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Science Advances · 2021 ·Vol. 7 ·期 52 · IF 14.143

Instant interfacial self-assembly for homogeneous nanoparticle monolayer enabled conformal “lift-on” thin film technology

Liping Song,Ben Bin Xu,Qian Cheng,Xiaoyuan Wang,Xiaoning Luo,Xue Chen,Tao Chen,Youju Huang

Thin film fabrication is of great importance in modern engineering. Here, we propose a universal and conformal thin film technique enabled by the wetting empowered interfacial self-assembly. By tailoring the contact angle of nanoparticle (NP), a NP monolayer can be assembled instantly (within 5 seconds) with an excellent harvesting efficiency (up to 97.5 weight %). This self-assembly strategy presents a universal applicability on various materials, e.g., nonmetal, metal, and core-shell structures, and can achieve a monolayer with same in-plane area as a 95 cm2 wafer in a single process, indicating great potential for scale-up manufacturing. Through a template transfer, we coat the surface of different substrates (plastic, paper, etc.) with the assembled film in a conformal and nondestructive “lift-on” manner and subsequently demonstrate fluorescent micropatterns. This self-assembly strategy has great implications in advancing thin film technology in a user-friendly and cost-effective fashion for applications in anti-counterfeiting, actuators, and wearable/flexible electronics.

研究领域: 材料科学 · 纳米技术 · 表面工程
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WATER RESEARCH · 2018 · IF 7.051

In situ measurement of perfluoroalkyl substances in aquatic systems using diffusive gradients in thin-films technique

Dong-Xing Guan,Ya-Qing Li,Nan-Yang Yu,Guang-Hui Yu,Si Wei,Hao Zhang,William Davison,Xin-Yi Cui,Lena Q. Ma,Jun Luo

To better understand the environmental impact of ubiquitous perfluoroalkyl substances (PFASs) in waters, reliable and robust measurement techniques are needed. As one of the most widely used passive sampling approaches, diffusive gradients in thin-films (DGT) is not only easy to handle but also provides time-weighted analyte concentrations. Based on DGT with XAD18 as a binding agent, we developed a new methodology to measure two frequently detected PFASs in surface waters and wastewaters, i.e. perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS). Their diffusion coefficients in the diffusive gel, measured using an independent diffusion cell, were 4.37 × 10 −6 and 5.08 × 10 −6  cm 2  s −1 at 25 °C, respectively. DGT had a high capacity for PFOA and PFOS at 196 and 246 μg per gel disk, suggesting the DGT sampler was suitable for deployment of several weeks. Time-integrated concentrations of PFOA and PFOS in a natural lake and river, and a municipal wastewater treatment plant effluent using DGT samplers deployed in situ for 12–33 d were comparable to those measured by a solid-phase extraction method coupled with high-frequency grab sampling. This study demonstrates that DGT is an effective tool for in situ monitoring of PFASs in natural waters and wastewaters.

研究领域: 环境科学 · 分析化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Highly Thermally Conductive Flexible Biomimetic APTES-BNNS/BC Nanocomposite Paper by Sol–Gel-Film Technology

Baokang Yu,Zhouai Luo,Yuhang Zhou,Qi Zhang,Jianxin He,Jie Fan

Owing to the evolution of 5G technology, new energy vehicles, flexible electronics, miniaturization and integration of microelectronic devices, high-frequency and high-power devices, and thermal management of materials must consider additional limitations such as electrical insulation, excellent transverse heat transfer, flexibility, and weight. Boron nitride nanosheets (BNNSs) are ideal insulating materials with high thermal conductivity. However, the problem of the 3D thermal conductivity pathway and toughness strength of nanocomposite paper loaded with inorganic thermal conductivity fillers remains a huge challenge. In this study, we propose a new method for preparing ultrathin, large, and uniformly thick BNNS for quantitative production. Bulk hexagonal boron nitride (hBN) layers were exfoliated using a simple and low-cost hydrothermal reaction, and large-scale fewer-layered BNNSs were efficiently prepared by ball milling with a high yield (up to 80%). Based on the aforementioned step, a flexible insulating composite film with high thermal conductivity and a natural “brick-mud” shell structure was constructed via the sol–gel-film conversion method. After prestretching and hot-pressing treatment, the hydrogels became denser, and the modified BNNS formed a three-dimensional (3D) network structure with an ordered orientation and interconnections in the bacterial cellulose (BC) matrix. After 100 folding cycles, the tensile strength of the nanofiber composite film reached 53 MPa, and the strength retention rate exceeded 42%. By optimizing the modified BNNS content, the thermal conductivity reached 24 W/(m·K). This simple approach has wide application potential in the next-generation electronic devices, providing options for designing thermal interface materials with excellent electrical insulation, high thermal stability, and flexibility.

