Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_...Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.展开更多
Fluorinated fused azobenzene boron(FBAz)is a novel electron-deficient building block for polymer electron acceptors in all-polymer solar cells(all-PSC).The B←N bridging units impart a fixed configuration and low-lyin...Fluorinated fused azobenzene boron(FBAz)is a novel electron-deficient building block for polymer electron acceptors in all-polymer solar cells(all-PSC).The B←N bridging units impart a fixed configuration and low-lying LUMO/HOMO energy.Three polymer acceptor materials(P2f,P3f and P5f)with different fluorine substitution positions by copolymerizing FBAz with indacenodithiophene(IDT),are synthesized and investigated to study the influence of fluorinated forms on the all-polymer solar cell performance.The FBAz units are synthesized in just three steps,facilitating the straightforward production of polymer acceptors P2f,P3f,and P5f.These acceptors exhibit strong light absorption in the visible to near-infrared range of 500-1000nm and possess suitable LUMO/HOMO energy levels of-3.99/-5.66 eV which are very complementary to that(E_(LUMO/HOMO)=-3.59/-5.20 eV)of the widely-used polymer donor poly[(ethylhexylthiophenyl)-benzodithiophene-(ethylhexyl)-thienothiophene](PTB7-Th).All-polymer solar cells(all-PSCs)with PTB7-Th as electron donor and P3f as electron acceptor exhibits highest power conversion efficiencies(PCE)2.70%.When PC_(61)BM is added as the third component,the device efficiency can reach 5.36%.These preliminary results indicate that FBAz is a promising strong electron acceptor for the development of n-type polymer semiconductors,especially in organic photovoltaics(OPVs).To the best of our knowledge,this is the first example demonstrating the unique photovoltaic properties of the N=N double bond as an acceptor material.展开更多
Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion bat...Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion batteries.However,the influence of dual exposure to air and liquid water as well as the heating treatment during aqueous slurry electrode processing on the high-nickel layered oxide electrode is yet to be understood.In this study,we systematically investigate the structural evolution and electro-chemical behaviors when LiNi_(0.83)Mn_(0.05)Co_(0.12)O_(2)(NMC83)is subjected to aqueous slurry processing.It was observed that the crystal structure near the surface of NMC83 is partially reconstructed to contain a mixture of rock-salt and layered phases when exposed to water,leading to the deteriorated rate capability of the NMC83 electrodes.This partial surface reconstruction layer completely converts into a pure rock-salt phase upon cycling,accompanied by the release of O_(2),Ni leaching,catalyzed decomposition of the electrolyte,and the formation of a thick cathode electrolyte interphase layer.The byproducts of the electrolyte and dissolved Ni could shuttle to the Li metal side,causing a crosstalk effect that results in a thick and unstable solid electrolyte interphase layer on the Li surface.These in combination severely undermined the cycling stability of the NMC83 electrodes obtained from the aqueous slurry.A mitigation strategy using molecular self-assembly technique was demonstrated to enhance the surface stability of water-treated NMC83.Our findings offer new insights for tailoring ambient environment stability and aqueous slurry processability for ultra-high nickel layered oxide and other water-sensitive cathode materials.展开更多
Periodontitis is an inflammatory disease caused by oxidative stress and initiated by bacterial infection.The endogenous enzyme system is dysfunctional in the periodontitis microenvironment.Currently,traditional clinic...Periodontitis is an inflammatory disease caused by oxidative stress and initiated by bacterial infection.The endogenous enzyme system is dysfunctional in the periodontitis microenvironment.Currently,traditional clinical treatment cannot efficiently eliminate bacteria or relieve inflammation.To address this issue,we developed ultrasmall ruthenium nanoparticles(US-RuNPs)with multienzyme-like activity.Our results indicated that US-RuNPs with an amplified electric field had a superior photothermal effect to large-sized RuNPs.Thus,US-RuNPs,through photothermal therapy(PTT),acted as“bacterial lysozyme”to eliminate planktonic pathogens and biofilms.In addition,the antioxidant enzyme-like activity of US-RuNPs was greater than that of large-sized RuNPs,and US-RuNPs could scavenge intracellular reactive oxygen species(ROS)and inhibit inflammation-related responses.More importantly,US-RuNPs demonstrated a satisfactory effect against periodontitis in vivo due to their synergistic antibacterial activity through PTT and antioxidant effects even in deep sites,decreasing the alveolar bone loss to root length ratio(ABL/RL)from 70.70%to 20.15%and increasing the collagen volume fraction from 16.88%to 57.64%.Thus,US-RuNPs with approximately 2 nm diameter,mimicking multienzyme activity,have great potential for the treatment of periodontitis.展开更多
Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction ...Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.展开更多
RNA offers distinct advantages for molecular self-assembly as a unique and programmable biomaterial.Recently,single-stranded RNA(ssRNA)origamis,capable of self-folding into defined nanostructures within a single-stran...RNA offers distinct advantages for molecular self-assembly as a unique and programmable biomaterial.Recently,single-stranded RNA(ssRNA)origamis,capable of self-folding into defined nanostructures within a single-stranded RNA molecule,are considered a promising platform for immune recognition and therapy.Here,we utilize single-stranded rod RNA origami(Rod RNA-OG)as functional nucleic acid to synthesize valence-programmed RNA structures in a one-pot manner.We discover that the polyvalent RNA origamis are resistant to RNase degradation and can be efficiently internalized by macrophages for subsequent innate immune activation,even in the absence of any external protective agents such as lipids or polymers.The valence-programmed RNA origamis thus hold great promise as novel agonists for immunotherapy.展开更多
