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Title: A NOVEL MEMBRANE REACTOR FOR DIRECT HYDROGEN PRODUCTION FROM COAL

Abstract

Gas Technology Institute is developing a novel concept of membrane gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying the potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate the candidate membrane performance under the gasification conditions, a high temperature/high pressure hydrogen permeation unit will be constructed in this project. During this reporting period, the design of this unit was completed. The unit will be capable of operating at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed ionic conducting membrane. The membranes to be tested will be in disc form with a diameter of about 3 cm. By operating at higher temperatures and higher hydrogen partial pressures, we expect to demonstrate commercially relevant hydrogen flux, 10 {approx} 50 cc/min/cm{sup 2}, from the membranesmore » made of the perovskite type of ceramic material. The construction of the unit is planned to be completed by the end of the next reporting period.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Gas Technology Institute (US)
Sponsoring Org.:
(US)
OSTI Identifier:
829544
DOE Contract Number:
FC26-03NT41851
Resource Type:
Technical Report
Resource Relation:
Other Information: PBD: 22 Jan 2004
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 01 COAL, LIGNITE, AND PEAT; CERAMICS; COAL; COAL GASIFICATION; ECONOMICS; EFFICIENCY; GASES; GASIFICATION; HYDROGEN; HYDROGEN PRODUCTION; MEMBRANES; PARTIAL PRESSURE; PEROVSKITE; SYNTHESIS; TESTING

Citation Formats

Shain Doong, Estela Ong, Mike Atroshenko, Francis Lau, and Mike Roberts. A NOVEL MEMBRANE REACTOR FOR DIRECT HYDROGEN PRODUCTION FROM COAL. United States: N. p., 2004. Web. doi:10.2172/829544.
Shain Doong, Estela Ong, Mike Atroshenko, Francis Lau, & Mike Roberts. A NOVEL MEMBRANE REACTOR FOR DIRECT HYDROGEN PRODUCTION FROM COAL. United States. doi:10.2172/829544.
Shain Doong, Estela Ong, Mike Atroshenko, Francis Lau, and Mike Roberts. 2004. "A NOVEL MEMBRANE REACTOR FOR DIRECT HYDROGEN PRODUCTION FROM COAL". United States. doi:10.2172/829544. https://www.osti.gov/servlets/purl/829544.
@article{osti_829544,
title = {A NOVEL MEMBRANE REACTOR FOR DIRECT HYDROGEN PRODUCTION FROM COAL},
author = {Shain Doong and Estela Ong and Mike Atroshenko and Francis Lau and Mike Roberts},
abstractNote = {Gas Technology Institute is developing a novel concept of membrane gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying the potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate the candidate membrane performance under the gasification conditions, a high temperature/high pressure hydrogen permeation unit will be constructed in this project. During this reporting period, the design of this unit was completed. The unit will be capable of operating at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed ionic conducting membrane. The membranes to be tested will be in disc form with a diameter of about 3 cm. By operating at higher temperatures and higher hydrogen partial pressures, we expect to demonstrate commercially relevant hydrogen flux, 10 {approx} 50 cc/min/cm{sup 2}, from the membranes made of the perovskite type of ceramic material. The construction of the unit is planned to be completed by the end of the next reporting period.},
doi = {10.2172/829544},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2004,
month = 1
}

Technical Report:

