Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor

Converting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-ri...

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Main Authors: Srirat Chuayboon, Stéphane Abanades
Format: Article
Language:English
Published: MDPI AG 2020-11-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/10/11/1356
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author Srirat Chuayboon
Stéphane Abanades
author_facet Srirat Chuayboon
Stéphane Abanades
author_sort Srirat Chuayboon
collection DOAJ
description Converting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-rich syngas and metallic Zn was demonstrated in a flexible solar thermochemical reactor prototype, driven by highly concentrated sunlight. Using solar energy as the process heat source in chemical-looping methane reforming with the ZnO/Zn oxygen carrier is a means to reduce the dependence on conventional energy resources and to reduce emissions of CO<sub>2</sub> and other pollutants, while upgrading the calorific value of the feedstock for the production of energy-intensive and high-value chemical fuels and materials. On-sun experiments were carried out with different operating parameters including operating temperatures (800–1000 °C), inlet methane flow-rates (0.1–0.4 NL/min), and inlet ZnO feeding-rates (0.5–1.0 g/min) both in batch and continuous modes under reduced (0.15 and 0.45 bar) and atmospheric pressures (0.90 bar), thereby demonstrating solar reactor flexibility and reliability. As a result, increasing the temperature promoted net ZnO conversion at the expense of favored methane cracking reaction, which can be lowered by decreasing pressure to vacuum conditions. Diminishing total pressure improved the net ZnO conversion but favored CO<sub>2</sub> yield due to insufficient gas residence time. Rising ZnO feeding rate under a constant over-stoichiometric CH<sub>4</sub>/ZnO molar ratio of 1.5 enhanced ZnO and methane consumption rates, which promoted Zn and syngas yields. However, an excessively high ZnO feeding rate may be detrimental, as ZnO could accumulate when the ZnO feeding rate is higher than the ZnO consumption rate. In comparison, continuous operation demonstrated greater performance regarding higher ZnO conversion (X<sub>ZnO</sub>) and lower methane cracking than batch operation. High-purity metallic Zn with a well-crystallized structure and of micrometric size was produced from both batch and continuous tests under vacuum and atmospheric pressures, demonstrating suitable reactor performance for the solar thermochemical methane-driven ZnO reduction process. The produced Zn metal can be further re-oxidized with H<sub>2</sub>O or CO<sub>2</sub> in an exothermic reaction to produce pure H<sub>2</sub> or CO by chemical-looping.
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spelling doaj.art-52116d4e911f4f1e87c1d3d3992f6e182023-11-20T21:48:39ZengMDPI AGCatalysts2073-43442020-11-011011135610.3390/catal10111356Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar ReactorSrirat Chuayboon0Stéphane Abanades1Department of Mechanical Engineering, King Mongkut’s Institute of Technology Ladkrabang, Prince of Chumphon Campus, Chumphon 86160, ThailandProcesses, Materials and Solar Energy Laboratory, PROMES-CNRS, 7 Rue du Four Solaire, 66120 Font-Romeu, FranceConverting sunlight into chemical fuels and metal commodities, via solar thermochemical conversion processes, is an attractive prospect for the long-term storage of renewable energy. In this study, the combined methane reforming and ZnO reduction in a single reaction for co-production of hydrogen-rich syngas and metallic Zn was demonstrated in a flexible solar thermochemical reactor prototype, driven by highly concentrated sunlight. Using solar energy as the process heat source in chemical-looping methane reforming with the ZnO/Zn oxygen carrier is a means to reduce the dependence on conventional energy resources and to reduce emissions of CO<sub>2</sub> and other pollutants, while upgrading the calorific value of the feedstock for the production of energy-intensive and high-value chemical fuels and materials. On-sun experiments were carried out with different operating parameters including operating temperatures (800–1000 °C), inlet methane flow-rates (0.1–0.4 NL/min), and inlet ZnO feeding-rates (0.5–1.0 g/min) both in batch and continuous modes under reduced (0.15 and 0.45 bar) and atmospheric pressures (0.90 bar), thereby demonstrating solar reactor flexibility and reliability. As a result, increasing the temperature promoted net ZnO conversion at the expense of favored methane cracking reaction, which can be lowered by decreasing pressure to vacuum conditions. Diminishing total pressure improved the net ZnO conversion but favored CO<sub>2</sub> yield due to insufficient gas residence time. Rising ZnO feeding rate under a constant over-stoichiometric CH<sub>4</sub>/ZnO molar ratio of 1.5 enhanced ZnO and methane consumption rates, which promoted Zn and syngas yields. However, an excessively high ZnO feeding rate may be detrimental, as ZnO could accumulate when the ZnO feeding rate is higher than the ZnO consumption rate. In comparison, continuous operation demonstrated greater performance regarding higher ZnO conversion (X<sub>ZnO</sub>) and lower methane cracking than batch operation. High-purity metallic Zn with a well-crystallized structure and of micrometric size was produced from both batch and continuous tests under vacuum and atmospheric pressures, demonstrating suitable reactor performance for the solar thermochemical methane-driven ZnO reduction process. The produced Zn metal can be further re-oxidized with H<sub>2</sub>O or CO<sub>2</sub> in an exothermic reaction to produce pure H<sub>2</sub> or CO by chemical-looping.https://www.mdpi.com/2073-4344/10/11/1356concentrated solar powersolar reactorchemical-looping methane reformingmetal oxideoxygen carriersyngas
spellingShingle Srirat Chuayboon
Stéphane Abanades
Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
Catalysts
concentrated solar power
solar reactor
chemical-looping methane reforming
metal oxide
oxygen carrier
syngas
title Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
title_full Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
title_fullStr Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
title_full_unstemmed Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
title_short Solar-Driven Chemical Looping Methane Reforming Using ZnO Oxygen Carrier for Syngas and Zn Production in a Cavity-Type Solar Reactor
title_sort solar driven chemical looping methane reforming using zno oxygen carrier for syngas and zn production in a cavity type solar reactor
topic concentrated solar power
solar reactor
chemical-looping methane reforming
metal oxide
oxygen carrier
syngas
url https://www.mdpi.com/2073-4344/10/11/1356
work_keys_str_mv AT sriratchuayboon solardrivenchemicalloopingmethanereformingusingznooxygencarrierforsyngasandznproductioninacavitytypesolarreactor
AT stephaneabanades solardrivenchemicalloopingmethanereformingusingznooxygencarrierforsyngasandznproductioninacavitytypesolarreactor