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Dynamic modulation of separation performance in electrically conductive polyamide membranes with scalable fabrication potential 具有可扩展制造潜力的导电聚酰胺膜分离性能的动态调制
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-22 DOI: 10.1038/s41545-025-00478-y
Haya Nassrullah, Sandra Aristizabal, Jamaliah Aburabie, Nidal Hilal, Raed Hashaikeh

Polyamide is the most commonly used selective layer in nanofiltration membranes at an industrial scale. However, polyamide membranes lack flexibility, as their performance in terms of rejection and flux becomes fixed once the membrane is formed. Although several studies have explored during- and post-fabrication modifications of polyamide membranes, these approaches result in irreversible changes to membrane properties. Herein, we developed an electrically conductive polyamide membrane with dynamically tunable salt rejection performance by applying external positive or negative potentials. The observed changes in membrane performance were reversible, indicating that the chemical and structural integrity of the membrane is maintained. Furthermore, unlike findings from previous studies, the salt rejection performance of this membrane remains uncompromised even at voltages that induce electrochemical reactions. These results highlight the potential of this membrane for adaptive filtration systems and applications requiring electrochemical reactions without sacrificing separation efficiency.

聚酰胺是工业规模纳滤膜中最常用的选择层。然而,聚酰胺膜缺乏柔韧性,因为一旦膜形成,它们在排斥和通量方面的性能就会固定。虽然已经有一些研究探索了聚酰胺膜在制造过程中和制造后的修饰,但这些方法会导致膜性质的不可逆变化。在此,我们开发了一种导电聚酰胺膜,该膜通过施加外部正或负电位来动态调节盐的抑制性能。观察到的膜性能变化是可逆的,表明膜的化学和结构的完整性是保持的。此外,与以前的研究结果不同,即使在诱发电化学反应的电压下,这种膜的盐排斥性能仍然不受影响。这些结果突出了这种膜在自适应过滤系统和需要电化学反应而不牺牲分离效率的应用中的潜力。
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引用次数: 0
A framework for tracing the sources of nitrate in surface water through remote sensing data coupled with machine learning 通过结合机器学习的遥感数据追踪地表水中硝酸盐来源的框架
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-21 DOI: 10.1038/s41545-025-00473-3
Di Tian, Xinfeng Zhao, Lei Gao, Tao Jiang, Zuobing Liang, Zaizhi Yang, Pengcheng Zhang, Qirui Wu, Kun Ren, Chenchen Yang, Rui Li, Shaoheng Li, Yingjie Cao, Yingxue Xuan, Jianyao Chen, Aiping Zhu

As an integral component of the global nitrogen cycle, nitrate are readily transferred from urban sewage discharge, agricultural activities, and atmospheric sedimentation to surface water. This paper introduces an innovative framework that combines multi-source remote sensing technology with stable nitrate nitrogen (δ15N-NO3) and oxygen (δ18O-NO3) isotopes mixing model, to identify nitrate sources quantitatively in surface water for the first time (R2 range from 0.50 to 0.99, RMSE range from 0.05‰ to 2.31‰, MAE range from 0.03‰ to 1.35‰). By reconstructing the historical nitrate isotopes from 2006 to 2023, we found that manure and sewage were the main contributing sources, followed by soil nitrogen, fertilizer and atmospheric deposition (contribution ratio of 3.5:2.5:2.5:1.5), wastewater discharge and fertilizer application in Xijiang river had a significant impact on this. This framework fills a gap in the research pertaining to remote sensing technology’s identification of surface nitrate sources, facilitating straightforward and user-friendly forecasting of nitrate source spatio-temporal sequences.

作为全球氮循环的一个组成部分,硝酸盐很容易从城市污水排放、农业活动和大气沉降转移到地表水中。采用多源遥感技术与稳定硝态氮(δ15N-NO3−)和氧(δ18O-NO3−)同位素混合模型相结合的创新框架,首次对地面水硝酸盐源进行了定量识别(R2范围为0.50 ~ 0.99,RMSE范围为0.05‰~ 2.31‰,MAE范围为0.03‰~ 1.35‰)。通过对2006 ~ 2023年历史硝酸盐同位素的重建,发现西江流域土壤氮、肥料和大气沉降对西江流域硝酸盐的贡献最大,贡献比分别为3.5:2.5:2.5:1.5,其中西江流域污水排放和化肥施用对西江流域硝酸盐的贡献影响显著。该框架填补了遥感技术在地表硝酸盐源识别研究中的空白,促进了对硝酸盐源时空序列的直接和用户友好的预测。
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引用次数: 0
FeIII-driven self-cycled Fenton via contact-electro-catalysis for water purification 接触式电催化驱动的自循环Fenton净水技术
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-20 DOI: 10.1038/s41545-025-00476-0
Dongmei Ma, Jin Zhang, Wei Li, Jinxing Ma, Kuanchang He, Kui Yang, Jianghu Cui, Qian Liu, Sihao Lv, Min Zhang, Faliang Cheng, Defeng Xing

