Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc...Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc-based HTMs in PSCs is still lagging behind their small molecule and polymeric counterparts, largely due to their relatively low hole mobility. Here, we report for the first time the application of a copper naphthalocyanine derivative(namely t Bu-Cu Nc) as a hole-transport material(HTM)in perovskite solar cells(PSCs), and systematically study its optoelectronic and photovoltaic property compared with its Cu Pc analog(t Bu-Cu Pc). Combined experiments disclose that the extension of π-conjugation from Pc to Nc core leads to not only an enhanced hole-carrier mobility associated with a stronger intermolecular interaction, but also an elevated glass transition temperature(T_g) of 252 °C. The resultant PSCs employing t Bu-Cu Nc deliver an excellent power conversion efficiency of 24.03%, which is the record efficiency reported for metal complex-based HTMs in PSCs. More importantly, the encapsulated t Bu-Cu Nc-based devices also show dramatically improved thermal stability than the devices using the well-known SpiroOMe TAD, with a T_(80)lifetime for more than 1,000 h under damp-heat stress. This study unfolds a new avenue for developing efficient and stable HTMs in PSCs.展开更多
Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,spec...Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.展开更多
Conjugated polymers are commonly used as effective hole transport materials(HTMs) for preparation of high-performance perovskite solar cells. However, the hydrophobic nature of these materials renders it difficult to ...Conjugated polymers are commonly used as effective hole transport materials(HTMs) for preparation of high-performance perovskite solar cells. However, the hydrophobic nature of these materials renders it difficult to deposit photovoltaic perovskite layers on top via solution processing. In this article, we report a generic surface modification strategy that enables the deposition of uniform and dense perovskite films on top of non-wetting interfaces. In contrast to the previous proposed chemical modifications which might alter the optoelectronic properties of the interfacial layers, we realized a nondestructive surface modification enabled by introducing a layer of insulating mesoporous aluminum oxide(Al2O3). The surface energies of the typical non-wetting hole-transport layers(PTAA, P3 HT, and Poly-TPD) were significantly reduced by the Al2O3 modification. Benefiting from the intact optoelectronic properties of the HTMs, perovskite solar cells deposited on these interface materials show full open-circuit voltages( V OC) with high fill factors(FF) up to 80%. Our method provides an effective avenue for exploiting the full potential of the existing as well as newly developed non-wetting interface materials for the fabrication of high-performance inverted perovskite solar cells.展开更多
Weak light imaging has drawn more and more attention because of its promising potential for practical applications in security monitoring and space exploration. In this work, all-inorganic Cs2AgBiBr6 double perovskite...Weak light imaging has drawn more and more attention because of its promising potential for practical applications in security monitoring and space exploration. In this work, all-inorganic Cs2AgBiBr6 double perovskite-based self-powered photodetectors containing inorganic copper thiocyanate(CuSCN) as hole-transport layers(HTLs) are successfully fabricated and applied for weak light imaging,which is the first report on the weak light imaging application of all-inorganic lead-free perovskite photodetectors. CuSCN films with favorable optical property and hole extraction capability are prepared via a cost efficient and fast solvent removal method, demonstrating the potential for high-performance perovskite-based devices as transparent components. It is revealed that the band alignment of the device is effectively optimized with the presence of CuSCN HTLs,which can availably transport holes while block electrons at the Cs2AgBiBr6/CuSCN interface, resulting in remarkable improvement of photoresponse performance. The responsivity and detectivity are 0.34 A W^-1 and 1.03×10^13 Jones,respectively. In particular, the light current has a boost of almost 10 times. Furthermore, the photodetectors are integrated into a self-built light detection imaging system utilizing the focused laser scanning imaging mode. With illumination of as low as 5 nW cm^-2(405 nm), the image involving graphics and words with a size of 5 cm×5 cm can still be distinctly recognized. These results suggest the promising potential of all-inorganic perovskite-based devices for weak light detection and imaging applications.展开更多
