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添加水蒸气对CH4-CO2重整催化剂Ni/CeO2-ZrO2-Al2O3中Ni组份结构影响的EXAFS研究 认领 引用
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作者 李春林 伏义路 +4 位作者 孟明 卞国柱 谢亚宁 胡天斗 张静 《北京同步辐射装置年报》 2002年第1期77-79,共3页
采用水热合成法制备了Ni/CeO2-ZrO2-A12O3催化剂。进行了添加和不添加水蒸气的CH4-CO2催化重整反应,测量了积碳量,并用EXAFS手段测试了催化剂Ni的K吸收边。结果表明,反应前后最近邻Ni—Ni配位距离无明显变化,而配位数却变化明显。... 采用水热合成法制备了Ni/CeO2-ZrO2-A12O3催化剂。进行了添加和不添加水蒸气的CH4-CO2催化重整反应,测量了积碳量,并用EXAFS手段测试了催化剂Ni的K吸收边。结果表明,反应前后最近邻Ni—Ni配位距离无明显变化,而配位数却变化明显。无水蒸气反应后Ni-Ni配位数有较大幅度的减少,而添加了水蒸汽,Ni—Ni配位数比反应前减少幅度小。水蒸气的添加能减少积碳量,稳定催化剂中Ni的结构,从而提高催化反应的稳定性。 展开更多
关键词 水蒸气 CH4 CO2 Ni/CeO2-ZrO2-A12O3催化剂 水热合成法 EXAFS 配位数 催化反应
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水蒸汽对Ni/CeO_2-ZrO_2-Al_2O_3催化剂上CO_2+CH_4重整反应的影响 认领 引用 被引量:11
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作者 李春林 伏义路 +4 位作者 孟明 卞国柱 谢亚宁 胡天斗 张静 《Chinese Journal of Chemical Physics》 SCIE CAS 北大核心 2004年第1期95-99,共5页
用水热合成法制备了Ni/CeO2 ZrO2 Al2 O3 催化剂 .进行了添加和不添加水蒸汽的CH4 +CO2 催化重整反应 ,测试了活性和稳定性 ,测量了积碳量 ,并用XAFS手段测试了催化剂Ni的K吸收边 .结果表明 ,在反应过程中有CeAlO3 的生成 ,但积碳是无... 用水热合成法制备了Ni/CeO2 ZrO2 Al2 O3 催化剂 .进行了添加和不添加水蒸汽的CH4 +CO2 催化重整反应 ,测试了活性和稳定性 ,测量了积碳量 ,并用XAFS手段测试了催化剂Ni的K吸收边 .结果表明 ,在反应过程中有CeAlO3 的生成 ,但积碳是无水蒸汽添加的反应活性降低的原因 .反应气中添加水蒸汽能够减少积碳 ,从而提高催化反应的稳定性 .由于碳原子插入Ni晶格 ,无水蒸汽反应后的最近邻Ni Ni配位数有较大幅度的减少 .添加了水蒸汽的反应 ,最近邻Ni Ni配位数比反应前减少幅度小 ,这主要是由于在反应气中添加水蒸汽减少了积碳 。 展开更多
关键词 CO2+CH4重整反应 添加水蒸汽 Ni/CeO2-ZrO2-Al2O3催化剂 XAFS 积碳
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Catalytic Partial Oxidation of Methane over Ni/CeO_2-ZrO_2-Al_2O_3 认领 引用 被引量:10
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作者 梅大江 陈耀强 +3 位作者 钟俊波 魏振玲 马迪 龚茂初 《Journal of Rare Earths》 SCIE EI CAS 2007年第3期311-315,共5页
Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron sp... Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron spectroscopy(XPS).Through the test of catalytic partial oxidation of methane(CPOM),Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts. 展开更多
关键词 Ni/CeO2-ZrO2-Al2O3 catalyst catalytic partial oxidation of methane carbon deposition rare earths
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Partial oxidation of methane on Ni/CeO_2-ZrO_2/γ-Al_2O_3 prepared using different processes 认领 引用 被引量:6
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作者 张青蔚 沈美庆 +2 位作者 温静 王军 费亚南 《Journal of Rare Earths》 SCIE EI CAS 2008年第3期347-351,共5页
