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Nanocage-modified reverse osmosis membrane for effective removal of neutral small-molecule nitrosamines from water 用于有效去除水中中性小分子亚硝胺的纳米改性反渗透膜
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-23 DOI: 10.1016/j.desal.2025.119805
Bozhan Ma , Zhiwei Qiu , Ya Xu, Wenxuan Zou, Yana Li, Ruobin Dai, Zhiwei Wang
Polyamide reverse osmosis (PA RO) membranes, increasingly applied in advanced wastewater treatment for their high separation precision, exhibit limited efficiency in removing neutral small-molecule nitrosamines. Current modification strategies for RO membranes often compromise water permeance while improving nitrosamine contaminants rejection. Herein, we developed a RO membrane by embedding nanocages into the PA layer (NCRO), achieving simultaneous enhancement of nitrosamine contaminants rejection and water permeance. The NCRO membrane demonstrated enhanced rejection of four nitrosamine contaminants—N-nitrosodimethylamine, N-nitrosomethylethylamine, N-nitrosopyrrolidine, and N-nitrosodiethylamine—with increases of 23.6 %, 8.0 %, 5.0 %, and 1.5 %, respectively, compared to the control membrane. The rejection of NaCl and nitrosamine contaminants by the NCRO membrane arises from the high energy barriers encountered during transport through the nanocages. A combination of experimental design and molecular dynamics simulations confirmed that nanocages function as the primary mass transfer channels dictating the separation performance of PA RO membranes. Due to nanocages serving as the primary mass transfer channels, the NCRO membrane demonstrated ultrahigh pure water permeance (4.2 L·m−2·h−1·bar−1). The improved water permeance mainly results from the hydrophobic and smooth inner surfaces of the nanocages, which increase the jump frequency of water molecules, enabling rapid slip flow. The NCRO membrane offers valuable insights for next-generation RO membrane design in water reuse applications.
聚酰胺反渗透膜(PA RO)因其分离精度高而越来越多地应用于污水深度处理,但在去除中性小分子亚硝胺方面效率有限。目前对反渗透膜的改性策略通常会在提高亚硝胺污染物排斥的同时损害透水性。在此,我们通过在PA层(NCRO)中嵌入纳米笼,开发了一种反渗透膜,同时增强了亚硝胺污染物的截除率和透水性。与对照膜相比,NCRO膜对n -亚硝基二甲胺、n -亚硝基somethy乙胺、n -亚硝基soprolidine和n -亚硝基二乙胺四种亚硝胺类污染物的去除率分别提高了23.6%、8.0%、5.0%和1.5%。NCRO膜对NaCl和亚硝胺类污染物的排斥是由于在通过纳米笼的运输过程中遇到了高能量垒。实验设计和分子动力学模拟的结合证实,纳米笼是决定PA - RO膜分离性能的主要传质通道。由于纳米笼作为主要的传质通道,NCRO膜具有超高的纯水渗透率(4.2 L·m−2·h−1·bar−1)。透水性的提高主要是由于纳米笼的疏水性和光滑的内表面增加了水分子的跳跃频率,从而实现了快速的滑移流动。NCRO膜为水再利用应用中的下一代RO膜设计提供了有价值的见解。
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引用次数: 0
On-site affordable acid and base production from seawater using bipolar membrane electrodialysis: ion transport and polyelectrolyte multilayer coating 利用双极膜电渗析:离子传输和聚电解质多层涂层,从海水中生产经济实惠的酸碱
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-23 DOI: 10.1016/j.desal.2025.119788
Alaaeldin A.E. Elozeiri , Dean Spasov , Huub H.M. Rijnaarts , Rob G.H. Lammertink , Jouke E. Dykstra
The ability to produce acids and bases on-site at low energy and cost is of great interest to seawater reverse osmosis desalination plants. Acid is needed to lower the seawater pH to mitigate scaling in reverse osmosis (RO) modules. Base is needed to shift the boron equilibrium in the permeate of the first RO stage towards borate, which can then be rejected by the membrane in a second RO stage. We investigated the direct use of synthetic seawater in a bipolar membrane electrodialysis (BMED) process to produce acids and bases on-site. When synthetic seawater was used in a conventional BMED stack, Mg(OH)2 scaling occurred inside the BMED stack, specifically in the salt compartments and the cation-exchange membranes (CEMs). The scaling resulted in a decline in current efficiency and raised the energy consumption of the BMED stack compared to using a pure NaCl stream. To mitigate the scaling, we used CEMs coated with a PAH/PSS multilayer to limit the transport of multivalent cations from the salt to the base compartment. Moreover, the salt compartment was acidified with a fraction of the produced protons to prevent the precipitation of Mg2+ and Ca2+. In the first run, the modified BMED stack successfully produced a 0.2 M OH and a 0.2 M H+ solution at 85% current efficiency and 0.05 kWh/mol OH. However, repeated operation showed a gradual decline in performance due to OH leakage through the CEM. To ensure long-term process stability, CEMs with improved OH retention must be developed for the BMED application.