Solution-processed cadmium-based quantum dots(QDs)light-emitting diodes(QLEDs)have shown promising for high-definition display panels due to their high colour purity and low-cost fabrication,but the toxicity still is ...Solution-processed cadmium-based quantum dots(QDs)light-emitting diodes(QLEDs)have shown promising for high-definition display panels due to their high colour purity and low-cost fabrication,but the toxicity still is a big threat.InP is considered as the most promising cadmium-free material to achieve high performance QLEDs,however,the performance of the InP-based QLEDs is far behind of the cadmium-based counterparts.Here,we report high efficiency InP-based QLEDs with more than 20%of external quantum efficiency(EQE)by suppressing hole injection loss.This suppression is achieved by doping a strong Lewis acid into a Lewis base poly(bis(4-phenyl)(2,4,6-trimethylphenyl)amine)to form a Lewis acid-base adduct hole-transport layer(HTL),which improves the hole mobility of the HTL,reduces the hole transfer barrier between HTL and QDs layer to increase hole transport capability.This eventually leads to a more balanced carrier-injection through accelerating hole-injection to match well with the rate of electron-injection,thus suppressing the hole injection loss in the QLED.The InP-based QLED shows EQE of 20.4%,current efficiency of 25.3 cd·A^(−1),turn-on voltage of 2.0 V,luminance of 24,000 cd·m^(−2).This strategy would be a constructive approach to reduce hole loss for p-n junction optoelectronics.展开更多
NiO_(x)-based inverted perovskite solar cells(PSCs)havepresented great potential toward low-cost,highly efficient and stablenext-generation photovoltaics.However,the presence of energy-levelmismatch and contact-interf...NiO_(x)-based inverted perovskite solar cells(PSCs)havepresented great potential toward low-cost,highly efficient and stablenext-generation photovoltaics.However,the presence of energy-levelmismatch and contact-interface defects between hole-selective contacts(HSCs)and perovskite-active layer(PAL)still limits device efficiencyimprovement.Here,we report a graded configuration based on bothinterface-cascaded structures and p-type molecule-doped compositeswith two-/three-dimensional formamidinium-based triple-halideperovskites.We find that the interface defects-induced non-radiativerecombination presented at HSCs/PAL interfaces is remarkably suppressedbecause of efficient hole extraction and transport.Moreover,astrong chemical interaction,halogen bonding and coordination bondingare found in the molecule-doped perovskite composites,whichsignificantly suppress the formation of halide vacancy and parasitic metallic lead.As a result,NiO_(x)-based inverted PSCs present a power-conversion-efficiency over 23%with a high fill factor of 0.84 and open-circuit voltage of 1.162 V,which are comparable to the best reported around 1.56-electron volt bandgap perovskites.Furthermore,devices with encapsulation present high operational stability over 1,200 h during T_(90) lifetime measurement(the time as a function of PCE decreases to 90%of its initial value)under 1-sun illumination in ambient-air conditions.展开更多
Four bipolar triphenylamine(TPA) charge transport materials were constructed by introducing imidazole and trifluoroacetyl groups into the TPA units, and characterized by the nuclear magnetic resonance spectrum(NMR) an...Four bipolar triphenylamine(TPA) charge transport materials were constructed by introducing imidazole and trifluoroacetyl groups into the TPA units, and characterized by the nuclear magnetic resonance spectrum(NMR) and mass spectrometry(MS). Among them, 4-(2-(1,3-trifluoroacetyl)imidazole)-phenyl-4,4?-di(4-methoxyphenyl)amine(2 Me OTPA-IOS, 1) was determined by X-ray single-crystal diffraction. The compound crystallizes in monoclinic system, space group P21/c with a = 24.338(5), b = 9.565(2), c = 11.456(2) ?, β = 99.427(3)°, Mr = 565.47, V = 2631.0(8) ?3,Z = 4,Dc = 1.428 g/cm3, μ = 0.125 mm–1, F(000) = 1160, the final R = 0.0559 and wR = 0.1265 for 5150 observed reflections with I > 2σ(I). The optimized configurations of the target compounds were obtained by quantum chemical calculation, and the bipolarity of transportable holes and electrons was predicted by the frontier molecular orbital(HOMO and LUMO), which was further confirmed by the time of flight(TOF) method. In addition, the introduction of the terminal flexible chain enhances the solubility, thermal stability(DSC and TGA) and film-forming property of all compounds, and the frontier orbital energy of the solid film of the compounds was also tested(UV-vis and PYS). Thus, these compounds have the bipolarity of transportable holes and electrons and show good solubility and thermal stability.展开更多
