Journal of Environmental Chemical Engineering最新文献

Advances in the application of graphene oxide composite loose nanofiltration membranes for dye and salt separation 氧化石墨烯复合松散纳滤膜在染料和盐分离方面的应用进展

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-30 DOI: 10.1016/j.jece.2024.114278

The wide application of loose nanofiltration (LNF) membranes in textile wastewater treatment has demonstrated the advantages of efficient separation of dyes and salts. Among them, the composite loose nanofiltration membranes prepared using graphene oxide (GO) showed more efficient dye retention and salt permeability due to its broad specific surface area and abundant oxygenated surface functional groups. In this paper, the four aspects of preparation method, separation mechanism, separation performance and application are described. In terms of preparation methods, this paper focuses on two main methods, phase transformation and interfacial polymerization. In addition, other preparation methods such as mussel-inspired deposition, co-deposition and self-assembly are also discussed. In terms of the separation mechanism, spatial repulsion and electrostatic effect are analyzed as the main mechanisms for the separation of dyes and salts by loose nanofiltration membranes. Moreover, this paper emphasizes the excellent contamination resistance, antimicrobial properties and long-term stability of GO composite loose nanofiltration membranes. In response to these properties, the advantages of the membrane in terms of separation performance are analyzed. Finally, this paper also presents the possible future challenges that loose nanofiltration membranes may face in a wide range of applications.

松散纳滤膜（LNF）在纺织废水处理中的广泛应用证明了其高效分离染料和盐分的优势。其中，利用氧化石墨烯（GO）制备的复合松散纳滤膜因其宽广的比表面积和丰富的含氧表面官能团，显示出更高效的染料截留性和盐分渗透性。本文从制备方法、分离机理、分离性能和应用四个方面进行了阐述。在制备方法方面，本文主要介绍了相变和界面聚合两种方法。此外，还讨论了贻贝启发沉积、共沉积和自组装等其他制备方法。在分离机理方面，分析了空间斥力和静电效应是松散纳滤膜分离染料和盐类的主要机理。此外，本文还强调了 GO 复合松散纳滤膜优异的抗污染性、抗菌性和长期稳定性。针对这些特性，本文分析了该膜在分离性能方面的优势。最后，本文还介绍了松散纳滤膜未来在广泛应用中可能面临的挑战。

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引用次数: 0

Neutralizing the threat: A comprehensive review of chemical warfare agent decontamination strategies 消除威胁：全面审查化学战剂去污战略

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-27 DOI: 10.1016/j.jece.2024.114243

Chemical warfare agents (CWAs) represent a significant threat, necessitating the development of effective decontamination strategies. This article reviews various decontamination methods, analysing their respective strengths and weaknesses against chemical warfare agents including vesicants: sulfur mustard (bis(2-chloroethyl) sulfide, HD; nitrogen mustards; bis(2-chloroethyl)ethylamine (HN1), bis (2-chloroethyl)methylamine (HN2), tris(2-chloroethyl)amine (NH3) and Lewisite; nerve agents sarin (isopropyl methylphosphonofluoridate, GB), soman (pinacolyl methylphosphonofluoridate, GD), tabun (Ethyl N,N’-dimethylphosphoroamidocyanidate, GA) and VX, (ethyl N-2-diisopropyl aminoethyl methylphosphonothiolate); vomiting agent Clark I (diphenylchloroarsine, DA). Traditional decontamination approaches include hydrolysis, which utilises water for CWA breakdown, and chlorine-based decontamination, known for its effectiveness despite environmental drawbacks. Advanced oxidation processes (AOPs) offer efficient CWA destruction using highly reactive radicals but can be complex to implement. Emerging materials such as metal-organic frameworks (MOFs) have the potential to revolutionise the field of chemical warfare agent decontamination due to their high surface area and tunable structures. Additionally, polyoxometalates (POMs), zeolites, and reactive polymers are being investigated for their catalytic and adsorptive properties in CWA degradation. This review highlights the necessity for continuous research to develop efficient, safe, and environmentally friendly decontamination methods. The potential of combining existing approaches and tailoring novel materials, such as MOFs and reactive polymers, paves the way for significant advancements in CWA decontamination.

