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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Revealing the internal β-phase PVDF membrane fouling tendency using double layer piezoelectrics

Qian Wang,Juan Li,Qiuyueming Zhou,Ting He,Zhaoliang Cui,Young Moo Lee,Weihong Xing

Dissolved organic matter (DOM) is recognized as a crucial factor contributing to the irreversible fouling of ultrafiltration membranes. Quartz crystal microbalance with dissipation (QCM-D) offers insights into the kinetics of fouling layer formation and its structure in-situ on a model membrane. However, a clear correlation between the membrane fouling process and the adsorption-desorption results obtained from QCM-D has yet to be established. In this study, piezoelectric β-phase PVDF membranes were prepared, and their fouling behavior in response to three model compounds (humic acid (HA), dextran (DEX), bovine serum albumin (BSA), and their mixed solutions was examined. It was firstly proposed that the spin-coated model PVDF membrane surface exhibited a typical β-phase structure, characterized by regular undulations resulting from strong stretching effects. A novel double layer piezoelectric sensor, consisting of a β-phase layer over a piezoelectric quartz substrate, was designed for QCM-D analysis to assess the mass and stiffness variations of the absorbed DOM layer. The fouling tendency followed the order of BSA > Mixture > DEX > HA, with the foulant monomeric units having a similar molecular mass of around tens of kDa. Irreversible fouling resistance in series model as well as frequency drop in QCM-D were listed as indicators of irreversible fouling caused by foulant-membrane interaction, which realized a well-defined match for the first time.

CAS / MDL: 127-19-5 674282-83-8
研究领域: 膜科学 · 环境工程 · 材料科学 · 分析化学
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JOURNAL OF HAZARDOUS MATERIALS · 2025 · IF 11.3

Trade-off between arsenic and straw-derived DOM immobilization in their co-sorption on γ-Al2O3: Implications for arsenic mobility and carbon sequestration in farmlands

Qiuyu Chen,Yongyi Zhang,Haiwang Liu,Peng Liu,Xinxin Ye,Xing Xia,Xiangwei Wu

Straw-derived dissolved organic matter (DOM) is widespread in farmland soils, but the relationship between straw-derived DOM and As in their co-sorption on minerals and the underlying mechanisms remain unclear. Here, batch experiments and spectroscopic analyses were employed to investigate the co-sorption of straw-derived DOM and As(III/V) on γ-Al 2 O 3 . Results showed a trade-off between the As(III/V) and DOM immobilization on γ-Al 2 O 3 under different pH levels, which was caused by competitive sorption. The rape straw-derived DOM (DOM_Ra) exhibited a stronger inhibition on As(III/V) sorption than rice straw-derived DOM (DOM_Ri). This could be due to more aromatic fractions in the DOM_Ra and DOM_Ri, which were preferentially sorbed by γ-Al 2 O 3 . In turn, the preferential sorption of aromatic DOM components was weakened by As(V) sorption, which, however, was not found in As(III) and DOM co-sorption. Furthermore, spectral results indicated that carboxylic groups on the sorbed DOM could provide additional binding sites for As(III/V) to form ternary complexes, but its role was overwhelmed by the DOM competitive sorption, which ultimately exhibited the inhibitory effect of DOM on As(III/V) sorption. These findings enhance the fundamental understanding of the co-sorption of As(III/V) and DOM on soil minerals and contribute to predicting As mobility and OM stability in As-contaminated farmlands with straw return.

CAS / MDL: 1344-28-1
研究领域: 环境科学 · 土壤化学 · 农业生态学
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WATER RESEARCH · 2025 · IF 12.4

Integrating dual-stage gas permeable membranes and humic acid recovery to optimize fenton oxidation of landfill leachate: Insights into full-process performance and DOM molecular-level transformation

Linjun Wu,Huan Li,Yanyue Gu,Zhiqiang Shen,Yuexi Zhou,Jiane Zuo

This research introduces an innovative full-process treatment technology that integrates dual-stage gas permeable membranes (GPM) and humic acid (HA) recovery to enhance Fenton oxidation of landfill leachate (LFL). In terms of full-process performance, this integrated approach (LFL-GPM-HA (Fenton)) synergistically combines LFL concentration, ammonia recovery, HA recovery, purified water reclamation, and efficient Fenton oxidation, thereby achieving holistic minimization, detoxification, and resource recovery of LFL. Specifically, under the conditions of low-intensity aeration and a temperature gradient of 65–55–25 °C, the GPM achieved an ammonia recovery rate exceeding 96 %, while the LFL was concentrated by a factor of 4.72 within 12 h. During HA recovery at pH 2, the HA yield from the concentrated LFL reached 3.68 g/L, representing an 88.72 % increase compared to the raw LFL. Due to the significant consumption of bicarbonate alkalinity during the GPM process, the required dosage of H₂SO₄ per gram of HA recovered was reduced by 86.72 %. Under different dimensionless oxidant dosages, the LFL-GPM-HA (Fenton) demonstrated a significant improvement in COD removal efficiency compared to standalone Fenton oxidation. In terms of dissolved organic matter (DOM) molecular-level transformation, ESI FT-ICR-MS analysis showed a significant enhancement in the removal of CHOS and CHONS in LFL-GPM-HA (Fenton), with a concurrent reduction in the produced sulfurous byproducts. Additionally, the LFL-GPM-HA (Fenton) notably increased the frequency of decarboxylation, desulfurization, and dealkylation reactions. In terms of operational stability and economic feasibility, this integrated system demonstrates excellent long-term stability and robust membrane fouling-cleaning recovery properties, achieving LFL treatment at a cost of approximately 12.142 $/m³, which is significantly more cost-effective than conventional full-process advanced treatment technologies (20–30 $/m³). In conclusion, the findings offer a pathway for developing more efficient and cost-effective strategies for LFL management.

