpotentials of 168 and 197 mV at 10 mA/cm^(2)for OER in 0.5 mol/L H_(2)SO_(4)and 1.0 mol/L KOH solution,respectively,and longterm catalytic stability.展开更多
Since the discovery of carbonized polymer dots(CPDs)two decades ago,this emerging family of carbonbased nanomaterials has rapidly risen to prominence.CPDs have found widespread applications in sensing,catalysis,energy...Since the discovery of carbonized polymer dots(CPDs)two decades ago,this emerging family of carbonbased nanomaterials has rapidly risen to prominence.CPDs have found widespread applications in sensing,catalysis,energy,and biomedicine due to their flexible precursors and synthesis methods,tunable photoluminescence(PL)properties,and excellent biocompatibility.This report presents the advancements made in the realm of CPD precursors,elucidates their luminescence properties and underlying mechanisms,and explores the diverse applications of CPD-based materials.It comprehensively addresses key issues by delving into several interconnected chapters:Initially exploring the intriguing fluorescence and afterglow properties exhibited by CPDs,subsequently unraveling the complex luminescence mechanisms that underlie these phenomena,emphasizing the crucial aspect of controllable synthesis of CPDs,and ultimately culminating in the precise construction of composite materials tailored for applications in laser and electroluminescent devices.Furthermore,this report aims to provide communication and assistance for the controlled synthesis and expanded applications of CPDs.展开更多
Aqueous zinc ion batteries(AZIBs)are considered to be one of the most promising energy storage devices due to the advantages of high cost-effectiveness,safety,and environmental friendliness.However,they suffer from pr...Aqueous zinc ion batteries(AZIBs)are considered to be one of the most promising energy storage devices due to the advantages of high cost-effectiveness,safety,and environmental friendliness.However,they suffer from problems such as Zn dendrites growth and by-product generation.Carbonized polymer dots(CPDs)with polar groups as additive have been introduced to modulate the solvated structure of Zn^(2+)and reduce the water activity,promoting the uniform deposition of Zn and inhibiting the occurrence of side reactions.However,CPDs with different functional group contents from different precursor molar ratios variably affect the electrochemical performance of aqueous electrolytes.Therefore,in this work,we designed and synthesized CPDs with different molar ratios of the precursors(citric acid and urea)as electrolyte additives for AZIBs and explore the optimal molar ratios of the precursors.The Zn//Zn symmetrical cells using electrolytes with the optimal ratios CPDs achieve an extended cycle life over 615 h at 2 mA∙cm^(−2) and 1 mAh∙cm^(−2).This work offers great potential for future practical applications of CPDs.展开更多
Stabilizing triplet excited states is important for room temperature phosphorescence(RTP)materials to achieve multifunctional applications in humid environment.However,due to the lack of preparation strategies,the rea...Stabilizing triplet excited states is important for room temperature phosphorescence(RTP)materials to achieve multifunctional applications in humid environment.However,due to the lack of preparation strategies,the realization of RTP materials in water still faces challenges.Herein,a new design strategy was presented to achieve RTP in water by confining carbonized polymer dots(CPDs)in amino functional mesoporous silica(MSNs-NH_(2)).The as-prepared MSNs-CPDs aqueous dispersion exhibited blue afterglow,lasting more than 3 s to naked eyes.The triplet excited states were protected from non-radiative deactivation by the double-confinement effect including covalent bonding fixation and mesoporous structure confinement.The MSNs-CPDs inherited the structure of MSNs-NH_(2),so the stability of morphology and properties were superior to CPDs and even most of silica-based CPDs RTP materials.A water-related encryption technique demonstrated the promising application of MSNs-CPDs as smart materials in the field of information security.Besides,the possibility of potential application in ion detection was also explored.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
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
