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Chinese Chemical Letters 2022年第1期33卷 1-10页

作者： Dongli Guo Shijie You Fang Li Yanbiao Liu State Key Laboratory of Urban Water Resource and Environment School of EnvironmentHarbin Institute of TechnologyHarbin 150090China Textile Pollution Controlling Engineering Center of Ministry of Environmental Protection College of Environmental Science and EngineeringDonghua UniversityShanghai 201620China

The engineering of carbon nanocatalysts for the persulfate activated elimination of emerging organic contaminants(EOCs)demonstrates promising potential compared with metal-based counterparts due to their unique advantage of high stability and low toxicity.The early reviews introduced the theoretical background of persulfate activation together with a detailed summary of different mechanisms responsible for degradation of EOCs.To further unify the state of knowledge,identify the research gaps,and prompt new research in this area,we present a thorough review on current trends in research on metal-free carbon nanocatalysts(e.g.,0D nanodiamond,1D carbon nanotubes and carbon nanofibers,2D graphene and graphitic carbon nitride,and 3D carbon nanocatalysts),with emphasis on their applications in persulfate activation and EOCs decontamination.We also discuss the current challenges and future perspectives in practically relevant applications.Last,we highlight that the development of sustainable carbon nanocatalysts/persulfate systems lies at the interface of multiple disciplines,which calls for future in-depth interdisciplinary collaborations.

关键词： Carbon nanocatalysts persulfate activation Advanced oxidation processes Emerging organic contaminants Water purification

Achieving high-efficient photocatalytic persulfate-activated degradation of tetracycline via carbon dots modified MIL-101(Fe)octahedrons

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Chinese Journal of Chemical Engineering 2024年第2期66卷 298-309页

作者： Hao Yuan Xinhai Sun Shuai Zhang Weilong Shi Feng Guo School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China

The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.

关键词： Carbon dots MIL-101(Fe) Photocatalytic persulfate activation Tetracycline degradation

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Overestimate of remediation efficiency due to residual sodium persulfate in PAHs contaminated soil and a solution

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Journal of Environmental Sciences 2022年第3期34卷 242-250页

作者： Liping He Jianhao Tong Yuanqiang Yang Jianxun Wu Linqian Li Zhonghua Wei Wei Long Jingli Pang Jiyan Shi Yunnan Research Academy of Eco-environmental Sciences Kunming 650034China Department of Environmental Engineering College of Environmental and Resource SciencesZhejiang UniversityHangzhou 310058China Beijing Construction Engineering Group Environmental Remediation Co.Ltd. Beijing 100015China

Oxidation remediation is a commonly used technology for PAHs contaminated soil presently,but the overestimate of efficiency due to ongoing remediation by residual oxidants during extraction and testing has not been paid enough attention.In this study,persulfate was activated by Fe(Ⅱ)to investigate the effects of residual oxidants on PAHs removal during detection process and the elimination effects of adding Na_(2)SO_(3) and extending sampling time on residual oxidants.Results verified that the residual oxidants removed PAHs in extraction process,making the results lower than the actual values:the detection recovery rate η of ΣPAHs and 3-6 ring PAHs ranged from 24.3%(25%Na_(2)S_(2)O_(8)treatment)to 87.4%(5%Na_(2)S_(2)O_(8)+4/4Fe^(2+) treatment),20.1%-99.0%,28.9%-87.9%,20.8%-89.4%,and 1.8.6%-76.9%,respectively.After adding Na_(2)SO_(3),the accuracy of detection results increased significantly:the η of ΣPAHs and 3-6 ring PAHs increased to 64.1%-96.5%,58.8%-95.5%,73.8%-114.4%,60.6%-95.6%,and 45.4%-77.1%,respectively.After 49 days of adding oxidants,residual oxidants had no considerable effect on the detection of PAHs,indicating it was appropriate to start soil remediation verification sampling49 days after the remediation was completed.The observed results will help scientific evaluation of the remediation effects of chemical oxidation on or-ganic contaminated soil.

关键词： persulfate activation Soil remediation Polycyclic aromatic hydrocarbons Residual oxidant removal

New insights into FeS/persulfate system for tetracycline elimination:Iron valence,homogeneous-heterogeneous reactions and degradation pathways

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Journal of Environmental Sciences 2022年第2期34卷 48-58页

作者： Jinhong Fan Ying Cai Shihao Shen Lin Gu State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

In this study,complete tetracycline(TTC)and above 50%of total organic carbon(TOC)were removed by Fe S/PS after 30 min under optimized conditions.Although free radicals and high-valent iron ions were identified to generate in the process,the apparent similarity between intermediate products of Fe S/PS,Fe/PS,and UV/PS systems demonstrated that the degradation of TTC was due to sulfate radicals(SO_(4)·^(-))and hydroxyl radicals(·OH).Based on the reaction between free radicals and organic matter,we speculated that TTC in the Fe S/PS system was decomposed and mineralized by dehydration,dehydrogenation,hydroxyl addition,demethylation,substitution,E-transfer,and ring-opening.Furthermore,a new understanding of Fe S-mediated PS activation based on stoichiometry and kinetic analysis showed that there were both homogeneous and heterogeneous reactions that occurred in the entire progress.However,due to the effect of p H on the dissolution of iron ions,the homogeneous reaction became the principal process with iron ions concentration exceeding 1.35 mg/L.This work provides a theoretical basis for the study of the degradation of TTC-containing wastewater by the iron-based advanced oxidation process.

