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Disclosing the Contribution of Vacancy Defects to Thermal Transport at liquid-Al/Graphene Adhesion Interface 揭示空位缺陷对液态铝/石墨烯粘合界面热传输的贡献
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-22 DOI: 10.1039/d4nr03590a
Yusong Ding, Fangming Lian, Yi Tao, Hao Cheng, Yun Dong
The adhesion properties of liquid-solid interfaces are of fundamental importance in performance and design of nanodevices. Modulating interfacial thermal transport has the potential to enhance interfacial heat dissipation in nanodevices. Here, the adhesive characteristics of the liquid-solid interface formed by liquid-Al/graphene are reported using molecular dynamics, and the intrinsic mechanism of interfacial adhesion evolution and energy heat transport is revealed. Specifically, an increase in temperature significantly reduces the adhesion and thermal transport capacity. Concurrently, the expansion of vacancy defects strengthens the interfacial adhesion property. This is due to the fact that the enlarged vacancy defects enhance the local contact and interfacial thermal conductance (ITC) between the atoms, thereby optimizing interfacial energy transport. The augmented ITC facilitates interfacial energy heat exchange and phonon participation rate (PPR), thus increases interfacial phonon modes and further reinforces the adhesion force. This paper elucidates the evolution of interfacial adhesion characteristics of liquid-Al/graphene, providing substantial guidance for a more comprehensive understanding of energy transport at the liquid-solid interface.
液固界面的粘附特性对纳米器件的性能和设计至关重要。调节界面热传输有可能增强纳米器件的界面散热。本文利用分子动力学报告了液态铝/石墨烯形成的液固界面的粘附特性,并揭示了界面粘附演化和能量热传输的内在机制。具体来说,温度升高会显著降低粘附力和热传输能力。同时,空位缺陷的扩展增强了界面粘附性。这是由于扩大的空位缺陷增强了原子间的局部接触和界面热传导(ITC),从而优化了界面能量传输。增强的 ITC 有利于界面能量热交换和声子参与率 (PPR),从而增加了界面声子模式并进一步增强了粘附力。本文阐明了液态铝/石墨烯界面粘附特性的演变,为更全面地了解液固界面的能量传输提供了实质性指导。
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引用次数: 0
Precursor Engineering towards Orange and Red-Emissive Carbon Dots for LEDs with Tunable Emission Colors 用于可调发光颜色 LED 的橙色和红色发光碳点前驱体工程
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-22 DOI: 10.1039/d4nr03184a
Jiaxin Sun, Wenjie Xu, Yixiang Liu, Bin Sun, Jie Xiong, Yongfu Lian, Yanhui Lou, Lai Feng
Carbon dots (CDs) have been of great interest due to their high potential in optoelectronic applications. Although various CDs have been synthesized via the “bottom-up” pathway, fewer focused on understanding the origins of the structural and optical diversities of CDs. In this work, two benzenoid acids with a slight structural variation (i.e., 9-oxo-9H-fluorene-2,7-dicarboxylic acid (FR) and 4,4'-biphenyl dicarboxylic acid (BP)) are employed as precursors, yielding orange and red-emissive CDs, respectively, with quantum yields of 43.1 ~ 30.9%. A combined experimental and theoretical study reveals that these CDs’ structural and optical diversities originate from the structural variation of precursors. Furthermore, we demonstrate that the light-emitting diodes (LEDs) based on the blended emissive layer of poly(N-vinyl carbazole) (PVK) and CDs display cyan and yellow lights, respectively, with moderate turn-on voltages of 4.0/4.5 V and maximum luminances of 454/276 cd m-2. Such different optoelectronic performances could be attributable to the different energy-level alignments of CDs-FR and CDs-BP. This study thus provides a typical example to understand the precursor-dependent diversities of CDs, which may contribute to the rational screening of precursors towards the CDs with desirable optical/optoelectronic properties.
