A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDS...A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDSP5 and a homoditopic guest G-(CN)_(2),which shows not only excellent fluorescence properties due to the AIE effect but also desirable ion-sensing abilities in both solution and solid states,holding great potential in the applicable fluorescence detection for Fe^(3+).The resultant G-(CN)_(2)⊂BXDSP5 can be transformed into supramolecular polymer gel at high concentration via multiple noncovalent interactions,showing multi-stimuli-responsiveness in response to temperature change,mechanical force,and competitive agent.Meanwhile,the xerogel of supramolecular polymer material has been successfully used to remove Fe^(3+)from water with high adsorption efficiency.In addition,an ionresponsive film based on supramolecular polymer has also been developed,which can serve as a practical and convenient fluorescence test kit for detecting Fe^(3+).展开更多
Covalent triazine frameworks(CTFs)are a class of unique two-dimensional nitrogen-rich triazine framework with adjustable chemical and electronic structures,rich porosity,good stability and excellent semiconductivity,w...Covalent triazine frameworks(CTFs)are a class of unique two-dimensional nitrogen-rich triazine framework with adjustable chemical and electronic structures,rich porosity,good stability and excellent semiconductivity,which enable great various applications in efficient gas/molecular adsorption and separation,energy storage and conversion,especially photo-and electrocatalysis.Different synthesis strategies strongly affect the morphology of CTFs and play an important role in their structure and properties.In this concept,we provide a comprehensive and systematic review of the synthesis methods such as ionothermal synthesis,phosphorus pentoxide catalytic method,polycondensation and ultra-strong acid catalyzed method,and applications of CTFs in photo-and electro-catalysis.Finally we offer some insights into the future development progress of CTFs materials for catalytic applications.展开更多
A series of novel side-chain liquid crystalline(SCLC)copolymers were synthesized by attaching two distinct mesogenic units,namely a chiral cholesteryl-based monomer(M1)and an achiral biphenyl-based monomer(M2),to a po...A series of novel side-chain liquid crystalline(SCLC)copolymers were synthesized by attaching two distinct mesogenic units,namely a chiral cholesteryl-based monomer(M1)and an achiral biphenyl-based monomer(M2),to a poly(3-mercaptopropylmethylsiloxane)(PMMS)backbone via thiol-ene click chemistry.The influence of side chain composition on the self-assembly behavior and phase structures of these SCLC copolymers was systematically investigated using different instrument.Results indicate that three distinct liquid crystalline phases and four unique molecular configurations were identified within the polymer series,with the emergence of the liquid crystalline phase being a synergistic outcome of the two distinct side chains.This study underscores the critical influence of side chain dimensions,rigidity,and spatial volume on the self-assembly structures and phase characteristics of liquid crystalline polymers,providing valuable insights for the rational design and development of advanced functional materials with tailored properties.展开更多
An ultrasensitive detection and effective removal material was successfully developed by using a pillar[n]arene-based supramolecular polymer gel(MTP5?HB).The MTP5?HB can ultrasensitively recognize Cu^2+and Fe^3+,and t...An ultrasensitive detection and effective removal material was successfully developed by using a pillar[n]arene-based supramolecular polymer gel(MTP5?HB).The MTP5?HB can ultrasensitively recognize Cu^2+and Fe^3+,and the limits of detection(LODs)for Cu^2+and Fe^3+are 1.55 and 2.68 nmol/L,respectively.Additionally,the in-situ generated metallogel MTP5?HB-Cu can exclusively detect CN,and the LOD for CN is 1.13 nmol/L.Noticeably,the xerogel of MTP5?HB-Cu can effectively remove CN from aqueous solution with 94.40%removal rate.Test kit based on MTP5?HB-Cu is also prepared for convenient detection of CN.展开更多
Hydrazine hydrate(DH)is an important fine chemical intermediate and as fuel for rockets,however,it also has serious toxic for humans and environment.Developing novel materials and methods for sensitive detection of DH...Hydrazine hydrate(DH)is an important fine chemical intermediate and as fuel for rockets,however,it also has serious toxic for humans and environment.Developing novel materials and methods for sensitive detection of DH in water and air is an important task.In order to effectively detect DH,a novel conductive supramolecular polymer metallogel(PQ-Ag)has been constructed by the coordination of bis-5-hydroxyquinoline functionalized pillar[5]arene(PQ5)with Ag+.The metallogel PQ-Ag could realize the multi-channel sensitive detection of DH through naked-eye,fluorescence,and electrochemical methods.The lowest limit of detection(LOD)is 0.1 mg/m^(3)in air and 2.68×10^(−8)mol/L in water,which is lower than the standard of the US Environmental Protection Agency(EPA)for DH of maximum allowable concentration in drinking water.More importantly,an electronic device for DH detection based on the metallogel PQ-Ag was designed and prepared,which can realize conveniently and efficiently multi-channel detection and alert of DH through sound and light alarms not only in water but also in air.展开更多
The effective materials and methods for detection and separation of pesticides are urgently needed because most of pesticides show very harmful influence on life and environment. As a new kind of macrocyclic host comp...The effective materials and methods for detection and separation of pesticides are urgently needed because most of pesticides show very harmful influence on life and environment. As a new kind of macrocyclic host compound, pillar[n]arenes show very good performance in the detection and separation of pesticides, especially for paraquat(PQ). For the pesticide detection and separation materials, their structures determine performance. Therefore, this review summarizes the recent progress of pillar[n]arenes-based materials for detection and separation of pesticides covering single/multi-pillar[n]arenes, pillar[n]arenes-based polymers, frameworks, composites, nanomaterials, etc.The structure-performance relationships of these materials have been discussed according to the cavity size, the synergistic or collaboration effect, the structure of the polymer or framework, the substrate of the composites and the size of nanomaterials and so on. Based on these, we also look forward to the future and point out the possible way for improving the pesticides detection sensitivity and separation efficiency of this kind of materials.展开更多
