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Manipulating the surface energy, and thereby the wetting properties of solids, has promise for various physical, chemical, biological and industrial processes. Typically, this is achieved by either chemical modification or by controlling the hierarchical structures of surfaces. Here we report a phenomenon whereby the wetting properties of vermiculite laminates are controlled by the hydrated cations on the surface and in the interlamellar space. We find that vermiculite laminates can be tuned from superhydrophilic to hydrophobic simply by exchanging the cations; hydrophilicity decreases with increasing cation hydration free energy, except for lithium. The lithium-exchanged vermiculite laminate is found to provide a superhydrophilic surface due to its anomalous hydrated structure at the vermiculite surface. Building on these findings, we demonstrate the potential application of superhydrophilic lithium exchanged vermiculite as a thin coating layer on microfiltration membranes to resist fouling, and thus, we address a major challenge for oil–water separation technology. Manipulation of surface energy and wetting properties of solids may impact a variety of processes, including membrane fouling. Here the authors tune properties of vermiculite laminates from superhydrophilic to hydrophobic by cation exchange, and demonstrate potential for fouling resistant oil–water separation.

Intelligent transport of molecular species across different barriers is critical for various biological functions and is achieved through the unique properties of biological membranes 1 – 4 . Two essential features of intelligent transport are the ability to (1) adapt to different external and internal conditions and (2) memorize the previous state 5 . In biological systems, the most common form of such intelligence is expressed as hysteresis 6 . Despite numerous advances made over previous decades on smart membranes, it remains a challenge to create a synthetic membrane with stable hysteretic behaviour for molecular transport 7 – 11 . Here we demonstrate the memory effects and stimuli-regulated transport of molecules through an intelligent, phase-changing MoS 2 membrane in response to external pH. We show that water and ion permeation through 1T′ MoS 2 membranes follows a pH-dependent hysteresis with a permeation rate that switches by a few orders of magnitude. We establish that this phenomenon is unique to the 1T′ phase of MoS 2 , due to the presence of surface charge and exchangeable ions on the surface. We further demonstrate the potential application of this phenomenon in autonomous wound infection monitoring and pH-dependent nanofiltration. Our work deepens understanding of the mechanism of water transport at the nanoscale and opens an avenue for the development of intelligent membranes. We demonstrate the memory effects and stimuli-regulated transport of molecules through an intelligent, phase-changing MoS 2 membrane in response to external pH, a phenomenon unique to the 1T′ phase of MoS 2 .

Intelligent transport of molecular species across different barriers is critical for various biological functions and is achieved through the unique properties of biological membranes . Two essential features of intelligent transport are the ability to (1) adapt to different external and internal conditions and (2) memorize the previous state . In biological systems, the most common form of such intelligence is expressed as hysteresis . Despite numerous advances made over previous decades on smart membranes, it remains a challenge to create a synthetic membrane with stable hysteretic behaviour for molecular transport . Here we demonstrate the memory effects and stimuli-regulated transport of molecules through an intelligent, phase-changing MoS membrane in response to external pH. We show that water and ion permeation through 1T' MoS membranes follows a pH-dependent hysteresis with a permeation rate that switches by a few orders of magnitude. We establish that this phenomenon is unique to the 1T' phase of MoS , due to the presence of surface charge and exchangeable ions on the surface. We further demonstrate the potential application of this phenomenon in autonomous wound infection monitoring and pH-dependent nanofiltration. Our work deepens understanding of the mechanism of water transport at the nanoscale and opens an avenue for the development of intelligent membranes.

Van der Waals (vdW) heterostructures continue to attract intense interest as a route of designing materials with novel properties that cannot be found in naturally occurring materials. Unfortunately, this approach is currently limited to only a few layers that can be stacked on top of each other. Here we report a bulk material consisting of superconducting monolayers interlayered with monolayers displaying charge density waves (CDW). This bulk vdW heterostructure is created by phase transition of 1T-TaS2 to 6R at 800 {\\deg}C in an inert atmosphere. Electron microscopy analysis directly shows the presence of alternating 1T and 1H monolayers within the resulting bulk 6R phase. Its superconducting transition (Tc) is found at 2.6 K, exceeding the Tc of the bulk 2H phase of TaS2. The superconducting temperature can be further increased to 3.6 K by exfoliating 6R-TaS2 and then restacking its layers. Using first-principles calculations, we argue that the coexistence of superconductivity and CDW within 6R-TaS2 stems from amalgamation of the properties of adjacent 1H and 1T monolayers, where the former dominates the superconducting state and the latter the CDW behavior.

The surface free energy is one of the most fundamental properties of solids, hence, manipulating the surface energy and thereby the wetting properties of solids, has tremendous potential for various physical, chemical, biological as well as industrial processes. Typically, this is achieved by either chemical modification or by controlling the hierarchical structures of surfaces. Here we report a phenomenon whereby the wetting properties of vermiculite laminates are controlled by the hydrated cations on the surface and in the interlamellar space. We find that by exploiting this mechanism, vermiculite laminates can be tuned from superhydrophillic to hydrophobic simply by exchanging the cations; hydrophilicity decreases with increasing cation hydration free energy, except for lithium. Lithium, which has a higher hydration free energy than potassium, is found to provide a superhydrophilic surface due to its anomalous hydrated structure at the vermiculite surface. Building on these findings, we demonstrate the potential application of superhydrophilic lithium exchanged vermiculite as a thin coating layer on microfiltration membranes to resist fouling, and thus, we address a major challenge for oil-water separation technology.

Intelligent transport of molecular species across different barriers is critical for various biological functions and is achieved through the unique properties of biological membranes. An essential feature of intelligent transport is the ability to adapt to different external and internal conditions and also the ability to memorise the previous state. In biological systems, the most common form of such intelligence is expressed as hysteresis. Despite numerous advances made over previous decades on smart membranes, it is still a challenge for a synthetic membrane to display stable hysteretic behaviour for molecular transport. Here we show the memory effects and stimuli regulated transport of molecules through an intelligent phase changing MoS\\(_2\\) membrane in response to external pH. We show that water and ion permeation through 1T' MoS\\(_2\\) membranes follows a pH dependent hysteresis with a permeation rate that switches by a few orders of magnitude. We demonstrate that this phenomenon is unique to the 1T' phase of MoS\\(_2\\) due to the presence of surface charge and exchangeable ions on the surface. We further demonstrate the potential application of this phenomenon in autonomous wound infection monitoring and pH-dependent nanofiltration. Our work significantly deepens understanding of the mechanism of water transport at the nanoscale and opens an avenue for developing neuromorphic applications, smart drug delivery systems, point-of-care diagnostics, smart sensors, and intelligent filtration devices.