碳点(CD)因其在光电应用中的巨大潜力而备受关注。虽然人们已经通过 "自下而上 "的途径合成了各种碳点,但很少有人专注于了解碳点结构和光学多样性的起源。本研究以两种结构略有不同的苯甲酸(即 9-氧代-9H-芴-2,7-二羧酸(FR)和 4,4'-联苯二羧酸(BP))为前体,分别制备出橙色和红色辐射型光盘,量子产率分别为 43.1% 和 30.9%。结合实验和理论研究发现,这些光盘的结构和光学多样性源于前驱体的结构变化。此外,我们还证明了基于聚(N-乙烯基咔唑)(PVK)和光盘混合发光层的发光二极管(LED)分别显示出青色和黄色光,开启电压适中,为 4.0/4.5 V,最大亮度为 454/276 cd m-2。这种不同的光电性能可能归因于 CDs-FR 和 CDs-BP 不同的能级排列。因此,这项研究提供了一个典型的例子来了解前驱体依赖的光盘多样性,这可能有助于合理筛选前驱体,以获得具有理想光学/光电特性的光盘。
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引用次数: 0
Correction: A multifunctional black phosphorus nanosheet-based immunomagnetic bio-interface for heterogeneous circulating tumor cell capture and simultaneous self-identification in gastric cancer patients 更正:基于黑磷纳米片的多功能免疫磁性生物表面,用于捕获胃癌患者体内的异质性循环肿瘤细胞并同时进行自我识别
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr90203c
Yifan Zuo, Yi Xia, Wenwen Lu, Yue Li, Yang Xiao, Shuai Gao, Zhiyi Zhou, Hao Xu, Xingqing Feng, Chenglin Li, Yanyan Yu
Correction for ‘A multifunctional black phosphorus nanosheet-based immunomagnetic bio-interface for heterogeneous circulating tumor cell capture and simultaneous self-identification in gastric cancer patients’ by Yifan Zuo et al., Nanoscale, 2023, 15, 3872–3883, https://doi.org/10.1039/D2NR04277K.
左一凡等人撰写的 "基于多功能黑磷纳米片的免疫磁性生物界面,用于胃癌患者异质循环肿瘤细胞捕获和同步自我识别 "的更正,《纳米尺度》,2023 年,15 期,3872-3883,https://doi.org/10.1039/D2NR04277K。
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引用次数: 0
Unveiling the potential of Cu‒Pd/CdS catalysts to supply and rectify electron transfer for H2 generation from water splitting† 揭示 Cu-Pd/CdS 催化剂在提供和整流电子传递以从水分裂中产生 H2 方面的潜力†。
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr03381g
Ejaz Hussain, Memuna Idrees, Muhammad Jalil, Zeeshan Abid, Khalid Aljohani, Khezina Rafiq
As foreseeable fuel, getting hydrogen from water can be the game changer promise for renewable energy sector. Reason is that it has potential to be used as alternative to the fossil fuels. Current project has been designed to develop catalysts that can produce hydrogen from water on sunlight. For the purpose, CdS, Cu/CdS, Pd/CdS, and Cu‒Pd/CdS catalysts have been successfully synthesised and utilized for hydrogen generation. Catalytic activity of pristine CdS has been potentially enhanced with Cu and Pd cocatalysts that were deposited via chemical reduction strategy. Morphology and optical characteristics have been assessed via XRD, Raman, UV-Vis/DRS, PL, SEM, HRTEM and AFM techniques. Phase purity, compositions and charge transfer have been confirmed by EDX, XPS and EIS studies. Using similar conditions, photoreactions and H2 evolution experiments were performed in quartz reactor (UK/Velp-Sci) and GC-TCD (Shimadzu, 2014) respectively. Overall, Cu‒Pd/CdS catalyst (0.2% Cu and 0.8% Pd) was found most active that has potentially delivered 33.71 mmolg‒1h‒1 of hydrogen. Higher efficiencies were attributed to the existence of Cu and Pd on CdS surfaces. It has been predicted that Cu cocatalysts increase the electron densities on CdS surfaces (i.e. active sites), while Pd cocatalysts reduce the back reactions (higher charge transportation) by forming Schottky junctions. Various factors like pH, temperature, intensity of light and catalyst dose have been evaluated and discussed. Based on the results and activities, it has been concluded that ascribed approach hold potential to replace the fossil fuels.
