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学者姓名:王榕
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采用柠檬酸络合法制备了钙钛矿型BaZrO3纳米材料,负载Ru以后用于催化氨合成反应,研究了BaZrO3前驱体焙烧温度对载体结构和Ru/BaZrO3催化剂氨合成反应性能的影响。以X射线衍射(XRD)、CO2程序升温脱附(CO2-TPD)、N2物理吸附、扫描电镜(SEM)和H2程序升温还原技术(H2-TPR)等方法对载体材料和催化剂进行了表征。结果表明,随着焙烧温度的升高,材料的比表面积和孔容均不断降低,但是有利于BaZrO3的生成。在750℃条件下焙烧得到的催化剂表现出最高的氨合成活性。在425℃,5 MPa,空速为10 000 h-1条件下,出口氨浓度可以达到9.12%,这可能是由于载体与活性...
Keyword :
氨合成 氨合成 焙烧温度 焙烧温度 金属-载体强相互作用 金属-载体强相互作用 钌 钌 锆酸钡 锆酸钡
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GB/T 7714 | 王自庆 , 林建新王 , 榕魏 et al. 钙钛矿型BaZrO_3负载钌催化剂氨合成和性能研究 [J]. | 无机化学学报 , 2013 , 29 (03) : 493-499 . |
MLA | 王自庆 et al. "钙钛矿型BaZrO_3负载钌催化剂氨合成和性能研究" . | 无机化学学报 29 . 03 (2013) : 493-499 . |
APA | 王自庆 , 林建新王 , 榕魏 , 可镁 . 钙钛矿型BaZrO_3负载钌催化剂氨合成和性能研究 . | 无机化学学报 , 2013 , 29 (03) , 493-499 . |
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采用柠檬酸络合法制备了含Ca,Sr和Ba的锆基钙钛矿材料,负载Ru后用于催化氨合成反应;研究了碱土金属对催化剂织构性能和载体材料表面碱性的影响,并与催化剂活性相关联.同时,采用程序升温脱附技术对催化剂表面H2脱附性能进行了表征.结果显示,碱土金属对催化剂活性的促进顺序为Ba>Sr>Ca.研究发现,不同锆基碱土金属钙钛矿材料表面均具有较强的碱性位,碱土金属的加入影响了载体碱性强度以及金属-载体的相互作用,其中BaZrO3可有效抑制H2的吸附.因此,Ru/BaZrO3催化剂表现出优异的氨合成活性.
Keyword :
氨合成 氨合成 碱土金属 碱土金属 钌催化剂 钌催化剂 钙钛矿 钙钛矿 锆 锆
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GB/T 7714 | 王自庆 , 马运翠 , 林建新 et al. 碱土金属对锆基钙钛矿材料负载钌催化剂氨合成性能的影响 [J]. | 催化学报 , 2013 , 34 (02) : 361-366 . |
MLA | 王自庆 et al. "碱土金属对锆基钙钛矿材料负载钌催化剂氨合成性能的影响" . | 催化学报 34 . 02 (2013) : 361-366 . |
APA | 王自庆 , 马运翠 , 林建新 , 王榕 , 魏可镁 . 碱土金属对锆基钙钛矿材料负载钌催化剂氨合成性能的影响 . | 催化学报 , 2013 , 34 (02) , 361-366 . |
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分别采用柠檬酸络合法、改性共沉淀法和湿浸渍法制备了掺Ba纳米ZrO2材料,负载Ru后用于催化氨合成反应.采用X射线衍射、CO2程序升温脱附(CO2-TPD)、N2物理低温吸附、H2程序升温还原技术(H2-TPR)、扫描电镜(SEM)、透射电镜(TEM)、X射线光电子能谱(XPS)和CO化学吸附对载体材料和催化剂进行了表征.结果表明,不同方法制备载体的物相结构和织构性能均有明显差别,负载Ru后催化剂的氨合成性能差别也较大.其中,以柠檬酸络合法制备的载体材料中Ba以BaZrO3的形式存在,钙钛矿型BaZrO3具有较强的供电子能力,电子可以通过Ru与载体间强相互作用传递到Ru表面,有效地促进N≡N的...
