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Engineering of dendritic dopant-free hole transport molecules:enabling ultrahigh fill factor in perovskite solar cells with optimized dendron construction

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Science China Chemistry 2021年第1期64卷 41-51页

作者： Wei Chen Yang Wang Bin Liu Yajun Gao Ziang Wu Yongqiang Shi Yumin Tang Kun Yang Yujie Zhang Weipeng Sun Xiyuan Feng Frédéric Laquai Han Young Woo Aleksandra B.Djurisic Xugang Guo Zhubing He Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China Department of Physics The University of Hong KongPokfulamHong KongChina King Abdullah University of Science and Technology KAUST Solar CenterPhysical Sciences and Engineering DivisionMaterial Science and Engineering ProgramThuwal 23955-6900Kingdom of Saudi Arabia Department of Chemistry Korea UniversitySeoul 02841South Korea

Developing dopant-free hole-transporting materials(HTMs)for high-performance perovskite solar cells(PVSCs)has been a very active research topic in recent years since HTMs play a critical role in optimizing interfacial charge carrier kinetics and in turn determining device ***,a novel dendritic engineering strategy is first utilized to design HTMs with a D-A type molecular framework,and diphenylamine and/or carbazole is selected as the building block for constructing *** HTMs show good thermal stability and excellent film morphology,and the key optoelectronic properties could be fine-tuned by varying the dendron *** them,MPA-Cz-BTI and MCz-Cz-BTI exhibit an improved interfacial contact with the perovskite active layer,and non-radiative recombination loss and charge transport loss can be effectively ***,high power conversion efficiencies(PCEs)of 20.8%and 21.35%are achieved for MPA-Cz-BTI and MCz-Cz-BTI based devices,respectively,accompanied by excellent long-term storage *** encouragingly,ultrahigh fill factors of 85.2%and 83.5%are recorded for both devices,which are among the highest values reported to *** work demonstrates the great potential of dendritic materials as a new type of dopant-free HTMs for high-performance PVSCs with excellent FF.

关键词： dendritic molecules hole-transporting materials dopant-free ultrahigh fill factor perovskite solar cells

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Highly stable perovskite solar cells with a novel Ni-based metal organic complex as dopant-free hole-transporting material

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Journal of Energy Chemistry 2022年第2期31卷 312-318页

作者： Tai Wu Linqin Wang Rongjun Zhao Rongshan Zhuang Kanghong Zhao Gaoyuan Liu Jing Huang Licheng Sun Yong Hua Yunnan Key Laboratory for Micro/Nano Materials&Technology International Joint Research Center for Optoelectronic and Energy MaterialsSchool of Materials and EnergyYunnan UniversityKunming 650091YunnanChina Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024ZhejiangChina Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024ZhejiangChina Department of Applied Physics KTH-Royal Institute of Technology16440 StockholmSweden

Hole-transporting material(HTM)plays a paramount role in enhancing the photovltaic performance of perovskite solar cells(PSCs).Currently,the vast majority of these HTMs employed in PSCs are organic small molecules and polymers,yet the use of organic metal complexes in PSCs applications remains less *** date,most of reported HTMs require additional chemical additives(***-TFSI,t-TBP)towards high performance,however,the introduction of additives decrease the PSCs device ***,an organic metal complex(Ni-TPA)is first developed as a dopant-free HTM applied in PSCs for its facile synthesis and efficient hole extract/transfer ***,the dopant-free Ni-TPAbased device achieves a champion efficiency of 17.89%,which is superior to that of pristine Spiro-OMeTAD(14.25%).Furthermore,we introduce a double HTM layer with a graded energy bandgap containing a Ni-TPA layer and a CuSCN layer into PSCs,the non-encapsulated PSCs based on the Ni-TPA/CuSCN layers affords impressive efficiency up to 20.39%and maintains 96%of the initial PCE after 1000 h at a relative humidity around 40%.The results have demonstrated that metal organic complexes represent a great promise for designing new dopant-free HTMs towards highly stable PSCs.

