LANGMUIR
·
2024
·
IF 3.7
Xuewei Du,Wanxue Zhang,Suyan Yi,Shaoguang Li,Hui Li,Fan Xia
Rapid, reagent-free, and ultrasensitive analysis of cardiac troponin I (cTnI) is of significance for early diagnosis of acute myocardial infarction (AMI). The electrochemical aptamer-based (EAB) sensors are promising candidates to fill this role as they are reagentless and can be directly interrogated in complex matrices (e.g., blood). To achieve high sensitivity, EAB sensors typically require nanomaterials or other amplification strategies, which often involves a cumbersome fabrication process. To circumvent this, here we develop a simple yet effective electrocatalytic electrochemical aptamer-based (Ec-EAB) sensor that utilizes target-induced regulation of the catalytic mechanism to achieve ultrasensitive measurement of cTnI. In this assay, we employed a probe-attached redox reporter (i.e., methylene blue, MB) and a solution-diffusive redox reporter (i.e., Fe(CN)63–) to generate two signals, of which the latter is used to catalyze MB to amplify aptamer-mediated charge transfer. The recognition of target altered the diffusion of catalysts (2.2 × 10–9 mol/cm2 in the target-free state versus 1.2 × 10–9 mol/cm2 in the target-bound state) and thus electrocatalytical efficiency, enabling ultrasensitive measurement of cTnI with a 1000-fold improvement in their sensitivity (a limit of detection value: 10 pg/mL).
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高影响因子
ACS Sensors
·
2024
·
IF 8.2
Lin He,Yan Zhou,Min Zhang,Mingjian Chen,Yuchen Wu,Lanlin Qi,Lamei Liu,Bin Zhang,Xiaohai Yang,Xiaoxiao He,Kemin Wang
Detection of slight pH changes in skin interstitial fluid (ISF) is crucial yet challenging for studying pathological processes and understanding personal health conditions. In this work, we construct an i-motif DNA based fluorescent ratiometric microneedle sensing patch (IFR-pH MN patch) strategy that enables minimally invasive, high-resolution, and sensitive transdermal monitoring of small pH variations in ISF. The IFR-pH MN patch with advanced integration of both ISF sampling and pH sensing was fabricated from the cross-linking of gelatin methacryloyl and methacrylated hyaluronic acid, wrapping with pH-sensitive hairpin-containing i-motif DNA based fluorescent ratiometric probes in the matrix. Because it is mechanically robust for skin penetration and has high swelling ability, the IFR-pH MN patch could be quickly extracted as sufficient liquid from agarose gel (∼56.4 μL in 10 min). Benefiting from conformation changes of the hairpin-containing i-motif DNA under pH variation and ratiometric fluorescence signal readout, the IFR-pH MN patch could quantitate pH over a small range between pH 6.2 and 6.9 with an accuracy of 0.2 pH units in the mimic skin model. Furthermore, in vivo testing on wound and tumor mouse models indicated the ability of the biocompatible IFR-pH MN patch to penetrate the skin for obtaining transdermal pH values, demonstrating the potential applications in monitoring and intervention of pathological states.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yonghou Xiao,Qiang Guo,Shuohan Yang,Qidong Zhao,Gaohong He
The cuprous-ion-based zeolites constructed by introducing Cu(I) adsorption active sites into zeolite Linde Type A have proved to be efficient in carbon monoxide (CO) adsorption with high selectivity and capacity. However, how to directly fabricate zeolite 4A containing copper species and effectively overcome cuprous ion aggregation during the preparation process is still a challenge. Here, we propose an efficient fabrication method to synthesize highly dispersed Cu(I)-modified octahedral zeolite 4A adsorbents using a molecular complex formed by a hydrogel with a silicon/aluminum molar ratio of 1:1, copper ions, and tetramethylammonium hydroxide (TMAOH) as the template. Zeolite 4A containing copper ions was directly obtained by incorporating the precursor of cuprous ions into the confined space between zeolite 4A channel walls and TMAOH. The target zeolite Cu(I)/4A adsorbent with highly dispersed Cu(I) was constructed after introducing VCl3 as the reducing agent via the solid-state dispersion method during the process of removing the template. In comparison with pristine zeolite 4A, a bimodal microporous pore size distribution was observed in as-synthesized Cu(I)/4A. Cu(I)/4A exhibited an enhanced static (1.15 mmol/g) and dynamic (0.0016 mmol g−1) CO adsorption capacity, respectively, at 25 °C and 1 bar. Moreover, Cu(I)/4A displayed a lower H2 adsorption capacity under identical conditions. Through calculation using the ideal adsorption solution theoretical (IAST) equation, the CO selectivity from the CO/H2 mixture on Cu(I)/4A attained ca. 16.95. Therefore, Cu(I)/4A with highly dispersed Cu(I) was successfully fabricated, and its excellent CO adsorption selectivity and capacity enable it to be potentially applied for the actual deep separation of CO/H2.