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Calcined Fe(III)-chelated poly(o-phenylenediamine-co-2-aminobenzenesulfonic acid) as cathode catalyst for anion-exchange membrane fuel cells 煅烧铁(III)螯合聚(邻苯二胺-co-2-氨基苯磺酸)作为阴离子交换膜燃料电池的阴极催化剂
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-30 DOI: 10.1016/j.apsadv.2026.100937
Chung-Wen Kuo , Ko-Shan Ho , Ruo-Yu Wang , Jeng-Kuei Chang , Yuan-Chung Lin , Pei-Rong Lu , Pei-Ying Lee , Tzi-Yi Wu
The oxygen reduction current of the cathode catalyst doped with both nitrogen and sulfur atoms is higher than that of the catalyst doped with only nitrogen atom or the catalyst doped with only sulfur atom. Nitrogen and sulfur dual-doped non-precious metal catalysts are synthesized through the pyrolysis of nitrogen- and sulfur-rich microporous polymeric precursor, specifically (poly(o-phenylenediamine-co-2-aminobenzenesulfonic acid) (P(OPD-co-SANI))). X-ray photoelectron spectroscopy (XPS) spectra reveal the presence of Fe-S bonds, pyridinic-N, pyridine-N oxide, graphitic-N, Fe-N, and pyrrolic-N within the FeNSC-900 composite. X-ray diffraction (XRD) analysis confirms a degree of graphitization in the NSC-1000, FeNC-900, FeNC-1000, FeNSC-900, and FeNSC-1000 catalysts. Scanning electron microscopy characterization indicates that the FeNSC-900 catalysts possess porous nanostructures, facilitating access to active sites essential for high oxygen reduction reaction (ORR) electrocatalytic activity. The FeNSC-900 catalyst demonstrates good electrocatalytic activity towards the ORR in KOH(aq), with an ORR half-wave potential of 0.76 V. In a single-cell test, membrane electrode assembly (MEA) utilizing the FeNSC-900 catalyst as the cathode achieves a peak power density of approximately 213.3 mW cm−2 at 60°C, suggesting that the FeNSC-900 catalyst is a promising alternative to platinum-based catalysts in anion exchange membrane fuel cell (AEMFC) applications.
同时掺杂氮原子和硫原子的阴极催化剂的氧还原电流高于只掺杂氮原子或只掺杂硫原子的催化剂。氮硫双掺杂非贵金属催化剂是通过富氮和富硫微孔聚合物前驱体(聚邻苯二胺-co-2-氨基苯磺酸)(P(OPD-co-SANI))的热解合成的。x射线光电子能谱(XPS)显示,fsc -900复合材料中存在Fe-S键、吡啶- n、吡啶- n氧化物、石墨- n、Fe-N和吡咯烷- n。x射线衍射(XRD)分析证实了NSC-1000、fenc900、fenc1000、fenc900和fenc1000催化剂中存在一定程度的石墨化。扫描电镜表征表明,fsc -900催化剂具有多孔纳米结构,有利于达到高氧还原反应(ORR)电催化活性所必需的活性位点。fsc -900催化剂在KOH(aq)中对ORR表现出良好的电催化活性,ORR半波电位为0.76 V。在单电池测试中,使用fsc -900催化剂作为阴极的膜电极组件(MEA)在60°C下达到了约213.3 mW cm - 2的峰值功率密度,这表明fsc -900催化剂在阴离子交换膜燃料电池(AEMFC)应用中是铂基催化剂的有前途的替代品。
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引用次数: 0
Understanding crystal surface anisotropy of organic materials via molecular modelling and facet-specific experimental characterization 通过分子模型和特定方面的实验表征来理解有机材料的晶体表面各向异性
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-29 DOI: 10.1016/j.apsadv.2026.100939
Emilia Prandini , Bruno Torre , Emanuele Bosurgi , Andrew G.P. Maloney , Chiaramaria Stani , Giovanni Birarda , Lisa Vaccari , Enzo Mario Di Fabrizio , Emmanuele Parisi , Elena Simone
The different facets of crystalline particles expose specific functional groups depending on their structure and morphology, thus, influencing surface properties of the resulting materials. As particle surface properties impact product performance, safety, and manufacturing efficiency, it is important to understand how crystal structure influences facet-specific surface properties. In this work, we focused on the effect of crystal structure and morphology on properties such as roughness, mechanical strength, and chemical features. Quercetin-dimethylformamide (QDMF), a solvated form of quercetin, was selected as a single-crystal model compound. By combining computational approaches with experimental validation, we developed a standardized procedure to correlate crystal structure packing and specific surface features. Experimental data collected using various techniques were then used to validate the simulations.
