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Identification of relevant active sites and a mechanism study for reverse water gas shift reaction over Pt/CeO_2 catalysts 被引量:7
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作者 Xiaodong Chen Xiong Su +5 位作者 Binglian Liang Xiaoli Yang Xinyi Ren Hongmin Duan Yanqiang Huang Tao Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2016年第6期1051-1057,共7页
Reverse water gas shift (RWGS) reaction can serve as a pivotal stage in the CO2 conversion processes, which is vital for the utilization of CO2. In this study, RWGS reaction was performed over Pt/CeO2 catalysts at the... Reverse water gas shift (RWGS) reaction can serve as a pivotal stage in the CO2 conversion processes, which is vital for the utilization of CO2. In this study, RWGS reaction was performed over Pt/CeO2 catalysts at the temperature range of 200-500 degrees C under ambient pressure. Compared with pure CeO2, Pt/CeO2 catalysts exhibited superior RWGS activity at lower reaction temperature. Meanwhile, the calculated TOF and E-a values are approximately the same over these Pt/CeO2 catalysts pretreated under various calcination conditions, indicating that the RWGS reaction is not affected by the morphologies of anchored Pt nanoparticles or the primary crystallinity of CeO2. TPR and XPS results indicated that the incorporation of Pt promoted the reducibility of CeO2 support and remarkably increased the content of Ce 3 + sites on the catalyst surface. Furthermore, the CO TPSR-MS signal under the condition of pure CO2 flow over Pt/CeO 2 catalyst is far lower than that under the condition of adsorbed CO2 with H-2 -assisted flow, revealing that CO2 molecules adsorbed on Ce3+ active sites have difficult in generating CO directly. Meanwhile, the adsorbed CO2 with the assistance of H-2 can form formate species easily over Ce3+ active sites and then decompose into Ce3+-CO species for CO production, which was identified by in-situ FTIR. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B. V. and Science Press. All rights reserved. 展开更多
关键词 RWGS reaction pt/ceo2 catalyst Formate intermediate MECHANISM
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Effect of active oxygen on the performance of Pt/CeO2 catalysts for CO oxidation 被引量:18
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作者 Anbin Zhou Jun Wang +3 位作者 Hui Wang Hang Li Jianqiang Wang Meiqing Shen 《Journal of Rare Earths》 SCIE EI CAS CSCD 2018年第3期257-264,共8页
This study was focused on the influence of active oxygen on the performance of Pt/CeO2 catalysts for CO oxidation. A series of CeO2 supports with different contents of active oxygen were obtained by adding surfactant ... This study was focused on the influence of active oxygen on the performance of Pt/CeO2 catalysts for CO oxidation. A series of CeO2 supports with different contents of active oxygen were obtained by adding surfactant at different synthesis steps. 0.25 wt% Pt was loaded on these CeO2 supports by incipientwetness impregnation methods. The catalysts were characterized by N2 adsorption, X-ray diffraction(XRD), high-resolution transmission electron microscopy(HRTEM), H2 temperature-programmed reduction(H2-TPR), dynamic oxygen storage capacity(DOSC) and in-situ DRIFTS technologies. For S-f supports, the surfactant was added into the solution before spray-drying in the synthesis process, which facilitates more active oxygen formation on the surface of CeO2. After loading Pt, the more active oxygen on CeO2 contributes to dispersing Pt species and enhancing the CO oxidation activity. As for the aged samples,Pt-R-h shows the highest activity above 190 ℃ because of the presence of more partly oxidized Pt^(δ+) species. Thus the activity is also influenced by the states of Pt and the Pt^(δ+) species may contribute to the high activity at elevated temperature. 展开更多
关键词 ceo2 Active oxygen pt/ceo2 catalyst pt dispersion CO oxidation Rare earths
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Boosting the water gas shift reaction on Pt/CeO_(2)-based nanocatalysts by compositional modification: Support doping versus bimetallic alloying 被引量:3
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作者 Kun Yuan Xiao-Chen Sun +4 位作者 Hai-Jing Yin Liang Zhou Hai-Chao Liu Chun-Hua Yan Ya-Wen Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第4期241-249,共9页