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Bin Pan,Yang Jin,Yan Chen,Juan Wang,Kangnan Wang,Sunfang Chen,Mingyang Lei,Wenguo Cui,Junjie Li,Yu Qian
The widespread abuse of antibiotics has led to the emergence of drug-resistant bacterial strains, severely complicating the treatment of infectious wounds. Traditional therapies are often limited to antibacterial or anti-inflammatory approaches, making it challenging to manage both early-stage infection and later-stage tissue regeneration simultaneously. Herein, a Cu 2−x Se nanoparticles (CSNPs) spray containing mixed-valence copper ions, enabling the programmed healing of infectious wounds is developed through light-controlled cascade regulation. In the early infection stages, the copper ions released from CSNPs exert antibacterial effects via chemodynamic therapy (CDT), with their activity significantly enhanced under near-infrared (NIR) irradiation. At later stages, Cu 2+ /Cu + ions enter cells, interact with cysteine residues in KEAP1 protein, and induce conformational changes, triggering deubiquitinase activity and suppressing macrophage-driven inflammation. Findings from in vitro and in vivo studies consistently revealed that CSNPs efficiently depleted glutathione and enhanced H 2 O 2 breakdown, leading to the generation of •OH and O 2 •- under NIR exposure, which resulted in an MRSA elimination rate exceeding 99%. Mechanistically, CSNPs bind to KEAP1, removing the ubiquitin linkage from NRF2, thereby inhibiting inflammation. This CSNPs spray provides a dual synergistic effect of antimicrobial and tissue-regenerative properties, offering an innovative approach for treating antibiotic-resistant infections in wounds.
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ACS Nano
·
2025
·
IF 16
Xiang Jiang,Lina Sun,Yuewu Zhao,Zhiyong Lu,Xuan He,Ying Xiang,Xingzhu Liu,Jine Wang,Renjun Pei
Sonodynamic therapy (SDT) has demonstrated promising potential in the treatment of tumors and has attracted widespread attention. The majority of sound-sensitive materials developed to date have been categorized as oxygen-dependent type II sonosensitizers (SSs), which are susceptible to tumor hypoxia and significantly limit their efficacy. In this study, highly active porphyrin-based metal–organic frameworks (Yb-TCPP PMOF) with type I/II SDT dual actions were constructed by regulating the electron transfer process between metal nodes and ligands, which can produce multiple reactive oxygen species (ROS) such as 1O2, O2•–, and •OH. After that, the energy level barrier of triplet SSs was reduced by in situ loading of Au nanoparticles with the electronic grab-transport (EGT) effect, and the ROS yield was increased by accelerating the electron transport. Intriguingly, the successful construction of Au/Yb-TCPP not only produced abundant oxygen vacancy defects but also reduced the band gap, which effectively facilitated the electron–hole separation of SSs and further improved the SDT efficiency by inhibiting its recombination process. Furthermore, we also found that these ultrasmall Au nanoparticles in the MOF structure can act as catalase and undergo cascade reactions with glucose oxidase and obtain a self-producing oxygen circulation system (Au/Yb-TCPP@GOx) by reducing glucose through the coordination of nanoenzyme and bioenzyme. This not only significantly alleviates the hypoxia state of tumors but also has a starvation effect on tumor cells. Finally, it was verified at the levels of tumor cells and mice that Au/Yb-TCPP@GOx can effectively inhibit tumors through the dual effects of enhanced type I and type II SDT, as well as the starvation effect. The composite materials constructed showed a multisynergistic enhancement effect, which has guiding significance for improving electron transport, alleviating tumor hypoxia, enhancing ROS yield, and constructing starvation treatment strategies.
