Enhanced stability of Fe-modified CuO-ZnO-ZrO2-Al2O3/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO2 hydrogenation

doi:10.1016/j.cjche.2020.11.031

Chinese Journal of Chemical Engineering ›› 2021, Vol. 38 ›› Issue (10): 106-113.DOI: 10.1016/j.cjche.2020.11.031

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

Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation

Xiao Fan¹, Shoujie Ren¹, Baitang Jin¹, Shiguang Li², Miao Yu³, Xinhua Liang¹

1. Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology, Rolla, MO 65409, United States;
2. Gas Technology Institute, 1700 South Mount Prospect Road, Des Plaines, IL 60018, United States;
3. Department of Chemical and Biological Engineering, Rensselaer Polytechnic Institute, Troy, NY 12180, United States

Received:2020-07-08 Revised:2020-10-26 Online:2021-12-02 Published:2021-10-28
Contact: Xinhua Liang
Supported by:
This work was supported by the U.S. Department of Energy through contract DE-AR0000806. We thank DOE ARPA-E Project Director, Dr. Grigorii Soloveichik, for his assistance and support.

Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation

Xiao Fan¹, Shoujie Ren¹, Baitang Jin¹, Shiguang Li², Miao Yu³, Xinhua Liang¹

1. Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology, Rolla, MO 65409, United States;
2. Gas Technology Institute, 1700 South Mount Prospect Road, Des Plaines, IL 60018, United States;
3. Department of Chemical and Biological Engineering, Rensselaer Polytechnic Institute, Troy, NY 12180, United States

通讯作者: Xinhua Liang
基金资助:
This work was supported by the U.S. Department of Energy through contract DE-AR0000806. We thank DOE ARPA-E Project Director, Dr. Grigorii Soloveichik, for his assistance and support.

Abstract

Abstract: A series of iron (Fe) modified CuO-ZnO-ZrO₂-Al₂O₃ (CZZA) catalysts, with various Fe loadings, were prepared using a co-precipitation method. A bifunctional catalyst, consisting of Fe-modified CZZA and HZSM-5, was studied for dimethyl ether (DME) synthesis via CO₂ hydrogenation. The effects of Fe loading, reaction temperature, reaction pressure, space velocity, and concentrations of precursor for the synthesis of the Fe-modified CZZA catalyst on the catalytic activity of DME synthesis were investigated. Long-term stability tests showed that Fe modification of the CZZA catalyst improved the catalyst stability for DME synthesis via CO₂ hydrogenation. The activity loss, in terms of DME yield, was significantly reduced from 4.2% to 1.4% in a 100 h run of reaction, when the Fe loading amount was 0.5 (molar ratio of Fe to Cu). An analysis of hydrogen temperature programmed reduction revealed that the introduction of Fe improved the reducibility of the catalysts, due to assisted adsorption of H₂ on iron oxide. The good stability of Fe-modified CZZA catalysts in the DME formation was most likely attributed to oxygen spillover that was introduced by the addition of iron oxide. This could have inhibited the oxidation of the Cu surface and enhanced the thermal stability of copper during long-term reactions.

Key words: CO₂ hydrogenation, Cu-ZnO based catalyst, Iron (Fe), Dimethyl ether (DME), Stability

摘要： A series of iron (Fe) modified CuO-ZnO-ZrO₂-Al₂O₃ (CZZA) catalysts, with various Fe loadings, were prepared using a co-precipitation method. A bifunctional catalyst, consisting of Fe-modified CZZA and HZSM-5, was studied for dimethyl ether (DME) synthesis via CO₂ hydrogenation. The effects of Fe loading, reaction temperature, reaction pressure, space velocity, and concentrations of precursor for the synthesis of the Fe-modified CZZA catalyst on the catalytic activity of DME synthesis were investigated. Long-term stability tests showed that Fe modification of the CZZA catalyst improved the catalyst stability for DME synthesis via CO₂ hydrogenation. The activity loss, in terms of DME yield, was significantly reduced from 4.2% to 1.4% in a 100 h run of reaction, when the Fe loading amount was 0.5 (molar ratio of Fe to Cu). An analysis of hydrogen temperature programmed reduction revealed that the introduction of Fe improved the reducibility of the catalysts, due to assisted adsorption of H₂ on iron oxide. The good stability of Fe-modified CZZA catalysts in the DME formation was most likely attributed to oxygen spillover that was introduced by the addition of iron oxide. This could have inhibited the oxidation of the Cu surface and enhanced the thermal stability of copper during long-term reactions.

