Citation: Hailian Tang, Siyuan Chen, Qiaoyun Liu, Guoyi Bai, Botao Qiao, Liu Fei. Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions[J]. Acta Physico-Chimica Sinica, ;2025, 41(4): 240800. doi: 10.3866/PKU.WHXB202408004 shu

Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions

Hailian Tang ^{1, 2,,} ,
Siyuan Chen ^{2, 3} ,
Qiaoyun Liu ^{2, 4} ,
Guoyi Bai ¹ ,
Botao Qiao ^{2, 5,,} ,
Liu Fei ^2,,

1.
School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China
2.
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
3.
College of Chemistry and Materials Science, Hebei University, Baoding 071002, Hebei Province, China
4.
College of Chemistry, Zhengzhou University, Zhengzhou 450001, China
5.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China

Corresponding author: Hailian Tang, hltang@email.tjut.edu.cn Botao Qiao, bqiao@dicp.ac.cn Liu Fei, fei.liu@dicp.ac.cn
Received Date: 4 August 2024
Revised Date: 14 September 2024
Accepted Date: 2 October 2024

Fund Project: the National Key R & D Program of China 2023YFA1506800National Natural Science Foundation of China 21902040National Natural Science Foundation of China 22108259Natural Science Foundation of Hebei Province B2019201158

