3D g-C3N4/WS2/Agarose Aerogel Photocatalyst for Near-Complete Degradation of Broad-Spectrum Antibiotics in Batch and Continuous Flow Modes

IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL ACS ES&T engineering Pub Date : 2024-10-29 DOI:10.1021/acsestengg.4c00579
Mario Vino Lincy Gnanaguru, Debanjali Dey, Makarand M. Ghangrekar, Ramkrishna Sen and Shamik Chowdhury*, 
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Abstract

Heterojunction-based photocatalysts are receiving tremendous scientific attention for eliminating consumer-derived micropollutants from aqueous environments. However, the inherent difficulty in recovering photocatalysts following treatment, due to their application in powder form, precludes their widespread use. Herein, a self-supporting and lightweight three-dimensional (3D) graphitic carbon nitride (g-C3N4)/tungsten disulfide (WS2)/agarose aerogel (GCWAA) was constructed via a facile and scalable radial freeze-casting approach. The as-synthesized 3D GCWAA proved extremely promising for the photocatalytic removal of three broad-spectrum antibiotic pollutants (ABPs), viz., tetracycline (94%), sulfamethoxazole (97%), and ofloxacin (96%), within 90 min of visible light irradiation in the batch regime. The enhanced photocatalytic performance of 3D GCWAA can be attributed to a Z-scheme electron flow from g-C3N4 to WS2 in the aerogel, as inferred from electronic band structure characterization. To further demonstrate the practical utility of the composite aerogel in water and wastewater treatment systems, the continuous flow photocatalysis of ABPs over 3D GCWAA was systematically studied. Specifically, the influence of several noteworthy operational parameters, such as flow rate, solution pH, and the presence of interfering ions was comprehensively investigated. Interestingly, under optimized conditions, GCWAA achieved a remarkable average removal efficiency of 95% for ABPs in continuous mode, with minimal loss of activity over time. More attractively, GCWAA exhibited decent photocatalytic performance for treating a ternary mixture of ABPs in both freshwaters and wastewaters in the continuous flow reactor. The results of this study showcase the ultimate lab-scale demonstration of the photocatalytic potential of 3D GCWAA for the degradation of emerging contaminants, paving the way for future scale-up.

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3D g-C3N4/WS2/琼脂糖气凝胶光催化剂在间歇和连续流动模式下近乎完全降解广谱抗生素
基于异质结的光催化剂在消除水中环境中消费者来源的微污染物方面受到了极大的科学关注。然而,由于光催化剂以粉末形式应用,在处理后回收光催化剂的固有困难阻碍了它们的广泛应用。本文通过一种简单、可扩展的径向冷冻铸造方法,构建了一种自支撑、轻质的三维(3D)石墨氮化碳(g-C3N4)/二硫化钨(WS2)/琼脂糖气凝胶(GCWAA)。合成的3D GCWAA被证明在可见光照射90分钟内具有光催化去除三种广谱抗生素污染物(ABPs)的潜力,即四环素(94%),磺胺甲新唑(97%)和氧氟沙星(96%)。三维GCWAA光催化性能的增强可归因于气凝胶中g-C3N4向WS2的z型电子流,这是由电子能带结构表征得出的。为了进一步证明复合气凝胶在水和废水处理系统中的实际应用,系统地研究了ABPs在3D GCWAA上的连续流光催化作用。具体来说,几个值得注意的操作参数,如流速、溶液pH和干扰离子的存在的影响进行了全面的研究。有趣的是,在优化的条件下,GCWAA在连续模式下对ABPs的平均去除效率达到了95%,并且随着时间的推移活性损失最小。更吸引人的是,在连续流反应器中,GCWAA对淡水和废水中的三元ABPs混合物均表现出良好的光催化性能。这项研究的结果展示了3D GCWAA在降解新出现的污染物方面的光催化潜力的最终实验室规模演示,为未来的扩大铺平了道路。
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来源期刊
ACS ES&T engineering
ACS ES&T engineering ENGINEERING, ENVIRONMENTAL-
CiteScore
8.50
自引率
0.00%
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0
期刊介绍: ACS ES&T Engineering publishes impactful research and review articles across all realms of environmental technology and engineering, employing a rigorous peer-review process. As a specialized journal, it aims to provide an international platform for research and innovation, inviting contributions on materials technologies, processes, data analytics, and engineering systems that can effectively manage, protect, and remediate air, water, and soil quality, as well as treat wastes and recover resources. The journal encourages research that supports informed decision-making within complex engineered systems and is grounded in mechanistic science and analytics, describing intricate environmental engineering systems. It considers papers presenting novel advancements, spanning from laboratory discovery to field-based application. However, case or demonstration studies lacking significant scientific advancements and technological innovations are not within its scope. Contributions containing experimental and/or theoretical methods, rooted in engineering principles and integrated with knowledge from other disciplines, are welcomed.
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