Pillar[5]arene-based supramolecular polymer gels(SPGs)show broad application prospects.To investigate the influence of the supramolecular monomers'structure on the assembly and properties of corresponding pillar[5...Pillar[5]arene-based supramolecular polymer gels(SPGs)show broad application prospects.To investigate the influence of the supramolecular monomers'structure on the assembly and properties of corresponding pillar[5]arene-based SPGs,a series of monomers based on different functionalized pillar[5]arene derivatives with various structures were synthesized.There are per-methylated pillar[5]arene(H1),bromobutane-functionalized pillar[5]arene(H2),4-hydroxybenzaldehyde-functionalized pillar[5]arene(H3),ethyl thioglycolate-functionalized pillar[5]arene(H4),thioacetylhydrazine-functionalized pillar[5]arene(H5),bola-type bis-pillar[5]arene(H6)and tripodal-type tri-pillar[5]arene(H7).Meanwhile,a neutral tripodal-guest TG was also employed to co-assemble with these pillar[5]arene-based monomers by host-guest interactions.As a result,under the same conditions(10%,DMSO-H_(2)O,w/v,10 mg·mL^(-1)=1%),H1 and H2 cannot assemble into SPGs with TG.Interestingly,mono-p[5]derivatives H3—H5 could assemble into SPGs with TG.More importantly,bis-p[5]H6 and tri-p[5]H7 could assemble into supramolecular polymer network gel(SPNG)and supramolecular polymer organic framework gel(SOFG)with TG,respectively.These gels all show blue aggregation-induced emission(ALE)properties.Among these SPGs,the SPNG shows the best viscoelastic behavior and self-healing properties.The result is attributed to the flexible network structure of SPNGs.In addition,the xerogels of SOFG and SPNG have shown nice adsorption and separation properties for organic dyes in water solution.展开更多
Altitude affects leaf stoichiometry by regulating temperature and precipitation,and influencing soil properties in mountain ecosystems.Leaf carbon concentration(C),leaf nitrogen concentration(N),leaf phosphorous conce...Altitude affects leaf stoichiometry by regulating temperature and precipitation,and influencing soil properties in mountain ecosystems.Leaf carbon concentration(C),leaf nitrogen concentration(N),leaf phosphorous concentration(P),and their stoichiometric ratios of Leontopodium lentopodioides(Willd.)Beauv.,a widespread species in degraded grasslands,were investigated to explore its response and adaptation strategy to environmental changes along four altitude gradients(2500,3000,3500,and 3800 m a.s.l.)on the northeastern Qinghai-Tibetan Plateau(QTP),China.The leaf C significantly varied but without any clear trend with increasing altitude.Leaf N showed an increasing trend,and leaf P showed a little change with increasing altitude,with a lower value of leaf P at 3500 m than those at other altitudes.Similarity,leaf C:P and N:P exhibited a little change with increasing altitude,which both had greater values at 3500 m than those at other altitudes.However,leaf C:N exhibited a decreasing trend with increasing altitude.Soil NH^(+)_(4)-N,soil pH,soil total phosphorus(STP),mean annual temperature(MAT),and mean annual precipitation(MAP)were identified as the main factors driving the variations in leaf stoichiometry of L.lentopodioides across all altitudes,with NH^(+)_(4)-N alone accounting for 50.8%of its total variation.Specifically,leaf C and N were mainly controlled by MAT,soil pH,and NH^(+)_(4)-N,while leaf P by MAP and STP.In the study area,it seems that the growth of L.lentopodioides may be mainly limited by STP.The results could help to strengthen our understanding of the plasticity of plant growth to environmental changes and provide new information on global grassland management and restoration.展开更多
CONSPECTUS:Perylene diimide(PDI)as a classical dye has some advantages,such as structural diversity,tunable optical and electronic properties,strong light absorption,high electron affinity,and good electron-transporti...CONSPECTUS:Perylene diimide(PDI)as a classical dye has some advantages,such as structural diversity,tunable optical and electronic properties,strong light absorption,high electron affinity,and good electron-transporting properties and stability.The PDI-based oligomers and polymers are good candidates for n-type semiconductors in organic electronics and photonic devices.A polymer solar cell(PSC)that converts sunlight into electricity is a promising renewable and clean energy technology and has some superiorities,such as simple preparation and being lightweight,low cost,semitransparent,and flexible.For a long time,fullerene derivatives(e.g.,PCBM)have been the most important electron acceptors used in the active layer of PSCs.However,PCBM suffers from some disadvantages,for example,weak absorption,a large amount of energy loss,and unstable morphology.Compared to PCBM,PDI-based materials present some advantages:intense visible-light absorption;lowest unoccupied molecular orbital(LUMO)energy levels can be modulated to achieve a suitable charge separation driving force and high open-circuit voltage(V_(OC));and the molecular configuration can be adjusted to achieve morphology stability.Thus,PDI-based oligomers and polymers are widely used as electron acceptors in the active layer of PSCs.In addition,PDI-based oligomers and polymers are widely used as n-type semiconductors in other electronic and photonic devices,such as organic field-effect transistors(OFETs),light-emitting diodes,lasers,optical switches,and photodetectors.展开更多
Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction ...Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.展开更多
The cyanide anion(CN^(–))is known to be one of the most toxic anions.Therefore,there is an urgent need to develop a reliable,sensitive,selective,rapid and effective method for the detection of CN^(–).Here,a self-ass...The cyanide anion(CN^(–))is known to be one of the most toxic anions.Therefore,there is an urgent need to develop a reliable,sensitive,selective,rapid and effective method for the detection of CN^(–).Here,a self-assembly strategy based on pillar[5]arene P5 and azine derivative AZ was used to construct supramolecular sensors,and it was found that the detection effect of CN^(–)was significantly improved by the assembly strategy.The sensitivity of the assembled sensor P5-AZ to CN^(–)is more than 10 times higher than that of AZ.The detect mechanism was further investigated by theoretical calculations and 1H NMR.The results showed that AZ detects CN–by a deprotonation process with fluorescence enhancement,while P5-AZ improves the sensitivity of CN^(–)recognition through hydrogen bonding,anion-πand anion-dipole interactions,as well as the strong bonding ability of the assembly.Supramolecular assembly P5-AZ has the advantages of low toxicity,high sensitivity,and more importantly,it provides a method to detect CN^(–)sensitivity in the aqueous phase and organisms by host-guest assembly.展开更多
