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Functionally graded MXene/asymmetric carbon aerogel architectures integrating micron-level electromagnetic signature management with phase-change energy storage 功能梯度MXene/不对称碳气凝胶结构集成微米级电磁特征管理与相变储能
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-27 DOI: 10.1016/j.carbon.2025.121103
Ke Xu , Junlin Liu , Rui Zhang, Shujuan Tan, Guanbgin Ji
Electromagnetic detection technologies, especially infrared surveillance which utilizes micro-level electromagnetic waves, present formidable battlefield threats by detecting thermal signatures of personnel and equipment, demanding innovative materials that reconcile micro-level electromagnetic wave camouflage. Furthermore, the advanced communication and sensor networks require continuous energy supply. This work develops an asymmetric trilayer MXene/carbon-based composite to achieve synchronized micro-level electromagnetic wave signature management and phase-change energy storage. The functionally graded architecture combines a low-emissivity MXene surface, paraffin-saturated phase-change interlayer, and insulating chitosan aerogel substrate. During simulated equipment operation, the coated regions maintain near-ambient temperatures with differentials up to 26.2 °C versus uncovered areas while providing 179–201 J g−1 latent heat capacity. Preheated composites function as persistent decoys through controlled heat dissipation kinetics. Mechanically robust with 158.96 kPa compressive strength and 79.77 % cyclic retention, the optimized 7 mm-thick structure reduces infrared emissivity by 0.372. This multifunctional platform enables dual-mode thermal deception for next-generation micro-level electromagnetic wave detection defense system.
电磁探测技术,特别是利用微电平电磁波的红外监视,通过探测人员和设备的热特征,提出了强大的战场威胁,要求创新材料调和微电平电磁波伪装。此外,先进的通信和传感器网络需要持续的能源供应。本研究开发了一种不对称的三层MXene/碳基复合材料,以实现同步微电平电磁波特征管理和相变储能。功能梯度结构结合了低发射率MXene表面,石蜡饱和相变中间层和绝缘壳聚糖气凝胶底物。在模拟设备运行过程中,涂层区域与未覆盖区域相比保持接近环境温度的差异高达26.2°C,同时提供179 - 201j g−1的潜热容。预热复合材料通过控制散热动力学作为持久诱饵。优化后的7 mm厚结构具有158.96 kPa的抗压强度和79.77%的循环保留率,使红外发射率降低0.372。该多功能平台可为下一代微电平电磁波探测防御系统提供双模热欺骗。
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引用次数: 0
Scalable wet-spinning of multifunctional carbon black-expanded graphite/thermoplastic polyurethane fibers for high-sensitivity wearable sensing and visibility 用于高灵敏度可穿戴传感和可视性的多功能炭黑膨胀石墨/热塑性聚氨酯纤维的可扩展湿纺
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-27 DOI: 10.1016/j.carbon.2025.121105
Zhaoxing Lin , Yingli Wu , Gang Zhao , Honghao Lin , Zhiheng Gu , Tingting Wu , Lihong Xu , Chunhong Zhu , Jian Shi , Xiangfang Peng , Tingjie Chen
Elastic and conductive fibers are critical for next-generation wearable electronics, where achieving simultaneous stretchability, durability, and sensing performance remains a challenge. Here, this study reports a scalable wet-spinning strategy to fabricate high elasticity conductive fibers composed of carbon black and expanded graphite (CB-EG) hybrids within a thermoplastic polyurethane (TPU) matrix. Synergistic interactions among CB, EG, and TPU promote uniform filler dispersion, regulate TPU microphase separation, and stabilize conductive pathways, resulting in enhanced electromechanical properties. The optimized fibers exhibit an electrical conductivity of 0.05 S/m, tensile strength of 728 kPa, and fracture elongation of ∼590 %. When applied as strain sensors, they achieve a GF up to 7645, a rapid response time of 120 ms, and enable precise, real-time monitoring of complex human motions, including gesture recognition during outdoor cycling. Furthermore, the integration of night-luminescent functionality significantly improved cyclist visibility under low-light conditions, thereby contributing to enhanced safety. These results highlight the potential of CB-EG/TPU fibers as multifunctional materials for advanced wearable electronics and smart textiles.
