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author:

Wang, X.-G. (Wang, X.-G..) [1] | Qiao, L.-Y. (Qiao, L.-Y..) [2] | Xu, L.-Y. (Xu, L.-Y..) [3] | Zeng, Y.-Y. (Zeng, Y.-Y..) [4] | Huang, Z.-S. (Huang, Z.-S..) [5] | Zong, S.-S. (Zong, S.-S..) [6] | Wang, J.-X. (Wang, J.-X..) [7] | Zhou, Z.-F. (Zhou, Z.-F..) [8] | Yao, Y.-G. (Yao, Y.-G..) [9]

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Abstract:

The intrinsic nature of irreducible oxides (e.g. Al2O3) makes it hard to tune the charge state of supported late-transition metals, then difficult to adjust the selectivity of catalysts in CO2 hydrogenation. Herein, we find that modifying the Pd/Al2O3 catalyst with alkali metals (especially potassium) is efficient to boost the CO formation in CO2 hydrogenation. In comparison to Pd/Al2O3, approximately twenty-fold promotion in reverse water–gas shift (RWGS) rate was achieved on K-modified catalysts with proper K/Pd proportions. Combined structural characterizations demonstrate that the enhanced Pd-O interactions through K mediation stabilize the ca. 2 nm sized Pd particles as well as the electron-deficient state of Pd, which are robust enough during long-termed evaluation with undamped performance. In situ spectroscopy unveils a bi-dentate *HCOO associated reaction mechanism taking effect on alkali-modified catalysts, which contributes to ∼ 100 % of CO selectivity and 3318.1 mmol∙gPd-1∙h−1 of CO formation rate at 340°C. © 2024 Elsevier B.V.

Keyword:

Alkali metal CO2 hydrogenation CO production Pd-based catalyst Reverse water–gas shift

Community:

  • [ 1 ] [Wang X.-G.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 2 ] [Wang X.-G.]College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 3 ] [Qiao L.-Y.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 4 ] [Xu L.-Y.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 5 ] [Xu L.-Y.]College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 6 ] [Zeng Y.-Y.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 7 ] [Zeng Y.-Y.]College of Chemistry and Materials Science, Fujian Normal University, Fuzhou, 350007, China
  • [ 8 ] [Huang Z.-S.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 9 ] [Huang Z.-S.]College of Chemistry and Materials Science, Fujian Normal University, Fuzhou, 350007, China
  • [ 10 ] [Zong S.-S.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 11 ] [Wang J.-X.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 12 ] [Wang J.-X.]College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 13 ] [Zhou Z.-F.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 14 ] [Yao Y.-G.]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China

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Source :

Chemical Engineering Journal

ISSN: 1385-8947

Year: 2024

Volume: 500

1 3 . 4 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 3

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