In an era where the concept of green development is deeply rooted, magnesium(Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improv...In an era where the concept of green development is deeply rooted, magnesium(Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products.Herein, three-dimensional mesopore hollow polypyrrole spheres(MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride(h-BN) lamellae, which allowed the hBN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/hBN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface(SHS). Finally, the slippery liquid infused porous surface(SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.展开更多
The dioecious plant,Hippophae rhamnoides,is a pioneer species in community succession on the Qinghai-Tibet Plateau(QTP),plays great roles in various ecosystem services.However,the males and females of the species diff...The dioecious plant,Hippophae rhamnoides,is a pioneer species in community succession on the Qinghai-Tibet Plateau(QTP),plays great roles in various ecosystem services.However,the males and females of the species differ both in their morphology and physiology,resulting in a change in the ratio of male to female plants depending on the environment.To further explore the functional traits critical to this sex-based distinctive response in the alpine grassland,we have surveyed the sex ratios,measured their photosynthetic parameters,height,leaf area and biomass allocation.The results showed that(i)The males had higher Pn,light saturation point,apparent quantum efficiency,A_(max) and lower water-use efficiency(WUE),which exhibited higher utilization efficiency or tolerance to strong light,while the females indicated higher utilization efficiency for low light and water.And it showed sex-specific biomass allocation patterns.(ii)H.rhamnoides populations across the successional stages all showed a male-biased sexual allocation,which was closely related to sex-specific WUE,Pn,root biomass/total biomass and root-crown ratio.(iii)The leaf traits of H.rhamnoides changed from higher N_(area),P_(area) and leaf mass per area in the early and late to lower in the middle,which meant they moved their growth strategy from resource rapid acquisition to conservation as the succession progressed.(iv)The increasing soil total phosphorus mostly contributed to regulating the sex bias of populations and variations of traits during the succession.The results are vital for the management of grassland degradation and restoration due to shrub encroachment on the QTP.展开更多
Improving the highly selective and sensitive binding of chemosensor to target guest is always very challenging.In order to solve this issue,herein,the enrichment effect was introduced into the design of chemosensor mo...Improving the highly selective and sensitive binding of chemosensor to target guest is always very challenging.In order to solve this issue,herein,the enrichment effect was introduced into the design of chemosensor molecule.A novel bi-fused-macrocyclic host molecule BPN1 was synthesized by bridging a pillar[5]arene and a naphthalene diimide(NDI)group through hydrogen-bond-rich chain.In the BPN1,the naphthalimide side ring is outside the cavity of the pillar[5]arene.In addition,Cr(VI)greatly threat human health and the environment due to its severe toxicity,and it is very important to develop effective chemosensor for sensitive and selective detection of Cr_(2)O_(7)^(2-)or its ion pairs.In this paper,the novel bi-fused-macrocyclic host molecule BPN1 can recognize Cr_(2)O_(7)^(2-)with high selectivity and sensitivity.The mechanism of BPN1 recognition of Cr_(2)O_(7)^(2-)was studied through experiments and density functional theory(DFT),the results show that BPN1 could supply enrichment effect to bind Cr_(2)O_(7)^(2-)through multiple weak interactions such as hydrogen bonds and anion-π,and achieve highly sensitive and selective detection of Cr_(2)O_(7)^(2-).It is a significant and feasible strategy for improve high selectivity and sensitivity of host to specific objects by using the enrichment effect of fused bi-macrocyclic.展开更多
Osteoarthritis(OA)has been regarded as a lubrication deficiency related joint disease.Combination of both joint lubrication and drug intervention may provide a promising nonsurgical strategy for treatment of OA.Develo...Osteoarthritis(OA)has been regarded as a lubrication deficiency related joint disease.Combination of both joint lubrication and drug intervention may provide a promising nonsurgical strategy for treatment of OA.Developing novel and simple approaches to fabricate superlubricating nanoparticles with drug release property is highly required.Herein,dopamine triggered one-step polymerization method was employed to fabricate polydopamine/poly(3-sulfopropyl methacrylate potassium salt)(PDA-PSPMA)conjugate coating on hollow silica(h-SiO_(2))nanosphere surfaces to engineer functional nanoparticles(h-SiO_(2)/PDA-PSPMA).The as-prepared h-SiO_(2)/PDA-PSPMA exhibits excellent aqueous lubrication performance on biomaterial substrates as well as natural bovine articular cartilage based on hydration effect of negatively charged PDA-PSPMA coating and"rolling"effect of h-SiO_(2)nanospheres.In vitro drug loading-release experiments demonstrate that PDA-PSPMA coating functionalized h-SiO_(2)nanospheres show high drug-loading and sustained-release capability of an anti-inflammatory drug,diclofenac sodium(DS).Such h-SiO_(2)/PDA-PSPMA nanospheres can be potentially used as a synergistic therapy agent for OA treatment combining by simultaneous joint lubrication anddrugrelease.展开更多
