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Simultaneous accelerated stress testing of membrane electrode assembly components in polymer electrolyte fuel cells 聚合物电解质燃料电池膜电极组件的同步加速应力测试
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-16 DOI: 10.1038/s41529-024-00524-z
Wataru Yoshimune, Akihiko Kato, Tetsuichiro Hayakawa, Satoshi Yamaguchi, Satoru Kato
The durability of polymer electrolyte fuel cells (PEFCs) in fuel cell electric vehicles is important for the shift from passenger cars to heavy-duty vehicles. The components of a PEFC, namely the proton exchange membrane (PEM), catalyst layer (CL), and gas diffusion layer (GDL), contribute to the degradation of the fuel cell performance. In this paper, we propose a method for simultaneously evaluating the degradation rates of these components by combining electrochemical characterization with operando synchrotron X-ray radiography. The open-circuit voltage, electrochemically active surface area (ECSA), and water saturation were used as the degradation indicators for the PEMs, CLs, and GDLs, respectively. The results of two accelerated stress tests (loading and start-stop cycles) after 10,000 cycles showed that the increase in water saturation owing to the loss of hydrophobicity due to carbon corrosion in the cathode GDL occurred on the same timescale as the degradation in the PEM and cathode CL. Specifically, during the load cycle AST, the cathode CL degraded with a 26% reduction in the ECSA along with the cathode GDL degradation with a 10% increase in water saturation. This suggests that more efforts should be devoted to studies on the durability of GDLs for heavy-duty applications.
燃料电池电动汽车中聚合物电解质燃料电池(PEFC)的耐用性对于从乘用车向重型车的转变非常重要。质子交换膜 (PEM)、催化剂层 (CL) 和气体扩散层 (GDL) 是 PEFC 的组成部分,它们都会导致燃料电池性能下降。在本文中,我们提出了一种通过将电化学表征与操作同步辐射 X 射线成像相结合来同时评估这些组件降解率的方法。开路电压、电化学活性表面积(ECSA)和水饱和度分别作为 PEM、CL 和 GDL 的降解指标。经过 10,000 次循环后进行的两次加速应力测试(加载和启停循环)结果表明,由于阴极 GDL 中的碳腐蚀导致疏水性丧失,水饱和度增加的时间与 PEM 和阴极 CL 的降解时间相同。具体来说,在负载循环 AST 期间,阴极 CL 降解,ECSA 降低 26%,同时阴极 GDL 降解,水饱和度增加 10%。这表明,应加大力度研究重型应用中 GDL 的耐用性。
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引用次数: 0
Hydrogen diffusion and trapping in a cryogenic processed high-Cr ferrous alloy 低温加工高铬铁合金中的氢扩散和捕获
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1038/s41529-024-00522-1
Patricia Jovičević-Klug, J. Manoj Prabhakar, Cristiano Kasdorf Giesbrecht, Tim M. Schwarz, Carsten Bonnekoh, Michael Rieth, Michael Rohwerder
The effect of hydrogen diffusion and trapping was studied in a high-Cr ferrous alloy using an inverted scanning Kelvin probe and thermal desorption spectroscopy in correlation with microstructure and residual stress study. In addition, different processing of ferritic/martensitic 9Cr1WTaV alloy (EUROFER97) was tested in correlation with observed selected properties to observe induced changes in material degradation and surface. The activation energies for hydrogen traps were shown to have distinct peaks corresponding to different trapping mechanisms, including matrix dislocations and grain boundaries. For the cryogenically treated sample, an additional peak was also identified and correlated with increased carbide precipitation.
使用倒置扫描开尔文探针和热解吸光谱法,结合微观结构和残余应力研究,对高铬铁合金中氢扩散和捕获的影响进行了研究。此外,还测试了铁素体/马氏体 9Cr1WTaV 合金(EUROFER97)的不同加工工艺与所观察到的选定特性之间的相关性,以观察材料降解和表面的诱导变化。结果表明,氢陷阱的活化能具有不同的峰值,与不同的陷阱机制相对应,包括基体位错和晶界。对于经过低温处理的样品,还发现了一个额外的峰值,并与碳化物析出的增加相关联。
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引用次数: 0
The microstructure-corrosion relationships in laser-welded dissimilar steel-to-aluminium joints 激光焊接异种钢铝接头的微观结构-腐蚀关系
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-11 DOI: 10.1038/s41529-024-00517-y
J. I. Ahuir-Torres, S. Jabar, P. Franciosa, D. Ceglarek, H. R. Kotadia
This study investigated the corrosion behaviour of dissimilar steel-to-aluminium laser-welded conduction, and keyhole mode (partial- and full-penetration) lap joints through electrochemical techniques and advanced microstructural characterisation. The corrosion resistance of the weld was found to be higher than the base materials, primarily due to the presence of cathodic FexAly (η-Fe2Al5, θ-Fe4Al13, β-FeAl) intermetallic compounds (IMCs) with high corrosion potential. The different micro and macro-galvanic corrosion mechanisms were found at various interfaces around the weld, resulting in localised pitting corrosion. The keyhole mode welding showed improved corrosion resistance, primarily attributed to the type, size, and distribution of IMCs.
