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Synergistic removal of lanthanide elements Via electroplating technology and adsorption and its mechanism research 电镀与吸附协同去除镧系元素及其机理研究
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-07 DOI: 10.1016/j.seppur.2026.137176
Houjun He, Yingcai Wang, Zeqi Tan, Qingrong Zhang, Zhongping Cheng, Zhibin Zhang, Yunhai Liu
To enable efficient removal of fission products and recycling of radioactive waste salts, this study proposes an innovative strategy that couples electroplating technology with high-temperature adsorption. This synergistic approach successfully achieves high-efficiency extraction of lanthanide elements from molten salt media, while addressing challenges such as low current efficiency and high energy consumption under conditions of low ion concentration. Firstly, a systematic examination of La (III)’s electrochemical characteristics indicated a diffusion-controlled, one-step process involving the transfer of three electrons. Then, constant potential plating on a nickel electrode enabled formation of a LaNi alloy plating and achieved an average extraction efficiency of 95.98%. Finally, the 5 A molecular sieve was employed to perform a high-temperature adsorption experiment on the salt obtained after electrolysis. The results indicated that the removal efficiency of re-adsorption after electrolysis could reach up to 95.34%. By integrating constant potential electrorefining with 5 A molecular sieve adsorption, the overall La(III) recovery efficiency was elevated to approximately 99.81%. Mechanistic insights were obtained through kinetic modeling—including the pseudo-first-order, pseudo-second-order, and intraparticle diffusion models. Analysis demonstrated that the adsorption behavior is governed by intraparticle diffusion and dominated by chemisorption, specifically via an ion-exchange mechanism. This technology not only enables the efficient removal of harmful cracking products to enable the reuse of spent radioactive salt, but also resolves the decline in current efficiency in final electrolysis stages, and is expected to be applied in the actual dry process of spent fuel reprocessing.
为了有效地去除裂变产物和回收放射性废盐,本研究提出了一种将电镀技术与高温吸附相结合的创新策略。这种协同方法成功地实现了从熔盐介质中高效提取镧系元素,同时解决了低离子浓度条件下电流效率低、能耗高的难题。首先,对La (III)的电化学特性进行了系统的研究,发现这是一个扩散控制的、涉及三个电子转移的一步过程。然后,在镍电极上进行恒电位电镀,形成LaNi合金镀层,平均萃取效率达到95.98%。最后,采用5a分子筛对电解后得到的盐进行高温吸附实验。结果表明,电解后再吸附的去除率可达95.34%。将恒电位电精炼与5a分子筛吸附相结合,将La(III)的总回收率提高到99.81%左右。通过动力学模型——包括伪一阶、伪二阶和颗粒内扩散模型——获得了机理见解。分析表明,吸附行为受颗粒内扩散控制,主要是化学吸附,特别是通过离子交换机制。该技术不仅能够高效去除有害裂解产物,实现乏放射性盐的再利用,而且解决了最后电解阶段电流效率下降的问题,有望应用于乏燃料后处理的实际干工艺中。
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引用次数: 0
Experimental study on the rapid formation and enhancement mechanism of CO2 hydrate in nanoparticle-based media: Implications for the rapid CO2 capture and storage 纳米颗粒介质中CO2水合物快速形成和增强机理的实验研究:对CO2快速捕获和储存的启示
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-01-31 DOI: 10.1016/j.seppur.2026.137118
Xuemin Zhang , Wenqiang Cui , Wenxin Dong , Jiacheng Liu , Jiale Chen , Jinping Li , Yingmei Wang , Qingbai Wu , Peng Zhang
Hydrate-based carbon dioxide capture and storage is an efficacious strategy for reducing atmospheric carbon dioxide emissions. Nevertheless, the efficient capture and separation of CO2 depends on the rapid formation of CO2 hydrate. In addition, hydrates are prone to heterogeneous nucleation, and the kinetic processes of CO2 hydrate formation are significantly influenced by the surface characteristics of the medium. In this work, the quantitative influence of different concentrations of hydrophilic and hydrophobic particle media (hydrophilic graphite-fluorinated graphite, graphene-graphene oxide, and hydrophilic-hydrophobic silica) and the surface characteristics on the CO2 hydrate formation were studied at 278.15 K and 3 MPa. The findings demonstrated that different concentrations of medium particles significantly influence the formation process of hydrate. The optimal concentration ranges for the hydrophilic graphite-fluorinated graphite, graphene-graphene oxide, and hydrophilic-hydrophobic silica systems are 0.10, 0.02 and 0.10 wt%, respectively. Furthermore, for different medium surface characteristics, hydrophilic nanoparticles generally perform better than hydrophobic nanoparticles in terms of cumulative gas consumption, gas-to-hydrate conversion rate, formation rate within the first 1 h, and T90. Additionally, it is worth noting that, when the hydrophobicity of solid particles is stronger, the formation rate of CO2 hydrates during the first hour of this process is superior to that of its corresponding hydrophilic nanoparticles. The relevant results provide a fundamental insight into the rapid formation mechanism of CO2 hydrates and propose a new strategy for constructing a hydration reaction system that facilitates, thereby promoting the industrialization process of rapid CO2 capture by the hydrate-based method.
