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Hierarchically porous films for ultrahigh-throughput characterization of chemical exposome in biological fluids 用于超高通量表征生物液体中化学暴露体的分层多孔薄膜
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-02 DOI: 10.1016/j.xcrp.2024.102136

Exposome science captures the totality of environmental drivers of human health. However, the comprehensive determination of numerous exogenous and endogenous compounds remains extremely challenging, restricting the purpose of exposome science to characterize both external and internal exposure. Herein, we develop hierarchically porous polymers of intrinsic microporosity (HPPIM) films to achieve ultrahigh-throughput determination of exo/endogenous molecules in biological fluids. The film’s porous properties, including three-stage micro-submicro-nanometer architectures, large specific surface area, and appropriate pore geometry and organophilicity enable fast molecular transport and high trapping capability, therefore achieving ultrahigh-throughput determination of exo/endogenous molecules in biological fluids. Further application in a small-scale cancer study demonstrates the unique advantages of HPPIM films over existing techniques, including broad coverage of analytes, satisfactory trapping efficiency, low-volume demand on specimens, high simplicity and reusability, and drastically reduced financial cost. Our work demonstrates the great potential of HPPIM for advancing exposome science from concept to utility.

暴露组科学捕捉到了影响人类健康的全部环境因素。然而,全面测定众多外源性和内源性化合物仍然极具挑战性,这限制了暴露组科学用于表征外部和内部暴露的目的。在此,我们开发了具有内在微孔的分层多孔聚合物(HPPIM)薄膜,以实现超高通量测定生物液体中的外源性/内源性分子。该薄膜的多孔特性,包括三级微亚微纳结构、大比表面积、适当的孔几何形状和亲有机性,可实现快速分子传输和高捕获能力,从而实现生物液体中外源性/内源性分子的超高通量测定。在一项小规模癌症研究中的进一步应用证明了 HPPIM 薄膜相对于现有技术的独特优势,包括对分析物的广泛覆盖、令人满意的捕获效率、对标本的低容量需求、高度简便性和可重复使用性以及大幅降低的经济成本。我们的工作证明了 HPPIM 在推动暴露组科学从概念走向实用方面的巨大潜力。
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引用次数: 0
Investigation of the impact of different electrode inhomogeneities on the voltage response of Li-ion batteries 不同电极不均匀性对锂离子电池电压响应影响的研究
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-02 DOI: 10.1016/j.xcrp.2024.102138

As commercial batteries and battery packs become larger and larger, one topic that is gaining interest is that of cell-to-cell variations and inhomogeneities. In this theoretical study, we use a degradation mode model along with a segmented cell approach to investigate the impact of different inhomogeneity modes on the performance of two typical Li-ion batteries. This unique approach shows that out of the nine considered modes (state of charge, rate, resistance, and capacity for each electrode as well as their offset), when at a mild level and randomly distributed, only three could affect performance, with two unlikely to happen in real cells because they would disappear during rest. Model results show that some of these inhomogeneities open the possibility of a snowball effect to induce local rate variations and lithiation inhomogeneities. Our study also shows that it is necessary to assess the level at which the paralleling occurs, electrode or full cell, as the model predicts an impact on how the current, and how much of it, is flowing within or in between the electrodes.

随着商用电池和电池组的体积越来越大,电池单元之间的变化和不均匀性日益受到关注。在这项理论研究中,我们使用退化模式模型和分段电池方法来研究不同不均匀性模式对两种典型锂离子电池性能的影响。这种独特的方法表明,在所考虑的九种模式(每个电极的充电状态、速率、电阻和容量以及它们的偏移)中,当处于温和水平且随机分布时,只有三种模式会影响性能,其中两种在实际电池中不太可能发生,因为它们会在静止时消失。模型结果表明,其中一些不均匀性可能会产生雪球效应,诱发局部速率变化和锂化不均匀性。我们的研究还表明,有必要评估发生并联的层次,是电极还是整个细胞,因为模型预测会影响电流在电极内或电极间流动的方式和程度。
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引用次数: 0
Yarn-grouping weaving soft robotics with directional inflation, bilateral bending, and self-sensing for healthcare 具有定向充气、双侧弯曲和自感应功能的纱线编织软机器人,可用于医疗保健领域
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.xcrp.2024.102137

Pneumatic soft robotics are highly desirable for interacting with humans and navigating uncertain environments. However, it remains a great challenge to simultaneously achieve high actuation efficiency, programmable deformations, real-time feedback, and robustness. Herein, a textile engineering approach is harnessed to integrate multifunctionality into woven actuators by tailoring yarn groupings using all-in-one industrial weaving technologies. The unique nearly zero Poisson’s ratio inflatable deformation of the actuators contributes to a large bending strain (2,250° m−1), a high output force (30 N MPa−1), and robust mechanical performance. Bilateral bending actuators with negative, zero, and positive curvatures are realized by hierarchical shape transformations of the woven layers. The embedded sensing yarns provide facile and effective methods to proprioceptively sense actuation deformation without compromising actuation performance. Moreover, this manufacturing method is cost efficient and highly scalable, which expands practical applications of soft actuators in healthcare and offers a new perspective on the structure design of customized soft actuators.

