Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals
Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals
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DOI：
10.1002/wcms.1446
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发表时间：
2019-10-17
影响因子：
11.4
通讯作者：
Keith, John A.
中科院分区：
文献类型：
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作者：
Basdogan, Yasemin;Maldonado, Alex M.;Keith, John A.
我们提供了一个关键的进展和挑战，在计算建模多步反应机制的催化和电催化。我们首先讨论如何化学和材料空间的能量有效的催化可以探索与计算化学。由于可再生能源催化反应可能涉及酸碱化学和/或离子在水溶液条件下，然后我们总结了如何溶剂化可以与量子化学方案使用隐式，混合隐式/显式，和完全显式溶剂化建模。我们将主要通过理解CO2还原反应机制的范围来讨论这些溶剂化模型的见解（和局限性），但这些也将适用于未来的工作，阐明对人类可持续发展至关重要的其他反应机制，如H2O氧化和N-2还原。本文分类在：结构与机理>反应机理与催化
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 N-2 reduction. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis