Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review ...Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.展开更多
The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with th...The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.展开更多
In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearl...In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearly indicate luminescence down-shifting(LDS) properties. On the basis of QDs, surface functional group multilayer LDS films(MLDSs) are fabricated through an electrostatic layer-by-layer(LBL) self-assembly method. The PL intensity increases linearly with the number of bilayers, showing a regular and uniform film growth. When the M-LDS is placed on the surface of a Si-based solar cell as an optical conversion layer for the first time, the external quantum efficiency(EQE) and shortcircuit current density(Jsc) notably increases for the LDS process. The EQE response improves in a wavelength region extending from the UV region to the blue region, and its maximum increase reaches more than 15% between 350 nm and 460 nm.展开更多
Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we...Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we have developed a solid additive-assisted layer-by-layer(SAA-LBL)processing to fabricate high-efficiency OSCs.By adding the solid additive of fatty acid(FA)into polymer donor PM6 solution,controllable pre-phase separation forms between PM6 and FA.This intermixed morphology facilitates the diffusion of acceptor Y6 into the donor PM6 during the LBL processing,due to the good miscibility and fast-solvation of the FA with chloroform solution dripping.Interestingly,this results in the desired morphology with refined phase-separated domain and vertical phase-separation structure to better balance the charge transport/collection and exciton dissociation.Consequently,the binary single junction OSCs based on PM6:Y6 blend reach champion power conversion efficiency(PCE)of 18.16%with SAA-LBL processing,which can be generally applicable to diverse systems,e.g.,the PM6:L8-BO-based devices and thick-film devices.The efficacy of SAA-LBL is confirmed in binary OSCs based on PM6:L8-BO,where record PCEs of 19.02%and 16.44%are realized for devices with 100 and 250 nm active layers,respectively.The work provides a simple but effective way to control the morphology for high-efficiency OSCs and demonstrates the SAA-LBL processing a promising methodology for boosting the industrial manufacturing of OSCs.展开更多
In this study,MnCo2O4 nanosheets were proposed to be utilized as an electrode material for supercapacitors.A two-step hydrothermal method with post-annealing treatment was employed in preparation of the nanostructures...In this study,MnCo2O4 nanosheets were proposed to be utilized as an electrode material for supercapacitors.A two-step hydrothermal method with post-annealing treatment was employed in preparation of the nanostructures.MnCo2O4 electrode delivered a high specific capacitance of 2000 F g^-1 at 0.5 A g^-1,remarkable high-rate capability of 1150 F g^-1 at 20 A g^-1,and an excellent cycling stability of 92.3%at 5 A g^-1 after 5000 cycles.It is found that a three-electrode supercapacitor based on MnCo2O4 exhibits a promising electrochemical performance,better than the other similar materials,benefited from the synergistic effects of MnCo2O4 nanosheets.In fact,the self-assembly of nanosheets structure with high specific surface area and mesoporous structure can potentially enhance the electrochemical performance of supercapacitors.展开更多
Here, large-scale and uniform hexagonal zinc oxide(ZnO) nanosheet films were deposited onto indium tin oxide(ITO)-coated transparent conducting glass substrates via a facile galvanic displacement deposition process. C...Here, large-scale and uniform hexagonal zinc oxide(ZnO) nanosheet films were deposited onto indium tin oxide(ITO)-coated transparent conducting glass substrates via a facile galvanic displacement deposition process. Compared with other commonly used solution methods, this process avoids high temperature and electric power as well as supporting agents to make it simple and cost-effective. The as-fabricated ZnO nanosheet films have uniform hexagonal wurtzite structure. The photoelectrochemical(PEC) cell based on ZnO nanosheet film/ITO photoelectrode was also fabricated and its performance was improved by optimizing the solution concentration. A higher photocurrent density of*500 l A cm^(-2)under AM 1.5 G simulated illumination of 100 m W cm^(-2)with zero bias potential(vs. Ag/AgCl electrode) was obtained, which may ascribe to the increased surface-to-volume ratio of disordered Zn O nanosheet arrays. Our developed method may be used to deposit other oxide semiconductors, and the Zn O nanosheet film/ITO PEC cell can be used to design low-cost optoelectronic and photoelectrochemical devices.展开更多
Monolayer chemically converted graphene （CCG） nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopr- opyl triethoxysilane （APTES） to form very thin graphene film. The CCG film was...Monolayer chemically converted graphene （CCG） nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopr- opyl triethoxysilane （APTES） to form very thin graphene film. The CCG film was characterized by FT-IR, XRD, SEM, TEM and AFM. Results show that CCG sheets formed monolayer film after assembled onto silicon wafer and there is a very tight chemical bond between sheets and wafer. Furthermore, the electrical measurements revealed that the monolayer graphene film has an excellent electrical conductivity.展开更多
Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin fi...Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.展开更多
Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of...Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions.Herein,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond.With this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties.Significantly,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high photostability.Moreover,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 nm.The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant.These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.展开更多
The employment of microwave absorbents is highly desirable to address the increasing threats of electromagnetic pollution.Importantly,developing ultrathin absorbent is acknowledged as a linchpin in the design of light...The employment of microwave absorbents is highly desirable to address the increasing threats of electromagnetic pollution.Importantly,developing ultrathin absorbent is acknowledged as a linchpin in the design of lightweight and flexible electronic devices,but there are remaining unprecedented challenges.Herein,the self-assembly VS_(4)/rGO heterostructure is constructed to be engineered as ultrathin microwave absorbent through the strategies of architecture design and interface engineering.The microarchitecture and heterointerface of VS_(4)/rGO heterostructure can be regulated by the generation of VS_(4) nanorods anchored on rGO,which can effectively modulate the impedance matching and attenuation constant.The maximum reflection loss of 2VS_(4)/rGO40 heterostructure can reach−43.5 dB at 14 GHz with the impedance matching and attenuation constant approaching 0.98 and 187,respectively.The effective absorption bandwidth of 4.8 GHz can be achieved with an ultrathin thickness of 1.4 mm.The far-reaching comprehension of the heterointerface on microwave absorption performance is explicitly unveiled by experimental results and theoretical calculations.Microarchitecture and heterointerface synergistically inspire multi-dimensional advantages to enhance dipole polarization,interfacial polarization,and multiple reflections and scatterings of microwaves.Overall,the strategies of architecture design and interface engineering pave the way for achieving ultrathin and enhanced microwave absorption materials.展开更多
In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long c...In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long cycle life and environmental friendliness [1]. Up to now, supercapacitors have been widely used in backup power, electric vehicles, mobile power and so on [2,3].展开更多
Recent advances in the study of magnetic atomic structures on noble metal surfaces are reviewed. These include one- dimensional strings, two-dimensional hexagonal superlattices, and novel structures stabilized by quan...Recent advances in the study of magnetic atomic structures on noble metal surfaces are reviewed. These include one- dimensional strings, two-dimensional hexagonal superlattices, and novel structures stabilized by quantum guiding. The combined techniques of low-temperature scanning tunneling microscopy, kinetic Monte Carlo simulations, and ab initio calculations reveal that surface-state-mediated adatom-step and adatom-adatom interactions are the driving forces for self- assembly of these structures. The formation conditions are further discussed by comparing various experimental systems and the kinetic Monte Carlo simulations. Using scanning tunneling spectroscopy and tight-binding calculations together, we reveal that the spectra of these well-ordered structures have characteristic peaks induced by electronic scattering processes of the atoms within the local environment. Moreover, it is demonstrated that quantum confinement by means of nano-size corrals has significant influence on adatom diffusion and self-assembly, leading to a quantum-guided self-assembly.展开更多
Molecular self-assembly is crucially fundamental to nature.However,the aqueous self-assembly of polymers is still a challenge.To achieve self-assembly of block copolymers [(polyacrylic acid-block-polyethylene glycol-b...Molecular self-assembly is crucially fundamental to nature.However,the aqueous self-assembly of polymers is still a challenge.To achieve self-assembly of block copolymers [(polyacrylic acid-block-polyethylene glycol-block-polyacrylic acid(PAA68-b-PEG86-b-PAA68)] in an aqueous phase,manganese oxide(MnO2) is first generated to drive phase separation of the PAA block to form the PAA68-b-PEG68-b-PAA68/MnO2 polymeric assembly that exhibits a stable structure in a physiological medium.The polymeric assembly exhibits vesicular morphology with a diameter of approximately 30 nm and high doxorubicin(DOX) loading capacity of approximately 94%.The transformation from MnO2 to Mn2+caused by endogenous glutathione(GSH)facilitates the disassembly of PAA68-b-PEG68-b-PAA68/MnO2 to enable its drug delivery at the tumor sites.The toxicity of DOXloaded PAA68-b-PEG68-b-PAA69/MnO2 to tumor cells has been verified in vitro and in vivo.Notably,drug-loaded polymeric vesicles have been demonstrated,especially in in vivo studies,to overcome the cardiotoxicity of DOX.We expect this work to encourage the potential application of polymer self-assembly.展开更多
Efficient and robust single-atom catalysts(SACs)based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia(NRR)under ambient conditions.Herein,for the first ti...Efficient and robust single-atom catalysts(SACs)based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia(NRR)under ambient conditions.Herein,for the first time,a Mn-N-C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly strategy.The spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom aggregation.Thanks to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix,the catalyst exhibits excellent activity for NRR with high activity and selectivity,achieving a high Faradaic efficiency of 32.02%for ammonia synthesis at−0.45 V versus reversible hydrogen electrode.Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N_(2) adsorption,activation and selective reduction to NH_(3) by the distal mechanism.This work provides a simple synthesis process for Mn-N-C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites.展开更多
