Pub Date : 2025-01-22DOI: 10.1016/j.seppur.2025.131744
Zhenzhen Zhang, Yucong Ge, Li Yang, Fang Liu, Xiao Yang, Qingfang Li, Yi Li, Kunlei Liu
Enhancing gas–liquid mass transfer efficiency while reducing operational energy consumption and cost is essential for the industrial application of amine-based CO2 capture technology. This study proposes a novel compact multi-fluid absorber that integrates spray, bubble and packed to reduce the absorber tower’s size. The absorbent is atomized into fine droplets, which then pass through a foaming network to form more bubbles, increasing the gas–liquid contact area and enhancing CO2 absorption. Four surfactants were evaluated for their foaming performance, viscosity, and surface tension when complexed with monoethanolamine (MEA). CO2 uptake and equilibrium solubility of these solutions were tested in a bubbling vessel and analyzed using Nuclear Magnetic Resonance (NMR). Based on these experiments, the most effective absorber was applied to the novel compact multi-fluid absorber. The effects of gas and liquid flow rates on CO2 performance were tested, revealing relationships between flow rates, bubble sizes, and absorption performance. The results show that the novel absorber improves absorption performance by over 30% compared to the unimproved version. It achieves a CO2 removal efficiency of 80% at gas–liquid ratios up to 160 and a total absorption rate of 3.77 kmol/m3·h.
{"title":"Innovative compact multi-fluid absorber for CO2 capture using advanced absorbents and microbubble technology","authors":"Zhenzhen Zhang, Yucong Ge, Li Yang, Fang Liu, Xiao Yang, Qingfang Li, Yi Li, Kunlei Liu","doi":"10.1016/j.seppur.2025.131744","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131744","url":null,"abstract":"Enhancing gas–liquid mass transfer efficiency while reducing operational energy consumption and cost is essential for the industrial application of amine-based CO<sub>2</sub> capture technology. This study proposes a novel compact multi-fluid absorber that integrates spray, bubble and packed to reduce the absorber tower’s size. The absorbent is atomized into fine droplets, which then pass through a foaming network to form more bubbles, increasing the gas–liquid contact area and enhancing CO<sub>2</sub> absorption. Four surfactants were evaluated for their foaming performance, viscosity, and surface tension when complexed with monoethanolamine (MEA). CO<sub>2</sub> uptake and equilibrium solubility of these solutions were tested in a bubbling vessel and analyzed using Nuclear Magnetic Resonance (NMR). Based on these experiments, the most effective absorber was applied to the novel compact multi-fluid absorber. The effects of gas and liquid flow rates on CO<sub>2</sub> performance were tested, revealing relationships between flow rates, bubble sizes, and absorption performance. The results show that the novel absorber improves absorption performance by over 30% compared to the unimproved version. It achieves a CO<sub>2</sub> removal efficiency of 80% at gas–liquid ratios up to 160 and a total absorption rate of 3.77 kmol/m<sup>3</sup>·h.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"11 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991897","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131717
Haitao Ren, Shuochen Wang, Abdelkader Labidi, Bao Pan, Jianmin Luo, Chuanyi Wang
Constructing low-cost and wide visible light response S-scheme heterojunctions is crucial for their photocatalytic efficiency and practical applications. Herein, a novel N-CQDs/UBWO composite was designed by combining nitrogen-doped carbon quantum dots (N-CQDs) obtained from bio-waste lignin with Bi2WO6 ultrathin nanosheets (UBWO) using in-situ hydrothermal approach. The work function analyses, electron paramagnetic resonance (EPR) and in-situ X-ray photoelectron spectroscopy (XPS) evidenced an S-scheme charge transfer mechanism between N-CQD and UBWO during photocatalytic reactions, which endows the composite system a high photocatalytic redox and charge space separation capabilities. Besides, the up-conversion properties of N-CQDs render N-CQDs/UBWO composites an enhanced visible light response. Therefore, the optimized 3 wt%N-CQD/UBWO S-scheme heterojunction exhibited favorable tetracycline degradation performance, with a degradation efficiency of 85.0 % within 40 min of reaction time, and first-order rate constant (k) of 2.6 and 20.3 times greater than that of UBWO and N-CQDs, respectively. Furthermore, referring to Fukui function calculations and liquid chromatography-mass spectrometry (LC-MS), degraded products and three degradation routes for tetracycline were proposed. The results of the toxicity estimation software tool (T.E.S.T) and mung bean cultivation demonstrated that the intermediate products of tetracycline degradation are of low toxicity. This study provides insights into designing superior S-scheme heterojunctions using CQDs derived from waste biomass for green and efficient removal of antibiotics from wastewater.