The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel cells.The influence of ... The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel cells.The influence of support doping and bimetallic alloying on the catalytic performance of Pt/Ce O_(2)-based nanocatalysts in water gas shift reaction was reported in this work.Various lanthanide ions and 3d transition metals were respectively introduced into the Ce O_(2)support or Pt to form Pt/Ce O_(2):Ln(Ln=La,Nd,Gd,Tb,Yb)and Pt M/Ce O_(2)(M=Fe,Co,Ni)nanocatalysts.The sample of Pt/Ce O_(2):Tb showed the highest activity(TOF at 200℃=0.051 s^(-1))among the Pt/Ce O_(2):Ln and the undoped Pt/Ce O_(2)catalysts.Besides,the sample of Pt Fe/Ce O_(2)exhibited the highest activity(TOF at 200℃=0.12 s^(-1))among Pt M/Ce O_(2)catalysts.The results of the multiple characterizations indicated that the catalytic activity of Pt/Ce O_(2):Ln catalysts was closely correlated with the amount of oxygen vacancies in doped ceria support.However,the different activity of Pt M/Ce O_(2)bimetallic catalysts was owing to the various Pt oxidation states of the bimetals dispersed on ceria.The study of the reaction pathway indicated that both the samples of Pt/Ce O_(2)and Pt/Ce O_(2):Tb catalyzed the reaction through the formate pathway,and the enhanced activity of the latter derived from the increased concentration of oxygen vacancies along with promoted water dissociation.As for the sample of Pt Fe/Ce O_(2),its catalytic mechanism was the carboxyl route with a higher reaction rate due to the moderate valence of Pt along with improved CO activation. 展开更多
关键词 pt/ceo_(2)catalysts Water–gas shift reaction Support doping Bimetallic alloying
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Propene and CO oxidation on Pt/Ce-Zr-SO_4^(2-) diesel oxidation catalysts:Effect of sulfate on activity and stability 被引量:9
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作者 顾蕾 陈晓 +3 位作者 周瑛 朱秋莲 黄海凤 卢晗锋 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第3期607-616,共10页
Platinum/cerium-zirconium-sulfate(Pt/Ce-Zr-SO_4^(2-)) catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate(SO_4^(2-))addition improv... Platinum/cerium-zirconium-sulfate(Pt/Ce-Zr-SO_4^(2-)) catalysts were prepared by wetness impregnation.Catalytic activities were evaluated from the combustion of propene and CO.Sulfate(SO_4^(2-))addition improved the catalytic activity significantly.When using Pt/Ce-Zr-SO_4^(2-) with 10 wt%SO_4^(2-),the temperature for 90%conversion of propene and CO decreased by 75℃ compared with Pt/Ce-Zr.The conversion exceeded 95%at 240℃ even after 0.02%sulfur dioxide poisoning for 20 h.Temperature-programmed desorption of CO and X-ray photoelectron spectroscopy analyses revealed an improvement in Pt dispersion onto the Ce-Zr-SO_4^(2-) support,and the increased number of Pt particles built up more Pt^(-)-(SO_4^(2-))^(-) couples,which resulted in excellent activity.The increased total acidity and new Bronsted acid sites on the surface provided the Pt/Ce-Zr-SO_4^(2-) with good sulfur resistance. 展开更多
关键词 Diesel oxidation catalyst pt/Ce-Zr-SO_4^(2-) catalyst Sulfur resistance Catalytic oxidation
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Enhanced CO oxidation over potassium-promoted Pt/Al_2O_3 catalysts:Kinetic and infrared spectroscopic study 被引量:1
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作者 刘欢欢 贾爱平 +2 位作者 王瑜 罗孟飞 鲁继青 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2015年第11期1976-1986,共11页
A series of K-promoted Pt/Al2O3 catalysts were tested for CO oxidation. It was found that the addition of K significantly enhanced the activity. A detailed kinetic study showed that the activation energies of the K-co... A series of K-promoted Pt/Al2O3 catalysts were tested for CO oxidation. It was found that the addition of K significantly enhanced the activity. A detailed kinetic study showed that the activation energies of the K-containing catalysts were lower than those of the K-free ones, particularly for catalysts with high Pt contents (51.6 k)/mol for 0.42K-2.0Pt/Al2O3 and 6:3.6 kJ/mol for 2.0Pt/Al2O3 ). The CO reaction orders were higher for the K-containing catalysts (about -0.2) than for the K-free ones (about -0.5), with the former having much lower equilibrium constants for CO adsorption than the latter. In situ Fourier-transform infrared spectroscopy showed that surface CO desorption from the 0.42K-2.0Pt/Al2O3 catalyst was easier than from 2.0Pt/Al2O3. The promoting effect of K was therefore caused by weakening of the interactions between CO and surface Pt atoms. This decreased coverage of the catalyst with CO and facilitated competitive O2 chemisorption on the Pt surface, and significantly lowered the reaction barrier between chemisorbed CO and O2 species. 展开更多