关键词: CO₂ hydrogenation, Cu-ZnO based catalyst, Iron (Fe), Dimethyl ether (DME), Stability

Xiao Fan, Shoujie Ren, Baitang Jin, Shiguang Li, Miao Yu, Xinhua Liang. Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation[J]. Chinese Journal of Chemical Engineering, 2021, 38(10): 106-113.

References

[1] A. Ateka, P. Pérez-Uriarte, M. Gamero, J. Ereña, A.T. Aguayo, J. Bilbao, A comparative thermodynamic study on the CO₂ conversion in the synthesis of methanol and of DME, Energy 120 (2017) 796-804
[2] G. Bonura, M. Cordaro, L. Spadaro, C. Cannilla, F. Arena, F. Frusteri, Hybrid Cu-ZnO-ZrO₂/H-ZSM5 system for the direct synthesis of DME by CO₂ hydrogenation, Appl. Catal. B 140-141 (2013) 16-24
[3] S.P. Naik, T. Ryu, V. Bui, J.D. Miller, N.B. Drinnan, W. Zmierczak, Synthesis of DME from CO₂/H₂ gas mixture, Chem. Eng. J. 167 (2011) 362-368
[4] G. Leonzio, State of art and perspectives about the production of methanol, dimethyl ether and syngas by carbon dioxide hydrogenation, J. CO 27 (2018) 326-354
[5] M. Martín, Optimal year-round production of DME from CO₂ and water using renewable energy, J. CO 13 (2016) 105-113
[6] S. Ren, S. Li, N. Klinghoffer, M. Yu, X. Liang, Effects of mixing methods of bifunctional catalysts on catalyst stability of DME synthesis via CO₂ hydrogenation, Carbon Resources Conversion 2 (2019) 85-94
[7] A. García-Trenco, A. Martínez, Direct synthesis of DME from syngas on hybrid CuZnAl/ZSM-5 catalysts: New insights into the role of zeolite acidity, Appl. Catal. A 411-412 (2012) 170-179
[8] Y. Tan, H. Xie, H. Cui, Y. Han, B. Zhong, Modification of Cu-based methanol synthesis catalyst for dimethyl ether synthesis from syngas in slurry phase, Catal. Today 104 (2005) 25-29
[9] A. Venugopal, J. Palgunadi, J.K. Deog, O. Joo, C. Shin, Dimethyl ether synthesis on the admixed catalysts of Cu-Zn-Al-M (M=Ga, La, Y, Zr) and γ-Al₂O₃: The role of modifier, J. Mol. Catal. A: Chem. 302 (2009) 20-27
[10] S. Ren, W.R. Shoemaker, X. Wang, Z. Shang, N. Klinghoffer, S. Li, M. Yu, X. He, T.A. White, X. Liang, Highly active and selective Cu-ZnO based catalyst for methanol and dimethyl ether synthesis via CO₂ hydrogenation, Fuel 239 (2019) 1125-1133
[11] J. Sun, G. Yang, Y. Yoneyama, N. Tsubaki, Catalysis chemistry of dimethyl ether synthesis, ACS Catal. 4 (2014) 3346-3356
[12] J.T. Sun, I.S. Metcalfe, M. Sahibzada, Deactivation of Cu/ZnO/Al₂O₃ methanol synthesis catalyst by sintering, Ind. Eng. Chem. Res. 38 (1999) 3868-3872
[13] M. Kurtz, H. Wilmer, T. Genger, O. Hinrichsen, M. Muhler, Deactivation of supported copper catalysts for methanol synthesis, Catal. Lett. 86 (2003) 77-80
[14] G.R. Moradi, M. Nazari, F. Yaripour, The interaction effects of dehydration function on catalytic performance and properties of hybrid catalysts upon LPDME process, Fuel Process. Technol. 89 (2008) 1287-1296
[15] Y. Wang, W. Gao, K. Li, Y. Zheng, Z. Xie, W. Na, J.G. Chen, H. Wang, Strong evidence of the role of H₂O in affecting methanol selectivity from CO₂ hydrogenation over Cu-ZnO-ZrO₂, Chem 6 (2020) 419-430
[16] J. Cao, Y. Wang, X. Yu, S. Wang, S. Wu, Z. Yuan, Mesoporous CuO-Fe₂O₃ composite catalysts for low-temperature carbon monoxide oxidation, Appl. Catal. B 79 (2008) 26-34
[17] R. Liu, Z. Qin, H. Ji, T. Su, Synthesis of dimethyl ether from CO₂ and H₂ using a Cu-Fe-Zr/HZSM-5 catalyst system, Ind. Eng. Chem. Res. 52 (2013) 16648-16655