First, we utilized Particle Informatics tools to analyse the surface chemistry and topology of specific QDMF crystal facets observed experimentally, namely {1–10}, {001}, and {200}. These computational results were then validated using Atomic Force Microscopy (AFM) integrated with Infrared (IR) spectroscopy, which provided topographical insights, chemical characterization, surface roughness measurements, and mechanical properties characterization (e.g., Young Modulus).
For chemical imaging at high spatial resolution, we employed advanced mid-infrared techniques, such as Optical Photothermal Infrared (OPTIR) microscopy and scattering-type Scanning Near-field Infrared Microscopy (s-SNIM). The experimental data were in agreement with the simulations, showing how Particle Informatics tools can assist in the design of crystalline materials with tailored surface properties.
晶体颗粒的不同侧面根据其结构和形态暴露出特定的官能团,从而影响所得材料的表面特性。由于颗粒表面特性影响产品性能、安全性和制造效率,因此了解晶体结构如何影响特定表面特性非常重要。在这项工作中,我们重点研究了晶体结构和形态对粗糙度、机械强度和化学特征等性能的影响。槲皮素的溶剂化形式槲皮素-二甲基甲酰胺(QDMF)被选为单晶模型化合物。通过将计算方法与实验验证相结合,我们开发了一个标准化的程序来关联晶体结构包装和特定表面特征。然后使用各种技术收集的实验数据来验证模拟。首先,我们利用粒子信息学工具分析了实验中观察到的特定QDMF晶体面的表面化学和拓扑结构,即{1-10},{001}和{200}。然后使用原子力显微镜(AFM)和红外(IR)光谱学对这些计算结果进行验证,从而提供地形分析、化学表征、表面粗糙度测量和机械性能表征(例如杨氏模量)。对于高空间分辨率的化学成像,我们采用了先进的中红外技术,如光学光热红外显微镜(OPTIR)和散射型扫描近场红外显微镜(s-SNIM)。实验数据与模拟结果一致,显示了粒子信息学工具如何帮助设计具有定制表面特性的晶体材料。
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引用次数: 0
Nanocrystalline graphite-patterned silicon substrates for molecularly imprinted biopolymer-based electrochemical detection of glyphosate 分子印迹生物聚合物电化学检测草甘膦的纳米晶石墨图案硅衬底
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-29 DOI: 10.1016/j.apsadv.2026.100940
Livia Alexandra Dinu , Catalin Parvulescu , Octavian Gabriel Simionescu , Oana Brincoveanu , Cosmin Romanitan , Cristina Pachiu , Ludmila Motelica , Dua Özsoylu , Sevinc Kurbanoglu
In this study, we present the fabrication and characterization of a miniaturized, single-chip electrochemical sensor implemented on a silicon/silicon dioxide platform. The device incorporates a nanocrystalline graphite (NCG) working electrode and gold reference and counter electrodes, all monolithically integrated on the same substrate. This configuration provides a compact and reliable sensing architecture, combining the electrochemical advantages of carbon with the precision and reproducibility of microfabrication. A molecularly imprinted biopolymer (MIP) layer for glyphosate (GLY) detection was subsequently formed by electrodepositing chitosan (CS) in the presence of the target analyte, directly onto the NCG surface. The resulting sensor exhibited high sensitivity and selectivity, allowing indirect detection of GLY at concentrations as low as 0.015 ppb. Validation tests demonstrated excellent recovery rates in spiked water samples, highlighting the sensor’s potential for environmental monitoring applications. This integrated platform offers a promising approach for the sensitive, portable, and cost-effective detection of GLY residues.
