基于非富勒烯小分子受体Y6的有机太阳能电池

徐翔; 李坤; 魏擎亚; 袁俊; 邹应萍

doi:10.7536/PC201016

化学进展 ›› 2021, Vol. 33 ›› Issue (2) :165-178 DOI: 10.7536/PC201016

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基于非富勒烯小分子受体Y6的有机太阳能电池

徐翔 ¹ ,
李坤 ¹ ,
魏擎亚 ¹ ,
袁俊 ¹ ,
邹应萍 ¹^,^*

作者信息 +

Organic Solar Cells Based on Non-Fullerene Small Molecular Acceptor Y6

Xiang Xu ¹ ,
Kun Li ¹ ,
Qingya Wei ¹ ,
Jun Yuan ¹ ,
Yingping Zou ¹^,^*

Author information +

文章历史 +

摘要

随着给/受体材料的不断发展,有机太阳能电池的器件效率不断取得进展。特别是非富勒受体分子Y6的出现,使单结有机太阳能电池的效率突破了15%。Y6已经应用到了有机太阳能电池各个方面并且极大提升了其性能。本综述主要总结了Y6在二元、三元和四元、逐层印刷、柔性、叠层和半透明等有机太阳能电池方面的研究情况,以及基于Y6三线态的有机太阳能电池的进展,最后对Y6的结构优化及在器件领域中的应用进行了展望。

Abstract

With the development of donor and acceptor materials, the power conversion efficiency(PCE) of organic solar cells(OSCs) has continuously made breakthrough in recent years. Particularly, the emergency of non-fullerene acceptor Y6 has enabled the device efficiency of OSCs over 15%. Y6 has been applied in many aspects and greatly improved its photovoltaic properties. This review focuses on the applications of Y6 in binary, ternary and quaternary, layer-by-layer, flexible, tandem and semitransparent organic solar cells, meanwhile, the future structure optimizations and device applications of Y6 have been outlooked.

Contents

1 Introduction

2 Binary organic solar cells based on Y6

2.1 Polymer donors matching with the Y6 acceptor

2.2 Small molecular donors matching with the Y6 acceptor

3 Ternary and quaternary organic solar cells based on Y6

4 LBL-processed OSCs based on Y6

5 Flexible OSCs based on Y6

6 Tandem OSCs based on Y6

7 Semi-transparent OSCs based on Y6

8 Research on OSCs based on Y6 triplet state

9 Conclusion and outlook

Graphical abstract

关键词

Y6 / 有机太阳能电池 / 非富勒烯小分子受体 / 效率 / 应用

Key words

Y6 / organic solar cells / non-fullerene small molecular acceptors / efficiency / applications

引用本文

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徐翔, 李坤, 魏擎亚, 袁俊, 邹应萍. 基于非富勒烯小分子受体Y6的有机太阳能电池[J]. 化学进展, 2021, 33(2): 165-178 DOI:10.7536/PC201016

Xiang Xu, Kun Li, Qingya Wei, Jun Yuan, Yingping Zou. Organic Solar Cells Based on Non-Fullerene Small Molecular Acceptor Y6[J]. Progress in Chemistry, 2021, 33(2): 165-178 DOI:10.7536/PC201016

