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Electrowetting is a simple way to induce the spreading and retraction of electrolyte droplets. This method is widely used in "device" applications, where a dielectric layer is applied between the electrolyte and the conducting substrate. Recent work, including contributions from our own laboratory, have shown that reversible electrowetting can be achieved directly on conductors. We have shown that graphite surfaces, in particular when combined with highly concentrated electrolyte solutions, show a strong wetting effect. The process is driven by the interactions between the electrolyte ions and the surface, hence models of double-layer capacitance are able to explain changes in the equilibrium contact angles. Herein, we extend the approach to the investigation of electrowetting on graphene samples of varying thickness, prepared by chemical vapor deposition. We show that the use of highly concentrated aqueous electrolytes induces a clear yet subtle electrowetting response due to the adsorption of ions and the suppression of the negative effect introduced by the surface impurities accumulating during the transfer process. The latter have been previously reported to fully hinder electrowetting at lower electrolyte concentrations. An amplified wetting response is recorded in the presence of strongly adsorbed/intercalated anions in both aqueous and non-aqueous electrolytes. The phenomenon is interpreted based on the anion-graphene interactions and their influence on the energetics of the interface. By monitoring the dynamics of wetting, an irreversible behaviour is identified in all cases as a consequence of the irreversibility of anion adsorption and/or intercalation. Finally, the effect of the underlying reactions on the timescales of wetting is also examined.

Wetting of carbon surfaces is one of the most widespread, yet poorly understood, physical phenomena. Control over wetting properties underpins the operation of aqueous energy-storage devices and carbon-based filtration systems. Electrowetting, the variation in the contact angle with an applied potential, is the most straightforward way of introducing control over wetting. Here, we study electrowetting directly on graphitic surfaces with the use of aqueous electrolytes to show that reversible control of wetting can be achieved and quantitatively understood using models of the interfacial capacitance. We manifest that the use of highly concentrated aqueous electrolytes induces a fully symmetric and reversible wetting behavior without degradation of the substrate within the unprecedented potential window of 2.8 V. We demonstrate where the classical "Young-Lippmann" models apply, and break down, and discuss reasons for the latter, establishing relations among the applied bias, the electrolyte concentration, and the resultant contact angle. The approach is extended to electrowetting at the liquid|liquid interface, where a concentrated aqueous electrolyte drives reversibly the electrowetting response of an insulating organic phase with a significantly decreased potential threshold. In summary, this study highlights the beneficial effect of highly concentrated aqueous electrolytes on the electrowettability of carbon surfaces, being directly related to the performance of carbon-based aqueous energy-storage systems and electronic and microfluidic devices., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

The development of intrinsically safe and environmentally sustainable energy storage devices is a significant challenge. Recent advances in aqueous rechargeable lithium-ion batteries (ARLIBs) have made considerable steps in this direction. In parallel to the ongoing progress in the design of aqueous electrolytes that expand the electrochemically stable potential window, the design of negative electrode materials exhibiting large capacity and low intercalation potential attracts great research interest. Herein, we report the synthesis of high purity nanoscale Chevrel Phase (CP) Mo 6 S 8 via a simple, efficient and controllable molecular precursor approach with significantly decreased energy consumption compared to the conventional approaches. Physical characterization of the obtained product confirms the successful formation of CP-Mo 6 S 8 and reveals that it is crystalline nanostructured in nature. Due to their unique structural characteristics, the Mo 6 S 8 nanocubes exhibit fast kinetics in a 21 m lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) electrolyte as a result of the shorter Li + ion diffusion distance. Full battery cells comprised of Mo 6 S 8 and LiMn 2 O 4 as negative and positive electrode materials, respectively, operate at 2.23 V delivering a high energy density of 85 W h kg -1 (calculated on the total mass of active materials) under 0.2 C-rate. At 4 C, the coulombic efficiency (CE) is determined to be 99% increasing to near 100% at certain cycles. Post-mortem physical characterization demonstrates that the Mo 6 S 8 anode maintained its crystallinity, thereby exhibiting outstanding cycling stability. The cell outperforms the commonly used vanadium-based (VO 2 (B), V 2 O 5 ) or (NASICON)-type LiTi 2 (PO 4 ) 3 anodes, highlighting the promising character of the nanoscale CP-Mo 6 S 8 as a highly efficient anode material. In summary, the proposed synthetic strategy is expected to stimulate novel research towards the widespread application of CP-based materials in various aqueous and non-aqueous energy storage systems.