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Direct synthesis of Cu-containing Beta zeolite without template for selective oxidation of cyclohexane

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Abstract

Cu-containing Beta zeolites (Cu-Beta) are straightforwardly synthesized in a one-pot method without template, where the crucial step is the co-hydrolysis/condensation of silica source and copper salt at the moderate acidic condition. In the solvent-free oxidation of cyclohexane with molecular oxygen (O2), the best cyclohexane conversion result (9.7%) with a KA-oil (cyclohexanone and cyclohexanol) selectivity of 94.1% is obtained over Cu-Beta(100). Structure—activity relationship analysis indicates that the isolated tetrahedral framework Cu2+ species and chemisorption oxygen species in high concentration on the catalyst surface enhannce the catalic performance. In addition, the catalyst can be easily separated and still remain stable after recycling five times, providing new insights into catalysts design for the catalytic oxidation of cyclohexane to KA-oil.

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References

  1. D. Yang, T. Wu, C. Chen, W. Guo, H. Liu, B. Han, Green. Chem. 19, 311 (2017)

    Article  CAS  Google Scholar 

  2. C. Xu, L. Jin, X. Wang, Y. Chen, L. Dai, Carbon 160, 287 (2020)

    Article  CAS  Google Scholar 

  3. D. Contreras, V. Melin, K. Márquez, G. Pérez-González, H.D. Mansilla, G. Pecchi, A. Henriquez, Appl. Catal. B 251, 17 (2019)

    Article  CAS  Google Scholar 

  4. M. Rezaei, A.N. Chermahini, H.A. Dabbagh, Chem. Eng. J. 31, 515 (2017)

    Article  Google Scholar 

  5. R. Jevtic, P.A. Ramachandran, M.P. Dudukovic, Ind. Eng. Chem. Res. 48, 7986 (2009)

    Article  CAS  Google Scholar 

  6. K.J. Betsy, C. Nayak, A. Lazar, A. Krishnan, D. Bhattacharyya, S.N. Jha, C.P. Vinod, ChemCatChem 10, 3291 (2018)

    Article  CAS  Google Scholar 

  7. F. Recupero, C. Punta, Chem. Rev. 107, 3800 (2007)

    Article  CAS  PubMed  Google Scholar 

  8. P. Wu, P. Bai, Z. Yan, G.X.S. Zhao, Sci. Rep. 6, 1 (2016)

    Article  Google Scholar 

  9. Y. Liu, H. Tsunoyama, T. Akita, S. Xie, T. Tsukuda, ACS Catal. 1, 2 (2011)

    Article  CAS  Google Scholar 

  10. N. Pal, M. Pramanik, A. Bhaumik, M. Ali, J. Mol. Catal. A 392, 299 (2014)

    Article  CAS  Google Scholar 

  11. P. Zhang, H. Lu, Y. Zhou, L. Zhang, Z. Wu, S. Yang, H. Shi, Q. Zhu, Y. Chen, S. Dai, Nat. Commun. 6, 1 (2015)

    Google Scholar 

  12. P.T. Huong, B.K. Lee, J. Kim, C.H. Lee, Mater. Design. 101, 210 (2014)

    Article  Google Scholar 

  13. X. Yang, L. Wang, T. Lu, B. Gao, Y. Su, L. Zhou, Catal Sci. Technol. 10, 8437 (2020)

    Article  CAS  Google Scholar 

  14. V. Van Speybroeck, K. Hemelsoet, L. Joos, M. Waroquier, R.G. Bell, C.R.A. Catlow, Chem. Soc. Rev. 44, 7044 (2015)

    Article  PubMed  Google Scholar 

  15. Z. Wu, Z. He, Y. Xu, J. Wang, X. Lu, Q. Xia, D. Zhou, J. Porous Mater. 28, 1041 (2021)

    Article  CAS  Google Scholar 

  16. A.W. Petrov, D. Ferri, O. Kröcher, J.A. van Bokhoven, ACS. Catal. 9, 2303 (2019)

    Article  CAS  Google Scholar 

  17. A. Koishybay, D.F. Shantz, J. Am. Chem. Soc. 142, 11962 (2020)

    Article  CAS  PubMed  Google Scholar 

  18. Z. Jin, L. Wang, E. Zuidema, K. Mondal, M. Zhang, J. Zhang, C. Wang, X. Meng, H. Yang, C. Mesters, F.S. Xiao, Science 367, 193 (2020)

