(4cg) Combining Molecular Level Insights with Advanced Synthesis Strategies to Design (Photo)Catalytic Materials: Efficient Chemical Processing Utilizing Thermal and Solar Stimuli

Developing energy efficient, environmentally friendly methods of producing industrial chemicals is an extremely important area of research for the 21st century. Herein a cross-disciplinary approach for catalyst design combining theoretical chemistry, to develop molecular level insights, with advanced materials synthesis techniques, for the synthesis of uniform materials with tailored physical properties is presented. The approach is applied to the development of more efficient catalysts for industrial thermo-catalytic processes, and creates a foundation for incorporating solar energy as an energy input for activating important chemical reactions.

Recent advances in computational chemistry and nanomaterials synthesis were utilized to design new catalysts for the industrially important ethylene epoxidation reaction. Density functional theory calculations were used to identify promising surface facets of Ag catalysts and advanced synthesis techniques, developed in the nano-science community, were used to synthesize particles with the targeted surface facets. These studies show that catalytic particles of controlled size and shape represent promising heterogeneous catalysts for selective production of chemicals and act as critical platforms to study heterogeneous catalytic process and identify crucial factors that impact process selectivity.

The metallic nanostructures utilized in our initial studies efficiently concentrate light at their surfaces. This effect, known as Localized Surface Plasmon Resonance, results in either: the absorption of photons thereby heating the nanostructure, intense re-emission of the photons or a transfer of energetic electrons to surrounding medium. The intensity, resonance energy and dominant decay mechanism can be tuned by changing the size and shape of the metallic nanoparticles and the external environment. We have exploited the tunable parameters of these optical properties to develop versatile photocatalytic chemical processing platforms that have opened countless possibilities for the development of chemical processes based on the use of multiple energy stimuli for efficient solar/thermal chemical processing.

This research highlights the utility of molecular insights in concert with well-defined metallic nanostructures for the development of new catalytic and photocatalytic materials for energy efficient, environmentally friendly chemical processing. In light of these results future work utilizing a similar over-arching approach towards environmentally friendly chemical processing will be discussed.