Co-Cr-O mixed oxides for low-temperature total oxidation of propane: Structural effects, kinetics, and spectroscopic investigation

doi:10.1016/S1872-2067(19)63480-7

Abstract

Abstract: A series of Co-Cr-O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane. The reaction behaviors are closely related to the structural features of the mixed oxides. The catalyst with a Co/Cr molar ratio of 1:2 (1Co2Cr) and a spinel structure has the best activity (with a reaction rate of 1.38 μmol g^-1 s^-1 at 250℃), which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility, as evidenced by the temperature-programmed desorption of ammonia, reduction of hydrogen, and surface reaction of propane. Kinetic study shows that the reaction orders of propane and oxygen on the 1Co2Cr catalyst (0.58 ± 0.03 and 0.34 ±0.05, respectively) are lower than those on the 2Co1Cr catalyst (0.77 ±0.02 and 0.98 ±0.16, respectively) and 1Co5Cr (0.66 ±0.05 and 1.30 ±0.11, respectively), indicating that the coverages of propane and oxygen on 1Co2Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility. In addition, in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1Co2Cr during the reaction are polydentate carbonate species, which accumulate on the surface at low temperatures (< 250℃) but decompose at relatively high temperatures.

Key words: Propane combustion, Co-Cr mixed oxides, Reducibility, Surface acidity, Kinetics

CLC Number:

Wen-Min Liao, Pei-Pei Zhao, Bing-Heng Cen, Ai-Ping Jia, Ji-Qing Lu, Meng-Fei Luo. Co-Cr-O mixed oxides for low-temperature total oxidation of propane: Structural effects, kinetics, and spectroscopic investigation[J]. Chinese Journal of Catalysis, 2020, 41(3): 442-453.

