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We develop an effective strategy to obtain polymer solar cells with high power conversion efficiency (17%) and remarkable mechanical robustness, by design of polymer donors with aliphatic flexible spacer incorporated into a rigid backbone.
Abstract Morphological stability is crucially important for the long‐term stability of polymer solar cells (PSCs). Many high‐efficiency PSCs suffer from metastable morphology, resulting in severe device degradation. Here, a series of copolymers is developed by manipulating the content of chlorinated benzodithiophene‐4,8‐dione (T1‐Cl) via a random copolymerization approach. It is found that all the copolymers can self‐assemble into a fibril nanostructure in films. By altering the T1‐Cl content, the polymer crystallinity and fibril width can be effectively controlled. When blended with several nonfullerene acceptors, such as TTPTT‐4F, O‐INIC3, EH‐INIC3, and Y6, the optimized fibril interpenetrating morphology can not only favor charge transport, but also inhibit the unfavorable molecular diffusion and aggregation in active layers, leading to excellent morphological stability. The work demonstrates the importance of optimization of fibril network morphology in realizing high‐efficiency and ambient‐stable PSCs, and also provides new insights into the effect of chemical structure on the fibril network morphology and photovoltaic performance of PSCs.
All-polymer solar cells (all-PSCs) are a highly attractive class of photovoltaics for wearable and portable electronics due to their excellent morphological and mechanical stabilities. Recently, new types of polymer acceptors (P A s) consisting of non-fullerene small molecule acceptors (NFSMAs) with strong light absorption have been proposed to enhance the power conversion efficiency (PCE) of all-PSCs. However, polymerization of NFSMAs often reduces entropy of mixing in PSC blends and prevents the formation of intermixed blend domains required for efficient charge generation and morphological stability. One approach to increase compatibility in these systems is to design P A s that contain the same building blocks as their polymer donor (P D ) counterparts. Here, a series of NFSMA-based P A s [P(BDT2BOY5-X), (X = H, F, Cl)] are reported, by copolymerizing NFSMA (Y5-2BO) with benzodithiophene (BDT), a common donating unit in high-performance P D s such as PBDB-T. All-PSC blends composed of PBDB-T PD and P(BDT2BOY5-X) P A show enhanced molecular compatibility, resulting in excellent morphological and electronic properties. Specifically, PBDB-T:P(BDT2BOY5-Cl) all-PSC has a PCE of 11.12%, which is significantly higher than previous PBDB-T:Y5-2BO (7.02%) and PBDB-T:P(NDI2OD-T2) (6.00%) PSCs. Additionally, the increased compatibility of these all-PSCs greatly improves their thermal stability and mechanical robustness. For example, the crack onset strain (COS) and toughness of the PBDB-T:P(BDT2BOY5-Cl) blend are 15.9% and 3.24 MJ m -3 , respectively, in comparison to the PBDB-T:Y5-2BO blends at 2.21% and 0.32 MJ m -3 .
Investigation of single wall carbon nanotube (SWNT)-polymer solar cells has been conducted towards developing alternative lightweight, flexible devices for space power applications. Photovoltaic devices were constructed with regioregular poly(3-octylthiophene)-(P3OT) and purified, >95% w/w, laser-generated SWNTs. The P3OT composites were deposited on ITO-coated polyethylene terapthalate (PET) and I-V characterization was performed under simulated AM0 illumination. Fabricated devices for the 1.0% w/w SWNT-P3OT composites showed a photoresponse with an open-circuit voltage (V(sub oc)) of 0.98 V and a short-circuit current density (I(sub sc)) of 0.12 mA/sq cm. Optimization of carrier transport within these novel photovoltaic systems is proposed, specifically development of nanostructure-SWNT complexes to enhance exciton dissociation.
