期刊
NANO TODAY
卷 35, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.nantod.2020.100944
关键词
Catalytic ozonation; S-VOCs; Tandem catalysis; Density functional calculations; Heterogeneous catalysis
资金
- National Natural Science Foundation of China [51578556, 21876212, 41573086, 41603097, 21976214]
- Natural Science Foundation of Guangdong Province [2015A030308005, S2013010012927, S2011010003416]
- Science and Technology Research Programs of Guangdong Province [2014A020216009, 2019A1515011015]
- Science and Technology Program of Guangzhou [201904010353]
- Fundamental Research Funds for the Central Universities [13lgjc10, 19lgpy157]
- Start-up Funds for High-Level Talents of Sun Yat-sen University [38000-18821111]
Tandem catalysis can carry out the sequential coupling of multiple reactions in one operation, which is promising for sulfur-containing volatile organic compounds (S-VOCs) control. Herein, a tandem catalyst (CuO/V-O-MnO2) consisting of well-dispersed CuO shell and oxygen vacancy-rich (V-O) hollow-structured MnO2 core exhibited superior adsorption and catalytic performance under the mild condition for the elimination of CH3SH. The optimum 5CuO/V-O-MnO2 can reach a significant improvement in CH3 SH elimination of 99 % conversion over bare CuO/ pristine MnO2 at 25 degrees C under a GHSV of 60,000 mL h(-1) g(-1), and an almost 4-fold enhanced catalytic activity of the individual 03 with similar to 99 % utilization of the applied 03 in the feed gas. The underlying tandem catalytic mechanism was in-depth identified by XPS, in situ DRIFTs and high-level computational study. The secret to the superior performance of CuO/V-O-MnO2 lies in that CH3SH was preferentially chemisorbed on multivalent CuO (Cu(I)/Cu(II)), then deeply oxidized into final product of SO42- /CO32- via the catalytic ozonation by multivalent CuO and oxygen vacancies of neighbouring V-O-MnO2. Attributed to the efficient electron replenishing interaction and cycling of active oxygen vacancies at the tandem reactive site of CuO/V-O-MnO2 interface ( Mn(IV) + Cu(II) + 20(latt) -> Mn(II)/Mn(III) + V-O + Cu(I) + O-2), its lifetime can extend to 300 min with limited loss of activity. These findings thus open up a way to address current multiple challenges in S-VOCs control using a single hierarchical core -shell structure with tandem catalysis. (C) 2020 Elsevier Ltd. All rights reserved.
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