TY  - 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 . .

TY  - JOUR
AU  - Bosnar, Sanja
AU  - Rac, Vladislav
AU  - Stošić, Dušan
AU  - Travert, Arnaud
AU  - Postole, Georgeta
AU  - Auroux, Aline
AU  - Škapin, Srečo
AU  - Damjanović-Vasilić, Ljiljana
AU  - Bronić, Josip
AU  - Du, Xuesen
AU  - Marković, Smilja
AU  - Pavlović, Vladimir
AU  - Rakić, Vesna
PY  - 2021
UR  - http://aspace.agrif.bg.ac.rs/handle/123456789/5961
AB  - Dual templating approach, using hexadecyltrimethylammonium bromide (CTAB), was employed in an attempt to synthesize hierarchical ZSM-5 zeolite. Amount of mesoporogen and the duration of aging of the precursor were varied. Majority of the synthesis routes resulted in phase separation, yielding separate ZSM-5 and amorphous mesoporous material. The relative amounts of the two phases were dependent on the CTAB amount ratio and also significantly on the duration of precursor aging before CTAB addition. One particular combination of the two factors led to the formation of a homogeneous hierarchical form of ZSM-5 with leafy morphology, consisting of intergrown thin crystalline sheets which formed flower-like structures. The hierarchical ZSM-5 possessed significant microporous (≈95 m2/g) and highly developed mesoporous surface (≈470 m2/g), with a relatively broad distribution of mesopore sizes (<20 nm). The acidity of all samples was studied in detail. Isothermal microcalorimetry/volumetry of ammonia adsorption provided quantitative data on the number and distribution of strength of acidic sites. In situ FTIR of pyridine and collidine adsorption was used to quantify Brønsted and Lewis acid sites, and to provide information on their location - in the micropores or mesopores/external surface. The hierarchical ZSM-5 possessed both Lewis and Brønsted acidity, with Brønsted sites located mainly in the micropores. All samples were fully characterized using XRD, low temperature nitrogen adsorption, FESEM and EDS. The synthetic route used for obtaining the ZSM-5 zeolite with flower-like morphology is a simple strategy for preparing hierarchical ZSM-5 forms targeting enhanced diffusivity and accessibility of catalytically active sites.
PB  - Elsevier B.V.
T2  - Microporous and Mesoporous Materials
T1  - Overcoming phase separation in dual templating: A homogeneous hierarchical ZSM-5 zeolite with flower-like morphology, synthesis and in-depth acidity study
SP  - 111534
VL  - 329
DO  - 10.1016/j.micromeso.2021.111534
ER  - 

@article{
author = "Bosnar, Sanja and Rac, Vladislav and Stošić, Dušan and Travert, Arnaud and Postole, Georgeta and Auroux, Aline and Škapin, Srečo and Damjanović-Vasilić, Ljiljana and Bronić, Josip and Du, Xuesen and Marković, Smilja and Pavlović, Vladimir and Rakić, Vesna",
year = "2021",
abstract = "Dual templating approach, using hexadecyltrimethylammonium bromide (CTAB), was employed in an attempt to synthesize hierarchical ZSM-5 zeolite. Amount of mesoporogen and the duration of aging of the precursor were varied. Majority of the synthesis routes resulted in phase separation, yielding separate ZSM-5 and amorphous mesoporous material. The relative amounts of the two phases were dependent on the CTAB amount ratio and also significantly on the duration of precursor aging before CTAB addition. One particular combination of the two factors led to the formation of a homogeneous hierarchical form of ZSM-5 with leafy morphology, consisting of intergrown thin crystalline sheets which formed flower-like structures. The hierarchical ZSM-5 possessed significant microporous (≈95 m2/g) and highly developed mesoporous surface (≈470 m2/g), with a relatively broad distribution of mesopore sizes (<20 nm). The acidity of all samples was studied in detail. Isothermal microcalorimetry/volumetry of ammonia adsorption provided quantitative data on the number and distribution of strength of acidic sites. In situ FTIR of pyridine and collidine adsorption was used to quantify Brønsted and Lewis acid sites, and to provide information on their location - in the micropores or mesopores/external surface. The hierarchical ZSM-5 possessed both Lewis and Brønsted acidity, with Brønsted sites located mainly in the micropores. All samples were fully characterized using XRD, low temperature nitrogen adsorption, FESEM and EDS. The synthetic route used for obtaining the ZSM-5 zeolite with flower-like morphology is a simple strategy for preparing hierarchical ZSM-5 forms targeting enhanced diffusivity and accessibility of catalytically active sites.",
publisher = "Elsevier B.V.",
journal = "Microporous and Mesoporous Materials",
title = "Overcoming phase separation in dual templating: A homogeneous hierarchical ZSM-5 zeolite with flower-like morphology, synthesis and in-depth acidity study",
pages = "111534",
volume = "329",
doi = "10.1016/j.micromeso.2021.111534"
}