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ANALYTICAL CHEMISTRY
·
2025
·
IF 6.7
Qingwei Song,Zixuan Liao,Lin Zheng,Pan Fu,Sihua Qian,Wei Liang,Jianping Zheng,Kaizhe Wang,Yuhui Wang
Fluorescence lateral flow immunoassays (FL-LFIA) have attracted considerable attention in clinical diagnosis due to their outstanding merits of affordable, sensitive, on-site, and quick detection. However, they are still plagued by significant signal interference, such as autofluorescence and scattered light. The development of high-performance and robust phosphors, i.e., label probes featuring with the character of low/no optical background, remains a great challenge. Herein, we report a novel visualized phosphorescence LFIA (Phos-LFIA), where the composite microspheres, i.e., carbon dots (CDs) covalently embedded in dendritic mesoporous silicon nanoparticles (DMSNs), were designed and selected as the report probes. The obtained CDs@DMSNs revealed uniform morphologies and particle sizes, as well as ultralong (lifetime: 1.14 s, visible for over 8 s to naked eyes) room temperature phosphorescence (RTP) in aqueous solution. As competitive nanotags, CDs@DMSNs were designed for an ultralong phosphorescence-based time-gated LFIA for cardiac troponin I (cTnI) without optical interference. The fabricated Phos-LFIA test strips demonstrated zero-background signal and were applied for highly sensitive cTnI detection in both buffer and a complex serum matrix, with corresponding limits of detection (LODs) of 0.19 and 0.21 ng/mL, respectively. For a clinical validation, the proposed Phos-LFIA revealed an excellent clinical analytical performance (sensitivity: 95.45%, specificity: 88.9%, κ value: 0.85), demonstrating its potential for rapid and accurate diagnosis of myocardial infarction. This work provided a promising background-free probe for FL-LFIA, and it would also open an opportunity for developing highly sensitive screening platforms for other targets through modifying different recognition ligands onto CDs@DMSNs.
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高影响因子
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Zhenjie Zheng,Jiarong Lin,Junyi Zhang,Fang Luo,Zuquan Weng,Jian Wang,Cuiying Lin,Bin Qiu,Zhenyu Lin,Hao Lin
Herein, we present the development of an ultra-sensitive immobilization-free homogeneous electrochemiluminescence (ECL) biosensor, leveraging the electrostatic repulsion between a negatively charged indium tin oxide (ITO) electrode and DNA and exonuclease I (Exo I)-powered signal amplification, to achieve highly efficient detection of thrombin. Specifically, the aptamer and the complementary DNA engage in the formation of a double-stranded DNA (dsDNA) complex. This negatively charged dsDNA structure subsequently associates with a positively charged ECL indicator, namely ruthenium phenanthroline (Ru(phen) 3 2+ ), resulting in the generation of the dsDNA-Ru(phen) 3 2+ ECL probe. The negatively charged dsDNA-Ru(phen) 3 2+ experiences electrostatic repulsion from the negatively charged ITO electrode, resulting in a low ECL signal. Nonetheless, upon the addition of thrombin, the aptamer preferentially binds to thrombin, triggering the releases of the embedded Ru(phen) 3 2+ facilitated by Exo I and hence resulting in a robust and enhanced ECL signal. The amplified ECL signal is linearly correlated with the logarithm of thrombin concentration within a detection range spanning from 10 fmol/mL to 50 pmol/mL, with a remarkable detection limit of 3.21 fmol/mL. This strategy eliminates the need for cumbersome labeling steps, avoids the electrode modification process, overcoming the low immobilization efficiency of aptamers and poor signal transduction of indicators labeled at the end of DNA.