Designing Fischer-Tropsch synthesis(FTS)catalysts to selectively produce liquid hydrocarbon fuels is a crucial challenge.Herein,we selectively introduced Co nanoparticles(NPs)into the micropores and mesopores of an or...Designing Fischer-Tropsch synthesis(FTS)catalysts to selectively produce liquid hydrocarbon fuels is a crucial challenge.Herein,we selectively introduced Co nanoparticles(NPs)into the micropores and mesopores of an ordered mesoporous MFI zeolite(OMMZ)through impregnation,which controlled the carbon number distribution in the FTS products by tuning the position of catalytic active sites in differently sized pores.The Co precursors coordinated by acetate with a size of 9.4×4.2×2.5Åand by 2,2'-bipyridine with a size of 9.5×8.7×7.9Å,smaller and larger than the micropores(ca.5.5Å)of MFI,made the Co species incorporated in OMMZ's micropores and mesopores,respectively.The carbon number products synthesized with the Co NPs confined in mesopores were larger than that in micropores.The high jet and diesel selectivities of 66.5%and 65.3%were achieved with Co NPs confined in micropores and mesopores of less acidic Na-type OMMZ,respectively.Gasoline and jet selectivities of 76.7%and 70.8%were achieved with Co NPs confined in micropores and mesopores of H-type OMMZ with Brönsted acid sites,respectively.A series of characterizations revealed that the selective production of diesel and jet fuels was due to the C-C cleavage suppressing of heavier hydrocarbons by the Co NPs located in mesopores.展开更多
The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is...The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is both robust and readily-functionalized through interfacial click polymerization.A water-in-oil emulsion was constructed to act as the reaction medium,the hydrophilic 1,3-butadiene diepoxide(BDE)in water phase reacted with the oleophilic 1,4-dibutanedithiol(BDT)in oil phase at the water-oil interface to form the amphiphilic ACP named poly(2,3-dihydroxy butylene-alt-butylene dithioether)(abbreviated as P(DHB-a-BDT)below),which would deposite in situ to form the micro-sized capsules.Significantly,the dried capsules are robust enough to be rehydrated once the water was added and almost restored their original morphologies.Further elucidation showed that the Young's modulus of these capsules exceeded 1 GPa.As long as we know,it is the first time for the mechanical properties of the ACP-based microstructures being investigated.Besides,functionalization could be achieved simultaneously with the formation process.As a proof of concept,positive-charged capsules were successfully obtained through click copolymerization.Stemming from the unique characteristics of amphiphilic ACPs which combined both merits of click chemistry and interfacial reactions,all these features of the current method as well as the resultant capsules may promote the application of the polymeric capsules.展开更多
Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible trans...Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible transmittance(AVT)and power conversion efficiency(PCE)remains a key issue of STOPVs.Herein,we innovatively applied a surface texturization strategy by integrating with a pseudo-planar heterojunction(PPHJ)structure to fabricate ST-OPVs,which possess outstanding photoelectric conversion and light management capability.The textured active layer performs significantly improved light capture capability and reduced optical loss due to that the micro-patterned arrays can deflect incident light multiple times.Moreover,the surface texturization strategy can enhance the crystallinity of the active layer and precisely control donor/acceptor inter-penetration,which magnifies exciton dissociation interface and forms ordered carrier dynamics.Consequently,the textured opaque device via blade-coating performs a record PCE of 19.17%(certified 19.02%)and the semi-transparent device achieves one of the highest light utilization efficiency(LUE)of 5.54%with prominent PCE(14.40%)and AVT(38.43%).Most importantly,the excellent thermal insulation performance and color rendering index of ST-OPVs are fitting for the agricultural greenhouses and insulation roofing,which shows that the surface texturization strategy can provide promising application prospects for ST-OPVs in economically sustainable agricultural development.展开更多
The structural change-mediated catalytic activity regulation plays a significant role in the biological functions of natural enzymes.However,there is virtually no artificial nanozyme reported that can achieve natural ...The structural change-mediated catalytic activity regulation plays a significant role in the biological functions of natural enzymes.However,there is virtually no artificial nanozyme reported that can achieve natural enzyme-like stringent spatiotemporal structure-based catalytic activity regulation.Here,we report a subnanostructural transformable gold@ceria(STGC-PEG)nanozyme that performs tunable catalytic activities via near-infrared(NIR)light-mediated sub-nanostructural transformation.The gold core in STGC-PEG can generate energetic hot electrons upon NIR irradiation,wherein an internal sub-nanostructural transformation is initiated by the conversion between CeO;and electron-rich state of CeO;-x,and active oxygen vacancies generation via the hot-electron injection.Interestingly,the sub-nanostructural transformation of STGC-PEG enhances peroxidase-like activity and unprecedentedly activates plasmon-promoted oxidase-like activity,allowing highly efficient low-power NIR light(50 m W cm;)-activated photocatalytic therapy of tumors.Our atomic-level design and fabrication provide a platform to precisely regulate the catalytic activities of nanozymes via a light-mediated sub-nanostructural transformation,approaching natural enzyme-like activity control in complex living systems.展开更多
Herein,we designed and constructed two metallacycles,1 and 2,to illustrate the conformational effect of isomeric AIE fluoropho res on the platfo rm of supramolecular coordination complexe s(SCCs).Specifically,the dang...Herein,we designed and constructed two metallacycles,1 and 2,to illustrate the conformational effect of isomeric AIE fluoropho res on the platfo rm of supramolecular coordination complexe s(SCCs).Specifically,the dangling phenyl rings in TPE units of the metallacycle 1 align completely outside the main cyclic structure,while in the metallacycle 2,these phenyl rings align half inside and half outside.The experimental results showed that two metallacycles exhibited different behaviors in terms of AIE fluorescence and chemical sensing,which could be attributed to the subtle structural difference of the TPE units.This work repre sents the unification of topics such as self-assembly,AIE,and chemical sensing,and further promotes the understanding for the structure-property relationship of isomeric AIE fluorophores.展开更多
