This dissertation presents a new perspective on the life, work and character of the Dutch physical chemist Jacobus Henricus van ’t Hoff, first recipient of the Nobel Prize in Chemistry, and one of... Show moreThis dissertation presents a new perspective on the life, work and character of the Dutch physical chemist Jacobus Henricus van ’t Hoff, first recipient of the Nobel Prize in Chemistry, and one of the most important and colourful scientists in Dutch history. The image of Van ’t Hoff that emerges from the research presented in this dissertation is that of someone with a strong drive to make a name in science, who nonetheless always remained an outsider. The only major biography was already published in 1912, and was rather uncritical, if not heroizing. Therefore, it was high time for a new one, covering all insights gained over the past hundred years into his scientific research, his personal life and their mutual influence. Public and family archives have delivered a wealth of previously unknown (personal) documents, letters, diaries etc. which to a large extent had never been studied before. They offer previously unknown insights into the character of Van ‘t Hoff and shed new light on the interaction between the personality and scientific work of this leading chemist of the nineteenth century. Apart from these biographical aspects the biography also covers more general historical issues like the internationalisation of science at the end of the nineteenth century, the founding of the new discipline of physical chemistry in the same period, and the changing relationship between education and research in Dutch universities and abroad. Show less
This thesis describes the development of a combined high-pressure/ultrahigh-vacuum flow reactor for the study of model catalysts by means of surface x-ray diffraction and grazing incidence small... Show moreThis thesis describes the development of a combined high-pressure/ultrahigh-vacuum flow reactor for the study of model catalysts by means of surface x-ray diffraction and grazing incidence small angle scattering. The system was used to measure a stability diagram for the different oxide phases (surface oxide, bulk-like oxides) that exist on Pd(100) during catalytic CO oxidation at near ambient pressures. As soon as an oxide was present the reactivity of the surface was found to be mass transfer limited by the flux of CO molecules reaching the surface. Experiments on spontaneous reaction oscillations of the CO oxidation rate on Pd(100) reveal that a high density of steps strongly alters the stability of the thin, catalytically active palladium oxide film. It is shown that stabilization of the metal, caused by the steps and consequent destabilization of the oxide, is at the heart of the well-known reaction rate oscillations exhibited during CO oxidation at atmospheric pressure. Lastly reaction oscillations on supported Pd nanoparticles are shown to be accompanied by shape changes of the particles consistent with the formation and removal of a thin palladium oxide film on the particles. Show less