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Advanced Science
·
2024
·
IF 14.3
Junce Wang,Jinfeng Chen,Ningning Liu,Jingjing Lei,Hong-Wen Gao,Fei Yu,Fanghui Pan,Jie Ma
Controlled synthesis and regulation of 2D nanomaterials with sufficient active sites are promising in electrochemical fluorine capture, but simultaneously achieving rapid rates and efficient activity of intercalation materials remains challengs. Herein, an integrated strategy of micro-regulation interlayer space and in situ modification of MXenes is proposed to enhance ion storage kinetics. The wedge-like microstructure of aluminum oxide/incomplete-Ti 3 C 2 T x MXene (Al 2 O 3 /i-Ti 3 C 2 T x ) is constructed by incomplete etching MAX and in situ derivation of A-layer element, in which the sub-nanoscale interlayer space is conducive to the small size ions intercalation, and the formation of “nanopump-like” effect boosted the ions diffusion. As evidenced by simulation calculations, Al 2 O 3 nanoparticles not only shorten the migration distance of electrons/hydrated ions in interlayers but also contribute a lower adsorption energy barrier, bringing excellent capture kinetics and stability. Benefiting from the interfacial conversion-intercalation pseudocapacitance, such electrode is endowed with a high defluoridation capacity (69.9 mg g −1 at 1.6V) and an outstanding instantaneous adsorption rate (9.51 mg g −1 min −1 ), and shows satisfactory stability in more than 200 cycles. The physicochemical coupling strategy opens a novel approach to optimizing the interlayer structure and in situ modification interface of MXene, which also provids a universal idea for efficient capture of varisized ions of intercalation materials.
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CARBOHYDRATE POLYMERS
·
2024
·
IF 10.7
Jinwen Huang,Huiqi Wang,Huaqun Chen,Zidong Liu,Xuedong Zhang,Hao Tang,Shiying Wei,Wangting Zhou,Xinzhou Yang,Yonghong Liu,Longyan Zhao,Qingxia Yuan
Avicennia marina (Forssk.) Vierh. is a highly salt-tolerant mangrove, and its fruit has been traditionally used for treating constipation and dysentery . In this study, a pectin (AMFPs-0-1) was extracted and isolated from this fruit for the first time, its structure was analyzed, and the effects on the human gut microbiota were investigated. The results indicated that AMFPs-0-1 with a molecular weight of 798 kDa had a backbone consisting of alternating →2)-α-L-Rha p -(1→ and →4)-α-D-Gal p A-(1→ residues and side chains composed of →3-α-L-Ara f -(1→-linked arabinan with a terminal β-L-Ara f , →5-α-L-Ara f -(1→-linked arabinan, and →4)-β-D-Gal p -(1→-linked galactan that linked to the C-4 positions of all α-L-Rha p residues in the backbone. It belongs to a type I rhamnogalacturonan (RG-I) pectin but has no arabinogalactosyl chains. AMFPs-0-1 could be consumed by human gut microbiota and increase the abundance of some beneficial bacteria, such as Bifidobacterium , Mitsuokella , and Megasphaera , which could help fight digestive disorders . These findings provide a structural basis for the potential application of A. marina fruit RG-I pectic polysaccharides in improving human intestinal health.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Lin Yang,Canzhi Shi,Bohan Li,Xia Liu,Xinxiang Gao,Yani Li,Yan Xu
The family of copper-based metal halides has drawn increasing attention owing to their structural flexibility and optical tunability. However, the controllable synthesis of isomers to further regulate luminescence reasonably and thoroughly understand the structure–luminescence–performance relationship remains a challenge. In this work, a pair of isomers of the hybrid copper iodide 4-BrBTP(Cu2I4)0.5 (1-α and 1-β, 4-BrBTP = (4-bromobenzyl)triphenylphosphonium bromide) were synthesized using the same precursors but varying the solvents and molar ratios. The Br⋯π and Br⋯I interactions of the bromobenzyl group may be considered as the driving forces for the growth of these two isomers. 