Journal of Power Sources最新文献_第10页

A simplified measurement method for gas permeability in multilayer polymer electrolyte membranes 多层聚合物电解质膜透气性的一种简化测量方法

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-09 DOI: 10.1016/j.jpowsour.2026.239546

Norihiro Fukaya , Zulfi Al Rasyid Gautama , Takahisa Suzuki , Kazunari Sasaki , Masamichi Nishihara

Polymer electrolyte membranes (PEMs) play a crucial role in determining the performance and durability of polymer electrolyte membrane fuel cells (PEMFCs), particularly by regulating gas crossover and facilitating ion conduction. In this study, a simple measurement setup was developed using galvanic and semiconductor sensors to evaluate the oxygen and hydrogen permeabilities of multilayer PEMs under various humidity and temperature conditions. A sandwich-structured membrane (SSM), composed of a high-gas-barrier layer of poly(vinyl alcohol)/poly(vinyl sulfonic acid) (PVA/PVS) between two Nafion layers, was compared with a conventional Nafion membrane. The SSM exhibited reduced oxygen permeability and enhanced chemical durability by suppressing radical formation. Under identical conditions (90 °C, 30% relative humidity), oxygen permeability was reduced to approximately one-third that of the conventional Nafion membrane. However, under high humidity, the permeability increased owing to the swelling of the PVA/PVS interlayer. These findings emphasize the need to optimize the interlayer structure and polymer composition to address the challenges posed by humid operating conditions. The proposed measurement method provides a simple and practical approach for quantitatively evaluating gas transport in PEMs, thereby supporting the accelerated development of advanced membrane materials for PEMFC applications.

聚合物电解质膜（pemm）在聚合物电解质膜燃料电池（pemfc）的性能和耐久性方面起着至关重要的作用，特别是通过调节气体交叉和促进离子传导。在这项研究中，我们开发了一个简单的测量装置，使用电偶和半导体传感器来评估多层PEMs在不同湿度和温度条件下的氧和氢透性。在两层Nafion膜之间由聚乙烯醇/聚乙烯醇磺酸（PVA/PVS）的高阻气层组成的三明治结构膜（SSM）与传统的Nafion膜进行了比较。SSM通过抑制自由基的形成，降低了氧的渗透性，提高了化学耐久性。在相同的条件下（90°C， 30%相对湿度），氧透性降低到传统Nafion膜的三分之一左右。而在高湿条件下，由于PVA/PVS夹层膨胀，透气性增加。这些发现强调了优化层间结构和聚合物组成的必要性，以应对潮湿操作条件带来的挑战。所提出的测量方法为定量评估PEMFC中的气体输送提供了一种简单实用的方法，从而支持加速开发用于PEMFC应用的先进膜材料。

{"title":"A simplified measurement method for gas permeability in multilayer polymer electrolyte membranes","authors":"Norihiro Fukaya , Zulfi Al Rasyid Gautama , Takahisa Suzuki , Kazunari Sasaki , Masamichi Nishihara","doi":"10.1016/j.jpowsour.2026.239546","DOIUrl":"10.1016/j.jpowsour.2026.239546","url":null,"abstract":"<div><div>Polymer electrolyte membranes (PEMs) play a crucial role in determining the performance and durability of polymer electrolyte membrane fuel cells (PEMFCs), particularly by regulating gas crossover and facilitating ion conduction. In this study, a simple measurement setup was developed using galvanic and semiconductor sensors to evaluate the oxygen and hydrogen permeabilities of multilayer PEMs under various humidity and temperature conditions. A sandwich-structured membrane (SSM), composed of a high-gas-barrier layer of poly(vinyl alcohol)/poly(vinyl sulfonic acid) (PVA/PVS) between two Nafion layers, was compared with a conventional Nafion membrane. The SSM exhibited reduced oxygen permeability and enhanced chemical durability by suppressing radical formation. Under identical conditions (90 °C, 30% relative humidity), oxygen permeability was reduced to approximately one-third that of the conventional Nafion membrane. However, under high humidity, the permeability increased owing to the swelling of the PVA/PVS interlayer. These findings emphasize the need to optimize the interlayer structure and polymer composition to address the challenges posed by humid operating conditions. The proposed measurement method provides a simple and practical approach for quantitatively evaluating gas transport in PEMs, thereby supporting the accelerated development of advanced membrane materials for PEMFC applications.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239546"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186597","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

Electrochemical proton injection and spillover: A perspective on high-conductivity pathways in ceria-based and related oxides 电化学质子注入和溢出：铈基及相关氧化物的高导电性途径

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-12 DOI: 10.1016/j.jpowsour.2026.239613

Junjiao Li , Deqiang Meng , M.A.K. Yousaf Shah , Sajid Rauf , Naveed Mushtaq , Muhammad Imran , Fei Wang , Yuzheng Lu

Proton conduction in oxide materials is fundamental to the operation of advanced electrochemical energy devices such as proton ceramic fuel cells (PCFCs). Traditional understanding, dominated by hydration-based equilibrium models and the Grotthuss and Vehicle mechanisms, has long imposed a fundamental ceiling on achievable proton conductivity. This review highlights an emerging framework that complements static defect chemistry by emphasizing the critical role of dynamic, field-driven processes under operational conditions. We focus on the transformative mechanisms of Electrochemical Proton Injection (EPI) and Proton-Electron Spillover (PES), which operate under real device conditions.

