Pub Date : 2025-12-03DOI: 10.1016/j.seppur.2025.136359
Quanyu Hu , Kaicong Wang , Guangming Yu , Chuanxiang Zu , Zhaoyou Zhu , Jianguang Qi , Yinglong Wang , Peizhe Cui
This study developed an enhanced extraction distillation process using a mixed entrainer for the ternary azeotropic system of tert-butanol/benzene/water in industrial wastewater. The optimal entrainer was selected through quantum chemical calculations and phase equilibrium analysis, and a balanced solution for annual total cost and gas emissions was obtained using multi-objective optimization. Based on this, heat pump-assisted and heat integration-assisted processes were added. The results indicate that the heat integration process demonstrates the best environmental benefits, with a 22.6% reduction in gas emissions. Exergy analysis confirms that thermal integration technology significantly reduces irreversible losses in the system. This technology provides a low-carbon, energy-efficient solution for the recovery of organic wastewater and holds significant implications for promoting the sustainable development of chemical separation processes.
{"title":"Design of process intensification technology for clean and efficient recovery of tert-butanol and benzene from industrial wastewater via extractive distillation with mixed entrainers","authors":"Quanyu Hu , Kaicong Wang , Guangming Yu , Chuanxiang Zu , Zhaoyou Zhu , Jianguang Qi , Yinglong Wang , Peizhe Cui","doi":"10.1016/j.seppur.2025.136359","DOIUrl":"10.1016/j.seppur.2025.136359","url":null,"abstract":"<div><div>This study developed an enhanced extraction distillation process using a mixed entrainer for the ternary azeotropic system of tert-butanol/benzene/water in industrial wastewater. The optimal entrainer was selected through quantum chemical calculations and phase equilibrium analysis, and a balanced solution for annual total cost and gas emissions was obtained using multi-objective optimization. Based on this, heat pump-assisted and heat integration-assisted processes were added. The results indicate that the heat integration process demonstrates the best environmental benefits, with a 22.6% reduction in gas emissions. Exergy analysis confirms that thermal integration technology significantly reduces irreversible losses in the system. This technology provides a low-carbon, energy-efficient solution for the recovery of organic wastewater and holds significant implications for promoting the sustainable development of chemical separation processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"384 ","pages":"Article 136359"},"PeriodicalIF":9.0,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658314","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 : 2025-12-03DOI: 10.1016/j.seppur.2025.136353
Rufaydah A. Hassan , Manar M. Taha , Maram G. Zonkol , Hanadi G. Salem , Nageh K. Allam
Addressing global freshwater scarcity requires desalination technologies that are both energy-efficient and sustainable. Capacitive deionization (CDI) has emerged as a promising low-voltage alternative to conventional methods; however, its performance strongly depends on the composition and structure of the electrode materials. In this work, nickel ferrite (NiFe₂O₄) nanoparticles were synthesized via a facile co-precipitation route and thermally treated at 450 °C and 550 °C to investigate the influence of annealing on their electrochemical and desalination behavior. Structural and surface analyses (XRD, FTIR, XPS, BET) confirmed the formation of a spinel NiFe₂O₄ phase with a mesoporous framework, while SEM/TEM imaging revealed that moderate annealing at 450 °C produced well-interconnected grains with an enhanced surface area. Electrochemical measurements demonstrated that the NiFe₂O₄ annealed at 450 °C (NF450) exhibited the highest specific capacitance and lowest charge-transfer resistance, attributed to its balanced crystallinity and optimized ion transport pathways. When used as a cathode in an asymmetric NiFe₂O₄//activated carbon CDI cell, the NF450 electrode achieved a remarkable salt adsorption capacity of 34.8 mg g−1 at 1.4 V, with superior charge efficiency (>90%) and nearly 100% capacitance retention over 150 cycles. To the best of our knowledge, this represents the highest reported cycle stability and charge efficiency for a spinel-based electrode in a traditional CDI configuration. These findings underscore the potential of morphology-engineered NiFe₂O₄ as a durable and high-performance electrode material for next-generation electrochemical desalination systems.
