耐高温纳米金催化剂的制备及其高温催化
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摘要
经过近三十多年的蓬勃发展,纳米金催化剂逐渐呈现出区别于其他贵金属纳米催化剂特征:显著的金纳米粒子尺寸效应和载体效应以及极差的热稳定性。小尺寸金纳米粒子的高催化活性和易烧结失活特性令人爱恨交加。大量的工作致力于解决纳米金催化剂的这一典型矛盾,但少有突破,纳米金催化剂应用仍局限于少数低温催化反应中。制备耐高温小尺寸金纳米粒子并探究其在高温催化反应中的性能仍然是一个巨大的挑战。本报告将汇报我们在稳定小尺寸金纳米粒子并将其应用于高温催化反应方面的进展。根据我们在稳定铂族金属纳米粒子方面发展的构筑晶格结构匹配的金属-氧化物外延界面结构原则,利用镓酸镁尖晶石负载金纳米粒子,在经过800oC在空气气氛中焙烧28天后,金纳米粒子尺寸仍保持在2-4 nm。以这一稳定催化剂为基础,添加不同性质的氧化物拓展制备了不同氧化物促进的纳米金催化剂,并考察了其在典型高温反应,如甲烷催化燃烧,高温水汽迁移等反应中的催化性能。结果表明,镓酸镁尖晶石稳定的金纳米粒子的活性仍保持对载体性质的依赖性,氧化还原性氧化物的修饰能使其在高温催化反应中具有良好的催化性能。
Heterogeneous gold catalysis has prospered in recent 30 years and comprehensive knowledge on its characteristics has been achieved. Much stronger Au size and support sensitivity and specificity and much poorer thermal stability than the platinum group metal catalysts constitute the trademark of current gold catalysts. It is greatly desired to improve the thermal stability of gold catalysts for taking the advantages of their preeminent catalytic properties. In this report we demonstrate our advantages in stabilizing Au nanoparticles and their use in high-temperature reactions. Magnesium gallate support Au nanoparticles can retain sizes in the range of 2-4 nm after severe aging at 800 ℃ in air for 28 days. With oxides having good redox property as promoters, the magnesium gallate support Au nano-catalysts show excellent catalytic activity for combustion of methane and water-gas shift reactions. These results open up many possibilities for the applications of gold nano-catalysts at elevated temperatures.
引文
[1]Li,W.-Z.;Kovarik,L.;Mei,D.;Liu,J.;Wang,Y.;Peden,C.H.F.Nat.Commun.2013,135:2481.
    [2]Li,W.-Z.;Kovarik,L.;Mei,D.;Engelhard,M.H.;Gao,F.;Liu,J.;Wang,Y.;Peden,C.H.F.Chem.Mater.2014,24:5475.

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