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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2020 ·Vol. 412 ·期 13 ·3073-3081 · IF 3.637

Highly sensitive electrochemiluminescence biosensor for VEGF165 detection based on a g-C3N4/PDDA/CdSe nanocomposite

Cheng Jin-long,Liu Xing-Pei,Chen Jing-Shuai,Mao Chang-jie,Jin Bao-Kang

In this work, an electrochemiluminescence (ECL) biosensor was fabricated for the selective detection of vascular endothelial growth factor (VEGF 165 ). g-C 3 N 4 /PDDA/CdSe nanocomposites were used as the ECL substrate. Then, DNA labeled at the 5′ end with amino groups (DNA 1 ) was immobilized on the surface of g-C 3 N 4 /PDDA/CdSe nanocomposite-modified glassy carbon electrode (GCE) by amido linkage. AuNP-labeled target DNA (Au-DNA 2 ) could hybridize with DNA 1 to form a double strand. The ECL of the g-C 3 N 4 /PDDA/CdSe nanocomposite was efficiently quenched due to the resonance energy transfer between CdSe QDs and Au NPs. After VEGF 165 was recognized and bound by Au-DNA 2 , the double helix was disrupted, and the energy transfer was broken. In this case, Au-DNA 2 was released from the electrode surface, and the ECL intensity recovered to a higher level. Under optimal conditions, this ECL biosensor possesses excellent selectivity, accuracy, and stability for VEGF 165 detection in a linear range of 2 pg mL −1 to 2 ng mL −1 with a detection limit of 0.68 pg mL −1 . In addition, this assay has been successfully applied to the determination of VEGF 165 in serum samples. Schematic representation of the electrochemiluminescence sensor based on a g-C3N4/PDDA/CdSe nanocomposite, which can be determined in the concentration of vascular endothelial growth factor in serum.

研究领域: 生物化学 · 分析化学 · 纳米技术 · 生物传感器
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Materials Today Chemistry · 2023 · IF 7.3

Interfacial properties of Co3O4/Gd–Fe2O3 p-n junction photoanode improved by PDDA functional layer for efficient photoelectrochemical water oxidation

H. Chai,R. Li,L. Gao,H. Niu,J. Jin

The phase interface properties of the p-n junction may profoundly affect its photoelectrochemical (PEC) water oxidation performance. Here, we introduced a non-conjugated polymer functional layer (poly(diallyl-dimethylammonium chloride, PDDA) between the interfaces of the p-n junction (Co 3 O 4 /Gd–Fe 2 O 3 ) to tune the interfacial properties . First, the PDDA modulates the band structure so that the composite photoanode (Co 3 O 4 /PDDA/Gd–Fe 2 O 3 ) has an enlarger band bending than the p-n junction. Then, PDDA passivates the surface trap, which synergizes with Co 3 O 4 to provide more active sites for water oxidation. Furthermore, PDDA improves the PEC water oxidation kinetics. Specifically, PDDA extracts holes and adsorbs water oxidation reactants, thus it efficiently transfers photogenerated holes to Co 3 O 4 , promoting the water oxidation reaction in the positive direction. With these positive modulations, PDDA can further enhance the PEC water oxidation performance of the p-n junction. This conceptual work provides insight into the role of the non-conjugated polymer in PEC water splitting .

研究领域: 材料科学 · 光电化学 · 能源材料
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RSC Advances · 2013 ·Vol. 3 ·期 35 ·15467-15474 · IF 2.562

Layer-by-layer self-assembly of PDDA/PSS-SPFEK composite membrane with low vanadium permeability for vanadium redox flow battery

