The development of renewable energy sources that are environmentally friendly and economical is of critical importance. The effective utilization of such energy sources relies on catalysts to facilitate the interconversion between electrical and chemical energy through multielectron, multiproton reactions. The design of effective catalysts for these types of energy conversion processes requires the ability to control the localization and movement of electrons and protons, as well as the coupling between them. Theoretical calculations, in conjunction with experimental validation and feedback, are playing a key role in these catalyst design efforts. A general theory has been developed for describing proton-coupled electron transfer (PCET) reactions, which encompass all reactions involving the coupled transfer of electrons and protons, including sequential and concerted mechanisms for multielectron, multiproton processes. In addition, computational methods have been devised to compute the input quantities for the PCET rate constant expressions and to generate free energy pathways for molecular electrocatalysts. These methods have been extended to heterogeneous PCET reactions to enable the modeling of PCET processes at electrode and nanoparticle surfaces.

中文翻译：

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通过理论控制电子和质子：纳米粒子的分子电催化剂

发展对环境友好且经济的可再生能源至关重要。这种能源的有效利用依赖于催化剂，以通过多电子，多质子反应促进电能与化学能之间的相互转化。设计用于这些类型的能量转换过程的有效催化剂需要具有控制电子和质子的定位和运动以及它们之间的耦合的能力。理论计算以及实验验证和反馈在这些催化剂设计工作中起着关键作用。已开发出用于描述质子耦合电子转移（PCET）反应的一般理论，该理论涵盖了所有涉及电子与质子耦合转移的反应，包括用于多电子，多质子过程的顺序机制和协调机制。另外，已经设计了计算方法以计算PCET速率常数表达式的输入量并生成分子电催化剂的自由能途径。这些方法已扩展到异构PCET反应，以能够在电极和纳米颗粒表面建立PCET过程的模型。