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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Selective Cu4Pd alloy nanoparticles anchoring on amine functionalized graphite nanosheets and their use as reusable catalysts for a C-C coupling reaction with the sacrificial role of Cu for Pd-regeneration
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Selective Cu4Pd alloy nanoparticles anchoring on amine functionalized graphite nanosheets and their use as reusable catalysts for a C-C coupling reaction with the sacrificial role of Cu for Pd-regeneration

机译:锚固在胺官能化的石墨纳米片上的选择性Cu4Pd合金纳米颗粒及其作为C-C偶联反应的可重用催化剂的用途,具有Cu在Pd再生中的牺牲作用

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摘要

A facile method for the synthesis of phase selective alloy nanoparticles (NPs), Cu4Pd and their in situ anchoring on the surface of amine functionalized graphite nanosheets (AFGNS) by solvothermal process has been demonstrated. It has been seen that upon adding CuCl2 center dot H2O and PdCl2 into the reaction medium containing AFGNS, the -NH2 group initially helps to immobilize Cu2+ ions from CuCl2 center dot H2O. During the solvothermal reaction in presence of N,N-dimethylformamide (DMF; solvent cum reducing agent) Pd2+ gets reduced first due to its higher reduction potential. These Pd NPs in turn help in the reduction of Cu2+ to Cu in an epitaxial manner. Finally at high temperature and long reaction time Cu and Pd combine to form the Cu4Pd alloy NPs along with a small fraction of Cu NPs. The conditions to obtain Cu4Pd NPs have been optimized through controlled reactions. The as prepared Cu4Pd@AFGNS composite has been successfully used for Suzuki-Miyuara C-C coupling reaction with sufficiently high yield and reusability of up to five cycles. The progress of the reaction was monitored using a fluorimeter. Interestingly, it has been observed that the small fraction of the Cu NPs present in the system played a sacrificial role in regenerating metallic Pd NPs in the first and second reaction cycles, followed by Cu from the Cu4Pd alloy itself from the third cycle onwards which played the sacrificial role to regenerate Pd(0). A probable reaction mechanism of the catalytic reaction with Cu4Pd@AFGNS has been suggested.
机译:已经证明了一种通过溶剂热法合成相选择合金纳米颗粒(NPs),Cu4Pd及其原位锚定在胺官能化石墨纳米片(AFGNS)表面上的简便方法。已经发现,在将CuCl 2中心点H 2 O和PdCl 2添加到包含AFGNS的反应介质中时,-NH 2基团最初有助于固定来自CuCl 2中心点H 2 O的Cu 2+离子。在N,N-二甲基甲酰胺(DMF;溶剂兼还原剂)存在下的溶剂热反应过程中,Pd2 +由于其较高的还原电位而首先被还原。这些Pd NPs有助于外延将Cu2 +还原为Cu。最终,在高温和较长的反应时间下,Cu和Pd结合在一起形成Cu4Pd合金NP,以及一小部分Cu NP。通过控制反应已优化了获得Cu4Pd NP的条件。制备的Cu4Pd @ AFGNS复合材料已成功用于Suzuki-Miyuara C-C偶联反应,具有足够高的收率和多达五个循环的可重复使用性。使用荧光计监测反应进程。有趣的是,已观察到系统中存在的一小部分Cu NP在第一和第二反应循环中对金属Pd NP的再生起了牺牲作用,随后从第三循环开始由Cu4Pd合金本身产生的Cu发挥了作用。再生Pd(0)的牺牲作用。提出了Cu4Pd @ AFGNS催化反应的可能反应机理。

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