文献类型：期刊文献

英文题名：In Situ Characterization of Dehydration during Ion Transport in Polymeric Nanochannels

作者：Lu, Chenghai[1,2];Hu, Chengzhi[1];Ritt, Cody L.[3];Hua, Xin[4];Sun, Jingqiu[1,2];Xia, Hailun[4];Liu, Yingya[4];Li, Da-Wei[4];Ma, Baiwen[1,2];Elimelech, Menachem[3];Qu, Jiuhui[1,2]

机构：[1]Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Aquat Chem, Beijing 100085, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[3]Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06520 USA;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2021

卷号：143

期号：35

起止页码：14242

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20213710879787);WOS:【SCI-EXPANDED(收录号:WOS:000696018700026)】；

基金：This work was supported by the National Natural Science Foundation of China (51978646 and 51738013), the Chinese Academy of Sciences, Key Research Program of Frontier Sciences (ZDBS-LYDQC014) and the,Excellent Innovation Project of Research Center for Eco-Environmental Sciences (RCEES-EEI-2019-02). We also acknowledge support from the United States National Science Foundation, Division of Graduate Education (DGE1752134) for C.L.R. and Division of Chemical, Bioengineering, Environmental, and Transport Systems (CBET-2001219) for M.E.

语种：英文

外文关键词：Molecules - Metal ions - Hydration - Nanopores - Metals - Secondary ion mass spectrometry - Solvation - Membranes

摘要：The transport of hydrated ions across nanochannels is central to biological systems and membrane-based applications, yet little is known about their hydrated structure during transport due to the absence of in situ characterization techniques. Herein, we report experimentally resolved ion dehydration during transmembrane transport using modified in situ liquid ToF-SIMS in combination with MD simulations for a mechanistic reasoning. Notably, complete dehydration was not necessary for transport to occur across membranes with sub-nanometer pores. Partial shedding of water molecules from ion solvation shells, observed as a decrease in the average hydration number, allowed the alkali-metal ions studied here (lithium, sodium, and potassium) to permeate membranes with pores smaller than their solvated size. We find that ions generally cannot hold more than two water molecules during this sterically limited transport. In nanopores larger than the size of the solvation shell, we show that ionic mobility governs the ion hydration number distribution. Viscous effects, such as interactions with carboxyl groups inside the membrane, preferentially hinder the transport of the mono- and dihydrates. Our novel technique for studying ion solvation in situ represents a significant technological leap for the nanofluidics field and may enable important advances in ion separation, biosensing, and battery applications.