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1 引言

有机太阳能电池具有质轻、材料来源广泛、可制备柔性和半透明器件等优势,已成为一种具有广阔前景的新能源技术^{[1⇓⇓⇓⇓⇓~7]}。1986年,邓青云等^[8]用酞菁铜(CuPC)和四羧基苝衍生物,制备了第一个双层异质结有机太阳能电池,器件效率达到1%(光强为75 mW/cm²)。近年来,得益于给/受体材料和界面材料的快速发展及器件结构和制备工艺的不断优化,有机太阳能电池效率不断取得突破^{[9⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~23]}。2015年,Zhan课题组^[19]以引达省并二噻吩(IDT)为中间核,双氰基茚满二酮(IC)为端基合成了ITIC,与PTB7-Th共混得到了6.8%的能量转换效率(PCE)。2016年,Hou课题组^[24]用能级更匹配、吸光系数更好的PBDB-T与ITIC共混作为活性层,器件效率提高到11.21%。2019年,Zou课题组^[23]报道了A-DA'D-A型非富勒烯小分子受体Y6,与PM6共混制备器件,效率达到15.7%,这也是单结有机太阳能电池效率首次突破15%。基于Y6分子,众多科研工作者开展了一系列的研究,进一步提升了有机光伏器件效率,推动有机光伏向市场化迈进^{[25⇓⇓⇓⇓⇓~31]}。

2017年,Zou课题组^[32]首次将电子受体单元苯并三氮唑引入非富勒烯受体稠环的中心核,形成一种DA'D稠环结构,进而合成了A-DA'D-A型有机小分子受体BZIC。该类新型非富勒烯小分子受体可以有效地拓宽吸收光谱,降低器件的电压损失,为新材料的设计提供了指导。随后,该课题组与加州大学洛杉矶分校(UCLA )的Yang Yang课题组合作,在中间核不变的前提下,用并二噻吩取代噻吩,将并五环拓展成并七环,采用不同的端基,合成了电子受体Y1和Y2^[33]。共轭环的拓展,拓宽了非富勒烯小分子受体材料的吸收光谱,同时进一步降低了器件的能量损失。同时,Zou课题组^[23]将苯并噻二唑取代苯并三唑作为稠环中间核,通过在并二噻吩的β位上引入烷基链来调节分子的溶解性和分子构象,合成了非富勒烯受体Y6,与PBDB-T-2F(PM6)共混,单结有机太阳能电池器件效率达到15.7%。随后,Y6被应用到有机太阳能电池的各个方面,并且极大提升了其光伏性能。

基于此,本文总结了近两年来基于Y6受体材料所开展的二元共混、三元和四元共混、逐层印刷、柔性器件、叠层电池和半透明太阳能电池等方面的研究,以期为未来有机太阳能电池的发展提供指导。

2 基于Y6的二元共混太阳能电池

Y6的出现使得聚合物给体/小分子受体和全小分子体系迅速发展,不断推动有机太阳能电池的效率突破。本节将分为聚合物给体/Y6和小分子给体/Y6两部分来阐述。

2.1 和Y6受体匹配的聚合物给体

国内外课题组针对Y6受体分子合成了与其吸收光谱和能级相匹配的聚合物给体材料,研究表明Y6受体具有好的兼容性,和大多数聚合物给体能很好的匹配。图1是聚合物给体材料,表1是与之相对应器件的光伏性能参数。2018年,Li等^[34]报道了宽带隙聚合物给体材料PTQ10,由于其成本低且合成步骤简单,使其成为一种潜在实际应用的给体材料。2020年,Li课题组^[35]用PTQ10与Y6共混制备的二元器件的PCE达到16.53%。Yan等^[36]用PM7作为给体材料,与PM6相比,PM7具有更低的HOMO能级,增加了E_HOMO-donor和E_{LUMO-acceptor}之间的带隙,为V_oc的提升提供了可能,与Y6共混制备的二元器件的PCE达到17.04%,其中开路电压(V_oc)达到了0.90 V,短路电流密度(J_sc)为25.64 mA/cm²,填充因子(FF)为0.74。Zhang 等^[37]用PM6和PBFTz中两个共聚单元按照4∶1的比例聚合得到PM1聚合物,PM1和Y6共混制备的器件性能达到了17.6%,其中V_oc为0.87 V、J_sc为25.9 mA/cm²、FF达到了0.78。PM1基器件性能优于PM6/Y6和PBFTz/Y6器件(光伏性能如表1所示)。除了优异的性能外,PM1基器件还具有很好的重复性。