化学战剂 (CWA) 是一种重大威胁，因此有必要制定有效的去污策略。本文综述了各种去污方法，分析了它们在对付包括膀胱剂在内的化学战剂时各自的优缺点：硫芥子气（双（2-氯乙基）硫化物，HD；氮芥；双（2-氯乙基）乙胺（HN1）、双（2-氯乙基）甲胺（HN2）、三（2-氯乙基）胺（NH3）和路易斯特；神经毒剂沙林（甲基膦酰氟异丙酯，GB）、索曼（甲基膦酰氟嚬哪醇酯，GD）、塔崩（N,N'-二甲基磷酰胺氰酸乙酯，GA）和 VX（N-2-二异丙基甲基膦硫酸氨基乙酯）；呕吐剂克拉克 I（二苯基氯胂，DA）。传统的去污方法包括利用水分解 CWA 的水解法和基于氯的去污法，前者以其有效性而著称，尽管存在环境方面的缺点。高级氧化工艺（AOPs）可利用高活性自由基高效销毁 CWA，但实施起来可能比较复杂。金属有机框架（MOFs）等新兴材料具有高表面积和可调结构，因此有可能在化学战剂净化领域掀起一场革命。此外，人们还在研究聚氧化金属（POMs）、沸石和活性聚合物在降解化学战剂过程中的催化和吸附特性。本综述强调了继续研究开发高效、安全和环境友好型去污方法的必要性。结合现有方法和定制新型材料（如 MOFs 和活性聚合物）的潜力为 CWA 去污的重大进展铺平了道路。

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引用次数: 0

Synthesis of bifunctional copolymeric nanofibers with selective extracting U(VI) from the solution and antibacterial property 从溶液中选择性提取铀(VI)并具有抗菌性能的双功能共聚纳米纤维的合成

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-27 DOI: 10.1016/j.jece.2024.114229

Facing the problem of future nuclear fuel shortage, developing high-performance adsorbent materials is key. In this work, the amidoxime group/imidazole functionalized ionic liquid copolymer fibers containing bromide salts, and fluoroborate salts (namely P(AO/VEIMBr)₈ and P(AO/VEIMBF₄)₆) were prepared by a one-pot method and free radical polymerization, hydroxyl amination reaction and electrostatic spinning, and characterized by SEM, FT-IR, and ¹ H NMR. The influence of solid-liquid ratio, ionic strength, and adsorption time on the adsorption performance was investigated by batch adsorption experiments. In the meanwhile, the adsorption kinetics and thermodynamic processes of U(VI) on the copolymer fibers was also studied. Adsorption mechanism of U (VI) on polymer fibers was explored by XPS spectroscopic analysis combined with DFT method. Finally, the antimicrobial properties of the copolymer fibers were tested. The experimental results showed that the polymer nanofibers synthesized for U(VI) has a fast adsorption, high adsorption capacity at ionic strength close to seawater, and excellent reusability. The adsorption process conformed to the pseudo-second-order kinetic model and Langmuir model, which indicated that chemical adsorption and monolayer adsorption are dominant for adsorption U(VI) on the polymer nanofibers, and exhibits the highest Uranium adsorption capacity (76.92 mg/g and 81.96 mg/g at pH=8.1+0.1, respectively). XPS result showed the amine nitrogen and oxime oxygen in the amidoxime functional group were coordinated with uranyl(VI) ions. The antibacterial experiments showed that the copolymer fibers have antimicrobial properties and the antibacterial rate is over 90 %. Therefore, the nanofibers may be a promising material for extracting uranium from the weak alkaline wastewater or seawater.

