Pub Date : 2025-02-25DOI: 10.1016/j.seppur.2025.132282
Siqi Dong, Boyu Liu, Kai Lv, Shuanglin Hu, Zirui Liu, Zhenghao Mao, Shunshun Xiong
Design and synthesis of porous solids materials for efficient separation and capture of inert gas Xe and Kr from the nuclear off-gas steam remain urgent and challenging issues. Herein, a new bromine functionalized Zr-based metal organic framework (MIP-203-F-Br) was successfully prepared using a facile synthetic method to effectively separate and capture Xe and Kr. The immobilization of bromine atoms into framework of MIP-203-F-Br creates a highly polarized pore environment in its 1D-channel with optimized pore size (4.6 Å), that maximizes confinement effects for Xe absorption. MIP-203-F-Br exhibits significantly high Xe adsorption affinity at low pressure with a high Xe uptake capacity (39.4 cm3·cm−3) at 10 kPa and 298 K and a record-breaking Henry-coefficient (27.2 mmol·g−1·bar−1) among the reported Zr-based MOFs. Through the breakthrough experiments carried out in dilute conditions (simulation of nuclear off-gases), the practical separation performance of MIP-203-F-Br was confirmed. Grand Canonical Monte Carlo (GCMC) simulations and Density Functional Theory (DFT) calculations were performed to elucidate the adsorption mechanism in MIP-203-F-Br, highlighting the significant role played by Br atoms in enhancing Xe adsorption. This work also provides a novel facile synthetic method to achieve bromine functionalized MOFs for potential various applications.
{"title":"Bromine functionalized zirconium–fumarate frameworks for enhanced xenon capture and separation","authors":"Siqi Dong, Boyu Liu, Kai Lv, Shuanglin Hu, Zirui Liu, Zhenghao Mao, Shunshun Xiong","doi":"10.1016/j.seppur.2025.132282","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132282","url":null,"abstract":"Design and synthesis of porous solids materials for efficient separation and capture of inert gas Xe and Kr from the nuclear off-gas steam remain urgent and challenging issues. Herein, a new bromine functionalized Zr-based metal organic framework (MIP-203-F-Br) was successfully prepared using a facile synthetic method to effectively separate and capture Xe and Kr. The immobilization of bromine atoms into framework of MIP-203-F-Br creates a highly polarized pore environment in its 1D-channel with optimized pore size (4.6 Å), that maximizes confinement effects for Xe absorption. MIP-203-F-Br exhibits significantly high Xe adsorption affinity at low pressure with a high Xe uptake capacity (39.4 cm<sup>3</sup>·cm<sup>−3</sup>) at 10 kPa and 298 K and a record-breaking Henry-coefficient (27.2 mmol·g<sup>−1</sup>·bar<sup>−1</sup>) among the reported Zr-based MOFs. Through the breakthrough experiments carried out in dilute conditions (simulation of nuclear off-gases), the practical separation performance of MIP-203-F-Br was confirmed. Grand Canonical Monte Carlo (GCMC) simulations and Density Functional Theory (DFT) calculations were performed to elucidate the adsorption mechanism in MIP-203-F-Br, highlighting the significant role played by Br atoms in enhancing Xe adsorption. This work also provides a novel facile synthetic method to achieve bromine functionalized MOFs for potential various applications.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"42 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485801","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132270
Chong Chen, Yukun Zhang, Changjiang Hu, Zhiwen Jiang, Jun Ma
Some well-established metal–organic frameworks (MOFs) have shown their commercialization for CO2 capture and conversion. However, the development of effective and scalable modification technologies that are broadly applicable to existing MOFs still face significant challenges. Here, in contrast to sophisticated synthesis, we report a general and facile upgrading strategy for kilogram-level MOFs including IRMOF, MIL, and ZIF through ambient, controllable and cost-effective electron-beam (e-beam) irradiation. Specially, the modified HKUST-1 achieves a 16.6% improvement in CO2 uptake with high selectivities for CO2/N2 mixtures, and a 2-fold production rate of CO under visible-light illumination. As demonstrated by newly-developed in-situ X-ray diffraction infrared Fourier transform (DRIFT) technology and theoretical calculations, e-beam induces the metal node reduction, ligand functionalization, and pore architecture manipulation via radiolysis of trapped water molecules, synergistically promoting the CO2 polarization and activation. Our study reveals the advantageous of e-beam irradiation effects for MOFs, which are often considered negative in many areas.
