Pub Date : 2025-07-10DOI: 10.1016/j.esci.2025.100452
Yi Chen , Ji Qian , Ke Wang , Tianyang Xue , Zhengqiang Hu , Fengling Zhang , Tong Lian , Xinhui Pan , Teng Zhao , Li Li , Feng Wu , Renjie Chen
Solid-state lithium metal batteries face challenges from irreversible interfacial degradation and sluggish ion transport. We propose an electron-funnel-mediated anion confinement strategy via atomic-level electronic field engineering. Incorporating electron-withdrawing –NO2 groups into Zr-based frameworks induces a 0.38 eV upward d-band center shift, generating a quantum-confined electrostatic gradient that polarizes TFSI− anions. This reduces TFSI− decomposition energy barrier (ΔG: −0.35 → −1.22 eV), selectively promoting LiF nucleation while suppressing side reactions. Concurrently, Zr4+-PEO Lewis interactions disrupt polymer crystallinity, enhancing ionic conductivity and Li+ transference number. Cryo-TEM tomography and TOF-SIMS mapping reveal a fractal LiF-rich interphase enabling dendrite-free lithium plating for > 11,000 h with polarization < 40 mV. LiFePO4 full cells achieve 86.3% capacity retention after 400 cycles at 1C (1.3 mAh cm−2). This work establishes anion confinement as a universal framework synchronizing ion transport and interfacial durability, advancing practical solid-state batteries with exceptional longevity.
固态锂金属电池面临着界面不可逆降解和离子传输缓慢等挑战。我们提出了一种电子通道介导的阴离子约束策略。将吸电子的-NO2基团加入到zr基框架中，诱导了0.38 eV向上的d波段中心位移，产生了量子限制的静电梯度，使TFSI -阴离子极化。这降低了TFSI -分解能垒（ΔG:−0.35→−1.22 eV），选择性地促进了LiF成核，同时抑制了副反应。同时，Zr4+-PEO路易斯相互作用破坏了聚合物的结晶度，提高了离子电导率和Li+转移数。低温tem断层扫描和TOF-SIMS图谱显示了一个分形的富liff界面，可以在极化40 mV下电镀11000 h的无枝晶锂。在1C （1.3 mAh cm−2）下循环400次后，LiFePO4全电池的容量保持率达到86.3%。这项工作建立了阴离子约束作为同步离子传输和界面耐久性的通用框架，推进了具有特殊寿命的实用固态电池。
{"title":"Electron-funnel mediated anion confinement enables ultra-reversible interphases in solid-state batteries","authors":"Yi Chen , Ji Qian , Ke Wang , Tianyang Xue , Zhengqiang Hu , Fengling Zhang , Tong Lian , Xinhui Pan , Teng Zhao , Li Li , Feng Wu , Renjie Chen","doi":"10.1016/j.esci.2025.100452","DOIUrl":"10.1016/j.esci.2025.100452","url":null,"abstract":"<div><div>Solid-state lithium metal batteries face challenges from irreversible interfacial degradation and sluggish ion transport. We propose an electron-funnel-mediated anion confinement strategy via atomic-level electronic field engineering. Incorporating electron-withdrawing –NO<sub>2</sub> groups into Zr-based frameworks induces a 0.38 eV upward d-band center shift, generating a quantum-confined electrostatic gradient that polarizes TFSI<sup>−</sup> anions. This reduces TFSI<sup>−</sup> decomposition energy barrier (ΔG: −0.35 → −1.22 eV), selectively promoting LiF nucleation while suppressing side reactions. Concurrently, Zr<sup>4+</sup>-PEO Lewis interactions disrupt polymer crystallinity, enhancing ionic conductivity and Li<sup>+</sup> transference number. Cryo-TEM tomography and TOF-SIMS mapping reveal a fractal LiF-rich interphase enabling dendrite-free lithium plating for > 11,000 h with polarization < 40 mV. LiFePO<sub>4</sub> full cells achieve 86.3% capacity retention after 400 cycles at 1C (1.3 mAh cm<sup>−2</sup>). This work establishes anion confinement as a universal framework synchronizing ion transport and interfacial durability, advancing practical solid-state batteries with exceptional longevity.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100452"},"PeriodicalIF":36.6,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Despite significant advancements in improving the power-conversion efficiency (PCE) of exceeding 27% in perovskite solar cells (PSCs), the insufficient operational stability of PSCs under illumination remains a critical challenge, posing a major obstacle to their commercial viability. This paper proposes a feasible hindered amine stabilization strategy (HASS) by using a hindered amine light stabilizer for grain and surface modulation of perovskite, thereby blocking the internal and external degradation pathways of perovskite. Its piperidine ring is easily oxidized to form Nitrogen monoxide (N–O•) radicals after absorbing light energy in an aerobic environment. The free superoxide radical () radicals react with perovskite and H+ in the decomposition products of perovskite, thereby improving the light stability of the device. In addition, the contained triazine and morpholine functional groups can coordinate with Pb2+, thereby reducing the interface defects and inhibiting the non-radiative recombination. The HASS-modulated PSC could reach the champion PCE of 26.74% (certified 26.56%), which is remarkable for inverted PSCs prepared under ambient conditions. Further, the unencapsulated device could maintain 95.4% of its initial PCE after more than 1000 h of aging at maximum power point tracking.
