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Microstructure modification strategies on P2-NaxNi1/3Fe1/3Mn1/3O2 cathode materials by high temperature solid-state method for enhanced sodium ion storage
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236872
Shao-hua Luo , Ge Wang , Guodong Hao , Xinru Tian , Liu Yang , Sheng-xue Yan
NaxNi1/3Fe1/3Mn1/3O2 cathode material with high stability and high capacity is favored by researchers. However, during the charge-discharge process, NaxNi1/3Fe1/3Mn1/3O2 undergoes a series of complex phase transitions, which lead to the attenuation of its electrochemical performance and severely limit its application. In this paper, a series of NaxNi1/3Fe1/3Mn1/3O2 (0.6 ≤ x ≤ 1.0) cathode materials are synthesized by the high-temperature solid-state method, and the influence of varying sodium contents on the structure, Na occupancy, and various performance of the materials is analyzed. The results indicate that all four samples are P2 phase. However, they have different sodium sites (directly under the transition metal element (Naf) and directly under the gap of the three transition metal elements (Nae)) occupancy. It is found that the Naf to Nae ratio of Na0.9Ni1/3Fe1/3Mn1/3O2 material is 0.55, at which time Naf/Nae is lower and the electrochemical performance is the best. Its initial discharge specific capacity is 112mAg−1, and after the multiplicative performance test, the discharge specific capacity is 95.7mAg−1. The study shows that by adjusting the initial sodium content, the occupancy rate of different sodium sites is changed, which significantly affects the morphology, capacity, and cycling stability of the material.
{"title":"Microstructure modification strategies on P2-NaxNi1/3Fe1/3Mn1/3O2 cathode materials by high temperature solid-state method for enhanced sodium ion storage","authors":"Shao-hua Luo ,&nbsp;Ge Wang ,&nbsp;Guodong Hao ,&nbsp;Xinru Tian ,&nbsp;Liu Yang ,&nbsp;Sheng-xue Yan","doi":"10.1016/j.jpowsour.2025.236872","DOIUrl":"10.1016/j.jpowsour.2025.236872","url":null,"abstract":"<div><div>Na<sub>x</sub>Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> cathode material with high stability and high capacity is favored by researchers. However, during the charge-discharge process, Na<sub>x</sub>Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> undergoes a series of complex phase transitions, which lead to the attenuation of its electrochemical performance and severely limit its application. In this paper, a series of Na<sub>x</sub>Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> (0.6 ≤ x ≤ 1.0) cathode materials are synthesized by the high-temperature solid-state method, and the influence of varying sodium contents on the structure, Na occupancy, and various performance of the materials is analyzed. The results indicate that all four samples are P2 phase. However, they have different sodium sites (directly under the transition metal element (Na<sub>f</sub>) and directly under the gap of the three transition metal elements (Na<sub>e</sub>)) occupancy. It is found that the Na<sub>f</sub> to Na<sub>e</sub> ratio of Na<sub>0.9</sub>Ni<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> material is 0.55, at which time Na<sub>f</sub>/Na<sub>e</sub> is lower and the electrochemical performance is the best. Its initial discharge specific capacity is 112mAg<sup>−1</sup>, and after the multiplicative performance test, the discharge specific capacity is 95.7mAg<sup>−1</sup>. The study shows that by adjusting the initial sodium content, the occupancy rate of different sodium sites is changed, which significantly affects the morphology, capacity, and cycling stability of the material.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236872"},"PeriodicalIF":8.1,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759836","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reversible hydrogen spillover enhances hydrogen evolution reaction on electrodeposited MoNi4/Ni17W3 with amorphous/crystalline heterostructure
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236912
Xiaoxiao Yin , Yujia Wang , Xiao Fu , Xu Liu , Yi Wang , Zhongqing Liu
Hydrogen spillover phenomena have recently created a new opportunity for ehancing the surface adsorption/desorption kinetics of reactants and intermediates, thereby effectively improving electrocatalytic activity. In this work, Mo elements are introduced into an electrolyte containing Ni, W, and Co, inducing the in-situ formation of an amorphous MoNi4 phase during electrodeposition. Consequently, a coral-like porous MoNi4/Ni17W3 heterostructure is constructed on a stainless steel mesh substrate. The MoNi4/Ni17W3 heterogeneous structure features abundant defect sites and oxygen vacancies, which promote enhanced interfacial charge transfer. This configuration optimizes the H∗ adsorption, transfer, and desorption processes by facilitating a reversible hydrogen spillover effect between MoNi4 and Ni17W3, as suggested by both experimental results and DFT calculations. These advancements notably improve the kinetics of the electrocatalytic hydrogen evolution reaction (HER), highlighting its promising potential for efficient hydrogen production. In a 1 M KOH solution, the MoNi4/Ni17W3 electrode affords the overpotentials of only 26 mV and 98 mV at current densities of 10 mA cm−2 and 100 mA cm−2, respectively. Moreover, the electrode maintain almost unchanged HER performance during a 48-h stability test at a current density of 100 mA cm−2. This work provides a new approach for designing and constructing high-performance non-noble-metal-based heterostructured electrocatalysts.