面对未来核燃料短缺的问题，开发高性能吸附材料是关键所在。本研究采用一锅法，通过自由基聚合、羟基胺化反应和静电纺丝制备了含溴盐和氟硼酸盐的脒肟基/咪唑功能化离子液体共聚纤维（即 P(AO/VEIMBr)8 和 P(AO/VEIMBF4)6），并利用扫描电镜、傅立叶变换红外光谱和 1 H NMR 对其进行了表征。通过批次吸附实验研究了固液比、离子强度和吸附时间对吸附性能的影响。同时，还研究了 U（VI）在共聚物纤维上的吸附动力学和热力学过程。通过 XPS 光谱分析结合 DFT 方法探讨了 U（VI）在聚合物纤维上的吸附机理。最后，测试了共聚物纤维的抗菌性能。实验结果表明，合成的聚合物纳米纤维对铀（Ⅵ）具有快速吸附的特性，在离子强度接近海水的情况下吸附能力强，并且具有良好的重复使用性。吸附过程符合伪二阶动力学模型和 Langmuir 模型，表明聚合物纳米纤维对铀（Ⅵ）的吸附以化学吸附和单层吸附为主，并表现出最高的铀吸附容量（pH=8.1+0.1 时分别为 76.92 mg/g 和 81.96 mg/g）。XPS 结果表明，脒肟官能团中的胺氮和肟氧与铀酰（VI）离子配位。抗菌实验表明，共聚物纤维具有抗菌性能，抗菌率超过 90%。因此，纳米纤维可能是一种很有前途的从弱碱性废水或海水中提取铀的材料。

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引用次数: 0

Non-radical activation of peracetic acid by Fe-Co sulfide modified activated carbon for the degradation of refractory organic matter 硫化钴铁改性活性炭对过氧乙酸的非辐射活化，用于降解难降解有机物

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-26 DOI: 10.1016/j.jece.2024.114258

Recently, the non radical activation system had attracted much attention due to its strong anti-interference ability. In this study, a novel FeCo₂S₄/activated carbon (AC) catalyst was prepared and used to construct a non radical dominated degradation system. Due to the electron-donating groups (C-OH) of AC and the conversion of free radicals generated from the activation of PAA by iron (Fe) and cobalt (Co) ions, a large amount of singlet oxygen (¹O₂) were produced, making the activation system possessed excellent universality and applicability for the removal of organic pollutants. Within 5 min, about 89.87 % of tetracycline hydrochloride (TCH) was removed in FeCo₂S₄ /AC + PAA. After only 20 min of reaction, the TCH removal efficiency reached 94.12 %, accompany with the reaction rate reached 0.099 min⁻¹. Other organic pollutants including ibuprofen (IBU), sulfamethoxazole (SMX), ciprofloxacin (CIP), p-nitrophenol (PNP) and atrazine (ATZ) were also efficiently removed within 20 min, with the removal efficiencies were 92.0 %, 91.5 %, 89.4 %, 88.3 %, and 84.5 %, respectively. When the solution pH changed from 5.01 to 9.48, FeCo₂S₄ /AC also showed excellent catalytic performances, with the TCH removal rates were maintained at over 85.18 %. Moreover, the removal rate of TCH still reached 90.23 % after 5 recycles. This study offered an efficient non-radical peracetic acid (PAA) activation system, which can be effectively used to degrade refractory organic pollutants from complex water environment.

近年来，非自由基活化体系因其强大的抗干扰能力而备受关注。本研究制备了一种新型的 FeCo2S4/活性炭（AC）催化剂，并将其用于构建非自由基主导的降解体系。由于活性炭中的电子供能基团（C-OH）以及铁（Fe）和钴（Co）离子活化 PAA 产生的自由基的转化作用，产生了大量的单线态氧（1O2），使得该活化体系在去除有机污染物方面具有很好的普遍性和适用性。在 FeCo2S4 /AC + PAA 中，盐酸四环素（TCH）在 5 分钟内就被去除了约 89.87%。仅经过 20 分钟的反应，TCH 的去除率就达到了 94.12%，同时反应速率也达到了 0.099 min-1。其他有机污染物包括布洛芬（IBU）、磺胺甲噁唑（SMX）、环丙沙星（CIP）、对硝基苯酚（PNP）和阿特拉津（ATZ）也在 20 分钟内被有效去除，去除率分别为 92.0%、91.5%、89.4%、88.3% 和 84.5%。当溶液 pH 值从 5.01 变为 9.48 时，FeCo2S4 /AC 也表现出优异的催化性能，三氯氢烷去除率保持在 85.18 % 以上。此外，经过 5 次循环后，三氯乙烷的去除率仍达到 90.23%。该研究提供了一种高效的非辐射过乙酸（PAA）活化体系，可有效用于降解复杂水环境中的难降解有机污染物。

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引用次数: 0

Better waste utilization: Mg-modified biochar from wetland plant waste for phosphorus removal and carbon sequestration 更好地利用废物：从湿地植物废弃物中提取镁改性生物炭，用于除磷和固碳