{"title":"Chemical inhibition of light-induced decomposition by hindered amine for efficient and stable perovskite solar cells","authors":"Yuqing Su , Jike Ding , Zuolin Zhang , Mengjia Li , Jiangzhao Chen , Jian-Xin Tang , Thierry Pauporté , Cong Chen","doi":"10.1016/j.esci.2025.100451","DOIUrl":"10.1016/j.esci.2025.100451","url":null,"abstract":"<div><div>Despite significant advancements in improving the power-conversion efficiency (PCE) of exceeding 27% in perovskite solar cells (PSCs), the insufficient operational stability of PSCs under illumination remains a critical challenge, posing a major obstacle to their commercial viability. This paper proposes a feasible hindered amine stabilization strategy (HASS) by using a hindered amine light stabilizer for grain and surface modulation of perovskite, thereby blocking the internal and external degradation pathways of perovskite. Its piperidine ring is easily oxidized to form Nitrogen monoxide (N–O•) radicals after absorbing light energy in an aerobic environment. The free superoxide radical (<span><math><mrow><msubsup><mi>O</mi><mn>2</mn><mrow><mo>·</mo><mo>−</mo></mrow></msubsup></mrow></math></span>) radicals react with perovskite and H<sup>+</sup> in the decomposition products of perovskite, thereby improving the light stability of the device. In addition, the contained triazine and morpholine functional groups can coordinate with Pb<sup>2+</sup>, thereby reducing the interface defects and inhibiting the non-radiative recombination. The HASS-modulated PSC could reach the champion PCE of 26.74% (certified 26.56%), which is remarkable for inverted PSCs prepared under ambient conditions. Further, the unencapsulated device could maintain 95.4% of its initial PCE after more than 1000 h of aging at maximum power point tracking.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100451"},"PeriodicalIF":36.6,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Like the vital role that multifunctional biological fluids play in living organisms, leveraging fluid multifunctionality offers a promising approach to enhance system capabilities without overcomplicating the hardware. However, creating a multifunctional fluid for soft fluidic systems remains a persistent challenge. Here, we report a multifunctional electrofluid that integrates actuation, sensing, self-healing, damage detection, and triboelectricity powering for the various function requirements of soft fluidic systems. We demonstrate that actuation, sensing, and damage detection can be achieved by activating electrons in the working fluid, and the system enables underwater self-healing through the incorporation of water-reactive self-healing agents into the working fluid. In addition, we achieve the fluid flow by transporting the electrons gathered by the triboelectric nanogenerator into the fluid, thereby making the system become a triboelectricity-powered machine. The fluid module developed based on electrofluids is self-contained and plug-and-play, providing good convenience for rapid construction of soft fluidic systems. We validate the effectiveness of the electronic fluids through soft robotic fish, soft octobot, and wearable devices, demonstrating that the proposed fluid enables multiple functions of the system without added weight or volume. As such, the proposed electrofluid provides a promising platform to achieve high integration and lightweight of multifunctional soft fluidic actuation by expanding the functionalities of the fluid itself.