本研究通过电化学技术和先进的微结构表征方法,研究了异种钢铝激光焊接传导接头和锁孔模式(部分穿透和完全穿透)搭接接头的腐蚀行为。研究发现,焊缝的耐腐蚀性高于母材,这主要是由于存在具有高腐蚀电位的阴极 FexAly(η-Fe2Al5、θ-Fe4Al13、β-FeAl)金属间化合物(IMC)。在焊缝周围的不同界面上发现了不同的微观和宏观电化学腐蚀机制,从而导致局部点蚀。锁孔模式焊接显示出更强的耐腐蚀性,这主要归因于 IMC 的类型、尺寸和分布。
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引用次数: 0
Nanoscale heterogeneities dictate corrosion pathways in a high-strength aluminum alloy 纳米级异质性决定了高强度铝合金的腐蚀途径
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-03 DOI: 10.1038/s41529-024-00520-3
S. Choudhary, R. G. Kelly
Micro-segregation and resulting nanoscale microstructural heterogeneities are unavoidable in wrought 7xxx aluminum alloys produced using current casting and thermomechanical processes. This study demonstrates that these nanoscale heterogeneities significantly impact pit growth in an extruded, age-hardened aluminum alloy 7075-T651. The alloy exhibits a complex microstructure with heterogeneously distributed E-Al18Mg3Cr2 dispersoids, which promote the precipitation of coarse ƞ-Mg(ZnAlCu)2 nanoparticles resulting in the formation of solute-depleted regions both within the grain interior and along the grain boundaries in dispersoid-rich areas. These alterations affect resistance to pit growth at the nanoscale, governing the transition of micro-galvanic sites into large pits with potential for crack initiation. This work underscores the necessity for modifying alloy composition and casting processes to develop superior aluminum alloys for critical applications.
在使用当前铸造和热机械工艺生产的锻造 7xxx 铝合金中,微偏析和由此产生的纳米级微结构异质性是不可避免的。本研究表明,这些纳米级异质性会严重影响挤压时效硬化铝合金 7075-T651 中凹坑的生长。该合金具有复杂的微观结构,其中 E-Al18Mg3Cr2 分散体分布不均,可促进粗ƞ-Mg(ZnAlCu)2 纳米颗粒的沉淀,从而在晶粒内部和分散体富集区的晶界上形成溶质贫化区。这些变化影响了纳米尺度的凹坑生长阻力,制约着微电镀点向大凹坑的过渡,并可能导致裂纹的产生。这项研究强调了改变合金成分和铸造工艺的必要性,以开发出适用于关键应用的优质铝合金。
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引用次数: 0
Inhibitor_Mol_VAE: a variational autoencoder approach for generating corrosion inhibitor molecules Inhibitor_Mol_VAE:生成缓蚀剂分子的变异自动编码器方法
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-10-01 DOI: 10.1038/s41529-024-00518-x
Haiyan Gong, Zhongheng Fu, Lingwei Ma, Dawei Zhang
Deep learning-based generative modeling demonstrates proven advantages as an effective approach in molecular discovery. This study introduces a generative-network based method called Inhibitor_Mol_VAE, which uses a variational autoencoder model to generate corrosion inhibitor molecules with targeted inhibition efficiency. We first evaluate the model’s ability to reconstruct molecules. Then, we assess the model’s ability to generate new inhibitor molecules using physiochemical properties (including MolWt, LogP, Vdw_volume, and Electronegativity). New molecules with high inhibition efficiencies at low concentrations, such as [ethoxy(methoxy)phosphoryl]-phenylmethanol and (alpha-methylamino-benzyl)-phosphonsaeure-monoaethylester are successfully discovered.
