Title:	Chemistry and Catalysis on surfaces and nanoparticles, functionalized 2D-materials and single atom catalysts
DNr:	SNIC 2022/5-161
Project Type:	SNIC Medium Compute
Principal Investigator:	Tore Brinck <tore@kth.se>
Affiliation:	Kungliga Tekniska högskolan
Duration:	2022-05-01 – 2023-05-01
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 catalysis, solar energy, space propulsion and medicine. Our efforts encompass atomic-level studies of the chemical processes that governs the chemistry at crystalline 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 materials chemistry and catalysis. MASP was recently reviewed in an invited article, i.e. Adv. Theory Simul., (2019), 2, 1800149. It opens up 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 Phys. Chem. Chem. Phys., (2019), 21, 17009. We are developing a new computer code for more automated computation and analysis of MASP properties. It has been incorporated into ASE, and allows the use of a variety of DFT codes, e.g. GPAW, CP2K and VASP. We are collaborating with Seoul National University who synthesize and characterize well-defined chiral gold nanoparticles. These are e.g. of interest for stereoselective electrocatalysis. Due to the particle sizes it is difficult to identify and characterize the active sites by conventional DFT-approaches, and this makes it highly interesting to preescreen the particles by MASP as a preparation for DFT modeling. In a joint study we have contributed to the development of chiral nanoparticles for use as electrocatalysts in a medical glucose sensor. We will continue to explore these very large systems for catalytic and medical applications. MASP and conventional DFT are used for other structural and mechanistic studies related to heterogeneous catalysis, including electrocatalysis, and solar energy applications. In particular, we work on the nitrogen reduction reaction (NRR), which is of central importance for reducing the global use of fossil fuels. Currently, we are working on boron doped silicon (BSi) and germanium (Ge) materials. They show very promising properties for the NRR in the sense that they bind N2 stronger than H2, which is key for efficient NRR catalysts. However, to determine the catalytic efficiency it is necessary to compute the free energy surface for the electrochemical reactions, which is computationally very demanding. We intend to explore 2D materials, crystalline surfaces as well as nanostructured materials (e.g. particles) to identify materials optimized for the NRR We have recently begun investigating the reactive adsorption of iodine on platinum in relation to the use of Pt electrodes in perovskite solar cells. Computations of adsorption geometries and energies and spectroscopic properties (XPS etc) will be compared to experimental surface characterization in collaboration with Physics KTH and Chemistry UU.