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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 mol_{N‐benzylaniline} mol_metal^-1 h^-1; this TOF outpaces that of reported stable non‐noble‐metal‐based catalysts by a factor of 2.