Yufei Wang,Shuanjin Wang,Min Xiao,Dongmei Han,Michael A. Hickner,Yuezhong Meng

Sulfonated poly(fluorenyl ether ketone) (SPFEK) membranes have been first modified by layer-by-layer (LbL) self-assembly of positively charged polyelectrolyte PDDA (poly(diallyldimethylammonium chloride)) and negatively charged PSS (poly(sodium styrene sulfonate)). The membranes were investigated as an ion exchange membrane for vanadium redox flow batteries (VRBs). The permeability of the vanadium ions in VRBs was effectively suppressed by depositing the LbL thin film on the SPFEK membrane. The permeability decreased with increasing the number of PDDA/PSS bilayers. For the membrane with two self-assembly bilayers of PDDA/PSS, 50% and 10% of vanadium ion permeability of a pristine SPFEK and Nafion 117 membranes can be afforded, respectively. Moreover, the oxidative stability of the PDDA/PSS-SPFEK composite membrane is improved remarkably compared with the pristine one. Consequently, the performance of VRBs using the PDDA/PSS-SPFEK composite membrane exhibits the highest coulombic efficiency (CE) of 82.1% at 30 mA cm−2 and the longest duration stability in the self-discharge test.

研究领域: 电化学 · 能源材料 · 膜科学 · 储能技术 · 高分子化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Solar driven thermal responsive polyionic liquid/PDDA semi-IPN hydrogel for near-room temperature membrane-free osmotic desalination

Xueyu Yuan,Jing Jiang,Zihao Zhou,Hongyu Pan,Chengwei Wang,Chor Yong Tay,Jinhua Hu,Li Liu,Bing Li,Yufeng Cai,Ming Liu

The designed thermally responsive polyionic liquid (TPIL)/ poly (diallyl dimethylammonium chloride) (PDDA) hydrogel with a semi-interpenetrating (semi-IPN) structure, containing highly charged chloride anions, was fabricated to explore the comprehensive capabilities of solar driven membrane-free osmotic desalination. Introducing linear PDDA polyelectrolyte with higher charge density has effectively excluded salt ions from entering the TPIL hydrogel matrix due to the strong charge concentration gradient established between the hydrogel and the saline reservoir. Meanwhile, the thermo-sensitivity of the polyionic liquid/PDDA semi-IPN (PNCl) hydrogel enabled the release of absorbed salt-depleted water at a temperature above the Lower Critical Solution Temperature (LCST). The multiple purification process established by partial submersion of PNCl hydrogel in saline enabled continual reduction of the salt ion concentration during the upwards transportation of water along the polyelectrolyte network. Moreover, a mushroom-shaped hydrogel demonstrated enhanced the effectiveness in long-term cyclic desalination. The “mushroom cap” was loaded with photo-thermal conversion fillers (Ti 3 C 2 T x MXene) to achieve higher photo-thermal conversion efficiency for water recovery. A record high salt rejection rate of more than 93% was obtained for membrane-free osmotic desalination. More importantly the whole desalination/water absorption/release process was solely supported by gently heating the PNCl hydrogel under the illumination of renewable solar energy.

研究领域: 材料科学 · 环境工程 · 水处理
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MICROCHEMICAL JOURNAL · 2020 · IF 3.594

Layer-by-layer self-assembly of MoS2/PDDA hybrid film in microfluidic chips for ultrasensitive electrochemical immunosensing of alpha-fetoprotein

Tao Hu,Man Zhang,Zhen Wang,Ke Chen,Xiao Li,Zhonghua Ni

Ultrasensitive detection of cancer biomarkers holds great promise for early stage detection and diagnosis of cancer. Microfluidic electrochemical immunochips have been assessed as powerful detection platforms due to their high sensitivity, low cost, portability, and ease of miniaturization. In this work, an ultrasensitive electrochemical immunochip based on MoS 2 /PDDA hybrid film is designed via layer-by-layer self-assembly method. An electrochemical impedance detection platform is developed for the detection of alpha-fetoprotein (AFP) by integrating a three-electrode system in the micro-channel, which introduces MoS 2 /PDDA film modified with antibodies as the working electrode, Ag/AgCl wire as the reference electrode and indium tin oxide (ITO) as the counter electrode. After MoS 2 /PDDA film is modified with AFP antibodies, the immobilization of various concentrations of AFP antigens is carried on which can cause changes in the electrochemical impedance value. This proposed approach exhibits a linear range from 0.1 ng/mL to 10 ng/mL and a low detection limit of 0.033 ng/mL (S/N = 3). The applicability of the MoS 2 /PDDA immunochip is further investigated by detecting human serum samples. This ultrasensitive microfluidic immunochip is proved to be highly selective with small input liquid volume, which could realize trace detection of AFP and be potentially applied in clinical diagnosis of other biomolecules.

