Despite its potential, self‐organization as a methodology for the synthesis of materials has not been developing at the pace required for the ample scale synthesis of materials with more complex structures. As there is an environmental demand for a fast change in the energy matrix, away from fossil fuels, by using materials with more complex composition and structure, this topic has been gaining potential. As complexity can be observed in many different fields of science, from biology to physical chemistry, this Review intends to focus on recent advances of self‐organization in electrochemical systems. To provide a deeper understanding of the literature being reviewed, the fundamentals of nonlinear dynamics in electrochemistry is discussed, based on classical literature. Following this, two electrochemical processes in which self‐organization is observed will be reviewed, namely electrodeposition and electrodissolution. In the final section, self‐organization is presented as a perspective for applied systems, where self‐organization is employed for the synthesis of materials of technological importance. This Review intends to reignite the debate on how self‐organization could be used to produce more complex materials than the traditional step‐by‐step approach could achieve.
Li-ion battery voltage oscillations during galvanostatic operation were recently reported for the first time. Although the oscillations were found to be induced after a chemical modification on the electrode's surface, the electrochemical properties that allowed for the emergence of oscillations were not further investigated. To contribute to this direction, we conduct numerical simulations of oscillating batteries using multiphase porous electrode theory, and the simulated results are compared with experimental oscillation reports. In both, the (dis)charge rate increase promoted an oscillation frequency decrease, and simulation data was used to describe this trend as means of local current distribution. The oscillation property dependence on operation direction was also reproduced in the simulations. It is shown and discussed how exchange current models impact the oscillation morphology and frequency, and the experimental reports are reinterpreted with this finding.
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