EES batteries最新文献

{"title":"A multiscale X-ray CT study of degradation and safety behaviour of different Li-ion battery positive electrode morphologies.","authors":"Hamish T Reid, Drasti Patel, Will J Dawson, James B Robinson, Rhodri Jervis, Paul R Shearing","doi":"10.1039/d6eb00099a","DOIUrl":"10.1039/d6eb00099a","url":null,"abstract":"<p><p>While battery thermal failures are rare, improving our understanding of battery state-of-safety is essential to further reduce failure rates and support the energy transition. Although batteries undergo rigorous certification, the evolution of safety characteristics with cell ageing remains poorly understood. Here, electrochemical testing accelerating rate calorimetry (ARC), and multiscale X-ray computed tomography (CT) are combined to investigate how state-of-safety of lithium-ion pouch cells containing single-crystal or polycrystalline NMC cathode evolves with cycling. Comparable pouch cells were assessed before and after cycling to 80% capacity retention. The single-crystal containing cells gave an approximate 50% improvement in cycle life compared with polycrystalline cells. In the pristine state, ARC showed that the single-crystal cells had a lower self-heating onset temperature but also a lower peak temperature than polycrystalline cells, indicating lower thermal stability but less destructive failure. After cycling, the single-crystal cells showed higher self-heating onset temperature and lower peak temperatures. In contrast, the polycrystalline cells showed reduced self-heating onset temperatures and thermal runaway initiation temperatures indicating a loss of thermal stability. Multiscale X-ray CT provided mechanistic insight into these changes by linking safety behaviour to degradation across multiple length scales. Whole-cell imaging revealed greater gas generation, electrode displacement, and loss of layer contact in the polycrystalline cells, while high-resolution CT identified extensive particle cracking and fragmentation that was largely absent in the single-crystal material. These observations suggest that ageing-induced particle fracture increases the reactive cathode-electrolyte interfacial area, accelerating exothermic reactions during thermal abuse and reducing thermal stability. This work demonstrates how multiscale X-ray CT can reveal the mechanisms that influence the changes in of battery state-of-safety with cycling and highlights the potential safety advantages of single-crystal cathode architectures in aged lithium-ion batteries.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13576674/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148979135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Revalidating KCrPDTA for aqueous redox flow batteries.","authors":"Graham Kimbell, Qirui Liu, Jeonghoon Ahn, Lina Camenisch, Rohat Celik, Talia Echeverria, Baban Deep Virk, Corsin Battaglia, David Reber","doi":"10.1039/d6eb00156d","DOIUrl":"10.1039/d6eb00156d","url":null,"abstract":"<p><p>Inconsistent reporting practices and single-cell performance claims complicate the comparison of redox flow battery electrolytes across laboratories. Reproducing reported performance metrics for KCrPDTA-based batteries proved challenging, motivating systematic revalidation of KCrPDTA synthesis and characterization, and testing in cells. We identify three compounding variability sources: (i) hydration state inconsistencies in isolated KCrPDTA introducing molar mass errors of up to 4% that propagate into state-of-charge calculations, (ii) impurities eliminated by selective KCrPDTA crystal isolation prior to complete evaporation of the reaction mixture, and (iii) cell assembly artefacts including membrane shorting which produces persistently low coulombic efficiencies unrelated to electrolyte properties. Using a standardized protocol across 22 fuel-cell-type KCrPDTA-K₄[Fe(CN)₆] cells, assembled by multiple operators using various material batches, we obtain reproducible average coulombic and energy efficiencies of 99.54 ± 0.08% and 86.3 ± 1.7% over 50 cycles to 80% nominal state-of-charge at 100 mA cm^-2, values that are statistically grounded in a way single-cell studies are not. Across four cell architectures, coulombic efficiency stays within 99.3 to 99.7% while energy efficiency ranges from roughly 80 to 89%, highlighting the impact of cell hardware on key performance metrics. To support transparent benchmarking, we share all underlying data in a machine-readable format with semantically annotated linked metadata, alongside an open-source analysis pipeline and a metadata reporting template.