Previously we outlined possible doping strategies to improve the aqueous electrocatalytic oxygen evolving activity of iron-doped nickel oxyhydroxide (Ni_1–xFe_xOOH). The strategies are based on two central mechanistic features of its efficient water oxidation: (1) metal-oxo bond formation and (2) three-electron reductive elimination of O₂. Here, we explore secondary dopants that may promote the latter by enhancing O–O bond formation. From periodic slab models using screened-exchange hybrid density functional theory, we predict that Fe³⁺-doped β-NiOOH codoped with Cu²⁺ or Ag³⁺ will have even more favorable O–O coupling and molecular O₂ desorption activity at the Fe sites. This work illustrates a mechanism-oriented design principle in the development of oxygen evolution catalysts.

中文翻译：

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二次过渡金属掺杂剂可增强Fe掺杂的β-NiOOH上电化学O _2的形成和脱附

先前，我们概述了可能的掺杂策略，以改善铁掺杂的羟基氧化镍（Ni _{1- x} Fe _x OOH）的水溶液电催化氧析出活性。该策略基于其有效水氧化的两个主要机理特征：（1）金属-氧键形成和（2）O _2的三电子还原消除。在这里，我们探索可以通过增强O-O键的形成来促进后者的次级掺杂剂。从使用屏蔽交换混合密度泛函理论的周期性平板模型中，我们预测，与Cu ²⁺或Ag ³⁺共掺杂的Fe ³⁺掺杂的β-NiOOH将具有更有利的O-O耦合和分子O ₂铁部位的解吸活性。这项工作说明了在析氧催化剂的开发中面向机制的设计原理。