The rapid expansion of nuclear energy has led to increased uranium contamination in wastewater, necessitating the development of efficient, cost-effective, and recyclable materials for uranium removal. Hydroxyapatite (HAP) has emerged as a promising candidate due to its exceptional surface properties, structural tunability, and environmental compatibility. This review systematically evaluates recent progress in HAP-based materials for uranium remediation, focusing on advanced synthesis techniques and modification strategies that enhance adsorption capacity and ion selectivity. We analyze the underlying mechanisms, particularly the roles of material morphology and solution pH in optimizing uranium removal efficiency. Current limitations in practical applications are critically discussed, along with future research priorities for developing next-generation HAP composites. By establishing structure-performance relationships and addressing current challenges, this review provides fundamental insights to guide the design of high-performance radioactive wastewater treatment materials.
{"title":"A comprehensive review on progress and prospects of modified hydroxyapatite for uranium fixation from water","authors":"Yanlin Chen, Qingyan Zhang, Xijun Fu, Yilin Liu, Rongzhong Wang, Qingyi Zeng","doi":"10.1016/j.seppur.2025.132599","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132599","url":null,"abstract":"The rapid expansion of nuclear energy has led to increased uranium contamination in wastewater, necessitating the development of efficient, cost-effective, and recyclable materials for uranium removal. Hydroxyapatite (HAP) has emerged as a promising candidate due to its exceptional surface properties, structural tunability, and environmental compatibility. This review systematically evaluates recent progress in HAP-based materials for uranium remediation, focusing on advanced synthesis techniques and modification strategies that enhance adsorption capacity and ion selectivity. We analyze the underlying mechanisms, particularly the roles of material morphology and solution pH in optimizing uranium removal efficiency. Current limitations in practical applications are critically discussed, along with future research priorities for developing next-generation HAP composites. By establishing structure-performance relationships and addressing current challenges, this review provides fundamental insights to guide the design of high-performance radioactive wastewater treatment materials.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"29 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660500","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}
Pub Date : 2025-03-19DOI: 10.1016/j.seppur.2025.132613
Jingjing Gao, Yandong Guo, Yaxi Yu, Zhenlei Wang, Kun Dong
Ionic liquids (ILs) have shown great potential as CO2 absorbents, but traditional experimental methods for screening ILs are both time-consuming and labor-intensive. To identify the most effective ILs with desirable properties, the computer-aided design approaches are essential. This study manifested a rapid screening method for ILs using graph neural network (GNN). Approximate 40,000 experimental data points were collected, including CO2 solubility, viscosity, melting point, and toxicity, to train high-precision GNN regression models and XGBoost classification models. Various strategies were examined for constructing molecular graphs based on IL structures and several GNN models were compared, ultimately proposing an effective GNN architecture that strongly enhances prediction accuracy. To realize high-throughput screening, a database containing 200,000 IL structures was built, further established screening criteria: melting point below 298.15 K, viscosity under 100 MPa·s, and the toxicity with log10EC50, is greater than 3.4 μM. Through this screening process, 12 ILs were successfully identified that showed the highest CO2 solubility. Density functional theory (DFT) calculations indicated that the main interaction mechanism between CO2 and ILs involves the C atom of CO2 being attracted by the O atom of the anion, while the O atoms of CO2 are attracted by the H atoms of the cation. This data-driven approach simplifies the selection and design of IL absorbents, thereby accelerating the development of CO2 capture technologies.