EPI actively generates and injects protons at the anode via the hydrogen oxidation reaction, thereby bypassing the limitations of passive hydration. Concurrently, PES manifested as proton-coupled electron transfer (PCET), enables spatially decoupled yet redox-coupled transport, in which protons migrate along interfaces while electronic charge is balanced by redox-active species. Supported by advanced in situ characterization techniques, such as electrochemical impedance spectroscopy combined with the distribution of relaxation times (EIS-DRT), this framework demonstrates proton conductivities exceeding 0.1 S cm⁻¹ at lower temperatures (300–500 °C), shattering previously accepted limits. This perspective focuses on ceria-based fluorites and related perovskites as primary exemplars to critically analyze the EPI/PES framework, from which we distill general material parameters and explicit design principles for engineering interfacial proton transport in electrochemical devices.

氧化物材料中的质子传导是先进电化学能源装置如质子陶瓷燃料电池（pcfc）运行的基础。传统的理解，以水合平衡模型和Grotthuss和Vehicle机制为主导，长期以来对可实现的质子电导率设置了一个基本的上限。这篇综述强调了一个新兴的框架，通过强调动态的、现场驱动的过程在操作条件下的关键作用来补充静态缺陷化学。我们重点研究了在实际设备条件下运行的电化学质子注入（EPI）和质子-电子溢出（PES）的转化机制。EPI通过氢氧化反应在阳极主动生成和注入质子，从而绕过了被动水化的限制。同时，PES表现为质子耦合电子转移（PCET），实现空间解耦但氧化还原耦合的传输，其中质子沿界面迁移，而电子电荷由氧化还原活性物质平衡。在先进的原位表征技术的支持下，如电化学阻抗谱与弛豫时间分布（EIS-DRT）相结合，该框架证明了质子电导率在较低温度（300-500°C）下超过0.1 S cm−1，打破了之前公认的极限。这一视角聚焦于以铈基萤石和相关的钙钛矿为主要范例，批判性地分析EPI/PES框架，从中我们提炼出电化学器件中工程界面质子传输的一般材料参数和明确的设计原则。

{"title":"Electrochemical proton injection and spillover: A perspective on high-conductivity pathways in ceria-based and related oxides","authors":"Junjiao Li , Deqiang Meng , M.A.K. Yousaf Shah , Sajid Rauf , Naveed Mushtaq , Muhammad Imran , Fei Wang , Yuzheng Lu","doi":"10.1016/j.jpowsour.2026.239613","DOIUrl":"10.1016/j.jpowsour.2026.239613","url":null,"abstract":"<div><div>Proton conduction in oxide materials is fundamental to the operation of advanced electrochemical energy devices such as proton ceramic fuel cells (PCFCs). Traditional understanding, dominated by hydration-based equilibrium models and the Grotthuss and Vehicle mechanisms, has long imposed a fundamental ceiling on achievable proton conductivity. This review highlights an emerging framework that complements static defect chemistry by emphasizing the critical role of dynamic, field-driven processes under operational conditions. We focus on the transformative mechanisms of Electrochemical Proton Injection (EPI) and Proton-Electron Spillover (PES), which operate under real device conditions.</div><div>EPI actively generates and injects protons at the anode via the hydrogen oxidation reaction, thereby bypassing the limitations of passive hydration. Concurrently, PES manifested as proton-coupled electron transfer (PCET), enables spatially decoupled yet redox-coupled transport, in which protons migrate along interfaces while electronic charge is balanced by redox-active species. Supported by advanced in situ characterization techniques, such as electrochemical impedance spectroscopy combined with the distribution of relaxation times (EIS-DRT), this framework demonstrates proton conductivities exceeding 0.1 S cm<sup>−1</sup> at lower temperatures (300–500 °C), shattering previously accepted limits. This perspective focuses on ceria-based fluorites and related perovskites as primary exemplars to critically analyze the EPI/PES framework, from which we distill general material parameters and explicit design principles for engineering interfacial proton transport in electrochemical devices.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239613"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186600","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

Production scraps to raw materials: low-cost method for implementing lithium iron phosphate cathode scraps back to production lines 生产废渣为原料：采用低成本的方法实现磷酸铁锂正极废渣返回生产线

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-10 DOI: 10.1016/j.jpowsour.2026.239558

Lotta Liina Lassila , Martina Bruno , Carlotta Francia , Annukka Santasalo-Aarnio , Matteo Gandolfo , Silvia Fiore

In recent years, the increased production of lithium-ion batteries (LIBs) has been causing significant amounts of production scraps that require efficient, economical, and environmentally viable recycling methods. This study investigates strategies for integrating low-temperature direct recycling of lithium iron phosphate (LFP) production scraps into battery manufacturing. Scrap LFP cathode active material (CAM) was direct recycled at 200 °C in air and 400 °C in N₂. The recycled CAM was blended in different amounts (100, 50, 30%-wt) with commercial CAM. Two slurry compositions were considered based on CAM: polyvinylidene fluoride: carbon black ratios (80:10:10 and 92:5:3), and coin cells were manufactured and tested. Results indicate that recycled CAM can be directly reprocessed in new batteries exhibiting excellent electrochemical performance (154 mAh g⁻¹, equivalent to pristine material) when the slurry included 30%-wt CAM recycled at 200 °C in air and 100%-wt CAM recycled at 400 °C in N₂. Compared to virgin slurry material cost (9.06 €/kg_slurry) and environmental impact (8.27 kg CO₂/kg_slurry), incorporating 30%-wt CAM recycled at 200 °C in air reduced costs to 6.59 €/kg_Slurry and emissions to 6.21 kgCO₂/kg_slurry, and 100%-wt CAM recycled at 400 °C in N₂ corresponded to 3.77 €/kg_Slurry and 2.45 kgCO₂/kg_slurry. These findings clearly demonstrate that closed-loop integration of low-temperature direct recycling of LFP cathode scraps into cell manufacturing reduces material costs and environmental impact while maintaining high electrochemical performance.

