The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potent...The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potential option in the activity-preferred ODS systems.Herein,we reported the redispersion of vanadium oxide(VO_(χ))on the mesoporous silica modified with manganese oxide(Mn_(3)O_(4)) through one progressive insertion approach of metal oxides in the silica.Impressively,mesoporeencaged vanadium-manganese oxides in the silica(VMn-MS)as the admirable output of excellent ODS catalyst was demonstrated compared to other monometal-modified counterparts and one-pot implanted one.The characterization results revealed the post-implanted VO_(χ) species not only deposited around the pre-covered Mn_(3)O_(4) on the mesoporous surface but also inserted the surface layer of Mn_(3)O_(4) inducing the amorphous evolution of aggregated Mn_(3)O_(4) and the reconstruction of final active sites.This integrated approach made the reconstructed active species afford more exposed catalytic sites and the tailored surface redox cycles owing to the electronic communication of V-Mn.The catalytic results demonstrated the excellent catalytic desulphurization efficiency(~100%)during 60 min at 80℃,which made the sulphur content reduce to 6 mg·L^(-1),remarkably superior to other comparative samples.The outstanding catalytic performance of VMn-MS catalyst can be ascribed to the synergistic effect of V-Mn dual metals rendering two different reaction pathways,which includes free-radical reaction and ring-forming reaction,where Mn site acted as active center triggering reactive free radicals which could be further optimized by surrounded V sites around Mn sites to promote the ODS process.展开更多
基金National Natural Science Foundation of China(No.21908085,21776129,and 21706121)Natural Science Foundation of Jiangsu Province(No.BK20170995 and BK20190961)+1 种基金General Program for University Natural Science Research of Jiangsu Province(No.16KJB530003)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘The oxidative desulphurization(ODS)has become mainly popular by rapid catalytic oxidation of dibenzothiophene(DBT)relied on efficient heterogeneous catalyst,V-based catalytic active species were regarded as the potential option in the activity-preferred ODS systems.Herein,we reported the redispersion of vanadium oxide(VO_(χ))on the mesoporous silica modified with manganese oxide(Mn_(3)O_(4)) through one progressive insertion approach of metal oxides in the silica.Impressively,mesoporeencaged vanadium-manganese oxides in the silica(VMn-MS)as the admirable output of excellent ODS catalyst was demonstrated compared to other monometal-modified counterparts and one-pot implanted one.The characterization results revealed the post-implanted VO_(χ) species not only deposited around the pre-covered Mn_(3)O_(4) on the mesoporous surface but also inserted the surface layer of Mn_(3)O_(4) inducing the amorphous evolution of aggregated Mn_(3)O_(4) and the reconstruction of final active sites.This integrated approach made the reconstructed active species afford more exposed catalytic sites and the tailored surface redox cycles owing to the electronic communication of V-Mn.The catalytic results demonstrated the excellent catalytic desulphurization efficiency(~100%)during 60 min at 80℃,which made the sulphur content reduce to 6 mg·L^(-1),remarkably superior to other comparative samples.The outstanding catalytic performance of VMn-MS catalyst can be ascribed to the synergistic effect of V-Mn dual metals rendering two different reaction pathways,which includes free-radical reaction and ring-forming reaction,where Mn site acted as active center triggering reactive free radicals which could be further optimized by surrounded V sites around Mn sites to promote the ODS process.
