物理化学学报2021，Vol.37Issue(10)：135-142,8.DOI:10.3866/PKU.WHXB202001025
富氮空心蠕虫状碳材料的合成及其苯甲醇非金属选择性催化氧化的高活性
Hollow Nitrogen-Rich Carbon Nanoworms with High Activity for Metal-Free Selective Aerobic Oxidation of Benzyl Alcohol
摘要
Abstract
Carbon materials have become one of the research hotspots in the field of catalysis as a typical representative of non-metallic catalytic materials.Herein,a facile synthetic strategy is developed to fabricate a series of hollow carbon nanoworms (h-NCNWs) that contain nitrogen up to 9.83 wt％ by employing graphitic carbon nitride (g-C3N4) as the sacrificing template and solid nitrogen source.The h-NCNWs catalysts were characterized by X-ray diffraction (XRD),high-resolution transmission electron microscope (HR-TEM),N2 adsorption-desorption,Fourier transform infrared spectroscopy (FT-IR),thermal gravimetric (TG),Raman spectra,and X-ray photoelectron spectroscopies (XPS).The catalytic activities of the h-NCNWs catalysts for selective oxidation of benzyl alcohol with O2 were also evaluated.The characterization results revealed that the h-NCNWs catalysts displayed a unique hollow worm-like nanostructure with turbostratic carbon shells.The nitrogen content and shell thickness can be tuned by varying the relative ratio of resorcinol to g-C3N4 during the preparation process.Furthermore,nitrogen is incorporated to the carbon network in the form of graphite (predominantly) and pyridine,which is critical for the enhancement of the catalytic activity of carbon catalysts for the selective oxidation of benzyl alcohol.At a reaction temperature of 120 ℃,a 24.9％ conversion of benzyl alcohol with ＞ 99％ selectivity to benzaldehyde can be achieved on the h-NCNWs catalyst prepared with a mass ratio of resorcinol to g-C3N4 of 0.5.However,the catalytic activities of the h-NCNWs catalysts were dependent on the amount of N dopants,in particular graphitic nitrogen species.The conversion of benzyl alcohol markedly decreased to 13.1％ on the h-NCNWs catalyst prepared with a mass ratio of resorcinol to g-C3N4 of 1.5.Moreover,the h-NCNWs catalyst showed excellent stability during the reaction process.The conversion of benzyl alcohol and the high selectivity to aldehyde can be kept within five catalytic runs over the h-NCNWs0.5 catalyst.These results indicate that rationally designed carbon materials have great potential as highly efficient heterogeneous catalysts for oxidation reactions.关键词
中空纳米结构/N掺杂/非金属催化剂/选择氧化/苯甲醇Key words
Hollow nanostructure/Nitrogen doping/Metal-free catalyst/Selective oxidation/Benzyl alcohol分类
化学化工引用本文复制引用
安平,付宇,韦丹蕾,郭杨龙,詹望成,张金水..富氮空心蠕虫状碳材料的合成及其苯甲醇非金属选择性催化氧化的高活性[J].物理化学学报,2021,37(10):135-142,8.基金项目
国家自然科学基金(21972022,U1805255),111项目(D16008),福建省自然科学基金(2018J01681)和能源与环境光催化国家重点实验室自主研究项目(SKLPEE-2017A03)资助项目 The project was supported by the National Natural Science Foundation of China (21972022,U1805255),the 111 Project (D16008),Natural Science Foundation of Fujian Province,China (2018J01681),and the Independent Research Project of State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-2017A03). （21972022,U1805255）
