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
Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/...Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/chemical stability.To enhance the performance of intrinsic g-CN,a supramolecular self-assembly strategy has been proposed to regulate the molecular structure of supramolecular precursors through non-covalent interactions across molecular building blocks,thereby optimizing the electronic structure of g-CN.This review provides a comprehensive overview of the recent progress in supramolecular self-assembly-derived graphitic carbon nitride(SM-CN)from both experimental and theoretical computational research in synthesis strategies,including synthesis methods and influencing factors,providing a theoretical foundation for the design of supramolecular assembly.It also discusses modification strategies,such as internal modification of the conjugated plane,interlayer optimization,and construction of heterointerfaces to improve the electronic structure of SM-CN owing to its unique layered structure.This review further summarizes the applications of SM-CN in environment and energy,including wastewater treatment,sterilization and disinfection/air purification,water splitting,H_(2)O_(2)production,organic synthesis/biomass conversion,CO_(2)reduction,photocatalytic coupling technology.Finally,perspectives and outlooks for the future development of SM-CN aim to inspire further innovation in the design and construction of high-performance SM-CN for broader applications.展开更多
Lysine-targeting reversible covalent inhibitors,particularly salicylaldehyde-based compounds such as the Food and Drug Administration(FDA)-approved drug Voxelotor,exhibit significant therapeutic potential but are limi...Lysine-targeting reversible covalent inhibitors,particularly salicylaldehyde-based compounds such as the Food and Drug Administration(FDA)-approved drug Voxelotor,exhibit significant therapeutic potential but are limited by challenges including instability and off-target effects.To overcome these limitations in kinase inhibitor A5,we devised a pH-responsive prodrug strategy by masking its reactive aldehyde group with an acid-labile hydrazone linkage and enhancing intracellular delivery through conjugation with FK506.The optimized prodrug demonstrated robust antitumor efficacy in K562 tumor-bearing mice.Furthermore,the incorporation of the photosensitizer chlorin e6(Ce6)led to the formation of self-assembled nanoparticles(AKNP),which not only improved physiological stability and prolonged tumor retention but also enabled light-triggered release of A5 in conjunction with photodynamic therapy(PDT).Our study thus presents a promising prodrug self-assembly strategy that combines the on-demand release of a novel lysine-targeting,reversible covalent kinase inhibitor with PDT in clinical cancer therapy.展开更多
Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.H...Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.Herein,we propose a self-assembly chemical strategy into the LCHEs induced by ordered nanostructure of zwitterionic co-solutes for highly efficient and ultrastable zinc(Zn)metal batteries.Through the systematic screening of six zwitterionic compounds,3-(decyldimethylammonio)propanesulfonate salt(C_(10))with the decyl chain and zwitterions was determined as an optimum to construct quasi-spherical aggregates with a periodic length of 3.77 nm,as confirmed by comprehensive synchronous small-angle X-ray scattering,Guinier,pair distance distribution function,Porod,and other spectroscopic characterizations and molecular dynamic simulation.In particularly,this self-assembled structure in electrolyte environments was attributed to increasing the proportion of both contact and aggregated ion pairs for the formation of LHCEs as well as to providing fast and selective Zn^(2+)conducting channels and uniform solid electrolyte interfaces for facilitated charge transfer kinetics.Moreover,the preferential adsorption of the self-assembled C_(10)on the Zn(002)surface modulated the electrical double layer to suppress hydrogen evolution and corrosion reactions.Consequently,the Zn‖Zn symmetric cells in Zn(OTf)_(2)/C_(10)electrolytes showed long-term plating/stripping behaviors over 2800 h at 1 mA cm^(-2)and 1 mAh cm^(-2)as well as over 1200 h even at 5 mA cm^(-2)and 5 mAh cm^(-2)with a very high depth of discharge of 42.7%.Furthermore,the ZnllVO_(2)/CNT full cells in Zn(OTf)_(2)/C_(10)electrolytes delivered a record-high capacity of 8.10 mAh cm^(-2)at an ultrahigh cathode mass loading of 50 mg cm^(-2)after 150 cycles.展开更多
Constructing nanofibers with specific therapeutic effects against cancer is a challenge.Here,we present the synthesis approach and application prospects of supramolecular nanofibers,which are based on cucurbit[8]uril(...Constructing nanofibers with specific therapeutic effects against cancer is a challenge.Here,we present the synthesis approach and application prospects of supramolecular nanofibers,which are based on cucurbit[8]uril(CB[8])as the host and terpyridine lanthanum ions metal complex as the vip,constructed by layer-by-layer self-assembly through supramolecular interaction.Moreover,nanofibers with lanthanide luminescence properties exhibit surprising pH-responsive deformation properties and antibacterial behavior.In the tumor micro-environment,the dramatic reduction in the size of the nanofibers enables specific and hierarchical release of anticancer drugs in tumor cells to exert an advanced therapeutic effect.In addition,the synergistic therapeutic efficacy was achieved by reducing the excess of Gram-positive and Gram-negative bacteria surrounding tumor cells.The novel supramolecular nanofibers with sequential drug release and combined therapeutic mode provide new guidance for the synthesis of drug carrier materials and direction for the promotion of nanomaterial-mediated cancer therapy.展开更多
Herbicides are indispensable for safeguarding global crop production,yet their effectiveness is often undermined by extensive environmental losses during application.Using herbicide Diuron as a model compound,we devel...Herbicides are indispensable for safeguarding global crop production,yet their effectiveness is often undermined by extensive environmental losses during application.Using herbicide Diuron as a model compound,we developed hierarchical nanoparticles constructed through host-vip molecular recognition followed by electrostatic coassembly,yielding a formulation that unites high delivery efficiency with enhanced environmental compatibility.Relative to conventional wettable powders,these nanoparticles exhibited temperature-responsive release behavior and significantly enhanced foliar adhesion and deposition,increasing leaf retention by more than 241.7%.They also demonstrated strong resistance to rainfall wash-off and a markedly reduced propensity for groundwater leaching,with leaching losses decreased by approximately 18.6%.Greenhouse and field evaluations further confirmed their superior weed control under practical conditions,achieving control efficacies of up to 70.1%against Abutilon theophrasti and 52.9%against Setaria faberi,compared with 53.7%and 39.1%,respectively,for the commercial formulation at the same application rate.Extensive ecotoxicological assessments encompassing seed germination,zebrafish and earthworm assays,in vitro cellular tests,and in vivo rat studies consistently revealed an improved safety profile compared with commercial and technical formulations.Together,these results highlight hierarchical self-assembled nanoparticles as a promising platform for next-generation herbicide delivery that combines high target utilization with lower environmental impact and greater sustainability.展开更多