{"title":"Multifunctional robotic electrofluid for soft fluidic actuation","authors":"Wei Tang , Pingan Zhu , Yu Hu, Xinyu Guo, Yonghao Wang, Kecheng Qin, Yiding Zhong, Qincheng Sheng, Huxiu Xu, Zhaoyang Li, Huayong Yang, Jun Zou","doi":"10.1016/j.esci.2025.100448","DOIUrl":"10.1016/j.esci.2025.100448","url":null,"abstract":"<div><div>Like the vital role that multifunctional biological fluids play in living organisms, leveraging fluid multifunctionality offers a promising approach to enhance system capabilities without overcomplicating the hardware. However, creating a multifunctional fluid for soft fluidic systems remains a persistent challenge. Here, we report a multifunctional electrofluid that integrates actuation, sensing, self-healing, damage detection, and triboelectricity powering for the various function requirements of soft fluidic systems. We demonstrate that actuation, sensing, and damage detection can be achieved by activating electrons in the working fluid, and the system enables underwater self-healing through the incorporation of water-reactive self-healing agents into the working fluid. In addition, we achieve the fluid flow by transporting the electrons gathered by the triboelectric nanogenerator into the fluid, thereby making the system become a triboelectricity-powered machine. The fluid module developed based on electrofluids is self-contained and plug-and-play, providing good convenience for rapid construction of soft fluidic systems. We validate the effectiveness of the electronic fluids through soft robotic fish, soft octobot, and wearable devices, demonstrating that the proposed fluid enables multiple functions of the system without added weight or volume. As such, the proposed electrofluid provides a promising platform to achieve high integration and lightweight of multifunctional soft fluidic actuation by expanding the functionalities of the fluid itself.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 6","pages":"Article 100448"},"PeriodicalIF":36.6,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145366118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-03DOI: 10.1016/j.esci.2025.100450
Tuo Lu , Nengneng Xu , Benji Zhou , Liyuan Guo , Xiaodan Wen , Shuaifeng Lou , Guicheng Liu , Woochul Yang , Nianjun Yang , Momo Safari , Haitao Huang , Jinli Qiao
Highly electrocatalytic and durable Co-Nx-C frameworks containing carbon nanofibers (CNFs)/carbon nitrides (CNs) are vital materials for rechargeable zinc–air batteries (RZABs). However, the existing Co-Nx-C frameworks experience severe agglomeration during synthesis and limited active site accessibility/mechanical robustness. In this work, a photo-enhanced bifunctional catalyst with a type II p-n heterojunction (g–C3N4–Co@CNT/Co–N4/C@CNF) is achieved through a combined “electrospinning + calcination + ball milling” approach. The composite integrates graphitic carbon nitride (g-C3N4) nanosheets with dual active Co sites (nanoparticles and Co–N4 single atoms) anchored on conductive carbon nanofibers. This architecture enables efficient charge separation, enhanced light absorption, and accelerated oxygen redox kinetics. DFT calculations reveal that g-C3N4 modulates the electronic structure and lowers the reaction free-energy barriers, leading the d-band center closer to the Fermi level. Under light irradiation, the g–C3N4–Co@CNT/Co–N4/C@CNF exhibits outstanding ORR/OER catalytic performance, with a small overpotential gap of 0.684 V (E1/2 = 0.930 V, Ej:10 = 1.614 V). In practical application: 1) light-enhanced liquid ZABs with g–C3N4–Co@CNT/Co–N4/C@CNF photoactive catalysts manifest a peak power density of 310 mW cm−2 and a long cycle life exceeding 1100 h. 2) Light-enhanced flexible ZABs also can reach a peak power density of 96 mW cm−2 and tolerate a wide range of bending angles (0°–180°–0°) during harsh operation. This work offers a new platform for designing efficient photo-electrocatalysts and advancing next-generation solar–electrochemical energy conversion systems.