作为一种可预见的燃料,从水中获取氢气可以改变可再生能源领域的游戏规则。原因是它有可能成为化石燃料的替代品。目前的项目旨在开发能在阳光下从水中制氢的催化剂。为此,已成功合成并利用 CdS、Cu/CdS、Pd/CdS 和 Cu-Pd/CdS 催化剂制氢。通过化学还原策略沉积的 Cu 和 Pd 助催化剂增强了原始 CdS 的催化活性。通过 XRD、Raman、UV-Vis/DRS、PL、SEM、HRTEM 和 AFM 技术对形态和光学特性进行了评估。EDX、XPS 和 EIS 研究证实了相纯度、组成和电荷转移。利用类似的条件,分别在石英反应器(UK/Velp-Sci)和 GC-TCD (岛津,2014 年)中进行了光反应和 H2 演化实验。总体而言,Cu-Pd/CdS 催化剂(0.2% Cu 和 0.8% Pd)的活性最高,可提供 33.71 mmolg-1h-1 的氢气。效率较高的原因是 CdS 表面存在 Cu 和 Pd。据预测,铜助催化剂会增加 CdS 表面(即活性位点)的电子密度,而钯助催化剂则会通过形成肖特基结来减少逆反应(更高的电荷传输)。对 pH 值、温度、光照强度和催化剂剂量等各种因素进行了评估和讨论。根据这些结果和活动,得出的结论是,上述方法具有替代化石燃料的潜力。
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引用次数: 0
Tunable Heteroassembly of 2D CoNi LDH and Ti3C2 Nanosheets with Enhanced Electrocatalytic Activity for Oxygen Evolution 二维 CoNi LDH 和 Ti3C2 纳米片的可调谐异质组装可增强氧进化的电催化活性
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr03679d
Xueyi Lu, Lulu Jia, Minchen Hou, Xuemin Wu, Chang Ni, Gaofei Xiao, Renzhi Ma, Xia Lu
The sluggish kinetics of oxygen evolution reaction (OER) are bottlenecks to develop hydrogen energy based on water electrolysis, which can be significantly improved using high performance catalyst. In this context, the CoNi layered double hydroxide (LDH)/Ti3C2 heterostructures are obtained using electrostatic attraction of the positively charged LDH and negatively charged Ti3C2 nanosheets as catalyst to optimize the OER performance. Such alternately stacking exhibits good catalytic activity with a lower overpotential and a small Tafel slope, outperforming their individual components. The results by density functional theory (DFT) simulation find that the charge transfers from Ti3C2 to CoNi LDH, not only adjust the electron distribution, but also increase the electron density of the interfacial active sites, thus enhances the electron transfer efficiency inside the heterostructures. Moreover, the Co2+ and Ni3+ ions exhibit a synergistic effect in supplying more electrons to adsorb the adjacent intermediates with the active hydrogen and oxygen vacancies, to improve the adsorption capability and reduce the reaction energy barriers. These findings provide a rewarding avenue towards the design of highly efficient electrocatalysts for OER.