Monolithic perovskite-silicon tandem solar cells(PSTs)represent a promising avenue for surpassing the efficiency limits of single-junction photovoltaics,but their performance is still hampered by significant open-circ...Monolithic perovskite-silicon tandem solar cells(PSTs)represent a promising avenue for surpassing the efficiency limits of single-junction photovoltaics,but their performance is still hampered by significant open-circuit voltage(V_(OC))losses arising from interfacial inefficient charge extraction and non-radiative recombination.To mitigate these losses,we introduce a push–pull bridging molecule,4′-amino-[1,1′-bi phenyl]-4-carboxylic acid(ABBA),which forms a 2 PACz/ABBA assembly through phosphor-amidate.The 2 PACz/ABBA assembly suppresses 2 PACz aggregation caused byπ-πstacking while simultaneously enhancing the interfacial dipole moment,thereby facilitating the built-in electric field to promote more efficient hole extraction.Meanwhile,–COOH groups within ABBA passivate deep-level defects(e.g.,uncoordinated Pb^(2+))at buried perovskite interface and contribute to the growth of perovskite films with large grains,reduced residual stress,and optimized energy level alignment.Consequently,the champion tandem device fabricated via the two-step sequential vapor-solution process achieves a PCE of 30.37% and an open-circuit voltage(V_(OC))of 1.891 V.Furthermore,unencapsulated devices maintain 88%of their initial performance after 1000 h under maximum power point tracking(MPPT),highlighting its superior stability.展开更多
Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended...Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended conjugation is designed and synthesized,named NaPh-4PACz.Compared to Ph-4PACz,NaPh-4PACz exhibits a larger adsorption energy with the ITO substrate,enabling the formation of a more uniform and dense film,thereby preventing direct contact between the perovskite and ITO.Additionally,NaPh-4PACz also has a stronger interaction with the perovskite,which can reduce buried interface defects and suppress non-radiative recombination.Consequently,NaPh-4PACz-based devices achieved a power conversion efficiency of 25.48%due to their interfacial“adhesive”ability.Importantly,the stability of the NaPh-4PACz-based devices was significantly improved.展开更多
Magnesium(Mg)and its alloys are considered as ideal biodegradable materials due to their excellent mechanical properties and biocompatibility.In order to improve the surface properties to allow better adaptation to th...Magnesium(Mg)and its alloys are considered as ideal biodegradable materials due to their excellent mechanical properties and biocompatibility.In order to improve the surface properties to allow better adaptation to the surrounding tissue of the body,surface modification has played a significant role in satisfying multiple clinical requirements such as corrosion resistance,biocompatibility,and antibacterial ability.Here,layer-by-layer(LbL)self-assembly,which can be applied for biodegradable Mg alloys due to its extensive choice of usable units,holds great promise among all the surface techniques.In this review,the mechanisms of the driving force(i.e.,electrostatic interaction,hydrogen bonding,charge transfer interaction and covalent bonding),cuttingedge advances in preparation methods(e.g.,dipping,spraying,and spinning)and the functional properties(corrosion resistance,antibacterial activity,and biocompatibility)that could be achieved by the LbL coatings are summarized.A reasonable trend of the potential development of LbL for bioMg alloys is also proposed at the end of this article.展开更多
Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （A...Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （Au-NPs） with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.展开更多
Orthopedic implants for the treatment of bone defects from various causes have been challenged by insufficient osseointegration,bacterial infection,oxidative stress,immune rejection,and insufficient individualized tre...Orthopedic implants for the treatment of bone defects from various causes have been challenged by insufficient osseointegration,bacterial infection,oxidative stress,immune rejection,and insufficient individualized treatment.These challenges not only impact treatment outcomes but also severely impact patients’daily lives.Layer-by-Layer(LbL)serves as a simple surface coating technique,in simple terms,to functionalize implants by sequentially adsorbing oppositely charged materials onto a substrate.In orthopaedics,LbL self-assembly technology solves some of the challenges by loading various drugs or biological agents on the implant surface and controlling their release precisely to the site of bone defects in a personalized way.This review will introduce the basic principle and the development of LbL in orthopaedics,review and analyze the chemical strategy of LbL in the preparation of bone implants to ensure the stability of the implant,and introduce the use of LbL bone implants in orthopaedics in recent years.The application of LbL includes the realization of programmed drug delivery and sustained release,thereby promoting osseointegration and the formation of new blood vessels,antibacterial,antioxidant,etc.This review focuses on the LbL technology,involving the technology selection for the preparation of bone implants,the chemical strategies of the stability guarantee of LbL implants,the pharmacological properties,loading and release mechanisms of loaded drugs,and the molecular mechanisms of osteogenesis and angiogenesis.The aim of this review is to provide an overview of current research advances,and a prospect in this field was also described.展开更多