Due to their inherent tunable spectrum,high brightness,excellent biostability and biocompatibility,and functionalization of surfaces,semiconducting polymer dots(Pdots)are now playing an essential role in fluorescent(F...Due to their inherent tunable spectrum,high brightness,excellent biostability and biocompatibility,and functionalization of surfaces,semiconducting polymer dots(Pdots)are now playing an essential role in fluorescent(FL)imaging and disease treatment through bioconjugation with peptides or biomimetic materials.In particular,biomimetic Pdots exhibit their capability in targeted imaging of lesion and increased efficacy for targeting disease treatment.This review will inspect the recent advances in the design and functionalization strategies of biomodified and biomimetic Pdots for enhanced disease detection and therapy.More importantly,the application of these two modifications in targeted FL imaging and cancer treatment is to be addressed in detail.Meanwhile,the main challenges and prospects of biomimetic and biomodified Pdots are to be discussed,which will pave a new avenue for improved disease detection and imaging-guided treatment.展开更多
Photodynamic therapy(PDT)has been emerged as a promising modality for cancer treatment.However,the development of drug delivery system enabling continuous release of photosensitizers(PSs)for long-term PDT treatment st...Photodynamic therapy(PDT)has been emerged as a promising modality for cancer treatment.However,the development of drug delivery system enabling continuous release of photosensitizers(PSs)for long-term PDT treatment still remains challenges.Herein,a H_(2)O_(2)-responsive injectable hydrogel,covalently crosslinked by N^(1)-(4-boronobenzyl)-N^(3)-(4-boronophenyl)-N^(1),N^(1),N^(3),N^(3)-tetramethylpropane-1,3-diaminium(TSPBA)with PVA containing polythiophene quaternary ammonium salt(PT2)polymer dots(PDots)as a photosensitizer was fabricated.Under the stimulation of H_(2)O_(2),the obtained injectable hydrogel gradually degrades and releases PDots.In vitro experiments suggested that the released PDots could realize efficient tumor cells inhibition through its robust singlet oxygen generation capability upon 577 nm laser irradiation.In vivo studies demonstrated a sustained retention of PDots for at least 7 days following single-dose administration,facilitating efficient tumor inhibition with light treatments for 3 times without apparent biotoxicity.This work presents an innovative polymer dots-based composite local drug delivery system for long-term PDT in cancer treatment.展开更多
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
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
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
Carbonized polymer dots(CPDs)modified layer-structured CdBiO_(2)Br(CPDs/CdBiO_(2)Br)Z-scheme heterojunction hybrid material has been synthesized via simple solvothermal method.The hybrid material with Z-scheme heteroj...Carbonized polymer dots(CPDs)modified layer-structured CdBiO_(2)Br(CPDs/CdBiO_(2)Br)Z-scheme heterojunction hybrid material has been synthesized via simple solvothermal method.The hybrid material with Z-scheme heterojunction can effectively maintain the original highly oxidizing holes of CdBiO_(2)Br and the highly reducing electrons of CPDs.In addition,the construction of heterostructure is beneficial to the migration and separation of photogenerated carriers.Under visible light irradiation,6 wt%CPDs/CdBiO_(2)Br showed the best catalytic activity for degradation of organic pollutants.Free radical capture experiments and ESR analysis confirmed that the main active species are·O_(2)^(-)and h^(+).The decomposition process of organic pollutants was analyzed by LC-MS.Finally,the probable visible light mechanism performance of CPDs/CdBiO_(2)Br as direct Z-scheme heterojunction photocatalytic materials was proposed.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
This letter describes semiconducting polymer dots （Pdots） doped with a photosensitizer and modified with a cell penetrating peptide for photodynamic therapy （PDT）. The resulting Pdots exhibited efficient singlet o...This letter describes semiconducting polymer dots （Pdots） doped with a photosensitizer and modified with a cell penetrating peptide for photodynamic therapy （PDT）. The resulting Pdots exhibited efficient singlet oxygen （^1O2） generation mediated by intraparticle energy transfer. Experimental results indicated that the peptide-coated Pdots could promote the cellular uptake and increase the penetration efficiency in vitro, and effectively suppressed tumor growth and enhanced the photodynamic effect in vivo. Our results demonstrate that Pdots with photosensitizer loading and peptide modification hold great promise for cancer therapy.展开更多
