Efficient and durable Au alloyed Pd single-atom catalyst for the Ullmann reaction of aryl chlorides in water

Leilei Zhang, Aiqin Wang, Jeffrey T. Miller, Xiaoyan Liu, Xiaofeng Yang, Wentao Wang, Lin Li, Yanqiang Huang, Chung Yuan Mou, Tao Zhang

Research output: Contribution to journalArticlepeer-review

182 Citations (Scopus)

Abstract

Ion exchange resin supported Au alloyed Pd single atoms have been explored to serve as an effective and robust catalyst for the Ullmann reaction of aryl halides under mild conditions in aqueous media, in particular for the activation of less reactive aryl chlorides. The catalysts were prepared with an ion exchange-NaBH4 reduction method and submitted to extensive characterizations by HRTEM, XRD, EXAFS, and DRIFTS techniques. XRD patterns demonstrated the formation of Au-Pd alloys. EXAFS and DRIFTS characterization results showed that with an increase of Au/Pd molar ratios, the continuous Pd ensembles on the surface were gradually separated and eventually isolated by Au atoms, confirming that the Au alloyed Pd single-atom catalyst was formed. The catalysts exhibited excellent performance for the Ullmann reaction of aryl chlorides, and the turnover number (TON) increased exponentially with a decrease of the amount of Pd in the catalysts. On the basis of these characterization and catalytic results, the Au alloyed Pd single-atom was proposed as the active site for the reaction. The catalyst exhibited excellent catalytic performance for a broad scope of substrates and could be reused at least 8 times with no change in yield. This Au alloyed Pd single-atom catalyst bridges the gap between homogeneous and heterogeneous catalysis in organic transformations and may open a new vision to develop other efficient single-atom catalysts for green synthesis of fine chemicals.

Original languageEnglish
Pages (from-to)1546-1553
Number of pages8
JournalACS Catalysis
Volume4
Issue number5
DOIs
Publication statusPublished - May 2 2014
Externally publishedYes

Keywords

  • aryl chlorides
  • Au-Pd alloy
  • heterogeneous catalyst
  • Pd single-atom
  • Ullmann reaction

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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