    Article  CAS  PubMed  Google Scholar 

  19. X. Xing, N. Li, J. Cheng, Y. Sun, Z. Zhang, X. Zhang, Z. Hao, J. Environ. Sci. 96, 55 (2020)

    Article  Google Scholar 

  20. S. Chen, Z. Shao, Z. Fang, Q. Chen, T. Tang, W. Fu, L. Zhang, T. Tang, J. Catal. 338, 38 (2016)

    Article  CAS  Google Scholar 

  21. E. Ivashkina, E. Khlebnikova, I. Dolganova, I. Dolganov, L.A. Khroyan, Ind. Eng. Chem. Res. 59, 14537 (2020)

    Article  CAS  Google Scholar 

  22. E. Dumitriu, V. Hulea, J. Catal. 218, 249 (2003)

    Article  CAS  Google Scholar 

  23. P. Losch, J.F. Kolb, A. Astafan, T.J. Daou, L. Pinard, P. Pale, B. Louis, Green Chem. 18, 4714 (2016)

    Article  CAS  Google Scholar 

  24. Y. Zhao, B. Choi, D. Kim, Chem. Eng. Sci. 164, 258 (2017)

    Article  CAS  Google Scholar 

  25. Q. Zhao, B. Chen, B. Zou, L. Yu, C. Shi, Catal Sci. Technol. 11, 646 (2021)

    Article  CAS  Google Scholar 

  26. N.E.U.S. Blanch-Raga, A.E. Palomares, J. Martínez-Triguero, S. Valencia, Appl. Catal. B 187, 90 (2016)

    Article  CAS  Google Scholar 

  27. W. Zhang, W. Hou, T. Meng, W. Zhuang, J. Xie, Y. Zhou, J. Wang, Catal Sci. Technol. 7, 6050 (2017)

    Article  CAS  Google Scholar 

  28. S. Zhang, T. Lv, Z. Feng, F. Wang, X. Liu, W. Wang, Y. Wang, C. Meng, Micropor. Mesopor. Mater. 278, 81 (2019)

    Article  CAS  Google Scholar 

  29. Y. Luo, Y. Zhu, J. Pan, X. Chen, Green Chem. 22, 1681 (2020)

    Article  CAS  Google Scholar 

  30. Y. Wu, J. Wang, W. Zhang, J. Gu, X. Wang, J. Am. Chem. Soc. 132, 17989 (2010)

    Article  CAS  PubMed  Google Scholar 

  31. E.A. Eilertsen, M. Haouas, A.B. Pinar, N.D. Hould, R.F. Lobo, K.P. Lillerud, F. Taulelle, Chem. Mater. 24, 571 (2012)

    Article  CAS  Google Scholar 

  32. S.V. Konnov, F. Dubray, E.B. Clatworthy, C. Kouvatas, J.P. Gilson, J.P. Dath, D. Minoux, C. Aquino, V. Valtchev, S. Moldovan, S. Koneti, N. Nesterenko, S. Mintova, Angew. Chem. Int. Ed. 59, 19553 (2020)

