Citation

Chang, Yee Hui Robin and Yeoh, Keat Hoe and Kim, Chanhyeok and Yoshiya, Masato and Goh, Boon Tong and Jiang, Junke and Mahat, Mohd Muzamir and Lim, Thong Leng and Leong, Siow Hoo and Tuh, Moi Hua (2026) Exploiting the interplay of H2O co-adsorption and O vacancies on a Zr2CO2 MXene for high sensitivity and real-time battery thermal runaway monitoring. Physical Chemistry Chemical Physics, 28 (33). pp. 20382-20397. ISSN 1463-9076

Text EXPLOI~1.PDF - Published Version Restricted to Repository staff only Download (394kB)

Abstract

The escalating integration of lithium-ion batteries (LIBs) in electric vehicles and grid storage necessitates advanced sensing technologies capable of detecting early-stage thermal runaway. Among emerging 2D materials, the widely studied Zr2CO2 MXene offers a unique combination of semiconducting behaviour and tunable surface chemistry, yet its performance in realistic, humid environments remains largely unexplored. Herein, combined first-principles density functional theory (DFT), non-equilibrium Green's function (NEGF) and statistical thermodynamics modelling were employed to investigate the sensing performance of the Zr2CO2 monolayer toward critical battery off-gases, namely, HF (toxicity marker), CO2 (volumetric marker) and CO (fire marker). To simulate realistic operating conditions, the co-adsorption of H2O was evaluated alongside an exhaustive search of adsorption sites and molecular orientations. Adsorption energy analysis reveals that target analytes display a hierarchical adsorption profile, with HF most strongly bound (−0.78 eV), followed by CO2 (−0.43 eV) and CO (−0.29 eV), with extremely weak interactions for background gases (H2, C2H4 and N2). Despite variations in adsorption strength, all gas interactions induce a consistent 10–12% modulation of the electronic bandgap (Eg), yielding calculated sensitivities between 79% and 100%. These interactions further trigger measurable shifts in work function, with HF producing the most significant modulation at 13.0%. Kinetic analysis at 300 K indicates a rapid recovery time of 0.12 µs for CO, while the more strongly bound HF exhibits a recovery of 15.71 s, suggesting a highly reversible sensing at a theoretical detection limit of 0.6 parts per quadrillion (ppq) under idealized, dilute conditions within the 50 °C early warning window, requiring no ultraviolet (UV) activation or external heating for sensor reset. These findings establish Zr2CO2 as a high temporal resolution platform for real-time multimodal battery safety monitoring, providing a theoretical blueprint for defect engineering strategies that enable detection under intermediate thermal runaway and extreme conditions.

Item Type:	Article
Uncontrolled Keywords:	carbon dioxide, lithium ion
Subjects:	Q Science > QC Physics > QC170-197 Atomic physics. Constitution and properties of matter Including molecular physics, relativity, quantum theory, and solid state physics
Divisions:	Faculty of Engineering and Technology (FET)
Depositing User:	Ms Rosnani Abd Wahab
Date Deposited:	03 Sep 2026 09:17
Last Modified:	03 Sep 2026 09:17
URII:	http://shdl.mmu.edu.my/id/eprint/16652

Downloads

Edit (login required)