First-principles study of WS2 monolayer decorated with noble metals (Pt, Rh, Ir) as the promising candidates to detect nitrogenous poisonous gases

IF 8.3 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces Pub Date : 2024-10-31 DOI:10.1016/j.surfin.2024.105363

Huihui Xiong , Shulin Zhang , Yingying Ma , Yifu Zhang , Haojie Huang , Junhui Li , Chengcheng Sun , Xiaocong Zhong

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Abstract

Rapid identification of nitrogenous toxic gases (NPGs, including NO, NO₂, NH₃, and HCN) emitted from industrial processes is essential for environmental preservation. In this research, the first-principles calculations have been employed to systematically investigate the adsorption behavior and sensing characteristics of Pt, Rh, Ir-modified WS₂ monolayers (Pt-WS₂, Rh-WS₂, and Ir-WS₂) towards these NPGs, with the aim of assessing the potential of WS₂-based gas sensors for NPG detection. The results show that Pt, Rh, and Ir atoms can be stably anchored on the WS₂ surface, enhancing its chemical stability and the quantity of active sites. Additionally, the strong orbital hybridization between these noble metal atoms and gas molecules enhances the adsorption capacity of WS₂, markedly boosting the adsorption potency of these modified substances towards NPGs (E_ads≥−0.69 eV) while maintaining high selectivity toward NPGs in the presence of interfering gases (H₂O, N₂, CO₂). Analysis of the density of states, charge density distribution, and electron localization function indicates weak chemical adsorption of HCN on Pt-WS₂, Rh-WS₂, and Ir-WS₂, while strong chemical adsorption is observed for NO, NO₂, and NH₃. Furthermore, the adsorption of NO and NO₂ leads to significant band gap changes (∆E_g > 30 %) of Pt-WS₂, Rh-WS₂, and Ir-WS₂, and the response of work function to NH₃ and HCN adsorption is similarly pronounced (∆Φ > 15 %). Finally, analysis of recovery time indicates that Pt-WS₂ and Rh-WS₂ can serve as work function gas sensors for HCN and as adsorbents for NO, NO₂, and NH₃ at room temperature, whereas Ir-WS₂ can function as a reusable gas sensor for the effective detection of HCN at high temperature. This investigation establishes a robust theoretical framework for the development and manufacture of high-performance WS₂-based gas sensors.

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贵金属（铂、铑、铱）装饰的 WS2 单层的第一性原理研究，有望用于检测含氮有毒气体

快速识别工业生产过程中排放的含氮有毒气体（NPGs，包括 NO、NO2、NH3 和 HCN）对环境保护至关重要。本研究利用第一性原理计算系统地研究了 Pt、Rh、Ir 改性 WS₂单层（Pt-WS2、Rh-WS2 和 Ir-WS2）对这些 NPG 的吸附行为和传感特性，旨在评估基于 WS2 的气体传感器检测 NPG 的潜力。结果表明，铂、铑和铱原子可以稳定地固定在 WS2 表面，从而提高了其化学稳定性和活性位点的数量。此外，这些贵金属原子与气体分子之间的强轨道杂化增强了 WS₂的吸附能力，显著提高了这些修饰物质对 NPG 的吸附效力（Eads≥-0.69 eV），同时在干扰气体（H2O、N2、CO2）存在的情况下保持了对 NPG 的高选择性。对状态密度、电荷密度分布和电子定位功能的分析表明，HCN 在 Pt-WS2、Rh-WS2 和 Ir-WS2 上的化学吸附较弱，而对 NO、NO2 和 NH3 的化学吸附较强。此外，NO 和 NO₂ 的吸附导致 Pt-WS2、Rh-WS2 和 Ir-WS2 的带隙发生显著变化（ΔEg > 30 %），功函数对 NH₃ 和 HCN 吸附的响应同样明显（ΔΦ > 15 %）。最后，对回收时间的分析表明，Pt-WS2 和 Rh-WS2 可作为工作功能气体传感器，在室温下检测 HCN 和吸附 NO、NO2 和 NH3，而 Ir-WS2 可作为可重复使用的气体传感器，在高温下有效检测 HCN。这项研究为开发和制造基于 WS₂的高性能气体传感器建立了坚实的理论框架。

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来源期刊

ACS Applied Materials & Interfaces 工程技术-材料科学：综合

CiteScore

16.00

自引率

6.30%

发文量

4978

审稿时长

1.8 months

期刊介绍： ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.