The goal of this thesis is to understand how interfacial parameters, such as the addition of organic additives, bulk pH or metal cations of the electrolyte, affect the relevant electrocatalytic reactions, i.e. electrochemical CO2 reduction reaction or hydrogen evolution reaction.

This thesis has shed light on some of the ways in which the local electrolyte composition can differ from the bulk and how these changes in the local reaction environment can determine the activity and/or selectivity of two important electrocatalytic reactions, namely, electrochemical CO2 reduction…

The adsorption of D2 and CO2 on catalyst surfaces is studied using a molecular beam in ultra-high vacuum.

With the energy transition toward a renewable energy supply and a CO2-neutral economy, electrification of the energy system is rising in importance, which leads to the challenge of long-term storage of renewable electricity.

In eight chapters, the thesis of Rafaël Vos covers the effect of temperature and pressure on the electrochemical CO2 reduction.

Bicarbonate buffer is largely found in nature due to its ability to regulate pH variations around neutral values. As the pH changes, so does the speciation of the buffer.

Plants could be regarded as small chemical factories, which produce chemical substances via photosynthesis. If we can imitate photosynthesis in an artificial system, we can make clean fuels and materials out of sunlight and CO2. Huub de Groot is very close to designing a system of this kind.

The role of the interfacial environment during electrochemical reactions has been increasingly valued, especially for those reactions involving protons or hydroxyl ions.

A key step in the synthesis of oligosaccharides and glycoconjugates is the formation of the glycosidic bond.

Despite the history of studies on methanol formation from CO2, the dominant elementary reaction steps that constitute the chemical mechanism for this catalyzed process are not determined.

Promotor: M.T.M. Koper, Co-Promotor: L.B.F. Juurlink

This thesis focuses on the synthesis, characterization and performance towards CO2 electroreduction of mono and bi-metallic particles based on p-block metals

The emissions of the Chinese industrial sector alone comprise 24.1% of global emissions (7.8 GtCyr−1 in 2015). This makes Chinese industrial emissions of unique national and international relevance in climate policy. This study reports a literature survey that quantitatively describes the evolution…

This thesis describes the use of a combined approach of computational and experimental techniques to gain novel insights to understand the glycosylation reaction and its reactive intermediates.

The local ordering of atoms at the surface of a metallic particle determines its catalytic activity and selectivity. As energy systems of the future will be based on efficient catalytic conversion of small molecules in closed cycles, we study how structural effects of catalysts can be used to our ad…

Heterogeneous catalysis is essential to many industrial applications. These catalysts are often comprised of supported nanoparticles, which contain various different surface sites.

Carbohydrates, or sugars, are the most diverse and most abundant biomolecules known. However, the isolation of carbohydrate samples in sufficient amounts and purity is often impractical or even impossible, so the chemical synthesis of glycosides becomes relevant. The glycosylation reaction, in which…

M.T.M. Koper, Co-promotor: D.G.H. Hetterscheid

Promotor: Prof.dr. T.J. Aartsma, Co-promotor: R.N. Frese

In this dissertation, the synthesis and characterization of a series of iron complexes based on different ligand platforms are described.

The glycosylation reaction is a pivotal reaction in creating new and complex oligosaccharides.

Promotor: Prof.dr. E. Bouwman

Heterogeneous catalyzed processes are highly significant to the chemical industry. Dissociative chemisorption (DC) of molecules on surfaces is always considered as a step with a high degree of rate control for heterogeneous catalysis.

Human civilization consumes a huge amount of fossil fuels, which has resulted in an atmospheric CO2 level which has not been higher in over 800 millennia.

A difficulty of studies on chemical kinetics are the reaction time scales and detection of their intermediates.

Promotor: A. Doelman, Co-promotor: J.D.M. Rademacher

Promotor: M.T.M. Koper, Co-Promotor: L.B.F. Juurlink

The research presented in this thesis makes use of small molecules (as H2 , D2 and O2 ) on well-defined single crystal surfaces (flat Pt(111), flat Cu(211) and curved Pt(111)) to elucidate the role of surface structure and degrees of freedom in the reactant in specific surface reactions.

This work describes several studies into the electroreduction of carbon dioxide (CO2RR), both regarding mechanistical aspects and catalyst stability considerations. Mechanistic insights into carbon-carbon bond formation on a silver catalyst are described in Ch 2, were we find an acetaldehyde-like surface…

Electrocatalysis allows for storing electricity or converting it into chemical bonds, producing chemical building blocks and fuels using renewable resources.

This perspective addresses four challenges facing theorists whose aim is to make quantitatively accurate predictions for reactions of molecules on metal surfaces, and suggests ways of meeting these challenges, focusing on dissociative chemisorption reactions of H2, N2, and CH4.

Promotores: G.W. Canters, T.J. Aartsma

A discovery made in Leiden helps not only to make natural gas from CO2 but also to store renewable energy. Research by Professor Marc Koper and PhD student Jing Shen shows how this process can be implemented in a cost-effective and controllable way. Nature Communications, 2 september 2015.

Jaroslaw Kantorowicz, assistant professor at the Institute of Security and Global Affairs, isolated the reaction of the public to the potential breach of constitutional fiscal rules from the reaction of other players, such as the opposition, media and civil society organizations.

Hydrogen peroxide (H2O2) is an important bulk chemical that is used in various industrial processes. More than 95% of the H2O2 used in industry is made via the anthraquinone process during which a large amount of energy is going to waste.

Promotor: E. Bouwman, Co-promotor: S. Bonnet

Promotor: Arjen Doelman, Co-promotor: Vivi Rottschäfer

Although it is often assumed that the stereochemistry in Ugi multicomponent reactions is determined in the final Mumm rearrangement step, experimental and computational evidence that Ugi reactions on hydroxylated pyrrolines proceed under kinetic control is reported.

Green hydrogen is produced via a process called water electrolysis. During electrolysis water is split into oxygen and hydrogen.

Artificial photosynthesis has recognised potential to produce green and sustainable fuels from earth-abundant resources such as water, carbon dioxide (CO2), and sunlight.

Yuvraj Birdja converted CO2 to formic acid to store energy in a sustainable way, with different catalysts. With this new knowledge, scientists are a step closer in industrially converting CO2 to chemicals and fuels. This can help reduce CO2 emission and the greenhouse effect.

In this thesis we have discussed several parameters that affect the electrochemical conversion of enviromentaly harmful molecules such as nitrates and carbon dioxide to more valuable and less deleterious compounds, in order to cast light onto the mechanism of the reaction to achieve an efficient and…

Promotor: Prof.dr. G.J. Kroes

Carbon dioxide capture and utilization technologies are necessary to create a truly circular economy. The electrochemical reduction of carbon dioxide to formate is an appealing carbon utilization method as it can be performed at room temperature and pressure, it only requires two electrons, and it has…

Promotor: Prof.dr. H.V.J. Linnartz, Co-Promotores: S. Ioppolo, H.M. Cuppen

Methods for accurately computing the interaction of molecules with metal surfaces are critical to understanding and thereby improving heterogeneous catalysis.

Fearing a trade-off with economic growth, countries feel discouraged to cut their CO2 emissions. But do the two really not go together? Environmental scientist Ranran Wang and her colleagues investigated the relationship between economic growth and CO2 emissions in 73 countries from 1970 to 2016. Wang:…

In this thesis, we consider various (electro)chemical phenomena at surfaces and nanoparticles and their underlying atomistic processes, which we studied using first-principles methods such as density functional theory.