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Competing host-guest interactions to explore the alkyl anion transport in photo-responsive, space-confined hydrogels 通过主客体间的竞争性相互作用探索光响应式空间封闭水凝胶中的烷基阴离子传输问题
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-26 DOI: 10.1016/j.xcrp.2024.102174
Bi-Ying Liu, Yongchao Qian, Min Zhou, Xiao-Yan Jin, Mei-Juan Jia, Di Quan, Xiang-Yu Kong, Liping Wen, Lei Jiang

Photo-responsive hydrogel systems have attracted significant attention for their controllability, intelligent responsiveness, and reversibility. This study delves into the effect of tunable space-confined networks on anion transport in photo-responsive hydrogels. Employing azobenzene (Azo) and β-cyclodextrin (β-CD), the hydrogel was loaded into anodic aluminum oxide (AAO) to form the AAO-hydrogel membrane. Sodium dodecyl sulfonate (SDS) is chosen to investigate mass transmembrane transport. In low-degree space-confined aluminum oxide-hydrogel membrane (LSAHM), a looser structure was formed due to the breakup of the connection between Azo and β-CD with ultraviolet (UV)-light irradiation. With visible-light (vis-light) irradiation, the SDS is replaced with trans-Azo due to the more stable trans-Azo@β-CD complex, resulting in narrow channels. For high-degree space-confined AHM (HSAHM), the interaction between SDS and β-CD could be omitted due to space confinement. Also, controllable SDS-assisted cationic peptide transport is achieved with HSAHM. This work provides a comprehensive analysis of hydrogel structure variations, offering nuanced approaches to hydrogel design.

光响应水凝胶系统因其可控性、智能响应性和可逆性而备受关注。本研究探讨了可调空间封闭网络对光响应水凝胶中阴离子传输的影响。利用偶氮苯(Azo)和β-环糊精(β-CD),将水凝胶负载到阳极氧化铝(AAO)中,形成 AAO-水凝胶膜。选择十二烷基磺酸钠(SDS)来研究质量跨膜传输。在低度空间封闭的氧化铝-水凝胶膜(LSAHM)中,由于紫外线(UV)照射导致偶氮和β-CD之间的连接断裂,从而形成了较松散的结构。在可见光(vis-light)照射下,由于反式偶氮@β-CD 复合物更为稳定,SDS 被反式偶氮取代,从而形成狭窄的通道。对于高度空间封闭的 AHM(HSAHM),由于空间封闭,SDS 和 β-CD 之间的相互作用可以省略。此外,HSAHM 还实现了可控的 SDS 辅助阳离子肽传输。这项研究全面分析了水凝胶结构的变化,为水凝胶设计提供了细致入微的方法。
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引用次数: 0
Electro-active polymer hydrogels exhibit emergent memory when embodied in a simulated game environment 电活性聚合物水凝胶在模拟游戏环境中表现出突发性记忆
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1016/j.xcrp.2024.102151
Vincent Strong, William Holderbaum, Yoshikatsu Hayashi

The goal of artificial neural networks is to utilize the functions of biological brains to develop computational algorithms. However, these purely artificial implementations cannot achieve the adaptive behavior found in biological neural networks (BNNs) via their inherent memory. Alternative computing mediums that integrate biological neurons with computer hardware have shown similar emergent behavior via memory, as found in BNNs. By applying current theories in BNNs, can emergent memory functions be achieved with alternative mediums? Electro-active polymer (EAP) hydrogels were embedded in the simulated game-world of Pong via custom multi-electrode arrays and feedback between motor commands and stimulation. Through performance analysis within the game environment, emergent memory acquisition was demonstrated, driven by ion migration through the hydrogels.

