以间苯二酚为原料,采用模板法制备了中空炭纳米球,并以三聚氰胺为氮源对其进行氮掺杂,采用扫描电子显微镜、透射电子显微镜、X射线衍射仪及物理化学吸附仪等对产物的形貌和结构进行了表征,最后以4-硝基苯酚的还原反应为模型考察了氮掺杂中空炭纳米球的催化性能。结果表明,中空炭纳米球具有明显的中空结构,表面光滑,形貌规则,尺寸均匀,平均直径约为300nm;氮掺杂中空炭纳米球具有无定型碳结构,孔结构表征结果表明材料具有较大的比表面积,且存在微孔-介孔分级结构。三聚氰胺与中空炭纳米球质量比(胺炭比)对材料的比表面积有明显的影响,随着胺炭比的逐渐增大,材料的比表面积先增大后减小,当胺炭比为0.6时,材料的比表面积最大,为236.54m2/g。氮掺杂中空炭纳米球对4-硝基苯酚的还原反应具有良好的催化作用,且胺炭比对材料的催化性能有显著影响,随着胺炭比的逐渐增大,4-硝基苯酚的转化率先增大后减小,胺炭比为0.6时制备的氮掺杂中空炭纳米球催化性能最好,转化率高达90.8%。这一方面是因为氮掺杂使得材料的比表面积增大,同时掺杂后使得材料的表面亲水性也得到改善,缺陷和活性位点增加,从而使得材料的催化性能显著提高。
Hollow carbon nanospheres were prepared by template method with resorcinol as the raw material,followed by nitrogen doping with melamine as the nitrogen source to obtain N-doped hollow carbon nanospheres (HCNSs-X).The morphology and structure of the products were characterized by scanning electron microscopy (SEM),transmission electron microscopy (TEM),X-ray diffraction (XRD),and physical adsorption analysis.At last,the catalytic performance of the HCNSs-X was evaluated using the reduction reaction of 4-nitrophenol as a model reaction.The results showed obviously that the hollow carbon nanospheres displayed hollow structure,with smooth surface and regular morphology.They were uniform in size and the average diameter was about 300nm.N-doped hollow carbon nanospheres exhibited amorphous carbon structure.The pore structure characterization revealed that HCNSs-X had a high specific surface area and a hierarchical micro-mesoporous structure.The mass ratio of melamine to hollow carbon nanospheres (amine-carbon ratio) had a significant impact on the specific surface area of the material.With the gradual increase of the amine-carbon ratio,the specific surface area of the material first increased and then decreased.When the amine-carbon ratio was 0.6,the material achieved the highest specific surface area of 236.54m2/g.The N-doped hollow carbon nanospheres demonstrated excellent catalytic performance in the reduction reaction of 4-nitrophenol.The amine-carbon ratio displayed significant influence on the catalytic activity of HCNSs-X.As the ratio increased gradually,the conversion of 4-nitrophenol first increased and then decreased.When the ratio was 0.6,HCNSs-X exhibited the best catalytic activity,achieving a conversion rate as high as 90.8%.This was because nitrogen doping increased the specific surface area of materials.Meanwhile,the surface hydrophilicity of the materials was improved,increasing more defects and active sites,thereby significantly improving the catalytic activity.
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基金资助
2022年度郑州工程技术学院技术研发推广与转化基金项目(zjz202207);2025年度河南省高等学校重点科研项目(25B430033)
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