{"title":"Box–Behnken design and machine learning optimization of PET fluorescent carbon quantum dots for removing fluoxetine and ciprofloxacin with molecular dynamics and docking studies as potential antidepressant and antibiotic","authors":"Christian Ebere Enyoh, Qingyue Wang","doi":"10.1016/j.seppur.2025.131975","DOIUrl":"10.1016/j.seppur.2025.131975","url":null,"abstract":"<div><div>This study investigates the optimization, multifunctional applications, and ADMET (Absorption, Distribution, Metabolism, Excretion, and Toxicity) evaluation of polyethylene terephthalate-derived fluorescent carbon quantum dots (PET-FCQDs, size: 9.98 ± 10.90 nm) for removing fluoxetine (FLX; 100–400 ng/L) and ciprofloxacin (CIP; 50–150 µg/L) from aqueous solutions and exploring their therapeutic potential as antidepressants and antibiotics. Box-Behnken Design (BBD) and machine learning models—Artificial Neural Networks (ANN) and Support Vector Machines (SVM)—optimized removal efficiencies of 95.19 % for FLX and 97.85 % for CIP, with ANN achieving superior prediction accuracy (R2: 0.82–0.88). Adsorption adhered to Langmuir (FLX; R2 > 0.999) and Freundlich isotherms (FLX and CIP; R2 > 0.998) with intraparticle diffusion kinetics (R2 > 0.94). Maximum monolayer adsorption capacities were 705 ng/g for CIP and 62.27 ng/g for FLX. Mechanistic studies via ATR-FTIR and molecular dynamics revealed hydrogen bonding, π-π stacking, and electrostatic interactions as key drivers. Molecular docking highlighted PET-FCQDs’ intrinsic antidepressant potential (docking score: −8.7 kcal/mol for SERT) and their synergy with CIP (−7.3 kcal/mol for topoisomerase IV). ADMET analysis via SwissADME and ADMETSAR server confirmed high gastrointestinal absorption, positive Blood Brain Barrier, non-carcinogenicity, and non-biodegradability. However, high toxicity to ecological organisms such fish, honey bee and Tetrahymena Pyriformis raises concerns about potential ecological risks if released into environments This comprehensive study integrates experimental and computational approaches to optimize PET-FCQDs for environmental and pharmaceutical applications, showcasing their dual role as effective adsorbents for removing contaminants and as potential therapeutic agents. The findings provide a framework for the sustainable utilization of PET waste in developing multifunctional nanomaterials.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131975"},"PeriodicalIF":8.1,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258135","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}
Hang Wang, Yujie Zhang, Yuchen Shi, Jiatong Ma, Ning Cai, Juanqin Xue, Haodi Song
{"title":"A 3D porous MnHCF/MXene electrode for enhanced deionization performance in high-salinity water","authors":"Hang Wang, Yujie Zhang, Yuchen Shi, Jiatong Ma, Ning Cai, Juanqin Xue, Haodi Song","doi":"10.1016/j.seppur.2025.131986","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131986","url":null,"abstract":"Capacitive deionization (CDI) technology shows great potential for the treatment of high-salinity wastewater generated by coal chemical industries. MXene has gained significant attention as a potential material for CDI applications, but the stacking of MXene layers limits its application. Thus, the MnHCF/MXene composite material with 3D porous structure was designed and prepared. The results showed that MnHCF/MXene composite with 3D okra-like structure was successfully synthesized, and the specific surface area was 84 m<sup>2</sup>/g, average pore diameter was 20 nm, and a pore volume was 0.47 cm<sup>3</sup> g<sup>−1</sup>, which were all better than those of MXene. These results highlighted a significantly enhanced porous structure. Furthermore, the composite exhibited an outstanding capacitance of 187.7F/g, and a low charge transfer resistance of 0.57 O cm<sup>2</sup> s<sup>−1</sup>, indicating excellent ion diffusion and electrochemical performance. The CDI experimental results showed that the composite electrode has an excellent desalination performance with 177.12 mg/g of desalination capacity, 9.84 mg/g min<sup>−1</sup> of desalination rate and only 0.58 Wh/g of energy consumption. The results of stability experiments shown that the specific capacitance of the MnHCF/MXene electrode retained 93.13 % and 91.31 % in CV and GCD during 150 cycles, respectively.This study provides valuable insights into the strategic structural design of advanced desalination materials and offers critical data to support the application of CDI technology in the treatment of high-salinity wastewater.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"20 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143191930","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}