近年来，锂离子电池（lib）产量的增加导致了大量的生产废料，需要高效、经济、环保的回收方法。本研究探讨了将磷酸铁锂（LFP）生产废料低温直接回收整合到电池制造中的策略。将废LFP阴极活性材料（CAM）在200℃空气和400℃N2中直接回收。将回收的CAM以不同的量（100、50、30%-wt）与商用CAM混合。基于CAM考虑了两种浆料组成：聚偏氟乙烯：炭黑比例（80:10:10和92:5:3），并制造了硬币电池并进行了测试。结果表明，当料浆中含有在200℃空气中回收的30%-wt的CAM和在400℃N2中回收的100%-wt的CAM时，回收的CAM可以直接用于新电池中，并具有优异的电化学性能（154 mAh g - 1，相当于原始材料）。与原浆材料成本（9.06欧元/千克浆）和环境影响（8.27千克二氧化碳/千克浆）相比，在200°C空气中回收30%重量的CAM，成本降至6.59欧元/千克浆，排放量降至6.21千克二氧化碳/千克浆，在400°C N2中回收100%重量的CAM，成本降至3.77欧元/千克浆，排放量降至2.45千克二氧化碳/千克浆。这些发现清楚地表明，将LFP阴极废料的低温直接回收集成到电池制造中可以降低材料成本和对环境的影响，同时保持较高的电化学性能。

{"title":"Production scraps to raw materials: low-cost method for implementing lithium iron phosphate cathode scraps back to production lines","authors":"Lotta Liina Lassila , Martina Bruno , Carlotta Francia , Annukka Santasalo-Aarnio , Matteo Gandolfo , Silvia Fiore","doi":"10.1016/j.jpowsour.2026.239558","DOIUrl":"10.1016/j.jpowsour.2026.239558","url":null,"abstract":"<div><div>In recent years, the increased production of lithium-ion batteries (LIBs) has been causing significant amounts of production scraps that require efficient, economical, and environmentally viable recycling methods. This study investigates strategies for integrating low-temperature direct recycling of lithium iron phosphate (LFP) production scraps into battery manufacturing. Scrap LFP cathode active material (CAM) was direct recycled at 200 °C in air and 400 °C in N<sub>2</sub>. The recycled CAM was blended in different amounts (100, 50, 30%-wt) with commercial CAM. Two slurry compositions were considered based on CAM: polyvinylidene fluoride: carbon black ratios (80:10:10 and 92:5:3), and coin cells were manufactured and tested. Results indicate that recycled CAM can be directly reprocessed in new batteries exhibiting excellent electrochemical performance (154 mAh g<sup>−1</sup>, equivalent to pristine material) when the slurry included 30%-wt CAM recycled at 200 °C in air and 100%-wt CAM recycled at 400 °C in N<sub>2</sub>. Compared to virgin slurry material cost (9.06 €/kg<sub>slurry</sub>) and environmental impact (8.27 kg CO<sub>2</sub>/kg<sub>slurry</sub>), incorporating 30%-wt CAM recycled at 200 °C in air reduced costs to 6.59 €/kg<sub>Slurry</sub> and emissions to 6.21 kgCO<sub>2</sub>/kg<sub>slurry</sub>, and 100%-wt CAM recycled at 400 °C in N<sub>2</sub> corresponded to 3.77 €/kg<sub>Slurry</sub> and 2.45 kgCO<sub>2</sub>/kg<sub>slurry</sub>. These findings clearly demonstrate that closed-loop integration of low-temperature direct recycling of LFP cathode scraps into cell manufacturing reduces material costs and environmental impact while maintaining high electrochemical performance.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239558"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186920","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

Enhancement of lithium-oxygen battery electrolytes using propylene oxide and its halides: Synergism between computations and experiments 使用环氧丙烷及其卤化物增强锂氧电池电解质：计算与实验之间的协同作用

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-11 DOI: 10.1016/j.jpowsour.2026.239581

Liwei Su , Kexin Cai , Lei Zhang , Hao Wu , Huan Chen , Lianbang Wang , Haifeng Lu

Currently, lithium-oxygen batteries (LOBs) suffer from unstable electrolytes, sluggish oxygen reaction kinetics, and lithium anode corrosion. This work systematically investigates propylene oxide and its halide additives, particularly epichlorohydrin (ECH), to modulate solid-liquid-gas interfaces and electrolyte properties. ECH enhances Li⁺ diffusion, alters Li-O reaction pathways, and suppresses Li dendrite growth. Batteries with ECH achieve an ultralow initial overpotential (∼0.2 V), a high discharge capacity of 11752 mAh g^-1, and over 40 cycles at a limited capacity of 1000 mAh g^-1. Combined DFT and experimental studies reveal that ECH regulates Li⁺ solvation, participates in forming a protective anode SEI layer, and leads to a new discharge product, ECH·LiO₂, reducing the initial overpotential to 0.16 V. This work reveals the synergistic mechanism of multifunctional electrolyte additives, offering a feasible path to achieve LOBs with long cycle life and high energy density.

