Hollow Nitrogen- or Boron-Doped Carbon Submicrospheres with a Porous Shell: Preparation and Application as Supports for Hydrodechlorination Catalysts
Hollow Nitrogen- or Boron-Doped Carbon Submicrospheres with a Porous Shell: Preparation and Application as Supports for Hydrodechlorination Catalysts
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DOI：
10.1021/acs.iecr.7b01183
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发表时间：
2017-06
影响因子：
4.2
通讯作者：
N. Alonso-Morales;C. Ruiz-García;J. Palomar;F. Heras;L. Calvo;J. J. Rodriguez-J.;M. A. Gilarranz
中科院分区：
文献类型：
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作者：
N. Alonso-Morales;C. Ruiz-García;J. Palomar;F. Heras;L. Calvo;J. J. Rodriguez-J.;M. A. Gilarranz
通过模板法制备了具有中空核和多孔壳的氮或硼掺杂的碳亚微球，并将其用作Pd/C催化剂的载体。碳前体是使用吡啶、1，10-菲咯啉和四苯硼钠作为掺杂剂生成为二氧化硅模板的酚醛树脂。掺杂碳中氮和硼的原子百分比分别达到0.5-3.6和0.03-0.67。达到了高达1846 m2/g的高比表面积，其中中孔具有重要贡献。由于载体的形态、多孔结构和掺杂，所制备的钯催化剂（1%w）表现出独特的特征。活性相作为具有窄尺寸分布（<10 nm）的纳米颗粒良好地分散在厚度为77-124 nm的外壳中。反应物所需的短扩散路径和壳层发达的中孔网络有助于减少传质限制。催化剂的活性为50-76 mmol/g。
Nitrogen- or boron-doped carbon submicrospheres with a hollow core and a porous shell were prepared via a template method and tested as supports for Pd/C catalysts. The carbon precursor was a phenol-formaldehyde resin that was generated into a silica template using pyridine, 1,10-phenantroline, and sodium tetraphenylborate as doping agents. The nitrogen and boron atomic percentages in doped carbon reached 0.5–3.6 and 0.03–0.67, respectively. High specific areas of up to 1846 m2/g with an important contribution of mesopores were achieved. The prepared Pd catalysts (1% w) exhibited unique features due to the morphology, porous structure, and doping of the support. The active phase was well-dispersed as nanoparticles with narrow size distribution (<10 nm) in an outer shell with a thickness of 77–124 nm. The short diffusion path needed for reactants and the well-developed network of mesopores of the shell contributed to diminish mass-transfer constraints. The catalysts showed remarkable activity (50–76 mmol/g...