Synthesis of γ-Mo<sub>2</sub>N/C catalysts and its performance on formic acid dehydrogenation

LU Jun; WANG Meijun; WANG Zhiqing; DONG Libo; YU Zhongliang; CHANG Liping

doi:10.19906/j.cnki.JFCT.2023063

Volume 52 Issue 1

Jan. 2024

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Article Navigation > Journal of Fuel Chemistry and Technology > 2024 > 52(1): 76-86

LU Jun, WANG Meijun, WANG Zhiqing, DONG Libo, YU Zhongliang, CHANG Liping. Synthesis of γ-Mo2N/C catalysts and its performance on formic acid dehydrogenation[J]. Journal of Fuel Chemistry and Technology, 2024, 52(1): 76-86. doi: 10.19906/j.cnki.JFCT.2023063

Citation:

LU Jun, WANG Meijun, WANG Zhiqing, DONG Libo, YU Zhongliang, CHANG Liping. Synthesis of γ-Mo₂N/C catalysts and its performance on formic acid dehydrogenation[J]. Journal of Fuel Chemistry and Technology, 2024, 52(1): 76-86. doi: 10.19906/j.cnki.JFCT.2023063

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Synthesis of γ-Mo₂N/C catalysts and its performance on formic acid dehydrogenation

doi: 10.19906/j.cnki.JFCT.2023063

LU Jun^{1, 2, 3
,},
WANG Meijun^{1, 2
,
,},
WANG Zhiqing^3
,,
DONG Libo^3
,,
YU Zhongliang^4
,,
CHANG Liping^{1, 2
,}

1.
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China
2.
Key Laboratory of Coal Science and Technology, Taiyuan University of Technology, Ministry of Education, Taiyuan 030024, China
3.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
4.
School of Chemistry and Environmental Science, Shangrao Normal University, Shangrao 334001, China

Received Date: 2023-03-02
Accepted Date: 2023-04-10
Rev Recd Date: 2023-04-09

Available Online: 2023-09-18

Publish Date: 2024-01-09

Abstract

Abstract

Formic acid (FA) has received much attention due to its high hydrogen content (4.4%), easy H₂ production and synthesis from small platform compounds. γ-Mo₂N/C is very selective for the decomposition of FA along the H₂ and CO₂ pathways, generating very little CO and showing high application value. In this study, γ-Mo₂N/C catalysts were prepared using aqueous p-phenylenediamine and ammonium molybdate solutions as precursors, and their FA decomposition performance was evaluated in-situ. The adsorption conformation of FA on the crystalline surface of γ-Mo₂N (200) was calculated by DFT, and on this basis, the catalyst performance and the decomposition mechanism of FA on its surface were investigated. The results showed that γ-Mo₂N/C exhibited very high catalytic activity at low temperatures and that improving the dispersion of γ-Mo₂N on the C carrier was effective in improving the FA conversion. The best catalytic performance was achieved at a molar ratio of 4∶1 between p-phenylenediamine and ammonium molybdate, and the catalyst showed stable performance and high H₂ selectivity (N₂ 40 mL/min, CO<5.0×10⁻⁵) in the FA decomposition experiments at 160 ℃ and 100 h. DFT calculations showed that the H atom of the O−H bond in FA was more likely to bind to the N atom on the crystalline surface of γ-Mo₂N/C (200), while the O atom of the C=O bond are more likely to bind to Mo atoms on the γ-Mo₂N/C (200) crystal plane. The above results help to clarify the mechanism of FA decomposition under the action of γ-Mo₂N/C and show the potential application of the non-precious metal catalyst γ-Mo₂N/C in the decomposition of FA for H₂ production.
- coal-based derivatives utilization,
- hydrogen production from formic acid,
- γ-Mo₂N,
- loaded catalyst,
- hydrogen energy

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References(32)

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