基于水合物的二氧化碳捕获和储存是减少大气二氧化碳排放的有效策略。然而,CO2的有效捕获和分离取决于CO2水合物的快速形成。此外,水合物容易发生非均相成核,并且CO2水合物形成的动力学过程受介质表面特性的显著影响。在278.15 K和3 MPa条件下,定量研究了不同浓度亲疏水颗粒介质(亲水性石墨-氟化石墨、石墨烯-氧化石墨烯、亲疏水性二氧化硅)和表面特性对CO2水合物形成的影响。结果表明,不同浓度的介质颗粒对水合物的形成过程有显著影响。亲水石墨-氟化石墨、石墨烯-氧化石墨烯和亲水-疏水二氧化硅体系的最佳浓度范围分别为0.10、0.02和0.10 wt%。此外,对于不同的介质表面特性,亲水纳米颗粒在累积耗气量、气-水合物转化率、前1 h内的形成速率和T90等方面普遍优于疏水纳米颗粒。此外,值得注意的是,当固体颗粒的疏水性较强时,该过程的第一个小时CO2水合物的形成速度优于其相应的亲水纳米颗粒的形成速度。相关研究结果对CO2水合物的快速形成机理提供了基础性的认识,并提出了构建有利于水化反应体系的新策略,从而促进水化方法快速捕集CO2的产业化进程。
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引用次数: 0
Harnessing Photothermal graphene oxide interlayers for high-flux solar-driven pervaporation desalination 利用光热氧化石墨烯中间层进行高通量太阳能驱动的渗透蒸发脱盐
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-03 DOI: 10.1016/j.seppur.2026.137136
Cheng Tang , Jie Hu , Tingting Yue , Xiufeng Hu , Wei Yu , Hui Lei
Seawater desalination is a crucial approach to addressing global freshwater scarcity, especially in coastal and arid regions. Pervaporation (PV) offers high salt rejection and strong fouling resistance, but conventional PV membranes often suffer from limited permeate flow rates and temperature polarization. In this study, solar energy was integrated with PV by incorporating graphene oxide (GO) as a photothermal material to directly heat the membrane surface, thereby reducing energy consumption and enhancing permeation flux. The composite membrane comprises an electrospun polyacrylonitrile (PAN) support layer, a GO-based intermediate layer crosslinked with polyethyleneimine (PEI), and a sodium alginate (SA) selective top layer. The GO interlayer converts the solar energy into localized heat and enhances surface wettability, facilitating the development of a uniform and ultrathin SA separation layer, while concurrently enhancing the structural stability of the membrane. By optimizing GO loading and SA thickness, the membrane structure was tailored to increase permeate flux and maintain high salt rejection. The optimized SA(10)/PEI-GO(250)/PAN membrane delivered a stable water flux averaging 2.9–3.0 kg/m2·h, while maintaining a salt removal efficiency above 99.9%. Extended operational trials validated the long-term reliability of the system. These findings highlight the feasibility of solar-driven PV (SPV) composites as a low-energy and eco-friendly approach to saline water treatment.
海水淡化是解决全球淡水短缺的关键方法,特别是在沿海和干旱地区。渗透蒸发膜(PV)具有较高的阻盐性和较强的抗污性,但传统的PV膜往往存在渗透速率有限和温度极化的问题。在本研究中,通过将氧化石墨烯(GO)作为光热材料直接加热膜表面,将太阳能与光伏相结合,从而降低了能耗,提高了渗透通量。该复合膜包括电纺丝聚丙烯腈(PAN)支撑层、与聚乙烯亚胺(PEI)交联的氧化石墨烯基中间层和海藻酸钠(SA)选择性顶层。氧化石墨烯中间层将太阳能转化为局部热,增强了表面润湿性,有利于形成均匀超薄的SA分离层,同时增强了膜的结构稳定性。通过优化氧化石墨烯的负载和SA的厚度,定制膜结构,以增加渗透通量并保持高的阻盐性。优化后的SA(10)/PEI-GO(250)/PAN膜具有稳定的水通量,平均为2.9 ~ 3.0 kg/m2·h,同时除盐效率保持在99.9%以上。扩展的操作试验验证了系统的长期可靠性。这些发现强调了太阳能驱动PV (SPV)复合材料作为一种低能耗和环保的盐水处理方法的可行性。
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引用次数: 0
Synergistic catalysis and orchestrated mineralization of toluene by cooperative surface hydroxyls and metallic Bi0 协同表面羟基与金属Bi0协同催化甲苯矿化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-09 DOI: 10.1016/j.seppur.2026.137202
Yizhou Xuan , Zibo Wang , Chunyan Yang, Haotian Liu, Shengyao Wang, Hao Chen, Peilin Yang, Xing Ding
The inefficient coupling between the initial oxidation and subsequent deep degradation steps remains a critical bottleneck for achieving complete photocatalytic mineralization of toluene. In this study, we developed a “dynamic dual-catalytic system” with synergistic surface hydroxyl groups and metallic Bi0 on a bismuth molybdate substrate. The optimized catalyst achieved 85.46% toluene conversion and 80.23% mineralization efficiency under light irradiation, which are 2.05 and 3.20 times higher than those of the pristine material, respectively. Through advanced in situ characterization and mechanistic studies, two complementary functions were elucidated: hydroxyl groups promote ·OH-mediated initial activation, enabling pre-oxidation of toluene, while metallic Bi0 enhances charge separation and facilitates ·O2 generation, leading to ring-opening reactions. These modifications operate in a synergistic and sequential manner to achieve complete mineralization of toluene. This work provides new insights into the role of organic intermediates in oxygen activation and proposes a promising strategy for developing next-generation photocatalysts for volatile organic compound elimination.