Novel donor-acceptor-donor structured small molecular hole transporting materials are developed through a facile route by crosslinking dithienopyrrolobenzothiadiazole and phenothiazine or triarylamine-based donor unit...Novel donor-acceptor-donor structured small molecular hole transporting materials are developed through a facile route by crosslinking dithienopyrrolobenzothiadiazole and phenothiazine or triarylamine-based donor units. The strong push/pull electron capability of dithienopyrrolobenzothiadiazole/ phenothiazine and large π-conjugated dithienopyrrolobenzothiadiazole facilitate hole mobility and high conductivity. The devices using the dithienopyrrolobenzothiadiazole/phenothiazine-based hole trans-porting material achieved a power conversion efficiency of 14.2% under 1 sun illumination and improved stability under 20% relative humidity at room temperature without encapsulation. The present finding highlights the potential of dithienopyrrolobenzothiadiazole-based donor-acceptor-donor small molecular hole transporting materials for perovskite solar cells.展开更多
b Département de Physique, Ecole Polythechnique Fédérale de Lausanne, EPFL, Lausanne, Switzerland c Department of Chemistry, Tsinghua University, Beijing 100084, China An excellent hole-transpor...b Département de Physique, Ecole Polythechnique Fédérale de Lausanne, EPFL, Lausanne, Switzerland c Department of Chemistry, Tsinghua University, Beijing 100084, China An excellent hole-transport material, 1,3-diphenyl-5-(9-phenanthryl)-2-pyrazoline (DPPhP) for OLEDs was studied. This compound not only offers high glass transition temperature (T g=96 ℃), good film forming ability, and high HOMO energy level, but also displays excellent hole-transport property. The electroluminescent device with a simple structure of ITO/DPPhP (60 nm)/AlQ (60 nm)/LiF (0.8 nm)/Al shows an external quantum efficiency as high as 1.6%.展开更多
Organolead halide perovskite solar ceils have achieved a certified power- conversion efficiency （PCE） of 22.1% and are thus among the most promising candidates for next-generation photovoltaic devices. To date, most...Organolead halide perovskite solar ceils have achieved a certified power- conversion efficiency （PCE） of 22.1% and are thus among the most promising candidates for next-generation photovoltaic devices. To date, most high-efficiency perovskite solar cells have employed arylamine-based hole-transport materials （HTMs）, which are expensive and have a low mobility. The complicated doping procedures and the potentially stability-adverse dopants used in these HTMs are among the major bottlenecks for the commercialization of perovskite solar cells （PSCs）. Herein, we present a polythiophene-based copolymer （PDVT-10） with a hole mobility up to 8.2 cm2-V-l.s-1 and a highest occupied molecular orbital level of -5.28 eV as a hole-transport layer （HTL） for a PSC. A device based on this new HTM exhibited a high PCE of 13.4% under 100 mW-cm-2 illumination, which is one of the highest PCEs reported for the dopant-free polymer-based HTLs. Moreover, PDVT-10 exhibited good solution processability, decent air stability, and thermal stability, making it a promising candidate as an HTM for PSCs.展开更多
To realize the commercialization of perovskite solar cells(PSCs), it is required to overcome the remaining challenges in device enlargement and operational stability. Here, we report an all-in-one strategy by integrat...To realize the commercialization of perovskite solar cells(PSCs), it is required to overcome the remaining challenges in device enlargement and operational stability. Here, we report an all-in-one strategy by integrating the oxidation of hole-transport material(HTM) with the formation of the passivation layer, which simultaneously solved the stability issues caused by HTM oxidation and realized the uniform defects in passivation over a large area. The resulting devices achieved a certified PCE of23.12% on average with an aperture area of 1.04 cm^(2) and are reproducible with high operational stability because of the exclusion of air exposure, hygroscopic Li-TFSI, and the lithium-based wastes, maintaining ca. 90% of their initial PCEs after operation at the maximum power point under continuous 1 sun illumination for 1,600 h. Our strategy simplifies the fabrication process of PSCs, which is compatible with commercial-scale methods, offering facile access to efficient and stable large-area PSCs.展开更多
High-performance,cost-effective hole-transport materials(HTMs)are greatly desired for the commercialization of perovskite solar cells(PVSCs).Herein,two new HTMs,TPA-FO and TPA-PDO,are devised and synthesized,which hav...High-performance,cost-effective hole-transport materials(HTMs)are greatly desired for the commercialization of perovskite solar cells(PVSCs).Herein,two new HTMs,TPA-FO and TPA-PDO,are devised and synthesized,which have a donor-acceptor-donor(D-A-D)type molecule design featuring carbonyl group-functionalized arenes as the acceptor(A)units.The carbonyl group at the central core of HTMs can not only tune frontier molecular orbital(FMO)energy levels and surface wettability,but also can enable efficient surface passivation effects,resulting in reduced recombination loss.When employed as HTMs in inverted PVSCs without using dopant,TPA-FO with one carbonyl group yields a high power conversion efficiency(PCE)of 20.24%,which is among the highest values reported in the inverted PVSCs with dopant-free HTMs.More importantly,the facile one-step synthetic process enables a low cost of 30 USD g^(-1) for TPA-FO,much cheaper than the most studied HTMs used for high-efficiency dopant-free PVSCs.These results demonstrate the potential of D-A-D type molecules with carbonyl group-functionalized arene core in developing the low-cost dopant-free HTMs toward highly efficient PVSCs.展开更多