{"title":"Scalable upgrading metal–organic frameworks through ambient and controllable electron-beam irradiation for CO2 capture and conversion","authors":"Chong Chen, Yukun Zhang, Changjiang Hu, Zhiwen Jiang, Jun Ma","doi":"10.1016/j.seppur.2025.132270","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132270","url":null,"abstract":"Some well-established metal–organic frameworks (MOFs) have shown their commercialization for CO<sub>2</sub> capture and conversion. However, the development of effective and scalable modification technologies that are broadly applicable to existing MOFs still face significant challenges. Here, in contrast to sophisticated synthesis, we report a general and facile upgrading strategy for kilogram-level MOFs including IRMOF, MIL, and ZIF through ambient, controllable and cost-effective electron-beam (e-beam) irradiation. Specially, the modified HKUST-1 achieves a 16.6% improvement in CO<sub>2</sub> uptake with high selectivities for CO<sub>2</sub>/N<sub>2</sub> mixtures, and a 2-fold production rate of CO under visible-light illumination. As demonstrated by newly-developed in-situ X-ray diffraction infrared Fourier transform (DRIFT) technology and theoretical calculations, e-beam induces the metal node reduction, ligand functionalization, and pore architecture manipulation via radiolysis of trapped water molecules, synergistically promoting the CO<sub>2</sub> polarization and activation. Our study reveals the advantageous of e-beam irradiation effects for MOFs, which are often considered negative in many areas.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"85 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485806","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132280
Qingcun Gu, Xiaoya Gao, Bingheng Liang, Xuhao Liu, Jiatian Wang, Teng Guo, Wenjie Zhu, Yongming Luo
Impurities play a crucial role in various catalytic systems. This study firstly investigated the effects of Ni and Co impurities in pyrite on peroxymonosulfate (PMS) activation to degrade emerging pollutants. The substitution of 6.30 % Ni and 5.64 % Co enhanced the catalytic activity of pyrite, with rate constants of 12 and 22 times greater than pure pyrite, respectively. Theoretical calculations revealed that impurities shifted PMS adsorption to a dual-site mode, leading to stronger adsorption energy and more electron transfer numbers than pure pyrite. The extension of oxygen–oxygen bond in PMS significantly promoted its cleavage to generate reactive oxygen species (particularly singlet oxygen of 74 times greater in 5.64 % Co-Py/PMS than that in the Py/PMS), which ensured the enhanced environment stability/adaptability and reduced pollutants toxicity within the 6.30 % Ni-Py and 5.64 % Co-Py systems. This study provides new insights into positively governing pyrite-based PMS advanced oxidation processes from the perspective of coexisting impurities.