CAS / MDL: 919-30-2
研究领域: 材料科学 · 纳米技术 · 热管理材料
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ENVIRONMENTAL TECHNOLOGY · 2025 · IF 2

Control of phosphorus release from sediment by humic acid-loaded ferrihydrite and magnetite

Longhai Ding,Jianwei Lin,Yanhui Zhan

This study investigated the efficacy and mechanisms of humic acid (HA)-loaded ferrihydrite (Fh) and magnetite (Mag) in suppressing phosphorus (P) release from sediment into the overlying water (OW) via direct capping, fabric-wrapped capping, and sediment amendment. The results showed that the direct capping, fabric-wrapped capping, and sediment amendment with HA-loaded ferrihydrite (HA-Fh) and magnetite (HA-Mag) effectively mitigated the sedimentary P migration into OW. Specifically, the average reduction efficiencies of soluble reactive phosphorus (SRP) in OW were 94.6%, 74.6%, and 45.0% for HA-Fh under direct capping, fabric-wrapped capping, and amendment conditions, respectively. For HA-Mag, the corresponding efficiencies were 83.9%, 71.1%, and 47.1%. Under HA-Fh and HA-Mag capping, P in the sediment continued to mobilise into the pore water through the microbial and sulphide-mediated chemical reduction of iron (III) (hydr)oxides. However, the capping layers significantly reduced the concentrations of pore water SRP and labile P measured by diffusive gradients in thin-films (DGT) in the upper sediment. This reduction was crucial for effectively intercepting the sedimentary P migration into OW by HA-Fh and HA-Mag. Our study demonstrates that HA-Fh and HA-Mag are effective capping materials for managing the sediment-derived internal P loading. In other words, even after HA aging treatment, Fh and Mag still remain effective sediment phosphorus release control materials. In addition, the direct capping methods using HA-Fh and HA-Mag are promising due to their high control efficiency and ease of application in preventing P release from sediment into OW.

CAS / MDL: 1415-93-6
研究领域: 环境地球化学 · 水体富营养化 · 沉积物修复 · 界面过程 · 生物地球化学循环
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Passive sampling of chlorophenols in water and soils using diffusive gradients in thin films based on β-cyclodextrin polymers

Yuanting Zhu,Guizhou Xu,Xueyao Wang,Xiaowen Ji,Xun Jia,Lin Sun,Xueyuan Gu,Xianchuan Xie

Chlorophenols (CPs) have been listed as priority control pollutants because of their high toxicity and wide range. An In-situ monitoring technique using diffusive gradients in thin films based on porous β-cyclodextrin polymers as binding materials (CDP-DGT), was established to monitor four typical CPs, namely, 4-Chlorophenol (4-CP), 2,4-Dichlorophenol (2,4-DCP), 2,4,5-Trichlorophenol (2,4,5-TCP), 2,4,6-Trichlorophenol (2,4,6-TCP) in water and soils. The performance of CDP-DGT are stable under the conditions of pH 3.5–9.3, ionic strength 0.001–0.500 mol L −1 and dissolved organic matter concentration 0–20 mol L −1 . The adsorption capacities of CDP-DGT for 4-CP, 2,4-DCP, 2,4,5-TCP, 2,4,6-TCP were 57.80 μg cm −2 , 98.82 μg cm −2 , 95.69 μg cm −2 and 98.91 μg cm −2 , respectively. The time-average weighted concentrations of four CPs determined by CDP-DGT at Sanjiangkou wharf (Yangtze river, China) were consistent with the results of grab sampling, indicating the feasibility of CDP-DGT application in actual water. In addition, the distribution of CPs in the red soil of Kunming and paddy soil of Yixing were also studied by CDP-DGT, and the desorption kinetics in the two soils were analyzed with the DIFS model. The higher the soil organic matter content is, the more CPs are distributed in the soil solid phase. CPs in both soils can be partially resupplied to soil solution from the soil solid phase and the higher the partition coefficient for labile CPs is, the stronger the supplement capacity is.

