Journal of Membrane Science最新文献_第4页

Engineering charge spatial distribution and transport highways in mix-charged polyamide nanofilms for ultra-permselective Li+/Mg2+ separation

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-20 DOI: 10.1016/j.memsci.2025.123882

Ping Hu , Minzheng Yu , Mengyang Yang , Zewen Xu , Dongxiao Yang , Haojie Song , Xiaozhuan Zhang , Meng You , Bingbing Yuan , Q. Jason Niu

In addition to pore structure and surface charge, the charge spatial distribution within NF membranes plays a crucial role in ion transport process. However, precisely tuning this charge distribution remains a significant challenge. Here, we construct the mix-charged thin-film nanocomposite (m-TFN) membranes with tailorable charge spatial distribution for highly efficient Li⁺/Mg²⁺ separation by incorporating quaternary ammonium-functionalized UiO-66-QA nanocrystals into the interfacial polymerization process. The UiO-66-QA nanocrystals are synthesized via a facile post-synthetic modification. The addition of UiO-66-QA nanocrystals benefits to narrow pore size distribution and lower inner negative charge of the mix-charged polyamide nanofilms. Furthermore, these nanocrystals serve as both templates for ordered nanostructure formation and additional transport pathways, significantly enhancing water permeance. As a result, the m-TFN membranes, characterized by a heterogeneous charge distribution and uniform pore structure, exhibit remarkable Li⁺/Mg²⁺ selectivity of 323.93, along with competitive salt/water flux ranging from 227.22 ± 13.3 to 250.2 ± 7.4 L m⁻² h⁻¹, striking a better trade-off between Li⁺/Mg²⁺ selectivity and permeability. Moreover, the SDEM model analysis further reveals that it evidences a higher Li purity and Li recovery compared to current state-of-the-art NF membranes. This work presents a promising strategy for fine-tuning charge distribution and pore structure to achieve high-performance ion separation.

{"title":"Engineering charge spatial distribution and transport highways in mix-charged polyamide nanofilms for ultra-permselective Li+/Mg2+ separation","authors":"Ping Hu , Minzheng Yu , Mengyang Yang , Zewen Xu , Dongxiao Yang , Haojie Song , Xiaozhuan Zhang , Meng You , Bingbing Yuan , Q. Jason Niu","doi":"10.1016/j.memsci.2025.123882","DOIUrl":"10.1016/j.memsci.2025.123882","url":null,"abstract":"<div><div>In addition to pore structure and surface charge, the charge spatial distribution within NF membranes plays a crucial role in ion transport process. However, precisely tuning this charge distribution remains a significant challenge. Here, we construct the mix-charged thin-film nanocomposite (m-TFN) membranes with tailorable charge spatial distribution for highly efficient Li<sup>+</sup>/Mg<sup>2+</sup> separation by incorporating quaternary ammonium-functionalized UiO-66-QA nanocrystals into the interfacial polymerization process. The UiO-66-QA nanocrystals are synthesized via a facile post-synthetic modification. The addition of UiO-66-QA nanocrystals benefits to narrow pore size distribution and lower inner negative charge of the mix-charged polyamide nanofilms. Furthermore, these nanocrystals serve as both templates for ordered nanostructure formation and additional transport pathways, significantly enhancing water permeance. As a result, the m-TFN membranes, characterized by a heterogeneous charge distribution and uniform pore structure, exhibit remarkable Li<sup>+</sup>/Mg<sup>2+</sup> selectivity of 323.93, along with competitive salt/water flux ranging from 227.22 ± 13.3 to 250.2 ± 7.4 L m<sup>−2</sup> h<sup>−1</sup>, striking a better trade-off between Li<sup>+</sup>/Mg<sup>2+</sup> selectivity and permeability. Moreover, the SDEM model analysis further reveals that it evidences a higher Li purity and Li recovery compared to current state-of-the-art NF membranes. This work presents a promising strategy for fine-tuning charge distribution and pore structure to achieve high-performance ion separation.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123882"},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Sustainable and exceptional Li+ /Mg2+selectivity through electrocoagulation enhanced triamino guanidine modified membrane

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-20 DOI: 10.1016/j.memsci.2025.123884

