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The hybrid Pt nanoclusters/Ru nanowires catalysts accelerating alkaline hydrogen evolution reaction 加速碱性氢气进化反应的铂纳米团簇/钌纳米线混合催化剂
Pub Date : 2024-06-12 DOI: 10.1016/j.apmate.2024.100214
Jingjing Yan , Rundong Wu , Guoqiang Jin , Litao Jia , Gang Feng , Xili Tong

Water electrolysis via alkaline hydrogen evolution reaction (HER) is a promising approach for large-scale production of high-purity hydrogen at a low cost, utilizing renewable and clean energy. However, the sluggish kinetics derived from the high energy barrier of water dissociation impedes seriously its practical application. Herein, a series of hybrid Pt nanoclusters/Ru nanowires (Pt/Ru NWs) catalysts are demonstrated to accelerate alkaline HER. And the optimized Pt/Ru NWs (10 ​% wt Pt) exhibits exceptional performance with an ultralow overpotential (24 ​mV at 10 ​mA ​cm−2), a small Tafel slope (26.3 ​mV dec−1), and long-term stability, outperforming the benchmark commercial Pt/C-JM-20 ​% wt catalyst. This amazing performance also occurred in the alkaline anion-exchange membrane water electrolysis devices, where it delivered a cell voltage of about 1.9 ​V at 1 ​A ​cm−2 and an outstanding stability (more than 100 ​h). The calculations have revealed such a superior performance exhibited by Pt/Ru NWs stems from the formed heterointerfaces, which significantly reduce the energy barrier of the decisive rate step of water dissociation via cooperative-action between Pt cluster and Ru substance. This work provides valuable perspectives for designing advanced materials toward alkaline HER and beyond.

通过碱性氢进化反应(HER)电解水是一种利用可再生清洁能源以低成本大规模生产高纯度氢气的可行方法。然而,水解离的高能障导致的缓慢动力学严重阻碍了其实际应用。本文展示了一系列铂纳米团簇/金纳米线(Pt/Ru NWs)混合催化剂,以加速碱性 HER。优化的 Pt/Ru NWs(10% wt Pt)表现出卓越的性能,具有超低的过电位(10 mA cm-2 时为 24 mV)、较小的塔菲尔斜率(26.3 mV dec-1)和长期稳定性,优于基准的商用 Pt/C-JM-20 % wt 催化剂。在碱性阴离子交换膜水电解装置中,这种催化剂也表现出了惊人的性能,在 1 A cm-2 的条件下,电池电压约为 1.9 V,而且稳定性极佳(超过 100 小时)。计算结果表明,铂/钌纳米线之所以能表现出如此优异的性能,是因为它形成了异质界面,通过铂簇和钌物质之间的协同作用,大大降低了水解离这一决定性速率步骤的能垒。这项工作为设计先进的碱性 HER 及其他材料提供了宝贵的前景。
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引用次数: 0
Recent developments in synthesis, properties, and applications of 2D Janus MoSSe and MoSexS(1-x) alloys 二维 Janus MoSSe 和 MoSexS(1-x)合金的合成、特性和应用的最新进展
Pub Date : 2024-05-23 DOI: 10.1016/j.apmate.2024.100204
Seetha Lakshmy , Brinti Mondal , Nandakumar Kalarikkal , Chandra Sekhar Rout , Brahmananda Chakraborty

