Hard templating ultrathin polycrystalline hematite nanosheets: effect of nano-dimension on CO 2 to CO conversion via the reverse water-gas shift reaction

Fishman, Zachary S.; He, Yulian; Yang, Ke R.; Lounsbury, Amanda W.; Zhu, Junqing; Tran, Thanh Minh; Zimmerman, Julie B.; Batista, Victor S.; Pfefferle, Lisa D.

doi:10.1039/c7nr03522e

Title: Hard templating ultrathin polycrystalline hematite nanosheets: effect of nano-dimension on CO ₂ to CO conversion via the reverse water-gas shift reaction

Journal Article · Sun Jan 01 00:00:00 EST 2017 · Nanoscale

DOI:https://doi.org/10.1039/c7nr03522e· OSTI ID:1492968

^[1]; He, Yulian ^[1]; Yang, Ke R. ^[2]; Lounsbury, Amanda W. ^[1]; Zhu, Junqing ^[3]; Tran, Thanh Minh ^[1]; Zimmerman, Julie B. ^[1]; Batista, Victor S. ^[2]; Pfefferle, Lisa D. ^[1]

Department of Chemical and Environmental Engineering; Yale University; New Haven; USA
Department of Chemistry and Energy Sciences Institute; Yale University; New Haven; USA
Department of Chemistry; Nankai University; Tianjin 300071; China

Understanding how nano-dimensionality impacts iron oxide based catalysis is central to a wide range of applications. Here, we focus on hematite nanosheets, nanowires and nanoparticles as applied to catalyze the reverse water gas shift (RWGS) probe reaction. We introduce a novel approach to synthesize ultrathin (4–7 nm) hematite nanosheets using copper oxide nanosheets as a hard template and propose a reaction mechanism based on density functional theory (DFT) calculations. Hematite nanowires and nanoparticles were also synthesized and characterized. H2 temperature programmed reduction (H2-TPR) and RWGS reactions were performed to glean insights into the mechanism of CO2 conversion to CO over the iron oxide nanomaterials and were compared to H2 binding energy calculations based on density functional theory. While the nanosheets did exhibit high CO2 conversion, 28% at 510 °C, we found that the iron oxide nanowires had the highest CO2 conversion, reaching 50% at 750 °C under atmospheric pressure. No products besides CO and H2O were detected.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE

OSTI ID:: 1492968

Journal Information:: Nanoscale, Vol. 9, Issue 35; ISSN 2040-3364

Country of Publication:: United States

Language:: English

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Title: Hard templating ultrathin polycrystalline hematite nanosheets: effect of nano-dimension on CO ₂ to CO conversion via the reverse water-gas shift reaction