{"title":"Overlooked role of transition metal impurities (cobalt and nickel) substitution in tuning pyrite to activate peroxymonosulfate for degradation of emerging pollutants","authors":"Qingcun Gu, Xiaoya Gao, Bingheng Liang, Xuhao Liu, Jiatian Wang, Teng Guo, Wenjie Zhu, Yongming Luo","doi":"10.1016/j.seppur.2025.132280","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132280","url":null,"abstract":"Impurities play a crucial role in various catalytic systems. This study firstly investigated the effects of Ni and Co impurities in pyrite on peroxymonosulfate (PMS) activation to degrade emerging pollutants. The substitution of 6.30 % Ni and 5.64 % Co enhanced the catalytic activity of pyrite, with rate constants of 12 and 22 times greater than pure pyrite, respectively. Theoretical calculations revealed that impurities shifted PMS adsorption to a dual-site mode, leading to stronger adsorption energy and more electron transfer numbers than pure pyrite. The extension of oxygen–oxygen bond in PMS significantly promoted its cleavage to generate reactive oxygen species (particularly singlet oxygen of 74 times greater in 5.64 % Co-Py/PMS than that in the Py/PMS), which ensured the enhanced environment stability/adaptability and reduced pollutants toxicity within the 6.30 % Ni-Py and 5.64 % Co-Py systems. This study provides new insights into positively governing pyrite-based PMS advanced oxidation processes from the perspective of coexisting impurities.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"24 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485805","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132281
Danilo Alexander Figueroa Paredes, Ramiro Julián Sánchez, Daniela Soledad Laoretani, Mauren Fuentes, María Belén Fernández, José Espinosa
Applied to IPA dehydration, this paper analyses the economic and environmental performance of two variants of the hybrid distillation/pervaporation process operated in batch wise mode; namely, distillation followed by pervaporation with either a polymeric membrane or a ceramic membrane. Both variants are also compared from an environmental standpoint resorting to a life cycle analysis (LCA). Conceptual models of the distillation step and the pervaporation stage were used in doing the performance comparison of variants considering commercial membranes CMC-CF-23 and HybSi. To build the conceptual model for the HybSi membrane, six dehydration experiments were conducted, starting with a feed composition of 80 wt% IPA at three temperatures (70 °C, 80 °C, and 90 °C) and two vacuum levels (3.7 and 6.7 kPa). A permeance model, incorporating the active pore fraction as a parameter, was fitted and showed good agreement with the experimental data. Finally, in order to improve the environmental performance of the distillation/HybSi variant, simulations of the pervaporation task at 90 °C with two vacuum levels (9.7 kPa, 6.7 kPa) consecutively applied were done. This variant was the most attractive from both an economic and environmental point of view. The resulting recovery cost at the optimum was 690 US$ t−1 and the operation at 90 °C was characterized by a distillate composition of 82 % by weight of IPA, a permeate flux of 2.64 kg m−2 h−1 and a permeate composition of 2.7 % IPA by weight. The consecutive condensation temperatures of permeates were 33 °C and 11 °C, respectively. As initially supposed, an enhancement of the environmental performance of this alternative with respect to the others measured from both a life cycle emissions (LCE) perspective and a life cycle impact assessment (LCIA) on human health, ecosystems and resources occurred.
{"title":"Variants of the hybrid distillation/pervaporation process: Conceptual model-based optimization and environmental analysis for IPA dehydration","authors":"Danilo Alexander Figueroa Paredes, Ramiro Julián Sánchez, Daniela Soledad Laoretani, Mauren Fuentes, María Belén Fernández, José Espinosa","doi":"10.1016/j.seppur.2025.132281","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132281","url":null,"abstract":"Applied to IPA dehydration, this paper analyses the economic and environmental performance of two variants of the hybrid distillation/pervaporation process operated in batch wise mode; namely, distillation followed by pervaporation with either a polymeric membrane or a ceramic membrane. Both variants are also compared from an environmental standpoint resorting to a life cycle analysis (LCA). Conceptual models of the distillation step and the pervaporation stage were used in doing the performance comparison of variants considering commercial membranes CMC-CF-23 and HybSi. To build the conceptual model for the HybSi membrane, six dehydration experiments were conducted, starting with a feed composition of 80 wt% IPA at three temperatures (70 °C, 80 °C, and 90 °C) and two vacuum levels (3.7 and 6.7 kPa). A permeance model, incorporating the active pore fraction as a parameter, was fitted and showed good agreement with the experimental data. Finally, in order to improve the environmental performance of the distillation/HybSi variant, simulations of the pervaporation task at 90 °C with two vacuum levels (9.7 kPa, 6.7 kPa) consecutively applied were done. This variant was the most attractive from both an economic and environmental point of view. The resulting recovery cost at the optimum was 690 US$ t<sup>−1</sup> and the operation at 90 °C was characterized by a distillate composition of 82 % by weight of IPA, a permeate flux of 2.64 kg m<sup>−2</sup> h<sup>−1</sup> and a permeate composition of 2.7 % IPA by weight. The consecutive condensation temperatures of permeates were 33 °C and 11 °C, respectively. As initially supposed, an enhancement of the environmental performance of this alternative with respect to the others measured from both a life cycle emissions (LCE) perspective and a life cycle impact assessment (LCIA) on human health, ecosystems and resources occurred.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"43 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485802","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}
