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.

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

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.

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

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.

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…

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

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

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

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

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.

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.

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

The electrochemical hydrogenation reaction is an alternative approach for the transformation of unsaturated bonds without the use of flammable dihydrogen gas.

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.

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.

This thesis aims to test in vitro pipelines to rapidly and cost-effectively identify molecular mechanisms that drive adverse outcomes in clinical use.

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.

Promotor: Arjen Doelman, Co-promotor: Vivi Rottschäfer

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

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

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

Promotor: Prof.dr. G.J. Kroes

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

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

Catalysis is of extreme relevance in the production of everyday materials and plays a central role in many aspects of our life.

In this dissertation iron-based homogeneous catalysts were synthesized, characterized and investigated for water oxidation activity.

This thesis explores how electron paramagnetic resonance (EPR) spectroscopy can be used to investigate key biochemical processes.

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

In this thesis chemical and physical processes in the ice mantles on interstellar dust grains are studied.

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

CO2-reductie door de CO2 eenvoudig met een soort oplaadbare batterij uit de lucht te halen, lijkt pure science fiction. Toch hebben Leidse scheikundigen zo’n ‘batterij’ – een gele koperoplossing die in contact met lucht groenblauw wordt – ontdekt. Hierover publiceren ze in Science van vrijdag 15 jan…

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…

Een Leidse ontdekking helpt om van CO2 aardgas te maken én om duurzame energie op te slaan. Onderzoek van professor Marc Koper en promovenda Jing Shen maakt duidelijk hoe dit proces goedkoop en controleerbaar kan verlopen. Nature Communications 1 september 2015.

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…

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…

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.

Several techniques are explored for going beyond the born-oppenheimer static surface model for molecule-surface reactions.

De stijging van de CO2 concentratie in de lucht neemt gestaag toe, met alle gevolgen van dien. Naast alle organisaties die zich bezig houden met het verminderen van de CO2 concentratie werkt de Universiteit Leiden op drie verschillende manieren aan het vergaren van fundamentele kennis met betrekking…

Energie winnen uit zonlicht en water: dát zou een oplossing zijn voor ons grootste milieuprobleem. Elektrochemicus Marc Koper onderzoekt de basis voor een CO2-neutrale toekomst. Over zijn werk staat nu een dossier online.