Acta MaterialiaPub Date : 2025-05-26DOI: 10.1016/j.actamat.2025.121180
Su-Jin Ha , Young Kook Moon , Hyun-Ae Cha , Jong-Jin Choi , Byung-Dong Hahn , Seong-Hui Choi , Il-Ryeol Yoo , Kyung-Hoon Cho , Kyoung-Seok Moon , Cheol-Woo Ahn
{"title":"Fundamental study to grow single crystals with high performances operated up to high temperatures in donor-doped materials for energy harvesting","authors":"Su-Jin Ha , Young Kook Moon , Hyun-Ae Cha , Jong-Jin Choi , Byung-Dong Hahn , Seong-Hui Choi , Il-Ryeol Yoo , Kyung-Hoon Cho , Kyoung-Seok Moon , Cheol-Woo Ahn","doi":"10.1016/j.actamat.2025.121180","DOIUrl":"10.1016/j.actamat.2025.121180","url":null,"abstract":"<div><div>An energy-harvesting material with high energy-conversion constant (d<sub>33</sub> × g<sub>33</sub>) and Curie temperature (T<sub>C</sub>) is required to effectively harvest the mechanical energy which has not been recycled into electrical energy. Here, we present an eco-friendly single-crystals, the 3rd generation material, for energy harvesting with the excellent d<sub>33</sub> × g<sub>33</sub> of 118 10<sup>–12</sup> m<sup>2</sup>N<sup>-1</sup> (d<sub>33</sub>=1030 pCN<sup>-1</sup>) and high T<sub>C</sub> of 390 °C, prepared by simple heat-treatment. A donor (not an acceptor) has been doped to (K,Na)NbO<sub>3</sub> (KNN)-based materials to obtain single-crystals through exceptionally abnormal grain growth (AGG). The severe AGG in a donor-doped KNN is explained by the donor effect to locally accelerate the volatilization of metals earlier. In particular, a donor-doped PbTiO<sub>3</sub> (PT + Bi<sup>3+</sup>) material as well as a donor-doped KNN material allows for the synthesis of a single-crystal seed through the simple molten salt method. These findings advance understanding of sintering mechanisms in metal-volatile oxides and offer significant progress in energy-harvesting materials.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"295 ","pages":"Article 121180"},"PeriodicalIF":8.3,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-24DOI: 10.1016/j.actamat.2025.121155
Robert Löser, Yug Joshi, Roham Talei, Petra Ebbinghaus, Guido Schmitz
{"title":"Electro-chemo-mechanical behavior of a layered cathode material upon cycling","authors":"Robert Löser, Yug Joshi, Roham Talei, Petra Ebbinghaus, Guido Schmitz","doi":"10.1016/j.actamat.2025.121155","DOIUrl":"https://doi.org/10.1016/j.actamat.2025.121155","url":null,"abstract":"The mechanical characteristics of lithium-ion cathode materials plays a critical role in determining battery performance such as durability, cycle life, and safety, especially when the battery is under external pressure which is typical for all-solid-state batteries. This study focuses on LiCoO<sub>2</sub> (LCO), a widely used hexagonal layer-structured cathode material for lithium-ion batteries, and investigates its mechanical properties during de-/lithiation using sputter-deposited thin films and nanoindentation. The values of the experimental Young’s modulus in pure (101) and (003) lattice orientations are quantified to 337.1 <span><math><mo is=\"true\">±</mo></math></span> 8.7 GPa and 267.9 <span><math><mo is=\"true\">±</mo></math></span> 7.2 GPa, respectively, in the fully lithiated state. Furthermore, a substantial texture-dependent decrease in Young’s modulus upon lithium deintercalation is demonstrated, probably due to modification of the bonding interactions between the cobalt oxide layers. The decrease of Li content also elevates the relative contribution of plastic deformation, indicating that dislocation glide becomes easier in deintercalated states. By extensive cycling, the Young’s modulus in higher lithiated charge-states decreases considerably which is most-likely due to irreversibility of phase transitions. In contrast, the material shows a significant increase of plastic hardness with cycling, understood as work hardening. The work provides valuable insight on the dynamic changes of the mechanical properties during electrochemical cycling of LiCoO<sub>2</sub>, which paves the way for all other layered cathode materials.","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"56 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133650","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-24DOI: 10.1016/j.actamat.2025.121174
Barak Ratzker , Martina Ruffino , Shiv Shankar , Dierk Raabe , Yan Ma
