RESUMEN
Laser carbonization is a rapid method to produce functional carbon materials for electronic devices, but many typical carbon precursors are not sustainable and/or require extensive processing for electrochemical applications. Here, a sustainable concept to fabricate laser patterned carbon (LP-C) electrodes from biomass-derived sodium lignosulfonate, an abundant waste product from the paper industry is presented. By introducing an adhesive polymer interlayer between the sodium lignosulfonate and a graphite foil current collector, stable, abrasion-resistant LP-C electrodes can be fabricated in a single laser irradiation step. The electrode properties can be systematically tuned by controlling the laser processing parameters. The optimized LP-C electrodes demonstrate a promising performance in supercapacitors and electrochemical dopamine biosensors. They exhibit high areal capacitances of 38.9 mF cm-2 in 1 M H2SO4 and high energy and power densities of 4.3 µW h cm-2 and 16 mW cm-2 in 17 M NaClO4, showing the best performance among biomass-derived LP-C materials reported so far. After 20 000 charge/discharge cycles, they retain a high capacitance of 81%. Dopamine was linearly detected in the range of 0.1 to 20 µM with an extrapolated limit of detection of 0.5 µM (S/N = 3) and high sensitivity (13.38 µA µM-1 cm-2), demonstrating better performance than previously reported biomass-derived LP-C dopamine sensors.
RESUMEN
Triazine-based graphitic carbon nitride is a semiconductor material constituted of cross-linked triazine units, which differs from widely reported heptazine-based carbon nitrides. Its triazine-based structure gives rise to significantly different physical chemical properties from the latter. However, it is still a great challenge to experimentally synthesize this material. Here, we propose a synthesis strategy via vapor-metal interfacial condensation on a planar copper substrate to realize homogeneous growth of triazine-based graphitic carbon nitride films over large surfaces. The triazine-based motifs are clearly shown in transmission electron microscopy with high in-plane crystallinity. An AB-stacking arrangement of the layers is orientationlly parallel to the substrate surface. Eventually, the as-prepared films show dense electrochemical lithium deposition attributed to homogeneous charge transport within this thin film interphase, making it a promising solution for energy storage.
RESUMEN
Developing high-performance carbonaceous anode materials for sodium-ion batteries (SIBs) is still a grand quest for a more sustainable future of energy storage. Introducing sulfur within a carbon framework is one of the most promising attempts toward the development of highly efficient anode materials. Herein, a microporous sulfur-rich carbon anode obtained from a liquid sulfur-containing oligomer is introduced. The sodium storage mechanism shifts from surface-controlled to diffusion-controlled at higher synthesis temperatures. The different storage mechanisms and electrode performances are found to be independent of the bare electrode material's interplanar spacing. Therefore, these differences are attributed to an increased microporosity and a thiophene-rich chemical environment. The combination of these properties enables extending the plateau region to higher potential and achieving reversible overpotential sodium storage. Moreover, in-operando small-angle X-ray scattering (SAXS) reveals reversible electron density variations within the pore structure, in good agreement with the pore-filling sodium storage mechanism occurring in hard carbons (HCs). Eventually, the depicted framework will enable the design of high-performance anode materials for sodium-ion batteries with competitive energy density.
RESUMEN
Sustainable, high-performance carbonaceous anode materials are highly required to bring sodium-ion batteries to a more competitive level. Here, we exploit our expertise to control the deposition of a nm-sized conformal coating of carbon nitride with tunable thickness to improve the electrochemical performance of anode material derived from sodium lignosulfonate. In this way, we significantly enhanced the electrochemical performances of the electrode, such as the first cycle efficiency, rate-capability, and specific capacity. In particular, with a 10 nm homogeneous carbon nitride coating, the specific capacity is extended by more than 30% with respect to the bare carbon material with an extended plateau capacity, which we attribute to a heterojunction effect at the materials' interface. Eventually, the design of (inter)active electrochemical interfaces will be a key step to improve the performance of carbonaceous anodes with a negligible increase in the material weight.
RESUMEN
In this work, we report the fabrication of continuous transparent and flexible supercapacitors by depositing a CNT network onto a polymer electrolyte membrane directly from an aerogel of ultra-long CNTs produced floating in the gas phase. The supercapacitors show a combination of a power density of 1370 kW kg-1 at high transmittance (ca. 70%), and high electrochemical stability during extended cycling (>94% capacitance retention over 20 000 cycles) and against repeated 180° flexural deformation. They represent a significant enhancement of 1-3 orders of magnitude compared to prior state-of-the-art transparent supercapacitors based on graphene, CNTs, and rGO. These features mainly arise from the exceptionally long length of CNTs, which makes the material behave as a bulk conductor instead of an aspect ratio-limited percolating network, even for electrodes with >90% transparency. The electrical and capacitive figures-of-merit for the transparent conductor are FoMe = 2.7, and FoMc = 0.46 F S-1 cm-2 respectively.
RESUMEN
The assembly of aligned carbon nanotubes (CNTs) into fibers (CNTFs) is a convenient approach to exploit and apply the unique physico-chemical properties of CNTs in many fields. CNT functionalization has been extensively used for its implementation into composites and devices. However, CNTF functionalization is still in its infancy because of the challenges associated with preservation of CNTF morphology. Here, we report a thorough study of the gas-phase functionalization of CNTF assemblies using ozone which was generated in situ from a UV source. In contrast with liquid-based oxidation methods, this gas-phase approach preserves CNTF morphology, while notably increasing its hydrophilicity. The functionalized material is thoroughly characterized by Raman spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy, and scanning electron microscopy. Its newly acquired hydrophilicity enables CNTF electrochemical characterization in aqueous media, which was not possible for the pristine material. Through comparison of electrochemical measurements in aqueous electrolytes and ionic liquids, we decouple the effects of functionalization on pseudocapacitive reactions and quantum capacitance. The functionalized CNTF assembly is successfully used as an active material and a current collector in all-solid supercapacitor flexible devices with an ionic liquid-based polymer electrolyte.
RESUMEN
This work presents a method to produce structural composites capable of energy storage. They are produced by integrating thin sandwich structures of CNT fiber veils and an ionic liquid-based polymer electrolyte between carbon fiber plies, followed by infusion and curing of an epoxy resin. The resulting structure behaves simultaneously as an electric double-layer capacitor and a structural composite, with flexural modulus of 60 GPa and flexural strength of 153 MPa, combined with 88 mF/g of specific capacitance and the highest power (30 W/kg) and energy (37.5 mWh/kg) densities reported so far for structural supercapacitors. In-situ electrochemical measurements during 4-point bending show that electrochemical performance is retained up to fracture, with minor changes in equivalent series resistance for interleaves under compressive stress. En route to improving interlaminar properties we produce grid-shaped interleaves that enable mechanical interconnection of plies by the stiff epoxy. Synchrotron 3D X-ray tomography analysis of the resulting hierarchical structure confirms the formation of interlaminar epoxy joints. The manuscript discusses encapsulation role of epoxy, demonstrated by charge-discharge measurements of composites immersed in water, a deleterious agent for ionic liquids. Finally, we show different architectures free of current collector and electrical insulators, in which both CNT fiber and CF act as active electrodes.