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Doped carbon nanostructures as metal-free catalysts for oxidative dehydrogenation of light alkanes

机译:掺杂碳纳米结构作为轻金属烷烃氧化脱氢的无金属催化剂

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摘要

Catalytic reactions are often carried out on various supported metals, these usually being noble metals or metal oxides. Even though metal based catalysts plays a major role in today s industrial processes, they still have several disadvantages, including high cost, proneness to gas poisoning, as well as disadvantageous effect on the environment. Recently, certain carbon nanomaterials have been in the spotlight of several research groups, as carbon has the advantages of wide availability, environmental acceptability, corrosion resistance, in addition to its unique surface properties. The goal is to use the carbon nanomaterials to produce better catalysts - without the use of noble metals.By doping carbon nanofibers and carbon nanotubes with other elements, one can significantly alter their physical and chemical properties, thus making them more reactive. Boron, nitrogen and phosphorus are some of the chemical elements that can be used as doping agents.In this study nitrogen doped carbon nanofibers was investigated, by using them in the oxidative dehydrogenation (ODH) of propane. The carbon nanofibers was synthesized by chemical vapor deposition (CVD), where ammonia and various carbon (CO, C2H6, C2H4) sources was decomposed over on Fe or Ni, supported on expandable graphite. After the synthesis, the nitrogen doped carbon fibers was treated with nitric acid to remove the metal from the growth catalyst, before the sample was annealed. Three iron based samples was compared during this project; the as synthesized CNFs, the CNFs after acid treatment, and the CNFs after annealing. In addition a sample of as synthesized nickel based catalyst was investigated.In addition to the activity testing, BET, XRD, TEM and XPS were carried out on the catalysts, which confirmed that the synthesis of the nitrogen doped carbon nanofibers was successful.The results from the ODH suggests that the nickel based catalyst have better activity than the iron based samples, in addition to producing less CO2. However, the selectivity towards propene was better for the iron based samples. This could be due to the differences in structure for the iron based and the nickel based catalyst, causing a difference in the distribution of nitrogen and oxygen groups on the surface.
机译:催化反应通常在各种负载的金属上进行,这些金属通常是贵金属或金属氧化物。尽管金属基催化剂在当今的工业过程中起着重要作用,但它们仍然具有一些缺点,包括高成本,易发生气体中毒以及对环境的不利影响。近来,某些碳纳米材料已经成为数个研究小组的关注焦点,因为碳除了具有独特的表面特性外,还具有广泛的实用性,环境可接受性,耐腐蚀性等优点。目标是使用碳纳米材料生产更好的催化剂-不使用贵金属。通过将碳纳米纤维和碳纳米管掺入其他元素,可以显着改变其物理和化学性质,从而使其更具反应性。硼,氮和磷是可以用作掺杂剂的一些化学元素。在本研究中,研究了氮掺杂的碳纳米纤维在丙烷的氧化脱氢(ODH)中的应用。碳纳米纤维是通过化学气相沉积(CVD)合成的,其中氨和各种碳(CO,C2H6,C2H4)源在负载在可膨胀石墨上的Fe或Ni上分解。合成后,在样品退火之前,用硝酸处理掺氮碳纤维,以从生长催化剂中去除金属。在此项目中,对三个铁基样品进行了比较;作为合成的CNF,酸处理后的CNF和退火后的CNF。此外,还对作为合成镍基催化剂的样品进行了研究,并进行了活性,BET,XRD,TEM和XPS的测试,证实了氮掺杂碳纳米纤维的合成是成功的。 ODH的数据表明,镍基催化剂除了产生较少的CO2外,其活性还比铁基样品好。但是,对于铁基样品,对丙烯的选择性更好。这可能是由于铁基和镍基催化剂的结构不同,从而导致了表面上氮和氧基团的分布不同。

著录项

  • 作者

    Jenssen Kaia Andersson;

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  • 年度 2014
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  • 原文格式 PDF
  • 正文语种 eng
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