PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Jun Ma,Yuanyuan Wang,Hang Xu,Mingmei Ding,Li Gao
Per- and polyfluoroalkyl substances (PFAS) are a class of ‘forever chemicals’ that have become a global concern owing to their innate chemical stability on humans and water resources. The separation of PFAS from water resources via membrane technologies are facing huge challenge. High permeance and rejection membrane are required for PFAS. To achieve this goal, herein, we propose an MXene-reinforced interfacial polymerization of negatively charged polyamide (PA) membranes for high rejection of short-chain PFAS. The morphologies and chemical properties were systematically investigated for the fabricated membrane. Attributed to the hydrophilic of MXene , the permeance of MXene-PA membranes increased without sacrificing rejection. Density functional theory (DFT) calculations and various experiments elucidated in detail the underlying mechanism of the interactions between the membrane and PFAS. The enhanced electrostatic interaction and hydrogen bonding leaded to increased PFAS rejection and permeance. Therefore, the MXene-regulated PA membrane effectively solved the trade-off between the selectivity and permeability. This work shows that MXene-regulated interfacial polymerization techniques can be used to tailor the effectiveness of PA nanofiltration membranes to overcome the trade-off phenomenon and pave the way for solving the crisis of short-chain PFAS.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Journal of Environmental Sciences
·
2024
·
IF 5.9
Shi-Ya Peng,Ya-Di Yang,Rong Tian,Naihao Lu
A key characteristic to be elucidated, to address the harmful health risks of environmental perfluorinated alkyl substances (PFAS), is their binding modes to serum albumin, the most abundant protein in blood. Hexafluoropropylene oxide-dimer acid (GenX or HFPO-DA) is a new industrial replacement for the widespread linear long-chain PFAS. However, the detailed interaction of new-generation short-chain PFAS with albumin is still lacking. Herein, the binding characteristics of bovine serum albumin (BSA) to GenX were explored at the molecular and cellular levels. It was found that this branched short-chain GenX could bind to BSA with affinity lower than that of legacy linear long-chain perfluorooctanoic acid (PFOA). Site marker competitive study and molecular docking simulation revealed that GenX interacted with subdomain IIIA to form BSA-GenX complex. Consistent with its weaker affinity to albumin protein, the cytotoxicity of branched short-chain GenX was less susceptible to BSA binding compared with that of the linear long-chain PFOA. In contrast to the significant effects of strong BSA-PFOA interaction, the weak affinity of BSA-GenX binding did not influence the structure of protein and the cytotoxicity of GenX. The detailed characterization and direct comparisons of serum albumin interaction with new generation short-chain GenX will provide a better understanding for the toxicological properties of this new alternative.
研究领域:
生物化学
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毒理学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
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IF 11.4
Yue Zhi,Xiaoqing Zhao,Ao Shuai,Yonghui Jia,Xinyi Cheng,Shihong Lin,Feng Xiao,Le Han,Hongxiang Chai,Qiang He,Caihong Liu
Nanofiltration (NF) effectively removes per- and polyfluoroalkyl substances (PFAS) from water but struggles with short-chain PFAS (i.e., those containing less than 6 perfluorinated carbons) due to size exclusion inefficiency. In this study, we developed layer-by-layer assembled NF membranes with PDADMAC/PSS terminal bilayers varying in chain lengths, hydrophilicity, and charge, and systematically assessed their removal of 16 representative PFAS species. The mechanisms between long-chain and short-chain PFAS were investigated and optimal strategies for enhancing PFAS selectivity were developed. Results demonstrated that the (PDADMAC/PSS) 3 membrane achieved the highest removal (86.1%-98.1%) for short-chain PFAS, including PFBA-PFHpA (C4-C6), PFBS (C4), PFMOPrA (C3), PFMOBA (C4), and GenX (C5), while effectively removing (>99.9%) long-chain counterparts (≥C7). As feed water pH increased from 3.5 to 9.0, average PFAS rejection rose from 16.6% to 32.0%, revealing more negative charged membrane surface endow stronger electrostatic repulsion, particularly for short-chain anionic PFAS. In addition, we also tested the PFAS removal efficacy of (PDADMAC/PSS) 3 membrane using real sewage plant effluent. Compared to the pristine membrane, the (PDADMAC/PSS) 3 membrane exhibited improved removal for most PFAS, with removal efficiencies ranging from 82.5% for PFOA to 96.7% for PFOS. The most significant improvements were observed in C4 compounds like PFBA and PFBS (increased by 6.0-11.5%). Our study suggests that PFAS removal efficiency by NF highly depends on size exclusion, with short-chain anionic PFAS more likely affected by electrostatic repulsion. Membrane surface manipulation can enhance selectivity, aiding in predicting NF treatment effectiveness for specific PFAS compounds.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 27
·e2219179120
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IF 11.1
Yuanji Shi,Hongxin Mu,Jiaqian You,Chenglong Han,Huazai Cheng,Jinfeng Wang,Haidong Hu,Hongqiang Ren
