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Ternary strategy with integration characteristics and adaptability is a simple and effective method for blooming of the performance of photovoltaic devices. Herein, a novel wideband gap polymer donor PBB2-Hs is synthesized as the guest component to optimize all-polymer solar cells (all-PSCs). High-energy photon absorption and long exciton lifetime of PBB2-Hs constitute efficient energy transfer. Good miscibility and cascade energy levels promote the formation of alloy-like structure between PBB2-Hs and host system. The dual working mechanisms greatly improve photon capture and charge transfer in active layers. Additionally, the introduction of PBB2-Hs also optimizes the ordered molecular stacking of acceptors and suppresses molecular peristalsis. Upon adding 15 wt% PBB2-Hs, the ternary all-PSC achieved a champion efficiency of 17.66%, and can still maintain 82% photostability (24 h) and 91% storage stability (1000 h) of the original PCE. Moreover, the strong molecular stacking and entanglement between PBB2-Hs and the host material increased the elongation at break of ternary blend film by 1.6 times (16.2%), allowing the flexible device to maintain 83% of the original efficiency after 800 bends (R = 5 mm). This work highlights the effectiveness of guest polymer on simultaneously improving photovoltaic performance, photostability and mechanical stability in all-PSCs.
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The layer-by-layer (LBL) fabrication method allows for controlled microstructure morphology and vertical component distribution, and also offers a reproducible and efficient technique for fabricating large-scale organic solar cells (OSCs). In this study, the polymers D18 and PYIT-OD are employed to fabricate all-polymer solar cells (all-PSCs) using the LBL method. Morphological studies reveal that the use of additives optimizes the microstructure of the active layer, enhancing the cells' crystallinity and charge transport capability. The optimized device with 2% CN additive significantly reduces bimolecular recombination and trap-assisted recombination. All-PSCs fabricated by the LBL method based on D18/PYIT-OD deliver a power conversion efficiency (PCE) of 15.07%. Our study demonstrates the great potential of additive engineering via the LBL fabrication method in regulating the microstructure of active layers, suppressing charge recombination, and enhancing the photovoltaic performance of devices.
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All-polymer solar cells (all-PSCs) have been regarded as one of the most promising candidates for commercial applications owing to their outstanding advantages such as mechanical flexibility, light weight and stable film morphology. However, compared to large amount of new-emerging excellent polymer acceptors, the development of high-performance polymer donor lags behind. Herein, a new D-π-A type polymer donor, namely QQ1, was developed based on dithienoquinoxalineimide (DTQI) as the A unit, benzodithiophene with thiophene-conjugated side chains (BDTT) as the D unit, and alkyl-thiophene as the π-bridge, respectively. QQ1 not only possesses a strong dipole moment, but also shows a wide band gap of 1.80â eV and a deep HOMO energy level of -5.47â eV, even without halogen substituents that are commonly indispensable for high-performance polymer donors. When blended with a classic polymer acceptor PY-IT, the QQ1-based all-PSC delivers an outstanding PCE of 18.81 %. After the introduction of F-BTA3 as the third component, a record PCE of 19.20 % was obtained, the highest value reported so far for all-PSCs. The impressive photovoltaic performance originates from broad absorption range, reduced energy loss, and compact π-π stacking. These results provide new insight in the rational design of novel nonhalogenated polymer donors for further development of all-PSCs.
