超临界co2辅助从金属有机框架中制备催化活性Pd/Ni纳米颗粒嵌入碳

IF 3.4 3区 工程技术 Q2 CHEMISTRY, PHYSICAL Journal of Supercritical Fluids Pub Date : 2024-12-19 DOI:10.1016/j.supflu.2024.106500
Kiyoshi Matsuyama , Masashi Eiro , Ayano Shoji , Takafumi Kato
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引用次数: 0

摘要

由金属有机骨架(mof)衍生的金属纳米颗粒(NP)-碳复合材料因其高催化活性而受到广泛关注。本研究开发了一种从mof制备Pd/Ni np包埋碳的简单方法。钯(Ⅱ)醋酸(Pd(OAc)2)用作Pd NPs的前驱体,并使用超临界二氧化碳(scCO₂)辅助固定化将其装载到Ni-MOF-74的孔隙中。通过Pd(OAc)2负载Ni- mof -74的还原和热解制备了Pd/Ni NPs。扫描透射电镜(STEM)清楚地显示,Pd/Ni NPs成功地固定在碳(Pd/Ni@C)中,并以10 nm左右的尺寸分散。Pd/Ni@C在Suzuki-Miyaura偶联反应中表现出高催化活性和高耐久性,尽管其Pd含量(4.7 wt%)低于市售Pd@C(10 wt%)。Pd/Ni@C上的活性钯(0)加速了Suzuki-Miyaura偶联反应,这是因为Pd/Ni NPs中的Ni起到了抵抗Pd氧化的牺牲作用。
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Supercritical CO2-assisted preparation of catalytically-active Pd/Ni nanoparticle-embedded carbon from a metal-organic framework
A metal nanoparticle (NP)-carbon composite derived from metal-organic frameworks (MOFs) has garnered significant attention for its high catalytic activity. This study develops a simple method for preparing Pd/Ni NP-embedded carbon from MOFs. Palladium(Ⅱ) acetate (Pd(OAc)2) is used as the precursor for Pd NPs and is loaded into the pores of Ni-MOF-74 using supercritical carbon dioxide (scCO₂) assisted immobilization. Pd/Ni NPs are prepared by reduction and pyrosis of Pd(OAc)2-loaded Ni-MOF-74. Scanning transmission electron microscopy (STEM) clearly reveals that the Pd/Ni NPs are successfully immobilized in the carbon (Pd/Ni@C) and dispersed with sizes around 10 nm. Pd/Ni@C demonstrates high catalytic activity and high durability in Suzuki–Miyaura coupling reactions, despite having lower Pd content (4.7 wt%) than commercially available Pd@C (10 wt%). The active palladium species Pd(0) on Pd/Ni@C accelerated the Suzuki-Miyaura coupling reactions, because the Ni in Pd/Ni NPs played the sacrificial role to resist Pd-oxidation.
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来源期刊
Journal of Supercritical Fluids
Journal of Supercritical Fluids 工程技术-工程:化工
CiteScore
7.60
自引率
10.30%
发文量
236
审稿时长
56 days
期刊介绍: The Journal of Supercritical Fluids is an international journal devoted to the fundamental and applied aspects of supercritical fluids and processes. Its aim is to provide a focused platform for academic and industrial researchers to report their findings and to have ready access to the advances in this rapidly growing field. Its coverage is multidisciplinary and includes both basic and applied topics. Thermodynamics and phase equilibria, reaction kinetics and rate processes, thermal and transport properties, and all topics related to processing such as separations (extraction, fractionation, purification, chromatography) nucleation and impregnation are within the scope. Accounts of specific engineering applications such as those encountered in food, fuel, natural products, minerals, pharmaceuticals and polymer industries are included. Topics related to high pressure equipment design, analytical techniques, sensors, and process control methodologies are also within the scope of the journal.
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