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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 43 ·2303832 · IF 19

Aromatic Ring–Mediated Nonspecific Signaling Mechanism and Nafion-Dominated Solution in Graphene Field-Effect Transistor–Based Nucleic Acid Biosensors

Shuo Chen,Yongkang Lyu,Yang Sun,Qin Wei,Chuansong Chen,Lei Chen,Xinhao Zhang,Heqi Ma,Tianyu Sun,Wen Gao,Yazhe Xu,Baoyuan Man,Qingtian Meng,Cheng Yang

Graphene field-effect transistors (G-FETs) have attracted widespread attention in disease diagnosis, benefiting from these advantages of high sensitivity, label-free, easy integration, and direct detection of nucleic acids (NAs) in liquid environments. However, the problem of nonspecific signals in G-FETs is not fundamentally solved due to a lack of systematic theoretical research to support the development of effective solutions. Thus, researchers have to rely on speculative mechanisms to minimize nonspecific signals in experiments as much as possible. Herein, the nonspecific signal mechanism caused by eight types of π – π interaction paths mediated by aromatic rings is theoretically determined. Based on theoretical simulation results, the feasibility of blocking nonspecific signal paths through Nafion functionalization methods is experimentally verified. Experiments confirm that Nafion-modified G-FETs (NMG-FETs) have excellent performance in avoiding nonspecific signals compared to traditional G-FETs. Furthermore, the NMG-FET achieves ultra-sensitive detection of Down syndrome–related DNA down to 1 aM and severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA down to 5 aM, and shows good specificity in base recognition. This study is expected to promote the theoretical advancement of the nonspecific signal mechanism in G-FET NA detection and offer a practical strategy for improving signal purity and accuracy.

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POLYMERS FOR ADVANCED TECHNOLOGIES · 2023 ·Vol. 34 ·期 10 ·3125-3136 · IF 3.4

Reducing the dielectric loss of poly(aryl ether)s by grafting

Longwei Shi,Zheng Zhao,Lishuai Zong,Jinyan Wang,Xigao Jian

Limiting molecules' polarized motion effectively reduces the dielectric loss of materials. This article synthesized side chains with different lengths using p-ethoxyphenol, p-hydroxybenzoic acid, and long-chain halohydrins through a two-step process. These chains' movement was almost unaffected by the main chain of polymers, so they can fill up the free volume of polymers under certain conditions. 1,2-dihydro-4-(4-hydroxyphenyl)phthalazine-1-(2H)-one(DHPZ), 4,4'-Difluorophenyl sulfone(DFS), and 4,4-Bis(4-hydroxyphenyl) valeric acid(HPV) obtained three polymers with different carboxyl groups (10%, 30%, and 50%) through nucleophilic substitution. They were then grafted and treated with hot-pressing. The introduction of side chains could reduce the free volume of polymers under hot-pressing conditions, so further reducing the dielectric loss of materials. Polymer with the shortest and least (10%) side chains showed the most obvious dielectric loss tangent, the reduction rate of the film's dielectric loss tangent was 13.11% (at T g + 15°C, while the non-grafted one was only 3.69%) and 20.70% (at T g + 80°C, while the non-grafted one was only 8.35%), respectively. In addition, WXRD and DMA tests showed that films' intermolecular chain spacing (“ d ”) and T g changed after the hot-pressing process, respectively. The change law of both was consistent with that of dielectric loss tangent. Confirm that grafting high-motility side chains can significantly reduce polymer's dielectric loss by enhancing the free volume reduction effect after hot-pressing.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Polyethyleneimine (PEI) based thin film nanocomposite (TFN) total heat exchange membranes (THEMs) composed of shaped ZIF-8 crystalline Micro-leaves (ZIF-L)

Shiyang Li,Longdou Tu,Yeqiang Lu,Mingjie Lin,Junmei Ma,Chaojie Bai,Congjie Gao,Lixin Xue

A novel strategy was developed to build high-performance thin film composite (TFC) total heat exchange membranes (THEMs) by in situ growing ZIF-8 crystalline micro-leaves (ZIF-L) from Polyethyleneimine (PEI) coated on polysulfone (PSF) ultra-filtration substrates. It was found that flexible PEI polymeric chains could tightly cross-link and seal large masses of ZIF-L micro-leaves (ZIF/PEI wt. ratio up to 18.5) to thwart CO 2 permeation, on top of PSF substrate. Such PEI cross-linking could also effectively open up the internal channels of ZIF-L micro-leaves to enhance moisture permeance and latent heat recovery without trading off CO 2 gas barring property. ZIF-L in varied shapes protruded into the air stream could provide ultra-rough surfaces with increased surface area for improved total energy recovery efficiency. Optimized PEI/ZIF-L TFC THEMs showed ultra-low CO 2 permeance of 0.5–8 GPU and ultra-high total heat recovery rates of 68–74%.

