Photo-assisted SCR(PSCR) offers a potential solution for removal of NO at room temperature. MnTiO_(x)as PSCR catalyst exhibits superior performance with NO removal of 100% at the room temperature. Electron paramagneti...Photo-assisted SCR(PSCR) offers a potential solution for removal of NO at room temperature. MnTiO_(x)as PSCR catalyst exhibits superior performance with NO removal of 100% at the room temperature. Electron paramagnetic resonance(EPR) analysis revealed the presence of numerous oxygen vacancies on MnTiO_(x). Optical carrier density functional theory(DFT) calculations showed that the threedimensional orbital hybridization of Mn and Ti is significantly enhanced under light irradiation. The MnTiO_(x)catalyst exhibited excellent electron–hole separation ability, which can adsorbe NH_(3)and dissociate to form NH_(2)fragments and H atoms. In-situ diffuse reflectance infrared fourier-transform spectroscopy(DRIFTS) indicated that the optical carrier enhanced NH_(3)adsorption on MnTiO_(x), which makes it possess excellent PSCR activity. This work provided an additional strategy to NO removal with PSCR catalysts and showed potential for use in photocatalysis.展开更多
Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assi...Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.展开更多
We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitatio...We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.展开更多
In this study,the ultralow specific surface area clay vermiculite(VMT)was selected to be a catalyst support for the NH_(3)-SCR process,and the active components MnCeFeO_(x)loaded on vermiculite was just like curling o...In this study,the ultralow specific surface area clay vermiculite(VMT)was selected to be a catalyst support for the NH_(3)-SCR process,and the active components MnCeFeO_(x)loaded on vermiculite was just like curling on ice from the TEM results.The de-NO_(x)performance of Mn-Ce-Fe/VMT exhibited almost complete NO conversion with a gas hourly space velocity(GHSV)of 15,300 h^(-1)at 150℃,which was 25%and 10%higher than that of Mn/VMT and Mn-Ce/VMT,respectively.Ce and Fe co-doping improved the BET surface area,the quantities of active Mn^(4+),the acid sites and NH_(3)adsorption energy of Mn/VMT,all of which contributed to the increase in low-temperature SCR activity.In situ DRIFT measurements suggested that NO_(x)removal over Mn-Ce-Fe/VMT followed both Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)mechanisms at 150℃,but the E-R mechanism played a dominant role.Corresponding Mn-Ce-Fe/VMT monolithic catalysts reached 90%NO conversion with a GHSV of 4000 h^(-1).展开更多
基金supported by Science and Technology Innovation Talents Program of Bingtuan (No.2019CB025)Major Scientific and Technological Project of Bingtuan (No.2018AA002)Project of Regional Innovation in Bingtuan (No.2021BB005)。
文摘Photo-assisted SCR(PSCR) offers a potential solution for removal of NO at room temperature. MnTiO_(x)as PSCR catalyst exhibits superior performance with NO removal of 100% at the room temperature. Electron paramagnetic resonance(EPR) analysis revealed the presence of numerous oxygen vacancies on MnTiO_(x). Optical carrier density functional theory(DFT) calculations showed that the threedimensional orbital hybridization of Mn and Ti is significantly enhanced under light irradiation. The MnTiO_(x)catalyst exhibited excellent electron–hole separation ability, which can adsorbe NH_(3)and dissociate to form NH_(2)fragments and H atoms. In-situ diffuse reflectance infrared fourier-transform spectroscopy(DRIFTS) indicated that the optical carrier enhanced NH_(3)adsorption on MnTiO_(x), which makes it possess excellent PSCR activity. This work provided an additional strategy to NO removal with PSCR catalysts and showed potential for use in photocatalysis.
