Functional additives have recently been regarded as emerging candidates to improve the performance and stability of perovskite solar cells(PSCs).Herein,nicotinamide(N),2-chloronicotinamide(2Cl),and 6-chloronicotinamid...Functional additives have recently been regarded as emerging candidates to improve the performance and stability of perovskite solar cells(PSCs).Herein,nicotinamide(N),2-chloronicotinamide(2Cl),and 6-chloronicotinamide(6Cl)were employed as O-ligands to facilitate the deposition of MAPbI_(3)(MA=methylammonium)and MA-free FA_(0.88)Cs_(0.12)PbI_(2.64)Br_(0.36)(FA=formamidinium)perovskite films by multifunctional anchoring.By density functional theory(DFT)calculations and ultraviolet photoelectron spectroscopy(UPS)measurements,it is identified that the highest occupied molecular orbital(HOMO)level for additive modified MAPbI_(3)perovskite could reduce the voltage deficit for hole extraction.Moreover,due to the most favorable charge distribution and significant improvements in charge mobility and defect passivation,the power conversion efficiency(PCE)of 2Cl-MAPbI_(3)PSCs was significantly improved from 19.32%to 21.12%.More importantly,the two-dimensional grazing-incidence wide-angle X-ray scattering(GIWAXS)analysis showed that PbI_(2) defects were effectively suppressed and femtosecond transient absorption(TA)spectroscopy demonstrated that the trap-assisted recombination at grain boundaries was effectively inhibited in the 2Cl-MA-free film.As a result,the thermally stable 2Cl-MA-free PSCs achieved a remarkable PCE of 23.13%with an open-circuit voltage(V_(oc))of 1.164 V and an ultrahigh fill factor(FF)of 85.7%.Our work offers a practical strategy for further commercializing stable and efficient PSCs.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(51702038,U21A20331,51773212 and 81903743)the Sichuan Science&Technology Program(2020YFG0061)+1 种基金National Science Fund for Distinguished Young Scholars(21925506)Natural Science Foundation of Ningbo(2021J192).
文摘Functional additives have recently been regarded as emerging candidates to improve the performance and stability of perovskite solar cells(PSCs).Herein,nicotinamide(N),2-chloronicotinamide(2Cl),and 6-chloronicotinamide(6Cl)were employed as O-ligands to facilitate the deposition of MAPbI_(3)(MA=methylammonium)and MA-free FA_(0.88)Cs_(0.12)PbI_(2.64)Br_(0.36)(FA=formamidinium)perovskite films by multifunctional anchoring.By density functional theory(DFT)calculations and ultraviolet photoelectron spectroscopy(UPS)measurements,it is identified that the highest occupied molecular orbital(HOMO)level for additive modified MAPbI_(3)perovskite could reduce the voltage deficit for hole extraction.Moreover,due to the most favorable charge distribution and significant improvements in charge mobility and defect passivation,the power conversion efficiency(PCE)of 2Cl-MAPbI_(3)PSCs was significantly improved from 19.32%to 21.12%.More importantly,the two-dimensional grazing-incidence wide-angle X-ray scattering(GIWAXS)analysis showed that PbI_(2) defects were effectively suppressed and femtosecond transient absorption(TA)spectroscopy demonstrated that the trap-assisted recombination at grain boundaries was effectively inhibited in the 2Cl-MA-free film.As a result,the thermally stable 2Cl-MA-free PSCs achieved a remarkable PCE of 23.13%with an open-circuit voltage(V_(oc))of 1.164 V and an ultrahigh fill factor(FF)of 85.7%.Our work offers a practical strategy for further commercializing stable and efficient PSCs.
