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Insights into the Role of Counterions on Polyelectrolyte-Modified Nanopore Accessibility
Langmuir ( IF 3.7 ) Pub Date : 2018-05-08 00:00:00 , DOI: 10.1021/acs.langmuir.8b00963 Laura Silies 1 , Estefania Gonzalez Solveyra 2 , Igal Szleifer 2 , Annette Andrieu-Brunsen 1
Langmuir ( IF 3.7 ) Pub Date : 2018-05-08 00:00:00 , DOI: 10.1021/acs.langmuir.8b00963 Laura Silies 1 , Estefania Gonzalez Solveyra 2 , Igal Szleifer 2 , Annette Andrieu-Brunsen 1
Affiliation
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Nanopores play a decisive role in different technologies from oil production, separation, and sensing to drug delivery or catalysis and energy conversion. In recent years, abilities to functionalize nanopores have advanced significantly. Thereby, nanopores functionalized with polyelectrolytes or responsive polymers show fascinating transport properties, such as gated or gradually controlled ionic permselectivity. Nonetheless, understanding the influence of external parameters such as ion type or concentration on nanopore performance, and thus on the mentioned applications, remains a challenge but is crucial for applications. In this work, the effect of different counterions on the wetting and ionic transport in poly(2-(methacryloyloxy)ethyltrimethylammonium chloride)-functionalized silica mesopores (pore diameter <10 nm) was experimentally and theoretically investigated. Static contact angles covered a range from 45 to almost 90° by exclusively changing the counterion. Ionic pore accessibility was also strongly dependent on the counterion present and was found to gradually change from accessible pores up to complete, pH-independent ion exclusion. On the basis of molecular theory calculations, these experimental observations were rationalized on the basis of ion binding between the [2-(methacryloyloxy)ethyl]trimethylammonium chloride monomers and the counterions. In addition, the theoretical framework provided a nanoscopic view into the molecular organization inside the pores, showing a strong dependence of ion concentration and ion distribution profiles along the pore radius in dependence of the present ions. The obtained insights on the role of counterion type and ion binding in nanopores are expected to have direct impact on the above-mentioned applications.
中文翻译：
平衡离子对聚电解质修饰的纳米孔可及性作用的见解
纳米孔在从石油生产，分离和传感到药物输送或催化和能量转换的不同技术中起着决定性的作用。近年来，功能化纳米孔的能力已大大提高。因此，用聚电解质或响应性聚合物官能化的纳米孔显示出令人着迷的传输性能，例如门控或逐步控制的离子渗透性。尽管如此，了解诸如离子类型或浓度之类的外部参数对纳米孔性能的影响，进而对上述应用的影响，仍然是一个挑战，但对应用而言至关重要。在这项工作中，不同的抗衡离子对聚（2-（甲基丙烯酰氧基）乙基三甲基氯化铵）-官能化二氧化硅介孔（孔径< 10 nm）进行了实验和理论研究。通过专门改变抗衡离子，静态接触角覆盖了从45°到几乎90°的范围。离子孔的可进入性也强烈依赖于存在的抗衡离子，并且发现离子的可进入性会逐渐从可进入的孔逐渐变为完全不依赖pH的离子排斥。在分子理论计算的基础上，基于[2-（甲基丙烯酰氧基氧基）乙基]三甲基氯化铵单体与抗衡离子之间的离子键合，使这些实验观察合理化。另外，理论框架提供了对孔内分子结构的纳米观察，显示了离子浓度和沿孔半径的离子分布轮廓与现有离子的强烈相关性。
更新日期：2018-05-08
中文翻译：
平衡离子对聚电解质修饰的纳米孔可及性作用的见解
纳米孔在从石油生产，分离和传感到药物输送或催化和能量转换的不同技术中起着决定性的作用。近年来，功能化纳米孔的能力已大大提高。因此，用聚电解质或响应性聚合物官能化的纳米孔显示出令人着迷的传输性能，例如门控或逐步控制的离子渗透性。尽管如此，了解诸如离子类型或浓度之类的外部参数对纳米孔性能的影响，进而对上述应用的影响，仍然是一个挑战，但对应用而言至关重要。在这项工作中，不同的抗衡离子对聚（2-（甲基丙烯酰氧基）乙基三甲基氯化铵）-官能化二氧化硅介孔（孔径< 10 nm）进行了实验和理论研究。通过专门改变抗衡离子，静态接触角覆盖了从45°到几乎90°的范围。离子孔的可进入性也强烈依赖于存在的抗衡离子，并且发现离子的可进入性会逐渐从可进入的孔逐渐变为完全不依赖pH的离子排斥。在分子理论计算的基础上，基于[2-（甲基丙烯酰氧基氧基）乙基]三甲基氯化铵单体与抗衡离子之间的离子键合，使这些实验观察合理化。另外，理论框架提供了对孔内分子结构的纳米观察，显示了离子浓度和沿孔半径的离子分布轮廓与现有离子的强烈相关性。
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