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Hierarchical porous carbon electrodes derived from bimetallic MOF on cellulose fibers for Electrical-Assisted adsorption of phosphate
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132205
Chenhui Wang , Bo Hu , Kairong Huang , Daxiong He , Shengcai Li , Zhenggang Wang , Xichao Liang
Pollution caused by the excessive use of phosphate has attracted widespread attention. In this study, Zr-La MOF-derived carbon (ZLMCs) electrode was prepared to remove phosphorus from water via the electroassisted adsorption (EAA) method. The crystal structure of ZLMOF induces defects that provide active sites for phosphate uptake. In comparison to alternative adsorption materials, ZLMC-16 achieves 143.0 mg g–1 (80 % full capacity) in one hour and 178.8 mg g–1 in three hours. In addition, the spontaneous adsorption of phosphorus was observed to be heat-absorbing, in line with the proposed pseudo-second-order kinetics and Langmuir isotherm model. FTIR and XPS analyses indicated that chemical bonding and electrostatic gravitational forces between La/Zr-O-P play a key role in the phosphate trapping mechanism. Under electric field, PO43- was rapidly transferred from the aqueous solution to the electrode surface and can reach deeper adsorption sites. Furthermore, ZLMC-16 demonstrated high selectivity for PO43- in the presence of common interfering ions (SO42-, Cl-, and NO3) and an efficient adsorption capacity between pH 3–7. In conclusion, our work shows that ZLMC electrodes with fiber additions have good potential for efficient phosphate removal and recovery, which will promote the application of electroassisted adsorption in wastewater treatment.
{"title":"Hierarchical porous carbon electrodes derived from bimetallic MOF on cellulose fibers for Electrical-Assisted adsorption of phosphate","authors":"Chenhui Wang ,&nbsp;Bo Hu ,&nbsp;Kairong Huang ,&nbsp;Daxiong He ,&nbsp;Shengcai Li ,&nbsp;Zhenggang Wang ,&nbsp;Xichao Liang","doi":"10.1016/j.seppur.2025.132205","DOIUrl":"10.1016/j.seppur.2025.132205","url":null,"abstract":"<div><div>Pollution caused by the excessive use of phosphate has attracted widespread attention. In this study, Zr-La MOF-derived carbon (ZLMCs) electrode was prepared to remove phosphorus from water via the electroassisted adsorption (EAA) method. The crystal structure of ZLMOF induces defects that provide active sites for phosphate uptake. In comparison to alternative adsorption materials, ZLMC-16 achieves 143.0 mg g<sup>–1</sup> (80 % full capacity) in one hour and 178.8 mg g<sup>–1</sup> in three hours. In addition, the spontaneous adsorption of phosphorus was observed to be heat-absorbing, in line with the proposed pseudo-second-order kinetics and Langmuir isotherm model. FTIR and XPS analyses indicated that chemical bonding and electrostatic gravitational forces between La/Zr-O-P play a key role in the phosphate trapping mechanism. Under electric field, PO<sub>4</sub><sup>3-</sup> was rapidly transferred from the aqueous solution to the electrode surface and can reach deeper adsorption sites. Furthermore, ZLMC-16 demonstrated high selectivity for PO<sub>4</sub><sup>3-</sup> in the presence of common interfering ions (SO<sub>4</sub><sup>2-</sup>, Cl<sup>-</sup>, and NO<sub>3</sub><sup>–</sup>) and an efficient adsorption capacity between pH 3–7. In conclusion, our work shows that ZLMC electrodes with fiber additions have good potential for efficient phosphate removal and recovery, which will promote the application of electroassisted adsorption in wastewater treatment.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132205"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463203","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
Estimating molecular weight cut off of porous membranes via “Positioning-Searching-Determining” triple-step method
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132197
Qun Wang, Fuling Huang, Qiang Wei, Demin Geng, Xiao Cheng, Yangguang Ren, Maowen Yue, Jian Wang, Jianlu Liu, Dongmei Xu, Jun Gao, Xi Wu
Although the molecular weight cut-off (MWCO) method is commonly used to assess the pore size of porous membranes, it requires a large quantity of standard substances. As such, a hybrid approach characterized by a “Positioning-Searching-Determining” three-step method was proposed to acquire a precise MWCO value for porous membranes more efficiently and cost-effectively. Firstly, the ratio of the convective flow permeability coefficient (Ld) to pure water permeability (A) was introduced to evaluate the surface defect of porous membranes. The mathematical modeling process depicting the approximate correlation among Ld/A, solute rejection (Rt), and MWCO showed that LnRt could be expressed by Ld/A, and Rt could also be expressed by lnMWCO in the form of polynomial functions. Subsequently, by measuring the values of Ld/A, Rt, and MWCO for commercial ultrafiltration (CUF) membranes with different pore sizes, the governing equations along with the corresponding fitting parameters were obtained. Then, the obtained governing equations were used to assess the MWCO of homemade porous composite membranes (PCMs). Comparative analysis revealed that the currently established mathematical equations among Rt, Ld/A, and MWCO caused a more significant divergence between the predicted and measured values for PCMs when Ld/A or Rt was outside the range of the selected CUF membranes, indicating that simply using the governing equations was more likely to provide not an exact but an approximate MWCO value. In view of this situation, the “Positioning-Searching-Determining” hybrid strategy was constructed by using the approximate equations to obtain the approximate MWCO value and then obtaining the precise MWCO value through solute rejection experiments for the selected two standard substances. Experimental results showed that utilization of the hybrid stratagem to acquire MWCO could constrict the error ambit to a narrower range (−5% to +14 %) and minimize the quantum of chemical reagents. Therefore, the proffered hybrid modus operandi coalesces the excellences of the sheer predictive mode and the sheer measurement mode, thereby enhancing the dependability and reducing the measurement outlay. Moreover, the proposed novel hybrid tactic has the ability to transmute the MWCO determining tactic from blind and simplistic seeking to sagacious positioning and purposeful seeking.
