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A new strategy for the comprehensive utilization of zinc leaching residue and spent carbon cathode to efficiently solidify zinc, fluorine and recover valuable elements 综合利用锌浸出残渣和废碳阴极以高效固化锌、氟并回收有价元素的新策略
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-22 DOI: 10.1016/j.seppur.2025.132211
Wang Heng, Tan Baolin, Tan Cheng, Yu Yong, Hu Jianhang, Wang Hua
Zinc (Zn) leaching residue, a globally prevalent hazardous waste containing Zn, is conventionally treated through redox smelting at 1523–1723 K. However, high residual Zn in slag causes environmental risks and valuable metal loss. Similarly, spent carbon cathode with soluble fluoride (F) and carbon (C), produced globally at over 1.7 million tons annually, threaten soil, groundwater, and biological safety. This study proposes a novel co-treatment strategy for hazardous waste comprehensive utilization. The effects of spent carbon cathode addition, temperature, and holding time on Zn, F, and Fe transformation pathways were examined. At 1373 K, ZnFe2O4 and Zn2SiO4 in the desulfurized Zn leaching residue transformed to Ca2ZnSi2O7, (Zn,Fe)O, and ((Zn,Fe)O)slag, and then reduced to Zn(g) and Fe through spent carbon cathode. F-containing phase from spent carbon cathode were immobilized in molten slag, enhancing Fe particle growth and Zn reduction. Subsequent cooling transformed to Ca4F2Si2O7, achieving a F solidification ratio of 99.92 % and a leaching content of 7.84 mg/L, thereby minimizing environmental risks. Compared with conventional methods, the proposed strategy improved Zn and Fe recovery ratios by 4 % and 78 %, respectively, and reduced Zn leaching content to 0.11 mg/L. This approach utilizes waste to treat waste, contributing to the sustainable development of the global Zn and Al industries.
{"title":"A new strategy for the comprehensive utilization of zinc leaching residue and spent carbon cathode to efficiently solidify zinc, fluorine and recover valuable elements","authors":"Wang Heng,&nbsp;Tan Baolin,&nbsp;Tan Cheng,&nbsp;Yu Yong,&nbsp;Hu Jianhang,&nbsp;Wang Hua","doi":"10.1016/j.seppur.2025.132211","DOIUrl":"10.1016/j.seppur.2025.132211","url":null,"abstract":"<div><div>Zinc (Zn) leaching residue, a globally prevalent hazardous waste containing Zn, is conventionally treated through redox smelting at 1523–1723 K. However, high residual Zn in slag causes environmental risks and valuable metal loss. Similarly, spent carbon cathode with soluble fluoride (F) and carbon (C), produced globally at over 1.7 million tons annually, threaten soil, groundwater, and biological safety. This study proposes a novel co-treatment strategy for hazardous waste comprehensive utilization. The effects of spent carbon cathode addition, temperature, and holding time on Zn, F, and Fe transformation pathways were examined. At 1373 K, ZnFe<sub>2</sub>O<sub>4</sub> and Zn<sub>2</sub>SiO<sub>4</sub> in the desulfurized Zn leaching residue transformed to Ca<sub>2</sub>ZnSi<sub>2</sub>O<sub>7</sub>, (Zn,Fe)O, and ((Zn,Fe)O)<sub>slag</sub>, and then reduced to Zn(g) and Fe through spent carbon cathode. F-containing phase from spent carbon cathode were immobilized in molten slag, enhancing Fe particle growth and Zn reduction. Subsequent cooling transformed to Ca<sub>4</sub>F<sub>2</sub>Si<sub>2</sub>O<sub>7</sub>, achieving a F solidification ratio of 99.92 % and a leaching content of 7.84 mg/L, thereby minimizing environmental risks. Compared with conventional methods, the proposed strategy improved Zn and Fe recovery ratios by 4 % and 78 %, respectively, and reduced Zn leaching content to 0.11 mg/L. This approach utilizes waste to treat waste, contributing to the sustainable development of the global Zn and Al industries.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132211"},"PeriodicalIF":8.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471068","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
Anchoring hydrogen bonding receptors into MOFs for enhancing simultaneous recovery of C2H4 and C3H6
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132190
Si-Ru Liu, Hai-Yu Duan, Li-Fei Wu, Jia-Hui Zhao, Yu-Jing Wang, Xiu-Yuan Li
To obtain both C2H4 and C3H6 simultaneously in one adsorption–desorption cycle for complicated ternary C2H4/C2H6/C3H6 mixtures is important but difficult process in petrochemical industries. To address this challenge, an efficient strategy that anchoring hydrogen bonding receptors into MOFs has been successfully exerted, and a series of isostructural pillared porous MOFs have been developed for olefin purification. In particular, 1-Cl2 can preferentially adsorb C3H6 and C2H6 rather than C2H4, and reveals high C3H6 uptake of 109.0 cm3 g−1 even under low pressure of 20 kPa and 298 K. The breakthrough experiments of C3H6/C2H4 and C2H6/C2H4 binary mixtures as well as C3H6/C2H6/C2H4 ternary mixtures demonstrated that the 1-Cl2 can more effectively yield high-purity C2H4 products (≥99.9 %) in one step and recover polymer-grade C3H6 (≥99.5 %) through a single adsorption–desorption cycle. GCMC simulation indicates multiple hydrogen bonds produced by plentiful Cl atoms in the channel is responsible for excellent olefin purification abilities of 1-Cl2.