Under appropriate physicochemical conditions, short peptide fragments and their synthetic mimics have been shown to form elongated cross-fl nanostructures through self-assembly. The self-assembly process and the resul...Under appropriate physicochemical conditions, short peptide fragments and their synthetic mimics have been shown to form elongated cross-fl nanostructures through self-assembly. The self-assembly process and the resultant peptide nanos- tructures are not only related to neurodegenerative diseases but also provide inspiration for the development of novel bionanomaterials. Both experimental and theoretical studies on peptide self-assembly have shown that the self-assembly process spans multiple time and length scales and is hierarchical, β-sheet self-assembly consists of three sub-processes from the microscopic to the mesoscopic level： β-sheet locking, lateral stacking, and morphological transformation. De- tailed atomistic simulation studies have provided insight into the early stages of peptide nanostructure formation and the interplay between different non-covalent interactions at the microscopic level. This review gives a brief introduction of the hierarchical peptide self-assembly process and focuses on the roles of various non-covalent interactions in the sub-processes based on recent simulation, experimental, and theoretical studies.展开更多
A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles cont...A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles containing a conductive PEG corona, fumed SiO2 and Li TFSI salt via polymerization-induced self-assembly is proposed. This method to prepare SPEs has the advantages of one-pot convenient synthesis, avoiding use of organic solvent and conveniently adding inorganic additives. CH3O-PEG-IC combines advantages of PEG and polycarbonate, the in situ synthesized PEG-b-PS nanoparticles containing a rigid polystyrene(PS) core and a PEG corona guarantee continuous lithium ion transport in the synthesized SPEs, and the fumed SiO2 optimizes the interfacial properties and improves the electrochemical stability, all of which afford SPEs a well considerable room temperature ionic conductivity of 1.73 × 10^-4S/cm, high lithium transference number of 0.53, and wide electrochemical stability window of 5.5 V(vs. Li^+/Li). By employing these SPEs, the assembled solid state cells of Li FePO4 |SPEs|Li exhibit considerable cell performance.展开更多
A versatile and reliable approach is created to fabricate wafer-scale colloidal crystal that consists of a monolayer of hexagonally close-packed polystyrene （PS） spheres. Making wafer-scale colloidal crystal is usua...A versatile and reliable approach is created to fabricate wafer-scale colloidal crystal that consists of a monolayer of hexagonally close-packed polystyrene （PS） spheres. Making wafer-scale colloidal crystal is usually challenging, and it lacks a general theoretical guidance for experimental approaches. To obtain the optimal conditions for self-assembly, a systematic statistical design and analysis method is utilized here, which applies the pick-the-winner rule. This new method combines spin-coating and thermal treatment, and introduces a mixture of glycol and ethanol as a dispersion system to assist self-assembly. By controlling the parameters of self-assembly, we improve the quality of colloidal crystal and reduce the effect of noise on the experiment. To our best knowledge, we are first to pave this path to harvest colloidal crystals. Importantly, a theoretical analysis using an energy landscape base on our process is also developed to provide insights into the PS spheres＇ self-assembly.展开更多
Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;howe...Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;however,the improvement of their energy density remains a challenge.Here,we design a green and universal approach to prepare the composite electrode material,which is composed of lignin-phenolformaldehyde resins derived hierarchical porous carbon(LR-HPC)as conductive skeletons and the self-assembly manganese cobaltite(MnCo_(2)O_(4))nanocrystals as active sites.The synthesized C@MnCo_(2)O_(4)composite has an abundant porous structure and superior electronic conductivity,allowing for more charge/electron mass transfer channels and active sites for the redox reactions.The composite shows excellent electrochemical performance,such as the maximum specific capacitance of~726 mF cm^(-2)at 0.5 mV s^(-1),due to the significantly enhanced interactive interface between LR-HPC and MnCo_(2)O_(4)crystals.The assembled all-solid-state asymmetric supercapacitor,with the LR-HPC and C@MnCo_(2)O_(4)as cathode and anode,respectively,exhibits the highest volumetric energy density of 0.68 mWh cm^(-3)at a power density of 8.2 mW cm^(-3).Moreover,this device shows a high capacity retention ratio of~87.6%at 5 mA cm^(-2)after 5000 cycles.展开更多
