Stability of Fe- and Zn-Promoted Mo/ZSM-5 Catalysts for Ethane Dehydroaromatization in Cyclic Operation Mode

被引:26
|
作者
Robinson, Brandon [1 ]
Bai, Xinwei [1 ]
Samanta, Anupam [1 ]
Abdelsayed, Victor [2 ,3 ]
Shekhawat, Dushyant [2 ]
Hu, Jianli [1 ]
机构
[1] West Virginia Univ, Dept Chem & Biomed Engn, 395 Evansdale Dr, Morgantown, WV 26505 USA
[2] US DOE, Natl Energy Technol Lab, 3610 Collins Ferry Rd, Morgantown, WV 26505 USA
[3] AECOM, 3610 Collins Ferry Rd, Morgantown, WV 26505 USA
关键词
METHANE DEHYDROAROMATIZATION; CH4; DEHYDROAROMATIZATION; MO/HZSM-5; CATALYSTS; H-ZSM-5; ZEOLITE; ACID SITES; 1073; K; AROMATIZATION; CONVERSION; DISPROPORTIONATION; REGENERATION;
D O I
10.1021/acs.energyfuels.8b01516
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
The stability of Fe-and Zn-promoted Mo/ZSM-5 catalysts was studied toward the ethane dehydroaromatization reaction. To elucidate the catalyst deactivation and regeneration mechanism, the catalytic performance was evaluated during five consecutive reaction-regeneration cycles. The addition of Zn to Mo/ZSM-5 resulted in an initial increase in aromatic selectivity; however, the loss of about 50% Zn resulted in a total decrease in aromatic selectivity over five reaction and regeneration cycles. The addition of Fe to Mo/ZSM-5 resulted in no decrease in aromatic selectivity or aromatic yield throughout these reaction cycles. The formation of carbon nanotubes was observed on the Fe-promoted Mo/ZSM-5 catalyst, which was believed to improve gas diffusion to micropores. The presence of Fe- and Mo- agglomerated particles on the catalyst surface was observed at low Fe/Mo atomic ratios, resulting in the formation of base-grown carbon nanotubes. When the Fe/Mo atomic ratio increased, the agglomerated particles were able to leave the zeolite surface, resulting in the formation of tip-growth carbon nanotubes. The temperature-programmed reduction profile of the Fe-promoted Mo/ZSM-S catalyst also suggested the formation of a more stable Mo and/or Fe species at 615 degrees C, enhancing carbon nanotube formation. The addition of Fe in the bipromoted Mo/ZSMS catalyst was found to stabilize the catalyst surface and reduce its Zn loss.
引用
收藏
页码:7810 / 7819
页数:10
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