离子液体（ILs）作为二氧化碳吸收剂已显示出巨大的潜力，但筛选离子液体的传统实验方法既耗时又耗力。要确定具有理想特性的最有效的离子液体，计算机辅助设计方法至关重要。本研究利用图神经网络（GNN）展示了一种快速筛选 IL 的方法。收集了大约 40,000 个实验数据点，包括 CO2 溶解度、粘度、熔点和毒性，用于训练高精度 GNN 回归模型和 XGBoost 分类模型。研究人员研究了基于IL结构构建分子图谱的各种策略，并对几种GNN模型进行了比较，最终提出了一种有效的GNN架构，可大大提高预测准确性。为实现高通量筛选，建立了包含 20 万个 IL 结构的数据库，并进一步确立了筛选标准：熔点低于 298.15 K，粘度低于 100 MPa-s，毒性 log10EC50 大于 3.4 μM。通过这一筛选过程，成功确定了 12 种二氧化碳溶解度最高的 IL。密度泛函理论（DFT）计算表明，CO2 与 IL 之间的主要相互作用机制是 CO2 的 C 原子被阴离子的 O 原子吸引，而 CO2 的 O 原子则被阳离子的 H 原子吸引。这种数据驱动的方法简化了IL吸收剂的选择和设计，从而加快了二氧化碳捕集技术的发展。
{"title":"Rationally design the ionic liquid-based absorbents for CO2 absorption using machine learning","authors":"Jingjing Gao, Yandong Guo, Yaxi Yu, Zhenlei Wang, Kun Dong","doi":"10.1016/j.seppur.2025.132613","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132613","url":null,"abstract":"Ionic liquids (ILs) have shown great potential as CO<sub>2</sub> absorbents, but traditional experimental methods for screening ILs are both time-consuming and labor-intensive. To identify the most effective ILs with desirable properties, the computer-aided design approaches are essential. This study manifested a rapid screening method for ILs using graph neural network (GNN). Approximate 40,000 experimental data points were collected, including CO<sub>2</sub> solubility, viscosity, melting point, and toxicity, to train high-precision GNN regression models and XGBoost classification models. Various strategies were examined for constructing molecular graphs based on IL structures and several GNN models were compared, ultimately proposing an effective GNN architecture that strongly enhances prediction accuracy. To realize high-throughput screening, a database containing 200,000 IL structures was built, further established screening criteria: melting point below 298.15 K, viscosity under 100 MPa·s, and the toxicity with log<sub>10</sub>EC<sub>50</sub>, is greater than 3.4 μM. Through this screening process, 12 ILs were successfully identified that showed the highest CO<sub>2</sub> solubility. Density functional theory (DFT) calculations indicated that the main interaction mechanism between CO<sub>2</sub> and ILs involves the C atom of CO<sub>2</sub> being attracted by the O atom of the anion, while the O atoms of CO<sub>2</sub> are attracted by the H atoms of the cation. This data-driven approach simplifies the selection and design of IL absorbents, thereby accelerating the development of CO<sub>2</sub> capture technologies.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"19 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660529","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132591
Yi Deng, Yilun Sun, Bin Wang, Yu Lin, Guoliang Chai, Yinghe Zhang
With the rapid development of clean energy industry, the demand for lithium resources has significantly risen. It makes brine-based lithium extraction into a focal point of research field. Here, we have addressed the challenge of selectively extracting lithium from high-salinity brine by incorporating 2,2′-(propane-1,3-diylbis(oxy))diphenol (PDD) crown-like ether materials onto layered titanium carbide nanosheet substrates, leveraging charge and size sieving mechanisms. The oxygen atoms in the crown-like ether framework of PDD exhibit optimal electronegativity, facilitating the rapid adsorption of metal cations. Simultaneously, the cavity structure of the crown ether remains intact, enabling the size-selective extraction of lithium ions. Separation experiments and simulation calculations, have validated that the crown ether structures exhibit selective lithium-ion extraction through charge and size sieving effects by using sets such as Li+/Na+ and Li+/Mg2+. In simulated Longmucuo salt lake brine with a Mg2+/Li+ mass ratio of approximately 87, the retention rate of Li+ using PDD reached 23.42%, and the separation factors for Li+/Na+, Li+/Mg2+, Li+/K+ were 6.85, 3.20, and 33.69, respectively. Compared to other crown ethers (12C4, 14C4, 15C4), this specific crown-like ether demonstrates superior lithium extraction performance. This innovative approach utilizing PDD crown-like ether for efficient lithium recovery enhances the feasibility of lithium extraction from brine, contributing significantly to the sustainable development of the global lithium supply.