The Janus MoSSe and alloy MoSxSe(1-x), belonging to the family of two-dimensional (2D) transition metal dichalcogenides (TMDs), have gained significant attention for their potential applications in nanotechnology. The unique asymmetric structure of Janus MoSSe provides intriguing possibilities for tailored applications. The alloy MoSxSe(1-x) offers a tunable composition, allowing for the fine-tuning of the properties to meet specific requirements. These materials exhibit remarkable mechanical, electrical, and optical properties, including a tunable band gap, high absorption coefficient, and photoconductivity. The vibrational and magnetic properties also make it a promising candidate for nanoscale sensing and magnetic storage applications. Properties of these materials can be precisely controlled through different approaches such as size-dependent properties, phase engineering, doping, alloying, defect and vacancy engineering, intercalation, morphology, and heterojunction or hybridisation. Various synthesis methods for 2D Janus MoSSe and alloy MoSxSe(1-x) are discussed, including hydro/solvothermal, chemical vapour transport, chemical vapour deposition, physical vapour depositio, and other approaches. The review also presents the latest advancements in Janus and alloy MoSSe-based applications, such as chemical and gas sensors, surface-enhanced Raman spectroscopy, field emission, and energy storage. Moreover, the review highlights the challenges and future directions in the research of these materials, including the need for improved synthesis methods, understanding of their stability, and exploration of new applications. Despite the early stages of research, both the MoSSe-based materials have shown significant potential in various fields, and this review provides valuable insights for researchers and engineers interested in exploring its potential.

Janus MoSSe 和合金 MoSxSe(1-x) 属于二维(2D)过渡金属二卤化物(TMDs)家族,因其在纳米技术中的潜在应用而备受关注。Janus MoSSe 独特的不对称结构为量身定制的应用提供了引人入胜的可能性。合金 MoSxSe(1-x) 具有可调成分,可对其性能进行微调以满足特定要求。这些材料具有卓越的机械、电气和光学特性,包括可调带隙、高吸收系数和光导率。振动和磁性使其成为纳米级传感和磁存储应用的理想候选材料。这些材料的特性可以通过不同的方法进行精确控制,如尺寸相关特性、相工程、掺杂、合金化、缺陷和空位工程、插层、形态学、异质结或杂化。文中讨论了二维 Janus MoSSe 和合金 MoSxSe(1-x) 的各种合成方法,包括水热法/溶热法、化学气相传输法、化学气相沉积法、物理气相沉积法和其他方法。综述还介绍了基于 Janus 和合金 MoSSe 的应用的最新进展,如化学和气体传感器、表面增强拉曼光谱、场发射和能量存储。此外,综述还强调了这些材料研究的挑战和未来方向,包括需要改进合成方法、了解其稳定性以及探索新的应用。尽管还处于早期研究阶段,但这两种基于 MoSSe 的材料已在各个领域显示出巨大的潜力,本综述为有兴趣探索其潜力的研究人员和工程师提供了宝贵的见解。
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引用次数: 0
Ultrahigh energy density in dielectric nanocomposites by modulating nanofiller orientation and polymer crystallization behavior 通过调节纳米填料取向和聚合物结晶行为实现介电纳米复合材料的超高能量密度
Pub Date : 2024-05-23 DOI: 10.1016/j.apmate.2024.100212
Ru Guo, Hang Luo, Di Zhai, Zhida Xiao, Haoran Xie, Yuan Liu, Fan Wang, Xun Jiang, Dou Zhang

High-energy density dielectrics for electrostatic capacitors are in urgent demand for advanced electronics and electrical power systems. Poly(vinylidene fluoride) (PVDF) based nanocomposites have attracted remarkable attention by intrinsic high polarization, flexibility, low density, and outstanding processability. However, it is still challenging to achieve significant improvement in energy density due to the common contradictions between electric polarization and breakdown strength. Here, we proposed a novel facile strategy that simultaneously achieves the construction of in-plane oriented BaTiO3 nanowires and crystallization modulation of PVDF matrix via an in-situ uniaxial stretch process. The polar phase transition and enhanced Young's modulus facilitate the synergetic improvement of electric polarization and voltage endurance capability for PVDF matrix. Additionally, the aligned distribution of nanowires could reduce the contact probability of nanowire tips, thus alleviating electric field concentration and hindering the conductive path. Finally, a record high energy density of 38.3 ​J/cm3 and 40.9 ​J/cm3 are achieved for single layer and optimized sandwich-structured nanocomposite, respectively. This work provides a unique structural design and universal method for dielectric nanocomposites with ultrahigh energy density, which presents a promising prospect of practical application for modern energy storage systems.