{"title":"Nanoengineering of ultrathin N-CQDs/Bi2WO6 S-scheme heterojunction for enhanced photodegradation of antibiotics as emerging contaminants: Mechanism insight and toxicity assessment","authors":"Haitao Ren, Shuochen Wang, Abdelkader Labidi, Bao Pan, Jianmin Luo, Chuanyi Wang","doi":"10.1016/j.seppur.2025.131717","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131717","url":null,"abstract":"Constructing low-cost and wide visible light response S-scheme heterojunctions is crucial for their photocatalytic efficiency and practical applications. Herein, a novel N-CQDs/UBWO composite was designed by combining nitrogen-doped carbon quantum dots (N-CQDs) obtained from bio-waste lignin with Bi<sub>2</sub>WO<sub>6</sub> ultrathin nanosheets (UBWO) using <em>in-situ</em> hydrothermal approach. The work function analyses, electron paramagnetic resonance (EPR) and <em>in-situ</em> X-ray photoelectron spectroscopy (XPS) evidenced an S-scheme charge transfer mechanism between N-CQD and UBWO during<!-- --> <!-- -->photocatalytic<!-- --> <!-- -->reactions, which endows the composite system a high photocatalytic redox and charge space separation capabilities. Besides, the up-conversion properties of N-CQDs render N-CQDs/UBWO composites an<!-- --> <!-- -->enhanced visible light response. Therefore, the optimized 3 wt%N-CQD/UBWO S-scheme heterojunction exhibited favorable tetracycline degradation performance, with a degradation efficiency of 85.0 % within 40 min of reaction time, and first-order rate constant (k) of 2.6 and 20.3 times greater than that of UBWO and N-CQDs, respectively. Furthermore, referring to Fukui function calculations and liquid chromatography-mass spectrometry (LC-MS), degraded products and three degradation routes for tetracycline were proposed. The results of the toxicity estimation software tool (T.E.S.T) and mung bean cultivation demonstrated that the intermediate products of tetracycline degradation are of low toxicity. This study provides insights into designing superior S-scheme heterojunctions using CQDs derived from waste biomass for green and efficient removal of antibiotics from wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"153 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020899","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}
The environmentally friendly batch preparation of metal-organic framework (MOF) adsorbents is a crucial step toward their application in ammonia capture and separation. Simultaneously, directly observing the adsorption structure of ammonia poses a highly challenging issue for the design of efficient ammonia adsorbents. Here, we report the green batch preparation of NiCl2(pyz)2 from waste Ni MH batteries for efficient ammonia adsorption and separation. It is found that the NH3 uptake of NiCl2(pyz)2 is as high as 21.7 mmol/g at 25 °C and 1.0 bar. This adsorbent has excellent low-concentration ammonia adsorption capacity and shows potential for use in protective equipment to reduce ammonia concentration in important scenarios, such as ammonia leakage. The binding of NH3 in the adsorbent was directly observed by the transition from a single crystal of NiCl2(pyz)2 to a single crystal structure of NiCl2(NH3)6. PXRD, UV-DRS, XPS, and FT-IR results showed that competitive coordination is the main adsorption mechanism. This work has become a typical example of environmentally friendly batch preparation of MOF adsorbents from waste Ni MH batteries for ammonia adsorption, and provides guidance for the design of new and efficient MOF adsorbents through the observation of single crystal structures.
{"title":"Efficient ammonia capture via reversible single crystal structural transformation of a simple Ni metal-organic framework","authors":"Zhiyong Li, Yibo Fu, Liyong Zhai, Zhenzhen Wang, Yunlei Shi, Qingchun Xia, Huiyong Wang","doi":"10.1016/j.seppur.2025.131743","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131743","url":null,"abstract":"The environmentally friendly batch preparation of metal-organic framework (MOF) adsorbents is a crucial step toward their application in ammonia capture and separation. Simultaneously, directly observing the adsorption structure of ammonia poses a highly challenging issue for the design of efficient ammonia adsorbents. Here, we report the green batch preparation of NiCl<sub>2</sub>(pyz)<sub>2</sub> from waste Ni MH batteries for efficient ammonia adsorption and separation. It is found that the NH<sub>3</sub> uptake of NiCl<sub>2</sub>(pyz)<sub>2</sub> is as high as 21.7 mmol/g at 25 °C and 1.0 bar. This adsorbent has excellent low-concentration ammonia adsorption capacity and shows potential for use in protective equipment to reduce ammonia concentration in important scenarios, such as ammonia leakage. The binding of NH<sub>3</sub> in the adsorbent was directly observed by the transition from a single crystal of NiCl<sub>2</sub>(pyz)<sub>2</sub> to a single crystal structure of NiCl<sub>2</sub>(NH<sub>3</sub>)<sub>6</sub>. PXRD, UV-DRS, XPS, and FT-IR results showed that competitive coordination is the main adsorption mechanism. This work has become a typical example of environmentally friendly batch preparation of MOF adsorbents from waste Ni MH batteries for ammonia adsorption, and provides guidance for the design of new and efficient MOF adsorbents through the observation of single crystal structures.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991898","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}
Carbon materials have garnered increasing attention due to their capacity for activating persulfate in pollutant degradation. Among these materials, acetylene black (AB), which possesses a distinct sp2 configuration compared to conventional carbon materials, has been reported as an efficient activator for PDS. However, challenges pertaining to separation and reusability impede its practical application. In this study, we synthesized magnetic acetylene black (MAB) through a facile hydrothermal method. Batch experiments demonstrated that MAB exhibits excellent adsorption performance for the target pollutant and can effectively activate PDS, resulting in over 99 % degradation of BPA when using 1 g/L of MAB and 1 mM PDS. Furthermore, MAB exhibited remarkable efficacy over a broad pH range, superior tolerance towards inorganic anionic species, and easy separation from solution facilitated by an external magnet. The results of radical quenching experiments and electron paramagnetic resonance confirmed the significant role played by an electron transfer pathway in the removal process. Additionally, the OCO groups of MAB (such as carboxyl) acted as reaction sites, facilitating this electron transfer mechanism. Moreover, the MAB + PDS system displayed exceptional selectivity for degrading electron-rich organic compounds, and the quantitative structure–activity relationships (QSAR) analysis revealed a strong linear correlation between removal performance and ionization potentials of these organics, further supporting the predominant contribution of the electron transfer pathway involved. Overall, this work not only presents a successful strategy for applying carbon materials in wastewater treatment but also contributes to understanding the mechanisms underlying persulfate activation using highly graphitized carbon materials.
