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2023 Outstanding Papers published in the Environmental Science journals of the Royal Society of Chemistry 在英国皇家化学学会《环境科学》期刊上发表 2023 篇优秀论文
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-09 DOI: 10.1039/D4EW90011A
Zongwei Cai, Neil Donahue, Graham Gagnon, Kevin C. Jones, Célia Manaia, Elsie Sunderland and Peter J. Vikesland

A graphical abstract is available for this content

本内容有图解摘要
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引用次数: 0
Thermal plasma-synthesized gray-black TiO2 with abundant oxygen vacancies for high-efficiency solar desalination† 热等离子体合成的具有丰富氧空位的灰黑色 TiO2 可用于高效太阳能海水淡化
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-06 DOI: 10.1039/D4EW00194J
Fei Li, Chang Liu, Yuanjiang Dong, Huacheng Jin, Baoqiang Li, Fei Ding and Fangli Yuan

The growing scarcity of freshwater resources has increased interest in sustainable seawater desalination methods utilizing solar radiation. Titanium dioxide (TiO2), known for its corrosion resistance and low cost, is an ideal material for photothermal applications. However, its wide bandgap limits the optimal utilization of visible and infrared light. To address this, a grey-black TiO2 material rich in oxygen vacancies was synthesized using high-frequency low-temperature plasma. This material was integrated into a three-dimensional seawater evaporator with modified polyvinylidene fluoride (PVDF) sponge and polystyrene foam. The resulting structure exhibited a broad spectral absorption profile, low thermal conductivity, and enhanced evaporation efficiency. Experimental results confirmed the effectiveness of oxygen vacancies in narrowing the TiO2 bandgap, improving light absorption and photothermal properties. In seawater desalination tests, the system achieved an impressive evaporation rate of 2.91 kg m−2 h−1 and a light-to-water evaporation efficiency of 75.52% under one sun irradiation, outperforming natural evaporation under sunlight conditions by a factor of 7.7. At the same time, the salinity of desalinated seawater significantly falls below the standard set by the World Health Organization (WHO) and even reaches levels comparable to soft water. This research offers insights for developing high-performance TiO2 photothermal materials and seawater evaporators, contributing to discussions on sustainable and efficient desalination technologies.

淡水资源日益匮乏,人们对利用太阳辐射的可持续海水淡化方法越来越感兴趣。二氧化钛(TiO2)以其耐腐蚀性和低成本而著称,是光热应用的理想材料。然而,其宽带隙限制了对可见光和红外线的最佳利用。为了解决这个问题,我们利用高频低温等离子体合成了一种富含氧空位的灰黑色二氧化钛材料。将这种材料与改性聚偏二氟乙烯(PVDF)海绵和聚苯乙烯泡沫集成到三维海水蒸发器中。由此产生的结构具有宽光谱吸收曲线、低热导率和更高的蒸发效率。实验结果证实了氧空位在缩小二氧化钛带隙、改善光吸收和光热特性方面的有效性。在海水淡化试验中,该系统的蒸发率达到了惊人的 2.91 kg m-2 h-1,在一个太阳光照射下的光-水蒸发效率为 75.52%,比日光条件下的自然蒸发效率高出 7.7 倍。同时,淡化海水的盐度大大低于世界卫生组织(WHO)规定的标准,甚至达到与软水相当的水平。这项研究为开发高性能二氧化钛光热材料和海水蒸发器提供了启示,有助于可持续和高效海水淡化技术的讨论。
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引用次数: 0
A review of modified and hybrid anaerobic baffled reactors for municipal wastewater treatment with a focus on emerging contaminants 改良型和混合型厌氧折流式反应器在城市污水处理中的应用综述,重点关注新出现的污染物
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-05 DOI: 10.1039/D3EW00822C
Poh Lin Lau and Antoine P. Trzcinski

