Dry Reforming of Methane Over Ru2/CeO2: Dynamic Behavior of Lattice Oxygen DOI
Pengfei Qu, Dong Fu, Gui‐Chang Wang

et al.

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 12, 2025

The reverse oxygen spillover (ROS) process is a critical factor in the dry reforming of methane (DRM). However, detailed mechanism remains unclear. In this study, we investigate ROS Ru/CeO2(111) (where n = 1, 2, 3, 4) using ab initio molecular dynamics simulations at realistic DRM reaction temperatures (1000 K). Our findings indicate that phenomenon observed exclusively Ru2/CeO2 system, while it absent Ru1, Ru3, and Ru4/CeO2 systems. Furthermore, additional investigations involving other transition metal (TM) systems, specifically TM2/CeO2 TM Co, Ni, Pd, Pt), reveal can also occur Co2/CeO2(111) system. primarily attributed to two factors. First, an electronic structure analysis suggests strong metal–support interaction "oxophilic" properties certain metals, such as Ru are significant contributors ROS. Second, from geometric perspective, coordination between Ru2 surface atoms CeO2(111) asymmetric, with coordinating three atoms. This configuration provides for possibility one into cluster. Notably, environment clusters plays more role than determining occurrence Through calculations mechanism, demonstrate vacancy created by facilitate CO2 activation, lattice spills interface lower energy barrier associated oxidation process. We anticipate our will provide theoretical insights design high-performance catalysts DRM, emphasizing importance considering interactions interface.

Language: Английский

Dry Reforming of Methane Over Ru2/CeO2: Dynamic Behavior of Lattice Oxygen DOI
Pengfei Qu, Dong Fu, Gui‐Chang Wang

et al.

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 12, 2025

The reverse oxygen spillover (ROS) process is a critical factor in the dry reforming of methane (DRM). However, detailed mechanism remains unclear. In this study, we investigate ROS Ru/CeO2(111) (where n = 1, 2, 3, 4) using ab initio molecular dynamics simulations at realistic DRM reaction temperatures (1000 K). Our findings indicate that phenomenon observed exclusively Ru2/CeO2 system, while it absent Ru1, Ru3, and Ru4/CeO2 systems. Furthermore, additional investigations involving other transition metal (TM) systems, specifically TM2/CeO2 TM Co, Ni, Pd, Pt), reveal can also occur Co2/CeO2(111) system. primarily attributed to two factors. First, an electronic structure analysis suggests strong metal–support interaction "oxophilic" properties certain metals, such as Ru are significant contributors ROS. Second, from geometric perspective, coordination between Ru2 surface atoms CeO2(111) asymmetric, with coordinating three atoms. This configuration provides for possibility one into cluster. Notably, environment clusters plays more role than determining occurrence Through calculations mechanism, demonstrate vacancy created by facilitate CO2 activation, lattice spills interface lower energy barrier associated oxidation process. We anticipate our will provide theoretical insights design high-performance catalysts DRM, emphasizing importance considering interactions interface.

Language: Английский

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