Bin Liu , Xinyue Cui , Xiaozhen Lu , Xuewu Zhu , Lin Wang , Junyong Zhu

Positively charged polyamide (PA) nanofiltration (NF) membranes with sub-nanopores show promise for lithium extraction from salt-lake brines with high Mg²⁺/Li⁺ ratios. This study introduces the use of triamino guanidine (TG), a highly positively charged molecule, to regulate grafting on monolayer PA membranes, resulting in dual-layer (PEI-TMC-TG) NF membranes. The monolayer PA membranes were created via spin-coating assisted interfacial polymerization between polyethyleneimine (PEI) and tricarbonyl chloride (TMC). The PEI/TMC-TG NF membranes exhibited several advantages over unmodified PEI-TMC NF membranes, including higher positive charge density, narrower pore size distribution, excellent hydrophilicity, and a more porous separation layer microstructure. Experimental results indicated that enhanced Donnan effect, size sieving, and dielectric repulsion within the sub-nanopores contributed to exceptional Li⁺/Mg²⁺ selectivity during filtration of East Taijiner brine (S_Li+_/Mg²⁺ = 64.5). Furthermore, the TG hydrophilic layer significantly improved water permeability (15.4 LMH/bar) and long-term stability. To reduce membrane fouling in the charge-positive NF process by removing organic matter from complex salt lake brine, we explored electrocoagulation as a pre-treatment method and identified optimal conditions for the EC-NF process. This strategy maximizes sustainable lithium recovery from brine in an economically viable green manner while enhancing the efficiency of NF membranes for lithium extraction from salt lakes.

{"title":"Sustainable and exceptional Li+ /Mg2+selectivity through electrocoagulation enhanced triamino guanidine modified membrane","authors":"Bin Liu , Xinyue Cui , Xiaozhen Lu , Xuewu Zhu , Lin Wang , Junyong Zhu","doi":"10.1016/j.memsci.2025.123884","DOIUrl":"10.1016/j.memsci.2025.123884","url":null,"abstract":"<div><div>Positively charged polyamide (PA) nanofiltration (NF) membranes with sub-nanopores show promise for lithium extraction from salt-lake brines with high Mg<sup>2+</sup>/Li<sup>+</sup> ratios. This study introduces the use of triamino guanidine (TG), a highly positively charged molecule, to regulate grafting on monolayer PA membranes, resulting in dual-layer (PEI-TMC-TG) NF membranes. The monolayer PA membranes were created via spin-coating assisted interfacial polymerization between polyethyleneimine (PEI) and tricarbonyl chloride (TMC). The PEI/TMC-TG NF membranes exhibited several advantages over unmodified PEI-TMC NF membranes, including higher positive charge density, narrower pore size distribution, excellent hydrophilicity, and a more porous separation layer microstructure. Experimental results indicated that enhanced Donnan effect, size sieving, and dielectric repulsion within the sub-nanopores contributed to exceptional Li<sup>+</sup>/Mg<sup>2+</sup> selectivity during filtration of East Taijiner brine (S<sub>Li</sub>+<sub>/Mg</sub><sup>2+</sup> = 64.5). Furthermore, the TG hydrophilic layer significantly improved water permeability (15.4 LMH/bar) and long-term stability. To reduce membrane fouling in the charge-positive NF process by removing organic matter from complex salt lake brine, we explored electrocoagulation as a pre-treatment method and identified optimal conditions for the EC-NF process. This strategy maximizes sustainable lithium recovery from brine in an economically viable green manner while enhancing the efficiency of NF membranes for lithium extraction from salt lakes.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123884"},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463391","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hydrophilic and hydrophobic dual-side-linked poly(carbazole-butanedione) anion exchange membranes for water electrolysis and fuel cells applications

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-20 DOI: 10.1016/j.memsci.2025.123840