人工神经网络的目标是利用生物大脑的功能来开发计算算法。然而,这些纯粹的人工实现无法通过其固有的内存实现生物神经网络(BNN)中的自适应行为。将生物神经元与计算机硬件整合在一起的替代计算介质通过内存显示出与生物神经网络类似的突现行为。应用当前的 BNN 理论,替代介质能否实现突发记忆功能?通过定制的多电极阵列和运动指令与刺激之间的反馈,电活性聚合物(EAP)水凝胶被嵌入到模拟的乒乓游戏世界中。通过在游戏环境中进行性能分析,在离子通过水凝胶迁移的驱动下,获得了新出现的记忆。
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引用次数: 0
A stable copper-modified bipyridine mediator for highly efficient dye-sensitized solar cells 用于高效染料敏化太阳能电池的稳定铜改性联吡啶介质
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1016/j.xcrp.2024.102159
Yu-Hsuan Chen, Ching-Chin Chen, Vinh Son Nguyen, Xiao-Tong Jiang, Yan-Da Chen, Ming-You Li, Sheng-Yang Chen, Tzu-Chien Wei, Chen-Yu Yeh

Dye-sensitized solar cells (DSSCs) have garnered significant research attention for their cost-effectiveness, transparency, flexibility, etc. In this work, a copper complex of a bipyridine-modified mediator, [Cu(dmodmbp)2]+/2+, is developed to minimize the loss in fill factor (FF). A DA2 dye, inspired by the structures of previously reported LC4 and LC5 dyes, incorporates cascade acceptors to enhance light absorption and increase the short-circuit current (JSC). These innovations lead to highly efficient DSSCs with an impressive power conversion efficiency (PCE) of 10.2% (JSC = 12.10 mA cm−2, open-circuit voltage [VOC] = 1.11 V, FF = 0.764) as well as a remarkable photostability. A test over 95 days shows that 88% of the initial PCE can be maintained, with VOC, JSC, and FF retaining 98%, 97%, and 93% of their initial values, respectively.

染料敏化太阳能电池(DSSC)因其成本效益、透明度和灵活性等优点而备受研究关注。在这项工作中,我们开发了一种双吡啶修饰介质的铜络合物 [Cu(dmodmbp)2]+/2+,以尽量减少填充因子(FF)的损失。DA2 染料受先前报道的 LC4 和 LC5 染料结构的启发,加入了级联受体,以增强光吸收并增加短路电流(JSC)。这些创新带来了高效的 DSSC,其功率转换效率 (PCE) 达到了惊人的 10.2%(JSC = 12.10 mA cm-2,开路电压 [VOC] = 1.11 V,FF = 0.764),并且具有显著的光稳定性。95 天的测试表明,初始 PCE 可保持 88%,VOC、JSC 和 FF 分别保持了初始值的 98%、97% 和 93%。
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引用次数: 0
Differential pulse voltammetry analytics for lithium-ion battery degradation 锂离子电池降解的差分脉冲伏安分析法
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-22 DOI: 10.1016/j.xcrp.2024.102168
Venkatesh Kabra, Conner Fear, Paul W.C. Northrop, J. Vernon Cole, Partha P. Mukherjee

With the growing need for lithium-ion batteries in high-power applications, an accurate estimation of battery state of health is critical for long cyclability. In this work, an analytics approach based on pulse voltammetry is presented for lithium-ion batteries. A physics-based modeling framework is developed to predict pulse voltammogram signatures for generic voltage pulses. In combination with a parameter estimation technique, this model presents an in situ diagnostic tool that captures key electrode-specific parameters with rapid accuracy. Using this approach, we quantify degradation descriptors such as the growth of the resistive layer, interfacial area evolution, and lithium-intercalation state. Pulse voltammetry signatures, obtained periodically during fast-charge cycling experiments, show distinct trends at low temperature and room temperature. Active particle cracking plays a major role in the low-temperature capacity fade of lithium-ion cells, while a combination of cracking and impedance rise is the major cause of degradation at room temperature.