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npj Materials Degradation · 2023 ·Vol. 7 ·期 1 ·1-10 · IF 5.1

High-throughput screening of zwitterion-based coatings towards improved mechanical stability and drug-loading capacity

Yang Jingzhi,Ran Yami,Huang Luyao,Ren Chenhao,Hao Xiangping,Ma Lingwei,Zhang Dawei

2-hydroxyethyl methacrylate (HEMA), poly(ethylene glycol) (PEG), and zwitterionic polymers are currently considered the most extensively studied antifouling hydrogel coatings. However, systematic identification of these coatings to unleash their potential properties is tremendously under-represented. Here, we report a high-throughput optimizing strategy that combines highly miniaturized hydrogel synthesis and screening to fine design zwitterion-based hydrogel coatings. Compared with the traditional one-by-one synthesis and characterization methods, the proposed high-throughput strategy accelerated the discovery of candidate materials with a high-efficiency and cost-effective approach. To tailor multiple parameters of coatings, 1575 unique coating combinations with continuous gradients were prepared only required 600 μL reactant. The mechanical stability and drug-loading capacity of the coating spots were sequentially evaluated via immersion swelling, flow, tape-peeling, and dye-retaining tests. This strategy could efficiently reveal the composition/structure-function relationships of the hydrogel coatings and also other materials, which is promising for the rapid screening and design of desired implantable device surfaces.

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LANGMUIR · 2023 · IF 3.9

Synchronously Enhanced Removal Ability and Stability of MXene through Biomimetic Modification

Qing Qing,Xian-ying Shi,Shao-zhong Hu,Liang Li,Ting Huang,Nan Zhang,Yong Wang

Increasing environmental problems intensify the demand for high-performance environmental purification materials. MXene is a typical transition-metal carbide/nitride material with a two-dimensional geometric feature and a good deal of functional groups, and it is considered as an efficient adsorbent for removing pollutants from wastewater. However, the easy oxidation and relatively low adsorption capacity greatly restrict its application. In this study, the MXene/polydopamine (PDA) composite particles were fabricated through the biomimetic modification method of inducing the self-polymerization of dopamine in an MXene aqueous solution. Microstructure characterizations demonstrate that PDA facilitates the exfoliation of MXene. Adsorption measurements show that MXene and PDA exhibit an apparent synergistic effect in removing chromium hexavalent Cr(VI) from aqueous solution, and more PDA content leads to a larger synergistic effect. Consequently, the composite particles exhibit an ultrahigh adsorption capacity (862.3 mg/g). Specifically, even if the composite particles were stored in aqueous solution for 2 months, they still exhibit high adsorption ability with only a 3.3% loss in adsorption capacity, indirectly confirming the enhanced stability of MXene induced by PDA. Furthermore, the composite particles also show reduction ability to Cr(VI) and about 54.3% Cr(VI) can be reduced to harmless chromium trivalent Cr(III). This study provides a new method for the preparation of MXene-based adsorbents with excellent adsorption capacity and high stability, which has broad application prospects in the field of wastewater treatment.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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TALANTA · 2023 · IF 6.1

Smartphone-assisted colorimetric aptasensor for rapid detection of carbendazim residue in agriculture products based on the oxidase-mimicking activity of octahedral Ag2O nanoparticles

Feng Luo,Yue Tang,Jia Zheng,Zhengmin Xie,Junjun Wang,Jianli Zhou,Yuangen Wu

Carbendazim (CBZ) is a widely used pesticides, and its excessive intake is serious damage to humans and animals. Herein, a stable and sensitive colorimetric aptasensor for rapid detection of CBZ residue has been established based on the enhancement of CBZ-specific aptamer (CZ-13) on oxidase-mimicking activity of octahedral Ag 2 O nanoparticles (NPs). The CZ-13 aptamer can significantly increase the catalytic activity by promoting the production of superoxide anion (·O 2 − ) on the surface of Ag 2 O NPs and enhancing the affinity of octahedral Ag 2 O NPs to 3,3′,5,5′-tetramethylbenzidine (TMB) molecules. In the presence of CBZ, the quantity of CZ-13 aptamer will be exhausted due to the specific binding to CBZ pesticide. Thus, the rest CZ-13 aptamer no longer enhanced the catalytic activity of octahedral Ag 2 O NPs, which leads to the change in color of sensing solution. The color change of sensing solution can be easily converted to the corresponding RGB value by a smartphone for quantitative and rapid detection of CBZ. The designed aptasensor has excellent sensitivity and specificity, and the limit of detection was determined as low as 7.35 μg L −1 for CBZ assay. Besides, the aptasensor exhibited good recoveries in the spiked cabbage, apple and cucumber, showing that it may have broad application prospects for detecting CBZ residues in agriculture products.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Protease-Loaded CuS Nanoparticles with Synergistic Photothermal/Dynamic Therapy against F. nucleatum-Induced Periodontitis

