First-principles Design of Novel Catalytic and Chemoresponsive Materials

Download or read book First-principles Design of Novel Catalytic and Chemoresponsive Materials written by Luke Tressel Roling and published by . This book was released on 2016 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt: An emerging trend in materials design is the use of computational chemistry tools to accelerate materials discovery and implementation. In particular, the parallel nature of computational models enables high-throughput screening approaches that would be laborious and time-consuming with experiments alone, and can be useful for identifying promising candidate materials for experimental synthesis and evaluation. Additionally, atomic-scale modeling allows researchers to obtain a detailed understanding of phenomena invisible to many current experimental techniques. In this thesis, we highlight mechanistic studies and successes in catalyst design for heterogeneous electrochemical reactions, discussing both anode and cathode chemistries. In particular, we evaluate the properties of a new class of Pd-Pt core-shell and hollow nanocatalysts toward the oxygen reduction reaction. We do not limit our study to electrochemical reactivity, but also consider these catalysts in a broader context by performing in-depth studies of their stability at elevated temperatures as well as investigating the mechanisms by which they are able to form. We also present fundamental surface science studies, investigating graphene formation and H2 dissociation, which are processes of both fundamental and practical interest in many catalytic applications. Finally, we extend our materials design paradigm outside the field of catalysis to develop and apply a model for the detection of small chemical analytes by chemoresponsive liquid crystals, and offer several predictions for improving the detection of small chemicals. A close connection between computation, synthesis, and experimental evaluation is essential to the work described herein, as computations are used to gain fundamental insight into experimental observations, and experiments and synthesis are in turn used to validate predictions of material activities from computational models.