催化学报 ›› 2016, Vol. 37 ›› Issue (10): 1694-1701.DOI: 10.1016/S1872-2067(16)62508-1

• 论文 • 上一篇    下一篇

沉积-沉淀法和沉积-还原法制备Nb2O5负载的金纳米粒子及其催化CO氧化活性

Toru Murayama, Masatake Haruta   

  1. 首都大学东京金化学研究中心, 东京192-0397, 日本
  • 收稿日期:2016-05-19 修回日期:2016-06-30 出版日期:2016-10-21 发布日期:2016-10-22
  • 通讯作者: Toru Murayama

Preparation of gold nanoparticles supported on Nb2O5 by deposition precipitation and deposition reduction methods and their catalytic activity for CO oxidation

Toru Murayama, Masatake Haruta   

  1. Research Center for Gold Chemistry, Tokyo Metropolitan University, F203-1-1 Minami-osawa, Hachioji, Tokyo 192-0397, Japan
  • Received:2016-05-19 Revised:2016-06-30 Online:2016-10-21 Published:2016-10-22
  • Contact: Toru Murayama

摘要:

采用不同的沉积法制备了氧化铌(Nb2O5)负载的金纳米粒子催化剂,即沉积-沉淀(DP)法、尿素辅助的DP法、沉积-还原(DR)法和一步法制备了1 wt% Au/Nb2O5催化剂.在众多类型Nb2O5(包括商业Nb2O5)中,采用水热法制备的层间型Nb2O5(Nb2O5(HT))最适合用作载体.结果表明,较大比表面积的Nb2O5(HT)使得金以纳米颗粒形式分散于其上.在优化的条件下,以DP和DR法沉积于Nb2O5(HT)上的金纳米粒子平均粒径为5 nm.采用DR法制备的Au/Nb2O5(HT)催化剂上CO转化率为50%时的温度为73℃.不沉积金的条件下,即使在250℃,Nb2O5(HT)对CO氧化反应也没有催化活性.因此,金的沉积对活性的促进作用非常明显.该简易Au/Nb2O5催化剂将金催化剂的类型扩展到酸性载体,这将增加新的应用.

关键词: 金纳米粒子, 氧化铌, 固体酸, CO氧化, 多相催化剂

Abstract:

Nanoparticulate gold catalysts supported on niobium oxides (Nb2O5) were prepared by different deposition methods. The deposition precipitation (DP) method, DP method with urea, deposition reduction (DR) method and one-pot method were used to prepare a 1 wt% Au/Nb2O5 catalyst. Layered-type Nb2O5 synthesized by a hydrothermal method (Nb2O5(HT)) was the most suitable as a support among various types of Nb2O5 including commercially available Nb2O5 samples. It appeared that the large BET surface area of Nb2O5(HT) enabled the dispersion of gold as nanoparticles (NPs). Gold NPs with a mean diameter of about 5 nm were deposited by both the DP method and DR method on Nb2O5(HT) under an optimized condition. The temperature for 50% CO conversion for Au/Nb2O5(HT) prepared by the DR method was 73℃. Without deposition of gold, Nb2O5(HT) showed no catalytic activity for CO oxidation even at 250℃. Therefore, the enhancement of the activity by deposition of gold was remarkable. This simple Au/Nb2O5 catalyst will expand the types of gold catalysts to acidic supports, giving rise to new applications.

Key words: Gold nanoparticulate, Niobium oxide, Solid acid, CO oxidation, Heterogeneous catalyst