Fangshu Qu , Zhuoran Yi , Qiaoyun Lai , Zhu Xiong , Chengwei Nie , Huarong Yu , Gaosheng Zhang , Shuaifei Zhao
{"title":"炭黑诱导氟化使膜蒸馏对垃圾填埋场渗滤液处理稳健","authors":"Fangshu Qu , Zhuoran Yi , Qiaoyun Lai , Zhu Xiong , Chengwei Nie , Huarong Yu , Gaosheng Zhang , Shuaifei Zhao","doi":"10.1016/j.watres.2025.124121","DOIUrl":null,"url":null,"abstract":"<div><div>Membrane wetting and fouling pose significant challenges for membrane distillation (MD), particularly in hypersaline wastewater treatment. To address these issues, a robust low-surface-energy polyvinylidene fluoride (PVDF)-based membrane was developed through carbon black-induced fluorination with 1H,1H,2H,2H-perfluorodecyltrichlorosilane (FDTS). Carbon black nanoparticles were deposited on a pristine PVDF membrane via vacuum filtration, forming loosely packed structures that served as anchoring sites for FDTS grafting. FDTS fluorination introduced -CF<sub>3</sub>/-CF<sub>2</sub> functional groups and Si-O-Si networks. It not only reduced the surface energy to 2.03 mN/m and decreased the pore size to 0.41 μm, but also significantly enhanced the membrane surface hydrophobicity (water contact angle 144°). Compared with the pristine PVDF and carbon black deposited PVDF membranes, the membrane modified by carbon black-induced fluorination exhibited superior water vapor transmission (6.05 × 10⁻⁶ m³/m²·Pa·s) and antiwetting properties due to its ultralow surface energy and robust air barrier. In MD desalination, the surface fluorinated PVDF membrane demonstrated stable fluxes exceeding 7.0 L/m²·h and almost 100 % rejection performance even when treating highly concentrated solutions (5.5 wt. % NaCl) or organic-polluted solutions. This performance remarkably outperformed the pristine PVDF membrane (flux decline >80 %) and carbon black deposited PVDF membrane (severe wetting). The surface fluorinated PVDF membrane also showed exceptional durability in treating real landfill leachate, maintaining fluxes above 6 L/m²·h over 72 h with minimal salt or organic leakage. Mechanistic investigations revealed that the carbon black-FDTS hybrid layer reinforced the air barrier, effectively mitigating foulant-membrane interactions and preventing pore wetting. This study presents a scalable and practical strategy for engineering antiwetting MD membranes, facilitating the reclamation of hypersaline and complex wastewaters.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"285 ","pages":"Article 124121"},"PeriodicalIF":12.4000,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Carbon black induced fluorination enables robust membrane distillation for landfill leachate treatment\",\"authors\":\"Fangshu Qu , Zhuoran Yi , Qiaoyun Lai , Zhu Xiong , Chengwei Nie , Huarong Yu , Gaosheng Zhang , Shuaifei Zhao\",\"doi\":\"10.1016/j.watres.2025.124121\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Membrane wetting and fouling pose significant challenges for membrane distillation (MD), particularly in hypersaline wastewater treatment. To address these issues, a robust low-surface-energy polyvinylidene fluoride (PVDF)-based membrane was developed through carbon black-induced fluorination with 1H,1H,2H,2H-perfluorodecyltrichlorosilane (FDTS). Carbon black nanoparticles were deposited on a pristine PVDF membrane via vacuum filtration, forming loosely packed structures that served as anchoring sites for FDTS grafting. FDTS fluorination introduced -CF<sub>3</sub>/-CF<sub>2</sub> functional groups and Si-O-Si networks. It not only reduced the surface energy to 2.03 mN/m and decreased the pore size to 0.41 μm, but also significantly enhanced the membrane surface hydrophobicity (water contact angle 144°). Compared with the pristine PVDF and carbon black deposited PVDF membranes, the membrane modified by carbon black-induced fluorination exhibited superior water vapor transmission (6.05 × 10⁻⁶ m³/m²·Pa·s) and antiwetting properties due to its ultralow surface energy and robust air barrier. In MD desalination, the surface fluorinated PVDF membrane demonstrated stable fluxes exceeding 7.0 L/m²·h and almost 100 % rejection performance even when treating highly concentrated solutions (5.5 wt. % NaCl) or organic-polluted solutions. This performance remarkably outperformed the pristine PVDF membrane (flux decline >80 %) and carbon black deposited PVDF membrane (severe wetting). The surface fluorinated PVDF membrane also showed exceptional durability in treating real landfill leachate, maintaining fluxes above 6 L/m²·h over 72 h with minimal salt or organic leakage. Mechanistic investigations revealed that the carbon black-FDTS hybrid layer reinforced the air barrier, effectively mitigating foulant-membrane interactions and preventing pore wetting. This study presents a scalable and practical strategy for engineering antiwetting MD membranes, facilitating the reclamation of hypersaline and complex wastewaters.</div></div>\",\"PeriodicalId\":443,\"journal\":{\"name\":\"Water Research\",\"volume\":\"285 \",\"pages\":\"Article 124121\"},\"PeriodicalIF\":12.4000,\"publicationDate\":\"2025-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Water Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0043135425010280\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0043135425010280","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Carbon black induced fluorination enables robust membrane distillation for landfill leachate treatment
Membrane wetting and fouling pose significant challenges for membrane distillation (MD), particularly in hypersaline wastewater treatment. To address these issues, a robust low-surface-energy polyvinylidene fluoride (PVDF)-based membrane was developed through carbon black-induced fluorination with 1H,1H,2H,2H-perfluorodecyltrichlorosilane (FDTS). Carbon black nanoparticles were deposited on a pristine PVDF membrane via vacuum filtration, forming loosely packed structures that served as anchoring sites for FDTS grafting. FDTS fluorination introduced -CF3/-CF2 functional groups and Si-O-Si networks. It not only reduced the surface energy to 2.03 mN/m and decreased the pore size to 0.41 μm, but also significantly enhanced the membrane surface hydrophobicity (water contact angle 144°). Compared with the pristine PVDF and carbon black deposited PVDF membranes, the membrane modified by carbon black-induced fluorination exhibited superior water vapor transmission (6.05 × 10⁻⁶ m³/m²·Pa·s) and antiwetting properties due to its ultralow surface energy and robust air barrier. In MD desalination, the surface fluorinated PVDF membrane demonstrated stable fluxes exceeding 7.0 L/m²·h and almost 100 % rejection performance even when treating highly concentrated solutions (5.5 wt. % NaCl) or organic-polluted solutions. This performance remarkably outperformed the pristine PVDF membrane (flux decline >80 %) and carbon black deposited PVDF membrane (severe wetting). The surface fluorinated PVDF membrane also showed exceptional durability in treating real landfill leachate, maintaining fluxes above 6 L/m²·h over 72 h with minimal salt or organic leakage. Mechanistic investigations revealed that the carbon black-FDTS hybrid layer reinforced the air barrier, effectively mitigating foulant-membrane interactions and preventing pore wetting. This study presents a scalable and practical strategy for engineering antiwetting MD membranes, facilitating the reclamation of hypersaline and complex wastewaters.
期刊介绍:
Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include:
•Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management;
•Urban hydrology including sewer systems, stormwater management, and green infrastructure;
•Drinking water treatment and distribution;
•Potable and non-potable water reuse;
•Sanitation, public health, and risk assessment;
•Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions;
•Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment;
•Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution;
•Environmental restoration, linked to surface water, groundwater and groundwater remediation;
•Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts;
•Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle;
•Socio-economic, policy, and regulations studies.