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Microporosity, Pore Size, and Diffusional Path Length Modulate Lipolysis Kinetics of Triglycerides Adsorbed onto SBA-15 Mesoporous Silica Particles.
Langmuir ( IF 3.7 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.langmuir.0c00253 Paul Joyce 1, 2 , Hanna Ulmefors 1, 2 , Alfonso Garcia-Bennett 3 , Clive A Prestidge 1, 2
Langmuir ( IF 3.7 ) Pub Date : 2020-03-24 , DOI: 10.1021/acs.langmuir.0c00253 Paul Joyce 1, 2 , Hanna Ulmefors 1, 2 , Alfonso Garcia-Bennett 3 , Clive A Prestidge 1, 2
Affiliation
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Understanding lipase-mediated hydrolysis mechanisms within solid-state nanocarriers is fundamental for the rational design of lipid-based formulations. In this study, SBA-15 ordered mesoporous silica (MPS) particles were engineered with well-controlled nanostructural properties to systematically elucidate the role of intrawall microporosity, mesopore size, and particle structure on lipase activity. The microporosity and diffusional path length were shown to be key modulators for lipase-provoked hydrolysis of medium chain triglycerides confined within MPS, with small changes in the pore size, between 9 and 13 nm, showing now a clear correlation to lipase activity. Lipid speciation within MPS after lipolysis, obtained through 1H NMR, indicated that free fatty acids preferentially adsorbed to rod-shaped MPS (RodMPS) particles with high microporosity. MPS that formed aggregated spindle-like structures (AggMPS) had intrinsically reduced microporosity, which was hypothesized to limit lipase/lipid diffusion to and from the MPS pores and thus retard lipolysis kinetics. A linear correlation between the microporosity and the extent of lipase-provoked hydrolysis was observed within both AggMPS and RodMPS, ultimately indicating that the intricate interplay between the microporosity and lipid/lipase diffusion can be harnessed to optimize lipolysis kinetics for silica–lipid hybrid carriers. The new insights derived in this study are integral to the future development of solid-state lipid-based nanocarriers that control the lipase activity for improving the absorption of poorly soluble bio-active compounds.
中文翻译：
微孔，孔径和扩散路径长度调节甘油三酸酯吸附到SBA-15中孔二氧化硅颗粒上的脂解动力学。
理解固态纳米载体中脂肪酶介导的水解机制是合理设计基于脂质的制剂的基础。在这项研究中，对SBA-15有序介孔二氧化硅（MPS）颗粒进行了工程设计，使其具有可控的纳米结构特性，从而系统地阐明了壁内微孔率，介孔尺寸和颗粒结构对脂肪酶活性的作用。结果表明，微孔和扩散路径长度是脂酶引起的中链甘油三酯（MPS内封闭）中链甘油三酸酯水解的关键调节剂，孔径在9至13 nm之间有很小的变化，从而显示出与脂酶活性的明显相关性。脂解后MPS中的脂质形态，通过1获得1 H NMR表明，游离脂肪酸优先吸附到具有高微孔率的棒状MPS（RodMPS）颗粒上。形成聚集的纺锤状结构（AggMPS）的MPS具有本质上降低的微孔性，据推测这会限制脂酶/脂质向MPS孔中的扩散以及从中扩散出来，从而阻碍脂解动力学。在AggMPS和RodMPS内均观察到微孔率与脂肪酶引起的水解程度之间存在线性相关性，最终表明微孔率与脂质/脂肪酶扩散之间的复杂相互作用可用于优化硅脂混合载体的脂解动力学。
更新日期：2020-03-26
中文翻译：
微孔，孔径和扩散路径长度调节甘油三酸酯吸附到SBA-15中孔二氧化硅颗粒上的脂解动力学。
理解固态纳米载体中脂肪酶介导的水解机制是合理设计基于脂质的制剂的基础。在这项研究中，对SBA-15有序介孔二氧化硅（MPS）颗粒进行了工程设计，使其具有可控的纳米结构特性，从而系统地阐明了壁内微孔率，介孔尺寸和颗粒结构对脂肪酶活性的作用。结果表明，微孔和扩散路径长度是脂酶引起的中链甘油三酯（MPS内封闭）中链甘油三酸酯水解的关键调节剂，孔径在9至13 nm之间有很小的变化，从而显示出与脂酶活性的明显相关性。脂解后MPS中的脂质形态，通过1获得1 H NMR表明，游离脂肪酸优先吸附到具有高微孔率的棒状MPS（RodMPS）颗粒上。形成聚集的纺锤状结构（AggMPS）的MPS具有本质上降低的微孔性，据推测这会限制脂酶/脂质向MPS孔中的扩散以及从中扩散出来，从而阻碍脂解动力学。在AggMPS和RodMPS内均观察到微孔率与脂肪酶引起的水解程度之间存在线性相关性，最终表明微孔率与脂质/脂肪酶扩散之间的复杂相互作用可用于优化硅脂混合载体的脂解动力学。
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