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FeO6 Octahedral Distortion Activates Lattice Oxygen in Perovskite Ferrite for Methane Partial Oxidation Coupled with CO2 Splitting
Abstract
Modulating lattice oxygen in metal oxides that conducts partial oxidation of methane in balancing C–H activation and syngas selectivity remains challenging. This paper describes the discovery of distorting FeO 6 octahedra in La 1– x Ce x FeO 3 ( x = 0, 0.25 0.5, 0.75, 1) orthorhombic perovskites for the promotion of lattice oxygen activation. By combined electrical conductivity relaxation measurements and density functional theory calculations studies, this paper describes the enhancement of FeO 6 octahedral distortion in La 1– x Ce x FeO 3 promoting their bulk oxygen mobility and surface oxygen exchange capability. Consequently, La 0.5 Ce 0.5 FeO 3 with the highest FeO 6 distortion achieves exceptional syngas productivity of ∼3 and 8 times higher than LaFeO 3 and CeFeO 3, respectively, in CH 4 partial oxidation step with simultaneous high CO 2 conversion (92%) in the CO 2 -splitting step at 850 °C. The results exemplify the feasibility to tailor the active lattice oxygen of perovskite by modulating the distortion of BO 6 in ABO 3, which ultimately influences their reaction performance in chemical looping processes.
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Cites
From ultrasoft pseudopotentials to the projector augmented-wave method
Kresse, G., & Joubert, D. (1999) · Physical Review B · doi:10.1103/physrevb.59.1758 · Cited by 85,307
Shannon, R. D. (1976) · Acta Crystallographica Section A · doi:10.1107/s0567739476001551 · Cited by 66,145
Cited by
Li, P., Zhou, Z., Wang, Q., Guo, M., Chen, S., Low, J., Long, R., Liu, W., Ding, P., Wu, Y., et al. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.0c05097 · Cited by 469
Self-citationC–H bond activation in light alkanes: a theoretical perspective
Wang, Y., Hu, P., Yang, J., Zhu, Y.-A., & Chen, D. (2021) · Chemical Society Reviews · doi:10.1039/d0cs01262a · Cited by 375
Xiao, K., Wang, Y., Wu, P., Hou, L., & Liu, Z. (2023) · Angewandte Chemie International Edition · doi:10.1002/anie.202301408 · Cited by 269
Metadata
- Authors
- Zhang, X., Pei, C., Chang, X., Chen, S., Liu, R., Zhao, Z.-J., Mu, R., & Gong, J.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-06-03
- Volume
- 142
- Issue
- 26
- Pages
- 11540-11549
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3030011157
- Cited by
- 410
- References
- 2
- FWCI
- 12.46
- Type
- journal article
- Language
- en
- Open access
- closed
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- Zhang, X., Pei, C., Chang, X., Chen, S., Liu, R., Zhao, Z.-J., Mu, R., & Gong, J. (2020). FeO6 Octahedral Distortion Activates Lattice Oxygen in Perovskite Ferrite for Methane Partial Oxidation Coupled with CO2 Splitting. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.0c04643
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