All-polymer solar cells (all-PSCs) have drawn growing attention and achieved tremendous progress recently, but their power conversion efficiency (PCE) still lags behind small-molecule-acceptor (SMA)-based PSCs due to the relative difficulty on morphology control of polymer photoactive blends. Here, in this work, low-cost PTQ10 is introduced as a second polymer donor (a third component) into the PM6:PY-IT blend to finely tune the energy-level matching and microscopic morphology of the polymer blend photoactive layer. The addition of PTQ10 decreases the π–π stacking distance, and increases the π–π stacking coherence length and the ordered face-on molecular packing orientation, which improves the charge separation and transport in the photoactive layer. Moreover, the deeper highest occupied molecular orbital energy level of the PTQ10 polymer donor than PM6 leads to higher open-circuit voltage of the ternary all-PSCs. As a result, a PCE of 16.52% is achieved for ternary all-PSCs, which is one of the highest PCEs for all-PSCs. In addition, the ternary devices exhibit a high tolerance of the photoactive layer thickness with high PCEs of 15.27% and 13.91% at photoactive layer thickness of ≈205 and ≈306 nm, respectively, which are the highest PCEs so far for all-PSCs with a thick photoactive layer.
A major challenge hindering the further development of all-polymer solar cells (all-PSCs) employing polymerized small-molecule acceptors is the relatively low fill factor (FF) due to the difficulty in controlling the active-layer morphology. The issues typically arise from oversized phase separation resulting from the thermodynamically unfavorable mixing between two macromolecular species, and disordered molecular orientation/packing of highly anisotropic polymer chains. Herein, a facile top-down controlling strategy to engineer the morphology of all-polymer blends is developed by leveraging the layer-by-layer (LBL) deposition. Optimal intermixing of polymer components can be achieved in the two-step process by tuning the bottom-layer polymer swelling during top-layer deposition. Consequently, both the molecular orientation/packing of the bottom layer and the molecular ordering of the top layer can be optimized with a suitable top-layer processing solvent. A favorable morphology with gradient vertical composition distribution for efficient charge transport and extraction is therefore realized, affording a high all-PSC efficiency of 17.0% with a FF of 76.1%. The derived devices also possess excellent long-term thermal stability and can retain >90% of their initial efficiencies after being annealed at 65 °C for 1300 h. In conclusion, these results validate the distinct advantages of employing an LBL processing protocol to fabricate high-performance all-PSCs.
Solid additives are crucial in layer-by-layer (LBL) polymer solar cells (PSCs). Despite its importance, the simultaneous application of solid additives into both donor and acceptor layers has been largely overlooked. In this work, two multifunctional solid additives are actively designed, and investigated the synergistic effect on both donor and acceptor layers. Incorporating the multifunctional solid additives into the donor layer could effectively enhance the aggregation and molecular stacking of the donor polymer, leading to reduced energy disorder and minimizing ΔE 2 . When the multifunctional solid additives are introduced into the acceptor layer, they just play a role in optimizing the morphology, thereby reducing the ΔE 3 . Excitedly, the simultaneous addition of the multifunctional solid additives into both donor and acceptor layers produced a synergistic effect for decreasing ΔE 2 and ΔE 3 simultaneously, especially adding SA2, thus enabling an excellent power conversion efficiency (PCE) of 19.95% (certified as 19.68%) with an open-circuit voltage (V oc ) of 0.921 V, a short circuit current density (J sc ) of 27.08 mA cm -2 and a fill factor (FF) of 79.98%. The work highlights the potential of multifunctional solid additives in independently regulating the properties of donor and acceptor layers, which is expected as a promising approach for further developing higher performance PSCs.
Photovoltaic performance and mechanical robustness of all-polymer solar cells are simultaneously enhanced by developing ester-functionalized, wide-bandgap PM7 derivatives.
High-performance eco-friendly all-polymer solar cells were realized by balancing the crystallinity and domain size via hot halogen-free solvent slot-die coating.
