Hyunji Kweon , Jungmin Kang , Bonyoung Ku , Sunha Hwang , Jinho Ahn , Lahyeon Jang , Myungeun Choi , Sang-Yeop Lee , Jihoe Lee , Hoseok Lee , Hun-Gi Jung , Jang-Yeon Hwang , Hee-Dae Lim , Jongsoon Kim
{"title":"Enhancing power capability and fast discharge behavior in P2-type K layered cathodes through structural stabilization via introducing Li-ions into TM layers","authors":"Hyunji Kweon , Jungmin Kang , Bonyoung Ku , Sunha Hwang , Jinho Ahn , Lahyeon Jang , Myungeun Choi , Sang-Yeop Lee , Jihoe Lee , Hoseok Lee , Hun-Gi Jung , Jang-Yeon Hwang , Hee-Dae Lim , Jongsoon Kim","doi":"10.1016/j.jechem.2025.06.019","DOIUrl":"10.1016/j.jechem.2025.06.019","url":null,"abstract":"<div><div>Mn-based layered oxides are widely recognized as cathode materials for potassium-ion batteries (KIBs) due to their high specific capacity derived from their low molar mass. However, the structural instability caused by the Jahn-Teller effect of Mn<sup>3+</sup> and the large ionic radius of K<sup>+</sup> results in poor electrochemical performance. Herein, we propose an effective structural stabilization strategy for P2-type Mn-based layered oxide cathodes of KIBs through Li-incorporation into the transition metal layer. Using the first-principles calculations and experiments, we demonstrate that the P2-K<sub>0.48</sub>[Li<sub>0.1</sub>Mn<sub>0.9</sub>]O<sub>2</sub> (P2-KLMO) delivers improved electrochemical performance, specific capacity and average discharge voltage of ∼124.4 mA h g<sup>−1</sup> and ∼2.7 V (vs. K<sup>+</sup>/K) at 0.05C (1C = 260 mA g<sup>−1</sup>), outperforming P2-K<sub>0.5</sub>MnO<sub>2</sub>. <em>Operando</em> X-ray diffraction analysis confirms the P2-OP4 phase transition and Mn<sup>3+</sup>-induced Jahn-Teller distortion are significantly suppressed in P2-KLMO. These improvements are attributed to the lithium introduction into transition metal layers, leading to strengthened structural stability and enhanced K<sup>+</sup> diffusion kinetics. Moreover, synthetic accessibility through the conventional solid-state method provides an additional advantage for practical application of Li-incorporated Mn-based P2-type cathodes in KIBs. We believe our study offers a simple yet effective strategy for designing high-performance and practical cathode materials for KIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 820-829"},"PeriodicalIF":13.1,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xinyu Zhang , Wenxin Li , Meihan Sun , Meng Wu , Fanfan Liu , Dan Zhou
{"title":"Rational design of MXene@VS4 heterostructures via interfacial coupling for advanced magnesium-ion batteries","authors":"Xinyu Zhang , Wenxin Li , Meihan Sun , Meng Wu , Fanfan Liu , Dan Zhou","doi":"10.1016/j.jechem.2025.06.011","DOIUrl":"10.1016/j.jechem.2025.06.011","url":null,"abstract":"<div><div>Rechargeable magnesium batteries (RMBs) have garnered significant attention in energy storage applications due to their high capacity, low cost, and high safety. However, the strong polarization effect and slow kinetic de-intercalation of Mg<sup>2+</sup> in the cathode limit their commercial application. This study presents a novel interface-coupled V<sub>2</sub>CT<em><sub>x</sub></em>@VS<sub>4</sub> heterostructure through a one-step hydrothermal process. In this architecture, V<sub>2</sub>CT<em><sub>x</sub></em> and VS<sub>4</sub> can mutually support their structural framework, which effectively prevents the structural collapse of V<sub>2</sub>CT<em><sub>x</sub></em> MXene and the aggregation of VS<sub>4</sub>. Crucially, interfacial coupling between V<sub>2</sub>CT<em><sub>x</sub></em> and VS<sub>4</sub> induces strong V–S bonds, substantially enhancing structural stability. Benefiting from these advantages, the heterostructure exhibits high specific capacity (226 mAh g<sup>−1</sup> at 100 mA g<sup>−1</sup>) and excellent long-cycle stability (89% capacity retention after 1000 cycles at 500 mA g<sup>−1</sup>). Furthermore, the Mg<sup>2+</sup> storage mechanism in the V<sub>2</sub>CT<em><sub>x</sub></em>@VS<sub>4</sub> composite was elucidated through a series of ex-situ characterizations. This work provides a feasible strategy for designing V<sub>2</sub>CT<em><sub>x</sub></em> MXene-based cathodes with high capacity and extended cyclability for RMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 566-575"},"PeriodicalIF":13.1,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144365044","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mingdan Wang , Qianyu Zhang , Kun Chen , Cong Lin , Huigang Wang , Yanying Zhao , Pengzuo Chen
