Lewis-base polymers have been widely utilized as additives to act as a template for the perovskite nucleation/crystal growth and passivate the under-coordinated Pb2+ sites.However,it is uncovered in this work that the...Lewis-base polymers have been widely utilized as additives to act as a template for the perovskite nucleation/crystal growth and passivate the under-coordinated Pb2+ sites.However,it is uncovered in this work that the polymer on the perovskite grain boundaries would significantly hinder the charge transport due to its low conductivity,which brings about free carrier recombination and photocurrent losses.To circumvent this issue while fully exploiting the benefits of polymers in passivating the trap states in perovskite,we incorporate highly conductive multiwall carbon nanotubes(CNTs) with Lewis-base polymers as coadditives in the perovskite film.Functionalizing the CNTs with-COOH group enables a selective hole-extraction and charge transport from perovskite to the hole transporting materials(HTM).By studying the charge transporting and recombination dynamics,we revealed the individual role of the polymer and CNTs in passivating the trap states and facilitating the charge transport,respectively.As a result,the perovskite solar cells(PSCs) with polymer-CNTs composites exhibit an impressive PCE of 21.7% for a small-area device(0.16 cm2) and 20.7% for a large-area device(1.0 cm2).Moreover,due to the superior mechanical flexibility of both polymer and CNTs,the polymer-CNTs composites incorporation in the perovskite film encourages the fabrication of flexible PSCs(f-PSCs) with an impressive PCE of 18.3%,and a strong mechanical durability by retaining 80%of the initial PCE after 1,000 times bending.In addition,we proved that the selection criteria of the polymers can be extended to other long-chain Lewis-base polymers,which opens new possibilities in design and synthesis of inexpensive material for this tactic towards the fabrication of high performance large-area PSCs and f-PSCs.展开更多
All-inorganic perovskite solar cells(PSCs)have developed rapidly in the field of photovoltaics due to their excellent thermal and light stability.However,compared with organic–inorganic hybrid perovskites,the phase i...All-inorganic perovskite solar cells(PSCs)have developed rapidly in the field of photovoltaics due to their excellent thermal and light stability.However,compared with organic–inorganic hybrid perovskites,the phase instability of inorganic perovskite under humidity still remains as a critical issue that ham-pers the commercialization of inorganic PSCs.We originally propose in this work that microstrains between the perovskite lattices/grains play a key role in affecting the phase stability of inorganic perovskite.To this end,we inno-vatively design theπ-conjugated p-type molecule bis(2-ethylhexyl)3,30((4,8-bis(5-(2-ethylhexyl)-3,4-difluorothiophen-2-yl)benzo[1,2-b:4,5-b0]dithiophene-2,6-di yl)bis(3,300-dioctyl[2,20:50,200-terthiophene]-500,5-diyl))(2E,20 E)-bis(2-cyanoacrylate)(BTEC-2F)to covalent with the Pb dangling bonds in CsPbI2Br perovskite film,which significantly suppress the trap states and release the defect-induced local stress between perovskite grains.The interplay between the microstrains and phase stability of the inorganic perovskite are scrutinized by a series of charac-terizations including x-ray photoelectron spectroscopy,photoluminescence,x-ray diffraction,scanning electron microscopy,and so forth,based on which,we conclude that weaker local stresses in the perovskite film engender superior phase stability by preventing the perovskite lattice distortion under humidity.By this rational design,PSCs based on CsPbI2Br perovskite system deliver an outstanding power conversion efficiency(PCE)up to 16.25%.The unencapsulated device also exhibits an exceptional moisture stability by retaining over 80%of the initial PCE after 500 h aging in ambient with relative humidity of(RH)25%.展开更多
