Regulating Phase Separation Kinetics for High-Efficiency and Mechanically Robust All-Polymer Solar Cells

All-polymer solar cells (all-PSCs) possess excellent operation stability and mechanical robustness than other types of organic solar cells, thereby attracting considerable attention for wearable flexible electron devices. However, the power conversion efficiencies (PCEs) of all-PSCs are still lagging behind those of small-molecule-acceptor-based systems owing to the limitation of photoactive materials and unsatisfactory blend morphology. In this work, a novel terpolymer, denoted as PBDB-TFCl (poly4,8-bis(5-(2-ethylhexyl)-4-fluorothiophen-2-yl)benzo[1,2-b:4,5-b '']dithiophene-1,3-bis(2-ethylhexyl)-5,7-di(thiophen-2-yl)-4H,8H-benzo[1,2-c:4,5-c '']dithiophene-4,8-dione-4,8-bis(4-chloro-5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b ']dithiophene), is used as an electron donor coupled with a ternary strategy to optimize the performance of all-PSCs. The addition of PBDB-TCl unit deepens the highest occupied molecular orbital energy level, reducing voltage losses. Moreover, the introduction of the guest donor (D18-Cl) effectively regulates the phase-transition kinetics of PBDB-TFCl:D18-Cl:PY-IT during the film formation, leading to ideal size of aggregations and enhanced crystallinity. PBDB-TFCl:D18-Cl:PY-IT devices exhibit a PCE of 18.6% (certified as 18.3%), judged as the highest value so far obtained with all-PSCs. Besides, based on the ternary active layer, the manufactured 36 cm2 flexible modules exhibit a PCE of 15.1%. Meanwhile, the ternary PSCs exhibit superior photostability and mechanical stability. In summary, the proposed strategy, based on molecular design and the ternary strategy, allows optimization of the all-polymer blend morphology and improvement of the photovoltaic performance for stable large-scale flexible PSCs. By synthesizing a random terpolymer PBDB-TFCl and combining a ternary blending strategy, favorable phase separation and reinforced molecular packing are obtained. Resulting flexible organic solar modules exhibit maximum power conversion efficiency of 12.7% and excellent mechanical properties and photostability.image

Automated summary

In this study, a novel terpolymer (PBDB-TFCl) was used as an electron donor in all-polymer solar cells (all-PSCs) to optimize their performance. The addition of PBDB-TCl unit and the introduction of a guest donor helped improve the blend morphology and crystallinity, resulting in high power conversion efficiencies (PCEs) of 18.6% for PBDB-TFCl:D18-Cl:PY-IT devices and 15.1% for flexible modules. These ternary PSCs also exhibited superior photostability and mechanical stability.