Density Functional Theory Screening of Transition Metal Nitrides for CO Electrochemical Reduction

Mohammadreza Karamad^a, Amir Barati Farimani^b, Rishikesh Magar^b, Samira Siahrostami^c, Ian Gates^a

^aDepartment of Physics and Astronomy, University of Calgary, University Drive Northwest, 2500, Calgary, Canada

^bDepartment of Mechanical Engineering, Carnegie Mellon University, University Doctor C, Pittsburgh, United States

^cDepartment of Chemistry, University of Calgary, University Way Northwest, 2975, Calgary, Canada

Materials for Sustainable Development Conference (MATSUS)
Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)

#Suschem- Materials and electrochemistry for sustainable fuels and chemicals

Barcelona, Spain, 2022 October 24th - 28th

Organizers: Marta Costa Figueiredo and Raffaella Buonsanti

Contributed talk, Mohammadreza Karamad, presentation 065
DOI: https://doi.org/10.29363/nanoge.nfm.2022.065
Publication date: 11th July 2022

Electrochemical reduction of CO₂ to fuels has attracted a great deal of attention in recent years as a potential solution to close the carbon cycle [1]. In search for novel catalyst materials, we present in this study density functional theory-based screening of heteroatom-doped transition metal nitrides [2]. We first examine zinc blend and rock salt polymorphs of transition metal nitrides and then consider doping the surface with 25% B, P, Sb, Bi, and C heteroatoms [3]. We fully assess the stability and activity of the examined catalysts. The catalytic activity is measured by the calculated limiting potential, and the stability is assessed against hydroxyl (*OH) poisoning as well as dissolution under CO reduction relevant potentials. Of the screened nitrides, many are predicted to be active for the CO reduction reaction but only a few are stable under electrochemical conditions. In particular, on nearly all of the metal nitrides with a desired catalytic activity for CO reduction, either the competing hydrogen evolution reaction prevails over CO reduction or *OH poisoning occurs at CO reduction onset potentials. We identify five promising candidates including P-doped NbN, C-doped VN, P-doped VN, TiN, and Sb-doped TiN. Ultimately, this study emphasizes the relevance of stability under electrochemical conditions and the importance of taking into account the competition between the CO reduction, hydrogen evolution, and *OH reduction reactions under electrochemical conditions.

References:

[1] Kortlever, R.; Shen, J.; Schouten, K. J. P.; Calle-Vallejo, F.; Koper, M. T. M. Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide. J. Phys. Chem. Lett. 2015, 6, 4073– 4082.

[2] Abghoui, Y.; Garden, A. L.; Hlynsson, V. F.; Björgvinsdóttir, S.; Ólafsdóttir, H.; Skúlason, E. Enabling Electrochemical Reduction of Nitrogen to Ammonia at Ambient Conditions through Rational Catalyst Design. Phys. Chem. Chem. Phys. 2015, 17, 4909– 4918.

[3] Karamad, M.; Barati Farimani, A.; Magar, R.; Siahrostami S.; Gates, I.D. Heteroatom-Doped Transition Metal Nitrides for CO Electrochemical Reduction: A Density Functional Theory Screening Study, J. Phys. Chem. C 2020, 124, 48, 26344–26351.

Acknowledgements:

The authors acknowledge support from the University of Calgary’s Canada First Research Excellence Fund program and the Global Research Initiative in Sustainable Low Carbon Unconventional Resources.

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