先进电子和电力系统急需用于静电电容器的高能量密度电介质。基于聚偏二氟乙烯(PVDF)的纳米复合材料因其固有的高极化性、柔韧性、低密度和出色的可加工性而备受关注。然而,由于电极化和击穿强度之间的常见矛盾,要实现能量密度的显著提高仍具有挑战性。在此,我们提出了一种新颖而简便的策略,通过原位单轴拉伸工艺同时实现了面内取向 BaTiO3 纳米线的构建和 PVDF 基体的结晶调制。极性相变和增强的杨氏模量促进了 PVDF 基体电极化和耐电压能力的协同改善。此外,纳米线的排列分布可以降低纳米线尖端的接触概率,从而减轻电场集中和阻碍导电路径。最后,单层和优化夹层结构纳米复合材料的能量密度分别达到了创纪录的 38.3 J/cm3 和 40.9 J/cm3。这项工作为具有超高能量密度的介电纳米复合材料提供了独特的结构设计和通用方法,为现代储能系统的实际应用带来了广阔前景。
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引用次数: 0
Theoretical design and experimental verification of high-entropy carbide ablative resistant coating 高熵碳化物耐烧蚀涂层的理论设计和实验验证
Pub Date : 2024-05-23 DOI: 10.1016/j.apmate.2024.100213
Lingxiang Guo, Shiwei Huang, Wei Li, Junshuai Lv, Jia Sun

Composition design of high-entropy carbides is a topic of great scientific interest for the hot-end parts in the aerospace field. A novel theoretical method through an inverse composition design route, i.e. initially ensuring the oxide scale with excellent anti-ablation stability, is proposed to improve the ablation resistance of the high-entropy carbide coatings. In this work, the (Hf0.36Zr0.24Ti0.1Sc0.1Y0.1La0.1)C1-δ (HEC) coatings were prepared by the inverse design concept and verified by the ablation resistance experiment. The linear ablation rate of the HEC coatings is −1.45 ​μm/s, only 4.78 % of the pristine HfC coatings after the oxyacetylene ablation at 4.18 ​MW/m2. The HEC possesses higher toughness with a higher Pugh's ratio of 1.55 in comparison with HfC (1.30). The in-situ formed dense (Hf0.36Zr0.24Ti0.1Sc0.1Y0.1La0.1)O2-δ oxide scale during ablation benefits to improve the anti-ablation performance attributed to its high structural adaptability with a lattice constant change not exceeding 0.19 % at 2000–2300 ​°C. The current investigation demonstrates the effectiveness of the inverse theoretical design, providing a novel optimization approach for ablation protection of high-entropy carbide coatings.

高熵碳化物的成分设计是航空航天领域热端部件的一个重要科学课题。为了提高高熵碳化物涂层的抗烧蚀性,我们提出了一种新的理论方法,即通过逆向成分设计途径,初步确保氧化鳞片具有优异的抗烧蚀稳定性。本研究采用反向设计理念制备了(Hf0.36Zr0.24Ti0.1Sc0.1Y0.1La0.1)C1-δ(HEC)涂层,并通过抗烧蚀实验进行了验证。在 4.18 MW/m2 氧乙炔烧蚀条件下,HEC 涂层的线性烧蚀率为-1.45 μm/s,仅为原始 HfC 涂层的 4.78%。与 HfC(1.30)相比,HEC 具有更高的韧性,普氏比为 1.55。在烧蚀过程中原位形成的致密(Hf0.36Zr0.24Ti0.1Sc0.1Y0.1La0.1)O2-δ氧化物鳞片有利于提高抗烧蚀性能,这归功于其结构适应性强,在 2000-2300 °C 时晶格常数变化不超过 0.19 %。目前的研究证明了反向理论设计的有效性,为高熵碳化物涂层的烧蚀保护提供了一种新的优化方法。
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引用次数: 0
Enhancing proton exchange membrane water electrolysis by building electron/proton pathways 通过建立电子/质子通路增强质子交换膜电解水能力
Pub Date : 2024-04-26 DOI: 10.1016/j.apmate.2024.100203
Liyan Zhu , Hao Zhang , Aojie Zhang , Tian Tian , Yuhan Shen , Mingjuan Wu , Neng Li , Haolin Tang

