Exceptionally Stable Cobalt Nanoclusters on Functionalized Graphene

V. Chesnyak, Srdjan Stavrić, M. Panighel, Daniele Povoledo, S. del Puppo, M. Peressi, Giovanni Comelli, C. Africh
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Abstract

To improve reactivity and achieve a higher material efficiency, catalysts are often used in the form of clusters with nanometer dimensions, down to single atoms. Since the corresponding properties are highly structure‐dependent, a suitable support is thus required to ensure cluster stability during operating conditions. Herein, an efficient method to stabilize cobalt nanoclusters on graphene grown on nickel substrates, exploiting the anchoring effect of nickel atoms incorporated in the carbon network is presented. The anchored nanoclusters are studied by in situ variable temperature scanning tunneling microscopy at different temperatures and upon gas exposure. Cluster stability upon annealing up to 200 °C and upon CO exposure at least up to 1 × 10−6 mbar CO partial pressure is demonstrated. Moreover, the dimensions of the cobalt nanoclusters remain surprisingly small (<3 nm diameter) with a narrow size distribution. Density functional theory calculations demonstrate that the interplay between the low diffusion barrier on graphene on nickel and the strong anchoring effect of the nickel atoms leads to the increased stability and size selectivity of these clusters. This anchoring technique is expected to be applicable also to other cases, with clear advantages for transition metals that are usually difficult to stabilize.

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功能化石墨烯上异常稳定的钴纳米团簇
为了提高反应活性并获得更高的材料效率,催化剂通常以纳米级(小至单个原子)的团簇形式使用。由于催化剂的相应特性与结构高度相关,因此需要合适的支撑物来确保催化剂在工作条件下的稳定性。本文介绍了一种在镍基底上生长的石墨烯上稳定钴纳米团簇的有效方法,该方法利用了碳网络中镍原子的锚定效应。通过原位变温扫描隧道显微镜在不同温度和气体暴露条件下对锚定的纳米团簇进行了研究。结果表明,簇在退火至 200 °C,以及接触二氧化碳(二氧化碳分压至少达到 1 × 10-6 mbar)时具有稳定性。此外,钴纳米团簇的尺寸仍然出奇地小(直径小于 3 纳米),尺寸分布窄。密度泛函理论计算表明,镍上石墨烯的低扩散阻力与镍原子的强锚定效应之间的相互作用提高了这些团簇的稳定性和尺寸选择性。这种锚定技术预计也适用于其他情况,对于通常难以稳定的过渡金属具有明显的优势。
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