随着锂离子电池在大功率应用中的需求日益增长,准确估计电池的健康状况对电池的长周期使用至关重要。在这项工作中,针对锂离子电池提出了一种基于脉冲伏安法的分析方法。我们开发了一个基于物理学的建模框架,用于预测通用电压脉冲的脉冲伏安图特征。结合参数估计技术,该模型提供了一种现场诊断工具,可快速准确地捕捉关键的特定电极参数。利用这种方法,我们可以量化降解描述符,如电阻层的增长、界面面积的演变和锂闰状态。在快速充电循环实验中定期获得的脉冲伏安特性显示了低温和室温下的不同趋势。活性颗粒开裂是锂离子电池低温容量衰减的主要原因,而开裂和阻抗上升的结合则是室温降解的主要原因。
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引用次数: 0
Chemical state of nickel nanoparticles during the oxygen evolution reaction in a carbonate-bicarbonate buffer solution 碳酸盐-碳酸氢盐缓冲溶液中氧进化反应过程中镍纳米颗粒的化学状态
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1016/j.xcrp.2024.102165
Bat-Or Shalom, Miguel A. Andrés, Ashley R. Head, Boruch Z. Epstein, Olga Brontvein, Virginia Pérez-Dieste, Ignacio J. Villar-Garcia, Alex S. Walton, Kacper Polus, Robert S. Weatherup, Baran Eren

The chemical state of nickel anodes during the oxygen evolution reaction can impact their electrocatalytic performance. Here, X-ray photoelectron and absorption spectroscopies reveal the chemical state of nickel nanoparticles under oxygen evolution reaction conditions in a mildly alkaline carbonate-bicarbonate buffer solution. Ni2+ and Ni3+ species are observed at the reaction onset potential with a 7:4 ratio, with no remaining metallic nickel. These species include NiO, which increasingly converts to other Ni2+ and Ni3+ species once the potential is increased above the onset potential. Conversely, when a 20-nm-thick nickel film is used instead of nickel nanoparticles, a significant amount of metallic nickel remains in the inner layers. Nickel nanoparticles also undergo significant morphological and structural changes during the reaction, as evidenced by ex situ transmission electron microscopy. Amorphization of the nanoparticles is attributed to significant H2O incorporation, with the oxygen intensity increasing both in operando and ex situ measurements.