低能耗、低成本就地生产酸碱的能力是海水反渗透淡化厂的一大兴趣。在反渗透(RO)模块中,需要酸来降低海水的pH值,以减轻结垢。需要碱来将第一级反渗透渗透物中的硼平衡转向硼酸盐,然后在第二级反渗透中被膜拒绝。我们研究了在双极膜电渗析(BMED)工艺中直接使用合成海水来现场生产酸和碱。当在传统的BMED堆中使用合成海水时,Mg(OH)2会在BMED堆内部发生结垢,特别是在盐室和阳离子交换膜(CEMs)中。与使用纯NaCl流相比,结垢导致电流效率下降,并增加了BMED堆栈的能耗。为了减轻结垢,我们使用涂有PAH/PSS多层膜的CEMs来限制多价阳离子从盐到基室的运输。此外,用部分产生的质子酸化盐室以防止Mg2+和Ca2+的沉淀。在第一次运行中,改进的BMED堆栈以85%的电流效率和0.05 kWh/mol OH -成功地产生了0.2 M OH -和0.2 M H+溶液。然而,由于OH−通过CEM渗漏,反复操作后性能逐渐下降。为了确保长期的工艺稳定性,必须为BMED应用开发具有改进OH -保留力的CEMs。
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引用次数: 0
Intelligent nanochannel topology engineering via integrated machine learning and optimization for high-performance osmotic energy conversion 基于集成机器学习和优化的高性能渗透能转换智能纳米通道拓扑工程
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119801
Tian-Hu Wang, Qiu-Yang Chang
Harnessing osmotic energy through nanochannel-based reverse electrodialysis offers a promising route for sustainable power generation, water treatment, and mineral recovery. However, the intrinsic trade-off between ion selectivity and permeability, manifested as the conflict between osmotic current and diffusion voltage, remains a fundamental challenge. Herein, we proposed an intelligent optimization method integrating finite element method (FEM), deep neural network (DNN), and non-dominated sorting genetic algorithm-II (NSGA-II), and demonstrated a novel design framework anchored in electric double layer (EDL) overlap optimization—a key governor of nanofluidic behavior. Our local-geometry-EDL matching design outperforms most conventional and uniformly tapered geometries in literature. In particular, substantial power output enhancements of 52.26 %, 77.34 %, and 196.29 % were achieved under low, moderate, and high concentration gradients, respectively, when compared with the trumpet-shaped nanochannel. Furthermore, we justified a concentration-sensitive and segment-specific design strategy based on EDL-structure modulation: nanochannel design must dynamically adapt to both salinity conditions and selectivity-permeability trade-off. We demonstrate that multi-segment heterogeneous geometries, combining tailored radial variations and wave-like structural features, are essential to overcome the performance limits of uniform channels. The performance improvement originates from the synergistic interplay between the concentration-responsive EDL and the locally modulated nanochannel geometry. This work presents a novel and sophisticated strategy for design of high-performance osmotic energy conversion systems.