Wenli Ma , Lin Tian , Qingzhi Zhang , Lijian Shangguan , Fanghui Wang , Hong Zhu

To overcome the imbalance between high ionic conductivity, dimensional stability and strong alkali resistance in anion exchange membranes (AEMs), this work discarded the traditional polymer structure with cationic main chains, while prepared n-DTMA-PHCZBDO AEMs with different alkyl chain lengths by combining hydrophilic bi-cationic side chains and hydrophobic alkyl long side chains. The performance test results showed that membrane 6-DTMA-PHCZBDO has high ionic conductivity (169.2 mS cm⁻¹), good dimensional stability (WU 140.3 %, SR 30.1 %) and excellent mechanical properties (55.3 MPa). Particularly, the ionic conductivity and tensile strength degradation rate of membrane 6-DTMA-PHCZBDO were less than 10 % after stabilization in 2 M NaOH at 80 °C for 2000 h, showing outstanding alkali resistance. Besides, It not only exhibited low resistance (R_ohm 0.134 Ω cm² and R_ct 0.035 Ω cm²), high current density at 40 °C (1.00 A cm⁻²), 50 °C (1.83 A cm⁻²) and 60 °C (2.40 A cm⁻²) in 2.2V, but also showed good durability (degradation rate 1.71 mV h⁻¹, at 1000 mA cm⁻² for 60 h) in anion exchange membrane water electrolysis (AEMWEs). Importantly, membrane 6-DTMA-PHCZBDO could be well realized for dual application of AEMWEs and fuel cells, which also had good H₂–O₂ fuel cell power density (490.93 mW cm⁻²). Therefore, the hydrophilic and hydrophobic dual side linking branches can enhance the comprehensive performance of AEMs and can facilitate the application of it in AEMWEs and H₂–O₂ fuel cell.

{"title":"Hydrophilic and hydrophobic dual-side-linked poly(carbazole-butanedione) anion exchange membranes for water electrolysis and fuel cells applications","authors":"Wenli Ma , Lin Tian , Qingzhi Zhang , Lijian Shangguan , Fanghui Wang , Hong Zhu","doi":"10.1016/j.memsci.2025.123840","DOIUrl":"10.1016/j.memsci.2025.123840","url":null,"abstract":"<div><div>To overcome the imbalance between high ionic conductivity, dimensional stability and strong alkali resistance in anion exchange membranes (AEMs), this work discarded the traditional polymer structure with cationic main chains, while prepared n-DTMA-PHCZBDO AEMs with different alkyl chain lengths by combining hydrophilic bi-cationic side chains and hydrophobic alkyl long side chains. The performance test results showed that membrane 6-DTMA-PHCZBDO has high ionic conductivity (169.2 mS cm<sup>−1</sup>), good dimensional stability (WU 140.3 %, SR 30.1 %) and excellent mechanical properties (55.3 MPa). Particularly, the ionic conductivity and tensile strength degradation rate of membrane 6-DTMA-PHCZBDO were less than 10 % after stabilization in 2 M NaOH at 80 °C for 2000 h, showing outstanding alkali resistance. Besides, It not only exhibited low resistance (R<sub>ohm</sub> 0.134 Ω cm<sup>2</sup> and R<sub>ct</sub> 0.035 Ω cm<sup>2</sup>), high current density at 40 °C (1.00 A cm<sup>−2</sup>), 50 °C (1.83 A cm<sup>−2</sup>) and 60 °C (2.40 A cm<sup>−2</sup>) in 2.2V, but also showed good durability (degradation rate 1.71 mV h<sup>−1</sup>, at 1000 mA cm<sup>−2</sup> for 60 h) in anion exchange membrane water electrolysis (AEMWEs). Importantly, membrane 6-DTMA-PHCZBDO could be well realized for dual application of AEMWEs and fuel cells, which also had good H<sub>2</sub>–O<sub>2</sub> fuel cell power density (490.93 mW cm<sup>−2</sup>). Therefore, the hydrophilic and hydrophobic dual side linking branches can enhance the comprehensive performance of AEMs and can facilitate the application of it in AEMWEs and H<sub>2</sub>–O<sub>2</sub> fuel cell.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123840"},"PeriodicalIF":8.4,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143487466","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancing gas selectivity in thin-film composite carbon molecular sieve membranes by platinum sputtering

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-19 DOI: 10.1016/j.memsci.2025.123880

Wojciech Ogieglo , Tiara Puspasari , Xiaofan Hu , Nimer Wehbe , Mohamed B. Hassine , Nabeel Aslam , Syed N.R. Kazmi , Ingo Pinnau

