Potassium and phosphorus co-doped g-C3N4 with improved carrier migration for efficient photocatalytic degradation of 2,4-dichlorophenoxyacetic acid under visible light

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES
Shan Liu , Simin Long , Yi Zhao , Zhonglin Chen , Jimin Shen , Gang Fu , Jiaxu Zhang , Jing Kang
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Abstract

The carrier migration efficiency of photocatalysts is important for the performance of photocatalysis. Hence, element doping was employed to improve the photogenerated carrier separation efficiency of carbon nitride in the graphite phase (CN). Melamine was calcined in order to create potassium (K) and phosphorus (P) co-doped CN (K+PCN) by adding ammonium dihydrogen phosphate and potassium hydroxide. The varying K doping amounts are denoted as 1-K+PCN, 2-K+PCN, and 3-K+PCN, respectively. Under visible light, 2-K + PCN possessed a 12 times faster degradation rate than CN for the photodegradation of 2,4-Dichlorophenoxyacetic acid, as well as good photodegradation performance in actual water. The combination of density functional theory calculations and spectroscopic characterization techniques has demonstrated that K and P doping can facilitate the transfer of electrons to the carbon-nitrogen aromatic heterocyclic framework. This process modulates the electronic band structure, leading to a reduction in the band gap. Consequently, there is a synergistic enhancement of carrier separation from two-dimensional to three-dimensional systems. Specifically, K+ ions facilitated the formation of an interfacial charge-transfer pathway within the CN matrix, while P atoms introduced electron-trapping sites that preferentially captured photogenerated electrons, thereby spatially isolating holes and electrons. Additionally, the co-doping approach greatly increased the modified CN surface's ability to adsorb dissolved oxygen, which encouraged the production of superoxide radicals. These radicals were identified as the predominant reactive species responsible for the oxidation of 2,4-dichlorophenoxyacetic acid. Valuable theoretical insights for the logical design of dual-element-doped CN materials to address challenges in environmental remediation and sustainable pollutant degradation are provided by this study.
钾磷共掺杂g-C3N4改善载流子迁移的光催化降解2,4-二氯苯氧乙酸
光催化剂的载流子迁移效率是影响光催化性能的重要因素。因此,采用元素掺杂的方法来提高氮化碳在石墨相(CN)中光生载流子的分离效率。以磷酸二氢铵和氢氧化钾为原料,对三聚氰胺进行煅烧制备钾、磷共掺CN (K+PCN)。不同K掺杂量分别记为1-K+PCN、2-K+PCN和3-K+PCN。在可见光下,2- k +PCN光降解2,4-二氯苯氧乙酸的速度比CN快12倍,在实际水中也有良好的光降解性能。密度泛函理论计算和光谱表征技术的结合表明,K和P掺杂可以促进电子向碳氮芳杂环框架的转移。这一过程调节了电子能带结构,导致带隙减小。因此,从二维到三维系统的载流子分离有协同增强作用。具体来说,K+离子促进了CN矩阵内界面电荷转移途径的形成,而P原子引入了电子捕获位点,优先捕获光生电子,从而在空间上隔离空穴和电子。此外,共掺杂方法大大提高了改性CN表面对溶解氧的吸附能力,从而促进了超氧自由基的产生。这些自由基被认为是2,4-二氯苯氧乙酸氧化的主要反应物质。本研究为双元素掺杂CN材料的逻辑设计提供了有价值的理论见解,以应对环境修复和可持续污染物降解的挑战。
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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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