{"title":"Elucidating the microstructure evolution during hydrogen-based direct reduction via a case study of single crystal hematite","authors":"Barak Ratzker , Martina Ruffino , Shiv Shankar , Dierk Raabe , Yan Ma","doi":"10.1016/j.actamat.2025.121174","DOIUrl":"10.1016/j.actamat.2025.121174","url":null,"abstract":"<div><div>Sustainable hydrogen-based direct reduction (HyDR) of iron oxide is an effective approach to reduce carbon emissions in steel production. As the reduction behaviour is closely related to the microstructure evolution, it is important to understand the microscopic reduction mechanisms. Industrial hematite pellets are microstructurally intricate systems with inherent porosity, defects, and impurities. Therefore, in the present study we investigated the HyDR of single crystal hematite (at 700 °C) to elucidate the reduction behaviour and microstructure evolution in a model system. The reduction kinetics of the single crystal (SC) were compared to those of industrial polycrystalline porous pellets using thermogravimetric analysis. Additional SC samples were prepared such that their faces are parallel to the (0001), (<span><math><mrow><mn>10</mn><mover><mn>1</mn><mo>¯</mo></mover><mn>0</mn></mrow></math></span>) and (<span><math><mrow><mn>1</mn><mover><mn>2</mn><mo>¯</mo></mover><mn>10</mn></mrow></math></span>) crystallographic planes of hematite, and then partially reduced to 16 and 80 % reduction degree. Their microstructure was thoroughly examined by scanning electron microscopy and electron backscatter diffraction (EBSD). Reaction fronts were thus shown to advance into the hematite by a shrinking core model while creating a percolating pore network in the magnetite layer; this was closely followed by wüstite and iron formation, as well as pore coarsening, with the retained oxides proceeding to reduce homogenously throughout the sample abiding by the pore/grain models. Notably, a “cell-like” morphology develops in the magnetite near the hematite/magnetite interface, with finely porous “cell interiors” surrounded by coarsely porous “cell walls”. Furthermore, the hierarchal pore formation, phase transformations, texture, and orientation relationships are considered.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"294 ","pages":"Article 121174"},"PeriodicalIF":8.3,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144130389","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Functionally graded NiTiHf high-temperature shape memory alloys using laser powder bed fusion: localized phase transformation control and multi-stage actuation","authors":"Abdelrahman Elsayed , Taresh Guleria , Haoyi Tian , Bibhu P. Sahu , Kadri C. Atli , Alaa Olleak , Alaa Elwany , Raymundo Arroyave , Dimitris Lagoudas , Ibrahim Karaman","doi":"10.1016/j.actamat.2025.121175","DOIUrl":"10.1016/j.actamat.2025.121175","url":null,"abstract":"<div><div>This study presents the successful additive manufacturing of functionally graded (FG) NiTiHf high-temperature shape memory alloys using Laser Powder Bed Fusion. A novel approach was implemented to achieve precise voxel-level control of local chemistry and microstructure starting from a single feedstock composition, enabling location-specific phase transformation characteristics. By systematically analyzing the relationships between volumetric energy density, Ni evaporation, and transformation temperatures, the study achieved accurate control of Ni content across different segments of the functionally graded materials (FGMs). Thermal modeling further elucidated the influence of thermal history change, due to changes in the process parameters and sample size, on Ni evaporation and oxide formation, findings that were experimentally validated by local transmission electron microscopy analyses. Wavelength dispersive spectroscopy confirmed the localized control of Ni content, while differential scanning calorimetry identified multiple transformation peaks in the FG NiTiHf samples, indicating multi-stage transformation behavior throughout the FG segments. The transformation range spanned over 150 °C, demonstrating the capability to engineer tailored thermomechanical responses across different regions within the printed components. A novel thermomechanical modeling approach effectively predicted the global actuation response of the FG parts, and mechanical testing demonstrated broader transformation ranges and high strain recovery in the samples. These results highlight the potential of FG HTSMAs for applications requiring tailored actuation and reliable performance across varying high-temperature ranges, offering a viable path forward for enhancing their high-temperature functionality.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"296 ","pages":"Article 121175"},"PeriodicalIF":8.3,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-23DOI: 10.1016/j.actamat.2025.121172