A new crosslinked polymer,called P65,with appropriate photo-electrochemical,opto-electronic,and thermal properties,has been designed and synthesized as an efficient,dopant-free,hole-transport material(HTM)for n-i-p ty...A new crosslinked polymer,called P65,with appropriate photo-electrochemical,opto-electronic,and thermal properties,has been designed and synthesized as an efficient,dopant-free,hole-transport material(HTM)for n-i-p type planar perovskite solar cells(PSCs).P65 is obtained from a low-cost and easily synthesized spiro[fluorene-9,90-xanthene]-30,60-diol(SFX-OH)-based monomer X65 through a freeradical polymerization reaction.The combination of a three-dimensional(3 D)SFX core unit,holetransport methoxydiphenylamine group,and crosslinked polyvinyl network provides P65 with good solubility and excellent film-forming properties.By employing P65 as a dopant-free hole-transport layer in conventional n-i-p type PSCs,a power conversion efficiency(PCE)of up to 17.7%is achieved.To the best of our knowledge,this is the first time a 3 D,crosslinked,polymeric dopant-free HTM has been reported for use in conventional n-i-p type PSCs.This study provides a new strategy for the future development of a 3 D crosslinked polymeric dopant-free HTM with a simple synthetic route and low-cost for commercial,large-scale applications in future PSCs.展开更多
A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the sy...A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the synthetic steps of BTPA-7 are greatly reduced from 6 to 3 and the synthetic cost of BTPA-7 is nearly a half that of spiro-OMeTAD.Moreover,BTPA-7 exhibits a relatively lower conductivity but higher hole mobility and higher glass transition temperature(Tg)than spiro-OMeTAD.Compared with the photovolatic performance for spiro-OMeTAD,FA0.85MA0.15PbI3 and MAPbI3 PSC devices based on BTPA-7 exhibit slightly lower PCEs with the values of 17.58%(18.88%for spiro-OMeTAD)and 11.90%(13.25%for spiro-OMeTAD),respectively.Nevertheless,a dramatically higher JSC of PSC based on BTPA-7is achieved,which arises from the higher hole mobility of BTPA-7.In addition,the relatively hydrophobic character of BTPA-7 eventually enhances the PSC device stability.Lower cost,higher hole mobility,higher Tg,satisfactory photovoltaic performance,and superior device stability of BTPA-7 can be utilized as a substitute for spiro-OMeTAD in PSCs.展开更多
基金supported by the National Natural Science Foundation of China (52161145408, 21975038, 22088102)the National Key R&D Program of China (2022YFA0911904)+2 种基金the Fundamental Research Funds for the Central Universities (DUT23LAB611)the Central Guidance for Local Scientific and Technological Development Funds in Liaoning Province (2023JH6/100500006)the Research and Innovation Team Project of Dalian University of Technology(DUT2022TB10)。
文摘Metal phthalocyanines(MPcs) have gained considerable research attention as hole-transport materials(HTMs) in perovskite solar cells(PSCs) because of their superb stability. However, the photovoltaic performance of MPc-based HTMs in PSCs is still lagging behind their small molecule and polymeric counterparts, largely due to their relatively low hole mobility. Here, we report for the first time the application of a copper naphthalocyanine derivative(namely t Bu-Cu Nc) as a hole-transport material(HTM)in perovskite solar cells(PSCs), and systematically study its optoelectronic and photovoltaic property compared with its Cu Pc analog(t Bu-Cu Pc). Combined experiments disclose that the extension of π-conjugation from Pc to Nc core leads to not only an enhanced hole-carrier mobility associated with a stronger intermolecular interaction, but also an elevated glass transition temperature(T_g) of 252 °C. The resultant PSCs employing t Bu-Cu Nc deliver an excellent power conversion efficiency of 24.03%, which is the record efficiency reported for metal complex-based HTMs in PSCs. More importantly, the encapsulated t Bu-Cu Nc-based devices also show dramatically improved thermal stability than the devices using the well-known SpiroOMe TAD, with a T_(80)lifetime for more than 1,000 h under damp-heat stress. This study unfolds a new avenue for developing efficient and stable HTMs in PSCs.
