Work

A Hybrid Intercalation and Conversion Mechanism for Reversible Lithium Storage in Layered Silicane (SiH) with Low Molar Volume Change

Year: 2025

Type: article

Abstract: High Resolution Image Download MS PowerPoint Slide Conversion-type anode materials generally suffer from significant volume change upon lithiation despite a high energy storage capacity. Here we report a new intercalation and conversion hybrid-type lithiation mechanism that enables a layered silicane (L-SiH) material to balance high capacity with low volume change. Using first-principles simulations of lithiation and delithiation processes, we predict L-SiH only shows a 3.8 cm 3 /mol volume expansion upon lithiation, significantly lower than that of crystalline Si (∼9.2 cm 3 /mol). During lithium intercalation, hydrogen in L-SiH is redox active, and LiH bonds are formed in the interlayer, without destruction of Si planes. The predicted lithiation proceeds via a two-phase coexisting process at an open-circuit voltage (OCV) plateau of ∼0.43 V, which coincides with experimental observation of a 0.4 V plateau upon the lithiation of synthesized L-SiH. This study introduces a promising anode material with a low volume change fulfilled by an intriguing mechanism.

Source: ACS Energy Letters

DOI: 10.1021/acsenergylett.4c03063

Authors: Wenzao Li, Jeffrey D. Cain, Nicholas Paul William Pieczonka, Zhongyi Liu, Sayed Youssef Sayed, Yue Qi

Institutions: Brown University, General Motors (United States)

Language: English

Topic: Advancements in Battery Materials

Subfield: Electrical and Electronic Engineering

Field: Engineering

Domain: Physical Sciences

SDG: Affordable and clean energy

Open Access status: hybrid

Estimated APC paid: $4,500