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
In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We intr...In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We introduce an in-situ targeted defect-healing strategy by incorporating butylamine formate(BAFa)ionic liquid into the spray ink.Ionic liquids,due to their long carbon chain structure,tend to target flow towards the CRE region during the droplet evaporation process.The coordination between the lone pair electrons in the C=O group of BAFa and Pb^(2+)effectively reduces defects in perovskite and suppresses non-radiative recombination losses.Simultaneously,amine ligands,which are repelled to the film surface and grain boundaries,form a thin insulating monolayer in the CRE areas,forcing charge carriers to transport through areas of the perovskite with fewer defects.This approach enables the crystallization control and defect-heal over the Cs_(0.19)FA_(0.81)PbI_(3-x-y)Br_(x)Cl_(y)perovskite films.Consequently,the champion perovskite solar cell achieved a power conversion efficiency of 22.04%,while mini-modules with an effective area of 64.8 cm^(2)reached a peak power conversion efficiency of 18.35%,demonstrating the significant potential for commercializing large-area perovskite solar cells.展开更多
Defects as non-radiative recombination centers hinder the further efficiency improvements of perovskite solar cells(PSCs).Additive engineering has been demonstrated to be an effective method for defect passivation in ...Defects as non-radiative recombination centers hinder the further efficiency improvements of perovskite solar cells(PSCs).Additive engineering has been demonstrated to be an effective method for defect passivation in perovskite films.Here,we employed(4-methoxyphenyl)potassium trifluoroborate(C_(7)H_(7)BF_(3)KO)with and K+functional groups to passivate spray-coated(FAPbI_(3))_(x)(MAPbBr_(3))_(1-x) perovskite and eliminate hysteresis.It is shown that the F of can form hydrogen bonds with the H atom in the amino group of MA+/FA+ions of perovskite,thus reducing the generation of MA+/FA+vacancies and improving device efficiency.Meanwhile,K+and reduced MA+/FA+vacancies can inhibit ion migration,thereby eliminating hysteresis.With the aid of C_(7)H_(7)BF_(3)KO,we obtained hysteresis-free PSCs with the maximum efficiency of 19.5%by spray-coating in air.Our work demonstrates that additive engineering is promising to improve the performance of spray-coated PSCs.展开更多
Although ultrablack surfaces are urgently needed in wide applications owing to their extremely low reflectance over a broadband wavelength,obtaining simultaneously the ultrablackness and mechanical robustness by simpl...Although ultrablack surfaces are urgently needed in wide applications owing to their extremely low reflectance over a broadband wavelength,obtaining simultaneously the ultrablackness and mechanical robustness by simple process technique is still a great challenge.Herein,by decoupling different light extinction effects to different layers of coating,we design an ultrablack coating that is all-sprayable in whole process.This coating presents low reflectance over visible–mid-infrared(VIS–MIR)wavelength(av.R≈1%in VIS),low multi-angle scattering(bidirectional reflection distribution function(BRDF)=10-2–10-3 sr-1),together with good substrate adhesion grade and self-cleaning ability,which are superior to most reported sprayable ultrablack surfaces.The light extinction effects of each layer are discussed.This method is also applicable in other material systems.展开更多
Superamphiphobic surfaces have attracted the attention of researchers because of their broad application prospects.Currently,superamphiphobicity is primarily achieved by minimizing the solid-liquid contact area.Over t...Superamphiphobic surfaces have attracted the attention of researchers because of their broad application prospects.Currently,superamphiphobicity is primarily achieved by minimizing the solid-liquid contact area.Over the past few decades,researchers have primarily focused on using physical deposition methods to construct superamphiphobic surfaces using fine-sized nanoparticles(<100 nm).However,porous hollow SiO_(2)particles(PH-SiO_(2)),which aretypically large spheres,have a highly hierarchical structure and can provide lower solid-liquid contact fractions than those provided byfine-sized particles.In this study,we used PH-SiO_(2)as building blocks and combined them with poly(dimethylsiloxane)to construct a mechanically robust coating on fiber by spray-coating.After chemical vapordeposition treatment,the coating exhibited excellent superamphiphobicity and could repel various liquids,covering a wide rangeof surfacetensions(27.4-72.0mN-m^(-1)).展开更多
