Iron/nitrogen/sulfur co-doped cyanobacteria derived carbon composites for enhanced hydroxychloroquine degradation via primary nonradical pathway in peroxymonosulfate-based fenton-like system

IF 9.7 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Tao Wang , Yuxuan Yang , Zheren Tang , Pin Zhao , Kunlun Yang , Xinhua Xu
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Abstract

A green and efficient Fe/N/S co-doped carbon catalysts (ITC-X-800) was successfully prepared from Fe/N-rich salvaged cyanobacteria and thiourea for catalyzing peroxymonosulfate (PMS) to degradate hydroxychloroquine (HCQ). Characterization tests confirmed that defect degree, electron transfer capability, and the content of main functional groups like π-π∗, Fe-NX, graphitic N and thiophene S etc. in ITC-X-800 was firstly increased and then decreased with the increasing doping S, indicating the critical role of S for regulating functional sites containing Fe/N on the carbon nanosheets. Optimized ITC-2-800 with appropriate S showed suitable HCQ adsorption ability, lowest resistance and more PMS activation sites. Almost 100% of HCQ could be removed via ITC-2-800/PMS system in 60 min within 0.5 mM PMS and 0.1 g/L ITC-2-800, whose HCQ degradation kinetic constant was 2.5 times that of Fe/N doped carbon catalyst. Based on the basic strong electron transfer ability and HCQ adsorption affinity of π-π∗, the high PMS adsorption and catalyzing capacity of Fe-NX, and the extra enhanced carbon skeleton activation of thiophene S, the synergistic effect of these groups in ITC-2-800 was proved to play a more important role in enhanced PMS activation and HCQ degradation. Ascribed to the synergistic effect of Fe/N/S, non-radical pathway based on 1O2 and high-valent iron-oxo species played a dominant role in HCQ degradation. Furthermore, ITC-2-800 showed high universality, stability, reusability and potential practicability during comprehensive test. This study provided deeper insights for the resourceful treatment of algae mud and the synergistic mechanism of heteroatoms in carbon-based catalysts for PMS activation.

Abstract Image

Abstract Image

铁/氮/硫共掺杂蓝藻衍生碳复合材料在过氧单硫酸盐基类芬顿体系中通过初级非自由基途径增强对羟氯喹的降解
以富铁/N的回收蓝藻和硫脲为原料,成功制备了绿色高效的Fe/N/S共掺杂碳催化剂(ITC-X-800),用于催化过氧单硫酸盐(PMS)降解羟氯喹(HCQ)。表征实验证实,随着掺杂S的增加,ITC-X-800的缺陷程度、电子转移能力以及主要官能团π-π*、Fe- nx、石墨N和噻吩S等的含量先增加后降低,表明S对碳纳米片上含Fe/N的功能位点的调节具有关键作用。优化后的ITC-2-800具有较好的HCQ吸附能力、较低的抗性和较多的PMS活化位点。在0.5 mM的PMS和0.1 g/L的tc -2-800/PMS条件下,在60 min内可脱除几乎100%的HCQ,其HCQ降解动力学常数是Fe/N掺杂碳催化剂的2.5倍。基于π-π*的碱性强电子转移能力和对HCQ的吸附亲和力,Fe-NX对PMS的高吸附和催化能力,以及噻吩S碳骨架活化的额外增强,证明了这些基团在tc -2-800中协同作用在增强PMS活化和HCQ降解中发挥更重要的作用。由于Fe/N/S的协同作用,基于1O2和高价氧化铁的非自由基途径在HCQ降解中起主导作用。综合测试表明,ITC-2-800具有较高的通用性、稳定性、可重用性和潜在的实用性。本研究为藻泥资源化处理及碳基催化剂中杂原子对PMS活化的协同作用机制提供了更深入的认识。
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来源期刊
Journal of Cleaner Production
Journal of Cleaner Production 环境科学-工程:环境
CiteScore
20.40
自引率
9.00%
发文量
4720
审稿时长
111 days
期刊介绍: The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.
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