This review discusses municipal wastewater treatment using anaerobic baffled reactors (ABRs) and modified ABRs. Conventional ABRs can convert organic carbon to renewable energy in the form of biogas. ABRs can achieve more than 90% COD removal at HRT as low as 8 hours at mesophilic temperatures, while COD removal in the range of 70–90% is typical at uncontrolled temperatures. However, effluents from ABRs do not meet discharge criteria and must be polished. Several techniques have been applied to improve the effluent quality including: pre-screening of raw wastewater using a mesh or sedimentation tank, inoculation with acclimatized sludge, effluent recirculation, electrocoagulation, microbial electrodes for improved VFA degradation, COD degradation and methane production, packing materials, carriers or meshes in individual compartments, polymeric membranes in the final compartment or external to the ABR, constructed wetlands and aerobic bioreactors. Recently, much research has focused on concurrent carbon and nitrogen removal in modified ABRs using novel strategies including microaeration, membrane aerated biofilms, an ABR followed by an aerobic membrane bioreactor with sludge recycling, anammox bacteria and nitrite/nitrate-dependent anaerobic methane oxidation bacteria. For P removal, promising chemical techniques include electrocoagulation and biological P removal includes denitrifying phosphate accumulating microorganisms. Some of these techniques applied in independent studies resulted in effluents containing <20 mg L−1 BOD, <1 mg L−1 TN and 0.2 mg L−1 TP, indicating the feasibility of mainstream anaerobic treatment of municipal wastewater, but pilot scale studies on biogas production and C, N and P removal are still lacking. Furthermore, ABRs have also been found to degrade concurrently emerging contaminants in municipal wastewater such as perchlorate, nitrophenols, and antibiotics with no effect on COD removal at typical concentrations found in municipal wastewater, but for some complex organics, an aerobic step is required for the complete oxidation.

本综述讨论了使用厌氧折流式反应器(ABR)和改进型厌氧折流式反应器处理城市污水的问题。传统厌氧沼气反应器可将有机碳转化为沼气形式的可再生能源。在嗜中温条件下,厌氧反应器的 HRT 低至 8 小时,COD 去除率可达 90% 以上,而在不受控温度条件下,COD 去除率通常在 70-90% 之间。然而,ABR 的出水不符合排放标准,必须进行抛光处理。为改善出水水质,已采用了多种技术,包括:使用网箱或沉淀池对原废水进行预筛选、接种适应性污泥、出水再循环、电凝、用于改善 VFA 降解、COD 降解和甲烷生产的微生物电极、填料、单个隔室中的载体或网箱、最后隔室中或 ABR 外部的聚合膜、建造湿地和好氧生物反应器。最近,许多研究都集中在改良型厌氧生物反应器中同时去除碳和氮,采用的新策略包括微曝气、膜充气生物膜、厌氧生物反应器后的带污泥循环的好氧膜生物反应器、厌氧细菌和依赖亚硝酸盐/硝酸盐的厌氧甲烷氧化细菌。在去除磷方面,有前景的化学技术包括电凝,而生物去除磷包括反硝化磷酸盐积累微生物。在独立研究中应用其中一些技术后,污水中的生化需氧量(BOD)为 20 毫克/升,总氮(TN)为 1 毫克/升,总磷(TP)为 0.2 毫克/升,这表明厌氧处理城市污水是可行的,但仍缺乏有关沼气生产以及碳、氮和磷去除的中试规模研究。此外,还发现厌氧生物反应器可同时降解城市污水中新出现的污染物,如高氯酸盐、硝基苯酚和抗生素,在城市污水中的典型浓度下对去除 COD 没有影响,但对于一些复杂的有机物,则需要一个好氧步骤才能完全氧化。
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引用次数: 0
Quantifying drought-driven temperature impacts on ozone disinfection credit and bromate control† 量化干旱导致的温度对臭氧消毒信用和溴酸盐控制的影响
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-05 DOI: 10.1039/D4EW00042K
Bilal Abada, Ariel J. Atkinson and Eric C. Wert

