A series of Ce-doped MnOx/TiO2 catalysts were prepared by impregnation method and used for catalytic oxidation of NO in the presence of excess O2. The sample with the Ce doping concentration of Ce/Mn=l/3 and calcined ...A series of Ce-doped MnOx/TiO2 catalysts were prepared by impregnation method and used for catalytic oxidation of NO in the presence of excess O2. The sample with the Ce doping concentration of Ce/Mn=l/3 and calcined at 300 ℃ shows a superior activity for NO oxidation to NO2. On Ce（1）Mn（3）Ti catalyst, 58% NO conversion was obtained at 200 ℃ and 85% NO conversion at 250 ℃ with a GHSV of 41000 h-1, which was much higher than that over MnOx/TiO2 catalyst （48% at 250 ℃）. Characterization results implied that the higher activity of Ce（1）Mn（3）Ti could be attributed to the enrichment of well-dispersed MnO2 on the surface and the abundance of Mn3＋ and Zi3＋ species. The addition of Ce into MnO2/TiO2 could improve oxygen storage capacity and facilitate oxygen mobility of the catalyst as shown by PL and ESR, so that its activity for NO oxidation could be enhanced. The effect of H2O and SO2 on the catalyst activity was also investigated.展开更多
Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA...Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA, XRD, H2-TPR and XPS. The catalytic activity of the CuO/TiO2-SnO2 catalysts was markedly depended on the loading of CuO, and the optimum CuO loading was 8 wt.% （Tloo = 80 ℃）. The CuO/TiO2-SnO2 catalysts exhibited much higher catalytic activity than the CuO/TiO2 and CuO/SnO2 catalysts. H2-TPR result indicated that a large amount of CuO formed the active site for CO oxidation in 8 wt.% CuO/TiO2-SnO2 catalyst.展开更多
Catalyst support is extremely important for future fuel cell devices.In this work,we developed doubleshelled C/TiO2(DSCT)hollow spheres as an excellent catalyst support via a template-directed method.The combination o...Catalyst support is extremely important for future fuel cell devices.In this work,we developed doubleshelled C/TiO2(DSCT)hollow spheres as an excellent catalyst support via a template-directed method.The combination of hollow structure,TiO2 shell and carbon layer results in excellent electron conductivity,electrocatalytic activity,and chemical stability.These uniformed DSCT hollow spheres are used as catalyst support to synthesize Pt/DSCT hollow spheres electrocatalyst.The resulting Pt/DSCT hollow spheres exhibited high catalytic performance with a current density of 462 mA mg^-1 for methanol oxidation reaction,which is 2.52 times higher than that of the commercial Pt/C.Furthermore,the increased tolerance to carbonaceous poisoning with a higher If/Ibratio and a better long-term stability in acid media suggests that the DSCT hollow sphere is a promising C/TiO2-based catalyst support for direct methanol fuel cells applications.展开更多
A new type of catalytic material for purification of automobile exhaust, Cu Mn Ce O/ γ Al 2O 3, has been studied. The factors affecting its catalytic activity, such as calcination temperature and the period of calcin...A new type of catalytic material for purification of automobile exhaust, Cu Mn Ce O/ γ Al 2O 3, has been studied. The factors affecting its catalytic activity, such as calcination temperature and the period of calcinations and so on have been investigated. Its catalytic activity after SO 2 poisoning was determined in a fixed bed reactor by exposing the sample to the atmosphere of 160?mL/min SO 2/air. The study reveals that the catalyst has shown high catalytic activities for the conversion of NH 3 oxidation by NO after sulfate. The conversion of NO reduction over the sulfated catalyst is somewhat higher than that over the fresh catalyst except that the optimum temperature has increased about 100?℃. Also at the optimum process for the experiment, the selective catalytic oxidation of CO by NO is over 76% and the conversion of NO reduction is over 80% by NH 3.展开更多
The supported Au/TiO2 and Au/TiO2-SiO2 catalysts were prepared by deposition precipitation method. The TPD study reveals that propylene oxide competes with propylene to be adsorbed on the same adsorptive center-Ti^n＋...The supported Au/TiO2 and Au/TiO2-SiO2 catalysts were prepared by deposition precipitation method. The TPD study reveals that propylene oxide competes with propylene to be adsorbed on the same adsorptive center-Ti^n＋ site on the surface of the catalyst and that the adisorbing capacity of the catalyst for propylene oxide is larger than that for propylene. Catalytic behavior for propylene epoxidation with H2 and O2 was tested in a micro-reactor. Under typical conditions, the selectivity for propylene oxide is over 87%. The TG curves show that PO successive oxidation cause carbon deposition on the active center and deactivation of the Au catalysts. Because the amounts of Tin＋ site decrease significantly, and consequently the separation between Ti^n＋ sites increases, the Au/TiO2-SiO2 catalyst is more stable than Au/TiO2.展开更多