{"title":"Anchoring hydrogen bonding receptors into MOFs for enhancing simultaneous recovery of C2H4 and C3H6","authors":"Si-Ru Liu, Hai-Yu Duan, Li-Fei Wu, Jia-Hui Zhao, Yu-Jing Wang, Xiu-Yuan Li","doi":"10.1016/j.seppur.2025.132190","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132190","url":null,"abstract":"To obtain both C<sub>2</sub>H<sub>4</sub> and C<sub>3</sub>H<sub>6</sub> simultaneously in one adsorption–desorption cycle for complicated ternary C<sub>2</sub>H<sub>4</sub>/C<sub>2</sub>H<sub>6</sub>/C<sub>3</sub>H<sub>6</sub> mixtures is important but difficult process in petrochemical industries. To address this challenge, an efficient strategy that anchoring hydrogen bonding receptors into MOFs has been successfully exerted, and a series of isostructural pillared porous MOFs have been developed for olefin purification. In particular, <strong>1-Cl<sub>2</sub></strong> can preferentially adsorb C<sub>3</sub>H<sub>6</sub> and C<sub>2</sub>H<sub>6</sub> rather than C<sub>2</sub>H<sub>4</sub>, and reveals high C<sub>3</sub>H<sub>6</sub> uptake of 109.0 cm<sup>3</sup> g<sup>−1</sup> even under low pressure of 20 kPa and 298 K. The breakthrough experiments of C<sub>3</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> binary mixtures as well as C<sub>3</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>6</sub>/C<sub>2</sub>H<sub>4</sub> ternary mixtures demonstrated that the <strong>1-Cl<sub>2</sub></strong> can more effectively yield high-purity C<sub>2</sub>H<sub>4</sub> products (≥99.9 %) in one step and recover polymer-grade C<sub>3</sub>H<sub>6</sub> (≥99.5 %) through a single adsorption–desorption cycle. GCMC simulation indicates multiple hydrogen bonds produced by plentiful Cl atoms in the channel is responsible for excellent olefin purification abilities of <strong>1-Cl<sub>2</sub></strong>.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"34 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463206","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
An efficient method for tin recovery in waste printed circuit boards: Ultrasonic coupled composite organic acid system
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132146
Yi Li, Mingrui Zhang, Junwei Guo, Ziyang Yu, Bo Zhang
Waste printed circuit boards are abundant in Sn and possess significant recycling potential. In this study, an ultrasonic coupled composite organic acid system was proposed to enhance the leaching of Sn from waste printed circuit boards. The composite organic acid system was constructed with citric acid as leaching agent and ascorbic acid as reducing agent to promote the conversion leaching of multivalent Sn ions. On this basis, the shock wave and high-speed micro-jet generated by the ultrasonic cavitation effect continuously impact the surface of Sn, accelerating the mass transfer rate at the solid–liquid interface, and effectively strengthening the leaching process of the Sn. The influence of ultrasonic intensity, leaching conditions and compound concentration of composite organic acid on the leaching effect of Sn was investigated. When the leaching agent concentration is 0.80 mol/L and the reducing agent concentration is 0.20 mol/L, the composite organic acid system has excellent reduction and leaching properties for Sn ions. When combined with the ultrasonic power of 96 W, the leaching rate of Sn is the highest (89.03 %). The cavitation mechanism of ultrasonic waves significantly enhances the Sn leaching process, increasing the leaching rate by over 15 %. And kinetic analysis revealed that the tin leaching process conformed to the pseudo-first-order model in the progressive conversion model, with an apparent activation energy of 64.37 kJ/mol. This study reveals the leaching mechanism of Sn by ultrasonic coupling composite organic acid system and provides a novel method for the efficient leaching of Sn from WPCBs.
