Title:	Chemistry on metal and metal oxide surfaces, and functionalized 2D-materials
DNr:	SNIC 2019/3-136
Project Type:	SNIC Medium Compute
Principal Investigator:	Tore Brinck <tore@kth.se>
Affiliation:	Kungliga Tekniska högskolan
Duration:	2019-04-01 – 2020-04-01
Classification:	10407 10403 10402
Homepage:	https://www.kth.se/profile/tore/
Keywords:

Abstract

The research is focused on fundamental problems in surface science with an emphasis that is being shifted from corrosion towards heterogeneous catalysis and electrochemical catalysis. Our efforts encompass atomic-level studies of the chemical processes that governs the chemistry at metal and metal oxide surfaces, but also two-dimensional materials (films), such as graphene and borophene, with metal add-atoms and chemical modifications. The computational approaches include the use of conventional density functional theory (DFT) methods, but also the development of new methods for characterizing surface reactivity based on the computation of DFT-based local surface properties. We have shown that our Molecular Surface Property Approach (MASP) can be used to analyze and predict chemical interactions of molecules, nanoparticles as well as extended surfaces [e.g. Brinck et al, J. Phys. Chem. A (2016), 120, 10023-10032; Stenlid et al J. Am. Chem. Soc. (2017), 139, 11012–11015; and Stenlid et al, Phys. Chem. Chem. Phys (2018), 20, 2676-2692]. The current status of the MASP was recently reviewed, i.e. Brinck and Stenlid, Adv. Theory Simul., (2019), 2, 1800149. This approach opens up new possibilities for computationally efficient predictions of local interactions at complex materials surfaces. We envisage that our approaches will be of great general use in, e.g., the surface and materials sciences, with application in areas such as electrochemistry and heterogeneous catalysis. In the upcoming year, we will continue the validation of our new methods by benchmarking the MASP predictions against detailed DFT calculations of extended systems. In parallel with the methods development, we also perform mechanistic studies of heterogeneous catalysis and electrochemical reactions. Our previous efforts have included understanding of the anoxic corrosion behavior of copper for the proposed application in the Swedish nuclear waste management program [e.g. Stenlid et al, Phys. Chem. Chem. Phys. (2016), 18, 30570-30584]. We have also obtained insight into the chemical interactions of methanol, carbon monoxide and sulfur dioxide molecules on the surface of Cu2O [e.g. Besharat et al, J. Chem. Phys. (2017), 149, 244702; Soldemo et al, J. Chem. Phys. C (2017), 121,24011, Tissot et al. J. Phys. Chem. C, 2019 in press]. These studies have been conducted in close collaboration with experimental groups at KTH and Stockholm University (SU). The experimental studies have largely employed surface sensitive microscopy and spectroscopy based on synchrotron radiation. The upcoming year the focus will largely be shifted toward electrochemical catalysis of the oxygen evolution reaction and the nitrogen reduction reaction. These reactions will analyzed in great detail with the purpose of facilitating the design of efficient catalysts. Potential catalysts that will be studied include nanoparticles as well as extended surfaces of metals and metal oxides and functionalized 2-D materials. In the design part, we will work in collaboration with the solar energy group of Licheng Sun (KTH). In this research we will carry out both static and dynamic density functional theory computations, and the size of our systems necessitates the use of high performance supercomputers.