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学者姓名：郑起
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Abstract ：
CuO/CeO2 is a kind of promising catalysts for the water-gas shift (WGS) reaction. Efforts were put in to improve its performance through modification of CeO2 support. In this study, portions of CeO2 prepared by a co-precipitation method were separately annealed at 300 degrees C in air, under vacuum and with H-2, and were used as supports for the fabrication of CuO/CeO2 catalysts. The physicochemical properties of the catalysts were characterized by X-ray diffraction, N-2-physisorption, inductively coupled plasma, Raman spectroscopy, CO2 temperature-programmed desorption, and H-2 temperature-programmed reduction techniques. The relation between catalytic performances and physicochemical properties of the CuO/CeO2 catalysts were discussed. Among the three catalysts, the one with CuO supported on H-2-reduced CeO2 shows the highest catalytic activity, mainly due to strong CuO-CeO2 synergetic interaction and high concentration of Frenkel-type oxygen vacancies. The superior catalytic activities can also be attributed to the Cu-0 crystals of small size and the oxygen vacancies in non-stoichiometric CeO2-x.
Keyword ：
cerium oxide cerium oxide copper oxide copper oxide oxygen vacancy oxygen vacancy synergetic interaction synergetic interaction water-gas shift water-gas shift
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| GB/T 7714 | Chen, Chongqi , Zhan, Yingying , Zhou, Jianke et al. Cu/CeO2 Catalyst for Water-Gas Shift Reaction: Effect of CeO2 Pretreatment [J]. | CHEMPHYSCHEM , 2018 , 19 (12) : 1448-1455 . |
| MLA | Chen, Chongqi et al. "Cu/CeO2 Catalyst for Water-Gas Shift Reaction: Effect of CeO2 Pretreatment" . | CHEMPHYSCHEM 19 . 12 (2018) : 1448-1455 . |
| APA | Chen, Chongqi , Zhan, Yingying , Zhou, Jianke , Li, Dalin , Zhang, Yanjie , Lin, Xingyi et al. Cu/CeO2 Catalyst for Water-Gas Shift Reaction: Effect of CeO2 Pretreatment . | CHEMPHYSCHEM , 2018 , 19 (12) , 1448-1455 . |
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Abstract ：
CuO/CeO2 is a promising catalyst for water-gas shift (WGS) reaction in H-2 production. Much effort has been devoted to improving its catalytic activity and stability by CeO2 support modification or introduction of secondary active species. Here a method to enhance the catalytic performance by controlling the deposition rate of copper is reported. The nature of CuO and CuO-CeO2 synergetic interaction are modulated by using different copper sources (Cu(NO3)(2) and Cu[(NH3)](4)(2+)) and controlling reaction temperatures. The as-prepared CuO-CeO2 catalysts show distinguish catalytic performances for the WGS reaction. The one prepared by using Cu[(NH3)](4)(2+)) at the reaction temperature of 30 degrees C (CuCe-30N) shows superior catalytic activity and stability. The CuCe-30N catalyst possesses the largest Cu-0 surface area (39.2 m(2) g(cat)(-1)) and strongest CuO-CeO2 synergetic interaction. The largest Cu-0 surface area provides the most active sites for CO adsorption thus leading to its highest activity. The strong synergetic interaction prevents Cu crystallites from sintering during the WGS reaction, thus improving its thermal stability.
