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Origin of the High Donor-Acceptor Composition Tolerance in Device Performance and Mechanical Robustness of All-Polymer Solar Cells
摘要： High tolerance regarding photovoltaic performance in terms of donor:acceptor (D:A) composition ratio is reported for all-polymer solar cells (all-PSCs), which is a crucial advantage in producing large-scale devices with high reproducibility. To understand the origin of high D:A ratio tolerance in all-PSCs, we investigate the molecular weight (MW) effects of the P(NDI2OD-T2) polymer acceptor (PA) on photovoltaic and mechanical robustness of PBDB-T:P(NDI2OD-T2) all-PSCs. Also, we compare the all-PSCs with other types of PSCs consisting of the same polymer donor but using small molecule acceptors (SMAs) including ITIC and PC71BM. It is observed that the D:A ratio tolerances of both the photovoltaic and mechanical properties are highly dependent on the PA MW and the acceptor material types. For example, at a high D:A ratio of 15:1, all-PSCs using high MW PA (number-average molecular weight (Mn)= 97 kg mol-1) exhibit 13 times higher normalized power conversion efficiency (PCE) than all-PSCs using low MW PA (Mn= 11 kg mol-1), and 20 times higher than ITIC-based PSCs. In addition, the electron mobilities in all-PSCs based on high MW PA are well maintained even at very high D:A ratio, whereas the electron mobilities in low MW PA all-PSCs and SMA-based PSCs decrease by 3- and 4-orders of magnitude, respectively, when the D:A ratio increases from 1:1 to 15:1. Thus, we suggest that the formation of tie molecules and chain entanglements by long polymer chains bridging adjacent crystalline domains is the main origin of excellent D:A tolerance in both mechanical robustness and photovoltaic performance. This work provides an important material design guideline for the reproducible production of flexible and stretchable all-PSCs.
关键词： molecular weight effects,mechanical robustness,donor-acceptor composition tolerance,photovoltaic performance,all-polymer solar cells
更新于2025-09-12 10:27:22
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Understanding the Impact of Side-chain on Photovoltaic Performance in Efficient All-polymer Solar Cells
摘要： In order to understand the impact of side-chain on photovoltaic performance and explore efficient All-polymer solar cells, chemical modifications on donor-acceptor based polymers containing benzo[1,2-b:4,5-b’]dithiophene (BDT) and thieno[3,4-c]pyrrole-4,6-dione (TPD) backbones were performed. Via side-chain fluorination, the molecular design resulted in lower highest occupied molecular orbital (HOMO) energy levels and enhanced backbone planarity. The intermolecular packing and solid-state ordering were found to significantly improve. These factors are considered as key influences for carrier transport. In contrast, introducing a bulky alkylthio substituent group was found to slightly distort the polymer backbone. As a result of the lower HOMO level, PTF8 exhibits an improved open circuit voltage (Voc) compared to the template polymer PT8. However, due to the increased crystallinity and aggregation, PTF8 and PTS8 experience an unfavorable phase separation in polymer-polymer bulk heterojunction blends, hindering the PCE to about 4%. Through introducing alkylthio side-chains and fluorination, the polymer PTFS8 exhibits an extremely low HOMO level (-5.73 eV). These reduced HOMO level limits charge separation between the donor and acceptor polymers. Without any fluorination and alkylthio side-chains, the wide bandgap polymer PT8 exhibits desired HOMO energy levels and crystallinity, delivering a best PCE of 8% together with a high Voc of 1.05 V, displaying its great potential for applications in efficient all-polymer optoelectronic devices.