×
share this article

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(19)63480-7

https://www.cjcatal.com/EN/Y2020/V41/I3/442

References

[1] T. Garcia, B. Solsona, D. M. Murphy, K. L. Antcliff, S. H. Taylor, J. Catal., 2005, 229, 1-11.
[2] M. N. Taylor, W. Zhou, T. Garcia, B. Solsona, A. F. Carley, C. J. Kiely, S. H. Taylor, J. Catal., 2012, 285, 103-114.
[3] L. Meng, J. J. Lin, Z. Y. Pu, L. F. Luo, A. P. Jia, W. X. Huang, M. F. Luo, J. Q. Lu, Appl. Catal. B:Environ., 2012, 119-120, 117-122.
[4] Y. R. Liu, X. Li, W. M. Liao, A. P. Jia, Y. J. Wang, M. F. Luo, J. Q. Lu, ACS Catal., 2019, 9, 1472-1481.
[5] J. Okal, M. Zawadzki, Appl. Catal. B:Environ., 2011, 105, 182-190.
[6] O. Sanz, J. J. Delgado, P. Navarro, G. Arzamendi, L. M. Gandia, M. Montes, Appl. Catal. B:Environ., 2011, 110, 231-237.
[7] Z. Hu, X. F. Liu, D. M. Meng, Y. Guo, Y. L. Guo, G. Z. Lu, ACS Catal., 2016, 6, 2265-2279.
[8] M. S. Avila, C. I. Vignatti, C. R. Apesteguia, T. F. Garetto, Chem. Eng. J., 2014, 241, 52-59.
[9] T. Garcia, S. Agouram, S.H. Taylor, D. Morgan, A. Dejoz, I. Vazquez, B. Solsona, Catal. Today, 2015, 254, 12-20.
[10] X. Li, Y. R. Liu, W. M. Liao, A. P. Jia, Y. J. Wang, J. Q. Lu, M. F. Luo, Appl. Surf. Sci., 2019, 475, 524-531.
[11] B. Solsona, T. Garcia, S. Agouram, G. J. Hutchings, S. H. Taylor, Appl. Catal. B:Environ., 2011, 101, 388-396.
[12] J. Y. Luo, M. Meng, Y. Q. Zha, L. H. Guo, J. Phys. Chem. C, 2008, 112, 8694-8701.
[13] M. Baldi, E. Finocchio, F. Milella, G. Busca, Appl. Catal. B:Envi-ron., 1998, 16, 43-51.
[14] Z. Z. Zhu, G. Z. Lu, Z. G. Zhang, Y. Guo, Y. L. Guo, Y. Q. Wang, ACS Catal., 2013, 3, 1154-1164.
[15] G. Salek, P. Alphonse, P. Dufour, S. Guillemet-Fritsch, C. Te-nailleau, Appl. Catal. B:Environ., 2014, 147, 1-7.
[16] Z. Ren, Z. L. Wu, W. Q. Song, W. Xiao, Y. B. Guo, J. Ding, S. L. Suib, P. X. Gao, Appl. Catal. B:Environ., 2016, 180, 150-160.
[17] Z. Hu, S. Qiu, Y. You, Y. Guo, Y. L. Guo, L. Wang, W. C. Zhan, G. Z. Lu, Appl. Catal. B:Environ., 2018, 225, 110-120.
[18] R. P. Marin, S. A. Kondrat, R. K. Pinnell, T. E. Davies, S. Golunski, J. K. Bartley, G. J. Hutchings, S. H. Taylor, Appl. Catal. B:Environ., 2013, 140-141, 671-679.
[19] B. Solsona, T. E. Davies, T. Garcia, I. Vazquez, A. Dejoz, S. H. Taylor, Appl. Catal. B:Environ., 2008, 84, 176-184.
[20] B. Solsona, T. Garcia, R. Sanchis, M. D. Soriano, M. Moreno, E. Rodriguez-Castellon, S. Agouram, A. Dejoz, J. M. Lopez Nieto, Chem. Eng. J., 2016, 290, 273-281.
[21] B. Puertolas, A. Smith, I. Vazquez, A. Dejoz, A. Moragues, T. Garcia, B. Solsona, Chem. Eng. J., 2013, 229, 547-558.
[22] P. M. Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, J. Catal., 2010, 272, 109-120.
[23] B. Faure, P. Alphonse, Appl. Catal. B:Environ., 2016, 180, 715-725.
[24] J. Chen, X. Zhang, H. Arandiyan, Y. Peng, H. Chang, J. Li, Catal. To-day, 2013, 201, 12-18.
[25] Y. Wang, A. P. Jia, M. F. Luo, J. Q. Lu, Appl. Catal. B:Environ., 2015, 165, 477-486.
[26] J. D. Liu, T. T. Zhang, A. P. Jia, M. F. Luo, J. Q. Lu, Appl. Surf. Sci., 2016, 369, 58-66.
