Efficient predictive tools for oxygen evolution reaction (OER) activity assessment are vital for rational design of anodes for green hydrogen production. Reaction mechanism prediction represents an important pre-requisite for such catalyst design. Even then, lattice oxygen evolution remains understudied and without reliable prediction methods. We propose a computational screening approach using density functional theory to evaluate the lattice oxygen evolution tendency in candidate surfaces. The method is based on a systematic assessment of the adsorption energies of oxygen evolution intermediates on model active sites with varying local structure. The power of the model is shown on model rutile (110) oriented surfaces of a) RuO2, b) Ru(1−x)Ni(x)O2 and c) Ru(1−x)Ti(x)O2. The model predicts a) no lattice exchange, b) lattice exchange at elevated electrode potentials and c) minor lattice exchange at elevated electrode potentials and high titanium content. While in the case of a) and b) the predictions provide sufficiently accurate agreement with experimental data, c) experimentally deviates from the above prediction by expressing a high tendency to evolve lattice oxygen at high titanium content (x = 0.20). This discrepancy can likely be attributed to the presence of structural defects in the prepared material, which are hard to accurately model with the applied methodology.

中文翻译：

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金红石 Ru(1−x)Ni(x)O2 电催化剂中晶格析氧

析氧反应（OER）活性评估的有效预测工具对于合理设计绿色制氢阳极至关重要。反应机理预测是此类催化剂设计的重要先决条件。即便如此，晶格氧的演化仍然没有得到充分研究，并且没有可靠的预测方法。我们提出了一种使用密度泛函理论的计算筛选方法来评估候选表面中的晶格氧演化趋势。该方法基于对具有不同局部结构的模型活性位点上析氧中间体的吸附能的系统评估。模型的功率显示在 a) RuO2、b) Ru(1−x)Ni(x)O2 和 c) Ru(1−x)Ti(x)O2 的模型金红石 (110) 取向表面上。该模型预测 a) 无晶格交换，b) 在升高的电极电势下发生晶格交换，以及 c) 在升高的电极电势和高钛含量下发生少量晶格交换。虽然在 a) 和 b) 的情况下，预测与实验数据提供了足够准确的一致性，但 c) 通过在高钛含量 (x = 0.20) 下表现出析出晶格氧的高趋势，在实验上偏离了上述预测。这种差异可能是由于制备的材料中存在结构缺陷，这些缺陷很难用所应用的方法进行准确建模。