{"title":"An efficient method for tin recovery in waste printed circuit boards: Ultrasonic coupled composite organic acid system","authors":"Yi Li, Mingrui Zhang, Junwei Guo, Ziyang Yu, Bo Zhang","doi":"10.1016/j.seppur.2025.132146","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132146","url":null,"abstract":"Waste printed circuit boards are abundant in Sn and possess significant recycling potential. In this study, an ultrasonic coupled composite organic acid system was proposed to enhance the leaching of Sn from waste printed circuit boards. The composite organic acid system was constructed with citric acid as leaching agent and ascorbic acid as reducing agent to promote the conversion leaching of multivalent Sn ions. On this basis, the shock wave and high-speed micro-jet generated by the ultrasonic cavitation effect continuously impact the surface of Sn, accelerating the mass transfer rate at the solid–liquid interface, and effectively strengthening the leaching process of the Sn. The influence of ultrasonic intensity, leaching conditions and compound concentration of composite organic acid on the leaching effect of Sn was investigated. When the leaching agent concentration is 0.80 mol/L and the reducing agent concentration is 0.20 mol/L, the composite organic acid system has excellent reduction and leaching properties for Sn ions. When combined with the ultrasonic power of 96 W, the leaching rate of Sn is the highest (89.03 %). The cavitation mechanism of ultrasonic waves significantly enhances the Sn leaching process, increasing the leaching rate by over 15 %. And kinetic analysis revealed that the tin leaching process conformed to the pseudo-first-order model in the progressive conversion model, with an apparent activation energy of 64.37 kJ/mol. This study reveals the leaching mechanism of Sn by ultrasonic coupling composite organic acid system and provides a novel method for the efficient leaching of Sn from WPCBs.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"20 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463173","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
Vibration-assisted ultrafiltration dramatically improves mRNA purification
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132179
Ali Behboudi, Amin Javidanbardan, Ziqiao Wang, Luolin Zhou, Andrew L. Zydney
The development of high-quality messenger RNA (mRNA) products depends critically on the development of effective methods for purification and formulation of these gene therapies. Conventional ultrafiltration processes have been successfully used for mRNA concentration, but membrane fouling and shear-induced mRNA degradation can limit their effectiveness. This study provides the first demonstration of Vibro Membrane Filtration (VMF) to perform vibration-assisted single pass tangential flow filtration (SPTFF) for the concentration and purification of mRNA produced by in vitro transcription. Data were obtained using 100 kDa polyethersulfone membranes using two mRNA constructs with very different sizes. The sustainable flux, protein removal, and extent of fouling were evaluated in the presence and absence of vibration. The vibration significantly reduces concentration polarization leading to an increase in the sustainable flux, a reduction in membrane fouling, and better mRNA purification. The VMF was able to provide continuous operation for 24 hr with 10X concentration factor without any loss in mRNA integrity. These results demonstrate the exciting potential of using VMF for the continuous and / or intensified bioprocessing of mRNA therapeutics.
开发高质量的信使核糖核酸(mRNA)产品,关键在于开发纯化和配制这些基因疗法的有效方法。传统的超滤工艺已成功用于浓缩 mRNA,但膜堵塞和剪切力引起的 mRNA 降解会限制其有效性。本研究首次展示了用振动膜过滤(VMF)进行振动辅助单程切向流过滤(SPTFF)浓缩和纯化体外转录产生的 mRNA 的方法。数据是使用 100 kDa 聚醚砜膜和两种不同大小的 mRNA 构建物获得的。在有振动和无振动的情况下,对可持续通量、蛋白质去除率和结垢程度进行了评估。振动大大降低了浓度极化,从而提高了持续通量,减少了膜堵塞,提高了 mRNA 纯化效果。VMF 能够以 10 倍浓缩因子连续运行 24 小时,而 mRNA 的完整性不会受到任何影响。这些结果表明,将 VMF 用于 mRNA 治疗的连续和/或强化生物处理具有令人兴奋的潜力。
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引用次数: 0
Synergetic dual co-catalyst and interfacial bonds in N-CQDs/NCN/BNQDs to promote photoremoval of uranium(VI)
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132193
Qixu Chen , Qianxiang Xiao , Feng He , Wen He , Kai Liu , Chongkun Zhao , Ziyang Chang , Hongqing Wang
