Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-23DOI: 10.1016/j.electacta.2026.148518
M.R. Bermejo , P. Moretti , M. Gómez , J. Castro , M. Merlo , J.J. Biendicho
{"title":"The role of electrochemistry in the direct recycling of lithium-ion batteries","authors":"M.R. Bermejo , P. Moretti , M. Gómez , J. Castro , M. Merlo , J.J. Biendicho","doi":"10.1016/j.electacta.2026.148518","DOIUrl":"10.1016/j.electacta.2026.148518","url":null,"abstract":"<div><div>The increasing demand for lithium-ion batteries, driven by their widespread use in electronic devices and electric vehicles, has raised concerns regarding their recycling and end-of-life management. Batteries contain valuable and potentially hazardous materials, necessitating efficient recovery strategies. In this context, direct recycling has emerged as a promising approach, enabling the regeneration of cathode active materials (CAMs) for reuse in new batteries, with reduced energy consumption and minimal environmental impact.</div><div>Among recycling strategies, electrochemical methods stand out for their efficiency in recovering critical materials via electrodeposition or ion insertion, generating minimal waste and reducing reagent consumption. In this work, the CAM from NMC-type lithium-ion batteries (Li₁Ni₀.₆Mn₀.₂Co₀.₂O₂, NMC622) was re-lithiated using chronopotentiometry as the electrochemical technique. The re-lithiation process was systematically optimized by evaluating the effects of lithium salt concentration, applied current density, temperature, and stirring conditions. After lithium insertion, the material underwent a heat treatment at 600 °C to restore its original crystalline structure.</div><div>X-ray diffraction (XRD) analysis confirmed that the regenerated CAM recovered the characteristic layered structure of commercial NMC622, with matching peak positions. Analysis of the I₀₀₃/I₁₀₄ intensity ratio revealed an increase in Li–Ni cation mixing compared with the pristine reference, indicating that while the global layered structure was restored, some degree of internal disorder remained.</div><div>These results highlight the potential of electrochemical re-lithiation as a sustainable strategy for the recovery and regeneration of degraded lithium-ion cathodes, contributing to circular economy approaches in battery materials management.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148518"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146777949","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-10DOI: 10.1016/j.electacta.2026.148431
Tewelde Hailay Gebregeorgis , Rodrigo Lopez Baez , Joan R. Busacker , Louis De Taeye , Mats Meeusen , Xinhua Zhu , Annick Hubin , Mesfin Haile Mamme
{"title":"Impact of electrode geometry on stress evolution and crack formation in solid-state batteries: Prediction and experimental validation","authors":"Tewelde Hailay Gebregeorgis , Rodrigo Lopez Baez , Joan R. Busacker , Louis De Taeye , Mats Meeusen , Xinhua Zhu , Annick Hubin , Mesfin Haile Mamme","doi":"10.1016/j.electacta.2026.148431","DOIUrl":"10.1016/j.electacta.2026.148431","url":null,"abstract":"<div><div>All-solid-state lithium-ion batteries (ASSLIBs) emerge as a promising next-generation technology, yet their realization is hindered by challenges, such as electrode/solid-electrolyte (SE) interface issues. Here, a combined experimental-computational approach is utilized to analyze the interplay between the geometrical structure of the electrode/SE interface configuration and electro-chemo-mechanical processes in an ASSLIB cell. Two types of physics-based models, which differ on the level of Multiphysics description, are developed: a pure electrochemical and a fully coupled electro-chemo-mechanical framework, to quantitatively compare their ability to predict experimentally observed ASSLIB behavior. The fully coupled model shows a strong agreement with experimental data, achieving less than 0.5% capacity difference at the end of discharge, while the pure model significantly deviates from experimental data, overestimating capacity by 26.5%. This underscores the importance of accounting for mechanical phenomena and Multiphysics coupling for accurate prediction. Following this validation, the coupled model is utilized to evaluate the impact of the planar and patterned (nonplanar) interface geometries on ASSLIB performance. It is observed that the patterned interface structure at/ near the pattern edges experiences the maximum gradient of lithium concentration and mechanical stress profiles. This is due to the sharp change in geometry, indicating a higher risk of mechanical failure, which is also experimentally confirmed as a critical area for crack formation. This study further investigates how variations in pattern geometric parameters affect ASSLIB performance, aiming to quantify the impact of pattern height, width, inter-distance, and base layer height. The results provide an in-depth analysis of the relationship between interface geometry type, lithium concentration, and stress profiles, offering guidance for optimizing geometric factors to limit mechanical failure.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148431"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-01-29DOI: 10.1016/j.electacta.2026.148337
