Iron mediated n → π* electron transitions and mid-gap states formation in CN under low-temperature secondary calcination enhances photodegradation of organic pollutants

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-05-01 Epub Date: 2024-10-22 DOI:10.1016/j.seppur.2024.130223
Meng Gao, Xuefeng Hu, Chao Wang, Yuhuan Fei, Zilong Li, Hao Xie, Mina Yang
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Abstract

Iron modified carbon nitride (CN) materials have attracted widespread attention from researchers in different application fields. In this paper, single atom iron anchored CN (FeCN) with mid-gap states and n → π* electron transition was synthesized through low temperature secondary calcination. The mid-gap states introduce surface states capable of trapping photogenerated electrons, enabling FeCN to absorb photons with energies lower than its intrinsic optical bandgap. 10%FeCN also exhibits distinct optical absorption above 490 nm derived from the n → π* electron transition, which expand the visible light response range of photocatalysts and enhance electron transport ability. Additionally, the Fe-Nx site enhances the separation and transmission efficiency of photoexcited charges. The prepared 10%FeCN exhibits extremely high photocatalysis and photo-Fenton activity. Mercaptobenzothiazole (MBT) degradation rate of 10%FeCN is 3.47 times higher than CN, achieving a mineralization rate of 86.7% in 100 min. Additionally, the oxytetracycline hydrochloride (OTC) degradation rate of 10%FeCN in photo-Fenton reaction is 11.9 times higher than CN. After five cycles, this catalyst still has good reactivity, indicating its good stability.
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在低温二次煅烧条件下,铁介导的 n → π* 电子跃迁和 CN 中隙态的形成可促进有机污染物的光降解
铁修饰的氮化碳(CN)材料在不同应用领域引起了研究人员的广泛关注。本文通过低温二次煅烧合成了具有中隙态和 n → π* 电子转变的单原子铁锚氮化碳(FeCN)。中隙态引入了能够捕获光生电子的表面态,使 FeCN 能够吸收能量低于其固有光带隙的光子。10 %FeCN 还表现出高于 490 纳米的明显光吸收,这种吸收来自 n → π* 电子转变,从而扩大了光催化剂的可见光响应范围,并增强了电子传输能力。此外,Fe-Nx 位点还能提高光激发电荷的分离和传输效率。制备的 10 %FeCN 具有极高的光催化和光 Fenton 活性。10 %FeCN 的巯基苯并噻唑(MBT)降解率是 CN 的 3.47 倍,100 分钟内矿化率达到 86.7%。此外,在光-芬顿反应中,10 %FeCN 的盐酸土霉素(OTC)降解率是 CN 的 11.9 倍。经过五个循环后,这种催化剂仍具有良好的反应活性,表明其具有良好的稳定性。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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