利用基于纳米通道的反电渗析来利用渗透能,为可持续发电、水处理和矿物回收提供了一条有前途的途径。然而,离子选择性和渗透性之间的内在权衡,表现为渗透电流和扩散电压之间的冲突,仍然是一个根本性的挑战。在此,我们提出了一种集成有限元法(FEM)、深度神经网络(DNN)和非主导排序遗传算法(NSGA-II)的智能优化方法,并展示了一种基于双电层(EDL)重叠优化的新型设计框架——纳米流体行为的关键调控因子。我们的局部几何- edl匹配设计优于文献中大多数传统的均匀锥形几何。与喇叭形纳米通道相比,在低、中、高浓度梯度下,输出功率分别提高了52.26%、77.34%和196.29%。此外,我们证明了基于edl结构调制的浓度敏感和片段特定设计策略:纳米通道设计必须动态适应盐度条件和选择性-渗透率权衡。我们证明了多段非均匀几何形状,结合定制的径向变化和波浪状结构特征,对于克服均匀通道的性能限制至关重要。性能的提高源于浓度响应EDL和局部调制纳米通道几何结构之间的协同相互作用。这项工作提出了一种新颖而复杂的策略,用于设计高性能渗透能量转换系统。
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引用次数: 0
Fabrication of customizable thin film composite membranes by electrospray assisted interfacial polymerization 电喷雾辅助界面聚合制备可定制的薄膜复合膜
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119798
Mert Can Hacifazlioglu , Salman Ahmadipouya , Deniz Ipekci , Mayur Ostwal , Edward Wazer , Matthew Coupin , Chenhao Yao , Jamie Warner , Manish Kumar , Ying Li , Yuepeng Zhang , Jeffrey R. McCutcheon
Reverse osmosis (RO) is the leading desalination method used in the world today. However, there are only a few types of RO membranes offered by commercial suppliers. While these membranes meet the needs for some traditional desalination processes (e.g. seawater desalination), state-of-the-art polyamide thin film composite (TFC) membranes lack the customizability that some emerging reverse osmosis processes, such as low salt rejection reverse osmosis or osmotically assisted reverse osmosis, require. In this article, electrospray assisted interfacial polymerization is used to manufacture thin-film composite membranes with customizable thickness and chemistry. Thickness was controlled by adjusting the total deposited monomers through the solvent flow rates and monomer concentrations. The control of chemistry was made possible through blending of different diamine monomers. The resulting membranes exhibited a wide and predictable, spectrum of sodium chloride rejection (8 to 98.8 %) and magnesium sulfate rejection (26.6 to 99.6 %) with corresponding water permeances between 0.37 and 36.8 L/m2.h.bar. Membrane yield (percentage of successful membranes made) is also included as an additional metric for evaluating membrane manufacturing methods.
反渗透(RO)是当今世界上使用的主要海水淡化方法。然而,只有少数类型的反渗透膜由商业供应商提供。虽然这些膜可以满足一些传统脱盐工艺(如海水淡化)的需求,但最先进的聚酰胺薄膜复合膜(TFC)缺乏一些新兴反渗透工艺(如低盐排斥反渗透或渗透辅助反渗透)所需的可定制性。在本文中,使用电喷雾辅助界面聚合来制造具有可定制厚度和化学性质的薄膜复合膜。通过溶剂流速和单体浓度调节沉积单体的总量来控制厚度。通过混合不同的二胺单体,使化学控制成为可能。所得膜具有较宽的可预测光谱,对氯化钠(8% ~ 98.8%)和硫酸镁(26.6% ~ 99.6%)的截留率在0.37 ~ 36.8 L/m2.h.bar之间。膜产量(成功制膜的百分比)也包括作为评价膜制造方法的附加指标。
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引用次数: 0
Surface-tuning of polyamide nanofiltration membranes via controlled solvent activation and graphene oxide coating 通过控制溶剂活化和氧化石墨烯涂层的聚酰胺纳滤膜的表面调谐
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119799
Zhen Hong Chang , Sandrine Boivin , Hideaki Sano , Osamu Nakagoe , Jing Yao Sum , Takuji Shintani , Takahiro Fujioka
Nanofiltration (NF) membranes are known for their higher permeance compared to reverse osmosis membranes and their capability to remove most impurities from water. However, they remain susceptible to fouling. This study aimed to develop a modification method for commercial NF membranes to achieve even higher permeance and reduced fouling propensity. The method involves ethanol-water-NaOH (EWN) activation, followed by graphene oxide (GO) coating through an amide coupling reaction. The two-step modification of a commercial NF membrane (NF270) using EWN and GO, referred to as the GO/EWN/NF270 membrane, resulted in a water permeance of 19 L/m2hbar, which is 31 % higher than that of the NF270 membrane, while maintaining a Na2SO4 rejection rate of over 96 %. Fouling tests conducted at constant transmembrane pressure (TMP) with similar initial permeate flux (40 L/m2h) using sodium alginate and real municipal wastewater showed that GO grafting significantly reduced flux decline, while EWN activation primarily enhanced intrinsic permeance and lowered the required operating TMP. Overall, the two-step strategy improves the permeability-fouling balance of the commercial NF membranes using an immersion-based process compatible with practical implementation.
