Theoretical evaluation of M/H-magadiite and Al modified M/H-[Al]-magadiites single-atom catalysts (M = Ag, Au, Pd, and Pt)

IF 2.1 4区 化学 Q3 CHEMISTRY, PHYSICAL Surface Science Pub Date : 2024-06-27 DOI:10.1016/j.susc.2024.122541
Monize F. Tôrres , Márcio F. Santos , Bruna Nádia N. Silva , Muhammad Adnan Saqlain , Florence P.N. Antunes , Heloise O. Pastore , Alexandre A. Leitão
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Abstract

This work intends to simulate the interaction of metal single-atom(s) supported on surfaces of H-magadiite (H4Si14O30) and Al substituted H-[Al]-magadiites (H5AlSi13O30), hereafter called M/H-magadiite and M/H-[Al]-magadiite (M = Ag, Au, Pt, Pd), using DFT calculations (PBE and PBE-D3 functionals). Three distinct positions were defined in all surfaces to optimize each simulated model: “hydroxyl”, “edge” and “cavity”. The Au/H-magadiite and Ag/H-magadiite models were more stable at the “hydroxyl” sites. Meanwhile, in the aluminated surfaces, the presence of an extra hydrogen atom (here called Hextra, located in the “edge” region) was responsible for a more stable situation of these metal atoms. On the other hand, the Pd and Pt single-atoms present in H-magadiite and H-[Al]-magadiites showed greater interaction with all the sites, compared to the Au- and Ag- models. Based on the binding energies and other electronic calculations, the aluminol site at H-[Al]-magadiites has the best capacity to support metal species. For example, the Pt/H-[Al]-magadiite showed the lowest binding energy (-2.64 eV for PBE and -2.93 eV for PBE-D3), the strongest charge interaction and the smallest Pt – Hextra distance (1.55 Å). The migration barriers (PBE) in Ag/H-magadiite, Au/H-magadiite, and Pd/H-magadiite were lower than 21.50 kJ·mol−1, suggesting the high possibility of metal sintering. For all the cases, the PBE-D3 overestimated the barriers. Contrarily, the Pt/H-magadiite structures stabilized in the “cavity” region, inside the silicon rings of the silicate, and presented a migration barrier greater than 200 kJ·mol−1. These calculations offered the first indications of the behavior of single-atoms, which will serve as the basis for a broader description, in future works, of the migration of metal species in the Al-models simulated here, as well as for modeling single-atom catalysts that can be used in stable conditions.

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M/H-方镁石和铝修饰的 M/H-[Al]-方镁石单原子催化剂(M = Ag、Au、Pd 和 Pt)的理论评估
这项工作旨在利用 DFT 计算(PBE 和 PBE-D3 函数)模拟 H-magadiite(HSiO)和 Al 取代的 H-[Al]-magadiite(HAlSiO)(以下称为 M/H-magadiite 和 M/H-[Al]-magadiite(M = Ag、Au、Pt、Pd))表面支持的金属单原子的相互作用。在所有表面中定义了三个不同的位置,以优化每个模拟模型:"羟基"、"边缘 "和 "空腔"。Au/H-magadiite 和 Ag/H-magadiite 模型在 "羟基 "位置更稳定。同时,在镀铝表面,由于存在一个额外的氢原子(此处称为 H,位于 "边缘 "区域),这些金属原子的情况更为稳定。另一方面,与 Au 和 Ag 模型相比,H-magadiite 和 H-[Al]-magadiite 中的钯和铂单原子与所有位点的相互作用更大。根据结合能和其他电子计算,H-[Al]-magadiites 的铝醇位点支持金属物种的能力最强。例如,Pt/H-[Al]-magadiite 的结合能最低(PBE 为 -2.64 eV,PBE-D3 为 -2.93 eV),电荷相互作用最强,Pt - H 间距最小(1.55 Å)。Ag/H-magadiite、Au/H-magadiite 和 Pd/H-magadiite 中的迁移势垒(PBE)均低于 21.50 kJ-mol,表明金属烧结的可能性很大。在所有情况下,PBE-D3 都高估了势垒。相反,Pt/H-magadiite 结构稳定在硅酸盐硅环内的 "空腔 "区域,其迁移势垒大于 200 kJ-mol。这些计算首次表明了单原子的行为,这将为今后工作中更广泛地描述此处模拟的铝模型中金属物种的迁移以及建立可在稳定条件下使用的单原子催化剂模型奠定基础。
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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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