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Molecular layer deposition of hybrid silphenylene-based dielectric film 杂化硅苯基介电膜的分子层沉积
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-10-11 DOI: 10.1007/s42114-023-00756-8
Xinzhi Li, Marko Vehkamäki, Mykhailo Chundak, Kenichiro Mizohata, Anton Vihervaara, Matti Putkonen, Markku Leskelä, Mikko Ritala

Molecular layer deposition (MLD) offers molecular level control in deposition of organic and hybrid thin films. This article describes a new type of inorganic–organic silicon-based MLD process where Aluminium chloride (AlCl3) and 1,4-bis(triethoxysilyl)benzene (BTEB) were used as precursors. Hybrid films were deposited at a temperature range of 300 to 500 °C and high growth per cycle (GPC) up to 1.94 Å was obtained. Field emission scanning electron microscopy (FESEM) and atomic force microscopy (AFM) were used to analyze the appearance of the film surface. The hybrid film was amorphous in low-magnification FESEM images but some particulates appeared in high-magnification FESEM images (200 k). Attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), Time-of-flight elastic recoil detection analysis (ToF-ERDA), and X-ray photoelectron spectroscopy (XPS) were employed to analyze the structure and composition of the hybrid film. The ratio of Al/Si in the hybrid film was 0.8. The storage environment of the films affected their capacitance, dielectric constant, leakage performance, and breakdown voltage. A film stored in a high vacuum (10–6 mbar) environment had low leakage current density (< 10–6 A × cm−2 at an applied voltage of 28 V) and a dielectric constant of 4.94, which was much smaller than after storing in a humid ambient environment.

Graphical abstract

分子层沉积(MLD)为有机薄膜和杂化薄膜的沉积提供了分子水平的控制。本文介绍了一种以氯化铝(AlCl3)和1,4-双(三乙氧基硅基)苯(BTEB)为前驱体的新型无机-有机硅基MLD工艺。在300 ~ 500℃的温度范围内沉积杂化膜,获得了高达1.94 Å的高生长周期(GPC)。采用场发射扫描电镜(FESEM)和原子力显微镜(AFM)对膜表面形貌进行了分析。利用衰减全反射傅立叶变换红外光谱(ATR-FTIR)、飞行时间弹性反冲检测分析(ToF-ERDA)和x射线光电子能谱(XPS)分析了杂化膜的结构和组成。杂化膜中Al/Si的比值为0.8。薄膜的储存环境对薄膜的电容、介电常数、漏电性能和击穿电压都有影响。在高真空(10-6 mbar)环境下存储的薄膜具有较低的漏电流密度(外加电压为28 V时为10-6 A × cm−2),介电常数为4.94,远小于在潮湿环境下存储的薄膜。图形抽象
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引用次数: 0
High-performance multifunctional energy storage-corrugated lattice core sandwich structure via continuous carbon fiber (CCF)/polyamide 6 (PA6) 3D printing 连续碳纤维(CCF)/聚酰胺6(PA6)3D打印高性能多功能储能波纹格芯夹芯结构
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-10-03 DOI: 10.1007/s42114-023-00761-x
Hui-Jin Um, Na-Hyun Jeon, Ji-Hwan Shin, Hak-Sung Kim

In this study, an energy storage multifunctional sandwich structure (ESMS) was designed to perform well-balanced and excellent multifunctional performance. The corrugated core sandwich structure was newly developed to prevent the degradation of mechanical properties even when lithium polymer (LiPo) batteries are integrated. The empty space of the corrugated core was used as an energy storage space, and the corrugated core was fabricated via 3D printing technology using a continuous carbon fiber filament. The energy storage characteristics were implemented using LiPo batteries embedded in the neutral axis of the sandwich structure. The static and fatigue bending properties of the ESMSs were analyzed through a three-point bending (3PB) test. A battery charge/discharge test was performed before and after the mechanical tests to analyze the effect of bending loading on the energy storage properties. The conventional foam-core ESMS showed negative changes in flexural properties such as strength (−27% in Foam-SH) and modulus (−22% in Foam-AD) due to the battery embedding. On the other hand, in the case of the 3D-printed core ESMS, no degradation in mechanical properties was observed even though the energy density was 1.7 times higher than that of the foam-core ESMS. Furthermore, no defects or delamination were found in the battery embedded in the 3D-printed core ESMS, unlike the battery embedded in the foam-core ESMS where delamination between the separator, anode, and cathodes occurred after the 3 PB test. Consequently, a 3D-printed core ESMS with superior balanced multifunctional performance can be implemented without degradation of both the mechanical properties and energy storage characteristics.

