能源化学(英文版)

能源化学(英文) ›› 2017, Vol. 26 ›› Issue (5): 1014-1025.DOI: 10.1016/j.jechem.2017.09.001

• ARTICLES • 上一篇    下一篇

Catalytic steam methane reforming enhanced by CO2 capture on CaO based bi-functional compounds

Francesca Michelia,b, Manuela Sciarrab, Claire Coursona, Katia Galluccib   

  1. a Institut de Chimie et Procédés pour l'Énergie, l'Environnement et la Santé, UMR CNRS 7515, ECPM, University of Strasbourg, 25 rue Becquerel, 67087 Strasbourg cedex 2, France;
    b Department of Industrial Engineering, University of L'Aquila, 18 via G. Gronchi, 67100 L'Aquila, Italy
  • 收稿日期:2017-06-01 修回日期:2017-09-08 出版日期:2017-09-15 发布日期:2017-11-10
  • 通讯作者: Claire Courson,E-mail address:claire.courson@unistra.fr
  • 基金资助:

    The financial support of European Contract 299732 UNIfHY is kindly acknowledged (UNIQUE For HYdrogen production, funded by FCH-JU under the topic SP1-JTI-FCH.2011.2.3:Biomass-toHydrogen thermal conversion processes).

Catalytic steam methane reforming enhanced by CO2 capture on CaO based bi-functional compounds

Francesca Michelia,b, Manuela Sciarrab, Claire Coursona, Katia Galluccib   

  1. a Institut de Chimie et Procédés pour l'Énergie, l'Environnement et la Santé, UMR CNRS 7515, ECPM, University of Strasbourg, 25 rue Becquerel, 67087 Strasbourg cedex 2, France;
    b Department of Industrial Engineering, University of L'Aquila, 18 via G. Gronchi, 67100 L'Aquila, Italy
  • Received:2017-06-01 Revised:2017-09-08 Online:2017-09-15 Published:2017-11-10
  • Contact: Claire Courson,E-mail address:claire.courson@unistra.fr
  • Supported by:

    The financial support of European Contract 299732 UNIfHY is kindly acknowledged (UNIQUE For HYdrogen production, funded by FCH-JU under the topic SP1-JTI-FCH.2011.2.3:Biomass-toHydrogen thermal conversion processes).

摘要： Sorption enhanced steam methane reforming (SE-SMR) was performed to maximize hydrogen production and contemporary remove CO2 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-Ca12Al14O33 sorbent system synthesized by wet mixing (CaO content of 100 wt%, 56 wt%, 30 wt%, or 0 wt% and balance of Ca12Al14O33) 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-Ca12Al14O33 (56 wt% of CaO and Ca12Al14O33 balance), was chosen to study the effect of different weight hourly space times (WHST) and CH4 stream compositions in SE-SMR activity. Impregnated mayenite at both micro and laboratory scales showed stable H2 content of almost 74%, with CH4 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 H2 content up to almost 94.5%. When the sorption enhanced reaction is performed roughly 89% of CH4 conversion is achieved, and after the pre-breakthrough, the catalyst worked at the thermodynamic level. During cycling sorption/regeneration experiments, even if CO2 removal efficiency slightly decreases, CH4 conversion and H2 yield remain stable.

关键词: Sorption enhanced steam methane, reforming, By-functional sorbent-catalyst compounds, Calcium oxide, Nickel catalyst, Mayenite

Abstract: Sorption enhanced steam methane reforming (SE-SMR) was performed to maximize hydrogen production and contemporary remove CO2 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-Ca12Al14O33 sorbent system synthesized by wet mixing (CaO content of 100 wt%, 56 wt%, 30 wt%, or 0 wt% and balance of Ca12Al14O33) 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-Ca12Al14O33 (56 wt% of CaO and Ca12Al14O33 balance), was chosen to study the effect of different weight hourly space times (WHST) and CH4 stream compositions in SE-SMR activity. Impregnated mayenite at both micro and laboratory scales showed stable H2 content of almost 74%, with CH4 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 H2 content up to almost 94.5%. When the sorption enhanced reaction is performed roughly 89% of CH4 conversion is achieved, and after the pre-breakthrough, the catalyst worked at the thermodynamic level. During cycling sorption/regeneration experiments, even if CO2 removal efficiency slightly decreases, CH4 conversion and H2 yield remain stable.

Key words: Sorption enhanced steam methane, reforming, By-functional sorbent-catalyst compounds, Calcium oxide, Nickel catalyst, Mayenite