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author:

Ye, Hanfeng (Ye, Hanfeng.) [1] | Xing, Wandong (Xing, Wandong.) [2] (Scholars:邢万东) | Zhao, Fei (Zhao, Fei.) [3] | Wang, Jiali (Wang, Jiali.) [4] | Yang, Can (Yang, Can.) [5] (Scholars:阳灿) | Hou, Yidong (Hou, Yidong.) [6] (Scholars:侯乙东) | Zhang, Jinshui (Zhang, Jinshui.) [7] (Scholars:张金水) | Yu, Jimmy C. (Yu, Jimmy C..) [8] | Wang, Xinchen (Wang, Xinchen.) [9] (Scholars:王心晨)

Indexed by:

EI Scopus SCIE

Abstract:

Understanding the relationship of competitive adsorption between reactants is the prerequisite for high activity and selectivity in heterogeneous catalysis, especially the difference between the adsorption energies (E-ads) of two reactive intermediates in Langmuir-Hinshelwood (L-H) models. Using oxidative dehydrogenation of hydrogen sulfide (H2S-ODH) as a probe, we develop various metal single atoms on nitrogen-doped carbon (M-NDC) catalysts for controlling E-ads-H2S, E-ads-O-2 and investigating the difference in activity and selectivity. Combining theoretical and experimental results, a Sabatier relationship between the catalytic performance and E-ads-O-2/E-ads-H2S emerges. Mn-NDC as the optimal catalyst shows excellent H2S conversion (>90 %) and sulfur selectivity (>90 %) in a wide range of O-2 concentrations over 100 h. Such a high-efficiency performance is attributed to appropriate E-ads-H2S and E-ads-O-2 on Mn-N-4 sites, boosting redox cycle between Mn2+ and Mn3+, as well as preferential formation of sulfur. This work provides a fundamental guidance for designing Sabatier optimal catalysts in L-H models.

Keyword:

high-efficiency reactivity descriptors nitrogen-doped carbon Sabatier principle selective oxidative desulfurization single atoms

Community:

  • [ 1 ] [Ye, Hanfeng]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 2 ] [Xing, Wandong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 3 ] [Zhao, Fei]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 4 ] [Wang, Jiali]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 5 ] [Yang, Can]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 6 ] [Hou, Yidong]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 7 ] [Zhang, Jinshui]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 8 ] [Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China
  • [ 9 ] [Yu, Jimmy C.]Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong 999077, NT, Peoples R China

Reprint 's Address:

  • 阳灿 王心晨

    [Yang, Can]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China;;[Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Fujian, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2024

Issue: 7

Volume: 64

1 6 . 1 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 1

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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