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Nanosensor quantitative monitoring of ROS/RNS homeostasis in single phagolysosomes of macrophages during bactericidal processes.
IF 4.3 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-04 DOI: 10.1039/d4cc05423g
Bing-Yi Guo, Yu-Ting Qi, Hui-Qian Wu, Ru-Yan Zha, Li-Jun Wang, Xin-Wei Zhang, Wei-Hua Huang

Reactive oxygen and nitrogen species (ROS/RNS) in macrophages have a potent killing effect on pathogens that infect the host. Here, we achieved in situ, quantitative detection of the homeostasis of four primary ROS/RNS (ONOO-, H2O2, NO, and NO2-) and their precursors (O2˙-, NO) in phagolysosomes of single RAW 264.7 macrophages after phagocytosis of Escherichia coli with platinum-black nanoelectrodes. Enhanced bactericidal activity of the macrophages was observed by an increase in the total amount of ROS/RNS as well as the level and proportion of ONOO-, a potent bactericidal species of RNS. Moreover, both the bactericidal process and the steady-state replenishment process were dominated by the production of RNS (NO-based), revealing differences in the enzyme kinetics of the bactericidal process.

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引用次数: 0
Expeditious and environmentally benign synthesis of imidazo[4,5,1-ij]quinolines via sequential Povarov reaction/reductive cyclization.
IF 2.9 3区 化学 Q1 CHEMISTRY, ORGANIC Pub Date : 2024-12-04 DOI: 10.1039/d4ob01588f
Laura A Heredia-Parra, Mónica C Ávila-Murillo, Cristian Ochoa-Puentes

In this contribution, a novel, simple, diastereoselective and environmentally benign two-step diversity-oriented synthesis of imidazo[4,5,1-ij]quinolines is described for the first time. The synthesis of the target compounds involves a deep eutectic solvent-mediated one-pot Povarov reaction leading to the obtention of 8-nitrotetrahydroquinolines, followed by a microwave-assisted reductive cyclocondensation employing different aromatic and aliphatic aldehydes. The target compounds were obtained in up to 70% overall yield starting from commercially available o-nitroanilines, natural phenylpropanoids (trans-anethole and trans-isoeugenol) and aromatic or aliphatic aldehydes. The eutectic solvent employed in the first step was reused in four runs without observing a drastic decrease in catalytic activity, and sodium dithionite showed to be an efficient and green reducing agent for the second step. This methodology provides significant advantages in terms of synthetic and green chemistry such as mild reaction conditions, short reaction time, energy-efficiency, simple work-up procedure, low cost, scalability and utilization of renewable substrates and a reusable solvent.

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引用次数: 0
Jamming crossovers in a confined driven polymer in solution. 溶液中受限驱动聚合物的干扰交叉。
IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-12-04 DOI: 10.1039/d4sm00761a
Setarehalsadat Changizrezaei, Mikko Karttunen, Colin Denniston

We use lattice-Boltzmann molecular dynamics (LBMD) simulations to study the compression of a confined polymer immersed in a fluid and pushed by a large spherical colloid with a diameter comparable to the channel width. We examined the chain's deformation with both purely repulsive and weakly attractive Lennard-Jones (LJ) potentials applied between the monomers. The sphere's velocity was varied over 3 orders of magnitude. The chain is in a non-dense state at low pushing velocities for both repulsive and attractive monomer interactions. When the velocity of the spherical colloid exceeds a threshold v*, the back end of the chain transitions to a high density state with low mean square monomer displacement (MSD) values. The front end, however, remains in a non-dense state with high MSD indicating a pseudo two-state coexistence. This crossover is also revealed through volume per monomer and MSD as a function of the sphere's velocity. We also studied polymer dynamics by investigating folding events at different times.

