理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池※

doi:10.6023/A21120620

化学学报 ›› 2022, Vol. 80 ›› Issue (6): 724-733.DOI: 10.6023/A21120620 上一篇下一篇

所属专题：中国科学院青年创新促进会合辑

研究论文

理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池^※

林文源^a^,^b, 朱清哲^a^,^b, 马云龙^b^,^*(), 王鹏^b^,^e, 万硕^b^,^d, 郑庆东^b^,^c^,^*()

a 福州大学化学学院福州 350108
b 中国科学院福建物质结构研究所结构化学国家重点实验室福州 350002
c 南京大学现代工程与应用科学学院南京 210093
d 中国科学院大学北京 100049
e 上海科技大学物质科学与技术学院上海 201210

投稿日期:2021-12-31 发布日期:2022-07-07
通讯作者: 马云龙, 郑庆东
作者简介:
^※庆祝中国科学院青年创新促进会十年华诞.
基金资助:
国家自然科学基金(22075287); 国家自然科学基金(52130306); 中科院青年创新促进会项目(2021000060)

Rationally Tuning Blend Miscibility of Polymer Donor and Nonfullerene Acceptor for Constructing Efficient Organic Solar Cells^※

Wenyuan Lin^a^,^b, Qingzhe Zhu^a^,^b, Yunlong Ma^b(), Peng Wang^b^,^e, Shuo Wan^b^,^d, Qingdong Zheng^b^,^c()

a College of Chemistry, Fuzhou University, Fuzhou 350108
b State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002
c College of Engineering and Applied Sciences, Nanjing University, Nanjing 210093
d University of Chinese Academy of Sciences, Beijing 100049
e School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210

Received:2021-12-31 Published:2022-07-07
Contact: Yunlong Ma, Qingdong Zheng
About author:
^※Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
National Natural Science Foundation of China(22075287); National Natural Science Foundation of China(52130306); Program of Youth Innovation Promotion Association CAS(2021000060)

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摘要/Abstract

除了非富勒烯受体的设计与合成, 聚合物给体的选择对非富勒烯太阳能电池的光伏性能同样重要. 本工作设计并合成一种共轭骨架无sp³杂化碳原子的新型非富勒受体(命名为MDB), 并将其作为模型化合物研究给受体混溶性和分子有序堆积对太阳能电池性能的影响. 本工作选择三种宽带隙聚合物给体(PM6、J71和P3HT)与MDB共混来制备太阳能电池. 得益于MDB和PM6之间适度的混溶性, 由二者组成的混合膜表现出合适的相分离, “face-on”的分子取向和更紧密有序的分子堆积, 从而促进了载流子传输, 并抑制了电荷复合. 因此基于PM6:MDB的器件实现了13.26%的优异光电转换效率, 远高于基于J71:MDB (8.16%)和P3HT:MDB (0.45%)的器件. 该工作证明了给体-受体之间合适的混溶性是实现高效率有机太阳能电池的关键因素之一, 这对有机光伏材料的设计与合成具有重要指导意义.

关键词: 有机太阳能电池, 非富勒烯受体, 聚合物给体, 混溶性, 光电转换效率

Besides the design and synthesis of nonfullerene acceptors, the selection of polymer donors is also critical in determining the photovoltaic performance of nonfullerene organic solar cells (OSCs). However, the selection criteria of polymer donors for nonfullerene OSCs has been rarely investigated. In this work, a novel nonfullerene acceptor (MDB) with sp³-hybridized-carbon-free ladder-type skeleton was developed and used as a model compound to study the effects of miscibility and molecular ordering in determining the performance of MDB-based solar cells. In order to achieve matched energy levels and complementary absorption, three wide-bandgap polymers (PM6, J71, and P3HT) with different chemical structures were selected to blend with MDB for OSCs. The donor:acceptor miscibilities of the three blends were estimated by contact angle measurements, while their crystallinity and phase separation were investigated by grazing incidence wide-angle X-ray scattering characterization and atomic force microscopy measurement, respectively. The interfacial tension values between MDB and PM6, MDB and J71, as well as MDB and P3HT were determined as 0.49, 0.16, and 2.00 mN•m^–1, in that order. Owing to the proper miscibility between MDB and PM6, the resulting blend film exhibits suitable phase separation, “face-on” molecular orientation as well as compact molecular π-π stacking, which promotes carrier transport and suppresses bimolecular recombination. As a result, the best-performance OSC based on PM6:MDB delivered an outstanding PCE of 13.26%. In contrast, J71:MDB-based devices exhibited a lower PCE of 8.16%, due to the excessively high miscibility of J71 and MDB. As for P3HT:MDB-based devices, the poor miscibility between P3HT and MDB provides the driving force for the formation of large phase separation, which leads to an extremely low PCE of 0.45%. This work demonstrates that suitable miscibility is one of the key factors to achieve high-performance OSCs, which is an important guideline for the design and selection of next-generation photovoltaic materials.

Key words: organic solar cells, nonfullerene acceptors, polymer donors, miscibility, power conversion efficiency

引用此文

林文源, 朱清哲, 马云龙, 王鹏, 万硕, 郑庆东. 理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池^※[J]. 化学学报, 2022, 80(6): 724-733.

