Autor Viliam Vretenár

A comparative life cycle assessment of graphene and activated carbon in a supercapacitor application

COSSUTTA, Matteo – VRETENÁR, Viliam – CENTENO, Teresa A. – KOTRUSZ, Peter – MCKECHNIE, Jon – PICKERING, Stephen J.

In Journal of Cleaner Production. Vol. 242, iss. 1 (2020)

https://doi.org/10.1016/j.jclepro.2019.118468

Abstract

Graphene shows substantial promise in improving the technical performance of a range of applications. For its development and before its potential mass adoption, it is critical to understand the associated cradle-to-grave life cycle environmental impacts. Previous studies on graphene environmental performance do not include end of life and the potential environmental credits generated by graphene reuse. This study undertakes a cradle-to-grave approach to evaluating graphene applications, considering a case study of supercapacitors manufactured with graphene and activated carbon active materials. The analysis includes active materials commercial-size production, supercapacitors production, supercapacitors use phase in an automotive application, and their end of life in which both devices are recycled. With current material performance and energy mixes, the graphene-based supercapacitor would increase impacts in all environmental categories analysed, ranging from 27% higher human toxicity to 213% greater ozone depletion and showing a 48% increase in GHG emissions. This unfavourable result arises due to the tested graphene material exhibiting inferior specific capacitance to the activated carbon comparator, as well as a more energy-intensive production process. Prospective analysis considers hypothetical performance where both active materials reach their theoretical specific capacitance, and the decarbonisation of electricity generation. The environmental impacts of both the activated carbon and graphene supercapacitors are reduced in these prospective scenarios, with the graphene based supercapacitor becoming the least impacting solution due to its lower active material requirements. The graphene-based device shows 36% lower GHG emission and overall shows lower impacts ranging from 14% less mineral, fossil and renewable resource depletion to 43% less photochemical ozone formation. These results support graphene as a valid candidate material for substituting activated carbon in supercapacitors provided graphene technical performance is improved, production optimised, and recycling developed.

Biomass waste-carbon/reduced graphene oxide composite electrodes for enhanced supercapacitors

GUARDIA, Laura – SUÁREZ, Loreto – QUEREJETA, Nausika – VRETENÁR, Viliam – KOTRUSZ, Peter – SKÁKALOVÁ, Viera – CENTENO, Teresa A.

In Electrochimica Acta. Vol. 298, iss. 3 (2019)

https://doi.org/10.1016/j.electacta.2018.12.160

Abstract

We present a simple and effective alternative which optimizes electrodes based on low-cost carbons for high-performance supercapacitors. The combination with reduced graphene oxide (rGO) greatly improves the operation of microporous carbons easily produced by one-pot activation of grape seeds. The use of composite electrodes with rGO lowers the supercapacitor resistance and enables a much higher rate capability.

The mixture of rGO flakes and particles of a highly porous carbon obtained by KOH activation allows retaining the high capacitance of 260 F g−1 of the standard electrodes at 1 mA cm−2 in aqueous H2SO4 whereas the value at 200 mA cm−2 is increased by around 2.4 times. Consequently, at high current density, the capacitor assembled with these composites stores eight times more energy and the power density is multiplied by four.

The synergy between rGO and an ultramicroporous carbon produced by CO2-activation results extremely profitable, the cell assembled with composite electrodes reaching three times more energy and power at 200 mA cm−2 than the best performance of the standard counterpart.

More importantly, the higher density of the composite electrodes leads to a capacitance of around 200 F cm−3 which translates into a remarkable improvement in the supercapacitor operation normalized to volume.

Chemical Oxidation of Graphite: Evolution of the Structure and Properties

SKÁKALOVÁ, Viera – KOTRUSZ, Peter – JERGEL, Matej – SUSI, Toma – MITTELBERGER, Andreas – VRETENÁR, Viliam – ŠIFFALOVIČ, Peter – KOTAKOSKI, J. – MEYER, Jannik C. – HULMAN, Martin

In Journal of Physical Chemistry C. Vol. 122, iss. 1 (2018)

https://doi.org/10.1021/acs.jpcc.7b10912

Abstract

Graphene oxide is a complex material whose synthesis is still incompletely understood. To study the time evolution of structural and chemical properties of oxidized graphite, samples at different temporal stages of oxidation were selected and characterized through a number of techniques: X-ray photoelectron spectroscopy for the content and bonding of oxygen, X-ray diffraction for the level of intercalation, Raman spectroscopy for the detection of structural changes, electrical resistivity measurements for probing charge localization on the macroscopic scale, and scanning transmission electron microscopy for the atomic structure of the graphene oxide flakes. We found a nonlinear behavior of oxygen uptake with time where two concentration plateaus were identified: Uptake reached 20 at % in the first 15 min, and after 1 h a second uptake started, reaching a highest oxygen concentration of >30 at % after 2 h of oxidation. At the same time, the interlayer distance expanded to more than twice the value of graphite and the electrical resistivity increased by seven orders of magnitude. After 4 days of chemical processing, the expanded structure of graphite oxide became unstable and spontaneously exfoliated; more than 2 weeks resulted in a significant decrease in the oxygen content accompanied by reaggregation of the GO sheets. These correlated measurements allow us to offer a comprehensive view into the complex oxidation process.