The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane (POM) were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were charac... The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane (POM) were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were characterized by XRD, TPR, H2-chemsorption, and TG-DTA. For fresh catalysts, the results showed that the salt precursor mixing catalyst (ATOM) presented better performance than the catalysts prepared by the precipitator mixing method (MOL) and the powder mechanically mixing method (MECH). The result of XRD suggested that the interaction between CeO2-ZrO2 and Al2O3 in ATOM sample was stronger than the others, which led to more lattice defects and thereby better initial activity. Moreover, the MECH sample had the best stability and the least coke deposition in 24 h stability tests. The results of TPR and H2-chemsorption indicated that the intimate contact of Ni-Al in MECH sample enhanced the ability of resisting coke deposition and metal sintering. 展开更多
关键词 POM CeO2-ZrO2,γ-Al2O3, Ni based catalyst rare earths
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添加水蒸气对CH_4-CO_2重整催化剂Ni/CeO_2-ZrO_2-Al_2O_3中Ni组分结构影响的EXAFS研究 认领 引用 被引量:3
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作者 李春林 伏义路 +4 位作者 孟明 卞国柱 谢亚宁 胡天斗 张静 《核技术》 EI CAS 北大核心 2002年第10期879-882,共4页
采用水热合成法制备了Ni/CeO2 -ZrO2 -Al2 O3催化剂。进行了添加和不添加水蒸气的CH4 -CO2 催化重整反应 ,测量了积碳量 ,并用EXAFS手段测试了催化剂Ni的K吸收边。结果表明 ,反应前后最近邻Ni-Ni配位距离无明显变化 ,而配位数却变化明... 采用水热合成法制备了Ni/CeO2 -ZrO2 -Al2 O3催化剂。进行了添加和不添加水蒸气的CH4 -CO2 催化重整反应 ,测量了积碳量 ,并用EXAFS手段测试了催化剂Ni的K吸收边。结果表明 ,反应前后最近邻Ni-Ni配位距离无明显变化 ,而配位数却变化明显。无水蒸气反应后Ni-Ni配位数有较大幅度的减少 ;而添加了水蒸气 ,Ni-Ni配位数比反应前减少幅度小。水蒸气的添加能减少积碳量 ,稳定催化剂中Ni的结构 。 展开更多
关键词 CH4 CO2 CeO2 ZrO2 Al2O3 Ni组分 水热合成法 铈锆固熔体 催化剂 EXAFS 水蒸汽 合成气 氧化铝 二氧化铈 甲烷 二氧化碳 氧化锆
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载体焙烧温度对Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂在甲烷自热重整制氢反应中催化性能的影响 认领 引用
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作者 蔡秀兰 邹汉波 林维明 《工业催化》 CAS 2010年第5期10-13,共4页
采用浸渍-共沉淀法制备Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂,Ni负载质量分数为10%。在固定床微反装置考察载体焙烧温度(600℃=、700℃、800℃和900℃)对Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂在甲烷自热重整制氢反应中催化性能的影响。结果表... 采用浸渍-共沉淀法制备Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂,Ni负载质量分数为10%。在固定床微反装置考察载体焙烧温度(600℃=、700℃、800℃和900℃)对Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂在甲烷自热重整制氢反应中催化性能的影响。结果表明,载体焙烧温度800℃制备的催化剂活性较好。由XRD和TPR分析可知,随着焙烧温度的升高,各衍射峰的峰强度增强,峰尖锐,说明随着焙烧温度的升高,催化剂中各氧化物晶粒增大。焙烧温度800℃的Ni/CuO-ZrO_2-CeO_2-Al_2O_3催化剂的NiO峰强度较小,说明在该催化剂上NiO以高度分散的状态存在于催化剂表面。 展开更多
关键词 催化剂工程 Ni/CuO-ZrO2-CeO2-Al2O3催化剂 甲烷 焙烧温度 自热重整 制氢
