Abstract In this work, a new type of multifunctional materials (MFMs) called self‐regenerative Ni‐doped CaTiO3/CaO is introduced for the integrated CO2capture and dry reforming of methane (ICCDRM). These materials consist of a catalytically active Ni‐doped CaTiO3and a CO2sorbent, CaO. The article proposes a concept where the Ni catalyst can be regenerated in situ, which is crucial for ICCDRM. Exsolved Ni nanoparticles are evenly distributed on the surface of CaTiO3under H2or CH4, and are re‐dispersed back into the CaTiO3lattice under CO2. The Ni‐doped CaTiO3/CaO MFMs show stable CO2capture capacity and syngas productivity for 30 cycles of ICCDRM. The presence of CaTiO3between CaO grains prevents CaO/CaCO3thermal sintering during carbonation and decarbonation. Moreover, the strong interaction of CaTiO3with exsolved Ni mitigates severe accumulation of coke deposition. This concept can be useful for developing MFMs with improved properties that can advance integrated carbon capture and conversion.
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Ce stabilized Ni–SrO as a catalytic phase transition sorbent for integrated CO 2 capture and CH 4 reforming
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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- Award ID(s):
- 1923468
- PAR ID:
- 10384479
- Date Published:
- Journal Name:
- Journal of Materials Chemistry A
- Volume:
- 10
- Issue:
- 6
- ISSN:
- 2050-7488
- Page Range / eLocation ID:
- 3077 to 3085
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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