The self-assembled nanoparticles(SAN)formed during the decoction process of traditional Chinese medicine(TCM)exhibit non-uniform particle sizes and a tendency for aggregation.Our group found that the p H-driven method...The self-assembled nanoparticles(SAN)formed during the decoction process of traditional Chinese medicine(TCM)exhibit non-uniform particle sizes and a tendency for aggregation.Our group found that the p H-driven method can improve the self-assembly phenomenon of Herpetospermum caudigerum Wall.,and the SAN exhibited uniform particle size and demonstrated good stability.In this paper,we analyzed the interactions between the main active compound,herpetrione(Her),and its main carrier,Herpetospermum caudigerum Wall.polysaccharide(HCWP),along with their self-assembly mechanisms under different p H values.The binding constants of Her and HCWP increase with rising p H,leading to the formation of Her-HCWP SAN with a smaller particle size,higher zeta potential,and improved thermal stability.While the contributions of hydrogen bonding and electrostatic attraction to the formation of Her-HCWP SAN increase with rising p H,the hydrophobic force consistently plays a dominant role.This study enhances our scientific understanding of the self-assembly phenomenon of TCM improved by p H driven method.展开更多
The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium...The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium alginate-based multilayer film is fabricated via a layer-by-layer(LBL)self-assembly method.With the help of superior interaction between the layers,the multilayer film possesses excellent mechanical properties(with a tensile strength of 50 MPa).Besides,the film displays outstanding water retention property(blocking moisture of 97.56%)and ultraviolet blocking property.Anthocyanin is introduced into the film to detect the food quality since it is one natural plant polyphenol that is sensitive to the pH changes ranging from 1 to 13 in food when spoilage occurs.It is noted that the film is also bacteriostatic which is desired for food packaging.This study describes a simple technique for the development of advanced multifunctional and fully biodegradable food packaging film and it is a sustainable alternative to plastic packaging.展开更多
Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to...Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to form a perfect layered structure,polymeric coating with graphene nanosheets usually needs micron-scale thickness to ensure the enhancement of corrosion protection.In this work,layer-by-layer stacked graphene nanocoatings were fabricated on stainless steel by self-assembly based on Marangoni effect.The anti-corrosion property of graphene coatings were studied through Tafel polarization curves,electrochemical impedance spectroscopy and accelerated corrosion test with extra applied voltage.The self corrosion current density of optimized three-layered graphene coated sample was one quarter of that of bare stainless steel.And the self corrosion potential of optimized sample is increased to-0.045 V.According to the results,graphene nanocoatings composed of layered nanosheets exhibits good anticorrosion property.Besides,the self-assembly method provide a promising approach to make layeredstructure coating for other researches about 2 D material nanosheets.展开更多
The increasing consciousness about the depletion of natural resources and the sustainability agenda are the major driving forces to try to reuse and recycle organic materials such as agri-food and industrial wastes.In...The increasing consciousness about the depletion of natural resources and the sustainability agenda are the major driving forces to try to reuse and recycle organic materials such as agri-food and industrial wastes.In this context,keratin fibers,as a waste from the tannery industry,represent a great opportunity for the development of green functional materials.In this paper,keratin fibers were surface functionalized using the Layer-by-Layer(LbL)deposition technique and then freeze-dried in order to obtain a lightweight,fire-resistant,and sustainable material.The LbL coating,made with chitosan and carboxymethylated cellulose nanofibers,is fundamental in enabling the formation of a self-sustained structure after freeze-drying.The prepared porous fiber networks(density 100 kg m^(-3))display a keratin fiber content greater than 95 wt%and can easily self-extinguish the flame during a flammability test in a vertical configuration.In addition,during forced combustion tests(50 kW m^(-2))the samples exhibited a reduction of 37% in heat release rate and a reduction of 75%in smoke production if compared with a commercial polyurethane foam.The results obtained represent an excellent opportunity for the development of fire-safe sustainable materials based on fiber wastes.展开更多
The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-ba...The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-based perovskite solar cells(PSCs)are limited by interfacial photocatalytic chemical reactions and energy level mismatch.Thus,phosphate-based self-assembled monolayers(SAMs)have been widely developed for delicate interfacial modification;however,they suffer from severe issues such as self-aggregation and high cost.Herein,a low-cost carboxylate-based SAM(pyrenebutyric acid,PyBA)was used to modify NiO_(x),achieving an improved surface chemical environment and interfacial properties,such as an increased Ni^(3+)/Ni2^(+)ratio,a reduced proportion of high-valence Ni^(≥3+),and better-aligned hole transport interface energy level.The introduction of PyBA also results in larger grain size,higher uniformity,and enhanced photoluminescence(PL)from the bottom of the perovskite,yielding a significant increase in efficiency from an initial 22.48%to 25.14%,while increasing the open-circuit voltage(VOC)from 1.077 to 1.192 V.Additionally,a perovskite module with an aperture area of 21 cm^(2)achieved an efficiency of 22.28%,demonstrating the excellent scalability of the PyBA treatment.Moreover,the well-modified buried interface combined with the chemical inertness and structural rigidity of pyrene ensures excellent ultraviolet(UV)stability(the target module maintained 92%of the initial efficiency after 200 h and the control device only retained 40%).展开更多
A new type of amphiphiles bearingmacrocycle such as cucurbit[7]uril(CB[7])spontaneously forms a nanomaterial in water,specifically vesicles(tACB[7]vesicles)with a positive surface charge,verified through various analy...A new type of amphiphiles bearingmacrocycle such as cucurbit[7]uril(CB[7])spontaneously forms a nanomaterial in water,specifically vesicles(tACB[7]vesicles)with a positive surface charge,verified through various analytical techniques including TIRF,DLS and TEM.Functional validation not only reveals the accessibility of the CB[7]portal on these vesicles allowing CB[7]-based host-vip interactions with various functional vip molecules such as fluorescein isothiocyanate conjugated adamantylammonium and spermine(FITC-AdA and FITC-SPM,respectively)using confocal laser scanning microscopy,but also showcases the effective internalization of tACB[7]vesicles into cancer cells with the anticancer drug oxaliplatin(OxPt),as a vip to CB[7],through in vitro cell experiments.Hence,this study provides a blueprint to impart amphiphilic properties to CB[7]through synthetic design and highlights the potential of CB[7]derivatives as a new class of unconventional amphiphiles self-assembling into functional nanomaterials for advanced drug delivery.展开更多
