The development of efficient, durable, and cost‐effective bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is essential in the advancement of solar fuels, metal–air batteries, and unitized regenerative fuel cells. This work demonstrates an effective approach of activating 2D carbon for highly efficient bifunctional oxygen reactions without N‐doping, let alone a transition metal–nitrogen (TM–N_x) moiety, the usual component needed for high oxygen electrocatalytic activities. A solvothermally synthesized ceria (CeO₂)–hydroxylated graphene hybrid catalyst shows excellent bifunctional ORR/OER activities both in alkaline and acidic solutions. Density functional theory calculations reveal that the activation of graphene occurs via topmost oxygens on ceria surface, but only when low coverage of hydroxyl groups is present on graphene. Furthermore, catalytically active forms of graphene share similar hydroxylated structural motifs. Finally, a simple approach of dramatically enhancing durability even in acidic media is demonstrated.

中文翻译：

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二氧化铈功能化石墨烯中实现的高活性双功能氧电催化位点

开发用于氧气还原反应（ORR）和氧气释放反应（OER）的高效，耐用且具有成本效益的双功能电催化剂对于太阳能，金属空气电池和组合式可再生燃料电池的发展至关重要。这项工作展示了一种无需进行N掺杂即可激活2D碳的高效双功能氧反应的有效方法，更不用说过渡金属-氮（TM-N _x）部分，这是高氧电催化活性所需的常用组分。溶剂热合成二氧化铈（CeO ₂）–羟基化的石墨烯杂化催化剂在碱性和酸性溶液中均具有出色的双官能ORR / OER活性。密度泛函理论计算表明，石墨烯的活化是通过二氧化铈表面的最高氧发生的，但仅当石墨烯上的羟基覆盖率较低时才发生。此外，石墨烯的催化活性形式具有相似的羟基化结构基序。最后，展示了一种即使在酸性介质中也能显着提高耐久性的简单方法。