ON–OFF Control of Marangoni Self‐propulsion via A Supra‐amphiphile Fuel and Switch

Marangoni self‐propulsion refers to motion of liquid or solid driven by a surface tension gradient, and has applications in soft robots/devices, cargo delivery, self‐assembly etc. However, two problems remain to be addressed for motion control (e.g., ON–OFF) with conventional surfactants as Marangoni fuel: (1) limited motion lifetime due to saturated interfacial adsorption of surfactants; (2) in‐ situ motion stop is difficult once Marangoni flows are triggered. Instead of covalent surfactants, supra‐amphiphiles with hydrophilic and hydrophobic parts linked noncovalently, hold promise to solve these problems owing to its dynamic and reversible surface activity responsively. Here, we propose a new concept of ‘supra‐amphiphile fuel and switch’ based on the facile synthesis of disodium‐4‐azobenzene‐amino‐1,3‐benzenedisulfonate (DABS) linked by a Schiff base, which has amphiphilicity for self‐propulsion, hydrolyzes timely to avoid saturated adsorption, and provides pH‐responsive control over ON‐OFF motion. The self‐propulsion lifetime is extended by 50‐fold with DABS and motion control is achieved. The mechanism is revealed with coupled interface chemistry involving two competitive processes of interfacial adsorption and hydrolysis of DABS based on both experiments and simulation. The concept of ‘supra‐amphiphile fuel and switch’ provides an active solution to prolong and control Marangoni self‐propulsive devices for the advance of intelligent material systems. We propose a concept of ‘supra‐amphiphile fuel and switch’ to realize ON–OFF control of Marangoni self‐propulsion of miniaturized devices. The supra‐amphiphile shows two competitive processes on water surface: adsorption and hydrolysis, whose competence is pH‐responsive. They have comparable rates under neutral conditions to prolong the motion by 50‐fold; when changing to acid, motion stop is realized owing to faster hydrolysis than adsorption.