在这项研究中,我们提出了一种小型化、单芯片电化学传感器的制造和表征,该传感器实现在硅/二氧化硅平台上。该装置集成了一个纳米晶石墨(NCG)工作电极和金参考电极和反电极,所有电极都集成在同一衬底上。这种结构提供了一个紧凑可靠的传感结构,结合了碳的电化学优势和微加工的精度和可重复性。随后,在目标分析物存在的情况下,通过电沉积壳聚糖(CS)直接在NCG表面形成用于草甘膦(GLY)检测的分子印迹生物聚合物(MIP)层。所得到的传感器具有高灵敏度和选择性,可以在低至0.015 ppb的浓度下间接检测GLY。验证测试表明,该传感器在加标水样中具有出色的回收率,突出了其在环境监测应用中的潜力。该集成平台为GLY残留的灵敏、便携和经济有效的检测提供了一种有前途的方法。
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引用次数: 0
Thermo-responsive nanostructured surface: Beeswax for enhanced condensation performance across solid, liquid, and transition states 热响应纳米结构表面:蜂蜡用于增强固体、液体和过渡态的冷凝性能
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1016/j.apsadv.2026.100936
Behzad Rezaee, Hossein Pakzad, Mohammadali Fakhri, Hossein Moosavi Shoar, Ali Moosavi, Masoud Aryanpour
The present work proposes a breakthrough technology that is focused on biocompatible bio-coating for increased efficiency of condensation in energy systems. By infusing anodized aluminum nanocavities with natural and histological beeswax, a cost-effective, scalable, and efficient solid-infused surface (SIS) is developed. Unlike a passive additive, the beeswax bio-coating modulates the surface behavior actively by adjusting contact angles and reducing contact angle hysteresis to less than 5° at operating conditions. This creates an efficient droplet formation and motion, even under high vapor flow, with a 44% improvement in the heat transfer coefficient (HTC) with respect to bare aluminum at a 16°C subcooling temperature and a 330 kW/m2 peak in heat flux at 24°C. In contrast to most studies focused on enhancing condensation with phase change materials (PCMs), in this work, the dynamic role of the beeswax coating, specifically its state transition—from solid to mushy to liquid—and its impact on droplet dynamics and thermal behavior, is emphasized. It outperforms conventional hydrophobic surfaces, especially under high subcooling conditions where flooding usually reduces efficiency. Durability tests reveal that beeswax-coated samples exhibit sustained enhanced performance even for 10 days of immersing in a wet environment or 100 hours of continuous condensation tests. Overall, the beeswax coating not only represents a breakthrough in enhancing condensation efficiency but also opens new avenues for future developments in desalination, thermal management, and renewable energy technologies.