We present a novel approach to significantly boost gas-pair selectivity of thin-film composite (TFC) carbon molecular sieve (CMS) membranes by sputtering platinum on the surface of the CMS precursor polymer prior to pyrolysis. A polyimide of intrinsic microporosity (PIM-PI), 6FDA-HTB, was selected as the CMS precursor which had previously been shown to transform into an excellent CMS membrane material at moderate pyrolysis temperatures (550–600 °C). Deposition of Pt at high ion currents combined with subsequent pyrolysis at 550 °C leads to the development of an ultrathin (10–20 nm thick) Pt/CMS intermix layer consisting of a CMS matrix with a large volume fraction of embedded, fused Pt nanoparticles. The Pt phase seems to stabilize the micropores of the intermixed CMS phase as well as limit the undesired impact of defects leading to a dramatic enhancement of gas-pair selectivity of the modified TFC CMS membranes (e.g. H₂/CH₄ > 1100, CO₂/CH₄ ∼100, O₂/N₂ ∼ 11) which represent improvements of 3300, 370, and 100 % in comparison to the non-Pt-sputtered CMS control membranes. This novel, simple and effective procedure may be extendable to other types of CMS polymer precursors, membrane supports, alternative sputtering metals and the deposition parameters can be easily tuned to balance the membrane permeance against the desired selectivity.

{"title":"Enhancing gas selectivity in thin-film composite carbon molecular sieve membranes by platinum sputtering","authors":"Wojciech Ogieglo , Tiara Puspasari , Xiaofan Hu , Nimer Wehbe , Mohamed B. Hassine , Nabeel Aslam , Syed N.R. Kazmi , Ingo Pinnau","doi":"10.1016/j.memsci.2025.123880","DOIUrl":"10.1016/j.memsci.2025.123880","url":null,"abstract":"<div><div>We present a novel approach to significantly boost gas-pair selectivity of thin-film composite (TFC) carbon molecular sieve (CMS) membranes by sputtering platinum on the surface of the CMS precursor polymer prior to pyrolysis. A polyimide of intrinsic microporosity (PIM-PI), 6FDA-HTB, was selected as the CMS precursor which had previously been shown to transform into an excellent CMS membrane material at moderate pyrolysis temperatures (550–600 °C). Deposition of Pt at high ion currents combined with subsequent pyrolysis at 550 °C leads to the development of an ultrathin (10–20 nm thick) Pt/CMS intermix layer consisting of a CMS matrix with a large volume fraction of embedded, fused Pt nanoparticles. The Pt phase seems to stabilize the micropores of the intermixed CMS phase as well as limit the undesired impact of defects leading to a dramatic enhancement of gas-pair selectivity of the modified TFC CMS membranes (e.g. H<sub>2</sub>/CH<sub>4</sub> > 1100, CO<sub>2</sub>/CH<sub>4</sub> ∼100, O<sub>2</sub>/N<sub>2</sub> ∼ 11) which represent improvements of 3300, 370, and 100 % in comparison to the non-Pt-sputtered CMS control membranes. This novel, simple and effective procedure may be extendable to other types of <span>CMS</span> polymer precursors, membrane supports, alternative sputtering metals and the deposition parameters can be easily tuned to balance the membrane permeance against the desired selectivity.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123880"},"PeriodicalIF":8.4,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474533","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A geometric model to predict protein retentions during skim milk microfiltration

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-19 DOI: 10.1016/j.memsci.2025.123865

Hilda Lucy Nyambura , Anja E.M. Janssen , Albert van der Padt , Remko M. Boom

Microfiltration membranes can retain dissolved proteins to some degree, as result of interactions with other components. This work presents a geometric model to describe the limiting transmembrane pressure, flux, and the transmission of dissolved proteins. The effects of temperature and membrane pore size are observed in other factors such as viscosity, membrane resistance and rate of mass transfer. The model could predict the experimental transmembrane flux values at different temperatures. With a decrease in temperature from 15 °C to 5 °C, the viscosity increased from 1.6 mPa s to 2.2 mPa s while the rate of mass transfer decreased with decreasing temperature of the same range from 0.9 × 10⁻⁶ m s⁻¹ to 2 × 10⁻⁶ m s⁻¹. With a change in temperature, there was insignificant difference between the transmission of whey proteins. The same was observed with different pore sizes. This confirmed the hypothesis that the concentration polarization layer that determines the protein transmission being a sieving layer at pressures higher than the limiting transmembrane pressure.