我们利用晶格-玻尔兹曼分子动力学(LBMD)模拟研究了浸入流体中的受限聚合物在直径与通道宽度相当的大球形胶体推动下的压缩过程。我们在单体间施加了纯排斥和弱吸引伦纳德-琼斯(LJ)势的情况下研究了链的变形。球体的速度变化超过 3 个数量级。在单体间的斥力和吸引力作用下,链在低推动速度时处于非致密状态。当球形胶体的速度超过临界值 v* 时,链的后端会过渡到高密度状态,平均平方单体位移(MSD)值较低。然而,前端仍处于非致密状态,MSD 值较高,这表明存在伪双态共存现象。每单体体积和 MSD 与球速的函数关系也揭示了这种交叉。我们还通过研究不同时间的折叠事件来研究聚合物动力学。
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引用次数: 0
The thickness-dependent response of aerosol-jet-printed ultrathin high-aspect-ratio electrochemical microactuators. 气溶胶喷射打印超薄高宽比电化学微执行器的厚度依赖性响应
IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-12-04 DOI: 10.1039/d4sm00886c
Ji Zhang, Jeremy J Baumberg, Sohini Kar-Narayan

Trilayer electrochemical actuators comprising an electrolyte layer sandwiched between two electrode layers have been shown to exhibit large deformations at low actuation voltages. Here we report the aerosol-jet printing (AJP) of high-aspect-ratio bending-type trilayer electrochemical microactuators comprised of Nafion as the electrolyte and poly(3,4-ethylenedioxythiophene)polystyrene sulfonate (PEDOT:PSS) as the electrode. We investigated how the thicknesses of the electrolyte and electrode layers affect the DC response of these actuators by fabricating high-aspect-ratio trilayer cantilevers with varied layer thicknesses (0.36 μm to 1.9 μm-thick electrodes, and 3.5 μm to 12 μm-thick electrolyte layers). We found that the transported charge and angular deflection are proportional to the applied voltage at steady state, and the charge-to-voltage ratio scales with the PEDOT:PSS thickness. The deflection-to-voltage ratio is found to be strongly affected by the Nafion electrolyte thickness, showing a decreasing trend, but is less affected by the PEDOT:PSS thickness in the range of dimensions fabricated. The timescales for deflection are found to be generally longer than the timescales for charge transfer and no clear trend is observed with respect to layer thicknesses. This work establishes an experimental protocol in geometry optimisation of printed electrochemical microactuators, verifies the applicability of a theoretical model, and lays the groundwork for designing and optimising more sophisticated printed electrochemical microactuation systems.

由夹在两个电极层之间的电解质层组成的三层电化学致动器在低致动电压下表现出较大的变形。在此,我们报告了以 Nafion 为电解质、聚(3,4-亚乙二氧基噻吩)聚苯乙烯磺酸盐 (PEDOT:PSS) 为电极的高纵横比弯曲型三层电化学微致动器的气溶胶喷射打印 (AJP)。我们通过制造具有不同层厚(0.36 μm 至 1.9 μm 厚的电极,以及 3.5 μm 至 12 μm 厚的电解质层)的高纵横比三层悬臂,研究了电解质层和电极层的厚度如何影响这些致动器的直流响应。我们发现,在稳定状态下,传输电荷和角偏转与外加电压成正比,电荷与电压之比随着 PEDOT:PSS 厚度的增加而增大。偏转电压比受 Nafion 电解质厚度的影响很大,呈下降趋势,但在制造的尺寸范围内,受 PEDOT:PSS 厚度的影响较小。研究发现,偏转的时间尺度通常长于电荷转移的时间尺度,而且没有观察到与层厚度有关的明显趋势。这项研究确立了印刷电化学微致动器几何优化的实验方案,验证了理论模型的适用性,并为设计和优化更复杂的印刷电化学微致动系统奠定了基础。
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引用次数: 0
Correction: Controllable biomolecule release from self-assembled organic nanotubes with asymmetric surfaces: pH and temperature dependence. 更正:具有不对称表面的自组装有机纳米管的可控生物分子释放:pH 值和温度依赖性。
IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2024-12-04 DOI: 10.1039/d4sm90187h
Naohiro Kameta, Hiroyuki Minamikawa, Mitsutoshi Masuda, Go Mizuno, Toshimi Shimizu

Correction for 'Controllable biomolecule release from self-assembled organic nanotubes with asymmetric surfaces: pH and temperature dependence' by Naohiro Kameta et al., Soft Matter, 2008, 4, 1681-1687, https://doi.org/10.1039/B803742F.