Yan-Hong Wei, Ming-Xing Li, Yan-Shu Xiong, Jia-Xin Wang, Mei Li, Wei Wei, Fu-Hou Lei, Wen Li
{"title":"Rose-inspired salt-responsive hierarchical microbead via in-situ growth of layered double hydroxide plates onto rosin-derived resin for efficient tetracycline removal: Ingenious design, advanced molecular simulations, and rethinking adsorption mass transfer","authors":"Yan-Hong Wei, Ming-Xing Li, Yan-Shu Xiong, Jia-Xin Wang, Mei Li, Wei Wei, Fu-Hou Lei, Wen Li","doi":"10.1016/j.seppur.2025.131952","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131952","url":null,"abstract":"Flower-like Ni/Al layered double hydroxides (Ni/Al-LDHs) were <em>in-situ</em> grown on rosin-derived resin to design a rose-inspired hierarchical microbead (RIHMB), which is efficient in removing tetracycline hydrochloride (TCH) from water system. The ingeniously designed dual-layer structure of RIHMB features an inner layer rich in quaternary ammonium (–R<sub>4</sub>N<sup>+</sup>) that strongly attracts negatively charged TCH, and a rose-like outer layer with numerous pores to accommodate the adsorbates. RIHMB exhibits exceptional reusability, achieving over 92 % TCH removal efficiency after five cycles. Molecular dynamics simulations demonstrate that RIHMB not only adsorbs TCH with high efficiency but also facilitates its remarkably rapid release (NaCl as desorbent). This outcome is attributed to the porous structure of Ni/Al-LDHs, which traps TCH and acts as a physical barrier, preventing direct interaction with –R<sub>4</sub>N<sup>+</sup>. Then, chloride ions in the desorbent neutralize the positive charge of RIHMB, reduces its adsorption affinity for TCH, and promotes rapid desorption. A novel Wen Li-Wei Wei adsorption mass transfer model is presented, which reveals the collective influence of liquid-film diffusion, pore mass transfer, and sorption onto active sites on adsorption mass transfer, providing valuable insights into the underlying mechanisms. Multiple quantum chemical theoretical calculations were integrated to quantify the contributions of charge interaction, hydrogen bonding, π-π interaction, and van der Waals force to adsorption. A scale-up experiment conducted on a real water system offers a promising strategy for the remediation of environments contaminated with antibiotics.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"136 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143191932","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}
{"title":"Harnessing solar energy by a self-driven photoelectrocatalytic system for versatile water purification: Radionuclides, organic pollutants and pathogen removal","authors":"Sixuan Cai , Fatemeh Sadat Mostafavi , Qingyan Zhang , Shuaifei Zhao , Junwen Lv , Qingyi Zeng","doi":"10.1016/j.seppur.2025.131992","DOIUrl":"10.1016/j.seppur.2025.131992","url":null,"abstract":"<div><div>Water purification technology that can simultaneously remove uranium, degrade organic pollutants, and inactivate pathogenic bacteria is crucial for protecting human health and the environment. In this study, we developed a self-driven photoelectrocatalytic (PEC) system using a sulfamic acid-modified carbon felt (CF/SA) cathode and a TiO<sub>2</sub> nanorod photoanode, both of which were obtained by hydrothermal methods. The system demonstrated excellent water purification performance in complex aqueous environments under sunlight illumination. The CF/SA cathode enabled improved interfacial charge transfer and more surface binding sites for uranium (UO<sub>2</sub><sup>2+</sup>) adsorption and reduction. In the presence of both UO<sub>2</sub><sup>2+</sup> and sulfamethoxazole, almost 100 % UO<sub>2</sub><sup>2+</sup> was removed within 30 min, and 98.98 % sulfamethoxazole was degraded within 1.5 h. The self-driven PEC system also demonstrated effective antibacterial properties by completely inactivating <em>E. coli</em> within 25 min. Variations in wastewater characteristics, such as ions, pH, and organic concentrations had minimal impacts on the stability of the system. It also functioned well under real sunlight and exhibited excellent stability in long-term operation. This work demonstrated an effective cathode material to enhance the uranium reduction and antibiotics decomposition in a self-driven PEC system and provided a new solution for inactivating aqueous pathogens using sunlight only.