期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 263, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2019.117829
关键词
Hg-0 catalytic oxidation; Molybdenum-manganese catalyst; Synergistic effect; Defect surface; DFT
资金
- National Key Research and Development Projects [2017YFB0603202]
- National Natural Science Foundation of China [51706114, 51836006]
- Ningbo 'Science and Technology Innovation 2025' Major Project
- Ningbo Natural Science Foundation [2017A610060]
- Postdoctoral International Exchange Program
The challenge of Hg-0 emission control has necessitated the development of catalytic oxidation technology. Herein, a combination of experimental and computational approach to explore the potential over Mo-Mn catalysts was conducted. Series of catalysts were synthesized and characterized with varying Mn and Mo loading (1-10%). Among the various compositions, 1.25Mo2 Mn catalyst exhibited the best Hg-0 removal performance with Hg(0 )removal efficiency > 98% (oxidation ratio > 50%, and better stability over 10 h period at 250 degrees C). Most importantly, the synergistic interaction between MoO3 and defective delta-MnO2 nanosheet was promoted by the adjusted activation energy, bond strength, Bronsted acidic sites and defects, which facilitated the catalytic oxidation of Hg-0 to Hg2+. Furthermore, DFT calculations suggested that the role of Mo enabled the reduction in the energy barrier for the desorption step, which was defined as the rate-determining step for catalytic oxidation of Hg-0 on Mn-based catalyst.
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