目前，锂氧电池（lob）存在电解质不稳定、氧反应动力学缓慢以及锂阳极腐蚀等问题。本工作系统地研究了环氧丙烷及其卤化物添加剂，特别是环氧氯丙烷（ECH）对固液气界面和电解质性能的调节作用。ECH促进Li+扩散，改变Li- o反应途径，抑制Li枝晶生长。具有ECH的电池具有超低的初始过电位（~ 0.2 V）， 11752 mAh g-1的高放电容量，以及在1000 mAh g-1的有限容量下超过40次循环。结合DFT和实验研究发现，ECH调节Li+溶剂化，参与保护阳极SEI层的形成，产生新的放电产物ECH·LiO2，使初始过电位降至0.16 V。本研究揭示了多功能电解质添加剂的协同作用机理，为实现长循环寿命、高能量密度的lob提供了一条可行的途径。

{"title":"Enhancement of lithium-oxygen battery electrolytes using propylene oxide and its halides: Synergism between computations and experiments","authors":"Liwei Su , Kexin Cai , Lei Zhang , Hao Wu , Huan Chen , Lianbang Wang , Haifeng Lu","doi":"10.1016/j.jpowsour.2026.239581","DOIUrl":"10.1016/j.jpowsour.2026.239581","url":null,"abstract":"<div><div>Currently, lithium-oxygen batteries (LOBs) suffer from unstable electrolytes, sluggish oxygen reaction kinetics, and lithium anode corrosion. This work systematically investigates propylene oxide and its halide additives, particularly epichlorohydrin (ECH), to modulate solid-liquid-gas interfaces and electrolyte properties. ECH enhances Li<sup>+</sup> diffusion, alters Li-O reaction pathways, and suppresses Li dendrite growth. Batteries with ECH achieve an ultralow initial overpotential (∼0.2 V), a high discharge capacity of 11752 mAh g<sup>-1</sup>, and over 40 cycles at a limited capacity of 1000 mAh g<sup>-1</sup>. Combined DFT and experimental studies reveal that ECH regulates Li<sup>+</sup> solvation, participates in forming a protective anode SEI layer, and leads to a new discharge product, ECH·LiO<sub>2</sub>, reducing the initial overpotential to 0.16 V. This work reveals the synergistic mechanism of multifunctional electrolyte additives, offering a feasible path to achieve LOBs with long cycle life and high energy density.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239581"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186923","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

Silicon-doped MnFe layered double hydroxide electrocatalysts with M-O-Si bonding for stable methanol-to-formate conversion via surface reconstruction and bulk phase stability enhancement 掺硅MnFe层状双氢氧化物电催化剂的M-O-Si键合通过表面重构和体相稳定性增强实现甲醇到甲酸酯的稳定转化

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-12 DOI: 10.1016/j.jpowsour.2026.239612

Baohong Xie , Ying Tang , Pei Chen , Jing Xie , Yaxin Sun , Yunxia Zhao , Zhen Yang , Jingwen Pu , Qian Yang , Tiantian Wang , Lili Zhang , Feng Yu

The methanol oxidation reaction (MOR) provides a low-energy pathway for hydrogen production by replacing the anodic oxygen evolution reaction. However, the operational stability of non-precious metal catalysts is critically limited by metal leaching. Herein, we report that silicon doping effectively addresses this issue in a model MnFe-LDH catalyst. The optimized Si-MnFe-LDH/NF electrode requires potentials of only 1.347 and 1.419 V to achieve 10 and 100 mA cm⁻², respectively, representing a 57 and 78 mV reduction compared to the pristine, undoped counterpart. Most notably, it exhibits enhanced stability, maintaining operation for over 150 and 100 h at the current densities of 50 and 100 mA cm⁻², respectively, far exceeding the performance of the undoped catalyst. A combined experimental and theoretical study reveals that the formed M-O-Si (M = Mn, Fe) bonds are key to this improvement, serving a dual function: they effectively anchor Fe sites to suppress leaching and irreversible FeOOH formation, while kinetically enabling a stable, reversible surface reconstruction centered on MnOOH. In contrast, the undoped catalyst lacks this stabilization and undergoes severe structural degradation. Furthermore, this Si-induced dynamic stabilization synergistically optimizes the electronic structure of active sites, boosting both reaction kinetics and formate selectivity.

甲醇氧化反应（MOR）取代阳极析氧反应，提供了一种低能制氢途径。然而，金属浸出严重限制了非贵金属催化剂的运行稳定性。在此，我们报告了硅掺杂在MnFe-LDH催化剂模型中有效地解决了这一问题。优化后的Si-MnFe-LDH/NF电极仅需1.347和1.419 V的电位即可分别达到10和100 mA cm - 2，与未掺杂的原始电极相比，分别降低了57和78 mV。最值得注意的是，它表现出增强的稳定性，在50和100 mA cm−2的电流密度下分别保持超过150和100小时的运行，远远超过未掺杂催化剂的性能。一项结合实验和理论的研究表明，形成的M- o - si （M = Mn, Fe）键是这种改进的关键，具有双重功能：它们有效地锚定Fe位点，抑制浸出和不可逆的FeOOH形成，同时在动力学上实现以MnOOH为中心的稳定、可逆的表面重建。相反，未掺杂的催化剂缺乏这种稳定性，并且会经历严重的结构降解。此外，这种硅诱导的动态稳定协同优化了活性位点的电子结构，提高了反应动力学和甲酸盐选择性。

{"title":"Silicon-doped MnFe layered double hydroxide electrocatalysts with M-O-Si bonding for stable methanol-to-formate conversion via surface reconstruction and bulk phase stability enhancement","authors":"Baohong Xie , Ying Tang , Pei Chen , Jing Xie , Yaxin Sun , Yunxia Zhao , Zhen Yang , Jingwen Pu , Qian Yang , Tiantian Wang , Lili Zhang , Feng Yu","doi":"10.1016/j.jpowsour.2026.239612","DOIUrl":"10.1016/j.jpowsour.2026.239612","url":null,"abstract":"<div><div>The methanol oxidation reaction (MOR) provides a low-energy pathway for hydrogen production by replacing the anodic oxygen evolution reaction. However, the operational stability of non-precious metal catalysts is critically limited by metal leaching. Herein, we report that silicon doping effectively addresses this issue in a model MnFe-LDH catalyst. The optimized Si-MnFe-LDH/NF electrode requires potentials of only 1.347 and 1.419 V to achieve 10 and 100 mA cm<sup>−2</sup>, respectively, representing a 57 and 78 mV reduction compared to the pristine, undoped counterpart. Most notably, it exhibits enhanced stability, maintaining operation for over 150 and 100 h at the current densities of 50 and 100 mA cm<sup>−2</sup>, respectively, far exceeding the performance of the undoped catalyst. A combined experimental and theoretical study reveals that the formed M-O-Si (M = Mn, Fe) bonds are key to this improvement, serving a dual function: they effectively anchor Fe sites to suppress leaching and irreversible FeOOH formation, while kinetically enabling a stable, reversible surface reconstruction centered on MnOOH. In contrast, the undoped catalyst lacks this stabilization and undergoes severe structural degradation. Furthermore, this Si-induced dynamic stabilization synergistically optimizes the electronic structure of active sites, boosting both reaction kinetics and formate selectivity.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239612"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146187041","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