Constructing anodes with fast ions/electrons transfer paths is an effective strategy to achieve high-performance sodium ion batteries(SIBs)/potassium ion batteries(PIBs). Amorphous carbon is a promising candidate anod...Constructing anodes with fast ions/electrons transfer paths is an effective strategy to achieve high-performance sodium ion batteries(SIBs)/potassium ion batteries(PIBs). Amorphous carbon is a promising candidate anode for SIBs/PIBs owing to its disordered carbon layers, abundant defects/pores, and lowcost resources. However, the larger radius of Na^(+)/K^(+) leading to depressed kinetics and poor cycling performance, impeding their further applications. Herein, we propose an efficient strategy to construct of nitrogen, sulfur co-doped hollow carbon nanospheres(NS-HCS) involving an in situ growth of polydopamine on nano-Ni(OH)2template with subsequent sulfur doping process. During the formation process, the produced Ni nanospheres play as the hard template and catalyst for the formation of hollow carbon nanosphere with partially graphite microcrystalline structure, while the sulfur doping process can enlarge the interlayer space and create more defects on the surface of carbon nanospheres, thus synchronous improve the Na^(+)/K^(+) insertion and adsorption ability in NS-HCS. With the synergistic control of the enlarged interlayer spacing, high content of pyridinic N/pyrrolic N and graphitization, a hybrid storage mechanism facilitates the transport kinetics and endows the NS-HCS electrode with high capacities and good cycling stability in SIBs and PIB. Benefit from the multiple effects, NS-HCS exhibits the improved capacity of 274.8 m Ah/g at 0.1 A/g and excellent cycling stability of 149.5 m Ah/g after 5000 cycles at2.5A/g in SIBs, as well as good potassium ion storage behavior with a high capacity retention of 76.5%after 700 cycles at 1.0 A/g, demonstrating the potential applications of NS-HCS for high-performance SIBs and PIBs.展开更多
Rational design of robust non-noble electrocatalysts with numerous oxygen vacancies and highly reactive activity for oxygen reduction reaction(ORR)towards Zn-air batteries is extremely paramount yet challenging.Herein...Rational design of robust non-noble electrocatalysts with numerous oxygen vacancies and highly reactive activity for oxygen reduction reaction(ORR)towards Zn-air batteries is extremely paramount yet challenging.Herein,a novel CeO_(2)C_(2)nanoparticles self-embedded in Fe,N co-doped carbon nanofibers(CeO_(2)C_(2)@Fe-N-C)heterostructure catalyst has been prepared by the in-site dual template assisted electrospinning technique and subsequent high temperature pyrolysis strategy.Thanks to the CeO_(2)C_(2)with oxygen-enriched vacancies and versatile Fe-N-C with rich reactive species and high conductivity,CeO_(2)C_(2)@Fe-N-C catalyst exhibits outstanding catalytic performance in the ORR process,and shows excellent methanol tolerance and cycle stability.In addition,CeO_(2)C_(2)@Fe-N-C delivers a nearly four-electron transfer process in the process of oxygen reduction catalysis,providing a fast-electrochemical kinetic rate,which makes it an efficient air cathode for the Zn-air battery.Importantly,the Zn-air battery fabricated with CeO_(2)C_(2)@Fe-N-C cathode achieves superior performance including large open-circuit voltage(1.5 V)and high specific capacity(780 mAh·g–1 at 10 mA·cm–2)together with superior reversibility and cycling stability,outperforming commercial Pt/C catalyst.The present work introduces a new strategy to design and develop highly active non-noble catalysts and highlights the synergy from heterostructure in oxygen electrocatalysis for advanced Zn-air batteries.展开更多
The construction of multi-responsive supramolecular systems for drug delivery is a challenging task.In this work,a Pd_(2)L_(4) metallacage 1·([BF_(4)]^(−))_(4) with four pyrene units was first designed and synthe...The construction of multi-responsive supramolecular systems for drug delivery is a challenging task.In this work,a Pd_(2)L_(4) metallacage 1·([BF_(4)]^(−))_(4) with four pyrene units was first designed and synthesized through coordination-driven self-assembly.After the introduction ofγ-CD,a supramolecular amphiphile 1–γ-CD was successfully constructed based on the host–guest molecular recognition betweenγ-CD and the pyrene unit of 1·([BF_(4)]^(−))_(4),which further self-assembled into dual-responsive supramolecular vesicles in aqueous solution.DOX·HCl was used as a model molecule to study the drug encapsulation and release behavior of the supramolecular vesicles.By adjusting the pH of the solution to acidic condition or adding a certain amount ofα-amylase,the vesicle structure was destroyed to achieve rapid and effective release of the drug molecules.This study provides an example for the rational design of efficient dual-responsive supramolecular nanocarriers,which have potential application value in the field of controlled drug delivery.展开更多
A series of nickel-doped copper tungstate/oxygen-rich TiO_(2) heterojunction-constructed composites of xNi-CuWO_(4)/OTiO_(2) were successfully prepared to demonstrate the enhancement of the visible-light photoactivity...A series of nickel-doped copper tungstate/oxygen-rich TiO_(2) heterojunction-constructed composites of xNi-CuWO_(4)/OTiO_(2) were successfully prepared to demonstrate the enhancement of the visible-light photoactivity through promoting the photogenerated charge carrier separation efficiency.Of all these composites,0.2Ni-CuWO_(4)/OTiO_(2) exhibits excellent and stable visible light photoactivity for the photooxidative coupling of benzylamine to the corresponding N-benzyl-1-phenymethanimine(BPMI)in air atmosphere.The conversion of benzylamine and the selectivity to BPMI reach 97%and 99%,respectively.The catalyst shows good cyclability with the conversion of benzylamine decreasing just by 22%after being repeated six times with the well-maintained selectivity of BPMI.The composite also exhibits excellent photo-bactericidal ability,which greatly inhibits the reproducing of both the Gram-positive bacteria(e.g.,S.epidermidis)and Gram-negative bacteria(e.g.,E.coli).展开更多
基金the Jilin Province University Cooperative Construction Project-Special Funds for New Materials(No.SXGJSF2017-3)for financial support。
文摘A stimuli-responsive supramolecular polymer network(G-(CN)_(2)⊂BXDSP5)with aggregation-induced emission(AIE)properties has been efficiently constructed by host-guest interactions between pillar[5]arene derivative BXDSP5 and a homoditopic guest G-(CN)_(2),which shows not only excellent fluorescence properties due to the AIE effect but also desirable ion-sensing abilities in both solution and solid states,holding great potential in the applicable fluorescence detection for Fe^(3+).The resultant G-(CN)_(2)⊂BXDSP5 can be transformed into supramolecular polymer gel at high concentration via multiple noncovalent interactions,showing multi-stimuli-responsiveness in response to temperature change,mechanical force,and competitive agent.Meanwhile,the xerogel of supramolecular polymer material has been successfully used to remove Fe^(3+)from water with high adsorption efficiency.In addition,an ionresponsive film based on supramolecular polymer has also been developed,which can serve as a practical and convenient fluorescence test kit for detecting Fe^(3+).
基金the National Natural Science Foundation of China(Nos.42167068 and 22269020)Gansu Province Higher Education Industry Support Plan Project(No.2023CYZC-68)the Hubei Province Outstanding Youth Fund Project(No.2023AFA108).