关键词： BDT-TPD backbone,side-chain,fluorination,All-polymer solar cells,alkylthio substitution,photovoltaic performance
更新于2025-09-12 10:27:22
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Improved Morphology and Interfacial Contact of PBDB-T:N2200-Based All-Polymer Solar Cells by Using the Solvent Additive p-anisaldehyde
摘要： All-polymer solar cells (all-PSCs) have been intensively investigated due to their excellent thermal and mechanical stabilities. However, the efficiency of all-PSCs is still far behind that of organic solar cells (OSCs), which are based on small molecule acceptors. Improving the efficiency of all-PSCs is of great urgency. In this work, the solvent additive named p-anisaldehyde (AA) was introduced to improve the performance of all-PSCs based on PBDB-T:N2200. It is demonstrated that AA helps to form a better network interpenetrating track and more uniform phase separation. With the assistance of AA, which has both an oleophilic methoxy group and a hydrophilic aldehyde group, the interfacial contact between the donor and the acceptor (D/A) is improved, increasing the contact area at D/A, and promoting efficient exciton dissociation. More importantly, AA acts as a "bridge" between the oleophilic active layer and the hydrophilic PEDOT:PSS layer, improving the interfacial compatibility between the active layer and the PEDOT:PSS layer, reducing the interfacial resistance, and facilitating the carrier transport. Finally, the all-PSCs based on PBDB-T:N2200 exhibits a superior power conversion efficiency (PCE) of 7.24% which is a record efficiency for the current all-PSCs with the same architecture. In this work, a promising and effective strategy for achieving high efficiency all-PSCs is provided.
关键词： additive,p-anisaldehyde,interfacial compatibility,interfacial contact,all-polymer solar cells
更新于2025-09-12 10:27:22
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A Narrow-Bandgap n-Type Polymer Semiconductor Enabling Efficient All-Polymer Solar Cells
摘要： Currently, n-type acceptors in high-performance all-polymer solar cells (all-PSCs) are dominated by imide-functionalized polymers, which typically show medium bandgap. Herein, a novel narrow-bandgap polymer, poly(5,6-dicyano-2,1,3-benzothiadiazole-alt-indacenodithiophene) (DCNBT-IDT), based on dicyanobenzothiadiazole without an imide group is reported. The strong electron-withdrawing cyano functionality enables DCNBT-IDT with n-type character and, more importantly, alleviates the steric hindrance associated with typical imide groups. Compared to the benchmark poly(naphthalene diimide-alt-bithiophene) (N2200), DCNBT-IDT shows a narrower bandgap (1.43 eV) with a much higher absorption coefficient (6.15 × 104 cm?1). Such properties are elusive for polymer acceptors to date, eradicating the drawbacks inherited in N2200 and other high-performance polymer acceptors. When blended with a wide-bandgap polymer donor, the DCNBT-IDT-based all-PSCs achieve a remarkable power conversion efficiency of 8.32% with a small energy loss of 0.53 eV and a photoresponse of up to 870 nm. Such efficiency greatly outperforms those of N2200 (6.13%) and the naphthalene diimide (NDI)-based analog NDI-IDT (2.19%). This work breaks the long-standing bottlenecks limiting materials innovation of n-type polymers, which paves a new avenue for developing polymer acceptors with improved optoelectronic properties and heralds a brighter future of all-PSCs.
关键词： polymer acceptors,high absorption coefficient,dicyanobenzothiadiazole,narrow bandgap,all-polymer solar cells
更新于2025-09-11 14:15:04
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Amorphous Polymer Acceptor Containing B ← N Units Matches Various Polymer Donors for All-Polymer Solar Cells
摘要： Polymer acceptors for high-efficiency all-polymer solar cells (all-PSCs) are generally semicrystalline. In this manuscript, we report an amorphous polymer acceptor, which matches well with a variety of polymer donors to produce efficient all-PSCs. The amorphous polymer acceptor (rr-PBN) is a regiorandom polymer consisting of alternating asymmetric B←N bridged thienylthiazole (BNTT) unit and pyridine-flanked diketopyrrolopyrrole (PyDPP) unit. It is amorphous in thin film because of its regiorandom structure and the large steric hindrance. rr-PBN shows deep LUMO/HOMO energy levels of ?3.71/?5.81 eV, strong sunlight harvesting capability and high electron mobility of 2.20 × 10?4 cm2 V?1 s?1. As a polymer acceptor, rr-PBN matches well with three commercially available polymer donors, J71, PTB7-Th, and PffBT4T-2OD to give excellent percolating bicontinuous network morphology in all-PSCs. We propose that the crystallization of polymer donors governs the film-forming process and dominates the phase separation morphology, leading to good phase separation morphology. The all-PSC devices all show power conversion efficiencies (PCEs) of 5.2?6.6%. This study provides a new direction to design polymer acceptors and a novel approach to control phase separation morphology of all-PSCs.