Pengyu Gao,Guotai Li,Zhiguo Wang,Hui Zhang,Yansheng Shan,Xin Yuan,Qiang Shi,Xue Dou,Qihui Zhou,Quanchen Xu

Periodontitis is a chronic inflammatory disease induced by a plaque biofilm, which can lead to the destruction of the periodontal support tissue and even teeth loss. The common strategies of periodontitis treatment are to eliminate bacterial/biofilm-related inflammation and subsequently inhibit alveolar bone resorption, for which antibiotic therapy is the most traditional one. However, impenetrable polymeric substances on bacterial biofilms make it difficult for traditional antimicrobial agents to take effect. In this study, a novel nanoparticle protease-loaded CuS NPs was developed, combining the advances of photodynamic and photothermal therapy from CuS and enzymatic degradation of the biofilm by a protease. The photothermal activity and the reactive oxygen generation capacity of the designed nanoparticles were verified by the experimental results, constituting the basis of antibacterial function. Next, the high antimicrobial activity of CuS@A NPs onFusobacterium nucleatumand its biofilm was demonstrated. The proper hemo/cytocompatibility of CuS-based NPs was demonstrated by in vitro assays. Last, effective treatment against periodontitis was achieved in a rat periodontitis model through the significant efficacy of inhibiting bone resorption and alleviating inflammation. Thus, the developed CuS@A NPs prove a promising material for the management of periodontitis.

CAS / MDL: 6066-82-6 7439-89-6
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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 49 ·2305766 · IF 19

Magnetic Responsive On-Site Switching of the Directional Droplet Self-Transport in Shape Memory Slippery Tube

Ruijie Wang,Fan Jin,Yufen Li,Junkai Gong,Hua Lai,Yuyan Liu,Zhongjun Cheng

The phenomenon of controlled droplet transport has promising application prospects in various fields. Active droplet transport mode is controllable through continuous external stimuli. By contrast, self-transport is a more environmentally friendly and energy-efficient passive transport mode but lacks controllability. In this study, controlled self-transport is achieved by constructing a shape memory polymer (SMP) tube with a lubricated magnetic-responsive gel inner surface. The asymmetrical shape of the tube, combined with the lubricated inner surface, enables directional self-transport of droplets without external stimuli. Furthermore, the resistance on the inner gel surface can be altered by regulating the magnetic field to achieve effective active control during the self-transport process. Thus, smart in situ control of droplet transport can be achieved by integrating the macroscale shape variation of the tube with the dynamic control of the inner surface microstructure. Owing to the fast magnetic responsivity and in situ controllability of the self-transport process, the SMP lubricated tube demonstrates the ability to transport a variety of liquids and can be designed as a micro-reactor for step-by-step droplet detection. The findings of this study may provide guidance for the development of intelligent interface materials and microfluidic devices.

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BIORESOURCE TECHNOLOGY · 2023 · IF 11.4

Promotion of nitrogen removal in a denitrification process elevated by zero-valent iron under low carbon-to-nitrogen ratio

Ze-Tong Feng,Xin Ma,Ying-Jun Sun,Jia-Min Zhou,Zu-Gang Liao,Zhi-Cong He,Fei Ding,Qian-Qian Zhang

The nitrogen removal efficiency and distribution of microbial community in a denitrification process aided by zero-valent iron (ZVI) under low carbon-to-nitrogen ratio (C/N) were assessed in this study. Experimental results demonstrated that the nitrogen removal efficiency (TNRE) increased to 96.4 ± 2.72% and 63.3 ± 4.02% after continuous addition of ZVI with molar ratio of ZVI to nitrate (NO 3 – -N) (ZVI/N) of 6 at C/N of 3 and 2, respectively, which was 4% and 7.7% higher than the blank one. Meanwhile, extracellular polymeric substance (EPS) could be used as electron transfer medium and endogenous carbon source for denitrification system and also the production of which increased by 28.43% and 53.10% under ZVI stimulation compared to the control group. Finally, a symbiotic system composed by autotrophic and heterotrophic denitrification bacteria was formed by aid of ZVI. This study proposed new insights into denitrification process improved by ZVI.