The photocatalytic efficiency of a catalyst is dependent on two main factors: the separation of excitons and the migration of photogenerated carriers. Therefore, we employed a strategy of defect engineering, co-catalyst co-modification and interfacial chemical bonding synergistic modification to prepare N-CQDs-x/NCN/BNQDs-y by introducing nitrogen defects in graphitic carbon nitride (NCN) and concomitantly incorporating boron nitride quantum dots (BNQDs) and nitrogen-doped carbon quantum dots (N-CQDs) onto its surface. And the N-CQDs-15/NCN/BNQDs-1 showed excellent photocatalytic removal of U(VI), which achieved 98.7 % after 120 min of illumination. Furthermore, the catalytic activities were ranked as follows: N-CQDs-15/NCN/BNQDs-1 > N-CQDs-15/NCN > NCN/BNQDs-1 > NCN > g-C3N4. Systematic investigations unveiled that the improved catalytic performance of N-CQDs-15/NCN/BNQDs-1 was mainly attributed to the nitrogen defects in g-C3N4 facilitating carrier separation, the C–C interface bonding between N-CQDs and g-C3N4 and the hydrogen bonding between BNQDs and g-C3N4, as well as co-catalysts transferring electrons and holes, respectively, promoting the simultaneous transfer of e- and h+. Simultaneously, the prepared photocatalytic materials exhibited outstanding cyclic stability, with the U(VI) removal rate by the catalyst remaining above 91 % after five consecutive photocatalytic experiments. This study not only presents an effective photocatalytic material for the remediation of uranium-containing wastewater but also offers insights into the design of efficient photocatalysts.
{"title":"Synergetic dual co-catalyst and interfacial bonds in N-CQDs/NCN/BNQDs to promote photoremoval of uranium(VI)","authors":"Qixu Chen ,&nbsp;Qianxiang Xiao ,&nbsp;Feng He ,&nbsp;Wen He ,&nbsp;Kai Liu ,&nbsp;Chongkun Zhao ,&nbsp;Ziyang Chang ,&nbsp;Hongqing Wang","doi":"10.1016/j.seppur.2025.132193","DOIUrl":"10.1016/j.seppur.2025.132193","url":null,"abstract":"<div><div>The photocatalytic efficiency of a catalyst is dependent on two main factors: the separation of excitons and the migration of photogenerated carriers. Therefore, we employed a strategy of defect engineering, co-catalyst co-modification and interfacial chemical bonding synergistic modification to prepare N-CQDs-x/NCN/BNQDs-y by introducing nitrogen defects in graphitic carbon nitride (NCN) and concomitantly incorporating boron nitride quantum dots (BNQDs) and nitrogen-doped carbon quantum dots (N-CQDs) onto its surface. And the N-CQDs-<sub>15</sub>/NCN/BNQDs-<sub>1</sub> showed excellent photocatalytic removal of U(VI), which achieved 98.7 % after 120 min of illumination. Furthermore, the catalytic activities were ranked as follows: N-CQDs-<sub>15</sub>/NCN/BNQDs-<sub>1</sub> &gt; N-CQDs-<sub>15</sub>/NCN &gt; NCN/BNQDs-<sub>1</sub> &gt; NCN &gt; g-C<sub>3</sub>N<sub>4</sub>. Systematic investigations unveiled that the improved catalytic performance of N-CQDs-<sub>15</sub>/NCN/BNQDs-<sub>1</sub> was mainly attributed to the nitrogen defects in g-C<sub>3</sub>N<sub>4</sub> facilitating carrier separation, the C–C interface bonding between N-CQDs and g-C<sub>3</sub>N<sub>4</sub> and the hydrogen bonding between BNQDs and g-C<sub>3</sub>N<sub>4</sub>, as well as co-catalysts transferring electrons and holes, respectively, promoting the simultaneous transfer of e<sup>-</sup> and h<sup>+</sup>. Simultaneously, the prepared photocatalytic materials exhibited outstanding cyclic stability, with the U(VI) removal rate by the catalyst remaining above 91 % after five consecutive photocatalytic experiments. This study not only presents an effective photocatalytic material for the remediation of uranium-containing wastewater but also offers insights into the design of efficient photocatalysts.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132193"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463171","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
Evaluation of a novel kaolinite loaded sulfidized nZVI aggregates for removing Cr(VI) and Cd(II) in water: New sulfurization strategy, morphological control, performance, and synergistic mechanisms
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132171
Jie Hu, Peiwei Hu
The morphology plays a crucial role in the performance of nanomaterials. Nano-zero-valent iron (nZVI) is commonly used in the treatment of heavy metal pollution in water, but its application is limited due to a variety of defects. In this study, a new method was used to successfully synthesize the vulcanized nano-zero-valent iron (S-nZVI@K) supported by kaolin, which has excellent properties compared with nZVI related materials. In the process of vulcanization, both the aggregates and the vulcanized states of zero-valent iron were obtained. The formation of zero-valent iron aggregates and the morphology of aggregates were found in the process of optimization synthesis. Characterization of the morphology and structure revealed that S-nZVI was uniformly distributed on the surface of kaolin, with particle shape being adjustable by varying hydrothermal conditions. Batch experiments demonstrated excellent adsorption performance of S-nZVI@K towards heavy metal ions. Kinetic analysis indicated that the removal process followed a pseudo-second-order model and Langmuir adsorption isotherm model, with maximum adsorption capacities reaching 88.88 mg/g for Cr(Ⅵ) and 174.69 mg/g for Cd(II), respectively. Furthermore, thermodynamic analysis confirmed that the removal of the heavy metals proceeded through spontaneous endothermic chemisorption. The removal mechanism of S-nZVI@K for Cr(VI) primarily involved adsorption, reduction, and co-precipitation processes, while complexation adsorption and precipitation played key roles in removing Cd(II).
