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A heteroatom-containing nano-carbon material, its preparation method and application, and a hydrocarbon oxidative dehydrogenation reaction method

A nano-carbon material and heteroatom technology, applied in the field of hydrocarbon oxidative dehydrogenation reaction, can solve the problem of insufficient catalytic activity, and achieve the effects of improving the utilization rate of raw materials and product yield, good stability and good catalytic activity

Active Publication Date: 2020-08-18
CHINA PETROLEUM & CHEM CORP +1
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] The purpose of the present invention is to overcome the technical problem that the catalytic activity of existing nano-carbon materials is still not high enough when they are used as catalysts for the oxidative dehydrogenation of hydrocarbons, and to provide a heteroatom-containing nano-carbon material, which contains heteroatom-containing nano-carbon materials When used as a catalyst for the oxidative dehydrogenation of hydrocarbons, it can not only obtain high catalytic stability, but also significantly improve the catalytic activity

Method used

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  • A heteroatom-containing nano-carbon material, its preparation method and application, and a hydrocarbon oxidative dehydrogenation reaction method
  • A heteroatom-containing nano-carbon material, its preparation method and application, and a hydrocarbon oxidative dehydrogenation reaction method
  • A heteroatom-containing nano-carbon material, its preparation method and application, and a hydrocarbon oxidative dehydrogenation reaction method

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preparation example Construction

[0052] 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:

[0053] Step A1, contacting the raw carbon nanomaterial with at least one oxidizing agent to obtain an oxidized carbon nanomaterial;

[0054] Step B1, contacting the oxidized carbon nanomaterial with at least one reducing agent under reduction reaction conditions to obtain the reduced carbon nanomaterial;

[0055] Step C1, contacting the reduced carbon nanomaterial with at least one phosphorus source.

[0056] 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 0.5-0.9% by weight; the content of the hydrogen element is 0.1-1% by weight, preferabl...

Embodiment 1

[0128] (1) 5g of multi-walled carbon nanotubes (diameter range of 1-8nm, specific surface area of ​​273m2) as raw material nano-carbon material 2 / g, the weight loss rate w in the temperature range of 400-800°C 800 , the weight loss rate w in the temperature range of 400-500°C 500 ,w 500 / w 800 0.13, the peroxy group content is 0mol / g, purchased from Chengdu Organic Chemistry Co., Ltd., Chinese Academy of Sciences) and 250mL 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 resulting 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 the ultrasound is 45kHz. After the ultrasonic treatment is completed, the dispersion liquid is filtered, and the collected solid matter is was...

Embodiment 2

[0132] Adopt the same method as Example 1 to prepare heteroatom-containing nano-carbon materials, the difference is that in step (2), 2g of oxidized nano-carbon materials are dissolved in 40mL tetrahydrofuran solution of lithium aluminum hydride (lithium aluminum hydride) The concentration is 0.05 mol / L, and the molar ratio of lithium tetrahydrogen to the content of oxygen in the oxidized nano-carbon material is 0.1:1), and reflux at a temperature of 70° C. for 12 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 nanocarbon material, its preparation method and application, and a hydrocarbon oxidative dehydrogenation reaction method. The heteroatom-containing nanocarbon material contains oxygen, hydrogen, phosphorus and carbon. The heteroatom-containing nanocarbon The concentration of peroxy groups in the material is 0.1×10 ‑6 mol / g to 3×10 ‑6 mol / g. The heteroatom-containing nanocarbon material of the present invention shows good catalytic activity in the oxidative dehydrogenation reaction of hydrocarbon substances, can achieve a good balance between raw material conversion rate and product selectivity, and effectively improves raw material utilization rate and product yield. . The heteroatom-containing nanocarbon material of the present invention still maintains the good characteristics of the nanocarbon material itself and has good stability. The preparation method of heteroatom-containing nanomaterials of the present invention can stably regulate the heteroatom content and existence form in the nanocarbon material, while having little impact on the structure of the nanocarbon material itself.

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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Patent Type & Authority Patents(China)
IPC IPC(8): C01B32/15C01B32/168C01B32/194C01B32/21C01B32/28C01B32/156B01J27/22B01J35/10B01J37/12B01J37/18B01J37/02C07C11/08C07C11/16C07C5/333
CPCC07C5/333B01J27/22B01J37/0201B01J37/12B01J37/18C01B2202/36C01B2202/32C01B2202/06C07C2527/22B01J35/23B01J35/615C07C11/08C07C11/16
Inventor 谢婧新荣峻峰李嘉权于鹏林伟国史春风宗明生
Owner CHINA PETROLEUM & CHEM CORP