(6dz) Enabling the Spectroscopic Tools That We Need to Get the Hidden Information We Want

Catalysis lies at the heart of the chemical industry and could be considered as the society’s gateway to the sustainable and petroleum-free future for the fuel and chemical production. Since the energy needs of the developed world are currently over-dependent on the utilization of finite mineral resources, enormous research efforts aim to the shift from petroleum supply to natural gas and renewables, such as biomass, for fuel and chemical production in an economic and efficient manner. In that sense, it is common knowledge that catalysts matter and can provide better ways to make new materials from various sources. Spectroscopy is the enabling tool for the knowledge based and hence time-effective catalyst design, which goes beyond the scope of an empirical observation. Monitoring the events taking place in such materials under realistic conditions is crucial for understanding the reaction mechanism of many important chemical processes and would allow the rational design of new or improve the existent catalysts.

Willing to investigate in depth the structural changes of supported metal oxide catalysts, my research as a graduate student relied on the utilization of vibrational spectroscopies under realistic reaction conditions. Operando Raman spectroscopy of MoO₃/TiO₂ catalysts for the Oxidative DeHydrogenation of ethane revealed that the terminal Mo=O functionalities present on the dispersed species could be responsible for the non-selective ethane to CO_x reactions underlining the importance of the anchoring Mo–O–Support bonds as the active site. Armed with my already acquired knowledge supported by my inherent eagerness to explore new scientific areas, my postdoctoral research lies on the critical issue of solvent selection in the field of biomass to fuels and chemicals applications. By coupling thorough spectroscopic measurements with ab-initio DFT calculations, we were able to provide an explanation of the enhanced 5-Hydroxylmethylfurfural (HMF) stability if polar aprotic solvents used as a co-solvents.

What I envision in my research plans is the rational utilization of spectroscopic techniques coupled with simultaneous measurements of catalytic reactivity (Operando spectroscopy). In this respect, my ultimate goal is to unravel novel structure-function relationships for heterogeneous and homogeneous catalytic systems. My approach lies first at the design of a multi-spectroscopic reactor that would be able to monitor under realistic reaction conditions the structure of the catalyst by means of Visible Raman, Surface Enhanced Raman and/or FTIR spectroscopies. However, one crucial drawback regarding Operando spectroscopy lies on the fact that cannot be directly applied for the study of homogeneous catalytic systems. For that reason, a new alternative will be proposed namely Operando Solvation that will allow to monitor changes in solvent structure that could be directly correlated with data of the catalytic reactivity for biomass to biofuels and chemical reactions.

Refernces

(1)         Tsilomelekis, G.; Boghosian, S. Phys Chem Chem Phys 2012, 14, 2216.

(2)         Tsilomelekis, G.; Boghosian, S. Catal Sci Technol 2013, 3, 1869.

(3)         Tsilomelekis, G.; Josephson, T. R.; Nikolakis, V.; Caratzoulas, S. Chemsuschem 2014, 7, 117.