Cyanoesterthiophene Based Low‐Cost Polymer Donors for High Efficiency Organic Solar Cells

To achieve commercial application of organic solar cells (OSCs), it is necessary to reduce material costs and improve device efficiency. This paper reports on the utilization of a multifunctional building block, namely 3‐cyanoesterthiophene, which exhibits simple structure and accessibility of synthetic for cost‐effective and high‐performance polymer donors (PDs). Meanwhile, ternary and terpolymerization strategies have been studied. Two similar PDs, PBTCl0‐TCA and PBTCl100‐TCA, are synthesized, and the devices exhibit less‐than‐satisfactory efficiency of 13.21% and 11.53% due to mismatching energy level and imperfect morphology. The two PDs with comparable structures and commendable compatibility easily form alloy‐like phase in active layer, which can effectively boost the efficiency of ternary devices to 14.17% with retained high JSC and significant improved open‐circuit voltage (VOC) and fill factor (FF). Encouraged by the ternary blending phenomenon, a polymer donor (PBTCl50‐TCA) with same ratio by random terpolymerization is designed. And over 17% efficiency binary OSCs using terpolymerization donor are demonstrated. The synergies of incorporation of the cyanoester‐group and terpolymer endow the developed PDs with deep‐lying energy levels, face‐on orientation, thermodynamic miscibility with the prevailing nonfullerene acceptor and appropriate polymer crystallinity. The findings study provide valuable insights and support for the advancement of cost‐effective and high‐performance PDs. Cost‐effective organic solar cells (OSCs) with low‐cost materials and high‐performance are critical to commercialization. Herein, based on synthesized easily cyanoesterthiophene group and easy‐adjusting random terpolymerization, a new polymer donor with 17.14% efficiency is reported, which is fully comparable with the currently polymer donor. This study not only reveals the impact of copolymerization and blending strategies on performance, but also provides valuable insights into applications in practical production.