Single-nickel-Atom heterogeneous Catalysis: OverComing the Hurdle of low single-atom dEnsity – SACOCHE

To be able to investigate how the reactivity of molecules is impacted by the isolated character of single-atom catalytic sites, and ultimately to optimize this reactivity by designing the catalyst properly, one must succeed in 1) isolating the catalytic sites homogeneously, without introducing a different kind of neighboring sites, and by preventing the possibility of sintering under reaction conditions, and 2) controlling the surface density of these isolated sites, i.e increasing it to the highest possible extent, if beneficial. The hitherto reported approaches to bring active metals onto supports (e.g surface organometallic chemistry, ion exchange, non-hydrolytic sol-gel) sometimes meet the first above requirement. They however hardly meet the second one, or have not been sufficiently explored for that purpose. The novel bottom-up route proposed in the present ANR-JCJC project has the potential to meet both the above requirements at once. It will open the door to a broad range of new in-depth investigations on single-atom catalysts in many different catalytic applications, for both fundamental and performance optimization purposes. The present project aims at controlling the processes involved in that novel approach within a first catalyst, Ni-substituted hydroxyapatite, and at exploiting the novel approach to study and optimize the reactivity of a first molecule, 1,3-butadiene, under hydrogenating conditions. 1,3-Butadiene is an impurity of industrial alkene streams that poisons the alkene polymerization catalysts. It is commonly removed by catalytic hydrogenation over supported Pd or Pt. Ni is an attractive candidate to replace the latter noble metals. The project will be coordinated by the young researcher Dr. Josefine Schnee who will implement the required in situ/operando characterization approaches in her host laboratory (Laboratoire de Réactivité de Surface) and supervise the PhD Student who will be hired.