Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

Chen, Xiaohan; Ye, Runping; Sun, Chunyan; Jin, Chengkai; Wang, Yuan; Arandiyan, Hamidreza; Lim, Kang Hui; Song, Guoqiang; Hu, Feiyang; Li, Claudia; Lu, Zhang-Hui; Feng, Gang; Zhang, Rongbin; Kawi, Sibudjing

doi:10.1016/j.cej.2024.149471

Cited by 15 publications

(1 citation statement)

References 70 publications

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“…All the samples exhibit only characteristic peaks attributed to CeO 2 with a typical cubic fluorite structure (PDF#34−0394). 28,29 No diffraction peaks of Ru or Bi species are detected, suggestive of the high dispersion of these species even after reduction at 400 °C. Furthermore, for bare supports, the 2θ value of the CeO 2 (111) peak decreases from 28.52°to 28.41°(Figure 1d) and the CeO 2 lattice parameter increases from 5.4032 to 5.4144 Å with increasing Bi content (Table S1), indicating that Bi ions may be dispersed at interstitial positions in the CeO 2 lattice.…”

Section: Morphological and Structuralmentioning

confidence: 99%

Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

Xie,

Chen,

Wen

et al. 2024

ACS Catal.

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Flexible tuning of the CO 2 hydrogenation selectivity through properly designed catalysts to obtain desired high-added-value products is a promising strategy for addressing environmental and energy issues but also a huge challenge. Herein, the CO 2 hydrogenation selectivity over the commonly used Ru/CeO 2 methanation catalysts was facilely overturned from ∼99% CH 4 to 100% CO by tailoring the local electron density of Ru through electronic interaction induced by electron acceptors (Bi, In, Sn, etc.). Systematically, in situ spectroscopic characterizations and DFT calculations reveal that owing to the electron-withdrawing role of the electron acceptor, Ru sites lose more charges than the unmodified catalyst, which weakens the binding strength of carbonyl to Ru sites and further induces the imbalance reaction energy barrier for carbonyl and formate intermediates. Thus, the original parallel reaction processes involving CH 4 generation (carbonyl route and formate route) are transformed into the preferential desorption of CO, finally acquiring opposite selectivity. Importantly, such an electronic interaction is general for overturning product selectivity and can be extended to other Ru catalysts and Ni catalysts. This discovery may offer a promising way to develop CO 2 hydrogenation catalysts with controllable product selectivity.

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Section: Morphological and Structuralmentioning

confidence: 99%

Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

Xie,

Chen,

Wen

et al. 2024

ACS Catal.

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Boosting low-temperature CO2 methanation activity through Tailored electronic structures and step-edge defects in Niε−-Ov-Ceδ+ inverse interfaces

Zang,

Wei,

et al. 2025

Applied Surface Science

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Promotional role of Ni photodepositing on Ru confined TiO2 nanotubes catalyzed CO2 methanation

Han,

Zhang,

Zhang

et al. 2024

Chemical Engineering Journal

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Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

Cited by 15 publications

References 70 publications

Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

Boosting low-temperature CO2 methanation activity through Tailored electronic structures and step-edge defects in Niε−-Ov-Ceδ+ inverse interfaces

Promotional role of Ni photodepositing on Ru confined TiO2 nanotubes catalyzed CO2 methanation

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Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

Cited by 15 publications

References 70 publications

Overturning CO2 Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO2 Catalysts

Overturning CO2 Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO2 Catalysts

Boosting low-temperature CO2 methanation activity through Tailored electronic structures and step-edge defects in Niε−-Ov-Ceδ+ inverse interfaces

Promotional role of Ni photodepositing on Ru confined TiO2 nanotubes catalyzed CO2 methanation

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Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts

Overturning CO₂ Hydrogenation Selectivity by Tailoring the Local Electron Density of Ru/CeO₂ Catalysts