Interlayer single-atomic Fe−N4 sites on carbon-rich graphitic carbon nitride for notably enhanced photo-Fenton-like catalytic oxidation processes towards recalcitrant organic micropollutants

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2024.123695

Lang Qin, Jiaqi Meng, Guang Yang, Yue Pan, Xinchun Gao, Yuxin Yang, Yihang Guo

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Abstract

Glucose-assisted supramolecule self-assembly of melamine and cyanuric acid in the presence of Fe(NO₃)₃ combined with thermal polymerization is designed to fabricate C-rich g-C₃N₄-embedded interlayer single-atomic Fe−N₄ sites catalyst (Fe₁/C-CN). Fe₁/C-CN exhibits outstanding photo-Fenton-like catalytic oxidation activity towards typical recalcitrant organic micropollutants. For example, the pseudo-first-order kinetic constant of Fe₁/C-CN photo-Fenton-like system is 7.5 and 21.1 times higher than Fe₁/C-CN photocatalysis and Fenton-like systems in degradation of p-nitrophenol, and TOC removal efficiency reaches up to 100% after reaction proceeds for 4 h. Mechanism studies reveal that synergy of maximum Fe atom utilization efficiency and boosted photoexcited charge separation dynamics accelerates regeneration of ≡Fe(II) and efficient H₂O₂ activation of Fe₁/C-CN, leading to plentiful active oxygen species for deep oxidation of organic micropollutants. Fe₁/C-CN also shows a robust reusability in long-term remediation of organic micropollutants, attributing to interlayer Fe−N coordination interactions for preventing single Fe atoms from agglomeration and leaching to reaction media.

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富碳氮化石墨上的层间单原子 Fe-N4 位点可显著增强对难降解有机微污染物的光-芬顿催化氧化过程

在 Fe(NO3)3 存在下，通过葡萄糖辅助三聚氰胺和三聚氰酸的超分子自组装，并结合热聚合反应，设计出了富含 C 的 g-C3N4 嵌入层间单原子 Fe-N4 位点催化剂（Fe1/C-CN）。Fe1/C-CN 对典型的难降解有机微污染物具有出色的光-芬顿催化氧化活性。例如，在降解对硝基苯酚时，Fe1/C-CN 光-Fenton 类体系的假一阶动力学常数分别是 Fe1/C-CN 光催化和 Fenton 类体系的 7.5 倍和 21.1 倍，反应进行 4 小时后 TOC 去除率高达 100%。机理研究表明，最大的铁原子利用效率和光激发电荷分离动力学的协同作用加速了 Fe1/C-CN 的铁(II)再生和 H2O2 的高效活化，从而产生了大量的活性氧，用于有机微污染物的深度氧化。此外，Fe1/C-CN 在长期修复有机微污染物方面还显示出强大的可再利用性，这归功于层间 Fe-N 配位相互作用，可防止单个铁原子团聚和沥滤到反应介质中。

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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.