{"title":"Estimating molecular weight cut off of porous membranes via “Positioning-Searching-Determining” triple-step method","authors":"Qun Wang, Fuling Huang, Qiang Wei, Demin Geng, Xiao Cheng, Yangguang Ren, Maowen Yue, Jian Wang, Jianlu Liu, Dongmei Xu, Jun Gao, Xi Wu","doi":"10.1016/j.seppur.2025.132197","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132197","url":null,"abstract":"Although the molecular weight cut-off (MWCO) method is commonly used to assess the pore size of porous membranes, it requires a large quantity of standard substances. As such, a hybrid approach characterized by a “Positioning-Searching-Determining” three-step method was proposed to acquire a precise MWCO value for porous membranes more efficiently and cost-effectively. Firstly, the ratio of the convective flow permeability coefficient (L<sub>d</sub>) to pure water permeability (A) was introduced to evaluate the surface defect of porous membranes. The mathematical modeling process depicting the approximate correlation among L<sub>d</sub>/A, solute rejection (R<sub>t</sub>), and MWCO showed that LnR<sub>t</sub> could be expressed by L<sub>d</sub>/A, and R<sub>t</sub> could also be expressed by lnMWCO in the form of polynomial functions. Subsequently, by measuring the values of L<sub>d</sub>/A, R<sub>t</sub>, and MWCO for commercial ultrafiltration (CUF) membranes with different pore sizes, the governing equations along with the corresponding fitting parameters were obtained. Then, the obtained governing equations were used to assess the MWCO of homemade porous composite membranes (PCMs). Comparative analysis revealed that the currently established mathematical equations among R<sub>t</sub>, L<sub>d</sub>/A, and MWCO caused a more significant divergence between the predicted and measured values for PCMs when L<sub>d</sub>/A or R<sub>t</sub> was outside the range of the selected CUF membranes, indicating that simply using the governing equations was more likely to provide not an exact but an approximate MWCO value. In view of this situation, the “Positioning-Searching-Determining” hybrid strategy was constructed by using the approximate equations to obtain the approximate MWCO value and then obtaining the precise MWCO value through solute rejection experiments for the selected two standard substances. Experimental results showed that utilization of the hybrid stratagem to acquire MWCO could constrict the error ambit to a narrower range (−5% to +14 %) and minimize the quantum of chemical reagents. Therefore, the proffered hybrid modus operandi coalesces the excellences of the sheer predictive mode and the sheer measurement mode, thereby enhancing the dependability and reducing the measurement outlay. Moreover, the proposed novel hybrid tactic has the ability to transmute the MWCO determining tactic from blind and simplistic seeking to sagacious positioning and purposeful seeking.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"27 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471053","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
Novel diamide covalent organic polymers (COPs) for arresting actinides U(VI), Pu(IV) and Am(III) from highly acidic nuclear stream 新型二酰胺共价有机聚合物 (COP),用于从高酸性核气流中捕获锕系元素 U(VI)、Pu(IV) 和 Am(III)
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132181
Prashant Yevale , Shiny S. Kumar , Pooja Agarkar , Gauravi Yashwantrao , Anjali Tripathi , Purav Badani , Ankita Rao , Satyajit Saha
Targeted towards the hitherto unaddressed challenge of actinide capture under harsh radiochemical conditions (nitric acid molarity ≥2 M, gamma radiation field 500 kGy), novel diamide covalent organic polymers (COPs) were successfully synthesized and characterized. The completely incinerable 1,3 and 1,4-Diamide COPs were endowed with exceptional radiochemical stability, high surface area (>1400 m2 g−1) and remarkable sorption capacity for the actinides viz. U(VI), Pu(IV) and Am(III). Batch sorption studies with Am(III), Pu(IV) and U(VI) from nitric acid medium revealed higher uptake with 1,3 over 1,4-Diamide COP, in general. Distribution co-efficient, kD was found to enhance with nitric acid molarity, attaining saturation after 4 M. Sorption was found to follow pseudo second order kinetics, Langmuir adsorption isotherm and was enthalpy driven. 1,3-Diamide COPs yielded high sorption capacity for U(VI), Pu(IV) and Am(III) (368.8, 452.3 and 189.3 mg g−1 respectively), from 4 M nitric acid medium. Actinide removal was >90 % from simulated nuclear streams. Mode of complexation of COPs with uranyl was probed experimentally by X-ray Photoelectron Spectroscopy and Fourier transform Infrared Spectroscopy. Additional insights for optimized ligand and metal–ligand binding geometries were obtained by theoretical modelling.
