Towards high-efficient microsupercapacitors based on reduced graphene oxide with optimized reduction degree


Reduced graphene oxide aerogels synthetized using different times of hydrothermal treatment have been tested as raw material to prepare electrochemical supercapacitors. The gravimetric electrochemical capacitance measured using 1M Na2SO4 as electrolyte was maximized for aerogels that underwent 45 min of hydrothermal treatment. The aerogels synthetized for longer durations of hydrothermal treatment exhibited higher electrical conductivity but the gravimetric capacitance drops dramatically due to an increasing resistance to diffusion of the electrolyte ions. The impeded diffusion is boosted by the intensified crosslinking between graphene sheets, which narrows the pores between them in the prepared electrode. The rGO aerogel attained for 45 min of hydrothermal treatment provided a high gravimetric capacitance of 400 F g-1 and 100 F g-1 at 50 A g-1 for three-electrode and two electrodes configuration, respectively, as well as good cyclic stability, competing with other similar carbon materials. Activation pretreatments or adding a second component (glucose, dopamine, Mn, Fe, CNT) did not provide significant change of capacitance respect to pristine rGO aerogel.

Unique Properties and Behavior of Nonmercerized Type-II Cellulose Nanocrystals as Carbon Nanotube Biocompatible Dispersants

Biomacromolecules 2019, 20, 8, 3147-3160

Nanocellulose is increasingly being investigated as a paradigm of a sustainable nanomaterial because of its extraordinary physical and chemical properties, together with its renewable nature and worldwide abundance. The rich structural diversity of cellulose materials is represented by different crystalline allomorphs, from which types I and II stand out. While type I is naturally and ubiquitously present, type II is man-made and requires harsh and caustic synthesis conditions such as the so-called mercerization process. Here, we provide an optimal scenario to obtain either type-I or II nanocrystalline cellulose (NCC) by a mercerization-free method consisting only of the acid hydrolysis commonly used to produce nanocellulose from microcellulose. The possibility of having nonmercerized type-II NCC acquires a great relevance since this nanostructure shows particularly appealing properties. Moreover, an entangled and wrapped system arises when used as a dispersing agent for single-walled carbon nanotubes (SWCNTs), significantly different from that of type I. The biological testing of each NCC type and their respective SWCNT–NCC dispersions in human intestinal (Caco-2) cells reveals a general innocuous behavior in both cancer and normal stages of differentiation; however, the type-II-based SWCNT–NCC dispersions display cytotoxicity for cancer cells while enhancing mitochondrial metabolism of normal cells.

Chemical Postdeposition Treatments To Improve the Adhesion of Carbon Nanotube Films on Plastic Substrates

ACS OMEGA, 2019, 4(2), pp 2804-2811

The robust adhesion of single-walled carbon nanotubes (SWCNTs) to plastic substrates is a key issue toward their use in flexible electronic devices. In this work, semitransparent SWCNT films were prepared by spray-coating on two different plastic substrates, specifically poly(ethylene terephthalate) and poly(vinylidene fluoride). The deposited SWCNT films were treated by dipping in suitable solvents separately, namely, 53% nitric acid (HNO3) and N-methyl pyrrolidone. Direct evidence of SWCNT adhesion to the substrate was obtained by a peel-off test carried out with an adhesive tape. Moreover, these treatments caused enhanced film transparency and electrical conductivity. Electron microscopy images suggested that SWCNTs were embedded in the plastic substrates, forming a thin layer of conductive composite materials. Raman spectroscopy detected a certain level of doping in the SWCNTs after the chemical …

Photoactivity improvement of TiO2 electrodes by thin hole transport layers of reduced graphene oxide

Electrochimica Acta,  2019, 298,  Pages 279-287

Nanostructured TiO2 and graphene-based materials constitute components of actual interest in devices related to solar energy conversion and storage. In this work, we show that a thin layer of electrochemically reduced graphene oxide (ECrGO), covering nanostructured TiO2 photoelectrodes, can significantly improve the photoactivity. In order to understand the working principle, ECrGO/TiO2 photoelectrodes with different ECrGO thicknesses were prepared and studied by a set of photoelectrochemical measurements. Methanol in alkaline conditions was employed as effective hole acceptor probe to elucidate the electronic phenomena in the electrode layers and interfaces. These studies underline the hole accepting properties of ECrGO and reveal the formation of a p-n junction at the interface between ECrGO and TiO2. It is shown for the first time that the resulting space charge region of about 10 nm defines the …

Reduced Graphene Oxide Aerogels with Controlled Continuous Microchannels for Environmental Remediation

ACS Appl. Nano Mater., 2019, 2 (3), pp 1210–1222

3D porous graphene microarchitectures with aligned and continuous channels are of paramount interest for several applications such as pollutant removal, energy storage, or biomedical engineering. For these applications, an accurate control over the pore microstructure is of capital importance. Freeze casting is a well-stablished technique to prepare graphene aerogels with unidirectional channels. This technique is typically applied to plain GO colloids, leading to discontinuous microchannels. Herein we have carried out the freeze process starting directly with partially reduced graphene (rGO) hydrogels prepared by a prior hydrothermal treatment in autoclave. This approach leads to the formation of aerogels with aligned and continuous microchannels, enabled by an intermediate cross-linking degree of the rGO nanosheets, carefully controlled by keeping the time of the prior hydrothermal process between the thresholds of 45–75 min. To the best of our knowledge, the effect of the degree of cross-linking in the freeze casting process is not yet reported. The resulting rGO aerogels with highly aligned microchannel structure reveal superior properties over its isotropic counterpart of randomly oriented pores for the absorption of nonpolar solvents and the selective adsorption of an aromatic compound dissolved in an alkane. Our combined hydrothermal freeze casting approach thus affords aligned microchannel rGO aerogels of enormous potential for environmental remediation.