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All-polymer solar cells have experienced rapid development in recent years by the emergence of polymerized small molecular acceptors (PSMAs). However, the strong chain entanglements of polymer donors (PDs) and polymer acceptors (PAs) decrease the miscibility of the resulting polymer mixtures, making it challenging to optimize the blend morphology. Herein, we designed three PAs, namely PBTPICm-BDD, PBTPICγ-BDD and PBTPICF-BDD, by smartly using a BDD unit as the polymerized unit to copolymerize with different Y-typed non-fullerene small molecular acceptors (NF-SMAs), thus achieving a certain degree of distortion and giving the polymer system enough internal space to reduce the entanglements of the polymer chains. Such effects increase the chances of the PD being interspersed into the acceptor material, which improve the solubility between the PD and PA. The PBTPICγ-BDD and PBTPICF-BDD displayed better miscibility with PBQx-TCl, leading to a well optimized morphology. As a result, high power conversion efficiencies (PCEs) of 17.50 % and 17.17 % were achieved for PBQx-TCl : PBTPICγ-BDD and PBQx-TCl : PBTPICF-BDD devices, respectively. With the addition of PYFT-o as the third component into PBQx-TCl : PBTPICγ-BDD blend to further extend the absorption spectral coverage and finely tune microstructures of the blend morphology, a remarkable PCE of 18.64 % was realized finally.
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Morphological control of all-polymer blends is quintessential yet challenging in fabricating high-performance organic solar cells. Recently, solid additives (SAs) have been approved to be capable in tuning the morphology of polymer: small-molecule blends improving the performance and stability of devices. Herein, three perhalogenated thiophenes, which are 3,4-dibromo-2,5-diiodothiophene (SA-T1), 2,5-dibromo-3,4-diiodothiophene (SA-T2), and 2,3-dibromo-4,5-diiodothiophene (SA-T3), were adopted as SAs to optimize the performance of all-polymer organic solar cells (APSCs). For the blend of PM6 and PY-IT, benefitting from the intermolecular interactions between perhalogenated thiophenes and polymers, the molecular packing properties could be finely regulated after introducing these SAs. In situ UV/Vis measurement revealed that these SAs could assist morphological character evolution in the all-polymer blend, leading to their optimal morphologies. Compared to the as-cast device of PM6 : PY-IT, all SA-treated binary devices displayed enhanced power conversion efficiencies of 17.4-18.3 % with obviously elevated short-circuit current densities and fill factors. To our knowledge, the PCE of 18.3 % for SA-T1-treated binary ranks the highest among all binary APSCs to date. Meanwhile, the universality of SA-T1 in other all-polymer blends is demonstrated with unanimously improved device performance. This work provide a new pathway in realizing high-performance APSCs.
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A polymer acceptor, named PX-1, is designed and synthesized using a polymerization strategy with grafted small molecule acceptors. This design approach allows for the freedom of end groups while maintaining efficient terminal packing, enhancing π-π interactions, and facilitating charge transport. All-polymer organic solar cells based on PM6: PX-1 demonstrate a promising efficiency of 13.55%. The result presents an alternative pathway for the design of high-efficiency polymer acceptors through the careful regulation of small molecule acceptor monomers and linker units.
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Bandagens , Polímeros , PolimerizaçãoRESUMO
The power conversion efficiency (PCE) of all-polymer solar cells (all-PSCs) has ascended rapidly arising from the development of polymerized small-molecule acceptor materials. However, numerous insulating long alkyl chains, which ensure the solubility of the polymer, result in inferior aggregation and charge mobility. Herein, this study proposes a facile random copolymerization strategy of two small molecule acceptor units with different lengths of alkyl side chains and synthesizes a series of polymer acceptors PYT-EHx, where x is the percentage of the short alkyl chain units. The aggregation strength and charge mobility of the acceptors rise linearly with increasing the proportion of short alkyl chain units. Thus, the PYT-EH20 reaches balanced aggregation with the star polymer donor PBDB-T, resulting in optimal morphology, fastest carrier transport, and reduced recombination and energy loss. Consequently, the PYT-EH20-based device yields a 14.8% PCE, a 16% improvement over the control PYT-EH0-based device, accompanied by an increase in open-circuit voltage (Voc ), short-circuit current density (Jsc ), and fill factor (FF). This work demonstrates that the random copolymerization strategy with short alkyl chain insertion is an effective avenue for developing high-performance polymer acceptors, which facilitates further advances in the efficiency of all-PSCs.