{"title":"Activation of peroxydisulfate for selective degradation of organic pollutants using magnetic acetylene black in sp2 configuration: Synthesis, performance, and mechanism","authors":"Fengkai Yang, Chenlin Hou, Liang Sun, Jinlong Yang, Tianxing Chen, Lipeng Wang, Xiaowei Kong, Yang Zhang","doi":"10.1016/j.seppur.2025.131737","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131737","url":null,"abstract":"Carbon materials have garnered increasing attention due to their capacity for activating persulfate in pollutant degradation. Among these materials, acetylene black (AB), which possesses a distinct sp<sup>2</sup> configuration compared to conventional carbon materials, has been reported as an efficient activator for PDS. However, challenges pertaining to separation and reusability impede its practical application. In this study, we synthesized magnetic acetylene black (MAB) through a facile hydrothermal method. Batch experiments demonstrated that MAB exhibits excellent adsorption performance for the target pollutant and can effectively activate PDS, resulting in over 99 % degradation of BPA when using 1 g/L of MAB and 1 mM PDS. Furthermore, MAB exhibited remarkable efficacy over a broad pH range, superior tolerance towards inorganic anionic species, and easy separation from solution facilitated by an external magnet. The results of radical quenching experiments and electron paramagnetic resonance confirmed the significant role played by an electron transfer pathway in the removal process. Additionally, the O<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>C<img alt=\"double bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/dbnd.gif\" style=\"vertical-align:middle\"/>O groups of MAB (such as carboxyl) acted as reaction sites, facilitating this electron transfer mechanism. Moreover, the MAB + PDS system displayed exceptional selectivity for degrading electron-rich organic compounds, and the quantitative structure–activity relationships (QSAR) analysis revealed a strong linear correlation between removal performance and ionization potentials of these organics, further supporting the predominant contribution of the electron transfer pathway involved. Overall, this work not only presents a successful strategy for applying carbon materials in wastewater treatment but also contributes to understanding the mechanisms underlying persulfate activation using highly graphitized carbon materials.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"52 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020901","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131740
Yao Tang, Xin-ran Zhang, Qiong-fang Yang, Yu-yang Yan, Wei Ding, Wei Du, Fei-nan Hu, Zeng-chao Geng, Chen-yang Xu
Chemical fertilizer products have greatly enhanced the yield and quality of crops, but excessive application has led to harmful accumulation of nitrate (NO3–) and phosphate (PO43-), causing contamination and exacerbating water eutrophication. Developing efficient adsorbent materials is an effective approach to remove excessive nutritional elements in water bodies. This study investigated the adsorption capacities of apple tree branch biochar (AB) for ammonia ion (NH4+), NO3–, and PO43- and also its modified products via the mechanical modification of ball milling (MAB), physical modification of KOH pretreatment (K-MAB), chemical modification of MgCl2/AlCl3 immersion (0.1 Mg-MAB, 0.3 Mg-MAB, 0.1Al-MAB, and 0.3Al-MAB). Results showed that the average diameters of modified biochars ranged from 152 to 438 nm. MAB exhibited an increase in specific surface area and porosity. AB and MAB were rich in calcium carbonate, whereas K-MAB contained potassium-rich carbonate and potassium chloride. Mg-MAB included magnesium nitrate, magnesium oxide, and magnesium hydroxide, while 0.3Al-MAB produced a new amorphous aluminum oxide. The AB, MAB and K-MAB were negatively charged, while the points of zero charge for 0.1 Mg-MAB, 0.3 Mg-MAB, 0.1Al-MAB, and 0.3Al-MAB were 4.0, 5.7, 9.2, and 9.0, respectively. K-MAB demonstrated the highest adsorption capacity for NH4+. NH4+ adsorption on the K-MAB surface was characterized by heterogeneous multilayer adsorption, primarily driven by electrostatic interactions and chemisorption. At pH 10 and 298 K, K-MAB reached a maximum adsorption capacity of 9.24 mg/g. 0.1Al-MAB had the highest adsorption capacity for NO3–. NO3– adsorption on the surface of 0.1Al-MAB primarily involved single-molecule adsorption dominated by chemical interactions. At 298 K, the maximum adsorption capacity of 0.1Al-MAB for NO3– was 43.70 mg/g. 0.3 Mg-MAB showed the best adsorption effect for PO43-. The adsorption mechanism of 0.3 Mg-MAB to PO43- was mainly single-layer chemisorption precipitation, regulated by electrostatic interactions. At pH 7 and 298 K, the maximum adsorption capacity of 0.3 Mg-MAB for PO43- reached 349.29 mg/g. The newly-developed modified apple branch biochar showed promising potential in removing contaminants from degraded water bodies. The results provide valuable insights for the preparation of low-cost, high-efficiency biochar-based adsorbent materials derived from agriculture and forestry-sourced wastes.
