揭示电子在全光谱响应e-LDH/t-BiOCl/Bi2S3中的多级短程迁移及其在Cr(VI)和难降解有机污染物解毒中的重要作用。

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Environmental Research Pub Date : 2025-02-01 Epub Date: 2024-11-30 DOI:10.1016/j.envres.2024.120479
Jing Bai, Chen Wang, Xiangling Zhang, Xuhao Li, Yajia Mao, Wei Liang, Cong Zhang, Xinlu Xiao, Jun Shen
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引用次数: 0

摘要

含有致癌物Cr(VI)和难降解染料的有毒印染废水对生态安全和人体健康构成严重威胁。本文构建了一种超薄夹层结构的新型复合光催化材料e-LDH/t-BiOCl/Bi2S3,在全光谱照明下,通过吸附-光催化协同机制,对Cr(VI)和活性红2的去除率分别为0.044和0.019 min-1。该结构利用界面条件和内置电场形成多层短程电荷迁移通道,实现了电子(e-)和空穴(h+)对Cr(VI)和偶氮染料的定向还原氧化。e-除了促进Cr(VI)的还原外,还可以提高h+的有效利用,并介导其他以RR2降解为目标的活性氧的形成。通过DFT计算、LC-MS表征和T.E.S.T.评价等方法探讨了RR2单体和Cr(VI)/RR2共存反应体系的降解机理、途径和生物毒性。此外,我们进一步研究了连续流动和真实水环境下e-LDH/t-BiOCl/Bi2S3系统的光催化活性和成本效益,并确定了影响光催化性能的主要水质参数。本研究为合理设计具有理想形貌和竞争性能的三元异质结构光催化剂提供了新的思路。
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Revealing multi-level shortrange migration of electrons on full-spectrum response e-LDH/t-BiOCl/Bi2S3 and their essential role in the detoxification of Cr(VI) and refractory organic pollutants.

The toxic dyeing wastewater containing both carcinogenic Cr(VI) and refractory dyes poses serious threats to ecological safety and human health. Herein, a novel composite photocatalytic material e-LDH/t-BiOCl/Bi2S3 with an ultrathin sandwich structure constructed achieves removal rate constants of 0.044 and 0.019 min-1 for Cr(VI) and reactive red 2 by adsorption-photocatalysis synergistic mechanism in full-spectrum illumination. This structure employs the interface conditions and built-in electric field to form multilevel short-range charge migration channel, achieving the targeted reduction and oxidation of Cr(VI) and azoxy dyes by electrons (e-) and holes (h+). Besides facilitating the reduction of Cr(VI), e- can also enhance the effective utilization of h+ and mediate the formation of other reactive oxygen species that target RR2 degradation. The degradation mechanism, pathway, and biological toxicity of RR2 single and Cr(VI)/RR2 coexistence reaction system were discussed by DFT calculation, LC-MS characterization, and T.E.S.T. evaluation. Moreover, we further investigated the photocatalytic activity and cost-effectiveness of the e-LDH/t-BiOCl/Bi2S3 system under continuous flow and real water settings, and determined the primary water quality parameters that influence photocatalytic performance. This work establishes a new concept for the rational design of robust ternary heterostructure photocatalysts with desirable morphology and competitive performance for photocatalytic applications.

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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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