In Situ Generation of (sub) Nanometer Pores in MoS Membranes for Ion-selective Transport

Overview

Journal Nat Commun

Specialty Biology

Date 2024 Sep 10

PMID 39256368

Authors

Eli Hoenig

Yu Han

Kangli Xu

Jingyi Li

Mingzhan Wang

Chong Liu

Affiliations

Soon will be listed here.

Abstract

Ion selective membranes are fundamental components of biological, energy, and computing systems. The fabrication of solid-state ultrathin membranes that can separate ions of similar size and the same charge with both high selectivity and permeance remains a challenge, however. Here, we present a method, utilizing the application of a remote electric field, to fabricate a high-density of (sub)nm pores in situ. This method takes advantage of the grain boundaries in few-layer polycrystalline MoS to enable the synthesis of nanoporous membranes with average pore size tunable from <1 to ~4 nm in diameter (with in situ pore expansion resolution of ~0.2 nm s). These membranes demonstrate selective transport of monovalent ions (K, Na and Li) as well as divalent ions (Mg and Ca), outperforming existing two-dimensional material nanoporous membranes that display similar total permeance. We investigate the mechanism of selectivity using molecular dynamics simulations and unveil that the interactions between cations and the sluggish water confined to the pore, as well as cation-anion interactions, result in the different transport behaviors observed between ions.

References

Cheng C, Iyengar S, Karnik R . Molecular size-dependent subcontinuum solvent permeation and ultrafast nanofiltration across nanoporous graphene membranes. Nat Nanotechnol. 2021; 16(9):989-995. DOI: 10.1038/s41565-021-00933-0. View

Bocquet L . Nanofluidics coming of age. Nat Mater. 2020; 19(3):254-256. DOI: 10.1038/s41563-020-0625-8. View

Marion S, Macha M, Davis S, Chernev A, Radenovic A . Wetting of nanopores probed with pressure. Phys Chem Chem Phys. 2021; 23(8):4975-4987. DOI: 10.1039/d1cp00253h. View

Zhao Y, Tong X, Chen Y . Fit-for-Purpose Design of Nanofiltration Membranes for Simultaneous Nutrient Recovery and Micropollutant Removal. Environ Sci Technol. 2021; 55(5):3352-3361. DOI: 10.1021/acs.est.0c08101. View

Koenig S, Wang L, Pellegrino J, Scott Bunch J . Selective molecular sieving through porous graphene. Nat Nanotechnol. 2012; 7(11):728-32. DOI: 10.1038/nnano.2012.162. View

Feng J, Liu K, Graf M, Lihter M, Bulushev R, Dumcenco D . Electrochemical Reaction in Single Layer MoS2: Nanopores Opened Atom by Atom. Nano Lett. 2015; 15(5):3431-8. DOI: 10.1021/acs.nanolett.5b00768. View

Yanagi I, Ishida T, Fujisaki K, Takeda K . Fabrication of 3-nm-thick Si3N4 membranes for solid-state nanopores using the poly-Si sacrificial layer process. Sci Rep. 2015; 5:14656. PMC: 4589763. DOI: 10.1038/srep14656. View

Li F, Zhu J, Sun P, Zhang M, Li Z, Xu D . Highly efficient and selective extraction of gold by reduced graphene oxide. Nat Commun. 2022; 13(1):4472. PMC: 9345893. DOI: 10.1038/s41467-022-32204-4. View

Graf M, Lihter M, Thakur M, Georgiou V, Topolancik J, Ilic B . Fabrication and practical applications of molybdenum disulfide nanopores. Nat Protoc. 2019; 14(4):1130-1168. DOI: 10.1038/s41596-019-0131-0. View

10.

Rollings R, Kuan A, Golovchenko J . Ion selectivity of graphene nanopores. Nat Commun. 2016; 7:11408. PMC: 4844701. DOI: 10.1038/ncomms11408. View

11.

Kong D, Wang H, Cha J, Pasta M, Koski K, Yao J . Synthesis of MoS2 and MoSe2 films with vertically aligned layers. Nano Lett. 2013; 13(3):1341-7. DOI: 10.1021/nl400258t. View

12.

Sahu S, Di Ventra M, Zwolak M . Dehydration as a Universal Mechanism for Ion Selectivity in Graphene and Other Atomically Thin Pores. Nano Lett. 2017; 17(8):4719-4724. PMC: 5614503. DOI: 10.1021/acs.nanolett.7b01399. View

13.

Macha M, Marion S, Tripathi M, Thakur M, Lihter M, Kis A . High-Throughput Nanopore Fabrication and Classification Using Xe-Ion Irradiation and Automated Pore-Edge Analysis. ACS Nano. 2022; 16(10):16249-16259. DOI: 10.1021/acsnano.2c05201. View

14.

Michaud-Agrawal N, Denning E, Woolf T, Beckstein O . MDAnalysis: a toolkit for the analysis of molecular dynamics simulations. J Comput Chem. 2011; 32(10):2319-27. PMC: 3144279. DOI: 10.1002/jcc.21787. View

15.

Zhang H, Li X, Hou J, Jiang L, Wang H . Angstrom-scale ion channels towards single-ion selectivity. Chem Soc Rev. 2022; 51(6):2224-2254. DOI: 10.1039/d1cs00582k. View

16.

Surwade S, Smirnov S, Vlassiouk I, Unocic R, Veith G, Dai S . Water desalination using nanoporous single-layer graphene. Nat Nanotechnol. 2015; 10(5):459-64. DOI: 10.1038/nnano.2015.37. View

17.

Razmjou A, Asadnia M, Hosseini E, Habibnejad Korayem A, Chen V . Design principles of ion selective nanostructured membranes for the extraction of lithium ions. Nat Commun. 2019; 10(1):5793. PMC: 6923379. DOI: 10.1038/s41467-019-13648-7. View

18.

Pedro de Souza J, Chow C, Karnik R, Bazant M . Nonlinear ion transport mediated by induced charge in ultrathin nanoporous membranes. Phys Rev E. 2021; 104(4-1):044802. DOI: 10.1103/PhysRevE.104.044802. View

19.

Storey B, Bazant M . Effects of electrostatic correlations on electrokinetic phenomena. Phys Rev E Stat Nonlin Soft Matter Phys. 2012; 86(5 Pt 2):056303. DOI: 10.1103/PhysRevE.86.056303. View

20.

Goutham S, Keerthi A, Ismail A, Bhardwaj A, Jalali H, You Y . Beyond steric selectivity of ions using ångström-scale capillaries. Nat Nanotechnol. 2023; 18(6):596-601. DOI: 10.1038/s41565-023-01337-y. View