关键词： all-polymer solar cells,phase separation morphology,B←N units,amorphous polymer acceptor,power conversion efficiencies
更新于2025-09-11 14:15:04
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Fine-Tuning Semiconducting Polymer Self-Aggregation and Crystallinity Enables Optimal Morphology and High-Performance Printed All-Polymer Solar Cells
摘要： Polymer aggregation and crystallization behavior play a crucial role in the performance of all-polymer solar cells (all-PSCs). Gaining control over polymer self-assembly via molecular design to influence bulk-heterojunction active-layer morphology, however, remains challenging. Herein, we show a simple yet effective way to modulate the self-aggregation of the commonly used naphthalene diimide (NDI)-based acceptor polymer (N2200), by systematically replacing a certain amount of alkyl side-chains with compact bulky side-chains (CBS). Specifically, we have synthesized a series of random co-polymer (PNDI-CBSx) with different molar fractions (x = 0–1) of the CBS units and have found that both solution-phase aggregation and solid-state crystallinity of these acceptor polymers are progressively suppressed with increasing x as evidenced by UV-Vis absorption, photoluminescence (PL) spectroscopies, thermal analysis and grazing incidence X-ray scattering (GIWAXS) techniques. Importantly, compared to the highly self-aggregating N2200, photovoltaic results show that blending of more amorphous acceptor polymers with donor polymer (PBDB-T) can enable all-PSCs with significantly increased PCE (up to 8.5%). The higher short-circuit current density (Jsc) results from the smaller polymer phase-separation domain sizes as evidenced by PL quenching and resonant soft X-ray scattering (R-SoXS) analyses. Additionally, we show that the lower crystallinity of the active layer is less sensitive to the film deposition methods. Thus, the transition from spin-coating to solution coating can be easily achieved with no performance losses. On the other hand, decreasing aggregation and crystallinity of the acceptor polymer too much, reduces the photovoltaic performance as the donor phase-separation domain sizes increases. The highly amorphous acceptor polymers appear to induce formation of larger donor polymer crystallites. These results highlight the importance of a balanced aggregation strength between the donor and acceptor polymers to achieve high-performance all-PSCs with optimal active layer film-morphology.
关键词： morphology control,crystallinity,polymer aggregation,naphthalene diimide,all-polymer solar cells
更新于2025-09-11 14:15:04
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Surpassing the 10% efficiency milestone for 1-cm2 all-polymer solar cells
摘要： Naphthalenediimide-based n-type polymeric semiconductors are extensively used for constructing high-performance all-polymer solar cells (all-PSCs). For such all-polymer systems, charge recombination can be reduced by using thinner active layers, yet suffering insufficient near-infrared light harvesting from the polymeric acceptor. Conversely, increasing the layer thickness overcomes the light harvesting issue, but at the cost of severe charge recombination effects. Here we demonstrate that to manage light propagation within all-PSCs, a thick bulk-heterojunction film of approximately 350 nm is needed to effectively enhance photo-harvesting in the near-infrared region. To overcome the severe charge recombination in such a thick film, a non-halogenic additive is used to induce a well-ordered micro-structure that inherently suppresses recombination loss. The combined strategies of light management and delicate morphology optimization lead to a promising efficiency over 10% for thick-film all-PSCs with active area of 1 cm2, showing great promise for future large-scale production and application of all-PSCs.
关键词： all-polymer solar cells,light management,naphthalenediimide,thick-film,morphology optimization
更新于2025-09-11 14:15:04
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Optimizing domain size and phase purity in all-polymer solar cells by solution order aggregation and confinement effect of the acceptor
摘要： Domain size, phase purity, and the interpenetrating network within the active layer of all-polymer solar cells (all-PSCs) are crucial for efficient charge generation and carrier transport. However, it is a great challenge to decrease domain size and enhance phase purity simultaneously because of the energetically disfavoring polymer-polymer mixing and chain entanglement. In this work, we manipulated the domain size and phase purity of J51:N2200 blends by promoting their solution ordered aggregation and the confinement of acceptor N2200 to J51 during phase separation. Thus, three solvents, chloroform (CF), mesitylene (Mes), and cyclopentyl methyl ether (CPME) were selected. The solubility of J51 and N2200 in these three solvents decreases solubility differences between J51 and N2200 increases gradually. Among these three solvents, only in CPME solution, N2200 possesses ordered structures, which reduces nucleation barrier to increase nucleation density and boosts template effect of N2200. During phase separation, the ordered aggregation of N2200 dominates solid-liquid phase separation and has the confinement effect of J51. Thus, the blend films cast from CPME have fine-scale phase separation in contrast to the films from CF. In addition, the "memory" effect of ordered aggregations transferred to films can enforce the order of blend films. As a result, the blend film with small domain size (≈21 nm), interpenetrating network structure, and a higher degree of crystallinity was obtained by processed from green solvent CPME. The improved morphology facilitated charge-generating process and carrier transport, resulting in higher short-circuit current (Jsc), fill factor (FF), and the power conversion efficiency (PCE).
