Pub Date : 2025-01-25DOI: 10.1016/j.seppur.2025.131774
Yuhong Lin, Wei Zheng, Anjun Ma, Hailong Li
Mechanochemical elemental sulfur-modified petroleum coke (MC-ES-PC) exhibits excellent elemental mercury (Hg0) removal from coal-fired flue gas in previous works. However, the detailed removal process and relevant Hg0 uptake mechanism have not been sufficiently elucidated or discussed. In this work, kinetic and isothermal adsorption equilibria were performed to analyze the mercury mechanism of MC-ES-PC sorbents under various flue gas components at different temperatures. The results showed that chemical adsorption, external mass transfer, and intraparticle diffusion occurred during Hg0 immobilization, and they were dominated by chemisorption. Additionally, a gas–solid adsorption equilibrium model for the equilibrium Hg0 concentration and adsorption time was established based on the solid–liquid adsorption model, and adsorption equilibrium was divided into several reaction stages by time. The Langmuir and Freundlich models were found to be more suitable for describing Hg0 adsorption process of MC-ES-PC, which implies that Hg0 adsorption was primarily controlled by its oxidation. This work provides valuable insights into Hg0 adsorption mechanism of typical adsorbents.
{"title":"Kinetic and isothermal adsorption equilibrium on mercury removal by Mechanochemical elemental sulfur modified petroleum coke","authors":"Yuhong Lin, Wei Zheng, Anjun Ma, Hailong Li","doi":"10.1016/j.seppur.2025.131774","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131774","url":null,"abstract":"Mechanochemical elemental sulfur-modified petroleum coke (MC-ES-PC) exhibits excellent elemental mercury (Hg<sup>0</sup>) removal from coal-fired flue gas in previous works. However, the detailed removal process and relevant Hg<sup>0</sup> uptake mechanism have not been sufficiently elucidated or discussed. In this work, kinetic and isothermal adsorption equilibria were performed to analyze the mercury mechanism of MC-ES-PC sorbents under various flue gas components at different temperatures. The results showed that chemical adsorption, external mass transfer, and intraparticle diffusion occurred during Hg<sup>0</sup> immobilization, and they were dominated by chemisorption. Additionally, a gas–solid adsorption equilibrium model for the equilibrium Hg<sup>0</sup> concentration and adsorption time was established based on the solid–liquid adsorption model, and adsorption equilibrium was divided into several reaction stages by time. The Langmuir and Freundlich models were found to be more suitable for describing Hg<sup>0</sup> adsorption process of MC-ES-PC, which implies that Hg<sup>0</sup> adsorption was primarily controlled by its oxidation. This work provides valuable insights into Hg<sup>0</sup> adsorption mechanism of typical adsorbents.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"61 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031348","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}
Metal-free catalysts featuring nitrogen defects have been developed rapidly in peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) for treating the organic wastewater. While a great deal of research has been conducted on the doped N sites such as pyridinic N, pyrrolic N and graphitic N, less attention has been paid to the role of modified N site (amino group) due to the low catalytic activity. To investigate the original activity of amino group over carbon, in this work, we selected two typical supports including a carbon support (graphene oxide) and a non-carbon support (silica), and subsequently functionalized both with amino groups. The phenol degradation performances in PMS-AOPs revealed that only amino-functionalized reduced graphene oxide could activate PMS, thus achieving the pollutant removal. To better understand the structure–activity relationship between amino groups and carbon supports, we enhanced the degree of reduction of graphene oxide by raising the synthesis temperature during amino group modification. Activity evaluation, reactive oxygen species analysis and density functional theory simulations demonstrated that as the content of hydroxyl groups decreased, both the adsorption and electron transfer of reactants were enhanced, thereby enhancing the contribution of non-radical pathway. Through this facile regulation of synthesis temperatures, the reaction rate constant for phenol degradation in PMS-AOPs using aminated graphene increased by approximately 4.8 times. This work provides a new insight into designing the efficient catalyst with amino sites for PMS-AOPs.