The self-assembly of symmetric diblock copolymers confined in the channels of variously shaped cross sections （regu- lar triangles, squares, and ellipses） is investigated using a simulated annealing technique. In th...The self-assembly of symmetric diblock copolymers confined in the channels of variously shaped cross sections （regu- lar triangles, squares, and ellipses） is investigated using a simulated annealing technique. In the bulk, the studied symmetric diblock copolymers form a lamellar structure with period LL. The geometry and surface property of the confining channels have a large effect on the self-assembled structures and the orientation of the lamellar structures. Stacked perpendicular lamellae with period LL are observed for neutral surfaces regardless of the channel shape and size, but each lamella is in the shape of the corresponding channel＇s cross section. In the case of triangle-shaped cross sections, stacked parallel lamel- lae are the majority morphologies for weakly selective surfaces, while morphologies including a triangular-prism-shaped B-cylinder and multiple tridentate lamellae are obtained for strongly selective surfaces. In the cases of square-shaped and ellipse-shaped cross sections, concentric lamellae are the signature morphology for strongly selective surfaces, whereas for weakly selective surfaces, stacked parallel lamellae, and several types of folding lamellae are obtained in the case of square-shaped cross sections, and stacked parallel lamellae are the majority morphologies in the case of ellipse-shaped cross sections when the length of the minor axis is commensurate with the bulk lamellar period. The mean-square end- to-end distance, the average contact number between different species and the surface concentration of the A-monomers are computed to elucidate the mechanisms of the formation of the different morphologies. It is found that the resulting morphology is a consequence of competition among the chain stretching, interfacial energy, and surface energy. Our results suggest that the self-assembled morphology and the orientation of lamellae can be manipulated by the shape, the size, and the surface property of the confining channels.展开更多
Three-dimensional(3D)micro-jet printing is a droplet deposition technique based on liquid-phase materials.To improve the deposition density and performance of energetic films with micro/nanoscale on an energetic chip,...Three-dimensional(3D)micro-jet printing is a droplet deposition technique based on liquid-phase materials.To improve the deposition density and performance of energetic films with micro/nanoscale on an energetic chip,polydopamine(PDA)was utilized as a linker bridge to induce the in-situ self-assembly of CL-20-based energetic film via 3D micro-jet printing.The self-assembly was extensively characterized by confocal laser scanning microscopy(CLSM),SEM,power-XRD,XPS,and DSC.The performance of the self-assembled film was verified by the mechanical properties and detonation properties,and a possible self-assembly mechanism in the layer-by-layer micro-jet printing process was proposed.The results indicated PDA-induced self-assembly enhanced the physical entanglement between the binders and energetic crystal,reduced the porosity from 15.87%to 11.28%,and improved the elastic modulus and the detonation performance of the CL-20-based energetic film.This work proposes a novel and promising energetic film design and fabrication strategy to enhance the interaction between the energetic composite layers in the micro-jet printing process.展开更多
基金financially supported by the National Key Research and Development Program of China (2021YFB3600403)the Fundamental Research Funds for the Central Universities (000-0903069032)。
文摘Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.
基金supported by the National Natural Science Foundation of China(22078211)the China Postdoctoral Science Foundation(2022M721115).
文摘The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.
基金Project supported by the Natural Science Foundation of Shandong Province,China(Grant No.ZR2017PF011)the National Natural Science Foundation of China(Grant No.E020701)the Doctoral Scientific Research Foundation of Binzhou University,China(Grant No.2014Y10)
文摘In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearly indicate luminescence down-shifting(LDS) properties. On the basis of QDs, surface functional group multilayer LDS films(MLDSs) are fabricated through an electrostatic layer-by-layer(LBL) self-assembly method. The PL intensity increases linearly with the number of bilayers, showing a regular and uniform film growth. When the M-LDS is placed on the surface of a Si-based solar cell as an optical conversion layer for the first time, the external quantum efficiency(EQE) and shortcircuit current density(Jsc) notably increases for the LDS process. The EQE response improves in a wavelength region extending from the UV region to the blue region, and its maximum increase reaches more than 15% between 350 nm and 460 nm.
基金supported by the National Key Research and Development Program of China(No.2019YFA0705900)the National Natural Science Foundation of China(Nos.52127806,52173185,21734008,and 61721005)+1 种基金the Fundamental Research Funds for the Central Universities(No.226-2022-00133 and No.226-2022-00209)research start up fund from Zhejiang University。
文摘Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we have developed a solid additive-assisted layer-by-layer(SAA-LBL)processing to fabricate high-efficiency OSCs.By adding the solid additive of fatty acid(FA)into polymer donor PM6 solution,controllable pre-phase separation forms between PM6 and FA.This intermixed morphology facilitates the diffusion of acceptor Y6 into the donor PM6 during the LBL processing,due to the good miscibility and fast-solvation of the FA with chloroform solution dripping.Interestingly,this results in the desired morphology with refined phase-separated domain and vertical phase-separation structure to better balance the charge transport/collection and exciton dissociation.Consequently,the binary single junction OSCs based on PM6:Y6 blend reach champion power conversion efficiency(PCE)of 18.16%with SAA-LBL processing,which can be generally applicable to diverse systems,e.g.,the PM6:L8-BO-based devices and thick-film devices.The efficacy of SAA-LBL is confirmed in binary OSCs based on PM6:L8-BO,where record PCEs of 19.02%and 16.44%are realized for devices with 100 and 250 nm active layers,respectively.The work provides a simple but effective way to control the morphology for high-efficiency OSCs and demonstrates the SAA-LBL processing a promising methodology for boosting the industrial manufacturing of OSCs.