Proton exchange membrane water electrolysis (PEMWE) plays a critical role in practical hydrogen production. Except for the electrode activities, the widespread deployment of PEMWE is severely obstructed by the poor electron-proton permeability across the catalyst layer (CL) and the inefficient transport structure. In this work, the PEDOT:F (Poly(3,4-ethylenedioxythiophene):perfluorosulfonic acid) ionomers with mixed proton-electron conductor (MPEC) were fabricated, which allows for a homogeneous anodic CL structure and the construction of a highly efficient triple-phase interface. The PEDOT:F exhibits strong perfluorosulfonic acid (PFSA) side chain extensibility, enabling the formation of large hydrophilic ion clusters that form proton-electron transport channels within the CL networks, thus contributing to the surface reactant water adsorption. The PEMWE device employing membrane electrode assembly (MEA) prepared by PEDOT:F-2 demonstrates a competitive voltage of 1.713 ​V under a water-splitting current of 2 ​A ​cm−2 (1.746 ​V at 2A cm−2 for MEA prepared by Nafion D520), along with exceptional long-term stability. Meanwhile, the MEA prepared by PEDOT:F-2 also exhibits lower ohmic resistance, which is reduced by 23.4 ​% and 17.6 ​% at 0.1 ​A ​cm−2 and 1.5 ​A ​cm−2, respectively, as compared to the MEA prepared by D520. The augmentation can be ascribed to the superior proton and electron conductivity inherent in PEDOT:F, coupled with its remarkable structural stability. This characteristic enables expeditious mass transfer during electrolytic reactions, thereby enhancing the performance of PEMWE devices.

质子交换膜电解水(PEMWE)在实际制氢过程中发挥着至关重要的作用。除电极活性外,催化剂层(CL)上电子-质子渗透性差和传输结构效率低严重阻碍了质子交换膜水电解法的广泛应用。在这项工作中,制备了具有混合质子-电子导体(MPEC)的 PEDOT:F(聚(3,4-亚乙二氧基噻吩):全氟磺酸)离子体,从而实现了均匀的阳极 CL 结构,并构建了高效的三相界面。PEDOT:F 具有很强的全氟磺酸(PFSA)侧链延伸性,能够形成大型亲水离子簇,在 CL 网络中形成质子-电子传输通道,从而促进表面反应物质水的吸附。采用 PEDOT:F-2 制备的膜电极组件(MEA)的 PEMWE 器件在 2 A cm-2 的分水电流下显示出 1.713 V 的竞争电压(Nafion D520 制备的 MEA 在 2A cm-2 时为 1.746 V),并且具有优异的长期稳定性。同时,PEDOT:F-2 制备的 MEA 还表现出较低的欧姆电阻,与 D520 制备的 MEA 相比,在 0.1 A cm-2 和 1.5 A cm-2 条件下,欧姆电阻分别降低了 23.4% 和 17.6%。质子和电子传导性的增强可归因于 PEDOT:F 固有的优异质子和电子传导性及其显著的结构稳定性。这一特性可在电解反应过程中加快传质,从而提高 PEMWE 器件的性能。
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引用次数: 0
Bound-state electrons synergy over photochromic high-crystalline C3N5 nanosheets in enhancing charge separation for photocatalytic H2 production 光致变色高晶 C3N5 纳米片上的束缚态电子协同作用可提高光催化制取 H2 的电荷分离能力
Pub Date : 2024-04-16 DOI: 10.1016/j.apmate.2024.100202
Yu Shen , Xin Du , Yuxing Shi , Loic Jiresse Nguetsa Kuate , Zhouze Chen , Cheng Zhu , Lei Tan , Feng Guo , Shijie Li , Weilong Shi

