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脂质双层包封和脂质组成对水中疏水性钯纳米颗粒的催化活性和胶体稳定性的影响。

Effects of lipid bilayer encapsulation and lipid composition on the catalytic activity and colloidal stability of hydrophobic palladium nanoparticles in water.

作者信息

Ortega Dominick D, Pavlakovich Nicholas, Shon Young-Seok

机构信息

Department of Chemistry and Biochemistry, California State University, Long Beach 1250 Bellflower Blvd. Long Beach CA 90840 Unites States

出版信息

RSC Adv. 2022 Aug 9;12(34):21866-21874. doi: 10.1039/d2ra03974e. eCollection 2022 Aug 4.

Abstract

This article shows the preparation of a lipid-nanoparticle assembly (LNA) which contains hydrophobic palladium nanoparticles (PdNPs) within the hydrophobic regions of the liposomal micelles. To understand the colloidal stability and catalytic activity of LNAs, the structure-property relationships of LNAs are investigated by manipulating the lipid composition and reaction temperature. The studies of LNAs using dynamic light scattering (DLS), differential scanning calorimetry (DSC), and transmission electron microscopy (TEM) show decreased colloidal stability with the incorporation of PdNPs compared to their counterpart 1,2-distearoyl--glycero-3-phosphocholine (DSPC) liposomes without PdNPs. LNAs with PdNPs catalyze the hydrogenation of 1-octene and its isomers to octane under one atm hydrogen gas and at room temperature within 24 h. The kinetic studies show that the isomerization of 1-octene to 2-octene occurs more favorably in the early stage of the reactions, which is followed by the subsequent hydrogenation of all octene isomers. The studies on temperature effects indicate that there is a significant increase in conversion yield of substrates when the reaction temperature increases from 22 to 37 °C, which correspond to room temperature and biological temperature, respectively. Phase transition of DSPC-PdNP LNAs from gel to liquid crystalline phase changing the fluidity of the bilayer is proposed to be the main reason for dramatic increases in the catalytic activity of the LNAs. It is also found that the rate of hydrogenation is dependent on the lipid composition of LNAs with the presence of cholesterol having a negative influence on the catalytic activity of LNAs while increasing their colloidal stability.

摘要

本文展示了一种脂质纳米颗粒组装体(LNA)的制备方法,该组装体在脂质体胶束的疏水区域内包含疏水性钯纳米颗粒(PdNP)。为了解LNA的胶体稳定性和催化活性,通过控制脂质组成和反应温度研究了LNA的结构-性质关系。使用动态光散射(DLS)、差示扫描量热法(DSC)和透射电子显微镜(TEM)对LNA进行的研究表明,与不含PdNP的对应物1,2-二硬脂酰-sn-甘油-3-磷酸胆碱(DSPC)脂质体相比,掺入PdNP后胶体稳定性降低。含PdNP的LNA在一个大气压氢气和室温下24小时内催化1-辛烯及其异构体加氢生成辛烷。动力学研究表明,1-辛烯异构化为2-辛烯在反应早期更有利,随后所有辛烯异构体进行后续加氢。温度效应研究表明,当反应温度从22℃升高到37℃时,底物的转化率显著增加,这两个温度分别对应室温及生物温度。DSPC-PdNP LNA从凝胶相到液晶相的相变改变了双层的流动性,被认为是LNA催化活性显著增加的主要原因。还发现加氢速率取决于LNA的脂质组成,胆固醇的存在对LNA的催化活性有负面影响,但会增加其胶体稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6995/9361304/884511c8d962/d2ra03974e-s1.jpg

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