Abstract
In modern Li-based batteries, alloying anode materials have the potential to drastically improve the volumetric and specific energy storage capacity. For the past decade silicon has been viewed as a “Holy Grail” among these materials; however, severe stability issues limit its potential. Herein, we present amorphous substoichiometric silicon nitride (SiNx) as a convertible anode material, which allows overcoming the stability challenges associated with common alloying materials. Such material can be synthesized in a form of nanoparticles with seamlessly tunable chemical composition and particle size and, therefore, be used for the preparation of anodes for Li-based batteries directly through conventional slurry processing. Such SiNx materials were found to be capable of delivering high capacity that is controlled by the initial chemical composition of the nanoparticles. They exhibit an exceptional cycling stability, largely maintaining structural integrity of the nanoparticles and the complete electrodes, thus delivering stable electrochemical performance over the course of 1000 charge/discharge cycles. Such stability is achieved through the in situ conversion reaction, which was herein unambiguously confirmed by pair distribution function analysis of cycled SiNx nanoparticles revealing that active silicon domains and a stabilizing Li2SiN2 phase are formed in situ during the initial lithiation.
Highlights
The development of energy storage solutions capable of delivering high energy density and fast charging is a key element for the further implementation of electrification and decarbonization technologies
With one notable exception,[34] validation of SiNx performance as a materials in more practical particle-based composite electrodes, which could be prepared through convention slurry-based process, as well as general understanding of their functionality is lacking. Such gap in the synthesis, fundamental understanding, application, and evaluation of SiNx materials under more practical circumstances is remedied in the present paper, where we demonstrate the performance and characteristics of anodes for Li-ion batteries (LIBs) based on amorphous and substoichiometric silicon nitride (SiNx) nanoparticles of different chemical compositions and particle’ sizes
Such a method has been successfully demonstrated for the preparation of nanoparticles of pure Si and allows to efficiently control the sizes of nanoparticles and their morphologies by controlling nucleation and growth in the gas phase.[36]
Summary
The development of energy storage solutions capable of delivering high energy density and fast charging is a key element for the further implementation of electrification and decarbonization technologies.
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