Shenyang National Laboratory for Materials Science Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, 110016, China.
Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, China.
Angew Chem Int Ed Engl. 2017 Jan 9;56(2):600-604. doi: 10.1002/anie.201609047. Epub 2016 Dec 7.
Metal-free carbocatalysts enriched with specific oxygenated groups with different morphology and size were synthesized from glucose by hydrothermal carbonization, in which cheap and widely available biomass could be converted into functionalized carbon using an environmentally benign process. The hydroxy- and carbonyl-enriched hydrothermal carbon (HTC) could be used in nitrobenzene reduction, and higher conversion was obtained on the sphere morphology with smaller size. In the Beckmann rearrangement of cyclohexanone oxime, carboxyl-enriched HTC exhibited superior performance compared with conventional solid acid (such as HY and HZSM-5), on which the strong acid sites and weak Lewis acid sites lead to high selectivity for the side product. Although the intrinsic acidity of carbon is weak, the carboxyl-enriched carbon was used in weak Brønsted acid-catalyzed reactions, such as the Beckmann rearrangement.
通过水热碳化,从葡萄糖中合成了富含特定含氧基团、具有不同形态和尺寸的无金属碳催化剂,其中廉价且广泛存在的生物质可通过环境友好的方法转化为功能化碳。富含羟基和羰基的水热碳(HTC)可用于硝基苯还原,且形态为球形且尺寸较小的物质转化率更高。在环己酮肟的贝克曼重排反应中,与传统固体酸(如 HY 和 HZSM-5)相比,富含羧基的 HTC 表现出更优异的性能,这是因为其强酸性位和弱路易斯酸性位导致副产物的选择性较高。尽管碳的本征酸性较弱,但富含羧基的碳可用于弱布朗斯台德酸催化反应,如贝克曼重排反应。