Solar-driven water splitting for photocatalytic hydrogen evolution is considered a highly promising and cost-effective solution to achieve a stable renewable energy supply. However, the sluggish kinetics of electron-hole pairs’ separation poses challenges in attaining satisfactory hydrogen production efficiency. Herein, we synthesized the exceptional performance of highly crystalline C3N5 (HC–C3N5) nanosheet as a photocatalyst, demonstrating a remarkable hydrogen evolution rate of 3.01 ​mmol ​h−1 ​g−1, which surpasses that of bulk C3N5 (B–C3N5) by a factor of 3.27. Experimental and theoretical analyses reveal that HC-C3N5 nanosheets exhibit intriguing macroscopic photoinduced color changes, effectively broadening the absorption spectrum and significantly enhancing the generation of excitons. Besides, the cyano groups in HC-C3N5 efficiently captures and converts photoexcited electrons into bound states, thereby prolonging their lifetimes and effectively separating electrons and holes into catalytically active regions. This research provides valuable insights into the establishment of bound electronic states for developing efficient photocatalysts.

太阳能驱动的水分裂光催化氢进化被认为是一种极具前景和成本效益的解决方案,可实现稳定的可再生能源供应。然而,电子-空穴对分离的缓慢动力学对获得令人满意的制氢效率提出了挑战。在此,我们合成了性能优异的高结晶 C3N5(HC-C3N5)纳米片作为光催化剂,其氢气进化率高达 3.01 mmol h-1 g-1,是块状 C3N5(B-C3N5)的 3.27 倍。实验和理论分析表明,HC-C3N5 纳米片在光诱导下表现出有趣的宏观颜色变化,有效拓宽了吸收光谱,并显著增强了激子的产生。此外,HC-C3N5 中的氰基还能有效捕获光激发电子并将其转化为束缚态,从而延长其寿命,并有效地将电子和空穴分离到催化活性区域。这项研究为建立束缚电子态以开发高效光催化剂提供了宝贵的见解。
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引用次数: 0
Oxygen vacancy mediated bismuth-based photocatalysts 氧空位介导的铋基光催化剂
Pub Date : 2024-04-09 DOI: 10.1016/j.apmate.2024.100201
Jiaqi Tian , Jianpeng Li , Yadan Guo , Zhongyi Liu , Bin Liu , Jun Li

Sunlight-driven photocatalysis, which can produce clean fuels and mitigate environmental pollution, has received extensive research attention due to its potential for addressing both energy shortages and environmental crises. Bismuth (Bi)-based photocatalysts with broad spectrum solar-light absorption and tunable structures, exhibit promising applications in solar-driven photocatalysis. Oxygen vacancy (OV) engineering is a widely recognized strategy that shows great potential for accelerating charge separation and small molecule activation. Based on OV engineering, this review focuses on Bi-based photocatalysts and provides a comprehensive overview including synthetic methods, regulation strategies, and applications in photocatalytic field. The synthetic methods of Bi-based photocatalysts with OVs (BPOVs) are classified into hydrothermal, solvothermal, ultraviolet light reduction, calcination, chemical etching, and mechanical methods based on different reaction types, which provide the possibility for the structural regulation of BPOVs, including dimensional regulation, vacancy creation, elemental doping, and heterojunction fabrication. Furthermore, this review also highlights the photocatalytic applications of BPOVs, including CO2 reduction, N2 fixation, H2 generation, O2 evolution, pollutant degradation, cancer therapy, and bacteria inactivation. Finally, the conclusion and prospects toward the future development of BPOVs photocatalysts are presented.