纳滤(NF)膜以其比反渗透膜更高的渗透性和去除水中大多数杂质的能力而闻名。然而,它们仍然容易受到污染。本研究旨在开发一种商用纳滤膜的改性方法,以获得更高的渗透率和降低污染倾向。该方法包括乙醇-水-氢氧化钠(EWN)活化,然后通过酰胺偶联反应涂覆氧化石墨烯(GO)。用EWN和氧化石墨烯对商用纳滤膜(NF270)进行两步改性,即GO/EWN/NF270膜,其透水性为19 L/m2hbar,比NF270膜提高了31%,同时Na2SO4的截留率保持在96%以上。在初始渗透通量相近(40 L/m2h)的恒定跨膜压力(TMP)下,采用海藻酸钠和真实城市污水进行的污染试验表明,氧化石墨烯接枝可显著降低通量下降,而EWN活化主要提高了固有渗透,降低了所需的运行TMP。总体而言,两步策略使用与实际实施兼容的浸入式工艺改善了商用纳滤膜的渗透-污染平衡。
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引用次数: 0
Dual waste-derived 3D solar evaporator with vertically aligned channels for efficient solar-driven desalination, wastewater purification, and thermoelectricity generation 双废物衍生的3D太阳能蒸发器,具有垂直对齐的通道,用于高效的太阳能驱动海水淡化,废水净化和热电发电
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119790
Xin Wang , Yicheng Wang , Xiao Sun , Xiaowen Cui , Tinghui Wu , Ting Wang , Yiran Luo , Yongqi Yang , Mengzhu Liu , Yongpeng Wang , Zhe Chen , Jing Li
Solar-driven interfacial evaporation (SDIE) represents a sustainable pathway for the co-production of freshwater and electricity, offering a promising solution to global water scarcity and energy deficits. However, the development of low-cost, easily fabricated, highly efficient, and salt-resistant water-electricity cogeneration systems remains a significant challenge. Herein, we fabricate a robust and cost-effective 3D solar evaporator (3D-CSC/SA@CF) by integrating corn straw-derived carbon (CSC), discarded cigarette filters (CF), and sodium alginate (SA) hydrogel. In this configuration, the CF scaffold serves as a hydrophilic, quasi-aligned porous substrate for rapid water transport, while the CSC layer functions as an efficient broadband solar absorber, endowing the evaporator with a high light absorption of 97.15 %. Benefiting from its abundant hydrophilic groups and rationally designed porous structure, the evaporation enthalpy is significantly reduced to 851 J g−1—far below that of pure water. As a result, the evaporator achieves an evaporation rate of 4.52 kg m−2 h−1 under one-sun irradiation (1 kW m−2, AM 1.5G), with a corresponding solar-to-vapor efficiency of 97.01 %. The system also exhibits remarkable salt-rejection performance, maintaining a stable evaporation rate of 3.22 kg m−2 h−1 in 20 wt% NaCl brine without salt accumulation, and effectively removes heavy metal ions, organic dyes, and antibiotics from simulated wastewater. Furthermore, we construct an integrated thermoelectric cogeneration system based on the evaporator, which delivers a maximum output power density of 307.1 mW m−2 under 1 sun illumination. This work not only demonstrates a sustainable waste-to-resource strategy but also provides a feasible and scalable approach to multifunctional hydro-energy cogeneration, highlighting its potential for practical applications in remote and resource-limited regions.