解决全球淡水短缺问题需要既节能又可持续的海水淡化技术。电容去离子（CDI）已成为传统方法的一种有前途的低压替代方案；然而，其性能在很大程度上取决于电极材料的组成和结构。本文采用易共沉淀法合成了铁酸镍（NiFe₂O₄）纳米颗粒，并在450℃和550℃下进行热处理，研究了退火对其电化学和脱盐行为的影响。结构和表面分析（XRD， FTIR， XPS， BET）证实形成了具有介孔框架的尖晶石NiFe₂O₄相，而SEM/TEM成像显示，450°C的中等退火产生了连接良好的晶粒，表面积增加。电化学测量表明，在450°C退火的NiFe₂O₄（NF450）具有最高的比电容和最低的电荷转移电阻，这归功于其平衡的结晶度和优化的离子传输途径。在非对称NiFe₂O₄//活性炭CDI电池中用作阴极时，NF450电极在1.4 V电压下的盐吸附量为34.8 mg g - 1，具有优异的充电效率（>90%）， 150次循环后的电容保持率接近100%。据我们所知，这代表了传统CDI结构中尖晶石基电极的最高循环稳定性和充电效率。这些发现强调了形态工程NiFe₂O₄作为下一代电化学脱盐系统的耐用和高性能电极材料的潜力。
{"title":"Synergistic structural and electrochemical engineering of NiFe₂O₄ spinel cathodes with record charge efficiency for sustainable water capacitive deionization","authors":"Rufaydah A. Hassan , Manar M. Taha , Maram G. Zonkol , Hanadi G. Salem , Nageh K. Allam","doi":"10.1016/j.seppur.2025.136353","DOIUrl":"10.1016/j.seppur.2025.136353","url":null,"abstract":"<div><div>Addressing global freshwater scarcity requires desalination technologies that are both energy-efficient and sustainable. Capacitive deionization (CDI) has emerged as a promising low-voltage alternative to conventional methods; however, its performance strongly depends on the composition and structure of the electrode materials. In this work, nickel ferrite (NiFe₂O₄) nanoparticles were synthesized via a facile co-precipitation route and thermally treated at 450 °C and 550 °C to investigate the influence of annealing on their electrochemical and desalination behavior. Structural and surface analyses (XRD, FTIR, XPS, BET) confirmed the formation of a spinel NiFe₂O₄ phase with a mesoporous framework, while SEM/TEM imaging revealed that moderate annealing at 450 °C produced well-interconnected grains with an enhanced surface area. Electrochemical measurements demonstrated that the NiFe₂O₄ annealed at 450 °C (NF450) exhibited the highest specific capacitance and lowest charge-transfer resistance, attributed to its balanced crystallinity and optimized ion transport pathways. When used as a cathode in an asymmetric NiFe₂O₄//activated carbon CDI cell, the NF<sub>450</sub> electrode achieved a remarkable salt adsorption capacity of 34.8 mg g<sup>−1</sup> at 1.4 <em>V</em>, with superior charge efficiency (>90%) and nearly 100% capacitance retention over 150 cycles. To the best of our knowledge, this represents the highest reported cycle stability and charge efficiency for a spinel-based electrode in a traditional CDI configuration. These findings underscore the potential of morphology-engineered NiFe₂O₄ as a durable and high-performance electrode material for next-generation electrochemical desalination systems.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"384 ","pages":"Article 136353"},"PeriodicalIF":9.0,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145674071","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 : 2025-12-03DOI: 10.1016/j.seppur.2025.136306
Fabiola Alcalde-Garcia, Jason Robert Tavares, Marie-Josée Dumont
{"title":"Epichlorohydrin-crosslinked chitosan hydrogels as recyclable adsorbents for phosphate removal from aqueous solutions and municipal wastewater","authors":"Fabiola Alcalde-Garcia, Jason Robert Tavares, Marie-Josée Dumont","doi":"10.1016/j.seppur.2025.136306","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136306","url":null,"abstract":"","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"29 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658102","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 : 2025-12-03DOI: 10.1016/j.seppur.2025.136301
Youyu Duan , Tao Yan , Yuhan Li , Zeyong Meng , Bicheng Zhu , Yi Zhang , Xuxu Zheng
Toluene (C7H8), characteristic of stable aromatic ring and inert C(sp3)–H bond, is a typical refractory volatile organic compound (VOC). Activating O2 for deep C7H8 mineralization under mild conditions remains a key challenge. Herein, an efficient indium-doped strontium stannate hydroxide photocatalyst (SSH-In60) was synthesized via a simple microwave-assisted method, exhibiting a remarkably high mineralization efficiency of 98.2 % for C7H8 to CO2 at room temperature. Structural characterizations and theoretical simulation calculations revealed that doped In atoms replaced Sr sites, forming localized electron-rich regions and modulating the surface electronic structures. The strong InO2 orbital hybridization significantly enhanced O2 adsorption and increased surface electron transfer by ∼4-fold, promoting superoxide radicals (∙O2−) generation. Furthermore, In doping regulates the synergistic adsorption of multiple reactants (C7H8, O2 and H2O) via surface charge redistribution, particularly improving C7H8 adsorption via covalent interaction. Consequently, The deep C7H8 oxidation involving “C7H8→benzyl alcohol→benzaldehyde→benzoic acid→CO2/H2O” pathway was significantly accelerated with suppressed phenolic byproducts. This work offers novel mechanistic insights and a facile strategy for designing efficient and robust photocatalysts for environmentally-friendly VOC treatment.
