Development of a CH4 dehydroaromatization-catalyst regeneration fluidized bed system

doi:10.1016/j.cjche.2018.03.035

Chin.J.Chem.Eng. ›› 2018, Vol. 26 ›› Issue (9): 1928-1936.DOI: 10.1016/j.cjche.2018.03.035

• Catalysis, Kinetics and Reaction Engineering • Previous Articles Next Articles

Development of a CH₄ dehydroaromatization-catalyst regeneration fluidized bed system

Peng Yan^1,2,3,4,5,6, Zhanguo Zhang⁷, Dapeng Li⁸, Xu Cheng^1,3,4,5,6, Xinzhuang Zhang^1,2,3,4,5,6, Fan Yang⁸, Chuanfeng Huang⁸, Xiaoxun Ma^1,3,4,5,6

1 School of Chemical Engineering, Northwest University, 229 North Taibai Road, Xi'an 710069, China;
2 Research Institute of Yanchang Petroleum(Group) Co. Ltd, Xi'an 710075, China;
3 Chemical Engineering Research Center of the Ministry of Education(MOE) for Advanced Use Technology of Shanbei Energy, Xi'an 710069, China;
4 Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Xi'an 710069, China;
5 Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi'an 710069, China;
6 International Scientific and Technological Cooperation Base of the Ministry of Science and Technology(MOST) for Clean Utilization of Hydrocarbon Resources, Xi'an 710069, China;
7 National Institute of Advanced Industrial Science and Technology(AIST), 16-1 Onogawa, Tsukuba, 305-8569, Ibaraki, Japan;
8 Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum(Group) Co. Ltd, Xi'an 710075, China

Received:2017-12-25 Revised:2018-03-26 Online:2018-10-17 Published:2018-09-28
Contact: Xiaoxun Ma,E-mail address:maxym@nwu.edu.cn
Supported by:
Supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum (Group) Co. Ltd, China (Contract No. HCRC-C13-010), and by the National Natural Science Foundation of China (21536009).

Development of a CH₄ dehydroaromatization-catalyst regeneration fluidized bed system

Peng Yan^1,2,3,4,5,6, Zhanguo Zhang⁷, Dapeng Li⁸, Xu Cheng^1,3,4,5,6, Xinzhuang Zhang^1,2,3,4,5,6, Fan Yang⁸, Chuanfeng Huang⁸, Xiaoxun Ma^1,3,4,5,6

1 School of Chemical Engineering, Northwest University, 229 North Taibai Road, Xi'an 710069, China;
2 Research Institute of Yanchang Petroleum(Group) Co. Ltd, Xi'an 710075, China;
3 Chemical Engineering Research Center of the Ministry of Education(MOE) for Advanced Use Technology of Shanbei Energy, Xi'an 710069, China;
4 Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Xi'an 710069, China;
5 Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi'an 710069, China;
6 International Scientific and Technological Cooperation Base of the Ministry of Science and Technology(MOST) for Clean Utilization of Hydrocarbon Resources, Xi'an 710069, China;
7 National Institute of Advanced Industrial Science and Technology(AIST), 16-1 Onogawa, Tsukuba, 305-8569, Ibaraki, Japan;
8 Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum(Group) Co. Ltd, Xi'an 710075, China

通讯作者: Xiaoxun Ma,E-mail address:maxym@nwu.edu.cn
基金资助:
Supported by Hydrocarbon High-efficiency Utilization Technology Research Center of Yanchang Petroleum (Group) Co. Ltd, China (Contract No. HCRC-C13-010), and by the National Natural Science Foundation of China (21536009).

Abstract

Abstract: A pilot-scale methane dehydroaromatization-H₂ regeneration fluidized bed system (MDARS) was developed. In the MDARS, the catalyst circulation between a fluidized bed reactor and a fluidized bed regenerator with the help of a catalyst feeder allowed methane dehydroaromatization (MDA) and H₂ regeneration to be carried out simultaneously, which is good for maintaining a stable MDA catalytic activity. A fixed bed reactor (FB) and a single fluidized bed reactor (SFB) were also used for a comparative study. The experimental results showed that the catalytic activity in the MDARS was more stable than that in the FB and SFB reactors. The effects of some parameters of MDARS on the CH₄ conversion and product selectivity were investigated. To verify the feasibility and reliability of the MDARS, an eight-hour long-term test was carried out, which demonstrated that the operation of the MDARS was stable and that the catalytic activity remained stable throughout the entire experimental period.

Key words: Methane dehydroaromatization, Hydrogen regeneration, Fluidized bed reactor, Pilot-scale, Catalyst circulation

摘要： A pilot-scale methane dehydroaromatization-H₂ regeneration fluidized bed system (MDARS) was developed. In the MDARS, the catalyst circulation between a fluidized bed reactor and a fluidized bed regenerator with the help of a catalyst feeder allowed methane dehydroaromatization (MDA) and H₂ regeneration to be carried out simultaneously, which is good for maintaining a stable MDA catalytic activity. A fixed bed reactor (FB) and a single fluidized bed reactor (SFB) were also used for a comparative study. The experimental results showed that the catalytic activity in the MDARS was more stable than that in the FB and SFB reactors. The effects of some parameters of MDARS on the CH₄ conversion and product selectivity were investigated. To verify the feasibility and reliability of the MDARS, an eight-hour long-term test was carried out, which demonstrated that the operation of the MDARS was stable and that the catalytic activity remained stable throughout the entire experimental period.