{"title":"A crown-like ether for lithium extraction from brine","authors":"Yi Deng, Yilun Sun, Bin Wang, Yu Lin, Guoliang Chai, Yinghe Zhang","doi":"10.1016/j.seppur.2025.132591","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132591","url":null,"abstract":"With the rapid development of clean energy industry, the demand for lithium resources has significantly risen. It makes brine-based lithium extraction into a focal point of research field. Here, we have addressed the challenge of selectively extracting lithium from high-salinity brine by incorporating 2,2′-(propane-1,3-diylbis(oxy))diphenol (PDD) crown-like ether materials onto layered titanium carbide nanosheet substrates, leveraging charge and size sieving mechanisms. The oxygen atoms in the crown-like ether framework of PDD exhibit optimal electronegativity, facilitating the rapid adsorption of metal cations. Simultaneously, the cavity structure of the crown ether remains intact, enabling the size-selective extraction of lithium ions. Separation experiments and simulation calculations, have validated that the crown ether structures exhibit selective lithium-ion extraction through charge and size sieving effects by using sets such as Li<sup>+</sup>/Na<sup>+</sup> and Li<sup>+</sup>/Mg<sup>2+</sup>. In simulated Longmucuo salt lake brine with a Mg<sup>2+</sup>/Li<sup>+</sup> mass ratio of approximately 87, the retention rate of Li<sup>+</sup> using PDD reached 23.42%, and the separation factors for Li<sup>+</sup>/Na<sup>+</sup>, Li<sup>+</sup>/Mg<sup>2+</sup>, Li<sup>+</sup>/K<sup>+</sup> were 6.85, 3.20, and 33.69, respectively. Compared to other crown ethers (12C4, 14C4, 15C4), this specific crown-like ether demonstrates superior lithium extraction performance. This innovative approach utilizing PDD crown-like ether for efficient lithium recovery enhances the feasibility of lithium extraction from brine, contributing significantly to the sustainable development of the global lithium supply.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"183 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640583","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132610
Ying Gao, Yang Wang, Yuxin Liu, Haoyu Wang, Guohui Dong
Recently, carbon-based materials (CNMs) have garnered significant interest within the domain of electrocatalytic pollutant remediation. However, the ambiguity surrounding the specific active sites on CNMs hinders the enhancement of their oxidation capabilities. Here, a series of samples were designed to elucidate the actual sites by manipulating the quantity of oxygen-containing functional groups and carbon defects on CNMs (DRG-x). Among the DRG-x, DRG-600 demonstrated superior activity in hydrogen peroxide (H2O2) generation, and exhibited the highest kinetic activity for tetracycline degradation. Interestingly, carbon defects, rather than oxygen − containing functional groups, predominantly boosted the generation of H2O2 and hydroxyl radicals (·OH), thereby endowing it with exceptional pollutant removal efficiency. Besides, through the systematic determinations of reactive oxygen species (H2O2, ·OH and singlet oxygen) within the electrolyte, it was evident that ·OH constitutes 79.3% and plays a pivotal role in the degradation process. This work provided a reference for strategically enhancing the activity of CNMs, particularly in terms of augmenting its electrocatalytic performance and organic degradation capabilities.
{"title":"Manipulating carbon defects for rapid H2O2 and ·OH formation: A strategy for efficient electrocatalytic organic pollutant degradation","authors":"Ying Gao, Yang Wang, Yuxin Liu, Haoyu Wang, Guohui Dong","doi":"10.1016/j.seppur.2025.132610","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132610","url":null,"abstract":"Recently, carbon-based materials (CNMs) have garnered significant interest within the domain of electrocatalytic pollutant remediation. However, the ambiguity surrounding the specific active sites on CNMs hinders the enhancement of their oxidation capabilities. Here, a series of samples were designed to elucidate the actual sites by manipulating the quantity of oxygen-containing functional groups and carbon defects on CNMs (DRG-<em>x</em>). Among the DRG-<em>x</em>, DRG-600 demonstrated superior activity in hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation, and exhibited the highest kinetic activity for tetracycline degradation. Interestingly, carbon defects, rather than oxygen − containing functional groups, predominantly boosted the generation of H<sub>2</sub>O<sub>2</sub> and hydroxyl radicals (·OH), thereby endowing it with exceptional pollutant removal efficiency. Besides, through the systematic determinations of reactive oxygen species (H<sub>2</sub>O<sub>2</sub>, ·OH and singlet oxygen) within the electrolyte, it was evident that ·OH constitutes 79.3% and plays a pivotal role in the degradation process. This work provided a reference for strategically enhancing the activity of CNMs, particularly in terms of augmenting its electrocatalytic performance and organic degradation capabilities.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"37 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143653621","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132605