{"title":"Insights into boosting molecular oxygen activation and deep toluene mineralization over in-doped SrSn(OH)6 photocatalyst via regulating orbital hybridization and charge redistribution","authors":"Youyu Duan , Tao Yan , Yuhan Li , Zeyong Meng , Bicheng Zhu , Yi Zhang , Xuxu Zheng","doi":"10.1016/j.seppur.2025.136301","DOIUrl":"10.1016/j.seppur.2025.136301","url":null,"abstract":"<div><div>Toluene (C<sub>7</sub>H<sub>8</sub>), characteristic of stable aromatic ring and inert C(sp<sup>3</sup>)–H bond, is a typical refractory volatile organic compound (VOC). Activating O<sub>2</sub> for deep C<sub>7</sub>H<sub>8</sub> mineralization under mild conditions remains a key challenge. Herein, an efficient indium-doped strontium stannate hydroxide photocatalyst (SSH-In60) was synthesized <em>via</em> a simple microwave-assisted method, exhibiting a remarkably high mineralization efficiency of 98.2 % for C<sub>7</sub>H<sub>8</sub> to CO<sub>2</sub> at room temperature. Structural characterizations and theoretical simulation calculations revealed that doped In atoms replaced Sr sites, forming localized electron-rich regions and modulating the surface electronic structures. The strong In<img>O<sub>2</sub> orbital hybridization significantly enhanced O<sub>2</sub> adsorption and increased surface electron transfer by ∼4-fold, promoting superoxide radicals (∙O<sub>2</sub><sup>−</sup>) generation. Furthermore, In doping regulates the synergistic adsorption of multiple reactants (C<sub>7</sub>H<sub>8</sub>, O<sub>2</sub> and H<sub>2</sub>O) <em>via</em> surface charge redistribution, particularly improving C<sub>7</sub>H<sub>8</sub> adsorption <em>via</em> covalent interaction. Consequently, The deep C<sub>7</sub>H<sub>8</sub> oxidation involving “C<sub>7</sub>H<sub>8</sub>→benzyl alcohol→benzaldehyde→benzoic acid→CO<sub>2</sub>/H<sub>2</sub>O” pathway was significantly accelerated with suppressed phenolic byproducts. This work offers novel mechanistic insights and a facile strategy for designing efficient and robust photocatalysts for environmentally-friendly VOC treatment.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"385 ","pages":"Article 136301"},"PeriodicalIF":9.0,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658325","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 : 2025-12-03DOI: 10.1016/j.seppur.2025.136351
Boqiong Jiang, Keyan Wei, Jingxuan Zhou, Kai Xu, Jun Liu, Qi Feng, Jingyi Han, Yi Zhang, Shaocai Yu, Yuhai Sun
In this study, a highly efficient Ru-modified Cr2O3 catalyst derived from MIL-101(Cr) (denoted as Rux/Cr2O3-MIL) was developed for chlorobenzene oxidation. With Ru modification, this catalyst exhibits exceptional performance in chlorobenzene oxidation. Notably, the Ru1/Cr2O3-MIL catalyst with 1 % Ru loading achieves 90 % chlorobenzene conversion at 221 °C, accompanied by an impressive CO2 selectivity of 96.25 %. Characterization studies revealed that Ru loading facilitates the formation of a Ru-O-Cr bridge structure. This distinctive structure introduced new adsorption sites, endowing the catalyst with a significantly higher chlorobenzene adsorption capacity than that provided by Brønsted acid. The Ru-O-Cr bridge also served as an “oxygen transport channel”, facilitating the migration of lattice oxygen from Cr3+/Cr2O3 to the Ru4+/Cr6+ active centers. Simultaneously, the formation of numerous oxygen vacancies enhanced the activity of surface Oads, enabling their participation in the reaction at lower temperatures. Mechanistic investigations further revealed that the Ru-O-Cr bridge performed a significant influence on the reaction pathway: after chlorobenzene was converted to phenol, this structure promoted para-oxidation, preferentially forming p-benzoquinone over o-benzoquinone to facilitate the generation of maleate, an easily degradable intermediate. Subsequently, the Ru-O-Cr bridge activated lattice oxygen, and the enhanced surface oxygen species accelerated the conversion of the maleate to acetate and formate, ultimately enhancing the complete oxidation of chlorobenzene.
