Adsorption and sensing properties of Pt-In2Se3 monolayer toward thermal runaway gases (H2, CO, CO2, CH4, C2H4) in LIBs: A DFT study

IF 4.6 3区工程技术 Q2 ENGINEERING, ELECTRICAL & ELECTRONIC

Materials Science in Semiconductor Processing Pub Date : 2025-09-12 DOI:10.1016/j.mssp.2025.110038

Jingzhi Zhao , Yongqing Qian , Zihan Xu , Xiaoxing Zhang , Beibei Xiao , Dachang Chen

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Abstract

The adsorption and sensing properties of pristine α-In₂Se₃ and Pt doped In₂Se₃ monolayers for five thermal runaway gases (H₂, CO, CO₂, CH₄, C₂H₄) have been investigated using density functional theory (DFT). The adsorption energy, charge transfer (Q_T), energy density of states, work function, recovery time and sensing response were compared to elucidate the gas adsorption behavior and electronic properties. The results indicate that, when Pt replaces doping the In₂Se₃(↑) surface, the phase state of α-In₂Se₃ changes, turning into a more stable β phase. However, in the Pt-In₂Se₃(↓) surface, no phase transition was observed in α-In₂Se₃. And for the adsorption of H₂, CO and C₂H₄, the introduction of Pt atoms significantly enhances the adsorption energies. Additionally, the absolute value of the integral crystal orbital Hamiltonian population (ICOHP) is the highest for CO adsorbed on Pt doped In₂Se₃ monolayer systems, with values of −2.73 and −2.77 for the upward and downward polarization directions, respectively. This indicates a stronger interaction between CO and Pt atoms, suggesting an enhanced potential for chemical bond formation at Pt sites. The adsorption of gas molecules has shown pronounced differences in its impact on the work function. The Pt-In₂Se₃(↑) surface exhibits considerable sensitivity to CO and CH₄, resulting in the most significant work function shift (work function shift of CO is 0.14 eV; work function shift of C₂H₄ is 0.3 eV), while its response to H₂, CO₂ and CH₄ is nearly negligible. Meanwhile, the adsorption of C₂H₄ on the Pt-In₂Se₃(↓) yields a significant work function shift of 0.49 eV, further indicating the material's potential for selective detection of specific gases. A comprehensive analysis of adsorption energy and work function further reveals that the Pt-In₂Se₃(↑) surface exhibits the most pronounced gas-sensing properties toward CO (adsorption energy of 1.26 eV and work function shift to 6.01 eV), while the Pt-In₂Se₃(↓) surface shows significant sensitivity to both CO (adsorption energy of 1.34 eV and work function shift to 5.31 eV) and C₂H₄ (adsorption energy of 1.05 eV and work function shift to 5.25 eV). When both sensitivity and recovery characteristics are taken into account, Pt-In₂Se₃ monolayers demonstrate a remarkable negative sensing response towards C₂H₄, with values of −99.61 % for the In₂Se₃(↑) surface and −96.87 % for the In₂Se₃(↓) surface. Furthermore, the recovery time for C₂H₄ on the Pt-In₂Se₃(↑) surface is as short as 4.19 × 10⁻³ s at 498 K, while on the Pt-In₂Se₃(↓) surface it is 4.56 × 10⁻² s. These findings indicate that Pt functionalization not only enables ultrahigh sensitivity but also allows for rapid recovery of the sensor after gas exposure, suggesting that Pt-doped In₂Se₃ monolayers are highly promising candidates for efficient and real-time detection of ethylene. These findings provide a theoretical basis for understanding the microscopic mechanisms of gas detection in In₂Se₃-based sensors and contribute to the design of advanced sensing materials for detecting thermal runaway gases in LIBs.