关键词： Perovskite solar cell Hole transporting material Organic metal complex dopant-free

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A crosslinked polymer as dopant-free hole-transport material for efficient n-i-p type perovskite solar cells

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Journal of Energy Chemistry 2021年第4期30卷 211-218页

作者： Linqin Wang Fuguo Zhang Tianqi Liu Wei Zhang Yuanyuan Li Bin Cai Lanlan He Yu Guo Xichuan Yang Bo Xu James M.Gardner Lars Kloo Licheng Sun Organic Chemistry Centre of Molecular DevicesDepartment of ChemistryKTH Royal Institute of TechnologySE-10044 StockholmSweden Applied Physical Chemistry Centre of Molecular DevicesDepartment of ChemistryKTH Royal Institute of TechnologySE-10044 StockholmSweden Wallenberg Wood Science Centre Department of Fibre and Polymer TechnologyKTH Royal Institute of TechnologySE-10044 StockholmSweden State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesDalian University of TechnologyDalian 116024LiaoningChina

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 *** 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 *** 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 *** 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 *** 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.

关键词： Perovskite solar cell Hole-transport material dopant-free Crosslinked polymer Spiro[fluorene-9,9’-xanthene](SFX)

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Recent Progresses on dopant-free Organic Hole Transport Materials toward Efficient and Stable Perovskite Solar Cells

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Chinese Journal of Chemistry 2023年第22期41卷 3133-3166页

作者： Gang Xie Jintao Chen Huiyu Li Jianxin Yu Haoran Yin Zhiping Wang Yaoyao Huang Chuizheng Feng Yang Pan Aihui Liang Yiwang Chen National Engineering Research Center for Carbohydrate Synthesis/Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education Jiangxi Normal University99Ziyang AvenueNanchangJiangxi330022China College of Chemistry and Chemical Engineering/Institute of Polymers and Energy Chemistry(IPEC) Nanchang University99 Xuefu AvenueNanchangJiangxi330031China

As the third generation new battery,the power conversion efficiency(PCE)of metal halide perovskite solar cells(PsCs)has increased from 3.8%in 2009 to 25.8%currently certified,which fully shows that they have great research value and development *** one of the main components of high-efficiency PSCs,hole transport materials(HTMs)play an important role in extracting and transporting holes and inhibiting charge ***,commonly used HTMs require doping,and the hygroscopicity and corrosiveness of the dopants will destroy the stability of PsCs and hinder their ***,it is of great significance to develop dopant-free HTMs.

关键词： Organic hole transport materials dopant-free Perovskite solar cells Efficient Stable

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Low-cost dopant-free fluoranthene-based branched hole transporting materials for efficient and stable n-i-p perovskite solar cells

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Chinese Chemical Letters 2024年第10期35卷 187-193页

作者： Xinyu Yu Fei Wu Xianglang Sun Linna Zhu Baoyu Xia Zhong'an Li Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China Chongqing Key Laboratory for Advanced Materials and Technologies of Clean Energy Faculty of Materials&EnergySouthwest UniversityChongqing 400715China

It has been widely recognized that hole transporting materials(HTMs)play a key role in the rapid progress of perovskite solar cells(PVSCs).However,common organic HTMs such as spiro-OMe TAD not only suffer from high synthetic costs,but also usually require the additional chemical doping process to improve their hole transport ability,which unfortunately induces the terrible stability ***,it is urgent to develop low-cost dopant-free HTMs for efficient and stable *** this work,we have successfully developed a new class of efficient dopant-free fluoranthene-based HTMs(TPF1–5)with quite low lab synthetic costs by combining donor-acceptor and branched structure *** detailed structure-property study revealed that tuning the twisted arms at different substitution sites would regulate the intermolecular interactions and film-forming ability,thereby significantly affecting the performance of the *** applying these HTMs in conventional PVSCs,the dopant-free TPF1-based devices not only achieved the best efficiency of 21.76%,which is comparable to that of the doped spiro-OMeTAD control devices,but also showed much better operational stability,which maintained over 87%of the initial efficiency under maximum power point tracking after 1038 h.