{"title":"Photo-electroactive p-n heterojunction catalyst with dual Co sites for high-performance light-enhanced zinc–air batteries","authors":"Tuo Lu , Nengneng Xu , Benji Zhou , Liyuan Guo , Xiaodan Wen , Shuaifeng Lou , Guicheng Liu , Woochul Yang , Nianjun Yang , Momo Safari , Haitao Huang , Jinli Qiao","doi":"10.1016/j.esci.2025.100450","DOIUrl":"10.1016/j.esci.2025.100450","url":null,"abstract":"<div><div>Highly electrocatalytic and durable Co-Nx-C frameworks containing carbon nanofibers (CNFs)/carbon nitrides (CNs) are vital materials for rechargeable zinc–air batteries (RZABs). However, the existing Co-Nx-C frameworks experience severe agglomeration during synthesis and limited active site accessibility/mechanical robustness. In this work, a photo-enhanced bifunctional catalyst with a type II p-n heterojunction (g–C<sub>3</sub>N<sub>4</sub>–Co@CNT/Co–N<sub>4</sub>/C@CNF) is achieved through a combined “electrospinning + calcination + ball milling” approach. The composite integrates graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) nanosheets with dual active Co sites (nanoparticles and Co–N<sub>4</sub> single atoms) anchored on conductive carbon nanofibers. This architecture enables efficient charge separation, enhanced light absorption, and accelerated oxygen redox kinetics. DFT calculations reveal that g-C<sub>3</sub>N<sub>4</sub> modulates the electronic structure and lowers the reaction free-energy barriers, leading the d-band center closer to the Fermi level. Under light irradiation, the g–C<sub>3</sub>N<sub>4</sub>–Co@CNT/Co–N<sub>4</sub>/C@CNF exhibits outstanding ORR/OER catalytic performance, with a small overpotential gap of 0.684 V (E<sub>1/2</sub> = 0.930 V, E<sub>j:10</sub> = 1.614 V). In practical application: 1) light-enhanced liquid ZABs with g–C<sub>3</sub>N<sub>4</sub>–Co@CNT/Co–N<sub>4</sub>/C@CNF photoactive catalysts manifest a peak power density of 310 mW cm<sup>−2</sup> and a long cycle life exceeding 1100 h. 2) Light-enhanced flexible ZABs also can reach a peak power density of 96 mW cm<sup>−2</sup> and tolerate a wide range of bending angles (0°–180°–0°) during harsh operation. This work offers a new platform for designing efficient photo-electrocatalysts and advancing next-generation solar–electrochemical energy conversion systems.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 1","pages":"Article 100450"},"PeriodicalIF":36.6,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145842060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2025.100373
Chi Zhang , Lei Zhang , Yu Tian , Zhengang An, Bo Li, Dachao Li
Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space, which are crucial for the advancement of metaverse applications. However, traditional hardware solutions, reliant on optical cameras or inertial sensors, are hampered by privacy concerns, spatial limitations, high costs, and calibration challenges. Here, we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers (TSSFs) and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement. TSSFs enable the dynamic capture of body postures and excel in sensitivity, linearity, and strain range, while maintaining mechanical stability, temperature resilience, and washability. The integrated algorithms accurately decouple posture signals — distinguishing between similar postures with the 1D-CNN algorithm, compensating for body-shape differences via a calibration algorithm, and determining spatial elements for avatar reconstruction using a decision-tree algorithm. Finally, leveraging Unity-3D, we achieve ultra-accurate dynamic 3D avatars with a joint angle error of <3.63° and demonstrate their effectiveness using VR fitness and entertainment applications, showing how they can offer users standardized yet engaging experiences.
{"title":"AI-enabled full-body dynamic avatar reconstruction using triboelectric smart clothing for metaverse applications","authors":"Chi Zhang , Lei Zhang , Yu Tian , Zhengang An, Bo Li, Dachao Li","doi":"10.1016/j.esci.2025.100373","DOIUrl":"10.1016/j.esci.2025.100373","url":null,"abstract":"<div><div>Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space, which are crucial for the advancement of metaverse applications. However, traditional hardware solutions, reliant on optical cameras or inertial sensors, are hampered by privacy concerns, spatial limitations, high costs, and calibration challenges. Here, we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers (TSSFs) and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement. TSSFs enable the dynamic capture of body postures and excel in sensitivity, linearity, and strain range, while maintaining mechanical stability, temperature resilience, and washability. The integrated algorithms accurately decouple posture signals — distinguishing between similar postures with the 1D-CNN algorithm, compensating for body-shape differences via a calibration algorithm, and determining spatial elements for avatar reconstruction using a decision-tree algorithm. Finally, leveraging Unity-3D, we achieve ultra-accurate dynamic 3D avatars with a joint angle error of <3.63° and demonstrate their effectiveness using VR fitness and entertainment applications, showing how they can offer users standardized yet engaging experiences.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100373"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2025.100394
Xueqian Li , Chenglong Deng , Mengyao Liu , Jiawei Xiong , Xiaodong Zhang , Qiaoyi Yan , Jiao Lin , Cen Chen , Feng Wu , Yi Zhao , Renjie Chen , Li Li
In the development of sustainable lithium-ion batteries, achieving the efficient and cost-effective recycling of all components, particularly spent graphite (SG) anodes, has become a critical requirement. While considerable efforts have been devoted to recovering and reusing SG materials under conventional conditions, limited attention has been given to recycling under extreme conditions. This review systematically elucidates the main failure mechanisms of graphite anodes, including lithium plating and dendrite formation, solid electrolyte interface film failure, structural degradation, and current collector corrosion, with a particular focus on low-temperature and fast-charging conditions. As a contribution toward optimizing resource utilization, this review comprehensively summarizes the industrial perspective on strategies for recycling SG anodes, which aim to produce high-purity regenerated graphite (RG) powders. We also analyze current methods for modifying RG, such as structural reconstruction and surface reconditioning, to bring added value to modified RG materials. A detailed examination of the technical challenges in SG recycling and RG upgrading is presented, offering guidance for the future development of graphite upcycling technologies. This review also provides valuable insights into achieving high efficiency, intelligence, and sustainability in graphite utilization.