Keyword ：
Cu-0 surface area Cu-0 surface area CuO/CeO2 catalysts CuO/CeO2 catalysts synergetic interactions synergetic interactions water-gas shift reaction water-gas shift reaction
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| GB/T 7714 | Chen, Chongqi , Zhan, Yingying , Li, Dalin et al. Preparation of CuO/CeO2 Catalyst with Enhanced Catalytic Performance for Water-Gas Shift Reaction in Hydrogen Production [J]. | ENERGY TECHNOLOGY , 2018 , 6 (6) : 1096-1103 . |
| MLA | Chen, Chongqi et al. "Preparation of CuO/CeO2 Catalyst with Enhanced Catalytic Performance for Water-Gas Shift Reaction in Hydrogen Production" . | ENERGY TECHNOLOGY 6 . 6 (2018) : 1096-1103 . |
| APA | Chen, Chongqi , Zhan, Yingying , Li, Dalin , Zhang, Yanjie , Lin, Xingyi , Jiang, Lilong et al. Preparation of CuO/CeO2 Catalyst with Enhanced Catalytic Performance for Water-Gas Shift Reaction in Hydrogen Production . | ENERGY TECHNOLOGY , 2018 , 6 (6) , 1096-1103 . |
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Abstract ：
分别以空气和氮气焙烧的ZrO2圆形纳米片(标记为ZrO2-Air和ZrO2-N2)为载体,采用沉积-沉淀法制得1％Au/ZrO2催化剂(标记为Au/ZrO2-Air和Au/ZrO2-N2).考察了富氢气氛下上述催化剂的水煤气变换反应(WGSR)催化性能,发现Au/ZrO2-Air的催化活性明显高于Au/ZrO2-N2,且显著优于Au负载量较高的Au/Fe2 O3和Au/CeO2催化剂.采用XRD、AAS、N2物理吸脱附、TEM、UV-Vis DRS及EPR等手段研究了两种气氛焙烧的ZrO2载体和相应Au/ZrO2催化剂的结构及表面性质.结果表明,两种ZrO2载体的晶相结构及织构性能无明显差异,但两种ZrO2载体上表面缺陷种类和浓度分布差别较大.相较于ZrO2-N2,ZrO2-Air的表面具有较多的配位不饱和Zr3+,这些位点有助于提高负载Au的分散度,使得Au/ZrO2-Air具有较高的催化活性.
Keyword ：
Au/ZrO2催化剂 Au/ZrO2催化剂 Au分散度 Au分散度 氮气焙烧 氮气焙烧 水煤气变换反应 水煤气变换反应 空气焙烧 空气焙烧 配位不饱和Zr3+ 配位不饱和Zr3+
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| GB/T 7714 | 张燕杰 , 陈崇启 , 詹瑛瑛 et al. ZrO2空气焙烧与氮气焙烧对Au/ZrO2水煤气变换催化剂性能的影响 [J]. | 闽江学院学报 , 2018 , 39 (2) : 54-61 . |
| MLA | 张燕杰 et al. "ZrO2空气焙烧与氮气焙烧对Au/ZrO2水煤气变换催化剂性能的影响" . | 闽江学院学报 39 . 2 (2018) : 54-61 . |
| APA | 张燕杰 , 陈崇启 , 詹瑛瑛 , 林棋 , 娄本勇 , 郑国才 et al. ZrO2空气焙烧与氮气焙烧对Au/ZrO2水煤气变换催化剂性能的影响 . | 闽江学院学报 , 2018 , 39 (2) , 54-61 . |
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ZrO2 doped with various concentrations of yttrium(0-5%) was prepared by a hydrothermal homogeneous co-precipitation method and CuO was then deposited on ZrO2 by a deposition-precipitation method to get the yttrium promoted CuO/ZrO2 catalyst; its performance in the water-gas shift reaction for producing hydrogen was then investigated. The results indicate that the catalytic activity of CuO/ZrO2 can be effectively improved by yttrium modification; over the yttrium promoted CuO/ZrO2 catalyst with an yttrium concentration of 2%, the CO conversion reaches 91.4% at 270, much higher than those over the conventional CuO/ZnO and CuO/CeO2 catalysts. The XRD, N2-physisorption, N2O titration, SEM and CO-TPR characterization results reveal that Y3+ is successfully incorporated into the lattice of ZrO2, which has a great influence on the structure and reducibility of the CuO/ZrO2 catalysts. Y3+ doping into ZrO2 introduces oxygen vacancies, improving the dispersion of CuO and increasing the proportion of catalytically active Cu-[O]-Zr species. In addition, the introduction of yttrium improves the monodispersity and modifies the texture properties of the CuO/ZrO2 catalysts. As a result, the superior activity of 2% yttrium promoted CuO/ZrO2 catalyst is probably attributed to the abundance of Cu-[O]-Zr species, high reducibility of Cu-[O]-Zr species and surface hydroxyl groups, high monodispersity and proper textural properties. © 2017, Science Press. All right reserved.