{"title":"A geometric model to predict protein retentions during skim milk microfiltration","authors":"Hilda Lucy Nyambura , Anja E.M. Janssen , Albert van der Padt , Remko M. Boom","doi":"10.1016/j.memsci.2025.123865","DOIUrl":"10.1016/j.memsci.2025.123865","url":null,"abstract":"<div><div>Microfiltration membranes can retain dissolved proteins to some degree, as result of interactions with other components. This work presents a geometric model to describe the limiting transmembrane pressure, flux, and the transmission of dissolved proteins. The effects of temperature and membrane pore size are observed in other factors such as viscosity, membrane resistance and rate of mass transfer. The model could predict the experimental transmembrane flux values at different temperatures. With a decrease in temperature from 15 °C to 5 °C, the viscosity increased from 1.6 mPa s to 2.2 mPa s while the rate of mass transfer decreased with decreasing temperature of the same range from 0.9 × 10<sup>−6</sup> m s<sup>−1</sup> to 2 × 10<sup>−6</sup> m s<sup>−1</sup>. With a change in temperature, there was insignificant difference between the transmission of whey proteins. The same was observed with different pore sizes. This confirmed the hypothesis that the concentration polarization layer that determines the protein transmission being a sieving layer at pressures higher than the limiting transmembrane pressure.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123865"},"PeriodicalIF":8.4,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474534","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Confinement of butanol-affinity polysiloxane nanolayer membrane into fast-diffusion nanoflake arrays for high-efficiency biofuel production

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-18 DOI: 10.1016/j.memsci.2025.123864

Yuecheng Wang , Yujie Ban , Jiayi Liu , Guangqi Zhu , Ziyi Hu , Weishen Yang

Pervaporation membranes with high n-butanol production have potential applications for the recovery of renewable biofuels from diluted fermentation broth. Proper structuring of membranes is necessary for pursuing combined performance metrics of high liquid flux and separation factors but poses a challenge. In this study, a loosely packed hydrophilic layer composed of a vertical nanoflake array was used to create a low-friction and low-barrier passage for n-butanol (as a fast diffusion layer), which took advantage of its surface areal topography to lock a cross-linked polysiloxane nanolayer for n-butanol capture (as a butanol affinity layer). The fast diffusion-butanol affinity (FD-BA) membranes demonstrated exceptional pervaporation performances for a 1.0 wt% aqueous n-butanol solution, achieving a flux of 15.8 kg m⁻² h⁻¹ and a separation factor of 24. When we coupled a single-pass membrane pervaporation with a simple liquid‒liquid phase separation technique at room temperature, 83.3 wt% n-butanol can be obtained. This FD-BA membrane can be scaled to large-area plate and tubular membranes.

正丁醇产量高的渗透膜在从稀释的发酵液中回收可再生生物燃料方面具有潜在的应用价值。膜的适当结构对于追求高液体通量和分离因子的综合性能指标是必要的，但也是一项挑战。在这项研究中，由垂直纳米片阵列组成的松散亲水层被用来为正丁醇（作为快速扩散层）创建一个低摩擦、低阻力的通道，该层利用其表面形貌锁定了一个用于捕获正丁醇的交联聚硅氧烷纳米层（作为丁醇亲和层）。快速扩散-丁醇亲和（FD-BA）膜在 1.0 wt% 的正丁醇水溶液中表现出卓越的渗透性能，通量达到 15.8 kg m-2 h-1，分离因子达到 24。当我们在室温下将单程膜渗透与简单的液-液相分离技术相结合时，可获得 83.3 wt% 的正丁醇。这种 FD-BA 膜可以扩展到大面积的板式膜和管式膜。

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引用次数: 0

Co-exchanged SSZ-13 zeolite membrane for boosting CO2/N2 separation

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-18 DOI: 10.1016/j.memsci.2025.123874

Dongxu Gai , Yixing Guan , Dan Ma , Yongyan Deng , Junchao Dong , Ziyang Wang , Jialu Li , I. Agirrezabal-Telleria , Xiaoqin Zou

