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Gas sensors based on nanoparticle-assembled interfaces and their application in breath detection of lung cancer 基于纳米粒子组装界面的气体传感器及其在肺癌呼吸检测中的应用
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-01 DOI: 10.1016/j.xcrp.2023.101678
Xinyuan Zhou, Manqing Qi, Kun Li, Zhenjie Xue, Tie Wang
Exhaled breath detection is a noninvasive method to diagnose diseases and is promising in the early screening of lung cancer. However, gas biomarkers of lung cancer within the exhaled breath are various and low content, and the exhaled breath has complex composition and strong fluidity, which puts forward high requirements for the performance of gas sensors. Hence, Wang’s team proposes a strategy for gas sensors based on nanoparticle-assembled interfaces. From the perspective of gas-sensing dynamics of exhaled breath, the microstructure of the sensing interface is designed to enhance their capture and adsorption efficiency via regulating the mass transfer behaviors of gas molecules so as to design high-performance sensors. In addition, from the three levels of cell, organ, and living body, this review summarizes the research strategy and progress of gas biomarkers of lung cancer and comments on the clinical application value of gas biomarkers in the breath detection of lung cancer. Then, this review introduces gas sensors with market application prospects, which promotes the breath detection of lung cancer from theoretical research to clinical application. Finally, breath sensors for lung cancer and prospected in smart homes are summarized.
呼气检测是一种无创的疾病诊断方法,在肺癌的早期筛查中具有广阔的应用前景。然而,呼出气体中肺癌气体生物标志物种类多、含量低,且呼出气体成分复杂、流动性强,这对气体传感器的性能提出了很高的要求。因此,王的团队提出了一种基于纳米粒子组装界面的气体传感器策略。从呼出气体的气敏动力学角度出发,设计传感界面的微观结构,通过调节气体分子的传质行为来提高其捕获和吸附效率,从而设计出高性能的传感器。此外,从细胞、器官、活体三个层面,综述了肺癌气体生物标志物的研究策略及进展,并对气体生物标志物在肺癌呼吸检测中的临床应用价值进行了评述。然后,本文介绍了具有市场应用前景的气体传感器,促进肺癌呼吸检测从理论研究走向临床应用。最后,对肺癌呼吸传感器及其在智能家居中的应用前景进行了总结。
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引用次数: 0
Advanced amino acid-based biomimetic Janus membrane for extracorporeal membrane oxygenation 用于体外膜氧合的先进氨基酸仿生Janus膜
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-01 DOI: 10.1016/j.xcrp.2023.101677
Yue Yang, Wenqing Gao, Yun Chang, Zhenyi Zhao, Hechen Shen, Zhi Wang, Tong Li, Song Zhao
Extracorporeal membrane oxygenation (ECMO) is a life support system that provides extracorporeal respiration and circulation. Current oxygenation membranes still face the challenges of plasma leakage, low gas exchange efficiency of O2 and CO2, and poor biocompatibility. Here, we describe the design and realization of a biomimetic Janus membrane to simulate the structural characteristics of the alveolar blood-gas barrier. The asymmetric structure is constructed by sequential assembly of a hydrophobic polydimethylsiloxane layer, hydrophilic amino acid layer, and sulfonate grafting layer, which provide the functions of preventing plasma leakage, improving gas exchange performance, and maintaining biocompatibility. Importantly, the membrane can offer efficient blood oxygenation, achieving O2 and CO2 transfer rates of ∼54 and ∼131 mL m−2 min−1, respectively. This work demonstrates that the smartly designed Janus structure provides the desired comprehensive properties of an oxygenation membrane and offers valuable guidance for the development of more advanced oxygenation membranes.