{"title":"Atomic vacancy engineering of Co(OH)F nanoarray toward high-performance ammonia electrosynthesis with waste plastics upgrading","authors":"Mingdan Wang , Qianyu Zhang , Kun Chen , Cong Lin , Huigang Wang , Yanying Zhao , Pengzuo Chen","doi":"10.1016/j.jechem.2025.06.012","DOIUrl":"10.1016/j.jechem.2025.06.012","url":null,"abstract":"<div><div>Developing energy-efficient nitrite-to-ammonia (NO<sub>2</sub>RR) conversion technologies while simultaneously enabling the electrochemical upcycling of waste polyethylene terephthalate (PET) plastics into high-value-added chemicals is of great significance. Herein, an atomic oxygen vacancy (V<sub>o</sub>) engineering is developed to optimize the catalytic performance of V<sub>o2</sub>-Co(OH)F nanoarray towards the NO<sub>2</sub>RR and PET-derived ethylene glycol oxidation reaction (EGOR). The optimal V<sub>o2</sub>-Co(OH)F achieves an ultralow operating potential of −0.03 V vs. RHE at −100 mA cm<sup>−2</sup> and a remarkable NH<sub>3</sub> Faradaic efficiency (FE) of 98.4% at −0.2 V vs. RHE for NO<sub>2</sub>RR, and a high formate FE of 98.03% for EGOR. Operando spectroscopic analysis and theoretical calculations revealed that oxygen vacancies play a crucial role in optimizing the electronic structure of V<sub>o2</sub>-Co(OH)F, modulating the adsorption free energies of key reaction intermediates, and lowering the reaction energy barrier, thereby enhancing its overall catalytic performance. Remarkably, the V<sub>o2</sub>-Co(OH)F-based NO<sub>2</sub>RR||EGOR electrolyzer realized high NH<sub>3</sub> and formate yield rates of 33.9 and 44.9 mg h<sup>−1</sup> cm<sup>−2</sup> at 1.7 V, respectively, while demonstrating outstanding long-term stability over 100 h. This work provides valuable insights into the rational design of advanced electrocatalysts for co-electrolysis systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 558-565"},"PeriodicalIF":13.1,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144331039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Runbo Zhao , Peng Mao , Jun Lv , Po-Chuan Yang , Mengyuan Li , Bing Wang , Weihui Bi , Shen Xing , Yufei Zhong , Zhigang Zou
{"title":"Atomic layer deposition processed interlayers in photovoltaics: applications, challenges and perspectives","authors":"Runbo Zhao , Peng Mao , Jun Lv , Po-Chuan Yang , Mengyuan Li , Bing Wang , Weihui Bi , Shen Xing , Yufei Zhong , Zhigang Zou","doi":"10.1016/j.jechem.2025.06.013","DOIUrl":"10.1016/j.jechem.2025.06.013","url":null,"abstract":"<div><div>Atomic layer deposition (ALD) has driven significant advancements in photovoltaic technologies by enabling the development of interlayers that improve both the efficiency and stability of devices. This review traces the evolution of ALD interlayers across various photovoltaic technologies, starting with early silicon solar cells and progressing into a variety of thin-film solar cells. We then delve into the role of ALD in state-of-the-art single-junction perovskite solar cells, particularly in optimizing the critical interfaces of perovskites/charge-transporting layers/electrodes. Apart from that, we screen the functionality of ALD processing, which consists of reducing surface/interfacial defects and thus mitigating energy loss. Particularly, it enables efficient stacking of multiple thin layers, making a variety of tandem solar cells possible (silicon/perovskite, etc.) for higher efficiency. Moreover, the ALD-processed interlayer prevents the ion migration between metals and perovskites, inhibiting the inter-diffusion-induced degradation of devices. Despite ALD technology extensively elevating the performance of above conventional/emerging solar cells, key challenges such as precursor flammability, cross-contamination during processing, and low deposition pace persist. We go over these challenges and expect our comprehensive overview of ALD techniques could shed light on pushing the envelope of photovoltaic efficiency.