Indacenodithiophene-4,9-dione-Based D-A-D Type Dopant-Free Hole Transporting Materials for Environmentally Robust 30% Efficient Indoor Perovskite Solar Cells

IF 5.3 3区 工程技术 Q2 ENERGY & FUELS
Sibu Manna, Prasun Kumar, Rahul Tiwari, Buddhadeb Mondal, Chitrak Ghosh, Ranbir Singh* and Suman Kalyan Samanta*, 
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Abstract

To develop low-light responsive materials for perovskite solar cells (PSCs), for the first time, we synthesized s-indaceno[1,2-b:5,6-b’]-dithiophene-4,9-dione core acceptor linked 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline and N,N-diphenylaniline end-cap donors based on symmetrical donor–acceptor–donor (D-A-D) type two hole-transporting materials (HTMs), TPA-IDT-OMe and TPA-IDT-H. The relative synthetic costs of the two HTMs, TPA-IDT-OMe and TPA-IDT-H, are about one-seventh and one-fifth times cheaper, respectively, compared to the commercially available spiro-OMeTAD. Both the symmetrical D-A-D type HTMs presented good thermal stability, remarkable photophysical and electrochemical properties, along with down-shifted HOMO energy levels, extended π-conjugation, and enhanced π-π stacking in the film state. Moreover, the methoxy group-bearing TPA-IDT-OMe exhibited superior hole extraction and hole mobilities with negligible bimolecular recombination at the perovskite/HTM interfaces due to the suitable band alignment with the perovskite energy levels, a more planar conjugated backbone, and improved intermolecular π-π stacking in the film state, which led to better interaction with the perovskite layer. As a result, the PSCs from dopant-free TPA-IDT-OMe yielded an impressive power conversion efficiency (PCE) value of 30.19%, with high open-circuit voltage (Voc), short-circuit current density (Jsc) and fill factor (FF) values of 0.89 V, 157.30 μA/cm2, and 70.30%, respectively, under indoor light illumination (1000 lx, 321.6 μW/cm2) which is comparable to the PCE value of the doped spiro-OMeTAD-based devices. Moreover, TPA-IDT-OMe showed remarkable UV stability after 240 h of aging and admissible moisture stability with relative humidity (RH) of (40% ± 5%) at room temperature due to its greater hydrophobicity compared to TPA-IDT-H and the reference spiro-OMeTAD. The poor solubility of TPA-IDT-H illustrates its poor film formation ability, which results in greater bimolecular and trap-assisted recombination and lower hole mobility, leading to a lower PCE value of 27.08% for the undoped TPA-IDT-H-based PSCs. This finding opens a new path to design low-light responsive D-A-D architecture-based small molecular HTMs for efficient and stable indoor perovskite solar cells.

Abstract Image

吲哚二噻吩-4,9-二酮基D-A-D型无掺杂空穴传输材料用于环境稳健的30%高效室内钙钛矿太阳能电池
为了开发钙钛矿太阳能电池(PSCs)的弱光响应材料,我们首次基于对称供体-受体-供体(D-A-D)型两种空穴传输材料(HTMs),合成了s-indaceno[1,2-b:5,6-b ']-二噻吩-4,9-二酮核心受体连接的4-甲氧基-N-(4-甲氧基苯基)-N-苯基苯胺和N,N-二苯基苯胺端帽给体TPA-IDT-OMe和TPA-IDT-H。两种HTMs, TPA-IDT-OMe和TPA-IDT-H的相对合成成本分别比市售的spiro-OMeTAD便宜约七分之一和五分之一。两种对称的D-A-D型HTMs均表现出良好的热稳定性、优异的光物理和电化学性能,且薄膜态下HOMO能级下移、π共轭扩展和π-π堆积增强。此外,含甲氧基的TPA-IDT-OMe在钙钛矿/HTM界面上表现出优异的空穴提取和空穴迁移率,而在钙钛矿界面上的双分子重组可以忽略,这是由于与钙钛矿能级合适的能带排列、更平面的共轭主链以及在膜态下改善的分子间π-π stacking,从而导致了与钙钛矿层更好的相互作用。结果表明,在室内光照(1000 lx, 321.6 μW/cm2)下,无掺杂的TPA-IDT-OMe制备的PSCs的功率转换效率(PCE)高达30.19%,开路电压(Voc)、短路电流密度(Jsc)和填充因子(FF)分别为0.89 V、157.30 μA/cm2和70.30%,与掺杂的spiro- ometad器件的PCE值相当。此外,与TPA-IDT-H和参考spiro-OMeTAD相比,TPA-IDT-OMe具有更强的疏水性,在老化240 h后表现出显著的紫外线稳定性和室温相对湿度(RH)为(40%±5%)时的允许水分稳定性。TPA-IDT-H的溶解度较差说明其成膜能力较差,导致双分子和陷阱辅助重组较多,空穴迁移率较低,导致未掺杂的TPA-IDT-H基psc的PCE值较低,为27.08%。这一发现为设计高效稳定的室内钙钛矿太阳能电池的低光响应D-A-D结构小分子HTMs开辟了一条新途径。
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来源期刊
Energy & Fuels
Energy & Fuels 工程技术-工程:化工
CiteScore
9.20
自引率
13.20%
发文量
1101
审稿时长
2.1 months
期刊介绍: Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.
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