弹性和导电纤维对下一代可穿戴电子产品至关重要,同时实现可拉伸性、耐用性和传感性能仍然是一个挑战。在这里,本研究报告了一种可扩展的湿纺策略,该策略可以在热塑性聚氨酯(TPU)基体中制造由炭黑和膨胀石墨(CB-EG)混合物组成的高弹性导电纤维。CB、EG和TPU之间的协同作用促进了填料的均匀分散,调节了TPU的微相分离,稳定了导电通路,从而提高了机电性能。优化后的纤维电导率为0.05 S/m,抗拉强度为728 kPa,断裂伸长率为~ 590%。当用作应变传感器时,它们的GF高达7645,快速响应时间为120毫秒,并且能够精确,实时地监测复杂的人体运动,包括户外骑行期间的手势识别。此外,夜光功能的集成显著提高了骑车者在弱光条件下的能见度,从而有助于提高安全性。这些结果突出了CB-EG/TPU纤维作为先进可穿戴电子产品和智能纺织品的多功能材料的潜力。
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引用次数: 0
A three-dimensional porous thermal interface material composed of multiple carbon-based fillers with outstanding thermal conductivity and electromagnetic shielding properties 一种由多种碳基填料组成的三维多孔热界面材料,具有优异的导热性能和电磁屏蔽性能
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-27 DOI: 10.1016/j.carbon.2025.121064
Jianrui Yao , Zhipeng Sun , Cheng Ma , Jitong Wang , Yinxu Zhang , Wenming Qiao
The increasing popularity of electronic devices is placing higher demands on thermal management and electromagnetic interference shielding effectiveness. polyamidoic acid (PAA), mesocarbon microbeads (MCMB), and graphene nanosheets (GNs) were effectively combined through directional freezing to form the three-dimensional porous material PMGN. Then, through flexible encapsulation and backfilling with PDMS, a composite material PDMS/PMGN with excellent thermal conductivity of 15.45 W/(m⋅K) and electromagnetic shielding effectiveness (EMI SE) of 94.13 dB was obtained. PDMS/PMGN successfully combines multiple carbon-based fillers in a synergistic manner, forming a highly efficient monolithic structure with great mechanical properties and thermal stability, which is suitable for high-frequency electronic devices, aerospace applications, and smart wearable devices.
电子设备的日益普及对热管理和电磁干扰屏蔽效能提出了更高的要求。将聚酰胺酸(PAA)、介碳微珠(MCMB)和石墨烯纳米片(GNs)通过定向冷冻有效结合,形成三维多孔材料PMGN。然后,通过PDMS柔性封装回填,得到导热系数为15.45 W/(m·K)、电磁屏蔽效能(EMI SE)为94.13 dB的复合材料PDMS/PMGN。PDMS/PMGN成功地将多种碳基填料协同结合,形成了具有良好机械性能和热稳定性的高效单片结构,适用于高频电子器件、航空航天应用和智能可穿戴设备。
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引用次数: 0
Electromagnetic wave absorbing composites with low filling ratio characteristic routed via introducing ZnO with different morphology on the surface of carbon fiber 通过在碳纤维表面引入不同形貌的ZnO,制备了具有低填充率特性的电磁波吸收复合材料
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-27 DOI: 10.1016/j.carbon.2025.121106
Yuhan Guo , Zhenxia Wang , Limin Tao , Hao Cai , Weiyu Cao
The requirement for structural materials with function of electromagnetic wave absorbing is to have excellent mechanical property, impedance matching and attenuation ability simultaneously. Since outstanding electromagnetic wave absorbing property is originated from the synergistic effects of multiple absorbing modes, a strategy of introducing ZnO with excellent dielectricity on the surface of carbon fiber with high mechanical performance and low density was proposed for obtaining electromagnetic wave absorbing composites in this study. ZnO with nanowire and nanosheet morphology was vertically grown on the surface of carbon fibers by the two-step solvothermal method. Benefit from great dielectric properties and improved impedance matching, the high performance absorbing materials were prepared. Both CF/ZnO composites with nanowire (CF@ZnO-NW) and nanosheet (CF@ZnO-NS) morphology have excellent and manageable electromagnetic wave absorption properties. At low filling ratio of only 5 %, CF@ZnO-NW exhibited significant electromagnetic wave absorption properties with an RLmin of −60.61 dB at a thickness of 2.4 mm while the RLmin was −54.95 dB for CF@ZnO-NS at 2.0 mm and 10 % filling rate. It is expected to contribute an effective route for the construction of carbon fiber based composites with better electromagnetic wave absorbing performance by morphological controlment of modification layer.
