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多孔球形/蛋黄壳/空心钯氮掺杂碳球催化剂对4-硝基苯酚催化还原的独特形貌效应

Distinctive morphology effects of porous-spherical/yolk-shell/hollow Pd-nitrogen-doped-carbon spheres catalyst for catalytic reduction of 4-nitrophenol.

作者信息

Long Yu, Liu Yansheng, Zhao Ziming, Luo Sha, Wu Wei, Wu Li, Wen He, Wang Ren-Qi, Ma Jiantai

机构信息

State Key Laboratory of Applied Organic Chemistry (SKLAOC), Gansu Provincial Engineering Laboratory for Chemical Catalysis, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, PR China.

State Key Laboratory of Applied Organic Chemistry (SKLAOC), Gansu Provincial Engineering Laboratory for Chemical Catalysis, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, PR China.

出版信息

J Colloid Interface Sci. 2017 Jun 15;496:465-473. doi: 10.1016/j.jcis.2017.02.051. Epub 2017 Feb 22.

Abstract

Pd-nitrogen-doped-carbon nanocatalysts (Pd-C/N) with different morphologies, such as porous spheres, yolk-shell and hollow structures, had been synthesized and compared. The yolk-shell Pd-nitrogen-doped-carbon nanocatalysts (YS-Pd-C/N) and hollow Pd-nitrogen-doped-carbon nanocatalysts (H-Pd-C/N) were prepared through different etch time using SiO spheres as hard-templates. The as-prepared catalysts were characterized thoroughly by TEM, BET, XRD, FT-IR, and XPS. Importantly, the catalysts have moderate BET specific surface area in the range from 200 to 300mg and pore volume between 0.2 and 0.3cmg. The reduction of 4-nitrophenol is chosen as a model reaction to research the morphology effects of these prepared Pd-C/N catalysts with the same chemical compositions. Interestingly, H-Pd-C/N exhibited the best catalytic performance, which could be attributed to its high nitrogen content, the uniform distribution of abundant active sites, as well as the synergistic effect of graphitic C/N shell and Pd species for the catalytic reaction. Especially, the unique hollow morphology and porous shell of H-Pd-C/N made it to be a nanoreactor, which was beneficial to improve the catalytic activities. In addition, H-Pd-C/N nanocatalysts exhibited favorable stability in the recycling reactions.

摘要

已合成并比较了具有不同形态的钯氮掺杂碳纳米催化剂(Pd-C/N),如多孔球体、蛋黄壳结构和中空结构。以SiO球体为硬模板,通过不同的蚀刻时间制备了蛋黄壳钯氮掺杂碳纳米催化剂(YS-Pd-C/N)和中空钯氮掺杂碳纳米催化剂(H-Pd-C/N)。通过透射电子显微镜(TEM)、比表面积测定(BET)、X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)和X射线光电子能谱(XPS)对所制备的催化剂进行了全面表征。重要的是,这些催化剂具有200至300mg范围内适中的BET比表面积和0.2至0.3cmg之间的孔体积。选择4-硝基苯酚的还原作为模型反应,以研究这些具有相同化学组成的制备的Pd-C/N催化剂的形态效应。有趣的是,H-Pd-C/N表现出最佳的催化性能,这可归因于其高氮含量、丰富活性位点的均匀分布以及石墨化C/N壳和钯物种对催化反应的协同作用。特别是,H-Pd-C/N独特的中空形态和多孔壳使其成为一个纳米反应器,这有利于提高催化活性。此外,H-Pd-C/N纳米催化剂在循环反应中表现出良好的稳定性。

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