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131992"},"PeriodicalIF":8.1,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Citric acid-induced defective MIL-53(Fe/Ce) for efficient amoxicillin degradation in electro-Fenton system","authors":"Hui Zhao, Tong Zhu, Zhirong Sun","doi":"10.1016/j.seppur.2025.131993","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131993","url":null,"abstract":"Metal-organic frameworks (MOFs) are widely used in electro-Fenton systems due to their large surface areas and superior conductivities. However, conventional MOFs with regular structures often suffer from limited active sites on their surfaces, constraining their catalytic performances. To address this limitation, through the competitive action of citric acid and 2-aminoterephthalic acid on graphite felt (GF), a novel defect-engineered MIL-53 framework (D-MIL-53(Fe/Ce)/400@GF) was synthesized. We successfully prepared D-MIL-53(Fe/Ce) powder by adding a small amount of citric acid during the solvothermal synthesis of MIL-53(Fe/Ce). After calcination under N<sub>2</sub> environment, the material was loaded onto GF via drip coating, resulting in the final preparation of D-MIL-53(Fe/Ce)/400@GF. This process introduced defect structures into MIL-53, significantly enhancing its catalytic properties. Raman spectroscopy confirmed a substantial increase in surface defects, with the <em>I</em><sub>D</sub>/<em>I</em><sub>G</sub> ratio rising from 0.68 (MIL-53(Fe/Ce)/400@GF) to 1.99 (D-MIL-53(Fe/Ce)/400@GF). In electro-Fenton system, H<sub>2</sub>O<sub>2</sub> generation by D-MIL-53(Fe/Ce)/400@GF was 2.02-fold greater than that of MIL-53(Fe/Ce)/400@GF. More importantly, the degradation of amoxicillin pollutant by D-MIL-53(Fe/Ce)/400@GF catalyst resulted in a 2.78-fold increased reaction rate when compared to MIL-53(Fe/Ce)/400@GF. Therefore, active sites provided by defect structures could effectively enhance cathodic catalytic performance. A degradation pathway of amoxicillin was proposed based on high-performance liquid chromatography-mass spectrometry combined with density functional theory results, demonstrating significantly reduced toxicity of degradation products. Overall, the proposed defective MOF composites have great potential for use in electro-Fenton technology for antibiotics and other pollutants decontamination.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"16 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258008","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}
{"title":"The mechanism and influential factors for radioactive iodide adsorption: A review","authors":"Chenhui Yan, Bowen Zhang, Yansong Liu, Zhibing He","doi":"10.1016/j.seppur.2025.131954","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131954","url":null,"abstract":"Radioactive iodide (I<sup>-</sup>) in the liquid phases poses a serious threat to the environment and human health. Fortunately, the adsorption method has been extensively studied as an effective technical. This review focuses on the removal mechanisms involved in adsorbing I<sup>-</sup>, including metal-based reactions, electrostatic interaction, anion exchange, coordination, redox reactions, and extraction methods. It briefly discusses the influence of environmental factors such as I<sup>-</sup> concentration, pH, coexisting anions, etc., and their impacts on the adsorbent and I<sup>-</sup>. Finally, it is hoped that this review can provide valuable references for designing new and effective materials for removing I<sup>-</sup> from aqueous media.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"61 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124904","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}
