Yang Yuying, Li Hong, Pei Supeng, Liu Feng, Feng Wei, Zhang Yongming
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Key Lab of Electrical Insulation and Thermal Aging, Shanghai Jiao Tong University No. 800 Dongchuan Rd., Minhang District Shanghai 200240 China
School of Chemical and Environmental Engineering, Shanghai Institute of Technology Shanghai 201418 China
RSC Adv. 2020 Nov 23;10(69):42408-42412. doi: 10.1039/d0ra05238h. eCollection 2020 Nov 17.
CO, the main greenhouse gas, has received considerable attention due to environmental issues. From a scientific perspective, CO as a cheap and abundant carbon source, could be applied in synthesizing more valuable chemicals such as urea, formic acid, and cyclic carbonates. However, the high bond energy of C[double bond, length as m-dash]O (750 kJ mol) and the non-polarity property make CO molecules difficult to activate. In this paper, we have carefully designed a low-cost, stable and, most importantly, highly efficient Co-based heterocatalyst Co@N C functionalized by nitrogen-doped carbon to activate CO molecules and convert it into cyclic carbonates. The CO conversion process could be triggered at very mild conditions (60 °C and 1 bar CO). We carefully adjusted the nitrogen content in the carbon support to enhance the catalytic performance of Co centers the interface effect. Consequently, the optimal catalyst displayed extraordinary activity toward the cycloaddition of CO with styrene oxide as high conversion (92%) and selectivity (>99%) were achieved in 4 h without byproducts.
一氧化碳作为主要的温室气体，由于环境问题已受到广泛关注。从科学角度来看，一氧化碳作为一种廉价且丰富的碳源，可用于合成更有价值的化学品，如尿素、甲酸和环状碳酸酯。然而，碳氧双键（键能为750 kJ/mol）的高键能以及非极性特性使得一氧化碳分子难以被活化。在本文中，我们精心设计了一种低成本、稳定且最重要的是高效的钴基异质催化剂Co@N C，通过氮掺杂碳对其进行功能化，以活化一氧化碳分子并将其转化为环状碳酸酯。一氧化碳转化过程可在非常温和的条件下（60℃和1 bar一氧化碳）触发。我们仔细调整了碳载体中的氮含量，以增强钴中心的催化性能——界面效应。因此，最佳催化剂对一氧化碳与环氧苯乙烯的环加成反应表现出非凡的活性，在4小时内实现了高转化率（92%）和高选择性（>99%），且无副产物。
