Stacking two-dimensional nanosheets into laminar membranes to create nanochannels has attracted widespread attention at both fundamental and practical levels in separation technology. Constructing space-tunable and long-term stable sub-nanometre channels provides original systems for nanofluidic investigations and accurate molecular sieving. Here we report a scalable strategy for the preparation of non-swelling, covalently functionalized MoS2 membranes with tunable cohesion energy and interlayer space ranging from 3.5 to 7.7 Å, depending on the nature of the functional groups attached to the MoS2 nanosheets. We evaluated the relationship between the capillary width, surface chemistry, stacking disorder and sieving behaviour of the membranes in forwards osmosis (FO). By combining experimental investigations and numerical simulations, we determined that functionalization with aryl groups induces the formation of a capillary width of 7.1 Å and an interlayer stiffness as low as 5.6 eV Å−2, leading to controlled stacking defects. We also report the fabrication of membranes with an area of up to 45 cm2 that demonstrate a salt rejection as high as 94.2% for a continuous operating time of 7 days. Furthermore, the desalination strategy in FO has a specific energy consumption of 4 × 10−3 kWh m−3, which compares favourably with commercial FO membranes.
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This study was supported by the French National Agency (ANR, programme 2D-MEMBA, ANR-21-CE09-0034-01). D.V., K.Q. and H.W. acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 804320). W.W., J. Liu and J. Li acknowledge Ph.D. scholarships from the China Scholarship Council (CSC). C.S. acknowledges funding from the French National Agency (ANR, JCJC programme, MONOMEANR-20-CE08-0009). K.Q. and Y.Z. acknowledge financial support from the China Postdoctoral Science Foundation (2018M633127) and the Natural Science Foundation of Guangdong Province (2018A030310602). J. Li acknowledges financial support from the National Natural Science Foundation of China (21808134). The French Région Ile-de-France – SESAME programme is acknowledged for financial support (700 MHz NMR spectrometer). GENCI granted access to the HPC resources of IDRIS under allocation 2021-2022-A0110913046 and 097535. L.L. acknowledges funding from the Andalusian regional government (FEDER-UCA-18-107490), the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 823717 – ESTEEM3), the Spanish Ministerio de Economía y Competitividad (PID2019-107578GA-I00), the Ministerio de Ciencia e Innovación MCIN/AEI/10.13039/501100011033 and the European Union ‘NextGenerationEU’/PRTR (RYC2021-033764-I, CPP2021-008986). The (S)TEM measurements were performed at the National Facility ELECMI ICTS (Division de Microscopía Electrónica, Universidad de Cádiz, DME-UCA).
The authors declare no competing interests.
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Wang, W., Onofrio, N., Petit, E. et al. High-surface-area functionalized nanolaminated membranes for energy-efficient nanofiltration and desalination in forward osmosis. Nat Water 1, 187–197 (2023). https://doi.org/10.1038/s44221-023-00036-1