Keyword ：
Catalyst activity Catalyst activity Cerium compounds Cerium compounds Chemical shift Chemical shift Copper oxides Copper oxides Hydrogen production Hydrogen production Oxygen vacancies Oxygen vacancies Precipitation (chemical) Precipitation (chemical) Textures Textures Water gas shift Water gas shift Yttrium Yttrium Zirconia Zirconia
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| GB/T 7714 | Zhang, Yan-Jie , Chen, Chong-Qi , Zhan, Ying-Ying et al. Highly active Y-promoted CuO/ZrO2 catalysts for the production of hydrogen through water-gas shift reaction [J]. | Journal of Fuel Chemistry and Technology , 2017 , 45 (9) : 1137-1145 . |
| MLA | Zhang, Yan-Jie et al. "Highly active Y-promoted CuO/ZrO2 catalysts for the production of hydrogen through water-gas shift reaction" . | Journal of Fuel Chemistry and Technology 45 . 9 (2017) : 1137-1145 . |
| APA | Zhang, Yan-Jie , Chen, Chong-Qi , Zhan, Ying-Ying , Lin, Qi , Lou, Ben-Yong , Zheng, Guo-Cai et al. Highly active Y-promoted CuO/ZrO2 catalysts for the production of hydrogen through water-gas shift reaction . | Journal of Fuel Chemistry and Technology , 2017 , 45 (9) , 1137-1145 . |
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采用水热法制备了具有不同Y掺杂量的单分散ZrO2纳米粒子(n(Y)/n(Y+Zr)=0-5％),并以其为载体采用沉积-沉淀法制得CuO/ZrO2催化剂;考察了富氢气氛下上述催化剂的水煤气变换反应(WGS)催化性能.结果表明,掺杂Y后催化剂的活性明显提高,其中,载体掺杂2％Y的催化剂具有最佳的催化活性,在270℃时的CO转化率高达91.4％,明显高于研究较多的CuO/ZnO和CuO/CeO2催化剂.X射线粉末衍射、N2物理吸附-脱附、N2O滴定、扫描电镜和CO程序升温还原等表征结果表明,Y3+掺入了ZrO2的晶格并对催化剂的结构和还原性能产生直接影响.Y助剂的引入一方面促进了CuO在ZrO2表面的分散,提高了催化剂表面活性Cu-[O]-Zr物种的含量;另一方面,改善了催化剂的颗粒单分散性和织构性能.载体掺杂2％Y助剂的样品具有较高的Cu-[O]-Zr物种含量、较佳的颗粒单分散性和织构性能,且其表面的Cu-[O]-Zr物种和活性羟基具有较佳的还原性能,因而表现出较高的催化活性.
Keyword ：
CuO/ZrO2催化剂 CuO/ZrO2催化剂 Y助剂 Y助剂 氧空位 氧空位 水煤气变换反应 水煤气变换反应 表面羟基 表面羟基
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| GB/T 7714 | 张燕杰 , 陈崇启 , 詹瑛瑛 et al. Y修饰CuO/ZrO2催化剂高效催化水煤气变换反应制氢 [J]. | 燃料化学学报 , 2017 , 45 (9) : 1137-1145 . |
| MLA | 张燕杰 et al. "Y修饰CuO/ZrO2催化剂高效催化水煤气变换反应制氢" . | 燃料化学学报 45 . 9 (2017) : 1137-1145 . |
| APA | 张燕杰 , 陈崇启 , 詹瑛瑛 , 林棋 , 娄本勇 , 郑国才 et al. Y修饰CuO/ZrO2催化剂高效催化水煤气变换反应制氢 . | 燃料化学学报 , 2017 , 45 (9) , 1137-1145 . |
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The water-gas shift reaction is studied using a series of Cu-Fe composite oxide catalysts, which were prepared by co-precipitation, deposition-precipitation, sol-gel, solid state reaction and mechanical mixing method, respectively. Distinct crystal structure and texture of the as-prepared catalysts were formed, and their reduction properties as well as surface