4.8 Article

Au decorated Pd nanowires for methane oxidation to liquid C1 products

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 308, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2022.121223

Keywords

Methane oxidation; Bimetallic PdAu nanowires; Selectivity; Reaction mechanism; Synergistic effects

Funding

  1. Technology Special Fund [(2022) 121223]
  2. National Nat-ural Science Foundation of China [ZDYF2020037, 2020207]
  3. Postdoctoral Science Foundation of Hainan Province [21805104, 22109034, 22109035, 52164028, 62105083]
  4. Innovative Research Projects for Grad-uate Students of Hainan Province [RZ2100007123]
  5. Basic and Applied Basic Research Foundation of Guangdong Province [Qhyb2021-20]
  6. Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province [2019A1515110558]
  7. Start-up Research Foundation of Hainan University (KYQD) [202021]
  8. [20082]
  9. [20083]
  10. [20084]
  11. [21065]
  12. [21125]

Ask authors/readers for more resources

Direct methane oxidation to high value-added C1 chemicals is a promising strategy. This study explores the atomic-level effect of PdAu atoms on the reaction and finds that Pd9Au1 nanowires exhibit the highest yield and selectivity.
The direct methane (CH4) oxidation to high value-added C1 chemicals is a great promising strategy to explore the CH4 resource utilization. However, the low activity and selectivity of catalytic performance remains a great conundrum due to the difficulty to activate the C-H bond and the unmanageable over oxidation. Herein, PdxAuy nanowires (NWs) with various Pd/Au atomic ratios are presented as ideal models to explore the atomic-level effect of PdAu atoms for the direct CH4 oxidation. The influence of reaction parameters are systematically investigated, and Pd9Au1 NWs display a maximum yield of 2890.3 mu mol g(-1) h(-1) with 99% selectivity for the liquid C1 oxygenated products. This enhanced performance is attributed to the combination of one-dimensional structure and the synergistic effect from the suitable portion of Au on Pd sites, which regulates bond strength between adsorbed radicals (center dot OH,center dot OOH, center dot CH3) and PdAu atoms, confirmed by the density function theory calculations.

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