初始氧化和随后的深度降解步骤之间的低效耦合仍然是实现完全光催化矿化甲苯的关键瓶颈。在这项研究中,我们在钼酸铋衬底上开发了一种具有协同表面羟基和金属Bi0的“动态双催化系统”。优化后的催化剂在光照射下甲苯转化率为85.46%,矿化效率为80.23%,分别是原始材料的2.05倍和3.20倍。通过先进的原位表征和机理研究,阐明了两个互补的功能:羟基促进·oh介导的初始活化,实现甲苯的预氧化,而金属Bi0促进电荷分离,促进·O2−的生成,导致开环反应。这些修饰以协同和顺序的方式起作用,以实现甲苯的完全矿化。这项工作为有机中间体在氧活化中的作用提供了新的见解,并为开发下一代光催化剂消除挥发性有机化合物提出了一个有希望的策略。
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引用次数: 0
Solar-driven ultrafast degradation of sodium p-perfluorous nonenoxybenzene sulfonate via oxygen-vacancy-rich MXene heterojunction photocatalytic ozonation 富氧空位MXene异质结光催化臭氧氧化超快降解对全氟壬烯氧苯磺酸钠
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-10 DOI: 10.1016/j.seppur.2026.137069
Yuhui Wang , Zhangtao Liu , Shuo Qi , Zhaojun Li , Yaqian Pang , Zhenyang Xu , Yongbing Zhu , Ning Xiao , Tingting Zhang
A novel MXene-based ternary catalyst was designed to overcome the rapid recombination of photogenerated charge carriers in photocatalytic ozonation (PCO) for the effective degradation of persistent per- and polyfluoroalkyl substances (PFAS). The optimized system achieved over 80% removal of sodium p-perfluorous nonenoxybenzene sulfonate (OBS) in 2 min, representing a 3.5-fold enhancement compared to PCO alone. Characterization results demonstrated that the superior performance originated from the introduction of indium, which not only narrowed the bandgap but also generated abundant oxygen vacancies (OVs). These OVs served as electron-regulating centers, steering the system toward a reaction pathway dominated by singlet oxygen (1O2). It was ultimately confirmed that 1O2 and holes acted as the primary reactive species, enabling efficient detoxification of OBS while also exhibiting strong stability in actual fluorinated firefighting wastewater. This study established an advanced oxidation strategy and highlighted the significant potential of vacancy-engineered MXene-based composites in treating recalcitrant PFAS in aquatic environments.