While self-cycled Fenton (SC-Fenton) systems represent an innovative advancement in water purification technologies, their practical implementation remains constrained by inefficient in situ H2O2 generation. To address this limitation, we developed a mechano-driven contact-electro-catalysis (CEC) platform employing fluorinated ethylene propylene (FEP) as a triboelectric catalyst. Under ultrasound irradiation, this system achieves an exceptional H2O2 generation rate of 7.67 mmol·gcat–1·h–1, outperforming conventional piezo-catalysis systems. Mechanistic studies reveal that a built interfacial electric field generated on the FEP surface effectively reduces the free energy for the indirect 2e water oxidation pathway. This unique characteristic promotes the generation of interfacial hydroxyl radical (*OH) and enhances its subsequent recombination into H2O2. The strategic integration of FeIII as a catalytic initiator with the CEC system enables the establishment of SC-Fenton reaction (FeIII/FEP/CEC). Notably, the contact-electrification electrons accumulated on the FEP interface drive efficient FeIII/FeII redox cycling, achieving a remarkable degradation rate for sulfadiazine at 0.125 min–1. This enhanced catalytic performance stems from FeIII-mediated amplification of dissociative hydroxyl radical (OH) generation. This study provides fundamental insights into the underlying mechanisms of CEC-mediated FeIII-initiated SC-Fenton reaction, offering new possibilities for sustainable water purification processes.

虽然自循环Fenton (SC-Fenton)系统代表了水净化技术的创新进步,但其实际实施仍然受到原位H2O2生成效率低下的限制。为了解决这一限制,我们开发了一种机械驱动的接触电催化(CEC)平台,采用氟化乙丙烯(FEP)作为摩擦电催化剂。在超声照射下,该体系H2O2生成速率为7.67 mmol·gcat-1·h-1,优于传统的压电催化体系。机理研究表明,在FEP表面产生的内置界面电场有效地降低了间接氧化途径的自由能。这种独特的特性促进了界面羟基自由基(*OH)的生成,并促进了其随后重组为H2O2。FeIII作为催化引发剂与CEC体系的战略性整合,使SC-Fenton反应(FeIII/FEP/CEC)得以建立。值得注意的是,积累在FEP界面上的接触通电电子驱动了FeIII/FeII的高效氧化还原循环,在0.125 min-1的时间内实现了对磺胺嘧啶的显著降解速率。这种增强的催化性能源于fei介导的离解羟基自由基(•OH)生成的扩增。该研究为cec介导的feii引发的SC-Fenton反应的潜在机制提供了基础见解,为可持续水净化工艺提供了新的可能性。
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引用次数: 0
Technology status to treat PFAS-contaminated water and limiting factors for their effective full-scale application pfas污染水体处理技术现状及制约其有效全面应用的因素
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-15 DOI: 10.1038/s41545-025-00457-3
C. S. Tshangana, S. T. Nhlengethwa, S. Glass, S. Denison, A. T. Kuvarega, T. T. I. Nkambule, B. B. Mamba, Pedro J. J. Alvarez, A. A. Muleja

Per- and polyfluoroalkyl substances (PFAS) are a class of synthetic chemicals that are highly resistant to degradation because of the strong C-F bond and their unique physico-chemical properties. Several techniques, both destructive and non-destructive, have been explored for removing PFAS from contaminated water. However, the most desirable techniques, ideally capable of effective separation and complete PFAS destruction and mineralization, have not progressed beyond bench-scale testing. This paper provides an overview of the existing treatment techniques demonstrated at laboratory, pilot, and industrial scales, and their associated treatment mechanisms. Insufficient data on pilot-scale and full-scale applications for PFAS remediation has limited the optimization and advancement of these systems at a large scale. Most research related to PFAS-remediation is based on laboratory-scale studies under ideal conditions that do not represent the complexity of PFAS-contaminated media. Factors such as inhibition by competing background compounds and secondary water or air pollution limit the application of some PFAS removal techniques at full-scale. Additionally, high energy intensity, cost, and inappropriate reactor design restrict the scalability of some proposed innovations. Here, we propose integrated systems and treatment trains as potential approaches to effectively remove and destroy PFAS from contaminated waters. This review also offers and contextualizes implementation barriers and scalable approaches for PFAS treatment.