对 Naohiro Kameta 等人撰写的《具有不对称表面的自组装有机纳米管的可控生物分子释放:pH 值和温度依赖性》的更正,《软物质》,2008 年,4 期,1681-1687,https://doi.org/10.1039/B803742F。
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引用次数: 0
Synthesis of the methyl ester of 17(R/S)-Me-RvD5n-3 DPA and relief of postoperative pain in male mice. 17(R/S)-Me-RvD5n-3 DPA 甲酯的合成及对雄性小鼠术后疼痛的缓解。
IF 2.9 3区 化学 Q1 CHEMISTRY, ORGANIC Pub Date : 2024-12-04 DOI: 10.1039/d4ob01534g
Karina Ervik, Yi-Ze Li, Ru-Rong Ji, Charles N Serhan, Trond V Hansen

The synthesis and biological evaluation of 17(R/S)-Me-RvD5n-3 DPA, an analog of the specialized pro-resolving mediators RvD5 and RvD5n-3 DPA, are presented. The synthesis was successfully accomplished utilizing Midland Alpine borane reduction, Sonogashira cross-coupling and a one-pot hydrozirconation/iodination protocol. In vivo evaluation of RvD5, RvD5n-3 DPA and 17(R/S)-Me-RvD5n-3 DPA in a mouse model of fracture revealed that all three compounds inhibited postoperative pain in male mice, but not in female mice.

本文介绍了 17(R/S)-Me-RvD5n-3 DPA 的合成和生物学评价,它是专门的促溶解介质 RvD5 和 RvD5n-3 DPA 的类似物。该合成利用米德兰阿尔卑斯硼烷还原、Sonogashira 交叉偶联和一锅氢氮化/碘化协议成功完成。在小鼠骨折模型中对 RvD5、RvD5n-3 DPA 和 17(R/S)-Me-RvD5n-3 DPA 进行体内评估后发现,这三种化合物都能抑制雄性小鼠的术后疼痛,但不能抑制雌性小鼠的术后疼痛。
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引用次数: 0
A pH-responsive dual-network biopolysaccharide hydrogel with enhanced self-healing and controlled drug release properties
IF 3.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-04 DOI: 10.1039/D4RA05775A
Yuan Ma, Yunfeng Tang, Jianwei Fan, Tianyu Sun, Xiaoyong Qiu, Luxing Wei and Xiaolai Zhang

Traditional hydrogels based on Schiff base reactions frequently encounter issues with rapid drug release when employed as drug delivery systems owing to their susceptibility to hydrolysis under acidic conditions. It is, therefore, necessary to implement improvements to regulate the drug release behavior. In this study, a dual-network and pH-responsive biopolysaccharide hydrogel was developed, which is self-healing, injectable and biocompatible. Most importantly, the hydrogel has excellent tunability for controlled drug release. The hydrogel consisted of a primary network of dibenzaldehyde-functionalized poly(ethylene glycol) (DP) and chitosan (CS) formed through a Schiff base reaction and a secondary network of sodium alginate (SA) and CS formed through electrostatic interactions. It was found that the DP–CS–2%SA hydrogel can prolong the release duration up to four-fold compared to the single-network DP–CS hydrogel at a given release threshold. Significantly, by adjusting the relationship between the two effects through the amount of SA, the release modifiability of drug delivery systems has been greatly enhanced. This study could significantly enhance the tunability of hydrogel drug delivery systems.

