Facile synthesis of direct Z-scheme PPy/NH2-UiO-66 heterojunction for enhanced photocatalytic Cr(VI) reduction, industrial electroplating wastewater treatment, and tetracycline degradation

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-12-28 DOI:10.1016/j.apcatb.2023.123669

Qi Wang , Shuzhen Zheng , Wanggang Ma , Jianying Qian , Lingye Huang , Hao Deng , Qi Zhou , Sirui Zheng , Shuangjun Li , Hao Du , Qiang Li , Derek Hao , Guoxiang Yang

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Abstract

Z-scheme heterojunction photocatalysts generally have excellent redox ability and robust removal efficiency for contaminants in water. Herein, we combined p-type PPy and n-type NH₂-UiO-66 by ball milling to prepare a direct Z-scheme PPy/NH₂-UiO-66 photocatalyst with ultra-high redox potential. Notably, the optimized efficiency of PPy/NH₂-UiO-66 (the mass ratio of PPy to NH₂-UiO-66 is 1 wt%, named PPy/NU-1) rapidly reduced Cr(VI) (>95%, 60 min) and TC degradation (>90%, 180 min) at 100 W LED light. Moreover, the PPy/NU-1 has high stability and good anti-interference ability, which can effectively remove Cr(VI) from industrial electroplating wastewater, and the Cr(VI) removal rate is 99%, which meets the industrial wastewater standard and has the potential attraction of actual wastewater treatment. In addition, the techniques of UV-Vis diffuse reflection, electron spin resonance (ESR), photoluminescence (PL), and photoelectrochemical measurement showed that PPy/NH₂-UiO-66 composites improved the light capture ability, thereby improving the photocatalytic efficiency. The PPy/NU-1 has a very high redox potential by constructing a Z-scheme heterojunction, enhances the interfacial charge transfer ability, and improves the separation efficiency of photogenerated carriers. Finally, the mechanism of the Z-scheme was systematically by nitroblue tetrazolium (NBT) and p-phthalic acid (TA) transformation, ESR experiments, and density functional theory (DFT) calculations. This work provides a strategy for the preparation of visible photocatalysts with excellent photocatalytic activity and provides new insights for interfacial charge transfer and molecular oxygen activation.

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便捷合成直接 Z 型 PPy/NH2-UiO-66 异质结，用于增强光催化还原 Cr(VI)、处理工业电镀废水和降解四环素

Z 型异质结光催化剂通常具有优异的氧化还原能力和强大的去除水中污染物的效率。在此，我们通过球磨将 p 型 PPy 和 n 型 NH2-UiO-66 结合在一起，直接制备出了具有超高氧化还原电位的 Z 型 PPy/NH2-UiO-66 光催化剂。值得注意的是，PPy/NH2-UiO-66（PPy与NH2-UiO-66的质量比为1 wt%，命名为PPy/NU-1）的效率得到了优化，在100 W LED光照下可快速还原Cr(VI)（95%，60分钟）和降解TC（90%，180分钟）。此外，PPy/NU-1稳定性高，抗干扰能力强，能有效去除工业电镀废水中的六价铬，六价铬去除率达99%，符合工业废水标准，具有实际废水处理的潜在吸引力。此外，紫外可见光漫反射、电子自旋共振（ESR）、光致发光（PL）和光电化学测量等技术表明，PPy/NH2-UiO-66 复合材料提高了光捕获能力，从而提高了光催化效率。PPy/NU-1 通过构建 Z 型异质结具有很高的氧化还原电位，增强了界面电荷转移能力，提高了光生载流子的分离效率。最后，通过硝基蓝四氮唑（NBT）和对邻苯二甲酸（TA）转化、ESR 实验和密度泛函理论（DFT）计算，系统地研究了 Z 型结构的机理。这项工作为制备具有优异光催化活性的可见光光催化剂提供了一种策略，并为界面电荷转移和分子氧活化提供了新的见解。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.