英语原文共 10 页

Peroxymonosulfate improved photocatalytic degradation of atrazine by activated carbon/graphitic carbon nitride composite under visible light irradiation

在可见光辐射的条件下，过氧化单硫酸盐能够提升阿特拉津在活性炭/石墨相氮化碳复合物的光催化降解效果。

Jean Marie Dangwang Dikdim ,Yan Gong ,Guy Bertrand Noumi,

Joseph Marie Sieliechi , Xu Zhao , Ning Ma , Min Yang , Jean Bosco Tchatchueng

饮用水科学与技术重点实验室，生态环境研究中心，中国科学院，北京，100085，中华人民共和国

农业工程与技术国际学院，恩冈代雷大学，邮政部门邮箱地址455，恩冈代雷，喀麦隆共和国

科学学院，恩冈代雷大学，邮政部门邮箱地址455，恩冈代雷，喀麦隆共和国

中国科学院大学，北京，100049，中华人民共和国

流域水资源绿色与可循环发展工程北京重点实验室，北京水科学与技术研究所，北京，100048，中华人民共和国

强调部分：

不同含量比例的活性炭成功负载在石墨相氮化碳中

活性炭的加入增强了光生电荷载体的分离和过氧化单硫酸盐对石墨相氮化碳的活化作用

通过加入过氧化单硫酸盐，活性炭/石墨相氮化碳复合材料在可见光辐射的条件下很好地表现出了对阿特拉津降解的光催化效果。

文献信息：

文献的时间：接受时间：2018年9月6月

接受并修改时间从2018年10月20日开始

收纳时间：2018年10月25日

网上查阅时间：2018年10月26日

管理编辑：Jun Huang

关键词：光催化剂、过氧化单硫酸盐、阿特拉津、碳基氮化碳、活性炭

Abstract：

The photocatalytic degradation of atrazine by activated carbon/graphitic carbon nitride composites with peroxymonosulfate (PMS) was investigated under visible light irradiation. The photocatalysts were prepared at different activated carbon (AC) loaded percentages and characterized by XRD, FT-IR, BET surface area, SEM, UV-Vis absorbance, photocurrent response and EIS. Several parameters which might influence the degradation efficiency were studied including PMS concentration, solution pH, catalyst dosage, initial atrazine concentration as well as water matrix effect. The results indicated that incorporation of AC contributes effectively in suppressing the recombination of electron-holes pairs and enhancing the photocatalytic performance of graphitic carbon nitride. More significantly, the degradation efficiency of atrazine showed remarkable improvement with PMS addition under visible light irradiation. The reaction rate constant of the 10% AC/g-C3N4/Vis/PMS system (0.0376 min-1) was approximately 2.9 times higher than that of g-C3N4/Vis/PMS system (0.0128 min-1). Results from quenching tests revealed that both sulfate and hydroxyl radicals were involved in the degradation of atrazine, while the latter is the main contributor. This paper constitutes an insight for the metal-free catalyst activation of PMS by photocatalysis for environmental remediation。

摘要：

本文研究了在可见光辐射的条件下，利用活性炭/石墨相氮化碳的复合物耦合过氧化单硫酸盐对阿特拉津的光催化分解作用。这种光催化剂是将不同比例的活性炭负载到复合物中进行制备的，并且该化合物通过X射线衍射仪、傅立叶变换红外光谱仪、BET法测比表面积仪、扫描电子显微镜、紫外可见分光光度计、光电流响应和电化学阻抗谱仪进行表征。本文研究了包括过氧化单硫酸盐浓度、溶液PH值、催化剂剂量、阿特拉津初始浓度和水分子的基体效应在内的重要参数对降解效率的影响。结果表明，活性炭的加入也能够高效的阻止了电子空穴对的重新组合并且提高了石墨相氮化碳的光催化效果。更重要的是，在可见光辐射的条件下，过氧化单硫酸盐的添加对阿特拉津的降解效率有显著的提高。10%wt的活性炭/石墨相氮化碳/可见光辐射/过氧化单硫酸盐体系的反应速率常数（0.0376 min^-1）比石墨相氮化碳/可见光辐射/过氧化单硫酸盐体系的反应速率常数大约高出了2.9倍。根据停止反应试验的结果来看，在对阿特拉津的降解过程中，硫酸根离子和羟基自由基同时存在于该反应中，但是后者是主要推动反应进行的物质。此文献主要关注于非金属中过氧化单硫酸盐作为催化剂活化物的光催化剂对环境的修复作用。