CAS / MDL: 7439-89-6
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Degradation of 1,2,3-trichloropropane in aqueous solution by ZVI-enhanced Fenton system: Performances and mechanisms

Jianxiong Gao,Longbin Zhang,Zhiqiang Xu,Xianxian Sheng,Dexiao Li,Yuantian Chen,Mudassir Habib,Shuguang Lyu

In this research, zero-valent iron (ZVI) was chosen as a reductant in the classic Fenton system to accelerate the generation of Fe(II). The removal of 1,2,3-trichloropropane (TCP) was only 65.3% in classic Fenton system, while with the addition of ZVI its removal could be enhanced to 95.4% in 120 min. Hydroxyl radicals (HO•) was confirmed to be the major radical during TCP degradation by electron paramagnetic resonance (EPR) detection and radical quenching tests. Moreover, the mechanism of TCP degradation in H 2 O 2 /Fe(II)/ZVI system was proposed. In the presence of ZVI, Fe(III) was reduced to Fe(II), further reacted with H 2 O 2 and produced more HO• for TCP removal. 2,3-Dichloro-1-propene and 2-chloro-2-propen-1-ol were the main intermediates in TCP degradation and two possible pathways were proposed. Finally, TCP removal in different solution matrixes and for other chlorinated contaminants removal were tested, revealing the broad-spectrum reactivity and excellent performance of ZVI-enhanced Fenton system in the remediation of chlorinated organic compounds.

CAS / MDL: 7439-89-6
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BIORESOURCE TECHNOLOGY · 2023 · IF 11.4

Achieving efficient methane production from protein-rich organic waste in anaerobic digestion: Using conductive materials or regulating inoculum-to-substrate ratios?

Muxiang Liang,Xiaohai Qin,Qi Chang,Chen Wang,Gang Guo,Xiejuan Lu,Xiaohui Wu,Feixiang Zan

The contribution of inoculum-to-substrate ratios (ISRs) and conductive materials (CMs) on the productivity of anaerobic digestion (AD) remains unclear, particularly for protein-rich organic waste. This study investigated whether the addition of CMs, i.e., biochar and iron powder, can overcome the limitations imposed by varying ISRs for the AD of protein as the sole substrate. Results indicate the ISR plays a decisive role in hydrolysis, acidification, and methanogenesis for protein conversion, irrespective of CMs addition. Methane production increased stepwise as the ISR escalated to 3:1. The addition of CMs provided limited improvement, and iron powder even inhibited methanogenesis at a low ISR. Bacterial community variations were contingent on the ISR, while iron powder supplementation significantly elevates the proportion of hydrogenotrophic methanogen. This study demonstrates that the addition of CMs could affect methanogenic efficiency but can not overcome the limitation of ISRs for the AD of protein.

CAS / MDL: 7439-89-6
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JOURNAL OF ENVIRONMENTAL MANAGEMENT · 2023 · IF 8.7

Zero-valent iron-peroxydisulfate as synergistic co-milling agents for enhanced mechanochemical destruction of 2,4-dichlorophenol: Coupling reduction with oxidation

Ludi Song,Lvren Lin,Wenjia Wei,Shengkun Zhang,Lei Wan,Zimo Lou,Jianming Yu,Xinhua Xu

Mechanochemical (MC) remediation with zero-valent iron (ZVI) as co-milling agent enables the non-combustion and solvent-free disposal of solid halogenated organic pollutants (HOPs) via solid-phase reaction, but suffers from incomplete dechlorination (especially for less chlorinated chemicals). Herein, a reduction-oxidation coupling strategy using ZVI and peroxydisulfate as synergistic (ZVI-PDS) co-milling agents was investigated, with 2,4-dichlorophenol (2,4-DCP) as probe contaminant. By revisiting the MC destruction process of 2,4-DCP by ZVI, the contribution of both reductive and oxidative routes is confirmed, and the inefficient •OH generation is addressed. With ball-to-material and reagent-to-pollutant mass ratios of 30:1 and 13:1, respectively, ZVI-PDS achieves higher dechlorination ratio (86.8%) for 2,4-DCP within 5 h, outcompeting sole ZVI (40.3%) or PDS (33.9%), due to the accumulation of numerous SO 4 •− . As suggested by a two-compartment kinetic model , the optimal ZVI/PDS molar ratio of 4:1 is determined, which balances the relative contribution of reductive/oxidative routes and leads to a maximum mineralization efficiency of 77.4%. The analysis on product distribution verifies the generation of dechlorinated, ring-opening and minor coupling products (with low acute toxicity). This work validates the necessity to couple reduction with oxidation in MC destruction for solid HOPs, and may provide information on reagent formulation.

CAS / MDL: 7439-89-6 75-65-0
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