太阳光驱动的光催化技术可以生产清洁燃料并减轻环境污染,因其在解决能源短缺和环境危机方面的潜力而受到广泛关注。基于铋(Bi)的光催化剂具有宽光谱太阳光吸收能力和可调结构,在太阳光驱动的光催化中具有广阔的应用前景。氧空位(OV)工程是一种广受认可的策略,在加速电荷分离和小分子活化方面具有巨大潜力。本综述以 OV 工程为基础,重点介绍 Bi 基光催化剂,并对其合成方法、调节策略以及在光催化领域的应用进行了全面概述。根据不同的反应类型,带 OV 的 Bi 基光催化剂(BPOVs)的合成方法分为水热法、溶热法、紫外光还原法、煅烧法、化学蚀刻法和机械法,这些方法为 BPOVs 的结构调控提供了可能,包括尺寸调控、空位产生、元素掺杂和异质结制造。此外,本综述还重点介绍了 BPOV 的光催化应用,包括 CO2 还原、N2 固定、H2 生成、O2 进化、污染物降解、癌症治疗和细菌灭活。最后,对 BPOVs 光催化剂的未来发展进行了总结和展望。
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引用次数: 0
Sepiolite: A new component suitable for 380 ​km/h high-speed rail brake pads 水帘石:适用于时速 380 公里高速铁路制动片的新成分
Pub Date : 2024-03-28 DOI: 10.1016/j.apmate.2024.100199
Jiaqi Wu, Zhuan Li, Guoyuan Wen, Zonglong Gao, Ye Li, Yang Li, Peng Xiao

To enhance the high-temperature adaptability of copper-based composite materials and C–C/SiC discs, this article innovatively introduces a method of replacing graphite with sepiolite, resulting in the successful fabrication of samples with exceptional mechanical and friction properties. The results reveal that moderate incorporation (less 6%) of sepiolite provides a particle reinforcement effect, resulting in an improvement of mechanical properties. Interestingly, the addition of sepiolite causes a change in the traditional saddle-shaped friction curve due to high temperature lubrication. Meanwhile, the primary advantage of sepiolite lies in its superior abrasion resistance, evident in the increased friction coefficient and altered wear mechanisms with higher sepiolite content. The wear resistance is optimal at 200 ​Km/h (400 ​°C). Particularly, the unique composition of the friction layer (outermost layer: a composite film consisting of B2O3, sepiolite, graphite, and metal oxide films; intermediate layer: metal oxide films) plays a pivotal role in improving friction stability. Finally, there are significant optimizations in the GA algorithm, especially GA-GB model has the best prediction effect on the maximum friction temperature.

为了提高铜基复合材料和 C-C/SiC 盘的高温适应性,本文创新性地介绍了一种用海泡石替代石墨的方法,从而成功制备出具有优异机械和摩擦性能的样品。研究结果表明,适度添加(少于 6%)的海泡石具有颗粒增强效果,从而改善了机械性能。有趣的是,由于高温润滑作用,海泡石的加入改变了传统的马鞍形摩擦曲线。同时,海泡石的主要优势在于其卓越的耐磨性,这体现在海泡石含量越高,摩擦系数越大,磨损机制越明显。耐磨性在 200 Km/h(400 °C)时达到最佳状态。特别是摩擦层的独特成分(最外层:由 B2O3、海泡石、石墨和金属氧化物薄膜组成的复合膜;中间层:金属氧化物薄膜)在提高摩擦稳定性方面发挥了关键作用。最后,对 GA 算法进行了重大优化,尤其是 GA-GB 模型对最高摩擦温度的预测效果最好。
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引用次数: 0
A powder-scale multiphysics framework for powder bed fusion of fiber-reinforced polymer composites 纤维增强聚合物复合材料粉末床融合的粉末尺度多物理场框架
Pub Date : 2024-03-27 DOI: 10.1016/j.apmate.2024.100190
Pengfei Tan , Meixin Zhou , Chao Tang , Kun Zhou

Additive manufacturing of fiber-reinforced polymer composites has garnered great interest due to its potential in fabricating functional products with lightweight characteristics and unique material properties. However, the major concern in polymer composites remains the presence of pore defects, as a thorough understanding of pore formation is insufficient. In this study, a powder-scale multiphysics framework has been developed to simulate the printing process of fiber-reinforced polymer composites in powder bed fusion additive manufacturing. This numerical framework involves various multiphysics phenomena such as particle flow dynamics of fiber-reinforced polymer composite powder, infrared laser–particle interaction, heat transfer, and multiphase fluid flow dynamics. The melt depths of one-layer glass fiber–reinforced polyamide 12 composite parts fabricated by selective laser sintering are measured to validate modelling predictions. The numerical framework is employed to conduct an in-depth investigation of pore formation mechanisms within printed composites. Our simulation results suggest that an increasing fiber weight fraction would lead to a lower densification rate, larger porosity, and lower pore sphericity in the composites.

