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关于硅氢化物吸附剂分离选择性起源的见解。

Insights into the origin of the separation selectivity with silica hydride adsorbents.

作者信息

Kulsing Chadin, Nolvachai Yada, Marriott Philip J, Boysen Reinhard I, Matyska Maria T, Pesek Joseph J, Hearn Milton T W

机构信息

School of Chemistry, Monash University , Melbourne, VIC 3800, Australia.

出版信息

J Phys Chem B. 2015 Feb 19;119(7):3063-9. doi: 10.1021/jp5103753. Epub 2015 Feb 6.

Abstract

In this study, the surface properties of type-B silica have been compared with an unmodified silica hydride phase, a diamond hydride phase and silica hydride phases modified with bidentate anchored octyl (BDC8), bidentate anchored octadecyl (BDC18), phenyl and cholesteryl groups. Atomic distributions of the surface elemental composition of each type of stationary phase were determined using energy-dispersive X-ray spectroscopy. For the type-B silica, unmodified silica hydride, diamond hydride as well as BDC18 and cholesteryl silica hydride phases, the increase in carbon contents correlated with more negative surface ζ potential values (R(2) = 0.92). The origin of these more negative ζ potentials has been evaluated with mobile phases up to 100% (v/v) methanol content, with this property attributed to either an increase in the amount of adsorbed hydroxide ions or a decrease in the amount of adsorbed protons on the surfaces modified silica hydride phases of higher carbon content. This property of chemically modified silica hydride phases is in accordance with the unique propensity for hydroxide ions to be preferentially adsorbed onto hydrophobic surfaces of low permittivity and effects due to the specific accumulated water molecules associated with the electrical interfacial double layer of the adsorbent.

摘要

在本研究中,已将B型硅胶的表面性质与未改性的硅氢化物相、金刚石氢化物相以及用双齿锚定的辛基(BDC8)、双齿锚定的十八烷基(BDC18)、苯基和胆固醇基改性的硅氢化物相进行了比较。使用能量色散X射线光谱法测定了每种固定相表面元素组成的原子分布。对于B型硅胶、未改性的硅氢化物、金刚石氢化物以及BDC18和胆固醇基硅氢化物相,碳含量的增加与更负的表面ζ电位值相关(R(2) = 0.92)。已用甲醇含量高达100%(v/v)的流动相评估了这些更负ζ电位的来源,该性质归因于在高碳含量的改性硅氢化物相表面上吸附的氢氧根离子量增加或吸附的质子量减少。化学改性硅氢化物相的这一性质与氢氧根离子优先吸附到低介电常数疏水表面上的独特倾向以及与吸附剂电界面双层相关的特定累积水分子的影响一致。

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