Pilot plant for chemical looping hydrogen generation using single-column packed bed and hydrogen generation method

Patent metadata

Field	Value
Publication number	US-10988378-B2
Application number	US-201715625738-A
Country	US
Kind code	B2
Filing date	Jun 16, 2017
Priority date	Jun 29, 2016
Publication date	Apr 27, 2021
Grant date	Apr 27, 2021

Abstract

A pilot plant for chemical looping hydrogen generation using a single-column packed bed and hydrogen generation method. The plant has a feeding system, reaction system, tail gas treatment and analysis system, and auxiliary system. The reaction system has a packed bed reactor, inside which a thermal storage layer, oxygen carrier layer and supporting layer are arranged successively from top to bottom. The feeding system has a delivery pipe, metering pump, mass flow controller and fuel mixer. The tail gas treatment and analysis system has a cooler, gas-liquid separator, mass flow meter, gas analyzer and tail gas pipe. The packed bed reactor is subjected to fuel reduction, purge, steam oxidation, purge, air combustion and purge stages successively under control of the feeding system. The pilot plant enables evaluation for oxygen carriers and identification for technological difficulties and can generate high-purity hydrogen without using complex gas purification devices.

First claim

The invention claimed is:

1. A method for chemical looping hydrogen generation using a pilot plant, wherein the method comprises following steps:
A. feeding stage: a feeding system mixes a fuel I with a fuel II via a fuel mixer and then delivers the mixture into a packed bed reactor of a reaction system, and other raw materials are delivered into the packed bed reactor of the reaction system after passing through corresponding raw material mass flow controllers;
B. reaction stage: mixed fuels I and II react with an oxygen carrier in the packed bed reactor and other raw materials enter the packed bed reactor successively under a control of the feeding system, so that the packed bed reactor is subjected to a fuel reduction stage, a first purge stage, a steam oxidation stage, a second purge stage, an air combustion stage and a third purge stage successively, wherein liquid water enters the packed bed reactor after the first purge stage; and
C. tail gas treatment stage: gases generated during the fuel reduction stage, the steam oxidation stage and the air combustion stage are cooled, separated, metered and analyzed by a tail gas treatment and analysis system before being discharged.

2. The method according to claim 1 , wherein gas generated during the steam oxidation stage is cooled and separated by a tail gas treatment and analysis system to obtain high-purity hydrogen, which is metered and analyzed before being discharged, wherein the high-purity hydrogen comprises at least 98.3% of hydrogen.

3. The method according to claim 2 , wherein reaction temperatures of the fuel reduction stage, the steam oxidation stage and the air combustion stage are 800° C.; and gases of the first purge stage, the second purge stage and the third purge stage are nitrogen.

4. The method according to claim 1 , wherein the pilot plant comprises a raw material mass flow controller comprising a metering pump, a fuel I mass flow controller and a fuel II mass flow controller, an air mass flow controller and a nitrogen mass flow controller, wherein the metering pump, the air mass flow controller and the nitrogen mass flow controller are each connected to the inlet of the reaction system, and an outlet of the fuel I mass flow controller and an outlet of the fuel II mass flow controller are connected to an inlet of the fuel mixer.

5. The method according to claim 1 , wherein a thermal storage layer, an oxygen carrier layer and a supporting layer are arranged successively from top to bottom inside the packed bed reactor, and wherein said liquid water entering the packed bed reactor is then vaporized on the thermal storage layer.

6. The method according to claim 5 , wherein the oxygen carrier layer of the packed bed reactor has a length-to-diameter ratio of 4:1 to 12:1.

7. The method according to claim 1 , wherein the tail gas treatment and analysis system comprises a cooler, a gas-liquid separator, a mass flow meter, a gas analyzer and a tail gas pipe in successively connection.

8. The method according to claim 7 , wherein a packed bed reactor inlet safety valve and a packed bed reactor outlet safety valve are connected with the tail gas pipe, and a packed bed reactor blowdown pipe is provided at a bottom of the packed bed reactor.

9. The method according to claim 1 , wherein an internal temperature of the packed bed reactor is measured by a packed bed reactor axial temperature measurement device, and a pressure drop of the packed bed reactor is measured by a packed bed reactor inlet pressure sensor and a packed bed reactor outlet pressure sensor.

10. The method according to claim 1 , wherein the feeding system comprises at least one raw material delivery pipe, at least one raw material mass flow controller and the fuel mixer, and wherein at least one outlet of the raw material mass flow controller is connected with an inlet of the fuel mixer, and other remaining outlets of the raw material mass flow controller are connected with an inlet of the reaction system.

11. The method according to claim 10 , wherein the tail gas treatment and analysis system comprises a cooler, a gas-liquid separator, a mass flow meter, a gas analyzer and a tail gas pipe in successively connection, and
wherein the pilot plant further comprises an auxiliary system that is connected with the feeding system, the reaction system and the tail gas treatment and analysis system, respectively, wherein the auxiliary system comprises a quartz heating furnace, a pilot plant control apparatus and an electrical apparatus.

12. The method according to claim 1 , wherein the packed bed reactor has a reaction temperature of 700° C. to 1100° C. at the fuel reduction stage, a reaction temperature of 700° C. to 1100° C. at the steam oxidation stage, and a reaction temperature of 700° C. to 1100° C. at the air combustion stage.

Assignees

• Univ Tsinghua

Inventors

• Wang Wei
• Hua Xiuning
• Xia Zhou

Classifications

• C01B3/10 Primary

  by reaction of water vapour with metals · CPC title

• C01B3/32 Primary

  by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air · CPC title

• B01J8/0453

  the beds being superimposed one above the other · CPC title

• B01J8/0496

  Heating or cooling the reactor · CPC title

• B01J2208/00088

  Flow rate measurement · CPC title