In order to uniformly disperse the ceramic reinforcements synthesized in-situ in the copper matrix composites,this study used Carbon Polymer Dot(CPD)as the carbon source and Cu–1.0%Ti alloy powder as the matrix for s...In order to uniformly disperse the ceramic reinforcements synthesized in-situ in the copper matrix composites,this study used Carbon Polymer Dot(CPD)as the carbon source and Cu–1.0%Ti alloy powder as the matrix for supplying Ti source to prepare in-situ synthesized TiC/Cu composites.The results show that TiC nano-precipitates,having the similar particle sizes with the CPD,form at the grains interior and grain boundaries,and maintain a uniform distribution state.Compared with the matrix,0.3 wt%CPD/Cu composite displays the best strengthplastic compatibility,the ultimate tensile strength achieves 385 MPa accompanied with a corresponding elongation of 21%,owing to the dislocation hindrance caused by nano-carbide and excellent interface bonding between nano TiC and the Cu matrix.The density function theory calculation supports our experimental results by showing a tighter and stronger interface contact.This work presents a new approach for studying in-situ carbide precipitates.展开更多
Carbon dots(CDs)are a class of zero-dimensional carbon-based nanomaterials with a size of less than 10 nm and remarkable fluorescence properties[1].Owing to their excellent fluorescence characteristics,chemical stabil...Carbon dots(CDs)are a class of zero-dimensional carbon-based nanomaterials with a size of less than 10 nm and remarkable fluorescence properties[1].Owing to their excellent fluorescence characteristics,chemical stability,biocompatibility,and low toxicity,CDs show great potential in biomedical,catalytic,and optoelectronic applications[2],[3].Based on their formation mechanisms,micro/nano structures,and properties.展开更多
As emerging carbon-based nanoparticles,carbon dots(CDs)have attracted widespread attention in recent decades.Among the large family of CDs,carbonized polymer dots(CPDs)exhibit amazing charm due to their unique highly ...As emerging carbon-based nanoparticles,carbon dots(CDs)have attracted widespread attention in recent decades.Among the large family of CDs,carbonized polymer dots(CPDs)exhibit amazing charm due to their unique highly functionalized structure and typical polymeric characteristics.The polymerization and crosslinking of precursors during the synthesis process lead to the formation of a distinctive core-shell structure in CPDs,which consists of a hydrophobic carbon core and a polymer shell layer with entangled chain segments.In previous research,CPDs have been highlighted from the perspective of their outstanding photoluminescence properties.However,few discussions or summaries are available concerning the polymeric characteristics of CPDs.Herein,we try to provide a detailed discussion of the typical polymeric characteristics of CPDs and related applications.We first make an introduction to CPD synthesis in terms of the formation process,synthetic methods,and precursor varieties.Subsequently,we give a summary of several typical polymeric characteristics of CPDs and relevant characterization techniques.Furthermore,we list various applications of CPDs related to polymer characteristics,including sensing,optoelectronic devices,anti-counterfeiting,and so on.Finally,we put forward some reflections and perspectives for the development of CPDs.展开更多
Stimulated emission depletion(STED)microscopy requires fluorescent probes to exhibit high brightness,good photostability,a sensitive optical depletion response,and narrow spectral features.There are great interests in...Stimulated emission depletion(STED)microscopy requires fluorescent probes to exhibit high brightness,good photostability,a sensitive optical depletion response,and narrow spectral features.There are great interests in using polymer dots(Pdots)for STED imaging due to their exceptional brightness and photobleaching resistance.However,the conven-tional Pdots either suffer from broad spectra or an unsatisfactory STED response.Herein,we developed a general method for obtaining Pdots with desirable optical properties for STED microscopy.Speciically,boron.dipyrromethene(BODIpY)chromophores were grafted on to a polystyrene backbone to obtain polymers with narrow spectral profiles.The grafting ratio was precisely controlled to minimize aggregation-induced quenching.Conjugating BODIpYs to side chains reduced interactions between the chromophores,resulting in a long excited state lifetime,which is critical for obtaining complete fluorescence depletion.Using this strategy,we synthesized three-color Pdots with narrow spectra features.Compared to directly encapsulating BODIpYs into nanoparticles,our strategy achieved 2-10 times higher single-particle brightness.We used Pdots for single-particle,cellular,and tissular STED imaging.The Pdots showed high spatial resolutions and could clearly resolve subdiffraction-limit structures in cells and tissue sections,indicating great application potential in in vitro diagnostics and biomedical imaging applications.展开更多
基金supported by the National Natural Science Foundation of China(NSFC)under Grant No.22035001 and No.52233005.