{"title":"Reversible hydrogen spillover enhances hydrogen evolution reaction on electrodeposited MoNi4/Ni17W3 with amorphous/crystalline heterostructure","authors":"Xiaoxiao Yin ,&nbsp;Yujia Wang ,&nbsp;Xiao Fu ,&nbsp;Xu Liu ,&nbsp;Yi Wang ,&nbsp;Zhongqing Liu","doi":"10.1016/j.jpowsour.2025.236912","DOIUrl":"10.1016/j.jpowsour.2025.236912","url":null,"abstract":"<div><div>Hydrogen spillover phenomena have recently created a new opportunity for ehancing the surface adsorption/desorption kinetics of reactants and intermediates, thereby effectively improving electrocatalytic activity. In this work, Mo elements are introduced into an electrolyte containing Ni, W, and Co, inducing the in-situ formation of an amorphous MoNi<sub>4</sub> phase during electrodeposition. Consequently, a coral-like porous MoNi<sub>4</sub>/Ni<sub>17</sub>W<sub>3</sub> heterostructure is constructed on a stainless steel mesh substrate. The MoNi<sub>4</sub>/Ni<sub>17</sub>W<sub>3</sub> heterogeneous structure features abundant defect sites and oxygen vacancies, which promote enhanced interfacial charge transfer. This configuration optimizes the H∗ adsorption, transfer, and desorption processes by facilitating a reversible hydrogen spillover effect between MoNi<sub>4</sub> and Ni<sub>17</sub>W<sub>3</sub>, as suggested by both experimental results and DFT calculations. These advancements notably improve the kinetics of the electrocatalytic hydrogen evolution reaction (HER), highlighting its promising potential for efficient hydrogen production. In a 1 M KOH solution, the MoNi<sub>4</sub>/Ni<sub>17</sub>W<sub>3</sub> electrode affords the overpotentials of only 26 mV and 98 mV at current densities of 10 mA cm<sup>−2</sup> and 100 mA cm<sup>−2</sup>, respectively. Moreover, the electrode maintain almost unchanged HER performance during a 48-h stability test at a current density of 100 mA cm<sup>−2</sup>. This work provides a new approach for designing and constructing high-performance non-noble-metal-based heterostructured electrocatalysts.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236912"},"PeriodicalIF":8.1,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Numerical evaluation of a novel integrated solar reactor for high-temperature H2O electrolysis with high scalability and solar-to-fuel efficiency
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236848
Liya Zhu , Weixu Yang , Fengshuang Han , Yunjin Ao , Youjun Lu
Solar-driven high temperature H2O electrolysis provides a promising path for green H2 production. In this work, a novel integrated solar-driven high temperature H2O electrolysis reactor was proposed, and its thermal and energy conversion performance was evaluated based on an optical-thermal-chemical coupling model. The results demonstrated that the temperature difference on the tubular SOEC under highly uneven solar radiation can be lowered by the novel multi-layer structure. A solar-to-fuel (STF) efficiency of 23.0 %, which is higher than those from references, was predicted due to close integration/coupling of the various processes in the reactor, and it may still be improved by increasing the direct normal irradiance (DNI) and operation voltage. The results also emphasize the importance of reaction kinetics to the efficiency of the system. Contrary to the thermodynamic estimation based on equilibrium, the efficiency in exothermic mode is shown to be higher than that in endothermic mode owing to way better kinetics of the former. The reactor provides a simple but effective strategy for addressing the temperature gradient caused by the uneven solar radiation and efficient heat exchange/recovery between the heating and electrolysis processes. Its modular design facilitates scaling, optimization and maintenance. The insights shown can be of guiding significance for designing and practical realization of the integrated reactor concept.