对具有电磁波吸收功能的结构材料的要求是同时具有优良的力学性能、阻抗匹配能力和衰减能力。由于优异的电磁波吸收性能源于多种吸收模式的协同作用,本研究提出了在高力学性能、低密度碳纤维表面引入介电性能优良的ZnO的策略,以获得电磁波吸收复合材料。采用两步溶剂热法在碳纤维表面垂直生长具有纳米线和纳米片形貌的ZnO。利用良好的介电性能和改进的阻抗匹配,制备了高性能吸波材料。具有纳米线(CF@ZnO-NW)和纳米片(CF@ZnO-NS)形态的CF/ZnO复合材料具有优异的可控电磁波吸收性能。当填充率仅为5%时,CF@ZnO-NW在厚度为2.4 mm时表现出显著的电磁波吸收特性,RLmin为−60.61 dB,而在2.0 mm和填充率为10%时,CF@ZnO-NS的RLmin为−54.95 dB。通过改性层的形态控制,有望为构建具有更好电磁波吸收性能的碳纤维基复合材料提供一条有效途径。
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引用次数: 0
Gelation failure mechanism of carbon nanotube cementitious composites 碳纳米管胶凝复合材料的凝胶破坏机理
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-27 DOI: 10.1016/j.carbon.2025.121104
Haoxin Lai, Qinghua Li, Guan Quan, Xiaoran Wang, Facheng Song, Yu Peng, Chaokun Hong, Shilang Xu
While the decreased mechanical properties of carbon nanotube cementitious composites (CNTCCs) have been widely attributed to CNT agglomeration, many studies implied that better dispersion does not always lead to higher strength. The identification of the weak phase in CNTCCs has been a big challenge, impeding a deeper understanding of the interactions between CNTs and cement paste. This study employed dilute paste experiments to amplify, separate, and characterize the weak phase in CNTCCs, specifically, an entangled, hemi-rigid network of the hydration products and CNTs. This newly-found microstructure in CNTCC naturally holds the ability to explain the rheology changes and refining effects caused by CNT. The deposition process of various particles was examined using X-CT and UV–Vis, and detailed phase analyses were conducted on the sediments. These methods described how the CNT-hydrate entanglement affected the density and phase distribution of the cement matrix. Finally, the impact of CNT-hydrate entanglement on mechanical-related properties was validated through SEM, compressive tests, and powder MIP. Destroying and rebuilding the interactions among hydration products made the impact of a very-high CNT content shift from enhancement to weakening. And how the CNT-hydrate entanglement misled the judgment from conventional MIP was illustrated. This study found that the essence of the decrease is attributed to the C–(A)–S–H gel appearing to lose its function of binding particles together; therefore, this mechanism is termed gelation failure.