设计了一种新型mxene三元催化剂,克服了光催化臭氧氧化(PCO)中光生载流子的快速重组,有效降解持久性全氟烷基和多氟烷基物质(PFAS)。优化后的系统在2分钟内对全氟壬烯氧苯磺酸钠(OBS)的去除率超过80%,与单独使用PCO相比提高了3.5倍。表征结果表明,优异的性能源于铟的引入,它不仅缩小了带隙,而且产生了丰富的氧空位(OVs)。这些OVs充当电子调节中心,引导系统向单线态氧(1O2)主导的反应途径发展。最终证实,1O2和孔洞是主要的反应物质,能够有效地解毒OBS,同时在实际的氟化消防废水中也表现出很强的稳定性。该研究建立了一种先进的氧化策略,并强调了真空工程mxene基复合材料在处理水生环境中顽固性PFAS方面的巨大潜力。
{"title":"Solar-driven ultrafast degradation of sodium p-perfluorous nonenoxybenzene sulfonate via oxygen-vacancy-rich MXene heterojunction photocatalytic ozonation","authors":"Yuhui Wang ,&nbsp;Zhangtao Liu ,&nbsp;Shuo Qi ,&nbsp;Zhaojun Li ,&nbsp;Yaqian Pang ,&nbsp;Zhenyang Xu ,&nbsp;Yongbing Zhu ,&nbsp;Ning Xiao ,&nbsp;Tingting Zhang","doi":"10.1016/j.seppur.2026.137069","DOIUrl":"10.1016/j.seppur.2026.137069","url":null,"abstract":"<div><div>A novel MXene-based ternary catalyst was designed to overcome the rapid recombination of photogenerated charge carriers in photocatalytic ozonation (PCO) for the effective degradation of persistent <em>per</em>- and polyfluoroalkyl substances (PFAS). The optimized system achieved over 80% removal of sodium p-perfluorous nonenoxybenzene sulfonate (OBS) in 2 min, representing a 3.5-fold enhancement compared to PCO alone. Characterization results demonstrated that the superior performance originated from the introduction of indium, which not only narrowed the bandgap but also generated abundant oxygen vacancies (OVs). These OVs served as electron-regulating centers, steering the system toward a reaction pathway dominated by singlet oxygen (<sup>1</sup>O<sub>2</sub>). It was ultimately confirmed that <sup>1</sup>O<sub>2</sub> and holes acted as the primary reactive species, enabling efficient detoxification of OBS while also exhibiting strong stability in actual fluorinated firefighting wastewater. This study established an advanced oxidation strategy and highlighted the significant potential of vacancy-engineered MXene-based composites in treating recalcitrant PFAS in aquatic environments.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137069"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172228","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
Ag+-coordination-driven rapid self-assembly of α-MnO2 nanowire building blocks into 3D porous macroscopic architectures for enhanced selective catalytic oxidation of ammonia Ag+配位驱动的α-MnO2纳米线快速自组装成三维多孔宏观结构,以增强氨的选择性催化氧化
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-02 DOI: 10.1016/j.seppur.2026.137128
Wang Ran , Shaopeng Rong , Shouzhi Chen, Tao Yu, Wenxuan Xu
In the context of the global transition to clean energy, ammonia (NH3) is widely considered a promising carbon-free energy carrier, yet its potential leakage poses serious risks to both environmental and human health. Selective catalytic oxidation of NH3 (NH3-SCO) using Ag-based catalysts represents an effective end-of-pipe abatement technology. Nevertheless, conventional Ag-based catalysts suffer from severe aggregation and low atomic utilization due to insufficient anchoring sites on carrier surface. Herein, we developed a novel Ag+-coordination-driven self-assembly strategy for constructing three-dimensional (3D) porous aerogel catalysts (Ag@3D-MnO2) using surface-hydroxylated α-MnO2 nanowires as building blocks. This 3D macroporous architecture offers dual functional advantages: It provides abundant adsorption sites and enhances the concentration of reactive oxygen species, while the atomically dispersed Ag+ ions significantly promote catalytic oxidation capabilities, facilitating the generation of oxygen species and superoxide radicals (•O2). The resulting Ag@3D-MnO2 aerogel catalyst, with a low Ag loading, achieves complete NH3 conversion at 140 °C, 70 °C lower than that of pristine α-MnO2 (T100 = 210 °C). Moreover, it demonstrates outstanding stability, maintaining high activity over a 60-h continuous test and four successive reaction cycles without obvious deactivation. This endogenous self-assembly strategy for constructing 3D macrostructures demonstrates a viable route to enhance Ag atom utilization, providing a highly efficient and durable catalyst for low-temperature NH3-SCO. The present work demonstrates considerable potential for practical applications in controlling NH3 emissions and ensuring the safe utilization of ammonia in clean energy systems.
在全球向清洁能源转型的背景下,氨(NH3)被广泛认为是一种有前景的无碳能源载体,但其潜在的泄漏对环境和人类健康构成严重风险。ag基催化剂选择性催化氧化NH3 (NH3- sco)是一种有效的管道末端治理技术。然而,传统的银基催化剂由于载体表面的锚定位点不足,存在严重的聚集和原子利用率低的问题。在此,我们开发了一种新的Ag+配位驱动的自组装策略,用于构建三维(3D)多孔气凝胶催化剂(Ag@3D-MnO2),使用表面羟基化α-MnO2纳米线作为构建块。这种3D大孔结构具有双重功能优势:它提供了丰富的吸附位点,提高了活性氧的浓度,而原子分散的Ag+离子显著提高了催化氧化能力,促进了氧和超氧自由基(•O2−)的产生。制备的Ag@3D-MnO2气凝胶催化剂在140℃下可实现NH3的完全转化,比原始α-MnO2 (T100 = 210℃)低70℃。此外,它表现出出色的稳定性,在连续60小时的测试和连续四个反应周期中保持高活性,没有明显的失活。这种构建三维宏观结构的内源性自组装策略为提高Ag原子的利用率提供了一条可行的途径,为低温NH3-SCO提供了一种高效耐用的催化剂。目前的工作在控制NH3排放和确保清洁能源系统中氨的安全利用方面具有相当大的实际应用潜力。