{"title":"Investigating the original activity of amino group over carbon in peroxymonosulfate-based advanced oxidation processes","authors":"Shuo Yang, Na Tang, Luwei Deng, Yongsheng Xu, Xiaomeng Guo, Yupu Bai, Wenchao Peng, Haiyang Zhang, Jinli Zhang","doi":"10.1016/j.seppur.2025.131808","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131808","url":null,"abstract":"Metal-free catalysts featuring nitrogen defects have been developed rapidly in peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) for treating the organic wastewater. While a great deal of research has been conducted on the doped N sites such as pyridinic N, pyrrolic N and graphitic N, less attention has been paid to the role of modified N site (amino group) due to the low catalytic activity. To investigate the original activity of amino group over carbon, in this work, we selected two typical supports including a carbon support (graphene oxide) and a non-carbon support (silica), and subsequently functionalized both with amino groups. The phenol degradation performances in PMS-AOPs revealed that only amino-functionalized reduced graphene oxide could activate PMS, thus achieving the pollutant removal. To better understand the structure–activity relationship between amino groups and carbon supports, we enhanced the degree of reduction of graphene oxide by raising the synthesis temperature during amino group modification. Activity evaluation, reactive oxygen species analysis and density functional theory simulations demonstrated that as the content of hydroxyl groups decreased, both the adsorption and electron transfer of reactants were enhanced, thereby enhancing the contribution of non-radical pathway. Through this facile regulation of synthesis temperatures, the reaction rate constant for phenol degradation in PMS-AOPs using aminated graphene increased by approximately 4.8 times. This work provides a new insight into designing the efficient catalyst with amino sites for PMS-AOPs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"58 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031252","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 : 2025-01-25DOI: 10.1016/j.seppur.2025.131760
Can Liu, Xinru Li, Haojie Ge, Xiaoping Yu, Yafei Guo, Tianlong Deng
The extreme pH and complex composition of radioactive wastewater pose great challenges to the chemical stability and properties of adsorbents. Herein, three kinds of metal-doped tin sulfides were developed by a simple one-pot method for cesium removal. DFT calculations combined with experiments were conducted to reveal their structures, stability, and adsorption properties. It was found that the crystal structures of tin sulfide became more stable after doping by Ni and Al. Particularly, the Al-doped material (NAlSS) exhibited the highest stability and adsorption performance because of the highest −COHP value of the Sn-S bond in NAlSS and the low binding energy between NAlSS and Cs+. The industrial application of the powdery NAlSS was further solved by wet spinning using glutaraldehyde cross-linked sodium alginate and hydroxyethyl cellulose (SHG) as the supporters. The obtained salt-resistant hydrogel fibers (SHG-NAlSS) exhibited excellent adsorption performance and stability in wide pH (2 ∼ 12) and temperature (298.15 ∼ 328.15 K) ranges. The maximum adsorption capacity reached 401.34 mg·g−1 within 10 min. The material was successfully applied for Cs+ removal from wastewater, and the distribution coefficient of Cs+ reached 255020.33 mL·g−1. After 10 adsorption–desorption cycles, the adsorbent maintained good stability. These results, along with the fixed-bed adsorption, demonstrate that the developed material can be used as a candidate for Cs+ removal from radioactive wastewater.
{"title":"Selective removal of cesium from wastewater by salt-resistant hydrogel fiber-supported Al-doped tin sulfide","authors":"Can Liu, Xinru Li, Haojie Ge, Xiaoping Yu, Yafei Guo, Tianlong Deng","doi":"10.1016/j.seppur.2025.131760","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131760","url":null,"abstract":"The extreme pH and complex composition of radioactive wastewater pose great challenges to the chemical stability and properties of adsorbents. Herein, three kinds of metal-doped tin sulfides were developed by a simple one-pot method for cesium removal. DFT calculations combined with experiments were conducted to reveal their structures, stability, and adsorption properties. It was found that the crystal structures of tin sulfide became more stable after doping by Ni and Al. Particularly, the Al-doped material (NAlSS) exhibited the highest stability and adsorption performance because of the highest −COHP value of the Sn-S bond in NAlSS and the low binding energy between NAlSS and Cs<sup>+</sup>. The industrial application of the powdery NAlSS was further solved by wet spinning using glutaraldehyde cross-linked sodium alginate and hydroxyethyl cellulose (SHG) as the supporters. The obtained salt-resistant hydrogel fibers (SHG-NAlSS) exhibited excellent adsorption performance and stability in wide pH (2 ∼ 12) and temperature (298.15 ∼ 328.15 K) ranges. The maximum adsorption capacity reached 401.34 mg·g<sup>−1</sup> within 10 min. The material was successfully applied for Cs<sup>+</sup> removal from wastewater, and the distribution coefficient of Cs<sup>+</sup> reached 255020.33 mL·g<sup>−1</sup>. After 10 adsorption–desorption cycles, the adsorbent maintained good stability. These results, along with the fixed-bed adsorption, demonstrate that the developed material can be used as a candidate for Cs<sup>+</sup> removal from radioactive wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"25 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031253","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}
A gas–liquid pulse-modulated plasma with bubbling coupled with plasma-derived heat system was developed for efficient degradation of octadecylamine (ODA) and 4-dodecylmorpholine (DMP). The structure–activity relationship between high-voltage electrode structures and the degradation activity of ODA and DMP was delved into using fluid dynamics simulations. The crucial role of bubbling is evident in the enhancement of ODA and DMP degradation efficiencies by 100 % and 47 % within 30 min, respectively. ODA and DMP degradation efficiencies reached 96 % and 100 % with treatment of 30 min, respectively, accompanied by a high mineralization efficiency of 80 %. An in-depth analysis was performed on the evolution of the physicochemical properties of the reaction solution during degradation. The plasma coupled with plasma-derived heat system exhibited remarkable synergistic effects, achieving synergistic intensities of 0.96 for ODA and 1.28 for DMP, with energy efficiencies increased by 31 % and 16 %. Analysis of the evolution of total nitrogen and nitrogen-containing species revealed that ODA and DMP degradation commenced with the decomposition of amino groups, ultimately converting them into <span><span><math><mrow is="true"><mi is="true" mathvariant="normal">N</mi><msubsup is="true"><mi is="true" mathvariant="normal">O</mi><mrow is="true"><mn is="true">3</mn></mrow><mo is="true">-</mo></msubsup></mrow></math></span><script type="math/mml"><math><mrow is="true"><mi mathvariant="normal" is="true">N</mi><msubsup is="true"><mi mathvariant="normal" is="true">O</mi><mrow is="true"><mn is="true">3</mn></mrow><mo is="true">-</mo></msubsup></mrow></math></script></span> and <span><span><math><mrow is="true"><mi is="true" mathvariant="normal">N</mi><msubsup is="true"><mi is="true" mathvariant="normal">H</mi><mrow is="true"><mn is="true">4</mn></mrow><mo is="true">+</mo></msubsup></mrow></math></span><script type="math/mml"><math><mrow is="true"><mi mathvariant="normal" is="true">N</mi><msubsup is="true"><mi mathvariant="normal" is="true">H</mi><mrow is="true"><mn is="true">4</mn></mrow><mo is="true">+</mo></msubsup></mrow></math></script></span>. Quenching tests and electron spin resonance characterization confirmed the generation of <span><span><math><mrow is="true"><mo is="true">·</mo><mi is="true" mathvariant="normal">O</mi><mi is="true" mathvariant="normal">H</mi></mrow></math></span><script type="math/mml"><math><mrow is="true"><mo is="true">·</mo><mi mathvariant="normal" is="true">O</mi><mi mathvariant="normal" is="true">H</mi></mrow></math></script></span>, <span><span><math><mrow is="true"><msup is="true"><mrow is="true"><mspace is="true" width="0.166667em"></mspace></mrow><mo is="true">·</mo></msup><msubsup is="true"><mi is="true" mathvariant="normal">O</mi><mrow is="true"><mn is="true">2</mn></mrow><mo is="true">-</mo></msubsup></mrow></math></span><script type="math/mml"><math><mrow is="true"><msup is="true"><mrow is="true"><mspace width="0.166667em" is=