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-26 DOI: 10.1016/j.jece.2024.114264

Withered wetland plants have become a treat to water ecological security. To address the issue of waste biomass disposal, a typical wetland plant, Hydrocotyle vulgaris, was utilized to produce Mg-modified biochar (MBC) for efficient phosphorus (P) removal and stable carbon sequestration. The adsorption behavior fit Langmuir isotherm and the pseudo second-order kinetic models, which revealed the nature of monolayer chemical adsorption of MBC. The removal of P was achieved through physical diffusion, Mg²⁺ precipitates, surface complexation and electrostatic attraction. Based on the analysis of thermodynamics models, it can be concluded that the adsorption behavior of P by MBC was spontaneous and endothermic. The MBC exhibited a maximum phosphorus adsorption capacity of 314.048 mg/g. Concurrently, the specific surface area was enhanced from 529.974 m²/g to 931.019 m²/g. The research has also recorded valuable data about the carbon sequestration potential of MBC with the carbon content reaching 0.51 g per g of biochar. It was found from the outcomes that Mg-modified biochar had outstanding carbon sequestration potential and significantly improved P removal efficiency.

湿地植物枯死已成为水生态安全的一大隐患。为了解决废弃生物质的处理问题，研究人员利用典型的湿地植物 Hydrocotyle vulgaris 生产镁改性生物炭 (MBC)，以达到高效除磷和稳定固碳的目的。吸附行为符合朗缪尔等温线和伪二阶动力学模型，揭示了 MBC 的单层化学吸附性质。P 的去除是通过物理扩散、Mg2+ 沉淀、表面络合和静电吸引实现的。根据热力学模型的分析，可以得出 MBC 对磷的吸附行为是自发的、内热的。MBC 的最大磷吸附容量为 314.048 mg/g。同时，比表面积从 529.974 m2/g 增加到 931.019 m2/g。研究还记录了有关 MBC 固碳潜力的宝贵数据，其碳含量达到每克生物炭 0.51 克。研究结果表明，镁改性生物炭具有出色的固碳潜力，并显著提高了对磷的去除效率。

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引用次数: 0

Unveiling the competitive mechanism between SO2 and PCDD/Fs on activated carbon adsorption 揭示二氧化硫和多氯二苯并对二恶英/多氯二苯并呋喃在活性炭吸附上的竞争机制

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-25 DOI: 10.1016/j.jece.2024.114254

In municipal solid waste incineration (MSWI) plants, activated carbon (AC) adsorption is the key technique for eliminating Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) from flue gases. This research thoroughly investigates the potential competitive adsorption between SO₂ and PCDD/Fs and examines how adsorption at the center and the edge of the AC layer impacts the adsorption process. The findings show a decline in the removal efficiency of PCDD/Fs from 86.8 % to 84.2 % and further to 74.4 % when using SO₂ pre-treated (AC-A3) and H₂SO₄-impregnated (AC-B2) activated carbon, respectively. Multiple characterization methods reveal that sulfur elements occupy active sites within the inner pores of the activated carbon, reducing the availability of its pore structure, particularly affecting microporous more than mesoporous structures. DFT calculations suggest that the π-π EDA effect facilitates the adsorption of 2,3,7,8-Tetrachlorodibenzo-p-dioxin (2,3,7,8-TCDD), whereas dispersion force drive SO₂ adsorption. Comparisons among various oxygenated functional groups show that the organic acid anhydride (CO-CO) has better adsorption selectivity toward TCDD and less adsorption to SO₂. This study provides a novel perspective on the adsorption mechanisms of PCDD/Fs on AC and the competitive dynamics of sulfur in the flue gas.