Density functional theory insights into quantum capacitance modulation in graphene quantum dots by geometry, defects and doping 密度泛函理论对石墨烯量子点中量子电容调制的几何、缺陷和掺杂的见解

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-11 DOI: 10.1016/j.jpowsour.2026.239550

Mahsa Abareghi, Beheshteh Sohrabi

This work investigates the quantum capacitance of graphene quantum dots (GQDs) using density functional theory, examining how size, edges, defects, dopants, and functional groups govern their electronic properties and quantum capacitance. Grounded in the fundamental definition of capacitance, we relate the density of states to the net charge accumulated, demonstrating that increasing GQD size narrows the energy gap. Zigzag edges have nonzero value capacitance at zero-bias, whereas armchair edges exhibit larger gaps and negligible capacitance at zero-bias, with appreciable values emerging only at higher voltages. Among rhombic geometries, zigzag and hybrid edges give rise to high zero-bias capacitances. Defects arising from electron–electron interactions enable earlier charge uptake and larger net charge at given potentials. n-type dopants reduce the gap and raise the Fermi level; p-type dopants have weaker, more localized effects; oxygen exerts a comparatively modest influence; and Si/Ge dopants decrease the gap with distinct patterns. Functional groups generally decrease the gap, with carboxyl (COOH) showing the smallest reduction. Collectively, these findings demonstrate that tuning GQD size, edge configuration, defect content, dopant type, and functionalization offers precise control over the quantum capacitance of graphene quantum dots, informing design strategies for nanoscale devices in energy storage and electrodes.

本研究利用密度泛函理论研究了石墨烯量子点（GQDs）的量子电容，研究了尺寸、边缘、缺陷、掺杂剂和官能团如何影响其电子特性和量子电容。根据电容的基本定义，我们将状态密度与累积的净电荷联系起来，表明GQD尺寸的增加缩小了能隙。锯齿形边缘在零偏压下具有非零值电容，而扶手椅边缘在零偏压下具有较大的间隙和可忽略的电容，只有在更高的电压下才会出现可观的值。在菱形几何中，锯齿形和混合边产生高的零偏置电容。电子-电子相互作用产生的缺陷使得在给定电位下更早的电荷吸收和更大的净电荷。n型掺杂物减小了间隙，提高了费米能级；p型掺杂剂的作用更弱、更局部；氧的影响相对较小；Si/Ge掺杂剂以不同的模式减小了间隙。官能团通常会减小间隙，羧基（COOH）的减小幅度最小。总的来说，这些发现表明，调整GQD尺寸、边缘配置、缺陷含量、掺杂类型和功能化可以精确控制石墨烯量子点的量子电容，为纳米级储能和电极器件的设计策略提供信息。

{"title":"Density functional theory insights into quantum capacitance modulation in graphene quantum dots by geometry, defects and doping","authors":"Mahsa Abareghi, Beheshteh Sohrabi","doi":"10.1016/j.jpowsour.2026.239550","DOIUrl":"10.1016/j.jpowsour.2026.239550","url":null,"abstract":"<div><div>This work investigates the quantum capacitance of graphene quantum dots (GQDs) using density functional theory, examining how size, edges, defects, dopants, and functional groups govern their electronic properties and quantum capacitance. Grounded in the fundamental definition of capacitance, we relate the density of states to the net charge accumulated, demonstrating that increasing GQD size narrows the energy gap. Zigzag edges have nonzero value capacitance at zero-bias, whereas armchair edges exhibit larger gaps and negligible capacitance at zero-bias, with appreciable values emerging only at higher voltages. Among rhombic geometries, zigzag and hybrid edges give rise to high zero-bias capacitances. Defects arising from electron–electron interactions enable earlier charge uptake and larger net charge at given potentials. n-type dopants reduce the gap and raise the Fermi level; p-type dopants have weaker, more localized effects; oxygen exerts a comparatively modest influence; and Si/Ge dopants decrease the gap with distinct patterns. Functional groups generally decrease the gap, with carboxyl (COOH) showing the smallest reduction. Collectively, these findings demonstrate that tuning GQD size, edge configuration, defect content, dopant type, and functionalization offers precise control over the quantum capacitance of graphene quantum dots, informing design strategies for nanoscale devices in energy storage and electrodes.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239550"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146187045","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

Assessments of thermal-runaway behaviors in a NCM811-based cylindrical lithium-ion battery 基于ncm811的圆柱形锂离子电池热失控行为的评估

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-07 DOI: 10.1016/j.jpowsour.2026.239555