{"title":"Numerical evaluation of a novel integrated solar reactor for high-temperature H2O electrolysis with high scalability and solar-to-fuel efficiency","authors":"Liya Zhu ,&nbsp;Weixu Yang ,&nbsp;Fengshuang Han ,&nbsp;Yunjin Ao ,&nbsp;Youjun Lu","doi":"10.1016/j.jpowsour.2025.236848","DOIUrl":"10.1016/j.jpowsour.2025.236848","url":null,"abstract":"<div><div>Solar-driven high temperature H<sub>2</sub>O electrolysis provides a promising path for green H<sub>2</sub> production. In this work, a novel integrated solar-driven high temperature H<sub>2</sub>O electrolysis reactor was proposed, and its thermal and energy conversion performance was evaluated based on an optical-thermal-chemical coupling model. The results demonstrated that the temperature difference on the tubular SOEC under highly uneven solar radiation can be lowered by the novel multi-layer structure. A solar-to-fuel (STF) efficiency of 23.0 %, which is higher than those from references, was predicted due to close integration/coupling of the various processes in the reactor, and it may still be improved by increasing the direct normal irradiance (DNI) and operation voltage. The results also emphasize the importance of reaction kinetics to the efficiency of the system. Contrary to the thermodynamic estimation based on equilibrium, the efficiency in exothermic mode is shown to be higher than that in endothermic mode owing to way better kinetics of the former. The reactor provides a simple but effective strategy for addressing the temperature gradient caused by the uneven solar radiation and efficient heat exchange/recovery between the heating and electrolysis processes. Its modular design facilitates scaling, optimization and maintenance. The insights shown can be of guiding significance for designing and practical realization of the integrated reactor concept.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236848"},"PeriodicalIF":8.1,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Novel intrinsic microporous binders in the cathode catalyst layer for high-performance alkaline water electrolysis
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236916
Xin Wang , Lei Liu , Nanwen Li
Anion exchange membrane water electrolysis (AEMWE) garners significant attention. However, systematic studies on the binder structure and content are scarce. Therefore, we report two novel quaternized polymers of intrinsic microporosity with pyrrolidinium and piperidinium cations (referred to as QPIM-Py and QPIM-Pi) as binder materials. Additionally, the effect of the microporosity structure on the AEMWE performance is compared to that of the control binder without microporosity (poly(p-terphenyl N,N-dimethylpiperidinium) referred to as PAP-TP-85, 85 is the molar ratio between N-methyl-4-piperidone and aryl monomers). The hydrogen permeabilities of QPIM-Py and QPIM-Pi membranes are found to be 60.5 and 32.4 barrer, which are significantly higher than that of the PAP-TP-85 (4.07 barrer). Moreover, the surface area of the QPIM-based catalyst layer (CL) is substantially higher than that of the control CL. Finally, with home-made PAP-TP-85 membrane and the aforementioned binders in the CL, it is demonstrated that the binder structure in the cathode CL has a considerable impact on the AEMWE performance. The AEMWE with QPIM-Py-10 % binder achieves the best performance, with a current density of 2000 mA/cm2 at a voltage of 2.04 V. Furthermore, the CL with modified binder demonstrates a much higher performance than that with microporosity-free binder in AEMWE.
