Probe the Localized Electrochemical Environment Effects and Electrode Reaction Dynamics for Metal Batteries using In Situ 3D Microscopy

Abstract

Uncontrollable dendrite growth is closely related to non‐uniform reaction environments. However, there is a lack of understanding and analysis methods to probe the localized electrochemical environment (LEE). Here the effects of the LEE are investigated, including localized ion concentrations, current density, and electric potential, on metal plating/stripping dynamics and dendrite minimization. A novel in situ 3D microscopy technique is developed to image the morphology dynamics and deposition rate of Zn plating/stripping processes on 3D Zn–Mn anodes. Using the in situ 3D microscope, the electrode morphology changes during the reactions are directly imaged and Zn deposition rate maps at different time points are obtained. It is found that reaction kinetics are highly correlated to LEE and electrode morphology. To further quantify the LEE effects, the digital twin technique is employed that allows the accurate calculation of the electrochemical environments, such as localized ion concentrations, current density, and electric potential, which cannot be directly measured from experiments. It is found that the curvature of the 3D electrode surface determines the LEE and significantly influences reaction kinetics. This provides a new strategy to minimize the dendrite formation by designing and optimizing the 3D geometry of the electrode to control the LEE.

Stable Zn Anodes with Triple Gradients

“…Construction of a 3D structured Zn anode with high surface area is another effective way to restrain the dendrite formation. [25][26][27] For example, a porous 3D Zn skeleton coated with a Zn@C protective layer exhibits high surface area and reduced local current density, thus possessing a smooth and dendrite-free interface after repeated Zn plating/stripping. [28] The indium-coated carbon-Zn composite anode is reported to be capable of achieving remarkable CE and long-term cyclic stability.…”

An Ultrahigh Rate and Stable Zinc Anode by Facet‐Matching‐Induced Dendrite Regulation

“…Because of the inevitable surface roughness/unevenness of a Zn anode, the initial Zn electroplating/stripping cannot be absolutely uniform. [8] Upon cycling, the surface roughness of Zn anode continuously increases due to uneven plating/stripping, till enough to significantly distort the electric field distribution over the anode, inducing dendrite formation and self-amplifying enlargement. [9,10] Such uncontrollability of dendrite growth typically leads to low coulombic efficiency, poor reversibility, or even short-circuit of ZIBs.Resource-abundant metal (e.g., zinc) batteries feature intrinsic advantages of safety and sustainability.…”

Solid Electrolyte Interface in Zn-Based Battery Systems

“…The irreversible Zn deposition will give rise to the formation of “death Zn”. An option-based in situ 3D microscope is developed to observe the 3D morphology of Zn electrode in electrochemical process [ 74 ]. It is found that the electrode morphology determines the local ion concentration distribution and local current density, and further affects the Zn plating/stripping rate.…”