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共沉淀法制备的CeO2-ZrO2-Al2O3材料及性能 认领 引用 被引量:11
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作者 李红梅 周菊发 +4 位作者 祝清超 曾少华 魏振玲 陈耀强 龚茂初 《高等学校化学学报》 SCIE CAS 北大核心 2009年第12期2484-2486,共3页
CeO2-based oxygen materials were prepared with co-precipitation method and characterized via Brunauer-Emmet Teller(BET)method,X-ray diffraction(XRD)and temperature-programmed reduction(H2-TPR).This paper revealed that... CeO2-based oxygen materials were prepared with co-precipitation method and characterized via Brunauer-Emmet Teller(BET)method,X-ray diffraction(XRD)and temperature-programmed reduction(H2-TPR).This paper revealed that three CeO2-based oxygen storage materials are all forming homogeneous solid solution.Among the samples,CeO2-ZrO2-Al2O3(CZA)has the best textural properties and excellent thermal stability.The specific surface area and pore volume of aged CZA are 90 m2/g and 0.29 mL/g.We proposed a viewpoint:Al3+ might insert among the interspace of fluorite structure or highly dispersal in solid solutions. 展开更多
关键词 CeO2-ZrO2-Al2O3 共沉淀法 热稳定性能 结构性能 固溶体
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Synthesis of neodymium modified CeO_2-ZrO_2-Al_2O_3 support materials and their application in Pd-only three-way catalysts 认领 引用 被引量:8
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作者 彭娜 周菊发 +3 位作者 陈山虎 罗秀超 陈耀强 龚茂初 《Journal of Rare Earths》 SCIE EI CAS CSCD 2012年第4期342-349,共8页
Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffTaction (XRD), low temperature nitrogen adsorption-desorption,... Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffTaction (XRD), low temperature nitrogen adsorption-desorption, oxygen pulsing technique, H2-temperamre programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The Pd-only three-way catalysts (Pd-TWC) supported on these materials were prepared by incipient wetness method and studied by activity tests. The results demonstrated that the CZAN supports obtained by the two methods showed better structural, textural and redox properties than the CZA without Nd2O3, and the addition of Nd203 improved the catalytic activity of TWC. Especially, the CZAN-i support prepared by impregnation method had better thermal stability and redox property. Meanwhile, the Pd/CZAN-i catalyst exhibited the best catalytic performance. XPS measurements indicated that the Nd-modified samples possessed more Ce3+ and oxygen vacancies on the surface of samples, which led to a better redox property. The excellent redox property of support materials helped to improve the catalytic activity of TWC. 展开更多