Superhydrophobic bagasse paper was successfully engineered by facile spray coating with a zeolitic imidazolate framework composite modified by 3,3,3-trifluoropropyltrimethoxysilane(FAS)and used as a filter membrane wi...Superhydrophobic bagasse paper was successfully engineered by facile spray coating with a zeolitic imidazolate framework composite modified by 3,3,3-trifluoropropyltrimethoxysilane(FAS)and used as a filter membrane with special wettability for oil/water separation.Surface characteristics such as surface morphology,surface moieties,roughness,and wettability were observed.The addition of FAS decreased the apparent surface energy between solid surfaces and liquids with a polar contribution of surface free energy as low as 0 mN m−1.The formation of the FAS layer was confirmed by transmission electron microscopy and X-ray photoelectron spectroscopy core-level spectra.Three-dimensional surface topography revealed an increase in the spray coating cycle that enhanced the hydrophobicity of the coated paper.The results confirmed that not only microstructures but also the presence of functional groups with low surface energy(such as FAS)can promote surface hydrophobicity.The spray-coated paper with FAS/ZIF in the presence of a small amount of nanocellulose provided a superhydrophobic surface after the first spray cycle.The separation efficiency was up to 85%and was slightly affected by oil viscosity.Moreover,this can be used as a filter membrane for water-in-oil emulsions.In the present work,simple spray-coated paper is a promising candidate material for gravity-driven oil/water separation and water repellent coating.展开更多
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(U21A20171,U20A20245)Natural Scienceof Hubei Province(2023AFA010)Independent Innovation Projects of the Hubei Longzhong Laboratory。
文摘In the process of spraying coating perovskite films,the"coffee ring"effect(CRE)leads to the problem of excessive organic ammonium salt accumulation in local areas that cannot be completely eliminated.We introduce an in-situ targeted defect-healing strategy by incorporating butylamine formate(BAFa)ionic liquid into the spray ink.Ionic liquids,due to their long carbon chain structure,tend to target flow towards the CRE region during the droplet evaporation process.The coordination between the lone pair electrons in the C=O group of BAFa and Pb^(2+)effectively reduces defects in perovskite and suppresses non-radiative recombination losses.Simultaneously,amine ligands,which are repelled to the film surface and grain boundaries,form a thin insulating monolayer in the CRE areas,forcing charge carriers to transport through areas of the perovskite with fewer defects.This approach enables the crystallization control and defect-heal over the Cs_(0.19)FA_(0.81)PbI_(3-x-y)Br_(x)Cl_(y)perovskite films.Consequently,the champion perovskite solar cell achieved a power conversion efficiency of 22.04%,while mini-modules with an effective area of 64.8 cm^(2)reached a peak power conversion efficiency of 18.35%,demonstrating the significant potential for commercializing large-area perovskite solar cells.
基金the National Natural Science Foundation of China(51861145101).
文摘Defects as non-radiative recombination centers hinder the further efficiency improvements of perovskite solar cells(PSCs).Additive engineering has been demonstrated to be an effective method for defect passivation in perovskite films.Here,we employed(4-methoxyphenyl)potassium trifluoroborate(C_(7)H_(7)BF_(3)KO)with and K+functional groups to passivate spray-coated(FAPbI_(3))_(x)(MAPbBr_(3))_(1-x) perovskite and eliminate hysteresis.It is shown that the F of can form hydrogen bonds with the H atom in the amino group of MA+/FA+ions of perovskite,thus reducing the generation of MA+/FA+vacancies and improving device efficiency.Meanwhile,K+and reduced MA+/FA+vacancies can inhibit ion migration,thereby eliminating hysteresis.With the aid of C_(7)H_(7)BF_(3)KO,we obtained hysteresis-free PSCs with the maximum efficiency of 19.5%by spray-coating in air.Our work demonstrates that additive engineering is promising to improve the performance of spray-coated PSCs.