氧进化反应(OER)的缓慢动力学是基于水电解开发氢能的瓶颈,而使用高性能催化剂可以显著改善这一问题。在此背景下,利用带正电荷的 LDH 和带负电荷的 Ti3C2 纳米片的静电吸引作用,获得了 CoNi 层状双氢氧化物(LDH)/Ti3C2 异质结构作为催化剂,以优化 OER 性能。这种交替堆叠表现出良好的催化活性,具有较低的过电位和较小的塔菲尔斜率,其性能优于它们的单独组分。密度泛函理论(DFT)模拟结果发现,从 Ti3C2 到 CoNi LDH 的电荷转移不仅调整了电子分布,还增加了界面活性位点的电子密度,从而提高了异质结构内部的电子传递效率。此外,Co2+ 和 Ni3+ 离子还能发挥协同作用,提供更多的电子来吸附邻近中间体的活性氢和氧空位,从而提高吸附能力并降低反应能垒。这些发现为设计用于 OER 的高效电催化剂提供了一条有益的途径。
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引用次数: 0
Bimetallic PdPt nanoparticles incorporated PEDOT:PSS/Guar gum blended membranes for enhanced CO2 separation 掺入 PEDOT:PSS/Guar 胶的双金属 PdPt 纳米粒子用于提高二氧化碳分离效果
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr03292f
Nishel Saini, Gaurav Pandey, Ankit Sharma, Kamakshi Pandey, Kamlendra Awasthi
To address the escalating demand for efficient CO2 separation technologies, we introduce novel membranes utilizing natural polymer guar gum (GG), conjugate polymer PEDOT:PSS, and bimetallic PdPt nanoparticles for efficient CO2 separation. Bimetallic PdPt nanoparticles were synthesized using the wet chemical method and characterized using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) techniques. The fabricated membranes were characterized using various techniques for their morphology, chemical bonds, functional groups, and mechanical properties. Through meticulous fabrication and characterization, the binary blended membranes demonstrated enhanced homogeneity and smoothness in the structure, attributed to the interaction between the polymers; and superior CO2 permeability due to the amphiphilic nature of PEDOT:PSS polymer. The gas separation experiments using H2, N2, and CO2 gases, confirmed that the 20% PEDOT:PSS/GG blended membranes showed the highest performance with sufficient mechanical properties. Moreover, the results demonstrated an increment of 172% in CO2 permeability and 138% in CO2/H2 selectivity, respectively. Further, integrating bimetallic PdPt nanoparticles provided an additional 197% increment in CO2/H2 selectivity, owing to the unique catalytic activities of noble metal nanoparticles. The study not only underscores the transformative potential of polymer blending and noble metal engineering but also highlights the significance of using natural polymers towards sustainable environmental solutions.
为了满足对高效二氧化碳分离技术不断增长的需求,我们介绍了利用天然聚合物瓜尔胶(GG)、共轭聚合物 PEDOT:PSS 和双金属 PdPt 纳米粒子实现高效二氧化碳分离的新型膜。采用湿化学方法合成了双金属钯铂纳米粒子,并利用 X 射线光电子能谱(XPS)和透射电子显微镜(TEM)技术对其进行了表征。利用各种技术对制备的膜的形态、化学键、官能团和机械性能进行了表征。通过精心制作和表征,二元共混膜的结构表现出更高的均匀性和平滑性,这归功于聚合物之间的相互作用;PEDOT:PSS 聚合物的两亲性使其具有优异的二氧化碳渗透性。使用 H2、N2 和 CO2 气体进行的气体分离实验证实,20% PEDOT:PSS/GG 混合膜具有最高的性能和足够的机械性能。此外,实验结果表明,二氧化碳渗透率和二氧化碳/ H2 选择性分别提高了 172% 和 138%。此外,由于贵金属纳米颗粒具有独特的催化活性,整合双金属钯铂纳米颗粒后,CO2/H2 选择性额外提高了 197%。这项研究不仅强调了聚合物混合和贵金属工程的变革潜力,还突出了利用天然聚合物实现可持续环境解决方案的重要意义。
{"title":"Bimetallic PdPt nanoparticles incorporated PEDOT:PSS/Guar gum blended membranes for enhanced CO2 separation","authors":"Nishel Saini, Gaurav Pandey, Ankit Sharma, Kamakshi Pandey, Kamlendra Awasthi","doi":"10.1039/d4nr03292f","DOIUrl":"https://doi.org/10.1039/d4nr03292f","url":null,"abstract":"To address the escalating demand for efficient CO2 separation technologies, we introduce novel membranes utilizing natural polymer guar gum (GG), conjugate polymer PEDOT:PSS, and bimetallic PdPt nanoparticles for efficient CO2 separation. Bimetallic PdPt nanoparticles were synthesized using the wet chemical method and characterized using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) techniques. The fabricated membranes were characterized using various techniques for their morphology, chemical bonds, functional groups, and mechanical properties. Through meticulous fabrication and characterization, the binary blended membranes demonstrated enhanced homogeneity and smoothness in the structure, attributed to the interaction between the polymers; and superior CO2 permeability due to the amphiphilic nature of PEDOT:PSS polymer. The gas separation experiments using H2, N2, and CO2 gases, confirmed that the 20% PEDOT:PSS/GG blended membranes showed the highest performance with sufficient mechanical properties. Moreover, the results demonstrated an increment of 172% in CO2 permeability and 138% in CO2/H2 selectivity, respectively. Further, integrating bimetallic PdPt nanoparticles provided an additional 197% increment in CO2/H2 selectivity, owing to the unique catalytic activities of noble metal nanoparticles. The study not only underscores the transformative potential of polymer blending and noble metal engineering but also highlights the significance of using natural polymers towards sustainable environmental solutions.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"10 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678912","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Magnetic field-assisted nanochain formation of intermixed catalytic Co-Pd nanoparticles. 磁场辅助纳米链形成混合催化 Co-Pd 纳米粒子。
