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Cobalt Single Atoms Embedded in Nitrogen‐Doped Graphene for Selective Oxidation of Benzyl Alcohol by Activated Peroxymonosulfate
Small ( IF 13.0 ) Pub Date : 2021-01-19 , DOI: 10.1002/smll.202004579 Jiaquan Li 1 , Shiyong Zhao 1 , Lianji Zhang 2 , San Ping Jiang 1 , Shi‐Ze Yang 3 , Shaobin Wang 4 , Hongqi Sun 5 , Bernt Johannessen 6 , Shaomin Liu 1, 7
Small ( IF 13.0 ) Pub Date : 2021-01-19 , DOI: 10.1002/smll.202004579 Jiaquan Li 1 , Shiyong Zhao 1 , Lianji Zhang 2 , San Ping Jiang 1 , Shi‐Ze Yang 3 , Shaobin Wang 4 , Hongqi Sun 5 , Bernt Johannessen 6 , Shaomin Liu 1, 7
Affiliation
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The development of novel single atom catalyst (SAC) is highly desirable in organic synthesis to achieve the maximized atomic efficiency. Here, a Co‐based SAC on nitrogen‐doped graphene (SACo@NG) with high Co content of 4.1 wt% is reported. Various characterization results suggest that the monodispersed Co atoms are coordinated with N atoms to form robust and highly effective catalytic centers to activate peroxymonosulfate (PMS) for organic selective oxidation. The catalytic performance of the SACo@NG/PMS system is conducted on the selective oxidation of benzyl alcohol (BzOH) showing high efficiency with over 90% conversion and benzaldehyde selectivity within 180 min under mild conditions. Both radical and non‐radical processes occurred in the selective oxidation of BzOH, but the non‐radical oxidation plays the dominant role which is accomplished by the adsorption of BzOH/PMS on the surface of SACo@NG and the subsequent electron transfer through the carbon matrix. This work provides new insights to the preparation of efficient transition metal‐based single atom catalysts and their potential applications in PMS mediated selective oxidation of alcohols.
中文翻译：
嵌入氮掺杂石墨烯中的钴单原子用于活化过氧单硫酸盐选择性氧化苄醇
在有机合成中，为了获得最大的原子效率，非常需要开发新型的单原子催化剂（SAC）。在此，据报道，Co含量为4.1 wt％的氮掺杂石墨烯（SACo @ NG）上的Co基SAC。各种表征结果表明，单分散的Co原子与N原子配位形成强大而高效的催化中心，以激活过氧单硫酸盐（PMS）进行有机选择性氧化。SACo @ NG / PMS系统的催化性能是在温和的条件下于180分钟内对苯甲醇（BzOH）进行选择性氧化而显示出高效率，超过90％的转化率和对苯甲醛的选择性。自由基和非自由基过程都发生在BzOH的选择性氧化中，但是非自由基氧化起主要作用，这是通过SACo @ NG表面上BzOH / PMS的吸附以及随后电子通过碳基质的转移来实现的。这项工作为高效过渡金属基单原子催化剂的制备及其在PMS介导的醇选择性氧化中的潜在应用提供了新见解。
更新日期：2021-01-19
中文翻译：
嵌入氮掺杂石墨烯中的钴单原子用于活化过氧单硫酸盐选择性氧化苄醇
在有机合成中，为了获得最大的原子效率，非常需要开发新型的单原子催化剂（SAC）。在此，据报道，Co含量为4.1 wt％的氮掺杂石墨烯（SACo @ NG）上的Co基SAC。各种表征结果表明，单分散的Co原子与N原子配位形成强大而高效的催化中心，以激活过氧单硫酸盐（PMS）进行有机选择性氧化。SACo @ NG / PMS系统的催化性能是在温和的条件下于180分钟内对苯甲醇（BzOH）进行选择性氧化而显示出高效率，超过90％的转化率和对苯甲醛的选择性。自由基和非自由基过程都发生在BzOH的选择性氧化中，但是非自由基氧化起主要作用，这是通过SACo @ NG表面上BzOH / PMS的吸附以及随后电子通过碳基质的转移来实现的。这项工作为高效过渡金属基单原子催化剂的制备及其在PMS介导的醇选择性氧化中的潜在应用提供了新见解。
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