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Heteroatom-containing carbon nanomaterial, preparation method and application of heteroatom-containing carbon nanomaterial and hydrocarbon oxidative dehydrogenation reaction method

A nano-carbon material and heteroatom technology, which is applied in the field of hydrocarbon oxidative dehydrogenation reaction, can solve the problems of catalyst poisoning and deactivation, carbon deposition, etc., and achieve the effects of good stability, small structural influence and good catalytic activity.

Active Publication Date: 2019-02-05
CHINA PETROLEUM & CHEM CORP +1
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Traditional metal catalysts are prone to carbon deposition during the reaction process, resulting in catalyst poisoning and deactivation
Although the emerging nano-carbon materials show good catalytic performance and stability, the performance of the catalyst needs to be further improved

Method used

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  • Heteroatom-containing carbon nanomaterial, preparation method and application of heteroatom-containing carbon nanomaterial and hydrocarbon oxidative dehydrogenation reaction method
  • Heteroatom-containing carbon nanomaterial, preparation method and application of heteroatom-containing carbon nanomaterial and hydrocarbon oxidative dehydrogenation reaction method
  • Heteroatom-containing carbon nanomaterial, preparation method and application of heteroatom-containing carbon nanomaterial and hydrocarbon oxidative dehydrogenation reaction method

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preparation example Construction

[0044] According to a second aspect of the present invention, the present invention provides a method for preparing a heteroatom-containing nano-carbon material, the method comprising:

[0045] Step A1, contacting the raw material nano-carbon material with at least one oxidizing agent to obtain an oxidized nano-carbon material,

[0046] Step B1, calcining the oxidized carbon nanomaterial at a temperature of 550-1200°C in an inert atmosphere to obtain the calcined carbon nanomaterial,

[0047] Step C1, contacting the calcined carbon nanomaterial with at least one phosphorus source.

[0048] According to the method of the present invention, the raw material nano carbon material contains oxygen element, hydrogen element and carbon element, based on the total amount of the raw material nano carbon material, in terms of elements, the content of the oxygen element is 0.1-1 weight %, preferably 0.15-0.9% by weight, more preferably 0.2-0.8% by weight; the content of the hydrogen elem...

Embodiment 1

[0105] (1) 10 g of multi-walled carbon nanotubes (purchased from Chengdu Organic Chemistry Co., Ltd., Chinese Academy of Sciences, whose property parameters are listed in Table 1) and 500 mL of acid solution (H 2 SO 4 The concentration is 1380g / L, HNO 3 The concentration of the acid solution is 227.5g / L, the solvent of the acid solution is water), and the obtained dispersion is placed in an ultrasonic cleaner for ultrasonic treatment, wherein the temperature of the dispersion in the ultrasonic cleaner is controlled to be 50°C, and the ultrasonic treatment The duration is 6 hours and the frequency of ultrasound is 45kHz. After the ultrasonic treatment is completed, the dispersion liquid is filtered, and the collected solid matter is washed with deionized water until the pH of the washing liquid is in the range of 6-7, and the washed solid matter is heated in an air atmosphere at 120°C Drying at a certain temperature for 12 hours to obtain an oxidized carbon nanomaterial.

[...

Embodiment 2

[0109] The same method as in Example 1 was used to prepare heteroatom-containing carbon nanomaterials, except that in step (2), the oxidized carbon nanomaterials were calcined in a nitrogen atmosphere at a temperature of 550° C. for 5 hours. The composition and property parameters of the prepared heteroatom-containing carbon nanomaterials are listed in Table 1.

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Abstract

The invention discloses a heteroatom-containing carbon nanomaterial, a preparation method and application of the heteroatom-containing carbon nanomaterial and a hydrocarbon oxidative dehydrogenation reaction method. The heteroatom-containing carbon nanomaterial contains oxygen, phosphorus, hydrogen and carbon, in the XPS spectrum, the molar ratio of the content of the oxygen element determined bythe spectral peak corresponding to a C-O group to the content of the oxygen element determined by the spectral peak corresponding to a group as shown in the specification is greater than 1. The heteroatom-containing carbon nanomaterial shows good catalytic activity in the oxidative dehydrogenation reaction of hydrocarbon, still keeps the good characteristics of a carbon nanomaterial and has relatively good stability. According to the preparation method for the heteroatom-containing nanomaterial, the content and the existence form of heteroatoms in the carbon nanomaterial can be stably adjustedand controlled, and meanwhile, the influence on the structure of the carbon nanomaterial is small.

Description

technical field [0001] The invention relates to a heteroatom-containing nano-carbon material and its preparation method and application, and also relates to a hydrocarbon oxidation dehydrogenation reaction method. Background technique [0002] Carbon materials exist in various morphological structures, including carbon nanotubes, graphite, graphene, nanodiamonds, activated carbon, onion carbon, etc. Compared with traditional metal oxide catalysts, carbon materials have the advantages of being environmentally friendly, renewable, and low energy consumption. Carbon materials also have good thermal conductivity, so the energy utilization rate is high, which is conducive to reducing the reaction temperature and improving product selectivity. At present, various types of carbon materials have been reported to be used in catalytic reactions such as alkane activation and oxidative dehydrogenation. For example, in the 1960s and 1970s, researchers discovered that coke can catalyze th...

Claims

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Application Information

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IPC IPC(8): B01J27/16C07C5/48C07C11/167
CPCC07C5/48C07C2527/167B01J35/613B01J35/615C07C11/167
Inventor 谢婧新荣峻峰李嘉权于鹏史春风林伟国宗明生
Owner CHINA PETROLEUM & CHEM CORP
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