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr02643h
Calle Preger, Lisa Rämisch, Johan Zetterberg, Sara Blomberg, Maria E Messing
Engineering on the nanoscale often involves optimizing performance by designing and creating new types of nanostructured materials. Multifunctional nanoparticles can be formed by combining elements that carry fundamentally different properties. The elements can be chosen based on the desired functionality, and by combining, e.g., magnetic, and catalytic elements, it is possible to self-assemble nanoparticles into catalytically active magnetic nanochains. However, mixing and assembling nanoparticles in a controlled way is challenging, and it is not obvious how the intermixing of the elements influences the properties of the individual nanoparticles. In this work, we synthesize and assemble intermixed magnetic and catalytic Cobalt-Palladium (Co-Pd) nanoparticles into multifunctional nanochains. The magnetic behavior is explored by studying the magnetic field-directed self-assembly of the nanoparticles into elongated nanochains. The catalytic properties are determined by measuring CO oxidation at elevated temperatures. Our results confirm that the magnetic and catalytic functionalities of the individual elements are retained when intermixed, which implies the potential to create nanochains with dual functionality that can be assembled in a controlled way.
纳米级工程通常涉及通过设计和创造新型纳米结构材料来优化性能。多功能纳米颗粒可通过组合具有根本不同特性的元素来形成。可以根据所需的功能来选择元素,例如,通过结合磁性和催化元素,可以将纳米粒子自组装成具有催化活性的磁性纳米链。然而,以可控的方式混合和组装纳米粒子具有挑战性,而且元素的混合如何影响单个纳米粒子的特性并不明显。在这项工作中,我们合成了磁性和催化钴钯(Co-Pd)纳米粒子,并将其组装成多功能纳米链。通过研究纳米粒子在磁场引导下自组装成拉长的纳米链,探索了其磁性行为。催化特性则是通过测量一氧化碳在高温下的氧化作用来确定的。我们的研究结果证实,单个元素的磁性和催化功能在相互混合时得以保留,这意味着有可能创造出具有双重功能的纳米链,并能以受控方式进行组装。
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引用次数: 0
An advanced plasmonic bimetallic nanostar composite for ultra-sensitive SERS detection of crystal violet 用于超灵敏 SERS 检测水晶紫的先进电浆双金属纳米柱复合材料
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr03299c
Sintayehu Leshe Kitaw, Yohannis Wondosen Ahmed, Andy Candra, Tsung-Yun Wu, Beyadgalem Endawoke Anley, Ying-Yu Chen, Yu-Ting Cheng, Kuan-Ju Chen, Chayaporn Thammaniphit, Chen Chu Hsu, Yi Ting Wu, Mahvash Hira Khan, Hsieh-Chih Tsai
The controlled synthesis of Ag/Au nanocomposite particles has remained a significant challenge in nanomaterial research. This study presents the synthesis, characterization, and surface-enhanced Raman scattering (SERS) performance of silver (Ag) and gold (Au) nanostar composites. The structural and plasmonic properties of these nanocomposites were optimized by varying the molar ratios of silver nanostars (AgNSs) and gold nanostars (AuNSs). By synthesizing composite nanostars with differing AgNS/AuNS ratios, we systematically compared their optical and spectroscopic behaviors. The results demonstrated that Ag/Au nanostar composites function as highly effective SERS substrates for the detection of rhodamine 6G (R6G), with solutions tested at concentrations from 10−15 to 10−6 M. Compared to individual AgNS or AuNS substrates, the Ag/Au nanocomposites exhibited significantly enhanced SERS signals, with superior consistency and sensitivity. Notably, the nanostar composite with a 75 : 25 Ag/Au ratio showed the highest SERS performance, achieving an enhancement factor of 8.9 × 106 and a detection limit of 10−15 M for R6G. Additionally, this composite demonstrated excellent long-term stability, maintaining performance until ten weeks of storage. To our knowledge, this represents the highest sensitivity reported for R6G detection using label-free SERS. The study further provides a detailed analysis of the composition-dependent SERS activity, underscoring the potential of Ag/Au nanocomposites as advanced SERS substrates for applications in chemical and biological sensing, as well as environmental monitoring.