虽然碳纳米管胶凝复合材料(CNTCCs)的力学性能下降被广泛归因于碳纳米管团聚,但许多研究表明,良好的分散并不一定意味着更高的强度。碳纳米管中弱相的识别一直是一个巨大的挑战,阻碍了对碳纳米管与水泥浆之间相互作用的更深入理解。本研究采用稀浆实验来放大、分离和表征CNTCCs中的弱相,特别是水化产物和碳纳米管的纠缠半刚性网络。这一新发现的碳纳米管微观结构自然能够解释碳纳米管引起的流变变化和精炼效应。利用X-CT和UV-Vis检测了各种颗粒的沉积过程,并对沉积物进行了详细的物相分析。这些方法描述了碳纳米管水合物纠缠如何影响水泥基体的密度和相分布。最后,通过扫描电镜、压缩测试和粉末MIP验证了碳纳米管水合物纠缠对机械相关性能的影响。破坏和重建水化产物之间的相互作用使得碳纳米管含量很高时的影响从增强变为减弱。并说明了碳纳米管水合物纠缠如何误导了传统MIP的判断。本研究发现,减少的本质是由于C - (A) - s - h凝胶似乎失去了将颗粒结合在一起的功能;因此,这种机制被称为胶凝失效。
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引用次数: 0
CeTi@C80: A tender single molecule magnet with electric and magnetic didipoles investigated with magnetometry and x-ray absorption spectroscopy CeTi@C80:一种具有电偶极子和磁偶极子的柔软单分子磁铁,用磁强计和x射线吸收光谱学进行了研究
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-26 DOI: 10.1016/j.carbon.2025.121098
Wei Chuang Lee , Lebin Yu , Zhanxin Jiang , Ziqi Hu , Ari Paavo Seitsonen , René Monnier , Bernard Delley , Matthias Muntwiler , Shangfeng Yang , Thomas Greber
In endohedral fullerenes otherwise unstable atomic clusters can be stabilized. Here we investigate the electronic and magnetic properties of the dimetallic endohedral fullerene CeTi@C80, a molecular system encapsulating nominally trivalent cations of Ce and Ti within a C80 carbon cage. Using low temperature magnetometry and temperature-dependent X-ray Absorption Spectroscopy (XAS) at the Ce M4,5-edge, we explore the magnetism and the orientation of the Ce–Ti endohedral unit. The magnetization measurements indicate “tender” single-molecule magnetism with small hysteresis and a 3.3 μB magnetic moment. The measured XA spectra of drop-cast molecules can be simulated with a ligand field of a didipole that consists of a C–Ti and an opposite Ce–C dipole. They confirm trivalent Ce with a Jz=5/2 ground state and random distribution of the Ce–Ti axes. Temperature-dependent XAS below room temperature shows minimal spectral change, indicating a thermally robust ground-state. These findings establish CeTi@C80 as a stable electric and magnetic didipole single molecule magnet.
在内嵌富勒烯中,不稳定的原子团簇可以稳定。在这里,我们研究了双金属内嵌富勒烯CeTi@C80的电子和磁性能,这是一种在C80碳笼中封装了名义上的Ce和Ti三价阳离子的分子体系。利用低温磁强计和温度相关的x射线吸收光谱(XAS)在Ce M4,5边,我们探索了Ce - ti内嵌单元的磁性和取向。磁化测量结果表明,该材料具有“柔软”的单分子磁性,磁滞小,磁矩为3.3 μB。用由C-Ti偶极子和相反的Ce-C偶极子组成的配体场可以模拟滴投分子的XA光谱。他们证实了三价Ce具有Jz=5/2基态和Ce - ti轴的随机分布。温度相关的XAS在室温下显示出最小的光谱变化,表明热稳定的基态。这些发现证实CeTi@C80是一个稳定的电和磁双偶极单分子磁体。
{"title":"CeTi@C80: A tender single molecule magnet with electric and magnetic didipoles investigated with magnetometry and x-ray absorption spectroscopy","authors":"Wei Chuang Lee ,&nbsp;Lebin Yu ,&nbsp;Zhanxin Jiang ,&nbsp;Ziqi Hu ,&nbsp;Ari Paavo Seitsonen ,&nbsp;René Monnier ,&nbsp;Bernard Delley ,&nbsp;Matthias Muntwiler ,&nbsp;Shangfeng Yang ,&nbsp;Thomas Greber","doi":"10.1016/j.carbon.2025.121098","DOIUrl":"10.1016/j.carbon.2025.121098","url":null,"abstract":"<div><div>In endohedral fullerenes otherwise unstable atomic clusters can be stabilized. Here we investigate the electronic and magnetic properties of the dimetallic endohedral fullerene CeTi@C<sub>80</sub>, a molecular system encapsulating nominally trivalent cations of Ce and Ti within a C<sub>80</sub> carbon cage. Using low temperature magnetometry