Magnetotactic Micro‐Nanorobots for Highly Efficient Nitroaromatic Conversion

Developing magnetic micro/nanorobots (MNRs) systems that convert external stimuli into nanoscale self‐sustained motion (such as self‐rotation) and integrate organic chemical transformations holds great potential, especially in green chemistry and efficient catalysis. However, precise control of motion faces multiple limitations in terms of engine designs of the MNRs. Here, magnetic MNRs consisting of Fe 3 O 4 @COF nanochains are assembled via tailored magnetic fields, with advantages such as maneuverability, magnetotaxis capability, and facile recovery. Guided by a programmed rotating magnetic field, the Fe 3 O 4 @COF‐Au MNRs can autonomously move in water with precise directional control, thereby promoting interfacial interactions with molecules. Further analysis of their motion reveals an “out‐of‐step” phenomenon determined by a critical frequency and elucidated the mechanism of its significant effect on velocity. Under the microfluidic domains or rotational vortices through the MNRs’ rotation in a rotating magnetic field, the Fe 3 O 4 @COF‐Au MNRs achieve efficient selective hydrogenation of nitroarenes, with a maximum turnover frequency (TOF) of 53 203 h −1 , exceeding all previously reported values. This study suggests an innovative strategy for engineering magnetic particles into intelligent MNRs to achieve efficient catalytic reactions.