Jiahao He, Yang Zhou, Shibo Wu, Jingrui Cao, Bin Han, Zhiqiang Wang, Zaizai Tong, Muslum Demir, Pianpian Ma
{"title":"Unlocking the Capacity and Stability Limitations of Perovskite Electrodes and Achieving the Design of a Flame-Retardant Supercapacitor Through the “Tree Canopy” Structure","authors":"Jiahao He, Yang Zhou, Shibo Wu, Jingrui Cao, Bin Han, Zhiqiang Wang, Zaizai Tong, Muslum Demir, Pianpian Ma","doi":"10.1021/acsenergylett.5c00154","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00154","url":null,"abstract":"The present study depicts innovative electrode and electrolyte designs to achieve advanced supercapacitor performance and stability. The mechanism of how the electronic structure of substitution ions impacts the phase structure and properties of SrCoO<sub>3−δ</sub> was in-depth elucidated, overcoming the inherent trade-off between specific capacity and cycle stability in perovskite materials. The as-prepared SrCo<sub>0.925</sub>Sc<sub>0.075</sub>O<sub>3−δ</sub> electrode achieves a high capacity of 467.7 C g<sup>–1</sup> (129.92 mAh g<sup>–1</sup>) at 1 A g<sup>–1</sup>, with retention of 97.4% of its initial capacity after 10,000 cycles. Inspired by canopy structures, a “branch”-like dual-network 3D gel system was created and in situ integrated with the electrode as the “trunk”. This unique structure offers robust mechanical strength and flame retardancy, establishing an efficient conductive network. Devices featuring this design show electrochemical stability and flexibility, ensuring safe operation at extreme temperatures while balancing the stability and energy density. This research opens avenues for high-performance supercapacitors and quasi-solid-state gel batteries tailored applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619053","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Energy Letters Pub Date : 2025-03-14DOI: 10.1021/acsenergylett.5c0063110.1021/acsenergylett.5c00631
Prashant V. Kamat*,
{"title":"Correlation, Causation and Comparison","authors":"Prashant V. Kamat*, ","doi":"10.1021/acsenergylett.5c0063110.1021/acsenergylett.5c00631","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00631https://doi.org/10.1021/acsenergylett.5c00631","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1540–1541 1540–1541"},"PeriodicalIF":19.3,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609087","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Eva Schlautmann, Janina Drews, Lukas Ketter, Martin A. Lange, Timo Danner, Arnulf Latz, Wolfgang G. Zeier
{"title":"Graded Cathode Design for Enhanced Performance of Sulfide-Based Solid-State Batteries","authors":"Eva Schlautmann, Janina Drews, Lukas Ketter, Martin A. Lange, Timo Danner, Arnulf Latz, Wolfgang G. Zeier","doi":"10.1021/acsenergylett.4c03243","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03243","url":null,"abstract":"Solid-state batteries present a promising technology to overcome the energy density limitations of lithium-ion batteries. However, achieving a high areal loading in cathodes without introducing significant transport limitations remains a key challenge, particularly in thick electrodes. In this work, we study the impact of a three-layer graded cathode design on the performance of a LiNi<sub>0.83</sub>Co<sub>0.11</sub>Mn<sub>0.06</sub>O<sub>2</sub> (NCM83)/Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) composite cathode using a combination of experiments and microstructure-resolved simulations. An increased LPSCl content at the separator and higher NCM83 content toward the current collector improve effective charge transport, resulting in better rate performance and reduced overpotentials at high current densities. This comprehensive experimental and theoretical study demonstrates that the optimization of cathode design has the potential to significantly enhance the performance of solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Fluorine-Free Electrolytes for Lithium Metal Batteries: Challenges and Opportunities in Solvation Structure and Interphase Design","authors":"Sapna L. Ramesh, Jeffrey Lopez","doi":"10.1021/acsenergylett.5c00319","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00319","url":null,"abstract":"Electrolyte