Nonradicals-dominated peroxymonosulfate activation of g-C3N4/CeO2 floating beads for enhanced inactivation of M. aeruginosa: Performance studies and mechanistic insights

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL Chemical Engineering Journal Pub Date : 2025-02-20 DOI:10.1016/j.cej.2025.160703
Dandan Wang, Jing Li, Rong Zhang, Beiyu Xin, Xueru Huang, Yang Wang, Jifeng Guo
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Abstract

Microcystis aeruginosa (M. aeruginosa) is a typical harmful algal associated with eutrophication, making the study of its inactivation critical for water restoration. In this research, g-C3N4/CeO2 composites with S-scheme heterojunctions were synthesized and incorporated into sodium alginate (SA) to successfully prepare photocatalytic gel beads with floating capabilities. A photocatalytic persulfate (g-C3N4/CeO2/SA/Vis/PMS) system was developed to systematically investigate the algal inactivation efficacy of floating catalysts. The g-C3N4/CeO2 S-scheme heterojunctions significantly enhanced algal inactivation efficiency, achieving up to 96.65 % inactivation within 80 min. The alterations in algal cell properties during the inactivation process were examined. A decrease in the content of algal bile proteins indicated a disruption of the photosynthetic system within the algal cells, while an increase in the concentrations of K+, Ca2+, and Mg2+ suggested further disruption of algal cell membranes and walls. Additionally, three-dimensional fluorescence spectroscopy (EEM) results indicated that the extracellular organic matter produced during the rupture of algal cells was degraded into humic acid-like substances. The energy bands and electronic structure of g-C3N4/CeO2 were calculated using density functional theory (DFT) to analyze the electron transfer mechanism involved in this process, which is consistent with the S-scheme electron transfer pathway. The effective inactivation of M. aeruginosa was successfully achieved through the combined action of the non-radical 1O2,·O2, and h+ generated during the photogenerated carrier transfer process. This approach offers a promising strategy for the management of algal blooms in eutrophic waters.

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非自由基主导的过氧单硫酸盐活化g-C3N4/CeO2浮珠增强铜绿假单胞菌的失活:性能研究和机制见解
铜绿微囊藻(Microcystis aeruginosa, M. aeruginosa)是一种典型的与富营养化有关的有害藻类,研究其失活对水体恢复至关重要。本研究合成了具有s型异质结的g-C3N4/CeO2复合材料,并将其加入到海藻酸钠(SA)中,成功制备了具有漂浮能力的光催化凝胶珠。建立了光催化过硫酸盐(g-C3N4/CeO2/SA/Vis/PMS)体系,系统考察了浮式催化剂的灭藻效果。g-C3N4/CeO2 S-scheme异质结显著提高了藻类的失活效率,在80 min内实现了96.65 %的失活。研究了在失活过程中藻细胞性质的变化。藻类胆蛋白含量的下降表明藻类细胞内光合系统的破坏,而K+、Ca2+和Mg2+浓度的增加表明藻类细胞膜和细胞壁的进一步破坏。此外,三维荧光光谱(EEM)结果表明,藻细胞破裂过程中产生的胞外有机物被降解为腐植酸样物质。利用密度泛函理论(DFT)计算了g-C3N4/CeO2的能带和电子结构,分析了这一过程的电子转移机理,与s型电子转移途径一致。通过光生载体转移过程中产生的非自由基1O2、·O2 -和h+的共同作用,成功地实现了M. aeruginosa的有效失活。这种方法为富营养化水域的藻华管理提供了一种有前途的策略。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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