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 702-725"},"PeriodicalIF":13.1,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144502453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Bridging chemical relithiation and alloying reaction to engineer a Li-Al-F interface for enhanced lithium storage kinetics","authors":"Haihang Huang, Yaoxiang Shan, Bingkun Zang, Longqing Zhang, Quanqiang Yuan, Xucai Yin, Zhangfa Tong, Yang Ren","doi":"10.1016/j.jechem.2025.05.066","DOIUrl":"10.1016/j.jechem.2025.05.066","url":null,"abstract":"<div><div>This study innovatively proposes a “chemical prelithiation/alloying-induced interfacial reconstruction” synergistic strategy that fundamentally improves the performance of Si-based anodes. Through a precisely controlled process leveraging orbital energetics and Lewis acid catalysis, we successfully engineer a Li-Al-F phase on the interface of SiO (denoted as Pre-SiO-Al) anodes via sequential chemical prelithiation and AlF<sub>3</sub>-driven interfacial alloying reactions. This novel approach breaks through the ion transport limitations of traditional LiF-dominated solid electrolyte interphase (SEI) layers, while concurrently addressing the critical challenges of low initial Coulombic efficiency (ICE) and severe volume expansion. Mechanism studies reveal that the Li-Al-F offers an ultralow Li<sup>+</sup> diffusion barrier (0.1 eV), significantly enhancing interfacial ion transport kinetics. Meanwhile, the high mechanical strength and dynamic stress dissipation capability of Li-Al-F effectively suppress SEI fracture caused by volume expansion, enabling coordinated deformation compatibility between the electrode and the interfacial layer. The Pre-SiO-Al anode maintains a high capacity of 682.6 mA h g<sup>−1</sup> after 2000 cycles at 1.0 A g<sup>−1</sup> with near 100% capacity retention. When paired with LiFePO<sub>4</sub> cathode, the Pre-SiO-Al||LFP full cell achieves impressive rate capability and cycling stability (93.8% capacity retention after 150 cycles at 0.5 C), demonstrating strong commercialization potential.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 541-549"},"PeriodicalIF":13.1,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144322255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanzhe Zhang , Zechen Li , Zheng Li , Wenwen Sun , Xuanyi Yuan , Haibo Jin , Yongjie Zhao
{"title":"Electron donor enabling Mn-Fe based layer oxide cathode with durable sodium ion storage","authors":"Yanzhe Zhang , Zechen Li , Zheng Li , Wenwen Sun , Xuanyi Yuan , Haibo Jin , Yongjie Zhao","doi":"10.1016/j.jechem.2025.06.008","DOIUrl":"10.1016/j.jechem.2025.06.008","url":null,"abstract":"<div><div>Enhancing the specific capacity of P2-type layered oxide cathodes via elevating the upper operation voltage would inevitably deteriorate electrochemical properties owing to the irreversible anionic redox reaction at high voltage. In this work, the strategy of the electron donor was utilized to address this issue. Remarkably, the earth-abundant P2-layered cathode Na<sub>2/3</sub>Al<sub>1/6</sub>Fe<sub>1/6</sub>Mn<sub>2/3</sub>O<sub>2</sub> with the presence of K<sub>2</sub>S renders superior rate capability (187.4 and 79.5 mA h g<sup>−1</sup> at 20 and 1000 mA g<sup>−1</sup>) and cycling stability (a capacity retention of 85.6% over 300 cycles at 1000 mA g<sup>−1</sup>) within the voltage region of 2–4.4 V Na<sup>+</sup>/Na. Furthermore, excellent electrochemical performance is also demonstrated in the full cell. Detailed structural analysis of as-proposed composite cathode illustrates that even at 4.4 V irreversible phase transition can be avoided as well as a cell volume variation of only 0.88%, which are attributed to the enhanced performance compared with the control group. Meanwhile, further investigation of charge compensation reveals the crucial role of sulfur ions in actively control of reversible redox reaction of oxygen species in the lattice structure. This work inspires a new strategy to enhance the structural stability of layered sodium ion cathode materials at high voltages.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 740-748"},"PeriodicalIF":13.1,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144502454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanchun Sun , Xiang Li , Rihui Li , Jiali Shou , Zhiyao Sun , Jian Yang , Haiyan Wang
