“…The generation of metallic nanoparticles, nanocrystals, and films has been a highly dynamic research area due to their uses and developments for various applications, including imaging, sensing to catalysis, etc. − Obtaining the desired metallic materials, free of contaminants, is essential for many applications. In that context, the use of organometallic or metalorganic precursors has shown to be advantageous. , Key criteria for choosing precursors include, in particular, specific reactivity (e.g., ease of reduction or thermolysis), relative stability, and preparation scalability, along with other physicochemical properties, such as volatility or solubility in specific solvents, to name but a few. , Overall, this decision boils down to choosing a suitable set of ligands that, at the same time, endow their stability and ensure that they can be readily removed to generate the desired (nano-)material, free of organic or other contaminants (e.g., halides or residual carbonaceous species). Of various synthetic methodologies interested in generating clean materials, surface organometallic chemistry (SOMC) has emerged as a privileged approach to provide better-defined catalytic materials, such as supported nanoparticles with tailored interfaces and compositions (Figure a). , SOMC enables the interrogation of promoter effects and the role of interfacial Lewis acidic sites and alloying in heterogeneous catalysis. ,− For SOMC, similar to atomic layer deposition (ALD), one important criterion is to identify precursors that can react selectively with surface functionalities, in particular, surface OH groups.…”