Xue Dang , Huaixi Chen , Weiying Huang , Chun Yu , Yanli Huang , Qingmao Kong , Chenlong Chen , Xianzeng Zhang , Yujing Liu , Yanjin Lu
{"title":"Corrosion resistance of Ti-1Al-8V-5Fe fabricated via laser powder bed fusion: Effect of post-heat treatment","authors":"Xue Dang , Huaixi Chen , Weiying Huang , Chun Yu , Yanli Huang , Qingmao Kong , Chenlong Chen , Xianzeng Zhang , Yujing Liu , Yanjin Lu","doi":"10.1016/j.electacta.2026.148337","DOIUrl":"10.1016/j.electacta.2026.148337","url":null,"abstract":"<div><div>This first study investigates how heat treatment affects the corrosion resistance of medical Ti-1Al-8V-5Fe (Ti-185) alloy in 0.9 wt.% NaCl solution, with emphasis on microstructural changes and passive film semiconductor properties. The as-fabricated alloy produced by laser powder bed fusion (LPBF) exhibits a single β-phase equiaxed grain structure. Heat treatment triggers α-phase precipitation, resulting in an α+β dual-phase structure. As annealing temperature increases, α-phase content rises progressively, while grain size and residual stress show an initial decrease followed by an increase. Corrosion testing reveals that at lower annealing temperature (480 °C), isolated α-phase islands within the β-matrix dissolve readily, accelerating corrosion. At higher temperature (730 °C), α-phase forms continuous bands that isolate β-phase, establishing microgalvanic cells where the anodic dissolution rate of α-phase surpasses the cathodic reduction rate of β-phase, thus enhancing overall corrosion. The sample annealed at 690 °C demonstrates superior corrosion resistance, showing the highest open-circuit potential, lowest corrosion current density, and maximum polarization resistance. Its passive film exhibits n-type semiconductor behavior with minimal donor concentration and maximum thickness, effectively blocking chloride ion penetration. This research establishes a viable post-heat treatment approach to improve Ti-185 alloy performance, advancing its application as a high-performance dental implant material.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148337"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146071868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-18DOI: 10.1016/j.electacta.2026.148479
Esra Kus, Murside Haciismailoglu
{"title":"Structural, magnetic and corrosion properties of Cr-Ni-Fe coatings electrodeposited by binary potential loop","authors":"Esra Kus, Murside Haciismailoglu","doi":"10.1016/j.electacta.2026.148479","DOIUrl":"10.1016/j.electacta.2026.148479","url":null,"abstract":"<div><div>Cr-Ni-Fe coatings were electrodeposited from an aqueous electrolyte consisting of chloride salts of each metal and boric acid. The boric acid effect was investigated. A binary potential loop of -0.7 V and -1.8 V was applied in sequence during the specified time interval and charge amount, respectively. Before electrodeposition, the solutions were optically and electrochemically analyzed by ultraviolet-visible spectroscopy and cyclic voltammetry (CV). The complexes of [Cr(H<sub>2</sub>O)<sub>6</sub>]<sup>3+</sup>, [Cr(H<sub>2</sub>O)<sub>5</sub>Cl]<sup>2+</sup> and [Cr(H<sub>2</sub>O)<sub>4</sub>Cl<sub>2</sub>]<sup>+</sup> formed natively in solution. Also, the crystal field, Racah and ligand field parameters were calculated for the solutions without and with boric acid. The boric acid makes the bonds less covalent in character. According to the CV curves, the current becomes smooth with the boric acid content due to the buffering effect. X-ray diffraction patterns showed that the coatings were crystallized in cubic δ-phase as a result of the dominance of Cr content. The reason for the cracks on the surface was studied by the Fourier-transformed infrared spectroscopy, optical profilometry, scanning electron microscopy and energy dispersive X-ray (EDX) spectroscopy. The magnetic properties were searched by vibrating sample magnetometry, which proved the magnetic content (Ni and Fe) of the coating, consistent with the EDX results. The corrosion behavior was studied by electrochemical impedance spectroscopy and Tafel plots. The highest corrosion resistance was found for the coatings deposited from a solution having 0.12 M boric acid.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148479"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146209996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-18DOI: 10.1016/j.electacta.2026.148492
