Interface dependent electron shunting in graphene-integrated intimately coupled photocatalytic biodegradation

IF 12.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2024-12-28 DOI:10.1016/j.watres.2024.123064

Ajinkya Kishor Ranade , Akira Yamaguchi , Masahiro Miyauchi , Sreenivasan Ramaswami , Chihiro Yoshimura

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Abstract

Intimately coupled photocatalytic biodegradation (ICPB) has been recently developed as an efficient wastewater treatment technique, particularly for removing persistent organic pollutants. However, photocatalyst/biofilm interaction in terms of photoelectron transfer and its effect on the overall performance of ICPB has not been explored. To investigate these points, interface-engineered composites of bismuth vanadate and reduced graphene oxide with low degree (BiVO₄/rGO-LC) and high degree of their contact (BiVO₄/rGO-HC) were fabricated and applied for ICPB. As a result, the composites displayed interface-dependent optical, structural and charge carrier separation properties. The photoelectrochemical measurements confirmed the presence of photoelectron shunting between photocatalyst and biofilm, while the current density was higher (smaller Nyquist arc) for BiVO₄/rGO-HC than BiVO₄/rGO-LC and BiVO₄ in ICPB protocol, confirming the crucial role of intimate interfacial contact for photoelectron shunting from BiVO₄ to biofilm. Consequently, the presence of graphene and its interfacial quality dictated the photoelectron shunting between photocatalyst and biofilm, enhancing photoelectron-holes separation and achieving superior degradation rate of tetracycline hydrochloride for BiVO₄/rGO-HC (0.035 h^-1) compared to BiVO₄/rGO-LC (0.0128 h^-1) and BiVO₄ (0.011 h^-1) in ICPB protocol. The electrical energy per order required for removal of tetracycline hydrochloride in the ICPB protocol exhibited the lowest value for BiVO₄/rGO-HC among the tested materials and treatment protocols. These results highlight the importance of photoelectron shunting in enhancing efficiency of ICPB by engineering graphene at the interface of photocatalyst and biofilm. This unveiled mechanism may serve as an excellent potential in designing energy-efficient ICPB systems targeting wastewater matrices.

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石墨烯集成紧密耦合光催化生物降解中界面依赖的电子分流

密切耦合光催化生物降解（ICPB）是近年来发展起来的一种高效的废水处理技术，特别是在去除持久性有机污染物方面。然而，光催化剂/生物膜在光电子转移方面的相互作用及其对ICPB整体性能的影响尚未得到探讨。为了研究这些问题，制备了低接触度（BiVO4/rGO-LC）和高接触度（BiVO4/rGO-HC）的钒酸铋与还原氧化石墨烯的界面工程复合材料，并将其应用于ICPB。结果表明，复合材料具有界面依赖的光学、结构和载流子分离性能。光电化学测量证实光催化剂和生物膜之间存在光电子分流，而在ICPB方案中，BiVO4/rGO-HC的电流密度比BiVO4/rGO-LC和BiVO4更高（Nyquist弧更小），证实了亲密界面接触对光电子从BiVO4分流到生物膜的关键作用。因此，石墨烯的存在及其界面质量决定了光催化剂和生物膜之间的光电子分流，增强了光电子空穴分离，并实现了BiVO4/rGO-HC对盐酸四环素的降解率（0.031 h-1），而BiVO4/rGO-LC （0.013 h-1）和BiVO4 （0.011 h-1）在ICPB方案中。在所有测试材料和处理方案中，BiVO4/rGO-HC去除盐酸四环素所需的每阶电能是最低的。这些结果强调了通过在光催化剂和生物膜的界面处设计石墨烯来提高ICPB效率的光电子分流的重要性。这一揭示的机制可能为设计针对废水基质的节能ICPB系统提供了良好的潜力。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.