Three-Dimensional Branched Crystal Carbon Nitride with Enhanced Intrinsic Peroxidase-Like Activity: A Hypersensitive Platform for Colorimetric Detection

Graphitic carbon nitride (g-C3N4) as a metal-free nanozyme has attracted huge attention for catalytic applications. However, the catalytic activity of pure g-C3N4 causes very moderate H2O2 activation. Herein, a novel three-dimensional (3D) branched carbon nitride nanoneedle (3DBC-C3N4) nanozyme has been proposed to overcome such shortcoming. This unique 3D branched structure of 3DBC-C3N4 facilitated effective mass transfer during catalytic reaction and induced a lightning rodlike effect to accelerate electron collection at the tip area for H2O2 activation. With improved H2O2 activation for hydroxyl radical (•OH) generation, 3DBC-C3N4 showed excellent peroxidase-like activity toward 3,3',5,5'-tetramethylbenzidine oxidation in the presence of H2O2. As for H2O2, the Vmax value of 3DBC-C3N4 was found to be 20 times higher than that of natural horseradish peroxidase. Moreover, the 3D branched structure of 3DBC-C3N4 offered large interface for the reversible conjugation of single-stranded DNA, which enhanced the colorimetric sensitivity. Moreover, 3DBC-C3N4 exhibited high sensitivity toward oxytetracycline detection, with the detection limit and quantitative limit of 1 and 50 μg/L, respectively.