{"title":"Reciprocal enhancement of iodine and manganese redox kinetics towards high-performance rechargeable zinc-iodine-manganese hybrid batteries","authors":"Yanchun Sun , Xiang Li , Rihui Li , Jiali Shou , Zhiyao Sun , Jian Yang , Haiyan Wang","doi":"10.1016/j.jechem.2025.06.009","DOIUrl":"10.1016/j.jechem.2025.06.009","url":null,"abstract":"<div><div>Aqueous Zn-I<sub>2</sub>-Mn hybrid batteries demonstrate enhanced capacity, superior redox reaction kinetics, and prolonged cycle life compared to their Zn-I<sub>2</sub> and Zn-Mn counterparts, making them promising candidates for grid-scale energy storage. Nevertheless, challenges remain in developing multifunctional positive electrode materials and elucidating the mechanistic synergy governing iodine and manganese redox reactions. Herein, we present a high-performance free-standing electrode composed of birnessite (KMnO) nanosheet arrays in situ grown on carbon cloth (CC@KMnO) for constructing a Zn-I<sub>2</sub>-Mn hybrid battery. Combined theoretical studies and in situ characterizations reveal that CC@KMnO enhances iodine species adsorption, lowers the Gibbs free energy change for iodine reduction, and significantly accelerates I<sup>−</sup>/I<sub>3</sub><sup>−</sup>/I<sub>5</sub><sup>−</sup> redox kinetics while suppressing polyiodide shuttling and corrosion effects. Synchronously, the ZnI<sub>2</sub> electrolyte facilitates the dissolution of residual and exfoliated KMnO, thereby improving manganese redox reaction kinetics, reversibility, and enhancing cycling stability. Leveraging this mutually reinforcing effect, the Zn-I<sub>2</sub>-Mn hybrid battery achieves an impressive areal capacity of 2.02 mAh cm<sup>−2</sup> and maintains long-term durability over 3600 cycles at 2 mA cm<sup>−2</sup>. This work provides valuable insights into designing efficient and durable hybrid energy storage systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 662-670"},"PeriodicalIF":13.1,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144491526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Meina Tan , Jingming Ge , Yang Qin , Jiaxin Luo , Yiping Wang , Fazhi Zhang , Xuhui Zhao , Xiaodong Lei
{"title":"The high performance of Al3+-preintercalated Cu9S5 derived from layered double hydroxide precursor in aqueous Cu-Al hybrid-ion battery","authors":"Meina Tan , Jingming Ge , Yang Qin , Jiaxin Luo , Yiping Wang , Fazhi Zhang , Xuhui Zhao , Xiaodong Lei","doi":"10.1016/j.jechem.2025.05.063","DOIUrl":"10.1016/j.jechem.2025.05.063","url":null,"abstract":"<div><div>Aqueous hybrid-ion batteries (AHBs) are a promising class of energy storage devices characterized by low cost, high safety, and high energy density. However, aqueous Cu-Al hybrid-ion batteries face challenges such as sluggish reaction kinetics and severe structural collapse of cathode materials, which limit their practical application. Here, a high-performance aqueous Cu-Al hybrid-ion battery is developed using aluminum pre-inserted Cu<sub>9</sub>S<sub>5</sub> (Al-Cu<sub>9</sub>S<sub>5</sub>) as the cathode material, derived from CuAl-layered double hydroxide (CuAl-LDH). The Al<sup>3+</sup> pre-intercalation strategy narrows the band gap, enhancing electron transport and improving electrochemical kinetics. The battery exhibits excellent rate performance (463 and 408 mA h g<sup>−1</sup> at current densities of 500 and 1000 mA g<sup>−1</sup>, respectively) and good cycle stability (with a capacity retention ratio of 81% after 300 cycles at a current density of 1000 mA g<sup>−1</sup>). Its performance surpasses that of most reported Al-ion batteries. Ex situ characterization and density functional theory (DFT) calculations reveal that the pre-intercalated Al<sup>3+</sup> in Al-Cu<sub>9</sub>S<sub>5</sub> participates in the reversible embedding/removal of Al ions during charge/ discharge processes. These findings provide valuable insights for designing pre-intercalated cathodes in aqueous Cu-Al hybrid-ion batteries with stable cycle life.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 531-540"},"PeriodicalIF":13.1,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144322254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhaochen Guo , Boyan Liu , Kang Wan , Peng Chen , Hongjing Wu , Songcan Wang