Layered double hydroxides (LDHs), despite their unique layered structure advantageous for removing high-molecular-weight antibiotics, suffer from limitations such as small specific surface area, uncontrollable morphology, and irregular spatial structure compared to metal–organic frameworks (MOFs). Therefore, in this study, ZIF-8 was used as a template to prepare LDHs with a hollow mesoporous structure (ZNF-HS), merging the benefits of both materials. ZNF-HS was then stably incorporated into sodium carboxymethylcellulose aerogels, resulting in ZNF-HS@CMC composites that facilitated easy solid–liquid separation and were effective in removing tetracycline (TC) and ciprofloxacin (CIP) from aqueous solution. Characterization of ZNF-HS@CMC was conducted using SEM, TEM, XRD, FTIR, XPS, BET, and TGA. ZNF-HS@CMC exhibited a specific surface area of 248.753 m2·g−1 and a pore volume of 0.568 cm3·g−1, surpassing traditional LDHs. The removal of TC and CIP by ZNF-HS@CMC followed the pseudo-second-order kinetic and Langmuir models, with maximum sorption capacities of 513.772 and 442.515 mg·g−1, respectively. pH significantly influenced the removal efficiencies, while NaNO3 concentration up to 0.25 mol·L-1 had negligible impact, maintaining removal efficiencies above 90 %. After five sorption–desorption cycles, the removal efficiencies remained above 80 %. The removal of TC and CIP by ZNF-HS@CMC was primarily achieved through surface complexation, hydrogen bonding, and π-π interactions, with electrostatic interactions also contributing. Overall, ZNF-HS@CMC exhibits the advantages of easy recycling, good reusability, strong resistance to salt interference, and high sorption capacity, making it promising for practical applications in the efficient removal of antibiotics from water.
{"title":"ZIF-8-templated synthesis of hollow porous layered double hydroxide/cellulose aerogel composites for efficient removal of antibiotics from aqueous solution","authors":"Zhiqiang Guo, Juanjuan Meng, Xinxin Li, Xinlong Wang, Yuan Li, Liangliang Hu","doi":"10.1016/j.seppur.2025.132264","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132264","url":null,"abstract":"Layered double hydroxides (LDHs), despite their unique layered structure advantageous for removing high-molecular-weight antibiotics, suffer from limitations such as small specific surface area, uncontrollable morphology, and irregular spatial structure compared to metal–organic frameworks (MOFs). Therefore, in this study, ZIF-8 was used as a template to prepare LDHs with a hollow mesoporous structure (ZNF-HS), merging the benefits of both materials. ZNF-HS was then stably incorporated into sodium carboxymethylcellulose aerogels, resulting in ZNF-HS@CMC composites that facilitated easy solid–liquid separation and were effective in removing tetracycline (TC) and ciprofloxacin (CIP) from aqueous solution. Characterization of ZNF-HS@CMC was conducted using SEM, TEM, XRD, FTIR, XPS, BET, and TGA. ZNF-HS@CMC exhibited a specific surface area of 248.753 m<sup>2</sup>·g<sup>−1</sup> and a pore volume of 0.568 cm<sup>3</sup>·g<sup>−1</sup>, surpassing traditional LDHs. The removal of TC and CIP by ZNF-HS@CMC followed the pseudo-second-order kinetic and Langmuir models, with maximum sorption capacities of 513.772 and 442.515 mg·g<sup>−1</sup>, respectively. pH significantly influenced the removal efficiencies, while NaNO<sub>3</sub> concentration up to 0.25 mol·L<sup>-1</sup> had negligible impact, maintaining removal efficiencies above 90 %. After five sorption–desorption cycles, the removal efficiencies remained above 80 %. The removal of TC and CIP by ZNF-HS@CMC was primarily achieved through surface complexation, hydrogen bonding, and π-π interactions, with electrostatic interactions also contributing. Overall, ZNF-HS@CMC exhibits the advantages of easy recycling, good reusability, strong resistance to salt interference, and high sorption capacity, making it promising for practical applications in the efficient removal of antibiotics from water.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"51 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485810","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132269
Yen-Yung Wu, Li-Chiang Lin
Reverse osmosis (RO) is a key technology to various separation applications, whose processes traditionally rely on the well-known size-exclusion mechanism to block the greater component in size. Interestingly, recent studies have also demonstrated RO processes that can selectively permeate larger molecules via their favorable adsorption. While these distinct behaviors have been observed, a comprehensive understanding on the design of RO membranes remains lacking. To this end, by employing molecular dynamics simulations, this study conducts a systematic evaluation on RO membranes with different pore dimensions for their separation performance of a binary mixture comprising components of varying molecular sizes, offering quantitative insights into the design of RO membranes. The outcomes show that, while the traditional size-exclusion design remains an effective approach, utilizing the adsorption-facilitated mechanism may lead to a notably enhanced performance with rich separation behaviors. Specifically, the pore size may be designed to be greater than both of the components for a boosted permeation flux. Moreover, through strategically exploiting the confinement effect for preferentially adsorbing a specific component, either the smaller or the greater one, effective RO processes to selectively permeate the either component can be achieved.