Keyword :
二氧化锆 二氧化锆 制备方法 制备方法 氨合成 氨合成 钌 钌 钡 钡
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GB/T 7714 | 王自庆 , 陈赓 , 林建新 et al. Ru/Ba-ZrO2催化剂的制备及其氨合成性能研究 [J]. | 化学学报 , 2013 , 71 (02) : 70-77 . |
MLA | 王自庆 et al. "Ru/Ba-ZrO2催化剂的制备及其氨合成性能研究" . | 化学学报 71 . 02 (2013) : 70-77 . |
APA | 王自庆 , 陈赓 , 林建新 , 王榕 , 魏可镁 . Ru/Ba-ZrO2催化剂的制备及其氨合成性能研究 . | 化学学报 , 2013 , 71 (02) , 70-77 . |
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The BaZrO3 material was synthesized by the citric acid method. A series of Ru/BaZrO3 catalyst samples were prepared using the above BaZrO3 calcined at different temperatures as the support. The support materials and catalyst samples were characterized by X-ray diffraction (XRD), H-2 temperature programmed reduction (H-2-TPR), CO2 temperature programmed desorption (CO2-TPD), N-2 adsorption-desorption isotherms and scanning electron microscopy (SEM). The results show that the catalytic performance is greatly influenced by the calcination temperature of the BaZrO3 support. The highest catalytic activity for ammonia synthesis is obtained on the Ru-based catalyst with the support calcined at 750 degrees C. The ammonia concentration of RBZ-750 can achieve to 9.12% under the condition of 425 degrees C, 5 MPa and 10 000 h(-1). The strong mental-support interaction and electron conductivity of the support may be the key factors for the high activity at low reaction temperature.
Keyword :
ammonia synthesis ammonia synthesis barium zirconate barium zirconate calcinations temperature calcinations temperature mental-support interaction mental-support interaction ruthenium ruthenium
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GB/T 7714 | Wang Zi-Qing , Lin Jian-Xin , Wang Rong et al. Ru-Based Catalysts Supported on Perovskite Type BaZrO3 for Ammonia Synthesis [J]. | CHINESE JOURNAL OF INORGANIC CHEMISTRY , 2013 , 29 (3) : 493-499 . |
MLA | Wang Zi-Qing et al. "Ru-Based Catalysts Supported on Perovskite Type BaZrO3 for Ammonia Synthesis" . | CHINESE JOURNAL OF INORGANIC CHEMISTRY 29 . 3 (2013) : 493-499 . |
APA | Wang Zi-Qing , Lin Jian-Xin , Wang Rong , Wei Ke-Mei . Ru-Based Catalysts Supported on Perovskite Type BaZrO3 for Ammonia Synthesis . | CHINESE JOURNAL OF INORGANIC CHEMISTRY , 2013 , 29 (3) , 493-499 . |
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Zirconium-based perovskite materials with different alkaline earth metals were synthesized by the citric acid method and used as supports for ruthenium catalysts to catalytic ammonia synthesis reaction. The effects of alkaline earth metals on the texture properties, basicity, and catalytic activity were discussed. Additionally, the desorption properties of H-2 on the surface of various catalysts were characterized by temperature-programmed desorption. The results showed that there were lots of strong basic sites appeared on the Ca, Sr, and Ba perovskite-style supports, and the order of activity was Ba > Sr > Ca. The addition of different alkaline earth metals not only affected the electron donating ability but also influenced the metal-support interaction as well as the adsorption-desorption properties of these catalysts. The adsorption of H2 was inhibited significantly by the presence of BaZrO3 and increased the number of active sites for dissociatively adsorbed N-2 which may be the major reason why the Ru/BaZrO3 catalyst exhibited so high activity for ammonia synthesis.
Keyword :
alkaline earth metal alkaline earth metal ammonia synthesis ammonia synthesis perovskite perovskite ruthenium catalysts ruthenium catalysts zirconium zirconium
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GB/T 7714 | Wang Ziqing , Ma Yuncui , Lin Jianxin et al. Effect of alkali earth metals on performance of zirconium-based perovskite composite oxides supported ruthenium for ammonia synthesis [J]. | CHINESE JOURNAL OF CATALYSIS , 2013 , 34 (2) : 361-366 . |
MLA | Wang Ziqing et al. "Effect of alkali earth metals on performance of zirconium-based perovskite composite oxides supported ruthenium for ammonia synthesis" . | CHINESE JOURNAL OF CATALYSIS 34 . 2 (2013) : 361-366 . |
APA | Wang Ziqing , Ma Yuncui , Lin Jianxin , Wang Rong , Wei Kemei . Effect of alkali earth metals on performance of zirconium-based perovskite composite oxides supported ruthenium for ammonia synthesis . | CHINESE JOURNAL OF CATALYSIS , 2013 , 34 (2) , 361-366 . |
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Ammonia synthesis reaction was performed over a novel ruthenium catalyst supported on perovskite-type BaTiO3. It was quite worth noting that Ru/BaTiO3 catalyst exhibited outstanding activity for ammonia synthesis. The results of XRD, CO2-TPD, H-2-TPR and TEM indicated that the strong metal-support interaction (SMSI) between a partially reduced support and Ru combined with strong basicity of support was responsible for such high catalytic activity. The electrons could be easily transferred from the support to the surface of Ru particles by the SMSI effect facilitated the cleavage of NN and greatly enhanced the activity for ammonia synthesis. Crown Copyright (C) 2012 Published by Elsevier B.V. All rights reserved.