CAS / MDL: 50-99-7
研究领域: 生物医学工程 · 分析化学 · 癌症研究
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OPTICAL FIBER TECHNOLOGY · 2024 · IF 2.6

Fiber optic dimethyl methyl phosphate fiber optic sensor based on ZIF-8@Ag/PDDA composite film

Yuhao Chen,Xiaozhan Yang

A Michelson interference dimethyl methyl phosphate (DMMP) fiber sensor with a single-mode (SMF)-dislocated single-mode (DSMF)-hollow-core fiber (HCF) structure is proposed. To fabricate the Michelson interference structure of SMF-DSMF-HCF, one end of the DSMF was misaligned and fused to the SMF, the other end was fused to the HCF to generate a reflective surface. The structure, elemental composition, and surface morphology of ZIF-8@Ag were analyzed using X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy after the ZIF-8@Ag/PDDA composite was coated on the surface of DSMF. The result shows that the sensitivity and the detection limit of the sensor are 45.71 dB/ppm and 0.1431 ppb, respectively, and the response/recovery time is around 14/12 s. The sensor also has excellent selectivity and stability.

研究领域: 光学工程 · 传感器技术 · 材料科学 · 化学传感
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LANGMUIR · 2024 · IF 3.7

PDDA-Assisted Synthesis of Magnetic Fluorescent Fe3O4@SiO2–CQD Composites

Lingwei Li,Huan Wang,Jixiang Fang

Magnetic fluorescent nanomaterials have broad application prospects as taggants in fields such as anticounterfeiting identification, suspicious object tracking, and potential fingerprint recognition in forensic medicine. It is a common method to synthesize magnetic fluorescent composite nanoparticles by preparing a shell on the surface of magnetic particles to load fluorescent materials. In this work, a magnetic fluorescence nanohybrid was synthesized by in situ encapsulation of carbon quantum dots (CQDs) during the preparation of a SiO2 shell on the surface of Fe3O4 nanoparticles. The traditional Stöber method was employed to synthesize the SiO2 shell. Meanwhile, CQDs were introduced into the hydrolysis process of tetraethyl orthosilicate. To address the issue of charge repulsion between the negatively charged hydrolysis intermediate of tetraethyl orthosilicate and the negatively charged CQDs, poly(diallyldimethylammonium chloride) with positive charge was introduced in the synthesis process. The repulsive charges in the reaction system were balanced by poly(diallyldimethylammonium chloride), allowing for the successful encapsulation of CQDs in the SiO2 shell. The structure, morphology, and magnetic and fluorescence properties of the prepared Fe3O4@SiO2–CQDs were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, a vibrating sample magnetometer, and a fluorescence spectrophotometer. The Fe3O4@SiO2–CQDs exhibited excellent magnetic and fluorescence properties, making them suitable for fluorescence labeling on various substrates and showing great potential in labeling, tracing, and fluorescence sensors.