The morphology manipulation of the active layers is important for improving the performance of organic photovoltaics(OPVs).The choice of processing solvent has great impact on the crystallization and phase separation ...The morphology manipulation of the active layers is important for improving the performance of organic photovoltaics(OPVs).The choice of processing solvent has great impact on the crystallization and phase separation during film formation,since solvent properties,including solvent effect on molecular crystallization,boiling point,and interaction parameters,can directly change the evolution pathways associated with thermodynamics and kinetics.Therefore,revealing the underlying solvent-regulated morphology mechanism is potential to provide guiding strategies for device optimization.In this study,chloroform,chlorobenzene,and toluene are used to process PM6:Y6 blends by slot-die printing to fabricate OPV devices.The chloroform printed film forms a fibrillar network morphology with enhanced crystallization,facilitating exciton dissociation,charge transport and extraction,resulting in an optimal power conversion efficiency of 16.22%.However,the addition of the additive chloronaphthalene in chloroform solution leads to over-crystallization of Y6,and thus,increasing domain size that exceeds the exciton diffusion length,resulting in lower device efficiency.In addition,both the chlorobenzene and toluene suppress the crystallization of Y6,which drastically decreased short-circuit current and fill factor.These results demonstrate the important role of processing solvent in dictating film morphology,which critically connects with the resultant printed OPV performance.展开更多
Quasi-two-dimensional(q2 D)conducting polymer thin film synergizes the advantageous features of longrange molecular ordering and high intrinsic conductivity,which are promising for flexible thin film-based micro-super...Quasi-two-dimensional(q2 D)conducting polymer thin film synergizes the advantageous features of longrange molecular ordering and high intrinsic conductivity,which are promising for flexible thin film-based micro-supercapacitors(MSCs).Herein,we present the high-performance flexible MSCs based on highly ordered quasi-two-dimensional polyaniline(q2 D-PANI)thin film using surfactant monolayer assisted interfacial synthesis(SMAIS).Owing to high electrical conductivity,rich redox chemistry,and thin-film morphology,the q2 D-PANI MSCs show high volumetric specific capacitance(ca.360 F/cm^(3))and energy density(17.9 m Wh/cm^(3)),which outperform the state-of-art PANI thin-film based MSCs and promise for future flexible electronics.展开更多
Dear Editor,Artemisinin,which has potent antimalarial properties,is a sesquiterpene endoperoxide originally isolated from the traditional Chinese medicinal plant Artemisia annua.However,the artemisinin content in wild...Dear Editor,Artemisinin,which has potent antimalarial properties,is a sesquiterpene endoperoxide originally isolated from the traditional Chinese medicinal plant Artemisia annua.However,the artemisinin content in wild-type(WT)A.annua is low(1-10 mg/g dry weight),leading to its erratic supply and price fluctuations[1].展开更多
Aqueous rechargeable Ni−Zn batteries are considered as a new generation of safe and reliable electro-chemical energy storage system.However,low electronic conductivity of Ni-based cathodes hinders the practical applic...Aqueous rechargeable Ni−Zn batteries are considered as a new generation of safe and reliable electro-chemical energy storage system.However,low electronic conductivity of Ni-based cathodes hinders the practical application of Ni-Zn batteries.This problem can be overcome by compositing the Ni-based cath-ode with highly conductive carbon substrates.A chemical oxidation pre-treatment is popularly applied to the carbon substrates to increase their hydrophilicity and thus facilitate the growth of active materials in aqueous systems.However,the anodic stability of the oxidized carbon substrates is greatly challenged,which has never been addressed in previous reports.In this work,we first compared the anodic stabil-ity of carbon fiber paper with and without oxidation treatment and find that carbon substrate with the chemical treatment caused remarkable oxidization current in the required voltage range.To take both anodic stability and fine growth of active materials into account,here we demonstrated a facile physical surface-treatment method of ethanol wetting to replace the chemical treatment.The ethanol infiltration removes gas adsorption on carbon substrates and thus promotes their hydrophilicity.This cost-effective strategy simultaneously achieves a high anodic stability and a fine growth and uniform distribution of nickel-cobalt hydroxide on the carbon microfibers.The resulting Ni-Zn battery provides a high discharge capacity of 219 mAh/g with an operation cell voltage of 1.75 V.展开更多
Metal-backboned polymers with anisotropy microstructures are promising for conductive,optoelectronic,and magnetic functional materials.However,the structure-property relationships governing the interplay between the c...Metal-backboned polymers with anisotropy microstructures are promising for conductive,optoelectronic,and magnetic functional materials.However,the structure-property relationships governing the interplay between the chemical structure and electromagnetic property of the metal-backboned polymer have been rarely investigated.Here we report a carbon/nickel hybrid from metal-backboned polymer to serve as electromagnetic wave-absorbing materials,which exhibit high microwave absorption capacity and tunable absorption band.The presence of nickel backbones promote the generation of heterogeneous interfaces with carbon during calcination,thereby enhancing the wave-absorbing capacity of the carbon/nickel hybrid.The C/Ni hybrids show a minimal reflection loss of-49.1 dB at 13.04 GHz,and its frequency of the absorption band can be adjusted by controlling the thickness of the absorption layer.展开更多
Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition be...Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.展开更多
Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, p...Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2) was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P^(5+) doping increased the distance between the (003) crystal planes from ~0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.展开更多
The hunt for agents that are suitable for actinide decorporation to reduce the whole-body load of actinide in accidental internal exposure is the ever-lasting goal in radiation protection and medical treatment in nucl...The hunt for agents that are suitable for actinide decorporation to reduce the whole-body load of actinide in accidental internal exposure is the ever-lasting goal in radiation protection and medical treatment in nuclear emergency.All current decorporation agents can be categorized as two groups,one is the molecular ligands,and the other is the nanoparticles decorated with molecular ligands.Here in this work,functional nanodiamonds(fN Ds)with ss DNA(the endogenous biomacromolecule rich in phosphate groups)loaded on the NDs is reported,which poses good uranyl adsorption selectivity,high cellular uptake,fast excretion,and effective decorporation of uranyl from rat renal proximal tubular epithelial cells(NRK-52E).All those results corroborate that f NDs can potentially serve as a brand new family of chelators for actinide decorporation.展开更多
Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential dep...Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential deposition method is used to fabricate the photoactive layers of all-PSCs comprising a polymer donor PTzBI-oF and a polymer acceptor PS1. The film morphology can be manipulated by incorporating amounts of a dibenzyl ether additive into the PS1 layer. Detailed morphology investigations by grazing incidence wide-angle X-ray scattering and a transmission electron microscope reveal that the combination merits of sequential deposition and DBE additive can render favorable crystalline properties as well as phase separation for PTzBI-oF:PS1 blends. Consequently, the optimized all-PSCs delivered an enhanced power conversion efficiency(PCE) of 15.21%along with improved carrier extraction and suppressed charge recombination. More importantly, the optimized all-PSCs remain over 90% of their initial PCEs under continuous thermal stress at 65 °C for over 500 h. This work validates that control over microstructure morphology via a sequential deposition process is a promising strategy for fabricating highly efficient and stable all-PSCs.展开更多
基金funding from the National Natural Science Foundation of China (Award 91745203) supplemented by Central Universities’ Basic Research Funds.
文摘Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.
基金supported by the National Natural Science Foundation of China(No.22375123)the Shuguang Program of Shanghai Education Development Foundation,the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(No.2022SXTD012)。
文摘Fluorinated fused azobenzene boron(FBAz)is a novel electron-deficient building block for polymer electron acceptors in all-polymer solar cells(all-PSC).The B←N bridging units impart a fixed configuration and low-lying LUMO/HOMO energy.Three polymer acceptor materials(P2f,P3f and P5f)with different fluorine substitution positions by copolymerizing FBAz with indacenodithiophene(IDT),are synthesized and investigated to study the influence of fluorinated forms on the all-polymer solar cell performance.The FBAz units are synthesized in just three steps,facilitating the straightforward production of polymer acceptors P2f,P3f,and P5f.These acceptors exhibit strong light absorption in the visible to near-infrared range of 500-1000nm and possess suitable LUMO/HOMO energy levels of-3.99/-5.66 eV which are very complementary to that(E_(LUMO/HOMO)=-3.59/-5.20 eV)of the widely-used polymer donor poly[(ethylhexylthiophenyl)-benzodithiophene-(ethylhexyl)-thienothiophene](PTB7-Th).All-polymer solar cells(all-PSCs)with PTB7-Th as electron donor and P3f as electron acceptor exhibits highest power conversion efficiencies(PCE)2.70%.When PC_(61)BM is added as the third component,the device efficiency can reach 5.36%.These preliminary results indicate that FBAz is a promising strong electron acceptor for the development of n-type polymer semiconductors,especially in organic photovoltaics(OPVs).To the best of our knowledge,this is the first example demonstrating the unique photovoltaic properties of the N=N double bond as an acceptor material.
基金financially supported by the National Key R&D Program of China(2021YFB3800300)the National Natural Science Foundation of China(22179143 and 22309202)+1 种基金the Jiangsu Funding Program for Excellent Postdoctoral Talentthe Gusu Leading Talents Program(ZXL2023190)。
文摘Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion batteries.However,the influence of dual exposure to air and liquid water as well as the heating treatment during aqueous slurry electrode processing on the high-nickel layered oxide electrode is yet to be understood.In this study,we systematically investigate the structural evolution and electro-chemical behaviors when LiNi_(0.83)Mn_(0.05)Co_(0.12)O_(2)(NMC83)is subjected to aqueous slurry processing.It was observed that the crystal structure near the surface of NMC83 is partially reconstructed to contain a mixture of rock-salt and layered phases when exposed to water,leading to the deteriorated rate capability of the NMC83 electrodes.This partial surface reconstruction layer completely converts into a pure rock-salt phase upon cycling,accompanied by the release of O_(2),Ni leaching,catalyzed decomposition of the electrolyte,and the formation of a thick cathode electrolyte interphase layer.The byproducts of the electrolyte and dissolved Ni could shuttle to the Li metal side,causing a crosstalk effect that results in a thick and unstable solid electrolyte interphase layer on the Li surface.These in combination severely undermined the cycling stability of the NMC83 electrodes obtained from the aqueous slurry.A mitigation strategy using molecular self-assembly technique was demonstrated to enhance the surface stability of water-treated NMC83.Our findings offer new insights for tailoring ambient environment stability and aqueous slurry processability for ultra-high nickel layered oxide and other water-sensitive cathode materials.