CAS / MDL: 68-12-2 111689-03-3
研究领域: 环境科学 · 分析化学
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ANALYTICA CHIMICA ACTA · 2018 · IF 5.123

Development of cerium oxide-based diffusive gradients in thin films technique for in-situ measurement of dissolved inorganic arsenic in waters

Feng Tan,Xiao Jiang,Xianliang Qiao,Daming Sun,Jinsuo Gao,Xie Quan,Jingwen Chen,Suyu Ren,Yi Wang

A diffusive gradients in thin films (DGT) method using a new high-capacity cerium oxide (CeO 2 ) binding gel, for the first time, was developed for measuring dissolved inorganic arsenic in freshwater and seawater . The capacities of the new CeO 2 binding gel were 682 μg and 375 μg for As III and As V , respectively. The masses of As III and As V accumulated by CeO 2 -DGT device increased linearly with time and agreed well with the theoretical value calculated by DGT equation. The arsenic accumulation by CeO 2 -DGT was independent of pH (4.05–9.04) and ionic strength (0.1–750 mM), and common anions including CO 3 2− , SO 4 2− , Cl − and PO 4 3− had no obvious interference. CeO 2 -DGT showed excellent long-term deployment performance in freshwater and synthetic seawater . Field trials with CeO 2 -DGT achieved successfully the time-weighted-average concentrations of total inorganic arsenic in reservoir water (1.38 ± 0.09 μg/L) and coastal seawater (0.45 ± 0.06 μg/L). The results were comparable to those measured by grab sampling. The proposed method was reliable and robust for in-situ measurements of dissolved inorganic arsenic in environmental waters.

研究领域: 环境化学 · 分析化学 · 水环境监测 · 环境地球化学 · 污染生态学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2018 · IF 4.61

Diffusive gradients in thin films based on MOF-derived porous carbon binding gel for in-situ measurement of antibiotics in waters

Suyu Ren,Jing Tao,Feng Tan,Ying Cui,Xiaona Li,Jingwen Chen,Xin He,Yi Wang

Diffusive gradients in thin films (DGT) can achieve the time-weighted-average (TWA) concentrations of analytes in the period of deployment. Here we developed an approach based on DGT with a novel binding gel using porous carbon material (PCM) derived from metal-organic framework (MOF) for in-situ measurement of antibiotics in water samples. The diffusion coefficients of 20 antibiotics (nine sulfonamides, ten fluoroquinolones, and trimethoprim) in agarose diffusive gel were 1.41 × 10 −6  cm 2 /s to 4.75 × 10 −6  cm 2 /s at 25 °C. The capacity of PCM binding gel toward the antibiotics was ~100 μg per gel disc. The masses of the antibiotics accumulated by PCM-based DGT increased linearly with time, and they were almost independent of pH (4.2–8.4) and ionic strength (1–500 mM). The performance of the novel DGT was evaluated using freshwater and synthetic seawater spiked with the antibiotics in laboratory. The results showed good agreement with the theoretical predications except sulfacetamide. The detection limits achieved by the DGT with three devices together for deploying up to seven days were 1.0–18.0 ng/L. Field deployment in municipal wastewater treatment plant effluent and seawater showed that the TWA concentrations of antibiotics were 3.8–1342.5 ng/L and 5.6–43.3 ng/L, respectively, which were comparable to those measured by grab sampling. The proposed DGT was an efficient tool for the measurement of antibiotics in environmental waters.

研究领域: 环境科学 · 分析化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Coupling mesoporous imprinted polymer based DGT passive samplers and HPLC: A new tool for in-situ selective measurement of low concentration tetrabromobisphenol A in freshwaters