全氟烷基和多氟烷基物质(PFAS)是一类合成化学品,由于其强大的C-F键和独特的物理化学性质,具有高度耐降解性。已经探索了几种从受污染的水中去除PFAS的技术,包括破坏性和非破坏性技术。然而,最理想的技术,理想地能够有效分离和完全的PFAS破坏和矿化,还没有超出实验规模的测试。本文概述了在实验室、中试和工业规模上展示的现有处理技术及其相关的处理机制。PFAS修复的中试规模和全面应用数据不足,限制了这些系统的大规模优化和进步。大多数与pfas修复相关的研究都是在理想条件下进行的实验室规模的研究,并不代表pfas污染介质的复杂性。竞争背景化合物的抑制作用和二次水或空气污染等因素限制了某些PFAS去除技术的全面应用。此外,高能量强度、成本和不适当的反应堆设计限制了一些拟议创新的可扩展性。在这里,我们提出了综合系统和处理系统作为有效去除和破坏污染水中PFAS的潜在方法。本综述还提供了PFAS治疗的实施障碍和可扩展的方法。
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引用次数: 0
Simultaneous adsorption of organic phosphonate and orthophosphate from municipal sewage on nanoparticle Fe3O4 with molecular simulation 纳米颗粒Fe3O4同时吸附城市污水中的有机磷酸盐和正磷酸盐的分子模拟
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-14 DOI: 10.1038/s41545-025-00453-7
Yubo Liu, Min Yao, Zhihao Jin, Yun Zhang

Organic and inorganic phosphonates often co-exist in municipal sewage, and it is a challenge to remove them simultaneously. Nanoparticle Fe3O4 (Fe3O4 NPs) has attracted significant attention due to its high adsorption activity, low cost, environmental friendliness, and magnetic separation. Herein, the adsorption performance and mechanism of hydroxyethylidene diphosphonic acid (HEDP) and orthophosphate (PO43−) onto Fe3O4 NPs were systematically investigated. When the dosages were 0.4 g/L, the removal efficiencies of HEDP and PO₄³ reached 96.3% and 95.1%, respectively. pH had no significant impact on the adsorption, whereas the presence of HCO3/CO32− markedly suppressed the removal of HEDP and PO43−. The adsorption of HEDP and PO43− onto Fe3O4 NPs conformed to the pseudo-second-order kinetics and Langmuir isotherm models in single and binary P systems. HEDP consistently inhibited the removal of PO43− in the binary P system. The adsorption mechanisms were primarily driven by the combined effect of electrostatic attraction, hydrogen bonding, and coordination complexation. DFT molecular simulation showed higher adsorption energy between HEDP and Fe3O4 NPs, and the simulation outcomes were in excellent agreement with the experimental data. Although the adsorption of HEDP and PO43− was competitive, total phosphorus in the effluent of municipal sewage could still meet the discharge standard.

有机磷酸盐和无机磷酸盐在城市污水中经常共存,同时去除它们是一个挑战。纳米颗粒Fe3O4 (Fe3O4 NPs)因其高吸附活性、低成本、环境友好、可磁分离等优点而受到广泛关注。本文系统地研究了羟乙基二膦酸(HEDP)和正磷酸盐(PO43−)在Fe3O4 NPs上的吸附性能和机理。当投加量为0.4 g/L时,对HEDP和po_4³−的去除率分别达到96.3%和95.1%。pH对吸附无显著影响,而HCO3−/CO32−的存在显著抑制了HEDP和PO43−的去除。HEDP和PO43−在Fe3O4 NPs上的吸附符合准二级动力学和Langmuir等温模型。在二元P体系中,HEDP持续抑制PO43−的去除。吸附机理主要由静电吸引、氢键和配位络合共同作用驱动。DFT分子模拟显示HEDP与Fe3O4 NPs之间具有较高的吸附能,模拟结果与实验数据吻合良好。虽然对HEDP和PO43−的吸附存在竞争,但城市污水出水中总磷仍能满足排放标准。
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引用次数: 0
Enhanced remediation of actual dye wastewater by hydrogenated bimetallic MOF derivative with active peracetic acid 活性过氧乙酸加氢双金属MOF衍生物对实际染料废水的强化修复
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-12 DOI: 10.1038/s41545-025-00465-3
Shengmei Tan, Liuwei Zhang, Zhiliang Cheng, Yuxin Peng, Jinshan Tang, Hongrui Zhu, Facheng Qiu

