金属镍中心在惰性金属基底中的自发分散,用于选择性氢化碳-碳三键

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-06-01 DOI:10.1016/S1872-2067(24)60048-3
Xin Deng , Caiyan Zheng , Weijie Li , Jiamin Wang , Di Yang , Zhenpeng Hu , Landong Li
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引用次数: 0

摘要

具有活性中心最大利用率和理想目标产物选择性的单位金属催化剂是学术界和工业界的热门研究课题。然而,合成策略通常比较复杂,需要精确控制金属中心和支撑材料之间的相互作用。本文利用过渡金属中心 Ni 在惰性基质(Al、Mg 和 Ti)中的自发分散行为,开发了一种简单的自发分散和通用策略,以构建含有孤立金属中心的全金属催化剂体系。Ni/Al 和 Ni/Mg 在乙炔半加氢模型反应中表现出卓越的性能,具有最先进的特定位点活性、高乙烯选择性和良好的稳定性。特别是 Ni/Al 被首次报道为碳-碳三键选择性加氢的合格低成本催化剂,超过了基准 Lindlar 催化剂。通过结合动力学分析、光谱研究和理论计算,镍/铝催化剂上乙炔半加氢反应机理得到了很好的阐明。本文开发的创新方法不仅拓展了单金属催化剂的合成策略,而且由于全金属体系的内在优势,有望在各种化学转化中得到实际应用。
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Spontaneous dispersion of metallic nickel centers in inert metal substrate for the selective hydrogenation of carbon-carbon triple bonds

Single-site metal catalysts with maximal utilization of active centers and desired target product selectivity represent a hot research topic within the realms of both academic and industry. However, the synthetic strategy is generally complicated and requires the precise control of interplay between metal centers and supporting materials. Herein, a simple spontaneous dispersion and universal strategy are developed to construct all-metal catalyst systems containing isolated metallic centers utilizing the spontaneous dispersion behaviors of transition metal centers Ni in inert substrate (Al, Mg and Ti). Ni/Al and Ni/Mg show remarkable performances in the model reaction of acetylene semi-hydrogenation with state-of-the-art site-specific activity, high ethylene selectivity and good stability. Especially, Ni/Al is reported for the first time to be an eligible low-cost catalyst for the selective hydrogenation of carbon-carbon triple bonds, surpassing the benchmark Lindlar catalyst. The reaction mechanism of acetylene semi-hydrogenation over Ni/Al catalyst is well clarified via the combination of kinetic analyses, spectroscopy investigation and theoretical calculations. The innovative approach developed herein not only expands the synthetic strategies toward single-site metal catalysts but also holds promise for practical applications in diverse chemical transformations due to the intrinsic advantages of all-metal systems.

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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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