Owing to the defined structure and large molecular size, giant molecular acceptors (GMAs) have exerted significant progress in device efficiencies and stability in organic solar cells. Differing from the classical synthesis of GMAs by Stille coupling which still suffers from high cost and lack of environmental sustainability, this work develops three GMAs via metal-free catalyzed reactions. By introducing varying quantities of malononitrile groups into the linker, the optoelectronic properties of GMAs are significantly regulated. The GMA containing only one malononitrile in the central linker unit, exhibits a favorable absorption range, energy levels, and molecular packing, consequently achieving a high efficiency and stability. Thereby, this work provides a feasible approach to develop low-cost and scalable GMAs.

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