[18] Y. Zhou, S. Wang, M. Xiao, D. Han, Y. Lu, Y. Meng, Novel Cu-Fe bimetal catalyst for the formation of dimethyl carbonate from carbon dioxide and methanol, RSC Adv. 2 (2012) 6831-6837
[19] K. Sirichaiprasert, A. Luengnaruemitchai, S. Pongstabodee, Selective oxidation of CO to CO₂ over Cu-Ce-Fe-O composite-oxide catalyst in hydrogen feed stream, Int. J. Hydrogen Energy 32 (2007) 915-926
[20] X. Zhou, T. Su, Y. Jiang, Z. Qin, H. Ji, Z. Guo, CuO-Fe₂O₃-CeO₂/HZSM-5 bifunctional catalyst hydrogenated CO₂ for enhanced dimethyl ether synthesis, Chem. Eng. Sci. 153 (2016) 10-20
[21] S. Ren, X. Fan, Z. Shang, W.R. Shoemaker, L. Ma, T. Wu, S. Li, N.B. Klinghoffer, M. Yu, X. Liang, Enhanced catalytic performance of Zr modified CuO/ZnO/Al₂O₃ catalyst for methanol and DME synthesis via CO₂ hydrogenation, J. CO 36 (2020) 82-95
[22] Y. Kanai, T. Watanabe, T. Fujitani, T. Uchijima, J. Nakamura, The synergy between Cu and ZnO in methanol synthesis catalysts, Catal. Lett. 38 (1996) 157-163
[23] R. van den Berg, G. Prieto, G. Korpershoek, L.I. van der Wal, A.J. van Bunningen, S. Laegsgaard-Jorgensen, P.E. de Jongh, K.P. de Jong, Structure sensitivity of Cu and CuZn catalysts relevant to industrial methanol synthesis, Nat. Commun. 7 (2016) 13057
[24] M. Gentzen, W. Habicht, D.E. Doronkin, J.D. Grunwaldt, J. Sauer, S. Behrens, Bifunctional hybrid catalysts derived from Cu/Zn-based nanoparticles for single-step dimethyl ether synthesis, Catal. Sci. Technol. 6 (2016) 1054-1063
[25] S.A. Kondrat, P.J. Smith, L. Lu, J.K. Bartley, S.H. Taylor, M.S. Spencer, G.J. Kelly, C.W. Park, C.J. Kiely, G.J. Hutchings, Preparation of a highly active ternary Cu-Zn-Al oxide methanol synthesis catalyst by supercritical CO₂ anti-solvent precipitation, Catal. Today 317 (2018) 12-20
[26] S. Kattel, P. Ramírez, J. Chen, J. Rodriguez, P. Liu, Active sites for CO₂ hydrogenation to methanol on Cu/ZnO catalysts, Science 355 (2017) 1296-1299
[27] C. Chen, Study of iron-promoted Cu/SiO₂ catalyst on high temperature reverse water gas shift reaction, Appl. Catal. A 257 (2004) 97-106
[28] H. Ban, C. Li, K. Asami, K. Fujimoto, Influence of rare-earth elements (La, Ce, Nd and Pr) on the performance of Cu/Zn/Zr catalyst for CH₃OH synthesis from CO₂, Catal. Commun. 54 (2014) 50-54
[29] S. Kiatphuengporn, P. Jantaratana, J. Limtrakul, M. Chareonpanich, Magnetic field-enhanced catalytic CO₂ hydrogenation and selective conversion to light hydrocarbons over Fe/MCM-41 catalysts, Chem. Eng. J. 306 (2016) 866-875
[30] B. Hu, Y. Yin, G. Liu, S. Chen, X. Hong, S.C.E. Tsang, Hydrogen spillover enabled active Cu sites for methanol synthesis from CO₂ hydrogenation over Pd doped CuZn catalysts, J. Catal. 359 (2018) 17-26
[31] I. Abbas, H. Kim, C.-H. Shin, S. Yoon, K.-D. Jung, Differences in bifunctionality of ZnO and ZrO₂ in Cu/ZnO/ZrO₂/Al₂O₃ catalysts in hydrogenation of carbon oxides for methanol synthesis, Appl. Catal. B 258 (2019) 117971
[32] K. Mondal, H. Lorethova, E. Hippo, T. Wiltowski, S.B. Lalvani, Reduction of iron oxide in carbon monoxide atmosphere-reaction controlled kinetics, Fuel Process. Technol. 86 (2004) 33-47
[33] G. Zhao, J. Li, X. Niu, K. Tang, S. Wang, W. Zhu, X. Ma, M. Ru, Y. Yang, Facile synthesis of Mn-doped Fe₂O₃ nanostructures: Enhanced CO catalytic performance induced by manganese doping, New J. Chem. 40 (2016) 3491-3498