在本研究中,设计了一种储能多功能夹层结构(ESMS),以实现良好的平衡和优异的多功能性能。波纹芯夹层结构是新开发的,即使在集成锂聚合物(LiPo)电池时也能防止机械性能的退化。将波纹芯的空隙用作储能空间,并使用连续碳纤维丝通过3D打印技术制造波纹芯。使用嵌入夹层结构的中性轴中的LiPo电池来实现能量存储特性。通过三点弯曲(3PB)试验分析了ESMS的静态和疲劳弯曲性能。在机械测试之前和之后进行电池充电/放电测试,以分析弯曲负载对储能性能的影响。由于电池嵌入,传统泡沫芯ESMS的弯曲性能如强度(在泡沫SH中为−27%)和模量(在泡沫AD中为−22%)出现了负面变化。另一方面,在3D打印芯ESMS的情况下,即使能量密度比泡沫芯ESMS高1.7倍,也没有观察到机械性能的退化。此外,与嵌入泡沫芯ESMS中的电池不同,嵌入3D打印芯ESMS的电池中没有发现缺陷或分层,在3 PB测试后,隔板、阳极和阴极之间发生分层。因此,可以在不降低机械性能和储能特性的情况下实现具有优异平衡多功能性能的3D打印芯ESMS。
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引用次数: 0
Microstructure and mechanical properties of extruded Mg-6Al-2X (X = Cu/Ni/Fe) alloy used degradable bridge plugs 可降解桥塞用挤压Mg-6Al-2X (X = Cu/Ni/Fe)合金的组织与力学性能
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-10-02 DOI: 10.1007/s42114-023-00753-x
Wentao Liu, Baosheng Liu, Shaohua Zhang, Zhiping Lin, Yuezhong Zhang, Pengpeng Wu, Hassan Algadi

Magnesium alloys have recently received much attention as fracturing tools for unconventional oil and gas development. It is well known that increasing micro-galvanic corrosion by doping elements in magnesium alloys is an effective method to get highly degradable alloys. The study aimed to evaluate the effect of different doping elements (i.e., copper, nickel and iron) on the mechanical and degradation behavior of hot extruded magnesium alloys. Nickel-containing alloys show high degradability and mechanical properties compared to the other two alloys. Specifically, the second phase of nickel-containing alloys has a dotted distribution, and this distribution favors the diffusion of corrosion. Meanwhile, the addition of nickel improves the mechanical properties of the alloy with a compressive strength of 430.6 MPa. In addition, based on the first principles and phase diagram simulations. With the addition of nickel, the compounds formed in the alloy act as drivers for the improved degradation properties, resulting in a corrosion rate of 1638.14 mm/year at 93 °C. Therefore, nickel-containing alloys that have been hot extruded show wide application prospects in the field of oil and gas extraction.

Graphical abstract

The influence of Cu/Ni/Fe elements on the microstructure, mechanical properties, and corrosion properties of Mg-6Al (wt. %) alloy was investigated using electrochemical tests, hydrogen evolution, and weight loss measurement.

