Singlet oxygen species induced by colloidal crystalline carbon nitride induced for efficient H2O2 synthesis with in situ antibacterial effect

Abstract

Solar-driven hydrogen (H2) and hydrogen peroxide (H2O2) generation over visible-light responsive carbon nitride (CN) photocatalysts for in situ efficient sterilization is a promising and eco-friendly strategy. Herein, a colloidal potassium-ion (K+) intercalated crystalline CN nanosheets (KCCN) photocatalyst was constructed for boosting synergetic H2O2 synthesis with isopropanol (IPA) oxidation and in situ antibacterial effect. The surface hydroxyl (−OH) and cyano (−CN) groups induced by molten salt (KCl)-assisted thermal treatments contributed to the colloidal nature of CN, facilitating for high wettability of KCCN in aqueous solution to gain active hydrogen (H+) from water sustainably. Meaningfully, the enhanced high-energy singlet oxygen species (1O2) produced by KCNN-2 were verified by electron paramagnetic resonance (EPR) and 9,10-anthracenediyl-bis(methylene)-dimalonic acid (ABDA)-fluorescent probe, significantly contributing to H2O2 production and antibacterial effect. Consequently, the optimal KCCN-2 exhibited a much enhanced H2 generation of 4.11 mmol g−1 h−1, and H2O2 production activity of 1.82 mmol L−1 h−1 with acetone yield rate of 47.3 mmol g−1 h−1 under visible-light (λ > 420 nm) irradiation in 10 vol% IPA solution. The in-situ generated H2O2 can be activated to produce reactive oxygen species (ROS), especially 1O2, to effectively kill the Escherichia coli, reaching an improved an antibacterial rate of 89.7% under stimulated sunlight irradiation in 1 h. This work could offer a new insight into the photoinduced ROS for aqueous H2O2 photosynthesis and antibacterial application.