Keyword :
Ammonia synthesis Ammonia synthesis Basicity Basicity Perovskite Perovskite Ruthenium catalyst Ruthenium catalyst SMSI SMSI
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GB/T 7714 | Wang, Ziqing , Lin, Jianxin , Wang, Rong et al. Ammonia synthesis over ruthenium catalyst supported on perovskite type BaTiO3 [J]. | CATALYSIS COMMUNICATIONS , 2013 , 32 : 11-14 . |
MLA | Wang, Ziqing et al. "Ammonia synthesis over ruthenium catalyst supported on perovskite type BaTiO3" . | CATALYSIS COMMUNICATIONS 32 (2013) : 11-14 . |
APA | Wang, Ziqing , Lin, Jianxin , Wang, Rong , Wei, Kemei . Ammonia synthesis over ruthenium catalyst supported on perovskite type BaTiO3 . | CATALYSIS COMMUNICATIONS , 2013 , 32 , 11-14 . |
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A series of Ag-Ru/CeO2 catalysts were prepared by conventional impregnation methods and characterized by XRD, BET, XPS, H-2-TPR, H-2-TPD-MS, and N-2-TPD. The activity test shows that ammonia concentration of the catalyst with 6% Ag is 9.4% at 10 MPa, 10,000 h(-1), 400 degrees C, which is 22% higher than that of Ru/CeO2. Such high catalytic activity was ascribed to three effects: electron donating property of partially reduced CeO2-x to Ru metal, the low workfunction of Ru atoms and the less competitive adsorbed between hydrogen and nitrogen on Ru atoms derived from the synergetic effect between Ag and Ru. Crown Copyright (c) 2012 Published by Elsevier B.V. All rights reserved.
Keyword :
Ammonia synthesis Ammonia synthesis CeO2 CeO2 Ruthenium catalyst Ruthenium catalyst Silver Silver SMSI SMSI
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GB/T 7714 | Lin, Jianxin , Zhang, Liuming , Wang, Ziqing et al. The effect of Ag as a promoter for Ru/CeO2 catalysts in ammonia synthesis [J]. | JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL , 2013 , 366 : 375-379 . |
MLA | Lin, Jianxin et al. "The effect of Ag as a promoter for Ru/CeO2 catalysts in ammonia synthesis" . | JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL 366 (2013) : 375-379 . |
APA | Lin, Jianxin , Zhang, Liuming , Wang, Ziqing , Ni, Jun , Wang, Rong , Wei, Kemei . The effect of Ag as a promoter for Ru/CeO2 catalysts in ammonia synthesis . | JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL , 2013 , 366 , 375-379 . |
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The Ba-doped ZrO2 materials were prepared by three methods and used as support for Ru catalysts for ammonia synthesis, i.e., citric acid sol-gel method (SG), modified co-precipitation (CP) and impregnation method (IP). The certain amount of analytical-grade Zr(NO3)(4)center dot 5H(2)O and Ba(NO3)(2) were dissolved in deionized water to form a transparent mixed nitrate solution. The citric acid was slowly added into the mixture to form a transparent solution and then heated to 80 degrees C under vigorous stirring until all the water evaporated and a viscous material was obtained. After calcination at 750 degrees C for 5 h and a puffy white powder was obtained. This was BZ-SG. The solution of NH3 center dot H2O and K2C2O4H2O was added dropwise to the mixture solution of Zr(NO3)(4)center dot 5H(2)O and Ba(NO3)(2) with vigorous stirring, and the obtained white suspension was aged at 60 degrees C for 60 min. The resulting precipitate was centrifuged and washed with distilled water for several times, and then calcined at 750 C for 5 h. The obtained white solid was named as BZ-CP. The Zr(OH)(4) was prepared by adding the KOH into the Zr(NO3)(4)center dot 5H(2)O solution. Then the obtained Zr(OH)(4) was baked at 300 C for 3 h and impregnated with aqueous solution of Ba(NO3)2. After dried at 85 degrees C for 12 h, the sample was heated at 750 degrees C for 5 h and obtained the BZ-IP sample. Ruthenium catalysts were prepared by impregnating the supports directly with K2RuO4 solution. After reduction with ethyl alcohol, then was dried at 120 degrees C for 12 h. The samples with 4 wt% Ru were labeled as RBZ-X (X= SG CP and IP). The molar ratio of Ba to Zr in all the samples is 1: 9. The composites materials and catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction of H-2 (H-2-TPR), temperature programmed desorption of CO2 (CO2-TPD), N-2 adsorption desorption isotherms, scanning electron microscopy (SEM), transmission electron microscopy (TEM) and CO chemisorption. The results displayed that the RBZ-SG catalyst showed the highest activity for ammonia synthesis compared to those of RBZ-CP and RBZ-IP. The optimum ammonia concentration over RBZ-SG catalyst is 5.72% under the conditions of 3 MPa, 10000h(-1) and 425 degrees C. This activity is 3.8 and 14.3 times of that of RBZ-CP and RBZ-IP, respectively. Such high activity is mainly resulted from the presence of BaZrO3, which has high electron-donating ability. Mobile electrons would be transferred from BaZrO3 to the Ru metal surface by means of the strong metal-support interaction existed between Ru and reduction BaZrO3, which can facilitate the cleavage of N equivalent to N and enhance the activity for ammonia synthesis sufficiently.