This study introduces a hydrogenated FeCo-MOF derivative catalyst (HC-FeCo@C350) to activate peracetic acid (PAA) for efficient degradation dye wastewater. Rhodamine B (RhB) as a model pollutant, the HC-FeCo@C350/PAA achieved a 99.33% removal efficiency within 20 min, with a rate constant 18 times higher than the non-hydrogenated system. Liquid chromatography-mass spectrometry (LC-MS) and the toxicity evaluation software (T.E.S.T.) confirmed reduced intermediate toxicity. Quenching experiments, electron paramagnetic resonance (EPR) tests, and density functional theory (DFT) calculation show that HC-FeCo@C350 can effectively activate PAA to produce 1O2, CH3C(O)O•, and CH3C(O)OO•. The magnetically recoverable catalyst maintained over 80% efficiency after 4 cycles. In actual dye wastewater treatment, the RE of chemical oxygen demand (COD), ammonia nitrogen (NH3-N), total nitrogen (TN), total phosphorus (TP) could reach approximately 53.57%, 53.23%, 29.25%, 19.2%, respectively, with reduced toxicity validated by mungbean germination experiment. This technology offers a promising approach for refractory dye wastewater treatment and reuse.

本研究介绍了一种氢化FeCo-MOF衍生物催化剂(HC-FeCo@C350),用于活化过氧乙酸(PAA)高效降解染料废水。以罗丹明B (Rhodamine B, RhB)为模型污染物,HC-FeCo@C350/PAA在20 min内的去除率达到99.33%,比非氢化体系的去除率高18倍。液相色谱-质谱(LC-MS)和毒性评价软件(T.E.S.T.)证实了中间毒性降低。淬火实验、电子顺磁共振(EPR)测试和密度泛函数理论(DFT)计算表明,HC-FeCo@C350能有效活化PAA生成1O2、CH3C(O)O•和CH3C(O)OO•。经过4次循环后,磁性可回收催化剂的效率保持在80%以上。在实际染料废水处理中,化学需氧量(COD)、氨氮(NH3-N)、总氮(TN)、总磷(TP)的RE分别可达53.57%、53.23%、29.25%、19.2%左右,通过绿豆萌发试验验证其毒性降低。该技术为难降解染料废水的处理和回用提供了一条有前景的途径。
{"title":"Enhanced remediation of actual dye wastewater by hydrogenated bimetallic MOF derivative with active peracetic acid","authors":"Shengmei Tan, Liuwei Zhang, Zhiliang Cheng, Yuxin Peng, Jinshan Tang, Hongrui Zhu, Facheng Qiu","doi":"10.1038/s41545-025-00465-3","DOIUrl":"https://doi.org/10.1038/s41545-025-00465-3","url":null,"abstract":"<p>This study introduces a hydrogenated FeCo-MOF derivative catalyst (HC-FeCo@C<sub>350</sub>) to activate peracetic acid (PAA) for efficient degradation dye wastewater. Rhodamine B (RhB) as a model pollutant, the HC-FeCo@C<sub>350</sub>/PAA achieved a 99.33% removal efficiency within 20 min, with a rate constant 18 times higher than the non-hydrogenated system. Liquid chromatography-mass spectrometry (LC-MS) and the toxicity evaluation software (T.E.S.T.) confirmed reduced intermediate toxicity. Quenching experiments, electron paramagnetic resonance (EPR) tests, and density functional theory (DFT) calculation show that HC-FeCo@C<sub>350</sub> can effectively activate PAA to produce <sup>1</sup>O<sub>2</sub>, CH<sub>3</sub>C(O)O•, and CH<sub>3</sub>C(O)OO•. The magnetically recoverable catalyst maintained over 80% efficiency after 4 cycles. In actual dye wastewater treatment, the <i>RE</i> of chemical oxygen demand (COD), ammonia nitrogen (NH<sub>3</sub>-N), total nitrogen (TN), total phosphorus (TP) could reach approximately 53.57%, 53.23%, 29.25%, 19.2%, respectively, with reduced toxicity validated by mungbean germination experiment. This technology offers a promising approach for refractory dye wastewater treatment and reuse.</p><figure></figure>","PeriodicalId":19375,"journal":{"name":"npj Clean Water","volume":"123 1","pages":""},"PeriodicalIF":11.4,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933518","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Coupled and coordinated development of water-energy-food-ecology-land system in the Yangtze River Delta, China 长三角水-能-粮-生态-地系统耦合协调发展
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-10 DOI: 10.1038/s41545-025-00472-4
Qing Qin, Weijun He, Liang Yuan, Dagmawi Mulugeta Degefu, Thomas Stephen Ramsey