{"title":"Boosting CO2 electroreduction to C2H4: Optimizing the local catalytic microenvironment with hydrophobic SiO2 Aerosol-Enhanced Cu-N4 catalysts","authors":"Zihan Zhang, Jiaqi Yu, Liguo Wei, Lishuang Zhao","doi":"10.1016/j.seppur.2025.131977","DOIUrl":"10.1016/j.seppur.2025.131977","url":null,"abstract":"<div><div>The electrocatalytic reduction of CO<sub>2</sub> into high-value-added feedstocks represents a promising strategy for electrical energy storage and carbon cycling. However, achieving high activity and selectivity for multi-carbon (C<sub>2+</sub>) products on copper-based electrocatalysts remains challenging due to the slow diffusion of CO<sub>2</sub> in solution and the highly competitive hydrogen evolution reaction. In this study, hydrophobic nano-SiO<sub>2</sub> aerosol was used to modify Cu–N coordinated compounds. This modification, combined with an in-situ electrochemical reconstruction method, resulted in the preparation of highly active and hydrophobic Cu-N<sub>4</sub> coordination catalysts, denoted as Act-Si-n-Cu-N<sub>4</sub> (n = 0 ∼ 4). The catalytic microenvironment of the electrocatalyst was regulated to enhance the Faradaic Efficiency (FE) of C<sub>2</sub>H<sub>4</sub> product while reducing the FE of H<sub>2</sub>. Various characterization techniques were employed to analyze the morphology and structure of the catalysts. Systematic CO<sub>2</sub> reduction performance experiments were conducted to investigate the effects of SiO<sub>2</sub> addition amount and applied potential on product distribution. The results demonstrated that the FE<sub>C2H4</sub> of Act-Si-2-Cu-N<sub>4</sub> reached up to 41.94 ± 1.70 % at −1.4 V vs. RHE, which is 1.34 times higher than that of unmodified Act-PHI-Cu-N<sub>4</sub> without microenvironmental regulation. The study revealed that hydrophobic modification significantly improves the reactivity and selectivity of electrocatalysts to C<sub>2</sub>H<sub>4</sub> product in the process of CO<sub>2</sub> reduction by changing the local microenvironment around the electrocatalyst. This work provides valuable insights into enhancing the C–C coupling process in the electrocatalytic reduction of CO<sub>2</sub> and offers a new perspective for designing high-performance electrocatalysts.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131977"},"PeriodicalIF":8.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143191933","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}
{"title":"Enhanced antibiotic removal via magnetic Ni@ZIF-8 composite nanotubes: Synergistic adsorption, facile recovery and adsorption mechanism","authors":"Chuanqi Zhang, Xiaomei Cheng, Ruirui Zhao, Mengxian Fu, Meifang Wang, Zhiming Chen, Changfang Zhang, Xiangzi Li","doi":"10.1016/j.seppur.2025.131988","DOIUrl":"https://doi.org/10.1016/j.seppur.2025.131988","url":null,"abstract":"The integration of metal–organic framework (MOF) materials with magnetic cores not only serves as an effective adsorbent but also facilitates the recovery post-adsorption. In this study, we synthesized Ni@ZIF-8 composite nanotubes by introducing ZIF-8 onto the surface of Ni nanotubes, which were used as adsorbents for antibiotic removal. The Ni@ZIF-8 composite nanotubes exhibited high-efficiency and recyclable antibiotic adsorption, with the maximum adsorption capacities for TC and CFX reaching 770.2 and 428.2 mg·g<sup>−1</sup>, respectively. The Ni nanotubes, acting as magnetic cores, facilitated magnetic recovery after adsorption. Furthermore, the introduction of ZIF-8 not only increased the surface roughness of the composite but also incorporated a significant number of functional groups. The pseudo-second-order model, Langmuir model and intra-particle diffusion models provided better fits to the isotherm and kinetic data of the two antibiotics. Density functional theory (DFT) calculations results indicate that the π-π interactions dominate the adsorption process of both tetracycline and cefixime onto ZIF-8. And the electrostatic potential (ESP) calculations and interaction analysis indicate that the Ni atom enhances the adsorption behavior through π-π interactions between the benzene ring or carbonyl group of both tetracycline and cefixime, and the imidazole of ZIF-8. This research offers a novel approach for the removal of antibiotics from contaminated water and environmental remediation using magnetic core-MOF composite materials.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"1 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143191936","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}
Ziping Wang , Qianhui Ma , Xuekairui Shen , Xiaowen Sun , Xiaofeng Li , Guofu Li , Di Chen , Qiang Li , Xun Yuan , Yong Liu