Conversion of CO_(2) into high-value products using electrochemical CO_(2) reduction(ECR)technology is an effective way to alleviate global warming and reach carbon neutrality.The oxygen vacancies in heterogenous cata...Conversion of CO_(2) into high-value products using electrochemical CO_(2) reduction(ECR)technology is an effective way to alleviate global warming and reach carbon neutrality.The oxygen vacancies in heterogenous catalysis are generally considered as a powerful method to enhance the performance of ECR by promoting CO_(2) adsorption and activation.However,the extent of defects in oxygen vacancies-activity relation has rarely been studied.Herein,we prepared Cu-Cd bimetallic catalysts with adjustable oxygen defect degree by controlling the amount of cadmium addition.Fourier transform infrared spectroscopy characterization results reveal that the formation of oxygen vacancies is attributed to the asymmetric stretching of Cu-O by the addition of cadmium.Electrochemical results show that the oxygen defect degree can modulate the selectivity of ECR products.A low degree of oxygen defects(CuO)is generally associated with lower product Faraday efficiency(FE_(C2)/FE_(C1)≈114%),but overabundant oxygen vacancies(CuO_(2.625)-CdO_(0.375))are not entirely favorable to improving ECR activity(FE_(C2)/FE_(C1)≈125%)and single selectivity,while an appropriate degree of oxygen vacancies(CuO_(2.75)-CdO_(0.25))can facilitate the ECR process toward single product selective production(FE_(C2)/FE_(C1)≈296%).The theoretical calculation showed that the O vacancy formed on CuO and the interface between CdO and CuO were conducive to enhancing the formation of ^(*)COOH intermediate and promoting the generation of ethylene products.This study provides a new approach and insight into the selective production of single products for future industrial applications of ECR.展开更多
PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation pe...PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation performance was compared to that using the commercial PtRu/C.Before the comparison,the effect of the catalyst loading on the power density of the DMFC was investigated using PtRu(18 wt%)/TECNF.The DMFC power density showed a maximum at about a 1.5 mg cm2 PtRu loading that corresponds to about an 80 mm layer thickness.A catalyst layer thicker than this value reduced the power density probably due to the concentration overvoltage.The PtRu content in the PtRu/TECNF was then increased to 30 wt%or more to reduce the layer thickness and to increase the power density.The DMFC performance was compared to that of different anode catalysts at a 1 mg cm2 PtRu loading.The power density was maximized using the PtRu30 wt%/TECNF,which showed a 173 mW cm2 at 353 K and had 66 mm layer thick,that was 26%higher than that of commercial PtRu/C.The current–voltage curve of the DMFC with the PtRu/TECNF suggested an improved mass transport overvoltage,but a little improvement in the activation one despite using the catalyst with about a 2 times higher activity compared to that of the commercial PtRu/C.This was attributed to the lower Pt utilization of the nanofiber catalyst layer.展开更多
基金supported by the National Natural Science Foundation of China (Grant No. 51078185)
文摘A series of Ce-doped MnOx/TiO2 catalysts were prepared by impregnation method and used for catalytic oxidation of NO in the presence of excess O2. The sample with the Ce doping concentration of Ce/Mn=l/3 and calcined at 300 ℃ shows a superior activity for NO oxidation to NO2. On Ce（1）Mn（3）Ti catalyst, 58% NO conversion was obtained at 200 ℃ and 85% NO conversion at 250 ℃ with a GHSV of 41000 h-1, which was much higher than that over MnOx/TiO2 catalyst （48% at 250 ℃）. Characterization results implied that the higher activity of Ce（1）Mn（3）Ti could be attributed to the enrichment of well-dispersed MnO2 on the surface and the abundance of Mn3＋ and Zi3＋ species. The addition of Ce into MnO2/TiO2 could improve oxygen storage capacity and facilitate oxygen mobility of the catalyst as shown by PL and ESR, so that its activity for NO oxidation could be enhanced. The effect of H2O and SO2 on the catalyst activity was also investigated.