研究领域: 环境科学 · 废水处理 · 分子生物学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Molecular insight into DOM fate using EEM-PARAFAC and FT-ICR MS and concomitant heavy metal behaviors in biologically treated landfill leachate during coagulation: Al speciation dependence

Libing Liu,Lei Du,Sen Lu,Bo Yang,Xu Zhao,Deli Wu,Xunchang Fei,Hongping He,Dongsheng Wang

Various combined processes with pre-coagulation have been developed for biologically treated landfill leachate , but the microscopic-level processes occurring during coagulation remain largely unknown. Herein, dissolved organic matter (DOM) fate using fluorescence excitation emission matrix spectroscopy combined with parallel factor analysis and electrospray ionization coupled Fourier transform-ion cyclotron resonance mass spectrometry and concomitant heavy metal (HM) behaviors were explored at the molecular level. In addition, AlCl 3 and two polyaluminum chloride (PACl) species (dominated by [AlO 4 Al 12 (OH) 24 (H 2 O) 12 ] 7+ and [(AlO 4 ) 2 Al 28 (OH) 56 (H 2 O) 26 ] 18+ , respectively) were used. The results show that all coagulants are efficient at removing DOM. PACl was found to be advantageous over AlCl 3 in overcoming pH fluctuation, which is ascribed to the different dominant mechanisms, namely, entrapment and sweep flocculation for AlCl 3 and charge neutralization for PACl. Consequently, PACl was more effective at removing humic substances , usually high-molecular-weight, oxygen-rich and unsaturated, than protein substances. For HM removal, PACl was likewise better and more stable, where As, Cu, Ni, Co and Hg were removed predominantly via adsorption, and Cr, Zn, Pb, Cd and Mn were removed via coprecipitation . Correlation analysis showed that humic substances tended to complex with HMs and be removed synergistically due to the ubiquitous occurrences of aromatic structures and oxygen-containing functional groups.

研究领域: 环境科学 · 分析化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Unraveling Potential Causative Components for the Deleterious Effect of Atmospheric Fine Particulate Matter on Red Blood Cells

Yuzhu Zhang,Laijin Zhong,Jing Zhan,Zhipeng Yin,Yao Pei,Dong Cao,Qian S. Liu,Qunfang Zhou,Qian Liu,Guibin Jiang

Atmospheric fine particulate matter (PM2.5) poses threats to the cardiovascular system. Red blood cells (RBCs) are the most abundant cells in blood, which are actively involved in multiple hematological diseases, such as blood clot formation and thrombosis. Exploring how PM2.5 with spatiotemporal heterogeneity influences the hematological system by targeting RBCs would help gain insights into the deleterious effects of PM2.5 and provide clues for finding the causative components therein. Herein, the PM2.5 samples collected from 3 urban sites in Beijing (i.e., Chaoyang, Shunyi, and Yanqing districts) during 4 seasons of 2022 were studied for their toxicities to mouse RBCs, and the main contributing components were further explored through chemical analysis and correlation measure. The results showed that exposure to PM2.5 samples decreased adenosine triphosphate (ATP) levels and increased phosphatidylserine (PS) externalization of RBCs, causing cell morphological deformity. The Pearson correlation analysis showed that the aromaticity of the dissolved organic matter (DOM) in PM2.5 samples was positively correlated with PS exposure of RBCs, showing that the lignin-like compounds were the potential contributors. The negative correlation of zeta potentials of PM2.5 samples with PS exposure of RBCs showed the particle-derived bioactivities of this airborne pollutant. The simulative test based on artificial nanomaterials of carbon black (CB) and oxidized CB (OCB) confirmed the crucial role of particulate carbon in PM2.5-induced effects on RBCs, and soot with a certain oxidation degree was, thus, recognized as another contributor, given its ubiquitous existence in PM2.5 samples. This study, for the first time, revealed PM2.5-induced PS exposure of RBCs, and the causative components of DOM and soot were unraveled. Considering the inevitable contact of airborne PM2.5 with RBCs in the blood circulatory system, the findings obtained herein would help bridge the gap between PM2.5 exposure and the risk of cardiovascular diseases, like thrombogenesis.