关键词： all-polymer solar cells,domain size,phase purity,solution ordered aggregation,confinement effect
更新于2025-09-11 14:15:04
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Small Band gap Boron Dipyrromethene-Based Conjugated Polymers for All-Polymer Solar Cells: The Effect of Methyl Units
摘要： Naphthalene diimide (NDI)-based conjugated polymers have been widely used as the nonfullerene electron acceptor for all-polymer solar cells (all-PSCs), but their low absorption coefficient in the near-infrared (NIR) region severely limits the light harvesting ability in solar cells and hence lowers their photovoltaic performance. In this work, two narrow band gap donor?acceptor conjugated polymers based on boron dipyrromethene (BODIPY) as the electron-deficient unit were developed as the electron donor to combine with a NDI-polymer acceptor in order to significantly improve the photoresponse in the NIR region. More importantly, we found that methyl substitution on the BODIPY segment played an important role in charge transport in these polymers. When methyl units were attached to the α-position of BODIPY, the polymer PMBBDT exhibited high-lying energy levels, improved crystallinity, and dramatically high hole mobility compared to the polymer PBBDT without methyl substitution. Consequently, the power conversion efficiencies (PCEs) could be enhanced from 0.32% for PBBDT- to 5.8% for PMBBDT-based all-PSCs, and the photoresponse covered from 300 to 900 nm. Our results demonstrate that methyl-substituted BODIPY-based conjugated polymers are promising candidates to solve the NIR absorption issue in NDI polymers and, therefore, can be potentially used to further boost the PCEs of all-PSCs similar with organic solar cells based on NIR-fused ring electron acceptors.
关键词： Boron dipyrromethene,Methyl substitution,Conjugated polymers,Near-infrared absorption,All-polymer solar cells
更新于2025-09-11 14:15:04
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Toxic Solvent‐ and Additive‐Free Efficient All‐Polymer Solar Cells via a Simple Random Sequence Strategy in Both Donor and Acceptor Copolymer Backbones
摘要： It is extremely important to develop nontoxic solvent and additive-processed high-performance all-polymer solar cells (all-PSCs) that are suitable for printing preparation of large-scale devices. Herein, it is demonstrates that a simple random copolymerization of two acceptor monomers (benzo[1,2-c:4,5-c′]dithiophene-4,8-dione (BDD) and 5,6-difluoro-2H-benzo[d][1,2,3] triazole (FTAZ)), alternating with Si atom-containing benzo[1,2-b:4,5-b′] dithiophene donor comonomer, forms a successful approach by which to synthesize donor copolymers with excellent solubility/processability for nontoxic-solvent-processed all-PSCs. The incorporation of a higher degree of BDD in the backbone lowers the frontier energy levels, as well as redshifts, with higher absorption coefficients; however, it adversely affects solubility in a 2-methyltetrahydrofuran (MeTHF). An impressive power conversion efficiency, of about 8.0%, is achieved from PJ25 (25 mol% BDD)-based all-PSC when paired with N2200-F30 acceptor random copolymer by using MeTHF as the processing solvent without any additive. Another interesting point is that the air stability of the all-PSCs increases with increasing FTAZ content due to strong noncovalent interaction and resistance to humidity and oxidation caused by the F-atoms in FTAZ units. Not only does this study establish a structure–property–performance relationship through a series of structural, morphological, and electrical characterization techniques, but it also provides a promising and easy way to develop nontoxic-solvent-processed high-performance all-PSCs.
关键词： compatibility,nontoxic solvents,random copolymers,additive-free processing,all-polymer solar cells
更新于2025-09-11 14:15:04