Water-ion permselectivity of narrow-diameter carbon nanotubes

Li, Yuhao; Li, Zhongwu; Aydin, Fikret; Quan, J.; Chen, Xi; Yao, Yun‐Chiao; Zhan, Cheng; Chen, Yunfei; Pham, Tuan Anh; Noy, Aleksandr

doi:10.1126/sciadv.aba9966

Cited by 71 publications

(87 citation statements)

References 63 publications

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“…Furnished with carboxyl groups at their ends, tube partitioning into the lipid bilayer is facilitated at low pH values since protonation of these groups renders them electrically neutral. A subsequent study reported a lower E A of only 5.3 kcal/mol (Li et al 2020). Since it neither investigated the pH-dependence of water flow nor cation permeation, their transport pathways remain elusive.…”

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

confidence: 98%

“…Thus, the plot indicates a negligible entropy of activation for water diffusion across lipid bilayers and membrane channels. Below, we list the sources of the plotted data next to the abbreviations used in the figure: aquaporin-1, AQP1 (Horner et al 2015;Zeidel et al 1992); aquaporin-Z, AQPZ (Horner et al 2015;Pohl et al 2001); bacterial potassium channel, KcsA (Horner et al 2015;Saparov and Pohl 2004); gramicidin A, gA (Pohl and Saparov 2000;Boehler et al 1978); aquaporin-0, AQP0 (Zampighi et al 1995;Kumar et al 2012); palmitoyl oleoyl phosphatidylcholine, POPC (Huster et al 1997); dioleoyl phosphatidylcholine, DOPC (Huster et al 1997); polar lipid extract from Escherichia coli, E. coli PLE (Saparov and Pohl 2004;Pluhackova and Horner 2021); egg and plant phosphatidylcholine, Egg PC and Plant PC (Fettiplace and Haydon 1980); CNT, CN-1 (Tunuguntla et al 2017); CNT, CN-2 (Li et al 2020); aquafoldamer, AQF (Shen et al 2020).…”

Section: • •mentioning

confidence: 99%

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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: 98%

Section: • •mentioning

confidence: 99%

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

2021

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“…water forming four H-bonds in bulk water 54,55 , the activation energies can be estimated to be 6.1, 6.3 and 4.1 kcal/mol for 3-LA, 4-LA and AQP1, respectively. These values are consistent with their respective experimental activation energies of 8.7, 8.3 and 5.0 kcal/mol.…”

Section: Simulation Of Water Transport and Proton Rejection Mechanismmentioning

confidence: 99%

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

et al. 2021

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The outstanding capacity of aquaporins (AQPs) for mediating highly selective superfast water transport 1-7 has inspired recent development of supramolecular monovalent ion-excluding artificial water channels (AWCs). AWC-based bioinspired membranes are proposed for desalination, water purification, and other separations applications [8][9][10][11][12][13][14][15][16][17][18] . While some recent progress has been made in synthesizing AWCs that approach the water permeability and ion selectivity of AQPs, a hallmark feature of AQPshigh water transport while excluding protons has not been reproduced. We report on a class of biomimetic, helically folded pore-forming polymeric foldamers, that can serve as long sought-after highly selective ultrafast water-conducting channels exceeding those of AQPs (1.1 × 10 10 H2O molecules/s for AQP1 7 ), with high water over monovalent ion transport selectivity (~10 8 water molecules over Clion) conferred by the modularly tunable hydrophobicity of the interior pore surface. The best-performing AWC reported here delivers water transport at an exceptionally high rate, 2.5 times that of AQP1, while concurrently rejecting salts (NaCl and KCl) and even protons.

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“…This knowledge is exquisitely important for the design of artificial channels [21][22][23][24][25][26][27] in material science, where the selectivity and permeability mechanism of AQPs serve as template to design artificial water channels envisioned to be used in next generation membrane-based separations and purifications. Similarly, AQPs [28][29][30][31][32][33][34][35] itself or carbon nanotubes 36 are envisioned as building blocks of biomimetic membranes. These highly permeable pore structures are envisioned to determine membrane performance, selectivity and functionality.…”

Section: Introductionmentioning

confidence: 99%