2019年,Huang等^[38]用酰亚胺苯并三氮唑(TzBI)缺电子基团的P2F-EHp作为聚合物给体,和Y6共混获得16.02%的器件效率,其中V_oc 达到了0.81 V,J_sc为26.68 mA/cm²,FF为0.74。他们进一步发现该体系大面积时依旧能获得优异的性能,当器件面积达到1 cm²时,器件效率达到了14.39%,当加入PCBM作三元共混器件时,器件效率提高到了15.13%,研究表明该体系具有突出的应用前景^[39]。2020年,他们^[40]基于TzBI单元合成了新的给体聚合物PTzBI-dF,和Y6共混器件效率达到16.8%,其中V_oc 达到0.85 V,J_sc为26.33 mA/cm²,FF为0.76。同时这个给体和其同分异构体PTzBI-pF相比,性能更加优异,研究表明氟原子取代的位置不同强烈地影响分子结构和形貌,进而影响光学吸收和电荷传输性能。

2019年,Zhou等^[41]合成了两个结构相似的共聚物J52-FS和PE2。J52-FS使用噻吩作为π桥,PE2使用噻吩并[3,2-b]噻吩作为π桥。PE2与Y6共混制备的二元器件PCE达到13.5%,其中V_oc 为0.83 V,J_sc为23.24 mA/cm²,FF为0.70;而J52-FS和Y6共混制备的二元器件PCE为10.58%,表明TT作为π桥是构建高效聚合物光伏材料较好的分子设计策略。同年,Zhou等^[42]再次用3-己基噻吩并[3,2-b]噻吩作为π桥合成聚合物给体材料PE4。PE4与Y6共混制备的二元器件PCE达到14.02%,其中V_oc 达到0.84 V,J_sc为23.77 mA/cm²,FF为0.75。相比于噻吩作为π桥,以3-己基噻吩并[3,2-b]噻吩作为π桥使得主链构象由锯齿形变为线形,从而促进更有序的层状堆积和较小的相畴。

2019年,Peng等^[43]合成了一个宽带隙聚合物给体PSFTZ(如图1所示)。PSFTZ具有与Y6互补的吸收和匹配的能级。然而由于PSFTZ的强聚集作用,活性层的相分离明显,增加了电荷复合的几率,与Y6共混制备的器件效率只有13.07%。通过添加少量的Pt(Ph)₂(DMSO)₂, 可使聚合物PSFTZ与Pt(Ph)₂(DMSO)₂发生铂(Ⅱ)络合。由于铂(Ⅱ)配合物上的苯环增加了空间位阻,抑制了聚合物的聚集,调控了相分离,因此,器件效率可提升至16.35%。Ding课题组^[44]用5H-二硫代[3,2-b:2',3'-d]硫吡咯-5-酮(DTTP)取代5H-二硫代[3,2-b:2',3'-d]吡咯-5-酮单元(DTP),合成聚合物给体D16,与Y6共混,器件效率达到16.72%。在D16的基础上,用DTBT代替DTTP,得到D18。与DTTP相比,DTBT具有更大的分子平面,从而DTBT基聚合物具有更高的空穴迁移率。D18:Y6基太阳能电池效率达到18.22%(NIM认证效率17.6%)^[45]。