{"title":"Evaluation of a novel kaolinite loaded sulfidized nZVI aggregates for removing Cr(VI) and Cd(II) in water: New sulfurization strategy, morphological control, performance, and synergistic mechanisms","authors":"Jie Hu, Peiwei Hu","doi":"10.1016/j.seppur.2025.132171","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132171","url":null,"abstract":"The morphology plays a crucial role in the performance of nanomaterials. Nano-zero-valent iron (nZVI) is commonly used in the treatment of heavy metal pollution in water, but its application is limited due to a variety of defects. In this study, a new method was used to successfully synthesize the vulcanized nano-zero-valent iron (S-nZVI@K) supported by kaolin, which has excellent properties compared with nZVI related materials. In the process of vulcanization, both the aggregates and the vulcanized states of zero-valent iron were obtained. The formation of zero-valent iron aggregates and the morphology of aggregates were found in the process of optimization synthesis. Characterization of the morphology and structure revealed that S-nZVI was uniformly distributed on the surface of kaolin, with particle shape being adjustable by varying hydrothermal conditions. Batch experiments demonstrated excellent adsorption performance of S-nZVI@K towards heavy metal ions. Kinetic analysis indicated that the removal process followed a pseudo-second-order model and Langmuir adsorption isotherm model, with maximum adsorption capacities reaching 88.88 mg/g for Cr(Ⅵ) and 174.69 mg/g for Cd(II), respectively. Furthermore, thermodynamic analysis confirmed that the removal of the heavy metals proceeded through spontaneous endothermic chemisorption. The removal mechanism of S-nZVI@K for Cr(VI) primarily involved adsorption, reduction, and co-precipitation processes, while complexation adsorption and precipitation played key roles in removing Cd(II).","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"7 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463202","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
Integrating machine learning regression and classification for enhanced interpretability in optimizing the Fenton process for real wastewater treatment conditions
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132182
Başak Temur Ergan , Ozgun Yucel , Erhan Gengec , Ebubekir Siddik Aydin
The Fenton process is an important process used in treating textile wastewater such as Jeans-wash wastewater (JWW). Predicting the results of this process according to Fenton parameters is a critical step to evaluating the treatment performance. One of the important ways to improve treatment performance is to use machine learning methods. Therefore, machine learning methods using experimental Fenton treatment data were proposed to mathematically demonstrate the effect of the hydrogen peroxide (H2O2) and iron sulfate (FeSO4) dosage on dye and total organic carbon (TOC) concentration within this research. To increase the predictive capability of machine learning methods, in addition to concentration of H2O2 and FeSO4 inputs, dye and TOC initial concentration values were used as inputs in the machine learning methods. Four regression techniques were used to forecast the dye and TOC concentration outputs of Fenton process, namely Random Forest Regression (RFR), Gaussian Process Regression (GPR), Decision Tree Regression (DTR), and Generalized Additive Model (GAM) in this study. Hold-out and k-fold cross-validation were used in combination to examine the effectiveness of the suggested regression techniques. Among these machine learning methods, GPR was more successful than the other proposed models with predicted the dye concentration as R2 > 0.97 and TOC concentration as R2 > 0.86. Finally, illustration of decision tree classifiers indicating the process operation were placed with interpretable machine learning. With these trees, the input-range/target result relationship depending on the input parameters of the process was established to eliminate the side reactions that occur due to the nature of the Fenton process.