All-polymer solar cells (all-PSCs) and all-polymer photodetectors (all-PPDs) are promising for application in flexible electronics, but their performance is greatly limited by the lack of polymer acceptors and the difficulties in morphology control. Herein, we report the use of a high-mobility n-type polymer semiconductor, PNDI-DTBT, for fabricating high-performance all-PSCs and all-PPDs. By pairing PNDI-DTBT with a matched polymer donor, a prominent power conversion efficiency of 8.5% was obtained in all-PSCs, demonstrating the great potential of high-mobility n-type polymers with a conventional donor–acceptor skeleton for photovoltaic application. Moreover, all-PPDs with a low dark current density of 1.32 × 10 –8 A cm –2 at –0.1 V bias and a high specific detectivity of 4.77 × 10 12 Jones were achieved, which belong to the best results of organic photodetectors. Morphology investigations revealed that the formation of a bicontinuous interpenetrating network with optimal phase separation scale, high domain purity, and preferential vertical composition distribution in the bulk-heterojunction active layer contribute to the remarkable device performance. Furthermore, these results suggest that combining high-mobility n-type polymers and morphology optimization is fruitful to achieving high-performance all-PSCs and all-PPDs.
An approach to slow down the polymer solar cell ink aging by employing an additive (i.e., PCBM variants) was developed. It is inferred that PCBMs in the ink act as a co-solvent and slow down the polymer pre-aggregation.
Abstract PM6 is a widely used D–A copolymer donor in the polymer solar cells (PSCs). Incorporating second electron‐withdrawing (A 2 ) units into PM6 backbone by ternary D–A 1 –D–A 2 random copolymerization strategy is an effective approach to further improve its photovoltaic performance. Here, the authors synthesize the PM6‐based terpolymers by introducing thiazolothiazole as the A 2 units connecting with thiophene π‐bridges attaching alkyl substituent towards the A 2 unit (PMT‐CT) or towards D‐unit (PMT‐FT), and study the effect of the alkyl substituent position on the photovoltaic performance of them. Two terpolymers PMT‐FT‐10 and PMT‐CT‐10 are obtained by incorporating 10% A 2 units in the terpolymers. The film of PMT‐CT‐10 shows slightly up‐shifted highest occupied molecular orbital (HOMO) energy levels while better co‐planar structure than that of PMT‐FT‐10. Meanwhile, the PMT‐CT‐10:Y6 blend film exhibits better molecular packing properties, more proper phase separation and more balanced hole and electron mobilities, which are beneficial to more efficient exciton dissociation, efficient charge transport and weaker bimolecular recombination. Consequently, the PMT‐CT‐10 based PSCs obtain the highest power conversion efficiency of 18.21%. The results indicate that side chain position on the thiophene π‐bridges influence the device performance of the terpolymer donors, and PMT‐CT‐10 is a high efficiency polymer donor for the PSCs.
All-polymer solar cells with low voltage loss for efficient outdoor and indoor photovoltaics.
Constructing terpolymer has attracted increasing attention as a strategy to improve the performance of polymer solar cell. Terpolymer usually offers an opportunity to lower the frontier molecular orbital energy level, introduces additional absorption band and sometimes optimizes the morphology of the active blend. Generally, the additional segment in terpolymer backbone inevitably introduces backbone disorder, which causes entropy rises. However, selecting a suitable dipole unit introduces extra driving forces for crystallization by enhancing intermolecular interactions. This provides a handy knob for tradeoff between intermolecular interaction and backbone disorder, thus regulating the blend morphology. In this study, a high dipole and electron-deficient group of pyrrolo[3,4-f ]benzotriazole-5,7(6H)-dione (TzBI) is incorporated into the high-performance donor polymer and a series of terpolymers with different content of TzBI are designed. As expected, the morphology is optimized gradually for improving charge generation and charge transport, also suppressing charge recombination. The champion device with 10% TzBI exhibited a power conversion efficiency (PCE) of 18.36%, which is 5% increase compared to the controlled device. This study presents a charming terpolymer strategy by highly electron-deficient and high dipole segment to realize a tradeoff between intermolecular interaction and backbone disorder, facilitating the optimization of morphology and elevation of fill factor and device efficiency.
