4.8 Article

A copper-phyllosilicate core-sheath nanoreactor for carbon-oxygen hydrogenolysis reactions

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NATURE COMMUNICATIONS
卷 4, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms3339

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资金

  1. National Natural Science Foundation of China [21276186, 21222604]
  2. National High Technology Research and Development Program of China [2011AA051002]
  3. Program for New Century Excellent Talents in University [NCET-10-0611]
  4. Specialized Research Fund for the Doctoral Program of Higher Education [20120032110024]
  5. Program of Introducing Talents of Discipline to Universities [B06006]

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Hydrogenolysis of carbon-oxygen bonds is a versatile synthetic tool in organic synthesis. Copper-based catalysts have been intensively explored as the copper sites account for the highly selective hydrogenation of carbon-oxygen bonds. However, the inherent drawback of conventional copper-based catalysts is the deactivation by metal-particle growth and unstable surface Cu-0 and Cu+ active species in the strongly reducing hydrogen and oxidizing carbon-oxygen atmosphere. Here we report the superior reactivity of a core (copper)-sheath (copper phyllosilicate) nanoreactor for carbon-oxygen hydrogenolysis of dimethyl oxalate with high efficiency (an ethanol yield of 91%) and steady performance (4300 h at 553 K). This nanoreactor, which possesses balanced and stable Cu-0 and Cu+ active species, confinement effects, an intrinsically high surface area of Cu-0 and Cu+ and a unique tunable tubular morphology, has potential applications in high-temperature hydrogenation reactions.

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