Climate change and drought can lead to unprecedented changes in surface water temperature requiring utilities to examine their ozone system's disinfection capability while minimizing bromate production. This pilot-scale study investigated temperature (15–30 °C) as a single/isolated variable affecting ozone operating performance (demand, decay rate, exposure (CT)) and the ability to achieve a Cryptosporidium log reduction value (LRV) of 0.5–1.5 logs, as defined by the United States Environmental Protection Agency (USEPA). When dosing 3.0 mg L−1 of ozone into a surface water with 2.5 mg L−1 of total organic carbon, an increase in temperature from 15 °C to 30 °C increased ozone demand in the dissolution zone from 1.0 mg L−1 to 1.6 mg L−1 (60%) and ozone decay rate from 0.07 min−1 to 0.27 min−1 (385%). Despite more rapid demand/decay, the required ozone dose to achieve an LRV of 1.5 logs remained at 2.4–2.8 mg L−1 due to the reduction in USEPA's CT requirement at higher temperatures (9.35 mg min L−1 at 15 °C vs. 2.31 mg min L−1 at 30 °C). Bromate formation exceeded the USEPA maximum contaminant level of 10 μg L−1 when ozone was dosed to achieve LRV > 0.5 log at all temperature conditions. Chlorine–ammonium pretreatment (0.5 mg L−1 Cl2, 0.1–0.5 mg L−1 NH4+-N) lowered bromate formation to <5 μg L−1 under ambient (80 μg L−1) and elevated (120 μg L−1) bromide concentrations at all temperatures. These results were applied to evaluate a full-scale ozone system designed to achieve an LRV of 1.5 logs if drought increases temperature from 13 °C to 26 °C. The study systematically examined the role of temperature on ozone system performance, which can assist utilities planning for future drought-driven changes.

气候变化和干旱会导致地表水温度发生前所未有的变化,这就要求公用事业部门在尽量减少溴酸盐产生的同时,检查臭氧系统的消毒能力。这项中试规模的研究将温度(15-30 °C)作为一个单一/独立的变量,对臭氧的运行性能(需求、衰减率、暴露(CT))以及实现美国环境保护局(USEPA)规定的 0.5-1.5 logs 的隐孢子虫对数减少值(LRV)的能力产生影响。向总有机碳含量为 2.5 毫克/升的地表水中添加 3.0 毫克/升的臭氧时,温度从 15 °C 升至 30 °C,溶解区的臭氧需求量从 1.0 毫克/升增至 1.6 毫克/升(60%),臭氧衰减率从 0.07 分钟/升增至 0.27 分钟/升(385%)。尽管需求/衰减速度更快,但实现 1.5 logs LRV 所需的臭氧剂量仍为 2.4-2.8 mg L-1,这是因为美国环保局的 CT 要求在较高温度下有所降低(15 °C 时为 9.35 mg min L-1 而 30 °C 时为 2.31 mg min L-1)。在所有温度条件下,当臭氧用量达到 LRV > 0.5 log 时,溴酸盐的形成超过了美国环保局规定的 10 μg L-1 的最大污染物含量。氯铵预处理(0.5 mg L-1 Cl2、0.1-0.5 mg L-1 NH4+-N)降低了溴酸盐的形成,在所有温度条件下,在环境(80 μg L-1)和升高(120 μg L-1)的溴化物浓度下,溴酸盐的形成均为 <5 μg L-1。这些结果被用于评估一个全面的臭氧系统,该系统的设计目的是在干旱将温度从 13 °C 提高到 26 °C 的情况下实现 1.5 logs 的 LRV。该研究系统地考察了温度对臭氧系统性能的影响,这有助于公用事业部门规划未来干旱引起的变化。
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引用次数: 0
Adsorption mechanisms of short-chain and ultrashort-chain PFAS on anion exchange resins and activated carbon† 短链和超短链 PFAS 在阴离子交换树脂和活性炭上的吸附机理
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-04 DOI: 10.1039/D3EW00959A
Swadhina P. Lenka, Melanie Kah, Jack L.-Y. Chen, Bryan Andres Tiban-Anrango and Lokesh P. Padhye

