氟相离子选择性pH电极：用于生理pH范围内测量的电极体和离子载体优化。,ACS Omega

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氟相离子选择性pH电极：用于生理pH范围内测量的电极体和离子载体优化。
ACS Omega ( IF 3.7 ) Pub Date : 2020-06-01 , DOI: 10.1021/acsomega.0c00582
Xin V Chen ₁ , Maral P S Mousavi ₁ , Philippe Bühlmann ₁

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由于它们的低极性和极化性，氟传感膜既是疏水的又是疏脂的，并且具有很高的离子选择性。在这里，我们报告了一种新的氟离子膜离子选择电极（ISE），其传感范围围绕生理相关的pH值。合成了氟三[全氟（辛基）丁基]胺（N [（CH ₂）₄ R _f8 ] ₃），并作为新的H ⁺进行了测试离子载体使用重新设计的电极体，可提供出色的机械密封并大大提高了测量可靠性。在具有挑战性的1 M KCl背景下，这些氟相ISE的感测范围为pH 2.2至11.2，这是迄今为止报道的基于离子载体的H ⁺ ISE的最宽的工作范围之一。确定了对常见干扰离子（如K ⁺，Na ⁺和Ca ^2+）的高选择性（选择性系数：log K _H，K^pot = – 11.6； log K _H，Na^pot = – 12.4； log K _H，Ca^pot <– 10.2）。N [（CH ₂）_4的使用与较低碱性的三[全氟（辛基）丙基]胺离子载体相比，R _f8 ] ₃离子载体具有-（CH ₂）_4-间隔基，可将氨基与强吸电子的全氟辛基基团分隔开来。N [（CH ₂）₄ R _f8 ] _3的使用还使得ISE在低pH下比使用三[全氟（辛基）戊基]胺更长的抗负离子失败（即Donnan失败）- （CH ₂）₅–间隔基，可更有效地保护氨基中心免受全氟辛基的影响。此外，我们将常规增塑的PVC相pH ISE和氟相pH ISE暴露于10％的血清中5天。结果表明，PVC相ISE失去了选择性，而氟相ISE没有。

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Fluorous-Phase Ion-Selective pH Electrodes: Electrode Body and Ionophore Optimization for Measurements in the Physiological pH Range.

Because of their low polarity and polarizability, fluorous sensing membranes are both hydrophobic and lipophobic and exhibit very high ion selectivities. Here, we report on a new fluorous-membrane ion-selective electrode (ISE) with a wide sensing range centered around physiologically relevant pH values. The fluorophilic tris[perfluoro(octyl)butyl]amine (N[(CH₂)₄R_f8]₃) was synthesized and tested as a new H⁺ ionophore using a redesigned electrode body that provides excellent mechanical sealing and much improved measurement reliability. In a challenging 1 M KCl background, these fluorous-phase ISEs exhibit a sensing range from pH 2.2 to 11.2, which is one of the widest working ranges reported to date for ionophore-based H⁺ ISEs. High selectivities against common interfering ions such as K⁺, Na⁺, and Ca²⁺ were determined (selectivity coefficients: logK_H, K^pot = – 11.6; logK_H, Na^pot = – 12.4; logK_H, Ca^pot < – 10.2). The use of the N[(CH₂)₄R_f8]₃ ionophore with its −(CH₂)₄– spacers separating the amino group from the strongly electron-withdrawing perfluorooctyl groups improved the potentiometric selectivity as compared to the less basic tris[perfluoro(octyl)propyl]amine ionophore. The use of N[(CH₂)₄R_f8]₃ also made the ISE less prone to counter anion failure (i.e., Donnan failure) at low pH than the use of tris[perfluoro(octyl)pentyl]amine with its longer −(CH₂)₅– spacers, which more effectively shield the amino center from the perfluorooctyl groups. In addition, we exposed both conventional plasticized PVC-phase pH ISEs and fluorous-phase pH ISEs to 10% serum for 5 days. Results show that the PVC-phase ISEs lost selectivity while their fluorous-phase counterparts did not.

更新日期：2020-06-01

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