文摘To achieve the target of carbon neutrality,it is crucial to develop an efficient and green synthesis methodology with good atomic economy to achieve sufficient utilization of energy and sustainable development.Photoinduced electron transfer reversible addition-fragmentation chain-transfer(PET-RAFT)polymerization is a precise methodology for constructing polymers with well-defined structures.However,conventional semiconductor-mediated PET-RAFT polymerization still has considerable limitations in terms of efficiency as well as the polymerization environment.Herein,sulfur-doped carbonized polymer dots(CPDs)were hydrothermally synthesized for catalysis of aqueous PET-RAFT polymerization at unprecedented efficiency with a highest propagation rate of 5.05 h-1.The resulting polymers have well-controlled molecular weight and narrow molecular weight dispersion(Ð<1.10).Based on the optoelectronic characterizations,we obtained insights into the photoinduced electron transfer process and proposed the mechanism for CPD-mediated PET-RAFT polymerization.In addition,as-synthesized CPDs for PET-RAFT polymerization were also demonstrated to be suitable for a wide range of light sources(blue/green/solar irradiation),numerous monomers,low catalyst loading(low as 0.01 mg mL^(-1)),and multiple polar solvent environments,all of which allowed to achieve efficiencies much higher than those of existing semiconductor-mediated methods.Finally,the CPDs were confirmed to be non-cytotoxic and catalyzed PET-RAFT polymerization successfully in cell culture media,indicating broad prospects in biomedical fields.
基金financially supported by the National Natural Science Foundation of China(No.22035001)the Natural Science Foundation of Jilin Province(No.***202402011)。
文摘Designing efficient and stable electrocatalysts for the oxygen evolution reaction(OER)is of paramount importance for many energy-related technologies and devices.Herein,we propose a controlled oxidation pyrolysis strategy to develop carbonized polymer dots(CPDs)-modified Rh-doped RuO_(2)electrocatalyst(Rh-RuO_(2)/CPDs).CPDs act as structure-directing agents,facilitating the formation of small-sized RhRuO_(2)/CPDs nanoparticles and engineering them with abundant defective structures and stable Ru-O sites.The experimental results and theoretical simulation unravel that the modulation effect of CPDs and Rh doping can effectively regulate the electronic structure,valence state and morphology of active Ru-O sites,thereby enhancing the electron transfer at the active site interface and optimizing the chemisorption behavior of oxygen intermediates.The resultant Rh-RuO_(2)/CPDs demonstrates overpotentials of 168 and 197 mV at 10 mA/cm^(2)for OER in 0.5 mol/L H_(2)SO_(4)and 1.0 mol/L KOH solution,respectively,and longterm catalytic stability.
基金financial support from the National Natural Science Foundation of China(Nos.52203244,22101267)the Key Scientific and Technological Project of Henan Province(No.222102310683)+1 种基金the China Postdoctoral Science Foundation(Nos.2021M692905,2024T170832)Natural Science Foundation of Henan Province(Nos.242300421068,242300421123)。
文摘Since the discovery of carbonized polymer dots(CPDs)two decades ago,this emerging family of carbonbased nanomaterials has rapidly risen to prominence.CPDs have found widespread applications in sensing,catalysis,energy,and biomedicine due to their flexible precursors and synthesis methods,tunable photoluminescence(PL)properties,and excellent biocompatibility.This report presents the advancements made in the realm of CPD precursors,elucidates their luminescence properties and underlying mechanisms,and explores the diverse applications of CPD-based materials.It comprehensively addresses key issues by delving into several interconnected chapters:Initially exploring the intriguing fluorescence and afterglow properties exhibited by CPDs,subsequently unraveling the complex luminescence mechanisms that underlie these phenomena,emphasizing the crucial aspect of controllable synthesis of CPDs,and ultimately culminating in the precise construction of composite materials tailored for applications in laser and electroluminescent devices.Furthermore,this report aims to provide communication and assistance for the controlled synthesis and expanded applications of CPDs.