basicities were modulated. The CO conversion in the water gas shift reaction is found to be correlation well with the Cu components in the temperature range of 200-350 degrees C, while the CO conversion is mainly controlled by Fe3O4 sites at temperature above 350 degrees C. The characterization results demonstrate that the formation of CuFe2O4 is ideal to obtain well dispersed Cu crystals; the weak basic sites are positive to the WGS reaction; and the strong interaction between copper and iron species can result in good Cu dispersion. The catalyst that was fabricated by the co-precipitation method, possesses the largest amount of CuFe2O4 and weak basic sites, as well as highly dispersed Cu crystals, thus showing the best catalytic activity and stability for the WGS reaction in our cases. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
Keyword ：
CuFe2O4 CuFe2O4 Cu-Fe composite Cu-Fe composite Surface copper species Surface copper species Water gas shift Water gas shift
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| GB/T 7714 | Lin, Xingyi , Li, Rule , Zhang, Yong et al. The role of surface copper species in Cu-Fe composite oxide catalysts for the water gas shift reaction [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2015 , 40 (4) : 1735-1741 . |
| MLA | Lin, Xingyi et al. "The role of surface copper species in Cu-Fe composite oxide catalysts for the water gas shift reaction" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 40 . 4 (2015) : 1735-1741 . |
| APA | Lin, Xingyi , Li, Rule , Zhang, Yong , Zhan, Yingying , Chen, Chongqi , Zheng, Qi et al. The role of surface copper species in Cu-Fe composite oxide catalysts for the water gas shift reaction . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2015 , 40 (4) , 1735-1741 . |
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Keyword ：
化肥催化剂 化肥催化剂 稀土 稀土
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| GB/T 7714 | 江莉龙 , 林炳裕 , 陈崇启 et al. 稀土在化肥催化剂中的应用 [C] //第二十届全国稀土催化学术会议论文集 . 2015 : 1-2 . |
| MLA | 江莉龙 et al. "稀土在化肥催化剂中的应用" 第二十届全国稀土催化学术会议论文集 . (2015) : 1-2 . |
| APA | 江莉龙 , 林炳裕 , 陈崇启 , 林性贻 , 詹瑛瑛 , 林建新 et al. 稀土在化肥催化剂中的应用 第二十届全国稀土催化学术会议论文集 . (2015) : 1-2 . |
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采用共沉淀法制备了系列铜负载量不同的Cu/Fe2O3水煤气变换(WGS)催化剂,并考察了铜负载量对催化剂结构和水煤气变换反应性能的影响.结果表明,Cu/Fe2O3催化剂呈现出良好的水煤气反应性能,当CuO质量分数为20%时,催化剂的WGS性能最优,250°C时CO转化率高达97.2%,同时热稳定性也最好.运用X射线粉末衍射(XRD)、N2物理吸脱附和H2程序升温还原(H2-TPR)等手段对Cu/Fe2O3催化剂的物相、织构特征及还原性能进行了表征,结果表明,CuFe2O4物种的存在极大地改善了催化剂的还原性能和WGS反应活性.这是由于CuFe2O4特殊的尖晶石结构有利于Cu微晶的稳定;同时,C...
