Abstract
Recently, printing techniques are increasingly investigated in the field of energy storage, especially for the fabrication of custom‐designed batteries. Thanks to its many advantages, the most industrially used gravure printing would offer an innovative boost to printed battery production, even if, to date, such a technique is still not well investigated. In this study, for the first time, gravure printing is successfully used to prepare high‐performance conversion/alloying anodes for lithium‐ion batteries. A multilayer approach allows obtainment of the desired mass loading (about 1.7 mg cm−2), reaching similar mass loadings to those obtained by commonly used lab‐scale tape‐casting methods, allowing for their comparison. High‐quality gravure‐printed layers are obtained showing a very high homogeneity, resulting in a high reproducibility of their electrochemical performance, very close to the theoretical value, and a long cycle life (up to 400 cycles). The good results are also due to the ink preparation method, using a ball‐milling mix of the powders for disaggregation and homogenization of the starting materials. This work demonstrates the possibility of using the highly scalable gravure printing not only in the industrial manufacturing of printed batteries, but also as a useful tool for the study of new materials.
Highlights
The gravure printing process can be described as a sequence of subprocesses, concurring to the final material arrangement in the printed layer: The microengraved cells on the cylinder are filled with ink; a blade removes the excessive ink from the cylinder; the ink is transferred onto the substrate by the pressure of a counter cylinder; single droplets of the ink coalesce on the substrate, forming a continuous film; and the solvent is removed from the film, causing the final arrangement of the layer.[24]
High-performance lithium-ion anodes based on Zn0.9Fe0.1O–C as the active material were successfully produced by gravure printing
Electrodes with mass loadings (>1.5 mg cmÀ2), comparable to those commonly made by tape casting, were produced
Summary
The used CAM, Zn0.9Fe0.1O–C, is composed of environmentally-friendly and abundant elements. The capacity remains excellently stable after the initial slight fading This performance is in line with previous results achieved on doctor blade coating, which is the commonly used technique for electrode preparation.[26] It should be noted here that limiting the upper cutoff provides two positive effects regarding the application of such electrodes in LiBs. First, it has been shown that cycling Zn0.9Fe0.1O–C in a wide voltage window (i.e., between 0.01 and 3.0 V) leads to an unstable solid electrolyte interphase and, second, leads to a lower energy efficiency and density.[31,32,35] such limitation to a narrower voltage range is beneficial for lithium-ion cells using such anodes if suitable prelithiation techniques are scaled up to the industrial level.[43]. The substantial reduction of the coating layer thickness by about 50% due to an optimization of the disaggregation technique (see Table 1) is certainly a key achievement, in combination with the described additional related advantages
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