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离子掺杂调控双钙钛矿量子点发光性能的研究进展

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高等学校化学学报 2024年第9期45卷 1-15页

作者：张丽媛王查斯娜胡井香詹传郎内蒙古师范大学化学与环境科学学院先进材料化学与器件内蒙古自治区高等学校重点实验室呼和浩特010022

铅基卤化物钙钛矿发光材料因具有灵活的晶体结构、带隙可调性、缺陷容忍性和高荧光量子产率等优异性能而备受关注.但金属铅的毒性和钙钛矿的稳定性一直是阻碍其商业应用急需解决的问题.因此,需要探索更绿色环保的非铅金属卤化物类钙钛... 详细信息

铅基卤化物钙钛矿发光材料因具有灵活的晶体结构、带隙可调性、缺陷容忍性和高荧光量子产率等优异性能而备受关注.但金属铅的毒性和钙钛矿的稳定性一直是阻碍其商业应用急需解决的问题.因此,需要探索更绿色环保的非铅金属卤化物类钙钛矿发光材料.近年来,通过替换铅离子发展起来的非铅双钙钛矿结构成功实现了低毒性和高稳定性,但由于其是间接带隙或因为宇称禁阻的直接带隙而造成光致发光效率极低.为了解决此问题,研究人员开发了离子掺杂策略,实现了光致发光效率的提升.本文综合评述了非铅双钙钛矿材料的晶体结构和发光性能,归纳了主族金属、稀土金属和过渡金属掺杂对非铅双钙钛矿发光性能的影响及其发光机制.最后,对离子掺杂策略的应用和进一步提升非铅双钙钛矿发光材料的性能进行了总结和展望.

关键词：双钙钛矿量子点离子掺杂光致发光量子效率自陷激子态发光

Polymerized A-DA'D-A type small-molecule acceptors for high performance all-polymer solar cells: progress and perspective

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中国科学:化学英文版 2023年第9期66卷 2513-2531页

作者： Ting Yang chuanlang zhan Key Laboratory of Advanced Materials Chemistry and Devices(AMC&DLab)of the Department of Education of Inner Mongolia Autonomous Region College of Chemistry and Environmental ScienceInner Mongolia Normal UniversityHuhhot 010022China

A-DA'D-A type polymerized small-molecule acceptors(PSMAs) have very recently received wide attention because they possess advantages such as synthetic flexibility, narrowed bandgap, low energy loss, and impressive mechanical properties. With efforts on design and synthesis of PSMAs and polymer donors, significant progress has been made on all polymer solar cells(allPSCs) with power conversion efficiencies exceeding 18%. In this review, we focus on structure-property-performance relationships of the A-DA'D-A type PSMAs. First, we in-depth review the regio-random, regio-regular, and random ternary series by focusing on their structural modification such as from aspects of side-chains, halogenation, selenophene-containing and linkers, respectively. Second, we review the mechanically flexible and stretchable properties, which helps to find structural gene that correlates the mechanical properties. Third, we review the impressive small energy loss. In all, this review provides structural and material's clues, helpfully for designing high-performance all-PSCs.

关键词： all-polymer solar cell polymerized small-molecule acceptor regio-random regio-regular terpolymer energy loss

Synthesis and photovoltaic properties of low bandgap dimeric perylene diimide based non-fullerene acceptors

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Science China Chemistry 2016年第2期59卷 209-217页

作者： Xin zhang Jiannian Yao chuanlang zhan Beijing National Laboratory of Molecular Science Key Laboratory of Photochemistry Chinese Academy of Sciences Institute of Chemistry Chinese Academy of Sciences