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引用次数: 0
Electrochemical storage systems for renewable energy integration: A comprehensive review of battery technologies and grid-scale applications
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236832
M.H. Taabodi, T. Niknam, S.M. Sharifhosseini, H. Asadi Aghajari, S. Shojaeiyan
The global transition toward sustainable energy systems has become one of the most critical challenges facing modern power infrastructure, particularly as nations worldwide seek to reduce their carbon footprint. The integration of renewable energy sources into existing power grids presents significant technical challenges due to their inherent variability and intermittency, requiring robust and reliable storage solutions to maintain grid stability and reliability. Electrochemical storage systems, encompassing technologies from lithium-ion batteries and flow batteries to emerging sodium-based systems, have demonstrated promising capabilities in addressing these integration challenges through their versatility and rapid response characteristics. This comprehensive review systematically analyzes recent developments in grid-scale battery storage technologies, examining fundamental materials advancement, integration strategies, performance optimization, and economic considerations, while distinctively focusing on the synergistic relationships between different storage technologies in hybrid configurations and their practical implementation in diverse geographic and market contexts. Unlike previous reviews that typically focus on individual technologies or specific applications, this work provides a comprehensive analysis of the entire ecosystem of grid-scale battery storage, from materials science to market implementation, offering unique insights into the interaction of technical advancement, economic viability, and environmental sustainability during the integration of renewable energy.
全球向可持续能源系统转型已成为现代电力基础设施面临的最严峻挑战之一,尤其是在世界各国都在努力减少碳足迹的情况下。由于可再生能源固有的多变性和间歇性,将其整合到现有电网中面临着巨大的技术挑战,需要稳健可靠的存储解决方案来维持电网的稳定性和可靠性。从锂离子电池和液流电池技术到新兴的钠基系统,电化学储能系统凭借其多功能性和快速响应特性,在应对这些整合挑战方面展现出了良好的能力。本综述系统分析了电网规模电池储能技术的最新发展,研究了基础材料进步、集成策略、性能优化和经济因素,同时特别关注混合配置中不同储能技术之间的协同关系,以及它们在不同地域和市场环境中的实际应用。与以往通常关注单项技术或具体应用的综述不同,本研究对电网规模电池储能的整个生态系统,从材料科学到市场实施进行了全面分析,为可再生能源整合过程中技术进步、经济可行性和环境可持续性之间的相互作用提供了独到的见解。
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引用次数: 0
Pt doped NiCo2O4 electrolysis for achieving highly efficient overall water splitting in alkaline condition
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236891
Wei Cheng , Zheng Cui , Siyu Xu , Shaoheng Cheng , Nan Gao , Min Yang , Hongdong Li
The development of efficient electrocatalysts to substitute Pt and Ir in overall water splitting is critical for advancing sustainable hydrogen generation. Transition metal oxides have attracted wide attention and shown promising catalytic activity in water splitting reaction. In this work, the doped bimetallic oxide Pt-NiCo2O4 catalyst having urchin-like structure surrounding with abundant nanoneedles is prepared by multi-step hydrothermal reaction, ion-exchange method and annealing process. In alkaline electrolyte (1.0 M KOH), the prepared electrocatalyst requires remarkably low overpotentials of 40 mV for hydrogen evolution reaction and 263 mV for oxygen evolution reaction at 10 mA cm−2. The assembled two-electrode alkaline electrolyzer achieves a current density of 10 mA cm−2 at a low cell voltage of 1.62 V, rivaling the performance of commercial electrodes. The unique urchin-like structure not only facilitates the gas emission, but also creates abundant active sites, which promote electron transfer and improve reaction kinetics. Furthermore, computational modeling reveals that optimized d-band center and energy barrier of H2O decomposition after Pt atoms doping. This work establishes a rational strategy for designing high-efficiency bifunctional electrocatalysts in overall water splitting under alkaline conditions.