Short-chain and ultrashort-chain per-/polyfluoroalkyl substances (PFAS) have become ubiquitous in aquatic environments worldwide, and their concentrations are rising. Studies have shown adsorption on activated carbon (AC) and anion exchange resins (AERs) as efficient removal techniques for long-chain PFAS (C ≥ 8). However, limited data are available on the adsorption of short-chain PFAS (C ≤ 4), especially ultrashort-chain PFAS. In this study, isotherm experiments were conducted to elucidate the possible adsorption mechanisms of widely detected short-chain perfluorobutanesulfonic acid (PFBS) and perfluorobutanoic acid (PFBA), and ultrashort-chain perfluoropropionic acid (PFPrA) on AC and AERs. Various factors, such as adsorbate concentration and characteristics, adsorbent properties, and the water matrix, influenced the adsorption of the target compounds. At concentrations > 1 mg L−1, strong base AER (A900) displayed the highest adsorption affinity among the four adsorbents investigated. An average 20 times decrease in the adsorption of three PFAS in the presence of competing CaCl2 salt affirmed the importance of ionic interactions. In contrast, both ionic interactions and hydrophobic interactions were equally important at concentrations < 1 mg L−1 for adsorption on AER and AC. The higher dipole moment of PFBS could be responsible for its higher adsorption on AERs compared to PFPrA and PFBA, while PFBS's greater adsorption on AC could be attributed to hydrophobic partitioning, which was supported by the calculated Langmuir and Freundlich model parameters. The isotherm data also suggested adsorption through additional mechanisms(s), which could include negative charge-assisted hydrogen bonds between PFBA and AC functional groups. Among the three short-chain PFAS, PFPrA exhibited the least adsorption and maximum desorption irrespective of the adsorbent type and adsorbate concentrations. Overall, our results suggest that AERs and ACs can be used to remove short-chain PFBA and PFBS through electrostatic and non-electrostatic interactions. This implies that an adsorption treatment train consisting of a series of stages, each targeting different interaction mechanisms, is needed to remove a wide range of PFAS.

短链和超短链过/聚氟烷基物质(PFAS)在全球水生环境中无处不在,其浓度也在不断上升。研究表明,活性炭 (AC) 和阴离子交换树脂 (AER) 吸附是去除长链 PFAS(C ≥ 8)的有效技术。然而,关于短链 PFAS(C ≤ 4),尤其是超短链 PFAS 的吸附数据却很有限。本研究进行了等温线实验,以阐明广泛检测到的短链全氟丁烷磺酸(PFBS)和全氟丁酸(PFBA)以及超短链全氟丙酸(PFPrA)在 AC 和 AER 上的可能吸附机理。吸附剂的浓度和特性、吸附剂的性质以及水基质等各种因素都会影响目标化合物的吸附。在浓度为 1 mg L-1 时,强碱 AER(A900)在四种吸附剂中显示出最高的吸附亲和力。在有 CaCl2 盐竞争的情况下,三种全氟辛烷磺酸的吸附量平均降低了 20 倍,这证明了离子相互作用的重要性。相反,在浓度为 1 mg L-1 时,离子相互作用和疏水相互作用对 AER 和 AC 的吸附同样重要。与 PFPrA 和 PFBA 相比,PFBS 的偶极矩更高,这可能是其在 AER 上吸附量更大的原因,而 PFBS 在 AC 上的吸附量更大可能是由于疏水分配作用,这一点得到了计算的 Langmuir 和 Freundlich 模型参数的支持。等温线数据还表明吸附是通过其他机制进行的,其中可能包括 PFBA 和 AC 官能团之间的负电荷辅助氢键。在三种短链 PFAS 中,无论吸附剂类型和吸附剂浓度如何,PFPrA 的吸附量最小,解吸量最大。总之,我们的研究结果表明,AER 和 AC 可通过静电和非静电相互作用来去除短链 PFBA 和 PFBS。这意味着,要想去除各种全氟辛烷磺酸,就必须采用由一系列阶段(每个阶段针对不同的相互作用机制)组成的吸附处理系统。
{"title":"Adsorption mechanisms of short-chain and ultrashort-chain PFAS on anion exchange resins and activated carbon†","authors":"Swadhina P. Lenka, Melanie Kah, Jack L.-Y. Chen, Bryan Andres Tiban-Anrango and Lokesh P. Padhye","doi":"10.1039/D3EW00959A","DOIUrl":"10.1039/D3EW00959A","url":null,"abstract":"<p >Short-chain and ultrashort-chain per-/polyfluoroalkyl substances (PFAS) have become ubiquitous in aquatic environments worldwide, and their concentrations are rising. Studies have shown adsorption on activated carbon (AC) and anion exchange resins (AERs) as efficient removal techniques for long-chain PFAS (C ≥ 8). However, limited data are available on the adsorption of short-chain PFAS (C ≤ 4), especially ultrashort-chain PFAS. In this study, isotherm experiments were conducted to elucidate the possible adsorption mechanisms of widely detected short-chain perfluorobutanesulfonic acid (PFBS) and perfluorobutanoic acid (PFBA), and ultrashort-chain perfluoropropionic acid (PFPrA) on AC and AERs. Various factors, such as adsorbate concentration and characteristics, adsorbent properties, and the water matrix, influenced the adsorption of the target compounds. At concentrations &gt; 1 mg L<small><sup>−1</sup></small>, strong base AER (A900) displayed the highest adsorption affinity among the four adsorbents investigated. An average 20 times decrease in the adsorption of three PFAS in the presence of competing CaCl<small><sub>2</sub></small> salt affirmed the importance of ionic interactions. In contrast, both ionic interactions and hydrophobic interactions were equally important at concentrations &lt; 1 mg L<small><sup>−1</sup></small> for adsorption on AER and AC. The higher dipole moment of PFBS could be responsible for its higher adsorption on AERs compared to PFPrA and PFBA, while PFBS's greater adsorption on AC could be attributed to hydrophobic partitioning, which was supported by the calculated Langmuir and Freundlich model parameters. The isotherm data also suggested adsorption through additional mechanisms(s), which could include negative charge-assisted hydrogen bonds between PFBA and AC functional groups. Among the three short-chain PFAS, PFPrA exhibited the least adsorption and maximum desorption irrespective of the adsorbent type and adsorbate concentrations. Overall, our results suggest that AERs and ACs can be used to remove short-chain PFBA and PFBS through electrostatic and non-electrostatic interactions. This implies that an adsorption treatment train consisting of a series of stages, each targeting different interaction mechanisms, is needed to remove a wide range of PFAS.</p>","PeriodicalId":75,"journal":{"name":"Environmental Science: Water Research & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595151","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Removal of phosphorus and fluorine from wastewater containing PF6−via accelerated decomposition by Al3+ and chemical precipitation for hydrometallurgical recycling of lithium-ion batteries† 通过 Al3+ 加速分解和化学沉淀去除含 PF6- 废水中的磷和氟,用于锂离子电池的湿法冶金循环利用
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-02 DOI: 10.1039/D3EW00854A
Takuto Miyashita, Kouji Yasuda and Tetsuya Uda