镁合金作为非常规油气开发中的压裂工具,近年来备受关注。众所周知,在镁合金中掺杂元素增加微电偶腐蚀是获得高降解镁合金的有效方法。本研究旨在评价不同掺杂元素(即铜、镍和铁)对热挤压镁合金力学和降解行为的影响。与其他两种合金相比,含镍合金具有较高的可降解性和力学性能。含镍合金的第二相呈点状分布,有利于腐蚀的扩散。同时,镍的加入提高了合金的力学性能,抗压强度达到430.6 MPa。此外,基于第一性原理和相图进行了仿真。随着镍的加入,合金中形成的化合物成为改善降解性能的驱动因素,在93℃时腐蚀速率为1638.14 mm/年。因此,经热挤压处理的含镍合金在油气开采领域具有广阔的应用前景。摘要采用电化学试验、析氢试验和失重试验研究了Cu/Ni/Fe元素对Mg-6Al (wt. %)合金显微组织、力学性能和腐蚀性能的影响。
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引用次数: 0
Biosynthesizing lignin dehydrogenation polymer to fabricate hybrid hydrogel composite with hyaluronic acid for cartilage repair 生物合成木质素脱氢聚合物制备透明质酸混合水凝胶复合材料用于软骨修复
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-30 DOI: 10.1007/s42114-023-00758-6
Wenhui Pei, Yalikun Yusufu, Yifei Zhan, Xucai Wang, Jian Gan, Liming Zheng, Peng Wang, Kai Zhang, Caoxing Huang

Lignin possesses a number of functional groups including phenolic hydroxyl and methoxy groups, which grant its bioactivity for the fabrication of bio-polymer-based composites in bone tissue engineering applications. However, the heterogeneity of natural lignin limits its use in biomedicine. In the present study, a bio-enzyme approach was proposed to synthesize lignin-dehydrogenated polymers from the precursors of arabinogalactan (DHP-A) and xylose (DHP-X), which possess more homogeneous substructures with appropriate functional groups. Both DHP-A and DHP-X showed excellent in vitro abilities for regulating biocompatibility, “pre-oxidation,” and chondrogenic differentiation, in which DHP-A possessed cartilage repair ability due to its abundant content of phenolic hydroxyl groups (3.00 mmol g−1). Hence, DHP-A was hybridized with hyaluronic acid (HA) to prepare a hydrogel (DHP-HA) composite, which exhibited the compressive strength and modulus of 810 kPa and 310 kPa, respectively. Notably, these properties closely resemble those of articular cartilage, which typically ranges from 320 to 810 kPa. The application of DHP-HA hydrogel composite in a rat cartilage defect model in vivo revealed that it promoted the regeneration of hyaline cartilage rather than hypertrophic cartilage, which could heal 66.22–79.26% of the cartilage defects compared to the control group. Pre-oxidation of DHP-A elicits a mechanism that activates the oxidative stress system, leading to an augmented stress response and consequent increase in stress resistance. This study introduces a pioneering enzymatic synthesis technique to prepare the biologically active lignin for creating bio-polymer-based composites, demonstrating its potential as an innovative avenue for therapeutic cartilage regeneration.

Graphical Abstract

Bioenzymatically synthesized lignin dehydrogenation polymers to hybridize with hyaluronic acid to prepare hydrogel composites for promoting cartilage defect repair.

木质素具有许多官能团,包括酚羟基和甲氧基,这赋予了其在骨组织工程应用中制造生物聚合物基复合材料的生物活性。然而,天然木质素的异质性限制了其在生物医学中的应用。在本研究中,提出了一种由阿拉伯半乳聚糖(DHP-a)和木糖(DHP-X)的前体合成木质素脱氢聚合物的生物酶方法,这些前体具有更均匀的亚结构和合适的官能团。DHP-A和DHP-X在体外均表现出优异的调节生物相容性、“预氧化”和软骨分化的能力,其中DHP-A由于其丰富的酚羟基含量(3.00mmol g−1)而具有软骨修复能力。因此,将DHP-A与透明质酸(HA)杂交制备水凝胶(DHP-HA)复合材料,其抗压强度和模量分别为810kPa和310kPa。值得注意的是,这些特性与关节软骨的特性非常相似,通常在320至810kPa的范围内。DHP-HA水凝胶复合材料在大鼠体内软骨缺损模型中的应用表明,它促进了透明软骨而不是肥大软骨的再生,与对照组相比,肥大软骨可以治愈66.22-79.26%的软骨缺损。DHP-A的预氧化引发了一种激活氧化应激系统的机制,导致应激反应增强,从而增强应激抵抗力。本研究介绍了一种开创性的酶合成技术,用于制备生物活性木质素,用于制造基于生物聚合物的复合材料,展示了其作为治疗性软骨再生的创新途径的潜力。生物酶合成木质素脱氢聚合物与透明质酸杂交,制备促进软骨缺损修复的水凝胶复合材料。
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引用次数: 2
Double-phase engineering of cobalt sulfide/oxyhydroxide on metal-organic frameworks derived iron carbide-integrated porous carbon nanofibers for asymmetric supercapacitors 用于不对称超级电容器的金属-有机框架上硫化钴/氢氧根的双相工程衍生的碳化铁集成多孔碳纳米纤维
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-30 DOI: 10.1007/s42114-023-00755-9
Debendra Acharya, Tae Hoon Ko, Roshan Mangal Bhattarai, Alagan Muthurasu, Taewoo Kim, Syafiqah Saidin, Jae-Shik Choi, Kisan Chhetri, Hak Yong Kim

