EES batteriesPub Date : 2025-04-11eCollection Date: 2025-06-09DOI: 10.1039/d5eb00050e
Jihoon Oh, Yeeun Sohn, Jang Wook Choi
{"title":"High-performance anode-less all-solid-state batteries enabled by multisite nucleation and an elastic network.","authors":"Jihoon Oh, Yeeun Sohn, Jang Wook Choi","doi":"10.1039/d5eb00050e","DOIUrl":"10.1039/d5eb00050e","url":null,"abstract":"<p><p>Anode-less all-solid-state batteries (ALASSBs) represent a promising energy storage platform for various upcoming green mobility applications, as they offer superior energy density, manufacturing feasibility, and enhanced safety. However, their practical implementation is hindered by the formation of heterogeneous lithium (Li) deposits during repeated cycling, particularly at ambient temperatures. In this study, we introduce a novel multi-seed strategy that integrates strategically distributed nucleation sites with a highly elastic and adhesive polymer matrix. The incorporation of multiple lithiophilic metallic seeds with a range of lithiation potentials promotes uniform Li deposition by facilitating diversified lithiation pathways. Simultaneously, the elastic polymer network enables stress dissipation across the protection layer, thereby effectively mitigating mechanical degradation. Even at room temperature (25 °C), the resulting anode-less full-cell retained 70% of its capacity after 100 cycles at a current density of 0.5C (1C = 2 mA cm<sup>-2</sup>). This study conveys a useful design principle for protective layers in ALASSBs: the advantageous synergistic effect created by combining multiple lithiophilic seeds with enlarged nucleation pathways and a stress-releasing elastic binder.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"566-575"},"PeriodicalIF":0.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12004216/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144045599","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}
EES batteriesPub Date : 2025-04-02eCollection Date: 2025-06-09DOI: 10.1039/d5eb00058k
Jeremy P Lowen, Teresa Insinna, Tharigopala V Beatriceveena, Mark P Stockham, Bo Dong, Sarah J Day, Clare P Grey, Emma Kendrick, Peter R Slater, Paul A Anderson, Joshua W Makepeace
{"title":"Probing the electrochemical behaviour of lithium imide as an electrolyte for solid-state batteries.","authors":"Jeremy P Lowen, Teresa Insinna, Tharigopala V Beatriceveena, Mark P Stockham, Bo Dong, Sarah J Day, Clare P Grey, Emma Kendrick, Peter R Slater, Paul A Anderson, Joshua W Makepeace","doi":"10.1039/d5eb00058k","DOIUrl":"10.1039/d5eb00058k","url":null,"abstract":"<p><p>All-solid-state batteries utilising a Li-metal anode have long promised to be the next-generation of high-performance energy storage device, with a step-change in energy density, cycling stability and cell safety touted as potential advantages compared to conventional Li-ion battery cells. A key to enabling this technology is the development of solid-state electrolytes with the elusive combination of high ionic conductivity, wide electrochemical stability and the ability to form a conductive and stable interface with Li metal. Presently, oxide and sulfide-based materials, particularly garnet and argyrodite-type structures, have proved most promising for this application. However, these still suffer from a number of challenges, including resistive lithium metal interfaces, poor lithium dendrite suppression (at high current density) and low voltage stability. Here we report the first application of lithium imide, an antifluorite-structured material, as a solid electrolyte in a Li-metal battery. Low-temperature synthesis of lithium imide produces promising Li-ion conductivity, reaching >1 mS cm<sup>-1</sup> at 30 °C using a modest post-synthetic mechanochemical treatment, as well as displaying at least 5 V stability <i>vs.</i> Li<sup>+</sup>/Li. <i>In situ</i> electrochemical operation of lithium imide with Li-metal electrodes reveals an apparent 1000-fold increase in its measured conductivity, whilst appearing to remain an electronic insulator. It is postulated that stoichiometry variation at the grain boundary may contribute to this conductivity improvement. Furthermore, the material is shown to possess impressive resistance to hard shorting under high current density conditions (70 mA cm<sup>-2</sup>) as well as the ability to operate in Li-metal battery cells. These results not only highlight the promising performance of lithium imide, but also its potential to be the basis for a new family of antifluorite based solid electrolytes.</p>","PeriodicalId":520508,"journal":{"name":"EES batteries","volume":" ","pages":"527-540"},"PeriodicalIF":0.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12001454/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144036111","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}