在城市固体废物焚烧（MSWI）厂中，活性炭（AC）吸附是消除烟气中多氯二苯并对二恶英和多氯二苯并呋喃（PCDD/Fs）的关键技术。这项研究深入探讨了二氧化硫和多氯二苯并对二恶英和多氯二苯并呋喃（PCDD/Fs）之间潜在的竞争性吸附，并研究了 AC 层中心和边缘的吸附如何影响吸附过程。研究结果表明，使用经二氧化硫预处理（AC-A3）和 H2SO4 浸渍（AC-B2）的活性炭时，多氯二苯并对二恶英和多氯二苯并呋喃的去除率分别从 86.8% 下降到 84.2%，再进一步下降到 74.4%。多种表征方法表明，硫元素占据了活性炭内孔的活性位点，降低了其孔隙结构的可用性，尤其是对微孔结构的影响大于中孔结构。DFT 计算表明，π-π EDA 效应促进了 2,3,7,8-四氯二苯并对二恶英（2,3,7,8-TCDD）的吸附，而分散力则推动了二氧化硫的吸附。对各种含氧官能团的比较表明，有机酸酐（CO-CO）对 TCDD 具有更好的吸附选择性，而对 SO2 的吸附能力较弱。这项研究为多氯二苯并对二恶英和多氯二苯并呋喃在 AC 上的吸附机制以及烟气中硫的竞争动态提供了一个新的视角。

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引用次数: 0

The removal of pollutants from synthetic bathroom greywater by coagulation-flocculation and filtration as a fit-for-purpose method 通过混凝-絮凝和过滤去除合成浴室中水污染物的适用方法

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-25 DOI: 10.1016/j.jece.2024.114250

It has been demonstrated that treated bathroom greywater (TBGW) is a useful substitute for fresh water for non-potable applications in households. Reuse of TBGW for irrigation, toilet flushing, car washing etc. offers a good opportunity to save drinking water and meet the sustainable development goals (SDGs). In this study, synthetic bathroom greywater (SBGW) was compiled in a controlled manner and used as a substitute for bathroom GW. Detailed statistical analysis also was performed to confirm the similarity between real and synthetic BGWs. SBGW is suitable for testing efficiency of applied treatment methods. It was confirmed that coagulation–flocculation with iron(III) chloride and sand filtration was the most effective method of the tested 7 systems. The best and affordable treatment combination generates good-quality treated SBGW (TSBGW) (pH = 7.54 ± 0.29, TURB = 0.54 ± 0.49 NTU, BOD₅ = 21 ± 10 mgL⁻¹, COD = 32 ± 11 mgL⁻¹, and TOC = 12.7 ± 6.7 mgL⁻¹) for different non-potable purposes by complying with the regulated limit values for reuse. The elemental analysis of raw, TSBGW and tap water (TW) samples by MP-AES method provided further support for safe recycling. This study leads to the conclusion that the generation of TBGW by fit-for-purpose treatment can effectively meet the circular economy goals at household level. The recycling of GW is of limited importance in the European Union (EU) and legal regulations are not available in many countries. This study provides novel support for regulating the reuse of water in Eastern European countries.

实践证明，经过处理的浴室中水（TBGW）可替代淡水用于家庭非饮用水应用。将浴室中水回用至灌溉、冲厕、洗车等用途为节约饮用水和实现可持续发展目标（SDGs）提供了良机。在本研究中，我们以受控方式编制了合成浴室中水（SBGW），并将其用作浴室中水的替代品。此外，还进行了详细的统计分析，以确认真实和合成浴室中水之间的相似性。SBGW 适用于测试应用处理方法的效率。结果表明，使用氯化铁（III）进行混凝絮凝和砂滤是所测试的 7 种系统中最有效的方法。最佳且经济实惠的处理组合可产生优质的处理后 SBGW（TSBGW）（pH = 7.54 ± 0.29，TURB = 0.54 ± 0.49 NTU，BOD5 = 21 ± 10 mgL-1，COD = 32 ± 11 mgL-1，TOC = 12.7 ± 6.7 mgL-1），用于不同的非饮用水用途，符合规定的再利用限值。采用 MP-AES 方法对原水、TSBGW 和自来水 (TW) 样品进行的元素分析进一步证明了回收利用的安全性。这项研究得出的结论是，通过适合目的的处理方法产生自来水，可有效实现家庭层面的循环经济目标。在欧盟（EU），GW 回收利用的重要性有限，许多国家都没有相关的法律法规。本研究为规范东欧国家的水再利用提供了新的支持。

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引用次数: 0

Differential insights into the distribution characteristics of archaeal communities and their response to typical pollutants in the sediments and soils of deep-water reservoir 对深水水库沉积物和土壤中古生物群落分布特征及其对典型污染物反应的不同见解

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-25 DOI: 10.1016/j.jece.2024.114256