基金supported by Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025)Major Scientific and Technological Project of Bingtuan(No.2018AA002)。
文摘Low temperature catalysts are attracting increasing attention in the selective catalytic reduction(SCR)of NO with NH3.Mn Ox-decorated Mg Al layered double oxide(Mn/Mg Al-LDO)was synthesized via a facile fast pour assisted co-precipitation(FP-CP)process.Compared to the Mn/Mg Al-LDO obtained via slow drop assisted coprecipitation(SD-CP)method,the Mn/Mg Al-LDO(FP-CP)has excellent activity.The Mn/Mg Al-LDO(FP-CP)catalyst was shown to possess a high NO conversion rate of 76%-100%from 25 to 150℃,which is much better than the control Mn/Mg Al-LDO(SD-CP)(29.4%-75.8%).In addition,the Mn/Mg Al-LDO(FP-CP)offered an enhanced NO conversion rate of 97%and a N2selectivity of 97.3%at 100℃;the NO conversion rate was 100%and the N2selectivity was 90%at 150℃with a GHSV of 60,000 h^-1.The Mn/Mg Al-LDO(FP-CP)catalyst exhibited a smaller fragment nano-sheet structure(sheet thickness of 7.23 nm).An apparent lattice disorder was observed in the HRTEM image confirming the presence of many defects.The H2-TPR curves show that the Mn/Mg Al-LDO(FP-CP)catalyst has abundant reducing substances.Furthermore,the enhanced surface acidity makes the NH3concentration of the Mn/Mg Al-LDO(FP-CP)catalyst lower than 100 ml·m^-3after the reaction from 25 to 400℃.This can effectively reduce the ammonia escape rate in the SCR reaction.Thus,the Mn/Mg Al-LDO(FP-CP)catalyst has potential applications in stationary industrial installations for environmentally friendly ultra-low temperature SCR.
基金supported by Major Scientific and Technological Project of Bingtuan (No.2018AA002)the Program for Changjiang Scholars and Innovative Research Team in University (No. IRT_15R46)
文摘We rationally designed a high performance denitration(De-NOx) catalyst based on a micrometer-sized spherical Mn–Ce–Fe–Ti(CP-SD)catalyst for selective catalytic reduction(SCR). This was prepared by a co-precipitation and spray drying(CP-SD) method. The catalyst was systematically characterized, and its morphological structure and surface properties were identified. Compare with conventional Mn–Ce–Fe–Ti(CP) catalysts, the Mn–Ce–Fe–Ti(CP-SD) catalyst had superior surface-adsorbed oxygen leading to enhanced 'fast NH3-SCR' reaction. The asobtained Mn–Ce–Fe–Ti(CP-SD) catalyst offered excellent NO conversion and N2 selectivity of 100.0% and 84.8% at 250℃, respectively, with a gas hourly space velocity(GHSV) of 40,000 h-1. The porous micro-spherical structure provides a larger surface area and more active sites to adsorb and activate the reaction gases. In addition, the uniform distribution and strong interaction of manganese, iron, cerium, and titanium oxide species improved H2O and SO2 resistance. The results showed that the Mn–Ce–Fe–Ti(CP-SD) catalyst could be used prospectively as a denitration(De-NOx) catalyst.
基金supported by the Program of Science and Technology Innovation Team in Bingtuan(No.2020CB006)Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025)Major Scientific and Technological Project of Bingtuan(No.2018AA002).
文摘In this study,the ultralow specific surface area clay vermiculite(VMT)was selected to be a catalyst support for the NH_(3)-SCR process,and the active components MnCeFeO_(x)loaded on vermiculite was just like curling on ice from the TEM results.The de-NO_(x)performance of Mn-Ce-Fe/VMT exhibited almost complete NO conversion with a gas hourly space velocity(GHSV)of 15,300 h^(-1)at 150℃,which was 25%and 10%higher than that of Mn/VMT and Mn-Ce/VMT,respectively.Ce and Fe co-doping improved the BET surface area,the quantities of active Mn^(4+),the acid sites and NH_(3)adsorption energy of Mn/VMT,all of which contributed to the increase in low-temperature SCR activity.In situ DRIFT measurements suggested that NO_(x)removal over Mn-Ce-Fe/VMT followed both Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)mechanisms at 150℃,but the E-R mechanism played a dominant role.Corresponding Mn-Ce-Fe/VMT monolithic catalysts reached 90%NO conversion with a GHSV of 4000 h^(-1).