Ricardo M. Souto , Hugh S. Isaacs , Javier Izquierdo
{"title":"Challenges to local potential measurement for chemical mapping with scanning microelectrochemical techniques due to the occurrence of galvanic coupling processes on magnesium alloys","authors":"Ricardo M. Souto , Hugh S. Isaacs , Javier Izquierdo","doi":"10.1016/j.electacta.2026.148492","DOIUrl":"10.1016/j.electacta.2026.148492","url":null,"abstract":"<div><div>The interaction between concentrations and potentials was modeled and quantified in relation to local potential measurements during corrosion processes. This modeling aimed to study the uncertainty generated by the description of potential distributions in the vicinity of active corrosion sites, assuming hemispherical symmetry of the currents and the transport of metal ions radiating from a point electrode. This work demonstrates the coupling of electrical and concentration gradients around anodic and cathodic sites in galvanic corrosion processes, a coupling that, in practice, will limit the interpretation of local electrochemical data and the quantification of corrosion mechanisms if it is not taken into account. A critical distance is defined beyond which the signal measured by a probe deviates from the linear dependence with a slope of −1, generally accepted to describe the variation of the probe signal with the tip-sample distance during scanning microelectrochemical measurements using passive microelectrodes as probes. Furthermore, the value of this critical distance depends strongly on the conductivity of the electrolytic test solution, being larger for more dilute solutions. In addition, the implications for estimating local corrosion currents using a noble metal, such as a platinum wire as a model current source for calibrating the potential signal in a validation cell, are also presented.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148492"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146209995","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-16DOI: 10.1016/j.electacta.2026.148462
J.H. Moss, K. Doblhoff-Dier
{"title":"If it fits, it sits: Geometric ordering of cations at electrochemical interfaces","authors":"J.H. Moss, K. Doblhoff-Dier","doi":"10.1016/j.electacta.2026.148462","DOIUrl":"10.1016/j.electacta.2026.148462","url":null,"abstract":"<div><div>The atomic-scale structure of solid–liquid interfaces is a cornerstone of many scientific fields, including electrochemistry, environmental science, and biology. Despite its importance, current models often struggle to accurately describe how ions and solvent molecules arrange near charged surfaces. Using 1M alkali chloride solutions at charged Pt(111) interfaces as model system, we investigate the behavior of cations at the surface. Since alkali cations can critically influence electrochemical reactions, understanding their arrangement at the Pt interface, including their arrangement relative to the water and their crowding behavior, is thus essential. Using classical molecular dynamics simulations, we examine the spatial distribution, solvation structure, and the phenomena governing interfacial ordering for lithium, sodium, and cesium ions near the electrode. To account for electrode charges, we use a polarizable electrode model featuring fluctuating atomic charges and fixed total surface charge. Our results reveal that even without any applied surface charge, ions preferentially occupy specific positions. These positions are defined by the geometric compatibility between the ions’ hydration shells and the layered water structure at the Pt(111) interface. The layered water essentially functions as a structural template for ions, leading to interfacial ion layering and ordering. Applied charge strengthens this ordering, promoting the formation of cation–cation pairs and cation clusters in which cations share their solvation shell. Our results shed more light on the crowding of ions at the interface and furthermore suggest a geometric “fit” mechanism governing ion layering that expands beyond purely electrostatic explanations, while, at the same time, providing an intuitive explanation of the cation’s behavior.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148462"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146209486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-19DOI: 10.1016/j.electacta.2026.148494