基金This study was supported by the National Nat-ural Science Foundation of China(No.22379105)the Natural Sci-ence Foundation of Shanxi Province(Nos.20210302123110 and 202303021211059)the Open Fund Project of Ningxia Sinostar Display Material Co.,Ltd.
文摘Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.
基金supported by the National Natural Science Foundation of China (Grant no. 61705090)
文摘Conjugated polymers are commonly used as effective hole transport materials(HTMs) for preparation of high-performance perovskite solar cells. However, the hydrophobic nature of these materials renders it difficult to deposit photovoltaic perovskite layers on top via solution processing. In this article, we report a generic surface modification strategy that enables the deposition of uniform and dense perovskite films on top of non-wetting interfaces. In contrast to the previous proposed chemical modifications which might alter the optoelectronic properties of the interfacial layers, we realized a nondestructive surface modification enabled by introducing a layer of insulating mesoporous aluminum oxide(Al2O3). The surface energies of the typical non-wetting hole-transport layers(PTAA, P3 HT, and Poly-TPD) were significantly reduced by the Al2O3 modification. Benefiting from the intact optoelectronic properties of the HTMs, perovskite solar cells deposited on these interface materials show full open-circuit voltages( V OC) with high fill factors(FF) up to 80%. Our method provides an effective avenue for exploiting the full potential of the existing as well as newly developed non-wetting interface materials for the fabrication of high-performance inverted perovskite solar cells.
基金supported by the National Natural Science Foundation of China (51772135)the Ministry of Education of China (6141A02022516)+4 种基金the Fundamental Research Funds for the Central Universities (11619103)China Postdoctoral Science Foundation (2019M663376)Guangdong Province Higher Vocational Colleges & Schools Pearl River Scholar Funded Scheme (2017)the Natural Science Foundation of Guangdong Province, China (2017A020215135 and 2018A030310659)the Science and Technology Program of Guangzhou, China (201804010432)。
文摘Weak light imaging has drawn more and more attention because of its promising potential for practical applications in security monitoring and space exploration. In this work, all-inorganic Cs2AgBiBr6 double perovskite-based self-powered photodetectors containing inorganic copper thiocyanate(CuSCN) as hole-transport layers(HTLs) are successfully fabricated and applied for weak light imaging,which is the first report on the weak light imaging application of all-inorganic lead-free perovskite photodetectors. CuSCN films with favorable optical property and hole extraction capability are prepared via a cost efficient and fast solvent removal method, demonstrating the potential for high-performance perovskite-based devices as transparent components. It is revealed that the band alignment of the device is effectively optimized with the presence of CuSCN HTLs,which can availably transport holes while block electrons at the Cs2AgBiBr6/CuSCN interface, resulting in remarkable improvement of photoresponse performance. The responsivity and detectivity are 0.34 A W^-1 and 1.03×10^13 Jones,respectively. In particular, the light current has a boost of almost 10 times. Furthermore, the photodetectors are integrated into a self-built light detection imaging system utilizing the focused laser scanning imaging mode. With illumination of as low as 5 nW cm^-2(405 nm), the image involving graphics and words with a size of 5 cm×5 cm can still be distinctly recognized. These results suggest the promising potential of all-inorganic perovskite-based devices for weak light detection and imaging applications.
基金the Beijing Municipal Natural Science Foundation(No.2222061)the National Natural Science Foundation of China(Nos.51961135107 and 51774034)the National Key Research and Development Program of China(No.2017YFE0119700).