本研究以MIL-101（Cr）为原料，开发了一种高效的ru改性Cr2O3催化剂（记为Rux/Cr2O3- mil），用于氯苯氧化。钌改性后，该催化剂在氯苯氧化中表现出优异的性能。值得注意的是，Ru负载为1 %的Ru1/Cr2O3-MIL催化剂在221 °C下达到90 %的氯苯转化率，并伴有令人印象深刻的96.25 %的CO2选择性。表征研究表明，Ru加载促进了Ru- o - cr桥结构的形成。这种独特的结构引入了新的吸附位点，使催化剂具有比Brønsted酸更高的氯苯吸附能力。Ru-O-Cr桥还作为“氧传输通道”，促进晶格氧从Cr3+/Cr2O3向Ru4+/Cr6+活性中心迁移。同时，大量氧空位的形成增强了表面负载的活性，使它们能够在较低温度下参与反应。机理研究进一步表明，Ru-O-Cr桥对反应途径有显著影响：在氯苯转化为苯酚后，这种结构促进了对氧化，优先生成对苯醌而不是对苯醌，从而促进了马来酸盐的生成，这是一种易于降解的中间体。随后，Ru-O-Cr桥激活了晶格氧，增强的表面氧加速了马来酸盐向醋酸盐和甲酸盐的转化，最终促进了氯苯的完全氧化。
{"title":"The promotional effect of Ru-O-Cr oxygen bridge on chlorobenzene oxidation over Rux/Cr2O3-MIL catalysts: New sites for adsorption and deep oxidation","authors":"Boqiong Jiang, Keyan Wei, Jingxuan Zhou, Kai Xu, Jun Liu, Qi Feng, Jingyi Han, Yi Zhang, Shaocai Yu, Yuhai Sun","doi":"10.1016/j.seppur.2025.136351","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136351","url":null,"abstract":"In this study, a highly efficient Ru-modified Cr<sub>2</sub>O<sub>3</sub> catalyst derived from MIL-101(Cr) (denoted as Ru<sub>x</sub>/Cr<sub>2</sub>O<sub>3</sub>-MIL) was developed for chlorobenzene oxidation. With Ru modification, this catalyst exhibits exceptional performance in chlorobenzene oxidation. Notably, the Ru<sub>1</sub>/Cr<sub>2</sub>O<sub>3</sub>-MIL catalyst with 1 % Ru loading achieves 90 % chlorobenzene conversion at 221 °C, accompanied by an impressive CO<sub>2</sub> selectivity of 96.25 %. Characterization studies revealed that Ru loading facilitates the formation of a Ru-O-Cr bridge structure. This distinctive structure introduced new adsorption sites, endowing the catalyst with a significantly higher chlorobenzene adsorption capacity than that provided by Brønsted acid. The Ru-O-Cr bridge also served as an “oxygen transport channel”, facilitating the migration of lattice oxygen from Cr<sup>3+</sup>/Cr<sub>2</sub>O<sub>3</sub> to the Ru<sup>4+</sup>/Cr<sup>6+</sup> active centers. Simultaneously, the formation of numerous oxygen vacancies enhanced the activity of surface O<sub>ads</sub>, enabling their participation in the reaction at lower temperatures. Mechanistic investigations further revealed that the Ru-O-Cr bridge performed a significant influence on the reaction pathway: after chlorobenzene was converted to phenol, this structure promoted para-oxidation, preferentially forming p-benzoquinone over o-benzoquinone to facilitate the generation of maleate, an easily degradable intermediate. Subsequently, the Ru-O-Cr bridge activated lattice oxygen, and the enhanced surface oxygen species accelerated the conversion of the maleate to acetate and formate, ultimately enhancing the complete oxidation of chlorobenzene.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"7 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658315","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 : 2025-12-02DOI: 10.1016/j.seppur.2025.136307
Yue Cao , Haining Liu , Zhiyue Han , Lirong Guo , Naicai Xu , Yanping Wang , Shaoju Bian
Efficient recovery of rubidium (Rb+) and cesium (Cs+) from salt-lake brines is of great significance due to their strategic importance and limited natural abundance. Herein, an environmentally benign tannic acid‑iron coordination complex (TA-Fe) was synthesized via a facile one-step assembly route for rapid and efficient adsorption of Rb+ and Cs+ from aqueous solutions. The physicochemical properties of TA-Fe were systematically characterized using SEM-EDS, XRD, FT-IR, BET, TGA and XPS analyses. The adsorption kinetics and isotherms indicated that Rb+ and Cs+ adsorption followed a pseudo-second-order kinetic model and fitted well with the Langmuir isotherm, suggesting a monolayer chemisorption mechanism. Remarkably, TA-Fe achieves adsorption equilibrium within 60 min, exhibiting maximum adsorption capacities of 0.759 mmol·g−1 for Rb+ and 0.953 mmol·g−1 for Cs+ at 298 K. Thermodynamic parameters confirmed the spontaneous and exothermic nature of the adsorption process. Furthermore, TA-Fe retained over 88 % of its initial adsorption capacity after five adsorption-desorption cycles (Rb+: 94.06 %, Cs+: 88.34 %), highlighting its excellent stability and reusability. This study demonstrates that TA-Fe is a promising adsorbent for the fast efficient extraction of Rb+ and Cs+ from aqueous solutions.