基金supported by the National Natural Science Foundation of China(22035001 and 22275030)Jilin Provincial Education Department(JJKH20231304KJ)the Fundamental Research Funds(Science and Technology Achievements Transformation)for the Central Universities of China(CGZH202203)
文摘Aqueous zinc ion batteries(AZIBs)are considered to be one of the most promising energy storage devices due to the advantages of high cost-effectiveness,safety,and environmental friendliness.However,they suffer from problems such as Zn dendrites growth and by-product generation.Carbonized polymer dots(CPDs)with polar groups as additive have been introduced to modulate the solvated structure of Zn^(2+)and reduce the water activity,promoting the uniform deposition of Zn and inhibiting the occurrence of side reactions.However,CPDs with different functional group contents from different precursor molar ratios variably affect the electrochemical performance of aqueous electrolytes.Therefore,in this work,we designed and synthesized CPDs with different molar ratios of the precursors(citric acid and urea)as electrolyte additives for AZIBs and explore the optimal molar ratios of the precursors.The Zn//Zn symmetrical cells using electrolytes with the optimal ratios CPDs achieve an extended cycle life over 615 h at 2 mA∙cm^(−2) and 1 mAh∙cm^(−2).This work offers great potential for future practical applications of CPDs.
基金financially supported by the National Natural Science Foundation of China (NSFC, No. 22035001)
文摘Stabilizing triplet excited states is important for room temperature phosphorescence(RTP)materials to achieve multifunctional applications in humid environment.However,due to the lack of preparation strategies,the realization of RTP materials in water still faces challenges.Herein,a new design strategy was presented to achieve RTP in water by confining carbonized polymer dots(CPDs)in amino functional mesoporous silica(MSNs-NH_(2)).The as-prepared MSNs-CPDs aqueous dispersion exhibited blue afterglow,lasting more than 3 s to naked eyes.The triplet excited states were protected from non-radiative deactivation by the double-confinement effect including covalent bonding fixation and mesoporous structure confinement.The MSNs-CPDs inherited the structure of MSNs-NH_(2),so the stability of morphology and properties were superior to CPDs and even most of silica-based CPDs RTP materials.A water-related encryption technique demonstrated the promising application of MSNs-CPDs as smart materials in the field of information security.Besides,the possibility of potential application in ion detection was also explored.
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University of Macao,Grant/Award Numbers:MYRG 2020-00067-FHS,MYRG2019-00082-FHS,MYRG2022-00081-FHSMacao Science and Technology Development Fund,Grant/Award Numbers:FDCT 0011/2018/A1,FDCT 0020/2019/AMJ,FDCT 0048/2021/AGJ+2 种基金Natural Science Foundation of Guangdong ProvinceNational Key R&D Program of China,Grant/Award Number:2019YFE0110400Higher Education Fund of Macao SAR Government,Grant/Award Number:CP-UMAC-2020-01。
文摘Due to their inherent tunable spectrum,high brightness,excellent biostability and biocompatibility,and functionalization of surfaces,semiconducting polymer dots(Pdots)are now playing an essential role in fluorescent(FL)imaging and disease treatment through bioconjugation with peptides or biomimetic materials.In particular,biomimetic Pdots exhibit their capability in targeted imaging of lesion and increased efficacy for targeting disease treatment.This review will inspect the recent advances in the design and functionalization strategies of biomodified and biomimetic Pdots for enhanced disease detection and therapy.More importantly,the application of these two modifications in targeted FL imaging and cancer treatment is to be addressed in detail.Meanwhile,the main challenges and prospects of biomimetic and biomodified Pdots are to be discussed,which will pave a new avenue for improved disease detection and imaging-guided treatment.