Non-fullerene organic acceptors have attracted increasing attention in recent years. One of the challenges in the synthesis of non-fullerene organic acceptors is to tune the absorption spectrum and molecular frontier orbitals, affording low bandgap molecules with improved absorption of the near-infrared solar photons. In this paper, we present the synthesis, optoelectronic and photovoltaic properties of a series of dimeric perylene diimide(PDI) based non-fullerene acceptors. These PDI dimers are bridged by oligothiophene(T) from 1T to 6T. With the increase of the oligothienyl size, the highest occupied molecular orbital(HOMO) energy is raised from ?5.65 to ?5.10 e V, while that of the lowest unoccupied molecular orbit(LUMO) is kept constant at ?3.84 e V, affording narrow bandgap from 1.81 to 1.26 e V. The absorption from the oligothiophene occurs between 350 and 500 nm, which is complementary to that from its bridged PDI units, leading to a wide spectral coverage from 350 to 850 nm. The optimal dihedral angle between the bridged two perylene planes is dependent on the oligothienyl size, varying from 5° to 30°. The solubility of the dimers depends on the oligothienyl size and can be tuned by the alkyl chains on the bridged thienyl units. The possible applications as the solution-processable non-fullerene organic acceptor is primarily studied using commercial P3 HT as the blend donor. The photovoltaic results indicate that 1T, 4T and 6T all yield a higher efficiency of ?1.2%, whereas 2T, 3T and 5T all give a lower efficiency of <0.5%. The difference in the cell performance is related with the tradeoff between the differences of absorption, HOMO level and film-morphology between these dimers.

关键词： non-fullerene acceptor organic photovoltaic cell perylene diimide solution-processed bulk-heterojuncti ~n

A Novel BODIPY-Based Low-Band-Gap Small-Molecule Acceptor for Efficient Non-fullerene Polymer Solar Cells

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Chinese Journal of Chemistry 2017年第12期35卷 1813-1823页

作者： Wenxu Liu Jiannian Yao chuanlang zhan Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China

We report herein an efficient A^1-C=C-A^2-C=C-A^1 type small-molecule 4,4＇-difluoro-4-bora-3a,4a-diaza-sindacene （BODIPY） acceptor （A^1= BODIPY and A^2= diketopyrrolopyrrole （DPP）） by following the A-to-A excited electron delocalization via the BODIPY meso-position, the inherent directionality for the excited electron delocalization. The lowest unoccupied molecular orbital （LUMO） delocalizes across over whole the two flanking A^1 and the central A^2, and the highest occupied molecular orbital （HOMO） localizes dominantly on the -C=C-DPP-C=C- segment. The excited electron upon light excitation of the DPP segment delocalizes over both the BODIPY and DPP segments. The acceptor in chloroform shows an unprecedented plateau-like broad absorption between 550 and 700 nm with a large FWHM value of 195 nm. Upon transition into solid film, the acceptor shows absorption in the whole near ultraviolet-visible-near infrared wavelength region （300-830 nm） with a low band gap of 1.5 eV and a maximum absorptivity of 0.85 × 10^5 cm^-1. Introduction of the ethynyl spacer between the A^1 and A^2 and the close BODIPY-to-DPP LUMO energy levels are crucial for the excited n-electron delocalization across over whole the conjugation backbone. A power conversion efficiency of 6.60% was obtained from the ternary non-fullerene solar cell with PTB7-Th：p-DTS（FBTTh2）2 （0.5 ; 0.5） as the donor materials, which is the highest value among the non-fullerene organic solar cells with BODIPY as the electron acceptor material.

关键词： BODIPY nonfullerene low band gap small molecule acceptor organic solar cell

17.1%-Efficiency organic photovoltaic cell enabled with two higher-LUMO-level acceptor guests as the quaternary strategy

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Science China Chemistry 2020年第4期63卷 490-496页

作者： Kun Li Yishi Wu Xuemei Li Hongbing Fu chuanlang zhan Department of Chemistry Capital Normal UniversityBeijing 100048China School of Chemistry&Chemical Engineering Linyi UniversityLinyi 276000China CAS Key Laboratory of Photochemistry Institute of ChemistryChinese Academy of SciencesBeijing 100190China

Quaternary blended organic solar cells utilize four blended material components(one donor plus three acceptors, two donors and two acceptors, or three donors plus one acceptor) as the active layer materials. The use of four material components allows us to have more material selections and more mechanism choices to improve the photon-to-electron conversion efficiency. In this contribution, we present a new case of quaternary material system, that shows 17.1% efficiency obtained by adding IDIC and PC71BM as the guest acceptors of the host binary of PM6:Y6. The lowest unoccupied molecular orbital(LUMO) levels of IDIC and PC71BM are both higher than that of Y6, which is one reason to obtain increased open-circuit voltage(Voc) in the quaternary device. Upon introduction of IDIC and PC71BM as the acceptor guests, the hole and electron mobilities are both increased, which contributes to the increased short-circuit current-density(Jsc). Effects of the weight ratios of the three acceptor components are investigated, which demonstrates that the increased hole and electron mobilities, the accelerated hole-transfer, and the reduced monomolecular recombination are the factors contributing to the increased Jscand fill-factor. This case of quaternary device demonstrates the applicability of the quaternary strategy in increasing the device functions and hence the efficiencies in the field of organic photovoltaic cells.