{"title":"Rapid and efficient adsorptive recovery of rubidium and cesium ions by a green tannic acid-iron coordination complex","authors":"Yue Cao , Haining Liu , Zhiyue Han , Lirong Guo , Naicai Xu , Yanping Wang , Shaoju Bian","doi":"10.1016/j.seppur.2025.136307","DOIUrl":"10.1016/j.seppur.2025.136307","url":null,"abstract":"<div><div>Efficient recovery of rubidium (Rb<sup>+</sup>) and cesium (Cs<sup>+</sup>) from salt-lake brines is of great significance due to their strategic importance and limited natural abundance. Herein, an environmentally benign tannic acid‑iron coordination complex (TA-Fe) was synthesized via a facile one-step assembly route for rapid and efficient adsorption of Rb<sup>+</sup> and Cs<sup>+</sup> from aqueous solutions. The physicochemical properties of TA-Fe were systematically characterized using SEM-EDS, XRD, FT-IR, BET, TGA and XPS analyses. The adsorption kinetics and isotherms indicated that Rb<sup>+</sup> and Cs<sup>+</sup> adsorption followed a pseudo-second-order kinetic model and fitted well with the Langmuir isotherm, suggesting a monolayer chemisorption mechanism. Remarkably, TA-Fe achieves adsorption equilibrium within 60 min, exhibiting maximum adsorption capacities of 0.759 mmol·g<sup>−1</sup> for Rb<sup>+</sup> and 0.953 mmol·g<sup>−1</sup> for Cs<sup>+</sup> at 298 K. Thermodynamic parameters confirmed the spontaneous and exothermic nature of the adsorption process. Furthermore, TA-Fe retained over 88 % of its initial adsorption capacity after five adsorption-desorption cycles (Rb<sup>+</sup>: 94.06 %, Cs<sup>+</sup>: 88.34 %), highlighting its excellent stability and reusability. This study demonstrates that TA-Fe is a promising adsorbent for the fast efficient extraction of Rb<sup>+</sup> and Cs<sup>+</sup> from aqueous solutions.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"384 ","pages":"Article 136307"},"PeriodicalIF":9.0,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145658320","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 : 2025-12-02DOI: 10.1016/j.seppur.2025.136218
Xingguang Hao , Ying Zhu , Kai Li , Fei Wang , Shuangyou Bao , Xin Sun , Lei Shi , Ping Ning
In the metallurgical industry, traditional methods for treating high arsenic wastewater required reagents and generate hazardous waste. The recovery of arsenic trioxide (As2O3) from arsenic-rich wastewater was critical for both pollution mitigation and resource reclamation. Herein, a high-concentration H2SO4 static (HCHS) method was used to recovery As2O3. The recovery efficiency was found to depend not on flow rate or gaseous As2O3 concentration, but on H2SO4 concentration. Besides, the kinetics of As2O3 recovery followed a pseudo-second-order model, with an activation energy of 39.99 kJ/mol. Raman spectroscopy revealed that H2SO4 promoted the formation of trihedrally coordinated interface water with fewer H-down configurations, weakening contact with As2O3 surface. Constrained ab initio molecular dynamics (AIMD) simulations demonstrated that two H2SO4 molecules stabilized interface water into a one-H-down configuration. Density functional theory (DFT) calculations with implicit solvation revealed that the H2O primally absorbed at H-OIV bridge site, with an adsorption energy of −0.28 eV. Hence, H2SO4 molecules induced interface water reorientation at the solid/liquid interface. This reorientation weakened water-As2O3 binding, thereby inhibiting the formation of H3AsO3 and improving As2O3 recovery efficiency. This work provides mechanistic insights into As2O3 recovery and offers a sustainable approach for wastewater treatment and resource recycling.