Designing advanced functional electrode materials with a tunable structure and multiphase/composition comprising a single metal via a one-step synthesis process for supercapacitor applications is challenging. Here, a dual-phase cobalt sulfide/cobalt oxyhydroxide (Co1-xS/HCoO2) hexagonal nanostructure on iron metal-organic framework (MIL-88A) derived iron carbide (Fe3C) integrated porous carbon nanofibers (PCNFs) is synthesized using a wet-chemical curing technique. MIL-88A is integrated by a physical blending process into a PAN/PMMA polymer matrix during the PCNFs preparation process. The integrated MIL-88A-derived iron carbide nanomaterial contributes to improving the electrochemical performance of electrode materials by lowering the inherent resistance. The optimal (Co1-xS/HCoO2)-1@Fe3C/PCNFs electrode exhibits a high specific capacitance of 1724 F g−1 at 1 A g−1 with an improved rate capability and exceptional cycling stability with 89.8% retention even after 10,000 cycles. These excellent electrochemical capabilities are predominantly attributed to the double-phase hybrid composites, which have a variety of abundant sites, a large active surface area, rapid electron and ion transport capability, and strong structural stability. A Co1-xS/HCoO2-1@Fe3C/PCNFs//Fe2O3/NPC@PCNFs asymmetric supercapacitor (ASC) demonstrates excellent electrochemical energy storage behavior, with a maximum energy density of 65.68 Wh kg−1 at a power density of 752.7 W kg−1 and excellent cycling stability (90.3% capacitance retention after 10,000 charge-discharge cycles at a constant current density of 20 A g−1). These electrochemical results indicate that this ASC outperforms previously reported asymmetric supercapacitors, showing that the heterophasic electrode (Co1-xS/HCoO2)-1@Fe3C/PCNFs has the potential to be applied in supercapacitor devices.

通过一步合成工艺设计具有可调结构和包括单一金属的多相/组成的先进功能电极材料用于超级电容器应用是具有挑战性的。本文采用湿法化学固化技术,在铁金属有机骨架(MIL-88A)衍生的碳化铁(Fe3C)集成多孔碳纳米纤维(PCNFs)上合成了一种双相硫化钴/羟基氧化钴(Co1-xS/HCoO2)六边形纳米结构。在PCNFs制备过程中,MIL-88A通过物理共混工艺集成到PAN/PMMA聚合物基体中。集成的MIL-88A衍生的碳化铁纳米材料通过降低固有电阻有助于提高电极材料的电化学性能。最佳(Co1-xS/HCoO2)-1@Fe3C/PCNFs电极在1 a g−1下表现出1724 F g−1的高比电容,具有改进的倍率能力和优异的循环稳定性,即使在10000次循环后仍保持89.8%的保留率。这些优异的电化学性能主要归功于双相杂化复合材料,它具有丰富的位点、大的活性表面积、快速的电子和离子传输能力以及强大的结构稳定性。Co1-xS/HCoO2-1@Fe3C/PCNFs//Fe2O3/NPC@PCNFs不对称超级电容器(ASC)表现出优异的电化学储能性能,在752.7 W kg−1的功率密度下,最大能量密度为65.68 Wh kg−1,循环稳定性优异(在20 a的恒定电流密度下,10000次充放电循环后,电容保持率为90.3% g−1)。这些电化学结果表明,这种ASC优于先前报道的不对称超级电容器,表明异相电极(Co1-xS/HCoO2)-1@Fe3C/PCNFs具有在超级电容器器件中应用的潜力。
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引用次数: 1
A “bird nest” bioinspired strategy deployed for inducing cellulose gelation without concomitant dissolution 一种“鸟巢”生物启发策略,用于诱导纤维素凝胶化而不伴随溶解
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-29 DOI: 10.1007/s42114-023-00745-x
Zhen Zhang, Noureddine Abidi, Lucian A. Lucia, Siyi Yu