Shaoshuo Wang, Liujun Yang, Wanyu Wei, Long Zhang, Yicheng Pan, Hua Li, Jianmei Lu
The removal of low-concentration pollutants from wastewater often depends on conventional porous adsorbents. However, disposing of these adsorbents as hazardous waste may result in secondary contamination. In this study, a new method to construct adsorption/catalytic bifunctional materials from donor-acceptor (D-A) type polyelectrolyte material using self-assembly and freeze-drying techniques was proposed. The material comprises a conjugated main chain, formed by the alternating copolymerization of electron-donating fluorene and electron-withdrawing benzothiadiazole, and a flexible carbon side chain terminated with an ammonium ion. Results found that the material could be constructed into a large-scale nanofilm using solvent-induced self-assembly followed by freeze-drying. The Nanofilm exhibited a rapid adsorption capacity of 374.53 mg g−1 for bisphenol A (BPA) within 3 min. Density functional theory (DFT) calculations and experimental results indicate that the rapid adsorption is facilitated by electrostatic and hydrogen-bonding interactions between the catalyst and BPA, along with π-π interactions. The alternating D-A structure of Nanofilm efficiently improves the separation of photogenerated carriers and photodegrades 50 ppm BPA in 40 min with high efficiency. This adsorption/catalysis dual-function Nanofilm presents a novel and effective solution for the continuous and efficient purification of BPA.
{"title":"Fabrication of dual-function Nanofilm incorporating hydrophobic conjugated main chains and hydrophilic side chains for water purification with adsorption/catalysis capabilities","authors":"Shaoshuo Wang, Liujun Yang, Wanyu Wei, Long Zhang, Yicheng Pan, Hua Li, Jianmei Lu","doi":"10.1016/j.seppur.2025.132605","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132605","url":null,"abstract":"The removal of low-concentration pollutants from wastewater often depends on conventional porous adsorbents. However, disposing of these adsorbents as hazardous waste may result in secondary contamination. In this study, a new method to construct adsorption/catalytic bifunctional materials from donor-acceptor (D-A) type polyelectrolyte material using self-assembly and freeze-drying techniques was proposed. The material comprises a conjugated main chain, formed by the alternating copolymerization of electron-donating fluorene and electron-withdrawing benzothiadiazole, and a flexible carbon side chain terminated with an ammonium ion. Results found that the material could be constructed into a large-scale nanofilm using solvent-induced self-assembly followed by freeze-drying. The Nanofilm exhibited a rapid adsorption capacity of 374.53 mg g<sup>−1</sup> for bisphenol A (BPA) within 3 min. Density functional theory (DFT) calculations and experimental results indicate that the rapid adsorption is facilitated by electrostatic and hydrogen-bonding interactions between the catalyst and BPA, along with π-π interactions. The alternating D-A structure of Nanofilm efficiently improves the separation of photogenerated carriers and photodegrades 50 ppm BPA in 40 min with high efficiency. This adsorption/catalysis dual-function Nanofilm presents a novel and effective solution for the continuous and efficient purification of BPA.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"20 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660536","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132250
Liping Zhang, Junfei Liu, Yingbo Dong, Yanrong Lu, Hai Lin
The pollutant removal performance of iron-loaded biochar synthesized through one-pot pyrolysis is limited by its defect characteristics. Herein, the manganous chloride (MnCl2) was employed to improve this process through being added to the precursors of cottonwood sawdust immersed by ferric trichloride (FeCl3) solution, before subjecting to one-pot pyrolysis at 500 °C (FMBC500) and 800 °C (FMBC800). It was found that MnCl2 effectively activated the composites, and the activation effect was significantly influenced by the pyrolysis temperature. At 500 °C, MnCl2 notably increased the porosity of the carbon skeleton while co-activation with FeCl3 at 800 °C notably enlarged the pores. The MnCl2 activation helped preserve the Fe3O4 during pyrolysis at 800 °C by preventing its reduction in a more reducing atmosphere, which is essential for solid–liquid separation of the composite. The morphology of Fe3O4 was altered due to the MnCl2 activation and pyrolysis temperature: FMBC800 loaded Fe3O4 nanosheet with 4.40 mmol·g−1 of Fe, whereas FMBC500 contained Fe3O4 sphere with 2.25 mmol·g−1 of Fe. This modification produced a biochar-Fe3O4 nanosheet composite at 800 °C. MnCl2 modification significantly improved the removal performance of the composites, particularly FMBC800, which exhibited the highest Sb(Ⅲ)/Sb(Ⅴ) adsorption amount at 157.83/57.32 mg·g−1. The loaded Fe-O bonds played a crucial role in the oxidation and adsorption of Sb ions. This study presents a viable strategy for optimizing the functionalities of ion-loaded biochar by adjusting the pyrolysis temperature and incorporating a modified reagent.