V. Murugesan, Remco Hartkamp, Johan T. Padding
{"title":"Microbial electrosynthesis for CO2 conversion: Process limiting steps investigated by micro-scale modeling","authors":"V. Murugesan, Remco Hartkamp, Johan T. Padding","doi":"10.1016/j.electacta.2026.148494","DOIUrl":"10.1016/j.electacta.2026.148494","url":null,"abstract":"<div><div>The advancement of microbial electrosynthesis systems (MES) towards industrialization is currently hindered by a limited understanding of the fundamental constraints affecting selective production of high-value chemicals. To address this challenge, we develop a comprehensive computational model that integrates microbial, electrochemical, and acid–base reactions with pore-scale transport processes within a three-dimensionally resolved biofilm. This study investigates the H<sub>2</sub>-mediated CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> fixation pathway to acetate, butyrate, and caproate. The effect of applied cathode potential and biofilm thickness on macroscopic parameters, such as efficiency and selectivity, is analyzed based on local concentrations and electrochemical and biochemical fluxes. Among the limiting factors, the availability of CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> emerges as the main limitation for biochemical reactions due to its low solubility and high half-saturation constant. Additionally, hydrogen – serving as the electron mediator – limits the reaction rate at low current densities and reduces electron transfer efficiency at higher current densities. A key insight from our study is the identification of an optimal electrode potential for each biofilm thickness, balancing both H<sub>2</sub> transfer and CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> consumption efficiencies. Furthermore, carbon selectivity shifts with increasing biofilm thickness: net acetate production declines while caproate production increases. This trend is attributed to the prolonged residence time of metabolic intermediates within thicker biofilms, promoting chain elongation pathways. Thus, our work takes an important step towards a fundamental understanding of caproate selectivity across different biofilms, which can be used to optimize the electrode structure and operating conditions to control the local biofilm thickness.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148494"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146223361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-17DOI: 10.1016/j.electacta.2026.148477
Dean Yost, Gary M. Koenig Jr.
{"title":"Impacts of electrolyte mixing method on aluminum anodization","authors":"Dean Yost, Gary M. Koenig Jr.","doi":"10.1016/j.electacta.2026.148477","DOIUrl":"10.1016/j.electacta.2026.148477","url":null,"abstract":"<div><div>Aluminum anodization is a widespread industrial process used in a variety of applications including energy storage devices, microstructure templating, and corrosion inhibition. Prior work has extensively investigated electrochemical process parameters that influence oxide growth and structure. On an industrial scale, anodization is performed using both batch and continuous processes. For batch anodization, direct scale-up from laboratory benchtop experiments to large scale manufacturing is more straightforward. However, a translating electrode-electrolyte interface relevant to continuous processing is less explored at laboratory scale or reported in the literature. In this work, the influence of modifying mixing conditions to include rotating the anodization sample itself was investigated and compared to more conventional processing with external agitation or lack of initiating mixing. For conditions where the mixing power was matched, active agitation using the aluminum coupon provided faster and more homogeneous growth of the oxide layer, resulting in improved current utilization.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148477"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146231323","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-20DOI: 10.1016/j.electacta.2026.148507
Wenjing Chen , Rugao Huang , Sifan Tan , Tao Xu , Xiaowu Hu
