Single-walled carbon nanotube (SWCNT) field-effect transistor (FET) devices have potential for memory storage applications. Devices fabricated with semiconducting SWCNT ink using dielectrophoresis were coated with a renewably sourced poly(oxacyclobutane) oligomer. It was found that this oligomer crystallizes with water to form a semicrystalline oligomer hydrate material. Crystallization also occurs on the SWCNT device surface in ambient conditions, resulting in dramatically increased hysteresis of the SWCNT-FET I-Vg curves. Using alternating current impedance measurements, we found that the oligomer hydrate crystals store charge, acting as a capacitor encapsulating the nanotube network. This capacitive material can serve to electrostatically gate the SWCNT network. The charge storage properties of the oligomer hydrate crystals were applied to store “0” and “1” bits separated by ∼4 orders of magnitude of current. Utilizing powder X-ray diffraction and simulation, we have demonstrated that this semicrystalline material contains aligned, hydrogen-bonded one-dimensional columns of water molecules which allows for charging of the material through electrostatic gating by mobile protons in the crystal structure.
Zinc/bromine flow batteries are a promising solution for utility-scale electrical energy storage. The behavior of complex Zn–halogen species in the electrolyte during charge and discharge is currently not well-understood, and is an important aspect to be addressed in order to facilitate future electrolyte formulations. The speciation of the primary zinc bromide electrolyte with and without a secondary zinc chloride electrolyte is studied in the present work. Raman spectroscopy was carried out on aqueous solutions of zinc bromide at 5 concentrations (2–4 M) to account for the initial and later stages of charging, with 3 concentrations (1–2 M) of zinc chloride. Mixed solutions containing various combinations of each primary and secondary electrolyte concentrations were also studied. Semi-quantitative analysis of peaks after Gaussian and Lorentzian peak deconvolution showed that the proportion of four-ligand coordinated Zn–halides (i.e. [ZnBr4]2− and [ZnCl4]2−) increases with higher salt concentration, as compared to complexes with lower halide coordination numbers. The presence of a previously unassigned peak was observed at the 220 cm−1 band in the Raman spectra of mixed electrolytes. Results from ab-initio molecular modeling using the GAUSSIAN 16 software package suggests this peak is due to the presence of the hybrid-halide anionic complex [ZnBr2Cl(H2O)]–. Increasing the Cl:Br ratio in electrolytes promotes hybridization and subsequently decreasing the proportion of single-halide Zn–Br complexes. While this speciation study is focused on Zn/Br batteries, the findings are also potentially applicable to other energy storage and electrochemical systems containing zinc halide electrolytes.
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