关键词 CO oxidation Potassium Kinetics pt/Al2O3 catalyst Promoting effect
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Influence of preparation methods on the physicochemical properties and catalytic performance of MnO_x-CeO_2 catalysts for NH_3-SCR at low temperature 被引量:48
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作者 Xiaojiang Yao Kaili Ma +4 位作者 Weixin Zou Shenggui He Jibin An Fumo Yang Lin Dong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第1期146-159,共14页
This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature.... This work examines the influence of preparation methods on the physicochemical properties and catalytic performance of MnOx‐CeO2 catalysts for selective catalytic reduction of NO by NH3 (NH3‐SCR) at low temperature. Five different methods, namely, mechanical mixing, impregnation,hydrothermal treatment, co‐precipitation, and a sol‐gel technique, were used to synthesizeMnOx‐CeO2 catalysts. The catalysts were characterized in detail, and an NH3‐SCR model reaction waschosen to evaluate the catalytic performance. The results showed that the preparation methodsaffected the catalytic performance in the order: hydrothermal treatment > sol‐gel > co‐precipitation> impregnation > mechanical mixing. This order correlated with the surface Ce3+ and Mn4+ content,oxygen vacancies and surface adsorbed oxygen species concentration, and the amount of acidic sitesand acidic strength. This trend is related to redox interactions between MnOx and CeO2. The catalystformed by a hydrothermal treatment exhibited excellent physicochemical properties, optimal catalyticperformance, and good H2O resistance in NH3‐SCR reaction. This was attributed to incorporationof Mnn+ into the CeO2 lattice to form a uniform ceria‐based solid solution (containing Mn‐O‐Cestructures). Strengthening of the electronic interactions between MnOx and CeO2, driven by thehigh‐temperature and high‐pressure conditions during the hydrothermal treatment also improved the catalyst characteristics. Thus, the hydrothermal treatment method is an efficient and environment‐friendly route to synthesizing low‐temperature denitrification (deNOx) catalysts. 展开更多
关键词 MnOx‐ceo2 catalyst Preparation method Nitrogen oxides Low‐temperature NH3‐SCR Electron interaction Surface acidity
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Preparation, Characterization of CuO/CeO_2 and Cu/CeO_2 Catalysts and Their Applications in Low-Temperature CO Oxidation 被引量:7
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作者 郑修成 韩东战 +4 位作者 王淑萍 张守民 王淑荣 黄唯平 吴世华 《Journal of Rare Earths》 SCIE EI CAS CSCD 2005年第1期47-51,共5页
CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were ... CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were examined by means of a microreactor-GC system, HRTEM, XRD, TPR and XPS techniques. The results show that CuO has not catalytic activity and the activity of CeO2 is quite low for CO oxidation. However, the catalytic activity of CuO/CeO2 and Cu/ CeO2 catalysts increases significantly. Furthermore, the activity of CuO/CeO2 is higher than that of Cu/CeO2 catalysts. 展开更多
关键词 catalytic chemistry CuO/ceo2 catalysts Cu/ceo2 catalysts carbon monoxide oxidation rare earths
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Screening of MgO- and CeO_2-Based Catalysts for Carbon Dioxide Oxidative Coupling of Methane to C_(2+) Hydrocarbons 被引量:5
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作者 Istadi Nor Aishah Saidina Amin 《Journal of Natural Gas Chemistry》 CAS CSCD 2004年第1期23-35,共13页
The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based so... The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively. 展开更多
关键词 catalyst screening carbon dioxide oxidative coupling METHANE ternary metal oxide binary metal oxide MGO ceo2 C2+ hydrocarbons
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CeO_2-Co_3O_4 Catalysts for CO Oxidation 被引量:3