and temperature-dependent X-ray Absorption Spectroscopy (XAS) at the Ce M<span><math><msub><mrow></mrow><mrow><mn>4</mn><mo>,</mo><mn>5</mn></mrow></msub></math></span>-edge, we explore the magnetism and the orientation of the Ce–Ti endohedral unit. The magnetization measurements indicate “tender” single-molecule magnetism with small hysteresis and a 3.3 <span><math><msub><mrow><mi>μ</mi></mrow><mrow><mi>B</mi></mrow></msub></math></span> magnetic moment. The measured XA spectra of drop-cast molecules can be simulated with a ligand field of a didipole that consists of a C–Ti and an opposite Ce–C dipole. They confirm trivalent Ce with a <span><math><msub><mrow><mi>J</mi></mrow><mrow><mi>z</mi></mrow></msub></math></span>=5/2 ground state and random distribution of the Ce–Ti axes. Temperature-dependent XAS below room temperature shows minimal spectral change, indicating a thermally robust ground-state. These findings establish CeTi@C<sub>80</sub> as a stable electric and magnetic didipole single molecule magnet.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"248 ","pages":"Article 121098"},"PeriodicalIF":11.6,"publicationDate":"2025-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145748437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
FWCNT-templated carbon fibers from a high carbonization yield, solution-processable p-phenylene 由高炭化率,可溶液加工的对苯制备的fwcnt模板碳纤维
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-26 DOI: 10.1016/j.carbon.2025.121096
Woojae Jeong , Dong Jun Kang , Junho Lee , Hwayoung Ko , Tae Hee Han , Jaeuk Sung
Current carbon fiber manufacturing relies heavily on polyacrylonitrile (PAN) precursors, which suffer from energy-intensive processing and limited carbon yields (∼50 %). Here, we demonstrated a solution-processable poly(benzophenone) (PBP) precursor system that bypasses oxidative stabilization while achieving exceptional carbonization yields of 74 % at 1000 °C. The rigid-rod aromatic structure of PBP provides thermodynamic favorability toward graphitic transformation, while benzophenone linkages enable solubility in aprotic solvents for continuous wet-spinning. Strategic incorporation of few-walled carbon nanotubes (FWCNTs) at 0.25–1.0 wt % creates a templated carbonization pathway through non-covalent π-π interactions between aromatic polymer chains and nanotube sidewalls. This FWCNT-guided structural evolution enhances graphitic ordering (ID/IG ratio changed from 0.89 to 0.71), promotes anisotropic carbon domain growth, and delivers concurrent improvements in mechanical, electrical, and thermal properties. Optimized PBP precursor with 1 wt % FWCNT (P-CNT-1.00) derived carbon fibers achieved tensile strength of 397 MPa, Young's modulus of 93 GPa, electrical conductivity of 207 S cm−1, and thermal conductivity of 19.5 W m−1 K−1, which represents a 1.3, 3.4, 1.7, and 4.8-fold improvements over pristine PBP, respectively. This molecularly engineered approach demonstrates the feasibility of solvent processable aromatic polymer as a practical carbon fiber precursor that not only shows higher carbonization yield and energy efficiency, but also can be further enhanced via FWCNT incorporation.