{"title":"Integrating machine learning regression and classification for enhanced interpretability in optimizing the Fenton process for real wastewater treatment conditions","authors":"Başak Temur Ergan ,&nbsp;Ozgun Yucel ,&nbsp;Erhan Gengec ,&nbsp;Ebubekir Siddik Aydin","doi":"10.1016/j.seppur.2025.132182","DOIUrl":"10.1016/j.seppur.2025.132182","url":null,"abstract":"<div><div>The Fenton process is an important process used in treating textile wastewater such as Jeans-wash wastewater (JWW). Predicting the results of this process according to Fenton parameters is a critical step to evaluating the treatment performance. One of the important ways to improve treatment performance is to use machine learning methods. Therefore, machine learning methods using experimental Fenton treatment data were proposed to mathematically demonstrate the effect of the hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) and iron sulfate (FeSO<sub>4</sub>) dosage on dye and total organic carbon (TOC) concentration within this research. To increase the predictive capability of machine learning methods, in addition to concentration of H<sub>2</sub>O<sub>2</sub> and FeSO<sub>4</sub> inputs, dye and TOC initial concentration values were used as inputs in the machine learning methods. Four regression techniques were used to forecast the dye and TOC concentration outputs of Fenton process, namely Random Forest Regression (RFR), Gaussian Process Regression (GPR), Decision Tree Regression (DTR), and Generalized Additive Model (GAM) in this study. Hold-out and k-fold cross-validation were used in combination to examine the effectiveness of the suggested regression techniques. Among these machine learning methods, GPR was more successful than the other proposed models with predicted the dye concentration as R<sup>2</sup> &gt; 0.97 and TOC concentration as R<sup>2</sup> &gt; 0.86. Finally, illustration of decision tree classifiers indicating the process operation were placed with interpretable machine learning. With these trees, the input-range/target result relationship depending on the input parameters of the process was established to eliminate the side reactions that occur due to the nature of the Fenton process.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132182"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463204","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
Performance and mechanism of peroxymonosulfate heterogeneous activation based on FeII-siderite&dithionite for carbamazepine degradation
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132170
Wei Song , Zhaosheng Lei , Hongze Fang , Caixia Fu , Yan Cang , Yuning Fang , Ruigang Wang , Bin Li , Xing Du , Zhihong Wang , Zhiwei Zhao
Sulfate radicals-based advanced oxidation process (SO4-AOPs) exhibits remarkable efficacy for emerging contaminants (ECs) eradication. In this work, we utilized natural FeII-siderite as a catalyst with dithionite (DTN) and peroxymonosulfate (PMS) precursors to engineer the FeII-siderite&DTN/PMS system. Carbamazepine (CBZ) elimination efficiency exceeded 90% in 10 min with reactive species of SO4 and OH, even in the anaerobic condition due to the sufficient oxidation species source from broken peroxy bond. The system generated various radicals (e.g., SO4, SO3, OH, and SO5) through redox cycles involving FeII-siderite, DTN, and PMS, with FeII/FeIII interconversion driven by PMS oxidation and DTN reduction. Enhanced electron shuttling and FeII/FeIII interconversion at the phase interface, the rate-limiting step in iron-based AOPs, facilitated PMS activation. CBZ degradation followed four pathways including deacylation, ring-opening oxidation, hydroxylation, decarboxylation, and deketonization, with reactive sites at CBZ-7C and CBZ-8C identified by LC-MS/MS and density functional theory (DFT). Oxygen consumption rate (OCR) toxicity assessments revealed persistent toxicity of intermediates, yet the FeII-siderite&DTN/PMS system detoxified them effectively based on T.E.S.T. evaluation. And the system demonstrates potential for ECs remediation, particularly in high salinity waters, due to the significant enhancement of higher Cl concentrations.