During hydrometallurgical recycling of lithium-ion batteries (LIBs), one important challenge is the efficient treatment of wastewater containing LiPF6 used as a lithium salt in the LIBs. The difficulty of the treatment is attributed to the persistence of PF6 in aqueous solutions. In this study, the accelerated decomposition of PF6 by Al3+ at an elevated temperature and the removal of phosphorus and fluorine by chemical precipitation were attempted. These reactions were analyzed using a pH electrode and fluoride-ion selective electrode, and by a distillation method for total fluorine analysis, ICP-AES, ion chromatography, XRD, and WDS. The results showed that when 10 mM LiPF6 aqueous solution containing 100 mM Al2(SO4)3 was kept at 90 °C for 24 h, more than 90% of the PF6 was decomposed into PO43− and F. The produced PO43− and F were coprecipitated with Ca6Al2(SO4)3(OH)12 (ettringite) by adding sufficient Ca(OH)2. The concentrations of the total phosphorus and total fluorine in the supernatant after precipitation were 0.028 mM and 0.77 mM, respectively. Here, the pH after the decomposition of 10 mM PF6 decreases to around 1 due to the formation of H+ during the decomposition, which may be too low for some practical cases. For this problem, the decomposition of PF6 in various pre-mixed solutions of Al2(SO4)3 and Ca(OH)2 was also examined. As a result, when the prepared molar ratio was Al/Ca > 2/3, the decomposition of PF6 proceeded, and the pH decrease accompanying the decomposition was alleviated due to the buffer effect of the Al(OH)3 precipitate.