{"title":"Reutilization and upcycling of spent graphite for sustainable lithium-ion batteries: Progress and perspectives","authors":"Xueqian Li , Chenglong Deng , Mengyao Liu , Jiawei Xiong , Xiaodong Zhang , Qiaoyi Yan , Jiao Lin , Cen Chen , Feng Wu , Yi Zhao , Renjie Chen , Li Li","doi":"10.1016/j.esci.2025.100394","DOIUrl":"10.1016/j.esci.2025.100394","url":null,"abstract":"<div><div>In the development of sustainable lithium-ion batteries, achieving the efficient and cost-effective recycling of all components, particularly spent graphite (SG) anodes, has become a critical requirement. While considerable efforts have been devoted to recovering and reusing SG materials under conventional conditions, limited attention has been given to recycling under extreme conditions. This review systematically elucidates the main failure mechanisms of graphite anodes, including lithium plating and dendrite formation, solid electrolyte interface film failure, structural degradation, and current collector corrosion, with a particular focus on low-temperature and fast-charging conditions. As a contribution toward optimizing resource utilization, this review comprehensively summarizes the industrial perspective on strategies for recycling SG anodes, which aim to produce high-purity regenerated graphite (RG) powders. We also analyze current methods for modifying RG, such as structural reconstruction and surface reconditioning, to bring added value to modified RG materials. A detailed examination of the technical challenges in SG recycling and RG upgrading is presented, offering guidance for the future development of graphite upcycling technologies. This review also provides valuable insights into achieving high efficiency, intelligence, and sustainability in graphite utilization.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100394"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633547","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2025.100376
Jun Ho Yu , Konstantin Köster , Natalia Voronina , Sungkyu Kim , Hyeon-Ji Shin , Kyung Sun Kim , Kyuwook Ihm , Hyungsub Kim , Hun-Gi Jung , Koji Yazawa , Olivier Guillon , Pierluigi Gargiani , Laura Simonelli , Payam Kaghazchi , Seung-Taek Myung
In exploring the frontier of high-energy-density cathode materials for lithium-ion batteries, substantial progress has been made by fine-tuning the composition of Ni-rich cathodes tailored for high-capacity operation. Equally promising are Li-rich cathode materials, which leverage the novel mechanism of oxygen-redox chemistry to achieve enhanced capacities. Nonetheless, the practical realization of these capacities remains elusive, falling short of the desired benchmarks. In this work, we pioneer a Mn-based, Co-free, reduced-nickel, high-capacity cathode material: Li0.75[Li0.15Ni0.15Mn0.7]O2 ionic exchanged from Na0.75[Li0.15Ni0.15Mn0.7]O2. This material is an O2-type layered structure, distinguished by honeycomb ordering within the transition-metal layer, as confirmed by comprehensive neutron and X-ray studies and extensive electrostatic screening. The material's unique structural integrity facilitates the delivery of an exceptional quantity of Li+ ions via O2−/ redox, circumventing oxygen release and phase transition. The de/lithiation process enables the delivery of a substantial reversible capacity of ∼284 mAh (g-oxide)−1 (956 Wh (kg-oxide)−1). Moreover, this structural and chemical stability contributes to an acceptable cycling stability for 500 cycles in full cells, providing improved thermal stability with lower exothermic heat generation and thus highlighting the feasibility of a Mn-based, Co-free, reduced-nickel composition. This investigation marks a pivotal advancement in layered lithium cathode materials.