2.2 和Y6受体匹配的小分子给体

与聚合物给体材料相比,小分子给体材料具有明确的分子结构、高重复性和高纯度等优点^{[46⇓⇓⇓⇓~51]}。在小分子给体设计与合成中,Ge课题组^[52]选择氟代二噻吩并苯并二噻吩作为核心基团构筑了两类A-π-D-π-A型小分子给体BTEC-1F和BTEC-2F(图2)。与BTEC-1F:Y6相比,基于BTEC-2F与Y6共混层,得到的器件性能参数为:V_oc =0.854 V,J_sc =21.55 mA/cm²,FF=0.72,PCE=13.34%,增强的相分离、紧凑的分子堆积以及高度有序的face-on 分子取向是其性能提升的原因。Lu课题组^[53]采用氯代的苯并二噻吩三噻吩罗丹宁(BTR)分子制备了BTR-Cl。BTR-Cl分子具有更加有序的液晶性能、更深的分子能级和较高结晶性,与Y6受体共混,得到合适的薄膜形貌,全小分子有机太阳能电池器件效率达到13.6%。在此基础上,引入PC₇₁BM作第三组分,最优的器件效率可以达到15.34%,其中FF大幅提升至0.77,研究表明PC₇₁BM的引入大幅降低了双分子复合从而导致FF提升^[54]。

Wei课题组^[55]报道了一种A-π-D-π-A结构的小分子给体ZR1(图2), 该给体和Y6吸收互补,器件效率最高达到了14.34%(认证效率达到14.1%),其中V_oc =0.86 V,J_sc =24.34 mA/cm²,FF=0.68。2020年,Li课题组^[56]合成了SM1-F小分子电子给体(图2),与Y6共混的器件性能参数为:V_oc =0.866 V,J_sc =23.25 mA/cm²,FF=0.70,PCE=14.07%。Zhang等^[57]合成了一种新的小分子给体BTTzR(图2), 基于BTTzR:Y6的全小分子体系的效率达到了13.9%,其中V_oc =0.88 V,J_sc =23.20 mA/cm²,FF=0.68,且该体系的非辐射复合能量损失仅为0.18 eV,接近无机太阳能电池。

3 基于Y6的三元和四元共混太阳能电池

近年来,二元有机太阳能电池不断取得进展^{[58⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓~69]}。然而由于较窄的光学吸收和HOMO与LUMO能级不匹配导致的高能量损失等因素,限制了二元有机太阳能电池效率的提高^{[70⇓⇓⇓⇓~75]}。为了解决上述问题,引入第三组分制备三元有机太阳能电池的策略被提出并得到广泛应用^{[76⇓⇓⇓⇓⇓~82]}。Y6与聚合物给体共混可以得到优异的PCEs,众多课题组的研究结果表明二元器件的效率可超过16%。对于PM6:Y6体系,可以通过添加第三组分(如富勒烯衍生物、非富勒烯小分子受体、聚合物给体或小分子给体以及固体添加剂) 来进一步提升PCEs^{[83⇓⇓~86]}。

2019年,Hou等^[87]在PM6:Y6二元体系的基础上,添加富勒烯衍生物PC₆₁BM作为第三组分,能增加电子迁移率,进而实现了平衡的电子/空穴电荷传输,同时PC₆₁BM可以分散Y6的自身聚集,提高电致发光效率,减少非辐射能量损失。制备的三元有机太阳能电池,V_oc、J_sc和 FF同时得到改善,效率达到16.5%。Zhan课题组^[85]把非富勒烯受体IDIC引入PM6:Y6中,制备的器件效率为16.5%。IDIC较高的LUMO能级是V_oc提升的一个原因。同时,在该体系中,IDIC提供一个额外的快速空穴转移通道,有助于载流子的产生。Sun等^[88]针对PM6:Y6体系,设计合成了新的小分子受体3TP3T-4F作为第三组分,得到的器件性能参数为V_oc =0.85 V,J_sc =25.9 mA/cm²,FF=0.75,PCE=16.7%。2020年,Bao等^[89]将小分子给体DRTB-T-C4加入到PM6:Y6体系中,获得了超过17%的效率,其中V_oc 为0.85 V,J_sc 为24.79 mA/cm²,FF为0.81,最终可获得17.13%的光电转换效率。DRTB-T-C4的加入可以同时提高空穴和电子迁移率,并使电荷传输更加平衡,此外,DRTB-T-C4与PM6:Y6共混物具有良好的兼容性。