基于深度学习的生成模型作为一种有效的分子发现方法,其优势已得到证实。本研究介绍了一种基于生成网络的方法 Inhibitor_Mol_VAE,它使用变异自动编码器模型生成具有目标抑制效率的腐蚀抑制剂分子。我们首先评估了该模型重构分子的能力。然后,我们评估了该模型利用理化特性(包括 MolWt、LogP、Vdw_volume 和电负性)生成新缓蚀剂分子的能力。我们成功地发现了在低浓度下具有高抑制效率的新分子,如[乙氧基(甲氧基)磷酰]-苯基甲醇和(α-甲基氨基-苄基)-磷酰-单乙酯。
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引用次数: 0
The dual role of dissolution at a crack tip 裂纹尖端溶解的双重作用
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-30 DOI: 10.1038/s41529-024-00513-2
Mingjie Zhao, Wenjia Gu, Derek H. Warner
The scientific literature is rife with conflicting reports regarding the effect of dissolution on fracture. The complexity arises, in part, due to dissolution often being intertwined with various other mechanisms such as hydrogen embrittlement and the formation of debris behind an advancing crack, which can obfuscate the sole contribution of dissolution. Here, we report on the effect of dissolution when acting in isolation via the utilization of an efficient atomistic-based multiscale modeling technique and a specialized interatomic potential. Our results reveal a dual role of dissolution on crack behavior, introducing an additional layer of complexity to the mechanistic basis of environmental effects. This finding, while challenging for engineering prognosis, provides a route for engineering improved materials. Recognizing and navigating this duality could be pivotal to precluding potentially disastrous consequences in a broad array of engineering applications, from harnessing earth’s energy resources to aerospace technologies.
关于溶解对断裂的影响,科学文献中充斥着相互矛盾的报道。造成这种复杂性的部分原因是溶解通常与其他各种机制交织在一起,例如氢脆和在前进的裂纹后形成碎屑,这可能会掩盖溶解的唯一作用。在此,我们利用基于原子的高效多尺度建模技术和专门的原子间势能,报告了溶解在单独作用时的效果。我们的研究结果揭示了溶解对裂纹行为的双重作用,为环境效应的机理基础引入了另一层复杂性。这一发现虽然对工程预测具有挑战性,但却为改进材料的工程设计提供了一条途径。认识并驾驭这种双重性,对于在从利用地球能源到航空航天技术等广泛的工程应用中避免潜在的灾难性后果至关重要。
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引用次数: 0
Mechanistic elucidation of the molecular weight dependence of corrosion inhibition afforded by polyetherimide coatings 从机理上阐明聚醚酰亚胺涂层的缓蚀作用与分子量的关系
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-29 DOI: 10.1038/s41529-024-00516-z
Tiffany E. Sill, Victor Ponce, Carlos Larriuz, Ron Chertakovsky, Caroline G. Valdes, Torrick Fletcher Jr, Jakob Nielsen, Kerry Fuller, Homero Castaneda, Rachel D. Davidson, Peter M. Johnson, Sarbajit Banerjee
Corrosion of critical metal components exacts a heavy toll in terms of maintenance and replacement costs and damage to ecosystems upon failure. Polymeric barrier coatings protect against corrosion; however, design principles for modulating polymer structure to improve corrosion inhibition remain contested and elusive. Here, we examine molecular-weight-dependent differences in the efficacy of corrosion inhibition on aluminum substrates afforded by polyetherimide (PEI) coatings. Analyses of coated substrates evidence a clear trend denoting improved corrosion inhibition for higher weighted-average molecular weight (MW) PEI. The more rigid and entangled macromolecular network of higher-MW variants exhibit stable impedance values, |Z|0.01 Hz ca. 1010 Ω/cm2, upon extended immersion in brine media, whereas lower-MW variants are readily hydrated and disentangled resulting in a significant reduction in impedance values. Results illuminate mechanistic understanding of molecular-weight-dependence in corrosion inhibition, advance a framework for considering the dynamical evolution of secondary structure, and exemplify generalizable design principles for corrosion inhibition.
关键金属部件的腐蚀会造成重大损失,包括维护和更换成本,以及失效后对生态系统的破坏。聚合阻挡涂层可以防止腐蚀;然而,调节聚合物结构以改善缓蚀效果的设计原则仍然存在争议,难以捉摸。在此,我们研究了聚醚酰亚胺(PEI)涂层对铝基材的缓蚀效果随分子量而产生的差异。对涂层基材的分析表明,加权平均分子量(MW)较高的 PEI 具有明显的缓蚀效果。在盐水介质中长期浸泡后,高分子量变体的大分子网络更加坚硬和缠结,表现出稳定的阻抗值(|Z|0.01 Hz,约为 1010 Ω/cm2),而低分子量变体则很容易水化和分散,导致阻抗值显著降低。研究结果阐明了对缓蚀中分子量依赖性的机理理解,推进了考虑二级结构动态演变的框架,并体现了可推广的缓蚀设计原则。
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引用次数: 0
Repairment of carbon steel oxide scale using Ce³⁺ and Ni²⁺ doped sol-gel technique 利用掺杂 Ce³⁺ 和 Ni²⁺ 的溶胶-凝胶技术修复碳钢氧化鳞片
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-18 DOI: 10.1038/s41529-024-00515-0
Yanwei Zeng, Peng Xu, Tianguan Wang, Yuhao Xie, Guoqiang Liu, Huixuan Qian, Zhiyuan Feng, Bing Lei, Ping Zhang, Guozhe Meng
Corrosion of carbon steel rebars in concrete structures significantly compromises their safety, reliability, and environmental performance. This work focuses on enhancing rebar corrosion resistance by repairing the defects of oxide scale. Here, sol-gel was employed as a carrier, by which Ce3+ and Ni2+ were transferred to the oxide scale defects based on the isoelectric point theory, and deposited at these defects with the pH variation as temperature. The repaired oxide scale showed enhanced uniform elemental distribution and improved electrochemical properties, maintaining integrity even under prolonged exposure to Cl−-rich environments. Notably, the impedance modulus at 0.01 Hz (|Z | 0.01Hz) of treated samples was six times higher than untreated ones, indicating superior performance against high electric fields. This strategy shows great potential for enhancing the durability of concrete structures.