{"title":"Novel diamide covalent organic polymers (COPs) for arresting actinides U(VI), Pu(IV) and Am(III) from highly acidic nuclear stream","authors":"Prashant Yevale ,&nbsp;Shiny S. Kumar ,&nbsp;Pooja Agarkar ,&nbsp;Gauravi Yashwantrao ,&nbsp;Anjali Tripathi ,&nbsp;Purav Badani ,&nbsp;Ankita Rao ,&nbsp;Satyajit Saha","doi":"10.1016/j.seppur.2025.132181","DOIUrl":"10.1016/j.seppur.2025.132181","url":null,"abstract":"<div><div>Targeted towards the hitherto unaddressed challenge of actinide capture under harsh radiochemical conditions (nitric acid molarity ≥2 M, gamma radiation field 500 kGy), novel diamide covalent organic polymers (COPs) were successfully synthesized and characterized. The completely incinerable <strong>1,3</strong> and <strong>1,4-Diamide COP</strong>s were endowed with exceptional radiochemical stability, high surface area (&gt;1400 m<sup>2</sup> g<sup>−1</sup>) and remarkable sorption capacity for the actinides viz. U(VI), Pu(IV) and Am(III). Batch sorption studies with Am(III), Pu(IV) and U(VI) from nitric acid medium revealed higher uptake with <strong>1,3</strong> over <strong>1,4-Diamide COP</strong>, in general. Distribution co-efficient, k<sub>D</sub> was found to enhance with nitric acid molarity, attaining saturation after 4 M. Sorption was found to follow pseudo second order kinetics, Langmuir adsorption isotherm and was enthalpy driven. <strong>1,3-Diamide COP</strong>s yielded high sorption capacity for U(VI), Pu(IV) and Am(III) (368.8, 452.3 and 189.3 mg g<sup>−1</sup> respectively), from 4 M nitric acid medium. Actinide removal was &gt;90 % from simulated nuclear streams. Mode of complexation of COPs with uranyl was probed experimentally by X-ray Photoelectron Spectroscopy and Fourier transform Infrared Spectroscopy. Additional insights for optimized ligand and metal–ligand binding geometries were obtained by theoretical modelling.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132181"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471083","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
Facet engineering of polycrystalline copper catalytic electrode through additive-assisted electrodeposition for nitrate reduction to ammonium
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132206
Jenn Fang Su, Yuan Chun Ye
The electrocatalytic reduction of nitrate to ammonia has become an upsurge in recent years. This approach uses nitrate from wastewater as the nitrogen source for ammonia production, providing a sustainable alternative to address the challenges associated with the traditional Haber-Bosch process. However, the scheme to synthesize a promising catalyst for electrochemically selective conversion of nitrate toward ammonia is not yet fully developed. Here we present a facile strategy to prepare a high-performance copper (Cu) electrode with well-controlled crystalline structures by modifying additive concentrations in the electrodeposition bath. At the applied potential of −0.9 V (vs. SCE), the designer Cu electrode exhibits an ammonium Faradaic efficiency of 44 % with a nitrate conversion of 96 % and ammonium selectivity of 66 %. Further analysis suggest that the enhanced reduction performance is attributed to the selective exposure of both Cu(111) and Cu(110) facets on the Cu electrode, which facilitate the critical nitrate to nitrite conversion and suppress the competing hydrogen evolution reaction.