氧进化反应过程中镍阳极的化学状态会影响其电催化性能。在此,X 射线光电子学和吸收光谱揭示了镍纳米颗粒在弱碱性碳酸盐-碳酸氢盐缓冲溶液中氧进化反应条件下的化学状态。在反应起始电位观察到的 Ni2+ 和 Ni3+ 物种比例为 7:4,没有剩余的金属镍。这些物种包括 NiO,一旦电位高于起始电位,NiO 会逐渐转化为其他 Ni2+ 和 Ni3+ 物种。相反,当使用 20 纳米厚的镍膜而不是纳米镍粒子时,大量金属镍仍留在内层。原位透射电子显微镜显示,纳米镍粒子在反应过程中也发生了显著的形态和结构变化。纳米颗粒的非晶化归因于大量 H2O 的加入,在操作和原位测量中氧的强度都在增加。
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引用次数: 0
Enhanced thermoelectric properties of flexible self-supporting carbon nanotube film/polypyrrole composites 增强柔性自支撑碳纳米管薄膜/聚吡咯复合材料的热电特性
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1016/j.xcrp.2024.102163
Xiaohua Liu, Jing Huang, Yong Du, Lei Wang, Per Eklund
For energy harvesting by flexible thermoelectrics, composite materials have prospects for wearable electronics and require processing methods yielding composites with high thermoelectric performance. Here, we report the fabrication of flexible carbon nanotube film (CNTF)/polypyrrole (PPy) composites by polymerization of PPy on the CNTF. The two-dimensional network structure of CNTF can solve the limitations on the thermoelectric performance of CNT/PPy caused by the poor dispersion and orientation of CNTs. The CNTF/PPy composites exhibit a maximum thermoelectric power factor of 369.2 μWmK at 300 K, which is nearly twice of that of the CNTF (191.2 μWmK). The composites also display flexibility under repeated bending. Composites treated with pre-stretching obtain a higher power factor of 403.8 μWmK at 320 K. This method provides a pathway for optimizing the thermoelectric properties of composites based on CNTF. The study is of importance for application prospects in the fields of thermoelectric conversion and multifunctional wearable electronics.
为了利用柔性热电材料进行能量收集,复合材料在可穿戴电子设备中具有广阔的应用前景,并且需要采用能够产生高热电性能复合材料的加工方法。在此,我们报告了通过在碳纳米管薄膜(CNTF)上聚合聚吡咯(PPy)制备柔性碳纳米管薄膜(CNTF)/聚吡咯(PPy)复合材料的方法。CNTF 的二维网络结构可以解决 CNT/PPy 因 CNT 的分散性和取向性差而对热电性能造成的限制。CNTF/PPy 复合材料在 300 K 时的最大热电功率因数为 369.2 μWmK,几乎是 CNTF(191.2 μWmK)的两倍。复合材料在反复弯曲时也显示出柔韧性。这种方法为优化基于 CNTF 的复合材料的热电特性提供了一条途径。该研究对热电转换和多功能可穿戴电子产品领域的应用前景具有重要意义。
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引用次数: 0
Naphthopyran-based photoswitching for simpler chemical sensing and imaging using phase-sensitive mode 基于萘吡喃的光开关,利用相敏模式实现更简单的化学传感和成像
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1016/j.xcrp.2024.102167
Yu Cheng, Yifu Wang, Jingying Zhai, Xiaojiang Xie

Intensity-based fluorescence imaging suffers from spectral overlap and optical background interference. As an alternative, fluorescence lifetime measurements on the nanosecond level are also largely constrained. Herein, we propose phase-sensitive detection of photoswitchable probes containing naphthopyran and fluorescent donors. The method features reaction kinetics in the millisecond-to-second regime, allowing frequency domain detection with cost-effective equipment. A phase shift (Δϕ) in the fluorescence of the probes is extracted by fast Fourier transform, establishing a dependence on the molar ratio of donor to acceptor. Thus, Δϕ is proposed as a self-referencing quantity for selective highlighting of fluorescent probes and a dynamic signal readout in chemical sensing. Phase-sensitive detection of protamine, a polycationic protein often used as a neutralizer of the anticoagulant heparin during surgery, is successfully realized based on the platform.

基于强度的荧光成像受到光谱重叠和光学背景干扰的影响。作为替代方法,纳秒级的荧光寿命测量在很大程度上也受到限制。在此,我们提出了对含有萘并吡喃和荧光供体的光开关探针进行相敏检测的方法。该方法的特点是反应动力学在毫秒到秒的范围内,可使用经济高效的设备进行频域检测。探针荧光中的相移(Δj)是通过快速傅立叶变换提取的,它与供体和受体的摩尔比有关。因此,Δj 被认为是选择性突出荧光探针的自参照量,也是化学传感中的动态信号读数。基于该平台,成功实现了对原胺的相敏检测,原胺是一种多阳离子蛋白质,在手术中常被用作抗凝剂肝素的中和剂。
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引用次数: 0
Focus on bioelectronics 关注生物电子学
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1016/j.xcrp.2024.102162
Sohini Kar-Narayan, Sahika Inal
No Abstract
无摘要
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引用次数: 0
Battery cumulative lifetime prognostics to bridge laboratory and real-life scenarios 电池累积寿命预报技术将实验室和现实生活场景融为一体
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-21 DOI: 10.1016/j.xcrp.2024.102164
Dongzhen Lyu, Bin Zhang, Enrico Zio, Jiawei Xiang

