Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming
Abstract
Integration of carbon dioxide capture from flue gas with dry reforming of CH4 represents an attractive approach for CO2 utilization. The selection of a suitable bifunctional material serving as a catalyst/sorbent is the key. This paper reports Ni decorated and CeOx-stabilized SrO (SrCe0.5Ni0.5) as a multi-functional, phase transition catalytic sorbent material. The effect of CeOx on the morphology, structure, decarbonation reactivity, and cycling stability of the catalytic sorbent was determined with TEM-EDX, XRD, in situ XRD, CH4-TPR and TGA. Here, cyclic process tests were conducted in a packed bed reactor. The results indicate that large Ni clusters were present on the surface of the SrNi sorbent, and the addition of CeO2 promoted even distribution of Ni on the surface. Moreover, the Ce–Sr interaction promoted a complex carbonation/decarbonation phase-transition, i.e. SrCO3 + CeO2 ↔ Sr2CeO4 + CO2 as opposed to the conventional, simple carbonation/decarbonation cycles (e.g. SrCO3 ↔ SrO + CO2). This double replacement crystalline phase transition mechanism not only adjusts the carbonation/calcination thermodynamics to facilitate SrCO3 decomposition at relatively low temperatures but also inhibits sorbent sintering. As a result, excellent activity and stability were observed with up to 91% CH4 conversion, >72% CO2 capture efficiency and ~100% residual O2 capturemore »
- Authors:
-
- North Carolina State University, Raleigh, NC (United States); Nanjing Institute of Technology (China)
- North Carolina State University, Raleigh, NC (United States); East China Univ. of Science and Technology, Shanghai (China)
- North Carolina State University, Raleigh, NC (United States)
- Publication Date:
- Research Org.:
- North Carolina State University, Raleigh, NC (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
- OSTI Identifier:
- 1978845
- Alternate Identifier(s):
- OSTI ID: 1839801
- Grant/Contract Number:
- EE0008809; CBET-1923468
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 6; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Gu, Haiming, Gao, Yunfei, Iftikhar, Sherafghan, and Li, Fanxing. Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming. United States: N. p., 2021.
Web. doi:10.1039/d1ta09967a.
Gu, Haiming, Gao, Yunfei, Iftikhar, Sherafghan, & Li, Fanxing. Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming. United States. https://doi.org/10.1039/d1ta09967a
Gu, Haiming, Gao, Yunfei, Iftikhar, Sherafghan, and Li, Fanxing. Fri .
"Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming". United States. https://doi.org/10.1039/d1ta09967a. https://www.osti.gov/servlets/purl/1978845.
@article{osti_1978845,
title = {Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming},
author = {Gu, Haiming and Gao, Yunfei and Iftikhar, Sherafghan and Li, Fanxing},
abstractNote = {Integration of carbon dioxide capture from flue gas with dry reforming of CH4 represents an attractive approach for CO2 utilization. The selection of a suitable bifunctional material serving as a catalyst/sorbent is the key. This paper reports Ni decorated and CeOx-stabilized SrO (SrCe0.5Ni0.5) as a multi-functional, phase transition catalytic sorbent material. The effect of CeOx on the morphology, structure, decarbonation reactivity, and cycling stability of the catalytic sorbent was determined with TEM-EDX, XRD, in situ XRD, CH4-TPR and TGA. Here, cyclic process tests were conducted in a packed bed reactor. The results indicate that large Ni clusters were present on the surface of the SrNi sorbent, and the addition of CeO2 promoted even distribution of Ni on the surface. Moreover, the Ce–Sr interaction promoted a complex carbonation/decarbonation phase-transition, i.e. SrCO3 + CeO2 ↔ Sr2CeO4 + CO2 as opposed to the conventional, simple carbonation/decarbonation cycles (e.g. SrCO3 ↔ SrO + CO2). This double replacement crystalline phase transition mechanism not only adjusts the carbonation/calcination thermodynamics to facilitate SrCO3 decomposition at relatively low temperatures but also inhibits sorbent sintering. As a result, excellent activity and stability were observed with up to 91% CH4 conversion, >72% CO2 capture efficiency and ~100% residual O2 capture efficiency from flue gas by utilizing the CeO2 ↔ Ce2O3 redox transition. This renders an intensified process with zero coke deposition. Moreover, the SLDRM with SrCe0.5Ni0.5 has the flexibility to produce concentrated CO via CO2-splitting while co-producing a syngas with tunable H2/CO ratios.},
doi = {10.1039/d1ta09967a},
journal = {Journal of Materials Chemistry. A},
number = 6,
volume = 10,
place = {United States},
year = {Fri Dec 24 00:00:00 EST 2021},
month = {Fri Dec 24 00:00:00 EST 2021}
}
Figures / Tables:
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