关键词 CeO2-ZrO2-Al2O3 support materials Nd2O3 Ce-O-Nd bonds Pd-only three-way catalysts redox property rare earths
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不同铈添加量对CeO_2-ZrO_2-Al_2O_3材料性能的影响 认领 引用 被引量:8
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作者 唐石云 焦毅 +4 位作者 李小双 王云 王键礼 龚茂初 陈耀强 《无机化学学报》 SCIE CAS CSCD 北大核心 2012年第5期965-970,共6页
采用共沉淀法制备了一系列不同铈添加量的CeO2-ZrO2-Al2O3(CZA)储氧材料,并通过XRD、低温N2吸附-脱附、氧脉冲吸附(OSC)和H2-TPR等手段进行了表征。XRD结果表明,在1 000和1 100℃高温焙烧后,当CeO2添加量为8%时样品具有最好的结构稳定... 采用共沉淀法制备了一系列不同铈添加量的CeO2-ZrO2-Al2O3(CZA)储氧材料,并通过XRD、低温N2吸附-脱附、氧脉冲吸附(OSC)和H2-TPR等手段进行了表征。XRD结果表明,在1 000和1 100℃高温焙烧后,当CeO2添加量为8%时样品具有最好的结构稳定性能。N2吸附-脱附结果表明,CeO2添加量为8%时样品具有最好的织构性能,1 000℃时,比表面积和孔容分别为:136.6 m2.g-1和0.38 mL.g-1;1 100℃时,比表面积和孔容分别为:83.7 m2.g-1和0.23 mL.g-1。OSC结果显示,CeO2添加量为8%时样品具有最大的储氧量,1 000℃和1 100℃分别为70μmol.g-1和31μmol.g-1。H2-TPR结果表明,CeO2添加量为8%时样品具有最佳的还原性能。 展开更多
关键词 CeO2-ZrO2-Al2O3 结构性能 储氧性能 还原性能
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Performance of Pd/CeO_2-ZrO_2-Al_2O_3 catalyst for motorcycle 认领 引用 被引量:5
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作者 赵明 陈山虎 +2 位作者 张晓玉 龚茂初 陈耀强 《Journal of Rare Earths》 SCIE EI CAS 2009年第5期728-732,共5页
The Pd-only catalysts for motorcycle were prepared by impregnating CeO2-ZrO2-Al2O3 and CeO2-ZrO2+Al2O3 with PdCl2 aqueous solution and characterized by X-ray diffraction (XRD), oxygen storage capacity (OSC) and H2-tem... The Pd-only catalysts for motorcycle were prepared by impregnating CeO2-ZrO2-Al2O3 and CeO2-ZrO2+Al2O3 with PdCl2 aqueous solution and characterized by X-ray diffraction (XRD), oxygen storage capacity (OSC) and H2-temperature-programmed reduction (H2-TPR) methods. The XRD result indicated that the CeO2-ZrO2-Al2O3 compound prepared by co-precipitation formed a single solid solution and had good thermal stability, and Pd phase was not observed in all catalysts. The TPR results showed that the reduction temperature of Pd/CeO2-ZrO2-Al2O3 catalyst was lower than that of Pd/CeO2-ZrO2+Al2O3 catalyst whether they were fresh or aged catalysts. The Pd/CeO2-ZrO2-Al2O3 exhibited high three-way catalytic activity at low temperature, high thermal stability, and wide working window, suggesting a great potential for applications. 展开更多
关键词 CeO2-ZrO2-Al2O3 palladium TWC H2-TPR motorcycle rare earths
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复合沉淀剂制备的CeO_2-ZrO_2-Al_2O_3材料及其负载的单Pd三效催化剂(英文) 认领 引用 被引量:6