{"title":"Tuning interface water dynamics with H2SO4: A route to recovery As2O3 from arsenic-rich wastewater","authors":"Xingguang Hao , Ying Zhu , Kai Li , Fei Wang , Shuangyou Bao , Xin Sun , Lei Shi , Ping Ning","doi":"10.1016/j.seppur.2025.136218","DOIUrl":"10.1016/j.seppur.2025.136218","url":null,"abstract":"<div><div>In the metallurgical industry, traditional methods for treating high arsenic wastewater required reagents and generate hazardous waste. The recovery of arsenic trioxide (As<sub>2</sub>O<sub>3</sub>) from arsenic-rich wastewater was critical for both pollution mitigation and resource reclamation. Herein, a high-concentration H<sub>2</sub>SO<sub>4</sub> static (HCHS) method was used to recovery As<sub>2</sub>O<sub>3</sub>. The recovery efficiency was found to depend not on flow rate or gaseous As<sub>2</sub>O<sub>3</sub> concentration, but on H<sub>2</sub>SO<sub>4</sub> concentration. Besides, the kinetics of As<sub>2</sub>O<sub>3</sub> recovery followed a pseudo-second-order model, with an activation energy of 39.99 kJ/mol. Raman spectroscopy revealed that H<sub>2</sub>SO<sub>4</sub> promoted the formation of trihedrally coordinated interface water with fewer H-down configurations, weakening contact with As<sub>2</sub>O<sub>3</sub> surface. Constrained ab initio molecular dynamics (AIMD) simulations demonstrated that two H<sub>2</sub>SO<sub>4</sub> molecules stabilized interface water into a one-H-down configuration. Density functional theory (DFT) calculations with implicit solvation revealed that the H<sub>2</sub>O primally absorbed at H-O<sub>IV</sub> bridge site, with an adsorption energy of −0.28 eV. Hence, H<sub>2</sub>SO<sub>4</sub> molecules induced interface water reorientation at the solid/liquid interface. This reorientation weakened water-As<sub>2</sub>O<sub>3</sub> binding, thereby inhibiting the formation of H<sub>3</sub>AsO<sub>3</sub> and improving As<sub>2</sub>O<sub>3</sub> recovery efficiency. This work provides mechanistic insights into As<sub>2</sub>O<sub>3</sub> recovery and offers a sustainable approach for wastewater treatment and resource recycling.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"384 ","pages":"Article 136218"},"PeriodicalIF":9.0,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145651434","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}
Composite membranes, which consist of a multi-layer membrane structure comprising an ultra-thin dense separation layer and a porous support layer, are used for gas separation. However, issues such as poor adhesion between layers often arise. In this study, a novel reverse-induced diffusion method was employed to achieve the in situ growth of a covalent organic framework COF (TaPa-1) on one side of polyacrylonitrile (PAN) at room temperature, resulting in the formation of a tightly bonded gutter layer. Subsequently, a metal-organic framework MOF (NH2-ZIF-8) was secondarily grown in situ on the TaPa-1 membrane to prepare a PAN/COF-MOF composite membrane with stable interlayer bonding. The TaPa-1 layer, with high gas permeability, and the NH2-ZIF-8 layer due to sheltering effect, with high gas selectivity, act synergistically to enable efficient gas sieving and rapid transport. When treating simulated flue gas (CO₂/N₂ = 1:4), the gas separation selectivity of the PAN/COF-MOF composite membrane reach 29.9, with a CO₂ permeability of 825 GPU, achieving excellent CO₂ separation performance. In this study, the PAN/COF-MOF composite membrane is constructed using the reverse-induced diffusion method, achieving stable interlayer bonding and synergistic separation, demonstrating excellent CO₂ permeability and selectivity.