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13583517/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148993416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"To tether or not to tether? The merits of adding functionality to Li-O₂ cell redox mediators.","authors":"Thukshan Samarakoon, Alex R Neale, Elliot Coulbeck, Daniel J Saccomando, Tyler Petek, Laurence J Hardwick","doi":"10.1039/d6eb00134c","DOIUrl":"10.1039/d6eb00134c","url":null,"abstract":"<p><p>The cycle life of lithium-oxygen (Li-O₂) cells is limited by the continual degradation of cell components by both potential-independent and high overpotential-induced parasitic reactions. Extending cell cycle life requires (i) driving electrochemical reactions at low overpotentials with high selectivity, (ii) stabilising the Li|electrolyte interface and (iii) mitigating reactive oxygen species (ROS)-induced electrolyte/electrode degradation. Charge redox mediators (RMs) present a promising strategy to facilitate low overpotential oxidation of Li₂O₂. By covalently linking or \"tethering\" the RM to motifs that can enhance cell discharge, quench ROS, and/or stabilise the Li|electrolyte interface, a single multifunctional species can be realised to improve cell lifetime. In this work, a series of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-tethered RMs based on ionic liquids/salts is reported. The effect of these additives on discharge capacities and cell cyclability was explored systematically in Li-O₂ cells. The tethered RMs gave superior performance relative to TEMPO when using Li_1-<i>x</i> FePO₄ as the counter electrode. Improved performance in Li metal-based cells with the tethered RMs was attained by substitution of the bis(trifluoromethanesulfonyl)imide ([TFSI]^-) anion of the RM with nitrate ([NO₃]^-), resulting in an exceptionally high Li₂O₂ yield close to 100% on discharge, almost 15% greater than for the analogous [TFSI]^--containing tethered RM. A marker for cell/RM failure was identified with <i>operando</i> gas evolution measurements to track charge mediation losses by the tethered RMs. Furthermore, degradation reactions with Li metal and superoxide, where superoxide-induced decomposition occurs at the TEMPO moiety, were identified as key RM degradation pathways, and the major bottleneck to achieving high cycling performance was established.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"1703-1720"},"PeriodicalIF":0.0,"publicationDate":"2026-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13551449/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148914791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Understanding the reactivity of copper current collectors in lithium batteries - an <i>operando</i> XAS study.","authors":"M A Koronfel, A Omirkhan, H Yadegari, D Thornton, W Xue, J S Zhang, L Guo, J Nelson Weker, J F W Mosselemans, M Kulzick, I E L Stephens, M P Ryan","doi":"10.1039/d6eb00072j","DOIUrl":"10.1039/d6eb00072j","url":null,"abstract":"<p><p>Copper is used as the anode current collector in lithium-ion batteries, as well as the electrode itself in other types of lithium batteries. It is nominally a stable material in the organic electrolytes under normal battery operating potentials. Copper dissolution in lithium battery electrolytes has been extensively shown to occur at potentials attainable only in over-discharge conditions. However, in this work, copper dissolution is shown to occur even under normal cycling conditions, contrary to thermodynamic prediction. Utilising the high chemical sensitivity of X-ray absorption spectroscopy, copper oxidation state and concentration are quantified <i>in operando</i>. The results raise concerns about the impact of copper on battery efficiency, lifetime and safety, along with resulting implications on battery cycling.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"1668-1677"},"PeriodicalIF":0.0,"publicationDate":"2026-08-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13556142/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148922516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Radiolysis study on PVDF binder - how does it affect the X-ray photoelectron spectroscopy characterisation of phospho-olivine electrodes?","authors":"Yuhan Liu, Prajna Bhatt, Will J Dawson, Alice Llewellyn, Joshua Dickerson, Robert Palgrave, Anna Regoutz, James Robinson, Rhodri Jervis","doi":"10.1039/d6eb00103c","DOIUrl":"https://doi.org/10.1039/d6eb00103c","url":null,"abstract":"<p><p>The reliability of surface characterisation in battery research is often compromised by the diagnostic techniques, which can induce unintended chemical changes during measurement. This is a particular concern for polyvinylidene fluoride (PVDF), which is a standard polymer binder used to maintain the structural integrity of battery electrodes. Such degradation creates measurement artefacts that can be easily mistaken for genuine electrochemical behaviour. This study utilizes X-ray photoelectron spectroscopy and kinetic modelling to investigate the X-ray-induced radiolysis of the PVDF binder. In addition, by comparing the behaviour of pure LiMn _<i>x</i> Fe_1-<i>x</i> PO₄ powder to electrodes cast with PVDF, we demonstrate that the presence of the active material fundamentally alters how the binder decomposes, which triggers a consistent reduction of Fe oxidation states across all electrodes post-exposure. Specifically, the degradation is PVDF-concentration-dependent. The 2 wt% PVDF electrode displays a more rapid overall formation of LiF on the surface than the 10 wt% PVDF electrode, which shows an accelerated initial fluorine loss but a stabilised LiF content after 5 hours. These findings provide essential guidelines for interpreting spectroscopic data of battery electrodes, enabling researchers to properly distinguish measurement-induced artefacts from genuine electrochemical phenomena.