{"title":"Design of reverse osmosis membranes for molecular separation: Size-exclusion vs. Adsorption-facilitation mechanisms","authors":"Yen-Yung Wu, Li-Chiang Lin","doi":"10.1016/j.seppur.2025.132269","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132269","url":null,"abstract":"Reverse osmosis (RO) is a key technology to various separation applications, whose processes traditionally rely on the well-known size-exclusion mechanism to block the greater component in size. Interestingly, recent studies have also demonstrated RO processes that can selectively permeate larger molecules via their favorable adsorption. While these distinct behaviors have been observed, a comprehensive understanding on the design of RO membranes remains lacking. To this end, by employing molecular dynamics simulations, this study conducts a systematic evaluation on RO membranes with different pore dimensions for their separation performance of a binary mixture comprising components of varying molecular sizes, offering quantitative insights into the design of RO membranes. The outcomes show that, while the traditional size-exclusion design remains an effective approach, utilizing the adsorption-facilitated mechanism may lead to a notably enhanced performance with rich separation behaviors. Specifically, the pore size may be designed to be greater than both of the components for a boosted permeation flux. Moreover, through strategically exploiting the confinement effect for preferentially adsorbing a specific component, either the smaller or the greater one, effective RO processes to selectively permeate the either component can be achieved.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"26 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485803","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132200
Bárbara M.C. Vaz, Maria Sofia C.T.S. Leite, Letícia S. Contieri, Leonardo M. de Souza Mesquita, Alexandra Conde, Joana P. Oliveira, Diana C.G.A. Pinto, Sónia P.M. Ventura
A marine bio-based economy has emerged as a sustainable and renewable solution to address the resource depletion of fossil fuels and ensure a responsible and sustainable utilization of natural resources by following a multi-product biorefinery approach. Macroalgae are a valuable source of several high-demand compounds including mycosporine-like amino acids (MAAs), which can absorb UV radiation and protect the skin from external damage. In this work, a sustainable and multi-product biorefinery was designed from Gracilaria sp. by applying a solid–liquid extraction followed by two purification steps, ultrafiltration and induced precipitation. This process enabled the recovery of three valuable compound fractions, one rich in phycobiliproteins, a second, rich in non-fluorescent proteins, and a third, rich in MAAs (main goal), specifically Porphyra-334. In addition, by 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) scavenging assay, MAAs-rich fraction revealed enhanced antioxidant activity. Lastly, a comprehensive conceptual design of the process was created, envisioning its implementation at an industrial scale.