Kaichao Zhang , Chao Lv , Guanqi Li , Zeyi Li , Xueyi Huo , Zhuangweici Sun , Zhengrui Li , Changshuo Zhang , Jiaxing Zheng , Kai Wang , Yulin Chen , Xinqing Zhao , Huilong Hou
{"title":"Introducing strain glass transition into high-entropy TiZrHfNiCuCo alloys exhibiting elastocaloric effect and quasi-linear superelasticity","authors":"Kaichao Zhang , Chao Lv , Guanqi Li , Zeyi Li , Xueyi Huo , Zhuangweici Sun , Zhengrui Li , Changshuo Zhang , Jiaxing Zheng , Kai Wang , Yulin Chen , Xinqing Zhao , Huilong Hou","doi":"10.1016/j.actamat.2025.121172","DOIUrl":"10.1016/j.actamat.2025.121172","url":null,"abstract":"<div><div>High entropy alloys (HEAs) have garnered significant attention due to their vast compositional space and tremendous potential for advanced structural and functional properties. While most studies on HEAs concentrate on optimizing one or two primary characteristics, there exists a transformative opportunity in designing HEAs that integrate multiple structural and functional attributes. In this work, we present equiatomic TiZrHfNiCuCo HEAs that exhibit a remarkable combination of mechanical and functional properties, including high strength, low elastic modulus, quasi-linear superelasticity, broad-temperature-range elastocaloric effect with a high coefficient of performance (<span><math><mrow><mi>C</mi><mi>O</mi><msub><mi>P</mi><mtext>material</mtext></msub></mrow></math></span>) spanning from 223 K to 423 K, elastic modulus softening, and exceptional fatigue stability exceeding 10<sup>5</sup> cycles. Through detailed nanoscale microstructural analysis, we demonstrate that these properties are linked to the strain glass transition in the HEAs, characterized by frequency-dependent modulus behavior, invariance of average structure, non-ergodicity, and the formation and growth of nanodomains. The high <span><math><mrow><mi>C</mi><mi>O</mi><msub><mi>P</mi><mtext>material</mtext></msub></mrow></math></span> elastocaloric effect, and long-term fatigue stability can be attributed to the quasi-linear superelasticity with narrow hysteresis that originates from the stress-induced continuous evolution of nanodomains. The elastic modulus softening arises from the combined contributions of the elastic modulus softening of the B2 matrix and the elastic modulus hardening of B19′ and R nanodomains, as well as other precipitates. Our work sheds light on the strategy to introduce strain glass transition into advanced HEAs for designing structural and functional properties.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"294 ","pages":"Article 121172"},"PeriodicalIF":8.3,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144122474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-23DOI: 10.1016/j.actamat.2025.121168
D. Wang , G. Zeng , J.W. Xian , K. Nogita , H. Yasuda , C.M. Gourlay
{"title":"Growth crystallography and in-situ imaging of nucleation and growth dynamics of Al8Mn5 solidifying in AZ magnesium alloys","authors":"D. Wang , G. Zeng , J.W. Xian , K. Nogita , H. Yasuda , C.M. Gourlay","doi":"10.1016/j.actamat.2025.121168","DOIUrl":"10.1016/j.actamat.2025.121168","url":null,"abstract":"<div><div>Many magnesium-aluminium-based alloys contain a small manganese addition to improve corrosion resistance. However, this introduces Al-Mn intermetallics which add complexity to the phase transformations. Here we study the crystal growth of the most common Al-Mn phase, Al<sub>8</sub>Mn<sub>5</sub>, in Mg-Al-Zn-Mn-based magnesium alloy solidification by combining electron microscopy of the faceted growth crystallography with in-situ synchrotron X-ray imaging of the Al<sub>8</sub>Mn<sub>5</sub> nucleation and growth dynamics. Three Al<sub>8</sub>Mn<sub>5</sub> morphologies, equiaxed, rod and plate, are shown to all come from cyclic twinned growth associated with the pseudo-cubic symmetry of rhombohedral Al<sub>8</sub>Mn<sub>5</sub>. X-ray imaging revealed Al<sub>8</sub>Mn<sub>5</sub> nucleated throughout the freezing range and grew with α-Mg dendrites over a wide temperature range by divorced eutectic solidification. This occurs because, in these alloys, Mn solute has little influence on the solute undercooling of growing α-Mg dendrites, although strongly affects the constitutional supercooling with respect to the Al<sub>8</sub>Mn<sub>5</sub> liquidus. Rod/plate growth of Al<sub>8</sub>Mn<sub>5</sub> is shown to be promoted by slow cooling rates and by divorced eutectic solidification. The findings provide new insights into the conditions that cause large, deleterious rods and plates, and explain why there is a large variation in Al<sub>8</sub>Mn<sub>5</sub> growth morphology after solidification.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"296 ","pages":"Article 121168"},"PeriodicalIF":8.3,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144130447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-23DOI: 10.1016/j.actamat.2025.121164
