Applied Catalysis2022，Vol.31521.DOI:10.1016/j.apcatb.2022.121533

CO2 hydrogenation: Selectivity control of CO versus CH4 achieved using Na doping over Ru/m-ZrO2 at low pressure

Martinelli, Michela Rabelo-Neto, Raimundo C. Almeida, Mayra P. Silveira, Erika B. Ayala, Martin Watson, Caleb D. Villarreal, Jesus Cronauer, Donald C. Kropf, A. Jeremy Noronha, Fabio B. Jacobs, Gary
Applied Catalysis2022，Vol.31521.DOI:10.1016/j.apcatb.2022.121533
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  • NSTL
  • Elsevier

CO2 hydrogenation: Selectivity control of CO versus CH4 achieved using Na doping over Ru/m-ZrO2 at low pressure

Martinelli, Michela 1Rabelo-Neto, Raimundo C. 2Almeida, Mayra P. 2Silveira, Erika B. 2Ayala, Martin 3Watson, Caleb D. 3Villarreal, Jesus 3Cronauer, Donald C. 4Kropf, A. Jeremy 4Noronha, Fabio B. 2Jacobs, Gary3
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作者信息

  • 1. Univ Kentucky Ctr Appl Energy Res
  • 2. Inst Nacl Tecnol
  • 3. Univ Texas San Antonio
  • 4. Argonne Natl Lab
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Abstract

By doping 1%Ru/m-ZrO2 with sodium, selectivity tuning between CO and CH4 during CO2 hydrogenation was achieved by controlling the relative rates of reverse water-gas shift and CO methanation. By increasing basicity through Na loading: (1) the formate C-H bond is weakened in DRIFTS of adsorbed CO, accelerating C-H bond formation of formate and promoting CO formation at the Ru/m-ZrO2 interface; and (2) the coverage of Na increases on ensembles of Ru atoms responsible for methanation. Increasing Na content shifts selectivity from CH4 (useful for synthetic natural gas) to CO, which can be used for Fischer-Tropsch synthesis or methanol-to-gasoline. Electronic modification of formate is likely due to enhanced basicity (strengthening bonding between catalyst and the-CO2 function of formate and weakening C-H). No electron transfer from Na to Ru was detected in XANES. DRIFTS as a function of time and XPS results showed that Na exacerbates site blocking and deactivation.

Key words

Ru/zirconia/Sodium doping/CO2 hydrogenation/Reverse water-gas shift/Methanation/WATER-GAS-SHIFT/RAY-ABSORPTION-SPECTROSCOPY/H BOND/CATALYST/ALKALI/DECOMPOSITION/METHANATION/FORMATE/ALUMINA/ZRO2

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN：0926-3373
被引量8
参考文献量51
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