四元有机共混太阳能电池是利用四种材料混合(一个给体和三个受体,两个给体和两个受体,或三个给体和一个受体)作为活性层材料,四种材料的组合使得科研工作者们可以选择更多的材料和更多的机制来提高PCE^{[90⇓⇓⇓⇓~95]}。图3和表3分别列举了一些高效的三元和四元有机太阳能电池中第三或第四组分的化学结构以及器件性能参数。2020年,Zhan课题组^[96]在PM6:Y6:IDIC的基础上,加入富勒烯衍生物PC₇₁BM组成一个四元体系,器件的性能为:V_oc =0.87 V,J_sc =26.19 mA/cm²,FF=0.75,PCE=17.07%。IDIC和PC₇₁BM较高的LUMO能级是其V_oc提高的原因,同时IDIC和PC₇₁BM的加入提高了电子和空穴迁移率,有利于提升J_sc 。2020年,Zhan课题组^[31]在PM6:Y6:PC₇₁BM体系中加入聚合物给体材料PhI-Se作为第四组分,得到的器件性能为:V_oc =0.85 V,J_sc =26.3 mA/cm²,FF=0.77,PCE=17.2%。研究表明PhI-Se客体可以形成单独的给体相,各个PhI-Se相的存在增强了太阳光的吸收,并且提供了额外的电荷分离和空穴传输路径,可以产生更多的电荷并传输更多的空穴。PhI-Se的加入还可以改善Y6受体相的结构有序度,从而改善了电子传输。Liu课题组^[97]在高效率的PM6:Y6的基础上,加入了聚合物给体PM7和富勒烯受体PC₇₁BM,通过物理表征手段发现四元共混中形成了一种双级联式的载流子传输通道,PM7居中的HOMO能级可以实现空穴的超快转移,增加了输出电流。同时,PC₇₁BM的引入降低了非辐射复合损耗,并且为电子提供了快速的转移通道。最终,器件实现了18.07%的PCE(NREL认证效率达到17.35%),其中V_oc 为0.86 V,J_sc 为26.55 mA/cm²,FF为0.79。

4 基于Y6的逐层加工太阳能电池

1986年,邓青云^[8]制备了第一个双层异质结有机太阳能电池。1995年,俞钢和Heeger等^[98]制备了第一个体相异质结结构(BHJ)的有机太阳能电池,该结构中聚合物给体和富勒烯受体形成了互穿网络结构,大大增加了给体和受体之间的接触面积。至今,随着光伏材料的发展,有机太阳能电池通过BHJ结构实现了高PCEs,但是在大面积制备过程中难以精确控制BHJ的形貌,不利于推动有机太阳能电池的产业化。近几年,逐层印刷制备的有机太阳能电池重新受到了科研工作者的关注, 与BHJ结构相比,逐层印刷的方法具有诸多优势,如可控的活性层薄膜形貌^[99,100]、良好的电荷传输和提取性能以及普适性^[101⇓~103]、对给/受体材料的合成批次不敏感等^[104]。

2019年,Yip等^[100]利用连续逐层加工(Layer-by-layer)的方式来调控三元有机太阳能电池的形貌。在PM6:Y6:FBR组成的三元LbL有机太阳能电池中可以得到16.4%的转换效率。研究表明LbL薄膜可以形成双连续互穿网络结构并且给受体的结晶性几乎不受影响,显示出高效的电荷产生、传输和收集特性,且三元LbL的PCE对于第三组分受体加入的比例不敏感,从而为优化器件性能提供了空间。2020年,Min等^[105]利用LbL方式来制备高性能大面积有机太阳能电池和组件。基于PM6:Y6体系,获得16.35%的PCE。研究表明LbL方法具有材料兼容、高吸光性、垂直相分离和实用性等优势。