Congbo Yin , Yanxin Zhang , Lei Sheng , Zhendong Zhang , Zhouxin Liao , Lei Feng

Excellent thermal safety management is pivotal for the safe operation of lithium-ion battery cells, especially the NCM 811-based cells with higher specific energy. This study proposes a quantitative framework to characterize the thermal runaway behavior of NCM811-based 21700 cylindrical cells under varying states of health (SOH) and states of charge (SOC). Key parameters, including onset time, temperature and voltage evolution, combustion behavior, TNT equivalence, and damage radius, are systematically evaluated. A reduction in SOH accelerates thermal runaway initiation, with the trigger time decreasing from 1730 s at 100% SOH to 608 s at 60% SOH, corresponding to an absolute reduction of 1122 s (64.8%). Concurrently, thermal runaway severity decreases with declining SOH, as evidenced by a reduction in mass loss ratio from 85.9% (100% SOH) to 45.9% (60% SOH). In contrast, SOC exhibits a strong positive correlation with thermal hazard at a given SOH. Specifically, the thermal runaway trigger time decreases from 1472 s at 25% SOC to 603 s at 100% SOC, corresponding to a 59.1% reduction. These results clarify the competing roles of aging and charge level in governing thermal runaway characteristics and provide quantitative guidance for the thermal safety design and risk mitigation of high-energy-density battery modules.

优秀的热安全管理对于锂离子电池的安全运行至关重要，特别是基于NCM 811的具有更高比能量的电池。本研究提出了一个定量框架来表征基于ncm811的21700圆柱形电池在不同健康状态（SOH）和充电状态（SOC）下的热失控行为。系统地评估了起爆时间、温度和电压演变、燃烧行为、TNT当量和损伤半径等关键参数。SOH的减少加速了热失控的发生，触发时间从100% SOH时的1730 s减少到60% SOH时的608 s，相当于绝对减少了1122 s（64.8%）。同时，热失控的严重程度随着SOH的降低而降低，质量损失率从85.9% （100% SOH）降至45.9% （60% SOH）。相反，在给定SOH下，SOC与热危害表现出强烈的正相关。具体来说，热失控触发时间从25%荷电状态下的1472秒减少到100%荷电状态下的603秒，减少了59.1%。这些结果阐明了老化和充电水平在控制热失控特性中的竞争作用，并为高能量密度电池模块的热安全设计和风险缓解提供了定量指导。

{"title":"Assessments of thermal-runaway behaviors in a NCM811-based cylindrical lithium-ion battery","authors":"Congbo Yin , Yanxin Zhang , Lei Sheng , Zhendong Zhang , Zhouxin Liao , Lei Feng","doi":"10.1016/j.jpowsour.2026.239555","DOIUrl":"10.1016/j.jpowsour.2026.239555","url":null,"abstract":"<div><div>Excellent thermal safety management is pivotal for the safe operation of lithium-ion battery cells, especially the NCM 811-based cells with higher specific energy. This study proposes a quantitative framework to characterize the thermal runaway behavior of NCM811-based 21700 cylindrical cells under varying states of health (SOH) and states of charge (SOC). Key parameters, including onset time, temperature and voltage evolution, combustion behavior, TNT equivalence, and damage radius, are systematically evaluated. A reduction in SOH accelerates thermal runaway initiation, with the trigger time decreasing from 1730 s at 100% SOH to 608 s at 60% SOH, corresponding to an absolute reduction of 1122 s (64.8%). Concurrently, thermal runaway severity decreases with declining SOH, as evidenced by a reduction in mass loss ratio from 85.9% (100% SOH) to 45.9% (60% SOH). In contrast, SOC exhibits a strong positive correlation with thermal hazard at a given SOH. Specifically, the thermal runaway trigger time decreases from 1472 s at 25% SOC to 603 s at 100% SOC, corresponding to a 59.1% reduction. These results clarify the competing roles of aging and charge level in governing thermal runaway characteristics and provide quantitative guidance for the thermal safety design and risk mitigation of high-energy-density battery modules.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239555"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135644","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

The effect of applied voltage on the behavior of Ni- gadolinium-doped ceria cathodes in SOECs using 2D comb-shaped patterned cells 外加电压对二维梳状电池中掺杂Ni-钆的铈阴极性能的影响

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-08 DOI: 10.1016/j.jpowsour.2026.239473

Xiaolin Shao , Riyan Achmad Budiman , Mina Yamaguchi , Hitoshi Takamura , Keiji Yashiro , Tatsuya Kawada

Solid oxide electrolysis cells (SOECs), which are used for steam or co-electrolysis of H₂O and CO₂, are a promising clean energy technology. For commercialization, it is essential to understand long-term degradation mechanisms. To address the complexity of the porous structure of commercial cells and the associated challenges, this study employs a two-dimensional comb-shaped patterned cell. These patterned electrodes reproduce the cross-sectional geometry of conventional cells while avoiding the complexity of porous microstructures. In this configuration, Ni metal was applied as the cathode, and electrolysis experiments were conducted under various applied voltages. The results indicate that the effect of applied voltage on delamination is nonlinear, as the delamination sites vary with voltage. At −0.22 V, slight delamination occurred at the tips of the Ni stripes; at −0.47 V delamination became more pronounced. At the higher voltage of −0.94 V, the Ni tips adhere more strongly to the substrate and GDC shows a pronounced tendency to diffuse onto the Ni surface, while delamination initiates from the center of the cathode. These results demonstrate that the interaction between Ni and GDC is strongly dependent on the applied voltage, providing insights into optimized operating strategies.