{"title":"Performance and mechanism of peroxymonosulfate heterogeneous activation based on FeII-siderite&dithionite for carbamazepine degradation","authors":"Wei Song ,&nbsp;Zhaosheng Lei ,&nbsp;Hongze Fang ,&nbsp;Caixia Fu ,&nbsp;Yan Cang ,&nbsp;Yuning Fang ,&nbsp;Ruigang Wang ,&nbsp;Bin Li ,&nbsp;Xing Du ,&nbsp;Zhihong Wang ,&nbsp;Zhiwei Zhao","doi":"10.1016/j.seppur.2025.132170","DOIUrl":"10.1016/j.seppur.2025.132170","url":null,"abstract":"<div><div>Sulfate radicals-based advanced oxidation process (SO<sub>4</sub><sup><img>−</sup>-AOPs) exhibits remarkable efficacy for emerging contaminants (ECs) eradication. In this work, we utilized natural Fe<sup>II</sup>-siderite as a catalyst with dithionite (DTN) and peroxymonosulfate (PMS) precursors to engineer the Fe<sup>II</sup>-siderite&amp;DTN/PMS system. Carbamazepine (CBZ) elimination efficiency exceeded 90% in 10 min with reactive species of SO<sub>4</sub><sup><img>−</sup> and <sup><img></sup>OH, even in the anaerobic condition due to the sufficient oxidation species source from broken peroxy bond. The system generated various radicals (e.g., SO<sub>4</sub><sup><img>−</sup>, SO<sub>3</sub><sup><img>−</sup>, <sup><img></sup>OH, and SO<sub>5</sub><sup><img>−</sup>) through redox cycles involving Fe<sup>II</sup>-siderite, DTN, and PMS, with Fe<sup>II</sup>/Fe<sup>III</sup> interconversion driven by PMS oxidation and DTN reduction. Enhanced electron shuttling and Fe<sup>II</sup>/Fe<sup>III</sup> interconversion at the phase interface, the rate-limiting step in iron-based AOPs, facilitated PMS activation. CBZ degradation followed four pathways including deacylation, ring-opening oxidation, hydroxylation, decarboxylation, and deketonization, with reactive sites at CBZ-7C and CBZ-8C identified by LC-MS/MS and density functional theory (DFT). Oxygen consumption rate (OCR) toxicity assessments revealed persistent toxicity of intermediates, yet the Fe<sup>II</sup>-siderite&amp;DTN/PMS system detoxified them effectively based on T.E.S.T. evaluation. And the system demonstrates potential for ECs remediation, particularly in high salinity waters, due to the significant enhancement of higher Cl<sup>−</sup> concentrations.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132170"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463210","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
Fe-based layered double hydroxides carbon cathode modulates oxygen reduction pathways and HO formation mechanism in electro-peroxone system
IF 8.6 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132212
Zekun Dong, Jiao Yang, Jie Yao, Yu Tang, Yan Zhang
Electro-peroxone (EP) is an emerging technology that combines electrochemistry and O3 to remove contaminants. However, conventional carbon cathodes primarily contribute to the synthesis of H2O2 in the system, which may scavenge HOradical dot. Herein, a series of Fe-based layered double hydroxides (LDH) was loaded onto graphite felt cathodes to strengthen the removal of organic contaminants. The EP system with CuFe-LDH/GF cathode (EP-CuFe-LDH/GF) demonstrated the highest removal rate (91.2 % within 20 min) of oxalic acid (OA), a typical ozone-resistance substance, approximately twice that of the EP-GF system. HOradical dot was identified the main reactive species. A new pathway for O2 reduction and the generation of HOradical dot was found. The loading of CuFe-LDH altered the reduction pathway of O2 on the GF cathode from 2e to 1e or 4e process. As a result, HOradical dot was produced by the combination of O3 and O2radical dot instead of O3 and H2O2, which avoided the quenching of HOradical dot by H2O2 and enhanced the removal of OA. Moreover, the breaking complexation by O3, cathodic O3 reduction and metal-OH catalyzed O3 processes also contributed to the HOradical dot formation. Furthermore, the system could efficiently remove OA across a broad pH range of 3.0 to 9.0, addressing the poor performance of conventional EP systems under acidic conditions. Overall, the finding of this significant mechanism advances the understanding of organic pollutants removal and broadens the potential applications of EP system.