基金supported by the National Key Research and Development Program of China(No.2023YFB3813000)the National Natural Science Foundation of China(Nos.82071085,82020108011,and 82122014)the Zhejiang Provincial Natural Science Foundation of China(No.LR21H140001).
文摘Periodontitis is an inflammatory disease caused by oxidative stress and initiated by bacterial infection.The endogenous enzyme system is dysfunctional in the periodontitis microenvironment.Currently,traditional clinical treatment cannot efficiently eliminate bacteria or relieve inflammation.To address this issue,we developed ultrasmall ruthenium nanoparticles(US-RuNPs)with multienzyme-like activity.Our results indicated that US-RuNPs with an amplified electric field had a superior photothermal effect to large-sized RuNPs.Thus,US-RuNPs,through photothermal therapy(PTT),acted as“bacterial lysozyme”to eliminate planktonic pathogens and biofilms.In addition,the antioxidant enzyme-like activity of US-RuNPs was greater than that of large-sized RuNPs,and US-RuNPs could scavenge intracellular reactive oxygen species(ROS)and inhibit inflammation-related responses.More importantly,US-RuNPs demonstrated a satisfactory effect against periodontitis in vivo due to their synergistic antibacterial activity through PTT and antioxidant effects even in deep sites,decreasing the alveolar bone loss to root length ratio(ABL/RL)from 70.70%to 20.15%and increasing the collagen volume fraction from 16.88%to 57.64%.Thus,US-RuNPs with approximately 2 nm diameter,mimicking multienzyme activity,have great potential for the treatment of periodontitis.
基金supported by the Beijing Nova Program(No.20220484215)National Key Research and Development Program of China(Nos.2022YFB3504100,2022YFB3506200,2021YFA1500300 and 2022YFA1500146)National Natural Science Foundation of China(Nos.22376217,22208373,22272090 and 22272106)。
文摘Herein,we fabricate an embedding structure at the interface between Pt nanoparticles(NPs)and CeO_(2)-{100}nanocubes with surface defect sites(CeO_(2)-SDS)through quenching and gas bubbling-assisted membrane reduction methods.The in-situ substitution of Pt NPs for atomic-layer Ce lattice significantly increases the amount of reactive oxygen species from 133.68μmol/g to 199.44μmol/g.As a result,the distinctive geometric structure of Pt/CeO_(2)-SDS catalyst substantially improves the catalytic activity and stability for soot oxidation compared with the catalyst with no quenching process,i.e.,its T_(50)and TOF values are 332°C and 2.915 h^(-1),respectively.Combined with the results of experimental investigations and density functional theory calculations,it is unveiled that the unique embedding structure of Pt/CeO_(2)-SDS catalyst can facilitate significantly electron transfer from Pt to the CeO_(2)-{100}support,and induce the formation of interfacial[Ce-O_(x)-Pt_(2)]bond chains,which plays a crucial role in enhancing the key step of soot oxidation through the dual activation of surface lattice oxygen and molecular O_(2).Such a fundamental revelation of the interfacial electronic transmission and corresponding modification strategy contributes a novel opportunity to develop high-efficient and stable noble metal catalysts at the atomic level.
基金supported by the National Key Research and Development Program of China(Nos.2021YFF1200300,2020YFA0909000)National Natural Science Foundation of China(Nos.22025404,32471426)+3 种基金Innovative Research Group of High-Level Local Universities in Shanghai(No.SHSMU-ZLCX20212602)Natural Science Foundation of Shanghai(No.23ZR1438700)Shanghai Municipal Health Commission(No.2022JC027)Shanghai Sailing Program(No.22YF1424400)。
文摘RNA offers distinct advantages for molecular self-assembly as a unique and programmable biomaterial.Recently,single-stranded RNA(ssRNA)origamis,capable of self-folding into defined nanostructures within a single-stranded RNA molecule,are considered a promising platform for immune recognition and therapy.Here,we utilize single-stranded rod RNA origami(Rod RNA-OG)as functional nucleic acid to synthesize valence-programmed RNA structures in a one-pot manner.We discover that the polyvalent RNA origamis are resistant to RNase degradation and can be efficiently internalized by macrophages for subsequent innate immune activation,even in the absence of any external protective agents such as lipids or polymers.The valence-programmed RNA origamis thus hold great promise as novel agonists for immunotherapy.
文摘Designing Fischer-Tropsch synthesis(FTS)catalysts to selectively produce liquid hydrocarbon fuels is a crucial challenge.Herein,we selectively introduced Co nanoparticles(NPs)into the micropores and mesopores of an ordered mesoporous MFI zeolite(OMMZ)through impregnation,which controlled the carbon number distribution in the FTS products by tuning the position of catalytic active sites in differently sized pores.The Co precursors coordinated by acetate with a size of 9.4×4.2×2.5Åand by 2,2'-bipyridine with a size of 9.5×8.7×7.9Å,smaller and larger than the micropores(ca.5.5Å)of MFI,made the Co species incorporated in OMMZ's micropores and mesopores,respectively.The carbon number products synthesized with the Co NPs confined in mesopores were larger than that in micropores.The high jet and diesel selectivities of 66.5%and 65.3%were achieved with Co NPs confined in micropores and mesopores of less acidic Na-type OMMZ,respectively.Gasoline and jet selectivities of 76.7%and 70.8%were achieved with Co NPs confined in micropores and mesopores of H-type OMMZ with Brönsted acid sites,respectively.A series of characterizations revealed that the selective production of diesel and jet fuels was due to the C-C cleavage suppressing of heavier hydrocarbons by the Co NPs located in mesopores.