气动软机器人技术在与人类互动和在不确定环境中导航方面非常理想。然而,同时实现高传动效率、可编程变形、实时反馈和鲁棒性仍然是一项巨大挑战。在此,我们利用纺织工程方法,通过一体化工业编织技术定制纱线组,将多功能性集成到编织致动器中。致动器独特的近零泊松比充气变形有助于实现大弯曲应变(2,250° m-1)、高输出力(30 N MPa-1)和稳健的机械性能。通过编织层的分层形状变换,实现了具有负曲率、零曲率和正曲率的双侧弯曲致动器。嵌入式传感纱线为本体感知致动器变形提供了简便有效的方法,同时不会影响致动器的性能。此外,这种制造方法还具有成本效益和高度可扩展性,从而扩大了软致动器在医疗保健领域的实际应用,并为定制软致动器的结构设计提供了新的视角。
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引用次数: 0
One-pot transition-metal-free synthesis of alkynes and enynes 炔烃和炔烃的单锅无过渡金属合成
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-01 DOI: 10.1016/j.xcrp.2024.102132
Alkynes are key motifs in chemistry, serving as precursors in many organic reactions toward the synthesis of bioactive compounds, polymers, and new ma…
炔烃是化学中的关键主题,在许多有机反应中都是合成生物活性化合物、聚合物和新材料的前体。
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引用次数: 0
Online multi-scenario impedance spectra generation for batteries based on small-sample learning 基于小样本学习的电池多场景阻抗谱在线生成
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-31 DOI: 10.1016/j.xcrp.2024.102134

The onboard acquisition of data from electrochemical impedance spectroscopy (EIS) is critically important to the state assessment and fault diagnosis of mobile batteries, but it is technically challenging due to the stringent test requirements, limited modeling data, and varying mechanisms among batteries with different chemistries. This paper, without requiring any additional sensors, extends the traditional EIS measurement to online generation and covers most battery-using scenarios, including different battery chemistries, aging degrees, remaining capacities, and temperatures. Virtual simulation and transfer techniques are employed to train a deep neural network with a significantly reduced dataset. Specifically, we train the network with no more than 24 groups of data and achieve an average relative error lower than 5%, outperforming most “big data”-involved algorithms of its kind. Our method lowers the threshold of using EIS onboard and unlocks new opportunities to monitor the battery’s performance in both time and frequency domain comprehensively in real time.

车载电化学阻抗谱(EIS)数据采集对于移动电池的状态评估和故障诊断至关重要,但由于测试要求严格、建模数据有限以及不同化学成分电池的机理各不相同,因此在技术上极具挑战性。本文不需要任何额外的传感器,就能将传统的 EIS 测量扩展到在线生成,并涵盖大多数电池使用场景,包括不同的电池化学成分、老化程度、剩余容量和温度。本文采用虚拟仿真和转移技术,利用大幅减少的数据集训练深度神经网络。具体来说,我们使用不超过 24 组数据训练网络,平均相对误差低于 5%,优于大多数涉及 "大数据 "的同类算法。我们的方法降低了车载 EIS 的使用门槛,为实时全面监控电池在时域和频域的性能带来了新的机遇。
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引用次数: 0
Purely electrical detection of electrolyte concentration through microfluidic impedance spectroscopy 通过微流控阻抗能谱对电解质浓度进行纯电检测
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-30 DOI: 10.1016/j.xcrp.2024.102133

Impedance spectroscopy enables the electrical properties of samples to be probed and is commonly used to characterize solids. Extending this technique to analyze fluids within microfluidic channels could enable the rapid characterization of bodily fluids such as sweat. Here, we present a low-cost microfluidic platform with integrated aerosol-jet printed electrodes for the electrical characterization of fluids via impedance spectroscopy. A novel analysis method is presented to accurately determine the concentration of several aqueous ionic chloride solutions, namely NaCl, KCl, CaCl2, and MgCl2. Importantly, we identify a key parameter, the turning point frequency of the capacitance-frequency graph, which is found to have a highly linear correlation with the solution concentration for each species spanning at least three orders of magnitude. This linear dependence is highly reproducible across different cationic species, making it useful for accurate fluid characterization. Applying this technique to analyze bodily fluids in real time has implications for remote health monitoring.