{"title":"Efficient extraction and purification of mycosporines-like amino acids (MAAs) following a multiproduct biorefinery approach","authors":"Bárbara M.C. Vaz, Maria Sofia C.T.S. Leite, Letícia S. Contieri, Leonardo M. de Souza Mesquita, Alexandra Conde, Joana P. Oliveira, Diana C.G.A. Pinto, Sónia P.M. Ventura","doi":"10.1016/j.seppur.2025.132200","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132200","url":null,"abstract":"A marine bio-based economy has emerged as a sustainable and renewable solution to address the resource depletion of fossil fuels and ensure a responsible and sustainable utilization of natural resources by following a multi-product biorefinery approach. Macroalgae are a valuable source of several high-demand compounds including mycosporine-like amino acids (MAAs), which can absorb UV radiation and protect the skin from external damage. In this work, a sustainable and multi-product biorefinery was designed from <em>Gracilaria</em> sp. by applying a solid–liquid extraction followed by two purification steps, ultrafiltration and induced precipitation. This process enabled the recovery of three valuable compound fractions, one rich in phycobiliproteins, a second, rich in non-fluorescent proteins, and a third, rich in MAAs (main goal), specifically Porphyra-334. In addition, by 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) scavenging assay, MAAs-rich fraction revealed enhanced antioxidant activity. Lastly, a comprehensive conceptual design of the process was created, envisioning its implementation at an industrial scale.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"30 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485804","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}
Developing anode materials significantly enhances the desalination performance of hybrid capacitive deionization (HCDI). Bismuth exhibits high selectivity for chloride ion removal. However, the sluggish kinetics and poor cycling stability of bismuth present considerable challenges for its application in high-capacitance deionization. In this study, we successfully prepared a binder-free Bi@MXene film electrode for chloride storage by employing an electrostatic self-assembly strategy to anchor Bi nanospheres into MXene layers. The bismuth nanospheres, as the pillars of MXene network, improve the self-stacking problem of Ti3C2TX layers. And MXene layers effectively mitigate the volume expansion of bismuth nanospheres through the spatial confinement effect. Benefiting from three-dimentional sandwich structure of Bi@MXene film, the HCDI system exhibits outstanding salt adsorption capacity (113.4 mg·g−1), excellent adsorption rate (4.2 mg·g−1·min−1) and a good desalination capacity retention of 84.6 % following 50 cycles at 100 mA·g−1. The development of this composite material provides insights for the design of efficient and stable chloride storage electrodes.
{"title":"Binder-free Bi@MXene film with 3D sandwich structure for highly hybrid capacitive deionization","authors":"Meng Xu, Zhiyou Tan, Yilong Tian, Feng Gong, Kebing Yi, Zhike He, Xinghu Ji","doi":"10.1016/j.seppur.2025.132263","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132263","url":null,"abstract":"Developing anode materials significantly enhances the desalination performance of hybrid capacitive deionization (HCDI). Bismuth exhibits high selectivity for chloride ion removal. However, the sluggish kinetics and poor cycling stability of bismuth present considerable challenges for its application in high-capacitance deionization. In this study, we successfully prepared a binder-free Bi@MXene film electrode for chloride storage by employing an electrostatic self-assembly strategy to anchor Bi nanospheres into MXene layers. The bismuth nanospheres, as the pillars of MXene network, improve the self-stacking problem of Ti<sub>3</sub>C<sub>2</sub>T<sub>X</sub> layers. And MXene layers effectively mitigate the volume expansion of bismuth nanospheres through the spatial confinement effect. Benefiting from three-dimentional sandwich structure of Bi@MXene film, the HCDI system exhibits outstanding salt adsorption capacity (113.4 mg·g<sup>−1</sup>), excellent adsorption rate (4.2 mg·g<sup>−1</sup>·min<sup>−1</sup>) and a good desalination capacity retention of 84.6 % following 50 cycles at 100 mA·g<sup>−1</sup>. The development of this composite material provides insights for the design of efficient and stable chloride storage electrodes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"16 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485809","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132287
Wenshuai Jiang, Yaning Wang, Yiheng Liu, Qianfang Jia, Caojie Zhao, Jin Yang, Wu Ren, Qingjun Liu