[27] H. Luo, X. Wu, D. Weng, S. Liu, R. Ran, Rare Metals., 2017, 36, 1-9.
[28] X. Wu, L. Zhang, D. Weng, S. Liu, Z. Si, J. Fan, J. Hazard. Mater., 2012, 225-226, 146-154.
[29] T. F. Garetto, E. Rincon, C. R. Apesteguia, Appl. Catal. B:Environ., 2004, 48, 167-174.
[30] P. Bracconi, L. C. Dufour, J. Phys. Chem., 1975, 79, 2400-2405.
[31] W. Tang, W. Xiao, S. Wang, Z. Ren, J. Ding, P. X. Gao, Appl. Catal. B:Environ., 2018, 226, 585-595.
[32] C. Suchomski, C. Reitz, K. Brezesinski, C. Tavares de Sousa, M. Rohne, K. Iimura, J. P. Esteves de Araujo, T. Brezesinki, Chem. Mater., 2011, 24, 155-165.
[33] J. Chen, W. Shi, S. Yang, H. Arandiyan, D. Li, J. Phys. Chem. C, 2011, 115, 17400-17408.
[34] R. H. Ma, P. J. Hu, L. Y. Jin, Y. J. Wang, J. Q. Lu, M. F. Luo, Catal. Today, 2011, 175, 598-602.
[35] J. W. Luo, J. D. Song, W. Z. Jia, Z. Y. Pu, J. Q. Lu, M. F. Luo, Appl. Surf. Sci., 2018, 433, 904-913.
[36] J. Chen, W. Shi, X. Zhang, h. Arandiyan, D. Li, J. Li, Environ. Sci. Technol., 2011, 45, 8491-8947.
[37] C. W. Tang, C. C. Kuo, M. C. Kuo, C. B. Wang, S. H. Chien, Appl. Catal. A:Gen., 2006, 309, 37-43.
[38] B. Bai, H. Arandiyan, J. Li, Appl. Catal. B:Environ., 2013, 142-143, 677-683.
[39] W. Zhang, F. Wu, J. Li, Z. You, Appl. Surf. Sci., 2017, 411, 136-143.
[40] C. A. Chagas, E. F. de Souza, R. L. Manfro, S. M. Landi, M. M. V. M. Souza, M. Schmal, Appl. Catal. B:Environ., 2016, 182, 257-265.
[41] Y. Luo, J. Zuo, X. Feng, Q. Qian, Y. Zheng. D. Lin, B. Huang, Q. Chen, Chem. Eng. J., 2019, 357, 395-403.
[42] X. Li, X. Li, X. Zeng, T. Zhu, Appl. Catal. A:Gen., 2019, 572, 61-70.
[43] L. F. Liotta, G. Di Carlo, G. Pantaleo, A. M. Venezia, G. Deganello, Appl. Catal. B:Environ., 2006, 66, 217-227.
[44] X. Wu, L. Zhang, D. Weng, S. Liu, Z. Si, J. Fan, J Hazard. Mater., 2012, 146, 225-226.
[45] C. F. Windisch, K. F. Ferris, G. J. Exarhos, S. K. Sharma, Thin Solid Films, 2002, 420-421, 89-99.
[46] D. C. Kim, S. K. Ihm, Environ. Sci. Technol., 2001, 35, 222-226.
[47] T. T. Zhang, J. D. Song, J. X. Chen, A. P. Jia, M. F. Luo, J. Q. Lu. Appl. Surf. Sci., 2017, 425, 1074-1081.
[48] M. P. Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, Appl. Catal. B:Environ., 2010, 95, 26-38.
[49] A. Urd?, A. Herraïz, Á. Rédey, I. C. Marcu, Catal. Commun., 2009, 10, 1651-1655.
[50] P. M. Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, Appl. Catal. B:Environ., 2009, 90, 295-306.
[51] V. Balcaen, H. Poelman, D. Poelman, G. B. Marin, J. Catal., 2011, 283(1), 75-88.
[52] O. Pozdnyakova, D. Teschner, A. Wootsch, J. Kröhnert, B. Stein-hauer, H. Sauer, L. Toth, F. C. Jentoft, A. Knop-Gericke, Z. Paál, R. Schlögl, J. Catal., 2006, 237(1), 17-28.
[53] E. M. Köck, M. Kogler, T. Bielz, B. Klötzer, S. Penner, J. Phys. Chem. C, 2013, 117, 17666-17673.Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, J. Catal., 2010, 272, 109-120.
[23] B. Faure, P. Alphonse, Appl. Catal. B:Environ., 2016, 180, 715-725.
[24] J. Chen, X. Zhang, H. Arandiyan, Y. Peng, H. Chang, J. Li, Catal. To-day, 2013, 201, 12-18.
