Citation: Shibo Zhang, Xiang Chu, Meng Zhao, Baokang Geng, Xiao Wang, Shuyan Song, Hongjie Zhang. Ba-doping to modulate surface electronic states in Eu_0.9Ba_0.1O_x catalysts for oxidation coupling of methane[J]. Chinese Chemical Letters, ;2026, 37(7): 111126. doi: 10.1016/j.cclet.2025.111126 shu

Ba-doping to modulate surface electronic states in Eu_0.9Ba_0.1O_x catalysts for oxidation coupling of methane

Shibo Zhang ^{a, b} ,
Xiang Chu ^{a, b} ,
Meng Zhao ^{a, *,} ,
Baokang Geng ^{a, b} ,
Xiao Wang ^{a, b, *,} ,
Shuyan Song ^{a, b, *,} ,
Hongjie Zhang ^{a, b, c, *,}

a.
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
b.
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China
c.
Department of Chemistry, Tsinghua University, Beijing 100084, China

Received Date: 11 January 2025
Revised Date: 14 March 2025
Accepted Date: 20 March 2025
Available Online: 20 March 2025

Figures(4)

The oxidative coupling reaction of methane (OCM) process offers a promising pathway for the direct conversion of methane into high value C₂ hydrocarbons (C₂H₆ and C₂H₄), albeit facing the challenges of harsh reaction conditions and competing overoxidation reaction. Herein, Ba-doped Eu₂O₃ synthesized via the spray pyrolysis method was employed as highly active dopant catalyst for the methane oxidative coupling reaction. The prepared Eu_0.9Ba_0.1O_x catalyst showed satisfactory reactivity and stability, with a C₂₊ product selectivity of 52.4%, a C₂₊ yield of 16.2%, and a stabilization time of at least 100 h. The incorporation of Ba atoms into Eu₂O₃ lattice leads to an increased molar ratio of Eu²⁺/Eu³⁺ and a higher oxygen vacancies (O_v) concentration. Such modulation of surface electronic state significantly improves the adsorption and activation behavior of oxygen, thereby accelerating the production of reactive oxygen species (O₂⁻). Meanwhile, the acid-base properties of Eu₂O₃ substrate also undergo obvious alteration with more basic site generation after Ba doping, which is conducive to the stabilization activated oxygen. O₂⁻ substances can promote the activation of methane into methyl radicals, and also facilitate the dehydrogenation of ethane into ethylene, thus improving the catalytic activity.
- Oxidative coupling of methane,
- Spray pyrolysis,
- Ba-doping,
- Oxygen vacancies,
- Europium oxide
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Ba-doping to modulate surface electronic states in Eu0.9Ba0.1Ox catalysts for oxidation coupling of methane

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通讯作者: 陈斌, bchen63@163.com

Ba-doping to modulate surface electronic states in Eu_0.9Ba_0.1O_x catalysts for oxidation coupling of methane