{"title":"Facet engineering of polycrystalline copper catalytic electrode through additive-assisted electrodeposition for nitrate reduction to ammonium","authors":"Jenn Fang Su, Yuan Chun Ye","doi":"10.1016/j.seppur.2025.132206","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132206","url":null,"abstract":"The electrocatalytic reduction of nitrate to ammonia has become an upsurge in recent years. This approach uses nitrate from wastewater as the nitrogen source for ammonia production, providing a sustainable alternative to address the challenges associated with the traditional Haber-Bosch process. However, the scheme to synthesize a promising catalyst for electrochemically selective conversion of nitrate toward ammonia is not yet fully developed. Here we present a facile strategy to prepare a high-performance copper (Cu) electrode with well-controlled crystalline structures by modifying additive concentrations in the electrodeposition bath. At the applied potential of −0.9 V (vs. SCE), the designer Cu electrode exhibits an ammonium Faradaic efficiency of 44 % with a nitrate conversion of 96 % and ammonium selectivity of 66 %. Further analysis suggest that the enhanced reduction performance is attributed to the selective exposure of both Cu(111) and Cu(110) facets on the Cu electrode, which facilitate the critical nitrate to nitrite conversion and suppress the competing hydrogen evolution reaction.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"2 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463205","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
Good modeling practice for calibration applied to ion exchange breakthrough prediction
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132192
Daniel Illana González, Mariane Yvonne Schneider, Juan Pablo Gallo, Ingmar Nopens, Elena Torfs
Ion exchange (IX) is a key technology in resource recovery processes for demineralization and fit-for-purpose water production due to its inherent ion-selective recovery properties. A major bottleneck in the optimization of the IX process is the accurate prediction of ion breakthrough times, which has the potential to save on regeneration chemicals by maximizing resin utilization. However, the models used to predict ion breakthrough times are often unreliable due to poor calibration methods and significant uncertainty in parameter estimates. Consequently, we conducted local and global sensitivity analyses to identify the design and operational parameters that contribute most to the prediction of breakthrough curves. The global sensitivity analysis enabled the selection of a limited subset of parameters for calibration, demonstrating that only two parameters, namely the maximum adsorption capacity isotherm parameter and the resin bead particle size, require thorough calibration, resulting in a 76 % improvement in the breakthrough prediction. We also showed that the calibration of additional, less sensitive or correlated parameters results in an insignificant improvement of the predictive power, with a 16 % to 60 % increased uncertainty in the breakthrough time prediction. The model was validated using three independent data sets, which showed a fairly accurate breakthrough time prediction, with a relative error ranging from 1 % to 11 %. Herein, we propose a robust calibration procedure, based on good modeling practice, that encompasses both sensitivity and uncertainty analyses and therefore provides a basis for process optimization. The framework is presented in a manner that allows for its application to analogous process settings.
{"title":"Good modeling practice for calibration applied to ion exchange breakthrough prediction","authors":"Daniel Illana González, Mariane Yvonne Schneider, Juan Pablo Gallo, Ingmar Nopens, Elena Torfs","doi":"10.1016/j.seppur.2025.132192","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132192","url":null,"abstract":"Ion exchange (IX) is a key technology in resource recovery processes for demineralization and fit-for-purpose water production due to its inherent ion-selective recovery properties. A major bottleneck in the optimization of the IX process is the accurate prediction of ion breakthrough times, which has the potential to save on regeneration chemicals by maximizing resin utilization. However, the models used to predict ion breakthrough times are often unreliable due to poor calibration methods and significant uncertainty in parameter estimates. Consequently, we conducted local and global sensitivity analyses to identify the design and operational parameters that contribute most to the prediction of breakthrough curves. The global sensitivity analysis enabled the selection of a limited subset of parameters for calibration, demonstrating that only two parameters, namely the maximum adsorption capacity isotherm parameter and the resin bead particle size, require thorough calibration, resulting in a 76 % improvement in the breakthrough prediction. We also showed that the calibration of additional, less sensitive or correlated parameters results in an insignificant improvement of the predictive power, with a 16 % to 60 % increased uncertainty in the breakthrough time prediction. The model was validated using three independent data sets, which showed a fairly accurate breakthrough time prediction, with a relative error ranging from 1 % to 11 %. Herein, we propose a robust calibration procedure, based on good modeling practice, that encompasses both sensitivity and uncertainty analyses and therefore provides a basis for process optimization. The framework is presented in a manner that allows for its application to analogous process settings.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"31 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471051","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
HKUST-1 bridged calcium alginate gel nanofiltration membrane for separating drugs from organic solvents 用于从有机溶剂中分离药物的 HKUST-1 桥接海藻酸钙凝胶纳滤膜
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132198
Haike Li , Zhiyun Kong , Huan Zhang , Xiaolei Wang , Xin Wei , Ruichao Yang , Xueyi Zhang
Organic solvent nanofiltration (OSN) membranes are suitable for separating drugs from solvents, especially heat-sensitive drugs. However, the trade-off effect between permeance and rejection limits the effective utilization of OSN membranes. In this study, a gel OSN membrane with high permeability-selectivity was prepared by bridging sodium alginate (SA) with HKUST-1 and then cross-linking with Ca2+ ions. The interspersed distribution of HKUST-1 among the flexible polymer chains results in three-dimensional pores of the gel membrane, which enriches the solvent transport channels. Meanwhile, SA is cross-linked by Cu2+ from HKUST-1 and Ca2+, which densifies the pore structure and enhances the solute rejection of the gel membrane. When the concentrations of HKUST-1, SA, and Ca2+ are 2.5 wt%, the gel membrane (HKUST-12.5%-CaSA) has strong hydrophilicity (11.1°), a small pore size (0.59 nm), and a relatively high porosity (56.89 %). The ethanol permeance of the HKUST-12.5%-CaSA gel membrane reaches 43.8 L·m−2·h−1·bar−1, with a tracycline (TC) rejection as high as 97 %. Moreover, the HKUST-12.5%-CaSA gel membrane is capable of achieving high rejection of TC in other organic solvents (acetone, ethyl acetate, and isopropanol). Even after being immersed in non-polar (n-hexane) and polar solvents (N,N-dimethylformamide, isopropanol, ethanol) for a period of 20 days, the separation performance of the gel OSN membrane remains consistent, confirming the excellent solvent resistance and potential in drug separation and solvent recovery.