Albeit the abundance, renewability, and biodegradability of the polymer known as cellulose, the insolubility and poor dispersibility in most common organic solvents make it incredibly difficult to facilitate conversion into hydrogels without concomitant dissolution. It is known that Swift family birds construct strong and sturdy nests with saliva that acts to bind fibers and twigs. Inspired by this charming hierarchical architecture, protonated carboxymethyl cellulose and cellulose were exploited as “saliva” and “twigs,” respectively, and by a combination of freeze–thaw treatments, cellulose hydrogels can be successfully induced without pre-dissolution representing a striking advancement over what is currently known or predicted. The gel materials displayed considerable increases in storage modulus, viscoelastic behaviors, and thermal stability as the cellulose content increases and exhibited unique omniphilic behaviors. Moreover, this bioinspired strategy is much more universal than originally surmised as found by the gelation of bamboo fibers (additionally containing lignin and hemicellulose), illustrative of the versatility. As a bio-inspired strategy, the current work is the first report on a straightforward, simple, green, yet effective gelation protocol to prepare cellulose-based soft materials.

尽管被称为纤维素的聚合物具有丰富性、可再生性和生物降解性,但在大多数常见的有机溶剂中的不溶性和较差的分散性使其难以在不伴随溶解的情况下促进转化为水凝胶。众所周知,雨燕科鸟类用唾液来连接纤维和树枝,从而建造坚固的巢穴。受这种迷人的分级结构的启发,质子化的羧甲基纤维素和纤维素分别被用作“唾液”和“树枝”,通过冷冻-解冻处理的组合,纤维素水凝胶可以在没有预溶解的情况下成功诱导,这比目前已知或预测的有了显著的进步。随着纤维素含量的增加,凝胶材料的储能模量、粘弹性行为和热稳定性显著提高,并表现出独特的全亲性行为。此外,这种受生物启发的策略比最初通过竹纤维(另外含有木质素和半纤维素)的凝胶化所推测的要普遍得多,这说明了它的多功能性。作为一种受生物启发的策略,目前的工作是第一份关于制备纤维素基软材料的直接、简单、绿色但有效的凝胶化方案的报告。
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引用次数: 0
Organic/inorganic hybrids for intelligent sensing and wearable clean energy applications 用于智能传感和可穿戴清洁能源应用的有机/无机混合材料
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-28 DOI: 10.1007/s42114-023-00751-z
Xiaotong Zhao, Yinxiao Du, Wei Li, Zebi Zhao, Ming Lei

With the rapid development of wearable electronics and the advent of the Internet of Things (IoT) era, it is imperative to research and explore the basic components to meet the application scenarios. In particular, it is becoming increasingly difficult to impart suitable properties to individual materials and realize appropriate physical dimensions in order to satisfy increasing demands of multifunctionality for fundamental studies, device designs, and performance optimization. Therefore, these challenges and opportunities can be addressed by designing (optical) electronic and energy devices with unique functionality and versatility through the combined advantages of multidimensional integration or hybridization of inorganic semiconductors, especially inorganic two-dimensional semiconductor materials, with various types of organic materials with potentially novel functions and unique properties. Herein, a comprehensive review of emerging integration or hybridization of inorganic semiconductor materials with organic materials from their individual components, and assembly fabrication to their state-of-the-art electronic, optoelectronic, magnetic, and energy applications is presented. Future opportunities and challenges associated with these organic/inorganic hybrids are highlighted.