体外膜氧合(Extracorporeal membrane oxygenation, ECMO)是一种提供体外呼吸和循环的生命支持系统。目前的氧合膜仍面临等离子体泄漏、O2和CO2气体交换效率低、生物相容性差等挑战。在这里,我们描述了仿生Janus膜的设计和实现,以模拟肺泡血气屏障的结构特征。通过疏水聚二甲基硅氧烷层、亲水性氨基酸层和磺酸盐接枝层序组装而成的不对称结构,具有防止等离子体泄漏、提高气体交换性能和维持生物相容性等功能。重要的是,该膜可以提供有效的血液氧合,O2和CO2的传递速率分别为~ 54和~ 131 mL m−2 min−1。这项工作表明,巧妙设计的Janus结构提供了所需的氧化膜的综合性能,并为开发更先进的氧化膜提供了有价值的指导。
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引用次数: 0
Flexible organic electrochemical transistors for bioelectronics 生物电子学用柔性有机电化学晶体管
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-01 DOI: 10.1016/j.xcrp.2023.101673
Zeyu Zhao, Zhiyuan Tian, Feng Yan
Flexible organic bioelectronic devices, which extract electronic signals from living systems, have been developed for sensing, recording, and monitoring various physiological states of biological systems. Organic electrochemical transistors (OECTs) have emerged as a promising platform for bioelectronics because of their inherent amplification function, high sensitivity, low cost, easy operation, and compatibility with flexible and wearable devices. This review provides a comprehensive overview of recent advancements in flexible OECTs for biosensing applications, including the fundamental principles and mechanisms of flexible OECTs, various channel materials used for biosensing, functionalization of OECTs for biosensing, use of flexible OECTs for the acquisition of biological signals, bioinformatics analysis of OECT-based biosensors, and development of biomimetic devices. The review concludes with a summary of the state-of-the-art technology for flexible OECT-based biosensors and the future outlook for this rapidly evolving field.
柔性有机生物电子器件是一种从生命系统中提取电子信号的器件,用于传感、记录和监测生物系统的各种生理状态。有机电化学晶体管(OECTs)因其固有的放大功能、高灵敏度、低成本、易于操作以及兼容柔性和可穿戴设备而成为生物电子学的一个有前途的平台。本文综述了柔性oect在生物传感领域的最新进展,包括柔性oect的基本原理和机制、用于生物传感的各种通道材料、用于生物传感的oect的功能化、柔性oect在生物信号采集中的应用、基于oect的生物传感器的生物信息学分析以及仿生装置的发展。该综述总结了基于oect的柔性生物传感器的最新技术以及这一快速发展领域的未来展望。
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引用次数: 0
Reassessing the intrinsic hydrogen evolution reaction activity of platinum using scanning electrochemical cell microscopy 用扫描电化学电池显微镜重新评价铂的本征析氢反应活性
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-01 DOI: 10.1016/j.xcrp.2023.101680
Emmanuel Batsa Tetteh, Moonjoo Kim, Alan Savan, Alfred Ludwig, Taek Dong Chung, Wolfgang Schuhmann
While promising catalysts are constantly being discovered for the electrochemical hydrogen evolution reaction (HER), none have surpassed platinum’s performance, despite its intrinsic activity being underestimated. A thorough assessment of intrinsic activity is therefore necessary to understand platinum’s superior performance. Here, we use scanning electrochemical cell microscopy to overcome limitations in proton and hydrogen mass transport at multiple scales. Reliable HER current transients with steady-state limiting current densities far above the exchange current density are recorded (jl of 4 A/cm2 with a 440 nm pipette) in acid electrolyte. Furthermore, exchange current density analysis shows that platinum’s intrinsic activity (230 ± 34 mA/cm2) is over 200-fold higher than reported in rotating disc measurements (1 mA/cm2), 3-fold higher than the H2 pump method (75 mA/cm2), and almost twice that from micropolarization analysis (140 mA/cm2). These findings demonstrate the importance of mass transport in achieving high-current-density electrocatalysis and reveal platinum’s underestimated intrinsic activity.