{"title":"HKUST-1 bridged calcium alginate gel nanofiltration membrane for separating drugs from organic solvents","authors":"Haike Li ,&nbsp;Zhiyun Kong ,&nbsp;Huan Zhang ,&nbsp;Xiaolei Wang ,&nbsp;Xin Wei ,&nbsp;Ruichao Yang ,&nbsp;Xueyi Zhang","doi":"10.1016/j.seppur.2025.132198","DOIUrl":"10.1016/j.seppur.2025.132198","url":null,"abstract":"<div><div>Organic solvent nanofiltration (OSN) membranes are suitable for separating drugs from solvents, especially heat-sensitive drugs. However, the trade-off effect between permeance and rejection limits the effective utilization of OSN membranes. In this study, a gel OSN membrane with high permeability-selectivity was prepared by bridging sodium alginate (SA) with HKUST-1 and then cross-linking with Ca<sup>2+</sup> ions. The interspersed distribution of HKUST-1 among the flexible polymer chains results in three-dimensional pores of the gel membrane, which enriches the solvent transport channels. Meanwhile, SA is cross-linked by Cu<sup>2+</sup> from HKUST-1 and Ca<sup>2+</sup>, which densifies the pore structure and enhances the solute rejection of the gel membrane. When the concentrations of HKUST-1, SA, and Ca<sup>2+</sup> are 2.5 wt%, the gel membrane (HKUST-1<sub>2.5%</sub>-CaSA) has strong hydrophilicity (11.1°), a small pore size (0.59 nm), and a relatively high porosity (56.89 %). The ethanol permeance of the HKUST-1<sub>2.5%</sub>-CaSA gel membrane reaches 43.8 L·m<sup>−2</sup>·h<sup>−1</sup>·bar<sup>−1</sup>, with a tracycline (TC) rejection as high as 97 %. Moreover, the HKUST-1<sub>2.5%</sub>-CaSA gel membrane is capable of achieving high rejection of TC in other organic solvents (acetone, ethyl acetate, and isopropanol). Even after being immersed in non-polar (n-hexane) and polar solvents (N,N-dimethylformamide, isopropanol, ethanol) for a period of 20 days, the separation performance of the gel OSN membrane remains consistent, confirming the excellent solvent resistance and potential in drug separation and solvent recovery.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132198"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471090","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
Novel 2D/3D Z-scheme heterojunction with Bi12O15Cl6 nanoplates anchored on MIL-53 (Fe) derived Fe2O3@C micro-rods for enhanced visible-light-mediated photocatalytic degradation of fluoroquinolones in wastewater
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132176
Adarsh Singh , Amit Bhatnagar , Ashok Kumar Gupta
Antibiotics, ubiquitous in environmental matrices, evade conventional wastewater treatment systems, posing a threat to humans and aquatic biota. In this context, a novel 2D/3D Z-scheme Bi12O15Cl6/Fe2O3@C (BFC) heterojunction photocatalyst was prepared by anchoring Bi12O15Cl6 nanoplates on perforated Fe2O3@C micro-rods via solvothermal route followed by calcination. The carbon framework surrounding Fe2O3 led to the partial surface metallization of Bi12O15Cl6 nanoplates, which proved beneficial for photoinduced charge separation. The treatment efficacy of the as-prepared materials was assessed by degrading a mixture of fluoroquinolone-based antibiotics (levofloxacin (LEV) and ciprofloxacin (CIP)) under visible light. Under optimal conditions, the degradation efficiencies of the photocatalyst for LEV and CIP reached around 96% and 91%, respectively, after 120 min. This could be related to the decreased recombination rate of photoinduced charge carriers and their enhanced separation efficacy. In addition, OH radicals were determined to be the principal reactive species supporting photocatalytic degradation of LEV and CIP, followed by O2·- and h+. The BFC photocatalyst demonstrated exceptional chemical stability, non-toxicity, and sustained photocatalytic activity across multiple cycles of reuse. Furthermore, the colony forming unit (CFU) assay performed on E. coli, along with the in silico toxicity prediction of transformation products (TPs), showed that the treated effluent and TPs exhibited lower toxicity compared to the parent compounds, respectively.