The Yangtze River Delta (YRD) region, a pivotal economic hub in China, relies on water, energy, food, ecology, land, for its prosperity development. Therefore, evaluating their coupling and coordination aids the YRD’s sustainable development. This study integrated ecology and land into the water-energy-food system to form a water-energy-food-ecology-land system (WEFEFS), and the entropy weight model, comprehensive evaluation index model and coupling coordination degree models were used to assess the WEFELS in the YRD (2005-2022), and identified key influencing factors through an obstacle model. The results demonstrate that the comprehensive evaluation index of WEFELS in the YRD rose slowly, with the food system contributing the most (22.15%) and the water system contributed the least (18.25%). The degree of coupling coordination (DCC) of WEFELS in the YRD improved from 0.561 to 0.653, exhibiting spatiotemporal heterogeneity, with Anhui Province leading spatially. The main obstacle factors were Per land GDP and Energy self-sufficiency rate.

长三角地区是中国重要的经济枢纽,其繁荣发展依赖于水、能源、粮食、生态、土地。因此,评估两者的耦合和协调有助于长三角的可持续发展。本研究将生态和土地纳入水-能-食物系统,形成水-能-食物-生态-土地系统(WEFEFS),采用熵权模型、综合评价指标模型和耦合协调度模型对长三角2005-2022年的WEFEFS进行评价,并通过障碍模型识别关键影响因素。结果表明:长江三角洲生态系统生态环境综合评价指标上升缓慢,其中粮食系统贡献最大(22.15%),水系统贡献最小(18.25%);长三角WEFELS的耦合协调度(DCC)从0.561提高到0.653,呈现出时空异质性,安徽省在空间上处于领先地位。主要阻碍因素是人均国内生产总值和能源自给率。
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引用次数: 0
Effective oil-in-water emulsion separation by self-cleaning superoleophobic hydrogel membrane composite with hierarchical structure 分层结构的自清洁超疏油水凝胶膜可有效分离油水乳液
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-10 DOI: 10.1038/s41545-025-00468-0
Hyun Woong Kwon, Ralph Rolly Gonzales, Pengfei Zhang, Bowen Li, Kwang Seop Im, Jun Ho Park, Tae Kyung Lee, Hideto Matsuyama, Sang Yong Nam

Hollow fiber membranes were fabricated using polyvinylidene fluoride (PVDF) via the thermally induced phase separation method for oil-water separation. By introducing glycerol triacetate (GTA) or propylene carbonate as an extruded solvent, membrane porosity and pore size were controlled, significantly enhancing water permeance. The highest porosity and permeance were achieved with GTA as the co-extruded solvent. To further improve separation performance, a polyvinyl alcohol (PVA) coating was applied, forming a superhydrophilic and superoleophobic membrane composite. The coated membranes exhibited complete water absorption (0° contact angle) while repelling oil, preventing droplet adhesion. Antifouling performance was significantly improved, with flux recovery ratios exceeding 90% compared to 2–26% for uncoated membranes. The best-performing membrane achieved a high oil-in-water emulsion permeance of 3551 LMH/bar and 99.2% soybean oil removal efficiency. These findings demonstrate the potential of superhydrophilic and superoleophobic membranes with controlled porosity for efficient oil-water separation.