1. Introduction

Nowadays, agricultural activities involve high amount of phytosanitary products such as fertilizers and pesticides in order to improve the production and satisfy the growing population at the same time. Usually, the farmers focus their objectives mainly on the optimal yield of production than respect of dosage norms leading to excessive use of these chemicals. Consequently, as a non-point source of pollution, there is undergoing severe environmental pollution and inherent impact on human health (Soliacute;s et al., 2016). Among these compounds, atrazine is an s-triazine herbicide which is one most commonly used throughout the world. Unfortunately, this compound also constitutes a risk for water quality due to its mobility in the environment, toxicity, solubility in water and low biodegradability (Ouyang et al., 2017; Xu et al., 2013). Atrazine and its by-products have been frequently found in groundwater and surface water at concentration exceeding authorized limits after long-term application (Vonberg et al., 2014; Ouyang et al., 2017). It is worthy to note that atrazine has been banned from European Union since 2004 and listed as priority substance which may cause harmful effects on the environment and human health via aquatic environment (EU, 2013). In addition, atrazine is an endocrine disruptor compound and potential human carcinogen (Chan and Chu, 2009; Khan et al., 2013; Ji et al., 2015). Regarding these harmful effects, various methods for atrazine removal from water have been applied such as adsorption (Shirmardi et al., 2016), biodegradation (Debasmita and Rajasimman, 2013) and advanced oxidation processes (Oturan et al., 2012)

1 介绍

当今社会中，为了能够提高农作物的产量并同时保证农作物生长过程的安全，农业生产中都会使用高剂量保证作物免疫的产品，例如肥料和杀虫剂。通常，农民常常只会关注与作物的最佳产量这样的问题，而忽略了对植物检疫剂量的标准规范，这样往往会导致这些化学物质的过量使用。因此，那些作为不定源的污染物，会对环境产生严重的污染并对人的健康产生不可逆转的伤害。在这些化合物当中，阿特拉津是一种全世界内广泛应用的均三嗪类除草剂。然而，这种化合物由于在环境中具有流动型，一定的毒性，水溶性以及低生物降解性，所以阿特拉津将会对水质有一定程度的危害。在对阿特拉津以及其副产物长期使用的过程中，其在地下水和地表水的浓度经常性的会被发现超过公认的最低限度。值得一提的是，自2004年开始，欧盟已经禁止了阿特拉津的使用并将其优先列为水污染性、对环境与人体有毒害作用的物质。另外，阿特拉津会扰乱人体的内分泌过程，也是一种潜在的致癌物质。关于阿特拉津所造成的种种危害来看，人们利用诸如：吸附、生物降解和高级氧化技术等多种方法对水中的阿特拉津进行去除。

Recently, sulfate radicals (SO₄`<sup>-</sup>) based advanced oxidation processes (AOP) are of increasing interest for water and wastewater treatment. The principle of these processes involves the in situ generation of SO<sub>4</sub>`^- radicals and degradation of organic pollutant. It has been admitted that SO₄<sup>`-</sup> radicals-based processes offers more advantages compared to classically hydroxyl radicals (HO`) - based AOP such as the independence of pH, high oxidation potential (E⁰= 2.5-3.2 V), stability and long life (Chan and Chu, 2009; Ghanbari and Moradi, 2017; Z

资料编号：[3659]