基金supported by the National Natural Science Foundation of China (51572194)the National Key Research and Development Program of China (2018YFB0105900)
文摘In this study,MnCo2O4 nanosheets were proposed to be utilized as an electrode material for supercapacitors.A two-step hydrothermal method with post-annealing treatment was employed in preparation of the nanostructures.MnCo2O4 electrode delivered a high specific capacitance of 2000 F g^-1 at 0.5 A g^-1,remarkable high-rate capability of 1150 F g^-1 at 20 A g^-1,and an excellent cycling stability of 92.3%at 5 A g^-1 after 5000 cycles.It is found that a three-electrode supercapacitor based on MnCo2O4 exhibits a promising electrochemical performance,better than the other similar materials,benefited from the synergistic effects of MnCo2O4 nanosheets.In fact,the self-assembly of nanosheets structure with high specific surface area and mesoporous structure can potentially enhance the electrochemical performance of supercapacitors.
基金supported by the National Major Basic Research Project of 2012CB934302the National 863 Program2011AA050518+1 种基金the Natural Science Foundation of China(Grant No.1117419711574203 and 61234005)
文摘Here, large-scale and uniform hexagonal zinc oxide(ZnO) nanosheet films were deposited onto indium tin oxide(ITO)-coated transparent conducting glass substrates via a facile galvanic displacement deposition process. Compared with other commonly used solution methods, this process avoids high temperature and electric power as well as supporting agents to make it simple and cost-effective. The as-fabricated ZnO nanosheet films have uniform hexagonal wurtzite structure. The photoelectrochemical(PEC) cell based on ZnO nanosheet film/ITO photoelectrode was also fabricated and its performance was improved by optimizing the solution concentration. A higher photocurrent density of*500 l A cm^(-2)under AM 1.5 G simulated illumination of 100 m W cm^(-2)with zero bias potential(vs. Ag/AgCl electrode) was obtained, which may ascribe to the increased surface-to-volume ratio of disordered Zn O nanosheet arrays. Our developed method may be used to deposit other oxide semiconductors, and the Zn O nanosheet film/ITO PEC cell can be used to design low-cost optoelectronic and photoelectrochemical devices.
基金a Chinese Ministry of Education "Changjiang" Innovative Research Team Program(IRT1169)"the Fundamental Research Funds for the Central Universities" (303-47110117,303-47110118,2012-yb-04,and 2012-Ia-008)+4 种基金NCET(NCET-11-0688)RFDP(20110143120006)NSFHB(2011CDB429)NFSC(51101115)Innovative Research Funds of SKLWUT(2011-la-024,2012-Ia-008,2011-PY-2,2011-PY-3)
文摘Monolayer chemically converted graphene （CCG） nanosheets can be homogeneously self-assembled onto silicon wafer modified by 3-aminopr- opyl triethoxysilane （APTES） to form very thin graphene film. The CCG film was characterized by FT-IR, XRD, SEM, TEM and AFM. Results show that CCG sheets formed monolayer film after assembled onto silicon wafer and there is a very tight chemical bond between sheets and wafer. Furthermore, the electrical measurements revealed that the monolayer graphene film has an excellent electrical conductivity.
基金financial support of the Swedish Research Council through the Marie Sklodowska-Curie International Career Grant (No.2015-00395,co-funded by Marie Sklodowska-Curie Actions, through the Project INCA 600398)the Formas Foundation through the Future Research Leaders Grant (No.2016-00496)+3 种基金the AForsk Foundation (Grant No.17-352)the Olle Engkvist Byggmastare Foundation (Grant No.2014/799)the Academy of Finland (Grant No.288945 and 319408)Academy of Finland Research Infrastructure "Printed Intelligence Infrastructure" (PII-FIRI,Grant No. 320019)
文摘Scalable fabrication of high-rate micro-supercapacitors(MSCs)is highly desired for on-chip integration of energy storage components.By virtue of the special self-assembly behavior of 2D materials during drying thin films of their liquid dispersion,a new inkjet printing technique of passivated graphene micro-flakes is developed to directly print MSCs with 3D networked porous microstructure.The presence of macroscale through-thickness pores provides fast ion transport pathways and improves the rate capability of the devices even with solid-state electrolytes.During multiple-pass printing,the porous microstructure effectively absorbs the successively printed inks,allowing full printing of 3D structured MSCs comprising multiple vertically stacked cycles of current collectors,electrodes,and sold-state electrolytes.The all-solid-state heterogeneous 3D MSCs exhibit excellent vertical scalability and high areal energy density and power density,evidently outperforming the MSCs fabricated through general printing techniques.