design has emerged as a key strategy to overcome performance and safety challenges in lithium metal batteries. In this Perspective, we examine the recent movement toward fluorinated electrolyte solvents for high performance lithium metal batteries. We highlight the state-of-the-art understanding of the role of fluorine in modifying solvent properties and influencing electrolyte reactivity and further discuss the role of fluorinated species in the interphases at both the anode and cathode. In light of risks associated with per- and polyfluoroalkyl substances (PFAS), we propose that a deeper understanding of the role of fluorine in electrolytes and interphases is essential to eventually design fluorine-free molecules for high performance batteries and discuss areas for further research.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"89 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hyunseok Moon, Myeong-Hwa Ryou, Anseong Park, Bo-Quan Li, Ha Neul Kim, Namjun Park, Eunbyoul Lee, Kyung Yoon Chung, Jia-Qi Huang, Taeeun Yim, Won Bo Lee, Sang-Young Lee
{"title":"Promoting Granular Lithium Sulfide Growth by Soft Acidic–Hard Basic Ionomer Binder for Lithium–Sulfur Batteries","authors":"Hyunseok Moon, Myeong-Hwa Ryou, Anseong Park, Bo-Quan Li, Ha Neul Kim, Namjun Park, Eunbyoul Lee, Kyung Yoon Chung, Jia-Qi Huang, Taeeun Yim, Won Bo Lee, Sang-Young Lee","doi":"10.1021/acsenergylett.4c03522","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03522","url":null,"abstract":"Electrode passivation limits the reversibility of lithium–sulfur (Li–S) batteries. Pivoting from the prevailing approaches that focus on electrode active materials and electrolytes, herein, we introduce a class of S electrode binders based on soft acidic–hard basic (SAHB) ionomers. The SAHB binder contains a soft cation (tetraallyl ammonium ion, TA<sup>+</sup>) paired with a hard counteranion (nitrate, NO<sub>3</sub><sup>–</sup>), allowing matched interactions with Li polysulfides (LiPS) via soft acid–soft base (TA<sup>+</sup>–S<sub><i>x</i></sub><sup>2–</sup>) and hard base–hard acid (NO<sub>3</sub><sup>–</sup>–Li<sup>+</sup>) pairings. This intermolecular coupling retards LiPS diffusion, promoting three-dimensional granular Li sulfide (Li<sub>2</sub>S) growth, guided by a high Damköhler number (<i>Da</i>). Consequently, the SAHB binder enables a Li–S cell to achieve a high specific capacity of 1545 mAh g<sub>sulfur</sub><sup>–1</sup> (corresponding to 92.3% S utilization) and stable capacity retention (71.5% after 300 cycles at a current density of 1 C), outperforming previously reported S electrode binders.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"42 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143619056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sanghwi Han, Sayantan Sasmal, Meikun Shen, Yifan Wu, Olivia T. Vulpin, Shujin Hou, Sungjun Kim, Jang Yong Lee, Jeyong Yoon, Shannon W. Boettcher
{"title":"Advancing SnO2-Based Water Dissociation Catalysis in Bipolar-Membrane Water Electrolyzers","authors":"Sanghwi Han, Sayantan Sasmal, Meikun Shen, Yifan Wu, Olivia T. Vulpin, Shujin Hou, Sungjun Kim, Jang Yong Lee, Jeyong Yoon, Shannon W. Boettcher","doi":"10.1021/acsenergylett.5c00309","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00309","url":null,"abstract":"Advancing water dissociation (WD) catalysis is important for bipolar membrane (BPM) technology for energy-conversion systems. We report a one-step strategy for synthesizing SnO<sub>2</sub>-based WD catalysts directly on a cation-conducting membrane, which is straightforward, fast, and scalable, while exhibiting record-high WD performance. Electrochemical and material analyses show that the thickness and heterogeneity of the SnO<sub>2</sub> layer are the primary factors governing ionic transport in the SnO<sub>2</sub> WD catalyst layer and influencing WD performance. At optimal deposition conditions, the SnO<sub>2</sub>-catalyzed BPM electrolyzer has a low total cell voltage at 1 A cm<sup>–2</sup> of 1.93 V and a WD overpotential (<i>η</i><sub>wd</sub>) of 41 ± 7 mV. These performance metrics were maintained across various 1.5 cm × 1.5 cm sections upon the fabrication of a 100 cm<sup>2</sup> BPM. This BPM electrolyzer, operating with pure-water feed in a membrane-electrode-assembly architecture, was durable, with a degradation rate of 0.5 mV h<sup>–1</sup> over 100 h at 1.0 A cm<sup>–2</sup> and the <i>η</i><sub>wd</sub> increase of 0.27 mV h<sup>–1</sup>.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"135 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanzeng Ge, Baoquan Liu, Daoxiong Wu, Yu Zhang, Si Tang, Haizhen Jiang, Jing Li, Hui Zhang, Xinlong Tian, Jinlin Yang