A significant challenge in developing block copolymer photonic crystals is constructing low-symmetric ordered phases,which are essential for achieving a complete photonic band gap.Here,we propose a promising strategy ...A significant challenge in developing block copolymer photonic crystals is constructing low-symmetric ordered phases,which are essential for achieving a complete photonic band gap.Here,we propose a promising strategy to create low-symmetric ordered morphologies by incorporating shape-anisotropic rod-like side chains into block copolymers.Using dissipative particle dynamics simulations,we demonstrate that block copolymers with longer rod-like side chains can self-assemble into a hexagonally packed columnar phase characterized by a low-symmetric rectangular cross-section.Photonic band structure calculations reveal that this low-symmetric columnar phase can exhibit a complete photonic band gap,with the gap size dependent on the aspect ratio of the rectangular cross-sections of the columns.Our findings suggest an effective approach to constructing low-symmetric photonic crystals through the self-assembly of block copolymers with shape-anisotropic segments.展开更多
Self-assembled monolayers(SAMs)are widely used as hole transport materials in inverted perovskite solar cells,offering low parasitic absorption and suitability for semitransparent and tandem solar cells.While SAMs hav...Self-assembled monolayers(SAMs)are widely used as hole transport materials in inverted perovskite solar cells,offering low parasitic absorption and suitability for semitransparent and tandem solar cells.While SAMs have shown to be promising in small-area devices(≤1 cm^(2)),their application in larger areas has been limited by a lack of knowledge regarding alternative deposition methods beyond the common spin-coating approach.Here,we compare spin-coating and upscalable methods such as thermal evaporation and spray-coating for[2-(9H-carbazol-9-yl)ethyl]phosphonic acid(2PACz),one of the most common carbazole-based SAMs.The impact of these deposition methods on the device performance is investigated,revealing that the spray-coating technique yields higher device performance.Furthermore,our work provides guidelines for the deposition of SAM materials for the fabrication of perovskite solar modules.In addition,we provide an extensive characterization of 2PACz films focusing on thermal evaporation and spray-coating methods,which allow for thicker 2PACz deposition.It is found that the optimal 2PACz deposition conditions corresponding to the highest device performances do not always correlate with the monolayer characteristics.展开更多
The optimization of hole transport layer(HTL)is crucial for achieving high efficiency and stability in inverted perovskite solar cells(PSCs)due to its role in facilitating hole transport and passivating the perovskite...The optimization of hole transport layer(HTL)is crucial for achieving high efficiency and stability in inverted perovskite solar cells(PSCs)due to its role in facilitating hole transport and passivating the perovskite bottom interface.While self-assembled monolayers(SAMs)are commonly used for this purpose,the inherent limitations of a single SAM,such as fixed energy levels and rigid structure,restrict their adaptability for different perovskite components and further efficiency enhancement.Here,we demonstrate a stepwise deposition method for SAM-based HTLs to address this issue.We regulated the energy level gradient by depositing two SAMs with distinct energy levels,while the interactions between the phosphate groups in the SAMs and perovskite effectively reduce defect density at the bottom interface of the perovskite film.The as-fabricated PSCs achieved enhanced efficiency and stability with PCEs of 25.7% and 24.0% for rigid and flexible PSCs,respectively;these devices maintain 90% of their initial PCE after 500 h of maximum power point tracking,and retain 98% of their initial PCE after 4,000 bending cycles,representing one of the most stable flexible PSCs reported to date.展开更多
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 Natural Science Foundation of China(NSFC No.52271228)the Natural Science Foundation of Shaanxi Province(No.2023-JC-ZD-21)the Doctoral Dissertation Innovation Fund of Xi'an University of Technology(No.101-252072301)。
文摘Graphitic carbon nitride(g-CN)stands out as the most promising candidate for solar energy conversion owing to its easy preparation,metal-free nature,flexible molecular structure,moderate bandgap,and excellent thermal/chemical stability.To enhance the performance of intrinsic g-CN,a supramolecular self-assembly strategy has been proposed to regulate the molecular structure of supramolecular precursors through non-covalent interactions across molecular building blocks,thereby optimizing the electronic structure of g-CN.This review provides a comprehensive overview of the recent progress in supramolecular self-assembly-derived graphitic carbon nitride(SM-CN)from both experimental and theoretical computational research in synthesis strategies,including synthesis methods and influencing factors,providing a theoretical foundation for the design of supramolecular assembly.It also discusses modification strategies,such as internal modification of the conjugated plane,interlayer optimization,and construction of heterointerfaces to improve the electronic structure of SM-CN owing to its unique layered structure.This review further summarizes the applications of SM-CN in environment and energy,including wastewater treatment,sterilization and disinfection/air purification,water splitting,H_(2)O_(2)production,organic synthesis/biomass conversion,CO_(2)reduction,photocatalytic coupling technology.Finally,perspectives and outlooks for the future development of SM-CN aim to inspire further innovation in the design and construction of high-performance SM-CN for broader applications.
基金supported by the grants from National Key R&D Program of China(No.2022YFA1104800)Shenzhen Science and Technology Program(No.JCYJ20210324124214038)+4 种基金National Natural Science Foundation of China(Nos.52072418,82300016)Natural Science Foundation of Guangdong Province(No.2023A1515140072)Shenzhen Key Laboratory of Neural Cell Reprogramming and Drug Research,Social Development Science and Technology Key Project of Dongguan(No.20231800940512)the National Medical Research Council(NMRC,No.23-0740-A0001)the Ministry of Education(MOE,No.T2EP10222-0002)of Singapore.