[34] D. Martin, D. Duprez, Mobility of surface species on oxides. 1. Isotopic exchange of ¹⁸O₂ with ¹⁶O of SiO₂, Al₂O₃, ZrO₂, MgO, CeO₂, and CeO₂-Al₂O₃. Activation by noble metals. Correlation with oxide basicity, J. Phys. Chem. 100 (1996) 9429-9438
[35] Z. Liu, Y. Liu, B. Chen, T. Zhu, L. Ma, Novel Fe-Ce-Ti catalyst with remarkable performance for the selective catalytic reduction of NOnull by NH₃, Catal. Sci. Technol. 6 (2016) 6688-6696
[36] A.M. Abdel-Mageed, A. Klyushin, A. Knop-Gericke, R. Schlogl, R.J. Behm, Influence of CO on the activation, O-vacancy formation, and performance of Au/ZnO catalysts in CO₂ hydrogenation to methanol, J. Phys. Chem. Lett. 10 (2019) 3645-3653
[37] A. Alvarez, A. Bansode, A. Urakawa, A.V. Bavykina, T.A. Wezendonk, M. Makkee, J. Gascon, F. Kapteijn, Challenges in the greener production of formates/formic acid, methanol, and DME by heterogeneously catalyzed CO₂ hydrogenation processes, Chem. Rev. 117 (2017) 9804-9838
[38] E. Catizzone, G. Bonura, M. Migliori, F. Frusteri, G. Giordano, CO₂ recycling to dimethyl ether: State-of-the-art and perspectives, Molecules 23 (2017) 31
[39] S. Dang, H. Yang, P. Gao, H. Wang, X. Li, W. Wei, Y. Sun, A review of research progress on heterogeneous catalysts for methanol synthesis from carbon dioxide hydrogenation, Catal. Today 330 (2019) 61-75
[40] A. Xin, Z. YiZan, Z. Qiang, W. Dezheng, W. Jinfu, Dimethyl ether synthesis from CO₂ hydrogenation on a CuO-ZnO-Al₂O₃-ZrO₂/HZSM-5 bifunctional catalyst, Ind. Eng. Chem. Res. 47 (2008) 6547-6554
[41] W. Chen, B. Lin, H. Lee, M. Huang, One-step synthesis of dimethyl ether from the gas mixture containing CO₂ with high space velocity, Appl. Energy 98 (2012) 92-101
[42] F. Frusteri, G. Bonura, C. Cannilla, G. Drago Ferrante, A. Aloise, E. Catizzone, M. Migliori, G. Giordano, Stepwise tuning of metal-oxide and acid sites of CuZnZr-MFI hybrid catalysts for the direct DME synthesis by CO₂ hydrogenation, Appl. Catal. B 176-177 (2015) 522-531
[43] G. Moradi, J. Ahmadpour, M. Nazari, F. Yaripour, Effects of feed composition and space velocity on direct synthesis of dimethyl ether from syngas, Ind. Eng. Chem. Res. 47 (2008) 7672-7679
[44] B. Liang, J. Ma, X. Su, C. Yang, H. Duan, H. Zhou, S. Deng, L. Li, Y. Huang, Investigation on deactivation of Cu/ZnO/Al₂O₃ catalyst for CO₂ hydrogenation to methanol, Ind. Eng. Chem. Res. 58 (2019) 9030-9037
[45] A. Ruiz Puigdollers, P. Schlexer, S. Tosoni, G. Pacchioni, Increasing oxide reducibility: The role of metal/oxide interfaces in the formation of oxygen vacancies, ACS Catal. 7 (2017) 6493-6513
[46] J.M. López, A.L. Gilbank, T. García, B. Solsona, S. Agouram, L. Torrente-Murciano, The prevalence of surface oxygen vacancies over the mobility of bulk oxygen in nanostructured ceria for the total toluene oxidation, Appl. Catal. B 174-175 (2015) 403-412
[47] J.S. Hayward, P.J. Smith, S.A. Kondrat, M. Bowker, G.J. Hutchings, The effects of secondary oxides on copper-based catalysts for green methanol synthesis, ChemCatChem 9 (2017) 1655-1662

Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation

Enhanced stability of Fe-modified CuO-ZnO-ZrO₂-Al₂O₃/HZSM-5 bifunctional catalysts for dimethyl ether synthesis from CO₂ hydrogenation

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