The difficulty of the oxygen evolution reaction (OER) is a fundamental impediment to the sustainable production of hydrogen, in which molecular catalysts show the most impressive activity in terms of turnover frequency. Here, we interrogate 444 automatically generated molecular water oxidation catalysts composed of well-known ligand scaffolds and 6 different transition metals (Cr, Mn, Fe, Ru, Co, and Ni). These data confirm the method-independent universal scaling relationship for water oxidation catalysts, describe routes toward circumventing this relationship, and justify the ascendency of Ru catalysts for this reaction. Leveraging this information while applying catalyst design principles, we summarize experimental results, giving credence to our prediction of 9 earth-abundant molecular catalysts with theoretical overpotentials ranging from 200 to 400 mV as promising leads for experimental investigation. We also establish insights into spin-dependent scaling relations for key OER intermediates. Altogether, this work outlines the first steps toward enabling inverse design for molecular OER catalysts.

析氧反应 (OER) 的困难是可持续生产氢气的根本障碍，其中分子催化剂在转换频率方面表现出最令人印象深刻的活性。在这里，我们询问了 444 种自动生成的分子水氧化催化剂，这些催化剂由众所周知的配体支架和 6 种不同的过渡金属（Cr、Mn、Fe、Ru、Co 和 Ni）组成。这些数据证实了与方法无关的水氧化催化剂的通用比例关系，描述了规避这种关系的途径，并证明了 Ru 催化剂在该反应中的优势。在应用催化剂设计原则的同时利用这些信息，我们总结了实验结果，相信我们对 9 种地球上丰富的分子催化剂的预测，其理论过电位范围为 200 到 400 mV，作为实验研究的有希望的线索。我们还深入了解了关键 OER 中间体的自旋相关缩放关系。总之，这项工作概述了实现分子 OER 催化剂逆向设计的第一步。