Zeolite membranes such as SSZ-13 combining the pore structures of 3.8 Å × 3.8 Å and membrane advantages of low energy consumption are promising for gas separation of CO₂ from N₂. However, the fabrication of high-quality SSZ-13 zeolite membranes with excellent CO₂/N₂ separation performance remains a challenge. In this work, a facile strategy of ion exchange is utilized in the fabrication of highly continuous crystallized Co-SSZ-13 membrane with modified pore chemistry. The Co-SSZ-13 membrane exhibits the optimal CO₂ permeance of 6.6 × 10⁻⁸ mol s⁻¹ m⁻² Pa⁻¹ and CO₂/N₂ separation factor (SF) of 27.7 which is 154 % and 80 % higher than Na-SSZ-13 and Ca-SSZ-13 membranes, respectively. Moreover, such outstanding performance of the Co-SSZ-13 membrane is long-term stabilized for CO₂/N₂ separation. The introduction of Co(II) ions in the SSZ-13 structure can effectively reduce the pore size and provide the high electron density and d-orbitals which enhance both electrostatic and coordination interactions with CO₂. This study provides guidance for the fabrication of advanced membranes with high-efficiency CO₂ separation performance.

{"title":"Co-exchanged SSZ-13 zeolite membrane for boosting CO2/N2 separation","authors":"Dongxu Gai , Yixing Guan , Dan Ma , Yongyan Deng , Junchao Dong , Ziyang Wang , Jialu Li , I. Agirrezabal-Telleria , Xiaoqin Zou","doi":"10.1016/j.memsci.2025.123874","DOIUrl":"10.1016/j.memsci.2025.123874","url":null,"abstract":"<div><div>Zeolite membranes such as SSZ-13 combining the pore structures of 3.8 Å × 3.8 Å and membrane advantages of low energy consumption are promising for gas separation of CO<sub>2</sub> from N<sub>2</sub>. However, the fabrication of high-quality SSZ-13 zeolite membranes with excellent CO<sub>2</sub>/N<sub>2</sub> separation performance remains a challenge. In this work, a facile strategy of ion exchange is utilized in the fabrication of highly continuous crystallized Co-SSZ-13 membrane with modified pore chemistry. The Co-SSZ-13 membrane exhibits the optimal CO<sub>2</sub> permeance of 6.6 × 10<sup>−8</sup> mol s<sup>−1</sup> m<sup>−2</sup> Pa<sup>−1</sup> and CO<sub>2</sub>/N<sub>2</sub> separation factor (SF) of 27.7 which is 154 % and 80 % higher than Na-SSZ-13 and Ca-SSZ-13 membranes, respectively. Moreover, such outstanding performance of the Co-SSZ-13 membrane is long-term stabilized for CO<sub>2</sub>/N<sub>2</sub> separation. The introduction of Co(II) ions in the SSZ-13 structure can effectively reduce the pore size and provide the high electron density and d-orbitals which enhance both electrostatic and coordination interactions with CO<sub>2</sub>. This study provides guidance for the fabrication of advanced membranes with high-efficiency CO<sub>2</sub> separation performance.</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":"722 ","pages":"Article 123874"},"PeriodicalIF":8.4,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143454567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rational study on the evolution mechanism of PVDF crystalline phase to prepare high-performance electroactive PVDF membranes

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-18 DOI: 10.1016/j.memsci.2025.123879

Xiao Kong , Qi-Zheng Wang , Ye-Fei Wang , Hao-Ming Huo , Jun Zhao , Xin Wu , Dandan Zhou , Yan-Jiao Chang , Zhong Ma

Compared with the routine anti-fouling methods, leveraging polarity and piezoelectricity of the electroactive PVDF membrane itself to improve the anti-fouling ability has been attracting increasing attention due to the better sustainability and stability. However, existing empirical research methods about the manipulation of crystal polymorphs lack in-depth scientific exploration regarding the formation and evolution mechanism of PVDF crystals, facing the trade-off dilemma between enhancing β-phase content and improving permeability of PVDF membranes. In this paper, from the viewpoint of intermolecular interaction during phase separation process, the effect of surfactant type on the crystal polymorphs, morphology and performance of PVDF membranes is thoroughly studied. A kind of biaxial traction effect (BTE) based on the polymer-solvent-coagulant interactions during the phase separation process is proposed. The introduction of ionic surfactants is discovered to enhance the BTE owing to the presence of ion-dipole interactions with –CH₂ groups of PVDF. As a result, the β-phase content of PVDF membranes is elevated to 97 %. Moreover, using ionic surfactants to enhance the BTE decreases the pore size while increases the number of through-pores, thus improving the perm-selectivity of the PVDF membranes (increased by 3.4 times). The continuous anti-fouling testing reveals that the vibration of piezoelectric PVDF membranes excited by AC signals has positive but limited effects on alleviating membrane fouling. This study inspires the rational manipulation of crystal polymorph and membrane performance of electroactive PVDF membranes.