{"title":"Gas-liquid pulse-modulated plasma with bubbling concomitant with plasma-derived heat enhanced degradation of the octadecylamine and 4-dodecylmorpholine: Performance and mechanism insight","authors":"Xuri Li, Siyuan Zhang, Liang Ma, Miao Lu, Jingbao Liu, Haining Liu, Zhijian Wu, Xiangmei Cui, Xiushen Ye","doi":"10.1016/j.seppur.2025.131758","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131758","url":null,"abstract":"A gas–liquid pulse-modulated plasma with bubbling coupled with plasma-derived heat system was developed for efficient degradation of octadecylamine (ODA) and 4-dodecylmorpholine (DMP). The structure–activity relationship between high-voltage electrode structures and the degradation activity of ODA and DMP was delved into using fluid dynamics simulations. The crucial role of bubbling is evident in the enhancement of ODA and DMP degradation efficiencies by 100 % and 47 % within 30 min, respectively. ODA and DMP degradation efficiencies reached 96 % and 100 % with treatment of 30 min, respectively, accompanied by a high mineralization efficiency of 80 %. An in-depth analysis was performed on the evolution of the physicochemical properties of the reaction solution during degradation. The plasma coupled with plasma-derived heat system exhibited remarkable synergistic effects, achieving synergistic intensities of 0.96 for ODA and 1.28 for DMP, with energy efficiencies increased by 31 % and 16 %. Analysis of the evolution of total nitrogen and nitrogen-containing species revealed that ODA and DMP degradation commenced with the decomposition of amino groups, ultimately converting them into <span><span><math><mrow is=\"true\"><mi is=\"true\" mathvariant=\"normal\">N</mi><msubsup is=\"true\"><mi is=\"true\" mathvariant=\"normal\">O</mi><mrow is=\"true\"><mn is=\"true\">3</mn></mrow><mo is=\"true\">-</mo></msubsup></mrow></math></span><script type=\"math/mml\"><math><mrow is=\"true\"><mi mathvariant=\"normal\" is=\"true\">N</mi><msubsup is=\"true\"><mi mathvariant=\"normal\" is=\"true\">O</mi><mrow is=\"true\"><mn is=\"true\">3</mn></mrow><mo is=\"true\">-</mo></msubsup></mrow></math></script></span> and <span><span><math><mrow is=\"true\"><mi is=\"true\" mathvariant=\"normal\">N</mi><msubsup is=\"true\"><mi is=\"true\" mathvariant=\"normal\">H</mi><mrow is=\"true\"><mn is=\"true\">4</mn></mrow><mo is=\"true\">+</mo></msubsup></mrow></math></span><script type=\"math/mml\"><math><mrow is=\"true\"><mi mathvariant=\"normal\" is=\"true\">N</mi><msubsup is=\"true\"><mi mathvariant=\"normal\" is=\"true\">H</mi><mrow is=\"true\"><mn is=\"true\">4</mn></mrow><mo is=\"true\">+</mo></msubsup></mrow></math></script></span>. Quenching tests and electron spin resonance characterization confirmed the generation of <span><span><math><mrow is=\"true\"><mo is=\"true\">·</mo><mi is=\"true\" mathvariant=\"normal\">O</mi><mi is=\"true\" mathvariant=\"normal\">H</mi></mrow></math></span><script type=\"math/mml\"><math><mrow is=\"true\"><mo is=\"true\">·</mo><mi mathvariant=\"normal\" is=\"true\">O</mi><mi mathvariant=\"normal\" is=\"true\">H</mi></mrow></math></script></span>, <span><span><math><mrow is=\"true\"><msup is=\"true\"><mrow is=\"true\"><mspace is=\"true\" width=\"0.166667em\"></mspace></mrow><mo is=\"true\">·</mo></msup><msubsup is=\"true\"><mi is=\"true\" mathvariant=\"normal\">O</mi><mrow is=\"true\"><mn is=\"true\">2</mn></mrow><mo is=\"true\">-</mo></msubsup></mrow></math></span><script type=\"math/mml\"><math><mrow is=\"true\"><msup is=\"true\"><mrow is=\"true\"><mspace width=\"0.166667em\" is=","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031356","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 : 2025-01-25DOI: 10.1016/j.seppur.2025.131806
Lijiao Yu, Lihong Deng, Jieyu Wu, Subhan Mahmood, Ke Yuan, Haoran Wu, Xiaodong Wang, Jing Zhang, Shun Yao
As a key component in tea tree oil (TTO), terpinen-4-ol exhibits ideal physiological activities. However, the high content of terpenes in crude TTO makes it challenging to enrich terpineol-4-ol. In this study, molecular simulations combined with experimental methods were used to select the optimal hydrogen bond acceptor (HBA), tetrabutylammonium chloride (TBAC), which forms a deep eutectic solvent (DES) with terpinen-4-ol in situ. Combined with necessary post-treatment process, it provided a feasible way for purification of TTO. Related DESs were prepared and characterized, and their main properties were also investigated. When the amount of TBAC was three times that of terpinen-4-ol, the formation of hydrogen bonds became more pronounced. At this point, the DES achieved its highest distribution coefficient for terpinen-4-ol (Dt = 15.02), as well as superior selectivity for terpinen-4-ol (St/c = 24.59, St/γ = 57.69). Water as the back-extractant and n-hexane as the auxiliary extractant facilitated the deep purification of terpinen-4-ol. Response surface analysis and experimental results confirmed that the optimal enrichment conditions were 30 min of enrichment time, an enrichment temperature of 60℃, and 0.5 g/g of n-hexane dosage. The back-enrichment and recovery of TBAC also proved to be satisfactory, and when applied to real tea oil, the developed method achieved over 90 % enrichment efficiency for terpinen-4-ol.
