CO2 methanation over Ni nanoparticles inversely loaded with CeO2 and Cr2O3: catalytic functions of metal oxide/Ni interfaces

Junbo Tian; Peng Zheng; Tengfei Zhang; Zhennan Han; Wenqing Xu; Fangna Gu; Fang Wang; Zhanguo Zhang; Ziyi Zhong; Fabing Su; Guangwen Xu

doi:10.1016/j.apcatb.2023.123121

CO2 methanation over Ni nanoparticles inversely loaded with CeO2 and Cr2O3: catalytic functions of metal oxide/Ni interfaces

Junbo Tian, Peng Zheng, Tengfei Zhang, Zhennan Han^*, Wenqing Xu^*, Fangna Gu^*, Fang Wang, Zhanguo Zhang, Ziyi Zhong^*, Fabing Su^*, Guangwen Xu^*

^*Corresponding author for this work

Chemical Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

Interfaces between active metal and metal oxide in a heterogenous catalyst often play an important role in catalysis. In this work, we intentionally synthesized a series of inverse CeO2-Cr2O3/Ni model catalysts with the formation of controlled CeO2-Ni and Cr2O3-Ni interfacial structures and investigated the roles of the oxide-metal interfaces in CO2 methanation performance through excluding the normal support effect. Experimental and DFT calculation results reveal that the formate pathway tends to occur on the catalyst with only CeO2-Ni interfaces. The Cr2O3-Ni interface formed after introducing Cr oxide alters the nearby CeO2-Ni interface by electron transfer through Ni, which brings an additional reaction pathway (CO pathway) on CeO2-Cr2O3/Ni. Furthermore, it shows a relatively lower CO2 absorption energy and activation energy barrier for CO2 dissociation to CO at the Cr2O3-Ni interface, favorable for CO2 activation and further hydrogenation, thus leading to excellent low-temperature activity.

Original language	English
Journal	Applied Catalysis B: Environmental
DOIs	https://doi.org/10.1016/j.apcatb.2023.123121
State	E-pub ahead of print - 18 Jul 2023

Access to Document

10.1016/j.apcatb.2023.123121

Cite this

@article{757d19f3f3d14938b735948659fad0ea,

title = "CO2 methanation over Ni nanoparticles inversely loaded with CeO2 and Cr2O3: catalytic functions of metal oxide/Ni interfaces",

abstract = "Interfaces between active metal and metal oxide in a heterogenous catalyst often play an important role in catalysis. In this work, we intentionally synthesized a series of inverse CeO2-Cr2O3/Ni model catalysts with the formation of controlled CeO2-Ni and Cr2O3-Ni interfacial structures and investigated the roles of the oxide-metal interfaces in CO2 methanation performance through excluding the normal support effect. Experimental and DFT calculation results reveal that the formate pathway tends to occur on the catalyst with only CeO2-Ni interfaces. The Cr2O3-Ni interface formed after introducing Cr oxide alters the nearby CeO2-Ni interface by electron transfer through Ni, which brings an additional reaction pathway (CO pathway) on CeO2-Cr2O3/Ni. Furthermore, it shows a relatively lower CO2 absorption energy and activation energy barrier for CO2 dissociation to CO at the Cr2O3-Ni interface, favorable for CO2 activation and further hydrogenation, thus leading to excellent low-temperature activity.",

author = "Junbo Tian and Peng Zheng and Tengfei Zhang and Zhennan Han and Wenqing Xu and Fangna Gu and Fang Wang and Zhanguo Zhang and Ziyi Zhong and Fabing Su and Guangwen Xu",

year = "2023",

month = jul,

day = "18",

doi = "10.1016/j.apcatb.2023.123121",

language = "英语",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

}

TY - JOUR

T1 - CO2 methanation over Ni nanoparticles inversely loaded with CeO2 and Cr2O3: catalytic functions of metal oxide/Ni interfaces

AU - Tian, Junbo

AU - Zheng, Peng

AU - Zhang, Tengfei

AU - Han, Zhennan

AU - Xu, Wenqing

AU - Gu, Fangna

AU - Wang, Fang

AU - Zhang, Zhanguo

AU - Zhong, Ziyi

AU - Su, Fabing

AU - Xu, Guangwen

PY - 2023/7/18

Y1 - 2023/7/18

N2 - Interfaces between active metal and metal oxide in a heterogenous catalyst often play an important role in catalysis. In this work, we intentionally synthesized a series of inverse CeO2-Cr2O3/Ni model catalysts with the formation of controlled CeO2-Ni and Cr2O3-Ni interfacial structures and investigated the roles of the oxide-metal interfaces in CO2 methanation performance through excluding the normal support effect. Experimental and DFT calculation results reveal that the formate pathway tends to occur on the catalyst with only CeO2-Ni interfaces. The Cr2O3-Ni interface formed after introducing Cr oxide alters the nearby CeO2-Ni interface by electron transfer through Ni, which brings an additional reaction pathway (CO pathway) on CeO2-Cr2O3/Ni. Furthermore, it shows a relatively lower CO2 absorption energy and activation energy barrier for CO2 dissociation to CO at the Cr2O3-Ni interface, favorable for CO2 activation and further hydrogenation, thus leading to excellent low-temperature activity.

AB - Interfaces between active metal and metal oxide in a heterogenous catalyst often play an important role in catalysis. In this work, we intentionally synthesized a series of inverse CeO2-Cr2O3/Ni model catalysts with the formation of controlled CeO2-Ni and Cr2O3-Ni interfacial structures and investigated the roles of the oxide-metal interfaces in CO2 methanation performance through excluding the normal support effect. Experimental and DFT calculation results reveal that the formate pathway tends to occur on the catalyst with only CeO2-Ni interfaces. The Cr2O3-Ni interface formed after introducing Cr oxide alters the nearby CeO2-Ni interface by electron transfer through Ni, which brings an additional reaction pathway (CO pathway) on CeO2-Cr2O3/Ni. Furthermore, it shows a relatively lower CO2 absorption energy and activation energy barrier for CO2 dissociation to CO at the Cr2O3-Ni interface, favorable for CO2 activation and further hydrogenation, thus leading to excellent low-temperature activity.

U2 - 10.1016/j.apcatb.2023.123121

DO - 10.1016/j.apcatb.2023.123121

M3 - 文章

SN - 0926-3373

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

ER -

CO2 methanation over Ni nanoparticles inversely loaded with CeO2 and Cr2O3: catalytic functions of metal oxide/Ni interfaces

Abstract

Access to Document

Fingerprint

Cite this