5 基于Y6的柔性有机太阳能电池

柔性是有机太阳能电池的一个突出优势,基于柔性有机太阳能电池的PCEs依然低于刚性基底的有机太阳能电池的PCEs,且由于缺乏高性能柔性透明电极,其机械稳定性目前也无法满足柔性电子产品的需求^{[73,106⇓⇓⇓⇓⇓⇓⇓ ~114]}。常用的铟锡氧化物电极(ITO)在有机太阳能电池领域占有主导地位,然而在塑料基底上进行涂覆时,由于在热退火和机械弯曲过程中基底材料收缩,ITO会破裂,从而导致方阻和漫反射率增加严重影响器件的机械稳定性^[108]。近年来,已有科研人员对柔性透明电极进行优化,并取得了众多成果。

2019年,Li等^[115]提出 “焊接”的概念。该课题组使用溶液处理的铝掺杂的ZnO(AZO)和银纳米线(AgNW)网络组成上部电极,利用毛细作用力和AZO的二次生长进行焊接,进而降低了AgNW结点的电阻。他们使用PM6:Y6体系作为活性层,采用Em-Ag/AgNWs:AZO-SG作为柔性基底,制备的柔性有机太阳能的PCE达到15.21%,并且在弯折近8000次之后,保持了初始效率的75%。2020年,Ge等 ^[116]分别使用三种经济环保的酸(柠檬酸,酒石酸和苹果酸)和多羟基化合物处理PEDOT:PSS电极制备高效可折叠柔性有机太阳能电池。基于PM6:Y6二元体系,制备得到了效率14.17%的柔性有机太阳能电池,其结果如图4所示。酸处理使得PEDOT:PSS具有高电导率,同时,多羟基化合物的掺杂有助于基底有更出色的弯曲柔韧性和可折叠性。Bao等^[26]在PM6:Y6体系中掺入5wt% 聚芳基醚(PAE)树脂,器件的PCE达到16.13%。更重要的是,掺入30wt% PAE时,器件的PCE仍可达到15.17%,展示出4.4倍的断裂伸长率。研究表明,PAE基质在不改变电荷传输通道的情况下显示出隧穿效应,而且还能抑制分子链的移动。柔性有机太阳能电池在可穿戴方面具有优势,同时提升器件的效率和柔性依然是继续努力的方向。

6 基于Y6的叠层有机太阳能电池

近年来,科研工作者们在新型给体,受体材料的开发方面取得了重要进展,特别是新型高效率非富勒烯受体材料的出现,推动了有机太阳能电池的PCEs不断取得突破,器件的PCEs已经超过了17%^{[19,23,45,116⇓⇓⇓ ~120]}。尽管如此,由于有机光伏材料本身的吸收范围较窄,这也导致有机太阳能电池不能充分利用太阳光谱,使得进一步提高有机太阳能电池的PCEs面临挑战^{[87,101,121⇓⇓ ~124]}, 通常采用多元共混和叠层电池等方法解决这一问题。相对于多元共混太阳能电池,叠层有机太阳能电池是将两个或者两个以上的单结器件通过串联或者并联的方式叠加在一起,能最大程度改善器件对于太阳光的吸收^{[125⇓⇓⇓⇓⇓~131]}。

自从2006年首次用溶液法制备第一个叠层电池以来,由于近红外(NIR)非富勒烯受体材料的发展,目前叠层有机太阳能电池器件的最高效率为17.3%^[132]。虽然Y6取得了巨大的成功,但在叠层上的应用却比较少。2020年,Ding等^[133]利用合成的中等带隙小分子非富勒烯受体IBCT,通过L1: IBCT作为前电池,L1:Y6作为后电池制备的叠层电池的器件效率达到了15.25%。Li和Meng等^[134]在Y6的在七元环和端基之间增加双键作为π桥,合成了光学带隙只有1.21 eV的受体BTPV-4F,通过PTB7-Th: BTPV-4F:PC₇₁BM为前电池,PM6:m-DTC-2F为后电池制备的叠层器件效率达到了16.4%。虽然基于Y6的叠层电池效率还不高,但是如果找到更合适的给体以及前电池,相信叠层器件的效率可以进一步突破^[130]。

