Startseite Assessing the effect of light intensity and light wavelength spectra on the photoreduction of formic acid using a graphene oxide material
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Assessing the effect of light intensity and light wavelength spectra on the photoreduction of formic acid using a graphene oxide material

  • Luis A. Ramos-Huerta , Lotte Laureys , Alexis G. Llanos , Patricio J. Valadés , Richard S. Ruiz und Carlos O. Castillo ORCID logo EMAIL logo
Veröffentlicht/Copyright: 24. August 2020
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Abstract

Photocatalysis has been a topic of interest in recent years for both, oxidation and reduction reactions, and although there is a broad variety of research regarding photocatalytic materials and the reaction itself, studies on reactor design and related phenomena, radiation transfer and its direct impact on reaction extent specifically, are usually neglected. From this end, the present work focuses on the elucidation of the effect of light intensity and wavelength spectra in the visible light region during the photoreduction reaction of formic acid using graphene oxide as a promising catalyst. By using formic acid, one of the main intermediaries in the photoreduction of carbon dioxide, the possibility of methanol production is evaluated without the thermodynamic constraints presented by carbon dioxide. A graphene oxide material, synthetized through a modified Hummer’s method, is assessed for the reduction of formic acid evaluating four different light sources (red, green, blue and white). An analysis of energy balances in the reaction set-up allows the determination of both the energy absorbed by the GO photocatalyst and isoactinity conditions at studied radiative operating conditions. At an isoactinity environment, the adsorption rate of formic acid and production rate of methanol are then evaluated, relating them to the absorbed energy achieved at the wavelength spectra and light intensities evaluated; IR spectroscopy is utilized to follow formic acid concentration as well as methanol production. The largest initial reaction rate (ca. 57%) relates to the use of the red wavelength at its largest intensity. Reaction rates at larger times start to be apparent being affected by adsorption, reaction and radiation conditions. The maximum conversion, 14%, is attained by using the white wavelength spectra at its lowest intensity. Thus, higher intensities will not necessarily yield higher conversions, nor the highest reaction rates. This, in turn, poses the necessity of quick, reliable assessments for whichever catalyst used in this type of reactions that leads to the correct election of operating conditions that maximize the product yield. Independent evaluation for every wavelength within the visible spectra and assessing carbon dioxide photoreduction are future steps into the elucidation of solar fuel production feasibility.


Corresponding author: Carlos O. Castillo, Laboratory of Catalytic Reactor Engineering Applied to Chemical and Biological Systems, Universidad Autónoma Metropolitana-Iztapalapa, Departamento de Ingeniería de Procesos e Hidráulica, 09340 Mexico City, Mexico,

Funding source: Authors express their gratitude to the Mexican National Council for Science and Technology (CONACYT) and Metropolitan Autonomous University, Iztapalapa, for financing this work

References

Anpo, M., H. Yamashita, Y. Ichihashi, and S. Ehara. 1995. “Photocatalytic Reduction of CO2 with H2O on Various Titanium Oxide Catalysts.” Journal of Electroanalytical Chemistry 396: 21–6, https://doi.org/10.1016/0022-0728(95)04141-A.Suche in Google Scholar

Brucato, A., F. Grisafi, L. Rizzuti, A. Sclafani, and G. Vella. 2007. “Quasi-Isoactinic Reactor for Photocatalytic Kinetics Studies.” Industrial & Engineering Chemistry Research 46: 7684–90, https://doi.org/10.1021/ie0703991.Suche in Google Scholar

Chen, C., W. Cai, M. Long, B. Zhou, Y. Wu, D. Wu, and Y. Feng. 2010. “Synthesis of Visible-Light Responsive Graphene Oxide/TiO2 Composites with P/n Heterojunction.” ACS Nano 4: 6425–32, https://doi.org/10.1021/nn102130m.Suche in Google Scholar PubMed

Eskandarian, M. R., H. Choi, M. Fazli, and M. H. Rasoulifard. 2016. “Effect of UV-LED Wavelengths on Direct Photolytic and TiO2 Photocatalytic Degradation of Emerging Contaminants in Water.” Chemical Engineering Journal, https://doi.org/10.1016/j.cej.2016.05.049.Suche in Google Scholar

Formic Acid [WWW Document], n.d. https://webbook.nist.gov/cgi/cbook.cgi?ID=C64186&Type=IR-SPEC&Index=1 (accessed November 20, 2019).Suche in Google Scholar