关键词： quaternary solar cell organic photovoltaic small-molecule acceptor nonfullerene fullerene

Achieving high short-circuit current and fill-factor via increasing quinoidal character on nonfullerene small molecule acceptor

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Chinese Chemical Letters 2018年第3期29卷 381-384页

作者： Wenxu Liu Weiping Li Jiannian Yao chuanlang zhan Beijing National Laboratory of Molecular Sdence CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

Recently, the fused-ring based low band gap （LBG） small molecule acceptors （SMAs） have emerged as efficient nonfullerene acceptors. So far, these LBG SMAs are mainly designed with IC （2-methylene-（3- （1,1 -dicyanomethylene）indanone）） or its analogs, the benzo-type electron-accepting （A） units. Compared to benzene, thiophene is less aromatic and thus the thiophene-involving semiconducting molecule has more quinoidal character, which effectively reduces the energy gap between the highest occupied molecular orbit （HOMO） and the lowest unoccupied molecular orbit （LUMO）. Herein, we show that replacing the IC units in ITIC with the CT （cyclopenta[c]thiophen-4-one-5-methylene-6-（1,1-dicyano- methylene））, a thiophene-fused A unit, the quinoidal character is enhanced from 0.0353 on ITIC to 0.0349 on ITCT, the CT-ended SMA. The increase in the quinoidal character reduces the optical band gap and enhances the near IR absorptivity. When blended with the wide band gap （WBG） polymer donor, PBDB-T, an average power conversion efficiency of 10.99% is obtained with a short-circuit current-density （Jso） of 17.88 mA/cm2 and a fill-factor （FF） of 0.723. For comparisons, theJsc is of 16.92 mA/cm2, FF is of 0.655 and PCE is of 9.94% obtained from the ITIC：PBDB-T device. This case indicates that the replacement of the benzene ring on the IC unit with a more polarizable five-member ring such as thiophene is an effective way to enhance the absorption of the near IR solar photons towards designing high-performance nonfullerene polymer solar cells.

关键词： Cyclopenta[c]thiophen-4-one-5- methylene-6-(13 -dicyanomethylene) Nonfullerene Small molecule acceptor Polymer solar cell

High-efficiency quaternary polymer solar cells enabled with binary fullerene additives to reduce nonfullerene acceptor optical band gap and improve carriers transport

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Science China Chemistry 2018年第12期61卷 1609-1618页

作者： Weiping Li Dong Yan Feng Liu Thomas Russell chuanlang zhan Jiannian Yao eijing National Laboratory for Molecular Sciences CAS Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Department of Physics and Astronomy and Collaborative Innovation Center of IFSA (CICIFSA) Shanghai Jiaotong University Shanghai 200240 China Department of Polymer Science and Engineering Room A516 Conte Research Center University of Massachusetts Amherst120 Governors Drive Amherst MA 01003 USA University of Chinese Academy of Sciences Beijing 100049 China

The polymer/small-molecule electron donor and nonfullerene organic electron acceptor are of structural similarity with both donor and acceptor molecules consisting of polycyclic fused-ring backbone and being decorated with *** this study,we report that the introduction of binary fullerenes(C_(60)-/C_(70)-PCBM and C_(60)-/C_(70)-ICBA)into a nonfullerene binary system PBDB-T:ITIC reduces the polymer-nonfullerene acceptor intermixing,obtaining higher crystallinity with(100)crystal coherence length from 28 to 29–33 nm for the ITIC,and from 14 to 20–24 nm for the PBDB-T,and improved electron and hole mobilities ***,such a protocol reduces the ITIC optical band gap from 1.59 to 1.55 *** consequences,higher short-circuit current-density(17.8–18.4 vs.15.8 m A/cm^2),open-circuit voltage(0.92 vs.0.90 V)and fill-factor(0.72–0.73 vs.0.68)are simultaneously obtained,which ultimately afford higher efficient quaternary polymer solar cells with power conversion efficiencies(PCEs)up to 12.0%–12.8%comparing to the host binary device with 9.9%*** the polymer,ITIC,and ICBA/PCBM ternary blends,11%PCEs were *** use of PCBM leads to larger red-shifting in thin film absorption and external quantum efficiency(EQE)*** effect is more pronounced when ICBA:PCBM mixture is *** results indicate the size and shape of C_(60)and C_(70)as well as the substituent position of the second indene unit on C_(60)-/C_(70)-ICBA affect not only the blend morphology but also the electronic coupling in BHJ mixtures:the quaternary device performance increased in sequences of C_(70)-PCBM:C_(70)-ICBA→C_(70)-PCBM:C_(60)-ICBA→C_(60)-PCBM:C_(70)-ICBA→C_(60)-PCBM:C_(60)-*** resonant soft X-ray scattering(RSoXS)data indicated the most refined phase separation in the C_(60)-PCBM:C_(60)-ICBA based blend,corresponding to its best device function among the quaternary *** results indicate that the using of binary fullerenes as the acceptor add