{"title":"Biochar-Fe3O4 nanosheet composite activated by manganous chloride for high-efficient antimony removal: Morphology modulation and temperature-dependence","authors":"Liping Zhang, Junfei Liu, Yingbo Dong, Yanrong Lu, Hai Lin","doi":"10.1016/j.seppur.2025.132250","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132250","url":null,"abstract":"The pollutant removal performance of iron-loaded biochar synthesized through one-pot pyrolysis is limited by its defect characteristics. Herein, the manganous chloride (MnCl<sub>2</sub>) was employed to improve this process through being added to the precursors of cottonwood sawdust immersed by ferric trichloride (FeCl<sub>3</sub>) solution, before subjecting to one-pot pyrolysis at 500 °C (FMBC500) and 800 °C (FMBC800). It was found that MnCl<sub>2</sub> effectively activated the composites, and the activation effect was significantly influenced by the pyrolysis temperature. At 500 °C, MnCl<sub>2</sub> notably increased the porosity of the carbon skeleton while co-activation with FeCl<sub>3</sub> at 800 °C notably enlarged the pores. The MnCl<sub>2</sub> activation helped preserve the Fe<sub>3</sub>O<sub>4</sub> during pyrolysis at 800 °C by preventing its reduction in a more reducing atmosphere, which is essential for solid–liquid separation of the composite. The morphology of Fe<sub>3</sub>O<sub>4</sub> was altered due to the MnCl<sub>2</sub> activation and pyrolysis temperature: FMBC800 loaded Fe<sub>3</sub>O<sub>4</sub> nanosheet with 4.40 mmol·g<sup>−1</sup> of Fe, whereas FMBC500 contained Fe<sub>3</sub>O<sub>4</sub> sphere with 2.25 mmol·g<sup>−1</sup> of Fe. This modification produced a biochar-Fe<sub>3</sub>O<sub>4</sub> nanosheet composite at 800 °C. MnCl<sub>2</sub> modification significantly improved the removal performance of the composites, particularly FMBC800, which exhibited the highest Sb(Ⅲ)/Sb(Ⅴ) adsorption amount at 157.83/57.32 mg·g<sup>−1</sup>. The loaded Fe-O bonds played a crucial role in the oxidation and adsorption of Sb ions. This study presents a viable strategy for optimizing the functionalities of ion-loaded biochar by adjusting the pyrolysis temperature and incorporating a modified reagent.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"55 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640575","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132611
Pengcheng Zhang, Siyi Wang, Lin Wang, Jipan Yu, Liyong Yuan, Zijie Li, Wangsuo Wu, Zhifang Chai, Weiqun Shi
The ocean holds vast reserves of uranium that can sustain the long-term fuel supply for nuclear power. However, current poly(amidoxime) (PAO)-based adsorbents usually suffer from insufficient exposure of active sites. In this study, we report an aerogel network structure composed of covalent organic framework (COF) nanosheets combined with PAO for uranium extraction from seawater. Here, the COF nanosheets not only contribute additional adsorption sites but also function as “adhesive tape” to effectively disperse polymer molecular chains. After further covalent cross-linking/ionic cross-linking, the stability of the aerogel in water is significantly improved. The cross-linked aerogels demonstrate excellent efficacy in removing U(VI), as evidenced by their high adsorption capacities (CP-150: 275 mg/g and CP-Ca: 206 mg/g in 8 ppm spiked simulated seawater) and high removal rates of uranium from various water samples (> 98 %). The adsorption behavior of U(VI) on CP-150/CP-Ca are in good accordance with the Langmuir adsorption isotherm model and the pseudo-second-order kinetic model. The η2 coordination structure of the oxime group with uranyl ion has been verified through extended X-ray absorption fine structure (EXAFS) analysis. This work offers new strategies for the construction of novel PAO-based adsorbents and highlights the potential application of 2D COFs in uranium extraction from seawater.