Processing additive plays an important role in the standard operation procedures for fabricating top performing polymer solar cells (PSCs) through efficient interactions with key photovoltaic materials. However, improving interaction study of acceptor materials to high performance halogenated aromatic additives such as diiodobenzene (DIB) is a widely neglected route for molecular engineering toward more efficient device performances. Here, in this work, two novel Y-type acceptor molecules of BTP-TT and BTP-TTS with different aromatic side chains on the outer positions are designed and synthesized. The resulting aromatic side chains significantly enhanced the interactions between the acceptor molecules and DIB through an arene/halogenated arene interaction, which improved the crystallinity of the acceptor molecules and induced a polymorph with better photovoltaic performances. Thus, high power conversion efficiencies (PCEs) of 18.04% and 19.22% are achieved in binary and ternary blend devices using BTP-TTS as acceptor and DIB as additive. Aromatic side chain engineering for improving additive interactions is proved to be an effective strategy for achieving much higher performance photovoltaic materials and devices.
A desired morphology is essential for achieving efficient polymer solar cells. Donors and acceptors with appropriate crystallization can lead to a suitable phase-separated morphology for effective photocurrent generation process. Inspired by the success of Y6 acceptors and the 2D side chain engineering on popular polymer donors and small molecule acceptors, the usage of unique 2D 3,4-ethylene dioxythiophene (EDOT) side chains on Y6 to regulate its crystallinity, compatibility, and thus the related blend morphology is explored. Here, in this study, two molecules of BTP-EDOT-4F and BTP-EDOT-4Cl with such unique 2D EDOT side chains are designed and synthesized. Due to the advantage of EDOT side chain, when these molecules are blended with PM6, the decent power conversion efficiencies (PCEs) of 16.78% and 15.87% are obtained. Furthermore, BTP-EDOT-4F is selected as the third component and added into PM6:L8-BO binary system to form ternary blends. The optimized crystallinity, compatibility, and morphology of such ternary blend are discovered in the presence of BTP-EDOT-4F, which enables efficient exciton dissociation and charge transport as well as decreased recombination, resulting in higher short circuit current density (J sc ) and fill factor. Finally, the outstanding PCE of 18.56% is achieved in ternary blends containing PM6, L8-BO, and BTP-EDOT-4F.
The power conversion efficiencies (PCEs) of small molecule acceptor (SMA)-based organic solar cells have already exceeded 18%. However, the development of polymer acceptors still lags far behind their SMA counterparts mainly due to the lack of efficient polymer acceptors. In this work, a series of polymer acceptors named PY-X (with X being the branched alkyl chain) are designed and synthesized by employing the same central core with the SMA L8-BO but with different branched alkyl chains on the pyrrole motif. It is found that the molecular packing of SMA-HD featuring 2-hexyldecyl side chain used in the synthesis of PY-HD is similar to L8-BO, in which the branched alkyl chains lead to condensed and high-order molecular assembly in SMA-HD molecules. When combined with PM6, PY-HD-based all polymer solar cell (all-PSC) exhibits a high PCE of 16.41%, representing the highest efficiency for the binary all-PSCs. Moreover, the side-chain modification on the pyrrole site position further improves the performance of the all-PSCs, and the PY-DT-based device delivers a new record high efficiency of 16.76% (certified as 16.3%). The work provides new insights for understanding the structure–property relationship of polymer acceptors and paves a feasible avenue to develop efficient conjugated polymer acceptors.
Simultaneously enhancing the short-circuit current density (J sc ) and open-circuit voltage (V oc ) of current state-of-the-art polymer solar cells (PSCs) containing wide bandgap polymers as donors and Y6 derivatives as acceptors is of great challenge but essential for further improvement of the photovoltaic performances. Here, in this work, two Y-type non-fullerene acceptors of BTP-T and BTP-TCl were designed and successfully synthesized with relatively weak electron-accepting thiophene based end groups, where blue-shifted absorption and upshifted LUMO energy levels were achieved to fill the well-known absorption gap at 700 nm of typical binary devices based Y-type molecules and rise the output voltage, respectively. Simultaneously increased J sc and V oc were achieved in ternary blend devices containing D18:BTP-eC9:BTP-TCl with a significantly improved PCE up to 19.15 %, which is over 7 % increase compared to the binary device. Our results illustrated the great potential of rational design of Y6 derivatives for constructing ternary PSCs to improve their performances.