{"title":"Pt doped NiCo2O4 electrolysis for achieving highly efficient overall water splitting in alkaline condition","authors":"Wei Cheng ,&nbsp;Zheng Cui ,&nbsp;Siyu Xu ,&nbsp;Shaoheng Cheng ,&nbsp;Nan Gao ,&nbsp;Min Yang ,&nbsp;Hongdong Li","doi":"10.1016/j.jpowsour.2025.236891","DOIUrl":"10.1016/j.jpowsour.2025.236891","url":null,"abstract":"<div><div>The development of efficient electrocatalysts to substitute Pt and Ir in overall water splitting is critical for advancing sustainable hydrogen generation. Transition metal oxides have attracted wide attention and shown promising catalytic activity in water splitting reaction. In this work, the doped bimetallic oxide Pt-NiCo<sub>2</sub>O<sub>4</sub> catalyst having urchin-like structure surrounding with abundant nanoneedles is prepared by multi-step hydrothermal reaction, ion-exchange method and annealing process. In alkaline electrolyte (1.0 M KOH), the prepared electrocatalyst requires remarkably low overpotentials of 40 mV for hydrogen evolution reaction and 263 mV for oxygen evolution reaction at 10 mA cm<sup>−2</sup>. The assembled two-electrode alkaline electrolyzer achieves a current density of 10 mA cm<sup>−2</sup> at a low cell voltage of 1.62 V, rivaling the performance of commercial electrodes. The unique urchin-like structure not only facilitates the gas emission, but also creates abundant active sites, which promote electron transfer and improve reaction kinetics. Furthermore, computational modeling reveals that optimized d-band center and energy barrier of H<sub>2</sub>O decomposition after Pt atoms doping. This work establishes a rational strategy for designing high-efficiency bifunctional electrocatalysts in overall water splitting under alkaline conditions.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236891"},"PeriodicalIF":8.1,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760566","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exploring the role of carbon binder domain morphology in enhancing the electrochemical performance of Li-ion battery
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1016/j.jpowsour.2025.236904
Wei Sun , Chun Huang
The electrochemical performance of Li-ion batteries (LIBs) is significantly influenced by electrode microstructure. The carbon and binder domain (CBD) plays an important role as it supports electronic conduction and maintains mechanical integrity. Despite its importance, the impact of CBD morphology on electrochemical performance remains poorly understood. One of the reasons is that CBD requires higher resolution to resolve the nanostructures, and techniques such as most X-ray computed tomography (XCT) machine cannot resolve CBD. This study establishes a workflow that incorporates active material (AM) particles obtained from XCT with numerically generated CBD morphology to build a 3D image-based and physics-resolved model to predict its electrochemical performance. Our model considers both explicit and implicit configurations of dense and nanoporous CBD during the electrochemical modelling process. Results indicate that the interface between AM and electrolyte significantly limits discharge capacity under explicit dense CBD configurations. In contrast, film-coating-like nanoporous CBD could enhance LIB longevity due to locally homogeneous lithiation in AM particles. Our findings also suggest that Li-ion transport is a major limitation in achieving higher (dis)charge rate capacities (5C) under implicit CBD considerations. This study highlights the crucial role of CBD morphology in optimising electrode design for improved battery performance.
锂离子电池(LIB)的电化学性能受电极微结构的影响很大。碳和粘结剂结构域(CBD)在支持电子传导和保持机械完整性方面发挥着重要作用。尽管 CBD 非常重要,但人们对其形态对电化学性能的影响仍然知之甚少。原因之一是 CBD 需要更高的分辨率来分辨纳米结构,而大多数 X 射线计算机断层扫描 (XCT) 设备等技术无法分辨 CBD。本研究建立了一个工作流程,将从 XCT 获得的活性材料 (AM) 颗粒与数值生成的 CBD 形态结合起来,建立一个基于三维图像和物理分辨的模型,以预测其电化学性能。在电化学建模过程中,我们的模型考虑了致密和纳米多孔 CBD 的显式和隐式配置。结果表明,在显式致密 CBD 配置下,AM 与电解质之间的界面极大地限制了放电容量。相比之下,薄膜涂层状的纳米多孔 CBD 可通过 AM 颗粒中局部均匀的锂化提高 LIB 的寿命。我们的研究结果还表明,锂离子传输是隐含 CBD 条件下实现更高(失)电率容量(5C)的主要限制因素。这项研究强调了 CBD 形态在优化电极设计以提高电池性能方面的关键作用。
