Continuous reaction device for synthesizing polyoxymethylene dimethyl ethers

Patent metadata

Field	Value
Publication number	US-2016185902-A1
Application number	US-201514980598-A
Country	US
Kind code	A1
Filing date	Dec 28, 2015
Priority date	Dec 26, 2014
Publication date	Jun 30, 2016
Grant date	—

Abstract

The present invention pertains to the technical field of energy resource chemical industry, and in particular relates to a continuous reaction device and process for synthesizing polyoxymethylene dimethyl ethers by using paraformaldehyde and methylal as feedstock or using trioxane and methylal as feedstock in the presence of an acidic catalyst. The continuous reaction device comprises multiple slurry bed stirred tank reactors connected in series or in combination of series connection and parallel connection, and also comprises an on-line solid-liquid separation device to perform separation of the reaction mixture from the catalyst. Each of the tank reactors is provided with an axial-flow stirring paddle having 2-6 blades per layer, to ensure sufficient mixing of the reactants with the catalyst. By using a distributed control pattern of reaction temperature and feedstock supplying to enhance the process and to optimize the operation, the reaction device of the present invention can effectively achieve large-scale continuous production of polyoxymethylene dimethyl ethers, and both the yield rates and the distribution of the reaction product are better than those of prior art.

First claim

1 . A continuous reaction device for synthesizing polyoxymethylene dimethyl ethers, the reaction using paraformaldehyde and methylal as feedstock or using trioxane and methylal as feedstock and being carried out in the presence of an acidic catalyst, wherein,
the continuous reaction device comprises multiple reactors connected in series or in combination of series connection and parallel connection, and also comprises an on-line solid-liquid separation device to perform solid-liquid separation of the reaction mixture from the catalyst; each of the tank reactors is independently controlled at a pressure of 1.0-4.0 MPa and a temperature of 50-120° C.; a molar ratio of paraformaldehyde or trioxane, metered in mole number of formaldehyde contained therein, to methylal in the feedstock is 0.5-5.0; and the amount of the catalyst is equal to 1.0-4.0 wt % of the total amount of the feedstock; each of the tank reactors is provided with an axial-flow stirring paddle having 2-6 blades per layer, to ensure sufficient mixing of the reactants and catalyst.

2 . The continuous reaction device in accordance with claim 1 , wherein, when paraformaldehyde powder and methylal are used as feedstock, the on-line solid-liquid separation device is arranged after the last one of the tank reactors, to perform the separation of the reaction mixture from the catalyst slurry; and a recycling pipeline is provided to recycle the catalyst, obtained after sufficient solid-liquid separation and blended with a part of the methylal, into the first one of the tank reactors, so that continuous and steady operation of the reaction device is achieved.

3 . The continuous reaction device in accordance with claim 1 , wherein, when sufficiently pre-depolymerized paraformaldehyde and methylal are used as feedstock or trioxane and methylal are used as feedstock, each of the tank reactors is provided with an on-line solid-liquid separation device arranged at the inside or outside thereof, to perform the separation of the reaction mixture from the catalyst.

4 . The continuous reaction device in accordance with claim 3 , wherein, the on-line solid-liquid separation device arranged at the inside of each of the tank reactors is composed of powder metallurgy filtering elements which is divided into two groups, with one group for filtering and the other group for purging, and with alternation switching performed automatically, so that the catalyst is retained within the tank reactor.

5 . The continuous reaction device in accordance with claim 3 , wherein, the on-line solid-liquid separation device arranged at the outside of each of the tank reactors is a multitubular filter performing on-line cross-flow filtering, so that the catalyst thick slurry is recycled back into the same one of the tank reactors for continuous use.

6 . The continuous reaction device in accordance with claim 1 , wherein, a difference in operation pressure between two adjacent ones of the tank reactors is utilized as a driving force of filtering, to achieve solid-liquid filtering separation as well as transport of the reaction mixture from one reactor to the next.