{"title":"Space-mediated confinement engineering of NaTi2(PO4)3 inside hollow carbon nanofibers via coaxial electrospinning: Enabling ultra-robust and highly-efficient faradic capacitive deionization","authors":"Ziping Wang , Qianhui Ma , Xuekairui Shen , Xiaowen Sun , Xiaofeng Li , Guofu Li , Di Chen , Qiang Li , Xun Yuan , Yong Liu","doi":"10.1016/j.seppur.2025.131978","DOIUrl":"10.1016/j.seppur.2025.131978","url":null,"abstract":"<div><div>NASICON-structured NaTi<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (NTP) has emerged as a promising cathode material for faradaic capacitive deionization (FDI) in desalination, owing to its high theoretical sodium storage capacity. However, its practical application is limited by poor conductivity and significant volume expansion, leading to slow desalination rates and rapid performance degradation. Previous efforts to anchor NTP onto carbon substrates have improved conductivity, but at the expense of reducing the availability of electrochemically active sites and causing irreversible damage to the carbon matrix during Na-ion intercalation and de-intercalation. To address these issues, we propose a space-mediated confinement strategy, incorporating NTP into hollow core–shell carbon nanofibers (<em>ch</em>-NTP@CNFs). This approach combines a buffered protective scaffold with a continuous electron-conductive network, mitigating structural degradation and conductivity limitations. The resulting <em>ch</em>-NTP@CNFs-based FDI system demonstrates significantly enhanced desalination kinetics (0.652 mg g<sup>−1</sup> s<sup>−1</sup>) and outstanding long-term stability, with only a 6.2 % capacity reduction over 200 cycles. These findings surpass the performance of most CDI systems reported to date. This study underscores the potential of space-mediated confinement and hollow core–shell designs in improving desalination kinetics and durability, advancing FDI anode development for sustainable water desalination technologies.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131978"},"PeriodicalIF":8.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124902","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}
Yinpeng Lu , Liangqing Hu , Yanming Guo , Minghao Zhao , Weichi Zhou , Yijin Ma , Haichao Wang , Zhidong Wen , Fuqiu Ma , Jing Feng
{"title":"The crucial roles of oxygen vacancies and homojunction in boosting the electrochemical nitrogen reduction of La-doping RGO/W18O49@WO3","authors":"Yinpeng Lu , Liangqing Hu , Yanming Guo , Minghao Zhao , Weichi Zhou , Yijin Ma , Haichao Wang , Zhidong Wen , Fuqiu Ma , Jing Feng","doi":"10.1016/j.seppur.2025.131938","DOIUrl":"10.1016/j.seppur.2025.131938","url":null,"abstract":"<div><div>The nitrogen reduction reaction (NRR) presents significant challenges due to the difficulty of adsorbing and activating nitrogen (N<sub>2</sub>) under mild conditions. In this work, reduced graphene oxide (RGO)/La-doped W<sub>18</sub>O<sub>49</sub>@WO<sub>3</sub> homojunction was synthesized using a one-pot solvothermal method as an efficient NRR catalyst. Notably, La-doping facilitated the in-situ formation of WO<sub>3</sub> within W<sub>18</sub>O<sub>49</sub>, while the incorporation of RGO introduced oxygen vacancies. The resulting RGO/La20-W<sub>18</sub>O<sub>49</sub>@WO<sub>3</sub> composite achieved an NH<sub>3</sub> yield rate of 21.9 μg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> and a Faradaic efficiency (FE) of 8.3%. The homojunction W<sub>18</sub>O<sub>49</sub>@WO<sub>3</sub> effectively enhance N<sub>2</sub> activation, oxygen vacancies promote N<sub>2</sub> adsorption, and RGO further accelerate the reaction kinetics of the NRR. This gave rise to the tandem process of N<sub>2</sub> adsorption, N<sub>2</sub> activation and N<sub>2</sub> reduction. Therefore, the synergistic effect of the homojunction W<sub>18</sub>O<sub>49</sub>@WO<sub>3</sub>, oxygen vacancies, and RGO improved the performance of RGO/La20-W<sub>18</sub>O<sub>49</sub>@WO<sub>3</sub>. This work developed an efficient and low-cost NRR catalyst, offering valuable insights into the design of W<sub>18</sub>O<sub>49</sub>-based catalysts and homojunction structures.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"362 ","pages":"Article 131938"},"PeriodicalIF":8.1,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143191938","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}