文摘Covalent triazine frameworks(CTFs)are a class of unique two-dimensional nitrogen-rich triazine framework with adjustable chemical and electronic structures,rich porosity,good stability and excellent semiconductivity,which enable great various applications in efficient gas/molecular adsorption and separation,energy storage and conversion,especially photo-and electrocatalysis.Different synthesis strategies strongly affect the morphology of CTFs and play an important role in their structure and properties.In this concept,we provide a comprehensive and systematic review of the synthesis methods such as ionothermal synthesis,phosphorus pentoxide catalytic method,polycondensation and ultra-strong acid catalyzed method,and applications of CTFs in photo-and electro-catalysis.Finally we offer some insights into the future development progress of CTFs materials for catalytic applications.
基金financially supported by the National Natural Science Foundation of China(Nos.52263033 and 52202081)China Postdoctoral Science Foundation Funded Project(No.2021M690954)+3 种基金Natural Science Foundation of Gansu Province(No.20JR10RA105)the Natural Science Foundation of Hunan Province(No.2022JJ30152)the graduate research funding project of Northwest Normal University(No.2023KYZZ-S157)Natural Science Foundation of Jiangxi Province,China(No.20232BAB204030)。
文摘A series of novel side-chain liquid crystalline(SCLC)copolymers were synthesized by attaching two distinct mesogenic units,namely a chiral cholesteryl-based monomer(M1)and an achiral biphenyl-based monomer(M2),to a poly(3-mercaptopropylmethylsiloxane)(PMMS)backbone via thiol-ene click chemistry.The influence of side chain composition on the self-assembly behavior and phase structures of these SCLC copolymers was systematically investigated using different instrument.Results indicate that three distinct liquid crystalline phases and four unique molecular configurations were identified within the polymer series,with the emergence of the liquid crystalline phase being a synergistic outcome of the two distinct side chains.This study underscores the critical influence of side chain dimensions,rigidity,and spatial volume on the self-assembly structures and phase characteristics of liquid crystalline polymers,providing valuable insights for the rational design and development of advanced functional materials with tailored properties.
基金supported by the National Natural Science Foundation of China(Nos.21661028,21662031,21574104)the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(No.IRT 15R56)。
文摘An ultrasensitive detection and effective removal material was successfully developed by using a pillar[n]arene-based supramolecular polymer gel(MTP5?HB).The MTP5?HB can ultrasensitively recognize Cu^2+and Fe^3+,and the limits of detection(LODs)for Cu^2+and Fe^3+are 1.55 and 2.68 nmol/L,respectively.Additionally,the in-situ generated metallogel MTP5?HB-Cu can exclusively detect CN,and the LOD for CN is 1.13 nmol/L.Noticeably,the xerogel of MTP5?HB-Cu can effectively remove CN from aqueous solution with 94.40%removal rate.Test kit based on MTP5?HB-Cu is also prepared for convenient detection of CN.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.22065031,22061039)the Top Leading Talents Project of Gansu Province,the Key R&D program of Gansu Province(No.21YF5GA066)+1 种基金Gansu Province College Industry Support Plan Project(No.2022CYZC-18)Natural Science Foundation of Gansu Province(Nos.2020-0405-JCC-630,20JR10RA088).
文摘Hydrazine hydrate(DH)is an important fine chemical intermediate and as fuel for rockets,however,it also has serious toxic for humans and environment.Developing novel materials and methods for sensitive detection of DH in water and air is an important task.In order to effectively detect DH,a novel conductive supramolecular polymer metallogel(PQ-Ag)has been constructed by the coordination of bis-5-hydroxyquinoline functionalized pillar[5]arene(PQ5)with Ag+.The metallogel PQ-Ag could realize the multi-channel sensitive detection of DH through naked-eye,fluorescence,and electrochemical methods.The lowest limit of detection(LOD)is 0.1 mg/m^(3)in air and 2.68×10^(−8)mol/L in water,which is lower than the standard of the US Environmental Protection Agency(EPA)for DH of maximum allowable concentration in drinking water.More importantly,an electronic device for DH detection based on the metallogel PQ-Ag was designed and prepared,which can realize conveniently and efficiently multi-channel detection and alert of DH through sound and light alarms not only in water but also in air.
基金supported by the National Natural Science Foundation of China (NSFC, Nos. 22065031, 22061039)the Key R&D program of Gansu Province (No. 21YF5GA066)+2 种基金Natural Science Foundation of Gansu Province (Nos. 2020-0405-JCC-630, 20JR10RA088)Fundamental Research Funds for the Central Universities (Nos. 31920190041, 31920200002, 31920190018,31920190013)Young Doctor Foundation of Gansu Province(No. 2021QB-148)。
文摘The effective materials and methods for detection and separation of pesticides are urgently needed because most of pesticides show very harmful influence on life and environment. As a new kind of macrocyclic host compound, pillar[n]arenes show very good performance in the detection and separation of pesticides, especially for paraquat(PQ). For the pesticide detection and separation materials, their structures determine performance. Therefore, this review summarizes the recent progress of pillar[n]arenes-based materials for detection and separation of pesticides covering single/multi-pillar[n]arenes, pillar[n]arenes-based polymers, frameworks, composites, nanomaterials, etc.The structure-performance relationships of these materials have been discussed according to the cavity size, the synergistic or collaboration effect, the structure of the polymer or framework, the substrate of the composites and the size of nanomaterials and so on. Based on these, we also look forward to the future and point out the possible way for improving the pesticides detection sensitivity and separation efficiency of this kind of materials.
基金This work was supported by the National Natural Science Foundation of China(NSFC)(Nos.22065031,22061039)the Natural Science Foundation of Gansu Province(Nos.2020-0405-JCC-630,20JR10RA088)the Fundamental Research Funds for the Central Universities(Nos.31920190041,31920200002,31920190018,31920190013).