{"title":"Ag+-coordination-driven rapid self-assembly of α-MnO2 nanowire building blocks into 3D porous macroscopic architectures for enhanced selective catalytic oxidation of ammonia","authors":"Wang Ran ,&nbsp;Shaopeng Rong ,&nbsp;Shouzhi Chen,&nbsp;Tao Yu,&nbsp;Wenxuan Xu","doi":"10.1016/j.seppur.2026.137128","DOIUrl":"10.1016/j.seppur.2026.137128","url":null,"abstract":"<div><div>In the context of the global transition to clean energy, ammonia (NH<sub>3</sub>) is widely considered a promising carbon-free energy carrier, yet its potential leakage poses serious risks to both environmental and human health. Selective catalytic oxidation of NH<sub>3</sub> (NH<sub>3</sub>-SCO) using Ag-based catalysts represents an effective end-of-pipe abatement technology. Nevertheless, conventional Ag-based catalysts suffer from severe aggregation and low atomic utilization due to insufficient anchoring sites on carrier surface. Herein, we developed a novel Ag<sup>+</sup>-coordination-driven self-assembly strategy for constructing three-dimensional (3D) porous aerogel catalysts (Ag@3D-MnO<sub>2</sub>) using surface-hydroxylated α-MnO<sub>2</sub> nanowires as building blocks. This 3D macroporous architecture offers dual functional advantages: It provides abundant adsorption sites and enhances the concentration of reactive oxygen species, while the atomically dispersed Ag<sup>+</sup> ions significantly promote catalytic oxidation capabilities, facilitating the generation of oxygen species and superoxide radicals (•O<sub>2</sub><sup>−</sup>). The resulting Ag@3D-MnO<sub>2</sub> aerogel catalyst, with a low Ag loading, achieves complete NH<sub>3</sub> conversion at 140 °C, 70 °C lower than that of pristine α-MnO<sub>2</sub> (T<sub>100</sub> = 210 °C). Moreover, it demonstrates outstanding stability, maintaining high activity over a 60-h continuous test and four successive reaction cycles without obvious deactivation. This endogenous self-assembly strategy for constructing 3D macrostructures demonstrates a viable route to enhance Ag atom utilization, providing a highly efficient and durable catalyst for low-temperature NH<sub>3</sub>-SCO. The present work demonstrates considerable potential for practical applications in controlling NH<sub>3</sub> emissions and ensuring the safe utilization of ammonia in clean energy systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137128"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172299","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
Investigation of forward osmosis membrane fouling mechanisms based on collision attachment theory: modeling and validation 基于碰撞附着理论的正向渗透膜污染机理研究:建模与验证
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-07 DOI: 10.1016/j.seppur.2026.137140
Tao Wang , Xiaozhen Lu , Lin Wang , Mingfei Zhu , Junxia Liu , Weiwei Huang , Tian Li , Zhao Li , Lijie Zhang , Yujie Zhu , Zhichao Huang , Huaqiang Chu , Daoji Wu , Feiyong Chen
Forward osmosis (FO) represents an energy-efficient membrane separation process that leverages osmotic pressure gradients for water treatment. Nevertheless, fouling induced by dissolved organic matter (DOM) remains a major obstacle to its practical application, underscoring the need for a deeper mechanistic understanding to enable effective fouling mitigation. This study systematically investigates FO membrane fouling mechanisms using the collision–attachment (CA) model as an analytical and predictive framework. Model foulants, including tannic acid (TA), sodium alginate (SA), bovine serum albumin (BSA), and natural DOM, were employed to elucidate the fouling behavior under varying hydrodynamic conditions, membrane orientations, and foulant concentrations. The CA model successfully unveiled fouling mechanisms, transitioning from foulant–membrane interactions at low total organic carbon (TOC ≤ 20 mg/L) to foulant–foulant interactions at high concentrations (TOC = 100 mg/L). Among the tested foulants, BSA and TA exhibited stronger fouling tendencies than SA. The active-layer-toward-draw-solution (AL–DS) configuration showed a higher initial flux but suffered more fouling development. Moreover, the validated CA model was effective in predicting natural DOM fouling under low TOC and low flux conditions. This investigation may provide mechanistic insights into FO membrane fouling and establish a validated framework for performance prediction and process optimization, contributing to more sustainable and efficient FO-based water treatment systems.