{"title":"Adhesive tape-inspired COF/Polymer crosslinked networks for efficient uranium extraction from seawater","authors":"Pengcheng Zhang, Siyi Wang, Lin Wang, Jipan Yu, Liyong Yuan, Zijie Li, Wangsuo Wu, Zhifang Chai, Weiqun Shi","doi":"10.1016/j.seppur.2025.132611","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132611","url":null,"abstract":"The ocean holds vast reserves of uranium that can sustain the long-term fuel supply for nuclear power. However, current poly(amidoxime) (PAO)-based adsorbents usually suffer from insufficient exposure of active sites. In this study, we report an aerogel network structure composed of covalent organic framework (COF) nanosheets combined with PAO for uranium extraction from seawater. Here, the COF nanosheets not only contribute additional adsorption sites but also function as “adhesive tape” to effectively disperse polymer molecular chains. After further covalent cross-linking/ionic cross-linking, the stability of the aerogel in water is significantly improved. The cross-linked aerogels demonstrate excellent efficacy in removing U(VI), as evidenced by their high adsorption capacities (CP-150: 275 mg/g and CP-Ca: 206 mg/g in 8 ppm spiked simulated seawater) and high removal rates of uranium from various water samples (> 98 %). The adsorption behavior of U(VI) on CP-150/CP-Ca are in good accordance with the Langmuir adsorption isotherm model and the pseudo-second-order kinetic model. The η<sup>2</sup> coordination structure of the oxime group with uranyl ion has been verified through extended X-ray absorption fine structure (EXAFS) analysis. This work offers new strategies for the construction of novel PAO-based adsorbents and highlights the potential application of 2D COFs in uranium extraction from seawater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"69 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640573","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132617
Gan Li, Ting Wang, Pengtao Guo, Bo Xue, Dahuan Liu
Recovery of valuable silver (Ag) from wastewater is essential for environmental protection and resource recovery but still faces challenges. Herein, the morphology and structure of the Zr-MOF (DUT-67-PZDC) were regulated using trifluoroacetic acid (TFA), formic acid (FA) and acetic acid (AA) as modifiers by a green and simple preparation method. Through optimization of the type and amount of acid modifiers addition, DUT-67-PZDC-AA exhibits a smaller and more homogeneous morphology compared to DUT-67-PZDC-TFA/FA, and the weak coordination ability of AA leads to unsaturated coordination of Zr clusters, which results in chelation with Cl in the precursor. Benefitting from small crystal size, N active sites, and the presence of Cl element, DUT-67-PZDC-AA achieves a good adsorption capacity (211.4 mg g−1), fast adsorption rate (5 min), as well as excellent interference resistance and adsorption selectivity for Ag+. Experimental characterization and theoretical calculation jointly prove that coordination interaction between Ag+ and N/O atoms and chemical precipitation facilitate Ag+ adsorption. Therefore, this work not only demonstrates the great potential of DUT-67-PZDC-AA in recovering Ag+ from wastewater but also provides insights into the effect of acid modifiers on the synthesis of high-efficiency MOF adsorbent.