文摘Pillar[5]arene-based supramolecular polymer gels(SPGs)show broad application prospects.To investigate the influence of the supramolecular monomers'structure on the assembly and properties of corresponding pillar[5]arene-based SPGs,a series of monomers based on different functionalized pillar[5]arene derivatives with various structures were synthesized.There are per-methylated pillar[5]arene(H1),bromobutane-functionalized pillar[5]arene(H2),4-hydroxybenzaldehyde-functionalized pillar[5]arene(H3),ethyl thioglycolate-functionalized pillar[5]arene(H4),thioacetylhydrazine-functionalized pillar[5]arene(H5),bola-type bis-pillar[5]arene(H6)and tripodal-type tri-pillar[5]arene(H7).Meanwhile,a neutral tripodal-guest TG was also employed to co-assemble with these pillar[5]arene-based monomers by host-guest interactions.As a result,under the same conditions(10%,DMSO-H_(2)O,w/v,10 mg·mL^(-1)=1%),H1 and H2 cannot assemble into SPGs with TG.Interestingly,mono-p[5]derivatives H3—H5 could assemble into SPGs with TG.More importantly,bis-p[5]H6 and tri-p[5]H7 could assemble into supramolecular polymer network gel(SPNG)and supramolecular polymer organic framework gel(SOFG)with TG,respectively.These gels all show blue aggregation-induced emission(ALE)properties.Among these SPGs,the SPNG shows the best viscoelastic behavior and self-healing properties.The result is attributed to the flexible network structure of SPNGs.In addition,the xerogels of SOFG and SPNG have shown nice adsorption and separation properties for organic dyes in water solution.
基金the Science and Technology Planning Project of Gansu Province,China(18JR4RA002)the Qilian Mountains Eco-Environment Research Center in Gansu Province,Northwest Institute of Eco-Environment and Resources,Chinese Academy of Sciences(QLS202002).
文摘Altitude affects leaf stoichiometry by regulating temperature and precipitation,and influencing soil properties in mountain ecosystems.Leaf carbon concentration(C),leaf nitrogen concentration(N),leaf phosphorous concentration(P),and their stoichiometric ratios of Leontopodium lentopodioides(Willd.)Beauv.,a widespread species in degraded grasslands,were investigated to explore its response and adaptation strategy to environmental changes along four altitude gradients(2500,3000,3500,and 3800 m a.s.l.)on the northeastern Qinghai-Tibetan Plateau(QTP),China.The leaf C significantly varied but without any clear trend with increasing altitude.Leaf N showed an increasing trend,and leaf P showed a little change with increasing altitude,with a lower value of leaf P at 3500 m than those at other altitudes.Similarity,leaf C:P and N:P exhibited a little change with increasing altitude,which both had greater values at 3500 m than those at other altitudes.However,leaf C:N exhibited a decreasing trend with increasing altitude.Soil NH^(+)_(4)-N,soil pH,soil total phosphorus(STP),mean annual temperature(MAT),and mean annual precipitation(MAP)were identified as the main factors driving the variations in leaf stoichiometry of L.lentopodioides across all altitudes,with NH^(+)_(4)-N alone accounting for 50.8%of its total variation.Specifically,leaf C and N were mainly controlled by MAT,soil pH,and NH^(+)_(4)-N,while leaf P by MAP and STP.In the study area,it seems that the growth of L.lentopodioides may be mainly limited by STP.The results could help to strengthen our understanding of the plasticity of plant growth to environmental changes and provide new information on global grassland management and restoration.
基金This work was supported by the National Key Research and Development Program of China(2020YFB1506400).
文摘CONSPECTUS:Perylene diimide(PDI)as a classical dye has some advantages,such as structural diversity,tunable optical and electronic properties,strong light absorption,high electron affinity,and good electron-transporting properties and stability.The PDI-based oligomers and polymers are good candidates for n-type semiconductors in organic electronics and photonic devices.A polymer solar cell(PSC)that converts sunlight into electricity is a promising renewable and clean energy technology and has some superiorities,such as simple preparation and being lightweight,low cost,semitransparent,and flexible.For a long time,fullerene derivatives(e.g.,PCBM)have been the most important electron acceptors used in the active layer of PSCs.However,PCBM suffers from some disadvantages,for example,weak absorption,a large amount of energy loss,and unstable morphology.Compared to PCBM,PDI-based materials present some advantages:intense visible-light absorption;lowest unoccupied molecular orbital(LUMO)energy levels can be modulated to achieve a suitable charge separation driving force and high open-circuit voltage(V_(OC));and the molecular configuration can be adjusted to achieve morphology stability.Thus,PDI-based oligomers and polymers are widely used as electron acceptors in the active layer of PSCs.In addition,PDI-based oligomers and polymers are widely used as n-type semiconductors in other electronic and photonic devices,such as organic field-effect transistors(OFETs),light-emitting diodes,lasers,optical switches,and photodetectors.
基金This study was financially supported by the National Natural Science Foundation of China(No.22165028)the Nature Science Foundation of Gansu Province(No.20JR10RA108).
文摘Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.
基金supported by the NSFC(Nos.22065031,22061039,22001214,22165027)the Fundamental Research Funds for the Central Universities(No.31920230145)+4 种基金the Top-Notch Talent Project in Gansu Province,the Key R&D Program of Gansu Province(No.21YF5GA066)Gansu Province College Industry Support Plan Project(No.2022CYZC-18)Natural Science Foundation of Gansu Province(Nos.2020-0405-JCC-630,20JR10RA088,21JR1RA220)Gansu Province Science Foundation for Youths(23JRRA690)Northwest Normal University Young Scholars Research Capacity Improvement Program(NWNU-LKQN2023-05).
文摘The cyanide anion(CN^(–))is known to be one of the most toxic anions.Therefore,there is an urgent need to develop a reliable,sensitive,selective,rapid and effective method for the detection of CN^(–).Here,a self-assembly strategy based on pillar[5]arene P5 and azine derivative AZ was used to construct supramolecular sensors,and it was found that the detection effect of CN^(–)was significantly improved by the assembly strategy.The sensitivity of the assembled sensor P5-AZ to CN^(–)is more than 10 times higher than that of AZ.The detect mechanism was further investigated by theoretical calculations and 1H NMR.The results showed that AZ detects CN–by a deprotonation process with fluorescence enhancement,while P5-AZ improves the sensitivity of CN^(–)recognition through hydrogen bonding,anion-πand anion-dipole interactions,as well as the strong bonding ability of the assembly.Supramolecular assembly P5-AZ has the advantages of low toxicity,high sensitivity,and more importantly,it provides a method to detect CN^(–)sensitivity in the aqueous phase and organisms by host-guest assembly.