{"title":"Novel 2D/3D Z-scheme heterojunction with Bi12O15Cl6 nanoplates anchored on MIL-53 (Fe) derived Fe2O3@C micro-rods for enhanced visible-light-mediated photocatalytic degradation of fluoroquinolones in wastewater","authors":"Adarsh Singh ,&nbsp;Amit Bhatnagar ,&nbsp;Ashok Kumar Gupta","doi":"10.1016/j.seppur.2025.132176","DOIUrl":"10.1016/j.seppur.2025.132176","url":null,"abstract":"<div><div>Antibiotics, ubiquitous in environmental matrices, evade conventional wastewater treatment systems, posing a threat to humans and aquatic biota. In this context, a novel 2D/3D Z-scheme Bi<sub>12</sub>O<sub>15</sub>Cl<sub>6</sub>/Fe<sub>2</sub>O<sub>3</sub>@C (BFC) heterojunction photocatalyst was prepared by anchoring Bi<sub>12</sub>O<sub>15</sub>Cl<sub>6</sub> nanoplates on perforated Fe<sub>2</sub>O<sub>3</sub>@C micro-rods via solvothermal route followed by calcination. The carbon framework surrounding Fe<sub>2</sub>O<sub>3</sub> led to the partial surface metallization of Bi<sub>12</sub>O<sub>15</sub>Cl<sub>6</sub> nanoplates, which proved beneficial for photoinduced charge separation. The treatment efficacy of the as-prepared materials was assessed by degrading a mixture of fluoroquinolone-based antibiotics (levofloxacin (LEV) and ciprofloxacin (CIP)) under visible light. Under optimal conditions, the degradation efficiencies of the photocatalyst for LEV and CIP reached around 96% and 91%, respectively, after 120 min. This could be related to the decreased recombination rate of photoinduced charge carriers and their enhanced separation efficacy. In addition, <sup>●</sup>OH radicals were determined to be the principal reactive species supporting photocatalytic degradation of LEV and CIP, followed by <span><math><msubsup><mi>O</mi><mrow><mn>2</mn></mrow><mrow><mo>·</mo><mo>-</mo></mrow></msubsup></math></span> and h<sup>+</sup>. The BFC photocatalyst demonstrated exceptional chemical stability, non-toxicity, and sustained photocatalytic activity across multiple cycles of reuse. Furthermore, the colony forming unit (CFU) assay performed on <em>E. coli</em>, along with the in silico toxicity prediction of transformation products (TPs), showed that the treated effluent and TPs exhibited lower toxicity compared to the parent compounds, respectively.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132176"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463209","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
Advancing energy-efficient CO2 capture with organic amine solutions using ionic liquid absorption promoters and zeolite molecular sieve desorption catalysts
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132094
Hang Liu, Yupeng Xing, Dongya Zhao, Shijian Lu, Yurong Chen, Shizhang Cui, Xinwang Song
Alkanolamine solutions have been widely used for CO2 capture due to their low cost and stable performance. However, their inherent structural limitations led to significant challenges, such as low CO2 absorption–desorption capacity and high energy demands for regeneration. To address these issues, this work proposes an efficient CO2 capture system that employs 2-(2-aminoethylamino)ethanol (AEEA) as the primary absorbent due to its stable performance, amino-functionalized ionic liquid (AIL) synthesized via a one-step method as absorption promoters, and an appropriate amount of solid acid catalyst (SAC) as desorption catalysts. The experimental results demonstrated that the composite system comprising 20 wt% AEEA (primary absorbent), 10 wt% [DETAH][Pz] (absorption promoter), and 0.1 wt% HZSM-5 (desorption catalyst) represents the optimal configuration. The system achieved a CO2 absorption capacity of 0.50172 g CO2/g amine for the fresh solution, which decreased to 0.42619 g CO2/g amine after five regeneration cycles, maintaining 84.95 % of the original capacity. The desorption ratio exceeded 85 %, while regeneration energy consumption was reduced by 30.22 % compared to the MEA/water system. Notably, the inclusion of the HZSM-5(21) catalyst significantly enhanced the CO2 desorption process during the initial 20 min. The desorption amount increased by 62.78 % relative to the non-catalytic system, the average desorption rate improved by 40.85 %, and the peak desorption rate rose by 31.94 %, resulting in a more efficient and complete CO2 desorption process. Analysis using 13C NMR demonstrated that the synergistic absorption effect between AEEA and [DETAH][Pz] significantly improved the CO2 absorption capacity of the system. Meanwhile, the Brønsted and Lewis acid sites on the HZSM-5(21) molecular sieve, along with [Pz]-H, effectively facilitated the decomposition of carbamates, thereby catalyzing the CO2 desorption process.
