Selective oxidation of aromatic alcohols to aldehydes with oxygen is of crucial importance for industrial catalysis, while obtaining high selectivity for easily over-oxidized target products at high conversion is challenging. Herein, Co single atoms supported by nitrogen doped carbon catalysts (Co₁/NC) were successfully prepared by a self-assembly–pyrolysis strategy and applied into the oxidation of benzyl alcohol to benzaldehyde. The reaction results showed that Co₁/NC catalysts exhibited excellent performance compared to Co nanoparticles supported by nitrogen doped carbon catalyst (Co_NPs/NC), among which the 4-Co₁/NC catalyst achieved 95.2% benzyl alcohol conversion and nearly 99.9% benzaldehyde selectivity. Advanced characterization combined with density functional theory calculations demonstrated that the exceptional catalytic performance of Co₁/NC catalysts was attributed to the formed CoN₄ sites, which could moderately activate oxygen and accelerate the desorption of generated benzaldehyde through the electron transfer from Co to the support. The work provides a new insight into the catalysis of single atom sites and their potential applications in alcohol oxidation.

中文翻译：

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Co1/NC 催化剂高选择性氧化苯甲醇生成苯甲醛

用氧气选择性氧化芳香醇生成醛对于工业催化至关重要，而在高转化率下获得易过度氧化的目标产物的高选择性具有挑战性。在此，通过自组装热解策略成功制备了氮掺杂碳催化剂负载的Co单原子（Co ₁ /NC），并将其应用于苯甲醇氧化为苯甲醛。反应结果表明，与氮掺杂碳负载的纳米粒子Co催化剂（Co _{NPs /NC）相比，Co 1} /NC催化剂表现出优异的性能，其中4-Co ₁ /NC催化剂实现了95.2%的苯甲醇转化率和近99.9%的苯甲醇转化率。苯甲醛的选择性。先进的表征结合密度泛函理论计算表明，Co ₁ /NC催化剂的优异催化性能归因于形成的CoN ₄位点，该位点可以适度活化氧并通过从Co到载体的电子转移加速生成的苯甲醛的解吸。这项工作为单原子位点的催化及其在醇氧化中的潜在应用提供了新的见解。