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Core-shell or Dimer Heterostructures? Synergistic Catalysis of Advanced Oxidation Process at the Exposed Interface under Illumination.

Carbonaceous materials are biocompatible and eco-friend catalysts for advanced oxidation process (AOP) in the treatment of wastewater, but their activity is not satisfactory compared to the conventional metal and oxide catalyst. Here, dimer heterostructures of ZnO and Ni, N co-doped carbon (NiNC) are found to possess greatly improved activity in a photo assisted AOP reaction. In the synthesis of the composite of ZnO and ZIF-8, the adding sequence of Ni(NO3)2 and 2-methylimidazole can guide the formation of ZnO@NiZIF and ZnO-NiZIF particles, which are further converted to core-shell particle of ZnO and NiNC (ZnO@NiNC) and dimer particle of ZnO and NiNC (ZnO-NiNC) by calcination in N2. Although these two particles have many similar physicochemical properties, the ZnO-NiNC dimer particles show greatly enhanced activity for degradation of RhB under UV-Vis illumination, where its reaction constant is 43 times as its own in dark and 13 times higher than that of ZnO@NiNC under the same condition. A group of experiments reveal a synergistic mechanism for ZnO-NiNC catalyst under illumination, in which the photo electrons directionally migrate towards the exposed ZnO/NiNC interface and react with potassium peroxymonosulfate (PMS) to produce more reactive hydroxyl and persulfate radicals to accelerate the AOP reaction.