基金supported by the National Natural Science Foundation of China (20771061 and 20871071)the 973 Program (2005CB623607)Science and Technology Commission Foundation of Tianjin (08JCYBJC00100 and 09JCYBJC03600)
文摘Nanometer SnO2 particles were synthesized by sol-gel dialytic processes and used as a support to prepare CuO supported catalysts via a deposition-precipitation method. The samples were characterized by means of TG-DTA, XRD, H2-TPR and XPS. The catalytic activity of the CuO/TiO2-SnO2 catalysts was markedly depended on the loading of CuO, and the optimum CuO loading was 8 wt.% （Tloo = 80 ℃）. The CuO/TiO2-SnO2 catalysts exhibited much higher catalytic activity than the CuO/TiO2 and CuO/SnO2 catalysts. H2-TPR result indicated that a large amount of CuO formed the active site for CO oxidation in 8 wt.% CuO/TiO2-SnO2 catalyst.
基金supported by the Scholarship from China Scholarship Council(CSC)(Grant no.201604910621)。
文摘Catalyst support is extremely important for future fuel cell devices.In this work,we developed doubleshelled C/TiO2(DSCT)hollow spheres as an excellent catalyst support via a template-directed method.The combination of hollow structure,TiO2 shell and carbon layer results in excellent electron conductivity,electrocatalytic activity,and chemical stability.These uniformed DSCT hollow spheres are used as catalyst support to synthesize Pt/DSCT hollow spheres electrocatalyst.The resulting Pt/DSCT hollow spheres exhibited high catalytic performance with a current density of 462 mA mg^-1 for methanol oxidation reaction,which is 2.52 times higher than that of the commercial Pt/C.Furthermore,the increased tolerance to carbonaceous poisoning with a higher If/Ibratio and a better long-term stability in acid media suggests that the DSCT hollow sphere is a promising C/TiO2-based catalyst support for direct methanol fuel cells applications.
文摘A new type of catalytic material for purification of automobile exhaust, Cu Mn Ce O/ γ Al 2O 3, has been studied. The factors affecting its catalytic activity, such as calcination temperature and the period of calcinations and so on have been investigated. Its catalytic activity after SO 2 poisoning was determined in a fixed bed reactor by exposing the sample to the atmosphere of 160?mL/min SO 2/air. The study reveals that the catalyst has shown high catalytic activities for the conversion of NH 3 oxidation by NO after sulfate. The conversion of NO reduction over the sulfated catalyst is somewhat higher than that over the fresh catalyst except that the optimum temperature has increased about 100?℃. Also at the optimum process for the experiment, the selective catalytic oxidation of CO by NO is over 76% and the conversion of NO reduction is over 80% by NH 3.
基金Supported by the National Natural Science Foundation of China (29773031).
