A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts (Ce:Mn:Al mole ratio=6:4:x, x=0.25, 0.5, 1, 2) were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorpo...A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts (Ce:Mn:Al mole ratio=6:4:x, x=0.25, 0.5, 1, 2) were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorporation of Al3+ into CeO2‐MnOx mixed oxides. CeO2‐MnOx, CeO2‐Al2O3, and MnOx‐Al2O3 mixed oxides, and CeO2 were prepared by the same method for comparison. The samples were characterized by XRD, Raman, N2 physisorption, H2‐TPR, XPS, and in situ DRIFTS. The catalytic re‐duction of NO by CO was chosen as a model reaction to evaluate the catalytic performance. The incorporation of a small amount of Al3+into CeO2‐MnOx mixed oxides resulted in a decrease of crys‐tallite size, with the increase of the BET specific surface area and pore volume, as well as the in‐crease of Ce3+and Mn4+. The former benefits good contact between catalyst and reactants, and the latter promotes the adsorption of CO and the desorption, conversion and dissociation of adsorbed NO. All these enhanced the catalytic performance for the NO+CO model reaction. A reaction mecha‐nism was proposed to explain the excellent catalytic performance of CeO2‐MnOx‐Al2O3 catalysts for NO reduction by CO.展开更多
By means of both a theory for pressure-induced shifts (PS) of energy spectra and a theory for shifts of energy spectra due to electron-phonon interaction (EPI), the 'pure electronic' PS and the PS due to EPI o...By means of both a theory for pressure-induced shifts (PS) of energy spectra and a theory for shifts of energy spectra due to electron-phonon interaction (EPI), the 'pure electronic' PS and the PS due to EPI of R<SUB>1</SUB> line, R<SUB>2</SUB> line, and U band of GSGG:Cr<SUP>3+</SUP> at 300 K have been calculated, respectively. The calculated results are in good agreement with all the experimental data. Their physical origins have also been explained. It is found that the mixing-degree of and base-wavefunctions in the wavefunctions of R<SUB>1</SUB> level of GSGG:Cr<SUP>3+</SUP> at 300 K is remarkable under normal pressure, and the mixing-degree rapidly decreases with increasing pressure. The change of the mixing-degree with pressure plays a key role not only for the 'pure electronic' PS of R<SUB>1</SUB> line and R<SUB>2</SUB> line but also the PS of R<SUB>1</SUB> line and R<SUB>2</SUB> line due to EPI. The pressure-dependent behaviors of the 'pure electronic' PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line) and the PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line) due to EPI are quite different. It is the combined effect of them that gives rise to the total PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line). In the range of about 15 kbar ~ 45 kbar, the mergence and/or order-reversal between levels and levels take place, which cause the fluctuation of the rate of PS for with pressure. At 300 K, both the temperature-dependent contribution to R<SUB>1</SUB> line (or R<SUB>2</SUB> line or U band) from EPI and the temperature-independent one are important.展开更多
基金supported by the National Natural Science Foundation of China (21507130)the Open Project Program of Chongqing Key Laboratory of Environmental Materials and Remediation Technology from Chongqing University of Arts and Sciences (CEK1405)+3 种基金the Open Project Program of Beijing National Laboratory for Molecular Sciences (20140142)the Open Project Program of Jiangsu Key Laboratory of Vehicle Emissions Control (OVEC001)the Open Project Program of Chongqing Key Laboratory of Catalysis and Functional Organic Molecules from Chongqing Technology and Business University (1456029)the Chongqing Science & Technology Commission (cstc2014pt-gc20002)~~
文摘A series of CeO2‐MnOx‐Al2O3 mixed oxide catalysts (Ce:Mn:Al mole ratio=6:4:x, x=0.25, 0.5, 1, 2) were prepared by a simple one‐step inverse co‐precipitation method to investigate the influence of the incorporation of Al3+ into CeO2‐MnOx mixed oxides. CeO2‐MnOx, CeO2‐Al2O3, and MnOx‐Al2O3 mixed oxides, and CeO2 were prepared by the same method for comparison. The samples were characterized by XRD, Raman, N2 physisorption, H2‐TPR, XPS, and in situ DRIFTS. The catalytic re‐duction of NO by CO was chosen as a model reaction to evaluate the catalytic performance. The incorporation of a small amount of Al3+into CeO2‐MnOx mixed oxides resulted in a decrease of crys‐tallite size, with the increase of the BET specific surface area and pore volume, as well as the in‐crease of Ce3+and Mn4+. The former benefits good contact between catalyst and reactants, and the latter promotes the adsorption of CO and the desorption, conversion and dissociation of adsorbed NO. All these enhanced the catalytic performance for the NO+CO model reaction. A reaction mecha‐nism was proposed to explain the excellent catalytic performance of CeO2‐MnOx‐Al2O3 catalysts for NO reduction by CO.
文摘By means of both a theory for pressure-induced shifts (PS) of energy spectra and a theory for shifts of energy spectra due to electron-phonon interaction (EPI), the 'pure electronic' PS and the PS due to EPI of R<SUB>1</SUB> line, R<SUB>2</SUB> line, and U band of GSGG:Cr<SUP>3+</SUP> at 300 K have been calculated, respectively. The calculated results are in good agreement with all the experimental data. Their physical origins have also been explained. It is found that the mixing-degree of and base-wavefunctions in the wavefunctions of R<SUB>1</SUB> level of GSGG:Cr<SUP>3+</SUP> at 300 K is remarkable under normal pressure, and the mixing-degree rapidly decreases with increasing pressure. The change of the mixing-degree with pressure plays a key role not only for the 'pure electronic' PS of R<SUB>1</SUB> line and R<SUB>2</SUB> line but also the PS of R<SUB>1</SUB> line and R<SUB>2</SUB> line due to EPI. The pressure-dependent behaviors of the 'pure electronic' PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line) and the PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line) due to EPI are quite different. It is the combined effect of them that gives rise to the total PS of R<SUB>1</SUB> line (or R<SUB>2</SUB> line). In the range of about 15 kbar ~ 45 kbar, the mergence and/or order-reversal between levels and levels take place, which cause the fluctuation of the rate of PS for with pressure. At 300 K, both the temperature-dependent contribution to R<SUB>1</SUB> line (or R<SUB>2</SUB> line or U band) from EPI and the temperature-independent one are important.