基金financially supported by the National Natural Science Foundation of China(Nos.52272052 and 51972315)。
文摘Photodynamic therapy(PDT)has been emerged as a promising modality for cancer treatment.However,the development of drug delivery system enabling continuous release of photosensitizers(PSs)for long-term PDT treatment still remains challenges.Herein,a H_(2)O_(2)-responsive injectable hydrogel,covalently crosslinked by N^(1)-(4-boronobenzyl)-N^(3)-(4-boronophenyl)-N^(1),N^(1),N^(3),N^(3)-tetramethylpropane-1,3-diaminium(TSPBA)with PVA containing polythiophene quaternary ammonium salt(PT2)polymer dots(PDots)as a photosensitizer was fabricated.Under the stimulation of H_(2)O_(2),the obtained injectable hydrogel gradually degrades and releases PDots.In vitro experiments suggested that the released PDots could realize efficient tumor cells inhibition through its robust singlet oxygen generation capability upon 577 nm laser irradiation.In vivo studies demonstrated a sustained retention of PDots for at least 7 days following single-dose administration,facilitating efficient tumor inhibition with light treatments for 3 times without apparent biotoxicity.This work presents an innovative polymer dots-based composite local drug delivery system for long-term PDT in cancer treatment.
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.
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 the National Natural Science Foundation of China(No.22108106,21676128)China Postdoctoral Science Foundation(No.2020M680065)+1 种基金Hong Kong Scholar Program(No.XJ2021021)Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province(No.KFKT2021005).
文摘Carbonized polymer dots(CPDs)modified layer-structured CdBiO_(2)Br(CPDs/CdBiO_(2)Br)Z-scheme heterojunction hybrid material has been synthesized via simple solvothermal method.The hybrid material with Z-scheme heterojunction can effectively maintain the original highly oxidizing holes of CdBiO_(2)Br and the highly reducing electrons of CPDs.In addition,the construction of heterostructure is beneficial to the migration and separation of photogenerated carriers.Under visible light irradiation,6 wt%CPDs/CdBiO_(2)Br showed the best catalytic activity for degradation of organic pollutants.Free radical capture experiments and ESR analysis confirmed that the main active species are·O_(2)^(-)and h^(+).The decomposition process of organic pollutants was analyzed by LC-MS.Finally,the probable visible light mechanism performance of CPDs/CdBiO_(2)Br as direct Z-scheme heterojunction photocatalytic materials was proposed.
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financial support from the National Science Foundation of China (No. 81641177)
文摘This letter describes semiconducting polymer dots （Pdots） doped with a photosensitizer and modified with a cell penetrating peptide for photodynamic therapy （PDT）. The resulting Pdots exhibited efficient singlet oxygen （^1O2） generation mediated by intraparticle energy transfer. Experimental results indicated that the peptide-coated Pdots could promote the cellular uptake and increase the penetration efficiency in vitro, and effectively suppressed tumor growth and enhanced the photodynamic effect in vivo. Our results demonstrate that Pdots with photosensitizer loading and peptide modification hold great promise for cancer therapy.
基金supported by the Chinese National Science Foundation(Grant No.52174345,52064032)the Yunnan Science and Technology Projects(Grant No.202002AB080001)Science and Technology Major Project of Yunnan Province(Grant No.202202AG050004).
文摘In order to uniformly disperse the ceramic reinforcements synthesized in-situ in the copper matrix composites,this study used Carbon Polymer Dot(CPD)as the carbon source and Cu–1.0%Ti alloy powder as the matrix for supplying Ti source to prepare in-situ synthesized TiC/Cu composites.The results show that TiC nano-precipitates,having the similar particle sizes with the CPD,form at the grains interior and grain boundaries,and maintain a uniform distribution state.Compared with the matrix,0.3 wt%CPD/Cu composite displays the best strengthplastic compatibility,the ultimate tensile strength achieves 385 MPa accompanied with a corresponding elongation of 21%,owing to the dislocation hindrance caused by nano-carbide and excellent interface bonding between nano TiC and the Cu matrix.The density function theory calculation supports our experimental results by showing a tighter and stronger interface contact.This work presents a new approach for studying in-situ carbide precipitates.
