International audienceA nanosilicon-based composite electrode that can achieve more than 700 cycles at a high capacity of 960 mAh/g of electrode was prepared using aqueous processing in an acidic medium. The buffering of the aqueous solution is mandatory to promote covalent bonding between Si particles and the carboxymethyl cellulose (CMC) binder. The latter is claimed to allow the formation of mechanically stronger contacts within the composite electrode in addition to the CMC bridging of the Si and carbon black particles

International audienceA Si-based anode with improved performance can be achieved using high-energy ball-milling as a cheap and easy process to produce Si powders prepared from a coarse-grained material. Ball-milled powders present all the advantages of nanometric Si powders, but not the drawbacks. Milled powders are nanostructured with micrometric agglomerates (median size [similar]10 μm), made of submicrometric cold-welded particles with a crystallite size of [similar]10 nm. The micrometric particle size provides handling and non-toxicity advantages compared to nanometric powders, as well as four times higher tap density. The nanostructuration is assumed to provide a shortened Li+ diffusion path, a fast Li+ diffusion path along grain boundaries and a smoother phase transition upon cycling. Compared to non-milled 1-5 μm powders, the improved performance of nanostructured milled Si powders is linked to a strong lowering of particle disconnection at each charge, while the irreversibility due to SEI formation remains unchanged. An electrode prepared in acidic conditions with the CMC binder achieves 600 cycles at more than 1170 mA h per gram of the milled Si-based electrode, in an electrolyte containing FEC/VC SEI-forming additives, with a coulombic efficiency above 99%, compared to less than 100 cycles at the same capacity for an electrode containing nanometric Si powder

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It is well known that the mechanical properties of lithium‐ion battery electrodes impact their electrochemical performance. This is especially critical for Si‐based negative electrodes, which suffer from large volume changes of the active mass upon cycling. Here, this study presents a postprocessing treatment (called maturation) that improves the mechanical and electrochemical stabilities of silicon‐based anodes made with an acidic aqueous binder. It consists of storing the electrode in a humid atmosphere for a few days before drying and cell assembly. This results in a beneficial in situ reactive modification of the interfaces within the electrode. First, the binder tends to concentrate at the silicon interparticle contacts. As a result, the cohesion of the composite film is strengthened. Second, the corrosion of the copper current collector, inducing the formation of copper carboxylate bonds, improves the adhesion of the composite film. The great improvement of the mechanical stability of the matured electrode is confirmed by in‐operando optical microscopy showing the absence of film delamination. The result is a significant electrochemical performance gain, up to a factor 10, compared to a not‐matured electrode. This maturation procedure can be applied to other types of electrodes for improving their electrochemical performance and also their handling during cell manufacturing.

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