基金the National Science Fund for Distinguished Young Scholars(21925506)the National Key R&D Program of China(2017YFE0106000)+3 种基金the National Natural Science Foundation of China(51773212)Ningbo S&T Innovation 2025 Major Special Programme(2018B10055)Ningbo Municipal Science and Technology Innovative Research Team(2015B11002,2016B10005)CAS Key Project of Frontier Science Research(QYZDB-SSW-SYS030)。
文摘Lewis-base polymers have been widely utilized as additives to act as a template for the perovskite nucleation/crystal growth and passivate the under-coordinated Pb2+ sites.However,it is uncovered in this work that the polymer on the perovskite grain boundaries would significantly hinder the charge transport due to its low conductivity,which brings about free carrier recombination and photocurrent losses.To circumvent this issue while fully exploiting the benefits of polymers in passivating the trap states in perovskite,we incorporate highly conductive multiwall carbon nanotubes(CNTs) with Lewis-base polymers as coadditives in the perovskite film.Functionalizing the CNTs with-COOH group enables a selective hole-extraction and charge transport from perovskite to the hole transporting materials(HTM).By studying the charge transporting and recombination dynamics,we revealed the individual role of the polymer and CNTs in passivating the trap states and facilitating the charge transport,respectively.As a result,the perovskite solar cells(PSCs) with polymer-CNTs composites exhibit an impressive PCE of 21.7% for a small-area device(0.16 cm2) and 20.7% for a large-area device(1.0 cm2).Moreover,due to the superior mechanical flexibility of both polymer and CNTs,the polymer-CNTs composites incorporation in the perovskite film encourages the fabrication of flexible PSCs(f-PSCs) with an impressive PCE of 18.3%,and a strong mechanical durability by retaining 80%of the initial PCE after 1,000 times bending.In addition,we proved that the selection criteria of the polymers can be extended to other long-chain Lewis-base polymers,which opens new possibilities in design and synthesis of inexpensive material for this tactic towards the fabrication of high performance large-area PSCs and f-PSCs.
基金CAS Key Project of Frontier Science Research,Grant/Award Number:QYZDBSSW-SYS030National Natural Science Foundation of China,Grant/Award Numbers:22005322,51773212,81903743+2 种基金National Science Fund for Distinguished Young Scholars,Grant/Award Number:21925506Ningbo S&T Innovation 2025 Major Special Programme,Grant/Award Number:2018B10055National Key R&D Program of China,Grant/Award Number:2017YFE0106000。
文摘All-inorganic perovskite solar cells(PSCs)have developed rapidly in the field of photovoltaics due to their excellent thermal and light stability.However,compared with organic–inorganic hybrid perovskites,the phase instability of inorganic perovskite under humidity still remains as a critical issue that ham-pers the commercialization of inorganic PSCs.We originally propose in this work that microstrains between the perovskite lattices/grains play a key role in affecting the phase stability of inorganic perovskite.To this end,we inno-vatively design theπ-conjugated p-type molecule bis(2-ethylhexyl)3,30((4,8-bis(5-(2-ethylhexyl)-3,4-difluorothiophen-2-yl)benzo[1,2-b:4,5-b0]dithiophene-2,6-di yl)bis(3,300-dioctyl[2,20:50,200-terthiophene]-500,5-diyl))(2E,20 E)-bis(2-cyanoacrylate)(BTEC-2F)to covalent with the Pb dangling bonds in CsPbI2Br perovskite film,which significantly suppress the trap states and release the defect-induced local stress between perovskite grains.The interplay between the microstrains and phase stability of the inorganic perovskite are scrutinized by a series of charac-terizations including x-ray photoelectron spectroscopy,photoluminescence,x-ray diffraction,scanning electron microscopy,and so forth,based on which,we conclude that weaker local stresses in the perovskite film engender superior phase stability by preventing the perovskite lattice distortion under humidity.By this rational design,PSCs based on CsPbI2Br perovskite system deliver an outstanding power conversion efficiency(PCE)up to 16.25%.The unencapsulated device also exhibits an exceptional moisture stability by retaining over 80%of the initial PCE after 500 h aging in ambient with relative humidity of(RH)25%.