Journal
CHEMSUSCHEM
Volume 10, Issue 17, Pages 3402-3408Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201700699
Keywords
chemical looping; hydrogen; perovskite; syngas; water splitting
Funding
- U.S. National Science Foundation [CBET-1254351, CBET-1510900]
- Kenan Institute at North Carolina State University
- Div Of Chem, Bioeng, Env, & Transp Sys
- Directorate For Engineering [1510900] Funding Source: National Science Foundation
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A rationalized strategy to optimize transition-metal-oxide-based redox catalysts for water splitting and syngas generation through a hybrid solar-redox process is proposed and validated. Monometallic transition metal oxides do not possess desirable properties for water splitting; however, density functional theory calculations indicate that the redox properties of perovskite-structured BaMnxFe1-xO3- can be varied by changing the B-site cation compositions. Specifically, BaMn0.5Fe0.5O3- is projected to be suitable for the hybrid solar-redox process. Experimental studies confirm such predictions, demonstrating 90% steam-to-hydrogen conversion in water splitting and over 90% syngas yield in the methane partial-oxidation step after repeated redox cycles. Compared to state-of-the-art solar-thermal water-splitting catalysts, the rationally designed redox catalyst reported is capable of splitting water at a significantly lower temperature and with ten-fold increase in steam-to-hydrogen conversion. Process simulations indicate the potential to operate the hybrid solar-redox process at a higher efficiency than state-of-the-art hydrogen and liquid-fuel production processes with 70% lower CO2 emissions for hydrogen production
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