{"title":"Fe-based layered double hydroxides carbon cathode modulates oxygen reduction pathways and HO formation mechanism in electro-peroxone system","authors":"Zekun Dong, Jiao Yang, Jie Yao, Yu Tang, Yan Zhang","doi":"10.1016/j.seppur.2025.132212","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.132212","url":null,"abstract":"Electro-peroxone (EP) is an emerging technology that combines electrochemistry and O<sub>3</sub> to remove contaminants. However, conventional carbon cathodes primarily contribute to the synthesis of H<sub>2</sub>O<sub>2</sub> in the system, which may scavenge HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup>. Herein, a series of Fe-based layered double hydroxides (LDH) was loaded onto graphite felt cathodes to strengthen the removal of organic contaminants. The EP system with CuFe-LDH/GF cathode (EP-CuFe-LDH/GF) demonstrated the highest removal rate (91.2 % within 20 min) of oxalic acid (OA), a typical ozone-resistance substance, approximately twice that of the EP-GF system. HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup> was identified the main reactive species. A new pathway for O<sub>2</sub> reduction and the generation of HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup> was found. The loading of CuFe-LDH altered the reduction pathway of O<sub>2</sub> on the GF cathode from 2e<sup>−</sup> to 1e<sup>−</sup> or 4e<sup>−</sup> process. As a result, HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup> was produced by the combination of O<sub>3</sub> and O<sub>2</sub><sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/>−</sup> instead of O<sub>3</sub> and H<sub>2</sub>O<sub>2</sub>, which avoided the quenching of HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup> by H<sub>2</sub>O<sub>2</sub> and enhanced the removal of OA. Moreover, the breaking complexation by O<sub>3</sub>, cathodic O<sub>3</sub> reduction and metal-OH catalyzed O<sub>3</sub> processes also contributed to the HO<sup><img alt=\"radical dot\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/rad.gif\" style=\"vertical-align:middle\"/></sup> formation. Furthermore, the system could efficiently remove OA across a broad pH range of 3.0 to 9.0, addressing the poor performance of conventional EP systems under acidic conditions. Overall, the finding of this significant mechanism advances the understanding of organic pollutants removal and broadens the potential applications of EP system.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"25 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471052","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 state-of-the-art review of explicit multicomponent isotherm models for the modeling of equilibrium data: From fundamentals to applications
IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2025-02-21 DOI: 10.1016/j.seppur.2025.132202
Qili Hu , Liting Hao , Qiuming Pei , Yunhui Zhang
This review provided a comprehensive analysis of explicit multicomponent isotherm models for the modeling of equilibrium data in adsorption processes, covering their fundamental principles and practical applications. The complexity of multicomponent adsorption was highlighted, and the potential effects of water molecules, pH, and initial concentration on the adsorption process were emphasized. The review systematically categorized explicit multicomponent isotherm models into predictive and correlative approaches, discussing their underlying assumptions, thermodynamic consistency, and practical applications. The predictive models relied only on single-component isotherm parameters but usually failed to account for the complex adsorption processes. In contrast, the correlative models could offer higher fitting quality due to the incorporation of interaction factors or competition coefficients. The review addressed common mistakes encountered in data processing, model selection, and parameter estimation, emphasizing the importance of accurate determination of isotherm data. Some typical cases were presented to demonstrate the practical application of these models in predicting competitive adsorption in water and wastewater treatment. Moreover, the review emphasized the necessity of using advanced statistical methods like Akaike information criterion (AIC) and Bayesian information criterion (BIC) for model comparison and indicated future research directions. This work aimed to enhance readers’ understanding of explicit multicomponent isotherm models and improve the design and optimization of adsorption-based separation processes.
{"title":"A state-of-the-art review of explicit multicomponent isotherm models for the modeling of equilibrium data: From fundamentals to applications","authors":"Qili Hu ,&nbsp;Liting Hao ,&nbsp;Qiuming Pei ,&nbsp;Yunhui Zhang","doi":"10.1016/j.seppur.2025.132202","DOIUrl":"10.1016/j.seppur.2025.132202","url":null,"abstract":"<div><div>This review provided a comprehensive analysis of explicit multicomponent isotherm models for the modeling of equilibrium data in adsorption processes, covering their fundamental principles and practical applications. The complexity of multicomponent adsorption was highlighted, and the potential effects of water molecules, pH, and initial concentration on the adsorption process were emphasized. The review systematically categorized explicit multicomponent isotherm models into predictive and correlative approaches, discussing their underlying assumptions, thermodynamic consistency, and practical applications. The predictive models relied only on single-component isotherm parameters but usually failed to account for the complex adsorption processes. In contrast, the correlative models could offer higher fitting quality due to the incorporation of interaction factors or competition coefficients. The review addressed common mistakes encountered in data processing, model selection, and parameter estimation, emphasizing the importance of accurate determination of isotherm data. Some typical cases were presented to demonstrate the practical application of these models in predicting competitive adsorption in water and wastewater treatment. Moreover, the review emphasized the necessity of using advanced statistical methods like Akaike information criterion (AIC) and Bayesian information criterion (BIC) for model comparison and indicated future research directions. This work aimed to enhance readers’ understanding of explicit multicomponent isotherm models and improve the design and optimization of adsorption-based separation processes.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"363 ","pages":"Article 132202"},"PeriodicalIF":8.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463172","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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