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WIREs Comput Mol Sci
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Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals

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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 CO2 reduction reaction mechanisms, but these will also be applicable for future work elucidating other reaction mechanisms of critical importance for human sustainability such as H2O oxidation and N2 reduction. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis
A “square‐scheme” diagram of hypothetical pathways for a multistep (de)hydrogenation process
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Simplistic view of umbrella sampling along a hypothetical constrained variable
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A model metadynamics simulation profile. Gaussian functions are placed on the free energy surface to flatten the energy wells over time during the simulation (lighter to darker curves). This is used to reduce oversampling of the local minima and pushes the system away from it
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A methanol molecule being explicitly solvated by water
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A model cluster with three explicit solvent molecules and implicit solvation
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(a) Illustration of a methanol molecule modeled within a cavity of a nonperiodic continuum solvation model. (b) Illustration of a methanol molecule modeled at a surface within a cavity of a periodic continuum solvation model
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(a) Pourbaix diagram showing stable states of the reactant, CO2; (b) Pourbaix diagram showing stable states of a hypothetical molecular catalyst, 1,10‐phenanthroline; (c) overlaid Pourbaix diagrams from (a) and (b) showing similar boundaries for hydrogen shuttling and CO2 reduction. Vertical lines represent pKas, the horizontal lines represent the pH‐independent standard redox potentials and the diagonal lines represent the pH‐dependent proton‐coupled electron transfer steps
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Structure and Mechanism > Reaction Mechanisms and Catalysis

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