Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals

Abstract

We provide a critical overview of progress and challenges in computationally modeling multistep reaction mechanisms relevant for catalysis and electrocatalysis.We first discuss how the chemical and materials space of energetically efficient catalysis can be explored with computational chemistry. Since reactions for renewable energy catalysis can involve acid-base chemistry and/or ions under aqueous conditions, we then summarize how solvation can be modeled with quantum chemistry schemes using implicit, mixed implicit/explicit, and fully explicit solvation modeling. We will discuss the insights (and limitations) of these solvation models primarily through the scope of understanding CO 2 reduction reaction mechanisms, but these will also be applicable for future work elucidating other reaction mechanisms of critical importance for human sustainability such as H 2 O oxidation and N 2 reduction. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis K E Y W O R D S cluster-continuum, CO 2 reduction, mixed implicit/explicit, phase diagrams, Pourbaix diagrams, solvation modeling

Assessing conformer energies using electronic structure and machine learning methods

“…[15] Moreover, much chemistry is performed in solution; thus, work on understanding conformer energies in solvation is also critical. [117,118] ACKNOWLEDGMENTS GRH and DLF acknowledge the National Science Foundation (CHE-1800435) for support and the University of Pittsburgh Center for Research…”

“…[ 15 ] Moreover, much chemistry is performed in solution; thus, work on understanding conformer energies in solvation is also critical. [ 117,118 ]…”

Assessing Conformer Energies using Electronic Structure and Machine Learning Methods

“…15 Moreover, much chemistry is performed in solution, work on understanding conformer energies in solvation is also critical. 117,118…”

Assessing Conformer Energies using Electronic Structure and Machine Learning Methods

“…[15] Moreover, much chemistry is performed in solution, thus work on understanding conformer energies in solvation is also critical. [119], [120]…”