化肥产品极大地提高了作物的产量和品质，但过量施用导致硝酸盐（NO3 -）和磷酸盐（PO43-）的有害积累，造成污染，加剧水体富营养化。开发高效吸附材料是去除水体中过量营养元素的有效途径。通过球磨机械改性（MAB）、KOH预处理物理改性（K-MAB）、MgCl2/AlCl3浸渍化学改性（0.1 Mg-MAB、0.3 Mg-MAB、0.1 al -MAB和0.3 al -MAB），研究了苹果树枝生物炭（AB）对氨离子（NH4+）、NO3 -和PO43-的吸附能力及其改性产物。结果表明，改性生物炭的平均直径为152 ~ 438 nm。MAB的比表面积和孔隙率均有所增加。AB和MAB含有丰富的碳酸钙，而K-MAB含有丰富的碳酸钾和氯化钾。Mg-MAB包括硝酸镁、氧化镁和氢氧化镁，0.3Al-MAB产生了一种新的无定形氧化铝。AB、MAB和K-MAB均带负电荷，0.1 Mg-MAB、0.3 Mg-MAB、0.1 al -MAB和0.3 al -MAB的零电荷点分别为4.0、5.7、9.2和9.0。K-MAB对NH4+的吸附能力最高。NH4+在K-MAB表面的吸附表现为非均相多层吸附，主要由静电相互作用和化学吸附驱动。在pH 10和298 K条件下，K- mab的最大吸附量为9.24 mg/g。al - mab对NO3 -的吸附量最高。NO3 -在0.1Al-MAB表面的吸附主要是以化学相互作用为主的单分子吸附。在298 K下，0.1Al-MAB对NO3 -的最大吸附量为43.70 mg/g。0.3 Mg-MAB对PO43-的吸附效果最好。0.3 Mg-MAB对PO43-的吸附机制主要为单层化学吸附沉淀，受静电相互作用调控。在pH 7和298 K条件下，0.3 mg - mab对PO43-的最大吸附量达到349.29 mg/g。新开发的改性苹果枝生物炭在去除降解水体中的污染物方面具有广阔的应用前景。研究结果为从农林废弃物中制备低成本、高效的生物炭基吸附材料提供了有价值的见解。
{"title":"Enhanced removal of the ammonium, nitrate and phosphate by biochars derived from apple tree branches via different modification methods","authors":"Yao Tang, Xin-ran Zhang, Qiong-fang Yang, Yu-yang Yan, Wei Ding, Wei Du, Fei-nan Hu, Zeng-chao Geng, Chen-yang Xu","doi":"10.1016/j.seppur.2025.131740","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131740","url":null,"abstract":"Chemical fertilizer products have greatly enhanced the yield and quality of crops, but excessive application has led to harmful accumulation of nitrate (NO<sub>3</sub><sup>–</sup>) and phosphate (PO<sub>4</sub><sup>3-</sup>), causing contamination and exacerbating water eutrophication. Developing efficient adsorbent materials is an effective approach to remove excessive nutritional elements in water bodies. This study investigated the adsorption capacities of apple tree branch biochar (AB) for ammonia ion (NH<sub>4</sub><sup>+</sup>), NO<sub>3</sub><sup>–</sup>, and PO<sub>4</sub><sup>3-</sup> and also its modified products via the mechanical modification of ball milling (MAB), physical modification of KOH pretreatment (K-MAB), chemical modification of MgCl<sub>2</sub>/AlCl<sub>3</sub> immersion (0.1 Mg-MAB, 0.3 Mg-MAB, 0.1Al-MAB, and 0.3Al-MAB). Results showed that the average diameters of modified biochars ranged from 152 to 438 nm. MAB exhibited an increase in specific surface area and porosity. AB and MAB were rich in calcium carbonate, whereas K-MAB contained potassium-rich carbonate and potassium chloride. Mg-MAB included magnesium nitrate, magnesium oxide, and magnesium hydroxide, while 0.3Al-MAB produced a new amorphous aluminum oxide. The AB, MAB and K-MAB were negatively charged, while the points of zero charge for 0.1 Mg-MAB, 0.3 Mg-MAB, 0.1Al-MAB, and 0.3Al-MAB were 4.0, 5.7, 9.2, and 9.0, respectively. K-MAB demonstrated the highest adsorption capacity for NH<sub>4</sub><sup>+</sup>. NH<sub>4</sub><sup>+</sup> adsorption on the K-MAB surface was characterized by heterogeneous multilayer adsorption, primarily driven by electrostatic interactions and chemisorption. At pH 10 and 298 K, K-MAB reached a maximum adsorption capacity of 9.24 mg/g. 0.1Al-MAB had the highest adsorption capacity for NO<sub>3</sub><sup>–</sup>. NO<sub>3</sub><sup>–</sup> adsorption