关键词: Methane dehydroaromatization, Hydrogen regeneration, Fluidized bed reactor, Pilot-scale, Catalyst circulation

Peng Yan, Zhanguo Zhang, Dapeng Li, Xu Cheng, Xinzhuang Zhang, Fan Yang, Chuanfeng Huang, Xiaoxun Ma. Development of a CH₄ dehydroaromatization-catalyst regeneration fluidized bed system[J]. Chin.J.Chem.Eng., 2018, 26(9): 1928-1936.

References

[1] L. Wang, L. Tao, M. Xie, G. Xu, J. Huang, Dehydrogenation and aromatization of methane under non-oxidizing conditions, Catal. Lett. 21(1-2) (1993) 35-41.

[2] Y.D. Xu, X.H. Bao, L.W. Lin, Direct conversion of methane under nonoxidative conditions, J. Catal. 216(2003) 386-395.

[3] J.J. Guo, H. Lou, X.M. Zheng, Energy-efficient coaromatization of methane and propane, J. Nat. Gas Chem. 18(2009)260-272.

[4] X. Dong, Y. Song, W. Lin, A new way to enhance the coke-resistance of Mo/HZSM-5 catalyst for methane dehydroaromatization, Catal. Commun. 8(3) (2007) 539-542.

[5] P. Wu, Q. Kan, X. Wang, D. Wang, H. Xing, Acidity and catalytic properties for methane conversion of Mo/HZSM-5 catalyst modified by reacting with organometallic complex, Appl. Catal. A Gen. 282(1-2) (2005) 39-44.

[6] P.L. Tan, C.T. Au, S.Y. Lai, Effects of acidification and basification of impregnating solution on the performance of Mo/HZSM-5 in methane aromatization, Appl. Catal. A Gen. 324(1) (2007) 36-41.

[7] L.L. Su, L. Liu, J. Zhuang, H. Wang, Y. Li, Creating mesopores in ZSM-5 zeolite by alkali treatment:a new way to enhance the catalytic performance of methane dehydroaromatization on Mo/HZSM-5 catalysts, Catal. Lett. 91(3-4) (2003) 155-167.

[8] Liu Ss, L. Wang, R. Ohnishi, M. Lchikawa, Bifunctional catalysis of Mo/HZSM-5 in the dehydroaromatization of methane with CO/CO 2 to benzene and naphthalene, Kinet. Catal. 41(1) (2000) 132-144.

[9] A.C.C. Rodrigues, J.L.F. Monteiro, CO₂ addition on the non-oxidative dehydroaromatization of methane over MoMCM-22, Catal. Lett. 117(3-4) (2007) 166-170.

[10] Y. Shu, R. Ohnishi, M. Ichikawa, Pressurized dehydrocondensation of methane toward benzene and naphthalene on Mo/HZSM-5 catalyst:optimization of reaction parameters and promotion by CO₂ addition, J. Catal. 206(1) (2002) 134-142.

[11] B. Cook, D. Mousko, W. Hoelderich, R. Zennaro, Conversion of methane to aromatics over Mo₂C/ZSM-5 catalyst in different reactor types, Appl. Catal. A Gen. 365(1) (2009) 34-41.

[12] M.P. Gimeno, J. Soler, J. Herguido, M. Menendez, Counteracting catalyst deactivation in methane aromatization with a two zone fluidized bed reactor, Ind. Eng. Chem. Res. 49(3) (2010) 996-1000.

[13] S.H. Morejudo, R. Zanón, S. Escolástico, I. Yustetirados, H. Malerodfjeld, Direct conversion of methane to aromatics in a catalytic co-ionic membrane reactor, Science 353(6299) (2016) 563-566.

[14] S. Park, M. Lee, J. Bae, D.Y. Hong, Y.K. Park, Plasma-assisted non-oxidative conversion of methane over Mo/HZSM-5 catalyst in DBD reactor, Top. Catal. 60(9-11) (2017) 735-742.

[15] D. Ma, D.Z. Wang, L.L. Su, Y.Y. Shu, Y.D. Xu, X.H. Bao, Carbonaceous deposition on Mo/HMCM-22 catalysts for methane aromatization:a TP technique investigation, J. Catal. 208(2) (2002)260-269.

[16] H. Ma, R. Kojima, R. Ohnishi, M. Ichikawa, Efficient regeneration of Mo/HZSM-5 catalyst by using air with NO in methane dehydro-aromatization reaction, Appl. Catal. A Gen. 275(1) (2004) 183-187.

[17] K. Honda, T. Yoshida, Z.G. Zhang, Methane dehydroaromatization over Mo/HZSM-5 in periodic CH₄-H₂ switching operation mode, Catal. Commun. 4(1) (2003)21-26.