{"title":"Exploring the role of carbon binder domain morphology in enhancing the electrochemical performance of Li-ion battery","authors":"Wei Sun ,&nbsp;Chun Huang","doi":"10.1016/j.jpowsour.2025.236904","DOIUrl":"10.1016/j.jpowsour.2025.236904","url":null,"abstract":"<div><div>The electrochemical performance of Li-ion batteries (LIBs) is significantly influenced by electrode microstructure. The carbon and binder domain (CBD) plays an important role as it supports electronic conduction and maintains mechanical integrity. Despite its importance, the impact of CBD morphology on electrochemical performance remains poorly understood. One of the reasons is that CBD requires higher resolution to resolve the nanostructures, and techniques such as most X-ray computed tomography (XCT) machine cannot resolve CBD. This study establishes a workflow that incorporates active material (AM) particles obtained from XCT with numerically generated CBD morphology to build a 3D image-based and physics-resolved model to predict its electrochemical performance. Our model considers both explicit and implicit configurations of dense and nanoporous CBD during the electrochemical modelling process. Results indicate that the interface between AM and electrolyte significantly limits discharge capacity under explicit dense CBD configurations. In contrast, film-coating-like nanoporous CBD could enhance LIB longevity due to locally homogeneous lithiation in AM particles. Our findings also suggest that Li-ion transport is a major limitation in achieving higher (dis)charge rate capacities (5C) under implicit CBD considerations. This study highlights the crucial role of CBD morphology in optimising electrode design for improved battery performance.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236904"},"PeriodicalIF":8.1,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759837","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chestnut shell-derived oxygen-rich porous carbon as a stable framework for dendrite-free Na metal anode
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1016/j.jpowsour.2025.236920
Xiaodong Sun , Wenlong Liu , Ning Zhang , Yehong Du , Jianzong Man , Juncai Sun
Metallic Na has a higher theoretical specific capacity (1165 mAh/g) and the lowest electrode potential (−2.71 vs. standard hydrogen electrode), which is conducive to the improvement of the energy density of Na secondary batteries. Nevertheless, dendrite growth and volume expansion caused by non-uniform Na deposition limit the development of Na metal anode. Here, the resource-rich and environmentally friendly chestnut shells are selected as the precursor, and oxygen-rich porous carbon is prepared by a one-step chemical activation method to solve the above issues. The high electronegativity of oxygen atom improves the polarity of the porous carbon, enhances the adsorption capacity of Na+, and reduces the Na nucleation barrier. Meanwhile, the massive polar sites facilitate the regulation of the distribution of Na+ on the carbon framework and directs uniform Na deposition. The porous structure increases the specific surface area, reduces the local current density and inhibits dendrite growth. The density functional theory calculations indicate that the oxygen-containing polar functional group (C=O, C-OH, and C-O-C) increases the binding energy to Na+. Thus, the full cell with Na3V2(PO4)3 cathode displays a high reversible capacity (88.6 mA h g−1) at 1C after 300 cycles. The results show that the application of chestnut shell-derived biocarbon materials on Na metal anode plays a positive role in achieving their commercialisation in battery systems.
{"title":"Chestnut shell-derived oxygen-rich porous carbon as a stable framework for dendrite-free Na metal anode","authors":"Xiaodong Sun ,&nbsp;Wenlong Liu ,&nbsp;Ning Zhang ,&nbsp;Yehong Du ,&nbsp;Jianzong Man ,&nbsp;Juncai Sun","doi":"10.1016/j.jpowsour.2025.236920","DOIUrl":"10.1016/j.jpowsour.2025.236920","url":null,"abstract":"<div><div>Metallic Na has a higher theoretical specific capacity (1165 mAh/g) and the lowest electrode potential (−2.71 vs. standard hydrogen electrode), which is conducive to the improvement of the energy density of Na secondary batteries. Nevertheless, dendrite growth and volume expansion caused by non-uniform Na deposition limit the development of Na metal anode. Here, the resource-rich and environmentally friendly chestnut shells are selected as the precursor, and oxygen-rich porous carbon is prepared by a one-step chemical activation method to solve the above issues. The high electronegativity of oxygen atom improves the polarity of the porous carbon, enhances the adsorption capacity of Na<sup>+</sup>, and reduces the Na nucleation barrier. Meanwhile, the massive polar sites facilitate the regulation of the distribution of Na<sup>+</sup> on the carbon framework and directs uniform Na deposition. The porous structure increases the specific surface area, reduces the local current density and inhibits dendrite growth. The density functional theory calculations indicate that the oxygen-containing polar functional group (C=O, C-OH, and C-O-C) increases the binding energy to Na<sup>+</sup>. Thus, the full cell with Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode displays a high reversible capacity (88.6 mA h g<sup>−1</sup>) at 1C after 300 cycles. The results show that the application of chestnut shell-derived biocarbon materials on Na metal anode plays a positive role in achieving their commercialisation in battery systems.