Insight of the stability and activity of platinum single atoms on ceria
- 64 Downloads
Single-atom catalysts (SACs) have recently attracted broad attention in the catalysis field due to their maximized atom efficiency and unique catalytic properties. An atomic-level understanding of the interaction between the metal atoms and support is vital for developing stable and high-performance SACs. In this work, Pt1 single atoms with loadings up to 4 wt.% were fabricated on ceria nanorods using the atomic layer deposition technique. To understand the Pt–O–Ce bond interfacial interactions, the stability of Pt1 single atoms in the hydrogen reducing environment was extensively investigated by using in situ diffuse reflectance infrared Fourier transform spectroscopy CO chemisorption measurements. It was found that ceria defect sites, metal loadings and high-temperature calcination are effective ways to tune the stability of Pt1 single atoms in the hydrogen environment. X-ray photoemission spectroscopy further showed that Pt1 single atoms on ceria are dominantly at a +2 valence state at the defect and step edge sites, while those on terrace sites are at a +4 state. The above tailored stability and electronic properties of Pt1 single atoms are found to be strongly correlated with the catalytic activity in the dry and water-mediated CO oxidation reactions.
Keywordssingle atom catalyst Pt1/CeO2 metal–support interaction stability water-mediated CO oxidation
Unable to display preview. Download preview PDF.
This work was supported by the National Natural Science Foundation of China (Nos. 21673215 and 21473169), the Fundamental Research Funds for the Central Universities (No. WK2060030029), and the Max-Planck Partner Group, Hefei Science Center, CAS, Users with Potential. The authors also gratefully thank the BL10B beamlines at National Synchrotron Radiation Laboratory (NSRL), China.
- Liu, J.; Yue, Y. Y.; Liu, H. Y.; Da, Z. J.; Liu, C. C.; Ma, A. Z.; Rong, J. F.; Su, D. S.; Bao, X. J.; Zheng, H. D. Origin of the robust catalytic performance of nanodiamond-graphene-supported Pt nanoparticles used in the propane dehydrogenation reaction. ACS Catal. 2017, 7, 3349–3355.CrossRefGoogle Scholar
- Li, T. B.; Liu, F.; Tang, Y.; Li, L.; Miao, S.; Su, Y.; Zhang, J. Y.; Huang, J. H.; Sun, H.; Haruta, M. et al. Maximizing the number of interfacial sites in single-atom catalysts for the highly selective, solvent-free oxidation of primary alcohols. Angew. Chem., Int. Ed. 2018, 57, 7795–7799.CrossRefGoogle Scholar
- DeRita, L.; Dai, S.; Lopez-Zepeda, K.; Pham, N.; Graham, G. W.; Pan, X. Q.; Christopher, P. Catalyst architecture for stable single atom dispersion enables site-specific spectroscopic and reactivity measurements of CO adsorbed to Pt atoms, oxidized Pt clusters, and metallic Pt clusters on TiO2. J. Am. Chem. Soc. 2017, 139, 14150–14165.CrossRefGoogle Scholar
- 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. Ultrastable hydroxyapatite/titaniumdioxide-supported gold nanocatalyst with strong metal-support interaction for carbon monoxide oxidation. Angew. Chem., Int. Ed. 2016, 55, 10606–10611.CrossRefGoogle Scholar
- Wang, L.; Zhang, J.; Zhu, Y. H.; Xu, S. D.; Wang, C. T.; Bian, C. Q.; Meng, X. J.; Xiao, F. S. Strong metal-support interactions achieved by hydroxide-to-oxide support transformation for preparation of sinter-resistant gold nanoparticle catalysts. ACS Catal. 2017, 7, 7461–7465.CrossRefGoogle Scholar
- Li, S. W.; Xu, Y.; Chen, Y. F.; Li, W. Z.; Lin, L. L.; Li, M. Z.; Deng, Y. C.; Wang, X. P.; Ge, B. H.; Yang, C. et al. Tuning the selectivity of catalytic carbon dioxide hydrogenation over iridium/cerium oxide catalysts with a strong metal-support interaction. Angew. Chem., Int. Ed. 2017, 56, 10761–10765.CrossRefGoogle Scholar
- Bruix, A.; Rodriguez, J. A.; Ramírez, P. J.; Senanayake, S. D.; Evans, J.; Park, J. B.; Stacchiola, D.; Liu, P.; Hrbek, J.; Illas, F. A new type of strong metal-support interaction and the production of H2 through the transformation of water on Pt/CeO2(111) and Pt/CeOx/TiO2(110) catalysts. J. Am. Chem. Soc. 2012, 134, 8968–8974.CrossRefGoogle Scholar
- Chen, J.Y.; Wanyan, Y. J.; Zeng, J. X.; Fang, H. H.; Li, Z. J.; Dong, Y. D.; Qin, R. X.; Wu, C. Z.; Liu, D. Y.; Wang, M. Z. et al. Surface engineering protocol to obtain an atomically dispersed Pt/CeO2 catalyst with high activity and stability for CO oxidation. ACS Sustainable Chem. Eng. 2018, 6, 14054–14062.CrossRefGoogle Scholar
- Bruix, A.; Lykhach, Y.; Matolínová, I.; Neitzel, A.; Skála, T.; Tsud, N.; Vorokhta, M.; Stetsovych, V.; Ševčíková, K.; Mysliveček, J. et al. Maximum noble-metal efficiency in catalytic materials: Atomically dispersed surface platinum. Angew. Chem., Int. Ed. 2014, 53, 10525–10530.CrossRefGoogle Scholar
- Ke, J.; Zhu, W.; Jiang, Y. Y.; Si, R.; Wang, Y. J.; Li, S. C.; Jin, C. H.; Liu, H. C.; Song, W. G.; Yan, C. H. et al. Strong local coordination structure effects on subnanometer PtOx clusters over CeO2 nanowires probed by low-temperature CO oxidation. ACS Catal. 2015, 5, 5164–5173.CrossRefGoogle Scholar