基金financially supported by the Fundamental Research Funds for Central Universities(No.24D110627)。
文摘The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is both robust and readily-functionalized through interfacial click polymerization.A water-in-oil emulsion was constructed to act as the reaction medium,the hydrophilic 1,3-butadiene diepoxide(BDE)in water phase reacted with the oleophilic 1,4-dibutanedithiol(BDT)in oil phase at the water-oil interface to form the amphiphilic ACP named poly(2,3-dihydroxy butylene-alt-butylene dithioether)(abbreviated as P(DHB-a-BDT)below),which would deposite in situ to form the micro-sized capsules.Significantly,the dried capsules are robust enough to be rehydrated once the water was added and almost restored their original morphologies.Further elucidation showed that the Young's modulus of these capsules exceeded 1 GPa.As long as we know,it is the first time for the mechanical properties of the ACP-based microstructures being investigated.Besides,functionalization could be achieved simultaneously with the formation process.As a proof of concept,positive-charged capsules were successfully obtained through click copolymerization.Stemming from the unique characteristics of amphiphilic ACPs which combined both merits of click chemistry and interfacial reactions,all these features of the current method as well as the resultant capsules may promote the application of the polymeric capsules.
基金the support from the National Natural Science Foundation of China(52333006)the support from the National Natural Science Foundation of China(52303232)+1 种基金the Natural Science Foundation of Jiangxi Province(20242BAB20184)the support from National Natural Science Foundation of China(52373186)。
文摘Semi-transparent organic photovoltaics(ST-OPVs)have great potential for photovoltaic building integration and agricultural greenhouse energy.However,the mutually constraining relationship between average visible transmittance(AVT)and power conversion efficiency(PCE)remains a key issue of STOPVs.Herein,we innovatively applied a surface texturization strategy by integrating with a pseudo-planar heterojunction(PPHJ)structure to fabricate ST-OPVs,which possess outstanding photoelectric conversion and light management capability.The textured active layer performs significantly improved light capture capability and reduced optical loss due to that the micro-patterned arrays can deflect incident light multiple times.Moreover,the surface texturization strategy can enhance the crystallinity of the active layer and precisely control donor/acceptor inter-penetration,which magnifies exciton dissociation interface and forms ordered carrier dynamics.Consequently,the textured opaque device via blade-coating performs a record PCE of 19.17%(certified 19.02%)and the semi-transparent device achieves one of the highest light utilization efficiency(LUE)of 5.54%with prominent PCE(14.40%)and AVT(38.43%).Most importantly,the excellent thermal insulation performance and color rendering index of ST-OPVs are fitting for the agricultural greenhouses and insulation roofing,which shows that the surface texturization strategy can provide promising application prospects for ST-OPVs in economically sustainable agricultural development.
基金We acknowledge financial support by the National Natural Science Foundation of China(32071374,32000985,81761148029,81620108028)Program of Shanghai Academic Research Leader under the Science and Technology Innovation Action Plan(21XD1422100)+3 种基金Leading Talent of“Ten Thousand Plan”-National High-Level Talents Special Support Plan,One Belt and One Road International Cooperation Project from Key Research and Development Program of Zhejiang Province(2019C04024)the Zhejiang Provincial Natural Science Foundation of China(LR22C100001,LGF19C100002,LQ21H300003)Zhejiang Province Medical and Health Science Research Project(2021KY666),and Zhejiang Pharmaceutical Association(2019ZYY12)Open access funding provided by Shanghai Jiao Tong University
文摘The structural change-mediated catalytic activity regulation plays a significant role in the biological functions of natural enzymes.However,there is virtually no artificial nanozyme reported that can achieve natural enzyme-like stringent spatiotemporal structure-based catalytic activity regulation.Here,we report a subnanostructural transformable gold@ceria(STGC-PEG)nanozyme that performs tunable catalytic activities via near-infrared(NIR)light-mediated sub-nanostructural transformation.The gold core in STGC-PEG can generate energetic hot electrons upon NIR irradiation,wherein an internal sub-nanostructural transformation is initiated by the conversion between CeO;and electron-rich state of CeO;-x,and active oxygen vacancies generation via the hot-electron injection.Interestingly,the sub-nanostructural transformation of STGC-PEG enhances peroxidase-like activity and unprecedentedly activates plasmon-promoted oxidase-like activity,allowing highly efficient low-power NIR light(50 m W cm;)-activated photocatalytic therapy of tumors.Our atomic-level design and fabrication provide a platform to precisely regulate the catalytic activities of nanozymes via a light-mediated sub-nanostructural transformation,approaching natural enzyme-like activity control in complex living systems.
基金This work was financially supported by the National Natrual Science Foundation of China(Nos.21901161 and 22071152)Natural Science Foundation of Shanghai(No.20ZR1429200)+1 种基金the China Postdoctoral Science Foundation(No.2020M671094)Basic Research Program of Xi'an Jiaotong University(No.XZY022020018).
