An ideal catalytic process for the selective oxidation of hydrocarbons should employ an efficient, recyclable, and cost-effective catalyst under solvent- and additive-free conditions with molecular oxygen as the only oxidant. This is an important goal in the catalysis community and remains a significant challenge. In this respect, we report the facile construction of a series of uniform CeO₂ nanoparticle-decorated Co₃O₄ microspheres (CeO₂/Co₃O₄) for the selective ethylbenzene oxidation reaction by molecular oxygen. Among the catalysts with various CeO₂ loading levels, CeO₂/Co₃O₄-3 (5 wt % loading of CeO₂) obtained by careful composition modulation exhibits the optimum reaction performance, with ethylbenzene conversion of 73.4% accompanied by a selectivity of 78.5% to acetophenone. The yield of acetophenone can achieve 57.6%, while the reaction rate can reach up to 401.3 mmol g_cat^–1 h^–1. In addition, CeO₂/Co₃O₄-3 presents robust stability and good recycling performance. The tailored CeO₂/Co₃O₄-3 catalyst is superior to the reported catalysts, and it is the state-of-the-art catalyst under the current challenging reaction system. Experimental evidence and mechanism analysis suggest that the interface synergy featured with −Ce–O_V–Co– active sites derived from the intimate connection between the two oxides is the dominant contributor in boosting the catalytic performance. This work can reinvigorate research into the exploitation of catalysts for the sustainable and green catalytic oxidation of ethylbenzene and beyond.

中文翻译：

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CeO ₂纳米颗粒修饰的Co ₃ O ₄微球在无溶剂和无添加剂条件下用分子氧选择性氧化乙苯

用于烃类选择性氧化的理想催化方法应在无溶剂和无添加剂的条件下，使用分子氧作为唯一氧化剂，使用高效，可回收且具有成本效益的催化剂。这是催化领域的重要目标，并且仍然是一项重大挑战。在这方面，我们报道了用于分子氧选择性乙苯氧化反应的一系列均匀的CeO ₂纳米粒子修饰的Co ₃ O ₄微球（CeO ₂ / Co ₃ O ₄）的简便构建。在具有不同CeO ₂负载量的催化剂中，CeO ₂ / Co ₃ O ₄通过仔细的组成调节获得的-3（5重量％的CeO ₂负载）表现出最佳的反应性能，乙苯转化率为73.4％，同时对苯乙酮的选择性为78.5％。苯乙酮的收率可以达到57.6％，而反应速率可以达到401.3 mmol g _cat ^–1 h ^–1。另外，CeO ₂ / Co ₃ O ₄ -3呈现出稳定的稳定性和良好的再循环性能。量身定制的CeO ₂ / Co ₃ O ₄-3催化剂优于已报道的催化剂，在当前具有挑战性的反应体系下，它是最先进的催化剂。实验证据和机理分析表明，源自两种氧化物之间紧密连接的-Ce–O _V –Co–活性位点的界面协同作用是促进催化性能的主要因素。这项工作可以重振对催化剂开发的研究，以实现乙苯及其他产品的可持续和绿色催化氧化。