李靖,王奖,贾美林.Ni-Al复合氧化物/介孔杭锦2#土负载Au催化剂制备及其CO氧化催化性能[J].分子催化,2018,32(6):530-539
Ni-Al复合氧化物/介孔杭锦2#土负载Au催化剂制备及其CO氧化催化性能
Preparation of Ni-Al Mixed Oxide/Mesoporous Hangjin 2# Clay-Supported Gold Catalyst and Their Catalytic Performance for CO Oxidation
投稿时间:2018-07-23  修订日期:2018-09-19
DOI:
中文关键词:  粘土  类水滑石  负载Au催化剂  CO催化氧化  金属-载体强相互作用
英文关键词:clay  layered double hydroxide  supported gold catalyst  CO catalytic oxidation  strong metal-support interaction
基金项目:内蒙古自治区水环境安全协同创新培育中心项目(XTCX003);内蒙古自然科学基金(2015MS0225).
作者单位E-mail
李靖 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022  
王奖 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022 wangjfree@163.com 
贾美林 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022 jml@imnu.edu.cn 
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中文摘要:
      采用导向剂共沉淀-水热法合成不同复合量3Ni-Al类水滑石(LDH)/酸化杭锦2#土载体前驱物.以液相还原-焙烧法制备不同Au负载量的Ni-Al复合氧化物/介孔杭锦2#土负载Au催化剂.采用电感耦合等离子体发射光谱(ICP-AES)、原子吸收光谱(AAS)、N2物理吸附-脱附、X射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)、X射线光电子能谱(XPS)等手段对催化剂进行表征;并考察其催化CO氧化活性及稳定性.结果表明,3Ni-Al LDH在酸化杭锦2#土上复合均匀;其负载Au后经500℃空气气氛焙烧,催化剂具有介孔结构,Au颗粒分散均匀、平均粒径小于10 nm;Ni-Al LDH复合量增加有利于纳米Au分散并抑制其粒径增大,且纳米Au与载体间存在较强相互作用;随Ni-Al LDH复合量和Au负载量增加,负载Au催化剂催化活性提高,当Ni-Al LDH复合量15%(Ni 3.47%),Au负载量3%时,所得负载Au催化剂性能最佳:T50为48℃,80℃时CO转化率大于90%,180℃连续反应10 h,CO转化率保持100%,空气放置110 d后,虽然其低温活性有所下降,但120℃时,仍可实现CO转化率大于90%.
英文摘要:
      A series of x% 3Ni-Al layered double hydroxide (LDH)/acidification Hangjin 2# clay were synthesized by a coprecipitation with directing agent-hydrothermal method. Ni-Al mixed oxide/mesoporous Hangjin 2# clay-supported gold catalysts with different Au loading were prepared by the liquid phase reduction-calcination method. The catalysts were characterized by Inductively Coupled Plasma Atomic Emission Spectrometer (ICP-AES), Atomic Absorption Spectrophotometer (AAS), N2 Physical Adsorption-desorption, X-ray Diffraction (XRD), Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), UV-Vis Diffuse Reflectance Spectroscopy (UV-Vis DRS), and X-ray Photoelectron Spectroscopy (XPS); and their CO oxidation activities and stabilities were investigated. The results show that 3Ni-Al LDH is uniformly mixed on the surface of the acidification Hangjin 2# clay; after calcinations at 500℃ in air atmosphere. The supported Au catalysts are mesoporous and the Au nanoparticles are uniformly dispersed with the average particle size less than 10 nm; the increase of the amount of Ni-Al LDH is beneficial to improve the dispersion of Au nanoparticles and could inhibit the aggregation of the particles due to the strong metal-support interactions between Au nanoparticles and the supports. The increase of Ni-Al LDH amount and the Au loading could improve the catalytic activity of the Au catalysts. The supported Au catalyst with 15% Ni-Al LDH amount (Ni 3.47%) and 3% Au loading gives the best catalytic performance:T50 is 48℃ CO conversion, the CO conversion is more than 90% at 80℃, 100% CO conversion could be maintained for 10 hours at the reaction temperature of 180℃. 90% CO conversion can still be kept at 120℃ after the catalyst was stored in air for 110 days.
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