Title:	Chemistry on metal and metal oxide surfaces and nanoparticles, functionalized 2D-materials and single atom catalysts
DNr:	SNIC 2021/5-156
Project Type:	SNIC Medium Compute
Principal Investigator:	Tore Brinck <tore@kth.se>
Affiliation:	Kungliga Tekniska högskolan
Duration:	2021-04-01 – 2022-04-01
Classification:	10407 10403 10402
Homepage:	https://www.kth.se/che/tfk/staff/seniors/brinck-1.80061
Keywords:

Abstract

The research is focused on analyzing chemical interactions in surface science and molecular sciences, including applications in corrosion, space propulsion, catalysis and medicine. Our efforts encompass atomic-level studies of the chemical processes that governs the chemistry at metal and metal oxide surfaces and nanoparticles, 2D materials, such as doped graphene and silicene, and further includes single atom catalysts and molecules in different matrices. Computational approaches include conventional ab initio and DFT methods, but also the development of new methods for characterizing surface reactivity based on the computation of DFT-based local surface properties (MASP). Our Molecular Surface Property Approach (MASP) is used to analyze chemical interactions of molecules, nanoparticles as well as extended surfaces, and has applications in electrochemistry and heterogeneous catalysis. MASP was recently reviewed in an invited article, i.e. Brinck and Stenlid, Adv. Theory Simul., (2019), 2, 1800149. MASP opens up new possibilities for inexpensive and computationally efficient predictions of local interaction sites and associated interactions strengths at complex materials surfaces. The extension to periodic DFT calculations was reported in Stenlid et al., Phys. Chem. Chem. Phys., (2019), 21, 17009. We have developed a new computer code for more automated computation and analysis of MASP properties. It is being incorporated into ASE, and allows the use of a variety of DFT codes, e.g. GPAW and VASP. We recently started to collaborate with Ki Tae Nan at Seoul National University who synthesize and characterize well-defined chiral gold nanoparticles. The nanoparticles are, among other applications, of interest for stereoselective electrocatalysis. Due to the particle sizes it is difficult to identify and characterize the active sites by conventional DFT-approaches, which makes the nanoparticles particularly interesting for the MASP. In a joint study we have contributed to the development of chiral nanoparticles for use as electrocatalysts in a medical glucose sensor. A manuscript for submission to the Science magazine is under preparation. In parallel with the methods development, we also perform structural and mechanistic studies related to corrosion and heterogeneous catalysis. In particular, we work on the nitrogen reduction reaction (NRR), which is of central importance for reducing the global use of fossil fuels. We have analyzed electrocatalysis of NRR in single atom based Vanadium catalysts incorporated into B/N doped carbon based 2 D materials, e.g. modified graphene, and a manuscript is being prepared. Currently, we are working on boron doped silicon (BSi) materials, which show very promising properties for the NRR reaction in the sense that they bind N2 stronger than H2. The poisoning of the catalysts by H2 is the major problem in NRR, and we have found BSi catalysts to provide an affordable and tunable solution. We will begin investigating alternative molecular propellants for use in electrical space propulsion. This will require us to run extensive DFT molecular dynamic (MD) simulations of ionized and thermally excited candidate molecules to investigate ion stabilities and fragmentation patterns. Chemical compatibility of plasma excited molecules and LaB6 cathode material is investigated by periodic DFT MD.