For the commercialization of perovskite solar cells(PSCs), it is more appealing to develop high-performance simplified PSCs where perovskite films are just sandwiched between the back and front electrodes, in order to...For the commercialization of perovskite solar cells(PSCs), it is more appealing to develop high-performance simplified PSCs where perovskite films are just sandwiched between the back and front electrodes, in order to simplify the fabrication process and to reduce the cost. However, to date, this kind of devices shows rather low performance, and there are few researches on this subject.Herein, we report on a kind of compact PSCs(CPSCs) that are free of independent charge transport layers(CTLs). The devices are realized by the use of organic monolayer-modified effective electrodes, along with the use of [6,6]-phenyl-C61-butyric acid methyl ester(PCBM)-assisted anti-solvent technique to obtain ultra-thin(~10 nm) PCBM-embedded perovskite films. Compared to control devices, CPSCs achieve a promising champion power conversion efficiency of 19.6% with largely reduced hysteresis. Moreover, the unencapsulated CPSC shows good stability under ambient atmosphere, with only 10% efficiency loss after 60 days’ storage. This work indicates that, by delicate design, CPSCs with smaller materials consumption in device architecture can perform competitively as conventional PSCs. Further reduction in the actual usage of costly CTL materials can be expected upon our CPSCs by developing more facile and economic methods to prepare ultra-thin CTLs.展开更多
Ionomer impregnation represents a milestone in the evolution of polymer electrolyte fuel cell （PEFC） catalyst layers. Ionomer acts as the binder, facilitates proton transport, and thereby drastically improves cataly...Ionomer impregnation represents a milestone in the evolution of polymer electrolyte fuel cell （PEFC） catalyst layers. Ionomer acts as the binder, facilitates proton transport, and thereby drastically improves catalyst utilization and effectiveness. However, advanced morpho- logical and functional characterizations have revealed that up to 60% of Pt nanoparticles can be trapped in the micropores of carbon support particles. Ionomer clusters and oxygen molecules can hardly enter into micropores, leading to low Pt utilization and effectiveness. Moreover, the ionomer thin-films covering Pt nanoparticles can cause significant mass transport loss especially at high current densities. Ionomer-free ultra-thin catalyst layers （UTCLs） emerge as a promising alternative to reduce Pt loading by improving catalyst utilization and effectiveness, while theoretical issues such as the proton conduction mechan- ism remain puzzling and practical issues such as the rather narrow operation window remain unsettled. At present, the development of PEFC catalyst layer has come to a crossroads： staying ionomer-impregnated or going iono- mer-free. It is always beneficial to look back into the past when coming to a crossroads. This paper addresses the characterization and modeling of both the conventional ionomer-impregnated catalyst layer and the emerging ionomer-free UTCLs, featuring advances in characterizing microscale distributions of Pt particles, ionomer, support particles and unraveling their interactions; advances in fundamental understandings of proton conduction and flooding behaviors in ionomer-free UTCLs; advances in modeling of conventional catalyst layers and especially UTCLs; and discussions on high-impact research topics in characterizing and modeling of catalyst layers.展开更多
The efficiency and stability of typical three-dimensional(3D)MAPbI_(3)perovskite-based solar cells are highly restricted,due to the weak interaction between methylammonium(MA^(+))and[PbI 6]4-octahedra in the 3D struct...The efficiency and stability of typical three-dimensional(3D)MAPbI_(3)perovskite-based solar cells are highly restricted,due to the weak interaction between methylammonium(MA^(+))and[PbI 6]4-octahedra in the 3D structure,which can cause the ion migration and the related defects.Here,we found that the in situ-grown perovskitoid TEAPbI_(3)layer on 3D MAPbI_(3)can inhibit the MA^(+)migration in a polar solvent,thus enhancing the thermal and moisture stability of perovskite films.The crystal structure and orientation of TEAPbI_(3)are reported for the first time by single crystal and synchrotron radiation analysis.The ultra-thin perovskitoid layer can reduce the trap states and accelerate photo-carrier diffusion in perovskite solar cells,as confirmed by ultra-fast spectroscopy.The power conversion efficiency of TEAPbI_(3)-MAPbI_(3)based solar cells increases from 18.87%to 21.79%with enhanced stability.This work suggests that passivation and stabilization by in situ-grown perovskitoid can be a promising strategy for efficient and stable perovskite solar cells.展开更多
