Boron-Doped and Ketonic Carbonyl Group-Enriched Graphdiyne as a Dual-Site Carbon Nanozyme with Enhanced Peroxidase-Like Activity.

Abstract

We demonstrate the preparation of a dual-site carbon nanozyme, boron-doped and ketonic carbonyl (-C=O) group-enriched graphdiyne (B-GDY), with an enhanced peroxidase-like activity. Taking advantage of acidic oxidation treatment, GDY oxide (GDYO) with abundant surface oxygen-containing groups is obtained from pristine bulk GDY. Upon further thermal annealing of GDYO with H3BO3 under an inert atmosphere, B is introduced into GDY, while the loading of -C=O groups is increased onto B-GDY. We discover that boron-doped and ketonic carbonyl group-enriched graphdiyne as a dual-site carbon nanozyme endows it with an enhanced peroxidase-like activity, which is nearly 4.2-fold higher than that of GDY without B atoms and 6.6-fold higher than that of GDYO without B atoms and with low loading of -C=O groups. The high peroxidase-like activity of B-GDY is ascribed to the dual active sites (-C=O group and B atom) within it, which facilitates the adsorption and decomposition of H2O2 into hydroxyl radicals revealed by experimental and theoretical studies. Moreover, B-GDY is successfully employed to develop a colorimetric method for the detection of glucose with good sensitivity and selectivity. This work probes into the intrinsic peroxidase activity and structure-reactivity correlation, creating effective strategies for the preparation of GDY-based nanozymes.