基金the National Natural Science Foundation of China(Nos.51772085 and U1830138)Hunan Provincial Innovation Foundation for Postgraduate(No.CX20190311)
文摘Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials.However,the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions.Herein,we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays(L-PCN)via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond.With this strategy,CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties.Significantly,this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9μmol h^−1 g^−1,rendering a^25.6-fold enhancement compared to bulk CN,and high photostability.Moreover,an apparent quantum efficiency of 6.93%is achieved for hydrogen evolution at 420±15 nm.The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant.These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.
基金supported by the National Key Research and Development Program of China(Nos.2018YFA0703500)the National Natural Science Foundation of China(Nos.52188101,52102153,52072029,51991340,51991342,51972022)+1 种基金the Overseas Expertise Introduction Projects for Discipline Innovation(B14003)the Fundamental Research Funds for Central Universities(FRF-TP-18-001C1).
文摘The employment of microwave absorbents is highly desirable to address the increasing threats of electromagnetic pollution.Importantly,developing ultrathin absorbent is acknowledged as a linchpin in the design of lightweight and flexible electronic devices,but there are remaining unprecedented challenges.Herein,the self-assembly VS_(4)/rGO heterostructure is constructed to be engineered as ultrathin microwave absorbent through the strategies of architecture design and interface engineering.The microarchitecture and heterointerface of VS_(4)/rGO heterostructure can be regulated by the generation of VS_(4) nanorods anchored on rGO,which can effectively modulate the impedance matching and attenuation constant.The maximum reflection loss of 2VS_(4)/rGO40 heterostructure can reach−43.5 dB at 14 GHz with the impedance matching and attenuation constant approaching 0.98 and 187,respectively.The effective absorption bandwidth of 4.8 GHz can be achieved with an ultrathin thickness of 1.4 mm.The far-reaching comprehension of the heterointerface on microwave absorption performance is explicitly unveiled by experimental results and theoretical calculations.Microarchitecture and heterointerface synergistically inspire multi-dimensional advantages to enhance dipole polarization,interfacial polarization,and multiple reflections and scatterings of microwaves.Overall,the strategies of architecture design and interface engineering pave the way for achieving ultrathin and enhanced microwave absorption materials.
基金financially supported by the Shandong Provincial Natural Science Foundation, China (ZR2019PB018)National Natural Science Foundation, China (21506210)。
文摘In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long cycle life and environmental friendliness [1]. Up to now, supercapacitors have been widely used in backup power, electric vehicles, mobile power and so on [2,3].
基金Project supported by the National Basic Research Program of China(Grant No.2010CB923401)the National Natural Science Foundation of China(Grant Nos.10974087,11374145,11304150,and 11023002)
文摘Recent advances in the study of magnetic atomic structures on noble metal surfaces are reviewed. These include one- dimensional strings, two-dimensional hexagonal superlattices, and novel structures stabilized by quantum guiding. The combined techniques of low-temperature scanning tunneling microscopy, kinetic Monte Carlo simulations, and ab initio calculations reveal that surface-state-mediated adatom-step and adatom-adatom interactions are the driving forces for self- assembly of these structures. The formation conditions are further discussed by comparing various experimental systems and the kinetic Monte Carlo simulations. Using scanning tunneling spectroscopy and tight-binding calculations together, we reveal that the spectra of these well-ordered structures have characteristic peaks induced by electronic scattering processes of the atoms within the local environment. Moreover, it is demonstrated that quantum confinement by means of nano-size corrals has significant influence on adatom diffusion and self-assembly, leading to a quantum-guided self-assembly.