阻抗光谱法可探测样品的电特性,常用于表征固体。将这一技术扩展到分析微流体通道内的流体,可实现对汗液等体液的快速表征。在这里,我们介绍了一种集成气溶胶喷射印刷电极的低成本微流控平台,用于通过阻抗光谱法对流体进行电学表征。我们提出了一种新颖的分析方法,可准确测定几种离子氯化物水溶液(即 NaCl、KCl、CaCl2 和 MgCl2)的浓度。重要的是,我们确定了一个关键参数,即电容-频率图的转折点频率,发现该频率与每种物质的溶液浓度高度线性相关,至少跨越三个数量级。这种线性关系在不同的阳离子物种之间具有很高的重现性,因此可用于准确的流体表征。应用这种技术实时分析体液对远程健康监测具有重要意义。
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引用次数: 0
Large-scale synthesis of transition metal dichalcogenides at atmospheric pressure in air 在常压空气中大规模合成过渡金属二钙化物
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-30 DOI: 10.1016/j.xcrp.2024.102124

Transition metal dichalcogenides (TMDs) have received considerable attention in recent years because of their intriguing chemical and physical properties. However, conventional synthesis methods, including chemical vapor deposition and wet-chemical synthesis, still face many challenges in mass production. Here, we develop a dynamic salt capsulation method to massively prepare TMDs (MoS2, WS2) at atmospheric pressure in air with a high yield of over 95%. With the help of binary salts (KCl, KBr), TMDs can be easily obtained for a short reaction time of 1 h at a relatively low temperature (400°C). The as-synthesized MoS2 powders show flower-like nanospheres, which exhibit a desired catalytic performance in hydrogen evolution reactions and good electrochemical performance as anode materials in lithium-ion batteries. This work provides a simple method to synthesize high-quality and large quantities of TMDs with low cost and time consumption, which has a great potential to integrate into industrial production.

近年来,过渡金属二卤化物(TMDs)因其引人入胜的化学和物理特性而受到广泛关注。然而,包括化学气相沉积和湿化学合成在内的传统合成方法在大规模生产中仍面临诸多挑战。在此,我们开发了一种动态盐封方法,可在常压空气中大规模制备 TMDs(MoS2、WS2),产率高达 95% 以上。借助二元盐(KCl、KBr),在相对较低的温度(400°C)下,只需 1 小时的短反应时间,即可轻松获得 TMD。合成的 MoS2 粉末呈花朵状纳米球,在氢气进化反应中具有理想的催化性能,作为锂离子电池的负极材料具有良好的电化学性能。这项工作提供了一种低成本、低耗时、高质量、大量合成 TMDs 的简单方法,具有融入工业生产的巨大潜力。
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引用次数: 0
Fluidic control programming for 3D magnetic soft metamaterials with reconfigurable mechanical behaviors 具有可重构机械行为的三维磁性软超材料的流体控制编程
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1016/j.xcrp.2024.102125

Active mechanical metamaterials are an attractive proposition for soft robotics, electronic devices, and biomedical devices. However, the utilization of their uncommon physical and mechanical behaviors remains underexplored because existing fabrication processes limit the decoupling of structural frameworks from the responsive mechanisms. Here, we propose a multi-step fluidic control programming strategy by fabricating three-dimensional (3D) magnetic soft materials (MSMs) with reconfigurable mechanical metamaterial behaviors, enabling magnetic-field-driven alteration between three different geometry modes in a single structure. The MSM lattices exhibit fast 3D transitions between positive (νmax = 3.41) and negative (νmax = −2.64) Poisson’s ratios. We then create MSMs with reconfigurable orthotropic behaviors, which demonstrate the positive and negative Poisson’s effect in perpendicular planes. In further demonstrations, the fast and wireless response is validated by manipulating falling loads and switching the states of electrical circuits. This research provides a controllable workflow for future magnetic soft metamaterials.

对于软机器人、电子设备和生物医学设备而言,主动机械超材料是一个极具吸引力的命题。然而,由于现有的制造工艺限制了结构框架与响应机制的解耦,对其不常见的物理和机械行为的利用仍未得到充分探索。在这里,我们提出了一种多步骤流体控制编程策略,通过制造具有可重新配置机械超材料行为的三维(3D)磁性软材料(MSM),在单一结构中实现磁场驱动的三种不同几何模式之间的改变。MSM 晶格在正(νmax = 3.41)和负(νmax = -2.64)泊松比之间表现出快速的三维转换。然后,我们创建了具有可重构各向同性行为的 MSM,在垂直平面上展示了正负泊松效应。在进一步的演示中,我们通过操纵下落负载和切换电路状态,验证了快速无线响应。这项研究为未来的磁性软超材料提供了一个可控的工作流程。
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引用次数: 0
Enhancing RNA inhibitory activity using clamp-G-modified nucleobases 利用钳夹-G修饰的核碱基增强 RNA 抑制活性
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1016/j.xcrp.2024.102120