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作者 李红梅 兰丽 +4 位作者 陈山虎 刘达玉 王卫 龚茂初 陈耀强 《物理化学学报》 SCIE CAS CSCD 北大核心 2016年第7期1734-1746,共13页
采用了一种由氨水和碳酸铵组成的复合沉淀剂来制备CeO_2-ZrO_2-Al_2O_3(CZA)复合氧化物。作为对比,分别采用氨水和碳酸铵为沉淀剂制备了另外两个CZA复合氧化物。系统地研究了各CZA材料在织构、结构、氧化还原性能、热老化行为之间的区别... 采用了一种由氨水和碳酸铵组成的复合沉淀剂来制备CeO_2-ZrO_2-Al_2O_3(CZA)复合氧化物。作为对比,分别采用氨水和碳酸铵为沉淀剂制备了另外两个CZA复合氧化物。系统地研究了各CZA材料在织构、结构、氧化还原性能、热老化行为之间的区别,以及其负载的单Pd三效催化剂的催化性能。结果表明,不同的沉淀剂制得的材料中其CeO_2-ZrO_2(CZ)和Al_2O_3之间的相互作用不同。用氨水做沉淀剂时,得到的材料中CZ和Al_2O_3之间的相互作用很小,导致其热稳定性较差。在碳酸铵做沉淀剂的情况下,CZ和Al_2O_3之间具有很强的相互作用,可以提高材料的热稳定性,但同时,CZ固溶体的均一性被严重破坏,使得材料的氧化还原性能不理想。而复合沉淀剂的使用可以有效地平衡CZ和Al_2O3_之间的相互作用,导致得到的CZA材料具有优异的织构、结构性能及良好的热稳定性。因此,其负载的单Pd催化剂表现出最为优异的氧化还原性能和三效催化活性。 展开更多
关键词 CeO2-ZrO2-Al2O3复合氧化物 复合沉淀剂 单Pd三效催化剂 相互作用 热稳定性
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Ni/CeO_2-Al_2O_3催化剂上CH_4-CO_2转化积炭性能的研究 认领 引用 被引量:23
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作者 杨咏来 徐恒泳 李文钊 《高等学校化学学报》 SCIE EI CAS 北大核心 2002年第11期2112-2116,共5页
采用脉冲微量反应技术研究了添加 n型半导体氧化物 Ce O2 对 Ni基催化剂上 CH4积炭 /CO2 消炭性能的影响 ,用 TPR,XPS和氢吸附技术对催化剂进行了表征 .结果表明 ,活性金属原子 Ni与半导体氧化物Ce O2 之间存在金属 -半导体相互作用 ( M... 采用脉冲微量反应技术研究了添加 n型半导体氧化物 Ce O2 对 Ni基催化剂上 CH4积炭 /CO2 消炭性能的影响 ,用 TPR,XPS和氢吸附技术对催化剂进行了表征 .结果表明 ,活性金属原子 Ni与半导体氧化物Ce O2 之间存在金属 -半导体相互作用 ( MSc I) ,Ce O2 的添加提高了活性原子 Ni0的 d电子密度 ,在一定程度上抑制了 CH4分子中 C—Hσ电子向 d轨道的迁移 ,降低了 CH4裂解积炭活性 ;可加强 Ni0原子 d轨道向CO2 空反键 π轨道的电子迁移 ,促进 CO2 分子的活化 ,提高 CO2 的消炭活性 ,使 Ni/Ce O2 -Al2 O3 催化剂具有较强的抗积炭性能 . 展开更多
关键词 Ni/CeO2-Al2O3催化剂 金属-半导体相互作用 金属-载体相互作用 CH4 积炭 CO2 消炭 氧化铈 氧化铝 载体 合成气 甲烷 二氧化碳
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CeO_2和Pd在Ni/γ-Al_2O_3催化剂中的助剂作用 认领 引用 被引量:17
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作者 杨咏来 徐恒泳 李文钊 《物理化学学报》 SCIE CAS 北大核心 2002年第4期321-325,共5页
采用脉冲微反技术研究了添加n型半导体氧化物CeO2及贵金属Pd对Ni/γ-Al2O3催化剂上CH4积炭/CO2消炭反应性能的影响,并运用BET、TPR、CO2-TPSR及氢吸附等技术对催化剂进行了表征.结果表明,n型半导体氧化物CeO2的添加可以降低Ni/γ-Al2O3... 采用脉冲微反技术研究了添加n型半导体氧化物CeO2及贵金属Pd对Ni/γ-Al2O3催化剂上CH4积炭/CO2消炭反应性能的影响,并运用BET、TPR、CO2-TPSR及氢吸附等技术对催化剂进行了表征.结果表明,n型半导体氧化物CeO2的添加可以降低Ni/γ-Al2O3催化剂上CH4裂解积炭活性,提高CO2消炭活性,添加少量贵金属Pd可以进一步改变载体Al2O3、助剂CeO2和活性组分Ni之间的相互作用,从而改善Ni/γ-Al2O3催化剂的抗积炭性能.通过Ni-Ce-Pd/γ-Al2O3催化剂上CH4积炭/CO2消炭模型对上述作用机制作出了新的解释. 展开更多
关键词 CeO2 贵金属Pd Ni/-Al2O3催化剂 助剂 CH4 积炭 CO2 消炭 甲烷 二氧化碳 镍催化剂 二氧化铈 催化重整
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镧、锰共掺杂改性CeO2-ZrO2-Al2O3固溶体的性能 认领 引用 被引量:5
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作者 张雪乔 信欣 +3 位作者 刘建英 刘盛余 赵明 陈耀强 《高等学校化学学报》 SCIE CAS CSCD 北大核心 2011年第10期2360-2366,共7页
