Core–shell Pd(0)@His-SiO2/CoFe2O4 nano-composite as a magnetically recoverable heterogeneous catalyst for the deprotection of oximes and Heck coupling†

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Reaction Chemistry & Engineering Pub Date : 2024-05-23 DOI:10.1039/D4RE00060A
Vrinda Sharma, Anu Choudhary, Surbhi Sharma, Gunjan Vaid and Satya Paul
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Abstract

With the advent of nanotechnology, the rational engineering of core–shell nanostructure-based catalysts has received significant attention owing to their potential for exhibiting unique properties such as durability, structural flexibility, and porous shell adaptability. In this study, we designed a magnetic core–shell based heterogeneous nanocatalyst [Pd(0)@His-SiO2/CoFe2O4] comprising a histidine functionalized silica supported cobalt ferrite core encapsulated with a Pd(0) nanoparticle shell. Cobalt ferrite was synthesized using a hydrothermal process and modified with silica to obtain homogeneous dispersion and a dense structure as well as to prevent self-agglomeration in the core. Further, the core moiety was functionalized using a non-toxic amine linker, i.e. histidine, which acts as a robust anchor for holding the Pd(0) shell. The catalytic activity of Pd(0)@His-SiO2/CoFe2O4 was evaluated for the oxidative deprotection of oximes and Heck coupling, and excellent results were obtained with high recyclability of the catalyst. Comparative study showed that the Pd(0) nanoparticle shell is the active species and the cobalt ferrite core plays a promotional role. XPS showed the existence of synergism between the core and the shell, suggesting that the electron density was drifted from the cobalt ferrite core towards the Pd(0) shell, which could be the reason for its enhanced catalytic performance. VSM demonstrated high saturation magnetization in both fresh and reused catalysts, which facilitates the separation of the catalyst from the reaction mixture. Thus the proposed approach based on the core–shell nanostructure provides a useful platform for the fabrication of an active metal such as Pd(0) with easy accessibility, excellent activity and convenient recovery.

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核壳 Pd(0)@His-SiO2/CoFe2O4 纳米复合材料作为磁性可回收异相催化剂用于肟的脱保护和赫克偶联
随着纳米技术的发展,基于核壳纳米结构的催化剂的合理工程设计受到了广泛关注,因为它们具有耐久性、结构灵活性、多孔壳适应性等独特性能。在本研究中,我们设计了一种基于核壳的磁性异相纳米催化剂 [Pd(0)@His-SiO2/CoFe2O4],它由组氨酸官能化二氧化硅支撑的钴铁氧体内核和 Pd(0) 纳米粒子外壳组成。钴铁氧体采用水热法合成,并用二氧化硅进行改性,以获得均匀的分散性和致密的结构,并防止在核心中自团聚。此外,还使用无毒的组氨酸胺连接剂对核心分子进行了功能化处理,使其成为固定钯(0)外壳的坚固锚。评估了 Pd(0)@His-SiO2/CoFe2O4 在肟氧化脱保护和 Heck 偶联方面的催化活性。比较研究表明,钯(0)纳米颗粒外壳是活性物种,而钴铁氧体内核则起促进作用。XPS 显示核心和外壳之间存在协同作用,即电子密度从钴铁氧体核心向 Pd(0) 外壳漂移,这可能是其催化性能增强的原因。VSM 显示了新催化剂和重复使用催化剂的高饱和磁化率,这有利于催化剂从反应混合物中分离出来。上述基于核壳纳米结构的方法为制备像 Pd(0)这样的活性金属提供了一个有用的平台,这种催化剂易于获得、活性优异且便于回收。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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