{"title":"Layered Organic Molecular Crystal with One-Dimensional Ion Migration Channel for Durable Magnesium-Based Dual-Ion Batteries","authors":"Yanzeng Ge, Baoquan Liu, Daoxiong Wu, Yu Zhang, Si Tang, Haizhen Jiang, Jing Li, Hui Zhang, Xinlong Tian, Jinlin Yang","doi":"10.1021/acsenergylett.5c00139","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00139","url":null,"abstract":"Mg-based dual-ion batteries (DIBs) represent promising battery technologies for next-generation sustainable energy storage; however, their advancement is strongly hindered by sluggish Mg<sup>2+</sup> diffusion and structural instability of anode materials. Herein, fast and reversible storage of Mg<sup>2+</sup> in nonaqueous and aqueous electrolyte is shown for a layered organic crystal, 5,7,12,14-pentacenetetrone (PT). The enolization redox chemistry of PT and its weakly stacked layered structure with rich 1D molecular channels promote Mg<sup>2+</sup> storage kinetics, providing a high diffusion coefficient on the order of 10<sup>–8</sup>–10<sup>–9</sup> cm<sup>2</sup> S<sup>–1</sup>. As expected, the nonaqueous Mg-DIBs exhibit a reversible capacity of 95 mAh g<sup>–1</sup> at 0.1 A g<sup>–1</sup>, wide-temperature operating capability (−20 to 50 °C), and good cycling stability over 2000 cycles. Interestingly, the applicability of PT as Mg<sup>2+</sup>-hosting materials extends to aqueous systems, enabling the construction of high-safety aqueous Mg-DIBs. This study provides crucial insights into the structural design of organic molecular crystal for multivalent ion-based DIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"56 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599556","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shijia Li, Xue Chen, Jingwen Zhao, Yibing Zhang, Kai Zhang, Kai Wang, Jiasen Shen, Peng Lv, Yu Jia, Ying Bai
{"title":"In Situ Construction of Organic–Inorganic Hybrid Interfacial Films via Electrolyte Additive for Advanced Aqueous Zinc-Ion Batteries","authors":"Shijia Li, Xue Chen, Jingwen Zhao, Yibing Zhang, Kai Zhang, Kai Wang, Jiasen Shen, Peng Lv, Yu Jia, Ying Bai","doi":"10.1021/acsenergylett.4c02684","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02684","url":null,"abstract":"Aqueous zinc ion batteries have garnered widespread attention due to their high safety, cost-effectiveness, and environmental friendliness. However, hydrogen precipitation, byproduct aggregation, and dendrite growth at zinc anode as well as material degradation of the cathode severely impede further practical development. Here, we construct organic–inorganic hybrid interfacial films on electrodes by employing trifluoroacetamide (CNF) as an additive. The interfacial films homogenize zinc deposition, inhibit the byproducts’ aggregation as well as hydrogen evolution on the anode, and enhance cathode morphological integrity upon cycling. The cycle life of Zn||Zn cells is significantly extended at a high current density. Meanwhile, a Coulombic efficiency of 99.9% is achieved at 10 mA cm<sup>–2</sup> after 4000 cycles for Zn||Cu cell. The Zn||Na<sub>2</sub>V<sub>6</sub>O<sub>16</sub>·3H<sub>2</sub>O full cells after 12000 cycles present 145 and 99 mAh g<sup>–1</sup> at 5 and 20 A g<sup>–1</sup>, respectively. Therefore, the efficient and convenient strategy of introducing an electrolyte additive provides a reliable solution to issues at the interfaces for other secondary battery systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608361","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nadesh Fiuza-Maneiro, Junzhi Ye, Shilendra Kumar Sharma, Sudip Chakraborty, Sergio Gómez-Graña, Robert L. Z. Hoye, Lakshminarayana Polavarapu