CAS / MDL: 56092-81-0
研究领域: 环境科学 · 毒理学 · 血液学 · 心血管疾病 · 空气污染
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Rational design of anti-interference Fe/Co MOF-coupled PMS process for As(III) removal in DOM-rich groundwater: 1O2-dominated As(III) oxidation and chemisorption of As(V)

Ying Fang,Qianwen Liu,Yang Song,Feiyue Jia,Ying Yang,Haipu Li

Dissolved organic matter (DOM) extensively exists in high-arsenic groundwater with relatively high concentration, which could not only compete with arsenic for adsorption sites, but also depress As(III) oxidation in persulfate-based advanced processes (PS-AOPs) through scavenging free radicals (SO 4 • − and •OH). In order to effectively avoid the negative effect of DOM , an Fe/Co bimetallic metal–organic framework (Fe/Co MOF)-coupled peroxymonosulfate (Fe/Co MOF-PMS) system was rationally constructed for non-radical-dominated As(III) oxidation and chemisorption-driven As(V) adsorption. Results showed that the Fe/Co MOF-PMS system did realize anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater, which was evidenced by no difference in As(III) immobilization efficiencies in the absence and presence of 20 mg/L humic acid (HA). During the oxidation process, 1 O 2 dominated As(III) oxidation while O 2 • − dominated HA oxidation, and the presence of HA significantly promoted the generation of 1 O 2 besides SO 4 • − and •OH. During the adsorption process, chemical adsorption mainly drove As(V) adsorption such as forming M-O-As (M = Fe, Co) bond, while physical adsorption forces played a major role in HA adsorption, such as π-π interaction, hydrogen bonding, and electrostatic attraction. The synergism of oxidation and adsorption processes made the anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater in Fe/Co MOF-PMS system come true. This work is believed to shed light on the highly efficient purification of DOM-rich high-arsenic groundwater.

研究领域: 环境科学 · 化学工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Enhancement of thioethers removal by pre-oxidation-coagulation: Effects of background organic matter

Mengze Geng,Xin Huang,Baoyou Shi,Jianwei Yu,Chunmiao Wang,Yuning Du,Yili Wang

Swampy/septic odor caused by thioethers has become the main taste and odor (T&O) problem in drinking water of China. Improving its removal performance by commonly traditional water treatment process is significant. In our study, we have found that pre-oxidation could modify the background dissolved organic matter (DOM) properties and thus improve the coagulation performance of thioethers , increasing the coagulation removal rates by 1.5–3 times. Particularly, after pre-ozonation only protein-like substances remained, and thioethers removal was 1.5 times higher than that after pre-chlorination (only coagulation not including oxidation). Compared with humic acid (HA), the thioethers compounds removal efficiencies under bovine serum albumin (BSA) as background DOM was increased by 0.3–3 times. Through Freundlich model analysis, the binding strength of BSA (K F = 20.712, at 298 K) to dimethyl disulfide (DMDS) was enhanced by 60 % compared to HA (K F = 12.778, at 298 K). According to thermodynamic parameters, the binding effect between HA/BSA and thioethers compounds was mainly van der Waals forces and hydrogen bond . BSA with more amino structure and oxygen groups was more easily to adsorb DMDS through hydrogen bond and thus achieved better coagulation performance. Therefore, pre-ozonation combined with coagulation was suggested to be more suitable for thioethers compounds control.

研究领域: 环境科学 · 水处理 · 化学工程
✓ 已验证 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Efficient removal of levofloxacin by iron (II) phthalocyanine/g-C3N4 activated peroxymonosulfate under high salinity conditions: Role of high-valent iron-oxo species

Yanbin Wang,Zezhou Shi,Haibo Shen,Qiushuang Xing,Yunqing Pi

Efficient and selective removal of organic contaminants using traditional radical-dominated Advanced Oxidation Processes (AOPs) in complex environmental matrices is challenging, especially under high salinity conditions. This study proposes an alternative approach using iron (II) phthalocyanine-supported g-C 3 N 4 composite (FePc/CN) as a peroxymonosulfate (PMS) activator to efficiently remove organic contaminants. The FePc/CN-PMS process was selective towards the elimination of various organic contaminants, and those compounds with lower ionization potential value can be effectively degraded after reaction for 10 min. Results from radical quenching experiments, electron spin resonance (ESR), and PMSO chemical probe indicated that the dominant active species in the FePc/CN-PMS process are high-valent iron-oxo species (Fe IV O 2+ ), rather than the long-recognized SO 4 •− and •OH radical. A total of 22 intermediate products resulting from the degradation of levofloxacin (LVF) were identified by LC-MS. Additionally, two degradation pathways of LVF were proposed, with the piperazine ring of LVF being the primary site of degradation. The 5%FePc/CN-PMS system demonstrates resistance to ubiquitous inorganic anions and dissolved organic matter (DOM) in an aquatic environment, enabling efficient removal of (LVF) even under high salinity conditions. Furthermore, the 5%FePc/CN catalyst exhibits good chemical stability and reusability, making it a viable option for practical water remediation.

研究领域: 环境科学 · 化学 · 水处理 · 材料科学
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