    Article  CAS  Google Scholar 

  33. H.V. Doan, K.M. Leung, V.P. Ting, A. Sartbaeva, CrystEngComm 23, 857 (2021)

    Article  CAS  Google Scholar 

  34. C.M. Chanquia, K. Sapag, E. Rodriguez-Castellon, E.R. Herrero, G.A. Eimer, J. Phys. Chem. C 114, 1481 (2010)

    Article  CAS  Google Scholar 

  35. A.L. Villa, C.A. Caro, C.M. de Correa, J. Mol. Catal. A 228, 233 (2005)

    Article  CAS  Google Scholar 

  36. L. Guo, S. Ming, S. Zhang, Q. Liu, L. Pang, P. Liu, Z. Chen, T. Li, Ind. Eng. Chem. Res. 59, 21275 (2020)

    Article  CAS  Google Scholar 

  37. T. Muñoz, A.M. Prakash, L. Kevan, K.J. Balkus, J. Phys. Chem. B 102, 1379 (1998)

    Article  Google Scholar 

  38. Q. Ke, M. Wu, H. Yu, G. Lu, ChemCatChem 9, 733 (2017)

    Article  CAS  Google Scholar 

  39. J. Wei, T. Wang, X. Cao, H. Liu, X. Tang, Y. Sun, X. Zeng, T. Lei, S.L. Liu, Appl. Catal. B 258, 117793 (2019)

    Article  CAS  Google Scholar 

  40. X. Zhou, H. Chen, G. Zhang, J. Wang, Z. Xie, Z. Hua, L. Zhang, J. Shi, J. Mater. Chem. A 3, 9745 (2015)

    Article  CAS  Google Scholar 

  41. B. Pereda-Ayo, U. De La Torre, M.J. Illán-Gómez, A. Bueno-López, J.R. González-Velasco, Appl. Catal. B 147, 420 (2014)

    Article  CAS  Google Scholar 

  42. V.I. Pârvulescu, P. Grange, B. Delmon, Appl. Catal. B 33, 223 (2001)

    Article  Google Scholar 

  43. J.F. Xu, W. Ji, Z.X. Shen, S.H. Tang, X.R. Ye, D.Z. Jia, X.Q. Xin, J. Solid State Chem. 147, 516 (1999)

    Article  CAS  Google Scholar 

  44. P. Sun, R. Guo, S. Liu, S. Wang, W. Pan, M. Li, Appl. Catal. A 531, 129 (2017)

    Article  CAS  Google Scholar 

  45. Z. Lian, F. Liu, H. He, X. Shi, J. Mo, Z. Wu, Chem. Eng. J. 250, 390 (2014)

    Article  CAS  Google Scholar 

  46. E. Muhumuza, P. Wu, T. Nan, L. Zhao, P. Bai, S. Mintova, Z. Yan, Ind. Eng. Chem. Res. 59, 21322 (2020)

    Article  CAS  Google Scholar 

  47. I. Graça, D. Chadwick, Micropor. Mesopor. Mater. 294, 109873 (2020)

    Article  Google Scholar 

  48. C. Xie, W. Wang, Y. Yang, L. Jiang, Y. Chen, J. He, J. Wang, Mol. Catal. 495, 111134 (2020)

    Article  CAS  Google Scholar 

  49. C. Pang, J. Xiong, G. Li, C. Hu, J. Catal. 366, 37 (2018)

    Article  CAS  Google Scholar 

Download references

Acknowledgements

The authors thank the National Natural Science Foundation of China (No. 21802008), Natural Science Foundation of Jiangsu Province (No. BK20170661), Science and Technology Foundation of Changzhou (No. CJ20200042), Natural Science Foundation of Changzhou Institute of Technology (No. YN18040) and 2019 Support Program for Young Scholars of Changzhou Institute of Technology (No. A3-3008-19-009).

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Authors and Affiliations

  1. Research Center of Resources and Environment, School of Chemical Engineering and Materials, Changzhou Institute of Technology, Changzhou, 213032, Jiangsu, People’s Republic of China

    Wei Zhang, Haonan Xue, Min Wang, Zeying Wu, Linlin Ding, Yaoyao Deng, Wei Wang, Xuejiao Wei, Zhenwei Zhang & Mei Xiang

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  1. Wei Zhang
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Zhang, W., Xue, H., Wang, M. et al. Direct synthesis of Cu-containing Beta zeolite without template for selective oxidation of cyclohexane. J Porous Mater 29, 371–380 (2022). https://doi.org/10.1007/s10934-021-01165-2

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