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Method for producing phenol by oxidizing benzene through nitrous oxide

A technology for nitrous oxide and benzene oxidation, which is applied in the production of bulk chemicals, chemical instruments and methods, and the preparation of organic compounds. It can solve problems such as difficult desorption, carbon deposition on catalysts, and deactivation, so as to avoid overheating The effect of sintering, slowing down the deactivation of carbon deposition and improving stability

Inactive Publication Date: 2011-04-20
BEIJING UNIV OF CHEM TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the disadvantage of this process is that the catalyst activity and stability are relatively poor.
Due to the strong adsorption of the product phenol on the surface of the catalyst, it is not easy to desorb from the active sites on the surface of the catalyst, further deep oxidation reaction occurs to form carbon deposits, and the catalyst is rapidly deactivated, which restricts the industrial application of this process technology
[0004] The common problem in the nitrous oxide one-step oxidation of benzene to produce phenol reported in the above literature is that all catalysts used are facing the problem of rapid deactivation, mainly due to the strong adsorption of active sites or acidic sites on the surface of the catalyst to the product phenol, etc., resulting in phenol deactivation. Further deep oxidation forms carbon deposits on the surface of the catalyst and causes catalyst deactivation. In this field, current research generally starts with catalyst preparation and modification to solve this problem, but there is no significant effect

Method used

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  • Method for producing phenol by oxidizing benzene through nitrous oxide

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Effect test

Embodiment 1

[0021] Example 1: Select 20 grams of H-ZSM-5 molecular sieve with a Si / Al ratio of 25, and put it into a three-necked flask as a carrier. Weigh 1.448 grams of Fe (NO 3 ) 3 9H 2 O, add 300 milliliters of distilled water to prepare a solution, pour this solution into a three-necked flask equipped with 20 grams of H-ZSM-5, reflux and stir at 100°C for 3 hours, then wash with deionized water and filter for 3 times, and then Dry at 110° C. for 12 hours, bake at 540° C. for 4 hours, and after cooling, grind the catalyst tablet into 180-300 μm particles. Then, steam is introduced into the fixed-bed reactor to carry out hydrothermal treatment on the catalyst at 650° C., and the Fe-ZSM-5 molecular sieve catalyst is obtained after cooling.

[0022] Load the prepared catalyst into the gas distribution plate in the fixed fluidized bed reactor of the present invention, activate it with helium at 500°C for 5 hours, and then feed nitrous oxide, benzene and diluent gas under normal pressur...

Embodiment 2

[0023] Embodiment 2: Catalyst preparation process is the same as embodiment 1. The reaction temperature is 500° C., and other reaction conditions remain unchanged. The highest yield of phenol can reach 68.51%, and the yield is still maintained above 61% after continuous reaction for 155 minutes.

Embodiment 3

[0024] Embodiment 3: The catalyst preparation process is the same as in Embodiment 1. Raw material benzene / N 2 O molar ratio is 13, and other reaction conditions are unchanged. The highest yield of phenol can reach 83.18%, and the yield is still maintained above 74% after continuous reaction for 155 minutes.

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Abstract

The invention relates to a process method for producing phenol by selectively oxidizing benzene through nitrous oxide, comprising the following steps of: placing a Fe-ZSM-5 molecular sieve catalyst on a distribution plate inside a fixed fluidized bed reactor; firstly activating the Fe-ZSM-5 molecular sieve catalyst by using helium at 400-600 DEG C; then introducing a gas containing the nitrous oxide and the benzene from the lower end inside the fixed fluidized bed reactor at normal pressure; controlling the reaction gas velocity of the gas between 0.040m / s and 0.072m / s through the gas distribution plate so that catalyst granules contact with the gas in a suspended state in the fixed fluidized bed reactor to carry out continuous reaction at the temperature between 300 DEG C and 500 DEG C and the normal pressure, wherein the mol ratio of the raw material benzene / N2O is between 4 and 16; and condensing and separating reaction products to obtain the phenol. The invention enables the Fe-ZSM-5 molecular sieve catalyst to contact with reaction fluids in the suspended state by utilizing the fixed fluidized bed reactor, therefore sliding velocity higher than terminal granule velocity exists between the gas and a solid; and in addition, the invention not only has very high contact efficiency, but also is beneficial to carrying out mass transfer between the gas and the solid and desorbing a product, i.e. the phenol, thereby alleviating the coking deactivation of the Fe-ZSM-5 molecular sieve catalyst.

Description

technical field [0001] The present invention relates to a method for effectively utilizing nitrous oxide as an oxidizing agent. In particular, it relates to a method for selectively oxidizing benzene with nitrous oxide to produce phenol. Background technique [0002] Nitrous oxide, chemical formula N 2 O, commonly known as laughing gas, not only can seriously destroy the ozone layer, but also has a strong greenhouse effect, and the elimination of nitrous oxide is of great significance to environmental protection. The current methods of eliminating nitrous oxide can be divided into pyrolysis, catalytic decomposition and recycling. If the method of simple decomposition is used to process nitrous oxide, it will not only cost a lot of money and energy, but also waste nitrous oxide resources. Therefore, in recent years, a lot of research has been carried out around the recovery and utilization of nitrous oxide at home and abroad. It is of great significance to use nitrous oxid...

Claims

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Application Information

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IPC IPC(8): C07C39/04C07C37/60B01J29/46
CPCY02P20/52
Inventor 李建伟米冠杰陈标华李英霞邱东
Owner BEIJING UNIV OF CHEM TECH
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