研究领域: 材料科学 · 纳米技术 · 生物医学工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Positively charged Ti3C2Tx membrane for enhanced Li+/Mg2+ sieving

Yanna Wu,Mengmeng Jia,Shuming Li,Zong Lu,Yanying Wei,Haihui Wang

Lithium extraction from salt lake is important for carbon neutrality, while obtaining both high Li + /Mg 2+ selectivity and high water permeance is still challenging. The burgeoning two-dimensional (2D) material membranes in decade show enormous potential to solve above problem due to its highly designable lamellar structure. In this work, a kind of positively charged laminated membranes using MXene nanosheets as building blocks with decoration of poly (diallyl dimethyl ammonium chloride) (PDDA) were proposed. Benefiting from the well–intercalated PDDA between MXene nanosheets, the interlayer spacing between neighboring nanosheets was greater than 2 nm, which was conductive to enhance water permeance. Simultaneously, the introduction of PDDA endowed the membrane with positive charge, which exhibited sharply improved Li + /Mg 2+ selectivity by an order of magnitude due to enhanced Donnan effect. The prepared MXene/PDDA membrane with a modification mass ratio of 1:10 exhibited high Li + /Mg 2+ selectivity of 29.3 with MgCl 2 saline solution permeance of 9.8 L m −2  h −1 ·bar −1 and pure water permeance of 32.3 L m −2  h −1 ·bar −1 , which was promising for lithium extraction. Such membrane constructing concept could be expanded to other kinds of membranes based on 2D nanosheets for effective ion sieving.

CAS / MDL: 26062-79-3
研究领域: 材料科学 · 环境科学
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Nanomaterials · 2023 ·Vol. 13 ·期 21 ·2885 · IF 5.3

Polycation-Intercalated MXene Membrane with Enhanced Permselective and Anti-Microbial Properties

Jie Yang,Shilin Zhu,Hongli Zhang

Two-dimensional (2D) nanomaterial-based membranes feature attractive properties for molecular separation and transport, which exhibit huge potential in various chemical processes. However, the low permeability and bio-fouling of the MXene membrane in water treatment become huge obstacles to its practical application. Herein, a highly permselective and anti-bacterial 2D nanofiltration membrane is fabricated by intercalating a polycation of polydiallyldimethylammonium chloride (PDDA) into the Ti3C2TxMXene laminar architecture through a facile and patternable electrostatic assembly strategy. As a result, the as-fabricated Ti3C2Tx/PDDA composite membrane exhibits higher water permeance up to 73.4 L m−2h−1with a rejection above 94.6% for MgCl2. The resultant membrane simultaneously possesses good resistance to swelling and long-term stability in water environments, even after 8 h. Additionally, the Ti3C2Tx/PDDA membrane also demonstrates a high flux recovery ratio of nearly 96.1% to bovine serum albumin proteins after being cleaned. More importantly, the current membrane shows excellent anti-adhesive and anti-microbial activity against Gram-negativeEscherichia coli(E. coli) and Gram-positiveStaphylococcus aureus(S. aureus), with inhibition rates of 90% and 95% againstE. coliandS. aureus, respectively. This holds great potential for the application of the polyelectrolyte-intercalated MXene membrane in serving as a promising platform to separate molecules and/or ions in an aquatic environment.Keywords:Ti3C2Tx;MXene membrane;nanofiltration;two-dimensional membrane;anti-biofouling;PDDA

研究领域: 材料科学 · 环境科学 · 生物学
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION · 2024 ·Vol. 39 ·期 4 ·937-944 · IF 1.3

Layer by Layer Self-assembly Fiber-based Flexible Electrochemical Transistor

Tan Yan,Hao Panpan,He Yang,Zhu Rufeng,Wang Yuedan

Poly(3, 4-ethylenedioxyethiophene)-polystyrene sulfonic acid (PEDOT:PSS)/polyallyl dimethyl ammonium chloride modified reduced graphene oxide (PDDA-rGO) was layer by layer self-assembled on the cotton fiber. The surface morphology and electric property was investigated. The results confirmed the dense membrane of PEDOT: PSS and the lamellar structure of PDDA-rGO on the fibers. It has excellent electrical conductivity and mechanical properties. The fiber based electrochemical transistor (FECTs) prepared by the composite conductive fiber has a maximum output current of 8.7 mA, a transconductance peak of 10 mS, an on time of 1.37 s, an off time of 1.6 s and excellent switching stability. Most importantly, the devices by layer by layer self-assembly technology opens a path for the true integration of organic electronics with traditional textile technologies and materials, laying the foundation for their later widespread application.

