Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts
Samo za registrovane korisnike
2024
Autori
Tang, TianYe, Lyumeng
Chen, Yanrong
Xue, Jingyu
Shen, Xiaoqiang
Chen, Jinfei
Quarcoo, Fiona Hammond
Rac, Vladislav
Rakić, Vesna
Li, Xinbao
Du, Xuesen
Članak u časopisu (Objavljena verzija)
Metapodaci
Prikaz svih podataka o dokumentuApstrakt
The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechan...ism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures.
Ključne reči:
CO oxidation / Copper−ceria interface / DFT+U / Mars-van Krevelen (M−vK)Izvor:
Applied Catalysis B: Environmental, 2024, 342, 123368-URI
https://www.sciencedirect.com/science/article/pii/S0926337323010111http://aspace.agrif.bg.ac.rs/handle/123456789/6464
Institucija/grupa
Poljoprivredni fakultetTY - JOUR AU - Tang, Tian AU - Ye, Lyumeng AU - Chen, Yanrong AU - Xue, Jingyu AU - Shen, Xiaoqiang AU - Chen, Jinfei AU - Quarcoo, Fiona Hammond AU - Rac, Vladislav AU - Rakić, Vesna AU - Li, Xinbao AU - Du, Xuesen PY - 2024 UR - https://www.sciencedirect.com/science/article/pii/S0926337323010111 UR - http://aspace.agrif.bg.ac.rs/handle/123456789/6464 AB - The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures. T2 - Applied Catalysis B: Environmental T2 - Applied Catalysis B: EnvironmentalApplied Catalysis B: Environmental T1 - Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts SP - 123368 VL - 342 DO - 10.1016/j.apcatb.2023.123368 ER -
@article{ author = "Tang, Tian and Ye, Lyumeng and Chen, Yanrong and Xue, Jingyu and Shen, Xiaoqiang and Chen, Jinfei and Quarcoo, Fiona Hammond and Rac, Vladislav and Rakić, Vesna and Li, Xinbao and Du, Xuesen", year = "2024", abstract = "The unique interface synergistic catalytic properties for metal oxide-supported catalysts have long been explored in several critical heterogeneous catalytic processes (e.g., CO oxidation reactions). However, interfacial synergistic catalysis is still a hitherto undescribed mechanism due to the lack of direct evidence at the atomic level. Thereinto, the CuOx-supported CeO2 (CuOx/CeO2) catalyst is a typical case. Herein, a combination study including representative theoretical calculations, in situ DRIFTS spectra and tailored molecular probe experiments supports a new carbonate-interface mediated Mars-van Krevelen (M−vK) mechanism for CO oxidation, i.e., CO molecules form carbonate intermediate species directly between spatial proximity (2.99 Å) double lattice oxygen sites with low oxygen vacancies formation energy (EformOv = 0.82 eV/0.83 eV) at the copper−ceria interface. The reaction energy barrier of this process is 0.32 eV, much lower than the 1.23 eV of the conventional M−vK mechanism. Besides, the spatial effect of double oxygen vacancies (Ov) generated by the depletion of intermediate carbonate species promotes the sustained and dynamic activation of O2, hence facilitating the efficient operation of the M−vK mechanism at low temperatures.", journal = "Applied Catalysis B: Environmental, Applied Catalysis B: EnvironmentalApplied Catalysis B: Environmental", title = "Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts", pages = "123368", volume = "342", doi = "10.1016/j.apcatb.2023.123368" }
Tang, T., Ye, L., Chen, Y., Xue, J., Shen, X., Chen, J., Quarcoo, F. H., Rac, V., Rakić, V., Li, X.,& Du, X.. (2024). Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts. in Applied Catalysis B: Environmental, 342, 123368. https://doi.org/10.1016/j.apcatb.2023.123368
Tang T, Ye L, Chen Y, Xue J, Shen X, Chen J, Quarcoo FH, Rac V, Rakić V, Li X, Du X. Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts. in Applied Catalysis B: Environmental. 2024;342:123368. doi:10.1016/j.apcatb.2023.123368 .
Tang, Tian, Ye, Lyumeng, Chen, Yanrong, Xue, Jingyu, Shen, Xiaoqiang, Chen, Jinfei, Quarcoo, Fiona Hammond, Rac, Vladislav, Rakić, Vesna, Li, Xinbao, Du, Xuesen, "Diving into the interface-mediated Mars-van Krevelen (M−vK) characteristic of CuOx-supported CeO2 catalysts" in Applied Catalysis B: Environmental, 342 (2024):123368, https://doi.org/10.1016/j.apcatb.2023.123368 . .