太阳能驱动界面蒸发(SDIE)代表了淡水和电力联合生产的可持续途径,为全球水资源短缺和能源短缺提供了一个有希望的解决方案。然而,开发低成本、易于制造、高效、耐盐的水电热电联产系统仍然是一个重大挑战。在此,我们通过整合玉米秸秆衍生碳(CSC),废弃香烟过滤器(CF)和海藻酸钠(SA)水凝胶,制造了一个坚固且具有成本效益的3D太阳能蒸发器(3D-CSC/SA@CF)。在这种结构中,CF支架作为亲水的准排列多孔衬底,用于快速水输送,而CSC层作为高效的宽带太阳能吸收器,赋予蒸发器高达97.15%的高光吸收率。由于其丰富的亲水性基团和合理设计的多孔结构,蒸发焓显著降低至851 J g−1,远低于纯水的蒸发焓。结果表明,在一次太阳照射(1 kW m−2,AM 1.5G)下,蒸发器的蒸发速率为4.52 kg m−2 h−1,太阳-蒸汽效率为97.01%。该系统还具有良好的脱盐性能,在20% NaCl的盐水中保持稳定的蒸发速率3.22 kg m−2 h−1,无盐积累,并能有效去除模拟废水中的重金属离子、有机染料和抗生素。此外,我们构建了一个基于蒸发器的集成热电联产系统,该系统在1个太阳光照下的最大输出功率密度为307.1 mW m−2。这项工作不仅展示了可持续的废物资源化战略,而且为多功能水能热电联产提供了可行和可扩展的方法,突出了其在偏远和资源有限地区实际应用的潜力。
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引用次数: 0
Techno-economic assessment of a demand-responsive RO-PRO superstructure for sustainable saline wastewater treatment 需求响应RO-PRO上层结构的技术经济评估,用于可持续的含盐废水处理
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119797
Usama Ali , Shahzeb Tariq , Sangyoun kim , Usman Safder , ChangKyoo Yoo
As global water scarcity and rising energy demands intensify, hybrid Reverse Osmosis Pressure Retarded Osmosis (RO-PRO) systems offer a promising solution for efficient water and power recovery. However, under fluctuating demand, membrane allocation can lead to higher specific energy consumption (SEC), reduced operational efficiency, raising concerns for long-term sustainability. To address these challenges, this study proposes a superstructure-based RO-PRO (S-RO-PRO) framework designed to maximize freshwater production and energy generation. The proposed methodology combines system-level, multi-stage RO and PRO unit configurations with demand-side management (DSM) strategies designed for building communities. The results showed that across different demand scenarios, the S-RO-PRO outperforms the conventional RO-PRO, achieving a 10–25 % reduction in SEC. Moreover, it sustains stable power densities of 2–5 W/m2 compared to 0–1 W/m2 in the conventional system, achieves energy cost reductions of 40.30–51.11 %, and maintains up to 55 % higher net present value under high-demand conditions, underscoring its strong cost-saving potential. Overall, the DSM-adapted S-RO-PRO can make a significant contribution to the development of efficient water-energy systems while supporting circular economy principles and long-term sustainability.
