13 January 2025
In his thesis, Pulcinella presents groundbreaking contributions to photocatalysis, a highly competitive field in chemistry. In particular, he developed methodologies that leverage light energy to cleave strong C–H bonds, applying the concepts of flow chemistry. His research was part of the Horizon 2020 Marie Curie ITN project ‘C-H Activation for Industrial Renewal’ (CHAIR).
With his research, Pulcinella has made substantial strides toward more environmentally friendly, sustainable practices in the chemical industry. His research has been published in high ranking journals and has led, amongst others, to a commercial reagent and a contribution to the Encyclopedia of Reagents for Organic Synthesis.
The distinction also honours Pulcinella’s creativity, independence and academic leadership. His collaborative spirit has consistently fostered a positive and motivating environment and he has mentored and inspired many students.
Pulcinella’s thesis presents the development of novel synthetic methodologies for the functionalization of feedstock chemicals under mild conditions, employing both batch and flow photochemical processes. Emphasizing the transformative role of radical chemistry, the work explores unique reactivity patterns that expand the synthetic toolbox available for organic chemists. A key achievement presented in this thesis is the photocatalytic conversion of abundant liquid and gaseous alkanes into value-added building blocks, enabled by the synergistic integration of photocatalysis with transition metal catalysis. The use of flow reactors is underscored for their critical role in facilitating fast, efficient, and safe handling of gaseous reagents under photochemical conditions. Furthermore, innovative metal-free photocatalytic approaches employing sulfonylhydrazones as radical acceptors have been developed to form C(sp3)−C(sp3) bonds. Using this new reactivity paradigm, a redesigned homologation of carboxylic acids highlights the potential of single-electron logic to address long-standing challenges in organic synthesis. Finally, a platform for synthesizing densely functionalized α-branched secondary amines via deoxygenative activation of the inert amide functionality using inexpensive reagents is presented. Overall, the thesis demonstrates the power of radical-based methodologies in advancing sustainable and efficient chemical transformations.
A. Pulcinella: Photocatalytic strategies for the valorization of feedstock chemicals in batch and flow. Download the thesis from the UvA repository.