{"title":"Effects of Ni-La Micro-alloying on Sn-Ag-Cu solders: Microstructure, dynamic mechanical properties and corrosion behavior","authors":"Wenjing Chen , Rugao Huang , Sifan Tan , Tao Xu , Xiaowu Hu","doi":"10.1016/j.electacta.2026.148507","DOIUrl":"10.1016/j.electacta.2026.148507","url":null,"abstract":"<div><div>As a vitamin for industry, the rare earth element La plays a key role in enhancing alloy performance. This study prepared SAC0307-0.5Ni-xLa (x=0.1, 0.2 wt.%) composite lead-free solder alloys and investigated the effects of Ni and La on the microstructure and properties. Microscopic characterization indicated that the introduction of Ni promotes the refinement of the Cu6Sn5 phase and the formation of (Cu, Ni)6Sn5 ternary compounds. Meanwhile, the addition of La led to the formation of dispersed LaSn3 phases and suppressed the coarsening of Ag3Sn phases. Notably, Composite microalloying of Ni and La reduced the average grain size of the alloy from 10.83 μm to 8.01 μm while simultaneously decreasing the proportion of large-angle grain boundaries. Besides, the dynamic compression test revealed that the combination of Ni-La notably enhanced the impact resistance of SAC0307 solder. Furthermore, the composite microalloying significantly improved the resistance to intergranular corrosion propagation. The electrochemical measurements showed that the corrosion current density (Icorr) of the Ni-La2 alloy was as low as 0.024 μA·cm-2, which is 97% lower than that of the SAC0307 alloy. Meanwhile, its passivation current density (Ip) was 0.00198 A·cm-2, representing a 32.4% reduction. X-ray photoelectron spectroscopy and Raman spectroscopy analyses indicated that the Ni-La composite microalloying increased the SnO2 content in the passivation film, enhanced its stability, and significantly inhibit the penetration of Cl-. The 3D morphological characterization further revealed that, compared with base alloy, the Ni-La2 alloy exhibited a 52.5% reduction in surface roughness (Sa = 13.47 nm) and a 67.7% reduction in maximum corrosion pit depth (5.02 μm). These results demonstrate the excellent corrosion resistance of Ni-La microalloyed alloys.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148507"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146778153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrochimica ActaPub Date : 2026-05-01Epub Date: 2026-02-20DOI: 10.1016/j.electacta.2026.148505
Yuying Yang, Qiannan Sun, Daying Xu, Min Zhou, Wenhui Zhang, Yihan Li, Zhongai Hu
{"title":"FeS/Co3S4/Mo2S3 ternary heterojunction nanoflowers regulated by interfacial electronic rearrangement as an efficient bifunctional electrocatalyst for water splitting","authors":"Yuying Yang, Qiannan Sun, Daying Xu, Min Zhou, Wenhui Zhang, Yihan Li, Zhongai Hu","doi":"10.1016/j.electacta.2026.148505","DOIUrl":"10.1016/j.electacta.2026.148505","url":null,"abstract":"<div><div>In this paper, a FeS/Co<sub>3</sub>S<sub>4</sub>/Mo<sub>2</sub>S<sub>3</sub> ternary heterojunction catalyst featuring a three-dimensional hierarchical nanoflower structure self-assembled from porous nanorods was successfully constructed on nickel foam (NF) by a stepwise hydrothermal synthesis strategy. At the heterointerface, part of the electrons from Co and Mo are transferred to the S atoms, resulting in a decrease in the electron density of the Co and Mo orbitals. Correspondingly, the S atoms that receive electrons from Co/Mo exhibit an increased electron density and further transfer electrons to Fe atoms through Fe‑S bonds (S‑bridges), thereby enhancing the electron density of Fe. This electron rearrangement process, induced by interfacial electronic interactions, optimizes the electronic structure of the electrocatalyst, which significantly enhances charge-transfer efficiency and accelerates the kinetic steps of the electrocatalytic reaction. Ultimately, this leads to a significant enhancement the bifunctional catalytic performance of the catalyst. The optimized catalyst exhibits excellent hydrogen evolution (10 mA cm<sup>-2</sup>@31 mV) and oxygen evolution activity (10 mA cm<sup>-2</sup>@222 mV) in alkaline medium. When assembled into a symmetrical total water splitting electrolytic cell, it only needs a low voltage of 1.54 V to drive a current density of 10 mA cm<sup>-2</sup>, and can maintain excellent stability in a constant current test for up to 200 h. This study not only confirms the great potential of multi-sulfide heterojunctions in electrolyzed water catalysis, but also opens up a multi-dimensional regulation path for the development of a new generation of non-noble metal bifunctional catalysts through the precise linkage design of ''structure-interface-performance''.</div></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"557 ","pages":"Article 148505"},"PeriodicalIF":5.6,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146777970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}