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合成方法对Rh/CeO2-ZrO2-La2O3催化剂的结构、表面性能及DeNOx活性的影响
引用本文:钟富兰,钟喻娇,杨黄根,肖益鸿,蔡国辉,郑 勇,魏可镁.合成方法对Rh/CeO2-ZrO2-La2O3催化剂的结构、表面性能及DeNOx活性的影响[J].无机化学学报,2011,27(12):2473-2483.
作者姓名:钟富兰  钟喻娇  杨黄根  肖益鸿  蔡国辉  郑 勇  魏可镁
作者单位:福州大学化肥催化剂国家工程研究中心,福州,350002
基金项目:国家科技支撑计划,This work was financially supported by Key Projects in the National Science & Technology Support Program
摘    要:用沉积沉淀法合成两种不同系列的CeO2-ZrO2-La2O3混合氧化物(ZrO2和La2O3沉积CeO2粒子(标记为A-x)以及CeO2和La2O3沉积ZrO2粒子(标记为B-x)),并用作Rh催化剂的载体。XRD、拉曼、TPR、XPS和O2脉冲等表征结果显示出不同的沉积顺序将导致不同的结构和氧化还原性能,且B-x具有更高的氧迁移性、储氧能力和表面Ce浓度。当其负载Rh后,Rh/B-x催化剂具有更高的NO和CO转化率及N2选择性,且Ce的最佳含量为50at%。这可能归因于Rh负载于富铈表面形成更多有利于NO分解的表面Ce3+活性位。

关 键 词:Rh/CeO2-ZrO2-La2O3氧化物  沉积沉淀  表面性能  NO还原

Effect of Synthesis Procedure on Structural Characteristics, Surface Properties and DeNOx Activity of Rh/CeO2-ZrO2-La2O3 Catalysts
ZHONG Fu-Lan,ZHONG Yu-Jiao,YANG Huang-Gen,XIAO Yi-Hong,CAI Guo-Hui,ZHENG Yong and WEI Ke-Mei.Effect of Synthesis Procedure on Structural Characteristics, Surface Properties and DeNOx Activity of Rh/CeO2-ZrO2-La2O3 Catalysts[J].Chinese Journal of Inorganic Chemistry,2011,27(12):2473-2483.
Authors:ZHONG Fu-Lan  ZHONG Yu-Jiao  YANG Huang-Gen  XIAO Yi-Hong  CAI Guo-Hui  ZHENG Yong and WEI Ke-Mei
Institution:National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China,National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China,National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China,National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China,National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China,National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China and National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China
Abstract:Two series of CeO2-ZrO2-La2O3 mixed oxides with a broad range of composition were synthesized by a deposition-precipitation route and used as support for Rh catalysts. The characterization results of XRD, Raman, TPR, XPS, and O2-pulse uptake reveal that the deposition of CeO2 and La2O3 on the ZrO2 particles (denoted as B-x) possesses better oxygen mobility, higher oxygen storage capacity, and higher surface Ce content, superior to the counterpart prepared by depositing ZrO2 and La2O3 on the CeO2 particles (denoted as A-x) as support of Rh catalysts for the NO reduction by CO. The catalytic results show that the Rh/B-x catalysts represent better catalytic activities for the conversions of NO and CO and the N2 selectivity than the Rh/A-x catalysts. A CeO2 content is responsible for the activity of NO+CO reaction on the Rh/CeO2-ZrO2-La2O3 catalysts. The optimal concentration of Ce is equal to 50at%, where the obtained Rh/B-0.5 catalyst has the best catalytic activity. The enhancement of NO reduction and CO oxidation over Rh/B-x catalysts should be ascribed to the formation of more amounts of surface Ce3+ cations, which are the sites for NO dissociation, thus favoring the NO reduction by removing oxygen.
Keywords:Rh/CeO2-ZrO2-La2O3 oxides  deposition-precipitation  surface properties  NO reduction
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