目前的碳纤维制造严重依赖聚丙烯腈(PAN)前体,这种前体受到能源密集型加工和碳产量有限(约50%)的影响。在这里,我们展示了一种可溶液加工的聚二苯甲酮(PBP)前体体系,该体系绕过氧化稳定,同时在1000°C下实现了74%的异常碳化收率。PBP的刚性棒芳香结构为石墨转化提供了热力学优势,而二苯甲酮键使其在非质子溶剂中具有溶解性,可以进行连续湿纺丝。0.25-1.0 wt %的低壁碳纳米管(FWCNTs)通过芳香聚合物链和纳米管侧壁之间的非共价π-π相互作用,形成了模板化的碳化途径。这种由fwcnt引导的结构演化增强了石墨的有序性(ID/IG比值从0.89变为0.71),促进了碳畴的各向异性生长,并同时改善了机械、电学和热性能。优化后的PBP前驱体含有1 wt %的FWCNT (P-CNT-1.00)衍生碳纤维,抗拉强度为397 MPa,杨氏模量为93 GPa,电导率为207 S cm−1,导热系数为19.5 W m−1 K−1,分别比原始PBP提高了1.3倍,3.4倍,1.7倍和4.8倍。这种分子工程方法证明了溶剂可加工芳香族聚合物作为碳纤维前驱体的可行性,不仅具有较高的炭化率和能源效率,而且通过加入FWCNT可以进一步提高炭化效率。
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引用次数: 0
Superelastic carbon aerogels with micro-arch lamellar reinforcement for efficient microwave absorption and multifunctionality 具有微拱形层状增强的超弹性碳气凝胶,具有高效的微波吸收和多功能性
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-26 DOI: 10.1016/j.carbon.2025.121086
Caiqin Gao , Yuru Wang , Yandong Wang , Kang Xu , Lu Chen , Yi Zhang , Xianchun Chen , Yuan Chen , Jinhong Yu , Yanqing Wang
The growing complexity and miniaturization of electronic devices have heightened the need for lightweight, flexible, and high-performance electromagnetic wave (EMW) absorbers. However, developing flexible carbon-based aerogels remains a significant challenge. This study introduces a bioinspired dynamic interface chemistry regulation strategy, utilizing a bidirectional freeze-casting and thermal etching approach to fabricate cellulose nanofibers (CNF)/polyhydroxyalkanoate (PHA)/graphene oxide (GO) aerogels. During thermal etching, PHA decomposes to release crotonic acid, which in situ reduces GO, forming an interface rich in sp2 carbon domains, defects, and polar functional groups (C–O, CO). This synergistic interface enhances conduction and polarization loss, enabling exceptional EMW absorption with a minimum reflection loss (RLmin) of −54.72 dB at a thickness of 1.86 mm and an effective absorption bandwidth (EAB) of 5.75 GHz. Specifically, it also exhibits excellent flexibility under subzero and ambient conditions (−20 °C–25 °C). Owing to excellent elasticity, the aerogels show fast response pressure sensing (capable of encoding Morse code), making them promising for integration into wearable electronics. Furthermore, the materials achieve highly stable Joule heating (15 s–65 °C at 10V), infrared stealth, effective hydrophobicity (water contact angle of 123°), and flame retardancy. This work provides a novel approach for designing flexible carbon-based aerogels for next-generation wearable electronic applications.