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":"2 5","pages":"1657-1667"},"PeriodicalIF":0.0,"publicationDate":"2026-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13655890/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149187703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Towards a courageous EU policy for recycling spent lithium-ion batteries: rethinking dismantling, standardization, and responsibility.","authors":"Alessandra Zanoletti, Alberto Mannu, Gavin D J Harper, Elza Bontempi","doi":"10.1039/d6eb00060f","DOIUrl":"https://doi.org/10.1039/d6eb00060f","url":null,"abstract":"<p><p>The rapid expansion of electric mobility across Europe is generating, and is expected to generate, unprecedented volumes of end-of-life lithium-ion batteries (LIBs), exposing structural weaknesses in the European Union's regulatory and industrial framework for battery recycling. We have crossed the point at which electric vehicles, for the first time, have out-sold petrol vehicles in Europe. Recent EU initiatives, including the Batteries Regulation, introduce significant advances, including carbon footprint reporting, mandatory recycled content, digital battery passports, sustainability and circularity requirements, and stronger extended producer responsibility. The heterogeneity of battery designs is widely recognized as a key constraint affecting dismantling efficiency, automation feasibility, and material recovery outcomes. These design issues directly impede automation, depress material recovery yields, and undermine the EU's circular economy and industrial sovereignty objectives. Drawing on assertive industrial policies, this paper argues that the EU should adopt a bolder stance. It proposes the introduction of harmonised design-for-disassembly requirements for all batteries placed on the EU internal market, alongside a reform of Extended Producer Responsibility and waste classification to recognise spent batteries as strategic secondary raw materials. It also calls for the development of publicly supported robotised dismantling hubs. The paper argues that the main limitation of current EU battery policy lies not only in downstream recycling performance, but more fundamentally in the absence of binding upstream design requirements that determine whether dismantling, and therefore high-quality recycling, can be technically and economically achieved.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":"2 5","pages":"1459-1467"},"PeriodicalIF":0.0,"publicationDate":"2026-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13655885/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149186810","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemical variability of natural mineral mixtures as electrode materials in Li-ion batteries.","authors":"John Donald Morley, Kathryn Hadler, Chandramohan George, Pablo R Brito-Parada","doi":"10.1039/d6eb00037a","DOIUrl":"https://doi.org/10.1039/d6eb00037a","url":null,"abstract":"<p><p>Natural mineral systems can be effectively used to make battery material supply chains more secure and sustainable. However, the impact of their multi-mineral electrochemistry must be considered for effective deployment. Mine tailings are shown as a potential sustainable natural mineral source. A simplified ternary system of pyrite, quartz and muscovite was examined for its trends in electrochemical performance. Mixing of minerals is shown to adversely affect charge transfer impedance (<i>R</i> _ct) and diffusion coefficient (<i>D</i> _Li⁺ ) values post-cycling; <i>R</i> _ct values are 10 times greater for mixtures than pure phase minerals, and <i>D</i> _Li⁺ values are an order of magnitude lower than pure phase minerals. Within mixtures, the component of capacity from pyrite decays more rapidly than in a pure mineral phase. A comparison with two mine tailings reveals the inclusion of lesser amounts of pyrite in a majority silicate mixture to boost electrochemical performance, while the opposite leads to reduced performance. The results convey that a clear link between mineral composition and expected electrochemical performance is required to fully realise the benefits of mixed natural mineral sources for sustainable battery electrodes.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":"2 5","pages":"1592-1607"},"PeriodicalIF":0.0,"publicationDate":"2026-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13655888/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149187748","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The behaviour of phenothiazines as catholytes in aqueous-organic redox flow batteries.","authors":"Nadia L Farag, Kieran Mylrea, Dominic Hey, Kawarpal Singh, Dominic S Wright, Clare P Grey","doi":"10.1039/d5eb00223k","DOIUrl":"10.1039/d5eb00223k","url":null,"abstract":"<p><p>A series of commercially available phenothiazine dyes was explored for their application in aqueous organic redox flow batteries. Of the dyes explored, Azure-A was found to have the most promising cycling performance and highest solubility, which was improved further with the use of nicotinamide as a 'hydrotrope' additive, which improved both solubility