混凝土结构中碳钢钢筋的锈蚀严重影响了其安全性、可靠性和环保性能。这项研究的重点是通过修复氧化鳞片缺陷来增强钢筋的耐腐蚀性。研究采用溶胶凝胶作为载体,根据等电点理论将 Ce3+ 和 Ni2+ 转移到氧化鳞片缺陷处,并随着 pH 值和温度的变化沉积在这些缺陷处。修复后的氧化鳞片显示出更均匀的元素分布和更好的电化学性能,即使长期暴露在富含 Cl 的环境中也能保持完整性。值得注意的是,经过处理的样品在 0.01 Hz 时的阻抗模量(|Z | 0.01Hz)比未经处理的样品高出六倍,这表明其在高电场下具有卓越的性能。这种策略在提高混凝土结构的耐久性方面显示出巨大的潜力。
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引用次数: 0
Dependency of tensile properties and biodegradation on molecular mass during hydrolysis of poly(butylene succinate) 聚丁二酸丁二醇酯水解过程中拉伸性能和生物降解与分子质量的关系
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-17 DOI: 10.1038/s41529-024-00512-3
Felix Eckel, Daniel Van Opdenbosch, Katharina Sophie Schandl, Cordt Zollfrank
The molecular mass of biodegradable polymers often explains the varying biodegradation results in outdoor environments and determines the mechanical properties and embrittlement of polymer samples. Accordingly, we have investigated the relationship between the molecular mass of poly(butylene succinate) (PBS) and its tensile properties and mineralisation. With decreasing molecular mass, we found that Young’s modulus was rising while tensile strength and elongation at break were decreasing. A ductile-brittle transition was found between a Mw of 80,000 g/mol and 110,000 g/mol. The dependency of mechanical properties on molecular mass as determined after hydrolysis differed significantly from a study performed on freshly synthesised PBS. Biodegradation to CO2 by microorganisms in a mixture of field soil and compost soil was found to begin at a Mw between 8060 g/mol and 26,666 g/mol. These results are essential for estimating the service life of products made from PBS.
可生物降解聚合物的分子质量通常可以解释室外环境中不同的生物降解结果,并决定聚合物样品的机械性能和脆性。因此,我们研究了聚(丁二酸丁二醇酯)(PBS)的分子质量与其拉伸性能和矿化之间的关系。我们发现,随着分子质量的降低,杨氏模量在上升,而拉伸强度和断裂伸长率在下降。在 Mw 为 80,000 g/mol 到 110,000 g/mol 之间发现了韧性-脆性转变。水解后测定的机械性能与分子质量的关系与对新鲜合成的 PBS 进行的研究有很大不同。在田间土壤和堆肥土壤的混合物中,微生物对二氧化碳的生物降解始于 8060 克/摩尔和 26666 克/摩尔之间的分子质量。这些结果对于估算用 PBS 制成的产品的使用寿命至关重要。
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引用次数: 0
Dynamic assessment of titanium surface oxides following mechanical damage reveals only partial passivation under inflammatory conditions 机械损伤后钛表面氧化物的动态评估显示,在炎症条件下只有部分钝化
IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-09-17 DOI: 10.1038/s41529-024-00514-1
Georgios A. Kotsakis, Li Xie, Danyal A. Siddiqui, Diane Daubert, Daniel J. Graham, Francisco Javier Gil
Motivated by clinical problems of titanium implant degradation, we developed a workflow that enabled assessment of surface oxide dynamics as a function of clinical interventions and inflammation conditions. We found that mechanical damage led to decrease of stoichiometric TiO2 ratio in the passivation oxide film and further resulted in accelerated degradation under inflammatory anaerobic conditions. This method can be employed for the assessment of surface oxides to monitor implant safety.
受钛植入物降解的临床问题的启发,我们开发了一套工作流程,可以评估表面氧化物动态与临床干预和炎症条件的关系。我们发现,机械损伤会导致钝化氧化膜中 TiO2 的化学计量比下降,并进一步导致炎症厌氧条件下的加速降解。这种方法可用于评估表面氧化物,以监测植入物的安全性。
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引用次数: 0
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npj Materials Degradation
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