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作者 许秀艳 李进军 郝郑平 《Journal of Rare Earths》 SCIE EI CAS CSCD 2006年第2期172-176,共5页
CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction (... CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction (TPR), and FT-IR, the influence of the cerium content on the catalytic performance of CeO2-Co3O4 was investigated. The results indicate that the prepared CeO2-Co3O4 catalysts exhibit a better activity than that of pure CeO2 or pure Co3O4. The catalyst with the Ce/Co atomic ratio 1 : 16 exhibits the best activity, which converts 77% of CO at room temperature and completely oxidizes CO at 45 ℃. 展开更多
关键词 CO oxidation ceo2 CO3O4 ceo2-Co3O4 catalyst rare earths
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Electronic and geometric structure of the copper-ceria interface on Cu/CeO2 catalysts 被引量:4
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作者 Yan Zhou Aling Chen +1 位作者 Jing Ning Wenjie Shen 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第6期928-937,共10页
The atomic structure of the active sites in Cu/CeO2 catalysts is intimately associated with the copper-ceria interaction. Both the shape of ceria and the loading of copper affect the chemical bonding of copper species... The atomic structure of the active sites in Cu/CeO2 catalysts is intimately associated with the copper-ceria interaction. Both the shape of ceria and the loading of copper affect the chemical bonding of copper species on ceria surfaces and the electronic and geometric character of the relevant interfaces. Nanostructured ceria, including particles(polyhedra), rods, and cubes, provides anchoring sites for the copper species. The atomic arrangements and chemical properties of the(111),(110) and(100) facets, preferentially exposed depending on the shape of ceria, govern the copper-ceria interactions and in turn determine their catalytic properties. Also, the metal loading significantly influences the dispersion of copper species on ceria with a specific shape, forming copper layers, clusters, and nanoparticles. Lower copper contents result in copper monolayers and/or bilayers while higher copper loadings lead to multi-layered clusters and faceted particles. The active sites are usually generated via interactions between the copper atoms in the metal species and the oxygen vacancies on ceria, which is closely linked to the number and density of surface oxygen vacancies dominated by the shape of ceria. 展开更多
关键词 Cu/ceo2 catalyst Ceria shape Oxygen vacancy Copper particle Copper-ceria interface Active site
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Evaluation of H2 Influence on the Evolution Mechanism of NOx Storage and Reduction over Pt–Ba–Ce/c-Al2O3 Catalysts 被引量:3
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作者 Pan Wang Jing Yi +2 位作者 Chuan Sun Peng Luo Lili Lei 《Engineering》 SCIE EI 2019年第3期568-575,共8页
In this investigation, Pt–Ba–Ce/c-Al2O3 catalysts were prepared by incipient wetness impregnation and experiments were performed to evaluate the influence of H2 on the evolution mechanism of nitrogen oxides (NOx) st... In this investigation, Pt–Ba–Ce/c-Al2O3 catalysts were prepared by incipient wetness impregnation and experiments were performed to evaluate the influence of H2 on the evolution mechanism of nitrogen oxides (NOx) storage and reduction (NSR). The physical and chemical properties of the Pt–Ba–Ce/c- Al2O3 catalysts were studied using a combination of characterization techniques, which showed that PtOx, CeO2, and BaCO3, whose peaks were observed in X-ray diffraction (XRD) spectra, dispersed well on the c-Al2O3, as shown by transmission electron microscope (TEM), and that the difference between Ce3+ and Ce4+, as detected by X-ray photoelectron spectroscopy (XPS), facilitated the migration of active oxygen over the catalyst. In the process of a complete NSR experiment, the NOx storage capability was greatly enhanced in the temperature range of 250–350℃, and reached a maximum value of 315.3μmol·gcat^-1 at 350℃, which was ascribed to the increase in NO2 yield. In a lean and rich cycling experiment, the results showed that NOx storage efficiency and conversion were increased when the time of H2 exposure (i.e., 30, 45, and 60 s) was extended. The maximum NOx conversion of the catalyst reached 83.5% when the duration of the lean and rich phases was 240 and 60 s, respectively. The results revealed that increasing the content of H2 by an appropriate amount was favorable to the NSR mechanism due to increased decomposition of nitrate or nitrite, and the refreshing of trapping sites for the next cycle of NSR. 展开更多