and cycle life. However, it was found that only ∼50% of theoretical capacity expected for Azure-A redox could be reached, regardless of cycling conditions. Through <i>in situ</i> and <i>ex situ</i> NMR, UV/vis and EPR spectroscopy as well as battery cycling using low-concentrations of the dye, this was ascribed to dimerisation of the redox-active species, which takes place at concentrations greater than 10 mM. Because of this, Azure-A is, in effect, only capable of a net 1e^- redox process under practical conditions. By combining novel electrochemical impedance spectroscopy processing methods (including distribution of relaxation times and general phase element analysis) with symmetric cell cycling, a degradation mechanism involving polymerisation and passivation of the electrode is proposed as one source of the decrease in capacity with cycling.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"1330-1342"},"PeriodicalIF":0.0,"publicationDate":"2026-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13312259/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148355373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrode surface engineering with electrolyte additives, improving reversibility of magnesium metal anode batteries.","authors":"Muath Radi, Deyana S Tchitchekova, Alexandre Ponrouch, Rémi Dedryvère","doi":"10.1039/d6eb00065g","DOIUrl":"10.1039/d6eb00065g","url":null,"abstract":"<p><p>Rechargeable magnesium batteries (RMBs) are promising energy storage systems because of magnesium's high volumetric capacity and abundance. However, RMBs' advancement has been hindered by the lack of suitable electrolytes that combine high oxidative stability and electrode compatibility. In this study, we investigate the effects of three mechanistically different additives, namely, boron trifluoride diethyl etherate (BF₃·O(C₂H₅)₂), iodine (I₂), and boron triiodide (BI₃), in an Mg(TFSI)₂/DME:DG electrolyte on magnesium plating and stripping kinetics, voltage hysteresis, coulombic efficiency, and the composition and thickness of the electrode interphase. BI₃ demonstrates the greatest beneficial effect among these additives by forming a thin (<5 nm) interphase, rich in iodide and boron species, that enhances the coulombic efficiency (from <60 to 80-90%), reduces voltage hysteresis (from 2000 mV to 250-350 mV), and improves Mg plating/stripping kinetics. Electrochemical tests against Mo₆S₈ cathodes demonstrate that substrate choice also affects performance: Mo₆S₈ supported on stainless steel yields stable cycling with full capacity retention, whereas titanium exhibits poor adhesion of the cathode composite material. Compared to state-of-the-art Mg[B(HFIP)₄]₂ electrolytes, Mg(TFSI)₂/DME:DG + BI₃ offers a simpler, more scalable, and practical route with engineered interphase chemistry, though further studies are needed to match the outstanding performance of Mg[B(HFIP)₄]₂ and to fully understand the Mg(TFSI)₂/DME:DG + BI₃ bulk electrolyte properties. This work provides key insights for designing improved-performance RMBs <i>via</i> innovative interphase engineering and electrolyte formulation.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"1353-1367"},"PeriodicalIF":0.0,"publicationDate":"2026-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13321050/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148379498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A fluorine-free electrolyte for calcium metal batteries.","authors":"Andrii Kachmar, Robert Markowski, Taniya Purkait, Darsi Rambabu, Petru Apostol, Da Tie, Roy Heyns, Jan Fransaer, Koen Binnemans, Alexandre Ponrouch, Alexandru Vlad","doi":"10.1039/d5eb00162e","DOIUrl":"10.1039/d5eb00162e","url":null,"abstract":"<p><p>Calcium metal batteries (CMBs) have emerged as a promising alternative to lithium(Li)-based technologies due to calcium's (Ca) low reduction potential, high volumetric capacity, and abundance. However, challenges such as poor Ca²⁺ transport across passivation layers and limited electrolyte compatibility hinder practical implementation. Here, we report a fluorine-free electrolyte formulation based on calcium bis(methanesulfonimide) (Ca(MSI)₂) in dimethylacetamide (DMAc). This system offers a safer, more sustainable, and environmentally benign alternative to conventional fluorinated electrolytes. Comparative physicochemical and electrochemical evaluations with the benchmark Ca(TFSI)₂/DMAc electrolyte reveal that Ca(MSI)₂ enables stable calcium plating/stripping over 1600 hours with lower overpotential and improved rate performance. In fact, spectroscopic analyses confirm the formation of a more uniform, fluorine-free interphase that supports better Ca²⁺ transport throughout the passivation layer. These findings highlight the potential of fluorine-free salts for enabling reversible room temperature calcium metal cycling and advance the development of safer, high-performance multivalent batteries.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"138-146"},"PeriodicalIF":0.0,"publicationDate":"2025-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12679347/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145703789","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}