7 . The continuous reaction device in accordance with claim 1 , wherein, each of the tank reactors is provided with a jacket or coiled half-pipe arranged outside a barrel of the reactor for serving as a heater when starting operation, and each of the reactors is provided with an internal heat exchanger arranged at the inside thereof for serving as a cooler during normal operation.

8 . The continuous reaction device in accordance with claim 1 , wherein, an interlock control system is provided at the bottom of each of the tank reactors for controlling the initial fluidization of the catalyst and the starting of the stirring paddle, to ensure operation safety when the added amount of the catalyst is relatively large.

9 . The continuous reaction device in accordance with claim 1 , wherein, the tank reactors are slurry bed stirred tank reactors, and the reaction device includes 2-8 reactors.

10 . The continuous reaction device in accordance with claim 9 , wherein, the operation temperature of the tank reactors decreases successively by 5-20° C. per reactor; or the entire reaction is controlled by feeding all the feedstock at the first one of the reactors or by distributed feedstock feeding.

11 . The continuous reaction device in accordance with claim 2 , wherein, a difference in operation pressure between two adjacent ones of the tank reactors is utilized as a driving force of filtering, to achieve solid-liquid filtering separation as well as transport of the reaction mixture from one reactor to the next.

12 . The continuous reaction device in accordance with claim 3 , wherein, a difference in operation pressure between two adjacent ones of the tank reactors is utilized as a driving force of filtering, to achieve solid-liquid filtering separation as well as transport of the reaction mixture from one reactor to the next.

13 . The continuous reaction device in accordance with claim 2 , wherein, each of the tank reactors is provided with a jacket or coiled half-pipe arranged outside a barrel of the reactor for serving as a heater when starting operation, and each of the reactors is provided with an internal heat exchanger arranged at the inside thereof for serving as a cooler during normal operation.

14 . The continuous reaction device in accordance with claim 3 , wherein, each of the tank reactors is provided with a jacket or coiled half-pipe arranged outside a barrel of the reactor for serving as a heater when starting operation, and each of the reactors is provided with an internal heat exchanger arranged at the inside thereof for serving as a cooler during normal operation.

15 . The continuous reaction device in accordance with claim 2 , wherein, an interlock control system is provided at the bottom of each of the tank reactors for controlling the initial fluidization of the catalyst and the starting of the stirring paddle, to ensure operation safety when the added amount of the catalyst is relatively large.

16 . The continuous reaction device in accordance with claim 3 , wherein, an interlock control system is provided at the bottom of each of the tank reactors for controlling the initial fluidization of the catalyst and the starting of the stirring paddle, to ensure operation safety when the added amount of the catalyst is relatively large.

17 . The continuous reaction device in accordance with claim 2 , wherein, the tank reactors are slurry bed stirred tank reactors, and the reaction device includes 2-8 reactors.

18 . The continuous reaction device in accordance with claim 17 , wherein, the operation temperature of the tank reactors decreases successively by 5-20° C. per reactor; or the entire reaction is controlled by feeding all the feedstock at the first one of the reactors or by distributed feedstock feeding.

19 . The continuous reaction device in accordance with claim 3 , wherein, the tank reactors are slurry bed stirred tank reactors, and the reaction device includes 2-8 reactors.

20 . The continuous reaction device in accordance with claim 19 , wherein, the operation temperature of the tank reactors decreases successively by 5-20° C. per reactor; or the entire reaction is controlled by feeding all the feedstock at the first one of the reactors or by distributed feedstock feeding.

Assignees

• Dongfang Hongsheng New Energy Applic Technology Res Inst Co Ltd
• Univ China Petroleum

Inventors

• Shang Hongyan
• Hong Zhengpeng
• Li Chengyue
• Feng Xiaoting
• Han Yu
• Xue Zhenzhen

Classifications

• B01J2208/00557

  controlling the residence time inside the reactor vessel · CPC title

• B01J2208/00867

  inside the bed, e.g. rotary mixer · CPC title

• B01J19/1862

  placed in series · CPC title

• B01J2208/00628

  Controlling the composition of the reactive mixture · CPC title

• C07C41/56 Primary

  by condensation of aldehydes, paraformaldehyde, or ketones · CPC title