虽然电化学析氢反应(HER)的催化剂不断被发现,但没有一种催化剂的性能超过铂,尽管它的内在活性被低估了。因此,要了解铂金的优异性能,对其内在活性进行彻底的评估是必要的。在这里,我们使用扫描电化学电池显微镜来克服质子和氢在多尺度上的质量传递的限制。在酸性电解质中记录了可靠的HER电流瞬态,稳态极限电流密度远高于交换电流密度(440nm移液器的jl为4a /cm2)。此外,交换电流密度分析表明,铂的固有活度(230±34 mA/cm2)比旋转圆盘测量法(1 mA/cm2)高200倍以上,比H2泵法(75 mA/cm2)高3倍,几乎是微极化分析法(140 mA/cm2)的两倍。这些发现证明了质量输运在实现高电流密度电催化中的重要性,并揭示了铂被低估的内在活性。
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引用次数: 0
DNA recognition and induced genome modification by a hydroxymethyl-γ tail-clamp peptide nucleic acid. 羟甲基-γ尾部钳肽核酸的DNA识别和诱导基因组修饰。
IF 7.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-18 DOI: 10.1016/j.xcrp.2023.101635
Stanley N Oyaghire, Elias Quijano, J Dinithi R Perera, Hanna K Mandl, W Mark Saltzman, Raman Bahal, Peter M Glazer

Peptide nucleic acids (PNAs) can target and stimulate recombination reactions in genomic DNA. We have reported that γPNA oligomers possessing the diethylene glycol γ-substituent show improved efficacy over unmodified PNAs in stimulating recombination-induced gene modification. However, this structural modification poses a challenge because of the inherent racemization risk in O-alkylation of the precursory serine side chain. To circumvent this risk and improve γPNA accessibility, we explore the utility of γPNA oligomers possessing the hydroxymethyl-γ moiety for gene-editing applications. We demonstrate that a γPNA oligomer possessing the hydroxymethyl modification, despite weaker preorganization, retains the ability to form a hybrid with the double-stranded DNA target of comparable stability and with higher affinity than that of the diethylene glycol-γPNA. When formulated into poly(lactic-co-glycolic acid) nanoparticles, the hydroxymethyl-γPNA stimulates higher frequencies (≥ 1.5-fold) of gene modification than the diethylene glycol γPNA in mouse bone marrow cells.

肽核酸(PNAs)可以靶向并刺激基因组DNA中的重组反应。我们已经报道了具有二甘醇γ-取代基的γPNA低聚物在刺激重组诱导的基因修饰方面比未修饰的PNA表现出更好的功效。然而,这种结构修饰带来了挑战,因为在前驱丝氨酸侧链的O-烷基化中存在固有的外消旋风险。为了规避这一风险并提高γPNA的可及性,我们探索了具有羟甲基-γ部分的γPNA寡聚物在基因编辑应用中的效用。我们证明,尽管预组织较弱,但具有羟甲基修饰的γPNA低聚物仍保留与双链DNA靶标形成杂交体的能力,该杂交体具有相当的稳定性和比二甘醇-γPNA更高的亲和力。当配制成聚乳酸-乙醇酸纳米颗粒时,在小鼠骨髓细胞中,羟甲基-γPNA比二甘醇γPNA刺激更高频率(≥1.5倍)的基因修饰。
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引用次数: 0
A multi-stimuli-responsive actuator for efficient thermal management and various biomimetic locomotion 一种多刺激响应驱动器,用于高效的热管理和各种仿生运动
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1016/j.xcrp.2023.101588
Xue-Fei Feng, Si-Zhe Sheng, Cheng Chen, Xin-Lin Li, Zhi-Yu Xian, Jian-Wei Liu
Creating flexible actuators that mimic natural organisms' movements and respond to various stimuli is highly significant for bionic soft robotics, electronics, and wearables. However, achieving a simultaneous response to multiple stimuli within a single actuator still has great challenges in terms of structural design. Here, by combining carbon nanotubes with high photothermal effect, bacterial cellulose with water-triggered expansion, and polyethylene with a large thermal expansion coefficient, a bilayer actuator is proposed with macroscopic and fast response to natural sunlight, low voltage, temperature, humidity, and organic solvents. Based on this, we propose a smart curtain that passively responds to light changes, lowering room temperature by 10.9°C to reduce the huge energy consumption for thermal management of buildings. Besides, a multi-stimulus response curtain that switches according to ambient humidity is designed. Interestingly, this soft actuator can also realize complex bionic motions such as bionic clamping, jumping, self-oscillation, and crawling.
