Reduction-Induced Self-Propelled Oscillatory Motion of Perylenediimides on Water

The emergence of macroscopic self-propelled oscillatory motion based on molecular design has attracted continual attention in relation to autonomous systems in living organisms. Herein, a series of perylenediimides (PDIs) with various imide side chains was prepared to explore the impact of molecular design and alignment on the self-propelled motion at the air-water interface. When placed on an aqueous solution containing a reductant, a solid disk of neutral PDI was reduced to form the water-soluble, surface-active PDI dianion species, which induces a surface tension gradient in the vicinity of the disk for self-propelled motion. We found that centimeter-scale oscillatory motion could be elicited by controlling the supply rate of PDI dianion species through the reductant concentration and the structure of the imide side chains. Furthermore, we found that the onset and speed of the self-propelled motion could be changed by the crystallinity of PDI at the water surface. This design principle using pi-conjugated molecules and their self-assemblies could advance self-propelled, non-equilibrium systems powered by chemical energy. Centimeter-scale autonomous oscillatory motion was achieved upon the reduction of a perylenediimide disk at the solid-water interface. This redox-activated, self-propelled system can be modulated through variations in chemical structure and molecular alignment, offering a unique avenue for the construction of molecularly designed active matter. image