随着全球水资源短缺和不断增长的能源需求加剧,混合反渗透压力延迟渗透(RO-PRO)系统为高效的水和电回收提供了一个有前途的解决方案。然而,在需求波动的情况下,膜分配可能导致更高的比能耗(SEC),降低操作效率,引起对长期可持续性的担忧。为了应对这些挑战,本研究提出了一种基于上层建筑的RO-PRO (S-RO-PRO)框架,旨在最大限度地提高淡水产量和能源产量。提出的方法将系统级、多阶段RO和PRO单元配置与为建设社区设计的需求侧管理(DSM)策略相结合。结果表明,在不同的需求场景下,S-RO-PRO优于传统RO-PRO,实现了10 - 25%的SEC降低。此外,与传统系统的0-1 W/m2相比,S-RO-PRO保持了2-5 W/m2的稳定功率密度,实现了40.30 - 51.11%的能源成本降低,并在高需求条件下保持高达55%的净现值,突出了其强大的成本节约潜力。总体而言,适应dsm的S-RO-PRO可以为高效水能系统的发展做出重大贡献,同时支持循环经济原则和长期可持续性。
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引用次数: 0
Construction of Ru-anchored MIL-53(Fe) derived α-Fe2O3 for sustainable water decontamination: A synergistic strategy of oxygen vacancy modulation and photo-self-Fenton degradation ru锚定MIL-53(Fe)衍生α-Fe2O3的可持续水净化构建:氧空位调制和光自fenton降解的协同策略
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119800
Zareen Suhara Nazeer Ali , Alanoud T. Alfagham , B. Janani , Asad Syed , Abdallah M. Elgorban , Ling Shing Wong , Meenakshi Verma , S. Sudheer Khan
In this study, Ru-anchored α-Fe2O3 clusters derived from MIL-53(Fe) (Ru-FO-1) nanomaterial (NM) was successfully fabricated and applied for the photocatalytic mineralization of norfloxacin (NOR), an emerging pharmaceutical pollutant. The scanning and transmission electron microscopic studies revealed the morphology of the NM found to be aggregated spheres. X-ray diffraction studies (XRD) revealed the presence of α-Fe2O3 (FO) phases, suggesting a conformational transformation within the MIL-53(Fe) framework. X-Ray photoelectron spectroscopy (XPS), analysis revealed the role of Ru as an electron sink. Meanwhile, electron spin resonance (ESR) indicated the presence of oxygen vacancies, which enhanced charge separation as confirmed through electron impedance (EIS). The NM achieved a high mineralization efficiency of 96.24 % within 50 min, corresponding to a rate constant of 0.0334 min-1, approximately 2.03-fold higher than pristine FO clusters. Furthermore, the NM demonstrated excellent reusability efficiency of 98.12 % after six consecutive photocatalytic cycles, and its stability were further determined by XPS studies. Mechanistic investigations through photoluminescence, EIS, radical scavenging, and ESR analyses confirmed the dominant role of •OH, and supported by the photo-Fenton reaction. Gas chromatography-mass spectroscopy analysis identified ten intermediates across three degradation pathways, which were ultimately mineralized to CO2 and water. Importantly, aquatic toxicology and mutagenicity evaluations using ECOSAR and T.E.S.T revealed that the majority of intermediates were less toxic and non-mutagenic compared to those reported for other advanced oxidation systems. The synergistic effect of Ru anchoring and oxygen vacancies thus provides a promising strategy for designing efficient and environmentally benign photocatalysts for emerging pollutant bearing waste water remediation. These results pave a way for manufacturing innovation in near future.
本研究成功制备了由MIL-53(Fe) (Ru-FO-1)纳米材料(NM)衍生的ru -锚定α-Fe2O3簇,并将其应用于光催化矿化新型药物污染物诺氟沙星(NOR)。扫描电镜和透射电镜研究发现纳米颗粒的形貌为聚集球形。x射线衍射研究(XRD)显示α-Fe2O3 (FO)相的存在,表明在MIL-53(Fe)框架内发生了构象转变。x射线光电子能谱(XPS)分析揭示了Ru作为电子汇的作用。同时,电子自旋共振(ESR)表明氧空位的存在,通过电子阻抗(EIS)证实了氧空位的存在促进了电荷分离。NM在50 min内实现了96.24%的高矿化效率,对应的速率常数为0.0334 min-1,比原始FO团簇高约2.03倍。在连续6次光催化循环后,纳米颗粒的重复利用效率达到了98.12%,并通过XPS进一步确定了其稳定性。通过光致发光、EIS、自由基清除和ESR分析的机制研究证实了•OH的主导作用,并得到了光-芬顿反应的支持。气相色谱-质谱分析鉴定了10种中间体,它们通过3种降解途径最终矿化为CO2和水。重要的是,使用ECOSAR和T.E.S.T进行的水生毒理学和致突变性评估显示,与其他高级氧化系统报道的中间体相比,大多数中间体的毒性和非致突变性更低。因此,Ru锚定和氧空位的协同效应为设计高效、环保的光催化剂用于新兴含污染物废水的修复提供了一种有前景的策略。这些结果为不久的将来的制造业创新铺平了道路。
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引用次数: 0
Ultrahigh efficiency uranium extraction from seawater using Ni0-modified boron nitride: Mechanistic insights and practical application 用ni0改性氮化硼萃取海水中铀:机理及实际应用
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119796
Yixin Pan , Mingze Qin , Yingying Zhou , Bo Sun , Man Huang , Xichun Tian , Ruichao Mao , Hongliang Dong