在探索锂离子电池高能量密度正极材料的前沿领域，为高容量运行量身定制的富镍阴极成分的微调取得了实质性进展。同样有前途的是富锂阴极材料，它利用氧氧化还原化学的新机制来实现增强的容量。尽管如此，这些能力的实际实现仍然难以实现，没有达到预期的基准。在这项工作中，我们开拓了一种mn基，无co，还原镍，高容量正极材料：由Na0.75[Li0.15Ni0.15Mn0.7]O2交换的Li0.75[Li0.15Ni0.15Mn0.7]O2离子。该材料是一种o2型层状结构，其特征是过渡金属层内的蜂窝状有序，经全面的中子和x射线研究和广泛的静电筛选证实。该材料独特的结构完整性有助于通过O2 - /O2n -氧化还原传递大量Li+离子，绕过氧气释放和相变。去锂化工艺能够提供相当大的可逆容量，约284 mAh (g-oxide)−1 （956 Wh (kg-oxide)−1）。此外，这种结构和化学稳定性有助于在全电池中进行500次循环，提供更好的热稳定性和更低的放热产热，从而突出了mn基，无co，还原镍成分的可行性。这项研究标志着层状锂正极材料的关键进展。
{"title":"Elevating Li-ion battery paradigms: Sophisticated ionic architectures in lithium-excess layered oxides for unprecedented electrochemical performance","authors":"Jun Ho Yu , Konstantin Köster , Natalia Voronina , Sungkyu Kim , Hyeon-Ji Shin , Kyung Sun Kim , Kyuwook Ihm , Hyungsub Kim , Hun-Gi Jung , Koji Yazawa , Olivier Guillon , Pierluigi Gargiani , Laura Simonelli , Payam Kaghazchi , Seung-Taek Myung","doi":"10.1016/j.esci.2025.100376","DOIUrl":"10.1016/j.esci.2025.100376","url":null,"abstract":"<div><div>In exploring the frontier of high-energy-density cathode materials for lithium-ion batteries, substantial progress has been made by fine-tuning the composition of Ni-rich cathodes tailored for high-capacity operation. Equally promising are Li-rich cathode materials, which leverage the novel mechanism of oxygen-redox chemistry to achieve enhanced capacities. Nonetheless, the practical realization of these capacities remains elusive, falling short of the desired benchmarks. In this work, we pioneer a Mn-based, Co-free, reduced-nickel, high-capacity cathode material: Li<sub>0.75</sub>[Li<sub>0.15</sub>Ni<sub>0.15</sub>Mn<sub>0.7</sub>]O<sub>2</sub> ionic exchanged from Na<sub>0.75</sub>[Li<sub>0.15</sub>Ni<sub>0.15</sub>Mn<sub>0.7</sub>]O<sub>2</sub>. This material is an O2-type layered structure, distinguished by honeycomb ordering within the transition-metal layer, as confirmed by comprehensive neutron and X-ray studies and extensive electrostatic screening. The material's unique structural integrity facilitates the delivery of an exceptional quantity of Li<sup>+</sup> ions <em>via</em> O<sup>2</sup><sup>−</sup>/<span><math><mrow><msup><msub><mi>O</mi><mn>2</mn></msub><mrow><mi>n</mi><mo>−</mo></mrow></msup></mrow></math></span> redox, circumventing oxygen release and phase transition. The de/lithiation process enables the delivery of a substantial reversible capacity of ∼284 mAh (g-oxide)<sup>−</sup><sup>1</sup> (956 Wh (kg-oxide)<sup>−</sup><sup>1</sup>). Moreover, this structural and chemical stability contributes to an acceptable cycling stability for 500 cycles in full cells, providing improved thermal stability with lower exothermic heat generation and thus highlighting the feasibility of a Mn-based, Co-free, reduced-nickel composition. This investigation marks a pivotal advancement in layered lithium cathode materials.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100376"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2025.100395
Lu Nie , Yang Li , Xiaoyan Wu , Mengtian Zhang , Xinru Wu , Xiao Xiao , Runhua Gao , Zhihong Piao , Xian Wu , Ya Song , Shaojie Chen , Yanfei Zhu , Yi Yu , Shengjie Ling , Ke Zheng , Guangmin Zhou
Ultrathin solid-state electrolytes (SSEs) with rapid Li+ transport are ideal for developing high-energy-density all-solid-state lithium metal batteries. However, a significant challenge remains in balancing the intrinsic trade-off between electrochemical performance and mechanical properties. Herein, Antheraea pernyi fibers recycled from waste silk textiles are utilized as the raw materials to construct a porous and strong supporting skeleton for fabricating ultrathin SSE. This skeleton not only provides efficient three-dimensional Li+ transport channels, but also immobilizes Li-salt anions, resulting in homogenized Li+ flux and local current density distribution, thereby promoting uniform Li deposition. As a result, the obtained ultrathin SSE exhibits excellent ion-regulated properties, enhanced electrochemical stability, and superior dendrite suppression. Additionally, the formation of an inorganic-rich solid electrolyte interface layer is beneficial for stabilizing the interface contact between the SSE and Li anode. The solid-state Li|sulfurized polyacrylonitrile (Li|SPAN) cell delivers an excellent capacity retention of 92.3% after 500 cycles at 1 C. Moreover, the prepared high-voltage Li|LiCoO2 pouch cell exhibits a capacity retention of 90.1% at 0.2 C after 200 cycles. This work presents an economically effective strategy for reutilizing waste textiles as ion-conducting mechanical supports for energy storage applications.