在锂离子电池(LIB)的湿法冶金回收过程中,一个重要的挑战是如何有效处理含有用作锂离子电池锂盐的 LiPF6 的废水。处理困难的原因在于 PF6- 在水溶液中的持久性。在本研究中,尝试在高温下用 Al3+ 加速分解 PF6-,并通过化学沉淀去除磷和氟。使用 pH 电极和氟离子选择电极,并通过蒸馏法进行总氟分析、ICP-AES、离子色谱法、XRD 和 WDS 对这些反应进行了分析。结果表明,当含有 100 mM Al2(SO4)3 的 10 mM LiPF6 水溶液在 90 °C 下保持 24 小时后,90% 以上的 PF6- 分解为 PO43- 和 F-。加入足量的 Ca(OH)2 后,生成的 PO43- 和 F- 与 Ca6Al2(SO4)3(OH)12(蚀变石)共沉淀。沉淀后上清液中总磷和总氟的浓度分别为 0.028 mM 和 0.77 mM。在这里,10 mM PF6- 分解后的 pH 值因分解过程中形成的 H+ 而降至 1 左右,这对于某些实际情况来说可能太低。针对这一问题,我们还研究了 PF6- 在 Al2(SO4)3 和 Ca(OH)2 的各种预混合溶液中的分解情况。结果表明,当配制的摩尔比为 Al/Ca > 2/3 时,PF6- 的分解继续进行,并且由于 Al(OH)3 沉淀的缓冲作用,伴随分解而来的 pH 值下降得到了缓解。
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引用次数: 0
Upcycling of plastic membrane industrial scraps and reuse as sorbent for emerging contaminants in water† 塑料膜工业下脚料的升级再循环和作为吸附剂用于水中新污染物的再利用
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-02 DOI: 10.1039/D3EW00900A
Sara Khaliha, Francesca Tunioli, Luca Foti, Antonio Bianchi, Alessandro Kovtun, Tainah Dorina Marforio, Massimo Zambianchi, Cristian Bettini, Elena Briñas, Ester Vázquez, Letizia Bocchi, Vincenzo Palermo, Matteo Calvaresi, Maria Luisa Navacchia and Manuela Melucci

Scraps obtained as waste of the industrial production of polysulfone and polysulfone–graphene oxide hollow fiber membranes (PSU-HF and PSU–GO-HF, respectively) were converted into granular materials and used as sorbents of several classes of emerging and standard water contaminants, such as drugs, heavy metal ions, and a mixture of per- and poly-fluoroalkyl substances (PFASs). The millimetric sized granules (PSU and PSU–GO, respectively) outperformed granular activated carbon (GAC), the industrial sorbent benchmark, in the adsorption of lead, diclofenac, and PFOA from tap water. Adsorption mechanism insight was achieved by molecular dynamics simulations, demonstrating the key role of graphene oxide (GO) on PSU–GO material performance. With respect to GAC, PSU–GO adsorption capacity was two times higher for diclofenac and PFOA and ten times higher for lead. Material safety was assessed by surface enhanced Raman spectroscopy, excluding GO nanosheets leaching, and combined potability test. Overall, our work proves that scrap conversion and reuse is a valuable strategy to reduce plastic industrial waste disposal and to integrate standard technology for enhanced water purification.

将聚砜和聚砜-氧化石墨烯中空纤维膜(分别为 PSU-HF 和 PSU-GO-HF)工业生产过程中产生的废料转化为颗粒材料,并将其用作几类新型和标准水污染物(如药物、重金属离子以及全氟和多氟烷基物质混合物)的吸附剂。在吸附自来水中的铅、双氯芬酸和全氟辛烷磺酸方面,毫米级颗粒(分别为 PSU 和 PSU-GO)的性能优于工业吸附剂基准颗粒活性炭(GAC)。分子动力学模拟深入揭示了吸附机理,证明了氧化石墨烯(GO)对 PSU-GO 材料性能的关键作用。与 GAC 相比,PSU-GO 对双氯芬酸和全氟辛酸的吸附能力高出两倍,对铅的吸附能力高出十倍。通过表面增强拉曼光谱、排除 GO 纳米片浸出和综合可饮用性测试,对材料的安全性进行了评估。总之,我们的工作证明,废料的转化和再利用是减少塑料工业废物处理和整合标准技术以提高水净化效果的重要策略。
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引用次数: 0
New insights into the iodination mechanism of tyrosine and its dipeptides and comparison with chlorination and bromination reactions† 酪氨酸及其二肽碘化机制的新见解以及与氯化和溴化反应的比较
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-04-01 DOI: 10.1039/D4EW00062E
Yue Qiu, Yong Dong Liu and Rugang Zhong