on the surface of 0.1Al-MAB primarily involved single-molecule adsorption dominated by chemical interactions. At 298 K, the maximum adsorption capacity of 0.1Al-MAB for NO<sub>3</sub><sup>–</sup> was 43.70 mg/g. 0.3 Mg-MAB showed the best adsorption effect for PO<sub>4</sub><sup>3-</sup>. The adsorption mechanism of 0.3 Mg-MAB to PO<sub>4</sub><sup>3-</sup> was mainly single-layer chemisorption precipitation, regulated by electrostatic interactions. At pH 7 and 298 K, the maximum adsorption capacity of 0.3 Mg-MAB for PO<sub>4</sub><sup>3-</sup> reached 349.29 mg/g. The newly-developed modified apple branch biochar showed promising potential in removing contaminants from degraded water bodies. The results provide valuable insights for the preparation of low-cost, high-efficiency biochar-based adsorbent materials derived from agriculture and forestry-sourced wastes.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"24 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991893","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131741
Afshin Tatar, Abbas Zeinijahromi, Manouchehr Haghighi
This research aims to enhance the predictive modelling of hydrogen gas (H2) solubility in n-alkanes using Explainable Artificial Intelligence (XAI) techniques. The focus is on elucidating the impact of key variables on solubility, optimizing model inputs, and ensuring data integrity. The study employed the Extra Trees (ET) regression model complemented by XAI approaches, including Partial Dependence Plots (PDP), Individual Conditional Expectation (ICE) plots, and Friedman H-statistics for assessing feature interactions. Feature importance (FI) was quantified using Permutation Feature Importance (PFI), Tree-based Feature Importance (TFI), and Partial Dependence Feature Importance (PDFI), which facilitated informed feature selection and model refinement. Analysis revealed that pressure (P), dimensionless P (PD), and dimensionless temperature (TD) significantly influence H2 solubility, demonstrating a near-linear relationship. The application of XAI not only optimized model inputs but also played a critical role in identifying and correcting data anomalies, enhancing overall data quality. The refined model, ET2_4, demonstrated improved accuracy, achieving a Root Mean Squared Error (RMSE) of 0.0085 on testing data, with H-statistics confirming strong interactions, particularly between P, PD, and TD. Notable deviations were observed for C1, suggesting specialized modelling considerations for atypical n-alkanes. The integration of XAI techniques provided profound insights into variable interactions and solubility dynamics, significantly advancing the accuracy of predictive models for H2 solubility (x) in n-alkanes. The findings emphasize the necessity of incorporating advanced analytical methods in chemical process simulations to ensure data reliability and model efficacy. Future research should explore alternative characterization methods to extend these insights across diverse chemical systems, especially for compounds exhibiting deviated behaviours.