研究领域: 材料科学 · 电子工程
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MICROCHEMICAL JOURNAL · 2026 · IF 5.2

Ratiometric electrochemical quantitation of methyl parathion based on NiHCF/PDDA@rGO nanocomposites

Xiaolin Jia,Miaomiao Li,Zhiguang Liu,Yujie Han,Hua-Zhong Yu,Lifang Fan,Yujing Guo

This work presents an on-off ratiometric electrochemical quantitation study of methyl parathion (MP), one of the most popularly used organophosphorus pesticides, based on electrode modification with a newly developed nanocomposite, i.e., reduced graphene oxide (rGO) functionalized with poly(diallyldimethylammonium chloride) (PDDA) and nickel hexacyanoferrate (NiHCF). It was shown that MP strongly adsorbs on the modified electrodes and produces a distinct reduction signal (-NO 2 ), which increases proportionally with its concentration; meanwhile, the intrinsic reduction signal (Fe(III)/(II)) from the nanocomposite (NiHCF/PDDA@rGO) decreases due to the inhibited electron-transfer process upon MP binding. Indeed, plotting the ratiometric signal (the ratio of decreased Fe(III)/(II) current and the increased MP current) as a function of the analyte (MP) concentration produces a linear calibration curve in the range of 0.05 μM to 10 μM (R 2  = 0.9987), with a limit of detection (LOD) of 16 nM. The method was further validated in real water samples, showing recoveries of 96.2–102% with relative standard deviations below 3.3%, which are comparable with standard HPLC results.

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JOURNAL OF MATERIALS SCIENCE · 2017 ·Vol. 53 ·期 7 ·5204-5215 · IF 2.599

PTFE/SPEEK/PDDA/PSS composite membrane for vanadium redox flow battery application

Teng Xiangguo,Yu Cong,Wu Xiufen,Dong Yichao,Gao Peng,Hu Huili,Zhu Yongming,Dai Jicui

How to solve the crossover of vanadium ions through ion exchange membrane is a key issue in vanadium redox flow battery (VRB), especially for ultra-thin membranes used for VRB to obtain a lower cell resistance. Herein, an ultra-thin (~ 30 μm) PTFE/SPEEK [polytetrafluoroethylene/sulfonated poly(ether ether ketone), P/S] membrane is successfully prepared and modified by using layer-by-layer (LBL) self-assembly technique with polycation poly(diallyldimethylammonium chloride) (PDDA) and polyanion poly(sodium styrene sulfonate) (PSS). P/S membranes are alternatively immersed in positively and negatively charged polyelectrolyte to form 2 to 8 bilayers onto its surface. Consequently, a series of P/S-[PDDA/PSS] n ( n is the number of multilayers) membranes are fabricated. Both the physicochemical properties and VRB performances of the P/S-[PDDA/PSS] n membranes are then investigated in detail. Results show that the ion selectivity of the P/S-[PDDA/PSS] n membranes is much higher than that of pristine P/S membrane, especially for P/S-[PDDA/PSS] 6 membrane. As a result, the VRB with the P/S-[PDDA/PSS] 6 membrane exhibits the highest coulombic efficiency (CE) of 96.5% at 80 mA cm −2 , the highest voltage efficiency of 94.7% at 40 mA cm −2 and the highest energy efficiency of 87.7% at both 40 and 50 mA cm −2 , respectively. In addition, 80 times charge–discharge test proves that the P/S-[PDDA/PSS] 6 membrane possesses high stability and no obvious CE decay after running. All the results show that the LBL technique is an effective way to prepare ultra-thin membrane with high ion selectivity for VRB application.

研究领域: 电化学 · 能源材料 · 膜科学 · 储能技术 · 高分子材料 · 电化学工程
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