CO2 capture and storage (CCS) is one of the key climate change mitigation technologies. However, this process is associated with high energy consumption and cost. Utilizing the captured CO2 instead for conversion into valuable chemicals and fuels could not only (partially) close the anthropogenic carbon cycle, but also be a cost-effective alternative to make CCS commercially viable. Among CO2 utilization routes, dry reforming of methane to syngas is promising since it couples CO2 utilization to fuels production. We have previously proposed “chemical looping dry reforming” (CLDR) as a promising process alternative to conventional dry reforming, and later extended this approach towards an alternate process configuration that directly produces fully separated syngas streams, i.e. separate effluent streams of H2 and CO. In the present paper, we analyze CLDR with the aim of maximizing H2 production by combining the dry reforming reaction with water gas shift for converting CO to H2, followed by CO2 capture, along with with power generation using waste heat recovery. The overall system is designed to produce a desired flow rate of H2 from natural gas, while maximizing the yield and minimizing the overall energy consumption. Different configurations are evaluated for supplying the heat required for the highly endothermic dry reforming reaction, including combustion of (i) CH4; (ii) a part of the CO produced in the CO2 reactor; and (iii) a fraction of the produced H2. All configurations include CO2 capture and H2 purification via pressure swing adsorption. Building on our previous fixed-bed experimental results, reactor-level mass and energy balance calculations are performed and coupled with a systems-level model that incorporates thermodynamic calculations of individual process components such as water gas shift reactors, blowers, feed compressors, CO2 capture, PSA, and heat recovery equipment as well as steam turbines. The different flow schemes are comparatively evaluated on performance metrics such as energy efficiency, chemical efficiency and net CO2 utilization, and the results are compared with a conventional H2 production pathway using steam methane reforming (SMR). Finally, an on-going preliminary cost assessment aims to evaluate the economic feasibility of a modular, small-scale CLDR-H2 process for decentralized application, such as distributed sources of natural gas (shale or stranded resources).

Chemical looping dry reforming of methane for production of H2: Process modeling and systems analysis

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.