Iodinated aromatic disinfection byproducts have attracted much attention owing to their high toxicity. However, little has been known about the iodination mechanism to date. In this study, the iodination of model aromatic precursors, tyrosine (Tyr) and its model dipeptides, by HOI and other iodinating agents was explored using a quantum chemical computational method, and the halogenation of Tyr by HOX (X = Cl, Br, and I) was compared. The results indicate that the phenolate salt plays a key role in the iodination of the phenol ring in Tyr compounds by HOI via the classic SEAr mechanism and the second deprotonation becomes the rate-limiting step, which explains why the kinetic isotope effect (KIE) was observed in the iodination of aromatic compounds. Among the seven possible iodinating agents present in chloramination, HOI is the predominant one, and I2 is the second in the iodination of the phenol ring under typical chloramination conditions. In the further investigation of bromination and chlorination, the KIE was found to also occur in the bromination of Tyr. More importantly, the different reactivity orders of HOX reacting with the phenol ring and the amino group in Tyr are related to the hardness of both HOX and substrates, which can be evaluated from the energy gap (ELUMO–HOMO) between the LUMO and HOMO energies. Following the “like–attracts–like” principle, the halogenating agent prefers the substrate with a similar ELUMO–HOMO value. The results are helpful in further understanding the iodination mechanism and identifying various halogenated products.

碘化芳香族消毒副产物因其毒性高而备受关注。但迄今为止,人们对其碘化机理知之甚少。本研究采用量子化学计算方法探讨了 HOI 和其他碘化剂对芳香族前体模型酪氨酸(Tyr)及其模型二肽的碘化作用,并比较了 HOX(X = Cl、Br 和 I)对 Tyr 的卤化作用。结果表明,HOI 通过经典的 SEAr 机制对 Tyr 化合物中的苯酚环进行碘化时,酚盐起着关键作用,第二去质子化成为限速步骤,这也解释了为什么在芳香化合物的碘化过程中会出现动力学同位素效应(KIE)。在氯化反应中可能存在的七种碘化剂中,HOI 是主要的碘化剂,而 I2 则是在典型氯化反应条件下苯酚环碘化反应的第二种碘化剂。在溴化和氯化的进一步研究中,发现 KIE 也出现在 Tyr 的溴化反应中。更重要的是,HOX 与苯酚环和 Tyr 中的氨基反应的不同反应顺序与 HOX 和底物的硬度有关,这可以通过 LUMO 和 HOMO 能量之间的能隙(ELUMO-HOMO)来评估。根据 "同类相吸 "原理,卤化剂偏爱 ELUMO-HOMO 值相似的基底。这些结果有助于进一步了解碘化机理和确定各种卤化产物。
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引用次数: 0
Phosphate-binding protein-loaded iron oxide particles: adsorption performance for phosphorus removal and recovery from water† 磷酸盐结合蛋白负载氧化铁颗粒:用于去除和回收水中磷的吸附性能
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-03-28 DOI: 10.1039/D4EW00052H
Faten B. Hussein, Andrew H. Cannon, Justin M. Hutchison, Christopher B. Gorman, Yaroslava G. Yingling and Brooke K. Mayer

Adsorbents featuring high-affinity phosphate-binding proteins (PBPs) have demonstrated highly selective and rapid phosphorus removal and recovery. While immobilized PBP is promising for inorganic phosphate (orthophosphate, Pi) removal and recovery, increased adsorption capacity of PBP-based materials is essential to enhance the feasibility of PBP for scaled implementation. Here, magnetic n-hydroxy succinimide (NHS)-activated iron oxide particles (IOPs) were used to immobilize PBP (PBP–IOPs). The PBP–IOPs provided rapid Pi removal, with more than 95% adsorption within 5 min. Slightly acidic pH, room temperature (20 °C), and low ionic strength (0.01 M KCl) demonstrated the best removal efficiency. The Pi adsorption capacity of PBP–IOPs was not affected by anions such as chloride, sulfate, nitrate, bicarbonate, and borate. PBP–IOPs released 99% of total adsorbed Pi using pH adjustment. Conjugation of PBP to higher surface area per mass IOPs increased Pi attachment capacity (0.044 mg g−1) relative to previous studies of PBP immobilized on Sepharose resin (0.0062 mg g−1). Accordingly, PBP–IOPs have the potential to rapidly, spontaneously, selectively, and reversibly capture Pi. Theoretical capacity calculations indicated that parallel improvements in surface area to mass ratio of the base immobilization material together with reducing the size of the Pi-binding amino acid sequence (while retaining Pi specificity) are needed to further advance design and implementation of PBP-based adsorbents.

