Modulating the precursors of carbon nitride to boost local electron delocalization for H2O2 photosynthesis to remove oxytetracycline and its antibiotic resistant genes

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2024.123690

Zhi Li , Hao Lv , Kangbo Tong , Yupeng He , Chunyang Zhai , Yang Yun , Mingshan Zhu

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Abstract

Artificial H₂O₂ photosynthesis, one of the brightest strategies toward H₂O₂ production, is always restricted by the intrinsically charge migration behaviors and redox kinetics of photocatalysts. Herein, different precursors of carbon nitride (C₃N₄) with urea and melamine (Mel) are synthesized, where C₃N₄-Urea has more delocalized electrons due to its smaller size and thickness, compared with C₃N₄-Mel. Under simulated sunlight irradiation, these abundant delocalized electrons rapid reduce oxygen into H₂O₂, with the rate of 4.9 mmol g⁻¹ h⁻¹ and 2e^- transfer selectivity of 98%. In addition, a self-photo-Fenton reaction system is constructed to remove oxytetracycline (OTC) pollutants and its antibiotic resistant genes (ARG) in water, with the degradation rate of 3.75 min⁻¹ for OTC and 0.08 min⁻¹ for tetC ARG. The current approach by modulating the precursors of C₃N₄ to boost the local electron delocalization offers a promising route for improving the efficiency of artificial H₂O₂ photosynthesis.

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调节氮化碳的前体，促进 H2O2 光合作用的局部电子脱定位，以清除土霉素及其抗生素耐药基因

人工 H2O2 光合作用是产生 H2O2 的最有效策略之一，但始终受到光催化剂内在电荷迁移行为和氧化还原动力学的限制。在这里，我们合成了含有尿素和三聚氰胺（Mel）的不同氮化碳（C3N4）前体，与 C3N4-Mel 相比，C3N4-尿素的尺寸和厚度更小，因此具有更多的脱局域电子。在模拟太阳光照射下，这些丰富的局域电子能迅速将氧气还原成 H2O2，还原速率为 4.9 mmol g-1 h-1，2e-转移选择性为 98%。此外，还构建了一个自光化芬顿反应系统，用于去除水中的土霉素（OTC）污染物及其抗生素耐药基因（ARG），其对 OTC 的降解速率为 3.75 min-1，对 tetC ARG 的降解速率为 0.08 min-1。目前通过调节 C3N4 的前体促进局部电子脱定位的方法为提高人工 H2O2 光合作用的效率提供了一条可行的途径。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.