基金supported by the National Natural Science Foundation of China(Nos.11832010,11890682 and 21721002)the National Key Basic Research Program of China(No.2018YFA0208403)the Austrian-Chinese Cooperative Research and Development Projects(No.GJHZ2043),Chinese Academy of Sciences.
文摘Although ultrablack surfaces are urgently needed in wide applications owing to their extremely low reflectance over a broadband wavelength,obtaining simultaneously the ultrablackness and mechanical robustness by simple process technique is still a great challenge.Herein,by decoupling different light extinction effects to different layers of coating,we design an ultrablack coating that is all-sprayable in whole process.This coating presents low reflectance over visible–mid-infrared(VIS–MIR)wavelength(av.R≈1%in VIS),low multi-angle scattering(bidirectional reflection distribution function(BRDF)=10-2–10-3 sr-1),together with good substrate adhesion grade and self-cleaning ability,which are superior to most reported sprayable ultrablack surfaces.The light extinction effects of each layer are discussed.This method is also applicable in other material systems.
基金the Natural Science Foundation of Zhejiang Province(LZ22C100002)the 521 Talent Project of Zhejiang Sci-Tech Universityfor providingfinancial support.
文摘Superamphiphobic surfaces have attracted the attention of researchers because of their broad application prospects.Currently,superamphiphobicity is primarily achieved by minimizing the solid-liquid contact area.Over the past few decades,researchers have primarily focused on using physical deposition methods to construct superamphiphobic surfaces using fine-sized nanoparticles(<100 nm).However,porous hollow SiO_(2)particles(PH-SiO_(2)),which aretypically large spheres,have a highly hierarchical structure and can provide lower solid-liquid contact fractions than those provided byfine-sized particles.In this study,we used PH-SiO_(2)as building blocks and combined them with poly(dimethylsiloxane)to construct a mechanically robust coating on fiber by spray-coating.After chemical vapordeposition treatment,the coating exhibited excellent superamphiphobicity and could repel various liquids,covering a wide rangeof surfacetensions(27.4-72.0mN-m^(-1)).
基金the Thailand Research Fund under the Distinguished Professor Grant No.DPG6080001 for Professor Suda Kiatkamjornwong,Thammasat University Research Fund(Contract no.TUFT 81/2564)Thammasat University Research Unit in Bioenergy and Catalysis.
文摘Superhydrophobic bagasse paper was successfully engineered by facile spray coating with a zeolitic imidazolate framework composite modified by 3,3,3-trifluoropropyltrimethoxysilane(FAS)and used as a filter membrane with special wettability for oil/water separation.Surface characteristics such as surface morphology,surface moieties,roughness,and wettability were observed.The addition of FAS decreased the apparent surface energy between solid surfaces and liquids with a polar contribution of surface free energy as low as 0 mN m−1.The formation of the FAS layer was confirmed by transmission electron microscopy and X-ray photoelectron spectroscopy core-level spectra.Three-dimensional surface topography revealed an increase in the spray coating cycle that enhanced the hydrophobicity of the coated paper.The results confirmed that not only microstructures but also the presence of functional groups with low surface energy(such as FAS)can promote surface hydrophobicity.The spray-coated paper with FAS/ZIF in the presence of a small amount of nanocellulose provided a superhydrophobic surface after the first spray cycle.The separation efficiency was up to 85%and was slightly affected by oil viscosity.Moreover,this can be used as a filter membrane for water-in-oil emulsions.In the present work,simple spray-coated paper is a promising candidate material for gravity-driven oil/water separation and water repellent coating.