关键词 pt–Ba–Ce/c-Al2O3 catalysts Physicochemical properties NOx storage and reduction emission H2 reductant
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Methane reforming with CO_2 to syngas over CeO_2-promoted Ni/Al_2O_3-ZrO_2 catalysts prepared via a direct sol-gel process 被引量:2
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作者 Hansheng Li Hang Xu Jinfu Wang 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2011年第1期1-8,共8页
CeO2-promoted Ni/Al2O3-ZrO2 (Ni/Al2O3-ZrO2-CeO2) catalysts were prepared by a direct sol-gel process with citric acid as gelling agent. The catalysts used for the methane reforming with CO2 was studied by infrared s... CeO2-promoted Ni/Al2O3-ZrO2 (Ni/Al2O3-ZrO2-CeO2) catalysts were prepared by a direct sol-gel process with citric acid as gelling agent. The catalysts used for the methane reforming with CO2 was studied by infrared spectroscopy (IR), thermal gravimetric analysis (TGA), microscopic analysis, X-ray diffraction (XRD) and temperature-programmed reduction (TPR). The catalytic performance for CO2 reforming of methane to synthesis gas was investigated in a continuous-flow micro-reactor under atmospheric pressure. TGA, IR, XRD and microscopic analysis show that the catalysts prepared by the direct sol-gel process consist of Ni particles with a nanostructure of around 5 nm and an amorphous-phase composite oxide support. There exists a chemical interaction between metallic Ni particles and supports, which makes metallic Ni well dispersed, highly active and stable. The addition of CeO2 effectively improves the dispersion and the stability of Ni particles of the prepared catalysts, and enhances the adsorption of CO2 on the surface of catalysts. The catalytic tests for methane reforming with CO2 to synthesis gas show that the Ni/Al2O3-ZrO2-CeO2 catalysts show excellent activity and stability compared with the Ni/Al2O3 catalyst. The excellent catalytic activity and stability of the Ni/Al2O3-ZrO2-CeO2 are attributed to the highly, uniformly and stably dispersed small metallic Ni particles, the high reducibility of the Ni oxides and the interaction between metallic Ni particles and the composite oxide supports. 展开更多
关键词 methane reforming with CO2 SYNGAS Ni-based catalyst ceo2 sol-gel process
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Catalytic Oxidative Properties and Characterization of CuO/CeO_2 Catalysts 被引量:1
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作者 蒋晓原 周仁贤 +2 位作者 袁骏 吕光烈 郑小明 《Journal of Rare Earths》 SCIE EI CAS CSCD 2003年第1期55-59,共5页
The oxidative properties and characterization of CuO, CeO 2 and CuO/CeO 2 cata lysts were examined by means of a CO micro-reactor GC system, TPR, XPS and X-r ay diffraction Rietveld methods. The results show that ei... The oxidative properties and characterization of CuO, CeO 2 and CuO/CeO 2 cata lysts were examined by means of a CO micro-reactor GC system, TPR, XPS and X-r ay diffraction Rietveld methods. The results show that either CuO or CeO 2 ac tivity is quite low for CO oxidation. However, when CuO and CeO 2 are mixed, the oxidative activity of the catalyst increases significantly, probably owing to the valency status of copper species (Cu 2+ and Cu+) on the CeO 2 surfa ce, the dispersion and reducibility. XPS surface analysis shows that CuO loading is very important in forming of either Cu 2+ or Cu+. Rietveld analysis s hows that some CuO, which has smaller ion radius than Ce 4+, enters the Ce O 2 lattice after CuO and CeO 2 are mixed. When the CuO loading reaches 5.0%, the size of CuO crystals is a minimum (6.1 nm) and the micro-strain value i s a maximum (2.86×10 -3), resulting in high surface energy and the best ac tivity for CO oxidation. 展开更多
关键词 physical chemistry CuO/ceo 2 catalysts CO micro-reactor GC system rare earths
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Effect of Addition of Base on Ceria and Reactivity of CuO/CeO_2 Catalysts for Low-Temperature CO Oxidation 被引量:1
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作者 Xiucheng Zheng Xiaoli Zhang +2 位作者 Shuping Wang Xiangyu Wang Shihua Wu 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2007年第2期179-185,共7页
