학술논문

Stoichiometry-Controlled Reversible Lithiation Capacity in Nanostructured Silicon Nitrides Enabled by in SituConversion Reaction
Document Type
Article
Source
ACS Nano; October 2021, Vol. 15 Issue: 10 p16777-16787, 11p
Subject
Language
ISSN
19360851; 1936086X
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 SiNxmaterials 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 situconversion reaction, which was herein unambiguously confirmed by pair distribution function analysis of cycled SiNxnanoparticles revealing that active silicon domains and a stabilizing Li2SiN2phase are formed in situduring the initial lithiation.