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引用次数: 0
A colorimetric strategy and smartphone-based test strip for the detection of glucose based on the peroxidase activity of a hemin-derived nanozyme.
IF 2.7 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-12-04 DOI: 10.1039/d4ay01878h
Ziqiang Yuan, Meizhen Fu, Xin Wang, Meng Wang, Yue Wei, Yanna Sun, Qingfeng Zhang, Yunyi Zhang, Bo Zhang

Nanozymes are nanomaterials with catalytic properties similar to enzymes and offer advantages over natural enzymes such as lower cost, ease of storage, and convenience for large-scale preparation. Thus, they have received increasing attention and are extensively applied in fields such as chemistry, sensing, food, environment, and medicine. Herein, a hemin-derived nanozyme (Hemin-CDs) was prepared using hemin as the precursor and used to substitute the natural horseradish peroxidase (HRP) for colorimetric detection. The prepared Hemin-CDs exhibit excellent water dispersibility, stability and superior peroxidase-like activity. They catalyze the oxidative coupling of colorless 4-aminoantipyrine (4-AAP) with N-ethyl-N-(2-hydroxy-3-sulfopropyl)-3-methylaniline sodium salt (TOOS) in the presence of H2O2, forming a purple quinone diimine dye with an absorption peak at 554 nm, which enables the quantification of H2O2 by measuring the absorbance. Quantitative detection of glucose was further demonstrated under physiological conditions. The detection of H2O2 and glucose takes only 10 minutes, with linear ranges of 1-150 μM and 2.5-300 μM, and LODs of 0.867 μM and 1.026 μM, respectively. Glucose in human serum was successfully detected with satisfactory recoveries (87.5-104.0%). Furthermore, a test strip was developed, and a smartphone was utilized to recognize the color of the test position, enabling rapid and accurate quantification of glucose concentrations within 5 minutes, which promises to enhance the accessibility and convenience of glucose testing.

{"title":"A colorimetric strategy and smartphone-based test strip for the detection of glucose based on the peroxidase activity of a hemin-derived nanozyme.","authors":"Ziqiang Yuan, Meizhen Fu, Xin Wang, Meng Wang, Yue Wei, Yanna Sun, Qingfeng Zhang, Yunyi Zhang, Bo Zhang","doi":"10.1039/d4ay01878h","DOIUrl":"https://doi.org/10.1039/d4ay01878h","url":null,"abstract":"<p><p>Nanozymes are nanomaterials with catalytic properties similar to enzymes and offer advantages over natural enzymes such as lower cost, ease of storage, and convenience for large-scale preparation. Thus, they have received increasing attention and are extensively applied in fields such as chemistry, sensing, food, environment, and medicine. Herein, a hemin-derived nanozyme (Hemin-CDs) was prepared using hemin as the precursor and used to substitute the natural horseradish peroxidase (HRP) for colorimetric detection. The prepared Hemin-CDs exhibit excellent water dispersibility, stability and superior peroxidase-like activity. They catalyze the oxidative coupling of colorless 4-aminoantipyrine (4-AAP) with <i>N</i>-ethyl-<i>N</i>-(2-hydroxy-3-sulfopropyl)-3-methylaniline sodium salt (TOOS) in the presence of H<sub>2</sub>O<sub>2</sub>, forming a purple quinone diimine dye with an absorption peak at 554 nm, which enables the quantification of H<sub>2</sub>O<sub>2</sub> by measuring the absorbance. Quantitative detection of glucose was further demonstrated under physiological conditions. The detection of H<sub>2</sub>O<sub>2</sub> and glucose takes only 10 minutes, with linear ranges of 1-150 μM and 2.5-300 μM, and LODs of 0.867 μM and 1.026 μM, respectively. Glucose in human serum was successfully detected with satisfactory recoveries (87.5-104.0%). Furthermore, a test strip was developed, and a smartphone was utilized to recognize the color of the test position, enabling rapid and accurate quantification of glucose concentrations within 5 minutes, which promises to enhance the accessibility and convenience of glucose testing.</p>","PeriodicalId":64,"journal":{"name":"Analytical Methods","volume":" ","pages":""},"PeriodicalIF":2.7,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142764575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A rolling circle amplification-based DNAzyme walker against intracellular degradation for imaging tumor cells' microRNA.
IF 4.3 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-12-04 DOI: 10.1039/d4cc05440g
Haoqi Yang, Huimin Niu, Chenxiao Zhao, Shusheng Zhang, Shujuan Sun, Pengfei Shi