基金financially supported by National Natural Science Foundation of China (Nos.51872245, 52103269)the Natural Science Key Foundation of Gansu Province+4 种基金China (No.23JRRA680)the Excellent Doctoral Student Project of Natural Science Foundation of Gansu Province (No.23JRRA695)the Gansu Province University Industrial Support Plan Project (No.2023CYZC-16)the Science and Technology Development Plan Project of Lanzhou City(No.2022-2-78)the Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional Materials and Longyuan Young Talent for financial support。
文摘In an era where the concept of green development is deeply rooted, magnesium(Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products.Herein, three-dimensional mesopore hollow polypyrrole spheres(MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride(h-BN) lamellae, which allowed the hBN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/hBN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface(SHS). Finally, the slippery liquid infused porous surface(SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.
基金supported by National Natural Science Foundation of China(32201525)the Gansu province’s Key Research and Development Plan(21YF5NA069)+2 种基金the Longyuan Talent Youth Innovation and Entrepreneurship Team projectthe Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education(YDZX20216200001007)the Foreign Expert Introduction Special Project of Gansu Province(22JR10KA010).
文摘The dioecious plant,Hippophae rhamnoides,is a pioneer species in community succession on the Qinghai-Tibet Plateau(QTP),plays great roles in various ecosystem services.However,the males and females of the species differ both in their morphology and physiology,resulting in a change in the ratio of male to female plants depending on the environment.To further explore the functional traits critical to this sex-based distinctive response in the alpine grassland,we have surveyed the sex ratios,measured their photosynthetic parameters,height,leaf area and biomass allocation.The results showed that(i)The males had higher Pn,light saturation point,apparent quantum efficiency,A_(max) and lower water-use efficiency(WUE),which exhibited higher utilization efficiency or tolerance to strong light,while the females indicated higher utilization efficiency for low light and water.And it showed sex-specific biomass allocation patterns.(ii)H.rhamnoides populations across the successional stages all showed a male-biased sexual allocation,which was closely related to sex-specific WUE,Pn,root biomass/total biomass and root-crown ratio.(iii)The leaf traits of H.rhamnoides changed from higher N_(area),P_(area) and leaf mass per area in the early and late to lower in the middle,which meant they moved their growth strategy from resource rapid acquisition to conservation as the succession progressed.(iv)The increasing soil total phosphorus mostly contributed to regulating the sex bias of populations and variations of traits during the succession.The results are vital for the management of grassland degradation and restoration due to shrub encroachment on the QTP.
基金This research was funded by the National Natural Science Foundation of China(42361041)the innovation project of education technology,Gansu Education Department(2022B-090).
基金supported by the National Natural Science Foundation of China(NSFC,Nos.22065031,22061039,22001214,22165027)the top-notch talent project in Gansu province,the Key R&D Program of Gansu Province(No.21YF5GA066)+2 种基金Gansu Province College Industry Support Plan Project(No.2022CYZC-18)Natural Science Foundation of Gansu Province(Nos.2020–0405-JCC-630,20JR10RA088)The star of innovation(No.2023CXZX244)。
文摘Improving the highly selective and sensitive binding of chemosensor to target guest is always very challenging.In order to solve this issue,herein,the enrichment effect was introduced into the design of chemosensor molecule.A novel bi-fused-macrocyclic host molecule BPN1 was synthesized by bridging a pillar[5]arene and a naphthalene diimide(NDI)group through hydrogen-bond-rich chain.In the BPN1,the naphthalimide side ring is outside the cavity of the pillar[5]arene.In addition,Cr(VI)greatly threat human health and the environment due to its severe toxicity,and it is very important to develop effective chemosensor for sensitive and selective detection of Cr_(2)O_(7)^(2-)or its ion pairs.In this paper,the novel bi-fused-macrocyclic host molecule BPN1 can recognize Cr_(2)O_(7)^(2-)with high selectivity and sensitivity.The mechanism of BPN1 recognition of Cr_(2)O_(7)^(2-)was studied through experiments and density functional theory(DFT),the results show that BPN1 could supply enrichment effect to bind Cr_(2)O_(7)^(2-)through multiple weak interactions such as hydrogen bonds and anion-π,and achieve highly sensitive and selective detection of Cr_(2)O_(7)^(2-).It is a significant and feasible strategy for improve high selectivity and sensitivity of host to specific objects by using the enrichment effect of fused bi-macrocyclic.
基金This work was financially supported by National Natural Science Foundation of China(52065061,22032006)Outstanding Youth Fund of Gansu Province(21JR7RA158,21JR7RA095)+1 种基金Innovation Fund for Universities of Gansu Province(2021A-015)Youth Innovation Promotion Association CAS(2019411).
文摘Osteoarthritis(OA)has been regarded as a lubrication deficiency related joint disease.Combination of both joint lubrication and drug intervention may provide a promising nonsurgical strategy for treatment of OA.Developing novel and simple approaches to fabricate superlubricating nanoparticles with drug release property is highly required.Herein,dopamine triggered one-step polymerization method was employed to fabricate polydopamine/poly(3-sulfopropyl methacrylate potassium salt)(PDA-PSPMA)conjugate coating on hollow silica(h-SiO_(2))nanosphere surfaces to engineer functional nanoparticles(h-SiO_(2)/PDA-PSPMA).The as-prepared h-SiO_(2)/PDA-PSPMA exhibits excellent aqueous lubrication performance on biomaterial substrates as well as natural bovine articular cartilage based on hydration effect of negatively charged PDA-PSPMA coating and"rolling"effect of h-SiO_(2)nanospheres.In vitro drug loading-release experiments demonstrate that PDA-PSPMA coating functionalized h-SiO_(2)nanospheres show high drug-loading and sustained-release capability of an anti-inflammatory drug,diclofenac sodium(DS).Such h-SiO_(2)/PDA-PSPMA nanospheres can be potentially used as a synergistic therapy agent for OA treatment combining by simultaneous joint lubrication anddrugrelease.
