Automated and high-throughput reactivity analysis in homogeneous catalysis: The deactivation complexity of Mn(I) hydrogenation catalysts

In this thesis, I highlighted a number of projects aimed at developing and testing new simulation methods for studying complex reactive systems, with a particular emphasis on simulation strategies based on the concept of bonding graphs. These mathematical structures provide useful tools for a variety of algorithms developed over the last few...

Insight into the multifunctionality of TiO2-based catalyst

Computational chemistry provides powerful research tools for catalysis. It potentially allows us to study the structures of the catalytic sites and reaction mechanisms, which are difficult to observe only by experiment. This is particularly true for supported heterogeneous catalysts, of which reactivity and catalytic behavior are directly...

Structures, activities, and mechanisms under the spectroscopes: the quest for unveiling the nature of active sites for highly selective CO2 hydrogenation to methanol

Since the industrial revolution in the 1760s, the CO2 concentration in the atmosphere has been rising incessantly driving global warming closer to the point of no return. The world requires urgent actions to not only reduce CO2 emissions but also capture the CO2 for utilization to mitigate the future environmental crisis. CO2 hydrogenation to...

Mapping the reaction landscape for the C1 chemistry

In this thesis, we have presented and investigated the possible strategies for modelling complex heterogeneous catalytic systems in operando regimes. By introducing modern computational approaches to sample the potential energy surface of the catalytic active site, we have attempted to account for the reactive conditions, solvent presence,...

Activation, Reactivity and Dynamics of Manganese Pincer Complexes in Hydrogenation Catalysis

The growing demands for sustainable chemical technologies have prompted a wave of searching new catalysts based on earth-abundant metals. In the field of (de)hydrogenation catalysis, however, the huge performance gap is commonly seen between the 3d-metal-based catalysts and their noble metal counterparts, which largely hampers their practical...

The hydrocarbon-pool chemistry of methanol conversions in zeolite catalysts

The MTH process is recognized as one of the key ingredients of the methanol (MeOH) economy concept enabling the production of crucial hydrocarbon building blocks, such as light olefins and aromatics, starting from CO2 as the primary carbon source. Besides the driving force of reducing reliance on fossil fuels, the highly tunable nature of this...

Homogeneous reduction by bifunctional manganese catalysis: a quantum chemical approach

Catalysis, chemistry, and automation: Addressing complexity to explore practical limits of homogeneous Mn catalysis

Catalysis is a critical enabling technology that directly contributes to higher standards of living. This is a remarkable feat for a technology that most consumers have no direct contact with and perhaps only vaguely know from their car’s catalytic converter. Even many technical users regard catalysts as ideal substances that promote a target...

Deactivation pathways in methane upgrading catalysis

The abundance of methane has led to a strong interest to use methane as a feedstock in the chemical industry. One of the main challenges is the initial activation of the methane molecule. In this thesis, heterogeneous catalysts for two different methane conversion processes are investigated. Firstly, the deactivation of supported Ni catalysts...

Modeling the carbon dioxide electrocatalysis system

Increasing level of atmospheric carbon dioxide (CO2) because of human activities is a serious threat to ecosystems on Earth due to global warming. A transition to net-zero CO2 emissions before 2050 is necessary to limit the global mean surface temperature rise to 1.5ºC-2ºC above preindustrial levels. Carbon capture and utilization technologies...

Catalytic methane conversion with single-site porous catalysts: a computational approach

In this thesis we presented comprehensive studies on methane activation by binuclear Fe-oxo sites located in porous MOF and zeolite frameworks. Many of such studies have been previously performed, however the main focus was usually on the C-H bond activation of methane. Here we focused on the whole reaction mechanism including the activation of...