{"title":"Explainable Artificial Intelligence in modelling hydrogen gas solubility in n-Alkanes","authors":"Afshin Tatar, Abbas Zeinijahromi, Manouchehr Haghighi","doi":"10.1016/j.seppur.2025.131741","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131741","url":null,"abstract":"This research aims to enhance the predictive modelling of hydrogen gas (H<sub>2</sub>) solubility in n-alkanes using Explainable Artificial Intelligence (XAI) techniques. The focus is on elucidating the impact of key variables on solubility, optimizing model inputs, and ensuring data integrity. The study employed the Extra Trees (ET) regression model complemented by XAI approaches, including Partial Dependence Plots (PDP), Individual Conditional Expectation (ICE) plots, and Friedman H-statistics for assessing feature interactions. Feature importance (FI) was quantified using Permutation Feature Importance (PFI), Tree-based Feature Importance (TFI), and Partial Dependence Feature Importance (PDFI), which facilitated informed feature selection and model refinement. Analysis revealed that pressure (<em>P</em>), dimensionless <em>P</em> (<em>PD</em>), and dimensionless temperature (<em>TD</em>) significantly influence H<sub>2</sub> solubility, demonstrating a near-linear relationship. The application of XAI not only optimized model inputs but also played a critical role in identifying and correcting data anomalies, enhancing overall data quality. The refined model, ET2_4, demonstrated improved accuracy, achieving a Root Mean Squared Error (<em>RMSE</em>) of 0.0085 on testing data, with H-statistics confirming strong interactions, particularly between <em>P</em>, <em>PD</em>, and <em>TD</em>. Notable deviations were observed for C1, suggesting specialized modelling considerations for atypical n-alkanes. The integration of XAI techniques provided profound insights into variable interactions and solubility dynamics, significantly advancing the accuracy of predictive models for H<sub>2</sub> solubility (<em>x</em>) in n-alkanes. The findings emphasize the necessity of incorporating advanced analytical methods in chemical process simulations to ensure data reliability and model efficacy. Future research should explore alternative characterization methods to extend these insights across diverse chemical systems, especially for compounds exhibiting deviated behaviours.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"74 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991890","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131683
Junhui Yue, Wei Guo, Shengxu Liang, Martin R. Tillotson, Yuhan Zhu, Dongyue Li, Linzhu Du, Jun Li, Xu Zhao
UV/persulfate (UV/PS) is considered an effective process for the degradation of emerging micropollutants in aquatic media. However, under the influence of complex water matrices such as wastewaters, radicals created during UV/PS will be reduced and transformed, so the chemical process of effectively obtaining the radicals in the system is very important to improving degradation efficiency. Thus, in the study, neotame (NEO, an artificial sweetener), as an emerging contaminant, was selected as the target compound to investigate in terms of its degradation and the role of free radicals in a range of water matrices during the UV/PS process. Based on the low concentration probe method (probe concentration ≤ 0.2 μm, more than 3-fold improvement in radical detection accuracy), kinetic modeling was developed to determine the role of primary (•OH and SO4•−) and secondary (e.g. Cl•, Cl2−•, CO3•−, and NO2•) radicals. Results indicated that UV/PS was effective in decomposing NEO (>93.7 %) within 7 min and was mainly attributed to •OH and SO4•−. Acidic environments promote NEO degradation with a greater contribution from SO4•−. Natural organic matter inhibited NEO degradation by quenching radicals (especially •OH). The kobs of NEO degradation in the presence of Cl− remained almost unchanged due to the production of Cl• and Cl2−• compensating the depletion of SO4•−. The presence of HCO3− quenched a part of primary radicals, which led to a decrease in kobs of NEO degradation, but CO3•− began to play a partial degradation role. In the presence of NO3−, UV-activated production of •OH and NO2• promoted NEO degradation. Based on 39 transformation products obtained, 3 degradation pathways and 7 radical attack ways were proposed for NEO degradation by primary and secondary radicals in the UV/PS system. This study provides meaningful insight into the role of primary and secondary radicals in NEO degradation using UV/PS systems.
{"title":"Kinetics, contributions, and pathways of the degradation of artificial sweeteners by primary and secondary radicals during UV/persulfate","authors":"Junhui Yue, Wei Guo, Shengxu Liang, Martin R. Tillotson, Yuhan Zhu, Dongyue Li, Linzhu Du, Jun Li, Xu Zhao","doi":"10.1016/j.seppur.2025.131683","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131683","url":null,"abstract":"UV/persulfate (UV/PS) is considered an effective process for the degradation of emerging micropollutants in aquatic media. However, under the influence of complex water matrices such as wastewaters, radicals created during UV/PS will be reduced and transformed, so the chemical process of effectively obtaining the radicals in the system is very important to improving degradation efficiency. Thus, in the study, neotame (NEO, an artificial sweetener), as an emerging contaminant, was selected as the target compound to investigate in terms of its degradation and the role of free radicals in a range of water matrices during the UV/PS process. Based on the low concentration probe method (probe concentration ≤ 0.2 μm, more than 3-fold improvement in radical detection accuracy), kinetic modeling was developed to determine the role of primary (•OH and SO<sub>4</sub>•<sup>−</sup>) and secondary (<em>e.g.