Abstract: With the dwindling fossil-based energy reserve and increasing environmental awareness, the quest for sustainable energy production has become an urgent social issue. At its heart, the design of functional catalytic materials guided by molecular understanding of the relationship between function and structure is the top priority. In particular, the catalysis research has witnessed a notable transition from a trial-and-error to rationally guided routine driven by molecular-level insights supported by density functional theory (DFT) calculations.

In this talk, two case studies, electroreduction of furfural and step-catalysis of ammonia synthesis, will be presented to demonstrate material design strategies via modeling. Despite the apparent differences in the chemistries and catalytic materials used, the molecular mechanism characterized by the calculated thermodynamics and kinetics of the elementary steps from DFT calculations can be used to establish the principles to identity the critical descriptors and to improve or overcome the intrinsic limitations of existing materials.

Moreover, the computational screening process can be further accelerated by the constructions of linear scaling relationships and the Brønsted–Evans–Polanyi (BEP) relationships. Under some circumstances, it is necessary to break the limitation of the linear scaling relationship in order to gain the desired performance. Computational strategies developed in these studies can be readily integrated into parallel experimental efforts to guide material synthesis that will ultimately enable the revolution of current technologies for key chemical production.