基金supported by the National Natural Science Foundation of China (No. 22165028)the Nature Science Foundation of Gansu Province (No. 20JR10RA108)the Innovation Fund of Gansu Universities (No. 2020A-013)。
文摘Constructing anodes with fast ions/electrons transfer paths is an effective strategy to achieve high-performance sodium ion batteries(SIBs)/potassium ion batteries(PIBs). Amorphous carbon is a promising candidate anode for SIBs/PIBs owing to its disordered carbon layers, abundant defects/pores, and lowcost resources. However, the larger radius of Na^(+)/K^(+) leading to depressed kinetics and poor cycling performance, impeding their further applications. Herein, we propose an efficient strategy to construct of nitrogen, sulfur co-doped hollow carbon nanospheres(NS-HCS) involving an in situ growth of polydopamine on nano-Ni(OH)2template with subsequent sulfur doping process. During the formation process, the produced Ni nanospheres play as the hard template and catalyst for the formation of hollow carbon nanosphere with partially graphite microcrystalline structure, while the sulfur doping process can enlarge the interlayer space and create more defects on the surface of carbon nanospheres, thus synchronous improve the Na^(+)/K^(+) insertion and adsorption ability in NS-HCS. With the synergistic control of the enlarged interlayer spacing, high content of pyridinic N/pyrrolic N and graphitization, a hybrid storage mechanism facilitates the transport kinetics and endows the NS-HCS electrode with high capacities and good cycling stability in SIBs and PIB. Benefit from the multiple effects, NS-HCS exhibits the improved capacity of 274.8 m Ah/g at 0.1 A/g and excellent cycling stability of 149.5 m Ah/g after 5000 cycles at2.5A/g in SIBs, as well as good potassium ion storage behavior with a high capacity retention of 76.5%after 700 cycles at 1.0 A/g, demonstrating the potential applications of NS-HCS for high-performance SIBs and PIBs.
基金supported by the National Natural Science Foundation of China(Nos.42167068,51863019)Outstanding Youth Fund of Gansu Province(20JR5RA539)Gansu Province Higher Education Industry Support Plan Project(2021CYZC-09).
文摘Rational design of robust non-noble electrocatalysts with numerous oxygen vacancies and highly reactive activity for oxygen reduction reaction(ORR)towards Zn-air batteries is extremely paramount yet challenging.Herein,a novel CeO_(2)C_(2)nanoparticles self-embedded in Fe,N co-doped carbon nanofibers(CeO_(2)C_(2)@Fe-N-C)heterostructure catalyst has been prepared by the in-site dual template assisted electrospinning technique and subsequent high temperature pyrolysis strategy.Thanks to the CeO_(2)C_(2)with oxygen-enriched vacancies and versatile Fe-N-C with rich reactive species and high conductivity,CeO_(2)C_(2)@Fe-N-C catalyst exhibits outstanding catalytic performance in the ORR process,and shows excellent methanol tolerance and cycle stability.In addition,CeO_(2)C_(2)@Fe-N-C delivers a nearly four-electron transfer process in the process of oxygen reduction catalysis,providing a fast-electrochemical kinetic rate,which makes it an efficient air cathode for the Zn-air battery.Importantly,the Zn-air battery fabricated with CeO_(2)C_(2)@Fe-N-C cathode achieves superior performance including large open-circuit voltage(1.5 V)and high specific capacity(780 mAh·g–1 at 10 mA·cm–2)together with superior reversibility and cycling stability,outperforming commercial Pt/C catalyst.The present work introduces a new strategy to design and develop highly active non-noble catalysts and highlights the synergy from heterostructure in oxygen electrocatalysis for advanced Zn-air batteries.
基金supported by the National Natural Science Foundation of China(22001214,21662031,21661028,22061039)B.S.thanks the Natural Science Foundation of Northwest Normal University(NWNU-LKQN2020-02)for financial support.
文摘The construction of multi-responsive supramolecular systems for drug delivery is a challenging task.In this work,a Pd_(2)L_(4) metallacage 1·([BF_(4)]^(−))_(4) with four pyrene units was first designed and synthesized through coordination-driven self-assembly.After the introduction ofγ-CD,a supramolecular amphiphile 1–γ-CD was successfully constructed based on the host–guest molecular recognition betweenγ-CD and the pyrene unit of 1·([BF_(4)]^(−))_(4),which further self-assembled into dual-responsive supramolecular vesicles in aqueous solution.DOX·HCl was used as a model molecule to study the drug encapsulation and release behavior of the supramolecular vesicles.By adjusting the pH of the solution to acidic condition or adding a certain amount ofα-amylase,the vesicle structure was destroyed to achieve rapid and effective release of the drug molecules.This study provides an example for the rational design of efficient dual-responsive supramolecular nanocarriers,which have potential application value in the field of controlled drug delivery.
基金financially supported by NSFC(52063026,21563026)the Program for Changjiang Scholars and Innovative Research Team in University(IRT15R56)+2 种基金the Innovation Team Basic Scientific Research Project of Gansu Province(1606RJIA324)the Science,Technology Program of GansuProvince(19JR2RA020)Education Department of Gansu Province:Excellent Graduate Student"lnnovation Star"Project(2021CXZX001).
文摘A series of nickel-doped copper tungstate/oxygen-rich TiO_(2) heterojunction-constructed composites of xNi-CuWO_(4)/OTiO_(2) were successfully prepared to demonstrate the enhancement of the visible-light photoactivity through promoting the photogenerated charge carrier separation efficiency.Of all these composites,0.2Ni-CuWO_(4)/OTiO_(2) exhibits excellent and stable visible light photoactivity for the photooxidative coupling of benzylamine to the corresponding N-benzyl-1-phenymethanimine(BPMI)in air atmosphere.The conversion of benzylamine and the selectivity to BPMI reach 97%and 99%,respectively.The catalyst shows good cyclability with the conversion of benzylamine decreasing just by 22%after being repeated six times with the well-maintained selectivity of BPMI.The composite also exhibits excellent photo-bactericidal ability,which greatly inhibits the reproducing of both the Gram-positive bacteria(e.g.,S.epidermidis)and Gram-negative bacteria(e.g.,E.coli).