文摘Solution-processed cadmium-based quantum dots(QDs)light-emitting diodes(QLEDs)have shown promising for high-definition display panels due to their high colour purity and low-cost fabrication,but the toxicity still is a big threat.InP is considered as the most promising cadmium-free material to achieve high performance QLEDs,however,the performance of the InP-based QLEDs is far behind of the cadmium-based counterparts.Here,we report high efficiency InP-based QLEDs with more than 20%of external quantum efficiency(EQE)by suppressing hole injection loss.This suppression is achieved by doping a strong Lewis acid into a Lewis base poly(bis(4-phenyl)(2,4,6-trimethylphenyl)amine)to form a Lewis acid-base adduct hole-transport layer(HTL),which improves the hole mobility of the HTL,reduces the hole transfer barrier between HTL and QDs layer to increase hole transport capability.This eventually leads to a more balanced carrier-injection through accelerating hole-injection to match well with the rate of electron-injection,thus suppressing the hole injection loss in the QLED.The InP-based QLED shows EQE of 20.4%,current efficiency of 25.3 cd·A^(−1),turn-on voltage of 2.0 V,luminance of 24,000 cd·m^(−2).This strategy would be a constructive approach to reduce hole loss for p-n junction optoelectronics.
基金supported by National Natural Science Foundation of China (62204099)Guangdong Basic and Applied Basic Research Foundation (2020A1515110462)+1 种基金Fundamental Research Funds for the Central Universities (21620347)the Special Funds for College Students’ Innovative Entrepreneurial Training Plan Program
文摘NiO_(x)-based inverted perovskite solar cells(PSCs)havepresented great potential toward low-cost,highly efficient and stablenext-generation photovoltaics.However,the presence of energy-levelmismatch and contact-interface defects between hole-selective contacts(HSCs)and perovskite-active layer(PAL)still limits device efficiencyimprovement.Here,we report a graded configuration based on bothinterface-cascaded structures and p-type molecule-doped compositeswith two-/three-dimensional formamidinium-based triple-halideperovskites.We find that the interface defects-induced non-radiativerecombination presented at HSCs/PAL interfaces is remarkably suppressedbecause of efficient hole extraction and transport.Moreover,astrong chemical interaction,halogen bonding and coordination bondingare found in the molecule-doped perovskite composites,whichsignificantly suppress the formation of halide vacancy and parasitic metallic lead.As a result,NiO_(x)-based inverted PSCs present a power-conversion-efficiency over 23%with a high fill factor of 0.84 and open-circuit voltage of 1.162 V,which are comparable to the best reported around 1.56-electron volt bandgap perovskites.Furthermore,devices with encapsulation present high operational stability over 1,200 h during T_(90) lifetime measurement(the time as a function of PCE decreases to 90%of its initial value)under 1-sun illumination in ambient-air conditions.
基金This project was supported by the Scientific Research Development Program of Shandong Provincial High School(J18KA082)the Under-graduate Training Program for Innovation and Entrepreneurship of Shandong Provincial High School(201710446042,2018A043)the Experimental Technology Research Program of Qufu Normal University(SJ201709)
文摘Four bipolar triphenylamine(TPA) charge transport materials were constructed by introducing imidazole and trifluoroacetyl groups into the TPA units, and characterized by the nuclear magnetic resonance spectrum(NMR) and mass spectrometry(MS). Among them, 4-(2-(1,3-trifluoroacetyl)imidazole)-phenyl-4,4?-di(4-methoxyphenyl)amine(2 Me OTPA-IOS, 1) was determined by X-ray single-crystal diffraction. The compound crystallizes in monoclinic system, space group P21/c with a = 24.338(5), b = 9.565(2), c = 11.456(2) ?, β = 99.427(3)°, Mr = 565.47, V = 2631.0(8) ?3,Z = 4,Dc = 1.428 g/cm3, μ = 0.125 mm–1, F(000) = 1160, the final R = 0.0559 and wR = 0.1265 for 5150 observed reflections with I > 2σ(I). The optimized configurations of the target compounds were obtained by quantum chemical calculation, and the bipolarity of transportable holes and electrons was predicted by the frontier molecular orbital(HOMO and LUMO), which was further confirmed by the time of flight(TOF) method. In addition, the introduction of the terminal flexible chain enhances the solubility, thermal stability(DSC and TGA) and film-forming property of all compounds, and the frontier orbital energy of the solid film of the compounds was also tested(UV-vis and PYS). Thus, these compounds have the bipolarity of transportable holes and electrons and show good solubility and thermal stability.
