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用于CO加氢的纯δ-NiGa薄膜的磁控溅射

Magnetron Sputtering of Pure δ-NiGa Thin Films for CO Hydrogenation.

作者信息

Romeggio Filippo, Schouenborg Jonathan F, Vesborg Peter C K, Hansen Ole, Kibsgaard Jakob, Chorkendorff Ib, Damsgaard Christian D

机构信息

DTU Physics, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.

DTU Nanolab, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.

出版信息

ACS Catal. 2024 Aug 6;14(16):12592-12601. doi: 10.1021/acscatal.4c03345. eCollection 2024 Aug 16.

Abstract

Previous studies have identified δ-NiGa as a promising catalyst for the hydrogenation of CO to methanol at atmospheric pressure. Given its recent discovery, the current understanding of this catalyst is very limited. Additionally, the presence of multiple thermodynamically stable crystal phases in the Ni/Ga system complicates the experiments and their interpretation. Conventional synthesis methods often result in the production of unwanted phases, potentially leading to incorrect conclusions. To address this issue, this study focuses on the synthesis of pure δ-NiGa using magnetron sputtering deposition followed by low-temperature H annealing. Extensive characterization confirmed the reproducible synthesis of well-defined δ-NiGa thin films. These films, deposited directly into state-of-the-art μ-reactors, demonstrated methanol production at low temperatures and maintained a high stability over time. This method allowed for detailed surface and bulk characterization before and after the reaction, providing a comprehensive understanding of the deactivation mechanism. Our findings significantly contribute to the understanding of the Ni/Ga system and its behavior during catalytic activity, deactivation, and regeneration. This study also sets an example of how physical synthesis methods such as magnetron sputtering can be effectively employed to investigate complex catalytic systems, offering a viable alternative to more elaborate chemical methods.

摘要

先前的研究已确定δ-NiGa是一种在常压下将CO加氢制甲醇的有前景的催化剂。鉴于其最近才被发现,目前对这种催化剂的了解非常有限。此外,Ni/Ga体系中存在多种热力学稳定的晶相,这使得实验及其解释变得复杂。传统的合成方法常常会产生不需要的相,可能导致错误的结论。为了解决这个问题,本研究专注于通过磁控溅射沉积然后进行低温H退火来合成纯δ-NiGa。广泛的表征证实了可重复合成明确的δ-NiGa薄膜。这些直接沉积到先进的微反应器中的薄膜在低温下展示了甲醇生成,并随时间保持了高稳定性。这种方法允许在反应前后对表面和体相进行详细表征,从而全面了解失活机制。我们的发现对理解Ni/Ga体系及其在催化活性、失活和再生过程中的行为有重大贡献。本研究还树立了一个范例,展示了如何有效地利用磁控溅射等物理合成方法来研究复杂的催化体系,为更复杂的化学方法提供了可行的替代方案。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0e91/11334101/f8bb2eb6097d/cs4c03345_0001.jpg

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