Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their s...Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.展开更多
Lead-free low melting glasses,ZnO-CuO-Bi_(2)O_(3)-B_(2)O_(3)-SiO_(2)system,with fixed contents of 15 mol%CuO and 20 mol%Bi_(2)O_(3),were prepared by using melt cooling method.Structure and thermal properties of the gl...Lead-free low melting glasses,ZnO-CuO-Bi_(2)O_(3)-B_(2)O_(3)-SiO_(2)system,with fixed contents of 15 mol%CuO and 20 mol%Bi_(2)O_(3),were prepared by using melt cooling method.Structure and thermal properties of the glasses were studied by using X-ray diffractometer(XRD),infrared spectrometer(FIT-IR),thermal dilatometer and differential thermal analyzer(DTA).Chemical durability of the glasses was studied by using dissolution rate method.Wettability of glasses on substrate was tested by using button sintering experiment.It is found that alkaline resistance of the glass solders is lower than that of plate glass and the water resistance is comparable with that of plate glass.The sealing temperatures are Ts=445-490℃,while the average thermal expansion coefficient from room temperature to 300℃is in the range of(65-82)×10^(−7)℃^(−1).At sealing temperature,the glass solders have good wettability on plate glass or alumina substrate.They are not crystallized even sintered at the sealing temperature for 30 min.The solder glasses are suitable for sealing plate glass,alumina and other inorganic non-metallic materials.展开更多
文摘Although metal oxide-zeolite hybrid materials have long been known to achieve enhanced catalytic activity and selectivity in NO_(x)removal reactions through the inter-particle diffusion of intermediate species,their subsequent reaction mechanism on acid sites is still unclear and requires investigation.In this study,the distribution of Brønsted/Lewis acid sites in the hybrid materials was precisely adjusted by introducing potassium ions,which not only selectively bind to Brønsted acid sites but also potentially affect the formation and diffusion of activated NO species.Systematic in situ diffuse reflectance infrared Fourier transform spectroscopy analyses coupled with selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR)reaction demonstrate that the Lewis acid sites over MnO_(x)are more active for NO reduction but have lower selectivity to N_(2)than Brønsted acids sites.Brønsted acid sites primarily produce N_(2),whereas Lewis acid sites primarily produce N_(2)O,contributing to unfavorable N_(2)selectivity.The Brønsted acid sites present in Y zeolite,which are stronger than those on MnO_(x),accelerate the NH_(3)-SCR reaction in which the nitrite/nitrate species diffused from the MnO_(x)particles rapidly convert into the N_(2).Therefore,it is important to design the catalyst so that the activated NO species formed in MnO_(x)diffuse to and are selectively decomposed on the Brønsted acid sites of H-Y zeolite rather than that of MnO_(x)particle.For the physically mixed H-MnO_(x)+H-Y sample,the abundant Brønsted/Lewis acid sites in H-MnO_(x)give rise to significant consumption of activated NO species before their inter-particle diffusion,thereby hindering the enhancement of the synergistic effects.Furthermore,we found that the intercalated K+in K-MnO_(x)has an unexpected favorable role in the NO reduction rate,probably owing to faster diffusion of the activated NO species on K-MnO_(x)than H-MnO_(x).This study will help to design promising metal oxide-zeolite hybrid catalysts by identifying the role of the acid sites in two different constituents.
基金National Natural Science Foundation of China(52172070)Jiangxi Provincial Natural Science Foundation(20242BAB25222)Jiangxi Provincial Graduate Innovation Special Fund Project(YC2022-S882 and YC2023-S808).
文摘Lead-free low melting glasses,ZnO-CuO-Bi_(2)O_(3)-B_(2)O_(3)-SiO_(2)system,with fixed contents of 15 mol%CuO and 20 mol%Bi_(2)O_(3),were prepared by using melt cooling method.Structure and thermal properties of the glasses were studied by using X-ray diffractometer(XRD),infrared spectrometer(FIT-IR),thermal dilatometer and differential thermal analyzer(DTA).Chemical durability of the glasses was studied by using dissolution rate method.Wettability of glasses on substrate was tested by using button sintering experiment.It is found that alkaline resistance of the glass solders is lower than that of plate glass and the water resistance is comparable with that of plate glass.The sealing temperatures are Ts=445-490℃,while the average thermal expansion coefficient from room temperature to 300℃is in the range of(65-82)×10^(−7)℃^(−1).At sealing temperature,the glass solders have good wettability on plate glass or alumina substrate.They are not crystallized even sintered at the sealing temperature for 30 min.The solder glasses are suitable for sealing plate glass,alumina and other inorganic non-metallic materials.