正向渗透(FO)是一种利用渗透压梯度进行水处理的节能膜分离过程。然而,溶解有机物(DOM)引起的污垢仍然是其实际应用的主要障碍,强调需要更深入地了解机制,以实现有效的污垢缓解。本研究使用碰撞-附着(CA)模型作为分析和预测框架,系统地研究了FO膜污染机制。模型污染物包括单宁酸(TA)、海藻酸钠(SA)、牛血清白蛋白(BSA)和天然DOM,以阐明不同流体动力条件、膜取向和污染物浓度下的污染行为。CA模型成功地揭示了污染机制,从低总有机碳(TOC≤20 mg/L)下的污染物-膜相互作用过渡到高浓度(TOC = 100 mg/L)下的污染物-污染物相互作用。在被试污染物中,牛血清白蛋白(BSA)和乙酸乙酯(TA)比乙酸乙酯(SA)表现出更强的污染倾向。主动层向引出溶液(AL-DS)结构表现出更高的初始通量,但受污染的影响更大。此外,经过验证的CA模型在低TOC和低通量条件下对DOM自然污染的预测是有效的。这项研究可能为FO膜污染提供机理见解,并为性能预测和工艺优化建立一个有效的框架,有助于建立更可持续和高效的FO水处理系统。
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引用次数: 0
An N-doped quaternary phosphonium-based ionic hypercrosslinked polymer for efficient and ultrafast removal of small-molecular phenolic pollutants 一种高效、超快去除小分子酚类污染物的n掺杂季磷基离子超交联聚合物
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-01-31 DOI: 10.1016/j.seppur.2026.137116
Lin Yao , Pu Xiong , Hao Chen , Li Zhang , Meng Wang , Yafen Dai , Yigang Ding
The treatment of small-molecular phenolic pollutants still faces numerous technical challenges. Herein, we selected benzyltriphenylphosphonium chloride(BPP) with multiple aromatic rings as the ionic monomer, benzene as the comonomer, and indole (IN), benzimidazole (BZD), and benzotriazole (BTA) as the N-heterocyclic monomers to prepare quaternary phosphonium-based ionic hyper-cross-linked polymers (IHCPs) with abundant microporous structures, high hydrophilicity, and excellent physicochemical stability through a one-pot knitting strategy. The Cl on BPP and N and H on the N-heterocyclic monomers can serve as potential hydrogen bonding sites. By adjusting the content of heteroatoms in the N-heterocyclic monomers, the pore structure and hydrophilicity of the material can be effectively improved. In addition, IHCP-BTA with abundant Smicro, Vmicro, heteroatom content, and low contact angle exhibits ultrafast adsorption rates and adsorption performance for small-molecule pollutants 4-nitrophenol (4-NP) and phenol (PH), reaching equilibrium in just 10 min, whereas for macromolecule tannic acid (TA) and chlortetracycline (CTC), it takes at least 60 min to reach equilibrium. According to the fitting calculations, the Qm values of IHCP-BTA for 4-NP, PH, TA, and CTC are 383.4, 204.1, 185.6, and 194.6 mg/g, respectively. Moreover, the adsorption performance of IHCP-BTA for other small-molecule pollutants is significantly superior to that for macromolecular pollutants, and it still demonstrates excellent adsorption performance under a wide pH range, different initial concentrations, high ionic concentrations, and humic acid concentrations. When using ethyl acetate, methanol, and 5% sodium hydroxide solution as desorbents, the regeneration performance of IHCP-BTA gradually decreases. Based on material characterizations and DFT calculations, the synergistic effects of micropore filling, intermolecular weak interactions, hydrophobic interaction, and hydrogen bonding contribute to the strong adsorption affinity of IHCP-BTA towards small-molecule pollutants.
小分子酚类污染物的处理仍面临许多技术挑战。本研究以具有多个芳环的苄基三苯基氯化磷(BPP)为离子单体,以苯为共聚单体,以吲哚(IN)、苯并咪唑(BZD)和苯并三唑(BTA)为n杂环单体,通过一锅编织法制备了微孔结构丰富、亲水性高、物化稳定性好的季磷基离子超交联聚合物(IHCPs)。BPP上的Cl−和N-杂环单体上的N和H可以作为潜在的氢键位点。通过调整n -杂环单体中杂原子的含量,可以有效改善材料的孔隙结构和亲水性。此外,具有丰富的smmicro, Vmicro,杂原子含量和低接触角的IHCP-BTA对小分子污染物4-硝基苯酚(4-NP)和苯酚(PH)具有超快的吸附速率和吸附性能,仅需10 min即可达到平衡,而对大分子单宁酸(TA)和氯四环素(CTC)则需要至少60 min才能达到平衡。通过拟合计算,IHCP-BTA对4-NP、PH、TA和CTC的Qm值分别为383.4、204.1、185.6和194.6 mg/g。此外,IHCP-BTA对其他小分子污染物的吸附性能明显优于对大分子污染物的吸附性能,在较宽的pH范围、不同的初始浓度、高离子浓度和腐植酸浓度下仍表现出优异的吸附性能。当以乙酸乙酯、甲醇和5%氢氧化钠溶液为脱附剂时,IHCP-BTA的再生性能逐渐降低。基于材料表征和DFT计算,微孔填充、分子间弱相互作用、疏水相互作用和氢键的协同作用是IHCP-BTA对小分子污染物具有强吸附亲和力的原因。
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引用次数: 0
Study on the influence of cone length in volute-type cyclone separators on flow field characteristics and energy consumption 蜗壳式旋风分离器锥长对流场特性和能耗影响的研究
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-05 DOI: 10.1016/j.seppur.2026.137032
Chonghao Liang, Zhongli Ji, Xiaolin Wu
This study investigates the effects of varying cone lengths on the flow field and separation performance of a volute-type cyclone separator. The turbulent flow is modeled using the Reynolds stress model. The effects of a high-concentration, polydisperse particle system on the flow field characteristics and energy consumption distribution of the gas-solid two-phase flow within the cyclone separator are examined through a coupled Population Balance Equation approach based on the Euler-Euler method. The effect of cone length on vortex motion within cyclone separators under different particle loading conditions was investigated using the Liutex vortex identification method. Furthermore, the distribution patterns of internal energy dissipation within cyclone separators across various systems were revealed through entropy production analysis based on the second law of thermodynamics. Research findings indicate that cone length under varying particle loading conditions influences vortex motion within the flow field. High particle loading attenuates turbulence intensity, resulting in the inability of strong vortex cores to extend throughout the entire fluid space in long-cone cyclones. Among the irreversible factors affecting flow field dissipation, wall dissipation and turbulent dissipation are the dominant contributors, while entropy production from temperature-difference heat transfer and viscous dissipation account for an extremely small proportion. Particle loading reduces turbulent dissipation in the flow field and wall friction. The variation in particle loading affects local dissipation in different regions of the cyclone separator while also weakening the influence of cone length on local dissipation within the cyclone separator.