Zhongmin Feng,Yun Wang,Lan Yang,Ting Sun

Accurate measurement of tetrabromobisphenol A (TBBPA) is very important because of its widespread environmental pollution . Diffusive gradients in thin films technique (DGT), an in-situ passive sampling method, is regarded as a reliable and robust measurement technique. A new DGT technique based on mesoporous imprinted polymer was combined with high-pressure liquid chromatography (HPLC) method for sampling, preconcentration and monitoring low concentration TBBPA in natural waters. The diffusion coefficient of TBBPA through the diffusive gel was measured by diffusion cell test and simulated using mathematical expression. The effects of different ambient conditions were tested under laboratory conditions and the performance of DGT sampler was validated in natural waters. The diffusion coefficient of TBBPA in the diffusive gel was measured as 2.18 × 10 −6  cm 2  s −1 and simulated as in the range 1.41–3.48 × 10 −6  cm 2  s −1 by Amsden model. Comparison of experimental and theoretical data, the validity of the experimental method can be verified by the mathematical model. The binding agent with mesoporous imprinted polymer showed selective affinity to TBBPA and its adsorption rate met the requirement of DGT device. The DGT method detection limit was at the level of ng L −1 for 7 days deployment. DGT sampler was suitable for application in aquatic environment with a range of pH (4.5–7.6), ionic strength (1 × 10 −4 - 0.5 mol L −1 ), and dissolved organic matter (DOM) concentration (0–10 mg C L −1 ). The coupling method of DGT and HPLC was a promising technique for in situ sampling, preconcentration and monitoring low concentration TBBPA in most typical natural waters.

CAS / MDL: 110-26-9
研究领域: 环境科学 · 分析化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Selective diffusive gradients in thin-films with molecularly imprinted polymer for measuring fluoroquinolone antibiotics in waters

Si-Si Liu,Jin-Ling Li,Lin-Ke Ge,Cai-Lin Li,Jian-Liang Zhao,Qian-Qian Zhang,Guang-Guo Ying,Chang-Er Chen

Fluoroquinolones (FQs) have raised significant concerns due to their ubiquitous occurrence and promoting of antimicrobial resistance (AMR). In this study, a molecularly imprinted polymer-diffusive gradient in thin-films (MIP-DGT) sampler is developed for selective measurement of FQs in waters by using a commercial available MIP material as the binding agent. The MIP-DGT shows selective adsorption of the FQs and linearly accumulates the FQs over the deployment time. MIP-DGT measurement is independent of pH (6–8) and ionic strength (IS) (0.01–0.5 M) but is affected by DOM at higher concentrations (~10 mg•L −1 ), which is due to the altered diffusion coefficients and reduced adsorption on the MIP binding gel. Significant interaction effects of DOM with pH or IS indicate that this is the predominant influence on the MIP-DGT performance, which results in a lower measurement by the MIP-DGT but this is curtailed to some extend with increasing IS or pH. The MIP-DGT measurements, however, correlate well with those by grab sampling in a wastewater treatment plant , suggesting it is reliable for measuring FQs in waters. For the first time, we demonstrate that key water chemistry parameters do have interaction effects on the DGT measurements, which should be considered for the data interpretation. The MIP-DGT is a promising tool to understand the interaction effects of the environmental parameters on the fate, behaviours and bioavailability/toxicity of organic contaminants and improve environmental risk assessments in the environment and modelling.

研究领域: 环境科学 · 分析化学
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CHEMOSPHERE · 2020 · IF 5.778

Development of a novel composite resin for dissolved divalent mercury measurement using diffusive gradients in thin films

Heng Yao,Yujie Zhao,Che-Jen Lin,Fengjiao Yi,Xuefeng Liang,Xinbin Feng

In this work, a composite resin gel incorporating thiol-modified metal double hydroxide ( TM-MDH) nanoparticles is developed for application in diffusive gradients in thin films (DGT) devices to sample and concentrate divalent Hg (Hg(II)) in water and sediment samples. The DGT device uses the TM-MDH resin as a sorption layer and an agarose gel as a diffusive layer. Complete digestion of the TM-MDH resin after sampling can be achieved in 5 mL of 12 N HCl solution for 30 min for direct aqueous Hg(II) analysis. The recovery of Hg(II) uptake onto the resin in aqueous solution reaches 95.4 ± 1.9%. The effect of ionic strength and pH on the performance of DGT device for Hg(II) is assessed. It is found that there is no significant difference on Hg(II) uptake over a pH range of 3.5–8.5 and an ionic strength range of 1–500 mM NaCl. The diffusion coefficient of Hg(II) at 25 °C was estimated to be 9.48 × 10 −6  cm 2 /s at 50 μg/L solution. The sorption capacity of TM-MDH-DGT for Hg(II) reaches 41.0 μg/cm 2 . Field validations performed in reservoir water and in contaminated paddy soil demonstrate that the developed TM-MDH DGT device can accurately determine Hg(II) concentrations in these samples and outperform traditional sampling methods for both high and low Hg(II) concentrations.