以聚偏氟乙烯(PVDF)为原料,采用热诱导相分离法制备了用于油水分离的中空纤维膜。通过引入三乙酸甘油(GTA)或碳酸丙烯酯作为挤压溶剂,控制了膜的孔隙率和孔径,显著提高了膜的透水性。以GTA为共挤溶剂,获得了最高的孔隙率和渗透率。为了进一步提高分离性能,采用聚乙烯醇(PVA)涂层,形成超亲水性和超疏油性复合膜。涂层膜具有完全的吸水性(0°接触角),同时排斥油,防止液滴粘附。与未涂覆膜的2-26%相比,涂覆膜的防污性能显著提高,通量回收率超过90%。性能最好的膜具有3551 LMH/bar的高水包油乳液渗透率和99.2%的豆油去除率。这些发现表明,控制孔隙度的超亲水和超疏油膜具有实现高效油水分离的潜力。
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引用次数: 0
Compounded fuzzy entropy-based derivation of uncertain critical factors causing corrosion in buried concrete sewer pipeline 基于复合模糊熵的埋地混凝土下水管道腐蚀不确定关键因素推导
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-05-06 DOI: 10.1038/s41545-025-00467-1
Tasaduq Ismail Wani, Srinivas Rallapalli, Anupam Singhal, Dilan Robert, Jayantha Kodikara, Biplob Kumar Pramanik, Shashi Bhushan Arya

Corrosion in buried concrete sewer pipelines remains a critical challenge for infrastructure sustainability, driven by the complex interplay of environmental, material, operational, pipe-related, and physical factors with inherent uncertainty and interdependency, aspects often overlooked previously. This study introduces a novel compounded fuzzy entropy-based approach to systematically prioritize critical corrosion-inducing factors, integrating environmental (H₂S, pH, humidity, temperature, O₂), material (cement content, alkalinity, w/c ratio, porosity, permeability), pipe-related (age, length, diameter, depth, slope), operational (flow velocity, water pressure, hydraulic energy loss, sewage residence time, sewer type), and physical (soil type, corrosivity, moisture, groundwater level, external load) factors. Results identify H₂S (0.2073), pH (0.2055), humidity (0.2031), pipe age (0.2039), length (0.2019), cement content (0.2026), alkalinity (0.2015), water pressure (0.2073), flow velocity (0.2043), soil type (0.2042), and soil corrosivity (0.2025) as the most influential contributors, enabling targeted corrosion mitigation strategies and enhancing infrastructure resilience.

由于环境、材料、操作、管道相关和物理因素的复杂相互作用,以及固有的不确定性和相互依赖性,埋地混凝土下水道管道的腐蚀仍然是基础设施可持续性的关键挑战,这些因素在以前经常被忽视。本研究引入了一种新的基于复合模糊熵的方法,通过综合环境(H₂S、pH值、湿度、温度、O₂)、材料(水泥含量、碱度、w/c比、孔隙度、渗透率)、管道相关(龄期、长度、直径、深度、坡度)、操作(流速、水压、水力能损失、污水停留时间、下水道类型)和物理(土壤类型、腐蚀性、湿度、地下水位、土壤质量)等因素,系统地对关键腐蚀诱导因素进行排序。外部负载)因素。结果表明,H₂S(0.2073)、pH(0.2055)、湿度(0.2031)、管道龄期(0.2039)、管道长度(0.2019)、水泥含量(0.2026)、碱度(0.2015)、水压(0.2073)、流速(0.2043)、土壤类型(0.2042)和土壤腐蚀性(0.2025)是影响最大的因素,有助于制定有针对性的腐蚀缓解策略,增强基础设施的复原力。
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引用次数: 0
Analysis of microstructure properties of Ni-Fe MOFs and their influence on selective recognition of single and binary dye systems Ni-Fe MOFs的微观结构及其对单双染料体系选择性识别的影响分析
IF 11.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-04-29 DOI: 10.1038/s41545-025-00470-6
Dan Xu, Xiaolin Cao, Jie Zhou, Zhihao Lin, Jing Wang, Jiatong Han, Ge Chen, Guangyang Liu, Xiaomin Xu, Yanguo Zhang, Donghui Xu