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Polímeros , Polimerização , SolubilidadeRESUMO
Currently, most of the disclosed ternary strategies to improve photovoltaic performance of all-polymer solar cells (all-PSCs) commonly focus on the guest polymers having similar structures with the host polymer donors or acceptors. Herein, this work develops a distinctive ternary method that adding an amorphous BâN embedded polymer named BN-Cl-2fT to a crystallized host polymer blend of PM6 (a commercialized polymer donor) and PY-TT (a copolymer of Y6 and thieno[3,2-b]thiophene). Although the structures between BN-Cl-2fT and PM6 and PY-TT are completely different, excellent miscibility is found between BN-Cl-2fT and both of the host PM6 and PY-TT, which can be interpreted by the crowded phenyl groups anchoring along the backbone of BN-Cl-2fT, leading to weak self-aggregation. Glazing incidence wide-angle X-ray diffraction (GIWAXS) measurements explicitly confirm the crystallization of PM6 and PY-TT and amorphous feature of BN-Cl-2fT. Furthermore, adding 10 wt% BN-Cl-2fT to PM6:PY-TT can significantly enhance the crystallization of the host polymers. Thus the ternary devices based on PM6:PY-TT:BN-Cl-2fT afford promote short-circuit current density (JSC , 23.29 vs. 21.80 mA cm-2 ), fill factor (FF, 62.4% vs. 60.0%), and power conversion efficiency (PCE, 13.70% vs. 12.23%) in contrast to these parameters of binary devices based on PM6:PY-TT. This work provides a unique and enlightening avenue to design high performance all-PSCs by adding amorphous BâN embedded polymers as guest component to enhance host-crystallization.
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Polímeros , Tiofenos , Cristalização , Difração de Raios XRESUMO
Developing robust materials is very critical and faces a big challenge for high-performance large-area all-polymer solar cells (all-PSCs) by printing methods. Herein, the authors combine the advantages of the terpolymerization strategy with the non-conjugated backbone strategy to regulate the molecular aggregation rationally during the film-forming printing process, facilitating a facile printing process for large-area all-PSCs. A series of terpolymer acceptors PYSe-Clx (x = 0, 10, 20, and 30) is also developed, which can effectively fine-tune the morphology and photoelectric properties of the active layer. The PBDB-T: PYSe-Cl20-based all-PSC delivers a significantly improved power cconversion efficiency (PCE) than the one with PBDB-T: PYSe (14.21% vs 12.45%). By addition of a small amount of non-conjugated polymer acceptor PTClo-Y, the ternary all-PSC reaches a PCE of 15.26%. More importantly, the regulation of molecular aggregation enables a facile blade-coating process of the large-area device. A record PCE of 13.81% for large-area devices (1.21 cm2 ) is obtained, which is the highest value for large-area all-PSCs fabricated by blade-coating. The environmentally friendly solvent processed large-area device also obtains an excellent performance of 13.21%. This work provides a simple and effective molecular design strategy of robust materials for high-performance large-area all-PSCs by a printing process.
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All-polymer solar cells (all-PSCs) have attracted considerable attention owing to their pronounced advantages of excellent mechanical flexibility/stretchability and greatly enhanced device stability as compared to other types of organic solar cells (OSCs). Thanks to the extensive research efforts dedicated to the development of polymer acceptors, all-PSCs have achieved remarkable improvement of photovoltaic performance, recently. This review summarizes the recent progress of polymer acceptors based on the key electron-deficient building blocks, which include bithiophene imide (BTI) derivatives, boron-nitrogen coordination bond (BâN)-incorporated (hetero)arenes, cyano-functionalized (hetero)arenes, and fused-ring electron acceptors (FREAs). In addition, single-component-based all-PSCs are also briefly discussed. The structure-property correlations of polymer acceptors are elaborated in detail. Finally, we offer our insights into the development of new electron-deficient building blocks with further optimized properties and the polymers built from them for efficient all-PSCs.