{"title":"Advancing energy-efficient CO2 capture with organic amine solutions using ionic liquid absorption promoters and zeolite molecular sieve desorption catalysts","authors":"Hang Liu, Yupeng Xing, Dongya Zhao, Shijian Lu, Yurong Chen, Shizhang Cui, Xinwang Song","doi":"10.1016/j.seppur.2025.132094","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132094","url":null,"abstract":"Alkanolamine solutions have been widely used for CO<sub>2</sub> capture due to their low cost and stable performance. However, their inherent structural limitations led to significant challenges, such as low CO<sub>2</sub> absorption–desorption capacity and high energy demands for regeneration. To address these issues, this work proposes an efficient CO<sub>2</sub> capture system that employs 2-(2-aminoethylamino)ethanol (AEEA) as the primary absorbent due to its stable performance, amino-functionalized ionic liquid (AIL) synthesized via a one-step method as absorption promoters, and an appropriate amount of solid acid catalyst (SAC) as desorption catalysts. The experimental results demonstrated that the composite system comprising 20 wt% AEEA (primary absorbent), 10 wt% [DETAH][Pz] (absorption promoter), and 0.1 wt% HZSM-5 (desorption catalyst) represents the optimal configuration. The system achieved a CO<sub>2</sub> absorption capacity of 0.50172 g CO<sub>2</sub>/g amine for the fresh solution, which decreased to 0.42619 g CO<sub>2</sub>/g amine after five regeneration cycles, maintaining 84.95 % of the original capacity. The desorption ratio exceeded 85 %, while regeneration energy consumption was reduced by 30.22 % compared to the MEA/water system. Notably, the inclusion of the HZSM-5(21) catalyst significantly enhanced the CO<sub>2</sub> desorption process during the initial 20 min. The desorption amount increased by 62.78 % relative to the non-catalytic system, the average desorption rate improved by 40.85 %, and the peak desorption rate rose by 31.94 %, resulting in a more efficient and complete CO<sub>2</sub> desorption process. Analysis using <sup>13</sup>C NMR demonstrated that the synergistic absorption effect between AEEA and [DETAH][Pz] significantly improved the CO<sub>2</sub> absorption capacity of the system. Meanwhile, the Brønsted and Lewis acid sites on the HZSM-5(21) molecular sieve, along with [Pz]-H, effectively facilitated the decomposition of carbamates, thereby catalyzing the CO<sub>2</sub> desorption process.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"15 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463208","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 comprehensive study on the influence of pH for dewatering performance and filter cake characteristics in solid–liquid separation of clean coal
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132208
Zeyu Feng, Ruxia Chen, Xianshu Dong, Yuping Fan, Xiaomin Ma
The pH of solution significantly influences the interplay between polymer flocculants and clean coal, thereby affecting dewatering performance. Herein, a comprehensive study on the influence of pH for dewatering performance of clean coal was investigated from the perspectives of particle interaction and filter cake structure. The results reveal that as the solution transitions from acidic to alkaline, the filtration rate diminishes and the cake moisture content elevates, regardless of flocculant presence. Atomic Force Microscope (AFM) measurements indicated a reduction in the adhesion force of particles as the pH increases. CT analysis demonstrated that the filter cake porosity at pH 4 is markedly greater than those at pH 7 and 10. Upon reaching a pH of 10, the cake porosity further decreases to 5.41%, while the ratio of isolated pores to total pores increases to 17.15%. In acidic environments, the development of pore space in filter cake is more uniform and well connected, which indicates a substantially lower capillary pressure compared to that at pH 7 and pH 10. The Lattice Boltzmann Method (LBM) simulation results indicate that the permeability of the cake formed at pH 10 is notably lower than that of pH7 and pH4.