To address the environmental threats posed by dye pollution, it is crucial to develop adsorbents with high selectivity and adsorption capacity for the removal of chemical dye pollutants. In this study, five types of Ni/Fe-MOFs were synthesized via a one-pot solvothermal method by varying the Ni/Fe molar ratio. Their physicochemical structures, surface morphologies, and compositions were characterized through a series of techniques, and their adsorption performances for different dyes were preliminarily investigated. The results demonstrated that the Ni/Fe ratio significantly affects the microstructure and adsorption performance of the MOFs. As the molar ratio of Ni/Fe increased, the structures of the five materials transformed from nanoflowers(Fe-MOFs) to nanospheres(Ni/Fe(3:1)MOFs), and eventually to rhombic blocks(Ni-MOFs). The specific surface area decreased from 281.3 m²/g(Fe-MOFs) to 67.11 m²/g(Ni/Fe(1:1)MOFs) and further to 0.5369 m²/g(Ni-MOFs). XPS analysis confirmed the synergistic coordination between Ni and Fe, and FT-IR spectra revealed characteristic peaks for hydroxyl groups on the MOF surface and carboxylate ligands. XRD analysis indicated that materials with higher Ni content were more prone to ligand decomposition, which is consistent with the weight loss observed in the TG-DSC between 230 and 350 °C. The materials exhibited selective adsorption for different dyes. Under optimal conditions, the maximum adsorption capacities for Eosin Y (EY), Neutral Red (NR), and Acid Fuchsin (AF) were 54.92 mg/g(Fe-MOFs), 636.31 mg/g(Ni-MOFs), and 79.30 mg/g(Ni/Fe(1:1)MOFs), respectively. The adsorption kinetics followed a pseudo-second-order model, and the adsorption isotherms conformed to the Langmuir model, while Fe-MOFs and Ni/Fe(1:1) MOFs also exhibited compatibility with the Freundlich model. The adsorption mechanism primarily involved monolayer adsorption as the dominant process, with localized multilayer adsorption, as well as chemisorption, hydrogen bonding, hydroxyl interactions, and electrostatic interactions. These MOFs demonstrated high dye removal efficiency in actual water samples and fruit and vegetable juices, exhibiting excellent reusability and anti-interference capabilities. Importantly, compared with the single system, Fe-MOFs and Ni/Fe(1:1)MOFs exhibit competitive adsorption, and Ni-MOFs exhibit synergistic adsorption in the binary system. This study confirms that by adjusting the Ni/Fe molar ratio, MOFs with high selectivity and adsorption performance for different dyes can be designed, providing new theoretical insights and technical support for environmental remediation and food safety applications.

为了解决染料污染对环境造成的威胁,开发高选择性和高吸附能力的吸附剂对化学染料污染物的去除至关重要。在本研究中,通过改变Ni/Fe的摩尔比,采用一锅溶剂热法合成了5种Ni/Fe- mofs。通过一系列技术表征了它们的理化结构、表面形貌和组成,并初步研究了它们对不同染料的吸附性能。结果表明,Ni/Fe比对mof的微观结构和吸附性能有显著影响。随着Ni/Fe摩尔比的增加,五种材料的结构从纳米花(Fe- mof)转变为纳米球(Ni/Fe(3:1) mof),最终转变为菱形块(Ni- mof)。比表面积从281.3 m²/g(Fe-MOFs)下降到67.11 m²/g(Ni/Fe(1:1)MOFs),进一步下降到0.5369 m²/g(Ni-MOFs)。XPS分析证实了Ni和Fe之间的协同配合,FT-IR光谱显示了MOF表面羟基和羧酸配体的特征峰。XRD分析表明,Ni含量越高的材料更容易发生配体分解,这与TG-DSC在230 ~ 350℃之间观察到的失重现象一致。材料对不同的染料表现出选择性吸附。在最佳条件下,对伊红Y (EY)、中性红(NR)和酸性紫红(AF)的最大吸附量分别为54.92 mg/g(Fe-MOFs)、636.31 mg/g(Ni-MOFs)和79.30 mg/g(Ni/Fe(1:1)MOFs)。吸附动力学符合拟二阶模型,吸附等温线符合Langmuir模型,而Fe- mof和Ni/Fe(1:1) mof也符合Freundlich模型。吸附机理主要包括以单层吸附为主,局部多层吸附为主,以及化学吸附、氢键、羟基相互作用、静电相互作用等。这些MOFs在实际水样和果蔬汁中表现出较高的染料去除效率,具有优异的可重复使用性和抗干扰能力。重要的是,与单一体系相比,Fe-MOFs和Ni/Fe(1:1)MOFs表现出竞争性吸附,而Ni-MOFs在二元体系中表现出协同吸附。本研究证实,通过调整Ni/Fe摩尔比,可以设计出对不同染料具有高选择性和高吸附性能的MOFs,为环境修复和食品安全应用提供了新的理论见解和技术支持。
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