关键词： Tetracycline persulfate activation Iron valence Homogeneous-heterogeneous reactions Degradation pathways

Carbon-based single-atom catalysts in advanced oxidation reactions for water remediation:From materials to reaction pathways

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Eco-Environment & Health 2023年第2期2卷 47-60页

作者： Junjie Zhang Xu Tang Yongjia Hong Guanyu Chen Yong Chen Li Zhang Wenran Gao Yang Zhou Bin Sun State Key Laboratory of Organic Electronics and Information Displays Institute of Advanced Materials(IAM)School of Material Science and EngineeringNanjing University of Posts and TelecommunicationsNanjing 210023China Joint International Research Laboratory of Biomass Energy and Materials Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesCollege of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037China

Single-atom catalysts(SACs)have been widely recognized as state-of-the-art catalysts in environment remediation because of their exceptional performance,100%metal atomic utilization,almost no secondary pollution,and robust structures.Most recently,the activation of persulfate with carbon-based SACs in advanced oxidation processes(AOPs)raises tremendous interest in the degradation of emerging contaminants in wastewater,owning to its efficient and versatile reactive oxidant species(ROS)generation.However,the comprehensive and critical review unraveling the underlying relationship between structures of carbon-based SACs and the corresponding generated ROS is still rare.Herein,we systematically summarize the fundamental understandings and intrinsic mechanisms between single metal atom active sites and produced ROS during AOPs.The types of emerging contaminants are firstly elaborated,presenting the prior pollutants that need to be degraded.Then,the preparation and characterization methods of carbon-based SACs are overviewed.The underlying material structure–ROS type relationship in persulfate-based AOPs is discussed in depth to expound the catalytic mechanisms.Finally,we briefly conclude the current development of carbon-based SACs in AOPs and propose the prospects for rational design and synthesis of carbon-based SACs with on-demand catalytic performances in AOPs in future research.

关键词： Single-atom catalysts Emerging contaminants Advanced oxidation processes persulfate activation Reactive oxidant species

燃烧合成高熵碳化物纳米颗粒活化过硫酸盐降解四环素污染物

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Science China Materials 2022年第11期65卷 3144-3149页

作者：褚衍辉余仁旺贺刚张婷董恒邓书香李江涛 School of Materials Science and Engineering South China University of TechnologyGuangzhou 510641China Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional CrystalCollege of Material Science and EngineeringTianjin University of TechnologyTianjin 300384China College of Environmental Science and Engineering Nankai UniversityTianjin 300350China Key Laboratory of Cryogenics Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China

高熵碳化物纳米颗粒的发展将为未来科技带来无限可能.然而,目前传统的合成方法很难实现该纳米材料的有效合成.为此,本文首次报道了一种简单、快速、低成本的燃烧合成方法,实现了高熵碳化物纳米颗粒的可控合成.即首先从热力学方面分析了... 详细信息

高熵碳化物纳米颗粒的发展将为未来科技带来无限可能.然而,目前传统的合成方法很难实现该纳米材料的有效合成.为此,本文首次报道了一种简单、快速、低成本的燃烧合成方法,实现了高熵碳化物纳米颗粒的可控合成.即首先从热力学方面分析了燃烧合成高熵碳化物纳米颗粒的可能性,然后以金属氧化物粉、碳粉、镁粉为反应原料以及氟化钠为熔盐介质,采用燃烧合成方法成功合成出(Ta_(0.25)Nb_(0.25)-Zr_(0.25)Ti_(0.25))C高熵碳化物纳米颗粒(燃烧温度:~1487 K,持续时间:63 s,升温速率:-68 K s^(-1)).实验结果表明:合成的高熵碳化物纳米颗粒不仅在所有组成元素的含量和分布上具有高度均匀性,而且氧杂质含量低,仅为2.98 wt%.此外,合成的高熵碳化物纳米颗粒可以作为硫酸盐活化剂用于降解去除地下水或污水中的四环素污染物,10小时内的去除率可达到~65.5%.

关键词： high-entropy carbides nanoparticles combustion synthesis persulfate activation oxidation catalyst

Efficient photodegradation of phenol assisted by persulfate under visible light irradiation via a nitrogen-doped titanium-carbon composite

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Frontiers of Chemical Science and Engineering 2021年第5期15卷 1125-1133页

作者： Yan Cui Zequan Zeng Jianfeng Zheng Zhanggen Huang Jieyang Yang State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan030001China

To realize the utilization of visible light and improve the photocatalytic efficiency of organic pollutant degradation in wastewater,a nitrogen-doped titanium-carbon composite(N-TiO_(2)/AC)prepared by sol-gel methods was applied in the photodegradation of phenol assisted by persulfate under visible light irradiation(named N-TiO_(2)/AC/PS/VIS).The results show that a synergistic effect exists between visible-light photocatalysis and persulfate activation.Compared with TiO_(2)/PS/VIS,the phenol degradation rate was found to be observably improved by 65%in the N-TiO_(2)/AC/PS/VIS system.This significant increase in degradation rate was mainly attributed to the following two factors:1)The N and C doping can change the crystal structure of TiO_(2),which extends the TiO_(2)absorption wavelength range to the visible light region.2)As an electron acceptor,PS can not only prevent electrons and holes from recombining with each other but can also generate strong oxidizing radicals such as·SO_(4)^(−) and·OH to accelerate the reaction dynamics.The process of phenol degradation was found to be consistent with the Langmuir pseudo-first-order kinetic model with an apparent rate constant k of 1.73 min^(−1).The N-TiO_(2)/AC/PS/VIS process was proven to be a facile method for pollutant degradation with high pH adaptability,excellent visible-light utilization and good application prospects.

关键词： N-TiO_(2)/AC visible light photocatalysis persulfate activation phenol