{"title":"Purification of crude tea tree oil through enrichment of terpinen-4-ol by in-situ formation of deep eutectic solvent","authors":"Lijiao Yu, Lihong Deng, Jieyu Wu, Subhan Mahmood, Ke Yuan, Haoran Wu, Xiaodong Wang, Jing Zhang, Shun Yao","doi":"10.1016/j.seppur.2025.131806","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131806","url":null,"abstract":"As a key component in tea tree oil (TTO), terpinen-4-ol exhibits ideal physiological activities. However, the high content of terpenes in crude TTO makes it challenging to enrich terpineol-4-ol. In this study, molecular simulations combined with experimental methods were used to select the optimal hydrogen bond acceptor (HBA), tetrabutylammonium chloride (TBAC), which forms a deep eutectic solvent (DES) with terpinen-4-ol in situ. Combined with necessary post-treatment process, it provided a feasible way for purification of TTO. Related DESs were prepared and characterized, and their main properties were also investigated. When the amount of TBAC was three times that of terpinen-4-ol, the formation of hydrogen bonds became more pronounced. At this point, the DES achieved its highest distribution coefficient for terpinen-4-ol (D<em><sub>t</sub></em> = 15.02), as well as superior selectivity for terpinen-4-ol (S<em><sub>t/c</sub></em> = 24.59, S<em><sub>t/γ</sub></em> = 57.69). Water as the back-extractant and n-hexane as the auxiliary extractant facilitated the deep purification of terpinen-4-ol. Response surface analysis and experimental results confirmed that the optimal enrichment conditions were 30 min of enrichment time, an enrichment temperature of 60℃, and 0.5 g/g of n-hexane dosage. The back-enrichment and recovery of TBAC also proved to be satisfactory, and when applied to real tea oil, the developed method achieved over 90 % enrichment efficiency for terpinen-4-ol.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"35 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031361","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 : 2025-01-24DOI: 10.1016/j.seppur.2025.131754
Jiali Cheng, Nanjiong Pang, Xian Liu, Wei Luo, Xuepin Liao, Bi Shi
The selective adsorption and separation of proteins are crucial in various fields. This study developed a novel affinity adsorbent, prepared by functionalizing collagen fibers with polyethyleneimine (CFs-PEI). Its adsorption and chromatographic separation performance for proteins were evaluated. It was found that the CFs-PEI exhibited satisfactory adsorption capacities of 462.29 mg/g for bovine serum albumin (BSA) and 159.99 mg/g for bovine hemoglobin (BHb) at pH 5.0. Furthermore, the separation factor (SFBSA/BHb) for BSA to BHb in a binary mixture solution at pH 5.0 reached 69.67, attributable to their distinct electrostatic interactions with CFs-PEI. In the chromatographic separation process, the BSA and BHb could be completely separated by stepwise elution with acetate buffer and citrate buffer. Meanwhile, the CFs-PEI column exhibited favorable reusability, maintaining a recovery rate exceeding 80 % for at least four cycles. This work presented a promising method for protein adsorption and separation using a naturally derived collagen fibers-based adsorbent, which was expected to show potential for applications ranging from biomolecule adsorption and separation to biomedical fields and food industries.
{"title":"High-performance separation of protein by the affinity adsorbent of polyethyleneimine-functionalized collagen fibers","authors":"Jiali Cheng, Nanjiong Pang, Xian Liu, Wei Luo, Xuepin Liao, Bi Shi","doi":"10.1016/j.seppur.2025.131754","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131754","url":null,"abstract":"The selective adsorption and separation of proteins are crucial in various fields. This study developed a novel affinity adsorbent, prepared by functionalizing collagen fibers with polyethyleneimine (CFs-PEI). Its adsorption and chromatographic separation performance for proteins were evaluated. It was found that the CFs-PEI exhibited satisfactory adsorption capacities of 462.29 mg/g for bovine serum albumin (BSA) and 159.99 mg/g for bovine hemoglobin (BHb) at pH 5.0. Furthermore, the separation factor (SF<sub>BSA/BHb</sub>) for BSA to BHb in a binary mixture solution at pH 5.0 reached 69.67, attributable to their distinct electrostatic interactions with CFs-PEI. In the chromatographic separation process, the BSA and BHb could be completely separated by stepwise elution with acetate buffer and citrate buffer. Meanwhile, the CFs-PEI column exhibited favorable reusability, maintaining a recovery rate exceeding 80 % for at least four cycles. This work presented a promising method for protein adsorption and separation using a naturally derived collagen fibers-based adsorbent, which was expected to show potential for applications ranging from biomolecule adsorption and separation to biomedical fields and food industries.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"51 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026775","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 : 2025-01-24DOI: 10.1016/j.seppur.2025.131778
Kun Liu, Jingxuan Cui, Aihu Feng, Junge Chen, Le Mi, Yang Yu, Xuebing Hu, Jianer Zhou, Yun Yu