目前的工作提出了一项突破性的技术,重点是生物相容性生物涂层,以提高能源系统中的冷凝效率。通过将天然蜂蜡注入阳极氧化铝纳米腔,开发了一种经济、可扩展、高效的固体注入表面(SIS)。与被动添加剂不同,蜂蜡生物涂层通过调节接触角来主动调节表面行为,并在操作条件下将接触角滞后减少到小于5°。这创造了一个有效的液滴形成和运动,即使在高蒸汽流量下,在16°C过冷温度下,相对于裸铝,传热系数(HTC)提高44%,在24°C时热流峰值为330 kW/m2。与大多数关注相变材料(PCMs)增强冷凝的研究相反,本研究强调了蜂蜡涂层的动态作用,特别是其从固体到糊状到液体的状态转变及其对液滴动力学和热行为的影响。它优于传统的疏水性表面,特别是在高过冷条件下,水驱通常会降低效率。耐久性测试表明,蜂蜡涂层样品即使在潮湿环境中浸泡10天或连续冷凝测试100小时,也能表现出持续增强的性能。总的来说,蜂蜡涂层不仅代表了提高冷凝效率的突破,而且为海水淡化、热管理和可再生能源技术的未来发展开辟了新的途径。
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引用次数: 0
Effect of electropolishing conditions on nanostructured anodized surfaces for enhanced superhydrophilicity and corrosion resistance of 304 and 316 L Stainless Steels 电抛光条件对纳米结构阳极氧化表面增强304和316l不锈钢超亲水性和耐腐蚀性的影响
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-23 DOI: 10.1016/j.apsadv.2026.100938
Jisoo Kim , Chanyoung Jeong
This study shows that variations in electropolishing (EP) conditions influence the stability and uniformity of the interfacial viscous layer on SUS 304 and SUS 316 L, resulting in distinct dissolution behavior and nanoscale morphology in the anodic oxide films. Under the EP1 condition, the thicker and less uniform viscous layer promoted localized dissolution, which formed a dual-layered oxide with wide and shallow polygonal pores, and with pronounced superhydrophilic and oleophilic wetting. In EP2, a thinner viscous layer was established, resulting in a denser nanoporous oxide with smaller and more uniform pores and moderate wettability. Importantly, these electropolishing-induced dimple structures acted as morphological templates, causing the anodic oxide films to develop markedly different pore sizes and thicknesses even under identical anodization conditions. XPS confirmed EP-induced redistribution of alloying elements (Cr, Ni, Mo) and the growth of multicomponent oxides after anodization. Electrochemical measurements demonstrated that EP2 significantly enhanced passivation performance, producing lower corrosion current density and higher Rfilm and Rct compared with untreated samples. Overall, this work clarifies how electropolishing conditions, in combination with alloy-dependent dissolution behavior, determine dimple formation, nanopore evolution, and corrosion performance. These insights identify EP2 as an effective pretreatment route for producing dense, stable oxide films with enhanced long-term durability on stainless steels. Importantly, this study demonstrates that variations in electropolishing conditions generate distinct micro-dimple morphologies, which in turn dictate the pore structure and thickness of the anodic oxide layer even under identical anodization parameters.
研究表明,电抛光条件的变化影响了sus304和sus316l表面黏结层的稳定性和均匀性,导致了阳极氧化膜中不同的溶解行为和纳米级形貌。在EP1条件下,较厚且较不均匀的粘性层促进了局部溶解,形成了具有宽而浅的多边形孔隙的双层氧化物,具有明显的超亲水和亲油润湿作用。在EP2中,建立了更薄的粘性层,形成了更致密的纳米孔氧化物,孔隙更小、更均匀,润湿性适中。重要的是,这些电抛光诱导的凹窝结构作为形态模板,即使在相同的阳极氧化条件下,也会导致阳极氧化膜产生显着不同的孔径和厚度。XPS证实了ep诱导合金元素(Cr, Ni, Mo)的重分布和阳极氧化后多组分氧化物的生长。电化学测量表明,与未经处理的样品相比,EP2显著增强了钝化性能,产生更低的腐蚀电流密度,更高的Rfilm和Rct。总的来说,这项工作阐明了电抛光条件如何结合合金依赖的溶解行为,决定了韧窝的形成、纳米孔的演化和腐蚀性能。这些见解表明,EP2是一种有效的预处理途径,可以在不锈钢上生产致密、稳定的氧化膜,并增强其长期耐久性。重要的是,该研究表明,即使在相同的阳极氧化参数下,电抛光条件的变化也会产生不同的微窝形态,这反过来又决定了阳极氧化层的孔结构和厚度。
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引用次数: 0
Deciphering the driving mechanisms of incubation in ultrashort pulse laser ablation 超短脉冲激光烧蚀中孵育的驱动机制解读
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-21 DOI: 10.1016/j.apsadv.2025.100928
Nicolas Thomae , Maximilian Spellauge , David Redka , Heinz P. Huber