随着电子设备的日益复杂化和小型化,对轻型、柔性和高性能电磁波(EMW)吸收器的需求日益增加。然而,开发柔性碳基气凝胶仍然是一个重大挑战。本研究介绍了一种受生物启发的动态界面化学调节策略,利用双向冷冻铸造和热蚀刻方法制备纤维素纳米纤维(CNF)/聚羟基烷酸酯(PHA)/氧化石墨烯(GO)气凝胶。在热蚀刻过程中,PHA分解释放出巴豆酸,巴豆酸在原位还原氧化石墨烯,形成一个富含sp2碳畴、缺陷和极性官能团(C-O, CO)的界面。这种协同界面增强了传导和极化损耗,使EMW吸收性能优异,在厚度为1.86 mm时,最小反射损耗(RLmin)为−54.72 dB,有效吸收带宽(EAB)为5.75 GHz。具体来说,它在零下和环境条件下(- 20°C - 25°C)也表现出出色的灵活性。由于优异的弹性,气凝胶表现出快速响应压力传感(能够编码摩尔斯电码),使它们有望集成到可穿戴电子产品中。此外,该材料具有高度稳定的焦耳加热(15 s-65°C, 10V)、红外隐身、有效疏水性(水接触角123°)和阻燃性。这项工作为设计下一代可穿戴电子应用的柔性碳基气凝胶提供了一种新方法。
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引用次数: 0
Breaking the salinity barrier: Hybrid graphene oxide – polyethylenimine dispersions in high ionic strength aqueous media 打破盐度障碍:高离子强度水介质中氧化石墨烯-聚乙烯亚胺杂化分散体
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-25 DOI: 10.1016/j.carbon.2025.121095
Raquel C.F.G. Lopes , Cláudia K.B. de Vasconcelos , Pollyanna R. dos Santos , Philipe A.P. Silva , Myriano H. Oliveira Jr. , Vinicius Caliman , Glaura G. Silva
Overcoming the salinity barrier remains a fundamental challenge in the deployment of carbon-based nanomaterials for applications in high ionic strength environments, such as water treatment, desalination and enhanced oil recovery. Herein, we report the covalent functionalization of graphene oxide (GO) with branched polyethyleneimine (PEI) to produce a novel GO–PEI hybrid nanomaterial capable of forming stable aqueous dispersions in saline solutions. The functionalization was achieved under mild conditions, yielding a hybrid with approximately 53 ± 2.5 wt% PEI, estimated from the thermogravimetric residues of GO, PEI, and GO–PEI using a linear mixing model, which shows enhanced thermal stability and a significantly altered surface chemistry. This estimation assumes linear additivity of residues, which may be affected by crosslinking or differing char formation between components. Therefore, the obtained value should be considered an approximation. Furthermore, the colloidal stability was greatly enhanced as observed through a thorough evaluation across different salt types, concentrations (50–500 ppm), and ionic strengths (0.0–3.0), revealing that GO–PEI dispersions exhibited high colloidal stability up to 21 days even at ionic strengths as high as 3.0, outperforming pristine GO. The positive surface charge and steric hindrance provided by the PEI chains were key to preventing aggregation, even under harsh conditions. This work introduces a straightforward strategy to extend the applicability of GO in highly saline media, offering significant potential for technological and environmental applications where nanomaterial dispersion stability is crucial.
克服盐度障碍仍然是碳基纳米材料在高离子强度环境中应用的一个基本挑战,例如水处理、海水淡化和提高石油采收率。在此,我们报道了氧化石墨烯(GO)与支化聚乙烯亚胺(PEI)的共价功能化,以产生一种新型的GO - PEI杂化纳米材料,能够在盐水溶液中形成稳定的水分散体。功能化是在温和的条件下实现的,通过线性混合模型,从GO、PEI和GO - PEI的热重残留物估计,得到了PEI约53±2.5 wt%的杂化产物,显示出增强的热稳定性和显著改变的表面化学性质。这种估计假设残基的线性可加性,这可能受到交联或组分之间不同的炭形成的影响。因此,得到的值应该被认为是近似值。此外,通过对不同盐类型、浓度(50-500 ppm)和离子强度(0.0-3.0)的全面评估,观察到胶体稳定性大大增强,表明GO - pei分散体即使在离子强度高达3.0的情况下也表现出长达21天的高胶体稳定性,优于原始氧化石墨烯。PEI链提供的正表面电荷和空间位阻是防止聚合的关键,即使在恶劣的条件下也是如此。这项工作介绍了一种直接的策略来扩展氧化石墨烯在高盐介质中的适用性,为纳米材料分散稳定性至关重要的技术和环境应用提供了巨大的潜力。