This study reported the synthesis of a novel Ni0@BN composite by anchoring zero-valent nickel nanoparticles onto hexagonal boron nitride through a liquid-phase reduction method. The composite exhibited outstanding performance for U(VI) extraction from aqueous solutions and seawater-relevant matrices. Batch adsorption experiments revealed an adsorption capacity (qe) of 1291 mg/g at 323 K, with 80.7 % adsorption efficiency (pH 5.0, dosage 0.01 g/L, C0 = 16 mg/L). Remarkably, Ni0@BN maintained high U(VI) uptake in the presence of major seawater ions and at trace concentrations Remarkably, even at a trace concentration prepared using seawater (C0 = 0.1 mg/L, 303 K, pH = 5, dosage = 0.001 g/L), Ni0@BN maintained high adsorption capacity of 82 mg/g with 82.0 % efficiency. Spectroscopic analyses together with DFT calculations suggested a redox-involved adsorption process in which Ni0 acted as an electron donor enabling partial U(VI) reduction, while the h-BN substrate played a supportive role in interfacial charge redistribution and coordination stabilization. XAFS and DFT results further indicated that uranium species retained axial UO features and were stabilized through equatorial U-O-Ni/B coordination environments. These findings provided mechanistic insights into Ni–BN interfacial coupling and offered guidance for designing redox-active adsorbents for uranium recovery under complex seawater-relevant conditions.
本研究报道了通过液相还原法将零价镍纳米颗粒锚定在六方氮化硼上合成一种新型Ni0@BN复合材料。该复合材料从水溶液和海水相关基质中提取U(VI)的性能优异。在323 K条件下(pH 5.0,投加量0.01 g/L, C0 = 16 mg/L),其吸附量为1291 mg/g,吸附效率为80.7%。值得注意的是,Ni0@BN在主要海水离子存在和微量浓度下保持了较高的U(VI)吸收率。值得注意的是,即使在用海水制备的微量浓度下(C0 = 0.1 mg/L, 303 K, pH = 5,剂量= 0.001 g/L), Ni0@BN也保持了82 mg/g的高吸收率,效率为82.0%。光谱分析和DFT计算表明,在氧化还原过程中,Ni0作为电子供体使部分U(VI)还原,而h-BN底物在界面电荷重新分配和配位稳定中起支持作用。XAFS和DFT结果进一步表明,铀保持轴向UO特征,并通过赤道U-O-Ni/B配位环境稳定。这些发现为Ni-BN界面耦合机理的研究提供了新的思路,并为设计在复杂海水条件下回收铀的氧化还原活性吸附剂提供了指导。
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引用次数: 0
Selective adsorption and separation of W(VI) and Mo(VI) ions using layered double hydroxides: From material design to mechanism understanding 层状双氢氧化物对W(VI)和Mo(VI)离子的选择性吸附和分离:从材料设计到机理理解
IF 9.8 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-12-22 DOI: 10.1016/j.desal.2025.119794
Fan Yang , Liwen Ma , Yahui Zhao , Yu Kang , Chenhao Liu , Xiaoli Xi , Zuoren Nie
Tungsten (W) and molybdenum (Mo) are critical transition metals in the process of becoming strategic. WMo separation is an indispensable step in conventional WMo metallurgy and secondary resource recovery. However, this process is extremely challenging. The adsorption technology utilizing layered double hydroxides (LDHs) represents a more promising and environmentally friendly separation method. In this study, the relationship between the composition and structure of the LDHs and their performance in terms of WMo adsorption and separation was explained. Optimal material properties were achieved at alaminar metal is Co and Al, Co/Al percentage of 2 and interlaminate ions is NO3 (i.e Co2Al-NO3-LDH). This structural characteristic enhances adsorption performance through: appropriate electronic structure, moderate charge density, expanded interlayer spacing and moderate grain size ensuring stability. Within one hour, the W adsorption capacity (qw) of Co2Al-NO3-LDH reached 132.4 mg/g and the separation factor of WMo (β) reached 27.2. Multiple characterization techniques and theoretical simulations confirm that the adsorption mechanism is driven by electrostatic attraction and dominated by surface coordination. The high selectivity and reusability of Co2Al-NO3-LDH further mitigate the environmental impact of hydrometallurgical processes. These findings not only contribute to the fundamental understanding of LDH-based adsorption processes but also offer practical insights for the application of LDH in the separation of WMo.