Incubation, the systematic reduction of the ablation threshold with pulse number, critically influences ultrashort pulse laser micromachining, yet its microscopic origin remains insufficiently understood despite its widespread relevance in applications. Here, multi-pulse experiments (500 fs pulse duration, 1040 nm wavelength) with fluences ranging from 0.75 to e2 times the ablation threshold and repetition rate of 1 Hz on aluminum and stainless steel were combined with pulse-resolved absorptance from Finite-Difference-Time-Domain simulations to disentangle the roles of global absorption, crater-edge near-field enhancements, and microscopic material weakening. For aluminum, surface roughening leads to an absorption increase reciprocal to the threshold, providing a sufficient explanation of incubation. In stainless steel, however, the threshold decreases despite nearly constant absorption, demonstrating that increased absorption is not a necessary condition for incubation. Edge-localized near-field enhancements provide an early but limited contribution, saturating after a few pulses. A porosity-based description within classical nucleation theory demonstrates that material weakening can only be explained microscopically by defect-induced reductions of the effective penetration depth together with pulse-dependent nucleation rates. These findings establish a microscopic and quantitative framework for incubation, advancing the physical understanding of the transition from single- to multi-pulse ablation, providing the basis for predictive models of multi-pulse ablation with ultrashort-pulses.
随着脉冲数的系统降低烧蚀阈值,孵育对超短脉冲激光微加工有重要影响,尽管其在应用中广泛相关,但其微观起源仍未得到充分了解。在这里,多脉冲实验(500 fs脉冲持续时间,1040 nm波长),影响范围为0.75到e2倍的烧蚀阈值和重复频率为1 Hz的铝和不锈钢,结合脉冲分辨吸收从有限差分时域模拟,以区分全局吸收,陨石坑边缘近场增强和微观材料弱化的作用。对于铝,表面粗化导致吸收增加与阈值的倒数,为孵化提供了充分的解释。然而,在不锈钢中,尽管吸收几乎恒定,阈值却降低,这表明吸收增加并不是孵化的必要条件。边缘定位的近场增强提供了早期但有限的贡献,在几个脉冲后饱和。经典成核理论中基于孔隙度的描述表明,材料的弱化只能通过缺陷引起的有效穿透深度的降低以及脉冲相关的成核速率来微观解释。这些发现建立了一个微观和定量的培养框架,推进了从单脉冲到多脉冲消融转变的物理认识,为超短脉冲多脉冲消融预测模型提供了基础。
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引用次数: 0
Corrosion inhibition evaluation of sulphur-doped pomegranate peel waste-derived carbon dots for carbon steel in acidic environment 掺硫石榴皮渣碳点对碳钢在酸性环境中的缓蚀性能评价
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-17 DOI: 10.1016/j.apsadv.2026.100935
Saviour A. Umoren , Ali M.Al Nasser , Hifsa Kurdshid , Hatim D.M Dafalla , Sidra Nayer , Moses M. Solomon
Sulphur-doped carbon dots (S-PPCDs) were synthesized from pomegranate peel waste through a one-step hydrothermal process and explored as green corrosion inhibitors for carbon steel in 5% hydrochloric acid. The nanomaterials were systematically characterized using TEM, FTIR, UV–Vis, SEM/EDAX, and fluorescence analysis, which confirmed their nanoscale dimensions (∼8.9 nm), spherical morphology, and the presence of oxygen-, nitrogen-, and sulphur-containing functional groups that promote adsorption. Corrosion inhibition performance was evaluated through gravimetric tests, electrochemical methods (EIS, LPR, PDP), and surface characterization (SEM, AFM, optical profilometry). The results reveal a strong concentration dependence, with maximum inhibition efficiency of ∼89.8% at 100 mg l-1 and 30 °C. At higher concentration (150 mg l-1), a slight decrease in efficiency was observed, attributed to multilayer formation or competitive adsorption. Elevated temperature (60 °C) reduced protection efficiency to ∼47%, indicating that the adsorption mechanism is predominantly physical. Potentiodynamic polarization results show that S-PPCDs act as a mixed-type inhibitor, reducing both anodic metal dissolution and cathodic hydrogen evolution. Surface analysis confirms the formation of a compact, adherent inhibitor layer that significantly reduced roughness and pitting compared to uninhibited samples. The findings highlight the dual benefits of waste valorization and sustainable corrosion protection, positioning S-PPCDs as an environmentally benign, low-cost, and highly efficient alternative to conventional toxic inhibitors for acidic environments.