</em> Cl•, Cl<sub>2</sub><sup>−</sup>•, CO<sub>3</sub>•<sup>−</sup>, and NO<sub>2</sub>•) radicals. Results indicated that UV/PS was effective in decomposing NEO (>93.7 %) within 7 min and was mainly attributed to •OH and SO<sub>4</sub>•<sup>−</sup>. Acidic environments promote NEO degradation with a greater contribution from SO<sub>4</sub>•<sup>−</sup>. Natural organic matter inhibited NEO degradation by quenching radicals (especially •OH). The <em>k</em><sub>obs</sub> of NEO degradation in the presence of Cl<sup>−</sup> remained almost unchanged due to the production of Cl• and Cl<sub>2</sub><sup>−</sup>• compensating the depletion of SO<sub>4</sub>•<sup>−</sup>. The presence of HCO<sub>3</sub><sup>−</sup> quenched a part of primary radicals, which led to a decrease in <em>k</em><sub>obs</sub> of NEO degradation, but CO<sub>3</sub>•<sup>−</sup> began to play a partial degradation role. In the presence of NO<sub>3</sub><sup>−</sup>, UV-activated production of •OH and NO<sub>2</sub>• promoted NEO degradation. Based on 39 transformation products obtained, 3 degradation pathways and 7 radical attack ways were proposed for NEO degradation by primary and secondary radicals in the UV/PS system. This study provides meaningful insight into the role of primary and secondary radicals in NEO degradation using UV/PS systems.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"74 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991900","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131746
Jingxuan Yang, Yingjie Li, Huaying Liu, Xiaoning Tang, Huan Li
Developing efficient catalytic antimicrobial materials is crucial for mitigating air microbial pollution. In this study, a monolayer Bi2MoO6 with a unique [BiO]+–[MoO4]2−–[BiO]+ interlayer substructure and “Bi–O” vacancy defects was synthesized through a simple exfoliation method using cetyltrimethylammonium bromide. These monolayers are chemically bonded to form a layered heterojunction. Under solar irradiation, holes are generated in the [BiO]+ layer, while electrons are produced in the [MoO4]2− layer, thereby facilitating efficient direct electron–hole separation. Additionally, the abundant “Bi–O” vacancy defects in the [BiO]+ layer result in crystal structure distortion, electron redistribution, and changes in the band gap energy of Bi2MoO6. The combination of layered heterostructures and vacancy defects significantly enhances solar light utilization and promotes photogenerated carrier separation, leading to excellent photocatalytic antimicrobial performance. Antibacterial tests reveal that after 20 min of irradiation, the monolayer Bi2MoO6 (0.20 mg/mL) deactivates 96.7 % of Escherichia coli and 74.5 % of Staphylococcus aureus. Notably, the antibacterial efficiency of the monolayer Bi2MoO6 is 1.9 and 2.7 times that of its multilayer counterpart for Escherichia coli and Staphylococcus aureus, respectively. This study provides novel insights and strategies for designing layered heterojunction Bi2MoO6 with enhanced photocatalytic antibacterial efficiency and tailored surface defects.
{"title":"Synergistic effects of monolayer Bi2MoO6 layered heterojunctions configuration and surface “Bi–O” vacancy defects of in enhanced photocatalytic antimicrobial performance","authors":"Jingxuan Yang, Yingjie Li, Huaying Liu, Xiaoning Tang, Huan Li","doi":"10.1016/j.seppur.2025.131746","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131746","url":null,"abstract":"Developing efficient catalytic antimicrobial materials is crucial for mitigating air microbial pollution. In this study, a monolayer Bi<sub>2</sub>MoO<sub>6</sub> with a unique [BiO]<sup>+</sup>–[MoO<sub>4</sub>]<sup>2−</sup>–[BiO]<sup>+</sup> interlayer substructure and “Bi–O” vacancy defects was synthesized through a simple exfoliation method using cetyltrimethylammonium bromide. These monolayers are chemically bonded to form a layered heterojunction. Under solar irradiation, holes are generated in the [BiO]<sup>+</sup> layer, while electrons are produced in the [MoO<sub>4</sub>]<sup>2−</sup> layer, thereby facilitating efficient direct electron–hole separation. Additionally, the abundant “Bi–O” vacancy defects in the [BiO]<sup>+</sup> layer result in crystal structure distortion, electron redistribution, and changes in the band gap energy of Bi<sub>2</sub>MoO<sub>6</sub>. The combination of layered heterostructures and vacancy defects significantly enhances solar light utilization and promotes photogenerated carrier separation, leading to excellent photocatalytic antimicrobial performance. Antibacterial tests reveal that after 20 min of irradiation, the monolayer Bi<sub>2</sub>MoO<sub>6</sub> (0.20 mg/mL) deactivates 96.7 % of <em>Escherichia coli</em> and 74.5 % of <em>Staphylococcus aureus</em>. Notably, the antibacterial efficiency of the monolayer Bi<sub>2</sub>MoO<sub>6</sub> is 1.9 and 2.7 times that of its multilayer counterpart for <em>Escherichia coli</em> and <em>Staphylococcus aureus</em>, respectively. This study provides novel insights and strategies for designing layered heterojunction Bi<sub>2</sub>MoO<sub>6</sub> with enhanced photocatalytic antibacterial efficiency and tailored surface defects.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"70 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991894","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}
High-flux loose nanofiltration membranes (LNMs) are ideal for treating and recovering dyes and salts from saline textile wastewater. In this study, a self-synthesized polyphenolic monomer (HCTT) was introduced into an interfacial polymerization (IP) system, establishing a dual physical and chemical constraint mechanism to regulate the reaction rate. Physically, HCTT exhibits a slow diffusion rate and reduces the diffusion rate of piperazine (PIP). Chemically, the phenolic hydroxyl groups of HCTT are less reactive than the amino groups of PIP, enhancing the controllability of the IP process. Using HCTT and anhydrous PIP as the aqueous phase and trimesoylchloride (TMC) as the oil phase, LNMs were prepared on hydrolyzed polyacrylonitrile (HPAN) substrates. The resulting membranes feature a negatively charged hydrophilic surface and a selective layer with a Turing structure, improving water permeability and mass transfer. The membranes achieved a flux of 124.8 LMH bar−1 with dye rejection rates exceeding 95 % for Congo Red (CR) and Methyl Violet (MV) while maintaining low salt rejection rates (14.1 % for Na2SO4 and 5.4 % for MgSO4), resulting in a dye/salt selectivity 14.9 times higher than conventional polyamide membranes. The membranes demonstrated excellent performance in mixed dye/salt solutions and maintained high stability after 48 h of continuous operation, achieving a flux recovery rate of 84.2 % after seven fouling cycles with CR. This study offers a novel and efficient strategy for developing LNMs for dye containing wastewater treatment and resource recovery.
