富勒烯吡咯烷衍生物的合成及其在反式钙钛矿太阳能电池中的应用  

Synthesis of fulleropyrrolidine derivatives and their applications in inverted perovskite solar cells

作　　者：戴乐山 李云飞 陈斌文 曹琨 邓林龙[1] 谢素原[2] 郑兰荪[2] DAI Leshan;LI Yunfei;CHEN Binwen;CAO Kun;DENG Linlong;XIE Suyuan;ZHENG Lansun(Pen-Tung Sah Institute of Micro-Nano Science and Technology,Xiamen University,Xiamen 361005,China;State Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China)

机构地区：[1]厦门大学萨本栋微米纳米科学技术研究院,福建厦门361005 [2]厦门大学化学化工学院,固体表面物理化学国家重点实验室,福建厦门361005

出　　处：《厦门大学学报（自然科学版）》2024年第1期56-62,110,共8页Journal of Xiamen University：Natural Science

基　　金：国家自然科学基金(92061122,92061204)。

摘　　要：[目的]由于目前在反式钙钛矿太阳能电池中使用最广泛的富勒烯基电子传输材料[6,6]-苯基-C_(61)-丁酸甲酯(PCBM)存在合成复杂、成本高的问题,因此开发低成本、可溶液处理的新型富勒烯电子传输材料具有非常重要的意义.[方法]采用Prato反应一步合成两种低成本的新型富勒烯吡咯烷衍生物F1和F2,并将其作为电子传输材料应用于反式钙钛矿太阳能电池.通过紫外-可见吸收光谱和循环伏安法研究了这两种富勒烯分子的能级,并研究了由这两种富勒烯吡咯烷衍生物作为电子传输层的反式钙钛矿太阳能电池的光伏性能.[结果]含有苯甲酸酯侧链的F2比含有烷基酸酯侧链的F1具有更高的电子迁移率,因此对应的器件获得了更高的填充因子和光电转换效率.最终,以F2作为电子传输层的反式钙钛矿太阳能电池获得了最高19.86%的光电转换效率,这一结果与同等实验条件下制备的基于PCBM的对照器件的效率基本一致.[结论]本研究采用Prato反应一步合成了两种富勒烯吡咯烷衍生物,并发现侧链对其光伏性能有重大影响.该项工作对于开发兼具高效率和低成本的可溶液处理的富勒烯基电子传输材料的设计具有一定的参考价值.[Objective] Inverted perovskite solar cells(PSCs) have attracted great attention due to their advantages,including large-scale low-temperature processing,improved operational stability and suitability for tandem cells.However,the most commonly used fullerene electron transport layer(ETL) [6,6]-phenyl-C_(61)-butyric acid methyl ester(PCBM) has high manufacturing cost due to its complex synthesis.Thus,developing low-cost,solution-processable fullerene electron transport materials is crucial for the commercialization of inverted PSCs.Herein,two fulleropyrrolidine derivatives,F1 and F2,were synthesized as alternative low-cost ETL to replace PCBM in inverted PSCs.[Methods] Inverted p-i-n perovskite solar cells were fabricated with the structure of ITO/poly(triaryl amine)(PTAA)/perovskite/fullerene/bathocuproine(BCP)/Ag.PTAA(2 mg/mL in toluene) was spin-coated onto a pre-cleaned ITO substrate at 2 000 r/min for 30 s and annealed at 100 ℃ for 10 min.The perovskite precursor solution was prepared by dissolving a mixed powder of formamidinium iodide(FAI),methylammonium iodide(MAI),CsI,PbI_2,and PbBr_(2) in N,N-dimethylformamide/dimethyl sulfoxide(4∶1,by vol) solutions.The precursor solution was spin-coated at 1 000 r/min for 15 s and then 5 000 r/min for 30 s,followed by chlorobenzene antisolvent treatment before the end of the spin-coating process.PCBM,F1 and F2(20 mg/mL in chlorobenzene) were spin-coated at 3 000 r/min for 20 s.Then,BCP(0.5 mg/mL in isopropanol) was spin-coated at 6 000 r/min for 30 s and annealed at 80 ℃ for 10 min.Finally,about 100 nm of Ag was thermally evaporated under high vacuum(2×10~(-4) Pa) to complete the device.[Results] F1 and F2 were synthesized using a one-pot Prato reaction,which is simple and cost-efficient.UV-Vis spectrometry and cyclic voltammetry measurements show that F1,F2 and PCBM have nearly the same HOMO and LUMO energy levels.PSCs based on F2 exhibit a power conversion efficiency(PCE) of 19.86%,which is much higher than that of F1-based devices(18.62%) and is very close to

关 键 词：钙钛矿太阳能电池 富勒烯吡咯烷 电子传输层 光伏性能 

分 类 号：O649.5[理学—物理化学]