基金financial support from the National Natural Science Foundation of China(21704093)Project funded by China Postdoctoral Science Foundation(2018M632795)+1 种基金Supports Plan for College Science and Technology Innovation Team of Henan Province(16IRTSTHN001)Science&Technology Innovation Talent Plan of Henan Province(174200510018)。
文摘Molecular self-assembly is crucially fundamental to nature.However,the aqueous self-assembly of polymers is still a challenge.To achieve self-assembly of block copolymers [(polyacrylic acid-block-polyethylene glycol-block-polyacrylic acid(PAA68-b-PEG86-b-PAA68)] in an aqueous phase,manganese oxide(MnO2) is first generated to drive phase separation of the PAA block to form the PAA68-b-PEG68-b-PAA68/MnO2 polymeric assembly that exhibits a stable structure in a physiological medium.The polymeric assembly exhibits vesicular morphology with a diameter of approximately 30 nm and high doxorubicin(DOX) loading capacity of approximately 94%.The transformation from MnO2 to Mn2+caused by endogenous glutathione(GSH)facilitates the disassembly of PAA68-b-PEG68-b-PAA68/MnO2 to enable its drug delivery at the tumor sites.The toxicity of DOXloaded PAA68-b-PEG68-b-PAA69/MnO2 to tumor cells has been verified in vitro and in vivo.Notably,drug-loaded polymeric vesicles have been demonstrated,especially in in vivo studies,to overcome the cardiotoxicity of DOX.We expect this work to encourage the potential application of polymer self-assembly.
基金The authors thank the financial support from the National Natural Science Foundation of China(No.51902204,52001214,21975163)Bureau of Industry and Information Technology of Shenzhen(No.201901171518)Shenzhen Science and Technology Program(KQTD20190929173914967).
文摘Efficient and robust single-atom catalysts(SACs)based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia(NRR)under ambient conditions.Herein,for the first time,a Mn-N-C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly strategy.The spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom aggregation.Thanks to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix,the catalyst exhibits excellent activity for NRR with high activity and selectivity,achieving a high Faradaic efficiency of 32.02%for ammonia synthesis at−0.45 V versus reversible hydrogen electrode.Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N_(2) adsorption,activation and selective reduction to NH_(3) by the distal mechanism.This work provides a simple synthesis process for Mn-N-C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites.
基金supported by the National Natural Science Foundation of China(Grant Nos.21373270 and 11504431)the Fundamental Research Funds for Central Universities of China(Grant No.15CX02025A)
文摘Under appropriate physicochemical conditions, short peptide fragments and their synthetic mimics have been shown to form elongated cross-fl nanostructures through self-assembly. The self-assembly process and the resultant peptide nanos- tructures are not only related to neurodegenerative diseases but also provide inspiration for the development of novel bionanomaterials. Both experimental and theoretical studies on peptide self-assembly have shown that the self-assembly process spans multiple time and length scales and is hierarchical, β-sheet self-assembly consists of three sub-processes from the microscopic to the mesoscopic level： β-sheet locking, lateral stacking, and morphological transformation. De- tailed atomistic simulation studies have provided insight into the early stages of peptide nanostructure formation and the interplay between different non-covalent interactions at the microscopic level. This review gives a brief introduction of the hierarchical peptide self-assembly process and focuses on the roles of various non-covalent interactions in the sub-processes based on recent simulation, experimental, and theoretical studies.
基金supported by the National Science Foundation for Distinguished Young Scholars (No. 21525419)the National Natural Science Foundation of China (No. 21474054)the National Key Research and Development Program of China (No. 2016YFA0202503)
文摘A facile one-pot synthesis of solid polymer electrolytes(SPEs), composed of carbonate terminated poly(ethylene glycol)(CH3O-PEG-IC), poly(ethylene glycol)-block-polystyrene(PEG-b-PS) block copolymer nanoparticles containing a conductive PEG corona, fumed SiO2 and Li TFSI salt via polymerization-induced self-assembly is proposed. This method to prepare SPEs has the advantages of one-pot convenient synthesis, avoiding use of organic solvent and conveniently adding inorganic additives. CH3O-PEG-IC combines advantages of PEG and polycarbonate, the in situ synthesized PEG-b-PS nanoparticles containing a rigid polystyrene(PS) core and a PEG corona guarantee continuous lithium ion transport in the synthesized SPEs, and the fumed SiO2 optimizes the interfacial properties and improves the electrochemical stability, all of which afford SPEs a well considerable room temperature ionic conductivity of 1.73 × 10^-4S/cm, high lithium transference number of 0.53, and wide electrochemical stability window of 5.5 V(vs. Li^+/Li). By employing these SPEs, the assembled solid state cells of Li FePO4 |SPEs|Li exhibit considerable cell performance.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11504264,51501128,and 61274064)
文摘A versatile and reliable approach is created to fabricate wafer-scale colloidal crystal that consists of a monolayer of hexagonally close-packed polystyrene （PS） spheres. Making wafer-scale colloidal crystal is usually challenging, and it lacks a general theoretical guidance for experimental approaches. To obtain the optimal conditions for self-assembly, a systematic statistical design and analysis method is utilized here, which applies the pick-the-winner rule. This new method combines spin-coating and thermal treatment, and introduces a mixture of glycol and ethanol as a dispersion system to assist self-assembly. By controlling the parameters of self-assembly, we improve the quality of colloidal crystal and reduce the effect of noise on the experiment. To our best knowledge, we are first to pave this path to harvest colloidal crystals. Importantly, a theoretical analysis using an energy landscape base on our process is also developed to provide insights into the PS spheres＇ self-assembly.