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Recently, the strategy of polymerized small-molecule acceptors (PSMAs) has attracted extensive attention for applications in all-polymer solar cells (all-PSCs). Although side-chain engineering is considered as a simple and effective strategy for manipulating polymer properties, the corresponding effect on photovoltaic performance of PSMAs in all-PSCs has not been systemically investigated. Herein, a series of PSMAs based on the benzotriazole (BTz)-core fused SMAs with different N-alkyl chains including branched 2-butyloctyl, linear n-octyl, and methyl on the BTz unit, namely PZT-C12, PZT-C8, and PZT-C1, respectively, is presented. Comparative studies show that the size of alkyl chains has a significant impact on the solid-state behavior of PZT polymers, which in turn affects their light absorption and charge transporting capacities, and subsequently the all-PSC performances. When combining with the polymer donor PBDB-T, PZT-C1 affords a champion power conversion efficiency of 14.9%, compared to 13.1% of PZT-C12, and 13.8% of PZT-C8 in the resultant all-PSCs, mainly benefiting from its better crystallinity and the more favorable blend morphology. This work emphasizes the importance of optimizing side-chain substituents on PSMAs for improving the device efficiency of all-PSCs.
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All-polymer solar cells (all-PSCs) are one of the most promising application-oriented organic photovoltaic technologies due to their excellent operational and mechanical stability. However, the power conversion efficiencies (PCEs) are mostly lower than 16%, restricting their core competitiveness. Furthermore, the improvement of mechanical durability is rarely paid attention to cutting-edge all-PSCs. This work deploys a low-cost "technical grade" PCBM (incompletely separated but pure mixtures containing ≥90% [70]PCBM or [60]PCBM), into the efficient PM6:PY-IT all-polymer blend, successfully yielding a high-performance ternary device with 16.16% PCE, among the highest PCE values for all-PSCs. Meanwhile, an excellent mechanical property (i.e., crack onset strain = 11.1%) promoted from 9.5% for the ternary system is also demonstrated. The "technical grade" PCBM slightly disrupts the crystallization of polymers, and disperses well into the amorphous polymer regions of the all-PSC blends, thus facilitating charge transport and improving film ductility simultaneously. All these results confirm introducing low-cost "technical grade" PCBM with high electron mobility into all-polymer blends can improve carrier mobility, reduce charge recombination, and optimize morphology of the amorphous polymer regions, thus yielding more efficient and mechanically durable all-PSCs.
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Developing organic solar cells based on a ternary active layer is one of the most effective approaches to improve their photovoltaic performance. However, limited success has been achieved in all-polymer solar cells (all-PSCs). In this study, a ternary all-PSC with improved efficiency and stability is realized by using J71 as the third component to adjust the host system of PBDB-T:PG1. The deeper highest occupied molecular orbital (HOMO) energy level of J71 downshifts the mixed HOMO energy levels of donors. The two polymer donors (PD s) have good miscibility and present Förster resonance energy transfer. When blended with PG1, the optimized morphology is obtained, showing enhanced crystallinity but meanwhile slightly reduced phase separation with improved exciton dissociation and collection efficiency, suppressed charge recombination, and reduced energy loss (0.55 eV). Combining the benefits mentioned above, the ternary all-PSC exhibits an excellent efficiency of 12.8% with simultaneously elevated open-circuit voltage (0.96 V), short-circuit current density (18.4 mA cm-2 ), and fill factor (72.2%). Moreover, the optimized ternary all-PSC shows improved storage and thermal stability. This study demonstrates that the utilization of a ternary all-polymer system based on two well-miscible PD s is an effective strategy to enhance the photovoltaic performance and stability of all-PSCs.