{"title":"Multidentate ligand-decorated indium tin oxide electrodes for efficient and durable perovskite solar cells","authors":"Zhaochen Guo , Boyan Liu , Kang Wan , Peng Chen , Hongjing Wu , Songcan Wang","doi":"10.1016/j.jechem.2025.05.064","DOIUrl":"10.1016/j.jechem.2025.05.064","url":null,"abstract":"<div><div>As commercial electron transport materials for perovskite solar cells (PSCs), pre-synthesized tin oxide (SnO<sub>2</sub>) nanoparticles suffer from colloidal agglomeration and inhomogeneous size distribution in aqueous solutions. The formed micro-size SnO<sub>2</sub> aggregates on the planar indium tin oxide (ITO) substrate not only create energy disorder to impair interfacial charge transfer but also hampers the growth of perovskite crystals, deteriorating the photovoltaic performance and device lifespan of PSCs. Here, a multidentate ligand of 1,2-cyclohexanedinitrilotetraacetic acid (CDTA) is developed to modify the surface chemistry of ITO substrates, facilitating the formation of pinhole-free and uniform SnO<sub>2</sub> electron transport layers for the crystallization of high-quality perovskite films. Moreover, the surface CDTA ligands lift the work function of ITO from 4.68 to 4.12 eV, enabling interfacial band alignment modification to improve the electron extraction from the ITO/SnO<sub>2</sub> interface. As a result, the CDTA-modified PSCs exhibit a significantly enhanced PCE of 24.67% and much prolonged device lifespan, retaining 91.3% and 92.8% of the initial PCEs under 2,000 h dark storage and after 500 h under one-sun illumination in nitrogen, respectively. This work demonstrates a simple yet efficient interfacial engineering strategy for the design of efficient and durable PSCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 550-557"},"PeriodicalIF":13.1,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144322708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuzhen Dang , Yurong Wu , Zhe Xu , Jianxing Wang , Runguo Zheng , Zhishuang Song , Zhiyuan Wang , Xiaoping Lin , Yanguo Liu , Dan Wang
{"title":"Entropy-mediated layered oxide cathodes: Synergistic channel expansion and strain control for sodium-ion batteries at cryogenic conditions","authors":"Yuzhen Dang , Yurong Wu , Zhe Xu , Jianxing Wang , Runguo Zheng , Zhishuang Song , Zhiyuan Wang , Xiaoping Lin , Yanguo Liu , Dan Wang","doi":"10.1016/j.jechem.2025.06.006","DOIUrl":"10.1016/j.jechem.2025.06.006","url":null,"abstract":"<div><div>O3-type layered oxide cathodes for sodium-ion batteries are promising owing to high theoretical capacity and broad temperature adaptability, yet hindered by structural degradation and sluggish Na<sup>+</sup> diffusion kinetics. Herein, we present a sodium-deficient high-entropy layered oxide cathode (Na<sub>0.85</sub>Ni<sub>0.3</sub>Mn<sub>0.3</sub>Fe<sub>0.1</sub>Co<sub>0.15</sub>Ti<sub>0.1</sub>Cu<sub>0.05</sub>B<sub>0.02</sub>O<sub>2</sub>, denoted as Na0.85-HEO), combining sodium content optimization and high-entropy composition design. Incorporating six transition metals and light element boron creates a unique high-entropy configuration, effectively mitigating local lattice distortion and internal strain through chemical disorder effects, thereby enabling highly reversible phase transitions (O3-P3-O3) and smaller volume change (0.6 Å<sup>3</sup>) during the initial cycle. The sodium-deficient high-entropy design effectively increases the sodium interlayer spacing to 0.322 nm, facilitating the Na<sup>+</sup> diffusion kinetics. Moreover, this high-entropy strategy enables the cathode to have a completely solid solution charge curve and significantly reduces the proportion of (O<sub>2</sub>)<em><sup>n</sup></em><sup>−</sup>, thereby suppressing gas release during the cycling process. The resultant cathode demonstrates exceptional cyclability (80% capacity retention after 400 cycles at 100 mA g<sup>−1</sup> in a full cell), and remarkable low-temperature performance (108.6 mAh g<sup>−1</sup> at −40 °C). This work guides the design of high-entropy electrode materials with tailored ionic transport channels for extreme-temperature energy storage applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 637-648"},"PeriodicalIF":13.1,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144491525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}