The strong metal-support interaction (SMSI) is a widely recognized concept in heterogeneous catalysis, known for significantly enhancing catalyst stability and potentially modulating catalytic performance. However, because the SMSI effect is generally reversible, it tends to diminish under redox conditions opposite to those used for its construction. Consequently, its application is typically limited to conditions that are the same or similar to those under which it was formed. Herein, we report the application of oxidative SMSI (O-SMSI) constructed on hydroxyapatite-supported Rh catalyst (Rh/HAP) in a reductive reaction, the hydrogenation of furfuryl alcohol. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and electron microscopy measurements reveal that high-temperature oxidation treatment at 500 ℃ induced the occurrence of O-SMSI on the Rh/HAP catalyst, accompanied by the encapsulation of Rh particles by the support. Upon the O-SMSI, the Rh species were effectively stabilized on the support surface, with significant suppression of sintering and leaching during liquid-phase reactions. As a result, the catalyst showed stable furfuryl alcohol conversion and cyclopentanone selectivity during recycling tests. Furthermore, it was found that the O-SMSI and the associated encapsulation behavior on the Rh/HAP system were only partially reversible rather than completely reversible. Even after high-temperature reduction at up to 600 ℃, a portion of the SMSI effect remains, ensuring the stability of the catalysts in reductive reactions. This discovery greatly expands the application scope of SMSI catalysts and provides a new way to prepare stable hydrogenation catalysts.
- Oxidative strong metal-support interaction,
- Hydroxyapatite,
- Rh,
- Stability,
- Hydrogenation
1. [1]
  Xu, M.; Peng, M.; Tang, H.; Zhou, W.; Qiao, B.; Ma, D. J. Am. Chem. Soc. 2024, 146, 2290. doi: 10.1021/jacs.3c09102 doi: 10.1021/jacs.3c09102
2. [2]
  Wu, G.; Liu, Y.; Wang, J. Accounts Chem. Res. 2024, 56, 911. doi: 10.1021/acs.accounts.2c00727 doi: 10.1021/acs.accounts.2c00727
3. [3]
  Tauster, S. J.; Fung, S. C.; Garten, R. L. J. Am. Chem. Soc. 1978, 100, 170. doi: 10.1021/ja00469a029 doi: 10.1021/ja00469a029
4. [4]
  Li, M.; Zhang, T.; Yang, S. -Z.; Sun, Y.; Zhang, J.; Polo-Garzon, F.; Siniard, K. M.; Yu, X.; Wu, Z.; Driscoll, D. M.; et al. ACS Catal. 2023, 13, 6114. doi: 10.1021/acscatal.2c05730 doi: 10.1021/acscatal.2c05730
5. [5]
  Dong, J.; Fu, Q.; Li, H.; Xiao, J.; Yang, B.; Zhang, B.; Bai, Y.; Song, T.; Zhang, R.; Gao, L.; et al. J. Am. Chem. Soc. 2020, 142, 17167. doi: 10.1021/jacs.0c08139 doi: 10.1021/jacs.0c08139
6. [6]
  Siniard, K. M.; Li, M.; Yang, S. Z.; Zhang, J.; Polo-Garzon, F.; Wu, Z.; Yang, Z.; Dai, S. Angew. Chem. -Int. Edit. 2023, e202214322. doi: 10.1002/anie.202214322 doi: 10.1002/anie.202214322
7. [7]
  Wang, H.; Wang, L.; Lin, D.; Feng, X.; Niu, Y.; Zhang, B.; Xiao, F. -S. Nat. Catal. 2021, 4, 418. doi: 10.1038/s41929-021-00611-3 doi: 10.1038/s41929-021-00611-3
8. [8]
  Tang, H.; Su, Y.; Zhang, B.; Lee, A. F.; Isaacs, M. A.; Wilson, K.; Li, L.; Ren, Y.; Huang, J.; Haruta, M.; et al. Sci. Adv. 2017, 3, e1700231. doi: 10.1126/sciadv.1700231 doi: 10.1126/sciadv.1700231
9. [9]
  Liu, X.; Liu, M. -H.; Luo, Y. -C.; Mou, C. -Y.; Lin, S. D.; Cheng, H.; Chen, J. -M.; Lee, J. -F.; Lin, T. -S. J. Am. Chem. Soc. 2012, 134, 10251. doi: 10.1021/ja3033235 doi: 10.1021/ja3033235
10. [10]
  Tang, H.; Wei, J.; Liu, F.; Qiao, B.; Pan, X.; Li, L.; Liu, J.; Wang, J.; Zhang, T. J. Am. Chem. Soc. 2016, 138, 56. doi: 10.1021/jacs.5b11306 doi: 10.1021/jacs.5b11306
11. [11]
  Tang, H.; Su, Y.; Guo, Y.; Zhang, L.; Li, T.; Zang, K.; Liu, F.; Li, L.; Luo, J.; Qiao, B.; et al. Chem. Sci. 2018, 9, 6679. doi: 10.1039/c8sc01392f doi: 10.1039/c8sc01392f
12. [12]
  Song, T. Y.; Dong, J. H.; Li, R. T.; Xu, X. Y.; Hiroaki, M.; Yang, B.; Zhang, R. K.; Bai, Y. X.; Xin, H.; Lin, L.; et al. J. Phys. Chem. Lett. 2021, 12, 4187. doi: 10.1021/acs.jpclett.1c00934 doi: 10.1021/acs.jpclett.1c00934
13. [13]