{"title":"Scalable ultrathin solid electrolyte from recycled Antheraea pernyi silk with regulated ion transport for solid-state Li–S batteries","authors":"Lu Nie , Yang Li , Xiaoyan Wu , Mengtian Zhang , Xinru Wu , Xiao Xiao , Runhua Gao , Zhihong Piao , Xian Wu , Ya Song , Shaojie Chen , Yanfei Zhu , Yi Yu , Shengjie Ling , Ke Zheng , Guangmin Zhou","doi":"10.1016/j.esci.2025.100395","DOIUrl":"10.1016/j.esci.2025.100395","url":null,"abstract":"<div><div>Ultrathin solid-state electrolytes (SSEs) with rapid Li<sup>+</sup> transport are ideal for developing high-energy-density all-solid-state lithium metal batteries. However, a significant challenge remains in balancing the intrinsic trade-off between electrochemical performance and mechanical properties. Herein, <em>Antheraea pernyi</em> fibers recycled from waste silk textiles are utilized as the raw materials to construct a porous and strong supporting skeleton for fabricating ultrathin SSE. This skeleton not only provides efficient three-dimensional Li<sup>+</sup> transport channels, but also immobilizes Li-salt anions, resulting in homogenized Li<sup>+</sup> flux and local current density distribution, thereby promoting uniform Li deposition. As a result, the obtained ultrathin SSE exhibits excellent ion-regulated properties, enhanced electrochemical stability, and superior dendrite suppression. Additionally, the formation of an inorganic-rich solid electrolyte interface layer is beneficial for stabilizing the interface contact between the SSE and Li anode. The solid-state Li|sulfurized polyacrylonitrile (Li|SPAN) cell delivers an excellent capacity retention of 92.3% after 500 cycles at 1 C. Moreover, the prepared high-voltage Li|LiCoO<sub>2</sub> pouch cell exhibits a capacity retention of 90.1% at 0.2 C after 200 cycles. This work presents an economically effective strategy for reutilizing waste textiles as ion-conducting mechanical supports for energy storage applications.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100395"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2024.100331
Yajun Zhao , Yueyang Wang , Jinze Li , Jiawei Xiong , Qi Li , Kovan Khasraw Abdalla , Yi Zhao , Zhao Cai , Xiaoming Sun
The invention of aqueous Zn batteries (AZBs) traces back to the eighteenth century. Recently, however, AZBs have been undergoing a renaissance due to the urgent need for renewable energy storage devices that are intrinsically safe, inexpensive, and environmentally benign. The escalating demand for high-energy, fast-charging AZBs, particularly in grid-scale energy storage systems, necessitates a profound exploration of the fundamental aspects of electrode chemistries. In particular, a comprehensive understanding from the viewpoints of thermodynamics and kinetics is crucial, with the aim of advancing the development of next-generation AZBs that have high power and energy densities. However, clarification about the fundamental issues in AZB chemistry has yet to be achieved. This review offers a thorough exploration of the thermodynamics and dynamic mechanisms at the anode and cathode, with the aim of helping researchers achieve high-performance AZBs. The inherent challenges and corresponding strategies related to electrode thermodynamic and dynamic optimization are summarized, followed by insights into future directions for developing high-energy, fast-charging AZBs. We conclude by considering the future prospects for AZBs and offering recommendations for making further advancements in discovering new redox chemistries, optimizing electrode architectures, and achieving integrated battery designs, all of which are considered essential and time-sensitive for making high-energy, fast-charging, and durable AZBs a reality.