固体氧化物电解电池（SOECs）是一种很有前途的清洁能源技术，用于蒸汽或H2O和CO2的共电解。为了商业化，必须了解长期的降解机制。为了解决商业电池多孔结构的复杂性和相关的挑战，本研究采用了一个二维梳状图案电池。这些有图案的电极再现了传统电池的横截面几何形状，同时避免了多孔微结构的复杂性。在该配置中，以Ni金属为阴极，在不同的外加电压下进行电解实验。结果表明，施加电压对分层的影响是非线性的，分层位置随电压的变化而变化。在−0.22 V时，Ni条纹的尖端出现了轻微的分层；−0.47 V时分层更加明显。在−0.94 V的高电压下，Ni尖端与衬底的粘附更强，GDC向Ni表面扩散的趋势明显，而脱层则从阴极中心开始。这些结果表明，Ni和GDC之间的相互作用强烈依赖于施加的电压，为优化操作策略提供了见解。

{"title":"The effect of applied voltage on the behavior of Ni- gadolinium-doped ceria cathodes in SOECs using 2D comb-shaped patterned cells","authors":"Xiaolin Shao , Riyan Achmad Budiman , Mina Yamaguchi , Hitoshi Takamura , Keiji Yashiro , Tatsuya Kawada","doi":"10.1016/j.jpowsour.2026.239473","DOIUrl":"10.1016/j.jpowsour.2026.239473","url":null,"abstract":"<div><div>Solid oxide electrolysis cells (SOECs), which are used for steam or co-electrolysis of H<sub>2</sub>O and CO<sub>2</sub>, are a promising clean energy technology. For commercialization, it is essential to understand long-term degradation mechanisms. To address the complexity of the porous structure of commercial cells and the associated challenges, this study employs a two-dimensional comb-shaped patterned cell. These patterned electrodes reproduce the cross-sectional geometry of conventional cells while avoiding the complexity of porous microstructures. In this configuration, Ni metal was applied as the cathode, and electrolysis experiments were conducted under various applied voltages. The results indicate that the effect of applied voltage on delamination is nonlinear, as the delamination sites vary with voltage. At −0.22 V, slight delamination occurred at the tips of the Ni stripes; at −0.47 V delamination became more pronounced. At the higher voltage of −0.94 V, the Ni tips adhere more strongly to the substrate and GDC shows a pronounced tendency to diffuse onto the Ni surface, while delamination initiates from the center of the cathode. These results demonstrate that the interaction between Ni and GDC is strongly dependent on the applied voltage, providing insights into optimized operating strategies.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239473"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135646","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

Low-barrier electrochemical urea-assisted energy-saving hydrogen production based on interface and structural engineering of hollow/porous NiP2/ZnP2/Sn nanoboxes 基于中空/多孔NiP2/ZnP2/Sn纳米盒界面和结构工程的低势垒电化学尿素辅助节能制氢

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-10 DOI: 10.1016/j.jpowsour.2026.239591

Mohana Heidary, Hadi Hosseini

Urea-assisted water splitting that includes hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) can produce high pure hydrogen and clean urea-rich wastewater, nonetheless the lack of effective design of highly active and economical multifunctional electrocatalysts hampers its application. Here, we introduce a novel hollow/porous NiP₂/ZnP₂/Sn nanoboxes by a facile precipitation method coupled with a simple ion exchange process and phosphorization step for the robust electrocatalytic HER and UOR processes. The specific porous hollow structure of NiP₂/ZnP₂/Sn boxes with large and abundant amount of edge active sites, improved electron/mass transportation, and modulated electronic structure offer superior electrocatalytic performance with bifunctional activities for both HER and UOR processes, with only 69 mV to achieve 10 mA cm⁻² for HER and 60 mV to reach 10 mA cm⁻² toward UOR with desirable long-term stability during 24 h. Moreover, the fabricated overall urea splitting systems based on NiP₂/ZnP₂/Sn as both cathode and anode electrodes, show very low cell voltages of 1.37 V to achieve 10 mA cm⁻², making it one of the most efficient catalysts toward overall urea splitting. This effective strategy for fabricating hollow/porous metal-based boxes offers a new avenue for designing high performance catalysts in environmental and sustainable energy utilization.

包括析氢反应（HER）和尿素氧化反应（UOR）在内的尿素辅助水分解反应可以产生高纯氢气和清洁的富尿素废水，但缺乏高效、经济的多功能电催化剂的有效设计阻碍了其应用。在这里，我们介绍了一种新型的中空/多孔NiP2/ZnP2/Sn纳米盒，该纳米盒采用易沉淀法结合简单的离子交换过程和磷酸化步骤，用于稳健的电催化HER和UOR工艺。特定的多孔中空结构的NiP2/ZnP2/Sn盒具有大量的边缘活性位点，改进的电子/质量传输和调制的电子结构，为HER和UOR过程提供了优越的电催化性能和双功能活性，HER仅需69 mV即可达到10 mA cm - 2， UOR仅需60 mV即可达到10 mA cm - 2，并且在24 h内具有理想的长期稳定性。制备的以NiP2/ZnP2/Sn为正极和负极的整体尿素分解体系，电池电压仅为1.37 V，达到10 mA cm−2，是最有效的整体尿素分解催化剂之一。这种有效的制造中空/多孔金属基盒子的策略为设计环境和可持续能源利用的高性能催化剂提供了新的途径。