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236920"},"PeriodicalIF":8.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143747004","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exploring nanoscale engineering for elevated electrochemical performance: A multiscale experimental and computational investigation of Co3O4@TiO2 nanocomposites
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1016/j.jpowsour.2025.236922
Bairi Sri Harisha , Bhargav Akkinepally , Jaesool Shim , Jiseok Lim
The novelty of this work lies in the utilization of Co3O4@TiO2 as a supercapacitor material, where Cobalt's abundance offers a sustainable and cost-effective source, while titanium's lightweight nature enhances the energy density. Together, this composite achieved an impressive power density of 4284 W kg−1 and energy density of 32.6 Wh·kg−1 at a current density of 1.7 A g−1, demonstrating its high-performance capabilities in energy storage application. The Co3O4@TiO2 composite was successfully prepared using a sequential process involving centrifugation, and calcination for Co3O4 nanopill synthesis, while TiO2 nanofibers were synthesized using a hydrothermal reaction followed by centrifugation and calcination. X-ray diffraction (XRD) analyses in conjunction with Scanning electron microscopy (SEM) detect the well-embedded Co3O4 nanopills, TiO2 nanofibers, and their phases within the composite structure. The composite achieves an exceptional specific capacitance of 555 F g−1 at 2 A g−1 and maintains 85.7 % capacitance retention at 10 A g−1 after 10,000 galvanostatic charge–discharge (GCD) cycles. Impedance spectroscopy results reveal that the composite exhibits great capacitive behavior, with a series resistance of 0.4 Ω. Furthermore, a Co3O4@TiO2 two-electrode arrangement demonstrates competent cyclic stability after 10,000 cycles. In addition, the Butler-Volmer numerical model is utilized in finite element modeling to simulate the potential distribution and concentration profiles of Co3O42+ and Co3O43+ ions within a one-dimensional (1-D) electrode-electrolyte configuration, facilitating the analysis of electron transfer kinetics.
{"title":"Exploring nanoscale engineering for elevated electrochemical performance: A multiscale experimental and computational investigation of Co3O4@TiO2 nanocomposites","authors":"Bairi Sri Harisha ,&nbsp;Bhargav Akkinepally ,&nbsp;Jaesool Shim ,&nbsp;Jiseok Lim","doi":"10.1016/j.jpowsour.2025.236922","DOIUrl":"10.1016/j.jpowsour.2025.236922","url":null,"abstract":"<div><div>The novelty of this work lies in the utilization of Co<sub>3</sub>O<sub>4</sub>@TiO<sub>2</sub> as a supercapacitor material, where Cobalt's abundance offers a sustainable and cost-effective source, while titanium's lightweight nature enhances the energy density. Together, this composite achieved an impressive power density of 4284 W kg<sup>−1</sup> and energy density of 32.6 Wh·kg<sup>−1</sup> at a current density of 1.7 A g<sup>−1</sup>, demonstrating its high-performance capabilities in energy storage application. The Co<sub>3</sub>O<sub>4</sub>@TiO<sub>2</sub> composite was successfully prepared using a sequential process involving centrifugation, and calcination for Co<sub>3</sub>O<sub>4</sub> nanopill synthesis, while TiO<sub>2</sub> nanofibers were synthesized using a hydrothermal reaction followed by centrifugation and calcination. X-ray diffraction (XRD) analyses in conjunction with Scanning electron microscopy (SEM) detect the well-embedded Co<sub>3</sub>O<sub>4</sub> nanopills, TiO<sub>2</sub> nanofibers, and their phases within the composite structure. The composite achieves an exceptional specific capacitance of 555 F g<sup>−1</sup> at 2 A g<sup>−1</sup> and maintains 85.7 % capacitance retention at 10 A g<sup>−1</sup> after 10,000 galvanostatic charge–discharge (GCD) cycles. Impedance spectroscopy results reveal that the composite exhibits great capacitive behavior, with a series resistance of 0.4 Ω. Furthermore, a Co<sub>3</sub>O<sub>4</sub>@TiO<sub>2</sub> two-electrode arrangement demonstrates competent cyclic stability after 10,000 cycles. In addition, the Butler-Volmer numerical model is utilized in finite element modeling to simulate the potential distribution and concentration profiles of Co<sub>3</sub>O<sub>4</sub><sup>2+</sup> and Co<sub>3</sub>O<sub>4</sub><sup>3+</sup> ions within a one-dimensional (1-D) electrode-electrolyte configuration, facilitating the analysis of electron transfer kinetics.