以石榴皮废料为原料,采用一步水热法合成了硫掺杂碳点(S-PPCDs),并对其作为碳钢在5%盐酸中的绿色缓蚀剂进行了探索。利用TEM, FTIR, UV-Vis, SEM/EDAX和荧光分析对纳米材料进行了系统表征,证实了它们的纳米尺寸(~ 8.9 nm),球形形貌以及含有促进吸附的含氧,含氮和含硫官能团的存在。通过重量测试、电化学方法(EIS、LPR、PDP)和表面表征(SEM、AFM、光学轮廓术)来评估缓蚀性能。结果表明,浓度依赖性强,在100 mg l-1和30°C条件下,最大抑制效率为89.8%。在较高的浓度(150 mg l-1)下,由于多层形成或竞争性吸附,观察到效率略有下降。温度升高(60°C),保护效率降低至47%,表明吸附机制主要是物理机制。动电位极化结果表明,S-PPCDs作为混合型缓蚀剂,既减少了阳极金属溶解,又减少了阴极析氢。表面分析证实,与未抑制的样品相比,形成了致密的粘附抑制剂层,显着降低了粗糙度和点蚀。研究结果强调了废物增值和可持续腐蚀保护的双重好处,使s - ppcd成为酸性环境中传统有毒抑制剂的环保、低成本和高效替代品。
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引用次数: 0
Role of Cu doping in promoting diffusion-assisted evolution of magnetic properties in equiatomic FeNi films Cu掺杂促进等原子FeNi薄膜磁性能扩散演化的作用
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-12 DOI: 10.1016/j.apsadv.2025.100929
Ashish Gupta , Deepak Prajapat , Ilya Sergeev , Rajeev Joshi , Rajeev Rawat , Anil Gome , V.R. Reddy , Mukul Gupta
The increasing need for environment-friendly substitutes for rare-earth-based magnets has sparked interest in materials such as the L10-ordered FeNi (tetrataenite) phase, which possesses high magnetocrystalline anisotropy and saturation magnetization. Despite being a promising candidate, preparation of this ordered phase in the laboratory remains a challenge due to the slow diffusion kinetics that prevent atomic ordering under normal conditions. From the theoretical estimations and experimental results, Cu is known for accelerating the atomic interdiffusion and promoting chemical disorder, which may facilitate the grain boundary diffusion. In the present work, chemically homogeneous multilayers of equiatomic FeNi and Cu-doped FeNi (5 at.%) were studied to investigate the correlation between self-diffusion and magnetism. Nuclear resonance reflectivity and forward scattering measurements on as-deposited and annealed samples showed that Cu doping substantially increases self-diffusion, which is in agreement with significant changes in the local magnetic environment, as supported by conversion electron Mössbauer spectroscopy. Although the net magnetic moment remained nearly unchanged, an enhancement in the coercivity at 573 K was observed in the Cu-doped sample, as quantified by SQUID-VSM. These observations highlight the potential of Cu-assisted diffusion channels to facilitate the formation of ordered phases in FeNi systems as a strategic approach to the development of rare-earth-free permanent magnets.