采用共沉淀法制备了一系列La,Mn共掺杂的CeO2-ZrO2-A12O3(CZA)复合氧化物,采用BET,XRD,H2-TPR,XPS和XRF等方法对样品进行表征.结果表明,全部样品均形成了稳定的CZA固溶体,经600℃焙烧后表现出良好的织构性能,1000℃老化后,La,Mn共掺杂... 采用共沉淀法制备了一系列La,Mn共掺杂的CeO2-ZrO2-A12O3(CZA)复合氧化物,采用BET,XRD,H2-TPR,XPS和XRF等方法对样品进行表征.结果表明,全部样品均形成了稳定的CZA固溶体,经600℃焙烧后表现出良好的织构性能,1000℃老化后,La,Mn共掺杂样品具有最佳的高温稳定性;H2-TPR测试表明,La,Mn之间存在正协同效应,共掺杂的样品具有最佳的低温还原性能和高温稳定性;XPS结果表明,掺杂La可有效抑制在焙烧过程中Mn向表面的迁移,从而保持较高的表面吸附氧浓度. 展开更多
关键词 CeO2-ZrO2-Al2O3 MnOx 还原性能
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Structures and oxygen storage capacities of CeO_2-ZrO_2-Al_2O_3 ternary oxides prepared by a green route:supercritical anti-solvent precipitation 认领 引用 被引量:9
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作者 黄盼 姜浩锡 张敏华 《Journal of Rare Earths》 SCIE EI CAS CSCD 2012年第6期524-528,共5页
CeO2-ZrO2-Al2O3 ternary oxides were successfully prepared by a green route of supercritical anti-solvent precipitation with supercritical CO2 as anti-solvent and methanol as solvent. The structures and oxygen storage ... CeO2-ZrO2-Al2O3 ternary oxides were successfully prepared by a green route of supercritical anti-solvent precipitation with supercritical CO2 as anti-solvent and methanol as solvent. The structures and oxygen storage capacities of these ternary oxides were characterized by XRD, Raman spectra and oxygen storage capacity measurements. It was found that Al3+ and Zr4+ inserted into CeO2 lattice, forming CeO2-ZrO2-Al2O3 solid solution. The concentration of aluminium isopropoxide in the solution affected the concentration of oxygen vacancy and the distortion of oxygen sublattice which were responsible for the oxygen storage capacity. The rapidest oxygen uptakeelease rate and maximum total oxygen storage capacity (122.0 mmolO2/molCeO2) were obtained with the aluminitun isopropoxide concentration at 0.2 wt.% in the solution. 展开更多
关键词 CeO2-ZrO2-Al2O3 solid solution supercritical anti-solvent precipitation oxygen storage capacity rare earths
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CeO_2-ZrO_2-La_2O_3-Al_2O_3 composite oxide and its supported palladium catalyst for the treatment of exhaust of natural gas engined vehicles 认领 引用 被引量:5
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作者 Xiaoyu Zhang Enyan,Long +5 位作者 Yile Li Jiaxiu Guo Lijuan Zhang Maochu Gong Minghua Wang Yaoqiang Chen 《Journal of Natural Gas Chemistry》 2009年第2期139-144,共6页
Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N... Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost. 展开更多
关键词 Pd catalysts natural gas vehicles exhaust methane oxidation NOx conversion CeO2-ZrO2-Al2O3 La2O3