创造灵活的执行器,模仿自然生物的运动,并对各种刺激做出反应,对于仿生软机器人、电子产品和可穿戴设备非常重要。然而,在结构设计方面,在单个执行器内实现对多个刺激的同时响应仍然存在很大挑战。本研究将具有高光热效应的碳纳米管、具有水触发膨胀的细菌纤维素和具有大热膨胀系数的聚乙烯相结合,提出了一种对自然光照、低电压、温度、湿度和有机溶剂具有宏观快速响应的双层致动器。基于此,我们提出了一种被动响应光线变化的智能窗帘,将室温降低10.9°C,为建筑的热管理减少巨大的能源消耗。此外,还设计了可根据环境湿度变化进行切换的多刺激响应幕。有趣的是,这种柔性驱动器还可以实现复杂的仿生运动,如仿生夹紧、仿生跳跃、自振荡、仿生爬行等。
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引用次数: 0
Differentiable graph-structured models for inverse design of lattice materials 晶格材料反设计的可微图结构模型
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1016/j.xcrp.2023.101586
Dominik Dold, Derek Aranguren van Egmond
Architected materials possessing physico-chemical properties adaptable to disparate environmental conditions embody a disruptive new domain of materials science. Fueled by advances in digital design and fabrication, materials shaped into lattice topologies enable a degree of property customization not afforded to bulk materials. A promising venue for inspiration toward their design is in the irregular micro-architectures of nature. However, the immense design variability unlocked by such irregularity is challenging to probe analytically. Here, we propose a new computational approach using graph-based representation for regular and irregular lattice materials. Our method uses differentiable message passing algorithms to calculate mechanical properties, allowing automatic differentiation with surrogate derivatives to adjust geometric structure and local attributes of individual lattice elements to achieve inversely designed materials with desired properties. We further introduce a graph neural network surrogate model for structural analysis at scale. The methodology is generalizable to any system representable as heterogeneous graphs.
建筑材料具有适应不同环境条件的物理化学特性,体现了材料科学的一个颠覆性新领域。在数字设计和制造技术进步的推动下,形成晶格拓扑结构的材料能够实现一定程度的属性定制,这是散装材料所无法提供的。他们的设计灵感来自于自然界不规则的微建筑。然而,这种不规则性释放的巨大设计可变性对分析探索具有挑战性。在这里,我们提出了一种新的计算方法,使用基于图形的表示规则和不规则晶格材料。我们的方法使用可微信息传递算法来计算力学性能,允许与替代导数的自动微分来调整单个晶格元素的几何结构和局部属性,以获得具有所需性能的逆向设计材料。我们进一步引入了一种用于结构分析的图神经网络代理模型。该方法可推广到任何可表示为异构图的系统。
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引用次数: 3
Kinetic control over co-self-assembly using an in situ dynamic covalent reaction resulting in a synergistic chemo-photodynamic therapy 利用原位动态共价反应对共自组装进行动力学控制,从而产生协同化学光动力治疗
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1016/j.xcrp.2023.101598
Xiaoxia Wu, Jie Xing, Yonglei Lyu, Jingjing Yu, Jinghui Yang, Dawei Qi, Xin Wang, Jie Lin, Guoliang Shao, Aiguo Wu, Jianwei Li
Multicomponent self-assembly offers a strategy to explore ordered, complex, and dynamic nanosystems and to harness the property of the whole system beyond that of each subcomponent. However, the spontaneous nature of co-self-assembly makes control of the process difficult. Here, we use a thiol-disulfide exchange reaction as an in situ dynamic covalent reaction to slowly produce disulfide macrocycles that subsequently trigger the co-self-assembly with an anticancer drug and a photosensitizer. The gradual concentration growth of products shows kinetic control over the concentration of self-assembling disulfides, resulting in a stable co-delivery nanosystem with high drug-loading efficiency (31.78%) and encapsulation efficiency (95.91%). The nanosystem possesses biocompatibility, tumor-accumulating ability, and biosafety and shows a synergistic chemotherapeutic and photodynamic anticancer effect in vitro and in vivo. Our findings suggest that in situ dynamic covalent chemistry advances control over co-self-assembly, paving the way to more functional nanosystems with potential applications in biomedicine, electronics, and renewable energy.
多组分自组装提供了一种探索有序、复杂和动态纳米系统的策略,并利用了整个系统的特性,而不仅仅是每个子组分。然而,共自组装的自发性使得控制过程变得困难。在这里,我们使用巯基-二硫交换反应作为原位动态共价反应,缓慢地产生二硫大环,随后触发与抗癌药物和光敏剂的自组装。产物浓度的逐渐增长对自组装二硫化物的浓度具有动力学控制,从而形成了稳定的共递送纳米体系,具有较高的载药效率(31.78%)和包封效率(95.91%)。该纳米系统具有生物相容性、肿瘤蓄积能力和生物安全性,并在体外和体内表现出协同化疗和光动力抗癌作用。我们的研究结果表明,原位动态共价化学促进了对共自组装的控制,为在生物医学、电子和可再生能源领域具有潜在应用的更多功能纳米系统铺平了道路。
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引用次数: 0
A simple and universal strategy for liquid-like coating suitable for a broad range of liquids on diverse substrates 一种简单而通用的液体状涂层策略,适用于各种基材上的各种液体
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1016/j.xcrp.2023.101593
Shouzheng Jiao, Yufen Li, Yang Zhang, Dongjie Zhang, Yuyan Liu, Zhongjun Cheng
Liquid-like PDMS brushes coating with low adhesion to droplets are significant in both fundamental research and practical application. Covalent grafting is a common strategy to prepare PDMS brushes with low adhesion to diverse liquids in a wide range of surface tensions, but it is only suitable for high active inorganic substrates. Casting of mixtures containing PDMS can solve this problem; however, homogeneity and low adhesion cannot be guaranteed. Here we report a simple method by step-by-step spraying for preparing PDMS brushes, which is suitable for both substrates. Droplets with a wide range of surface tension can slide off the coating with a sliding angle less than 10°. Research results indicate that the polyamine with flexible molecular chain and high functionality is beneficial for brushes coating with high grafting density and excellent surface lubricity. Finally, good stability and diverse applications in fouling resistance, self-cleaning, anti-bursting, etc. are also demonstrated.