Bosnar, S., Rac, V., Stošić, D., Travert, A., Postole, G., Auroux, A., Škapin, S., Damjanović-Vasilić, L., Bronić, J., Du, X., Marković, S., Pavlović, V.,& Rakić, V.. (2021). Overcoming phase separation in dual templating: A homogeneous hierarchical ZSM-5 zeolite with flower-like morphology, synthesis and in-depth acidity study. in Microporous and Mesoporous Materials
Elsevier B.V.., 329, 111534.
https://doi.org/10.1016/j.micromeso.2021.111534

Bosnar S, Rac V, Stošić D, Travert A, Postole G, Auroux A, Škapin S, Damjanović-Vasilić L, Bronić J, Du X, Marković S, Pavlović V, Rakić V. Overcoming phase separation in dual templating: A homogeneous hierarchical ZSM-5 zeolite with flower-like morphology, synthesis and in-depth acidity study. in Microporous and Mesoporous Materials. 2021;329:111534.
doi:10.1016/j.micromeso.2021.111534 .

Bosnar, Sanja, Rac, Vladislav, Stošić, Dušan, Travert, Arnaud, Postole, Georgeta, Auroux, Aline, Škapin, Srečo, Damjanović-Vasilić, Ljiljana, Bronić, Josip, Du, Xuesen, Marković, Smilja, Pavlović, Vladimir, Rakić, Vesna, "Overcoming phase separation in dual templating: A homogeneous hierarchical ZSM-5 zeolite with flower-like morphology, synthesis and in-depth acidity study" in Microporous and Mesoporous Materials, 329 (2021):111534,
https://doi.org/10.1016/j.micromeso.2021.111534 . .

TY  - JOUR
AU  - Nie, Hua
AU  - Li, Wei
AU  - Wu, Qirong
AU  - Rac, Vladislav
AU  - Rakić, Vesna
AU  - Du, Xuesen
PY  - 2020
UR  - http://aspace.agrif.bg.ac.rs/handle/123456789/5343
AB  - Poisoning effects by alkali metal chlorides is one of the major reasons for the deactivation of SCR catalyst in biomass-fired plants. In this study, the influence of KCl on two vanadium-based catalysts with different promoters, V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2, was investigated. The catalytic activity of the fresh V2O5-WO3/TiO2 was higher than that of V2O5-Ce(SO4)(2)/TiO2 at low temperatures. V2O5-Ce(SO4)(2)/TiO2 performed better than V2O5-WO3/TiO2 when KCl was deposited on the catalyst surface. Both poisoned catalysts were efficiently regenerated by SO2 treatment. The characterization results show that the reducibility and acidity of the catalysts were weakened by KCl deposition but regenerated by SO2.
PB  - MDPI, BASEL
T2  - Catalysts
T1  - The Poisoning of V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2 SCR Catalysts by KCl and The Partial Regeneration by SO2
IS  - 2
VL  - 10
DO  - 10.3390/catal10020207
ER  - 

@article{
author = "Nie, Hua and Li, Wei and Wu, Qirong and Rac, Vladislav and Rakić, Vesna and Du, Xuesen",
year = "2020",
abstract = "Poisoning effects by alkali metal chlorides is one of the major reasons for the deactivation of SCR catalyst in biomass-fired plants. In this study, the influence of KCl on two vanadium-based catalysts with different promoters, V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2, was investigated. The catalytic activity of the fresh V2O5-WO3/TiO2 was higher than that of V2O5-Ce(SO4)(2)/TiO2 at low temperatures. V2O5-Ce(SO4)(2)/TiO2 performed better than V2O5-WO3/TiO2 when KCl was deposited on the catalyst surface. Both poisoned catalysts were efficiently regenerated by SO2 treatment. The characterization results show that the reducibility and acidity of the catalysts were weakened by KCl deposition but regenerated by SO2.",
publisher = "MDPI, BASEL",
journal = "Catalysts",
title = "The Poisoning of V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2 SCR Catalysts by KCl and The Partial Regeneration by SO2",
number = "2",
volume = "10",
doi = "10.3390/catal10020207"
}

Nie, H., Li, W., Wu, Q., Rac, V., Rakić, V.,& Du, X.. (2020). The Poisoning of V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2 SCR Catalysts by KCl and The Partial Regeneration by SO2. in Catalysts
MDPI, BASEL., 10(2).
https://doi.org/10.3390/catal10020207

Nie H, Li W, Wu Q, Rac V, Rakić V, Du X. The Poisoning of V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2 SCR Catalysts by KCl and The Partial Regeneration by SO2. in Catalysts. 2020;10(2).
doi:10.3390/catal10020207 .

Nie, Hua, Li, Wei, Wu, Qirong, Rac, Vladislav, Rakić, Vesna, Du, Xuesen, "The Poisoning of V2O5-WO3/TiO2 and V2O5-Ce(SO4)(2)/TiO2 SCR Catalysts by KCl and The Partial Regeneration by SO2" in Catalysts, 10, no. 2 (2020),
https://doi.org/10.3390/catal10020207 . .