{"title":"Unlocking Brightness in CsPbCl3 Perovskite Nanocrystals: Screening Ligands and Metal Halides for Effective Deep Trap Passivation","authors":"Nadesh Fiuza-Maneiro, Junzhi Ye, Shilendra Kumar Sharma, Sudip Chakraborty, Sergio Gómez-Graña, Robert L. Z. Hoye, Lakshminarayana Polavarapu","doi":"10.1021/acsenergylett.5c00185","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00185","url":null,"abstract":"Despite the significant advances made in achieving green (CsPbBr<sub>3</sub>)- and red (CsPbI<sub>3</sub>)-emitting halide perovskite nanocrystals (NCs) with high quantum yields and colloidal stability through surface engineering, obtaining bright violet/blue-emitting CsPbCl<sub>3</sub> NCs with long-term stability is still a grand challenge due to their defect sensitivity. In this work, we have screened the surface passivation of CsPbCl<sub>3</sub> NCs using ligands with different functional groups (amine, sulfonic, and phosphonic acid) and metal halides (mono- and bivalent) with the aim of improving the emission yield and stability of CsPbCl<sub>3</sub> NCs. This enabled us to find that phosphonic acids are the ligands that showed the highest efficiency as they occupy Cl vacancies and covalently bind to the Pb on the surface of NCs, together with the incorporation of bivalent metal chlorides that showed substantial enhancements in PLQY. Consequently, the most effective passivators were those that passivate Cl vacancies, indicating these to be among the most detrimental traps. This is further validated through Density Functional Theory (DFT), suggesting that the trend in adsorption energies is as follows: hexylphosphonic < hexylsulfonic < oleylamine < tetrabutyl ammonium, which is also coherent with the charge transfer mechanism and corresponding electronic structure of the halide perovskite surface with the ligands. Furthermore, after evaluating different passivation strategies, we identified <i>in situ</i> passivation as the most effective method for obtaining highly luminescent CsPbCl<sub>3</sub> NCs that exhibit stability for over 6 months. Thus, this work is expected to guide the perovskite NC researchers to choose effective passivating agents and passivation strategies toward bright blue luminescent colloidal halide perovskites and beyond.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kun-Hee Ko, Hyeokjun Park, Jaesang Yoon, Seok Hyun Song, Eugene Choi, Sungjae Seo, Jaesub Kwon, Sunyoung Lee, Jaehoon Heo, Sangwook Han, Jooha Park, Wonju Kim, Yong-Tae Kim, Jongwoo Lim, Yun Seog Lee, Hyungsub Kim, Kisuk Kang
{"title":"Multiscale Defect Regulation of Cobalt-Free Layered Oxides for High-Energy and Long-Lasting Cathodes","authors":"Kun-Hee Ko, Hyeokjun Park, Jaesang Yoon, Seok Hyun Song, Eugene Choi, Sungjae Seo, Jaesub Kwon, Sunyoung Lee, Jaehoon Heo, Sangwook Han, Jooha Park, Wonju Kim, Yong-Tae Kim, Jongwoo Lim, Yun Seog Lee, Hyungsub Kim, Kisuk Kang","doi":"10.1021/acsenergylett.5c00207","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00207","url":null,"abstract":"Reducing the reliance on cobalt in electrode chemistry is a promising step toward more sustainable and cost-effective lithium-ion batteries. However, the elimination of cobalt in layered oxides generally results in a significant decrease in capacity and/or a compromised cycle stability. Herein, we show that these intertwined issues of the cobaltless systems can be remedied by meticulously tailoring inherent defects induced at multiscale. It is demonstrated that a simple excess incorporation of lithium in the structure can effectively reduce the cation disorder and unexpectedly alter the microstructure forming routes, thereby enhancing electro-chemo-mechanical stabilities of layered cathodes. Our investigations reveal that this surplus lithium facilitates topotactic lithiation of precursors during calcination, rendering mechanically robust particles with fewer nanoporous defects and reduced cation disorder. Defect-regulated cobalt-free layered oxides successfully deliver a reversible capacity of 189 mAh g<sup>–1</sup> at 0.5C with a retention of ∼85% after 300 cycles under commercial-level electrode loading.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"54 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}