{"title":"Low-barrier electrochemical urea-assisted energy-saving hydrogen production based on interface and structural engineering of hollow/porous NiP2/ZnP2/Sn nanoboxes","authors":"Mohana Heidary, Hadi Hosseini","doi":"10.1016/j.jpowsour.2026.239591","DOIUrl":"10.1016/j.jpowsour.2026.239591","url":null,"abstract":"<div><div>Urea-assisted water splitting that includes hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) can produce high pure hydrogen and clean urea-rich wastewater, nonetheless the lack of effective design of highly active and economical multifunctional electrocatalysts hampers its application. Here, we introduce a novel hollow/porous NiP<sub>2</sub>/ZnP<sub>2</sub>/Sn nanoboxes by a facile precipitation method coupled with a simple ion exchange process and phosphorization step for the robust electrocatalytic HER and UOR processes. The specific porous hollow structure of NiP<sub>2</sub>/ZnP<sub>2</sub>/Sn boxes with large and abundant amount of edge active sites, improved electron/mass transportation, and modulated electronic structure offer superior electrocatalytic performance with bifunctional activities for both HER and UOR processes, with only 69 mV to achieve 10 mA cm<sup>−2</sup> for HER and 60 mV to reach 10 mA cm<sup>−2</sup> toward UOR with desirable long-term stability during 24 h. Moreover, the fabricated overall urea splitting systems based on NiP<sub>2</sub>/ZnP<sub>2</sub>/Sn as both cathode and anode electrodes, show very low cell voltages of 1.37 V to achieve 10 mA cm<sup>−2</sup>, making it one of the most efficient catalysts toward overall urea splitting. This effective strategy for fabricating hollow/porous metal-based boxes offers a new avenue for designing high performance catalysts in environmental and sustainable energy utilization.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239591"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186591","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

From density functional theory to machine learning: Emerging paradigms in energy materials discovery 从密度泛函理论到机器学习：能源材料发现中的新兴范式

IF 7.9 2区工程技术 Q1 CHEMISTRY, PHYSICAL

Journal of Power Sources

Pub Date : 2026-04-15 Epub Date: 2026-02-13 DOI: 10.1016/j.jpowsour.2026.239478

M.V. Jyothirmai , Shrish Nath Upadhyay , S. Muthu Krishnan , Sudipta Roy , Jayant K. Singh

Sustainable and efficient energy conversion technologies are driving significant progress in electrocatalysis, which is a crucial pathway for developing selective and high-performance catalytic materials. Density functional theory (DFT) provides a fundamental framework for understanding catalytic activity by offering quantitative insights into adsorption energetics, reaction pathways, and electronic structure-property relationships at the atomic scale. The review highlights atomic-level design strategies such as doping, defect engineering, heterostructure formation, and single-atom catalysis, which have introduced new pathways for enhancing catalytic performance by modulating active site geometry and electronic structure. We discuss dynamic simulation techniques such as ab initio molecular dynamics (AIMD), kinetic Monte Carlo (KMC), and machine learning potentials (MLP), which enhance the ability to incorporate finite-temperature effects, solvent dynamics, and reaction timescales into catalytic studies. In parallel, ML frameworks have emerged as powerful tools for high-throughput screening, property prediction, and inverse design, utilizing high-quality datasets and advanced descriptors to efficiently identify promising candidates. Through the combination of electronic structure theory and ML tools, we establish an integrated pipeline for identifying catalytic materials with improved activity and durability. We also highlight future directions, including generative models for inverse design, active learning to enable autonomous discovery, multiscale simulation strategies, and the development of physics-informed neural networks that embed domain-specific knowledge.

可持续和高效的能量转换技术正在推动电催化的重大进展，这是开发选择性和高性能催化材料的重要途径。密度泛函理论（DFT）通过在原子尺度上对吸附能量学、反应途径和电子结构-性质关系提供定量的见解，为理解催化活性提供了一个基本框架。本文重点介绍了掺杂、缺陷工程、异质结构形成和单原子催化等原子级设计策略，这些策略为通过调节活性位点几何形状和电子结构来提高催化性能提供了新的途径。我们讨论了动态模拟技术，如从头算分子动力学（AIMD）、动力学蒙特卡罗（KMC）和机器学习势（MLP），这些技术增强了将有限温度效应、溶剂动力学和反应时间尺度纳入催化研究的能力。与此同时，机器学习框架已经成为高通量筛选、属性预测和逆向设计的强大工具，利用高质量的数据集和高级描述符有效地识别有前途的候选对象。通过电子结构理论和机器学习工具的结合，我们建立了一个完整的管道来识别具有更高活性和耐久性的催化材料。我们还强调了未来的方向，包括逆向设计的生成模型，实现自主发现的主动学习，多尺度模拟策略，以及嵌入特定领域知识的物理信息神经网络的发展。

{"title":"From density functional theory to machine learning: Emerging paradigms in energy materials discovery","authors":"M.V. Jyothirmai , Shrish Nath Upadhyay , S. Muthu Krishnan , Sudipta Roy , Jayant K. Singh","doi":"10.1016/j.jpowsour.2026.239478","DOIUrl":"10.1016/j.jpowsour.2026.239478","url":null,"abstract":"<div><div>Sustainable and efficient energy conversion technologies are driving significant progress in electrocatalysis, which is a crucial pathway for developing selective and high-performance catalytic materials. Density functional theory (DFT) provides a fundamental framework for understanding catalytic activity by offering quantitative insights into adsorption energetics, reaction pathways, and electronic structure-property relationships at the atomic scale. The review highlights atomic-level design strategies such as doping, defect engineering, heterostructure formation, and single-atom catalysis, which have introduced new pathways for enhancing catalytic performance by modulating active site geometry and electronic structure. We discuss dynamic simulation techniques such as ab initio molecular dynamics (AIMD), kinetic Monte Carlo (KMC), and machine learning potentials (MLP), which enhance the ability to incorporate finite-temperature effects, solvent dynamics, and reaction timescales into catalytic studies. In parallel, ML frameworks have emerged as powerful tools for high-throughput screening, property prediction, and inverse design, utilizing high-quality datasets and advanced descriptors to efficiently identify promising candidates. Through the combination of electronic structure theory and ML tools, we establish an integrated pipeline for identifying catalytic materials with improved activity and durability. We also highlight future directions, including generative models for inverse design, active learning to enable autonomous discovery, multiscale simulation strategies, and the development of physics-informed neural networks that embed domain-specific knowledge.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"671 ","pages":"Article 239478"},"PeriodicalIF":7.9,"publicationDate":"2026-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186593","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