CO Adsorption on a Single-Atom Catalyst Stably Embedded in Graphene

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-01-16 DOI:10.1002/anie.202421757
Daniele Perilli, Valeria Chesnyak, Aldo Ugolotti, Mirco Panighel, Stefano Vigneri, Francesco Armillotta, Pardis Naderasli, Matus Stredansky, Monika Schied, Paolo Lacovig, Silvano Lizzit, Cinzia Cepek, Giovanni Comelli, Harald Brune, Cristina Africh, Cristiana Di Valentin
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Abstract

Confined single metal atoms in graphene-based materials have proven to be excellent catalysts for several reactions and promising gas sensing systems. However, whether the chemical activity arises from the specific type of metal atom or is a direct consequence of the confinement itself remains unclear.

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稳定嵌入石墨烯的单原子催化剂对一氧化碳的吸附
石墨烯基材料中受约束的单金属原子已被证明是几种反应的优秀催化剂和有前途的气体传感系统。然而,化学活性是由特定类型的金属原子引起的,还是由限制本身直接导致的,目前还不清楚。在这项工作中,通过结合密度泛函理论和实验表面科学研究,我们通过研究嵌入在Ni(111)载体上的石墨烯(Gr)中的Co和Ni单原子来解决这个问题。这两种单原子催化剂(SACs)对一氧化碳(CO)气体分子表现出相反的行为:在RT下,CO稳定地与CO结合,而不与Ni结合。我们通过π回给CO时被困金属dxz和dyz态的能量位置来解释这种差异:而对于CO,这些态位于费米能级,因为Ni位于费米能级以下。这一结论得到了一个概念验证实验的证实,该实验将含有稳定Ni和Co单原子的Gr/Ni(111)样品暴露在5·10-7毫巴的Co分压下。扫描隧道显微镜(STM)、x射线光电子能谱(XPS)和程序升温解吸(TPD)测量证实了CO在RT下对CO的选择性吸附。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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