Activating Cobalt Nanoparticles via the Mott–Schottky Effect in Nitrogen-Rich Carbon Shells for Base-Free Aerobic Oxidation of Alcohols to Esters,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Activating Cobalt Nanoparticles via the Mott–Schottky Effect in Nitrogen-Rich Carbon Shells for Base-Free Aerobic Oxidation of Alcohols to Esters
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-01-06 , DOI: 10.1021/jacs.6b10710
Hui Su ₁ , Ke-Xin Zhang ₁ , Bing Zhang ₁ , Hong-Hui Wang ₁ , Qiu-Ying Yu ₁ , Xin-Hao Li ₁ , Markus Antonietti ₂ , Jie-Sheng Chen ₁

Affiliation

Heterogeneous catalysts of inexpensive and reusable transition-metal are attractive alternatives to homogeneous catalysts; the relatively low activity of transition-metal nanoparticles has become the main hurdle for their practical applications. Here, the de novo design of a Mott-Schottky-type heterogeneous catalyst is reported to boost the activity of a transition-metal nanocatalyst through electron transfer at the metal/nitrogen-doped carbon interface. The Mott-Schottky catalyst of nitrogen-rich carbon-coated cobalt nanoparticles (Co@NC) was prepared through direct polycondensation of simple organic molecules and inorganic metal salts in the presence of g-C3N4 powder. The Co@NC with controllable nitrogen content and thus tunable Fermi energy and catalytic activity exhibited a high turnover frequency (TOF) value (8.12 mol methyl benzoate mol-1 Co h-1) for the direct, base-free, aerobic oxidation of benzyl alcohols to methyl benzoate; this TOF is 30-fold higher than those of the state-of-the-art transition-metal-based nanocatalysts reported in the literature. The presented efficient Mott-Schottky catalyst can trigger the synthesis of a series of alkyl esters and even diesters in high yields.

中文翻译：

通过富氮碳壳中的莫特-肖特基效应活化钴纳米颗粒，用于醇类无碱有氧氧化成酯类

廉价且可重复使用的过渡金属的多相催化剂是均相催化剂的有吸引力的替代品；过渡金属纳米粒子相对较低的活性已成为其实际应用的主要障碍。在这里，据报道，莫特-肖特基型多相催化剂的从头设计通过金属/氮掺杂碳界面的电子转移来提高过渡金属纳米催化剂的活性。在g-C3N4粉末存在下，通过简单有机分子和无机金属盐的直接缩聚反应制备了富氮碳包覆钴纳米粒子（Co@NC）的Mott-Schottky催化剂。具有可控氮含量、从而可调费米能量和催化活性的 Co@NC 表现出高周转频率 (TOF) 值 (8. 12 mol 苯甲酸甲酯 mol-1 Co h-1) 用于将苯甲醇直接、无碱、有氧氧化成苯甲酸甲酯；该 TOF 比文献中报道的最先进的基于过渡金属的纳米催化剂的 TOF 高 30 倍。所提出的高效莫特-肖特基催化剂可以引发一系列烷基酯甚至二酯的高产率合成。

更新日期：2017-01-06

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南