Wenyuan Lin, Qingzhe Zhu, Yunlong Ma, Peng Wang, Shuo Wan, Qingdong Zheng. Rationally Tuning Blend Miscibility of Polymer Donor and Nonfullerene Acceptor for Constructing Efficient Organic Solar Cells^※[J]. Acta Chimica Sinica, 2022, 80(6): 724-733.

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图/表 9

图1. 受体MDB的合成路线

Figure 1. Synthetic route of the acceptor MDB

图2. (a) PM6、J71和P3HT的分子结构; (b) MDB、PM6、J71和P3HT的溶液或薄膜吸收光谱; (c)本工作中所使用材料的能级图

Figure 2. (a) Molecular structures of PM6, J71 and P3HT; (b) normalized absorption spectra of MDB, PM6, J71, and P3HT in solution or thin film state; (c) energy level diagram of the materials utilized in this work

Molecule	ε/(×10⁵ L•mol^–1•cm^–1)	λ_max^solution^a/nm	λ_max^film^b/nm	E_g^opt^c/eV	HOMO^d/eV	LUMO^d/eV
MDB	2.06	745	771	1.39	–5.58	–3.97

表1. MDB的光学和电化学特性

Table 1. Optical and electrochemical properties of MDB

图3. 基于PM6:MDB, J71:MDB和P3HT:MDB最佳器件的(a) J-V曲线和(b)外量子效率光谱

Figure 3. (a) J-V curves and (b) EQE spectra of the best-performing PSC devices based on PM6:MDB, J71:MDB, and P3HT:MDB

D:A	V_oc^a/V	J_sc^a/(mA•cm^–2)	Integrated J_sc^b/(mA•cm^–2)	FF^a/%	PCE^a/%
PM6:MDB	0.91 (0.91±0.01)	21.64 (21.58±0.23)	21.00	67.65 (66.92±1.32)	13.26 (13.14±0.12)
J71:MDB	0.92 (0.92±0.01)	17.26 (17.13±0.31)	17.09	51.46 (50.89±3.26)	8.16 (8.02±0.22)
P3HT:MDB	0.48 (0.48±0.01)	2.07 (2.03±0.11)	1.98	45.08 (42.11±4.26)	0.45 (0.41±0.08)

表2. 基于PM6:MDB, J71:MDB和P3HT:MDB器件的光伏参数

Table 2. Photovoltaic parameters of the devcies based on PM6:MDB, J71:MDB, and P3HT:MDB

图4. 基于MDB和不同给体器件的(a) Jph-Veff曲线; (b)空穴和电子迁移率; (c) Jsc相对Plight特征曲线以及(d) Voc相对Plight的特征曲线

Figure 4. (a) Jph-Veff curves; (b) hole and electron mobilities; (c) Jsc versus Plight characteristics and (d) Voc versus Plight characteristics of the devices based on MDB with different donors

图5. (a, d) PM6:MDB, (b, e) J71:MDB和(c, f) P3HT:MDB混合薄膜的AFM高度图和相应的粘附力图(500 nm×500 nm)

Figure 5. AFM height images and the corresponding adhesion images of (a, d) PM6:MDB, (b, e) J71:MDB, and (c, f) P3HT:MDB blend films (500 nm×500 nm)

图6. (a)纯MDB, PM6, J71和P3HT薄膜上的水和二碘甲烷液滴的接触角图像; (b) MDB, PM6, J7和P3HT的色散力(γd)和极性力(γp)分量; (c) MDB和不同给体之间的界面张力(γA-B)和Flory-Huggins相互作用参数(χA-B)

Figure 6. (a) Contact angle images of water and diiodomethane droplets on the neat films of MDB, PM6, J71 and P3HT; (b) dispersion (γd) and polarity (γp) components of MDB, PM6, J71 and P3HT; (c) interfacial tension (γA-B) and Flory-Huggins interaction parameters (χA-B) between MDB and different donors

图7. 纯MDB薄膜, PM6:MDB, J71:MDB和P3HT:MDB混合膜的(a~d) 2D掠入射广角X射线衍射图和(e)相应的面内(IP)和面外(OOP)方向的1D线切剖面图

Figure 7. (a~d) The 2D GIWAXS patterns, and (e) corresponding in-plane (IP) and out-of-plane (OOP) 1D integral curves of pure MDB film, PM6:MDB, J71:MDB, and P3HT:MDB blend films

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理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池^※

Rationally Tuning Blend Miscibility of Polymer Donor and Nonfullerene Acceptor for Constructing Efficient Organic Solar Cells^※

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理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池※

Rationally Tuning Blend Miscibility of Polymer Donor and Nonfullerene Acceptor for Constructing Efficient Organic Solar Cells※

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理性调控聚合物给体-非富勒烯受体的混溶性制备高效率有机太阳能电池^※

Rationally Tuning Blend Miscibility of Polymer Donor and Nonfullerene Acceptor for Constructing Efficient Organic Solar Cells^※