Graphene is widely acknowledged as an exceptional electrode material for Capacitive Deionization (CDI) technology, owing to its unique crystal structure and electron transport properties. Typically, three-dimensional graphene is formed by stacking graphene nanosheets in a card-like manner. However, the assembly of these nanosheet layers results in numerous closed and narrow slit-like pores, which diminish pore connectivity and consequently limit its ion storage and capacitive deionization performance. Here, we employed KOH-assisted low-temperature rapid etching of three-dimensional reduced graphene oxide to construct a three-dimensional porous graphene (3D-PG) structure, thereby optimizing the distribution of pores. The 3D-PG electrode retained the open, interconnected three-dimensional structure and excellent conductivity of graphene. The unobstructed pores facilitated deeper ion diffusion and increased ion storage sites, significantly enhancing the ion storage capacity. Therefore, the 3D-PG electrodes exhibit exceptional electrochemical and CDI performance, with a specific capacitance of up to 348F/g at 1 A/g, retaining 99.7 % of this capacitance after 5000 cycles. Additionally, at an initial NaCl concentration of 1000 mg/L and a voltage of 1.6 V, the salt adsorption capacity (SAC) reached 24.5 mg/g, significantly outperforming many other graphene materials. These findings pave the way for synthesizing high-performance graphene-based materials on a large scale, with extensive potential for application in CDI and beyond.
{"title":"Pore optimization engineering for enhancing ion storage and capacitive deionization properties of graphene","authors":"Kun Liu, Jingxuan Cui, Aihu Feng, Junge Chen, Le Mi, Yang Yu, Xuebing Hu, Jianer Zhou, Yun Yu","doi":"10.1016/j.seppur.2025.131778","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131778","url":null,"abstract":"Graphene is widely acknowledged as an exceptional electrode material for Capacitive Deionization (CDI) technology, owing to its unique crystal structure and electron transport properties. Typically, three-dimensional graphene is formed by stacking graphene nanosheets in a card-like manner. However, the assembly of these nanosheet layers results in numerous closed and narrow slit-like pores, which diminish pore connectivity and consequently limit its ion storage and capacitive deionization performance. Here, we employed KOH-assisted low-temperature rapid etching of three-dimensional reduced graphene oxide to construct a three-dimensional porous graphene (3D-PG) structure, thereby optimizing the distribution of pores. The 3D-PG electrode retained the open, interconnected three-dimensional structure and excellent conductivity of graphene. The unobstructed pores facilitated deeper ion diffusion and increased ion storage sites, significantly enhancing the ion storage capacity. Therefore, the 3D-PG electrodes exhibit exceptional electrochemical and CDI performance, with a specific capacitance of up to 348F/g at 1 A/g, retaining 99.7 % of this capacitance after 5000 cycles. Additionally, at an initial NaCl concentration of 1000 mg/L and a voltage of 1.6 V, the salt adsorption capacity (SAC) reached 24.5 mg/g, significantly outperforming many other graphene materials. These findings pave the way for synthesizing high-performance graphene-based materials on a large scale, with extensive potential for application in CDI and beyond.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"58 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031365","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}
Spent coffee grounds (SCGs) represent a significant by-product with a high potential of extract bioactive compounds. This study investigates the potential of SCGs as a source for the extraction of phenolic compounds, which have applications in the pharmaceutical, cosmetic and food industries. In this work, several solvents and two extraction techniques were studied: Soxhlet as a reference and dynamic maceration for understanding the yield of extraction and the possible compounds that can be obtained. For dynamic maceration with a single liquid phase, higher extraction yields were observed for solvents with medium to high polarity, notably acetone (19.64 % ± 0.05) and isopropanol (14.66 % ± 0.76). Whereas ethanol (23.85 % ± 0.47) and acetone (20.03 % ± 0.27) led to best yields for Soxhlet. The primary phenolic compounds extracted were gallic acid, caffeic acid, 2,4-dihydroxybenzoic acid, 5-HMF, and furfural. In addition, when dynamic maceration and Soxhlet were tested with two liquid phases (a polar and a non-polar solvent), the yields were even better: 16.28 ± 2.01 % and 28.45 ± 2.48 %, respectively. A sustainability assessment was also made. Analytical Greenness Calculator indicated dynamic maceration (score: 0.6) as greener than the reference Soxhlet extraction (score: 0.5), requiring less energy, solvent, and time. These findings underscore the critical role of solvent selection in optimizing extraction processes, as well as the importance of selecting appropriate extraction techniques to maximize yield of value compounds in by-product like SCGs.
