摘要
Sorption enhanced steam methane reforming（SE-SMR） was performed to maximize hydrogen production and contemporary remove COfrom the product stream using bi-functional sorbent-catalyst compounds.Samples were tested at two different scales: micro and laboratory. The CaO amount varied in the CaO-CaAlOsorbent system synthesized by wet mixing(CaO content of 100 wt%, 56 wt%, 30 wt%, or 0 wt% and balance of CaAlO) which were upgraded to bi-functional compounds by impregnation of 3 wt% of Ni. Nitrogen adsorption（BET/BJH）, X-Ray Diffraction（XRD）, Temperature-Programmed Reduction（TPR） and Scanning and Transmission Electronic Microscopy（SEM and TEM, respectively） analyses were performed to characterize structural and textural properties and reducibility of the bi-functional materials and evaluate their catalytic behavior. A fixed sorbent composition CaO-CaAlO(56 wt% of CaO and CaAlObalance), was chosen to study the effect of different weight hourly space times（WHST） and CHstream compositions in SE-SMR activity. Impregnated mayenite at both micro and laboratory scales showed stable Hcontent of almost 74%, with CHconversion of 72% similarly to the values reported by the sample containing 30 wt% of CaO in the post-breakthrough.Sample with 30 wt% of CaO showed promisingly behavior, enhancing Hcontent up to almost 94.5%.When the sorption enhanced reaction is performed roughly 89% of CHconversion is achieved, and after the pre-breakthrough, the catalyst worked at the thermodynamic level. During cycling sorption/regeneration experiments, even if COremoval efficiency slightly decreases, CHconversion and Hyield remain stable.
Sorption enhanced steam methane reforming(SE-SMR) was performed to maximize hydrogen production and contemporary remove CO_2 from the product stream using bi-functional sorbent-catalyst compounds.Samples were tested at two different scales: micro and laboratory. The CaO amount varied in the CaO-Ca_(12)Al_(14)O_(33) sorbent system synthesized by wet mixing(CaO content of 100 wt%, 56 wt%, 30 wt%, or 0 wt% and balance of Ca_(12)Al_(14)O_(33)) which were upgraded to bi-functional compounds by impregnation of 3 wt% of Ni. Nitrogen adsorption(BET/BJH), X-Ray Diffraction(XRD), Temperature-Programmed Reduction(TPR) and Scanning and Transmission Electronic Microscopy(SEM and TEM, respectively) analyses were performed to characterize structural and textural properties and reducibility of the bi-functional materials and evaluate their catalytic behavior. A fixed sorbent composition CaO-Ca_(12)Al_(14)O_(33)(56 wt% of CaO and Ca_(12)Al_(14)O_(33) balance), was chosen to study the effect of different weight hourly space times(WHST) and CH_4 stream compositions in SE-SMR activity. Impregnated mayenite at both micro and laboratory scales showed stable H_2 content of almost 74%, with CH_4 conversion of 72% similarly to the values reported by the sample containing 30 wt% of CaO in the post-breakthrough.Sample with 30 wt% of CaO showed promisingly behavior, enhancing H_2 content up to almost 94.5%.When the sorption enhanced reaction is performed roughly 89% of CH_4 conversion is achieved, and after the pre-breakthrough, the catalyst worked at the thermodynamic level. During cycling sorption/regeneration experiments, even if CO_2 removal efficiency slightly decreases, CH_4 conversion and H_2 yield remain stable.
基金
The financial support of European Contract 299732 UNIfHY(UNIQUE For HYdrogen production, funded by FCH-JU under the topic SP1-JTI-FCH.2011.2.3: Biomass-toHydrogen thermal conversion processes)
