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

IF 19.3 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2025-02-06 DOI:10.1021/acsenergylett.4c03063

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

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Abstract

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 cm³/mol volume expansion upon lithiation, significantly lower than that of crystalline Si (∼9.2 cm³/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.

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来源期刊

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.