Meng Liu, Qianning Guo, Jingwei Zhao, Zhenshan Liu, Kaixin Chen, Yiheng Cao, Ting Chen, Feng Qian, Shiwei Pan, Xingzhong Cao, Huan Zhao, Gang Sha, Zi Yang, John Banhart, Pizhi Zhao
{"title":"Modulated clustering and precipitation in an Al–Mg–Si alloy AA 6014 via enhanced pre-aging","authors":"Meng Liu, Qianning Guo, Jingwei Zhao, Zhenshan Liu, Kaixin Chen, Yiheng Cao, Ting Chen, Feng Qian, Shiwei Pan, Xingzhong Cao, Huan Zhao, Gang Sha, Zi Yang, John Banhart, Pizhi Zhao","doi":"10.1016/j.actamat.2025.121164","DOIUrl":"https://doi.org/10.1016/j.actamat.2025.121164","url":null,"abstract":"The effect of an additional short spike aging treatment (SA: 180 to 220°C, in tens of seconds) between solution heat treatment and conventional pre-aging (PA: 85°C, in hours) on the mechanical properties of an AA 6014 alloy after paint baking was evaluated. Tensile tests show that such enhanced pre-aging including SA and PA can significantly improve the paint bake response compared to conventional pre-aging (PA only). To interpret this phenomenon, Positron Annihilation Lifetime Spectroscopy, Electrical Resistivity Measurements, Differential Scanning Calorimetry, Transmission Electron Microscopy, Atom Probe Tomography and MatCalc calculations were applied to identify the microstructural changes in different aging stages. It is found that the excess vacancies available after quenching assist in rapid nucleation of clusters during SA, which grow during subsequent PA and transform easily to β\" precipitates during paint baking owing to their similar chemistry. The densely distributed β\" precipitates are considered responsible for the improved paint bake strength as thy efficiently hinder dislocation movement.","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"26 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144133737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-22DOI: 10.1016/j.actamat.2025.121161
Weiren Wang , Xue Jiang , Wenyao Li , Chi Zhang , Pei Liu , Shaohan Tian , Turab Lookman , Yanjing Su
{"title":"Design of superalloys with multiple properties via multi-task learning","authors":"Weiren Wang , Xue Jiang , Wenyao Li , Chi Zhang , Pei Liu , Shaohan Tian , Turab Lookman , Yanjing Su","doi":"10.1016/j.actamat.2025.121161","DOIUrl":"10.1016/j.actamat.2025.121161","url":null,"abstract":"<div><div>The development of new materials requires the collaborative design of multiple properties, requiring an analysis of the interactions amongst material composition, processing methods, and individual properties. Traditional data-driven materials design approaches typically rely on single-task models that operate independently, often neglecting the shared insights across related tasks. To overcome this limitation, we propose a collaborative design framework that employs multi-task learning for the development of novel Co-based superalloys. In this framework, six thermodynamic and microstructural property tasks share a common encoder, which effectively captures the underlying influence of alloy compositions across different properties. Each task then utilizes its own dedicated decoder to ensure precise predictions. As a result, the average normalized error for the predictions of the six properties is reduced by 37.5 % compared to conventional single-task learning methods. Furthermore, latent high-dimensional variables are extracted from the common encoder, and utilized to identify promising exploration directions for optimal properties, as indicated by the projection of these variables, which aids in screening new alloys. We successfully designed new alloys that satisfy the targeted criteria: low density (<9 g cm<sup>-3</sup>), suitable freezing ranges (<60 °C) and processing windows (>80 °C), optimal γ′ sizes (<550 nm after aging at 1100 °C for 168 h and <200 nm after aging at 1000 °C for 24 h), high γ′ solvus temperature (>1200 °C) without detrimental phases, and strong oxidation resistance. This framework represents a promising approach for collaborative materials design, leveraging shared information to enhance the development of multiple properties.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"294 ","pages":"Article 121161"},"PeriodicalIF":8.3,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113792","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-22DOI: 10.1016/j.actamat.2025.121169
