High-capacity thermochemical CO2 dissociation using iron-poor ferrites

Zhai, Shang; Rojas, Jimmy; Ahlborg, Nadia; Lim, Kipil; Cheng, Chung Hon Michael; Xie, Chenlu; Toney, Michael F.; Jung, In-Ho; Chueh, William C.; Majumdar, Arun

doi:10.1039/c9ee02795e

Title: High-capacity thermochemical CO₂ dissociation using iron-poor ferrites

Journal Article · Wed Jan 08 00:00:00 EST 2020 · Energy & Environmental Science

DOI:https://doi.org/10.1039/c9ee02795e· OSTI ID:1608946

Zhai, Shang ^[1]; Rojas, Jimmy ^[1]; Ahlborg, Nadia ^[1]; Lim, Kipil ^[2]; Cheng, Chung Hon Michael ^[3]; Xie, Chenlu ^[1];

^[4]; Jung, In-Ho ^[5];

^[2];

^[1]

Stanford Univ., CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Harvard Univ., Cambridge, MA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Seoul National Univ. Seoul (South Korea)

Dissociation of CO₂ to form CO can play a key role in decarbonizing our energy system. We report here a two-step thermochemical cycle using a variety of iron-poor (Fe-poor) ferrites (Fe_yM_1-yO_x where y < 2/3) that produce CO with unusually high yield using Fe as the redox active species. Conventional wisdom suggests that increasing the Fe fraction would increase the capacity for CO₂ dissociation. Here, we report the opposite result: at partial pressure ratio CO : CO₂ = 1 : 100, we demonstrated CO yields of 8.0 ± 1.0 mL-CO per gram from Fe_0.35Ni_0.65O_x, and 3.7 ± 1.0 mL-CO per gram from Fe_0.45Co_0.55O_x, at a thermal reduction temperature of 1300 °C; remarkably, these CO₂ dissociation capacities are significantly higher than those of state-of-the-art materials such as spinel ferrites (Fe₂MO₄), (substituted) ceria, and Mn-based perovskite oxides. Optimization of the kinetics of Fe-poor ferrites with a ZrO₂ support resulted in higher CO yields per gram of ferrite. The unexpected CO yield vs. Fe ratio trend is consistent with the prediction of calculated ternary phase diagrams, which suggest a swing between spinel and rocksalt phases. Finally, these Fe-poor ferrites open new opportunities for tuning the redox properties of oxygen exchange materials.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: N00014-17-1-2918; AC02-76SF00515

OSTI ID:: 1608946

Alternate ID(s):: OSTI ID: 1593476

Journal Information:: Energy & Environmental Science, Vol. 13, Issue 2; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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