钨(W)和钼(Mo)是战略转型过程中至关重要的过渡金属。WMo分离是常规WMo冶金和二次资源回收中不可缺少的步骤。然而,这个过程极具挑战性。利用层状双氢氧化物(LDHs)吸附技术是一种更有前途和环保的分离方法。在本研究中,从吸附和分离WMo的角度解释了LDHs的组成和结构与其性能之间的关系。当层间金属为Co和Al, Co/Al比例为2,层间离子为NO3−(即Co2Al-NO3−-LDH)时,材料性能达到最佳。这种结构特性通过适当的电子结构、适度的电荷密度、扩大的层间间距和适度的晶粒尺寸来提高吸附性能,从而保证了吸附的稳定性。在1 h内,Co2Al-NO3−-LDH对W的吸附量(qw)达到132.4 mg/g,对WMo (β)的分离系数达到27.2。多种表征技术和理论模拟证实了吸附机理由静电吸引驱动,表面配位主导。Co2Al-NO3−-LDH的高选择性和可重复使用性进一步减轻了湿法冶金过程对环境的影响。这些发现不仅有助于对LDH基吸附过程的基本认识,而且为LDH在WMo分离中的应用提供了实践见解。
{"title":"Selective adsorption and separation of W(VI) and Mo(VI) ions using layered double hydroxides: From material design to mechanism understanding","authors":"Fan Yang ,&nbsp;Liwen Ma ,&nbsp;Yahui Zhao ,&nbsp;Yu Kang ,&nbsp;Chenhao Liu ,&nbsp;Xiaoli Xi ,&nbsp;Zuoren Nie","doi":"10.1016/j.desal.2025.119794","DOIUrl":"10.1016/j.desal.2025.119794","url":null,"abstract":"<div><div>Tungsten (W) and molybdenum (Mo) are critical transition metals in the process of becoming strategic. W<img>Mo separation is an indispensable step in conventional W<img>Mo metallurgy and secondary resource recovery. However, this process is extremely challenging. The adsorption technology utilizing layered double hydroxides (LDHs) represents a more promising and environmentally friendly separation method. In this study, the relationship between the composition and structure of the LDHs and their performance in terms of W<img>Mo adsorption and separation was explained. Optimal material properties were achieved at alaminar metal is Co and Al, Co/Al percentage of 2 and interlaminate ions is NO<sub>3</sub><sup>−</sup> (i.e Co<sub>2</sub>Al-NO<sub>3</sub><sup>−</sup>-LDH). This structural characteristic enhances adsorption performance through: appropriate electronic structure, moderate charge density, expanded interlayer spacing and moderate grain size ensuring stability. Within one hour, the W adsorption capacity (q<sub>w</sub>) of Co<sub>2</sub>Al-NO<sub>3</sub><sup>−</sup>-LDH reached 132.4 mg/g and the separation factor of W<img>Mo (β) reached 27.2. Multiple characterization techniques and theoretical simulations confirm that the adsorption mechanism is driven by electrostatic attraction and dominated by surface coordination. The high selectivity and reusability of Co<sub>2</sub>Al-NO<sub>3</sub><sup>−</sup>-LDH further mitigate the environmental impact of hydrometallurgical processes. These findings not only contribute to the fundamental understanding of LDH-based adsorption processes but also offer practical insights for the application of LDH in the separation of W<img>Mo.</div></div>","PeriodicalId":299,"journal":{"name":"Desalination","volume":"622 ","pages":"Article 119794"},"PeriodicalIF":9.8,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145837982","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
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Desalination
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