Synergistically flexible-robust effects mediate the dynamic reconfiguration of perylene diimide polymer to enhance piezo-photocatalytic nitrate reduction

Identifying the spatial dynamic reconstruction of π-conjugated polymers for efficient carrier transport and controlling the intermediate process of the reaction are urgent and formidable challenges. In this study, a fresh perspective has emerged proposing to synergistically enhance the adaptability and resilience of dynamic torsion patterns in π-conjugated polymers to mediate charge separation and molecular activation. Excitingly, the highest flexible-robust structure and polarity of naphthalene-linked perylene diimide polymer (N-PDA) demonstrates a highest nitrate reduction rate of 5.36 mmol g h under light irradiation and ultrasonic condition, which is 7.5 times that of H-PDA. Theoretical calculations and experimental observations indicate that the strongest flexible-robust structure of N-PDA enhances the inclination of the rigid plane and atomic bond length, resulting in an accelerated uneven distribution of charges, molecular polarity, and electronic coupling to facilitate charge separation dynamics. Moreover, it exposes active sites that promote the adsorption and activation of NO ions while simultaneously regulating intermediate hydrogenation processes. Our study offers innovative prospects for enhancing catalytic efficiency through the implementation of spatial steric configuration of π-conjugated polymers.