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Title: Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1

Abstract

This is the first semi-annual progress report for the program "Integrated High Temperature Coal to Hydrogen System with CO2 Separation." The objective of the program is to develop a detailed design for a single high-temperature syngas-cleanup module to produce a pure stream of H2 from a coal-based system and to develop the new high-temperature membrane materials at the core of that design. The novel one-box process combines a shift reactor with a high-temperature CO2-selective membrane to convert CO to CO2, remove sulfur compounds, and remove CO2 in a simple, compact, fully integrated system. In the first six months of the program, a conceptual design for the one-box system was developed in Task 1 and the performance targets for the system and the membrane were evaluated. In Task 2.1 processes were developed for creating pore architectures in ceramics that are applicable to membrane structures. In Task 2.2, candidate materials were identified that have the potential for separation of CO2 and H2S at high temperatures.

Authors:
; ; ;
Publication Date:
Research Org.:
GE Global Research
Sponsoring Org.:
USDOE - Office of Fossil Energy (FE)
OSTI Identifier:
861563
Report Number(s):
DOE-NT-42451-1
DOE Contract Number:
FC26-05NT42451
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 36 MATERIALS SCIENCE; coal gasification; CO2 separation; syngas cleanup; membrane

Citation Formats

Ruud, J A, Ku, A, Ramaswamy, V, and Wei, W. Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1. United States: N. p., 2005. Web. doi:10.2172/861563.
Ruud, J A, Ku, A, Ramaswamy, V, & Wei, W. Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1. United States. doi:10.2172/861563.
Ruud, J A, Ku, A, Ramaswamy, V, and Wei, W. Wed . "Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1". United States. doi:10.2172/861563. https://www.osti.gov/servlets/purl/861563.
@article{osti_861563,
title = {Integrated High Temperature Coal to Hydrogen System with CO2 Separation: Semi-Annual Progress Report 1},
author = {Ruud, J A and Ku, A and Ramaswamy, V and Wei, W},
abstractNote = {This is the first semi-annual progress report for the program "Integrated High Temperature Coal to Hydrogen System with CO2 Separation." The objective of the program is to develop a detailed design for a single high-temperature syngas-cleanup module to produce a pure stream of H2 from a coal-based system and to develop the new high-temperature membrane materials at the core of that design. The novel one-box process combines a shift reactor with a high-temperature CO2-selective membrane to convert CO to CO2, remove sulfur compounds, and remove CO2 in a simple, compact, fully integrated system. In the first six months of the program, a conceptual design for the one-box system was developed in Task 1 and the performance targets for the system and the membrane were evaluated. In Task 2.1 processes were developed for creating pore architectures in ceramics that are applicable to membrane structures. In Task 2.2, candidate materials were identified that have the potential for separation of CO2 and H2S at high temperatures.},
doi = {10.2172/861563},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Wed Dec 21 00:00:00 EST 2005},
month = {Wed Dec 21 00:00:00 EST 2005}
}

Technical Report:

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  • A significant barrier to the commercialization of coal-to-hydrogen technologies is high capital cost. The purity requirements for H{sub 2} fuels are generally met by using a series of unit clean-up operations for residual CO removal, sulfur removal, CO{sub 2} removal and final gas polishing to achieve pure H{sub 2}. A substantial reduction in cost can be attained by reducing the number of process operations for H{sub 2} cleanup, and process efficiency can be increased by conducting syngas cleanup at higher temperatures. The objective of this program was to develop the scientific basis for a single high-temperature syngas-cleanup module to producemore » a pure stream of H{sub 2} from a coal-based system. The approach was to evaluate the feasibility of a 'one box' process that combines a shift reactor with a high-temperature CO{sub 2}-selective membrane to convert CO to CO{sub 2}, remove sulfur compounds, and remove CO{sub 2} in a simple, compact, fully integrated system. A system-level design was produced for a shift reactor that incorporates a high-temperature membrane. The membrane performance targets were determined. System level benefits were evaluated for a coal-to-hydrogen system that would incorporate membranes with properties that would meet the performance targets. The scientific basis for high temperature CO{sub 2}-selective membranes was evaluated by developing and validating a model for high temperature surface flow membranes. Synthesis approaches were pursued for producing membranes that integrated control of pore size with materials adsorption properties. Room temperature reverse-selectivity for CO{sub 2} was observed and performance at higher temperatures was evaluated. Implications for future membrane development are discussed.« less
  • A method of polishing coal synthesis gas by an electrochemical membrane operation is being perfected. The operation takes advantage of an electrochemical potential gradient rather than conventional techniques, separating the H{sub 2}S from the coal gas stream, leaving only H{sub 2} to enrich the exiting fuel gases. Sulfur is the by-product that is carried away by a separate inert sweep gas and condensed downstream. The technology is attractive due to simplicity as well as economics when compared to alternatives. Experimental analysis was not possible this quarter due to a change of laboratories. This change makes possible improved experimental conditions. Predominantmore » work dealt with improving the current process, improving the oven structure to accommodate a controlled atmosphere heating, regulating oven conditions using resistance control, etc.« less
  • The cobalt cathode used in the EMS proved stable and efficient. Removal of H{sub 2}S was deterred by the possibility of hydrogen cross-over from process gases creating alternate reactions unfavorable to the removal system. Application of back pressure from the anode side of the cell would be the simplest solution to H{sub 2} cross-over. Examination of water proof of the vapor in the anode exit gases would provide proof of the aforementioned reaction hypothesis. Cobalt aluminate formation should not prove problematic, since degradation of the Co Cathode did not occur as a result. Once equilibrium is reached electrolyte addition ismore » not necessary, therefore not a major concern.« less
  • A method of polishing coal synthesis by electrochemical operation is being perfected. An electrochemical potential gradient is used to remove H{sub 2}S from the coal gas stream, leaving only H{sub 2} to enrich the exiting polished gases. Sulfur byproduct is swept away by an inert sweep gas and later condensed. Current experiments are based on improving selective removal from low initial H{sub 2}S contents (10 ppm). High flow rate data is also being investigated along with sealing the cell housings. Latest option for consistent removal and seals is Zircar manufactured membranes.
  • An advanced process for the separation of hydrogen sulfide from coal gasification product streams through an electrochemical membrane is being developed using the funds from this grant. H{sub 2}S is removed from the syn-gas stream, split into hydrogen, which enriches the syn-gas, and sulfur, which can be condensed from an inert gas sweep stream. The process allows removal of H{sub 2}S without cooling the gas stream and with neglible pressure loss through the separator. The process is economically attractive by the lack of adsorbents and the lack of a Claus process for sulfur recovery.