This study focused on the Fengshuba deep-water reservoir in South China, and systematically explored the distribution characteristics of archaeal communities in the sediment and soil in water level fluctuation zones and their response mechanisms to typical pollutants. The results show that Euryarchaeota and Bathyarchaeota are the dominant phyla in sediment archaeal communities, while Thaumarchaeota dominates in soil. The absolute abundance of archaea in the sediments was lower than that in the soils, but the diversity and richness of archaeal communities were higher than those in the soils. Seasonal changes affected the composition of sediment archaeal communities, and the archaeal compositions in the two habitats also showed significant differences. The neutral community model indicates that the assembly of archaeal communities in sediments is mainly governed by stochastic processes, while deterministic processes dominate in soils. The responses of archaeal communities to pollutants in the two habitats were significantly different. Among them, the carbon-nitrogen ratio and tetracycline concentration are the key factors driving seasonal changes in the archaeal communities in the sediment. Structural equation modeling further showed that the archaeal community in the sediment was positively correlated with organochlorine pesticides and antibiotics, while the archaeal community in the soil showed an opposite trend. This study provides new insights into the complexity of interactions between archaeal communities and typical contaminants in reservoir systems.

本研究以华南枫树坝深水水库为研究对象，系统探讨了水位波动区沉积物和土壤中古生物群落的分布特征及其对典型污染物的响应机制。结果表明，沉积物古菌群落的优势菌门为水螅古菌门（Euryarchaeota）和藻类古菌门（Bathyarchaeota），土壤古菌群落的优势菌门为藻类古菌门（Thaumarchaeota）。沉积物中古细菌的绝对丰度低于土壤，但古细菌群落的多样性和丰富度却高于土壤。季节变化影响了沉积物古细菌群落的组成，两种生境的古细菌组成也有显著差异。中性群落模型表明，沉积物中考古群落的形成主要受随机过程的支配，而土壤中则以确定性过程为主。两种生境中的古菌群落对污染物的反应存在显著差异。其中，碳氮比和四环素浓度是导致沉积物中古细菌群落季节性变化的关键因素。结构方程模型进一步表明，沉积物中的古菌群落与有机氯农药和抗生素呈正相关，而土壤中的古菌群落则呈现相反的趋势。这项研究为了解水库系统中古生物群落与典型污染物之间相互作用的复杂性提供了新的视角。

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引用次数: 0

Activation of peroxymonosulfate by boron nitride loaded with Co mixed oxides and boron vacancy for ultrafast removal of drugs in surface water 氮化硼负载钴混合氧化物和硼空位活化过一硫酸盐，超快去除地表水中的药物

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-24 DOI: 10.1016/j.jece.2024.114241

The mediation of vacancy in catalysts is crucial for the enhancement of oxidant activation. Here the boron nitride loaded with Co mixed oxides (Co₂O₃-CoO) and boron vacancy (B_v) catalyst (Co/BN-X) was prepared to degrade sulfamethoxazole (SMX) by activating peroxymonosulfate (PMS). Under dark condition, Co/BN-3+PMS system can completely remove SMX in surface water within 15 min, and its removal efficiency constant (0.5154 min⁻¹) was 4.0 and 6.7 times greater than those of Co/BN-2+PMS (0.1284 min⁻¹) and Co/BN-1+PMS (0.0771 min⁻¹), respectively. The system showed excellent performance in different influencing factors and cyclic experiments, and exhibited good practical application potential in secondary effluent. Electron paramagnetic resonance, radical quenching and electrochemical tests certified that singlet oxygen (¹O₂) was the major active species, followed by •O₂^–, and SO₄^•–, further elaborating the activation pathway of PMS in Co/BN-3+PMS system. The density functional theory (DFT) calculations confirmed that CoO and PMS-O₂ sites were the main reaction sites, and the existence of B_v reduced the adsorption energy of Co/BN-3 for PMS. This work reveals the synergistic effect between Co oxide sites and B_v on the catalyst surface and offers a potential modification method to accelerate Fenton-like reaction.