Keyword :
ammonia synthesis ammonia synthesis barium barium preparation method preparation method ruthenium catalysts ruthenium catalysts zirconium zirconium
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GB/T 7714 | Wang Ziqing , Chen Geng , Lin Jianxin et al. Preparation of Ru/Ba-ZrO2 Catalyst and Its Performance for. Ammonia Synthesis [J]. | ACTA CHIMICA SINICA , 2013 , 71 (2) : 205-212 . |
MLA | Wang Ziqing et al. "Preparation of Ru/Ba-ZrO2 Catalyst and Its Performance for. Ammonia Synthesis" . | ACTA CHIMICA SINICA 71 . 2 (2013) : 205-212 . |
APA | Wang Ziqing , Chen Geng , Lin Jianxin , Wang Rong , Wei Kemei . Preparation of Ru/Ba-ZrO2 Catalyst and Its Performance for. Ammonia Synthesis . | ACTA CHIMICA SINICA , 2013 , 71 (2) , 205-212 . |
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采用柠檬酸络合法制备了一系列不同含量Ba掺杂的ZrO2,再用浸渍法制备了K-Ru/Ba-ZrO2催化剂并将其用于氨合成反应.采用X射线衍射和CO2程序升温脱附技术考察了Ba含量对催化剂结构与性能的影响.结果表明,Ba掺入ZrO2后形成的BaZrO3有助于其负载的Ru催化剂氨合成活性的显著提高.在5.0MPa,10000h–1,425oC时,Ru/Ba-ZrO2(Ba:Zr摩尔比为1:1)催化剂活性最高,出口氨浓度和反应速率分别达9.24%和29.77mmol/(g·h).这主要归因于载体的强电子传导性能和碱性提高.
Keyword :
二氧化锆 二氧化锆 氨合成 氨合成 电子作用 电子作用 钌 钌 钡 钡
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GB/T 7714 | 林建新 , 王自庆 , 张留明 et al. 柠檬酸络合法制备Ba促进ZrO_2负载Ru催化剂上氨合成反应性能 [J]. | 催化学报 , 2012 , 33 (07) : 1075-1079 . |
MLA | 林建新 et al. "柠檬酸络合法制备Ba促进ZrO_2负载Ru催化剂上氨合成反应性能" . | 催化学报 33 . 07 (2012) : 1075-1079 . |
APA | 林建新 , 王自庆 , 张留明 , 倪军 , 王榕 , 魏可镁 . 柠檬酸络合法制备Ba促进ZrO_2负载Ru催化剂上氨合成反应性能 . | 催化学报 , 2012 , 33 (07) , 1075-1079 . |
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采用氧化-还原共沉淀法制备了Pr掺杂的Ru/CeO2-PrO2氨合成催化剂,并运用N2物理吸附、X射线粉末衍射、H2程序升温还原、CO化学吸附、N2程序升温脱附、场发射扫描电镜、高分辨透射电镜和X射线光电子能谱等技术对其进行了表征,考察了Pr添加量对催化剂表面结构和性能的影响.结果表明,Pr掺杂对Ru/CeO2催化剂的比表面积和Ru分散度都有所影响.当CeO2中Pr掺杂量为4%时,在425oC,10MPa,10000h–1的反应条件下,氨合成转化频率可达到12.13×10–2s–1,较Ru/CeO2催化剂提高了58%,这主要归结于复合材料电子传导性能的提高.
Keyword :
二氧化铈 二氧化铈 氨合成 氨合成 电子传递 电子传递 负载型催化剂 负载型催化剂 钌 钌 镨 镨
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GB/T 7714 | 林建新 , 张留明 , 王自庆 et al. Pr掺杂对Ru/CeO_2催化剂结构和氨合成性能的影响 [J]. | 催化学报 , 2012 , 33 (03) : 536-542 . |
MLA | 林建新 et al. "Pr掺杂对Ru/CeO_2催化剂结构和氨合成性能的影响" . | 催化学报 33 . 03 (2012) : 536-542 . |
APA | 林建新 , 张留明 , 王自庆 , 王榕 , 魏可镁 . Pr掺杂对Ru/CeO_2催化剂结构和氨合成性能的影响 . | 催化学报 , 2012 , 33 (03) , 536-542 . |
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