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Currently, rational design of polymer acceptors is desirable but there is still a challenge to develop high-performance all-polymer solar cells (all-PSCs). In this work, brominated thienyl-fused malononitrile-based monomer is employed to copolymerize with indacenodithiophene (IDT) and benzodithiophene (BDT)-based linking units to develop two polymerized small molecule acceptors (PSMAs) PIDT and PBDT, respectively, for all-PSCs. The two PSMAs show similar absorption edges, while PBDT shows a slightly higher lowest unoccupied molecular orbital (LUMO) energy level than PIDT. Benefitted from the relatively high LUMO levels of the two polymer acceptors, notable open-circuit voltage (Voc ) values over 1.0 V are achieved when using them as acceptor to blend with PTQ10 as polymer donor. Particularly, the all-PSC based on PTQ10:PIDT demonstrates a power conversion efficiency of 10.19%, with an outstanding Voc of 1.10 V benefitted from the higher LUMO energy level of PIDT acceptor. The results demonstrate a feasible strategy to design PSMAs by selecting appropriate linking units for increasing the Voc and improving the efficiency of all-PSCs.
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All-polymer solar cells (All-PSCs), whose electron donor and acceptors are both polymeric materials, have attracted great research attention in the past few years. However, most all-PSC devices with top-of-the-line efficiencies are processed from chloroform. In this work, we apply the sequential processing (SqP) method to fabricate All-PSCs from an aromatic hydrocarbon solvent, toluene, and obtain efficiencies up to 17.0%. By conducting a series of characterizations on our films and devices, we demonstrate that the preparation of SqP devices using toluene can effectively reduce carrier recombination, enhance carrier mobility and promote the fill factor of the device.
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Conjugated molecules and polymers with intrinsic quinoidal structure are promising n-type organic semiconductors, which have been reported for application in field-effect transistors and thermoelectric devices. In principle, the molecular and electronic characteristics of quinoidal polymers can also enable their application in organic solar cells. Herein, two quinoidal polymers, named PzDP-T and PzDP-ffT, based on dipyrrolopyrazinedione were synthesized and used as electron acceptors in all-polymer solar cells (all-PSCs). Both PzDP-T and PzDP-ffT showed suitable energy levels and wide light absorption range that extended to the near-infrared region. When combined with the polymer donor PBDB-T, the resulting all-PSCs based on PzDP-T and PzDP-ffT exhibited a power conversion efficiency (PCE) of 1.33 and 2.37 %, respectively. This is the first report on the application of intrinsic quinoidal conjugated polymers in all-PSCs. The photovoltaic performance of the all-PSCs was revealed to be mainly limited by the relatively poor and imbalanced charge transport, considerable charge recombination. Detailed investigations on the structure-performance relationship suggested that synergistic optimization of light absorption, energy levels, and charge transport properties is needed to achieve more successful application of intrinsic quinoidal conjugated polymers in all-PSCs.
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All-polymer solar cells (all-PSCs) have drawn tremendous research interest in recent years, due to their inherent advantages of good film formation, stable morphology, and mechanical flexibility. The most representative and most widely used n-CP acceptor was the naphthalene diimide based D-A copolymer N2200 before 2017, and the power conversion efficiency (PCE) of the all-PSCs based on N2200 reached over 8% in 2016. However, the low absorption coefficient of N2200 in the near-infrared (NIR) region limits the further increase of its PCE. In 2017, we proposed a strategy of polymerizing small-molecule acceptors (SMAs) to construct new-generation polymer acceptors. The polymerized SMAs (PSMAs) possess low band gap and strong absorption in the NIR region, which attracted great attention and drove the PCE of the all-PSCs to over 15% recently. In this Minireview we explain the design strategies of the molecular structure of PSMAs and describe recent research progress. Finally, current challenges and future prospects of the PSMAs are analyzed and discussed.