Malik Wagih , Tianjiao Lei , Daniel Ng , Christopher A. Schuh
{"title":"Grain boundary segregation in BCC vanadium-based alloys: Quantum-accurate computed segregation spectra and targeted experimental validations","authors":"Malik Wagih , Tianjiao Lei , Daniel Ng , Christopher A. Schuh","doi":"10.1016/j.actamat.2025.121169","DOIUrl":"10.1016/j.actamat.2025.121169","url":null,"abstract":"<div><div>Grain boundaries are critically important to the material performance of fusion reactor materials such as vanadium, particularly mechanical properties and irradiation resistance. A key challenge to the design and control of grain boundaries in vanadium alloys is the lack of quantitative data on grain boundary segregation. In this study, we combine computational and experimental methods to address this gap. Using a machine learning-accelerated quantum mechanics/molecular mechanics approach, we calculated the segregation spectra for 28 transition metal elements in polycrystalline vanadium, and validated these predictions experimentally for a subset of solutes that sample a range of segregation behavior, specifically zirconium, titanium, and tungsten, using analytical transmission electron microscopy. The agreement between experiment and theory highlights the predictive capability of our approach. Critically, this work provides a comprehensive database of quantum-accurate solute segregation enthalpies in vanadium, enabling the development of advanced alloys for fusion reactors applications.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"294 ","pages":"Article 121169"},"PeriodicalIF":8.3,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113790","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Acta MaterialiaPub Date : 2025-05-22DOI: 10.1016/j.actamat.2025.121165
Xianqiang Yu , Ruikai Qi , Linfeng Zhang , Li Deng , Mengxiao Zhong , Zheng-jie Chen , Xiaofeng Lu
{"title":"Ruthenium-cobalt oxide solid solution nanofiber: a robust bifunctional electrocatalyst for overall water splitting with superior ampere-grade-current-density electrocatalytic performance","authors":"Xianqiang Yu , Ruikai Qi , Linfeng Zhang , Li Deng , Mengxiao Zhong , Zheng-jie Chen , Xiaofeng Lu","doi":"10.1016/j.actamat.2025.121165","DOIUrl":"10.1016/j.actamat.2025.121165","url":null,"abstract":"<div><div>Constructing high-performance bifunctional electrocatalysts for water electrolysis under an ampere-grade current density is crucial for practical application. Herein, ruthenium-cobalt oxide (RuCoO<sub>x</sub>) solid solution nanofibers (SSNFs) are fabricated as robust bifunctional electrocatalyst for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). Typically, the optimized Ru<sub>2</sub>Co<sub>1</sub>O<sub>x</sub> SSNFs exhibit an ultra-low overpotential of 362 mV at 1000 mA cm<sup>-2</sup> for OER, not only significantly superior to the prepared RuO<sub>x</sub> nanofibers (NFs), CoO<sub>x</sub> and commercial RuO<sub>2</sub> catalyst but also outperforming many reported typical OER electrocatalysts. In addition, the representative Ru<sub>1</sub>Co<sub>1</sub>O<sub>x</sub> SSNFs catalyst presents a good HER performance with an overpotential of only 149 mV at 1000 mA cm<sup>-2</sup> and excellent stability over 120 h, surpassing the benchmark Pt/C catalyst. Furthermore, these catalysts are assembled to construct an alkaline overall water splitting cell, demonstrating a better performance than most of the recently reported water electrolyzers. Density functional theory calculations reveal that the addition of Co effectively modulates the <em>d</em>-orbitals of Ru and reduces the reaction energy barriers of O*→OOH*, benefitting to enhance the OER property. Additionally, the hybridization of Co and Ru is beneficial for modulating the strength of H* adsorption in an alkaline solution, which promotes the alkaline HER efficiency.</div></div>","PeriodicalId":238,"journal":{"name":"Acta Materialia","volume":"294 ","pages":"Article 121165"},"PeriodicalIF":8.3,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}