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引用次数: 0

Exploring Nafion's microstructural changes and the impact on the performance of PEMFC under high-energy radiation

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-18 DOI: 10.1016/j.memsci.2025.123867

Shuai Yang, Yiyang Zeng, Chengjian Xiao, Mao Yang, Hongbing Chen, Qiang Liu, Wei Huang, Yu Gong, Shuming Peng

PEMFCs, crucial for space energy needs, rely on Nafion for proton conductivity and durability. High-energy radiation in space can degrade PEMFC performance. Therefore, in-depth research on the microstructural evolution of Nafion under high-energy radiation and its impact on PEMFC's performance is of great significance for promoting the application of fuel cell technology in the space field. This work combines experimental and computational simulation methods to propose the evolution mechanism of C–O–C rupture and –COOH generation in Nafion under high-energy radiation. The new molecular structure formed has increased chain spacing and free volume, enhanced water absorption and swelling properties, and decreased structural stability. When the radiation absorption dose exceeds 400 kGy, Nafion completely becomes brittle and cannot be used. The change in Nafion at 0–400 kGy structure resulted in a significant overall decrease in mechanical properties (decreased by 73.76 %), proton conductivity (decreased by 40.59 %), output power density (from 480.00 to 30.00 mW/cm²), hydrogen permeation (from 2.26 to 60.75 mA/cm²), and open-circuit voltage (from 1.01 to 0.27 V). This study not only enhances the understanding of Nafion's structural evolution and performance degradation under high-energy radiation but also provides important research directions for developing high-performance PEMFCs suitable for the space environment.

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引用次数: 0

A “grab-and-throw” access for monomer diffusion in interfacial polymerization process for high-efficiency polyamide membrane in water purification

IF 8.4 1区工程技术 Q1 ENGINEERING, CHEMICAL

Journal of Membrane Science

Pub Date : 2025-02-18 DOI: 10.1016/j.memsci.2025.123871

Xiyue Cai , Yonggang li , Zhenyu Xi , Chen Yun , Lianghong Yin , Jing Guo , Yaohan Chen , Shenghai Li , Suobo Zhang

The surface structures of polyamide (PA) layer are closely related to the monomers diffusion during interfacial polymerization (IP) process and is one of the significant issues affecting nanofiltration separation performance. However, nanofiltration membrane prepared by the conventional interfacial polymerization method usually has a relatively smooth surface, which limits the effective filtration area leading to low water permeation. Effective strategies to control monomer diffusion also need to be developed. To solve these problems, carbon disulfide (CS₂) is inferred as an additive to form piperazine n-dithiocarbonate (PIP-CS₂) in aqueous phase, which can reversibly protonate piperazine (PIP) into PIP-CS₂^- anion and PIP-H⁺ cation. Due to the amphiphilic piperazine part, PIP-CS₂ and PIP-CS₂^-/PIP-H⁺ ion pair tend to gather at water-oil interface offering a special “grab-and-throw” access for free PIP monomer. In this way, the diffusion of PIP monomer is well-controlled to fabricate an ordered nanoscale hollow surface of polyamide layer. The exceptional surface structure significantly affects the properties of nanofiltration membrane. the pure water flux enlarged from 6.53 to 17.65 L m⁻¹ h⁻¹ bar⁻¹. Na₂SO₄ rejection was maintained at more than 98 %. the separation coefficient of Cl⁻ and SO₄²⁻ enhanced from 19.14 to 54.80. This work provided a novel and effective way to increase the flux and adjust the surface structure and cross-linking degree in nanofiltration membrane production.

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引用次数: 0