Foldamer-based ultrapermeable and highly selective artificial water channels that exclude protons

Roy, Arundhati; Shen, Jie; Joshi, Himanshu; Song, Woochul; Tu, Yu-Ming; Chowdhury, Ranjana; Ye, Ruijuan; Li, Ning; Ren, Changliang; Kumar, Manish; Aksimentiev, Aleksei; Zeng, Huaqiang

doi:10.1038/s41565-021-00915-2

Cited by 62 publications

(69 citation statements)

References 71 publications

(154 reference statements)

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“…Interestingly, a variety of artificial water channels have been reported to have high unitary water permeabilities, p f , and, at the same time, high E A values for water transport. Besides narrow sub-8-Å CNTs (Tunuguntla et al 2017 ; Li et al 2020 ), aquafoldamers (Shen et al 2020 ; Roy et al 2021 ) provide an additional example. At first glance, the combination of high p f and high E A appears odd because a steeply uphill pathway is seldom a fast one.…”

Section: Single-file Water Transport and Selectivity In Artificial Channelsmentioning

confidence: 99%

The energetic barrier to single-file water flow through narrow channels

2021

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Various nanoscopic channels of roughly equal diameter and length facilitate single-file diffusion at vastly different rates. The underlying variance of the energetic barriers to transport is poorly understood. First, water partitioning into channels so narrow that individual molecules cannot overtake each other incurs an energetic penalty. Corresponding estimates vary widely depending on how the sacrifice of two out of four hydrogen bonds is accounted for. Second, entropy differences between luminal and bulk water may arise: additional degrees of freedom caused by dangling OH-bonds increase entropy. At the same time, long-range dipolar water interactions decrease entropy. Here, we dissect different contributions to Gibbs free energy of activation, ΔG‡, for single-file water transport through narrow channels by analyzing experimental results from water permeability measurements on both bare lipid bilayers and biological water channels that (i) consider unstirred layer effects and (ii) adequately count the channels in reconstitution experiments. First, the functional relationship between water permeabilities and Arrhenius activation energies indicates negligible differences between the entropies of intraluminal water and bulk water. Second, we calculate ΔG‡ from unitary water channel permeabilities using transition state theory. Plotting ΔG‡ as a function of the number of H-bond donating or accepting pore-lining residues results in a 0.1 kcal/mol contribution per residue. The resulting upper limit for partial water dehydration amounts to 2 kcal/mol. In the framework of biomimicry, our analysis provides valuable insights for the design of synthetic water channels. It thus may aid in the urgent endeavor towards combating global water scarcity.

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Section: Single-file Water Transport and Selectivity In Artificial Channelsmentioning

confidence: 99%

The energetic barrier to single-file water flow through narrow channels

2021

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“…S47), i.e., p f,NaCl / p f,sucrose ( 10 ). RC is unity when the channel does not permeate NaCl ( 13 ) and smaller than unity when the channel does not reflect NaCl ( 28 ). The calculated RC for the thinnest F12 NC 4 ( A = 0.64 nm 2 ) was 1.02, indicating a substantially perfect reflection of NaCl (Fig.…”

mentioning

confidence: 99%

“…In general, charge neutrality is requested in the permeation of salt. Hence, if its cation or anion part does not permeate, the salt is considered to be reflected ( 28 ). Although the b Cl values of F12 NC 4 and F15 NC 5 were smaller than the detection limit, F18 NC 6 exhibited Cl – -induced fluorescence decay characteristics corresponding to b Cl = 9.7 × 10 −19 cm 3 s –1 per channel.…”

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confidence: 99%

Ultrafast water permeation through nanochannels with a densely fluorous interior surface

Itoh

Chen

Hirahara

et al. 2022

Science

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Ultrafast water permeation in aquaporins is promoted by their hydrophobic interior surface. Polytetrafluoroethylene has a dense fluorine surface, leading to its strong water repellence. We report a series of fluorous oligoamide nanorings with interior diameters ranging from 0.9 to 1.9 nanometers. These nanorings undergo supramolecular polymerization in phospholipid bilayer membranes to form fluorous nanochannels, the interior walls of which are densely covered with fluorine atoms. The nanochannel with the smallest diameter exhibits a water permeation flux that is two orders of magnitude greater than those of aquaporins and carbon nanotubes. The proposed nanochannel exhibits negligible chloride ion (Cl – ) permeability caused by a powerful electrostatic barrier provided by the electrostatically negative fluorous interior surface. Thus, this nanochannel is expected to show nearly perfect salt reflectance for desalination.

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“…They also have finite ionic permeability (<6 pS) for K + but are impermeable to Na +58 . The latest study has demonstrated 2.5 times water permeability than that of AQP1 with foldamer-based artificial water channels 59 .…”

Section: De Novo Design Of Water Selective Materialsmentioning

confidence: 99%

A bibliometric study on biomimetic and bioinspired membranes for water filtration

et al. 2021

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Insights into the biological channels and synthetic pore-forming assemblies have elucidated many fundamental aspects of selective water and solute transport over the last few decades. This has led to the development of novel technologies with unique selectivity and permeability. In terms of membrane separation technology, this development has proceeded by adapting either of two approaches: (i) one where biological channel proteins are reconstituted in suitable materials mimicking the biological bilayer membrane and (ii) one where selective transport is mimicked in synthetic structures. The development of water filtration membranes in the former approach takes advantage of aquaporin proteins as representative building blocks and that of carbon nanotubes and molecular pore-forming assemblies in the latter approach. The first approach is often referred to as the field dominated by biomimetic membranes and the latter referred to as artificial water channels. In this study, a bibliometric analysis was conducted to investigate trends in these two areas based on growing publication trends, peer-reviewed journal selection, countries, institutions, authors, and collaborative networks. A total of 3199 records available from Scopus between 1962 and 2021 were extracted and analyzed. The results showed strong international collaborations and highlighted leading researchers and hubs of excellence in these two areas. This is very timely considering that the UN climate change conference (COP26) in Glasgow, UK later this year will bring focus to the global need for water treatment technologies. This work can serve as a quick reference for early-career researchers and industries working in the area of membrane development for water purification/filtration.

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Foldamer-based ultrapermeable and highly selective artificial water channels that exclude protons

Cited by 62 publications

References 71 publications

The energetic barrier to single-file water flow through narrow channels

The energetic barrier to single-file water flow through narrow channels

Ultrafast water permeation through nanochannels with a densely fluorous interior surface

A bibliometric study on biomimetic and bioinspired membranes for water filtration

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