{"title":"Continuous interface-coupled COF-MOF membranes for precise CO₂/N₂ gas sieving","authors":"Qingping Xin , Zhaoqi Qu , Xinghui Zhang , Xingwei Wang , Jiaxin Wu , Dengdi Wu , Wei Huang , Mengke Wang , Ningning Gao , Xiaoli Ding , Yuzhong Zhang","doi":"10.1016/j.seppur.2025.136304","DOIUrl":"10.1016/j.seppur.2025.136304","url":null,"abstract":"<div><div>Composite membranes, which consist of a multi-layer membrane structure comprising an ultra-thin dense separation layer and a porous support layer, are used for gas separation. However, issues such as poor adhesion between layers often arise. In this study, a novel reverse-induced diffusion method was employed to achieve the in situ growth of a covalent organic framework COF (TaPa-1) on one side of polyacrylonitrile (PAN) at room temperature, resulting in the formation of a tightly bonded gutter layer. Subsequently, a metal-organic framework MOF (NH<sub>2</sub>-ZIF-8) was secondarily grown in situ on the TaPa-1 membrane to prepare a PAN/COF-MOF composite membrane with stable interlayer bonding. The TaPa-1 layer, with high gas permeability, and the NH<sub>2</sub>-ZIF-8 layer due to sheltering effect, with high gas selectivity, act synergistically to enable efficient gas sieving and rapid transport. When treating simulated flue gas (CO₂/N₂ = 1:4), the gas separation selectivity of the PAN/COF-MOF composite membrane reach 29.9, with a CO₂ permeability of 825 GPU, achieving excellent CO₂ separation performance. In this study, the PAN/COF-MOF composite membrane is constructed using the reverse-induced diffusion method, achieving stable interlayer bonding and synergistic separation, demonstrating excellent CO₂ permeability and selectivity.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"385 ","pages":"Article 136304"},"PeriodicalIF":9.0,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145651435","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 : 2025-12-02DOI: 10.1016/j.seppur.2025.136319
Neng Wei, Yaqun He, Guangwen Zhang, Jinyan Liu, Yi Feng, Zuomin Li, Weiran Zuo
The efficient recycling of spent lithium-ion batteries (LIBs) represents both an environmental imperative and a critical strategy for resource sustainability. This study proposes an innovative integrated process combining in-situ thermal reduction with mild electrochemical leaching to recover valuable metals from industrial mixed electrode powders. The in-situ thermal reduction successfully decomposed the layered cathode material using internal reducing agents, enabling 73.4 % Li preferential extraction via water leaching. Subsequent electrochemical leaching leached out 99.27 % Li, 95.99 % Ni, 98.68 % Co, 99.01 % Mn, 94.47 % Al, and 92.31 % Cu under optimal conditions of 60 g/L slurry concentration, 0.3 M H2SO4, 0.7 A, 60 min, room temperature. The electrochemical method showed clear advantages over conventional acid leaching, particularly in dissolving metallic phases of Ni, Co and Cu, through a multi-path oxidation mechanism. This process demonstrates exceptional adaptability to complex industrial feedstocks under mild conditions while successfully addressing the challenge of over-reduced metallic phases in battery recycling.