7 基于Y6的半透明有机太阳能电池

半透明有机太阳能电池(ST-OSCs)可吸收大量近红外光来转换为电能,同时可透过大部分的可见光,在建筑一体化、光伏玻璃、温室农业和可穿戴设备等领域具有广阔的应用前景,引起了学术界和产业界的浓厚兴趣^{[135⇓⇓~138]}。ST-OSCs可以通过改变活性层材料的组成选择性吸收可见光区和近红外(NIR)区。在AM1.5G太阳光谱的能量分布图中,47%的太阳能分布在可见光区,而51%的太阳能分布在近红外区,表明近红外区能量的利用在提升光电转化方面发挥着重要作用^[139]。随着非富勒烯受体材料和半透明器件结构的发展,ST-OSCs目前已取得了快速的发展。平均可见光透过率(AVT)和PCE被认为是评估ST-OSCs的两个关键性能参数^[140]。近年来,ST-OSCs的PCEs达到10%~12%,AVTs约为25%,然而由于ST-OSCs需要在PCEs和AVTs之间权衡,所以ST-OSCs的发展依然落后于不透明的有机太阳能电池^[141]。

在ST-OSCs发展的早期,活性层材料主要是基于中或窄带隙聚合物给体材料和富勒烯衍生物^[142]。近年来吸收红外光的非富勒烯电子受体得到了快速发展,这类受体可以有效地利用红外光子,透过可见光区的光子,是组成ST-OSCs的理想活性层受体材料^{[23,26,94,143⇓ ~145]}。Y6作为目前的明星非富勒烯受体分子,在近红外区有较强的吸收,可以保证有足够的光吸收,适合于制备ST-OSCs。2019年,Li等^[84]通过化学沉淀的方法制备了SnO₂颗粒用作ST-OSCs电子收集层。由于具有出色的透明度和光反射率,SnO₂层可以有效地调节整个ST-OSCs中各层入射光的光分布。在时域差分有限法(FDTD)和光学矩阵传递法(TMF)的模拟指导下,有效地解决了PCEs和AVTs之间的矛盾,结合上述优点,用PM6:Y6制备的反向ST-OSCs,PCE达到12.88%,AVT为25.6%,显色指数(CRI)为97.6,满足商业化玻璃应用的要求。2020年,Li和Yip等^[146]设计了新的Fabry-PÉrot(F-P)电极。F-P电极的引入主要为了尽可能降低透过光谱的带宽从而减小半透明电池的透过颜色失真度。这类电极的设计通常是金属/绝缘体/金属这种三层夹心结构,通过F-P电极的干涉作用可以调制透过光特定波段的波长。半透明器件结构如图5所示,在光学模拟的辅助下,器件效率可以超过14%并且最大透光率大于31% 。

8 基于Y6三线态的有机太阳能电池研究

为了提升有机太阳能电池的PCEs,拓宽光谱吸收和减少能量损失是至关重要的。在有机半导体中存在单线态和三线态两种激发态。单线态激子寿命通常在10~100 ps,激子扩散距离在3~10 nm,性能受限于BHJ活性层的厚度与形貌。原则上,由于三线态复合被禁阻,三线态激子比单线态激子有更长的寿命和扩散距离。并且当T₁能级越接近³CT时,三线态激子解离将变得更容易,同时高效的系间窜越也有助于提升对三线态激子的利用率从而有助于提升器件的性能。因此,三线态材料的开发和研究对于实现高性能的OSCs也很重要^{[147⇓⇓~150]}。