{"title":"Insights on selective Ag+ adsorption in zirconium–based metal–organic frameworks: Morphology and structural regulation","authors":"Gan Li, Ting Wang, Pengtao Guo, Bo Xue, Dahuan Liu","doi":"10.1016/j.seppur.2025.132617","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132617","url":null,"abstract":"Recovery of valuable silver (Ag) from wastewater is essential for environmental protection and resource recovery but still faces challenges. Herein, the morphology and structure of the Zr-MOF (DUT-67-PZDC) were regulated using trifluoroacetic acid (TFA), formic acid (FA) and acetic acid (AA) as modifiers by a green and simple preparation method. Through optimization of the type and amount of acid modifiers addition, DUT-67-PZDC-AA exhibits a smaller and more homogeneous morphology compared to DUT-67-PZDC-TFA/FA, and the weak coordination ability of AA leads to unsaturated coordination of Zr clusters, which results in chelation with Cl in the precursor. Benefitting from small crystal size, N active sites, and the presence of Cl element, DUT-67-PZDC-AA achieves a good adsorption capacity (211.4 mg g<sup>−1</sup>), fast adsorption rate (5 min), as well as excellent interference resistance and adsorption selectivity for Ag<sup>+</sup>. Experimental characterization and theoretical calculation jointly prove that coordination interaction between Ag<sup>+</sup> and N/O atoms and chemical precipitation facilitate Ag<sup>+</sup> adsorption. Therefore, this work not only demonstrates the great potential of DUT-67-PZDC-AA in recovering Ag<sup>+</sup> from wastewater but also provides insights into the effect of acid modifiers on the synthesis of high-efficiency MOF adsorbent.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"9 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143653679","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132574
Kai Chen, Yong-Hua Cao, Sunny Yadav, Periyayya Uthirakumar, Gyu-Cheol Kim, Vandung Dao, Yan Li, In-Hwan Lee
Considering the rapidly growing energy demand, electrocatalytic decomposition of water is much promising as an ideal cleaning energy to help mankind energy conservation and emission reduction. However, the inadequate intrinsic activity and slow kinetics of precious-metal-free electrocatalysts in water oxidation processes are still limited. Herein, porous iron oxide/iron phosphide heterostructure packaged in nitrogen, sulfur co-doped graphene (labeled as p-Fe3O4/FeP@N,S-Gr) with mesoporous morphology and abundant interface is prepared using facile electronic and structural engineering for efficient electrochemical water oxidation. The catalyst of p-Fe3O4/FeP@N,S-Gr showed superior electrocatalytic activity and kinetic compared with porous iron oxide packaged in nitrogen, sulfur co-doped graphene (p-Fe3O4@N,S-Gr), and porous iron oxide (p-Fe3O4) catalyst for oxygen evolution reaction (OER). The overpotential (240 mV at 10 mA/cm2) and the tafel slope (45.1 mV dec-1) of p-Fe3O4/FeP@N,S-Gr in OER process is significantly lower than that of p-Fe3O4 (289 mV at 10 mA/cm2 and 63.5 mV dec-1), p-Fe3O4@N,S-Gr (257 mV at 10 mA/cm2 and 61.3 mV dec-1), RuO2 (308 mV at 10 mA/cm2 and 99.0 mV dec-1) and other reported relevant literature. Meanwhile, theoretical calculations indicate that constructing heterojunctions can significantly increase electron transfer capability and effectively reduce the adsorption energy barrier of intermediates (OH*→O* and O*→OOH*). This work demonstrates a practical and economical strategy toward the fabrication of transition metal catalysts for water oxidation.
{"title":"Rational green design of porous iron oxide/phosphide heterogeneous nanospheres embedded in hybrid graphene for efficient water oxidation","authors":"Kai Chen, Yong-Hua Cao, Sunny Yadav, Periyayya Uthirakumar, Gyu-Cheol Kim, Vandung Dao, Yan Li, In-Hwan Lee","doi":"10.1016/j.seppur.2025.132574","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132574","url":null,"abstract":"Considering the rapidly growing energy demand, electrocatalytic decomposition of water is much promising as an ideal cleaning energy to help mankind energy conservation and emission reduction. However, the inadequate intrinsic activity and slow kinetics of precious-metal-free electrocatalysts in water oxidation processes are still limited. Herein, porous iron oxide/iron phosphide heterostructure packaged in nitrogen, sulfur co-doped graphene (labeled as p-Fe<sub>3</sub>O<sub>4</sub>/FeP@N,S-Gr) with mesoporous morphology and abundant interface is prepared using facile electronic and structural engineering for efficient electrochemical water oxidation. The catalyst of p-Fe<sub>3</sub>O<sub>4</sub>/FeP@N,S-Gr showed superior electrocatalytic activity and kinetic compared with porous iron oxide packaged in nitrogen, sulfur co-doped graphene (p-Fe<sub>3</sub>O<sub>4</sub>@N,S-Gr), and porous iron oxide (p-Fe<sub>3</sub>O<sub>4</sub>) catalyst for oxygen evolution reaction (OER). The overpotential (240 mV at 10 mA/cm<sup>2</sup>) and the tafel slope (45.1 mV dec<sup>-1</sup>) of p-Fe<sub>3</sub>O<sub>4</sub>/FeP@N,S-Gr in OER process is significantly lower than that of p-Fe<sub>3</sub>O<sub>4</sub> (289 mV at 10 mA/cm<sup>2</sup> and 63.5 mV dec<sup>-1</sup>), p-Fe<sub>3</sub>O<sub>4</sub>@N,S-Gr (257 mV at 10 mA/cm<sup>2</sup> and 61.3 mV dec<sup>-1</sup>), RuO<sub>2</sub> (308 mV at 10 mA/cm<sup>2</sup> and 99.0 mV dec<sup>-1</sup>) and other reported relevant literature. Meanwhile, theoretical calculations indicate that constructing heterojunctions can significantly increase electron transfer capability and effectively reduce the adsorption energy barrier of intermediates (OH*→O* and O*→OOH*). This work demonstrates a practical and economical strategy toward the fabrication of transition metal catalysts for water oxidation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"42 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143653681","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}
Pub Date : 2025-03-18DOI: 10.1016/j.seppur.2025.132597
Jiang Liu, Tianxiang Nan, Anbang Su, Ke Bai, Qiang Zhu, Pengfei Shi, Chaobo Tang, Hanbing He, Zhengguang Ma, Jianguang Yang
The surging number of waste lithium-ion batteries has brought great challenges to the recycling industry, and the efficient and low-cost extraction of valuable components in waste lithium-ion batteries is meaningful. In this study, a gas–solid oxidative deintercalation method is proposed to efficiently extract lithium from spent lithium iron phosphate (LFP) batteries. Specifically, chlorine was utilized to oxidize Fe(II) in the LFP to Fe(III), thereby resulting in the release of lithium ions from the LFP lattice. Sequentially, the deintercalation lithium ions react with in-situ chloride ions to form lithium chloride that is easily extracted by water leaching. The results show that the gas–solid oxidative deintercalation accompanies strong exotherm, which can occur rapidly at normal temperature. After oxidative deintercalation (25 °C for 20 min) – water leaching (30 °C for 30 min), the leaching efficiency of lithium was 98.57 %, while the leaching efficiencies of iron, phosphorus, and aluminium were less than 1.5 %. Meanwhile, the main component in the leaching residue is FePO4 with stable crystal structure, which can be used for the re-generation of LFP batteries. The regenerated LFP cathode material demonstrates a spherical morphology, with an initial discharge capacity of 153.34 mAh g−1 at 0.1 C. Compared with the traditional lithium recycling process, this novel process presents remarkable advantages in production cost and efficiency. Overall, these findings provide a new insight for the recycling of waste lithium-ion batteries.
{"title":"In-situ selective extracting lithium from waste LiFePO4 cathode by gas–solid oxidative deintercalation","authors":"Jiang Liu, Tianxiang Nan, Anbang Su, Ke Bai, Qiang Zhu, Pengfei Shi, Chaobo Tang, Hanbing He, Zhengguang Ma, Jianguang Yang","doi":"10.1016/j.seppur.2025.132597","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132597","url":null,"abstract":"The surging number of waste lithium-ion batteries has brought great challenges to the recycling industry, and the efficient and low-cost extraction of valuable components in waste lithium-ion batteries is meaningful. In this study, a gas–solid oxidative deintercalation method is proposed to efficiently extract lithium from spent lithium iron phosphate (LFP) batteries. Specifically, chlorine was utilized to oxidize Fe(II) in the LFP to Fe(III), thereby resulting in the release of lithium ions from the LFP lattice. Sequentially, the deintercalation lithium ions react with in-situ chloride ions to form lithium chloride that is easily extracted by water leaching. The results show that the gas–solid oxidative deintercalation accompanies strong exotherm, which can occur rapidly at normal temperature. After oxidative deintercalation (25 °C for 20 min) – water leaching (30 °C for 30 min), the leaching efficiency of lithium was 98.57 %, while the leaching efficiencies of iron, phosphorus, and aluminium were less than 1.5 %. Meanwhile, the main component in the leaching residue is FePO<sub>4</sub> with stable crystal structure, which can be used for the re-generation of LFP batteries. The regenerated LFP cathode material demonstrates a spherical morphology, with an initial discharge capacity of 153.34 mAh g<sup>−1</sup> at 0.1 C. Compared with the traditional lithium recycling process, this novel process presents remarkable advantages in production cost and efficiency. Overall, these findings provide a new insight for the recycling of waste lithium-ion batteries.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"25 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143654185","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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