对稀土基磁体的环保替代品的需求日益增长,引发了人们对l10有序FeNi(四钛酸盐)相等材料的兴趣,该材料具有高磁晶各向异性和饱和磁化强度。尽管这是一个很有前途的候选物,但在实验室中制备这种有序相仍然是一个挑战,因为在正常条件下,缓慢的扩散动力学阻碍了原子的有序。从理论估计和实验结果来看,Cu具有加速原子间扩散和促进化学无序的作用,这可能有利于晶界扩散。在本工作中,化学均匀的多层等原子FeNi和cu掺杂FeNi (5at)。%)来研究自扩散与磁性之间的关系。沉积态和退火态样品的核共振反射率和正向散射测量表明,Cu掺杂大大增加了自扩散,这与局部磁环境的显著变化相一致,转换电子Mössbauer谱也支持了这一点。尽管净磁矩几乎保持不变,但通过SQUID-VSM量化,在573 K时,cu掺杂样品的矫顽力有所增强。这些观察结果强调了cu辅助扩散通道在FeNi体系中促进有序相形成的潜力,作为开发无稀土永磁体的战略途径。
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引用次数: 0
Multi-dimensional conductive carbon conglomeration as conductive additives for tailoring graphite/silicon alloy anodes in lithium ion batteries 多维导电碳团聚体作为锂离子电池石墨/硅合金阳极的导电添加剂
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-10 DOI: 10.1016/j.apsadv.2026.100930
Myeong-Hun Jo, Dan-Bi Moon, Hyo-Jin Ahn
To satisfy the ever-increasing demand for high-capacity and fast-charging anodes in lithium-ion batteries, the use of Si-based materials has been regarded as the most promising strategy because of their distinct lithiation capacities and kinetics. However, Si-based anodes are vulnerable to particle pulverization during repeated charge-discharge cycles, which causes the electrical isolation of Si particles. This study proposes a novel strategy to prevent the electrical isolation of micro Si alloy-based electrodes by employing multi-dimensional carbon conglomeration as a conductive additive. A multi-dimensional carbon conglomeration containing N-doped reduced graphene oxide and carbon black (NrGO/CB) was fabricated by a scalable dry method without using solvents through a mechano-fusion process. NrGO/CB functions as a valid electron transfer mechanism by activating new types of electron transfer pathways within the carbon particles through cross-linked sp3–sp2 hybrid covalent bonds. Unlike the typical sp3-hydridized system, the presence of conjugated π bonds next to the sp3-hydridized carbon causes the electrons to be delocalized at the sp3-hydridized carbon, thereby significantly enhancing electron mobility of NrGO/CB. Furthermore, the addition of a small amount of graphite functions as an initiative to integrate multi-dimensional NrGO/CB with the Si alloy particles, thereby extending the electron transfer network across the entire electrode scale. Accordingly, Si alloy anodes integrated with NrGO/CB and graphite demonstrated electrochemical performances with exceptional initial Coulombic efficiency (90.26 %) and cycling stability (101.9 % after 100 cycles at 0.1 C) compared to those of conventional carbon additives.