  Matsubu, J. C.; Zhang, S.; DeRita, L.; Marinkovic, N. S.; Chen, J. G.; Graham, G. W.; Pan, X.; Christophe, P. Nat. Chem. 2017, 9, 120. doi: 10.1038/NCHEM.2607 doi: 10.1038/NCHEM.2607
14. [14]
  Li, Z.; Cui, Y.; Wu, Z.; Milligan, C.; Zhou, L.; Mitchell, G.; Xu, B.; Shi, E.; Miller, J. T.; Ribeiro, F. H.; et al. Nat. Catal. 2018, 1, 349. doi: 10.1038/s41929-018-0067-8 doi: 10.1038/s41929-018-0067-8
15. [15]
  Lunkenbein, T.; Schumann, J.; Behrens, M.; Schlögl, R.; Willinger, M. G. Angew. Chem. -Int. Edit. 2015, 54, 4544. doi: 10.1002/anie.201411581 doi: 10.1002/anie.201411581
16. [16]
  Tauster, S. J.; Fung, S. C.; Baker, R. T. K.; Horsle, J. A. Science 1981, 211, 1120. doi: 10.1126/science.211.4487.1121 doi: 10.1126/science.211.4487.1121
17. [17]
  Han, B.; Li, Q.; Jiang, X.; Guo, Y.; Jiang, Q.; Su, Y.; Li, L.; Qiao, B. Small 2022, 18, 2204490. doi: 10.1002/smll.202204490 doi: 10.1002/smll.202204490
18. [18]
  Guo, Y.; Li, Y.; Du, X.; Li, L.; Jiang, Q.; Qiao, B. Nano Res. 2022, 15, 10037. doi: 10.1007/s12274-022-4376-5 doi: 10.1007/s12274-022-4376-5
19. [19]
  Han, B.; Guo, Y. L.; Huang, Y. K.; Xi, W.; Xu, J.; Luo, J.; Qi, H. F.; Ren, Y. J.; Liu, X. Y.; Qiao, B. T.; et al. Angew. Chem. -Int. Edit. 2020, 59, 11824. doi: 10.1002/anie.202003208 doi: 10.1002/anie.202003208
20. [20]
  Tang, H. L.; Liu, F.; Wei, J. K.; Qiao, B. T.; Zhao, K. F.; Su, Y.; Jin, C. Z.; Li, L.; Liu, J. Y.; Wang, J. H.; et al. Angew. Chem. -Int. Edit. 2016, 55, 10606. doi: 10.1002/anie.201601823 doi: 10.1002/anie.201601823
21. [21]
  Renz, M.; Corma, A. Eur. J. Org. Chem. 2004, 2004, 2036. doi: 10.1002/ejoc.200300778 doi: 10.1002/ejoc.200300778
22. [22]
  Akashi, T.; Sato, S.; Takahashi, R.; Sodesawa, T.; Inui, K. Catal. Commun. 2003, 4, 411. doi: 10.1016/s1566-7367(03)00095-5 doi: 10.1016/s1566-7367(03)00095-5
23. [23]
  Mori, K.; Kanai, S.; Hara, T.; Mizugaki, T.; Ebitani, K.; Jitsukawa, K.; Kaneda, K. Chem. Mater. 2007, 19, 1249. doi: 10.1021/cm061388l doi: 10.1021/cm061388l
24. [24]
  Tauster, S. J.; Fung, S. C. J. Catal. 1978, 55, 29.
25. [25]
  Vimont, A.; Thibault-Starzyk, F.; Daturi, M. Chem. Soc. Rev. 2010, 39, 4928. doi: 10.1039/b919543m doi: 10.1039/b919543m
26. [26]
  Lamberti, C.; Zecchina, A.; Groppo, E.; Bordiga, S. Chem. Soc. Rev. 2010, 39, 4951. doi: 10.1039/c0cs00117a doi: 10.1039/c0cs00117a
27. [27]
  Li, L.; Wang, A. Q.; Qiao, B. T.; Lin, J.; Huang, Y. Q.; Wang, X. D.; Zhang, T. J. Catal. 2013, 299, 90. doi: 10.1016/j.jcat.2012.11.019 doi: 10.1016/j.jcat.2012.11.019
28. [28]
  Zhao, K.; Tang, H.; Qiao, B.; Li, L.; Wang, J. ACS Catal. 2015, 5, 3528. doi: 10.1021/cs5020496 doi: 10.1021/cs5020496
29. [29]
  Lang, R.; Li, T.; Matsumura, D.; Miao, S.; Ren, Y.; Cui, Y. T.; Tan, Y.; Qiao, B.; Li, L.; Wang, A.; et al. Angew. Chem. -Int. Edit. 2016, 55, 16054. doi: 10.1002/anie.201607885 doi: 10.1002/anie.201607885
30. [30]
  Wu, J.; Qiao, L. -Y.; Zhou, Z. -F.; Cui, G. -J.; Zong, S. -S.; Xu, D. -J.; Ye, R. -P.; Chen, R. -P.; Si, R.; Yao, Y. -G. ACS Catal. 2019, 9, 932. doi: 10.1021/acscatal.8b03319 doi: 10.1021/acscatal.8b03319
31. [31]
  Mou, J. L.; Chen, L. L.; Fan, J.; Zeng, L.; Jiang, X.; Jiao, Y.; Wang, J. L.; Chen, Y. Q. Acta Phys. -Chim. Sin. 2023, 39, 2302041. doi: 10.3866/PKU.WHXB202302041 doi: 10.3866/PKU.WHXB202302041
32. [32]
  Marchionni, V.; Newton, M. A.; Kambolis, A.; Matam, S. K.; Weidenkaff, A.; Ferri, D. Catal. Today 2014, 229, 80. doi: 10.1016/j.cattod.2013.10.082 doi: 10.1016/j.cattod.2013.10.082
33. [33]
  Machida, M.; Minami, S.; Ikeue, K.; Hinokuma, S.; Nagao, Y.; Sato, T.; Nakahara, Y. Chem. Mater. 2014, 26, 5799. doi: 10.1021/cm503061g doi: 10.1021/cm503061g
34. [34]
  Machida, M.; Minami, S.; Hinokuma, S.; Yoshida, H.; Nagao, Y.; Sato, T.; Nakahara, Y. J. Phys. Chem. C 2014, 119, 373. doi: 10.1021/jp509649r doi: 10.1021/jp509649r
35. [35]
  Machida, M. Chem. Rec. 2016, 16, 2219. doi: 10.1002/tcr.201600037 doi: 10.1002/tcr.201600037
36. [36]
  Gol'dshleger, N. F.; Azbel', B. I.; Isakov, Y. I.; Shpiro, E. S.; Minachev, K. M. J. Mol. Catal. A: Chem. 1996, 106, 159.
37. [37]
  Andersson, S. L. T.; Scurre, M. S. J. Catal. 1981, 71, 233.
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