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Abstract Electroosmosis on nonuniformly charged surfaces often gives rise to intriguing flow behaviors, which can be utilized in applications such as mixing processes and designing micromotors. Here, we demonstrate nonuniform electroosmosis induced by electrochemical reactions. Water electrolysis creates pH gradients near the electrodes that cause a spatiotemporal change in the wall zeta potential, leading to nonuniform electroosmosis. Such nonuniform EOFs induce multiple vortices, which promote the continuous accumulation of particles that subsequently form a colloidal band. The band develops vertically into a “wall” of particles that spans from the bottom to the top surface of the chamber. Such a flow‐driven colloidal band can be potentially used in colloidal self‐assembly and separation processes irrespective of the particle surface properties. For instance, we demonstrate these vortices can promote rapid segregation of soft colloids such as oil droplets and fat globules. 

Manipulating the transport and assembly of colloidal particles to form segregated bands or ordered supracolloidal structures plays an important role in many aspects of science and technology, from understanding the origin of life to synthesizing new materials for next-generation manufacturing, electronics, and therapeutics. One commonly used method to direct colloidal transport and assembly is the application of electric fields, either AC or DC, due to its feasibility. However, as colloidal segregation and assembly both require active redistribution of colloidal particles across multiple length scales, it is not apparent at first sight how a DC electric field, either externally applied or internally induced, can lead to colloidal structuring. In this Perspective, we briefly review and highlight recent advances and standing challenges in colloidal transport and assembly enabled by DC electrokinetics.