We explore the potential of clamp-G nucleobase-modified peptide nucleic acids (cGPNAs) as microRNA and messenger RNA inhibitors. For proof of concept, we target miR-155, which is upregulated in diffuse large B cell lymphoma. cGPNA shows significant downregulation of miR-155 and the upregulation of its downstream targets in multiple lymphoma cell lines. Also, cGPNA treatment in vivo reduced tumor growth and improved survival in the U2932 cell-derived xenograft mouse model. To assess the broad application of cGPNA as an antisense modality, we also target transthyretin (TTR) mRNA. We establish a dose-dependent effect of antisense cGPNA on TTR mRNA levels. For in vivo studies, we conjugated cGPNA-based TTR antisense with lactobionic acid-based targeting ligand for in vivo liver delivery. We establish that cGPNA exhibits significant TTR protein knockdown compared to unmodified peptide nucleic acid (PNA) in vivo. Overall, we confirm that clamp-G-modified PNA analogs are a robust antisense therapy platform.

我们探索了钳形核糖核酸修饰多肽核酸(cGPNA)作为 microRNA 和信使 RNA 抑制剂的潜力。为了验证这一概念,我们以弥漫大 B 细胞淋巴瘤中上调的 miR-155 为靶点。在多个淋巴瘤细胞系中,cGPNA 显示出对 miR-155 的显著下调及其下游靶点的上调。此外,在 U2932 细胞衍生异种移植小鼠模型中,体内 cGPNA 治疗可减少肿瘤生长并提高存活率。为了评估 cGPNA 作为反义方式的广泛应用,我们还以转甲状腺素(TTR)mRNA 为靶点。我们建立了反义 cGPNA 对 TTR mRNA 水平的剂量依赖性效应。在体内研究中,我们将基于 cGPNA 的 TTR 反义与基于乳糖酸的靶向配体共轭,用于体内肝脏递送。我们证实,与未修饰的肽核酸(PNA)相比,cGPNA 在体内可显著敲除 TTR 蛋白。总之,我们证实钳夹-G修饰的PNA类似物是一种强大的反义治疗平台。
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引用次数: 0
High-volumetric pseudocapacitive sodium storage in densely packed mesoporous titanium dioxide-carbon composite 在致密介孔二氧化钛-碳复合材料中储存高容积伪电容钠
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-26 DOI: 10.1016/j.xcrp.2024.102123

Transition metal oxides with small grain sizes are promising candidates for capacitive charge storage. However, the overall performance of such oxide materials is still limited by low tap density and finite conductivity. Here, we present a type of densely packed titanium dioxide (TiO2) composite that comprises three-dimensional aligned mesoporous TiO2 microspheres and coated ultrathin mesoporous carbon shells. The fabricated mesoporous meso-TiO2@meso-C complex possesses a highly accessible surface area (134 m2 g−1), dual mesopore channels (11.8 and 21.6 nm), and a much higher tap density (1.52 g cm−3). As expected, this designed mesoporous composite achieves superior electrochemical performance, including both a maximized specific capacity of 255 mAh g−1 and a volumetric capacity of 390 mAh cm−3 at 0.025 A g−1. Our mesoscopic composite electrode that enables fast redox reaction reveals the importance of incorporating conductive and dense mesostructures as an alternative pathway for high-volumetric pseudocapacitive materials.

晶粒尺寸较小的过渡金属氧化物是电容式电荷存储的理想候选材料。然而,这种氧化物材料的整体性能仍然受到低点密度和有限电导率的限制。在这里,我们提出了一种致密堆积的二氧化钛(TiO2)复合材料,它由三维排列的介孔二氧化钛微球和涂覆的超薄介孔碳壳组成。所制备的介孔介孔二氧化钛@介孔碳复合材料具有高可达表面积(134 m2 g-1)、双介孔通道(11.8 nm 和 21.6 nm)和更高的敲击密度(1.52 g cm-3)。不出所料,这种设计的介孔复合材料实现了卓越的电化学性能,包括 255 mAh g-1 的最大比容量和 0.025 A g-1 时 390 mAh cm-3 的体积容量。我们的介观复合电极可实现快速氧化还原反应,揭示了将导电致密介观结构作为高容量伪电容材料替代途径的重要性。
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引用次数: 0
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Cell Reports Physical Science
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