基金Financial support from the 973 Program of China(No.2014CB643506)the NSFC Major International(Regional)Joint Research Project NSFC-SNSF(51661135023)+2 种基金NSFC(21673091,21702147)the Fundamental Research Funds For the Central Universities HUST(2018KFYXKJC034)the Opening Project of Zhejiang Provincial Top Key Discipline of Pharmaceutical Sciences
文摘Novel donor-acceptor-donor structured small molecular hole transporting materials are developed through a facile route by crosslinking dithienopyrrolobenzothiadiazole and phenothiazine or triarylamine-based donor units. The strong push/pull electron capability of dithienopyrrolobenzothiadiazole/ phenothiazine and large π-conjugated dithienopyrrolobenzothiadiazole facilitate hole mobility and high conductivity. The devices using the dithienopyrrolobenzothiadiazole/phenothiazine-based hole trans-porting material achieved a power conversion efficiency of 14.2% under 1 sun illumination and improved stability under 20% relative humidity at room temperature without encapsulation. The present finding highlights the potential of dithienopyrrolobenzothiadiazole-based donor-acceptor-donor small molecular hole transporting materials for perovskite solar cells.
文摘b Département de Physique, Ecole Polythechnique Fédérale de Lausanne, EPFL, Lausanne, Switzerland c Department of Chemistry, Tsinghua University, Beijing 100084, China An excellent hole-transport material, 1,3-diphenyl-5-(9-phenanthryl)-2-pyrazoline (DPPhP) for OLEDs was studied. This compound not only offers high glass transition temperature (T g=96 ℃), good film forming ability, and high HOMO energy level, but also displays excellent hole-transport property. The electroluminescent device with a simple structure of ITO/DPPhP (60 nm)/AlQ (60 nm)/LiF (0.8 nm)/Al shows an external quantum efficiency as high as 1.6%.
文摘Organolead halide perovskite solar ceils have achieved a certified power- conversion efficiency （PCE） of 22.1% and are thus among the most promising candidates for next-generation photovoltaic devices. To date, most high-efficiency perovskite solar cells have employed arylamine-based hole-transport materials （HTMs）, which are expensive and have a low mobility. The complicated doping procedures and the potentially stability-adverse dopants used in these HTMs are among the major bottlenecks for the commercialization of perovskite solar cells （PSCs）. Herein, we present a polythiophene-based copolymer （PDVT-10） with a hole mobility up to 8.2 cm2-V-l.s-1 and a highest occupied molecular orbital level of -5.28 eV as a hole-transport layer （HTL） for a PSC. A device based on this new HTM exhibited a high PCE of 13.4% under 100 mW-cm-2 illumination, which is one of the highest PCEs reported for the dopant-free polymer-based HTLs. Moreover, PDVT-10 exhibited good solution processability, decent air stability, and thermal stability, making it a promising candidate as an HTM for PSCs.
基金supported by the National Natural Science Foundation of China (11834011, 12074245, 52102281, 51901132)the Young Elite Scientists Sponsorship Program by China Association for Science and Technology (2021QNRC001)+1 种基金Shanghai Sailing Program (21YF1421600)the University of Tokyo was supported by JSPS KAKENHI (JP21H02040)。
文摘To realize the commercialization of perovskite solar cells(PSCs), it is required to overcome the remaining challenges in device enlargement and operational stability. Here, we report an all-in-one strategy by integrating the oxidation of hole-transport material(HTM) with the formation of the passivation layer, which simultaneously solved the stability issues caused by HTM oxidation and realized the uniform defects in passivation over a large area. The resulting devices achieved a certified PCE of23.12% on average with an aperture area of 1.04 cm^(2) and are reproducible with high operational stability because of the exclusion of air exposure, hygroscopic Li-TFSI, and the lithium-based wastes, maintaining ca. 90% of their initial PCEs after operation at the maximum power point under continuous 1 sun illumination for 1,600 h. Our strategy simplifies the fabrication process of PSCs, which is compatible with commercial-scale methods, offering facile access to efficient and stable large-area PSCs.
基金the National Natural Science Foundation of China(NSFC,No.21801124)X.G.is grateful to the Shenzhen Science and Technology Innovation Commission(No.JCYJ20180504165709042)We are grateful for the assistance of SUSTech Core Research Facilities.PL and TRPL characterizations were supported by Shenzhen Key Laboratory of Full Spectral Solar Electricity Generation(FSSEG)from the Shenzhen Key Laboratory Project(No.ZDSYS201602261933302).