催化剂中空位的调解对于提高氧化剂活化至关重要。本文制备了负载钴混合氧化物（Co2O3-CoO）和硼空位（Bv）的氮化硼催化剂（Co/BN-X），通过活化过一硫酸盐（PMS）来降解磺胺甲噁唑（SMX）。在黑暗条件下，Co/BN-3+PMS 系统能在 15 分钟内完全去除地表水中的 SMX，其去除效率常数（0.5154 min-1）分别是 Co/BN-2+PMS （0.1284 min-1）和 Co/BN-1+PMS （0.0771 min-1）的 4.0 倍和 6.7 倍。该系统在不同影响因素和循环实验中均表现出优异的性能，在二级污水中具有良好的实际应用潜力。电子顺磁共振、自由基淬灭和电化学测试证明，单线态氧（1O2）是主要的活性物种，其次是-O2-和SO4--，进一步阐明了Co/BN-3+PMS体系中PMS的活化途径。密度泛函理论（DFT）计算证实，CoO 和 PMS-O2 位点是主要的反应位点，Bv 的存在降低了 Co/BN-3 对 PMS 的吸附能。这项研究揭示了催化剂表面 Co 氧化位点和 Bv 之间的协同效应，为加速 Fenton 类反应提供了一种潜在的改性方法。

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引用次数: 0

Candle soot-modified rPET electrospun nanofibrous membrane for separating on-demand oil-water mixture and emulsions 用于按需分离油水混合物和乳液的烛烟改性 rPET 电纺纳米纤维膜

IF 7.4 2区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Environmental Chemical Engineering

Pub Date : 2024-09-24 DOI: 10.1016/j.jece.2024.114235

The CS-rPET electrospun nanofibrous membrane is fabricated from recycled polyethylene terephthalate (rPET) through electrospinning and enhanced with candle soot (CS) to separate oil-water mixtures and emulsions when pre-wetted by oil or water. Using rPET polymers and CS waste reduces the environmental impact of plastic bottle waste and improves its value. The CS-rPET electrospun nanofibrous membrane showed excellent separation performance in oil-water mixtures, achieving over 81.18 % and 71.38 % of separation efficiency through 40 separation cycles after pre-wetting by oil and after washing with ethanol and pre-wetting by water, respectively. The membrane maintained high separation performance after being pre-wetted by oil for water-in-oil emulsions with efficiencies above 99 % and flux exceeding 12,200 L m⁻² h⁻¹. Similarly, the efficiencies remained above 98 % for oil-in-water emulsions after being pre-wetted by water, with a flux over 8000 L m⁻² h⁻¹. Additionally, the CS-rPET electrospun nanofibrous membrane exhibited high separation efficiencies above 97 % and flux over 14,000 L m⁻² h⁻¹ after pre-wetting by oil and 7700 L m⁻² h⁻¹ after pre-wetting by water in harsh environmental conditions. Its adaptability of switchable wettability on-demand after pre-wetting by oil or water highlights its potential for a wide range of challenging oil-water separation applications. However, multiple separation cycles, separation efficiency and flux were reduced, indicating the necessity to improve the membrane's efficiency and reduce the chance of water accumulation in multicycle separation.

CS-rPET 电纺丝纳米纤维膜是用回收的聚对苯二甲酸乙二酯（rPET）通过电纺丝制成的，并用蜡烛烟灰（CS）增强了其分离油水混合物和乳化液的能力。使用 rPET 聚合物和 CS 废弃物可减少塑料瓶废弃物对环境的影响，并提高其价值。CS-rPET 电纺纳米纤维膜在油水混合物中表现出优异的分离性能，在被油预湿、乙醇洗涤和水预湿后的 40 个分离循环中，分离效率分别达到 81.18% 和 71.38%。对于油包水型乳剂，该膜在被油预湿后仍能保持较高的分离性能，分离效率超过 99%，通量超过 12,200 升 m-2 h-1。同样，水包油型乳液在被水预湿后，分离效率仍保持在 98% 以上，通量超过 8000 升/米-2 小时-1。此外，在恶劣的环境条件下，CS-rPET 电纺纳米纤维膜在被油预湿后的分离效率高达 97 % 以上，通量超过 14,000 L m-2 h-1，在被水预湿后的通量超过 7700 L m-2 h-1。在油或水预润湿后，其可按需切换润湿性的适应性突显了其在各种具有挑战性的油水分离应用中的潜力。然而，多次分离循环后，分离效率和通量都有所降低，这表明有必要提高膜的效率，并减少多循环分离过程中的积水机会。

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