The electrocatalytic two-electron oxygen reduction reaction (2e ORR) synthesis of hydrogen peroxide (HO) is an eco-friendly process. In this study, density functional theory (DFT) and machine learning (ML) were utilized to systematically explore various single metal atoms anchored on mono-vacancy fullerene C (TM@C) for HO production Among 19 single-atom catalysts (SACs), Sc@C and Y@C were identified for high the thermodynamic feasibility of HO formation, exhibiting overpotentials of 0.01 V and 0.02 V, respectively. Moreover, competitive four-electron oxygen reduction reaction (4e ORR) and hydrogen evolution reaction (HER) were significantly suppressed on these two catalysts. The formation of peroxide intermediates on the two screened SACs was identified as key to achieving high activity and selectivity for HO formation. Analysis using ML methods also revealed that the balance between bond strengths and adsorption energies for O is crucial in regulating the performance of 2e ORR. These results offer important insights for electrocatalytic HO production.

中文翻译：

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使用嵌入碳空位富勒烯C60中的单一过渡金属原子筛选用于合成过氧化氢的高效电催化剂


电催化双电子氧还原反应（2e ORR）合成过氧化氢（H2O）是一种生态友好的过程。在这项研究中，利用密度泛函理论（DFT）和机器学习（ML）系统地探索了锚定在单空位富勒烯C（TM@C）上的各种单金属原子用于H2O生产的19种单原子催化剂（SAC）中， Sc@C 和 Y@C 被认为具有 H2O 形成的高热力学可行性，分别表现出 0.01 V 和 0.02 V 的过电势。此外，这两种催化剂显着抑制了竞争性四电子氧还原反应（4e ORR）和析氢反应（HER）。两个筛选的 SAC 上过氧化物中间体的形成被认为是实现 H2O 形成高活性和选择性的关键。使用ML方法的分析还表明，O的键强度和吸附能之间的平衡对于调节2e ORR的性能至关重要。这些结果为电催化 H2O 生产提供了重要的见解。