[25] Y. Wang, A. P. Jia, M. F. Luo, J. Q. Lu, Appl. Catal. B:Environ., 2015, 165, 477-486.
[26] J. D. Liu, T. T. Zhang, A. P. Jia, M. F. Luo, J. Q. Lu, Appl. Surf. Sci., 2016, 369, 58-66.
[27] H. Luo, X. Wu, D. Weng, S. Liu, R. Ran, Rare Metals., 2017, 36, 1-9.
[28] X. Wu, L. Zhang, D. Weng, S. Liu, Z. Si, J. Fan, J. Hazard. Mater., 2012, 225-226, 146-154.
[29] T. F. Garetto, E. Rincon, C. R. Apesteguia, Appl. Catal. B:Environ., 2004, 48, 167-174.
[30] P. Bracconi, L. C. Dufour, J. Phys. Chem., 1975, 79, 2400-2405.
[31] W. Tang, W. Xiao, S. Wang, Z. Ren, J. Ding, P. X. Gao, Appl. Catal. B:Environ., 2018, 226, 585-595.
[32] C. Suchomski, C. Reitz, K. Brezesinski, C. Tavares de Sousa, M. Rohne, K. Iimura, J. P. Esteves de Araujo, T. Brezesinki, Chem. Mater., 2011, 24, 155-165.
[33] J. Chen, W. Shi, S. Yang, H. Arandiyan, D. Li, J. Phys. Chem. C, 2011, 115, 17400-17408.
[34] R. H. Ma, P. J. Hu, L. Y. Jin, Y. J. Wang, J. Q. Lu, M. F. Luo, Catal. Today, 2011, 175, 598-602.
[35] J. W. Luo, J. D. Song, W. Z. Jia, Z. Y. Pu, J. Q. Lu, M. F. Luo, Appl. Surf. Sci., 2018, 433, 904-913.
[36] J. Chen, W. Shi, X. Zhang, h. Arandiyan, D. Li, J. Li, Environ. Sci. Technol., 2011, 45, 8491-8947.
[37] C. W. Tang, C. C. Kuo, M. C. Kuo, C. B. Wang, S. H. Chien, Appl. Catal. A:Gen., 2006, 309, 37-43.
[38] B. Bai, H. Arandiyan, J. Li, Appl. Catal. B:Environ., 2013, 142-143, 677-683.
[39] W. Zhang, F. Wu, J. Li, Z. You, Appl. Surf. Sci., 2017, 411, 136-143.
[40] C. A. Chagas, E. F. de Souza, R. L. Manfro, S. M. Landi, M. M. V. M. Souza, M. Schmal, Appl. Catal. B:Environ., 2016, 182, 257-265.
[41] Y. Luo, J. Zuo, X. Feng, Q. Qian, Y. Zheng. D. Lin, B. Huang, Q. Chen, Chem. Eng. J., 2019, 357, 395-403.
[42] X. Li, X. Li, X. Zeng, T. Zhu, Appl. Catal. A:Gen., 2019, 572, 61-70.
[43] L. F. Liotta, G. Di Carlo, G. Pantaleo, A. M. Venezia, G. Deganello, Appl. Catal. B:Environ., 2006, 66, 217-227.
[44] X. Wu, L. Zhang, D. Weng, S. Liu, Z. Si, J. Fan, J Hazard. Mater., 2012, 146, 225-226.
[45] C. F. Windisch, K. F. Ferris, G. J. Exarhos, S. K. Sharma, Thin Solid Films, 2002, 420-421, 89-99.
[46] D. C. Kim, S. K. Ihm, Environ. Sci. Technol., 2001, 35, 222-226.
[47] T. T. Zhang, J. D. Song, J. X. Chen, A. P. Jia, M. F. Luo, J. Q. Lu. Appl. Surf. Sci., 2017, 425, 1074-1081.
[48] M. P. Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, Appl. Catal. B:Environ., 2010, 95, 26-38.
[49] A. Urd?, A. Herraïz, Á. Rédey, I. C. Marcu, Catal. Commun., 2009, 10, 1651-1655.
[50] P. M. Heynderickx, J. W. Thybaut, H. Poelman, D. Poelman, G. B. Marin, Appl. Catal. B:Environ., 2009, 90, 295-306.
[51] V. Balcaen, H. Poelman, D. Poelman, G. B. Marin, J. Catal., 2011, 283(1), 75-88.
[52] O. Pozdnyakova, D. Teschner, A. Wootsch, J. Kröhnert, B. Stein-hauer, H. Sauer, L. Toth, F. C. Jentoft, A. Knop-Gericke, Z. Paál, R. Schlögl, J. Catal., 2006, 237(1), 17-28.
[53] E. M. Ko?ck, M. Kogler, T. Bielz, B. Klo?tzer, S. Penner, J. Phys. Chem. C, 2013, 117, 17666-17673.