Novel inorganic/organic Z-scheme heterojunction rGO@PANI/SnO2 with enhanced photocatalytic activity for degradation of sulfadiazine

IF 6.9 2区环境科学与生态学 Q1 ENGINEERING, CHEMICAL

Process Safety and Environmental Protection Pub Date : 2025-01-02 DOI:10.1016/j.psep.2024.12.125

Yujie Zhang, Zexin Cui, Rongfang Yuan, Huilun Chen, Beihai Zhou

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引用次数: 0

Abstract

As the persistent contamination of water sources with antibiotics poses a growing environmental challenge, effective strategies for the degradation of such pollutants are urgently needed. Herein, a novel organic-inorganic Z-scheme heterojunction material, reduced Graphene Oxide (rGO)@PANI/SnO2, was prepared for the photocatalytic degradation of sulfadiazine (SD). When the PANI/SnO2 with PANI doping amount of 1 % was loaded on 1 % rGO, the catalyst showed the best photocatalytic activity, with a reaction rate constant of 0.184 h−1, which was 32.8 and 7.19 times higher than that of PANI and SnO2, respectively. The improved photocatalytic activity was mainly due to the high electrical conductivity of rGO and the formation of a Z-scheme heterojunction between PANI and SnO2, which effectively facilitated the transfer of photogenerated carriers. Quenching experiments showed that ·OH is the main active species. Besides, Density Functional Theory (DFT) calculations found that the sulfonamide bond and pyrimidine heterocyclic were vulnerable site in the SD. Then, four possible degradation pathways were proposed, primarily involving the breaking of the sulfonamide bond and the ring-opening of the pyrimidine heterocycle. The response surface method (RSM) was used to confirm that the removal of SD was affected by the single factor of initial SD concentration, pH value and catalyst dosage, and the magnitude of the effect of different parameters was in the order of pH > catalyst dosage > SD concentration. It was found that Cl- and SO42- inhibited the photocatalytic process, whereas HCO3- facilitated the process through its ability to produce ·OH by hydrolysis and provide a weakly alkaline environment. This work provides novel ideas for the preparation of organic-inorganic heterojunction photocatalysts and enhances the application of organic materials in the photocatalytic degradation of antibiotics in water.

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新型无机/有机z型异质结rGO@PANI/SnO2光催化降解磺胺嘧啶活性增强

随着抗生素对水源的持续污染对环境构成越来越大的挑战，迫切需要有效的降解此类污染物的策略。本文制备了一种新型的有机-无机Z-scheme异质结材料，还原氧化石墨烯（rGO）@PANI/SnO2，用于光催化降解磺胺嘧啶（SD）。当PANI掺杂量为1 %的PANI/SnO2负载在1 %的rGO上时，催化剂表现出最好的光催化活性，反应速率常数为0.184 h−1，分别是PANI和SnO2的32.8倍和7.19倍。提高的光催化活性主要是由于氧化石墨烯的高导电性和PANI与SnO2之间形成Z-scheme异质结，有效地促进了光生载流子的转移。猝灭实验表明，·OH是主要的活性物质。此外，密度泛函理论（DFT）计算发现，磺胺键和嘧啶杂环是SD中的易损位点。然后，提出了四种可能的降解途径，主要涉及磺酰胺键断裂和嘧啶杂环开环。通过响应面法（RSM）证实，SD的去除率受SD初始浓度、pH值和催化剂用量这一单一因素的影响，不同参数的影响程度依次为pH >； 催化剂用量>； SD浓度。发现Cl-和SO42-抑制了光催化过程，而HCO3-通过其水解生成·OH的能力和提供弱碱性环境促进了这一过程。本研究为有机-无机异质结光催化剂的制备提供了新的思路，并促进了有机材料在光催化降解水中抗生素中的应用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Process Safety and Environmental Protection 环境科学-工程：化工

CiteScore

11.40

自引率

15.40%

发文量

929

审稿时长

8.0 months

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