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掺杂锆对CeO2-ZrO2-Al2O3复合氧化物还原热处理性能的影响 认领 引用 被引量:2
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作者 杨黄根 谭喻方 +5 位作者 韦庆敏 晏全 陈渊 朱立刚 覃利琴 肖益鸿 《材料工程》 EI CAS CSCD 北大核心 2020年第12期90-96,共7页
采用共沉淀法制备铈锆铝复合氧化物CZ x A(Ce,Zr,Al摩尔比为1∶x∶2,其中x=0,0.5,1,1.5,2)新鲜样品,分别在空气和10%H 2/Ar气氛下进行热处理,利用X射线粉末衍射、N 2吸脱附BET法、O 2脉冲吸附、H 2程序升温还原(H 2 temperature-program... 采用共沉淀法制备铈锆铝复合氧化物CZ x A(Ce,Zr,Al摩尔比为1∶x∶2,其中x=0,0.5,1,1.5,2)新鲜样品,分别在空气和10%H 2/Ar气氛下进行热处理,利用X射线粉末衍射、N 2吸脱附BET法、O 2脉冲吸附、H 2程序升温还原(H 2 temperature-programmed reduction,H 2-TPR)等手段研究复合氧化物的结构及性能。结果表明:CZ x A系列样品随着Zr含量的增加,经1100℃还原热处理的CZ 1.5 A-H 2-1100和CZ 2A-H 2-1100样品没有观察到CeAlO 3晶相;其储氧量分别为713,548μmol·g-1,远大于CZA-H 2-1100的23μmol·g-1;H 2-TPR耗氢量分别为1995,2087μmol·g-1,而CZA-H 2-1100样品H 2-TPR耗氢量显著减小,仅为310μmol·g-1,CZ x A储氧性能受还原热处理时CeAlO 3形成的影响,与H 2-TPR耗氢量的变化结果相吻合。研究发现CA样品经还原热处理更易生成CeAlO 3,而在CA中掺杂一定量Zr元素后的CZ 1.5 A,CZ 2A样品能抑制CeAlO 3的形成,从而显著改善材料的储氧性能和H 2-TPR耗氢量,且铈锆铝材料经还原热处理,均具有更好的低温还原性能。 展开更多
关键词 CeO2-ZrO2-Al2O3 还原热处理 CeAlO3 储氧性能 还原性能
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Autothermal reforming of methane over Ni catalysts supported over ZrO2-CeO2-Al2O3 认领 引用 被引量:6
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作者 Xiulan Cai Yuanxing Cai Weiming Lin 《Journal of Natural Gas Chemistry》 2008年第2期201-207,共7页
Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated.... Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. The relationship between the structures and catalytic activities of the catalysts was discussed. The results showed that the catalytic activity and stability of the Ni/ZrO2-CeO2-Al2O3 catalyst was better than those of other catalysts with the highest CH4 conversion, H2/CO and H2/COx ratio at 750 ℃. The catalyst showed a little deactivation along the reaction time during its 72 h on stream with the mean deactivation rate of 0.08%/h. The catalytic performance of the Ni/ZrO2-CeO2-Al2O3 catalyst was also affected by reaction temperature, no2 : nCH4 molar ratio and nH2O : nCH4 molar ratio. TPR, XRD and XPS measurements indicated that the formation of ZrO2-CeO2 solid solution could improve the dispersion of NiO, and inhibit the formation of NiAl2O3, and thus significantly promoted the catalytic activity of the Ni/ZrO2-CeO2-Al2O3 catalyst. 展开更多
关键词 methane autothermal reforming hydrogen Ni/ZrO2-CeO2-Al2O3
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掺杂不同量Nd_2O_3对CeO_2-ZrO_2-Al_2O_3材料性能的影响 认领 引用 被引量:3
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作者 彭娜 陈山虎 +2 位作者 周菊发 陈耀强 龚茂初 《无机材料学报》 SCIE EI CAS CSCD 北大核心 2012年第11期1138-1144,共7页