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  • Gas Technology Institute is developing a novel concept of membrane gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate the performances of the candidatemore » membranes under the gasification conditions, a high temperature/high pressure hydrogen permeation unit will be constructed in this project. During this reporting period, the mechanical construction of the permeation unit was completed. Commissioning and shake down tests are being conducted. The unit is capable of operation at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed ionic conducting membrane. The membranes to be tested will be in disc form with a diameter of about 3 cm. Operation at these high temperatures and high hydrogen partial pressures will demonstrate commercially relevant hydrogen flux, 10{approx}50 cc/min/cm{sup 2}, from the membranes made of the perovskite type of ceramic material. Preliminary modeling was also performed for a tubular membrane reactor within a gasifier to estimate the required membrane area for a given gasification condition. The modeling results will be used to support the conceptual design of the membrane reactor.« less
  • Gas Technology Institute is developing a novel concept of membrane gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal-derived synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate the performances of the candidatemore » membranes under the gasification conditions, a high temperature/high pressure hydrogen permeation unit has been constructed in this project. During this reporting period, the unit has been fully commissioned and is operational. The unit is capable of operating at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed ionic conducting membrane. A double-seal technique has been developed and tested successfully to achieve leak-tight seal for the membranes. Initial data for a commercial Palladium-Gold membrane were obtained at temperatures to 450 C and pressures to 13 atm. Tests for the perovskite membranes are being performed and the results will be reported in the next quarter. A membrane gasification reactor model was developed to consider the H{sub 2} permeability of the membrane, the kinetics and the equilibriums of the gas phase reactions in the gasifier, the operating conditions and the configurations of the membrane reactor. The results show that the hydrogen production efficiency using the novel membrane gasification reactor concept can be increased by about 50% versus the conventional gasification process. This confirms the previous evaluation results from the thermodynamic equilibrium calculation. A rigorous model for hydrogen permeation through mixed proton-electron conducting ceramic membranes was also developed based on non-equilibrium thermodynamics. The results from the simulation work confirm that the hydrogen flux increases with increasing partial pressure of hydrogen. The presence of steam in the permeate side can have a small negative effect on the hydrogen flux, in the order of 10%. When the steam partial pressure is greater than 1 atm, the hydrogen flux becomes independent of the steam pressure.« less
  • Gas Technology Institute is developing a novel concept of membrane gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal-derived synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate the performances of the candidatemore » membranes under the gasification conditions, a high temperature/high pressure hydrogen permeation unit has been constructed in this project. The unit is designed to operate at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed ionic conducting membrane. The unit was fully commissioned and is operational. Several perovskite membranes based on the formulations of BCN (BaCe{sub 0.8}Nd{sub 0.2}O{sub 3-x}) and BCY (BaCe{sub 0.8}Y{sub 0.2}O{sub 3-x}) were prepared by GTI and tested in the new permeation unit. These membranes were fabricated by either uniaxial pressing or tape casting technique with thickness ranging from 0.2 mm to 0.7 mm. Hydrogen permeation data for the BCN perovskite membrane have been successfully obtained for temperatures between 800 and 950 C and pressures from 1 to 12 bar. The highest hydrogen flux was measured at 1.6 STPcc/min/cm{sup 2} at a hydrogen feed pressure of 12 bar and 950 C with a membrane thickness of 0.22 mm. A membrane gasification reactor model was developed to consider the H{sub 2} permeability of the membrane, the kinetics and the equilibriums of the gas phase reactions in the gasifier, the operating conditions and the configurations of the membrane reactor. The results show that the hydrogen production efficiency using the novel membrane gasification reactor concept can be increased by about 50% versus the conventional gasification process. This confirms the previous evaluation results from the thermodynamic equilibrium calculation. A rigorous model for hydrogen permeation through mixed proton-electron conducting ceramic membranes was also developed based on non-equilibrium thermodynamics. The hydrogen flux predicted from the modeling results are in line with the data from the experimental measurement. The simulation also shows that the presence of steam in the permeate side or the feed side of the membrane can have a small negative effect on the hydrogen flux, in the order of 10%.« less
  • Gas Technology Institute is developing a novel concept of membrane reactor coupled with a gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal-derived synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. To evaluate themore » performances of the candidate membranes under the gasification conditions, a high temperature/high pressure hydrogen permeation unit has been constructed in this project. The unit is designed to operate at temperatures up to 1100 C and pressures to 60 atm for evaluation of ceramic membranes such as mixed protonic-electronic conducting membrane. Several perovskite membranes based on the formulations of BCN (BaCe{sub 0.8}Nd{sub 0.2}O{sub 3-x}), BCY (BaCe{sub 0.8}Y{sub 0.2}O{sub 3-x}), Eu-doped SrCeO{sub 3} (SCE) and SrCe{sub 0.95}Tm{sub 0.05}O{sub 3} (SCTm) were successfully tested in the new permeation unit. During this reporting period, a thin BCN membrane supported on a porous BCN layer was fabricated. The objective was to increase the hydrogen flux with a further reduction of the thickness of the active membrane layer. The thinnest dense layer that could be achieved in our laboratory currently was about 0.2 mm. Nevertheless, the membrane was tested in the permeation unit and showed reasonable flux compared to the previous BCN samples of the same thickness. A long term durability test was conducted for a SCTm membrane with pure hydrogen in the feed side and nitrogen in the sweep side. The pressure was 1 bar and the temperature was around 1010 C. No decline of hydrogen flux was observed after continuous running of over 250 hours. This long term test indicates that the perovskite membrane has good thermal stability under the reducing conditions of the hydrogen atmosphere. A conceptual design of the membrane reactor configuration for a 1000 tons-per-day (TPD) coal gasifier was completed. The design considered a tubular membrane module located within the freeboard area of a fluidized bed gasifier. The membrane ambipolar conductivity was based on the value calculated from the measured permeation data. A membrane thickness of 25 micron was assumed in the calculation. The GTI's gasification model combined with a membrane reactor model were used to determine the dimensions of the membrane module. It appears that a membrane module can be configured within a fluidized bed gasifier without substantial increase of the gasifier dimensions.« less
  • Gas Technology Institute is developing a novel concept of membrane reactor coupled with a gasifier for high efficiency, clean and low cost production of hydrogen from coal. The concept incorporates a hydrogen-selective membrane within a gasification reactor for direct extraction of hydrogen from coal-derived synthesis gases. The objective of this project is to determine the technical and economic feasibility of this concept by screening, testing and identifying potential candidate membranes under high temperature, high pressure, and harsh environments of the coal gasification conditions. The best performing membranes will be selected for preliminary reactor design and cost estimates. Hydrogen permeation datamore » for several perovskite membranes BCN (BaCe{sub 0.9}Nd{sub 0.1}O{sub 3-x}), SCE (SrCe{sub 0.9}Eu{sub 0.1}O{sub 3}) and SCTm (SrCe{sub 0.95}Tm{sub 0.05}O{sub 3}) have been successfully obtained for temperatures between 800 and 950 C and pressures from 1 to 12 bar in this project. However, it is known that the cerate-based perovskite materials can react with CO{sub 2}. Therefore, the stability issue of the proton conducting perovskite materials under CO{sub 2} or H{sub 2}S environments was examined. Tests were conducted in the Thermo Gravimetric Analyzer (TGA) unit for powder and disk forms of BCN and SCE. Perovskite materials doped with zirconium (Zr) are known to be resistant to CO{sub 2}. The results from the evaluation of the chemical stability for the Zr doped perovskite membranes are presented. During this reporting period, flowsheet simulation was also performed to calculate material and energy balance based on several hydrogen production processes from coal using high temperature membrane reactor (1000 C), low temperature membrane reactor (250 C), or conventional technologies. The results show that the coal to hydrogen process employing both the high temperature and the low temperature membrane reactors can increase the hydrogen production efficiency (cold gas efficiency) by more than 50% compared to the conventional process. Using either high temperature or low temperature membrane reactor process also results in an increase of the cold gas efficiencies as well as the thermal efficiencies of the overall process.« less