还原二维晶体 MoO3 单层

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL
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引用次数: 0

摘要

通过表面科学表征技术和密度泛函理论(DFT)计算,探索了有序氧化钼(MoO3)单层在钯(100)基底上逐渐热还原形成的氧化钼薄膜的原子结构。研究发现了两个主要的还原阶段。首先,通过改变畴界长度、取向和原子结构,逐渐消除了最初的氧过量。然而,薄膜仍然富含 O 原子,具有大量末端氧原子(形成 MoO 基团),功函数升高。其次,形成了多个有序的 O-lean 相,其特征是极少或没有末端氧原子,表面功函数小得多。根据计算,在第一阶段,钯基底的正电荷稳定了过剩的氧,但在第二还原阶段,基底变成了负电荷,稳定了增强的阳离子氧化态。在此基础上,揭示了氧从初始 c(2 × 2) 域释放的机制。实验表明,薄膜还原是完全可逆的,这凸显了 MoO3/Pd 系统在异相催化方面极具潜力的特性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Reduction of a two-dimensional crystalline MoO3 monolayer

Reduction of a two-dimensional crystalline MoO3 monolayer

The atomic structure of MoOx films formed upon a gradual thermal reduction of an ordered MoO3 monolayer on the Pd(100) substrate was explored via surface science characterization techniques and density functional theory (DFT) calculations. Two main reduction stages were identified. First, the initial oxygen excess was gradually eliminated by altering the domain boundary length, orientation, and atomic structure. The films nevertheless remained O-rich, with numerous terminal oxygen atoms (formation of MoO groups), and an elevated work function. Second, multiple ordered O-lean phases were formed, characterized by either very few or no terminal oxygen atoms, and a much smaller surface work function. According to calculations, the positive charging of the Pd substrate stabilizes the oxygen excess during the first stage, but during the second reduction stage, the substrate becomes negatively charged, stabilizing enhanced cation oxidation states. On their basis, the mechanisms underlying the oxygen release from the initial c(2 × 2) domains were disclosed. The experiments showed that the film reduction is perfectly reversible, which highlights the very promising properties of the MoO3/Pd system for heterogeneous catalysis.

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来源期刊
Surface Science
Surface Science 化学-物理:凝聚态物理
CiteScore
3.30
自引率
5.30%
发文量
137
审稿时长
25 days
期刊介绍: Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.
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