研究了不同锥长对蜗壳式旋风分离器流场和分离性能的影响。紊流是用雷诺应力模型来模拟的。采用基于欧拉-欧拉法的耦合种群平衡方程方法,研究了高浓度多分散颗粒体系对旋风分离器内气固两相流流场特性和能耗分布的影响。采用柳特克斯涡旋识别方法,研究了不同颗粒载荷条件下,锥长对旋风分离器内涡旋运动的影响。基于热力学第二定律的熵产分析揭示了旋风分离器内部能量耗散在不同系统中的分布规律。研究结果表明,不同颗粒载荷条件下的锥长会影响流场内的涡动。在长锥气旋中,高颗粒载荷会减弱湍流强度,导致强涡核无法扩展到整个流体空间。在影响流场耗散的不可逆因素中,壁面耗散和湍流耗散占主导地位,而温差换热和粘性耗散产生的熵占很小的比例。颗粒载荷减少了流场中的湍流耗散和壁面摩擦。颗粒载荷的变化影响了旋风分离器内不同区域的局部耗散,同时也减弱了锥长对旋风分离器内局部耗散的影响。
{"title":"Study on the influence of cone length in volute-type cyclone separators on flow field characteristics and energy consumption","authors":"Chonghao Liang,&nbsp;Zhongli Ji,&nbsp;Xiaolin Wu","doi":"10.1016/j.seppur.2026.137032","DOIUrl":"10.1016/j.seppur.2026.137032","url":null,"abstract":"<div><div>This study investigates the effects of varying cone lengths on the flow field and separation performance of a volute-type cyclone separator. The turbulent flow is modeled using the Reynolds stress model. The effects of a high-concentration, polydisperse particle system on the flow field characteristics and energy consumption distribution of the gas-solid two-phase flow within the cyclone separator are examined through a coupled Population Balance Equation approach based on the Euler-Euler method. The effect of cone length on vortex motion within cyclone separators under different particle loading conditions was investigated using the Liutex vortex identification method. Furthermore, the distribution patterns of internal energy dissipation within cyclone separators across various systems were revealed through entropy production analysis based on the second law of thermodynamics. Research findings indicate that cone length under varying particle loading conditions influences vortex motion within the flow field. High particle loading attenuates turbulence intensity, resulting in the inability of strong vortex cores to extend throughout the entire fluid space in long-cone cyclones. Among the irreversible factors affecting flow field dissipation, wall dissipation and turbulent dissipation are the dominant contributors, while entropy production from temperature-difference heat transfer and viscous dissipation account for an extremely small proportion. Particle loading reduces turbulent dissipation in the flow field and wall friction. The variation in particle loading affects local dissipation in different regions of the cyclone separator while also weakening the influence of cone length on local dissipation within the cyclone separator.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137032"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135568","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
CuO/carbon spheres/g-C3N4 with 3D hierarchical porous structure and functional carbon bridge for efficient CO2 adsorption and photocatalytic reduction 具有三维分层多孔结构和功能碳桥的CuO/碳球/g-C3N4用于高效CO2吸附和光催化还原
IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-06-19 Epub Date: 2026-02-12 DOI: 10.1016/j.seppur.2026.137212
Lin Qiao, Ze Zhang, Dong Fu
Utilizing photocatalysis to reduce CO2 into value-added products is a promising and sustainable pathway. This study reports the fabrication of a low-cost CuO/carbon spheres/g-C3N4 composite material without the use of precious metals, featuring a p-n heterojunction between CuO and g-C3N4 interconnected by a conductive carbon bridge. The optimal sample has suitable CO2 adsorption capacity (1.4 mmol/g at 1 bar, 25 °C) and exceptional CO2 photocatalytic performance. The optimal sample achieves CO and CH4 production yields of 110.95 and 9.9 μmol/g h−1, respectively, with 73.7% CO selectivity. Photoelectrochemical tests reveal that the CuO/g-C3N4 heterojunction facilitates rapid electron transfer via the carbon medium, achieving effective electrons(e)-holes(h+) separation. In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in-situ DRIFTS) analysis and Density Functional Theory (DFT) calculations collaboratively verify the efficient reaction pathway via key intermediates (COOH*, CHO*, CH2O*, and CH3O*) and elucidate the electronic structure driving the enhanced charge dynamics. Furthermore, property-performance correlation analysis indicates that the charge separation efficiency is the main performance driving factor. A life cycle assessment (LCA) demonstrates that avoiding the use of precious metals during catalyst preparation leads to a significant reduction in the environmental footprint of CuO/carbon spheres/g-C3N4. The main environmental impact comes from electricity consumption during production. This work provides a sustainable blueprint for designing efficient photocatalysts by integrating interfacial engineering with mechanistic understanding for solar-driven CO2 valorization.