在研究三线态激子对于OSCs的影响中,Y6作为代表性的非富勒烯受体分子,受到了科研工作者的关注。2020年,Yi等^[151]通过ITIC、IT-4F和Y6三种具有代表性的非富勒烯受体分子,来研究端基的π-π堆积在降低ΔE_ST(单线态和三线态之间的能隙) 的重要作用。通过分子内的推-拉效应可以降低ΔE_ST,合适的推-拉效应对于实现高的振子强度和中等ΔE_ST是至关重要的。在三种非富勒烯受体体系中,PM6:Y6体系有最小的E_g和ΔE_ST,获得了最高的PCE 。Huang等^[152]合成两个与Y6相似的A-DA'D-A非富勒烯电子受体H1和H2(化学结构式如图6所示)。其中,PBDB-T:H1的器件效率可以达到14.06%(其中V_oc =0.76 V,J_sc =25.74 mA/cm²,FF=0.71),PBDB-T:H2的器件效率可以达到15.12% (其中V_oc =0.79 V,J_sc =25.82 mA/cm²,FF=0.73)。通过稳态瞬态光致发光、吸收光谱、电子顺磁共振(EPR) 和磁-光电流(MPC) 等表征证明H1和H2是三线态非富勒烯受体材料。通过对三线态激子的机理研究,发现扭曲的D-A结构可以导致大的自旋轨道耦合(SOC)和小的ΔE_ST,从而实现高效的系间窜越。根据摄动理论,

K ISC ∝ < 1 ψ | H SO ⌢ | 3 ψ > / exp Δ E ST 2

, 其中

< 1 ψ | H SO ⌢ | 3 ψ >

表示自旋轨道耦合矩阵元,

H SO ⌢

表示自旋轨道耦合哈密顿量,ΔE_ST表示单线态和三线态之间的能级差,

K ISC

表示系间窜越的速率常数。这个公式说明大的自旋轨道耦合量和小的ΔE_ST可以提升系间窜越的速率。T₁的能级更接近³CT,有利于三线态激子转变为自由电荷。

9 结论与展望

随着非富勒烯受体材料的发展,有机太阳能电池的器件效率近年来不断取得突破。A-DA'D-A型受体结构为设计高性能有机半导体材料提供了新思路^[153]。Y6作为近两年来具有代表性的明星非富勒烯受体分子,具有较强的吸收、较窄的带隙(1.33 eV)和优异的电子迁移率,与PM6共混制备的二元器件的PCE已超过16%,基于PM6:Y6的三元器件PCE已超过17%。同时,Y6在其他有机半导体应用领域如有机光电探测器^[154]等方面也具有较好的发展潜力。

为了提升Y6在有机太阳能电池器件中的应用,提升其商业价值,未来还需要在给受体材料合成和器件制备工艺等方面进行优化,进一步提升器件的PCE及稳定性。

(1) 首先合成与Y6更加匹配的给体材料,拓宽混合膜的吸收光谱,优化能级匹配来进一步提升光伏性能。比如可引入高效的电子受体单元合成光伏给体材料,降低给体材料的HOMO能级,为提高V_oc提供可能性。

(2) 选择合适的给/受体材料作为第三组分,利用三元策略进一步提高Y6体系的性能参数。第三组分的引入可以拓宽吸收光谱,改善结晶性,提高载流子迁移率。同时优化器件结构。

(3) 对Y6分子结构进行修饰。首先,大部分A-DA'D-A型分子是并七环骨架,因此可以将骨架结构拓宽到七环以上,改善电子传输性能和光收集性能。其次,还可以运用侧链工程对Y6进行修饰。通过不同的烷基链,调节分子的溶解度、结晶性以及混溶性,改善载流子迁移率。最后,引入不同端基。除了IC系列的端基外,还可以应用其他种类的端基来改善光伏性能。

(4) 优化器件的制备工艺。除旋涂活性层外,探索其他种类活性层溶液的加工方式,简化活性层的加工条件。例如采用卷对卷及喷涂的方式来制备大面积器件,为有机太阳能电池的实际应用进行更多的探索。

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