{"title":"Investigating the influence of solvents and extraction methods on the efficacy of phenolic compound recovery from spent coffee grounds","authors":"Naira Linhares Sabino, Henrique Maziero Fogarin, Sarha Lucia Murillo-Franco, Mariana Oliviera Bérgamo, Leticia Vicente Moreno, Debora Danielle Virginio da Silva, Cristiano Soleo Funari, Kelly Johana Dussán","doi":"10.1016/j.seppur.2025.131793","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131793","url":null,"abstract":"Spent coffee grounds (SCGs) represent a significant by-product with a high potential of extract bioactive compounds. This study investigates the potential of SCGs as a source for the extraction of phenolic compounds, which have applications in the pharmaceutical, cosmetic and food industries. In this work, several solvents and two extraction techniques were studied: Soxhlet as a reference and dynamic maceration for understanding the yield of extraction and the possible compounds that can be obtained. For dynamic maceration with a single liquid phase, higher extraction yields were observed for solvents with medium to high polarity, notably acetone (19.64 % ± 0.05) and isopropanol (14.66 % ± 0.76). Whereas ethanol (23.85 % ± 0.47) and acetone (20.03 % ± 0.27) led to best yields for Soxhlet. The primary phenolic compounds extracted were gallic acid, caffeic acid, 2,4-dihydroxybenzoic acid, 5-HMF, and furfural. In addition, when dynamic maceration and Soxhlet were tested with two liquid phases (a polar and a non-polar solvent), the yields were even better: 16.28 ± 2.01 % and 28.45 ± 2.48 %, respectively. A sustainability assessment was also made. Analytical Greenness Calculator indicated dynamic maceration (score: 0.6) as greener than the reference Soxhlet extraction (score: 0.5), requiring less energy, solvent, and time. These findings underscore the critical role of solvent selection in optimizing extraction processes, as well as the importance of selecting appropriate extraction techniques to maximize yield of value compounds in by-product like SCGs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"34 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026774","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}
In the process of interfacial polymerization for the fabrication of composite membrane, the addition of non-reactive materials in the aqueous or organic phase environment were often used to regulate the reaction rate in order to prepare composite membranes with a good performance, while ignoring the problem of difficult recycle of materials resulting in a waste of resources and secondary pollution. Herein, a reactive aqueous monomer 2-hydroxyethylhydrazin (0.05 % v/v) could combine with an ultra-low concentration piperazine (0.005 % w/v) to form a “transition state” coupling unit by the polar intermolecular dipole–dipole interaction, which could regulate the interfacial polymerization state under the concentration of impossible-formed membrane for forming a complete polyester-amide active layer. The membrane showed excellent performance with a Na2SO4 rejection of 96.76 % and a pure water flux of 12.77 L⋅m−2⋅h−1⋅bar−1. The mechanism of dipole–dipole interaction induced regulation of interfacial polymerization reaction rate was revealed through multi-scale assisted analyses such as the physicochemical characterization, the molecular dynamics simulation and the density functional theory calculation. This study provided a novel method for preparing nanofiltration membranes with low energy consumption and high efficiency, which could have a positive effect on the development of membrane technology.
