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Hydrogen Evolution Reaction Activity of Heterogeneous Materials: A Theoretical Model
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Physics.ORCID iD: 0000-0001-9239-0541
Umeå University, Faculty of Science and Technology, Department of Physics.ORCID iD: 0000-0002-5080-8273
2020 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 124, no 38, p. 20911-20921Article in journal (Refereed) Published
Abstract [en]

In this study, we present a new comprehensive methodology to quantify the catalytic activity of heterogeneous materials for the hydrogen evolution reaction (HER) using ab initio simulations. The model is composed of two parts. First, the equilibrium hydrogen coverage is obtained by an iterative evaluation of the hydrogen adsorption free energies (ΔGH) using density functional theory calculations. Afterward, the ΔGH are used in a microkinetic model to provide detailed characterizations of the entire HER considering all three elementary steps, i.e., the discharge, atom + ion, and combination reactions, without any prior assumptions of rate-determining steps. The microkinetic model takes the equilibrium and potential-dependent characteristics into account, and thus both exchange current densities and Tafel slopes are evaluated. The model is tested on several systems, from polycrystalline metals to heterogeneous molybdenum disulfide (MoS2), and by comparing to experimental data, we verify that our model accurately predicts their experimental exchange current densities and Tafel slopes. Finally, we present an extended volcano plot that correlates the electrical current densities of each elementary reaction step to the coverage-dependent ΔGH.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2020. Vol. 124, no 38, p. 20911-20921
National Category
Physical Chemistry Condensed Matter Physics
Identifiers
URN: urn:nbn:se:umu:diva-176146DOI: 10.1021/acs.jpcc.0c05243ISI: 000575823600029Scopus ID: 2-s2.0-85095916115OAI: oai:DiVA.org:umu-176146DiVA, id: diva2:1478505
Funder
Swedish Research Council, 2017-04862Swedish Research Council, 2018-03937Swedish Energy Agency, 45419-1Olle Engkvists stiftelse, 186-0637Available from: 2020-10-22 Created: 2020-10-22 Last updated: 2023-03-24Bibliographically approved
In thesis
1. Electrocatalysts for sustainable hydrogen energy: disordered and heterogeneous nanomaterials
Open this publication in new window or tab >>Electrocatalysts for sustainable hydrogen energy: disordered and heterogeneous nanomaterials
2021 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

With the current global greenhouse gas emissions, our remaining carbon budget is depleted in only 7 years. After that, several biophysical systems are predicted to collapse such as the arctic ice, coral reefs and the permafrost, leading to potentially irreversible consequences. Our emissions are strongly correlated to access of energy and even if we are aware of the planetary emergency today, our emissions still continue to grow. Electrical vehicles have the possibility to reduce the emissions in the transportation sector significantly. However, these vehicles are still expensive and impractical for long-distance or heavy transportation. While political actions and technological development are essential to keep prices down, the driving dis- tance can be increased by replacing the batteries for onboard electricity production. 

In hydrogen fuel cells, electricity is produced by combining hydrogen gas (H2) and oxygen with only water as the by-product and if employed in electrical vehicles, distances of 500 km are enabled with a refueling time in 5 minutes. For other uses than in vehicles, H2 is also promising for large-scale electricity storage and for several industrial processes such as manufacturing CO2-free steel, ammonia and synthetic fuels. However, today most H2 production methods relies on fossil fuels and releases huge amounts of CO2. 

Electrolysis of water is an alternative production method where H2, along with oxygen are produced from water. To split the water, electricity has to be added and if renewable energy sources are used, the method has zero emissions and is considered most promising for a sustainable hydrogen energy economy. The tech- nique is relatively expensive compared to the fossil fuel-based methods and relies on rare noble metals such as platinum as catalysts for decreasing the required energy to split water. For large scale productions, these metals need to be replaced by more sustainable and abundant catalysts to lower the cost and minimize the environmental impacts. 

In this thesis we have investigated such candidates for the water splitting reaction but also to some extent for the oxygen reduction reaction in fuel cells. By combining theory and experiments we hope to aid in the development and facilitate a transition to clean hydrogen energy. We find among other things that i) defects in catalytic materials plays a significant role the performance and efficiency, and that ii) heterogeneity influence the adsorption energies of reaction intermediates and hence the catalytic efficiency and iii) while defects are not often studied for electrocatalytic reactions, these may inspire for novel materials in the future. 

Place, publisher, year, edition, pages
Umeå: Umeå Universitet, 2021. p. 88
Keywords
Water splitting, Electrochemistry, Nanomaterials, Density functional theory, Hydrogen evolution, MoS2, Fuel cell
National Category
Condensed Matter Physics
Research subject
nanomaterials; Physics; Physical Chemistry
Identifiers
urn:nbn:se:umu:diva-180130 (URN)978-91-7855-482-9 (ISBN)978-91-7855-481-2 (ISBN)
Public defence
2021-03-11, BIO.A.206 – Aula Anatomica, Umeå, 09:00 (English)
Opponent
Supervisors
Available from: 2021-02-18 Created: 2021-02-15 Last updated: 2021-02-16Bibliographically approved

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Ekspong, JoakimGracia-Espino, EduardoWågberg, Thomas

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