Continuous visible-light photodegradation of emerging pollutants via in-situ cascade Fenton catalysis through dual active sites catalyst

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2025-07-30 Epub Date: 2025-01-29 DOI:10.1016/j.seppur.2025.131859
Yu Jiang , Zeyang Sun , Si Wang , Chaoyu Li , Zihang Wang , Cheng Qian , Rui Wang , Ye Tan , Xuchao Sun , Shou-Dao Li , Feiyan Tang , Qiong Liu
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Abstract

The photocatalytic treatment of emerging pollutants has garnered increasing attention by using continuous photodegradation system; however, limitations such as insufficient reactant adsorption and the lack of strong oxidative sites hinder its broader application. In this study, dual active sites functionalized polymeric carbon nitride (PCN) nanorods were synthesized through co-modified with loading of Fe and potassium. The resulting dual-site PCN catalyst exhibited significantly enhanced photocatalytic performance in the degradation of emerging pollutants, including bisphenol A, acetaminophen, carbamazepine, and oxytetracycline, under visible-light irradiation. The introduction of alkali metals as Lewis acid sites efficiently promoted oxygen adsorption and facilitated the generation of reactive H2O2. Simultaneously, the incorporation of Fe species enabled cascade catalysis with H2O2, forming reactive oxygen radicals via an in situ photo-Fenton system. The degradation pathway of bisphenol A involved C–C bond cleavage, hydroxylation, esterification, and ring-opening processes, while acetaminophen degradation occurred primarily through acetyl-amino group attack. To demonstrate its scalability, a fixed-bed reactor was constructed. It achieved continuous degradation of bisphenol A and acetaminophen with high removal efficiency and stable performance over five days. This long-term continuous photodegradation system, enabled by the dual-functionalized PCN, highlights its significant potential for solar-driven, large-scale wastewater treatment.

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双活性位点催化原位级联Fenton催化连续可见光降解新污染物
利用连续光降解系统对新兴污染物进行光催化处理已受到越来越多的关注;然而,诸如反应物吸附不足和缺乏强氧化位点等限制阻碍了其广泛应用。在本研究中,通过负载铁和钾的共改性,合成了双活性位点功能化的聚合氮化碳纳米棒。所制得的双位点PCN催化剂在可见光照射下对双酚A、对乙酰氨基酚、卡马西平和土霉素等新兴污染物的降解表现出显著增强的光催化性能。碱金属作为Lewis酸位点的引入有效地促进了氧的吸附,促进了活性H2O2的生成。同时,Fe的加入使得与H2O2的级联催化作用得以实现,通过原位光- fenton系统形成活性氧自由基。双酚A的降解途径包括C-C键裂解、羟基化、酯化和开环过程,而对乙酰氨基酚的降解主要通过乙酰氨基攻击进行。为了证明其可扩展性,建造了一个固定床反应器。连续降解双酚A和对乙酰氨基酚5天,去除率高,性能稳定。这种长期连续的光降解系统,由双功能化PCN实现,突出了其在太阳能驱动的大规模废水处理方面的巨大潜力。
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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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