{"title":"The interfacial polymerization reaction induced by intermolecular dipole–dipole interaction for the preparation of nanofiltration membrane under the low concentration of the aqueous monomers","authors":"Yuliang Wu, Chen Chen, Rui Meng, Yuliang Chen, Libo Ba, Yijiang Liu, Weiwei Huang, Fei Yang, Jun Cheng, Yong Wang, Xuesong Yi","doi":"10.1016/j.seppur.2025.131750","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131750","url":null,"abstract":"In the process of interfacial polymerization for the fabrication of composite membrane, the addition of non-reactive materials in the aqueous or organic phase environment were often used to regulate the reaction rate in order to prepare composite membranes with a good performance, while ignoring the problem of difficult recycle of materials resulting in a waste of resources and secondary pollution. Herein, a reactive aqueous monomer 2-hydroxyethylhydrazin (0.05 % v/v) could combine with an ultra-low concentration piperazine (0.005 % w/v) to form a “transition state” coupling unit by the polar intermolecular dipole–dipole interaction, which could regulate the interfacial polymerization state under the concentration of impossible-formed membrane for forming a complete polyester-amide active layer. The membrane showed excellent performance with a Na<sub>2</sub>SO<sub>4</sub> rejection of 96.76 % and a pure water flux of 12.77 L⋅m<sup>−2</sup>⋅h<sup>−1</sup>⋅bar<sup>−1</sup>. The mechanism of dipole–dipole interaction induced regulation of interfacial polymerization reaction rate was revealed through multi-scale assisted analyses such as the physicochemical characterization, the molecular dynamics simulation and the density functional theory calculation. This study provided a novel method for preparing nanofiltration membranes with low energy consumption and high efficiency, which could have a positive effect on the development of membrane technology.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"38 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031366","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 : 2025-01-24DOI: 10.1016/j.seppur.2025.131689
Xueying Liu, Wei Yang, Ali Zaoui, Chenghui Guo, Renpeng Chen
Chromium and its compounds, as industrial solid wastes featuring high storage capacity but low utilization rate and high environmental risk. Therefore, a liner composed of cetyltrimethylammonium bromide modified bentonite (CMB), polymer modified bentonite (PMB), and sand was developed to remove chromium pollution in groundwater of chromium slag landfills. Microscopic characterizations and molecular dynamic simulations were employed to elucidate the modification and adsorption/impermeability mechanisms of CMB and PMB. The cetyltrimethylammonium (CTMA+) chains were intercalated into the interlayer space of NaB, with the adsorption mechanism attributed to electrostatic interactions between the head groups of CTMA+ and CrO42-. SEM-EDS revealed that PMB exhibited an enhanced three-dimensional network structure woven by entangled polymer chains and the orthogonally aligned stacks of bentonite plates prevented NaB from undergoing cation exchange, a key mechanism for impermeability enhancement. Five long-term column tests were conducted to determine the transport parameters of chromium in the modified liner. The hydraulic conductivity of the single-liner CPBS and double-liner D-PC was 2.18 × 10-10 m/s and 2.50 × 10-12 m/s, respectively, meeting the typical requirement of hydraulic barriers for contaminant containment. Analytic calculations were employed to evaluate the service life of CPBS and D-PC liners under varying hydraulic gradients in chromium-contaminated groundwater. Notably, the D-PC exhibits minimal sensitivity to changes in hydraulic gradient, with a required thickness of approximately 0.09 m for a 50-year service life, indicating broad prospects in control of environmental risks associated with groundwater contamination at polluted sites.
{"title":"Enhanced chromium removal from contaminated groundwater using modified bentonite-sand liners: Experimental and simulation insights","authors":"Xueying Liu, Wei Yang, Ali Zaoui, Chenghui Guo, Renpeng Chen","doi":"10.1016/j.seppur.2025.131689","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131689","url":null,"abstract":"Chromium and its compounds, as industrial solid wastes featuring high storage capacity but low utilization rate and high environmental risk. Therefore, a liner composed of cetyltrimethylammonium bromide modified bentonite (CMB), polymer modified bentonite (PMB), and sand was developed to remove chromium pollution in groundwater of chromium slag landfills. Microscopic characterizations and molecular dynamic simulations were employed to elucidate the modification and adsorption/impermeability mechanisms of CMB and PMB. The cetyltrimethylammonium (CTMA<sup>+</sup>) chains were intercalated into the interlayer space of NaB, with the adsorption mechanism attributed to electrostatic interactions between the head groups of CTMA<sup>+</sup> and CrO<sub>4</sub><sup>2-</sup>. SEM-EDS revealed that PMB exhibited an enhanced three-dimensional network structure woven by entangled polymer chains and the orthogonally aligned stacks of bentonite plates prevented NaB from undergoing cation exchange, a key mechanism for impermeability enhancement. Five long-term column tests were conducted to determine the transport parameters of chromium in the modified liner. The hydraulic conductivity of the single-liner CPBS and double-liner D-PC was 2.18 × 10<sup>-10</sup> m/s and 2.50 × 10<sup>-12</sup> m/s, respectively, meeting the typical requirement of hydraulic barriers for contaminant containment. Analytic calculations were employed to evaluate the service life of CPBS and D-PC liners under varying hydraulic gradients in chromium-contaminated groundwater. Notably, the D-PC exhibits minimal sensitivity to changes in hydraulic gradient, with a required thickness of approximately 0.09 m for a 50-year service life, indicating broad prospects in control of environmental risks associated with groundwater contamination at polluted sites.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026773","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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