随着可穿戴电子的快速发展和物联网时代的到来,研究和探索满足应用场景的基本组件势在必行。特别是,为了满足基础研究、器件设计和性能优化对多功能性的日益增长的需求,给单个材料赋予合适的性能并实现合适的物理尺寸变得越来越困难。因此,这些挑战和机遇可以通过设计具有独特功能和多功能性的(光学)电子和能源设备来解决,通过无机半导体,特别是无机二维半导体材料的多维集成或杂交的组合优势,具有各种类型的具有潜在新颖功能和独特性质的有机材料。本文对无机半导体材料与有机材料的新兴集成或杂交进行了全面综述,从其单个组件、组件制造到其最先进的电子、光电、磁性和能源应用。强调了与这些有机/无机杂化物相关的未来机遇和挑战。
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引用次数: 0
Ultralight, hierarchical metal–organic framework derivative/graphene hybrid aerogel for electromagnetic wave absorption 用于电磁波吸收的超轻、分层金属-有机框架衍生物/石墨烯混合气凝胶
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-28 DOI: 10.1007/s42114-023-00762-w
Jingpeng Lin, Jing Qiao, Haoyuan Tian, Lutong Li, Wei Liu, Lili Wu, Jiurong Liu, Zhihui Zeng

On the basis of high-efficiency electrostatic assembly, a type of ultralight, hydrophobic, hierarchically porous aerogels composed of metal–organic framework (MOF)-derived magnetic γ-Fe2O3@C/graphene are prepared via facile, scalable freeze-drying followed by annealing approach. The interaction between MOF and graphene oxide leads to the uniform dispersion of MOF-derived magnetic nanoparticles in the graphene-based cell walls, endowing the aerogels with high conductive and magnetic losses as well as polarization loss capacity derived from abundant heterogeneous interfaces. Both the core–shell microstructure of MOF derivative and the hierarchical pores of aerogels are instrumental in the multiple scattering of electromagnetic waves (EMWs), further promoting the EMW loss capability. Combined with the optimized impedance matching arising from the synergy between dielectric and magnetic components, an excellent EMW absorption performance of aerogel is achieved. At a filling ratio of merely 5 wt%, a minimum reflection loss of − 60.5 dB and a broad effective absorption bandwidth of 7.76 GHz covering the entire Ku-band are accomplished, significantly outperforming previously reported MOF- or graphene aerogel-based EMW absorbers. This work thus offers an efficient design strategy to prepare ultralight MOF-based aerogels for high-efficiency EMW absorbing materials in applications of electromagnetic compatibility and aerospace.

Graphical Abstract

在高效静电组装的基础上,一种由金属-有机框架(MOF)衍生的磁性γ组成的超轻、疏水、分级多孔气凝胶-Fe2O3@C/石墨烯是通过简单、可扩展的冷冻干燥和退火方法制备的。MOF和氧化石墨烯之间的相互作用导致MOF衍生的磁性纳米颗粒在石墨烯基细胞壁中均匀分散,赋予气凝胶高的导电和磁损耗以及源自丰富的异质界面的极化损耗能力。MOF衍生物的核壳微观结构和气凝胶的分级孔隙都有助于电磁波(EMW)的多次散射,进一步提高EMW的损失能力。结合电介质和磁性成分之间的协同作用产生的优化阻抗匹配,气凝胶获得了优异的EMW吸收性能。在仅5wt%的填充率下 − 60.5dB和覆盖整个Ku波段的7.76GHz的宽有效吸收带宽,显著优于先前报道的基于MOF或石墨烯气凝胶的EMW吸收剂。因此,这项工作为制备超轻MOF基气凝胶提供了一种有效的设计策略,用于电磁兼容性和航空航天应用中的高效EMW吸收材料。图形摘要
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引用次数: 2
Construction of interface-engineered coral-like nickel phosphide@cerium oxide hybrid nanoarrays to boost electrocatalytic hydrogen evolution performance in alkaline water/seawater electrolytes 界面工程珊瑚状镍的构建phosphide@cerium氧化物杂化纳米阵列在碱性水/海水电解质中提高电催化析氢性能
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-27 DOI: 10.1007/s42114-023-00750-0
Chaojie Lyu, Jiarun Cheng, Huichao Wang, Yuquan Yang, Kaili Wu, Peng Song, Woon-ming Lau, Jinlong Zheng, Xixi Zhu, Hui Ying Yang