文摘High-performance,cost-effective hole-transport materials(HTMs)are greatly desired for the commercialization of perovskite solar cells(PVSCs).Herein,two new HTMs,TPA-FO and TPA-PDO,are devised and synthesized,which have a donor-acceptor-donor(D-A-D)type molecule design featuring carbonyl group-functionalized arenes as the acceptor(A)units.The carbonyl group at the central core of HTMs can not only tune frontier molecular orbital(FMO)energy levels and surface wettability,but also can enable efficient surface passivation effects,resulting in reduced recombination loss.When employed as HTMs in inverted PVSCs without using dopant,TPA-FO with one carbonyl group yields a high power conversion efficiency(PCE)of 20.24%,which is among the highest values reported in the inverted PVSCs with dopant-free HTMs.More importantly,the facile one-step synthetic process enables a low cost of 30 USD g^(-1) for TPA-FO,much cheaper than the most studied HTMs used for high-efficiency dopant-free PVSCs.These results demonstrate the potential of D-A-D type molecules with carbonyl group-functionalized arene core in developing the low-cost dopant-free HTMs toward highly efficient PVSCs.
基金the support of the Swedish Energy Agency and Swedish Foundation for Strategic Research(SSF)for their financial supportthe China Scholarship Council(CSC)for its financial support。
文摘A new crosslinked polymer,called P65,with appropriate photo-electrochemical,opto-electronic,and thermal properties,has been designed and synthesized as an efficient,dopant-free,hole-transport material(HTM)for n-i-p type planar perovskite solar cells(PSCs).P65 is obtained from a low-cost and easily synthesized spiro[fluorene-9,90-xanthene]-30,60-diol(SFX-OH)-based monomer X65 through a freeradical polymerization reaction.The combination of a three-dimensional(3 D)SFX core unit,holetransport methoxydiphenylamine group,and crosslinked polyvinyl network provides P65 with good solubility and excellent film-forming properties.By employing P65 as a dopant-free hole-transport layer in conventional n-i-p type PSCs,a power conversion efficiency(PCE)of up to 17.7%is achieved.To the best of our knowledge,this is the first time a 3 D,crosslinked,polymeric dopant-free HTM has been reported for use in conventional n-i-p type PSCs.This study provides a new strategy for the future development of a 3 D crosslinked polymeric dopant-free HTM with a simple synthetic route and low-cost for commercial,large-scale applications in future PSCs.
基金financially supported by the National Key Research and Development Program of China(2016YFA0202403)the National University Research Fund(GK261001009)+7 种基金the Changjiang Scholar and Innovative Research Team(IRT_14R33)the Overseas Talent Recruitment Project(B14041)the Chinese National 1000talent plan program(Grant No.111001034)the JSPS Kakenhi grants(No.26288113 and 15K05486)support from the Strategic Research Foundation at Private Universities(Nihon University and the MEXT,Japan)the Natural Science Foundation of Shaanxi Province(2019JQ-423)the Fundamental Research Funds for the Central Universities(GK201903053)Key Lab of photovoltaic and Energy Conservation Materials,Chinese Academy of Sciences(No.PECL2019KF019)。
文摘A novel hole-transport material(HTM)based on an anthradithiophene central bridge named BTPA-7 is developed.In comparison to spiro-OMeTAD(2,2’,7,7’-tetrakis-(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluorene),the synthetic steps of BTPA-7 are greatly reduced from 6 to 3 and the synthetic cost of BTPA-7 is nearly a half that of spiro-OMeTAD.Moreover,BTPA-7 exhibits a relatively lower conductivity but higher hole mobility and higher glass transition temperature(Tg)than spiro-OMeTAD.Compared with the photovolatic performance for spiro-OMeTAD,FA0.85MA0.15PbI3 and MAPbI3 PSC devices based on BTPA-7 exhibit slightly lower PCEs with the values of 17.58%(18.88%for spiro-OMeTAD)and 11.90%(13.25%for spiro-OMeTAD),respectively.Nevertheless,a dramatically higher JSC of PSC based on BTPA-7is achieved,which arises from the higher hole mobility of BTPA-7.In addition,the relatively hydrophobic character of BTPA-7 eventually enhances the PSC device stability.Lower cost,higher hole mobility,higher Tg,satisfactory photovoltaic performance,and superior device stability of BTPA-7 can be utilized as a substitute for spiro-OMeTAD in PSCs.