{"title":"Preparation of high-flux loose nanofiltration membranes for efficient dye/salt separation by controlling interface polymerization through physical and chemical dual constraints","authors":"Haoshuo Li, Shujuan Xiao, Xiang Zhao, Jianguo Yuan, Shouwu Yu","doi":"10.1016/j.seppur.2025.131720","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131720","url":null,"abstract":"High-flux loose nanofiltration membranes (LNMs) are ideal for treating and recovering dyes and salts from saline textile wastewater. In this study, a self-synthesized polyphenolic monomer (HCTT) was introduced into an interfacial polymerization (IP) system, establishing a dual physical and chemical constraint mechanism to regulate the reaction rate. Physically, HCTT exhibits a slow diffusion rate and reduces the diffusion rate of piperazine (PIP). Chemically, the phenolic hydroxyl groups of HCTT are less reactive than the amino groups of PIP, enhancing the controllability of the IP process. Using HCTT and anhydrous PIP as the aqueous phase and trimesoylchloride (TMC) as the oil phase, LNMs were prepared on hydrolyzed polyacrylonitrile (HPAN) substrates. The resulting membranes feature a negatively charged hydrophilic surface and a selective layer with a Turing structure, improving water permeability and mass transfer. The membranes achieved a flux of 124.8 LMH bar<sup>−1</sup> with dye rejection rates exceeding 95 % for Congo Red (CR) and Methyl Violet (MV) while maintaining low salt rejection rates (14.1 % for Na<sub>2</sub>SO<sub>4</sub> and 5.4 % for MgSO<sub>4</sub>), resulting in a dye/salt selectivity 14.9 times higher than conventional polyamide membranes. The membranes demonstrated excellent performance in mixed dye/salt solutions and maintained high stability after 48 h of continuous operation, achieving a flux recovery rate of 84.2 % after seven fouling cycles with CR. This study offers a novel and efficient strategy for developing LNMs for dye containing wastewater treatment and resource recovery.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"11 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992213","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 : 2025-01-22DOI: 10.1016/j.seppur.2025.131685
Yilong Zhu, Huifang Xing, Shan Ni, Ke Xu, ZhaoXiang Zhong, Liangrong Yang
The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g–1. In addition, it showed high affinity for Pd ions, the Kd value was 4.1 × 104 ml·g–1. After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h–1, significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.
{"title":"Recovery of palladium from solution by defective Carbon nitride and Regenerating as a hydrogenation catalysis","authors":"Yilong Zhu, Huifang Xing, Shan Ni, Ke Xu, ZhaoXiang Zhong, Liangrong Yang","doi":"10.1016/j.seppur.2025.131685","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131685","url":null,"abstract":"The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g<sup>–1</sup>. In addition, it showed high affinity for Pd ions, the <em>K<sub>d</sub></em> value was 4.1 × 10<sup>4</sup> ml·g<sup>–1</sup>. After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h<sup>–1</sup>, significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"9 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991891","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}
C
O groups of MAB (such as carboxyl) acted as reaction sites, facilitating this electron transfer mechanism. Moreover, the MAB + PDS system displayed exceptional selectivity for degrading electron-rich organic compounds, and the quantitative structure–activity relationships (QSAR) analysis revealed a strong linear correlation between removal performance and ionization potentials of these organics, further supporting the predominant contribution of the electron transfer pathway involved. Overall, this work not only presents a successful strategy for applying carbon materials in wastewater treatment but also contributes to understanding the mechanisms underlying persulfate activation using highly graphitized carbon materials.
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