{"title":"Recycling valuable metals from spent lithium-ion batteries by an integrated in-situ thermal reduction and electrochemical leaching strategy","authors":"Neng Wei, Yaqun He, Guangwen Zhang, Jinyan Liu, Yi Feng, Zuomin Li, Weiran Zuo","doi":"10.1016/j.seppur.2025.136319","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136319","url":null,"abstract":"The efficient recycling of spent lithium-ion batteries (LIBs) represents both an environmental imperative and a critical strategy for resource sustainability. This study proposes an innovative integrated process combining in-situ thermal reduction with mild electrochemical leaching to recover valuable metals from industrial mixed electrode powders. The in-situ thermal reduction successfully decomposed the layered cathode material using internal reducing agents, enabling 73.4 % Li preferential extraction via water leaching. Subsequent electrochemical leaching leached out 99.27 % Li, 95.99 % Ni, 98.68 % Co, 99.01 % Mn, 94.47 % Al, and 92.31 % Cu under optimal conditions of 60 g/L slurry concentration, 0.3 M H<sub>2</sub>SO<sub>4</sub>, 0.7 A, 60 min, room temperature. The electrochemical method showed clear advantages over conventional acid leaching, particularly in dissolving metallic phases of Ni, Co and Cu, through a multi-path oxidation mechanism. This process demonstrates exceptional adaptability to complex industrial feedstocks under mild conditions while successfully addressing the challenge of over-reduced metallic phases in battery recycling.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"9 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145651451","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 : 2025-12-02DOI: 10.1016/j.seppur.2025.136316
Niloofar Salehpour, Saeed Nojavan
Efficiently implementing technologies for enantiomeric resolution in the pharmaceutical industry presents a significant challenge, given that chiral compounds are known for their distinct and critical biological activities. Here, a novel chiral composite, carboxymethyl maltodextrin-functionalized layered double hydroxide (CMMD/MgAl-LDH), was developed and evaluated for ibuprofen enantiomers separation using multiple operational modes such as batch adsorption, cartridge, and circulatory enantioseparation systems. The CMMD/MgAl-LDH exhibited strong chiral recognition and selective adsorption capabilities, highlighting its effectiveness as a chiral selector with enantioseparation efficiencies of 27.06 %, 34.57 %, and 42.24 % across the respective methods. Building on this, a mixed matrix membrane (MMM) was fabricated by incorporating CMMD/MgAl-LDH into a polyethylene glycol-cellulose triacetate (PEG-CTA) matrix, resulting in enhanced enantioselective separation performance. Characterization techniques confirmed the composite's successful synthesis and stable integration into the membrane. Comparative evaluation revealed that the CMMD/MgAl-LDH/PEG-CTA MMM outperformed CMMD/MgAl-LDH alone, achieving an enantiomeric excess (e.e.) of approximately 56.32 % and a permeability rate of 10.88 mmol m−2 h−1, along with excellent mechanical and chemical stability. Further investigations validated the suitability of MMM as an effective enantioseparation mode for chiral amino acids, phenylalanine and tryptophan, achieving excellent e.e. values of 98.52 % and 85.71 %, respectively. Molecular docking simulation and empirical investigations clarified the retarded transport mechanisms, highlighting the pivotal contribution of various hydrogen bonding, hydrophobic and electrostatic interactions, enabling effective enantiomeric discrimination. This study presents a promising approach combining novel chiral composite materials and membrane technology for advanced analytical applications in pharmaceutical enantiomer resolution.
{"title":"Chiral carboxymethyl maltodextrin-functionalized MgAl-layered double hydroxide composite: an efficient material for enantioseparation of ibuprofen and amino acids via multimode operational techniques","authors":"Niloofar Salehpour, Saeed Nojavan","doi":"10.1016/j.seppur.2025.136316","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.136316","url":null,"abstract":"Efficiently implementing technologies for enantiomeric resolution in the pharmaceutical industry presents a significant challenge, given that chiral compounds are known for their distinct and critical biological activities. Here, a novel chiral composite, carboxymethyl maltodextrin-functionalized layered double hydroxide (CMMD/MgAl-LDH), was developed and evaluated for ibuprofen enantiomers separation using multiple operational modes such as batch adsorption, cartridge, and circulatory enantioseparation systems. The CMMD/MgAl-LDH exhibited strong chiral recognition and selective adsorption capabilities, highlighting its effectiveness as a chiral selector with enantioseparation efficiencies of 27.06 %, 34.57 %, and 42.24 % across the respective methods. Building on this, a mixed matrix membrane (MMM) was fabricated by incorporating CMMD/MgAl-LDH into a polyethylene glycol-cellulose triacetate (PEG-CTA) matrix, resulting in enhanced enantioselective separation performance. Characterization techniques confirmed the composite's successful synthesis and stable integration into the membrane. Comparative evaluation revealed that the CMMD/MgAl-LDH/PEG-CTA MMM outperformed CMMD/MgAl-LDH alone, achieving an enantiomeric excess (e.e.) of approximately 56.32 % and a permeability rate of 10.88 mmol m<sup>−2</sup> h<sup>−1</sup>, along with excellent mechanical and chemical stability. Further investigations validated the suitability of MMM as an effective enantioseparation mode for chiral amino acids, phenylalanine and tryptophan, achieving excellent e.e. values of 98.52 % and 85.71 %, respectively. Molecular docking simulation and empirical investigations clarified the retarded transport mechanisms, highlighting the pivotal contribution of various hydrogen bonding, hydrophobic and electrostatic interactions, enabling effective enantiomeric discrimination. This study presents a promising approach combining novel chiral composite materials and membrane technology for advanced analytical applications in pharmaceutical enantiomer resolution.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"28 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145657883","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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