Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO2 capture and CH4 reforming

Gu, Haiming; Gao, Yunfei; Iftikhar, Sherafghan; Li, Fanxing

doi:10.1039/d1ta09967a

Title: Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO₂ capture and CH₄ reforming

Journal Article · 24 December 2021 · Journal of Materials Chemistry. A

DOI: https://doi.org/10.1039/d1ta09967a · OSTI ID:1978845

Gu, Haiming ^[1]; Gao, Yunfei ^[2]; Iftikhar, Sherafghan ^[3];

^[3]

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)

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 CeO_x-stabilized SrO (SrCe_0.5Ni_0.5) as a multi-functional, phase transition catalytic sorbent material. The effect of CeO_x 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 SrCe_0.5Ni_0.5 has the flexibility to produce concentrated CO via CO₂-splitting while co-producing a syngas with tunable H₂/CO ratios.

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Research Organization:: North Carolina State University, Raleigh, NC (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); USDOE

Grant/Contract Number:: EE0008809; CBET-1923468

OSTI ID:: 1978845

Alternate ID(s):: OSTI ID: 1839801

Journal Information:: Journal of Materials Chemistry. A, Vol. 10, Issue 6; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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