文摘Lysine-targeting reversible covalent inhibitors,particularly salicylaldehyde-based compounds such as the Food and Drug Administration(FDA)-approved drug Voxelotor,exhibit significant therapeutic potential but are limited by challenges including instability and off-target effects.To overcome these limitations in kinase inhibitor A5,we devised a pH-responsive prodrug strategy by masking its reactive aldehyde group with an acid-labile hydrazone linkage and enhancing intracellular delivery through conjugation with FK506.The optimized prodrug demonstrated robust antitumor efficacy in K562 tumor-bearing mice.Furthermore,the incorporation of the photosensitizer chlorin e6(Ce6)led to the formation of self-assembled nanoparticles(AKNP),which not only improved physiological stability and prolonged tumor retention but also enabled light-triggered release of A5 in conjunction with photodynamic therapy(PDT).Our study thus presents a promising prodrug self-assembly strategy that combines the on-demand release of a novel lysine-targeting,reversible covalent kinase inhibitor with PDT in clinical cancer therapy.
基金financially supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2020R1A3B2079803 and No.RS-2024-00453815),Republic of Korea。
文摘Localized high-concentration electrolytes(LHCEs)are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures.Herein,we propose a self-assembly chemical strategy into the LCHEs induced by ordered nanostructure of zwitterionic co-solutes for highly efficient and ultrastable zinc(Zn)metal batteries.Through the systematic screening of six zwitterionic compounds,3-(decyldimethylammonio)propanesulfonate salt(C_(10))with the decyl chain and zwitterions was determined as an optimum to construct quasi-spherical aggregates with a periodic length of 3.77 nm,as confirmed by comprehensive synchronous small-angle X-ray scattering,Guinier,pair distance distribution function,Porod,and other spectroscopic characterizations and molecular dynamic simulation.In particularly,this self-assembled structure in electrolyte environments was attributed to increasing the proportion of both contact and aggregated ion pairs for the formation of LHCEs as well as to providing fast and selective Zn^(2+)conducting channels and uniform solid electrolyte interfaces for facilitated charge transfer kinetics.Moreover,the preferential adsorption of the self-assembled C_(10)on the Zn(002)surface modulated the electrical double layer to suppress hydrogen evolution and corrosion reactions.Consequently,the Zn‖Zn symmetric cells in Zn(OTf)_(2)/C_(10)electrolytes showed long-term plating/stripping behaviors over 2800 h at 1 mA cm^(-2)and 1 mAh cm^(-2)as well as over 1200 h even at 5 mA cm^(-2)and 5 mAh cm^(-2)with a very high depth of discharge of 42.7%.Furthermore,the ZnllVO_(2)/CNT full cells in Zn(OTf)_(2)/C_(10)electrolytes delivered a record-high capacity of 8.10 mAh cm^(-2)at an ultrahigh cathode mass loading of 50 mg cm^(-2)after 150 cycles.
基金supported by the National Natural Science Foundation of China(No.82273919)Natural Science Foundation of Heilongjiang Province(No.LH2024H013)China Postdoctoral Science Foundation(No.2022MD723781).
文摘Constructing nanofibers with specific therapeutic effects against cancer is a challenge.Here,we present the synthesis approach and application prospects of supramolecular nanofibers,which are based on cucurbit[8]uril(CB[8])as the host and terpyridine lanthanum ions metal complex as the vip,constructed by layer-by-layer self-assembly through supramolecular interaction.Moreover,nanofibers with lanthanide luminescence properties exhibit surprising pH-responsive deformation properties and antibacterial behavior.In the tumor micro-environment,the dramatic reduction in the size of the nanofibers enables specific and hierarchical release of anticancer drugs in tumor cells to exert an advanced therapeutic effect.In addition,the synergistic therapeutic efficacy was achieved by reducing the excess of Gram-positive and Gram-negative bacteria surrounding tumor cells.The novel supramolecular nanofibers with sequential drug release and combined therapeutic mode provide new guidance for the synthesis of drug carrier materials and direction for the promotion of nanomaterial-mediated cancer therapy.
基金supported by the University Synergy Innovation Program of Anhui Province(GXXT-2021-059)the National Key Research and Development Program of China(2023YFD1702102)the Major Natural Science Research Project of Anhui Universities(2023AH040143).
文摘Herbicides are indispensable for safeguarding global crop production,yet their effectiveness is often undermined by extensive environmental losses during application.Using herbicide Diuron as a model compound,we developed hierarchical nanoparticles constructed through host-vip molecular recognition followed by electrostatic coassembly,yielding a formulation that unites high delivery efficiency with enhanced environmental compatibility.Relative to conventional wettable powders,these nanoparticles exhibited temperature-responsive release behavior and significantly enhanced foliar adhesion and deposition,increasing leaf retention by more than 241.7%.They also demonstrated strong resistance to rainfall wash-off and a markedly reduced propensity for groundwater leaching,with leaching losses decreased by approximately 18.6%.Greenhouse and field evaluations further confirmed their superior weed control under practical conditions,achieving control efficacies of up to 70.1%against Abutilon theophrasti and 52.9%against Setaria faberi,compared with 53.7%and 39.1%,respectively,for the commercial formulation at the same application rate.Extensive ecotoxicological assessments encompassing seed germination,zebrafish and earthworm assays,in vitro cellular tests,and in vivo rat studies consistently revealed an improved safety profile compared with commercial and technical formulations.Together,these results highlight hierarchical self-assembled nanoparticles as a promising platform for next-generation herbicide delivery that combines high target utilization with lower environmental impact and greater sustainability.