基金The authors gratefully acknowledge the financial support from the National Key R&D Program of China(2021YFC2101304)China Postdoctoral Science Foundation(BX2021041)。
文摘Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications,such as the electrodes of supercapacitors;however,the improvement of their energy density remains a challenge.Here,we design a green and universal approach to prepare the composite electrode material,which is composed of lignin-phenolformaldehyde resins derived hierarchical porous carbon(LR-HPC)as conductive skeletons and the self-assembly manganese cobaltite(MnCo_(2)O_(4))nanocrystals as active sites.The synthesized C@MnCo_(2)O_(4)composite has an abundant porous structure and superior electronic conductivity,allowing for more charge/electron mass transfer channels and active sites for the redox reactions.The composite shows excellent electrochemical performance,such as the maximum specific capacitance of~726 mF cm^(-2)at 0.5 mV s^(-1),due to the significantly enhanced interactive interface between LR-HPC and MnCo_(2)O_(4)crystals.The assembled all-solid-state asymmetric supercapacitor,with the LR-HPC and C@MnCo_(2)O_(4)as cathode and anode,respectively,exhibits the highest volumetric energy density of 0.68 mWh cm^(-3)at a power density of 8.2 mW cm^(-3).Moreover,this device shows a high capacity retention ratio of~87.6%at 5 mA cm^(-2)after 5000 cycles.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11204215,51302187,20990234,20925414,21204040,and 91227121)the Natural Science Foundation of Tianjin City,China(Grant Nos.12JCYBJC32500 and 14JCZDJC32100)+1 种基金the Program for Changjiang Scholars and Innovative Research Team in University(PCSIRT)(Grant No.IRT1257)the 111 Project.A.C.Shi gratefully acknowledges the supports from the Natural Sciences and Engineering Research Council(NSERC)of Canada
文摘The self-assembly of symmetric diblock copolymers confined in the channels of variously shaped cross sections （regu- lar triangles, squares, and ellipses） is investigated using a simulated annealing technique. In the bulk, the studied symmetric diblock copolymers form a lamellar structure with period LL. The geometry and surface property of the confining channels have a large effect on the self-assembled structures and the orientation of the lamellar structures. Stacked perpendicular lamellae with period LL are observed for neutral surfaces regardless of the channel shape and size, but each lamella is in the shape of the corresponding channel＇s cross section. In the case of triangle-shaped cross sections, stacked parallel lamel- lae are the majority morphologies for weakly selective surfaces, while morphologies including a triangular-prism-shaped B-cylinder and multiple tridentate lamellae are obtained for strongly selective surfaces. In the cases of square-shaped and ellipse-shaped cross sections, concentric lamellae are the signature morphology for strongly selective surfaces, whereas for weakly selective surfaces, stacked parallel lamellae, and several types of folding lamellae are obtained in the case of square-shaped cross sections, and stacked parallel lamellae are the majority morphologies in the case of ellipse-shaped cross sections when the length of the minor axis is commensurate with the bulk lamellar period. The mean-square end- to-end distance, the average contact number between different species and the surface concentration of the A-monomers are computed to elucidate the mechanisms of the formation of the different morphologies. It is found that the resulting morphology is a consequence of competition among the chain stretching, interfacial energy, and surface energy. Our results suggest that the self-assembled morphology and the orientation of lamellae can be manipulated by the shape, the size, and the surface property of the confining channels.
文摘Three-dimensional(3D)micro-jet printing is a droplet deposition technique based on liquid-phase materials.To improve the deposition density and performance of energetic films with micro/nanoscale on an energetic chip,polydopamine(PDA)was utilized as a linker bridge to induce the in-situ self-assembly of CL-20-based energetic film via 3D micro-jet printing.The self-assembly was extensively characterized by confocal laser scanning microscopy(CLSM),SEM,power-XRD,XPS,and DSC.The performance of the self-assembled film was verified by the mechanical properties and detonation properties,and a possible self-assembly mechanism in the layer-by-layer micro-jet printing process was proposed.The results indicated PDA-induced self-assembly enhanced the physical entanglement between the binders and energetic crystal,reduced the porosity from 15.87%to 11.28%,and improved the elastic modulus and the detonation performance of the CL-20-based energetic film.This work proposes a novel and promising energetic film design and fabrication strategy to enhance the interaction between the energetic composite layers in the micro-jet printing process.