关键词： Perovskite solar cells Holetransporting materials dopant-free Fluoranthene Low-cost

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One-Pot Synthesis of Tetraarylpyrrolo[3,2-b]pyrrole dopant-free Hole-Transport Materials for Inverted Perovskite Solar Cells

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Chinese Journal of Chemical Physics 2021年第2期34卷 217-226,I0002页

作者： Liang-sheng Duan Quan-ping Wu Yuan-yuan Xu Hui Wang Zhe Sun Yu Chen Song Xue School of Materials Science and Engineering Tianjin Key Laboratory of the Design and Intelligent Control of the Advanced Mechanical SystemSchool of Mechanical EngineeringTianjin University of TechnologyTianjin 300384China

Four organic smallmolecule hole transport materials(D41, D42,D43 and D44) of tetraarylpyrrolo[3,2-b]pyrroles were prepared. They can be used without doping in the manufacture of the inverted planar perovskite solar cells. Tetraarylpyrrolo[3,2-b]pyrroles are accessible for one-pot synthesis.D42, D43 and D44 possess acceptor-π-donor-π-acceptor structure, on which the aryl bearing substitutes of cyan, fluorine and trifluoromethyl, respectively. Instead, the aryl moiety of D41 is in presence of methyl with a donor-π-donor-π-donor structure. The different substitutes significantly affected their molecular surface charge distribution and thin-film morphology, attributing to the electron-rich properties of fused pyrrole ring. The size of perovskite crystalline growth particles is affected by different molecular structures,and the electron-withdrawing cyan group of D42 is most conducive to the formation of large perovskite grains. The D42 fabricated devices with power conversion efficiency of17.3% and retained 55% of the initial photoelectric conversion efficiency after 22 days in dark condition. The pyrrolo[3,2-b]pyrrole is efficient electron-donating moiety for hole transporting materials to form good substrate in producing perovskite thin film.

关键词： Pyrrole[3,2-b]pyrrole Hole-transporting materials Organic small molecules dopant-free Perovskite solar cells

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dopant-free Coplanar D-π-D Hole-Transporting Materials for Highly Efficient Perovskite Solar Cells with Enhanced Fill Factors

Dopant-Free Coplanar D-π-D Hole-Transporting Materials for ...

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第六届新型太阳能电池材料科学与技术学术研讨会

作者： Yatong Chen Xiuwen Xu Ning Cai Sai-Wing Tsang School of Chemical Engineering and Light Industry Guangdong University of Technology Department of Materials Science and Engineering City University of Hong Kong City University of Hong Kong Shenzhen Research Institute

Recently, a large amount of dopant-free HTMs including small molecules and conjugated polymers have been vigorously explored, however, in most of cases, perovskite solar cells exhibit much lower FFs(mostly less than 75%) , which may derive from inefficient charge extraction or current leakage through shunts and accompanying additional recombination losses. Herein, hole extraction through the dopant-free HTL plays a key role in avoiding charge transport losses and maximizing the FF. Nevertheless, significantly less effort has been devoted to improve the FF of PSCs and to probe inherent structure-property correlations. In this study, we designed and synthesized two novel D-p-D hole-transporting materials(HTM), coded BDT-PTZ and BDT-POZ, which consists of benzo[1,2-b:4,5-b’]dithiophene(BDT) as p conjugated linker, and phenothiazine(PTZ)/phenoxazine(POZ) as donor units. Herein, BDT-PTZ and BDT-POZ were utilized in p-i-n perovskite solar cells as dopant-free hole transporting layers, exhibiting excellent power conversion efficiencies of 18.26% and 19.16%, respectively. Particularly, BDT-POZ demonstrated a superior fill factor of 82%, which is consistent with its more efficient hole extract and hole transport demonstrated by steady state/transient fluorescence spectra and space-charge-limited current(SCLC) technique. Single crystal XRD characterization implies these two HTM molecules present diverse packing tendencies, which may account for various interfacial hole transport ability in perovskite solar cells.