液态聚甲基丙烯酸甲酯(PDMS)刷涂具有较低的液滴附着力,具有重要的基础研究和实际应用价值。共价接枝是制备在大范围表面张力下对各种液体具有低粘附性的PDMS刷的常用策略,但它只适用于高活性无机基底。铸造含有PDMS的混合物可以解决这一问题;但不能保证均匀性和低附着力。在这里,我们报告了一种简单的方法,一步一步喷涂制备PDMS刷,适用于两种基材。具有大范围表面张力的液滴可以以小于10°的滑动角从涂层上滑动。研究结果表明,具有柔性分子链和高功能化的多胺有利于制备具有高接枝密度和良好表面润滑性的毛刷涂层。最后,还展示了良好的稳定性和在耐污、自洁、防爆裂等方面的广泛应用。
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引用次数: 0
Processing dynamics of carbon nanotube-epoxy nanocomposites during 3D printing 碳纳米管-环氧纳米复合材料在3D打印过程中的加工动态
2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1016/j.xcrp.2023.101617
Ali Zein Khater, M.A.S.R. Saadi, Sohini Bhattacharyya, Alex Kutana, Manoj Tripathi, Mithil Kamble, Shaowei Song, Minghe Lou, Morgan Barnes, Matthew D. Meyer, Vijay Vedhan Jayanthi Harikrishnan, Alan B. Dalton, Nikhil Koratkar, Chandra Sekhar Tiwary, Peter J. Boul, Boris Yakobson, Hanyu Zhu, Pulickel M. Ajayan, Muhammad M. Rahman
Carbon nanotube (CNT)-reinforced polymer nanocomposites are promising candidates for a myriad of applications. Ad hoc CNT-polymer nanocomposite fabrication techniques inherently pose roadblocks to optimized processing, resulting in microstructural defects, i.e., void formation, poor interfacial adhesion, wettability, and agglomeration of CNTs inside the polymer matrix. Here, we show that a 3D printing technique offers improved processing of CNT-polymer nanocomposites. During printing, the shear-induced flow of an engineered nanocomposite ink through the micronozzle is beneficial, as it reduces the number of voids within the epoxy matrix, improves CNT dispersion and adhesion with epoxy, and partially aligns the CNTs. Such microstructural changes result in enhanced mechanical and thermal properties of the nanocomposites compared to their mold-cast counterparts. This work demonstrates the advantages of 3D printing in achieving improved processing dynamics for the fabrication of CNT-polymer nanocomposites with better structural and functional properties.
碳纳米管(CNT)增强聚合物纳米复合材料具有广阔的应用前景。特别的碳纳米管-聚合物纳米复合材料制造技术本身就给优化加工带来了障碍,导致微观结构缺陷,即孔隙形成、界面粘附性差、润湿性差以及碳纳米管在聚合物基体内的团聚。在这里,我们展示了3D打印技术提供了碳纳米管聚合物纳米复合材料的改进加工。在打印过程中,工程纳米复合油墨通过微喷嘴的剪切诱导流动是有益的,因为它减少了环氧基体内的空隙数量,改善了碳纳米管的分散和与环氧树脂的粘附性,并部分对齐了碳纳米管。这种微观结构的变化导致纳米复合材料的力学和热性能比模铸的同类材料增强。这项工作证明了3D打印在制造具有更好结构和功能特性的碳纳米管聚合物纳米复合材料方面的优势。
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引用次数: 0
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Cell Reports Physical Science
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