基金supported by the National Key Research and Development Program of China(No.2023YFB4202501)the National Natural Science Foundation of China(No.62274026)+1 种基金the Sichuan Science and Technology Program(No.2024NSFSC0216)the Fundamental Research Funds for the Central Universities of China(ZYGX2025XT010 and ZYGX2025TS005)。
文摘Monolithic perovskite-silicon tandem solar cells(PSTs)represent a promising avenue for surpassing the efficiency limits of single-junction photovoltaics,but their performance is still hampered by significant open-circuit voltage(V_(OC))losses arising from interfacial inefficient charge extraction and non-radiative recombination.To mitigate these losses,we introduce a push–pull bridging molecule,4′-amino-[1,1′-bi phenyl]-4-carboxylic acid(ABBA),which forms a 2 PACz/ABBA assembly through phosphor-amidate.The 2 PACz/ABBA assembly suppresses 2 PACz aggregation caused byπ-πstacking while simultaneously enhancing the interfacial dipole moment,thereby facilitating the built-in electric field to promote more efficient hole extraction.Meanwhile,–COOH groups within ABBA passivate deep-level defects(e.g.,uncoordinated Pb^(2+))at buried perovskite interface and contribute to the growth of perovskite films with large grains,reduced residual stress,and optimized energy level alignment.Consequently,the champion tandem device fabricated via the two-step sequential vapor-solution process achieves a PCE of 30.37% and an open-circuit voltage(V_(OC))of 1.891 V.Furthermore,unencapsulated devices maintain 88%of their initial performance after 1000 h under maximum power point tracking(MPPT),highlighting its superior stability.
基金supported by the National Natural Science Foundation of China(61904053,22279033)the National Key Research and Development Program of China(2023YFB4204502)+2 种基金the 111 Project(B16016)the Fundamental Research Funds for the Central Universities(2025MS043)the Special Foundation for Carbon Peak Carbon Neutralization Technology Innovation Program of Jiangsu Province(BE2022026).
文摘Molecular tailoring of self-assembled hole-transporting monolayers(SAMs)has been proven as an efficient approach for improving the device performance of inverted perovskite solar cells.Herein,a novel SAM with extended conjugation is designed and synthesized,named NaPh-4PACz.Compared to Ph-4PACz,NaPh-4PACz exhibits a larger adsorption energy with the ITO substrate,enabling the formation of a more uniform and dense film,thereby preventing direct contact between the perovskite and ITO.Additionally,NaPh-4PACz also has a stronger interaction with the perovskite,which can reduce buried interface defects and suppress non-radiative recombination.Consequently,NaPh-4PACz-based devices achieved a power conversion efficiency of 25.48%due to their interfacial“adhesive”ability.Importantly,the stability of the NaPh-4PACz-based devices was significantly improved.
基金supported by the National Natural Science Foundation of China(52071191)Shandong University of Science and Technology(SDUST)Research Fund(2014TDJH104)the Science and Technology Innovation Fund of SDUST for graduate students(SDKDYC180371)。
文摘Magnesium(Mg)and its alloys are considered as ideal biodegradable materials due to their excellent mechanical properties and biocompatibility.In order to improve the surface properties to allow better adaptation to the surrounding tissue of the body,surface modification has played a significant role in satisfying multiple clinical requirements such as corrosion resistance,biocompatibility,and antibacterial ability.Here,layer-by-layer(LbL)self-assembly,which can be applied for biodegradable Mg alloys due to its extensive choice of usable units,holds great promise among all the surface techniques.In this review,the mechanisms of the driving force(i.e.,electrostatic interaction,hydrogen bonding,charge transfer interaction and covalent bonding),cuttingedge advances in preparation methods(e.g.,dipping,spraying,and spinning)and the functional properties(corrosion resistance,antibacterial activity,and biocompatibility)that could be achieved by the LbL coatings are summarized.A reasonable trend of the potential development of LbL for bioMg alloys is also proposed at the end of this article.
基金financially supported by the National Natural Science Foundation of China(No.51273063 and 51003028)the Fundamental Research Funds for the Central Universities+1 种基金the Higher School Specialized Research Fund for the Doctoral Program(No.20110074110003)111 Project Grant(No.B08021)
文摘Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （Au-NPs） with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.
文摘Orthopedic implants for the treatment of bone defects from various causes have been challenged by insufficient osseointegration,bacterial infection,oxidative stress,immune rejection,and insufficient individualized treatment.These challenges not only impact treatment outcomes but also severely impact patients’daily lives.Layer-by-Layer(LbL)serves as a simple surface coating technique,in simple terms,to functionalize implants by sequentially adsorbing oppositely charged materials onto a substrate.In orthopaedics,LbL self-assembly technology solves some of the challenges by loading various drugs or biological agents on the implant surface and controlling their release precisely to the site of bone defects in a personalized way.This review will introduce the basic principle and the development of LbL in orthopaedics,review and analyze the chemical strategy of LbL in the preparation of bone implants to ensure the stability of the implant,and introduce the use of LbL bone implants in orthopaedics in recent years.The application of LbL includes the realization of programmed drug delivery and sustained release,thereby promoting osseointegration and the formation of new blood vessels,antibacterial,antioxidant,etc.This review focuses on the LbL technology,involving the technology selection for the preparation of bone implants,the chemical strategies of the stability guarantee of LbL implants,the pharmacological properties,loading and release mechanisms of loaded drugs,and the molecular mechanisms of osteogenesis and angiogenesis.The aim of this review is to provide an overview of current research advances,and a prospect in this field was also described.