1-α exhibits orange emission centered at 601 nm, while 1-β shows yellow emission centered at 552 nm at room temperature. Particularly, 1-α could be transformed into 1-β by soaking in methanol, accompanied by photoluminescence switching from orange to yellow. The experiments reveal that the orange light of 1-α stems from self-trapped exciton (STE) emission, whereas the yellow emission of 1-β is attributed to metal-to-ligand charge transfer or halide-to-ligand charge transfer (MLCT/HLCT) and cluster-centered (CC) excited states. Taking advantage of their water stability, the performance of the two isomers was evaluated in detecting the antibiotic furaltadone hydrochloride (FTD) in water. The results showed that 1-α has a detection limit that is an order of magnitude lower than that of 1-β. Furthermore, the spectral overlap between the FTD and two isomers combined with the theoretical calculations of energy levels was conducted to clarify the potential sensing mechanisms. This work achieved luminescence regulation between copper iodide isomers, laying the foundation for the development of 0D organic–inorganic hybrid metal halide (OIMH) luminescent sensors and promoting their potential application in detecting antibiotics in real samples.
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Advanced Science
·
2022
·Vol. 9
·期 26
·2201573
·
IF 17.521
Fangwen Cheng,Fang Cao,Binwen Chen,Xinfeng Dai,Ziheng Tang,Yifei Sun,Jun Yin,Jing Li,Nanfeng Zheng,Binghui Wu
Power conversion efficiency (PCE) and long-term stability are two vital issues for perovskite solar cells (PSCs). However, there is still a lack of suitable hole transport layers (HTLs) to endow PSCs with both high efficiency and stability. Here, NiO x nanoparticles are promoted as an efficient and 85 °C/85%-stable inorganic HTL for high-performance n-i-p PSCs, with the introduction of perovskite quantum dots (QDs) between perovskite and NiO x as systematic interfacial engineering. The QD intercalation enhances film morphology and assembly regulation of NiO x HTLs . Due to structure–function correlations, hole mobility within NiO x HTL is improved. And the hole extraction from perovskite to NiO x is also facilitated, resulting from reduced trap states and optimized energy level alignments. Hence, the promoted NiO x -based n-i-p PSCs exhibit high PCE (21.59%) and excellent stability (sustaining 85 °C aging in air without encapsulation). Furthermore, encapsulated solar modules with QDs-promoted NiO x HTLs show impressive stability during 85 °C/85% aging test for 1000 hours. With high transparency, QDs-promoted NiO x is also demonstrated to be an advanced HTL for semitransparent PSCs. This work develops promising NiO x inorganic HTL in n-i-p PSCs for manufacturing next-generation photovoltaic devices.
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Molecular Catalysis
·
2025
·
IF 4.9
Haoyu Jia,Jinyue Hu,Le Zhao,Xiaoke Zheng,Weisheng Feng
Baohuoside I, a valuable flavonoid derivative of Herba Epimedii , exhibits superior bioactivities compared to its precursor, icariin. The conversion of icariin to baohuoside I using β-glucosidase (β-G) is an efficient approach for industrial production. Herein, β-G was successfully immobilized into a porous materials metal-organic frameworks (MOFs) via a simple one-pot coprecipitation method. The β-G@MOF biocomposite exhibited high encapsulation efficiency and excellent tolerance to extreme pH, high temperature, organic solvent and glucose. Remarkably, β-G@MOF retained its full initial activity even at 200 mM glucose. The β-G@MOF has a lower K m value compared with the free β-G, indicating enhanced substrate affinity. A conversion of 99.8 % was achieved in the hydrolysis of icariin to baohuoside I within 2 h. Additionally, β-G@MOF exhibited significantly reusability, maintaining 70.5 % yield after eight cycles at 60 °C. This study provides a simple, efficient, and sustainable approach for industrial production of baohuoside I and has potential for hydrolyzing other poorly soluble flavonoids.
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