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Integration of carbon dioxide capture from flue gas with dry reforming of CH 4 represents an attractive approach for CO 2 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 0.5 Ni 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, CH 4 -TPR and TGA. 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 CeO 2 promoted even distribution of Ni on the surface. Moreover, the Ce–Sr interaction promoted a complex carbonation/decarbonation phase-transition, i.e. SrCO 3 + CeO 2 ↔ Sr 2 CeO 4 + CO 2 as opposed to the conventional, simple carbonation/decarbonation cycles ( e.g. SrCO 3 ↔ SrO + CO 2 ). This double replacement crystalline phase transition mechanism not only adjusts the carbonation/calcination thermodynamics to facilitate SrCO 3 decomposition at relatively low temperatures but also inhibits sorbent sintering. As a result, excellent activity and stability were observed with up to 91% CH 4 conversion, >72% CO 2 capture efficiency and ∼100% residual O 2 capture efficiency from flue gas by utilizing the CeO 2 ↔ Ce 2 O 3 redox transition. This renders an intensified process with zero coke deposition. Moreover, the SLDRM with SrCe 0.5 Ni 0.5 has the flexibility to produce concentrated CO via CO 2 -splitting while co-producing a syngas with tunable H 2 /CO ratios.
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Sorption-enhanced steam reforming of toluene using multifunctional perovskite phase transition sorbents in a chemical looping scheme
Abstract Sorption-enhanced steam reforming (SESR) of toluene (SESRT) using catalytic CO2sorbents is a promising route to convert the aromatic tar byproducts formed in lignocellulosic biomass gasification into hydrogen (H2) or H2-rich syngas. Commonly used sorbents such as CaO are effective in capturing CO2initially but are prone to lose their sorption capacity over repeated cycles due to sintering at high temperatures. Herein, we present a demonstration of SESRT using A- and B-site doped Sr1−xA’xFe1−yB’yO3−δ(A’ = Ba, Ca; B’ = Co) perovskites in a chemical looping scheme. We found that surface impregnation of 5–10 mol% Ni on the perovskite was effective in improving toluene conversion. However, upon cycling, the impregnated Ni tends to migrate into the bulk and lose activity. This prompted the adoption of a dual bed configuration using a pre-bed of NiO/γ–Al2O3catalyst upstream of the sorbent. A comparison is made between isothermal operation and a more traditional temperature-swing mode, where for the latter, an average sorption capacity of ∼38% was witnessed over five SESR cycles with H2-rich product syngas evidenced by a ratio of H2: COx> 4.0. XRD analysis of fresh and cycled samples of Sr0.25Ba0.75Fe0.375Co0.625O3-δreveal that this material is an effective phase transition sorbent—capable of cyclically capturing and releasing CO2without irreversible phase changes occurring.
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- Award ID(s):
- 1923468
- PAR ID:
- 10422473
- Publisher / Repository:
- IOP Publishing
- Date Published:
- Journal Name:
- Journal of Physics: Energy
- Volume:
- 5
- Issue:
- 3
- ISSN:
- 2515-7655
- Page Range / eLocation ID:
- Article No. 035004
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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