基金supported by the National Natural Science Foundation of China(Nos.81873092,82174074)。
文摘The self-assembled nanoparticles(SAN)formed during the decoction process of traditional Chinese medicine(TCM)exhibit non-uniform particle sizes and a tendency for aggregation.Our group found that the p H-driven method can improve the self-assembly phenomenon of Herpetospermum caudigerum Wall.,and the SAN exhibited uniform particle size and demonstrated good stability.In this paper,we analyzed the interactions between the main active compound,herpetrione(Her),and its main carrier,Herpetospermum caudigerum Wall.polysaccharide(HCWP),along with their self-assembly mechanisms under different p H values.The binding constants of Her and HCWP increase with rising p H,leading to the formation of Her-HCWP SAN with a smaller particle size,higher zeta potential,and improved thermal stability.While the contributions of hydrogen bonding and electrostatic attraction to the formation of Her-HCWP SAN increase with rising p H,the hydrophobic force consistently plays a dominant role.This study enhances our scientific understanding of the self-assembly phenomenon of TCM improved by p H driven method.
基金National Undergraduate Training Program for Innovation and Entrepreneurship of China (Grant No.202210288027).
文摘The abuse of plastic food packaging has brought about severe white pollution issues around the world.Developing green and sustainable biomass packaging is an effective way to solve this problem.Hence,a chitosan/sodium alginate-based multilayer film is fabricated via a layer-by-layer(LBL)self-assembly method.With the help of superior interaction between the layers,the multilayer film possesses excellent mechanical properties(with a tensile strength of 50 MPa).Besides,the film displays outstanding water retention property(blocking moisture of 97.56%)and ultraviolet blocking property.Anthocyanin is introduced into the film to detect the food quality since it is one natural plant polyphenol that is sensitive to the pH changes ranging from 1 to 13 in food when spoilage occurs.It is noted that the film is also bacteriostatic which is desired for food packaging.This study describes a simple technique for the development of advanced multifunctional and fully biodegradable food packaging film and it is a sustainable alternative to plastic packaging.
基金the financial support by the National Natural Science Foundation of China(Nos.51573201,51501209,201675165 and 61901460)NSFC-Zhejiang Joint Fund for the Integration of Industrialization and Informatization(No.U1709205)+7 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA22000000)Scientific Instrument Developing Project of the Chinese Academy of Sciences(No.YZ201640)Science and Technology Major Project of Ningbo(Nos.2016S1002 and 2016B10038)International S&T Cooperation Program of Ningbo(No.2017D10016)China Postdoctoral Science Foundation(No.2019M653125)for financial supportthe Chinese Academy of Sciences for Hundred Talents ProgramChinese Central Government for Thousand Young Talents Program3315 Program of Ningbo。
文摘Graphene nanosheets are widely used in anti-corrosion polymeric coating as filler,owing to the excellent electrochemical inertness and barrier property.However,as the arrangement of graphene nanosheets is difficult to form a perfect layered structure,polymeric coating with graphene nanosheets usually needs micron-scale thickness to ensure the enhancement of corrosion protection.In this work,layer-by-layer stacked graphene nanocoatings were fabricated on stainless steel by self-assembly based on Marangoni effect.The anti-corrosion property of graphene coatings were studied through Tafel polarization curves,electrochemical impedance spectroscopy and accelerated corrosion test with extra applied voltage.The self corrosion current density of optimized three-layered graphene coated sample was one quarter of that of bare stainless steel.And the self corrosion potential of optimized sample is increased to-0.045 V.According to the results,graphene nanocoatings composed of layered nanosheets exhibits good anticorrosion property.Besides,the self-assembly method provide a promising approach to make layeredstructure coating for other researches about 2 D material nanosheets.
基金supported by the Italian Ministry of University(MIUR)call PRIN 2017 with the project“PANACEA:A technology Platform for the sustainable recovery and advanced use of NAnostructured CEllulose from Agro-food residues”(grant No.2017LEPH3M).
文摘The increasing consciousness about the depletion of natural resources and the sustainability agenda are the major driving forces to try to reuse and recycle organic materials such as agri-food and industrial wastes.In this context,keratin fibers,as a waste from the tannery industry,represent a great opportunity for the development of green functional materials.In this paper,keratin fibers were surface functionalized using the Layer-by-Layer(LbL)deposition technique and then freeze-dried in order to obtain a lightweight,fire-resistant,and sustainable material.The LbL coating,made with chitosan and carboxymethylated cellulose nanofibers,is fundamental in enabling the formation of a self-sustained structure after freeze-drying.The prepared porous fiber networks(density 100 kg m^(-3))display a keratin fiber content greater than 95 wt%and can easily self-extinguish the flame during a flammability test in a vertical configuration.In addition,during forced combustion tests(50 kW m^(-2))the samples exhibited a reduction of 37% in heat release rate and a reduction of 75%in smoke production if compared with a commercial polyurethane foam.The results obtained represent an excellent opportunity for the development of fire-safe sustainable materials based on fiber wastes.
基金Y.Zhan acknowledges funding support from the National Key Research and Development Program of China(2022YFE0137400)the National Natural Science Foundation of China(62274040)+5 种基金A.Yu acknowledges funding support from the National Natural Science Foundation of China(62304046)the National Key Research and Development Program of China(2022YFB2802802)the Key Laboratory of Rare Earths,Ganjiang Innovation Academy,Chinese Academy of SciencesX.Zhang acknowledges funding from the China Postdoctoral Science Foundation(GZC20230463)X.Li acknowledges funding from the China Postdoctoral Science Foundation(GZC20230461)We also acknowledge support from the Shanghai Science and Technology Innovation Action Plan 2023 Special Project for Supporting Carbon Peak Carbon Neutrality Project(23DZ1200400).