Graphene oxide (GO) and MXene-based membranes have been widely used in the field of water purification due to their excellent separation properties. However, the poor stabilities of these species in water and the ‘trade-off’ effect between permeability and retention greatly limit their practical applications. In this study, modified GO/MXene composite membranes were prepared via double regulation with sodium alginate (SA) and KOH. During the modulation process, SA formed more hydrogen bonds with GO/MXene nanosheets. Meanwhile, SA acts as a “mortar” during the assembly of GO/MXene nanosheets, avoiding their aggregation and disordered stacking. During the subsequent regulation in the KOH solution, K+ not only enlarged the interlayer spacing of the composite membrane, but also interacted with the oxidation groups on the GO (cation-π) to play a fixed role in fixing the interlayer spacing of the composite membrane to reduce the swelling of the composite membrane. Furthermore, the number of oxygen-containing functional groups on the surfaces of the GO/MXene composite membranes was significantly reduced under alkaline conditions, which further enhanced the selectivity of the composite membranes to the selectivity of the composite membrane to the dye molecules. Due to the synergistic effect generated by the dual regulation of SA and KOH, the K+/GO/MXene composite membranes exhibited excellent water treatment performance, in terms of their permeability and dye retention, as well as high physical stability. By optimizing the content of SA and the ratio of GO/MXene, the composite membrane with the optimal separation performance was successfully synthesized. Compared with ordinary GO/MXene composite membranes, the water flux of the K+/GO/MXene-SA composite membrane was enhanced from 48 to 88.07 Lm−2 h−1 bar−1.The K+/GO/MXene-SA composite membrane has excellent MB dye separation performance, with a removal rate of more than 97.75 %. In addition, the K+/GO/MXene-SA composite membrane demonstrated an excellent structural stability in acidic and alkaline solutions. The filtered composite membrane still maintains excellent stability and has good recyclability after desorption.These results therefore provide new insights into the design of two-dimensional membrane separation materials for use in the purification of dye effluents.
{"title":"Enhanced water purification through the double regulation of GO/MXene membranes with sodium alginate and KOH","authors":"Wenshuai Jiang, Yaning Wang, Yiheng Liu, Qianfang Jia, Caojie Zhao, Jin Yang, Wu Ren, Qingjun Liu","doi":"10.1016/j.seppur.2025.132287","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132287","url":null,"abstract":"Graphene oxide (GO) and MXene-based membranes have been widely used in the field of water purification due to their excellent separation properties. However, the poor stabilities of these species in water and the ‘trade-off’ effect between permeability and retention greatly limit their practical applications. In this study, modified GO/MXene composite membranes were prepared via double regulation with sodium alginate (SA) and KOH. During the modulation process, SA formed more hydrogen bonds with GO/MXene nanosheets. Meanwhile, SA acts as a “mortar” during the assembly of GO/MXene nanosheets, avoiding their aggregation and disordered stacking. During the subsequent regulation in the KOH solution, K+ not only enlarged the interlayer spacing of the composite membrane, but also interacted with the oxidation groups on the GO (cation-π) to play a fixed role in fixing the interlayer spacing of the composite membrane to reduce the swelling of the composite membrane. Furthermore, the number of oxygen-containing functional groups on the surfaces of the GO/MXene composite membranes was significantly reduced under alkaline conditions, which further enhanced the selectivity of the composite membranes to the selectivity of the composite membrane to the dye molecules. Due to the synergistic effect generated by the dual regulation of SA and KOH, the K+/GO/MXene composite membranes exhibited excellent water treatment performance, in terms of their permeability and dye retention, as well as high physical stability. By optimizing the content of SA and the ratio of GO/MXene, the composite membrane with the optimal separation performance was successfully synthesized. Compared with ordinary GO/MXene composite membranes, the water flux of the K+/GO/MXene-SA composite membrane was enhanced from 48 to 88.07 Lm<sup>−2</sup> h<sup>−1</sup> bar<sup>−1</sup>.The K+/GO/MXene-SA composite membrane has excellent MB dye separation performance, with a removal rate of more than 97.75 %. In addition, the K+/GO/MXene-SA composite membrane demonstrated an excellent structural stability in acidic and alkaline solutions. The filtered composite membrane still maintains excellent stability and has good recyclability after desorption.These results therefore provide new insights into the design of two-dimensional membrane separation materials for use in the purification of dye effluents.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"31 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143485800","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 : 2025-02-25DOI: 10.1016/j.seppur.2025.132261