We present a novel DNA molecular machine (RCA-D-Walker) that integrates a DNAzyme-based molecular beacon with RCA-based vectors for miRNA imaging in tumor cells. It can accurately target tumor cells through the sgc8 aptamer. The target miRNA can restore the DNAzyme's ability to cleave the substrate, which in turn produces an amplified fluorescent signal. The RCA-D-Walker exhibits enhanced tumor cell targeting, improved cell permeability, and greater resistance to nuclease degradation. Utilizing this strategy, we achieved accurate and efficient imaging of miRNA-21 in tumor cells.

{"title":"A rolling circle amplification-based DNAzyme walker against intracellular degradation for imaging tumor cells' microRNA.","authors":"Haoqi Yang, Huimin Niu, Chenxiao Zhao, Shusheng Zhang, Shujuan Sun, Pengfei Shi","doi":"10.1039/d4cc05440g","DOIUrl":"https://doi.org/10.1039/d4cc05440g","url":null,"abstract":"<p><p>We present a novel DNA molecular machine (RCA-D-Walker) that integrates a DNAzyme-based molecular beacon with RCA-based vectors for miRNA imaging in tumor cells. It can accurately target tumor cells through the sgc8 aptamer. The target miRNA can restore the DNAzyme's ability to cleave the substrate, which in turn produces an amplified fluorescent signal. The RCA-D-Walker exhibits enhanced tumor cell targeting, improved cell permeability, and greater resistance to nuclease degradation. Utilizing this strategy, we achieved accurate and efficient imaging of miRNA-21 in tumor cells.</p>","PeriodicalId":67,"journal":{"name":"Chemical Communications","volume":" ","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142764595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An integrated microfluidic device for sorting of tumor organoids using image recognition.
IF 6.1 2区 工程技术 Q1 BIOCHEMICAL RESEARCH METHODS Pub Date : 2024-12-04 DOI: 10.1039/d4lc00746h
Xingyang Yan, Deng Tan, Lei Yu, Danyu Li, Zhenghao Wang, Weiren Huang, Hongkai Wu

Tumor organoids present a challenge in drug screening due to their considerable heterogeneity in morphology and size. To address this issue, we proposed a portable microfluidic device that employs image processing algorithms for specific target organoid recognition and microvalve-controlled deflection for sorting and collection. This morphology-activated organoid sorting system offers numerous advantages, such as automated classification, portability, low cost, label-free sample preparation, and gentle handling of organoids. We conducted classification experiments using polystyrene beads, F9 tumoroids and patient-derived tumor organoids, achieving organoid separation efficiency exceeding 88%, purity surpassing 91%, viability exceeding 97% and classification throughput of 800 per hour, thereby meeting the demands of clinical organoid medicine.

{"title":"An integrated microfluidic device for sorting of tumor organoids using image recognition.","authors":"Xingyang Yan, Deng Tan, Lei Yu, Danyu Li, Zhenghao Wang, Weiren Huang, Hongkai Wu","doi":"10.1039/d4lc00746h","DOIUrl":"https://doi.org/10.1039/d4lc00746h","url":null,"abstract":"<p><p>Tumor organoids present a challenge in drug screening due to their considerable heterogeneity in morphology and size. To address this issue, we proposed a portable microfluidic device that employs image processing algorithms for specific target organoid recognition and microvalve-controlled deflection for sorting and collection. This morphology-activated organoid sorting system offers numerous advantages, such as automated classification, portability, low cost, label-free sample preparation, and gentle handling of organoids. We conducted classification experiments using polystyrene beads, F9 tumoroids and patient-derived tumor organoids, achieving organoid separation efficiency exceeding 88%, purity surpassing 91%, viability exceeding 97% and classification throughput of 800 per hour, thereby meeting the demands of clinical organoid medicine.</p>","PeriodicalId":85,"journal":{"name":"Lab on a Chip","volume":" ","pages":""},"PeriodicalIF":6.1,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142764709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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