基金supported in part by the National Natural Science Foundation of China(U24A2079 and 82570162)the Natural Science Foundation of Henan Province(252300421125).
文摘Carbon dots(CDs)are a class of zero-dimensional carbon-based nanomaterials with a size of less than 10 nm and remarkable fluorescence properties[1].Owing to their excellent fluorescence characteristics,chemical stability,biocompatibility,and low toxicity,CDs show great potential in biomedical,catalytic,and optoelectronic applications[2],[3].Based on their formation mechanisms,micro/nano structures,and properties.
基金supported by the Natural Science Foundation of Jilin Province(no.202402011)the National Natural Science Foundation of China(NSFC)under Grant No.22035001.
文摘As emerging carbon-based nanoparticles,carbon dots(CDs)have attracted widespread attention in recent decades.Among the large family of CDs,carbonized polymer dots(CPDs)exhibit amazing charm due to their unique highly functionalized structure and typical polymeric characteristics.The polymerization and crosslinking of precursors during the synthesis process lead to the formation of a distinctive core-shell structure in CPDs,which consists of a hydrophobic carbon core and a polymer shell layer with entangled chain segments.In previous research,CPDs have been highlighted from the perspective of their outstanding photoluminescence properties.However,few discussions or summaries are available concerning the polymeric characteristics of CPDs.Herein,we try to provide a detailed discussion of the typical polymeric characteristics of CPDs and related applications.We first make an introduction to CPD synthesis in terms of the formation process,synthetic methods,and precursor varieties.Subsequently,we give a summary of several typical polymeric characteristics of CPDs and relevant characterization techniques.Furthermore,we list various applications of CPDs related to polymer characteristics,including sensing,optoelectronic devices,anti-counterfeiting,and so on.Finally,we put forward some reflections and perspectives for the development of CPDs.
基金support from the Public Welfare Fund(YXD23H0301)from the Natural Science Foundation of Zhejiangthe National Natural Science Foundation of China(22374134,22004123,and the Excellent Young Scientists Fund)+5 种基金the National Key Scientific Program of China(2022YFA1304500 and 2022YFC3401003)the Zhejiang Leading Innovation and Entrepreneurship Team(2022R01006)the“Pioneer”and“Leading Goose”R&D Program of Zhejiang(2023SDYXS0001)the Hangzhou Institute of Medicine,the Chinese Academy of Sciences(2024ZZBS04)the KEY R&D Program of Zhejiang(2023C03058)the Natural Science Foundation of Shandong Province(ZR2022YQ12).
文摘Stimulated emission depletion(STED)microscopy requires fluorescent probes to exhibit high brightness,good photostability,a sensitive optical depletion response,and narrow spectral features.There are great interests in using polymer dots(Pdots)for STED imaging due to their exceptional brightness and photobleaching resistance.However,the conven-tional Pdots either suffer from broad spectra or an unsatisfactory STED response.Herein,we developed a general method for obtaining Pdots with desirable optical properties for STED microscopy.Speciically,boron.dipyrromethene(BODIpY)chromophores were grafted on to a polystyrene backbone to obtain polymers with narrow spectral profiles.The grafting ratio was precisely controlled to minimize aggregation-induced quenching.Conjugating BODIpYs to side chains reduced interactions between the chromophores,resulting in a long excited state lifetime,which is critical for obtaining complete fluorescence depletion.Using this strategy,we synthesized three-color Pdots with narrow spectra features.Compared to directly encapsulating BODIpYs into nanoparticles,our strategy achieved 2-10 times higher single-particle brightness.We used Pdots for single-particle,cellular,and tissular STED imaging.The Pdots showed high spatial resolutions and could clearly resolve subdiffraction-limit structures in cells and tissue sections,indicating great application potential in in vitro diagnostics and biomedical imaging applications.
