Insight into the Dynamic Nature of the Pt–CeO<sub>2</sub> Interface in Dry Reforming of Methane

Shen, Dongyang; Li, Zhe; Bai, Yue; Li, Jing; Lyu, Shuai; Zhang, Yuhua; Li, Jinlin; Li, Lin

doi:10.1021/acs.langmuir.4c00834

Langmuir

2024

DOI: 10.1021/acs.langmuir.4c00834

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Insight into the Dynamic Nature of the Pt–CeO₂ Interface in Dry Reforming of Methane

Dongyang Shen,

Zhe Li,

Yue Bai

et al.

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A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)

Qu,

Wang

2024

ACS Appl. Mater. Interfaces

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In this work, the mechanism of dry reforming of methane (DRM) over a series of CeO 2 (111)-supported transition metal (TM) clusters, TM 4 /CeO 2 (111) (TM = Ru, Pt, Co, Ni), was investigated by using density functional theory (DFT) and microkinetic modeling. According to the results of DFT calculations, Ru 4 /CeO 2 (111) and Co 4 /CeO 2 (111) exhibit strong oxygen adsorption capabilities due to the oxophilic properties of Ru and Co metals, which facilitate CO 2 activation more effectively than other metals. Ru 4 / CeO 2 (111) demonstrates the highest efficiency for both CH 4 and CO 2 activation. Pt 4 /CeO 2 (111) has great anticoking ability because the C* coupling has a higher energy barrier. Microkinetic simulations indicate that the turnover frequency (TOF) rate follows the trend: Ru 4 /CeO 2 (111) > Pt 4 / CeO 2 (111) > Co 4 /CeO 2 (111) > Ni 4 / CeO 2 (111). Ru/CeO 2 exhibits the highest activity and selectivity. Pt/CeO 2 has the best ability for anticoking due to the high energy barrier of C* coupling. Co/CeO 2 is prone to deactivation from oxygen poisoning, attributed to its strong oxophilic properties and weak CH 4 activation ability, Ni/CeO 2 shows the poorest activity and stability, as it is easily deactivated by coke formation and has the lowest selectivity. The analysis of key steps indicates that there are different rate-controlled steps for various metals due to inherent differences in their properties. We anticipate that our results will offer a strategy for designing DRM catalysts by selecting the appropriate metal catalysts.

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A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)

Qu,

Wang

2024

ACS Appl. Mater. Interfaces

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show abstract

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Insight into the Dynamic Nature of the Pt–CeO₂ Interface in Dry Reforming of Methane

Cited by 1 publication

References 39 publications

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)

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Insight into the Dynamic Nature of the Pt–CeO2 Interface in Dry Reforming of Methane

Cited by 1 publication

References 39 publications

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO2-Supported TM4 clusters (TM = Ru, Pt, Co, Ni)

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO2-Supported TM4 clusters (TM = Ru, Pt, Co, Ni)

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Product

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Insight into the Dynamic Nature of the Pt–CeO₂ Interface in Dry Reforming of Methane

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)

A Comprehensive Mechanistic Study for Dry Reforming of Methane over CeO₂-Supported TM₄ clusters (TM = Ru, Pt, Co, Ni)