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Grouping effect of single Ni-N4 sites in N-doped carbon boosts hydrogen transfer coupling of alcohols and amines

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Antonietti,  Markus
Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society;

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Citation

Su, H., Gao, P., Wang, M.-Y., Zhai, G.-Y., Zhang, J.-J., Zhao, T.-J., et al. (2018). Grouping effect of single Ni-N4 sites in N-doped carbon boosts hydrogen transfer coupling of alcohols and amines. Angewandte Chemie International Edition, 57(46), 15194-15198. doi:10.1002/anie.201809858.


Cite as: http://hdl.handle.net/21.11116/0000-0002-542E-D
Abstract
As a new type of heterogeneous catalyst with “homogeneous‐like” activity, single‐site transition‐metal materials are usually treated as integrated but separate active centers. A novel grouping effect is reported for single Ni−N4 sites in nitrogen‐doped carbon (Ni/NC), where an effective ligand‐stabilized polycondensation method endows Ni/NC nanocatalysts with a high content of single‐site Ni up to 9.5 wt %. The enhanced electron density at each single Ni−N4site promotes a highly efficient hydrogen transfer, which is exemplified by the coupling of benzyl alcohol and aniline into N‐benzylaniline with a turnover frequency (TOF) value of 7.0 molN‐benzylaniline molmetal-1 h-1; this TOF outpaces that of reported stable non‐noble‐metal‐based catalysts by a factor of 2.