文摘Herein,we designed and constructed two metallacycles,1 and 2,to illustrate the conformational effect of isomeric AIE fluoropho res on the platfo rm of supramolecular coordination complexe s(SCCs).Specifically,the dangling phenyl rings in TPE units of the metallacycle 1 align completely outside the main cyclic structure,while in the metallacycle 2,these phenyl rings align half inside and half outside.The experimental results showed that two metallacycles exhibited different behaviors in terms of AIE fluorescence and chemical sensing,which could be attributed to the subtle structural difference of the TPE units.This work repre sents the unification of topics such as self-assembly,AIE,and chemical sensing,and further promotes the understanding for the structure-property relationship of isomeric AIE fluorophores.
基金financially supported by the National Natural Science Foundation of China(Nos.51973110,21734009,21905102 and 22109094)the Program of Shanghai Science and Technology Commission science and technology innovation action plan(Nos.20ZR1426200,20511103800,20511103802 and 20511103803)+2 种基金the Natural Science Foundation of Shandong Province(No.ZR2019LFG005)the Key research project of Shandong Province(No.2020CXGC010403)the Center of Hydrogen Science,Shanghai Jiao Tong University,China。
文摘The morphology manipulation of the active layers is important for improving the performance of organic photovoltaics(OPVs).The choice of processing solvent has great impact on the crystallization and phase separation during film formation,since solvent properties,including solvent effect on molecular crystallization,boiling point,and interaction parameters,can directly change the evolution pathways associated with thermodynamics and kinetics.Therefore,revealing the underlying solvent-regulated morphology mechanism is potential to provide guiding strategies for device optimization.In this study,chloroform,chlorobenzene,and toluene are used to process PM6:Y6 blends by slot-die printing to fabricate OPV devices.The chloroform printed film forms a fibrillar network morphology with enhanced crystallization,facilitating exciton dissociation,charge transport and extraction,resulting in an optimal power conversion efficiency of 16.22%.However,the addition of the additive chloronaphthalene in chloroform solution leads to over-crystallization of Y6,and thus,increasing domain size that exceeds the exciton diffusion length,resulting in lower device efficiency.In addition,both the chlorobenzene and toluene suppress the crystallization of Y6,which drastically decreased short-circuit current and fill factor.These results demonstrate the important role of processing solvent in dictating film morphology,which critically connects with the resultant printed OPV performance.
基金financially supported by the ERC Grant2DMATERESF Young Researcher Group‘GRAPHD’+1 种基金the EC under the Graphene Flagship(No.CNECTICT-604391)the Excellent Youth Foundation of Zhejiang Province of China(No.LR21E030001)。
文摘Quasi-two-dimensional(q2 D)conducting polymer thin film synergizes the advantageous features of longrange molecular ordering and high intrinsic conductivity,which are promising for flexible thin film-based micro-supercapacitors(MSCs).Herein,we present the high-performance flexible MSCs based on highly ordered quasi-two-dimensional polyaniline(q2 D-PANI)thin film using surfactant monolayer assisted interfacial synthesis(SMAIS).Owing to high electrical conductivity,rich redox chemistry,and thin-film morphology,the q2 D-PANI MSCs show high volumetric specific capacitance(ca.360 F/cm^(3))and energy density(17.9 m Wh/cm^(3)),which outperform the state-of-art PANI thin-film based MSCs and promise for future flexible electronics.
基金This work was supported by National Key R&D Program of China(2018YFA0900600)the Bill&Melinda Gates Foundation(OPP1199872 and INV-027291)+6 种基金the China Postdoctoral Science Foundation(2022M722851)the National Natural Science Foundation of China(82274047,31770327,32070329,82003889)SJTU Trans-med Awards Research(20190104)SJTU Global Strategic Partnership Fund(2020 SJTU-CORNELL)Zhejiang Provincial Natural Science Foundation of China(LQ21H280004)National Young Qihuang Scholars Training Programthe National‘Ten-thousand Talents Program’for Leading Talents of Science and Technology Innovation in China.
文摘Dear Editor,Artemisinin,which has potent antimalarial properties,is a sesquiterpene endoperoxide originally isolated from the traditional Chinese medicinal plant Artemisia annua.However,the artemisinin content in wild-type(WT)A.annua is low(1-10 mg/g dry weight),leading to its erratic supply and price fluctuations[1].
基金supported by National Natural Science Foun-dation of China(No.21905206),Shanghai Sail Program(No.19YF1450800).
文摘Aqueous rechargeable Ni−Zn batteries are considered as a new generation of safe and reliable electro-chemical energy storage system.However,low electronic conductivity of Ni-based cathodes hinders the practical application of Ni-Zn batteries.This problem can be overcome by compositing the Ni-based cath-ode with highly conductive carbon substrates.A chemical oxidation pre-treatment is popularly applied to the carbon substrates to increase their hydrophilicity and thus facilitate the growth of active materials in aqueous systems.However,the anodic stability of the oxidized carbon substrates is greatly challenged,which has never been addressed in previous reports.In this work,we first compared the anodic stabil-ity of carbon fiber paper with and without oxidation treatment and find that carbon substrate with the chemical treatment caused remarkable oxidization current in the required voltage range.To take both anodic stability and fine growth of active materials into account,here we demonstrated a facile physical surface-treatment method of ethanol wetting to replace the chemical treatment.The ethanol infiltration removes gas adsorption on carbon substrates and thus promotes their hydrophilicity.This cost-effective strategy simultaneously achieves a high anodic stability and a fine growth and uniform distribution of nickel-cobalt hydroxide on the carbon microfibers.The resulting Ni-Zn battery provides a high discharge capacity of 219 mAh/g with an operation cell voltage of 1.75 V.