银/金纳米复合粒子的可控合成一直是纳米材料研究中的重大挑战。本研究介绍了银(Ag)和金(Au)纳米柱状复合材料的合成、表征和表面增强拉曼散射(SERS)性能。通过改变银纳米柱(AgNSs)和金纳米柱(AuNSs)的摩尔比,优化了这些纳米复合材料的结构和等离子特性。通过合成具有不同 AgNS/AuNS 比例的复合纳米柱,我们系统地比较了它们的光学和光谱行为。结果表明,Ag/Au 纳米柱复合材料可作为高效的 SERS 基底检测罗丹明 6G (R6G),测试溶液的浓度为 10-15 到 10-6 M。值得注意的是,银/金比例为 75 : 25 的纳米柱复合材料显示出最高的 SERS 性能,对 R6G 的增强因子达到 8.9 × 106,检测限为 10-15 M。此外,这种复合材料还表现出卓越的长期稳定性,在储存十周后仍能保持性能。据我们所知,这是目前报道的使用无标记 SERS 检测 R6G 的最高灵敏度。该研究进一步详细分析了随成分变化的 SERS 活性,强调了银/金纳米复合材料作为先进 SERS 基底在化学和生物传感以及环境监测领域的应用潜力。
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引用次数: 0
Dynamic regulation of ion transport through a bis(1,3-propanediol)-based channel via allosteric azobenzene photoswitching 通过异位偶氮苯光开关动态调节双(1,3-丙二醇)基通道的离子传输
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr01711k
Manzoor Ahmad, Susmita Sarkar, Ravindra Bhogade, Abhishek Mondal, Debashis Mondal, Jagannath Mondal, Pinaki Talukdar
The transportation of ions across cell membranes is vital in biological functions and is frequently controlled by external triggers like light, ligands, and voltage. Synthetic ion transport systems, particularly those featuring gating mechanisms, have attracted considerable interest. In this research, we engineered self-assembled barrel rosette ion channels using a photoresponsive azobenzene integrated at an allosteric site. Morphological studies verified more effective self-assembly of the trans form in contrast to the cis form. The restricted self-assembly of the cis form can be ascribed to the nonplanar structure of cis azobenzene moieties, which inhibits favorable π-π stacking interactions. The ion transport studies demonstrated the formation of ion channels by the trans form with anion antiport as the primary transport mechanism. In contrast, the cis form exhibited lower efficiency. Based on these observations, dynamically gated ion transport was achieved by employing two sets of electromagnetic radiations at 365 nm and 450 nm, respectively. Molecular dynamics simulation studies demonstrated that the channel formed by assembling trans monomers exhibited greater stability when compared to the channel formed by cis monomers. Additionally, the trans channel was found to recognize and transport chloride effectively.