利用光催化将二氧化碳转化为增值产品是一种有前途的可持续途径。本研究报道了一种不使用贵金属的低成本CuO/碳球/g-C3N4复合材料的制备,其特点是CuO和g-C3N4之间的p-n异质结通过导电碳桥连接。最佳样品具有合适的CO2吸附量(1 bar, 25°C时为1.4 mmol/g)和优异的CO2光催化性能。最优样品CO和CH4的产率分别为110.95和9.9 μmol/g h−1,CO选择性为73.7%。光电化学测试表明,CuO/g-C3N4异质结促进了电子通过碳介质的快速转移,实现了电子(e−)和空穴(h+)的有效分离。原位漫反射红外傅立叶变换光谱(原位DRIFTS)分析和密度泛函理论(DFT)计算共同验证了通过关键中间体(COOH*、CHO*、CH2O*和ch30 *)的有效反应途径,并阐明了驱动电荷动力学增强的电子结构。此外,性能相关性分析表明,电荷分离效率是驱动性能的主要因素。生命周期评估(LCA)表明,在催化剂制备过程中避免使用贵金属可以显著减少CuO/碳球/g-C3N4的环境足迹。主要的环境影响来自生产过程中的电力消耗。这项工作为设计高效的光催化剂提供了一个可持续的蓝图,通过将界面工程与太阳能驱动二氧化碳增值的机制理解相结合。
{"title":"CuO/carbon spheres/g-C3N4 with 3D hierarchical porous structure and functional carbon bridge for efficient CO2 adsorption and photocatalytic reduction","authors":"Lin Qiao,&nbsp;Ze Zhang,&nbsp;Dong Fu","doi":"10.1016/j.seppur.2026.137212","DOIUrl":"10.1016/j.seppur.2026.137212","url":null,"abstract":"<div><div>Utilizing photocatalysis to reduce CO<sub>2</sub> into value-added products is a promising and sustainable pathway. This study reports the fabrication of a low-cost CuO/carbon spheres/g-C<sub>3</sub>N<sub>4</sub> composite material without the use of precious metals, featuring a p-n heterojunction between CuO and g-C<sub>3</sub>N<sub>4</sub> interconnected by a conductive carbon bridge. The optimal sample has suitable CO<sub>2</sub> adsorption capacity (1.4 mmol/g at 1 bar, 25 °C) and exceptional CO<sub>2</sub> photocatalytic performance. The optimal sample achieves CO and CH<sub>4</sub> production yields of 110.95 and 9.9 μmol/g h<sup>−1</sup>, respectively, with 73.7% CO selectivity. Photoelectrochemical tests reveal that the CuO/g-C<sub>3</sub>N<sub>4</sub> heterojunction facilitates rapid electron transfer via the carbon medium, achieving effective electrons(e<sup>−</sup>)-holes(h<sup>+</sup>) separation. In-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in-situ DRIFTS) analysis and Density Functional Theory (DFT) calculations collaboratively verify the efficient reaction pathway via key intermediates (COOH*, CHO*, CH<sub>2</sub>O*, and CH<sub>3</sub>O*) and elucidate the electronic structure driving the enhanced charge dynamics. Furthermore, property-performance correlation analysis indicates that the charge separation efficiency is the main performance driving factor. A life cycle assessment (LCA) demonstrates that avoiding the use of precious metals during catalyst preparation leads to a significant reduction in the environmental footprint of CuO/carbon spheres/g-C<sub>3</sub>N<sub>4</sub>. The main environmental impact comes from electricity consumption during production. This work provides a sustainable blueprint for designing efficient photocatalysts by integrating interfacial engineering with mechanistic understanding for solar-driven CO<sub>2</sub> valorization.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"392 ","pages":"Article 137212"},"PeriodicalIF":9.0,"publicationDate":"2026-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146160184","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}
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Separation and Purification Technology
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