{"title":"Thermodynamic and kinetic insights for manipulating aqueous Zn battery chemistry: Towards future grid-scale renewable energy storage systems","authors":"Yajun Zhao , Yueyang Wang , Jinze Li , Jiawei Xiong , Qi Li , Kovan Khasraw Abdalla , Yi Zhao , Zhao Cai , Xiaoming Sun","doi":"10.1016/j.esci.2024.100331","DOIUrl":"10.1016/j.esci.2024.100331","url":null,"abstract":"<div><div>The invention of aqueous Zn batteries (AZBs) traces back to the eighteenth century. Recently, however, AZBs have been undergoing a renaissance due to the urgent need for renewable energy storage devices that are intrinsically safe, inexpensive, and environmentally benign. The escalating demand for high-energy, fast-charging AZBs, particularly in grid-scale energy storage systems, necessitates a profound exploration of the fundamental aspects of electrode chemistries. In particular, a comprehensive understanding from the viewpoints of thermodynamics and kinetics is crucial, with the aim of advancing the development of next-generation AZBs that have high power and energy densities. However, clarification about the fundamental issues in AZB chemistry has yet to be achieved. This review offers a thorough exploration of the thermodynamics and dynamic mechanisms at the anode and cathode, with the aim of helping researchers achieve high-performance AZBs. The inherent challenges and corresponding strategies related to electrode thermodynamic and dynamic optimization are summarized, followed by insights into future directions for developing high-energy, fast-charging AZBs. We conclude by considering the future prospects for AZBs and offering recommendations for making further advancements in discovering new redox chemistries, optimizing electrode architectures, and achieving integrated battery designs, all of which are considered essential and time-sensitive for making high-energy, fast-charging, and durable AZBs a reality.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100331"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-07-01DOI: 10.1016/j.esci.2024.100333
Genxiang Wang , Ao Chen , Yao Chen , Fen Qiao , Junfeng Wang , Nianjun Yang , Hao Zhang , Zhenhai Wen
The application of electrochemical technologies for chemical and fuel synthesis offers a significantly more eco-friendly method than traditional industrial practice. However, electrochemical synthesis in aqueous solutions often involves a sluggish oxygen evolution reaction (OER) at the anode, yielding products that are less economically viable and leading to inefficient energy use. This challenge has prompted extensive research into replacing the OER with fast, value-added oxidation reactions (OER alternatives) in electrolysis systems. In this review, we summarize the latest research progress in coupled electrochemical systems that integrate OER alternatives with reduction reactions, beyond hydrogen evolution reactions, in aqueous solutions to synthesize dual value-added products. After providing a general overview, we start by introducing two key factors: (i) electrolytic devices and (ii) advanced characterization techniques for mechanism investigation. The focus then shifts to catalysts developed so far and their corresponding catalytic mechanisms, and to the electrochemical performance of these hybrid electrolysis systems. Finally, we outline and discuss the challenges and prospects for these integrated electrochemical systems to offer insights into future research directions and applications. We envision that this review will provide a panorama of electrolysis systems for dual value-added products, thereby fostering the development of green synthesis with zero carbon emissions.
{"title":"Advancements in electrochemical synthesis: Expanding from water electrolysis to dual-value-added products","authors":"Genxiang Wang , Ao Chen , Yao Chen , Fen Qiao , Junfeng Wang , Nianjun Yang , Hao Zhang , Zhenhai Wen","doi":"10.1016/j.esci.2024.100333","DOIUrl":"10.1016/j.esci.2024.100333","url":null,"abstract":"<div><div>The application of electrochemical technologies for chemical and fuel synthesis offers a significantly more eco-friendly method than traditional industrial practice. However, electrochemical synthesis in aqueous solutions often involves a sluggish oxygen evolution reaction (OER) at the anode, yielding products that are less economically viable and leading to inefficient energy use. This challenge has prompted extensive research into replacing the OER with fast, value-added oxidation reactions (OER alternatives) in electrolysis systems. In this review, we summarize the latest research progress in coupled electrochemical systems that integrate OER alternatives with reduction reactions, beyond hydrogen evolution reactions, in aqueous solutions to synthesize dual value-added products. After providing a general overview, we start by introducing two key factors: (i) electrolytic devices and (ii) advanced characterization techniques for mechanism investigation. The focus then shifts to catalysts developed so far and their corresponding catalytic mechanisms, and to the electrochemical performance of these hybrid electrolysis systems. Finally, we outline and discuss the challenges and prospects for these integrated electrochemical systems to offer insights into future research directions and applications. We envision that this review will provide a panorama of electrolysis systems for dual value-added products, thereby fostering the development of green synthesis with zero carbon emissions.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"5 4","pages":"Article 100333"},"PeriodicalIF":42.9,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144633525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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