具有高亲和力磷酸盐结合蛋白(PBPs)的吸附剂已证明具有高度选择性并能快速除磷和回收磷。虽然固定化 PBP 在无机磷酸盐(正磷酸盐,Pi)的去除和回收方面前景广阔,但要提高 PBP 材料的吸附能力,就必须增强其规模化应用的可行性。在这里,磁性正羟基琥珀酰亚胺(NHS)活化氧化铁颗粒(IOPs)被用来固定 PBP(PBP-IOPs)。PBP-IOPs 能够快速去除 Pi,5 分钟内吸附率超过 95%。微酸性 pH 值(6)、室温(20 ℃)和低离子强度(0.01 M KCl)条件下的去除效率最佳。PBP-IOPs 的π吸附能力不受氯化物、硫酸盐、硝酸盐、碳酸氢盐和硼酸盐等阴离子的影响。通过调节 pH 值,PBP-IOPs 释放了总吸附量的 99%。与之前研究的固定在 Sepharose 树脂上的 PBP(0.0062 mg g-1)相比,将 PBP 连接到表面积更大的 IOPs 增加了π的吸附能力(0.044 mg g-1)。因此,PBP-IOPs 具有快速、自发、选择性和可逆地捕获 Pi 的潜力。理论容量计算表明,要进一步推进基于 PBP 的吸附剂的设计和实施,需要同时改进基底固定材料的表面积与质量比,并减少 Pi 结合氨基酸序列的大小(同时保留 Pi 特异性)。
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引用次数: 0
Geochemistry, health risk assessment and statistical source identification of dissolved trace elements in surface water of the Chishui River, China 中国赤水河地表水溶解微量元素的地球化学、健康风险评估和统计源识别
IF 5 4区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-03-28 DOI: 10.1039/D3EW00740E
Xiwei Song, Liqiang Chao, Xutao Jiang, Kejia Liu and Xunchi Pu

As the most famous wine industry area in China, the concentration of dissolved trace elements (DTEs) in surface water of the Chishui River has attracted attention. Ten DTEs including Li, V, Cr, Mn, Fe, Ni, As, Cd, Tl and Pb in surface water were determined from five specific sampling sites in the Chishui River. The concentrations of DTEs were between 0.001 μg L−1 and 77.6 μg L−1. The DTEs showed a different spatial distribution. Among the ten DTEs, the average concentration of Fe at five sites was the highest (39.2 μg L−1). The results indicated that the concentrations of ten DTEs in the Chishui River were within the allowed standard of safe water guidelines, and at a lower level compared with most rivers in China. The hazard quotient (HQ) and the hazard index (HI) value levels of the ten DTEs in all sampling sites did not exceed the acceptable risk limits of non-carcinogenic value. Adults are less sensitive to the risks than children, and oral intake was the primary exposure pathway. Pearson's correlation analysis, principal component analysis (PCA), and cluster analysis (CA) indicated that V, Cr, Fe and Pb were mainly derived from the parent material of soil, geochemical action and various municipal wastewater. The sources of Li, As, and Tl were closely related to municipal and industrial wastewater. Mn, Ni and Cd were mainly derived from agricultural non-point sources.

赤水河作为中国最知名的葡萄酒产区,其地表水中溶解性微量元素(DTEs)的浓度一直备受关注。在赤水河五个特定采样点测定了地表水中 Li、V、Cr、Mn、Fe、Ni、As、Cd、Tl 和 Pb 等 10 种 DTEs。DTEs 的浓度在 0.001µg /L 至 77.6µg /L 之间。DTEs 呈现出不同的空间分布。在 10 种 DTEs 中,5 个地点的铁平均浓度最高(39.2µg /L)。结果表明,赤水河中 10 种 DTE 的浓度均在安全水准则允许的标准范围内,与中国大多数河流相比处于较低水平。所有采样点中 10 种 DTEs 的危害商数 (HQ) 和危害指数 (HI) 值水平均未超过非致癌的可接受风险限值。成人对风险的敏感度低于儿童,口服是主要的暴露途径。皮尔逊相关分析、主成分分析和聚类分析表明,钒、铬、铁和铅主要来源于土壤母质、地球化学作用和各种城市污水。锂、砷和钛的来源与城市和工业废水密切相关。锰、镍和镉主要来自农业非点源。
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引用次数: 0
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Environmental Science: Water Research & Technology
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