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Pt-In2Se3单层膜对lib中热失控气体（H2， CO, CO2, CH4, C2H4）的吸附和传感性能：DFT研究

利用密度泛函理论（DFT）研究了原始α-In2Se3和掺杂Pt的In2Se3单层对5种热失控气体（H2、CO、CO2、CH4、C2H4）的吸附和传感性能。通过比较吸附能、电荷转移（QT）、态能密度、功函数、恢复时间和传感响应来阐明气体吸附行为和电子性质。结果表明，当Pt取代掺杂的In2Se3（↑）表面时，α-In2Se3的相态发生变化，变为更稳定的β相。而在Pt-In2Se3（↓）表面，α-In2Se3未发生相变。对于H2、CO和C2H4的吸附，Pt原子的引入显著提高了吸附能。此外，在铂掺杂的In2Se3单层体系中，CO吸附的积分晶体轨道哈密顿族（ICOHP）的绝对值最高，在向上和向下极化方向分别为- 2.73和- 2.77。这表明CO和Pt原子之间的相互作用更强，表明在Pt位点形成化学键的潜力增强。气体分子的吸附对功函数的影响表现出明显的差异。Pt-In2Se3（↑）表面对CO和CH4表现出相当的敏感性，导致最显著的功函数位移（CO的功函数位移为0.14 eV， C2H4的功函数位移为0.3 eV），而对H2、CO2和CH4的响应几乎可以忽略不计。同时，Pt-In2Se3（↓）对C2H4的吸附产生了0.49 eV的显著功函数位移，进一步表明该材料具有选择性检测特定气体的潜力。对吸附能和功函数的综合分析进一步表明，Pt-In2Se3（↑）表面对CO（吸附能为1.26 eV，功函数为6.01 eV）表现出最明显的气敏性质，而Pt-In2Se3（↓）表面对CO（吸附能为1.34 eV，功函数为5.31 eV）和C2H4（吸附能为1.05 eV，功函数为5.25 eV）都表现出显著的气敏性质。当同时考虑灵敏度和回收率特性时，Pt-In2Se3单层膜对C2H4表现出显著的负感知响应，In2Se3（↑）表面的值为−99.61%,In2Se3（↓）表面的值为−96.87%。此外，C2H4在Pt-In2Se3（↑）表面在498 K下的恢复时间为4.19 × 10−3 s，而在Pt-In2Se3（↓）表面的恢复时间为4.56 × 10−2 s。这些发现表明，Pt功能化不仅可以实现超高灵敏度，而且可以在气体暴露后快速恢复传感器，这表明Pt掺杂的In2Se3单层是非常有前途的高效实时检测乙烯的候选材料。这些发现为理解基于in2se3的传感器中气体检测的微观机制提供了理论基础，并有助于设计用于检测lib中热失控气体的先进传感材料。

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来源期刊

Materials Science in Semiconductor Processing 工程技术-材料科学：综合

CiteScore

8.00

自引率

4.90%

发文量

780

审稿时长

42 days

期刊介绍： Materials Science in Semiconductor Processing provides a unique forum for the discussion of novel processing, applications and theoretical studies of functional materials and devices for (opto)electronics, sensors, detectors, biotechnology and green energy. Each issue will aim to provide a snapshot of current insights, new achievements, breakthroughs and future trends in such diverse fields as microelectronics, energy conversion and storage, communications, biotechnology, (photo)catalysis, nano- and thin-film technology, hybrid and composite materials, chemical processing, vapor-phase deposition, device fabrication, and modelling, which are the backbone of advanced semiconductor processing and applications. Coverage will include: advanced lithography for submicron devices; etching and related topics; ion implantation; damage evolution and related issues; plasma and thermal CVD; rapid thermal processing; advanced metallization and interconnect schemes; thin dielectric layers, oxidation; sol-gel processing; chemical bath and (electro)chemical deposition; compound semiconductor processing; new non-oxide materials and their applications; (macro)molecular and hybrid materials; molecular dynamics, ab-initio methods, Monte Carlo, etc.; new materials and processes for discrete and integrated circuits; magnetic materials and spintronics; heterostructures and quantum devices; engineering of the electrical and optical properties of semiconductors; crystal growth mechanisms; reliability, defect density, intrinsic impurities and defects.