文摘The supported Au/TiO2 and Au/TiO2-SiO2 catalysts were prepared by deposition precipitation method. The TPD study reveals that propylene oxide competes with propylene to be adsorbed on the same adsorptive center-Ti^n＋ site on the surface of the catalyst and that the adisorbing capacity of the catalyst for propylene oxide is larger than that for propylene. Catalytic behavior for propylene epoxidation with H2 and O2 was tested in a micro-reactor. Under typical conditions, the selectivity for propylene oxide is over 87%. The TG curves show that PO successive oxidation cause carbon deposition on the active center and deactivation of the Au catalysts. Because the amounts of Tin＋ site decrease significantly, and consequently the separation between Ti^n＋ sites increases, the Au/TiO2-SiO2 catalyst is more stable than Au/TiO2.
基金funded by the National Natural Science Foundation of Zhejiang Province(Nos.LQ21B030007 and LTGS23B030002)“Leading Goose”R&D Program of Zhejiang(No.2023C01191)+2 种基金the National Natural Science Foundation of China(No.22005269)Science and Technological program of Ningbo(No.2021S136)The Open Research Subject of Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control(No.2022Z02)。
文摘Conversion of CO_(2) into high-value products using electrochemical CO_(2) reduction(ECR)technology is an effective way to alleviate global warming and reach carbon neutrality.The oxygen vacancies in heterogenous catalysis are generally considered as a powerful method to enhance the performance of ECR by promoting CO_(2) adsorption and activation.However,the extent of defects in oxygen vacancies-activity relation has rarely been studied.Herein,we prepared Cu-Cd bimetallic catalysts with adjustable oxygen defect degree by controlling the amount of cadmium addition.Fourier transform infrared spectroscopy characterization results reveal that the formation of oxygen vacancies is attributed to the asymmetric stretching of Cu-O by the addition of cadmium.Electrochemical results show that the oxygen defect degree can modulate the selectivity of ECR products.A low degree of oxygen defects(CuO)is generally associated with lower product Faraday efficiency(FE_(C2)/FE_(C1)≈114%),but overabundant oxygen vacancies(CuO_(2.625)-CdO_(0.375))are not entirely favorable to improving ECR activity(FE_(C2)/FE_(C1)≈125%)and single selectivity,while an appropriate degree of oxygen vacancies(CuO_(2.75)-CdO_(0.25))can facilitate the ECR process toward single product selective production(FE_(C2)/FE_(C1)≈296%).The theoretical calculation showed that the O vacancy formed on CuO and the interface between CdO and CuO were conducive to enhancing the formation of ^(*)COOH intermediate and promoting the generation of ethylene products.This study provides a new approach and insight into the selective production of single products for future industrial applications of ECR.
基金the Element Innovation Project,Ministry of Education,Japan,and by KAKENHI(26289300).
文摘PtRu supported on TiO2-embedded carbon nanofibers(PtRu/TECNF),which was recently reported as a highly-active catalyst for methanol oxidation,was applied to a direct methanol fuel cell(DMFC),and the power generation performance was compared to that using the commercial PtRu/C.Before the comparison,the effect of the catalyst loading on the power density of the DMFC was investigated using PtRu(18 wt%)/TECNF.The DMFC power density showed a maximum at about a 1.5 mg cm2 PtRu loading that corresponds to about an 80 mm layer thickness.A catalyst layer thicker than this value reduced the power density probably due to the concentration overvoltage.The PtRu content in the PtRu/TECNF was then increased to 30 wt%or more to reduce the layer thickness and to increase the power density.The DMFC performance was compared to that of different anode catalysts at a 1 mg cm2 PtRu loading.The power density was maximized using the PtRu30 wt%/TECNF,which showed a 173 mW cm2 at 353 K and had 66 mm layer thick,that was 26%higher than that of commercial PtRu/C.The current–voltage curve of the DMFC with the PtRu/TECNF suggested an improved mass transport overvoltage,but a little improvement in the activation one despite using the catalyst with about a 2 times higher activity compared to that of the commercial PtRu/C.This was attributed to the lower Pt utilization of the nanofiber catalyst layer.