文摘The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-based perovskite solar cells(PSCs)are limited by interfacial photocatalytic chemical reactions and energy level mismatch.Thus,phosphate-based self-assembled monolayers(SAMs)have been widely developed for delicate interfacial modification;however,they suffer from severe issues such as self-aggregation and high cost.Herein,a low-cost carboxylate-based SAM(pyrenebutyric acid,PyBA)was used to modify NiO_(x),achieving an improved surface chemical environment and interfacial properties,such as an increased Ni^(3+)/Ni2^(+)ratio,a reduced proportion of high-valence Ni^(≥3+),and better-aligned hole transport interface energy level.The introduction of PyBA also results in larger grain size,higher uniformity,and enhanced photoluminescence(PL)from the bottom of the perovskite,yielding a significant increase in efficiency from an initial 22.48%to 25.14%,while increasing the open-circuit voltage(VOC)from 1.077 to 1.192 V.Additionally,a perovskite module with an aperture area of 21 cm^(2)achieved an efficiency of 22.28%,demonstrating the excellent scalability of the PyBA treatment.Moreover,the well-modified buried interface combined with the chemical inertness and structural rigidity of pyrene ensures excellent ultraviolet(UV)stability(the target module maintained 92%of the initial efficiency after 200 h and the control device only retained 40%).
基金supported by the National Research Foundation of Korea[NRF-2023–00211758].
文摘A new type of amphiphiles bearingmacrocycle such as cucurbit[7]uril(CB[7])spontaneously forms a nanomaterial in water,specifically vesicles(tACB[7]vesicles)with a positive surface charge,verified through various analytical techniques including TIRF,DLS and TEM.Functional validation not only reveals the accessibility of the CB[7]portal on these vesicles allowing CB[7]-based host-vip interactions with various functional vip molecules such as fluorescein isothiocyanate conjugated adamantylammonium and spermine(FITC-AdA and FITC-SPM,respectively)using confocal laser scanning microscopy,but also showcases the effective internalization of tACB[7]vesicles into cancer cells with the anticancer drug oxaliplatin(OxPt),as a vip to CB[7],through in vitro cell experiments.Hence,this study provides a blueprint to impart amphiphilic properties to CB[7]through synthetic design and highlights the potential of CB[7]derivatives as a new class of unconventional amphiphiles self-assembling into functional nanomaterials for advanced drug delivery.
基金financially supported by the National Key R&D Program of China(No.2022YFB3707300)the National Natural Science Foundation of China(Nos.22133002,22373089)the support from the Excellent Youth Foundation of Henan Scientific Committee(No.242300421032).
文摘A significant challenge in developing block copolymer photonic crystals is constructing low-symmetric ordered phases,which are essential for achieving a complete photonic band gap.Here,we propose a promising strategy to create low-symmetric ordered morphologies by incorporating shape-anisotropic rod-like side chains into block copolymers.Using dissipative particle dynamics simulations,we demonstrate that block copolymers with longer rod-like side chains can self-assemble into a hexagonally packed columnar phase characterized by a low-symmetric rectangular cross-section.Photonic band structure calculations reveal that this low-symmetric columnar phase can exhibit a complete photonic band gap,with the gap size dependent on the aspect ratio of the rectangular cross-sections of the columns.Our findings suggest an effective approach to constructing low-symmetric photonic crystals through the self-assembly of block copolymers with shape-anisotropic segments.
基金supported by funding from the Energy Materials and Surface Sciences Unit of the Okinawa Institute of Science and Technology Graduate University,the OIST R&D Cluster Research Program,the OIST Proof of Concept(POC)Program,the JSPS KAKENHI Grant Number JP21F21754 and Alexander von Humboldt Foundation。
文摘Self-assembled monolayers(SAMs)are widely used as hole transport materials in inverted perovskite solar cells,offering low parasitic absorption and suitability for semitransparent and tandem solar cells.While SAMs have shown to be promising in small-area devices(≤1 cm^(2)),their application in larger areas has been limited by a lack of knowledge regarding alternative deposition methods beyond the common spin-coating approach.Here,we compare spin-coating and upscalable methods such as thermal evaporation and spray-coating for[2-(9H-carbazol-9-yl)ethyl]phosphonic acid(2PACz),one of the most common carbazole-based SAMs.The impact of these deposition methods on the device performance is investigated,revealing that the spray-coating technique yields higher device performance.Furthermore,our work provides guidelines for the deposition of SAM materials for the fabrication of perovskite solar modules.In addition,we provide an extensive characterization of 2PACz films focusing on thermal evaporation and spray-coating methods,which allow for thicker 2PACz deposition.It is found that the optimal 2PACz deposition conditions corresponding to the highest device performances do not always correlate with the monolayer characteristics.
基金supported by the National Natural Science Foundation of China(22305119,12204234)the Natural Science Foundation of Jiangsu Province(BK20220878)+3 种基金the Fundamental Research Funds for the Central Universities(NS2023059)the China Postdoctoral Science Foundation(2022TQ0157,2023M741695)the Liaoning University Talent Introduction Research Startup Project(d295000048)the Center for Microscopy and Analysis of Nanjing University of Aeronautics and Astronautics for characterization support。
文摘The optimization of hole transport layer(HTL)is crucial for achieving high efficiency and stability in inverted perovskite solar cells(PSCs)due to its role in facilitating hole transport and passivating the perovskite bottom interface.While self-assembled monolayers(SAMs)are commonly used for this purpose,the inherent limitations of a single SAM,such as fixed energy levels and rigid structure,restrict their adaptability for different perovskite components and further efficiency enhancement.Here,we demonstrate a stepwise deposition method for SAM-based HTLs to address this issue.We regulated the energy level gradient by depositing two SAMs with distinct energy levels,while the interactions between the phosphate groups in the SAMs and perovskite effectively reduce defect density at the bottom interface of the perovskite film.The as-fabricated PSCs achieved enhanced efficiency and stability with PCEs of 25.7% and 24.0% for rigid and flexible PSCs,respectively;these devices maintain 90% of their initial PCE after 500 h of maximum power point tracking,and retain 98% of their initial PCE after 4,000 bending cycles,representing one of the most stable flexible PSCs reported to date.