In this work, we have reported the influence of the addition of base (KOH) on the physicochemical property of ceria synthesized by alcohothermal process, and the alcohothermal mechanism was also put forward. Further... In this work, we have reported the influence of the addition of base (KOH) on the physicochemical property of ceria synthesized by alcohothermal process, and the alcohothermal mechanism was also put forward. Furthermore, the prepared CeO2 was used as the support to prepare CuO/CeO2 catalysts via the wet impregnation method. The samples were characterized by N2 adsorption-desorption, X-ray powder diffraction (XRD), high resolution transmission electron microscopy (HRTEM), and temperatureprogrammed reduction by H2 (H2-TPR). The catalytic properties of the CuO/CeO2 catalysts for lowtemperature CO oxidation were studied using a microreactor-GC system. The crystal size of CeO2-A was much smaller than that of CeO2-B, and the corresponding copper oxide catalysts exhibited higher catalytic activity than that of the CeO2-B-supported catalysts under the same reaction conditions. The alcohothermal mechanism indicated that KOH plays a key role in determining the physicochemical and catalytic properties of ceria-based materials. 展开更多
关键词 alcohothermal synthesis CERIA CuO/ceo2 catalyst CO oxidation alcohothermal mechanism
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Effects of ZrO_2 Content on Structure and Performance of Cu/CeO_2-ZrO_2 Catalysts for Water-Gas Shift Reaction 被引量:1
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作者 郑云弟 林性贻 +3 位作者 郑起 詹瑛瑛 李达林 魏可镁 《Journal of Rare Earths》 SCIE EI CAS CSCD 2005年第6期685-689,共5页
Cu/CeO2-ZrO2 catalysts for water-gas shift (WGS) reaction were prepared with co-precipitation method, and the influence of ZrO2 content on the catalytic structure and properties was investigated by the techniques of... Cu/CeO2-ZrO2 catalysts for water-gas shift (WGS) reaction were prepared with co-precipitation method, and the influence of ZrO2 content on the catalytic structure and properties was investigated by the techniques of N2 physical adsorption analysis, XRD and H2-TPR. The results indicate that the BET surface areas of the catalysts are increased in varying degrees due to the presence of ZrO2. With increasing ZrO2 content, the pore size distribution is centered on 1.9 nm. ZrO2 can efficiently restrain the growth of Cu crystal particles. The appropriate amount of ZrO2 in the Cu/CeO2 catalysts can help the catalyst keep better copper dispersion in the WGS reaction, which can lead to both higher catalytic activity and better thermal stability. When ZrO2 content is 10% (atom fraction), Cu/CeO2-Zr02 catalyst reaches a CO conversion rate of 73.7% at the reaction temperature of 200℃. 展开更多
关键词 water-gas shift Cu/ceo2-ZrO2 catalyst rare earths
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Different roles of MoO_(3)and Nb_(2)O_(5)promotion in short-chain alkane combustion over Pt/ZrO_(2)catalysts 被引量:1
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作者 Bingheng Cen Cen Tang +2 位作者 Jiqing Lu Jian Chen Mengfei Luo 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第12期2287-2295,共9页
Pt/ZrO_(2)catalysts promoted with MoO_(3)and Nb_(2)O_(5)were tested for the combustion of short-chain alkanes(namely,methane,ethane,propane,and n-hexane).For short-chain alkane combustion,the inhibition of MoO_(3)(for... Pt/ZrO_(2)catalysts promoted with MoO_(3)and Nb_(2)O_(5)were tested for the combustion of short-chain alkanes(namely,methane,ethane,propane,and n-hexane).For short-chain alkane combustion,the inhibition of MoO_(3)(for the methane reaction)dramatically transformed to promotion(for the ethane,propane,and n-hexane reactions)as the carbon chain length increased,whereas the remarkable promotion of Nb_(2)O_(5)gradually weakened with an increase in the carbon chain length.Based on a detailed study of the oxidation reactions of methane and propane over the catalysts,the different roles of the promoters in the reactions were ascribed to differences in the acidic properties of the surface and the oxidation or reduction states of the Pt species.The MoO_(3)promoter could decorate the surface of the Pt species for a Pt-Mo/ZrO_(2)catalyst,whereas the Nb_(2)O_(5)promoter