UC Davis

The development of carbon dioxide (CO2) reduction electrocatalysts is an intensively studied area in the development of CO2 capture, utilization, and storage strategies. In this work, density functional theory (DFT) and ab initio molecular dynamics (AIMD) are employed to study redox properties and the pathway of a side reaction of CO2 reduction electrocatalyst [Fe4N(CO)12]-. The material of this chapter was published as an article titled “Quantum chemical studies of redox properties and conformational changes of a four-center iron CO2 reduction electrocatalyst” in Chemical Science (2018). I also present the multifaceted development of a molecular mechanics force field, an important piece of molecular mechanics simulations that is widely used for molecular structure and property prediction. An open-source Python package for restrained electrostatic potential (RESP), respyte is implemented for developing improved electrostatic potentials (ESP) based charge models for a better description of electrostatic interactions in force fields. I describe further improvements in Open Force Field small molecule force field after the first optimized small molecule force field from Open Force Field Initiative, which includes modification of parameter set for improved performance in certain chemical spaces, and a more careful design of quantum mechanics (QM) training data used to re-optimize bonded parameters.