Manipulating nanoscopic objects by external stimuli is the cornerstone of nanoscience. Here, we report the implementation of dynamic covalent chemistry in the reversible binding and directional motion of fluorescent nanodiamond particles at a functionalized graphene surface via imine linkages. The dynamic connections allow for controlling the formation and rupture of these linkages by external stimuli. By introduction of pH gradients, the nanoparticles are driven to move along the gradient due to the different rates of the imine condensation and hydrolysis in the two environments. The multivalent nature of the particle-to-surface connection ensures that particles remain attached to the surface, whereas its dynamic character allows for exchange reaction, thus leading to displacement yet bound behavior in two-dimensional space. These results open a pathway for thermodynamically controlled manipulation of objects on the nanoscale.

1st Faculty of Medicine Charles University Kateřinská 32 121 08 Prague Czech Republic

Department of Inorganic Chemistry Faculty of Science Charles University Hlavova 2030 128 40 Prague 2 Czech Republic

Institut de Science et d'Ingénierie Supramoléculaires Université de Strasbourg 8 allée Gaspard Monge 670 00 Strasbourg France

Institute of Organic Chemistry and Biochemistry of the Czech Academy of Sciences Flemingovo náměstí 2 166 10 Prague Czech Republic

J Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences Dolejškova 2155 3 182 23 Prague Czech Republic

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