on the support could be partially covered by Pt particles for a Pt-Nb/ZrO_(2)catalyst.The formation of accessible Pt-MoO_(3)interfacial sites,a high concentration of metallic Pt species,and a high surface acidity in Pt-Mo/ZrO_(2)were responsible for the enhanced activity for catalytic propane combustion.The lack of enough accessible Pt-Nb_(2)O_(5)interfacial sites but an enhanced surface acid sites in Pt-Nb/ZrO_(2)explained the slight improvement in activity for catalytic propane combustion.However,the stabilized Pt^(n+)species in Pt-Nb/ZrO_(2)were responsible for the much-improved activity for methane combustion,whereas the Pt^(n+)species in Pt-Mo/ZrO_(2)could be reduced during the oxidation reaction,and the fewer exposed surface Pt species because of MoO_(3)decoration accounted for the inhibited activity for methane combustion.In addition,it can be concluded that MoO_(3)promotion is favorable for the activation of C-C bonds,whereas Nb_(2)O_(5)promotion is more beneficial for the activation of C-H bonds with high energy. 展开更多
关键词 pt/ZrO_(2)catalyst Alkanes combustion MoO_(3)promoter Nb_(2)O_(5)promoter Active site
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Structures and reactivities of the CeO2/Pt(111)reverse catalyst:A DFT+U study
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作者 Zhu-Yuan Zheng Dong Wang +2 位作者 Yi Zhang Fan Yang Xue-Qing Gong 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第9期1360-1368,共9页
For heterogeneous catalysts,the build-up of interface contacts can influence markedly their activities.Being different from the conventional supported metal/oxide catalysts,the reverse type of oxide/metal structures,e... For heterogeneous catalysts,the build-up of interface contacts can influence markedly their activities.Being different from the conventional supported metal/oxide catalysts,the reverse type of oxide/metal structures,e.g.the ceria/Pt composite,have emerged as novel catalytic materials in many fields.However,it remains challenging to determine the optimal interface structure and/or the metal-oxide synergistic effect that can boost catalytic activities.In this work,we conducted density functional theory calculations with on-site Coulomb interaction correction to determine the optimal structures and investigate the physical as well as catalytic properties of various Ce O2/Pt(111)composites containing Ce O2(111)monolayer,bilayer,and trilayer at Pt(111).We found that the interaction strength between Ce O2(111)and Pt(111)substrate first reduces as the ceria slab grows from monolayer to bilayer,and then largely gets converged when the trilayer occurs.Such trend was well rationalized by analyzing the number and distances of O–Pt bonds at the interface.Calculated Bader charges uncovered the significant charge redistribution occurring around the interface,whereas the net electron transfer across the interface is non-significant and decreases as ceria thickness increases.Moreover,comparative calculations on oxygen vacancy formation energies clarified that oxygen removal can be promoted on the Ce O2/Pt(111)composites,especially at the interface.We finally employed CO oxidation as a model reaction to probe the surface reactivity,and determined an intrinsic activity order of monolayer Ce O2(111)>monolayer Ce O2(111)/Pt(111)>regular Ce O2(111).More importantly,we emphasized the significant role of the moderate ceria-Pt interaction at the interface that endows the Ce O2/Pt reverse catalyst both good thermostability and high catalytic activity.The monolayer Ce O2(111)/Pt(111)composite was theoretically predicted highly efficient for catalyzing CO oxidation. 展开更多
关键词 ceo2/pt reverse catalyst Interface structure Oxygen vacancy CO oxidation Density functional theory
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Effect of yttrium addition on water-gas shift reaction over CuO/CeO_2 catalysts
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作者 佘育生 李雷 +3 位作者 詹瑛瑛 林性贻 郑起 魏可镁 《Journal of Rare Earths》 SCIE EI CAS CSCD 2009年第3期412-418,共7页