Geim, A. K. and K. S. Novoselov. 2007. “The Rise of Graphene.” Nature Materials 6: 183–91, https://doi.org/10.1038/nmat1849.Suche in Google Scholar PubMed

Glaze, W. H., J.-W. Kang, and D. H. Chapin. 1987. “The Chemistry of Water Treatment Processes Involving Ozone, Hydrogen Peroxide and Ultraviolet Radiation.” Ozone Science & Engineering 9: 335–52, https://doi.org/10.1080/01919518708552148.Suche in Google Scholar

Hsu, H. C., I. Shown, H. Y. Wei, Y. C. Chang, H. Y. Du, Y. G. Lin, C. A. Tseng, C. H. Wang, L. C. Chen, Y. C. Lin, and K. H. Chen. 2013. “Graphene Oxide as a Promising Photocatalyst for CO2 to Methanol Conversion.” Nanoscale 5: 262–8, https://doi.org/10.1039/c2nr31718d.Suche in Google Scholar PubMed

Inoue, T., A. Fujishima, S. Konishi, and K. Honda. 1979. “Photoelectrocatalytic Reduction of Carbon Dioxide in Aqueous Suspensions of Semiconductor Powders.” Nature 277: 637–3, https://doi.org/10.1038/277637a0.Suche in Google Scholar

Li, K., X. An, K. H. Park, M. Khraisheh, and J. Tang. 2014. “A Critical Review of CO2 Photoconversion: Catalysts and Reactors.” Catalysis Today 224: 3–12, https://doi.org/10.1016/j.cattod.2013.12.006.Suche in Google Scholar

Li, X., J. Wen, J. Low, Y. Fang, and J. Yu. 2014. “Design and Fabrication of Semiconductor Photocatalyst for Photocatalytic Reduction of CO2 to Solar Fuel.” Science China Materials 57: 70–100, https://doi.org/10.1007/s40843-014-0003-1.Suche in Google Scholar

Liu, B. and X. Zhao. 2010. “A Kinetic Model for Evaluating the Dependence of the Quantum Yield of Nano-TiO2 Based Photocatalysis on Light Intensity, Grain Size, Carrier Lifetime, and Minority Carrier Diffusion Coefficient: Indirect Interfacial Charge Transfer.” Electrochimica Acta 55: 4062–70, https://doi.org/10.1016/j.electacta.2010.01.087.Suche in Google Scholar

Marugán, J., R. van Grieken, C. Pablos, M. L. Satuf, A. E. Cassano, and O. M. Alfano. 2013. “Modeling of a Bench-Scale Photocatalytic Reactor for Water Disinfection from Laboratory-Scale Kinetic Data.” Chemical Engineering Journal 224: 39–45, https://doi.org/10.1016/j.cej.2012.11.082.Suche in Google Scholar

Ola, O., and M. M. Maroto-Valer. 2015. “Review of Material Design and Reactor Engineering on TiO2 Photocatalysis for CO2 Reduction.” Journal of Photochemistry and Photobiology C: Photochemistry Reviews, https://doi.org/10.1016/j.jphotochemrev.2015.06.001.Suche in Google Scholar

Song, P., X. Zhang, M. Sun, X. Cui, and Y. Lin. 2012. “Graphene Oxide Modified TiO2 Nanotube Arrays: Enhanced Visible Light Photoelectrochemical Properties.” Nanoscale 4: 1800–4, https://doi.org/10.1039/c2nr11938b.Suche in Google Scholar PubMed

Valadés-Pelayo, P. J., J. Moreira del Rio, P. Solano-Flores, B. Serrano, and H. de Lasa. 2014. “Establishing Photon Absorption Fields in a Photo-CREC Water II Reactor Using a CREC-Spectroradiometric Probe.” Chemical Engineering Science 116: 406–17, https://doi.org/10.1016/j.ces.2014.04.041.Suche in Google Scholar

Wang, J. and R.J. Boyd. 1996. “A Hybrid Quantum Mechanical Force Field Molecular Dynamics Simulation of Liquid Methanol: Vibrational Frequency Shifts as a Probe of the Quantum Mechanical/molecular Mechanical Coupling.” Journal Chemical Physics 104: 7261–9, https://doi.org/10.1063/1.471439.Suche in Google Scholar

Received: 2020-01-07
Accepted: 2020-07-21
Published Online: 2020-08-24

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Heruntergeladen am 24.9.2025 von https://www.degruyterbrill.com/document/doi/10.1515/ijcre-2020-0008/html
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