基金supported by the Guangdong High-level Personnel of Special Support Program-Outstanding young scholar in science and technology innovation(Grant No.2015TQ01C543)the National Key Research and Development Project funding from the Ministry of Science and Technology of China(Grants Nos.2016YFA0202400 and 2016YFA0202404)+3 种基金the Peacock Team Project funding from Shenzhen Science and Technology Innovation Committee(Grant No.KQTD2015033110182370)the National Natural Science Foundation of China(Grant No.51776094)the Guangdong Natural Science Funds for Distinguished Young Scholars(Grant No.2015A030306044)the Guangdong-Hong Kong joint innovation project(Grant No.2016A050503012)
文摘For the commercialization of perovskite solar cells(PSCs), it is more appealing to develop high-performance simplified PSCs where perovskite films are just sandwiched between the back and front electrodes, in order to simplify the fabrication process and to reduce the cost. However, to date, this kind of devices shows rather low performance, and there are few researches on this subject.Herein, we report on a kind of compact PSCs(CPSCs) that are free of independent charge transport layers(CTLs). The devices are realized by the use of organic monolayer-modified effective electrodes, along with the use of [6,6]-phenyl-C61-butyric acid methyl ester(PCBM)-assisted anti-solvent technique to obtain ultra-thin(~10 nm) PCBM-embedded perovskite films. Compared to control devices, CPSCs achieve a promising champion power conversion efficiency of 19.6% with largely reduced hysteresis. Moreover, the unencapsulated CPSC shows good stability under ambient atmosphere, with only 10% efficiency loss after 60 days’ storage. This work indicates that, by delicate design, CPSCs with smaller materials consumption in device architecture can perform competitively as conventional PSCs. Further reduction in the actual usage of costly CTL materials can be expected upon our CPSCs by developing more facile and economic methods to prepare ultra-thin CTLs.
文摘Ionomer impregnation represents a milestone in the evolution of polymer electrolyte fuel cell （PEFC） catalyst layers. Ionomer acts as the binder, facilitates proton transport, and thereby drastically improves catalyst utilization and effectiveness. However, advanced morpho- logical and functional characterizations have revealed that up to 60% of Pt nanoparticles can be trapped in the micropores of carbon support particles. Ionomer clusters and oxygen molecules can hardly enter into micropores, leading to low Pt utilization and effectiveness. Moreover, the ionomer thin-films covering Pt nanoparticles can cause significant mass transport loss especially at high current densities. Ionomer-free ultra-thin catalyst layers （UTCLs） emerge as a promising alternative to reduce Pt loading by improving catalyst utilization and effectiveness, while theoretical issues such as the proton conduction mechan- ism remain puzzling and practical issues such as the rather narrow operation window remain unsettled. At present, the development of PEFC catalyst layer has come to a crossroads： staying ionomer-impregnated or going iono- mer-free. It is always beneficial to look back into the past when coming to a crossroads. This paper addresses the characterization and modeling of both the conventional ionomer-impregnated catalyst layer and the emerging ionomer-free UTCLs, featuring advances in characterizing microscale distributions of Pt particles, ionomer, support particles and unraveling their interactions; advances in fundamental understandings of proton conduction and flooding behaviors in ionomer-free UTCLs; advances in modeling of conventional catalyst layers and especially UTCLs; and discussions on high-impact research topics in characterizing and modeling of catalyst layers.
基金This work was supported by the NSFC(Grant 51861145101,21777096,22025505)Program of Shanghai Academic Technology Research Leader(Grant 20XD1422200)+1 种基金Cultivating fund of Frontiers Science Center for Transformative Molecules(2019PT02)China Postdoctoral Science Foundation(2020M671110).
文摘The efficiency and stability of typical three-dimensional(3D)MAPbI_(3)perovskite-based solar cells are highly restricted,due to the weak interaction between methylammonium(MA^(+))and[PbI 6]4-octahedra in the 3D structure,which can cause the ion migration and the related defects.Here,we found that the in situ-grown perovskitoid TEAPbI_(3)layer on 3D MAPbI_(3)can inhibit the MA^(+)migration in a polar solvent,thus enhancing the thermal and moisture stability of perovskite films.The crystal structure and orientation of TEAPbI_(3)are reported for the first time by single crystal and synchrotron radiation analysis.The ultra-thin perovskitoid layer can reduce the trap states and accelerate photo-carrier diffusion in perovskite solar cells,as confirmed by ultra-fast spectroscopy.The power conversion efficiency of TEAPbI_(3)-MAPbI_(3)based solar cells increases from 18.87%to 21.79%with enhanced stability.This work suggests that passivation and stabilization by in situ-grown perovskitoid can be a promising strategy for efficient and stable perovskite solar cells.