This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 cata... This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 catalysts with yttrium content in the range of 0-5wt.%. Properties of the obtained samples were characterized and analyzed by X-ray diffraction (XRD), Raman spectroscopy, H2-TPR, cyclic voltammetry (CV) and the BET method. The results revealed that catalytic activity was increased with the yttrium content at first, but then decreased with the further increase of yttrium content. Herein, CuO/CeO2 catalyst doped with 2wt.% of yttrium showed the highest catalytic activity (CO conversion reaches 93.4% at 250 ℃) and thermal stability for WGS reaction. The catalytic activity was correlated with the surface area, the area of peak γ of H2-TPR profile (i.e., the reduction of surface copper oxide (crystalline forms) interacted with surface oxygen vacancies on ceria), and the area of peak C2 and A1 (Cu^0→←Cu^2+ in cyclic voltammetry process), respectively. Besides, Raman spectra provided evidences for a synergistic Cu-Ovacancy interaction, and it was indicated that doping yttrium may facilitate the formation of oxygen vacancies on ceria. 展开更多
关键词 CuO/ceo2 catalyst water-gas shift YTTRIUM cyclic voltammetry rare earths
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Influence of CeO2 on Properties and Activity of Oxide Catalysts in Carbon Monoxide Oxidation
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作者 Hoang Tien Cuong Luu Cam Loc Ho Si Thoang 《Journal of Chemistry and Chemical Engineering》 2010年第2期48-55,共8页
A series of catalysts on the basis of 10 wt.% CuO/y-AI203, 10 wt.% CuO + 10 wt.% Cr2O3/y-AI203 and 15 wt.% MnO2/y -A1203 have been prepared and modified by CeO2 with contents up to 20 wt.%. Physico-chemical propertie... A series of catalysts on the basis of 10 wt.% CuO/y-AI203, 10 wt.% CuO + 10 wt.% Cr2O3/y-AI203 and 15 wt.% MnO2/y -A1203 have been prepared and modified by CeO2 with contents up to 20 wt.%. Physico-chemical properties of the catalysts were determined by the methods of BET Adsorption, XRD, and TPR. Oxidative activity of the catalysts was studied at the temperature range 90-220 ℃and CO concentration of 3 mol.%. Addition of CeO2 led to changes in physico-chemical properties of the catalysts and formation of novel active centres that increased the activity of CuO and Cr203 containing catalysts, but decreased the activity of those, containing MnO2. The catalyst sample containing 10 wt.% CuO and 15 wt.% CeO2 has been shown to be the best one for complete conversion of CO. At the given conditions on this catalyst the complete oxidation of CO to CO2 occurred at 130 ~C during more than 500 h. 展开更多
关键词 ceo2 carbon monoxide oxide catalysts oxidation.
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Effects of CuO-CeO<sub>2</sub>Addition on Structure and Catalytic Properties of Three Way Catalysts
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作者 Nguyen The Luong Nguyen Duy Tien +2 位作者 Eiji Yamasue Hideyuki Okumura Keiichi N. Ishihara 《Journal of Materials Science and Chemical Engineering》 2017年第12期28-39,共12页
The noble metals (Pt, Pd, Rh) supported on Cu-Ce mixed oxides with γ-Al2O3 washcoat/FeCrAl substrate were investigated as catalytic performance of Three Way Catalysts (TWC) under simulated automotive exhaust feed gas... The noble metals (Pt, Pd, Rh) supported on Cu-Ce mixed oxides with γ-Al2O3 washcoat/FeCrAl substrate were investigated as catalytic performance of Three Way Catalysts (TWC) under simulated automotive exhaust feed gas. The structural, morphological features and catalytic activity were observed by X-ray diffractometry (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS) and GC-TCD (Varian CP-4900). The catalytic performance of noble metals (Pt, Rh, Pd) supported on Cu-Ce mixed oxides with γ-Al2O3 washcoat/FeCrAl substrate was be compared with noble metals (Pt, Rh, Pd) supported on Ce-Zr mixed oxides with γ-Al2O3 washcoat/FeCrAl substrate and only γ-Al2O3 washcoat/FeCrAl substrate at various stoichiometric ratio of oxygen. The results showed that the addition of Cu-Ce mixed oxides improved CO oxidation reaction at lower temperature during stable lambda of 1, the highest CO conversion of 99% is observed for the noble metals (Pt, Pd, Rh) support on Cu-Ce with γ-Al2O3 washcoat/FeCrAl substrate. The results also showed that, the addition of Cu-Ce mixed oxides promoted released oxygen, thus it improved strongly CO and C3H8 conversion at lean oxygen stoichiometric operation. 展开更多
关键词 Three-Way catalysts (TWCs) NOBLE Metals γ-Al2O3 WASHCOAT CuO-ceo2 ceo2-ZRO2
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