As one photovoltaic supernova,perovskite solar cells(PSCs)have exhibited certified power conversion efficiencies exceeding 27%.Yet,the presence of enormous defects,mainly for the dominant iodine vacancy(VI),always ind...As one photovoltaic supernova,perovskite solar cells(PSCs)have exhibited certified power conversion efficiencies exceeding 27%.Yet,the presence of enormous defects,mainly for the dominant iodine vacancy(VI),always induces nonradiative recombination,ion migration,and triggers autocatalytic iodine oxidation into volatile I_(2) and charge-localization-mediated metallic Pb0clusters,which accelerate device failure and therefore hamper commercialization.However,popularly reported strategies that simultaneously enable vacancy passivation and iodine scavenging remain insufficient,highlighting the need for new additives.Herein,we employ 4-cyanophenylhydrazine hydrochloride(CPHCl)as an iodine-related synergistic redox-coordination stabilizer to address intrinsic instability and interface chemistry issues.After systematically characterizations,we demonstrate that CPHCl not only specifically eliminates I_(2) intermediates by leveraging the redox-active hydrazine group(NH–NH_(2))(I_(2)+NH–NH_(2)→2HI+N=NH),but also passivates Pb^(2+)/FA^(+) related defects viaπ-backdonation and hydrogen bonding by the electron-donating cyano(C≡N)group,synergistically modulating the crystallization kinetics and improving the final quality of the perovskite film.As a result,vacancy-mediated I-ion migration and degradation are significantly relieved,enabling an enhanced efficiency of 25.56%for the p-i-n inverted PSC with exceptional operational stability.This work provides a deep insight into screening perovskite stabilizers for advancing toward commercial longevity.展开更多
基金partly funded by the National Natural Science Foundation of China(62204098,62304124,62374105,22309107)Natural Science Foundation of Shandong Province(ZR2024QE036,ZR2024QB021,ZR2023QB281)+1 种基金Special Fund of Taishan Scholar Program of Shandong Province(tsqnz20221141)Qingdao Natural Science Foundation(24-4-4-zrjj-21-jch,25-1-1-114-zyydjch)。
文摘As one photovoltaic supernova,perovskite solar cells(PSCs)have exhibited certified power conversion efficiencies exceeding 27%.Yet,the presence of enormous defects,mainly for the dominant iodine vacancy(VI),always induces nonradiative recombination,ion migration,and triggers autocatalytic iodine oxidation into volatile I_(2) and charge-localization-mediated metallic Pb0clusters,which accelerate device failure and therefore hamper commercialization.However,popularly reported strategies that simultaneously enable vacancy passivation and iodine scavenging remain insufficient,highlighting the need for new additives.Herein,we employ 4-cyanophenylhydrazine hydrochloride(CPHCl)as an iodine-related synergistic redox-coordination stabilizer to address intrinsic instability and interface chemistry issues.After systematically characterizations,we demonstrate that CPHCl not only specifically eliminates I_(2) intermediates by leveraging the redox-active hydrazine group(NH–NH_(2))(I_(2)+NH–NH_(2)→2HI+N=NH),but also passivates Pb^(2+)/FA^(+) related defects viaπ-backdonation and hydrogen bonding by the electron-donating cyano(C≡N)group,synergistically modulating the crystallization kinetics and improving the final quality of the perovskite film.As a result,vacancy-mediated I-ion migration and degradation are significantly relieved,enabling an enhanced efficiency of 25.56%for the p-i-n inverted PSC with exceptional operational stability.This work provides a deep insight into screening perovskite stabilizers for advancing toward commercial longevity.
