LAUSR

Metal‐free carbocatalysis has been widely utilized for aerobic oxidative reactions. Here, we report that oxygen‐rich carbon quantum dots (O‐CQDs) demonstrate a catalytic performance superior to graphene oxide, if used as a metal‐free nanocatalyst for the direct transformation of amines and alcohols, under mild and solvent‐free conditions. O‐CQDs show a yield of 75 % for the oxidative coupling of amine to imine (with 5 wt % catalyst loading) and a conversion of 3.8 % for benzyl alcohol (with 2 wt % catalyst loading). The catalytic activities of thermally treated O‐CQDs are further improved for benzylamine, for example, indicated by a yield of up to 98 % with 4 wt % catalyst loading. In addition, O‐CQDs show a photoenhanced catalytic ability of amine (98 % yield with 5 wt % catalyst loading for 6 h reaction). Characterizations and simulations show that numerous carboxyl oxygen functional groups and unpaired electrons at the edge sites of O‐CQDs are likely involved in the aerobic oxidation of amines.