FONDECYT Initiation: Computational chemistry for elucidating reaction mechanisms of graphene with relevant oxygen containing molecules
Funded by ANID-Chile through the FONDECYT INITIATION scheme.
Index
Role
As principal investigator of this project, I was in change of selecting the necessary equipment and preparing a training course for theses students working in this project. Three theses were supervised in order to complete the objectives, and three more are derived from this project. Finally, the scientific outcomes were presented in conferences and later transformed into publications. Relationships with other group had multiple positive impacts in our work.
Dr. Andrea Oyarzún
Principal investigator, Professor at Universidad de Magallanes.
Objective
This project aims to better understand the reaction mechanisms of the reactions of graphene with O2, NO, NO2, N2O, H2O, CO2 and for comparison H2 has been included.
Outcomes
This project studied oxygen transfer reaction mechanisms. We focused into the mechanistic differences of the graphene reaction with H2O and CO2, including the effect of zigzag vs. armchair sites and their availability, also comparing with previous work on the NO and O2 reactions. We also compared models of graphene clusters vs. the extended edges of nanoribbons. We briefly studied the reaction of graphene with NO, N2O and NO2, and we made emphasis on the interactions of curved and non-curved extended edges with H2 and O2. An experimental plan was prepared to better understand the NO reaction, but the experiment was postponed due to the pandemic. Publications and manuscripts include thermodynamic and kinetics information of the reactions, and databases with calculated files and multimedia information. Three theses, one of them about NOx pollution, and a collaboration proposal with a soot formation modeling group were written. Three derived theses and a manuscript are in development.
Publications
We finished an article, published two more, and wrote two more manuscripts. We also presented four conference papers.
Published
1. Oyarzún-Aravena, A.M., Gottschalk-Ojeda, C., Moya-Barría, I., and Vallejos-Burgos, F., Edge type effect in the gasification mechanism of graphene clusters with H2O and/or CO2: armchair vs. zigzag. Carbon, 2022. 193: p. 412-427.
2. Oyarzún-Aravena, A. M., Moya-Barría, I. I. & Navarro-Pérez, D. J. (2022). Formación en química computacional y sus aplicaciones a través de un proyecto de investigación desarrollado en la Patagonia chilena. Formación universitaria, 15103-116.
3. Oyarzún, A., García, X., and Radovic, L., IRC data for a mechanistic route starting with H2O adsorption and finishing with H2 desorption from graphene. Data in Brief, 2020. 30: p. 105362.
4. Oyarzún, A.M., García-Carmona, X., and Radovic, L.R., Kinetics of oxygen transfer reactions on the graphene surface. Part II. H2O vs. CO2. Carbon, 2020. 164: p. 85-99.
5. Oyarzún, A.M., Latham, C.D., Radovic, L.R., Briddon, P.R., and Rayson, M.J., Spin density distributions on graphene clusters and ribbons with carbene-like active sites. PCCP, 2018. 20(42): p. 26968-26978.
Manuscripts
(All currently published)
Two in development.
Conference papers
1. Oyarzún-Aravena, A. and Gottschalk-Ojeda, C., Poster: Graphene reactions with water and carbon dioxide on armchair sites., in Carbon 2019. 2019: Lexington, USA.
2. Oyarzún-Aravena, A. and Moya-Barría, I.I., Curvature effects on the reactivity of nanomaterials., in Carbon 2019, C. Kulaots, Editor. 2019: Lexington, USA.
3. Oyarzún-Aravena, A., Poster: Novel kinetic interpretation of the carbon-NO reaction: N2O vs. NO2 as intermediates., in Carbon 2018: The World Conference on Carbon. 2018: Madrid, Spain.
4. Oyarzún-Aravena, A., Salgado-Casanova, A., Radovic, L., and García-Carmona, X., Thermodynamics and kinetics of graphene and H2O/CO2 reactions: insights of multiple-site edge effects., in Carbon 2018: The World Conference on Carbon. 2018, GEC: Madrid, Spain.
Datasets
1. Oyarzún, Andrea; Garcia, Ximena; Radovic, Ljubisa (2020), “IRC data for a mechanistic route starting with H2O adsorption and finishing with H2 desorption from graphene.”, Mendeley Data, V2, doi: 10.17632/6nwmtzcfxr.2
Collaborators
Researchers in the field and students collaborated with the PI in different aspects of this project.
Prof. José Rodriguez-Mirasol
Professor at University of Málaga. Visited Chile. Collaborated with suggestions, teaching material, evaluated theses and planned an experiment.
Dr. Fernando Vallejos-Burgos
Collaborated with suggestions for an article.
Ms. Daniela Navarro-Pérez
Ms. and Chemical engineer. Collaborated with suggestions for a pedagogical article.
Catalina Gottschalk
Chemical engineer. Worked as thesis student and as Technical Support.
Iván Moya
Chemical engineer. Worked as thesis student and as Technical Support.
María Ruiz. Chemistry and Environment engineer. Worked as thesis student.
Hugo Ramos. Works as thesis student.
Pablo Araya. Works as thesis student.
Boris Gomez. Works as thesis student.
Past supervisors also provided advice and contributed with comments to the manuscripts.
Prof. Ljubisa Radovic
Professor at Pen State University and University of Concepción. Collaborated with suggestions for two articles.
Dr. Christopher Latham
Physicist. Provided advise on the selection of the computer system, and collaborated with an article.
Research groups visited
Loughborough University
Cambridge, UK
The Computational Modelling Group (CoMo), directed by Prof. Markus Kraft and associated to the Department of Chemical Engineering and Biotechnology.
Outreach and Teaching
Explora program
The PI participated in the 1000 scientists, 1000 classrooms program, presenting this project to a school in Punta Arenas.
Workshop: Computational Chemistry
A workshop was developed to train theses students. The workshop was also taught to postgraduate students.
Explora week at UMAG
To enhance the interest of school students in chemistry, we include models of this project in the annual university-open-doors activity.
Seminar at the Engineering Faculty
Together with professor José Rodriguez-Mirasol, wee presented a series of talks for students and invited authorities. (Spanish)
Researchers talks at UMAG
The university prepared a virtual space for researchers to disseminate their work to the community. (Spanish)
Talks
1. Oyarzún-Aravena, A., Navarro-Pérez, D., and Moya-Barría, I., Formación en química computacional y sus aplicaciones a través de un proyecto de investigación in CIFCOM 2021. 2021: Bogotá (online, oral presentation only).
Equipment and tools
Servers and software required for performing computational chemistry calculations were provided and installed.
Teaching materials including models and books are also available.
Acknowledgements
Funded by ANID-Chile through the FONDECYT INITIATION scheme.
Hosted by the Department of Chemical Engineering of the Universidad de Magallanes.