[18] Y. Shu, H. Ma, R. Ohnishi, M. Ichikawa, Highly stable performance of catalytic methane dehydrocondensation towards benzene on Mo/HZSM-5 by a periodic switching treatment with H₂ and CO₂, Chem. Commun. 1(1) (2002) 86-87.

[19] N. Kosinov, F.J.A.G. Coumans, G.N. Li, E. Uslamin, B. Mezari, Stable Mo/HZSM-5 methane dehydroaromatization catalysts optimized for high-temperature calcinationregeneration, J. Catal. 346(2017) 125-133.

[20] Y. Lu, Z.S. Xu, Z.J. Tian, T. Zhang, L.W. Lin, Methane aromatization in the absence of an added oxidant and the bench scale reaction test, Catal. Lett. 62(1999)215-220.

[21] C.Y. Sun, G.Z. Fang, X.G. Guo, Y.L. Hu, S.Q. Ma, T.H. Yang, J. Han, H. Ma, D. Tan, X.H. Bao, Methane dehydroaromatization with periodic CH₄-H₂ switch:A promising process for aromatics and hydrogen, J. Energy Chem. 24(2015)257-263.

[22] Y.B. Xu, J.Y. Lu, J. Wang, Y. Suzuki, Z.G. Zhang, The catalytic stability of Mo/HZSM-5 in methane dehydroaromatization at severe and periodic CH₄-H₂ switch operating conditions, Chem. Eng. J. 168(1) (2011) 390-402.

[23] Y.B. Xu, Y. Song, Z.G. Zhang, A binder-free fluidizable Mo/HZSM-5 catalyst for nonoxidative methane dehydroaromatization in a dual circulating fluidized bed reactor system, Catal. Today 279(2017) 115-123.

[24] Y.B. Xu, H.T. Tao, Y. Yamamoto, Y. Suzuki, Z.G. Zhang, Comparison of the activities of binder-addedandbinder-freeMo/HZSM-5catalystsinmethanedehydroaromatization at 1073 K in periodic CH₄-H₂ switch operation mode, J. Nat. Gas Sci. Eng. 21(2012) 729-744.

[25] Z.G. Zhang, Y.B. Xu, Y. Song, H.T. Ma, Y. Yamamoto, Development of a two-bed circulating fluidized bed reactor system for nonoxidative aromatization of methane over Mo/HZSM-5 catalyst, Environ. Prog. Sustain. 35(2016) 325-333.

[26] X.Z. Zhang, P. Yan, F. Yang, X. Cheng, D.P. Li, An activation method for the preparation of aromatics catalysts in a cyclic fluidized reaction system using methane, Chinese Pat., 201310744964.2. (2013).

[27] H.M. Liu, L.L. Su, H.X. Wang, W.J. Shen, X.H. Bao, Y.D. Xu, The chemical nature of carbonaceous deposits and their role in methane dehydro-aromatization on Mo/MCM-22 catalysts, Appl. Catal. A Gen. 236(1) (2002)263-280.

[28] F. Solymosi,J.Cserenyi, A.Szoke,T.Bánsági,A.Oszkó, Aromatization of methaneover supported and unsupported Mo-based catalysts, J. Catal. 165(2) (1997) 150-161.

[29] H.M. Liu, T. Li, B.L. Tian, Y.D. Xu, Study of the carbonaceous deposits formed on a Mo/HZSM-5 catalyst in methane dehydro-aromatization by using TG and temperatureprogrammed techniques, Appl. Catal. A Gen. 213(1) (2001) 103-112.

[30] T.T.H. Vu, V.T. Le, P. Meriaudeau, C. Naccache, Aromatization of methane over zeolite supported molybdenum:active sites and reaction mechanism, J. Mol. Catal. A Chem. 181(1) (2002)283-290.

[31] H.T. Ma, R. Kojima, S. Kikuchi, M. Ichikawa, Hydrogen effect on coke removal and catalytic performance in pre-carburization and methane dehydro-aromatization reaction on Mo/HZSM-5, J. Nat. Gas Chem. 14(3) (2005) 129-139.

[32] B.S. Liu, Y. Zhang, J.F. Liu, M. Tian, F.M. Zhang, Characteristic and mechanism of methane dehydroaromatization over Zn-based/HZSM-5 catalysts under conditions of atmospheric pressure and supersonic jet expansion, J. Phys. Chem. C 115(34) (2011) 16954-16962.

[33] Y.B. Cui, Y.B. Xu, Y. Suzuki, Z.G. Zhang, Experimental evidence for three ratecontrolling regions of the non-oxidative methane dehydroaromatization over Mo/HZSM-5 catalyst at 1073 K, Catal. Sci. Technol. 1(5) (2011) 823-829.

[34] X. Cheng, P. Yan, X.Z. Zhang, F. Yang, C.Y. Dai, D.P. Li, X.X. Ma, Enhanced methane dehydroaromatization in the presence of CO₂ over Fe-and Mg-modified Mo/ZSM-5, Mol. Catal. 437(2017) 114-120.

Development of a CH₄ dehydroaromatization-catalyst regeneration fluidized bed system

Development of a CH₄ dehydroaromatization-catalyst regeneration fluidized bed system

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