arXiv subjects

Juan José Vilatela

Publications and source records attributed to Juan José Vilatela.

5 recordsLinked to original sources

arXiv2021

Pore structure and electrochemical properties of CNT-based electrodes studied by in situ small/wide angle X-ray scattering

Macroscopic ensembles of nanocarbons, such as fibres of carbon nanotubes (CNT), are characterised by a complex hierarchical structure combining coherent crystalline regions with a large porosity arising from imperfect packing of the large rigid building blocks. Such structure is at the centre of a wide range of charge storage and transfer processes when CNT fibres are used as electrodes and/or current collectors. This work introduces a method based on wide and small-angle X-ray scattering (WAXS/SAXS) to obtain structural descriptors of CNT fibres and which enables in situ characterisation during electrochemical processes. It enables accurate determination of parameters such as specific surface area, average pore size and average bundle size from SAXS data after correction for scattering from density fluctuations arising from imperfect packing of graphitic planes. In situ and ex situ WAXS/SAXS measurements during electrochemical swelling of CNT fibre electrodes in ionic liquid provide continuous monitoring of the increase in effective surface area caused by electrostatic separation of CNT bundles in remarkable agreement with capacitance changes measured independently. Relative contributions from quantum and Helmholtz capacitance to total capacitance remaining fairly constant. The WAXS/SAXS analysis is demonstrated for fibres of either multi- and single-walled CNTs, and is expected to be generally applicable to operando studies on nanocarbon-based electrodes used in batteries, actuators and other applications

physics.app-ph↗

arXiv2021

Photoelectrocatalytic detection of NADH on n-type silicon semiconductors facilitated by carbon nanotube fibers

NADH is a key biomolecule involved in many biocatalytic processes as cofactor and its quantification can be correlated to specific enzymatic activity. Many efforts have been taken to obtain clean electrochemical signals related to NADH presence and lower its redox overpotential to avoid interferences. Suppression of background and secondary signals can be achieved by including a switchable electroactive surface, for instance, by using semiconductors able to harvest light energy and drive the excited electrons only when irradiated. Here we present the combination of a n-type Si semiconductor with fibers made of carbon nanotubes as electroactive surface for NADH quantification at low potentials only upon irradiation. The resulting photoelectrode responded linearly to NADH concentrations from 50 μ M to 1.6 mM with high sensitivity (54 $μ$ A cm$^{-2}$ mM${-1}$). This system may serve as a biosensing platform for detection and quantification of dehydrogenases activity.

physics.app-ph↗

arXiv2020

Understanding interlaminar toughening of unidirectional CFRP laminates with carbon nanotube veils

The introduction of nanostructured interlayers is one of the most promising strategies for interlaminar reinforcement in structural composites. In this work, we study the failure mechanism and interlayer microstructure of aerospace-grade structural composites reinforced with thin veils of carbon nanotube produced using an industrialised spinning process. Samples of unidirectional carbon fibre/epoxy matrix composites interleaved with different composition CNT veils were prepared using hot press method and tested for interlaminar fracture toughness (IFT), measured in Mode-I (opening) and Mode-II (in-plane shear), and for interlaminar shear strength (ILSS), evaluated by the short beam shear (SBS) test. The crack propagation mode could be directly determined through fractography analysis by electron microscopy and resin/CNT spatial discrimination by Raman spectroscopy, showing a clear correlation between interlaminar reinforcement and the balance between cohesive/adhesive failure mode at the interlayer region. Composites with full resin infiltration of the CNT veils give a large increase of Mode II IFT (88%) to 1500 J/m2 and a slight enhancement of apparent interlaminar shear strength (6.5%), but a decrease of Mode I IFT (-21%). The results help establish the role of interlayer infiltration, interlaminar crossings and formation of a carbon fibre bridgings, for interlaminar reinforcement with interleaves.

cond-mat.mtrl-sci↗

arXiv2020

Revealing the Mechanism of Electrochemical Lithiation of Carbon Nanotube Fibers

Fabrics of continuous fibers of carbon nanotubes (CNTFs) are attractive materials for multifunctional energy storage devices, either as current collector, or as active material. Despite a similar chemical composition, lithiation/delithiation in CNTFs is substantially different from traditional graphite electrodes. In CNTFs this process is dominated by surface processes, insertion in the bundles interstices, electrochemical doping and often-overlooked partial degradation of the sp2 lattice upon cycling. Through extensive electrochemical analysis, together with in situ Raman spectroscopy measurements, we analyzed the complex lithiation behavior of highly crystalline fibers of CNTs. CNTF can store lithium reversibly with high specific capacity and rate capability, thanks to a large capacitive contribution. Upon lithiation, they undergo electrochemical doping, with longitudinal conductivity increasing by as much as 100 %, concomitant with large downshifts in Raman spectra. However, CNTF are also affected by high first-cycle irreversible capacity, voltage hysteresis and amorphization upon cycling. Electrochemical analysis confirms that SEI formation is responsible for the first-cycle irreversible capacity. Voltage hysteresis is attributed primarily to the trapping of lithium ions in the interstices between stacked nanotubes. Another dominant feature is pre-existing defects, which promote capacitive storage but lead to progressive amorphization of the CNTFs. Indeed, it is evidenced that undesired amorphization is hindered in ultra-pure CNTF without pre-existing defects.

physics.app-ph↗

arXiv2019

Interlaminar toughening in structural carbon fiber/epoxy composites interleaved with carbon nanotube veils

The susceptibility to delamination is one of the main concerns in fiber reinforced polymer composites (FRPs). This work demonstrates improvements of 60% in Mode-I fracture toughness after integration of thin (~30 micron), continuous veils of carbon nanotubes (CNTs) directly deposited onto carbon fiber fabric as the CNT are drawn from the gas-phase using a semi-industrial process. A combination of optical imaging, scanning electron microscopy and a Raman spectroscopy provide a new rapid tool to unambiguously determine the crack propagation path by simple visual inspection of fracture surface. The results show that interlaminar crossing between CNT veil/CF interfaces is of paramount importance. The crack front alternatingly propagates above and below the CNT-toughened interlayer, significantly improving the fracture toughness of resultant laminates. This mechanism is strongly influenced by the method used to integrate the veils onto the CF. CNT veils directly deposited onto the fabrics as a low-density layer lead to large improvements in interlaminar properties, whereas compact CNT veils densified by solvent exposure prior to their integration in the lay-up act as defects.

physics.app-ph↗