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引用次数: 0
Machine learning-assisted first-principles study of structural, electronic, optical, thermal, and mechanical properties of novel s-triazine-based organic framework monolayers 基于机器学习辅助的新型s-三嗪基有机骨架单层结构、电子、光学、热学和机械性能第一性原理研究
IF 11.6 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-24 DOI: 10.1016/j.carbon.2025.121092
Bohayra Mortazavi , Fazel Shojaei , Masoud Shahrokhi , Xiaoying Zhuang
Nanoporous carbon-nitride covalent organic frameworks (CN-COFs) represent an emerging class of nanomaterials with tunable architectures and scalable synthesis routes. Recent advances introduced four novel CN-COFs nanosheets, featuring hybrid benzene/s-triazine cores. Using these advances as a foundation, we designed four CN-COFs with identical structures but slightly different chemistry. We evaluated structural stability, electronic/optical properties, mechanical strength, and thermal transport using a hybrid approach combining density functional theory (DFT) and machine learning interatomic potentials (MLIPs). Complex stable atomic configurations, along with thermal and mechanical properties, were efficiently identified using MLIPs, while electronic and optical properties were accurately analyzed through single-step DFT calculations. Structurally, four frameworks exhibit Kagome lattice symmetry, hosting unique electronic features like flat and Dirac bands, while corrugated configurations induce modified band structures. These semiconductors display band gaps ranging from 2.73 to 3.72 eV, allowing strong photon absorption across the UV–visible spectrum and aligning well with water redox potentials, making them promising for optoelectronic and photocatalytic applications. Despite their highly porous nature, CN-COFs demonstrate impressive mechanical resilience, sustaining strain levels up to around 0.3 and tensile strengths exceeding 10 GPa, significantly surpassing conventional polymers. Crucially, we demonstrate that fine-tuning the chemistry of the linkages allows for the occurrence of significan out-of-plane corrugations, resulting in ultralow lattice thermal conductivity, which is particularly attractive for thermoelectric and thermal insulating applications. Our comprehensive findings confirm the stability, mechanical robustness, ultralow thermal conductivity and appealing semiconducting nature of CN-COFs, highlighting their application prospects in flexible, high-performance optoelectronics and energy storage and conversion systems.
纳米多孔碳氮共价有机骨架(CN-COFs)是一类具有可调结构和可扩展合成路线的新型纳米材料。最近的进展介绍了四种新型的CN-COFs纳米片,其核心是苯/s-三嗪杂化。以这些进展为基础,我们设计了四种结构相同但化学成分略有不同的CN-COFs。我们使用结合密度泛函理论(DFT)和机器学习原子间势(MLIPs)的混合方法评估了结构稳定性、电子/光学性质、机械强度和热输运。使用MLIPs可以有效地识别复杂的稳定原子构型,以及热性能和力学性能,而通过单步DFT计算可以准确地分析电子和光学性能。在结构上,四个框架表现出Kagome晶格对称,拥有独特的电子特征,如平面和狄拉克带,而波纹结构诱导修改带结构。这些半导体显示的带隙范围为2.73至3.72 eV,允许在紫外可见光谱中强光子吸收,并且与水氧化还原电位很好地匹配,使其在光电和光催化应用中具有前景。尽管具有高度多孔性,但CN-COFs具有令人印象深刻的机械弹性,可维持高达0.3左右的应变水平,抗拉强度超过10 GPa,大大超过传统聚合物。至关重要的是,我们证明了微调连接的化学性质允许发生显着的面外波纹,从而导致超低的晶格热导率,这对于热电和隔热应用特别有吸引力。我们的综合研究结果证实了CN-COFs的稳定性,机械鲁棒性,超低导热性和吸引人的半导体性质,突出了它们在柔性,高性能光电子和能量存储和转换系统中的应用前景。
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