采用共沉淀法制备了一系列Nd2O3含量为0~13wt%的CeO2-ZrO2-A12O3(CZA)复合氧化物,并通过X射线衍射(XRD)、低温N2吸附–脱附、氧脉冲吸附(OSC)、H2–程序升温还原(H2-TPR)及扫描电子显微镜(SEM)等方法对所制备的材料进行了表征.研究结... 采用共沉淀法制备了一系列Nd2O3含量为0~13wt%的CeO2-ZrO2-A12O3(CZA)复合氧化物,并通过X射线衍射(XRD)、低温N2吸附–脱附、氧脉冲吸附(OSC)、H2–程序升温还原(H2-TPR)及扫描电子显微镜(SEM)等方法对所制备的材料进行了表征.研究结果表明,Nd2O3在CZA固溶体中的溶解限约为10wt%,过量Nd的添加会出现分相形成Nd0.5Ce0.5O1.75氧化物.掺杂适量Nd能有效抑制氧化物晶粒的长大,提高材料的热稳定性和氧化还原性能.Nd2O3的掺杂量为10wt%时,样品的织构稳定性最好,1000℃老化5 h后,比表面积和孔容分别达97.14 m2/g和0.44 mL/g.Nd2O3的掺杂量为7wt%时,样品有高的储氧量,经600℃和1000℃焙烧后储氧量分别为938.01μmol/g和821.72μmol/g;体相氧的移动能力最强,还原性能最佳,老化后还原峰温由465℃升高到483℃.SEM结果表明,所制备的材料均为球形颗粒,Nd2O3的添加可以有效阻止高温焙烧过程中粒子的团聚. 展开更多
关键词 CeO2-ZrO2-A12O3 织构性能 氧化还原性能
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Structure and mechanical properties of ZrO_2-mullite nano-ceramics in SiO_2-Al_2O_3-ZrO_2 system 认领 引用 被引量:6
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作者 梁叔全 谭小平 +1 位作者 李少强 唐艳 《Journal of Central South University of Technology》 2007年第1期1-6,共6页
ZrO2-mullite nano-ceramics were fabricated by in-situ controlled crystallizing from SiO2-Al2O3-ZrO2 amorphous bulk. The thermal transformation sequences of the SiO2-Al2O3-ZrO2 amorphous bulk were investigated by X-ray... ZrO2-mullite nano-ceramics were fabricated by in-situ controlled crystallizing from SiO2-Al2O3-ZrO2 amorphous bulk. The thermal transformation sequences of the SiO2-Al2O3-ZrO2 amorphous bulk were investigated by X-ray diffraction, infrared spectrum, scanning electron microscope and differential scanning calorimetric. And the mechanical properties of the nano-ceramics were studied. The results show that the bulks are still in amorphous state at 900 ℃ and the t-ZrO2 forms at about 950 ℃ with a faint spinel-like phase which changes into mullite on further heating. ZrO2 and mullite become major phases at 1 100 ℃ and an amount of m-ZrO2 occur at the same time. The sample heated at 950 ℃ for 2 h and then at 1 100 ℃ for 1 h shows very dense and homogenous microstructure with ball-like grains in size of 20-50 nm. With the increase of crystallization temperature up to 1 350 ℃, the grains grow quickly and some grow into lath-shaped grains with major diameter of 5 μm. After two-step treatment the highest micro-hardness, flexural strength and fracture toughness of the samples are 13.72 GPa, 520 MPa and 5.13 MPa·m1/2, respectively. 展开更多
关键词 SiO2-Al2O3-ZrO2 system amorphous bulk heat treatment structural change mechanical properties
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