Electrified thermochemical reaction systems with high-frequency metamaterial reactors

Electrocatalysis plays a central role in clean energy conversion, enabling a number of sustainable processes for future technologies. This review discusses design strategies for state-of-the-art heterogeneous electrocatalysts and associated materials for several different electrochemical transformations involving water, hydrogen, and oxygen, using theory as a means to rationalize catalyst performance. By examining the common principles that govern catalysis for different electrochemical reactions, we describe a systematic framework that clarifies trends in catalyzing these reactions, serving as a guide to new catalyst development while highlighting key gaps that need to be addressed. We conclude by extending this framework to emerging clean energy reactions such as hydrogen peroxide production, carbon dioxide reduction, and nitrogen reduction, where the development of improved catalysts could allow for the sustainable production of a broad range of fuels and chemicals.

Photocatalysis based on optically active, “plasmonic” metal nanoparticles has emerged as a promising approach to facilitate light-driven chemical conversions under far milder conditions than thermal catalysis. However, an understanding of the relation between thermal and electronic excitations has been lacking. We report the substantial light-induced reduction of the thermal activation barrier for ammonia decomposition on a plasmonic photocatalyst. We introduce the concept of a light-dependent activation barrier to account for the effect of light illumination on electronic and thermal excitations in a single unified picture. This framework provides insight into the specific role of hot carriers in plasmon-mediated photochemistry, which is critically important for designing energy-efficient plasmonic photocatalysts.

Metamaterials, artificial composite structures with exotic material properties, have emerged as a new frontier of science involving physics, material science, engineering and chemistry. This critical review focuses on the fundamentals, recent progresses and future directions in the research of electromagnetic metamaterials. An introduction to metamaterials followed by a detailed elaboration on how to design unprecedented electromagnetic properties of metamaterials is presented. A number of intriguing phenomena and applications associated with metamaterials are discussed, including negative refraction, sub-diffraction-limited imaging, strong optical activities in chiral metamaterials, interaction of meta-atoms and transformation optics. Finally, we offer an outlook on future directions of metamaterials research including but not limited to three-dimensional optical metamaterials, nonlinear metamaterials and "quantum" perspectives of metamaterials (142 references).