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Stoichiometry-controlled reversible lithiation capacity in nanostructured silicon nitrides enabled by in situ conversion reaction

DOI: 10.1021/acsnano.1c06927 DOI Help

Authors: Asbjørn Ulvestad (Institute for Energy Technology) , Marte O. Skare (Institute for Energy Technology) , Carl Erik Foss (Institute for Energy Technology) , Henrik Krogsæter (Institute for Energy Technology; Norwegian University of Science and Technology) , Jakob F. Reichstein (Institute for Energy Technology) , Thomas J. Preston (Institute for Energy Technology) , Jan Petter Mæhlen (Institute for Energy Technology) , Hanne F. Andersen (Institute for Energy Technology) , Alexey Y. Koposov (Institute for Energy Technology; University of Oslo)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Nano

State: Published (Approved)
Published: September 2021
Diamond Proposal Number(s): 23125

Open Access Open Access

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.

Journal Keywords: silicon-based materials; nanoparticles; pair distribution function; conversion anode; lithium-ion batteries

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Materials, Chemistry, Energy

Instruments: I15-1-X-ray Pair Distribution Function (XPDF)

Added On: 29/09/2021 08:41


Discipline Tags:

Physical Chemistry Energy Energy Storage Materials Science Energy Materials Nanoscience/Nanotechnology Chemistry

Technical Tags:

Scattering Pair Distribution Function (PDF)