Keyword ：
Cu/Fe2O3催化剂 Cu/Fe2O3催化剂 CuFe2O4 CuFe2O4 水煤气变换 水煤气变换 铜负载量 铜负载量
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| GB/T 7714 | 林性贻 , 马俊涛 , 陈崇启 et al. 铜物种对Cu/Fe_2O_3水煤气变换反应催化剂性能的影响 [J]. | 物理化学学报 , 2014 , 30 (01) : 157-163 . |
| MLA | 林性贻 et al. "铜物种对Cu/Fe_2O_3水煤气变换反应催化剂性能的影响" . | 物理化学学报 30 . 01 (2014) : 157-163 . |
| APA | 林性贻 , 马俊涛 , 陈崇启 , 詹瑛瑛 , 郑起 . 铜物种对Cu/Fe_2O_3水煤气变换反应催化剂性能的影响 . | 物理化学学报 , 2014 , 30 (01) , 157-163 . |
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本发明公开了一种用于水煤气变换反应的CuO-CeO2催化剂及其制备方法，是采用络合沉积沉淀法，将铈盐溶液与碱溶液进行混合，经陈化、冷却、离心、洗涤、干燥得到CeO2载体；然后将载体分散在铜氨络合溶液中，并向其中加入碱溶液进行反应，再经陈化、冷却、离心、洗涤、干燥、焙烧制得CuO-CeO2催化剂。与通常采用沉积沉淀法制得的CuO-CeO2催化剂相比，本发明采用Cu2+络合成[Cu(NH3)4]2+的方式沉积CuO，使活性组分CuO微晶高度分散，对水煤气变换反应具有较高的活性，适用温区宽，适用于制氢工艺中以天然气、轻油等低含硫原料的水煤气变换反应。
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| GB/T 7714 | 陈崇启 , 林性贻 , 詹瑛瑛 et al. 用于水煤气变换反应的CuO-CeO2催化剂及其制备方法 : CN201410285884.X[P]. | 2014/6/25 . |
| MLA | 陈崇启 et al. "用于水煤气变换反应的CuO-CeO2催化剂及其制备方法" : CN201410285884.X. | 2014/6/25 . |
| APA | 陈崇启 , 林性贻 , 詹瑛瑛 , 郑起 . 用于水煤气变换反应的CuO-CeO2催化剂及其制备方法 : CN201410285884.X. | 2014/6/25 . |
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The precipitation processes of CuO-CeO2 catalysts preparation were modified, and their optimized copper content were also studied in detail. As indicated by the experimental results, the WGS catalytic activities of the CuO-CeO2 catalysts can be ranked as: stepwise precipitation (SP) > deposition-precipitation (DP) > co-precipitation (CP), suggesting that stepwise precipitation (i.e., a modified DP) is a convenient and effective method to prepare CuO-CeO2 WGS catalysts. The optimized copper contents of CuO-CeO2-SP and CuO-CeO2-CP catalysts are 20 wt.% and 25 wt.%, respectively. Their catalytic activities can be strongly correlated with the results from XRD, XPS, Raman, N-2-physisorption, N2O chemisorption and H-2-TPR. For DP and SP, a certain amount of copper has substitutively incorporated into ceria lattice with multiple Ce3+ and oxygen vacancies, which is considered as one relatively strong interaction between copper and ceria support. The substitutional incorporation of copper creates larger lattice distortion, lattice defect (embodying as larger lattice cell contraction of CeO2, microstrain and Raman shift) and stronger reducibility (i.e., lower reduction temperature of H2-TPR), as a consequence, higher surface energy and catalytic activity for WGS reaction. While for CP, copper nitrate and cerium nitrate were simultaneously precipitated, resulting in the burial of many copper species in ceria supports, i.e., occupancy incorporation of isolated copper into ceria lattice vacant site, which is considered as another weak interaction between copper and ceria support. Accordingly, combined with N2O chemisorption results, it is demonstrated that surface copper species of CuO-CeO2-CP are fewer and less active than those of CuO-CeO2-DP and CuO-CeO2-SP. Lastly, there is a direct relationship between the pore volume along with most probable pore size of the as-synthesized catalysts and their corresponding catalytic activities for WGS reaction. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
Keyword ：
Copper content Copper content CuO-CeO2 catalysts CuO-CeO2 catalysts Occupancy incorporation Occupancy incorporation Precipitation processes Precipitation processes Substitutional incorporation Substitutional incorporation Water-gas shift reaction Water-gas shift reaction
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| GB/T 7714 | Li, Lei , Song, Li , Chen, Chongqi et al. Modified precipitation processes and optimized copper content of CuO-CeO2 catalysts for water-gas shift reaction [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2014 , 39 (34) : 19570-19582 . |
| MLA | Li, Lei et al. "Modified precipitation processes and optimized copper content of CuO-CeO2 catalysts for water-gas shift reaction" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 39 . 34 (2014) : 19570-19582 . |
| APA | Li, Lei , Song, Li , Chen, Chongqi , Zhang, Yanjie , Zhan, Yingying , Lin, Xingyi et al. Modified precipitation processes and optimized copper content of CuO-CeO2 catalysts for water-gas shift reaction . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2014 , 39 (34) , 19570-19582 . |
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