Fabricating a functional heterogeneous interface to enhance catalytic performance is quite significant for developing high-efficiency electrocatalysts. Herein, a coral-like nickel phosphide@cerium oxide (Ni2P@CeO2) hybrid nanoarray on nickel foam was designed via selective-phosphorization of nickel hydroxide@cerium oxide (Ni(OH)2@CeO2). Benefiting from CeO2 as the “electron pump,” it leads to electron transfer from Ni2P to the CeO2 side, and induces electron redistribution in the interface boundary, thereby optimizing the H* adsorption free energy in the hydrogen evolution reaction (HER) process. As hypothesized, the water molecules will preferentially adsorb on the CeO2 side due to its better affinity for oxygen-containing species, and will readily break down into OH* and H* at a lower energy barrier. Subsequently, benefiting from the lower H* adsorption free energy of P sites, the generated H* will migrate to the Ni2P side through the spillover process. Contributing to the synergistic effect of double-active sites, the Ni2P@CeO2/NF electrode exhibits brilliant catalytic performance for HER with 62 mV to attain 10 mA/cm2 and exceptional durability over 100 h in alkaline solution at ~ 100 mA/cm2. Meanwhile, attributing to the similar interface electron redistribution effect, the precursor Ni(OH)2@CeO2/NF likewise displays excellent oxygen evolution reaction (OER) electrocatalytic performance, which only requires 229 mV to arrive at 10 mA/cm2, even better than benchmark ruthenium dioxide (RuO2). Hence, the assembled Ni(OH)2@CeO2/NF||Ni2P@CeO2/NF system only needs 1.53 V to achieve 10 mA/cm2 in alkaline solution. Moreover, the electrolyzer also presents brilliant electrocatalytic activity and stability in alkaline natural seawater electrolyte with higher reserves on earth.

Graphical Abstract

“Electrons pump” effect of CeO2 ensures that interface-engineered Ni2P@CeO2 hybrid nanoarrays prepared via selective-phosphorization treatment present superior HER catalytic performance

构建功能性非均相界面以提高催化性能对于开发高效电催化剂具有重要意义。这里,一个珊瑚状的镍phosphide@cerium氧化物(Ni2P@CeO2)通过对镍的选择性磷化,设计了泡沫镍上的混合纳米阵列hydroxide@cerium氧化物(Ni(OH)2@CeO2)。得益于CeO2作为“电子泵”,它导致电子从Ni2P转移到CeO2侧,并在界面边界诱导电子重新分布,从而优化析氢反应(HER)过程中的H*吸附自由能。正如假设的那样,由于水分子对含氧物质具有更好的亲和力,水分子将优先吸附在CeO2侧,并将在较低的能垒下容易分解为OH*和H*。随后,受益于P位点较低的H*吸附自由能,产生的H*将通过溢出过程迁移到Ni2P侧。有助于双活性位点的协同效应Ni2P@CeO2/NF电极对HER表现出出色的催化性能,62mV可达到10mA/cm2,在碱性溶液中100小时内具有优异的耐久性 ~ 同时,由于类似的界面电子再分配效应,前体Ni(OH)2@CeO2/NF同样表现出优异的析氧反应(OER)电催化性能,其仅需要229mV就可以达到10mA/cm2,甚至比基准二氧化钌(RuO2)更好。因此,组装的Ni(OH)2@CeO2/NF||Ni2P@CeO2/NF系统在碱性溶液中仅需1.53V即可达到10mA/cm2。此外,该电解槽在地球上储量较高的碱性天然海水电解质中也表现出优异的电催化活性和稳定性。图形摘要CeO2的“电子泵”效应确保界面工程Ni2P@CeO2选择性磷处理制备的杂化纳米阵列具有优异的HER催化性能
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引用次数: 0
Wood-based hierarchical porous nitrogen-doped carbon/manganese dioxide composite electrode materials for high-rate supercapacitor 高倍率超级电容器用木基分层多孔氮掺杂碳/二氧化锰复合电极材料
IF 20.1 2区 材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Pub Date : 2023-09-26 DOI: 10.1007/s42114-023-00744-y
Lin Shan, Yu Zhang, Ying Xu, Minjie Gao, Ting Xu, Chuanling Si