纤维增强聚合物复合材料的快速成型技术在制造具有轻质特性和独特材料属性的功能性产品方面具有巨大潜力,因而备受关注。然而,由于对孔隙形成的理解不够透彻,聚合物复合材料中存在的主要问题仍然是孔隙缺陷。本研究开发了一个粉末尺度多物理场框架,用于模拟粉末床熔融增材制造中纤维增强聚合物复合材料的打印过程。该数值框架涉及多种多物理现象,如纤维增强聚合物复合材料粉末的粒子流动力学、红外激光与粒子相互作用、热传递和多相流体流动动力学。测量了通过选择性激光烧结制造的单层玻璃纤维增强聚酰胺 12 复合材料部件的熔深,以验证建模预测。利用数值框架对印刷复合材料中的孔隙形成机制进行了深入研究。我们的模拟结果表明,纤维重量分数的增加会导致复合材料的致密化率降低、孔隙率增大和孔隙球形度降低。
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引用次数: 0
Investigating the failure mechanism of solid electrolyte interphase in silicon particles from an electrochemical-mechanical coupling perspective 从电化学-机械耦合角度探究硅颗粒中固体电解质间相的失效机理
Pub Date : 2024-03-26 DOI: 10.1016/j.apmate.2024.100200
Junjie Ding , Xueyan Li , Lili Gong , Peng Tan

Silicon is considered one of the most promising anode materials owing to its high theoretical energy density, however, the volume expansion/contraction during electrochemical lithiation/delithiation cycles leads to instability of the solid electrolyte interphase (SEI), which ultimately results in capacity degradation. Herein, the local stress and deformation evolution status of an SEI layer on an anode particle are investigated through a quantitative electrochemical-mechanical model. The impacts of structural uniformity, mechanical strength, and operating conditions on the stability of the SEI layer are investigated in detail. The simulation results demonstrate that when the silicon particle radius decreases from 800 ​nm to 600 and 400 ​nm, the failure time increases by 29% and 65%, respectively, of the original failure time; When the structural defect depth ratio is reduced from 0.6 to 0.4 and 0.2, the failure time increases by 72% and 132%, respectively; For the discharge rate, the condition at 0.1 C has 34% and 139% longer time to failure than that at 0.2 C and 0.3 C, respectively. This work provides insight into the rational design of stable SEI layers and sheds light on possible methods for constructing silicon-based lithium-ion batteries with longer cycling lives.

硅因其理论能量密度高而被认为是最有前途的阳极材料之一,然而,在电化学锂化/退锂循环过程中,体积膨胀/收缩会导致固体电解质相间层(SEI)不稳定,最终导致容量下降。本文通过定量电化学-力学模型研究了阳极颗粒上 SEI 层的局部应力和变形演变状态。详细研究了结构均匀性、机械强度和工作条件对 SEI 层稳定性的影响。模拟结果表明,当硅颗粒半径从 800 nm 减小到 600 nm 和 400 nm 时,失效时间分别比原来增加了 29% 和 65%;当结构缺陷深度比从 0.6 减小到 0.4 和 0.2 时,失效时间分别增加了 72% 和 132%;在放电速率方面,0.1 C 条件下的失效时间分别比 0.2 C 和 0.3 C 条件下的失效时间延长了 34% 和 139%。这项研究为合理设计稳定的 SEI 层提供了启示,并为构建循环寿命更长的硅基锂离子电池提供了可能的方法。
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Advanced Powder Materials
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