The global ecological crisis of perfluoroalkyl and polyfluoroalkyl substances (PFASs) in drinking water has gradually shifted from long-chain to short-chain PFASs; however, the widespread established PFAS adsorption technology cannot cope with the impact of such hydrophilic pollutants given the inherent defects of solid–liquid mass transfer. Herein, we describe a reagent-free and low-cost strategy to reduce the energy state of short-chain PFASs in hydrophobic nanopores by employing an in situ constructed confined water structure in activated carbon (AC). Through direct (driving force) and indirect (assisted slip) effects, the confined water introduced a dual-drive mode in the confined water–encapsulated activated carbon (CW-AC) and completely eliminated the mass transfer barrier (3.27 to 5.66 kcal/mol), which caused the CW-AC to exhibit the highest adsorption capacity for various short-chain PFASs (C-F number: 3-6) among parent AC and other adsorbents reported. Meanwhile, benefiting from the chain length– and functional group–dependent confined water–binding pattern, the affinity of the CW-AC surpassed the traditional hydrophobicity dominance and shifted toward hydrophilic short-chain PFASs that easily escaped treatment. Importantly, the ability of CW-AC functionality to directly transfer to existing adsorption devices was verified, which could treat 21,000 bed volumes of environment-related high-load (~350 ng/L short-chain PFAS each) real drinking water to below the World Health Organization’s standard. Overall, our results provide a green and cost-effective in situ upgrade scheme for existing adsorption devices to address the short-chain PFAS crisis.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
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IF 11.3
Hao Yu,Peng Zhang,Dongbao Song,Hao Chen,Peng Huang,Srđan D. Rončević,Hongwen Sun
The global concern of per- and polyfluoroalkyl substance (PFAS) contamination has gradually shifted from long- to ultrashort- and short-chain PFAS, but the widely used pyrogenic carbons (PCs) are almost ineffective at removing such hydrophilic pollutants. Herein, a polypyrrole (PPy) nanostructured coating strategy was proposed to modify PCs (PPy@P-BC) for rapid and efficient removal of ultrashort- and short-chain PFAS from water. Static batch tests revealed that the sorption rate constant and sorption capacity of PFAS (C2–C6) on PPy@P-BC are at least 38 times and 5 times greater than those on undecorated PCs and benchmark materials of granular activated carbon, respectively, and their sorption equilibrium time is within 300 s. The outstanding sorption performance of PPy@P-BC is maintained in dynamic column tests (>3120 bed volumes) and different types of real water contaminated by 36 PFAS, including 11 previously identified emerging PFAS (removal >95.3%). PPy@P-BC also exhibited excellent regeneration and reusability. The following dual-drive mechanisms for PFAS removal were identified based on experimental results and density functional theory (DFT) calculations: (i) electrostatic attraction between amino functional groups (especially −NH•+−) on the nanostructured PPy coating and anionic PFAS and (ii) pore filling facilitated by the well-preserved porous structure via construction of the nanostructured coating. Overall, these results provide a promising solution to address the ultrashort- and short-chain PFAS crisis.
研究领域:
环境科学
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水处理技术
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纳米技术
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吸附过程
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化学工程
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材料科学
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污染控制
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环境化学
✓ 已验证
DOI
PubMed
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Wei Chen,Mingxiang Liu,Mingmei Ding,Lei Zhang,Shibao Dai
Membrane separation technology has been favorably applied to acquire non-polluting permeate in conditions of contaminative aqueous environment . However, some emerging contaminants with critical impacts on human health and environmental safety such as poly- and perfluoroalkyl (PFAS) compounds composed of various molecular chains are frequently found in water treatment process steps. Especially, short-chain PFASs remain poorly understood in nanofiltration membrane. A thin-film composite membrane with a hyaluronic acid interlayer (TFCi) had been finely tailored to simultaneously gain ameliorative permeate and rejection. Experiments were performed on a small-scale installation to investigate the correlation between operating parameters and short-chain PFASs removal performances. Results showed effectual trace short-chain PFASs rejection during various pressure, temperature, pH, concentration and fouling conditions. Alginate fouling micelles increased PFAS retention and generated a rapid flux decline; nevertheless, the pollutant could be largely removed by washing. Furthermore, molecular dynamics simulations were utilized to reveal the mechanism of the trace short-chain PFASs rejection competence. The hyaluronic acid interlayer was able to suppress the diffusion rate toward the reaction boundary, facilitating the formation of fast water transport pores with good rejection performance for PFAS in polyamides . These results provide important insights into the mechanism of trace hydrophobic contaminants removal system and the interlayer design approach for efficient short-chain PFAS removal using nanofiltration membranes.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）