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题名: Efficient and Durable Au Alloyed Pd Single-Atom Catalyst for the Ullmann Reaction of Aryl Chlorides in Water
作者: Zhang, Leilei1, 2;  Wang, Aiqin1;  Miller, Jeffrey T.3;  Liu, Xiaoyan1;  Yang, Xiaofeng1;  Wang, Wentao1;  Li, Lin1;  Huang, Yanqiang1;  Mou, Chung-Yuan4;  Zhang, Tao1
关键词: Ullmann reaction ;  aryl chlorides ;  heterogeneous catalyst ;  Au-Pd alloy ;  Pd single-atom
刊名: ACS CATALYSIS
发表日期: 2014-05-01
DOI: 10.1021/cs500071c
卷: 4, 期:5, 页:1546-1553
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
英文摘要: 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.
关键词[WOS]: HETEROGENEOUS PALLADIUM CATALYSTS ;  CROSS-COUPLING REACTION ;  SUZUKI-MIYAURA ;  AQUEOUS-MEDIA ;  CO ADSORPTION ;  NANOPARTICLES ;  GOLD ;  CARBON ;  TEMPERATURE ;  ACTIVATION
语种: 英语
WOS记录号: WOS:000335491200035
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/145828
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Argonne Natl Lab, CSE, Argonne, IL 60439 USA
4.Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan

Recommended Citation:
Zhang, Leilei,Wang, Aiqin,Miller, Jeffrey T.,et al. Efficient and Durable Au Alloyed Pd Single-Atom Catalyst for the Ullmann Reaction of Aryl Chlorides in Water[J]. ACS CATALYSIS,2014,4(5):1546-1553.
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