{"title":"A comprehensive study on the influence of pH for dewatering performance and filter cake characteristics in solid–liquid separation of clean coal","authors":"Zeyu Feng, Ruxia Chen, Xianshu Dong, Yuping Fan, Xiaomin Ma","doi":"10.1016/j.seppur.2025.132208","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132208","url":null,"abstract":"The pH of solution significantly influences the interplay between polymer flocculants and clean coal, thereby affecting dewatering performance. Herein, a comprehensive study on the influence of pH for dewatering performance of clean coal was investigated from the perspectives of particle interaction and filter cake structure. The results reveal that as the solution transitions from acidic to alkaline, the filtration rate diminishes and the cake moisture content elevates, regardless of flocculant presence. Atomic Force Microscope (AFM) measurements indicated a reduction in the adhesion force of particles as the pH increases. CT analysis demonstrated that the filter cake porosity at pH 4 is markedly greater than those at pH 7 and 10. Upon reaching a pH of 10, the cake porosity further decreases to 5.41%, while the ratio of isolated pores to total pores increases to 17.15%. In acidic environments, the development of pore space in filter cake is more uniform and well connected, which indicates a substantially lower capillary pressure compared to that at pH 7 and pH 10. The Lattice Boltzmann Method (LBM) simulation results indicate that the permeability of the cake formed at pH 10 is notably lower than that of pH7 and pH4.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"30 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471049","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
NiFe2O4@MoS2 heterojunction induces the changes of PMS activation mode in PMS/Vis system for the directed generation of 1O2
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-20 DOI: 10.1016/j.seppur.2025.132175
Xiaoyi Qi , Siyu Xu , Ling Zhang , Qianqian Cao , Longquan Zhang , Xiaoguo Shi , Yawei Gu , Chen Wang
Peroxymonosulfate-based advanced oxidation is a promising approach for water treatment, but how to simply achieve the efficient PMS activation is still a great challenge. In this study, NiFe2O4@MoS2 heterojunction was synthesized via hydrothermal method to achieve rapid degradation of sulfadiazine (SDZ) in the synergistic PMS/Visible light photocatalysis system (PMS/Vis). Almost complete elimination of sulfadiazine (SDZ) can be accomplished in 8 min (kobs of 0.4038 min−1), and forming a synergistic SDZ degradation mechanism including a predominant non-radical pathway (1O2) and complementary radical pathway (⋅O2). The special heterojunction structure of NiFe2O4@MoS2 could induce the directional separation of photogenerated carriers under visible light. Unlike the conventional transition metal-activated PMS process, the photogenerated electron-hole pairs of NiFe2O4@MoS2 could serve as ceaseless PMS activator for ROS generation. The photocatalytic-assisted PMS system (PMS/Vis system) simultaneously solves the problems of variable metal cycling and ion solubilization in the traditional transition metal-activated PMS process, and enhances the material stability. LC-MS analysis identifies products and degradation pathways during SDZ reactions. Ecotoxicity assessment and total organic carbon results confirmed the degradation and mineralization of SDZ. This study shed light on the understanding of innovative heterostructured photocatalysts for enhanced PMS oxidation processes.
{"title":"NiFe2O4@MoS2 heterojunction induces the changes of PMS activation mode in PMS/Vis system for the directed generation of 1O2","authors":"Xiaoyi Qi ,&nbsp;Siyu Xu ,&nbsp;Ling Zhang ,&nbsp;Qianqian Cao ,&nbsp;Longquan Zhang ,&nbsp;Xiaoguo Shi ,&nbsp;Yawei Gu ,&nbsp;Chen Wang","doi":"10.1016/j.seppur.2025.132175","DOIUrl":"10.1016/j.seppur.2025.132175","url":null,"abstract":"<div><div>Peroxymonosulfate-based advanced oxidation is a promising approach for water treatment, but how to simply achieve the efficient PMS activation is still a great challenge. In this study, NiFe<sub>2</sub>O<sub>4</sub>@MoS<sub>2</sub> heterojunction was synthesized via hydrothermal method to achieve rapid degradation of sulfadiazine (SDZ) in the synergistic PMS/Visible light photocatalysis system (PMS/Vis). Almost complete elimination of sulfadiazine (SDZ) can be accomplished in 8 min (k<sub>obs</sub> of 0.4038 min<sup>−1</sup>), and forming a synergistic SDZ degradation mechanism including a predominant non-radical pathway (<sup>1</sup>O<sub>2</sub>) and complementary radical pathway (⋅O<sub>2</sub><sup>–</sup>). The special heterojunction structure of NiFe<sub>2</sub>O<sub>4</sub>@MoS<sub>2</sub> could induce the directional separation of photogenerated carriers under visible light. Unlike the conventional transition metal-activated PMS process, the photogenerated electron-hole pairs of NiFe<sub>2</sub>O<sub>4</sub>@MoS<sub>2</sub> could serve as ceaseless PMS activator for ROS generation. The photocatalytic-assisted PMS system (PMS/Vis system) simultaneously solves the problems of variable metal cycling and ion solubilization in the traditional transition metal-activated PMS process, and enhances the material stability. LC-MS analysis identifies products and degradation pathways during SDZ reactions. Ecotoxicity assessment and total organic carbon results confirmed the degradation and mineralization of SDZ. This study shed light on the understanding of innovative heterostructured photocatalysts for enhanced PMS oxidation processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132175"},"PeriodicalIF":8.1,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463240","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
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Separation and Purification Technology
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