关键词： dopant-free hole-transporting materials perovskite solar cells

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Rational Design of dopant-free Coplanar D-pi-D Hole-Transporting Materials for High-Performance Perovskite Solar Cells with Fill Factor Exceeding 80%

Rational Design of Dopant-Free Coplanar D-pi-D Hole-Transpor...

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第七届新型太阳能电池材料科学与技术学术研讨会

In this paper, we report two novel D-pi-D hole-transporting materials(HTM),abbreviated as BDT-PTZ and BDT-POZ,which consists of 4,8-di(hexylthio)-benzo[1,2-b:4,5-b’]dithiophene(BDT) as conjugated linker,and N-(6-bromohexyl) phenothiazine(PTZ)/N-(6-bromohexyl) phenoxazine(POZ) as donor *** above two HTMs were deployed in p-i-n perovskite solar cells as dopant-free hole transporting layers,exhibiting excellent power conversion efficiencies of 18.26% and 19.16% ***,BDT-POZ demonstrated a superior fill factor of 81.7%,which is consistent with its more efficient hole extraction and transport verified via steady state/transient fluorescence spectra and space-charge-limited current *** crystal XRD characterization and analysis implies molecule packing mode and distance of redox center located on adjacent molecules may affect the intrinsic hole extract and transport ability of HTM in perovskite solar cells,which will pave a way for further designing low-cost,high-performance HTM molecules.

关键词： perovskite solar cells dopant-free hole transporting materials hole mobility

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Highly π-extended copolymer as additive-free hole- transport material for perovskite solar cells

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Nano Research 2018年第1期11卷 185-194页

作者： Jie Liu Qianqing Ge Weifeng Zhang Jingyuan Ma Jie Ding Gui Yu Jinsong Hu Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CASResearch/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing 100049 China

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.

关键词： perovskite solar cell hole-transport layer dopant-free PDVT-IO stability

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A non-wetting and conductive polyethylene dioxothiophene hole transport layer for scalable and flexible perovskite solar cells

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Science China Chemistry 2021年第5期64卷 834-843页

作者： Chenxiang Gong Lin Zhang Xiangchuan Meng Zhi Xing Li Rao Hongyu Wang Zengqi Huang Licheng Tan Ting Hu Xiaotian Hu Yiwang Chen College of Chemistry Nanchang UniversityNanchang 330031China Institute of Polymers and Energy Chemistry Nanchang UniversityNanchang 330031China Hunan Key Laboratory for Super Microstructure and Ultrafast Process School of Physics and ElectronicsCentral South UniversityChangsha 410083China School of Materials Science and Engineering Nanchang UniversityNanchang 330031China Institute of Advanced Scientific Research(iASR) Jiangxi Normal UniversityNanchang 330022China

The regulated crystallization of perovskite and highly repeatable preparation are decisive challenges for large-scale flexible perovskite solar cells(PSCs).Herein,we synthesize an oil-soluble poly(3,4-ethylenedioxythiophene)(Oil-PEDOT)as a hole transport layer(HTL).The non-wetting Oil-PEDOT HTL can promote the quality of large-area flexible perovskite films because of its optimized crystallinity and *** Oil-PEDOT layer also delivers desirable conductivity and charge transport without a complex ***,the flexible PSCs with Oil-PEDOT HTL achieve an efficiency of 19.51%and 16.70%based on 1.05 and 22.50 cm^(2),***,these large-scale flexible PSCs demonstrate remarkable mechanical robustness,and the efficiency exhibits 93%retention after 7,000 bending *** results show that the Oil-PEDOT is a potentially efficient HTL for fabricating efficient large-scale flexible PSCs.

关键词： non-wetting dopant-free hole transport layer flexible solar cells large-scale

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