关键词： quaternary bulk-heterojunction polymer solar cell nonfullerene acceptor fullerene-free fullerene

The self-assemblies of a newly designed star-shaped molecule end-capped with bromine atoms studied by scanning tunneling microscopy

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Chinese Chemical Letters 2020年第2期31卷 353-356页

作者： Jingfei Hou Bin Tu Qingdao Zeng chuanlang zhan Jiannian Yao Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of PhotochemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100080China CAS Key Laboratory of Standardization and Measurement for Nanotechnology CAS Center for Excellence in NanoscienceNational Center for Nanoscience and Technology(NCNST)Beijing 100190China University of Chinese Academy of Sciences Beijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100149China

A new star-shaped molecule StOF-Br_3 containing oligofluorenes and halogen atoms(Bromine) has been synthesized and studied by Scanning Tunneling Microscopy(STM) at the highly oriented pyrolytic graphite(HOPG) *** have obtained the high-resolution self-assembled STM images,from which the highly ordered and closely packed non-porous arrangements of the StOF-Br_3 molecular selfassemblies at the heptanoic acid/HOPG surface could be *** molecular models and selfassembled StOF-Br_3 architectures have been given in the following ***,we have also figured out the surface free energy by the density functional theory(DFT) calculation,which proved that the halogen...halogen interaction was strong enough to stabilize the ordered molecular *** work verifies the existence of bromine...bromine interactions,and meanwhile provides a kind of effective approach for quickly building ordered molecular nanoarchitectures with large areas and different geometries.

关键词： Molecular self-assemblies Star-shaped molecules Scanning tunneling microscopy(STM) Halogen...halogen interactions Bromine atoms

Design a thieno[3,2-b]thiophene bridged nonfullerene acceptor to increase open-circuit voltage,short-circuit current-density and fill factor via the ternary strategy

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Chinese Chemical Letters 2020年第5期31卷 1243-1247页

作者： Xiaofang Li Kun Li Dan Su Fugang Shen Shuying Huo Hongbing Fu chuanlang zhan College of Chemistry and Environmental Science Hebei UniversityBaoding 071002China CAS key Laboratory of Photochemistry Institute of ChemistryChinese Academy of SciencesBeijing 100190China Department of Chemistry Capital Normal UniversityBeijing 100048China

In this study,we report a new small molecule acceptor(named TT-4 F)which uses 3,6-dimethoxylthieno[3,2-b]thiophene(TT)as theπ-*** of 0.05 weight ratio amount of TT-4 F into the host binary blend of PTB7-Th:IEICO-4 F,resulting in a ternary blend in a weight ratio of 1:1:0.05,enables increased open-circuit voltage(Voc),short-circuit curre nt-density(Jsc),and fill-factor(FF)at the same ***,12.1%efficiency is *** to the 3-(2-ethylhexyloxylthiophene)bridge on IEICO-4 F,the additional methoxyl group on the TT-6 position is involved in the lowest unoccupied molecular orbital(LUMO)and the largerπ-system on TT increases the electron-donating nature,both of which help to raise the LUMO level,one reason of the increased *** addition of 0.05 TT-4 F,the hole mobility is increased,the monomolecular recombination is reduced,and the charge dissociation and collection is *** of these contribute to the increased Jsc and FF.

关键词： Fullerene-free Polymer solar cell Small molecule acceptor Ternary solar cell Organic photovoltaic