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Polymerization sites of small molecule acceptors (SMAs) play vital roles in determining device performance of all-polymer solar cells (all-PSCs). Different from our recent work about fluoro- and bromo- co-modified end group of IC-FBr (a mixture of IC-FBr1 and IC-FBr2), in this paper, we synthesized and purified two regiospecific fluoro- and bromo- substituted end groups (IC-FBr-o & IC-FBr-m), which were then employed to construct two regio-regular polymer acceptors named PYF-T-o and PYF-T-m, respectively. In comparison with its isomeric counterparts named PYF-T-m with different conjugated coupling sites, PYF-T-o exhibits stronger and bathochromic absorption to achieve better photon harvesting. Meanwhile, PYF-T-o adopts more ordered inter-chain packing and suitable phase separation after blending with the donor polymer PM6, which resulted in suppressed charge recombination and efficient charge transport. Strikingly, we observed a dramatic performance difference between the two isomeric polymer acceptors PYF-T-o and PYF-T-m. While devices based on PM6:PYF-T-o can yield power conversion efficiency (PCE) of 15.2 %, devices based on PM6:PYF-T-m only show poor efficiencies of 1.4 %. This work demonstrates the success of configuration-unique fluorinated end groups in designing high-performance regular polymer acceptors, which provides guidelines towards developing all-PSCs with better efficiencies.
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All-polymer solar cells (all-PSCs) progressed tremendously due to recent advances in polymerized small molecule acceptors (PSMAs), and their power conversion efficiencies (PCEs) have exceeded 15 %. However, the practical applications of all-PSCs are still restricted by a lack of PSMAs with a broad absorption, high electron mobility, low energy loss, and good batch-to-batch reproducibility. A multi-selenophene-containing PSMA, PFY-3Se, was developed based on a selenophene-fused SMA framework and a selenophene π-spacer. Compared to its thiophene analogue PFY-0Se, PFY-3Se shows a ≈30â nm red-shifted absorption, increased electron mobility, and improved intermolecular interaction. In all-PSCs, PFY-3Se achieved an impressive PCE of 15.1 % with both high short-circuit current density of 23.6â mA cm-2 and high fill factor of 0.737, and a low energy loss, which are among the best values in all-PSCs reported to date and much better than PFY-0Se (PCE=13.0 %). Notably, PFY-3Se maintains similarly good batch-to-batch properties for realizing reproducible device performance, which is the first reported and also very rare for the PSMAs. Moreover, the PFY-3Se-based all-PSCs show low dependence of PCE on device area (0.045-1.0â cm2 ) and active layer thickness (110-250â nm), indicating the great potential toward practical applications.
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A new polymer acceptor poly{(N,N'-bis(2-ethylhexyl)-1,4,5,8-naphthalenedicarboximide-2,6-diyl)-alt-5,5-(3,3'-didodecyl-2,2'-bifuran)} (NDI-BFR) made from naphthalenediimide (NDI) and furan-derived head-to-head-linked 3,3'-dialkyl-2,2'-bifuran (BFR) units is reported in this study. Compared to the benchmark polymer poly(naphthalenediimide-alt-bithiophene) (N2200), NDI-BFR exhibits a larger bathochromic shift of absorption maxima (842 nm) with a much higher absorption coefficient (7.2 × 104 m-1 cm-1 ), leading to an ultranarrow optical bandgap of 1.26 eV. Such properties ensure good harvesting of solar light from visible to the near-infrared region in solar cells. Density functional theory calculation reveals that the polymer acceptor NDI-BFR possesses a higher degree of backbone planarity versus the polymer N2200. The polymer NDI-BFR exhibits a decent electron mobility of 0.45 cm2 V-1 s-1 in organic thin-film transistors (OTFTs), and NDI-BFR-based all-polymer solar cells (all-PSCs) achieve a power conversion efficiency (PCE) of 4.39% with a very small energy loss of 0.45 eV by using the environmentally friendly solvent 1,2,4-trimethylbenzene. These results demonstrate that incorporating head-to-head-linked BFR units in the polymer backbone can lead to increased planarity of the polymer backbone, reduced optical bandgap, and improved light absorbing. The study offers useful guidelines for constructing n-type polymers with narrow optical bandgaps.