Yijian Li , Xin Zhou , Anqi Zhang , Lei Sun , Shuai Wang , Feng Liu
In this work, sulfur self-doped hierarchical porous carbons (KLC-X-Y) were fabricated via one-pot method using inexpensive sodium lignosulphonate as carbon and sulfur source and potassium hydroxide (KOH) as activator. Through detailed analysis, it was found that the carbonization temperature and KOH addition exhibited significant effects on the porosity, phase composition, functional groups and morphology of KLC-X-Y. Among them, KLC-700–2 possessed a hierarchical porous structure, high specific surface area (851.3 m2·g−1), large pore volume (0.53 cm3·g−1), appropriate pore size distribution (D = 2.49 nm), and abundant oxygen- (COOH and OH) and sulfur-containing (SO3H and SH) functional groups. Notably, the synthesized KLC-700–2 displayed excellent adsorption performance for Tl(I) with a maximum adsorption amount of 523.7 mg·g−1. After five consecutive adsorption–desorption processes, the adsorption amount of Tl(Ⅰ) by KLC-700–2 decreased slightly, which still reached 85.6 % of the initial adsorption amount, and its own structural properties didn’t change significantly, indicating that KLC-700–2 had good stability and reusability. The adsorption process of Tl(Ⅰ) on KLC-700–2 was verified to be spontaneous and endothermic, and conformed to the pseudo second order and Langmuir models by adsorption kinetic, isotherm, and thermodynamic studies. By comparing the physicochemical properties of KLC-700–2 before and after adsorption of Tl(I), it was confirmed that the adsorption of Tl(Ⅰ) on KLC-700–2 was co-controlled by chemical and physical adsorption, including ion exchange, precipitation reaction, surface complexation, pore filling and electrostatic attraction.
{"title":"Sulfur self-doped hierarchical porous carbon materials synthesized by one-pot method for efficient adsorption of thallium(I)","authors":"Yijian Li , Xin Zhou , Anqi Zhang , Lei Sun , Shuai Wang , Feng Liu","doi":"10.1016/j.seppur.2025.132261","DOIUrl":"10.1016/j.seppur.2025.132261","url":null,"abstract":"<div><div>In this work, sulfur self-doped hierarchical porous carbons (KLC-X-Y) were fabricated via one-pot method using inexpensive sodium lignosulphonate as carbon and sulfur source and potassium hydroxide (KOH) as activator. Through detailed analysis, it was found that the carbonization temperature and KOH addition exhibited significant effects on the porosity, phase composition, functional groups and morphology of KLC-X-Y. Among them, KLC-700–2 possessed a hierarchical porous structure, high specific surface area (851.3 m<sup>2</sup>·g<sup>−1</sup>), large pore volume (0.53 cm<sup>3</sup>·g<sup>−1</sup>), appropriate pore size distribution (D = 2.49 nm), and abundant oxygen- (<img>COOH and <img>OH) and sulfur-containing (<img>SO<sub>3</sub>H and <img>SH) functional groups. Notably, the synthesized KLC-700–2 displayed excellent adsorption performance for Tl(I) with a maximum adsorption amount of 523.7 mg·g<sup>−1</sup>. After five consecutive adsorption–desorption processes, the adsorption amount of Tl(Ⅰ) by KLC-700–2 decreased slightly, which still reached 85.6 % of the initial adsorption amount, and its own structural properties didn’t change significantly, indicating that KLC-700–2 had good stability and reusability. The adsorption process of Tl(Ⅰ) on KLC-700–2 was verified to be spontaneous and endothermic, and conformed to the pseudo second order and Langmuir models by adsorption kinetic, isotherm, and thermodynamic studies. By comparing the physicochemical properties of KLC-700–2 before and after adsorption of Tl(I), it was confirmed that the adsorption of Tl(Ⅰ) on KLC-700–2 was co-controlled by chemical and physical adsorption, including ion exchange, precipitation reaction, surface complexation, pore filling and electrostatic attraction.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132261"},"PeriodicalIF":8.1,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143478721","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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