研究领域: 环境科学 · 材料科学
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AGRICULTURAL WATER MANAGEMENT · 2025 · IF 6.5

Study on the regulatory effect of biochar-based materials on the migration and accumulation of perfluoroalkyl substances in paddy soil-water-plant systems

Jian Zhang,Renjie Hou,Anshuang Su,Miao Wang,Heqiang Sun,Hai Xu,Wei Huang,Fei Peng,Shan Zhao

Perfluoroalkyl substances (PFAS), as persistent emerging contaminants, can migrate into rice systems through the soil-water interface (SWI) during irrigation, threatening food security and human health. However, the diffusion characteristics of PFAS at the SWI under carbon-based material regulation and their solute exchange kinetics remain unclear, particularly the quantitative differences between short-chain (PFBA) and long-chain (PFOA) PFAS behaviors. To address this, this study innovatively integrated molecularly imprinted polymer-diffusive gradients in thin films (MIP-DGT) and high-resolution pore water sampling (HR-Peeper) techniques to systematically investigate the regulatory mechanisms of control (WBC), rice husk biochar (RBC), and montmorillonite-modified biochar (MBC) on the migration and accumulation of PFBA and PFOA in the paddy sediment-water-plant system. The results showed that in WBC-treated soil, the surface C DGT -PFBA and C DGT -PFOA concentrations were 6.76 ± 1.44 ng L −1 and 7.21 ± 2.14 ng L −1 , respectively, while biochar treatments significantly inhibited PFAS migration to deeper layers. Compared to WBC, RBC reduced C DGT -PFBA and C DGT -PFOA in deeper soil layers by 32.80 % and 87.50 %, respectively, with modified biochar exhibiting even stronger retention effects. The constructed 2D-DIFS (DGT-induced fluxes in soils/sediments) model indicated that PFAS re-supply capacity (R-value) from soil to pore water declined with irrigation cycles. PFBA had shorter response times (T c ) and higher mobility, while PFOA was more immobilized due to higher adsorption rate (k −1 ) and partition coefficient (K d ). Notably, compared to WBC, RBC reduced PFBA and PFOA accumulation in rice organs by 24.21 ~ 26.26 %, confirming the dual role of carbon-based materials in altering PFAS interfacial behavior and thereby inhibiting plant uptake. This study clarifies PFAS migration and biotransport responses to carbon-based materials under irrigation, supporting strategies to mitigate PFAS contamination in farmland.

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JOURNAL OF HAZARDOUS MATERIALS · 2025 · IF 11.3

MOF-derived DGT for selective monitoring of quinolones and tetracyclines: Tracking antibiotics risks in urban wastewater treatment plant

Yixuan Liang,Hanbing Li,Yaming Li,Lei Yan,Sumei Li,Xiaowei Wang,Danyang Li,Sha Chen

Environmental challenges of antibiotics contamination have emerged to address severe impacts on ecological stability and human health. Active sampling methods are not well-fitted to study the emerging pollutants since complicated and unstable enrichment devices/chemicals are significantly required for measurements. Diffusive gradients in thin-films (DGT) are proved to be useful for organic compound detection, but limited by its non-specificity for quinolones (QNs) and tetracyclines (TCs) in waters. Consequently, a metal-organic framework derived carbon specific to QNs and TCs was used as binding agent to develop selective DGT (qt-DGT) in this study. qt-DGT had highly selective adsorption capacity for QNs at 85.45–112.59 μg and TCs at 79.19–85.92 μg in a pH range of 4–9 and ionic strength from 0.001 to 0.05 M. Masses of antibiotics accumulated by qt-DGT increased linearly with time in 24 h. After the deployment in a wastewater treatment plant (WWTP) of Beijing, the qt-DGT exhibited stable and selective uptake of QNs and TCs in comparison with traditional HLB-DGT and active sampling methods. With qt-DGT measurements, QNs and TCs up to 1202.3 ng/L from influent forced WWTP became the major sink of antibiotics, and 830.1–966.3 ng/L from effluent warned the inefficient treatment leading to elevated threats on natural waters.

研究领域: 环境科学 · 分析化学 · 污染物监测 · 水处理 · 药物代谢 · 生态毒理学
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