Citation: Qinghao Shang, Nanfang Tang, Haifeng Qi, Shuai Chen, Guoliang Xu, Chuntian Wu, Xiaoli Pan, Xiaodong Wang, Yu Cong. A palladium single-atom catalyst toward efficient activation of molecular oxygen for cinnamyl alcohol oxidation[J]. Chinese Journal of Catalysis, ;2020, 41(12): 1812-1817. doi: 10.1016/S1872-2067(20)63651-8 shu

A palladium single-atom catalyst toward efficient activation of molecular oxygen for cinnamyl alcohol oxidation

a CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China

Received Date: 27 February 2020
Revised Date: 31 March 2020

Fund Project: This work was supported by National Natural Science Foundation of China (21802134) and National Science and Technology Major Project of China (2017-III-0005-0030).

Selective aerobic oxidation of alcohols under mild conditions is of great importance yet challenging, with the activation of molecular oxygen (O₂) as a crucial capability of the catalysts. Herein, we demonstrate that an Al₂O₃-supported Pd single-atom catalyst leads to higher activity and selectivity compared to Pd nanoparticles for the oxidation of cinnamyl alcohol. The Al₂O₃ support used in this study is rich in coordinately unsaturated Al³⁺ sites, which are apt for binding to Pd atoms through oxygen bridges and present a distinct metal-support interaction (MSI). The suitable MSI then leads to a unique electronic characteristic of the Pd single atoms, which can be confirmed via X-ray photoelectron spectroscopy, normalized X-ray absorption near-edge structure, and diffuse reflectance Fourier transform infrared spectroscopy. Moreover, this unique electronic state is proposed to be responsible for its high catalytic activity. With the help of in-situ UV-vis spectra and electron spin resonance spectra, a specific alcohol oxidation route with O₂ activation mechanism is then identified. Active oxygen species behaving chemically like singlet-O₂ are generated from the interaction of O₂ with Pd₁/Al₂O₃, and then oxidize the partially dehydrogenated intermediates produced by the adsorbed allylic alcohols and Pd atoms to the desired alkenyl aldehyde. This work provides a promising path for the design and development of high-activity catalysts for aerobic oxidation reactions.
- Single-atom catalysis,
- Palladium,
- Alcohol oxidation,
- Oxygen activation,
- Metal support interaction
1. [1]
2. [2]
3. [3]
4. [4]
5. [5]
6. [6]
7. [7]
8. [8]
9. [9]
10. [10]
11. [11]
12. [12]
13. [13]
14. [14]
15. [15]
16. [16]
17. [17]
18. [18]
19. [19]
20. [20]
21. [21]
22. [22]
23. [23]
24. [24]
25. [25]
26. [26]
27. [27]
28. [28]
29. [29]
30. [30]
31. [31]
32. [32]
33. [33]
34. [34]
35. [35]
36. [36]
1. [1]
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