While 2D/3D heterostructures are widely employed to improve the stability of perovskite optoelectronic devices,their effectiveness is fundamentally governed by the crystallinity of the interfacial structure -a factor ...While 2D/3D heterostructures are widely employed to improve the stability of perovskite optoelectronic devices,their effectiveness is fundamentally governed by the crystallinity of the interfacial structure -a factor often overlooked.Disordered interfaces exhibit thermodynamic metastability,where ion diffusion induces sequential phase transitions from low-n to high-n phases.Here,we construct atomically ordered 2D/3D interfaces using phase-pure 2D perovskite capping layers,which reduce the interfacial phase transition rate by 95%and effectively suppress ion migration.As a result,devices exhibit outstanding operational stability,retaining over 99%of their initial power conversion efficiency after 1500 h of continuous operation,along with excellent thermal durability at 85℃.These findings identify interfacial order as a critical parameter for regulating ion dynamics and phase behavior,providing a robust design principle for achieving high-efficiency,long-lifetime perovskite technologies.展开更多
The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process o...The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.展开更多
Perovskite solar cells(PSCs)incorporating 2D/3D heterostructures have exhibited remarkable improvements in both power conversion efficiency and operational stability.Nevertheless,the prevalent spin-coating fabrication...Perovskite solar cells(PSCs)incorporating 2D/3D heterostructures have exhibited remarkable improvements in both power conversion efficiency and operational stability.Nevertheless,the prevalent spin-coating fabrication technique presents formidable challenges for scalable manufacturing processes.Herein,we present a blade-coating compatible methodology for fabricating highperformance 2D/3D PSCs utilizing a low-volatility t-amyl alcohol(t-AmOH)-dimethylformamide(DMF)mixed solvent system.Through systematic materials characterization and comprehensive device performance analysis,we demonstrate that this approach facilitates uniform spatial distribution of butylammonium iodide(BAI)organic spacers,thereby promoting the formation of a high-quality 2D/3D perovskite architecture characterized by enhanced crystallinity and substantially reduced defect density.The optimized device achieves a champion power conversion efficiency of 22.25%while demonstrating exceptional operational stability,retaining 83%of its initial performance after prolonged exposure under ambient conditions(45%relative humidity)for 1000 h.展开更多
基金funding supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB1140000)National Natural Science Foundation of China(22379156,U23A20141)+1 种基金Qingdao New Energy Shandong Laboratory(QIBEBT/SEI/QNESL S202305)Key R&D Program of Shandong Province,China(2024SFGC0102)。
文摘While 2D/3D heterostructures are widely employed to improve the stability of perovskite optoelectronic devices,their effectiveness is fundamentally governed by the crystallinity of the interfacial structure -a factor often overlooked.Disordered interfaces exhibit thermodynamic metastability,where ion diffusion induces sequential phase transitions from low-n to high-n phases.Here,we construct atomically ordered 2D/3D interfaces using phase-pure 2D perovskite capping layers,which reduce the interfacial phase transition rate by 95%and effectively suppress ion migration.As a result,devices exhibit outstanding operational stability,retaining over 99%of their initial power conversion efficiency after 1500 h of continuous operation,along with excellent thermal durability at 85℃.These findings identify interfacial order as a critical parameter for regulating ion dynamics and phase behavior,providing a robust design principle for achieving high-efficiency,long-lifetime perovskite technologies.
基金financial support provided by the Sichuan Science and Technology Program(No.2022NSFSC0226)Sichuan Science and Technology Program(No.2023ZYD0163)+6 种基金the Production-Education Integration Demonstration Project of Sichuan Provincethe Photovoltaic Industry Production-Education Integration Comprehensive Demonstration Base of Sichuan Province(Sichuan Financial Education[2022]No.106)China Tianfu Yongxing Laboratory Science and Technology Key Project(2023KJGG15)National Key Research and Development Program of China(2022YFB3803300)Beijing Natural Science Foundation(IS23037)the Department for Energy Security and Net Zero(project ID:NEXTCCUS)the ACT program(Accelerating CCS Technologies,Horizon2020 project NO.691712)。
文摘The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.
基金supported by ational Natural Science Foundation of China(Nos.62405293,62301509,62304209)Key Research and Development Program of Shanxi Province(No.202302030201001)Fundamental Research Program of Shanxi Province(Nos.202303021212191,202203021222079,20210302123203,202103021223185).
文摘Perovskite solar cells(PSCs)incorporating 2D/3D heterostructures have exhibited remarkable improvements in both power conversion efficiency and operational stability.Nevertheless,the prevalent spin-coating fabrication technique presents formidable challenges for scalable manufacturing processes.Herein,we present a blade-coating compatible methodology for fabricating highperformance 2D/3D PSCs utilizing a low-volatility t-amyl alcohol(t-AmOH)-dimethylformamide(DMF)mixed solvent system.Through systematic materials characterization and comprehensive device performance analysis,we demonstrate that this approach facilitates uniform spatial distribution of butylammonium iodide(BAI)organic spacers,thereby promoting the formation of a high-quality 2D/3D perovskite architecture characterized by enhanced crystallinity and substantially reduced defect density.The optimized device achieves a champion power conversion efficiency of 22.25%while demonstrating exceptional operational stability,retaining 83%of its initial performance after prolonged exposure under ambient conditions(45%relative humidity)for 1000 h.