基金This work was financially supported by MOST(Nos.2022YFA1203001 and 2022YFA1203002)NSFC(Nos.T2321003,22335003 and 22105045)STCSM(Nos.21511104900 and 20JC1414902).
文摘Metal-backboned polymers with anisotropy microstructures are promising for conductive,optoelectronic,and magnetic functional materials.However,the structure-property relationships governing the interplay between the chemical structure and electromagnetic property of the metal-backboned polymer have been rarely investigated.Here we report a carbon/nickel hybrid from metal-backboned polymer to serve as electromagnetic wave-absorbing materials,which exhibit high microwave absorption capacity and tunable absorption band.The presence of nickel backbones promote the generation of heterogeneous interfaces with carbon during calcination,thereby enhancing the wave-absorbing capacity of the carbon/nickel hybrid.The C/Ni hybrids show a minimal reflection loss of-49.1 dB at 13.04 GHz,and its frequency of the absorption band can be adjusted by controlling the thickness of the absorption layer.
基金supported by the National Natural Science Foundation of China (52302292, 52302058, 52302085)the China Postdoctoral Science Foundation (2021M702225)+1 种基金the Anhui Province University Natural Science Research Project (2023AH030093, 2023AH040301)the Startup Research Fund of Chaohu University (KYQD-2023005, KYQD-2023051)。
文摘Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.
基金This work was supported by the National Natural Science Foundation of China(U1564205)the Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges under the Beijing Municipality(IDHT20180508).Naser Tavajohi acknowledges financial support from the Kempe Foundation.
文摘Owing to their high theoretical specific capacity and low cost, lithium- and manganese-rich layered oxide (LMR) cathode materials are receiving increasing attention for application in lithium-ion batteries. However, poor lithium ion and electron transport kinetics plus side effects of anion and cation redox reactions hamper power performance and stability of the LMRs. In this study, LMR Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2) was modified by phosphorus (P)-doping to increase Li+ conductivity in the bulk material. This was achieved by increasing the interlayer spacing of the lithium layer, electron transport and structural stability, resulting in improvement of the rate and safety performance. P^(5+) doping increased the distance between the (003) crystal planes from ~0.474 nm to 0.488 nm and enhanced the structural stability by forming strong covalent bonds with oxygen atoms, resulting in an improved rate performance (capacity retention from 38% to 50% at 0.05 C to 5 C) and thermal stability (50% heat release compared with pristine material). First-principles calculations showed the P-doping makes the transfer of excited electrons from the valence band to conduction band easier and P can form a strong covalent bond helping to stabilize material structure. Furthermore, the solid-state electrolyte modified P5+ doped LMR showed an improved cycle performance for up to 200 cycles with capacity retention of 90.5% and enhanced initial coulombic efficiency from 68.5% (pristine) or 81.7% (P-doped LMR) to 88.7%.
基金supported by grants from the National Natural Science Foundation of China(Nos.82050005,21976127,22022410)the Youth Innovation Promotion Association of CAS(No.2016236)+2 种基金the Natural Science Foundation of Jiangsu Province(Nos.BK20190044,BK20210736)funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the China Postdoctoral Science Foundation(No.2020M681431)。
文摘The hunt for agents that are suitable for actinide decorporation to reduce the whole-body load of actinide in accidental internal exposure is the ever-lasting goal in radiation protection and medical treatment in nuclear emergency.All current decorporation agents can be categorized as two groups,one is the molecular ligands,and the other is the nanoparticles decorated with molecular ligands.Here in this work,functional nanodiamonds(fN Ds)with ss DNA(the endogenous biomacromolecule rich in phosphate groups)loaded on the NDs is reported,which poses good uranyl adsorption selectivity,high cellular uptake,fast excretion,and effective decorporation of uranyl from rat renal proximal tubular epithelial cells(NRK-52E).All those results corroborate that f NDs can potentially serve as a brand new family of chelators for actinide decorporation.
基金financially supported by Guangdong Major Project of Basic and Applied Basic Research (No.2019B030302007)National Key Research and Development Program of China (No. 2019YFA0705900) funded by MOSTthe financial support by State Key Lab of Luminescent Materials and Devices,South China University of Technology (Skllmd-2022-03)。
文摘Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential deposition method is used to fabricate the photoactive layers of all-PSCs comprising a polymer donor PTzBI-oF and a polymer acceptor PS1. The film morphology can be manipulated by incorporating amounts of a dibenzyl ether additive into the PS1 layer. Detailed morphology investigations by grazing incidence wide-angle X-ray scattering and a transmission electron microscope reveal that the combination merits of sequential deposition and DBE additive can render favorable crystalline properties as well as phase separation for PTzBI-oF:PS1 blends. Consequently, the optimized all-PSCs delivered an enhanced power conversion efficiency(PCE) of 15.21%along with improved carrier extraction and suppressed charge recombination. More importantly, the optimized all-PSCs remain over 90% of their initial PCEs under continuous thermal stress at 65 °C for over 500 h. This work validates that control over microstructure morphology via a sequential deposition process is a promising strategy for fabricating highly efficient and stable all-PSCs.