Supercapacitor is an important energy storage device with rapid charge/discharge, long cycle life, and high-power density. The macron vertical channel structure in wood can provide an effective buffer space for the transport and storage of electrolyte ions. The transport kinetics of the electrolyte with wood-derived carbon electrode has an important effect on its capacitance performance. Herein, the wood branch of cedar is employed to construct supercapacitor electrode with high-rate performance by facile carbonization and KOH activation. The cedar demonstrates arranged pore structure and high specific surface area. The special pore structure is retained after carbonization. Furthermore, the carbonization temperature and carbonization process are explored. As the optimized, the wood-derived porous carbon electrode displays high specific capacitance of 108 F/g at a higher current rate of 15 A/g, implying its good rate capability. Moreover, after compounding MnO2, the specific capacitance of composite electrode delivers 162.4 F/g at 0.5 A/g. The assembled symmetric supercapacitor shows high energy density of 3.01 Wh/kg at the power density of 250 W/kg. This work offers an idea for developing clean and efficient new energy technologies with high-rate performance.

超级电容器是一种重要的储能器件,具有充放电快、循环寿命长、高功率密度等特点。木材中的马克龙垂直通道结构可以为电解质离子的运输和储存提供有效的缓冲空间。木质碳电极电解质的迁移动力学对其电容性能有重要影响。本文利用雪松木树枝,通过简单的碳化和KOH活化,构建了具有高速率性能的超级电容器电极。雪松表现出排列有序的孔隙结构和高比表面积。碳化后保留了特殊的孔结构。并对炭化温度和炭化过程进行了探讨。作为优化的,木材衍生的多孔碳电极在15A/g的较高电流速率下显示出108F/g的高比电容,这意味着其良好的倍率能力。此外,在复合MnO2后,复合电极的比电容在0.5A/g下为162.4F/g。组装的对称超级电容器在250W/kg的功率密度下显示出3.01Wh/kg的高能量密度。这项工作为开发具有高速率性能的清洁高效新能源技术提供了思路。
{"title":"Wood-based hierarchical porous nitrogen-doped carbon/manganese dioxide composite electrode materials for high-rate supercapacitor","authors":"Lin Shan,&nbsp;Yu Zhang,&nbsp;Ying Xu,&nbsp;Minjie Gao,&nbsp;Ting Xu,&nbsp;Chuanling Si","doi":"10.1007/s42114-023-00744-y","DOIUrl":"10.1007/s42114-023-00744-y","url":null,"abstract":"<div><p>Supercapacitor is an important energy storage device with rapid charge/discharge, long cycle life, and high-power density. The macron vertical channel structure in wood can provide an effective buffer space for the transport and storage of electrolyte ions. The transport kinetics of the electrolyte with wood-derived carbon electrode has an important effect on its capacitance performance. Herein, the wood branch of cedar is employed to construct supercapacitor electrode with high-rate performance by facile carbonization and KOH activation. The cedar demonstrates arranged pore structure and high specific surface area. The special pore structure is retained after carbonization. Furthermore, the carbonization temperature and carbonization process are explored. As the optimized, the wood-derived porous carbon electrode displays high specific capacitance of 108 F/g at a higher current rate of 15 A/g, implying its good rate capability. Moreover, after compounding MnO<sub>2</sub>, the specific capacitance of composite electrode delivers 162.4 F/g at 0.5 A/g. The assembled symmetric supercapacitor shows high energy density of 3.01 Wh/kg at the power density of 250 W/kg. This work offers an idea for developing clean and efficient new energy technologies with high-rate performance. </p></div>","PeriodicalId":7220,"journal":{"name":"Advanced Composites and Hybrid Materials","volume":"6 5","pages":""},"PeriodicalIF":20.1,"publicationDate":"2023-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s42114-023-00744-y.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50049000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
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Advanced Composites and Hybrid Materials
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