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236922"},"PeriodicalIF":8.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143747568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Preparation of highly-crystalline large silicon nanoparticles for high-performance lithium-ion batteries in room temperature ionic liquid systems
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1016/j.jpowsour.2025.236926
Yanan Xu, Yu Zhang, Shiyue Zhang, Qing Hu, Hao Li, Wenkai Wang, Hongbin Du
The reported reaction systems employed for the synthesis of nano-silicon typically involve high temperatures, costly apparatus, meticulously controlled inert atmospheres, or highly reactive reducing agents. As a result, these factors inevitably lead to substantial energy expenditure, safety risks, and intricate operational procedures. Herein, an innovative approach is presented for the synthesis of large-size and highly-crystalline nano-Si through an ionic liquid reaction system. This unique room temperature ionic liquid system effectively facilitates the internal kinetic reactions and synthesizes large-size nano-Si with primary particle sizes ranging from 63 to 155 nm by varying the reaction temperature. Remarkably, when employed as the anode material in lithium-ion batteries, the resulting nano-Si-200 without the need for carbon coating and hydrofluoric acid etching treatment exhibits exceptional long-term cycling stability, with a superior capacity retention rate of 98.8 % at 0.5 A g−1 after 300 cycles. Moreover, the retention rate remains at 80.2 % while maintaining a specific capacity of 1097 mA h g−1 after 700 cycles at 2 A g−1, and persistently endures for 1000 cycles at 3 A g−1 with a specific capacity of 962 mA h g−1. This preparative system provides a new avenue for the synthesis of large nano-Si and holds promise for inspiring advancements of nano-Si in various fields.
{"title":"Preparation of highly-crystalline large silicon nanoparticles for high-performance lithium-ion batteries in room temperature ionic liquid systems","authors":"Yanan Xu,&nbsp;Yu Zhang,&nbsp;Shiyue Zhang,&nbsp;Qing Hu,&nbsp;Hao Li,&nbsp;Wenkai Wang,&nbsp;Hongbin Du","doi":"10.1016/j.jpowsour.2025.236926","DOIUrl":"10.1016/j.jpowsour.2025.236926","url":null,"abstract":"<div><div>The reported reaction systems employed for the synthesis of nano-silicon typically involve high temperatures, costly apparatus, meticulously controlled inert atmospheres, or highly reactive reducing agents. As a result, these factors inevitably lead to substantial energy expenditure, safety risks, and intricate operational procedures. Herein, an innovative approach is presented for the synthesis of large-size and highly-crystalline nano-Si through an ionic liquid reaction system. This unique room temperature ionic liquid system effectively facilitates the internal kinetic reactions and synthesizes large-size nano-Si with primary particle sizes ranging from 63 to 155 nm by varying the reaction temperature. Remarkably, when employed as the anode material in lithium-ion batteries, the resulting nano-Si-200 without the need for carbon coating and hydrofluoric acid etching treatment exhibits exceptional long-term cycling stability, with a superior capacity retention rate of 98.8 % at 0.5 A g<sup>−1</sup> after 300 cycles. Moreover, the retention rate remains at 80.2 % while maintaining a specific capacity of 1097 mA h g<sup>−1</sup> after 700 cycles at 2 A g<sup>−1</sup>, and persistently endures for 1000 cycles at 3 A g<sup>−1</sup> with a specific capacity of 962 mA h g<sup>−1</sup>. This preparative system provides a new avenue for the synthesis of large nano-Si and holds promise for inspiring advancements of nano-Si in various fields.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"641 ","pages":"Article 236926"},"PeriodicalIF":8.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143747002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Journal of Power Sources
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