离子在细胞膜上的运输对生物功能至关重要,而且经常受到光、配体和电压等外部触发因素的控制。合成离子传输系统,尤其是那些具有门控机制的系统,引起了人们的极大兴趣。在这项研究中,我们利用集成在异构位点的光致伸缩偶氮苯,设计了自组装桶状玫瑰花形离子通道。形态学研究证实,反式离子通道的自组装比顺式离子通道更有效。顺式的自组装受限可归因于顺式偶氮苯分子的非平面结构抑制了有利的π-π堆叠相互作用。离子传输研究表明,反式形成的离子通道以阴离子反向传输为主要传输机制。相比之下,顺式的效率较低。基于这些观察结果,我们采用两组分别波长为 365 纳米和 450 纳米的电磁辐射实现了动态门控离子传输。分子动力学模拟研究表明,与顺式单体形成的通道相比,反式单体组装形成的通道具有更高的稳定性。此外,研究还发现反式通道能有效识别和传输氯化物。
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引用次数: 0
Tough, Durable and Strongly Bonded Self-Healing Cartilage-mimicking Noncovalent Assembly Hydrogel Nanostructures: The Interplay of Experiment and Theory 坚韧、耐用和强粘合的自愈合仿软骨非共价组装水凝胶纳米结构:实验与理论的相互作用
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4nr03322a
Shikha Awasthi, Sarvesh Kumar Pandey, Hulikere Jagdish Shwetha, Nehal Jakhar, Sankar Selvaraj
High-strength, strongly bonded and self-healing materials would be of great interest for several applications, however, the experimental and in-silico design of all such properties in a single material is challenging. In the present work, encouraged by cartilage tissue, polyacrylamide (PAM)-based tough and durable dimers (PAM-Ag and PAM-BNOH) and trimer (PAM-Ag-BNOH) nanocomposites were synthesized by encapsulating silver (Ag) and hydroxylated hexagonal boron nitride (BNOH). The strong interfacial interaction was achieved by introducing (computational modelling and DFT approaches) noncovalent bonds involved in the dimer and trimer nanohybrids. The fabricated PAM-Ag-BN nanocomposite showed higher mechanical strength (0.31 MPa compressive strength and 0.29 MPa Young’s modulus) than that of dimer hydrogel composites. The long-term durability of the hydrogel samples was tested by electrochemical testing of hydrogels in simulated body fluid and the higher corrosion resistance (icorr 2.65 × 10-5 A/cm2) was obtained for trimer hydrogel. Moreover, the supramolecular cross-linked assembly of PAM-Ag-BN perfectly showed the bioactivity including bone formation ability, self-healing performance, restricted cytotoxicity, and anti-microbial activity. The synergistic effect of nano and micron-sized particles in PAM-Ag-BN ensued in the strong interfacial interlocking through the formation of hydrogen bonding between Ag, BNOH and PAM. Therefore, the fabricated tough hydrogel composite can be a leading biomaterial for soft tissue (articular cartilage) regeneration. The present research opens new directions in developing smart self-healing nanocomposites vastly used in cartilage tissue engineering.
高强度、强粘合和自愈合材料在多个应用领域都具有重大意义,然而,在单一材料中实现所有这些特性的实验和模拟设计却极具挑战性。本研究受软骨组织的启发,通过封装银(Ag)和羟基化六方氮化硼(BNOH),合成了基于聚丙烯酰胺(PAM)的坚韧耐用的二聚体(PAM-Ag 和 PAM-BNOH)和三聚体(PAM-Ag-BNOH)纳米复合材料。通过引入(计算建模和 DFT 方法)二聚体和三聚体纳米杂化所涉及的非共价键,实现了强大的界面相互作用。制备的 PAM-Ag-BN 纳米复合材料显示出比二聚体水凝胶复合材料更高的机械强度(0.31 兆帕抗压强度和 0.29 兆帕杨氏模量)。通过在模拟体液中对水凝胶进行电化学测试,检验了水凝胶样品的长期耐久性,结果表明三聚水凝胶具有更高的耐腐蚀性(icorr 2.65 × 10-5 A/cm2)。此外,PAM-Ag-BN 的超分子交联组装完美地展现了生物活性,包括骨形成能力、自愈合性能、限制性细胞毒性和抗微生物活性。PAM-Ag-BN 中纳米级和微米级微粒的协同效应通过 Ag、BNOH 和 PAM 之间形成的氢键产生了强大的界面互锁。因此,所制备的韧性水凝胶复合材料可作为软组织(关节软骨)再生的主要生物材料。本研究为开发可广泛应用于软骨组织工程的智能自愈合纳米复合材料开辟了新方向。
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引用次数: 0
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Nanoscale
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