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...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℃and 247℃,respectively,for toluene conversion,as well as 213℃and 273℃for CO_(2) yield under saturated vapor with a weight hourly space velocity of 60000 ml g^(−1)h^(−1),which were far superior to the performances of Mn/Cu-2(233℃and 274℃;237℃and 300℃)and MnO_(x)(242℃and 294℃;255℃and 315℃).Meanwhile,the most active catalyst Mn/Sm-4 exhibited complete mineralization of chlorobenzene under saturated vapor and a weight hourly space velocity of 60000 ml g^(−1)h^(−1)at 350℃.In addition,the Mn/Sm-4 catalyst also showed a high TOFMn value(8.35×10^(−6)s^(−1))at 140℃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,N_(2)adsorption–desorption,FESEM,XPS,O2-TPD and H_(2)-TPR results confirmed that more surface defects and surface oxygen vacancies were introduced into MnO_(x)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.展开更多
基金the National Natural Science Foundation of China(Grant No:21876107,21507082,21377083)the special development fund of the Shanghai Zhangjiang National Innovation Demonstration Zone(Grant No:201505-Q P-B108-006)for their financial support.
文摘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℃and 247℃,respectively,for toluene conversion,as well as 213℃and 273℃for CO_(2) yield under saturated vapor with a weight hourly space velocity of 60000 ml g^(−1)h^(−1),which were far superior to the performances of Mn/Cu-2(233℃and 274℃;237℃and 300℃)and MnO_(x)(242℃and 294℃;255℃and 315℃).Meanwhile,the most active catalyst Mn/Sm-4 exhibited complete mineralization of chlorobenzene under saturated vapor and a weight hourly space velocity of 60000 ml g^(−1)h^(−1)at 350℃.In addition,the Mn/Sm-4 catalyst also showed a high TOFMn value(8.35×10^(−6)s^(−1))at 140℃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,N_(2)adsorption–desorption,FESEM,XPS,O2-TPD and H_(2)-TPR results confirmed that more surface defects and surface oxygen vacancies were introduced into MnO_(x)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.