Battery operating data from real-life scenarios are riddled with randomness, complexity, and multi-cell grouping, posing significant challenges for applying lifetime prognostic approaches developed from laboratory scenarios. To address this, we have conducted extensive experimental investigations into battery degradation across laboratory and real-life scenarios spanning a 4 year period, involving a total of approximately 546,000 charge-discharge cycles across hundreds of cells and packs. In addition to our experimental investigations, we develop a lifetime prognosis approach by creatively incorporating the concept of cumulative utilization lifetime. Our approach highlights the significant potential of transferring knowledge gained from standardized laboratory scenarios to diverse real-world conditions. It consistently improves performance from early prediction to real-time prediction, achieving a remarkable error margin of around 5% and millisecond-level computational efficiency on a portable laptop with no dedicated graphics. Furthermore, our experimental investigations underscore the beneficial effects of seasonal low temperatures on prolonging battery lifetime.

现实生活中的电池运行数据充满了随机性、复杂性和多电池组,这给应用实验室场景开发的寿命预测方法带来了巨大挑战。为了解决这个问题,我们在实验室和现实生活场景中对电池退化进行了广泛的实验研究,时间跨度长达 4 年,涉及数百个电池和电池组,总计约 546,000 次充放电循环。除实验研究外,我们还创造性地融入了累积使用期限的概念,从而开发出一种使用寿命预报方法。我们的方法凸显了将从标准化实验室场景中获得的知识转移到各种实际条件中的巨大潜力。从早期预测到实时预测,该方法的性能不断提高,在没有专用图形处理器的便携式笔记本电脑上实现了约 5% 的显著误差率和毫秒级的计算效率。此外,我们的实验研究还强调了季节性低温对延长电池寿命的有利影响。
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引用次数: 0
Thermal-controlled cholesteric liquid crystal wavelength filter lens for photosensitive epilepsy treatment 用于光敏癫痫治疗的热控胆固醇液晶波长滤光透镜
IF 8.9 2区 综合性期刊 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-08-20 DOI: 10.1016/j.xcrp.2024.102158
Yuanjie Xia, Zubair Ahmed, Affar Karimullah, Nigel Mottram, Hadi Heidari, Rami Ghannam

Cholesteric liquid crystals (CLCs) exhibit optical properties that are highly responsive to temperature or electric fields. Here, we report an approach to aiding in photosensitive epilepsy treatment by developing a thermal-controlled CLC wavelength filter lens. This lens demonstrates exceptional optical tunability, enabling it to dynamically change its stopband in response to temperature changes. At room temperature, the stopband of the CLC lens is outside the visible spectrum, rendering the lens functionally similar to normal glass. As the temperature rises to 36.5°C, the lens efficiently blocks light within the 660- to 720-nm wavelength range, which is the known trigger wavelength for photosensitive epilepsy. CLC materials with opposite handedness are used to achieve over 98% light cutoff at the stopband. We propose a control system for dynamically controlling the temperature in real time. The tunable lenses offer a solution for mitigating the effects of specific light stimuli on affected individuals.

胆甾型液晶(CLC)具有对温度或电场高度敏感的光学特性。在此,我们报告了一种通过开发热控制胆甾型液晶波长滤光透镜来辅助光敏性癫痫治疗的方法。这种透镜具有出色的光学可调谐性,能够根据温度变化动态改变其挡带。在室温下,CLC 透镜的阻带在可见光谱之外,因此透镜的功能与普通玻璃相似。当温度升至 36.5 摄氏度时,透镜能有效阻挡 660 至 720 纳米波长范围内的光线,而这正是已知的光敏性癫痫的触发波长。我们使用了具有相反手性的 CLC 材料,从而在止带处实现了 98% 以上的截光率。我们提出了一种实时动态控制温度的控制系统。可调谐透镜为减轻特定光刺激对患者的影响提供了一种解决方案。
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引用次数: 0
期刊
Cell Reports Physical Science
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