为了满足锂离子电池对高容量和快速充电阳极日益增长的需求,硅基材料因其独特的锂化能力和动力学特性而被认为是最有前途的策略。然而,硅基阳极在反复的充放电循环中容易受到颗粒粉碎,这导致了硅颗粒的电隔离。本研究提出了一种新的策略,以防止微硅基电极的电隔离,采用多维碳团聚作为导电添加剂。采用不使用溶剂的可伸缩干法,通过机械熔接工艺制备了含n掺杂还原性氧化石墨烯和炭黑(NrGO/CB)的多层碳团聚体。NrGO/CB作为一种有效的电子转移机制,通过交联sp3-sp2杂化共价键激活碳颗粒内新型的电子转移途径。与典型的sp3-氢化体系不同,sp3-氢化碳附近共轭π键的存在导致电子在sp3-氢化碳上离域,从而显著提高了NrGO/CB的电子迁移率。此外,少量石墨的加入可以主动将多维NrGO/CB与Si合金颗粒整合,从而在整个电极尺度上扩展电子传递网络。因此,与传统的碳添加剂相比,NrGO/CB和石墨集成的Si合金阳极具有优异的初始库仑效率(90.26%)和循环稳定性(0.1 C循环100次后101.9%)。
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引用次数: 0
Interface engineering of template free Zn2V2O7 nanoparticle embedded on Ti3C2Tx MXene hybrid supercapacitor for long term cyclic stability 无模板Zn2V2O7纳米粒子嵌入Ti3C2Tx MXene混合超级电容器的界面工程
IF 8.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-10 DOI: 10.1016/j.apsadv.2026.100932
S. Maruthasalamoorthy, R. Navamathavan
Pyrovanadate compounds are considered promising electrode candidates for advanced energy storage systems, owing to the superior multivalent redox behavior of vanadium and its inherently high electronic conductivity. In this study, Zn₂V₂O₇ nanoparticles were synthesized via a template-free approach. The high crystallinity of Zn₂V₂O₇, coupled with its indirect band gap characteristics, facilitates enhanced electrochemical performance. The semiconducting transport characteristics of Zn₂V₂O₇ (Eg ≈ 2.85 eV) enable a facile charge-transfer mechanism during redox processes, which in turn yields a high specific capacitance of 954 Fg⁻¹ at a current density of 1 Ag⁻¹. In two-dimensional titanium carbide (Ti₃C₂Tₓ) MXenes, the inherent self-stacking of nanosheets, together with the nature of the surface termination groups, critically governs both electronic conductivity and ion transport behavior. In the Zn₂V₂O₇/Ti₃C₂Tₓ composite, the uniform distribution of Zn₂V₂O₇ nanoparticles across the Ti₃C₂Tₓ surface establishes a well-defined interfacial architecture, resulting in a markedly enhanced specific capacitance of 1130 Fg⁻¹ at a current density of 1 Ag⁻¹. The solid-state device based on the Zn₂V₂O₇/Ti₃C₂Tₓ//AC configuration exhibits hybrid supercapacitive behavior, delivering a high areal capacitance of 266 mFcm⁻² at a current density of 2 mAg⁻¹. The fabricated hybrid supercapacitor demonstrates outstanding cycling stability (∼98% capacitance retention, 99% coulombic efficiency after 15,000 cycles at 10 Ag⁻¹) and delivers an energy density of 83.43 mWhkg⁻¹ with a power density of 3300 mW·kg⁻¹ at 2 mA·g⁻¹, underscoring its potential for practical applications.
由于钒优异的多价氧化还原性能及其固有的高电子导电性,焦钒酸盐化合物被认为是先进储能系统的有前途的电极候选者。本研究采用无模板法合成了Zn₂V₂O₇纳米颗粒。Zn₂V₂O₇的高结晶度,加上其间接带隙特性,有助于提高电化学性能。Zn₂V₂O₇(Eg≈2.85 eV)的半导体输运特性使其在氧化还原过程中具有简单的电荷转移机制,从而在1 Ag⁻¹的电流密度下产生954 Fg⁻¹的高比电容。在二维碳化钛(Ti₃C₂Tₓ)MXenes中,纳米片固有的自堆叠以及表面端基的性质对电子导电性和离子输运行为起着关键作用。在Zn₂V₂O₇/Ti₃C₂Tₓ复合材料中,Zn₂V₂O₇纳米颗粒在Ti₃C₂Tₓ表面的均匀分布建立了一个明确的界面结构,从而在电流密度为1 Ag⁻¹时显着提高了1130 Fg⁻¹的比电容。基于Zn₂V₂O₇/Ti₃C₂Tₓ//AC结构的固态器件表现出混合超电容行为,在电流密度为2 mAg⁻²时提供266 mFcm的高面电容。制作的混合超级电容器具有出色的循环稳定性(在10 mA·g⁻¹下循环15,000次后,电容保持率为98%,库仑效率为99%),能量密度为83.43 mWhkg⁻¹,功率密度为3300 mW·kg⁻¹,强调了其实际应用的潜力。
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引用次数: 0
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Applied Surface Science Advances
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