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Self-molten-polymerization synthesis of highly defected Mn/Sm binary oxides with mesoporous structures for efficient removal of toluene and chlorobenzene

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Abstract

A simple and effective self-molten-polymerization strategy utilizing the molten metal salts from heated solid metal salt sources as the solvents to dissolve a self-polymerizable monomer, which acted as a mingling agent, was successfully applied to homogeneously synthesize a series of highly defected manganese/samarium (Mn/Sm-x, where x represents the molar ratio of Mn to Sm) hybrid bimetallic oxides with a mesoporous structure. The values of T50 and T90 over Mn/Sm-2 were 206 °C and 247 °C, respectively, for toluene conversion, as well as 213 °C and 273 °C for CO2 yield under saturated vapor with a weight hourly space velocity of 60 000 ml g−1 h−1, which were far superior to the performances of Mn/Cu-2 (233 °C and 274 °C; 237 °C and 300 °C) and MnOx (242 °C and 294 °C; 255 °C and 315 °C). Meanwhile, the most active catalyst Mn/Sm-4 exhibited complete mineralization of chlorobenzene under saturated vapor and a weight hourly space velocity of 60 000 ml g−1 h−1 at 350 °C. In addition, the Mn/Sm-4 catalyst also showed a high TOFMn value (8.35 × 10−6 s−1) at 140 °C for toluene oxidation and good stability for the catalytic oxidation of toluene and chlorobenzene under a long-term test running for 200 h of uninterrupted reaction. The XRD, Raman, N2 adsorption–desorption, FESEM, XPS, O2-TPD and H2-TPR results confirmed that more surface defects and surface oxygen vacancies were introduced into MnOx using proper doping with Sm. Combined with the in situ DRIFTS and on-line MS measurements, the mechanism for chlorobenzene oxidation over Mn/Sm-4 was also revealed. This work presents an important interpretation for developing improved catalysts to control air pollution.

Graphical abstract: Self-molten-polymerization synthesis of highly defected Mn/Sm binary oxides with mesoporous structures for efficient removal of toluene and chlorobenzene

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Publication details

The article was received on 10 Jan 2019, accepted on 11 Mar 2019 and first published on 12 Mar 2019


Article type: Research Article
DOI: 10.1039/C9QI00039A
Citation: Inorg. Chem. Front., 2019, Advance Article

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    Self-molten-polymerization synthesis of highly defected Mn/Sm binary oxides with mesoporous structures for efficient removal of toluene and chlorobenzene

    L. Liu, H. Zhang, M. Guo, P. Zhou, X. Min, J. Jia and T. Sun, Inorg. Chem. Front., 2019, Advance Article , DOI: 10.1039/C9QI00039A

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