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Achieving high-voltage polymer-based all-solid-state batteries based on thermodynamic and kinetic degradation insights 实现基于热力学和动力学降解的高压聚合物全固态电池

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-26 DOI: 10.1016/j.esci.2025.100433

Xiaoyan Yu , Yun Su , Hang Su , Ruizhi Liu , Jingyi Qiu , Xiayu Zhu , Rui Wen , Hao Zhang , Xiaohui Rong , Yong-Sheng Hu , Gaoping Cao

Understanding the mechanisms behind the degradation in cyclic stability of polymer-based all-solid-state batteries (ASSBs) at high voltages is important for facilitating their commercial application. Beyond the examination of specific material properties, from the perspectives of thermodynamic and kinetic factors, we find that the operating temperature critically influences the stability of the electrodes, electrolytes and electrode/electrolyte interfaces within the ASSBs. In this study, we constructed polymer-based ASSBs and comprehensively investigated the cyclic stability and changes in failure mechanisms with different operating temperatures at high voltages. Notably, a lower operating temperature enhanced the cyclic stability by suppressing structural collapse of the cathode and decomposition of the electrolytes while inhibiting lithium dendrites growth. The assembled lithium coin cells exhibited a superior capacity retention of 81.8% after 400 cycles at a voltage of 3.0–4.45 V and operating temperature of 40 °C. In addition, both lithium pouch cells and sodium coin cells were prepared and demonstrated excellent performances. This work provides a rational guide for the development of advanced polymer-based ASSBs.

了解聚合物基全固态电池（assb）在高压下循环稳定性下降背后的机制对于促进其商业应用非常重要。除了对特定材料性能的考察之外，从热力学和动力学因素的角度来看，我们发现工作温度对assb内电极、电解质和电极/电解质界面的稳定性有重要影响。在这项研究中，我们构建了基于聚合物的assb，并全面研究了在不同工作温度下的高压循环稳定性和失效机制的变化。值得注意的是，较低的工作温度通过抑制阴极的结构崩溃和电解质的分解而增强了循环稳定性，同时抑制了锂枝晶的生长。在3.0 ~ 4.45 V电压和40℃工作温度下，经过400次循环后，电池容量保持率高达81.8%。此外，还制备了锂袋电池和钠硬币电池，并表现出优异的性能。该工作为先进聚合物基assb的开发提供了合理的指导。

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引用次数: 0

Interface-engineered metalized plastic current collectors for fast-charging lithium-ion batteries with high safety and stability 界面工程金属化塑料集流器，用于快速充电锂离子电池，具有高安全性和稳定性

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-24 DOI: 10.1016/j.esci.2025.100432

Chaofan Liang , Jie Ji , Yaqi Liao , Tianyi Hou , Zhikang Liu , Hongbin Xie , Kui Li , Xinpeng Pi , Donghai Wang , Xiaoyu Jin , Weichen Du , Long Qie

Adopting the metalized plastic current collector (MPCC) enhances the safety and specific energy density of lithium-ion batteries (LIBs) but sacrifices the rate capability. The reduced rate capability is customarily ascribed to the lower electronic conductivity of MPCC as compared with the metal ones (e.g., Al and Cu) due to the less metal usage. Here, we demonstrate that the interfacial contact between the current collector (CC) and the active-material layer, rather than the electronic conductivity of CC, accounts for the rate performance of the cells. By introducing a thin carbon coating (∼300 nm) onto the surface of MPCC (e.g., 1 μm thick aluminum deposited on both sides of 10 μm polyethylene terephthalate (PET) film, Al-PET), we reduced the contact resistance between MPCC and cathode materials. Using the carbon-coated Al-PET (C@Al-PET) as CC, the 6.0-Ah graphite/LiCoO₂ pouch cell delivers significantly improved fast-charge capability and cycling stability, which are identified as the homogenized potential distribution and electrode utilization with multiphysical field simulations. Most importantly, the cell with C@Al-PET CC could still pass the harsh impact test, promising its applications in high-rate LIBs with superior safety.

采用金属化塑料集流器（MPCC）可以提高锂离子电池的安全性和比能量密度，但牺牲了倍率能力。速率能力的降低通常归因于MPCC的电子导电性低于金属材料（例如Al和Cu），因为金属用量较少。在这里，我们证明了电流集电极（CC）和活性材料层之间的界面接触，而不是CC的电子导电性，决定了电池的速率性能。通过在MPCC表面引入薄碳涂层（~ 300 nm）（例如，在10 μm聚对苯二甲酸乙二醇酯（PET）薄膜Al-PET的两侧沉积1 μm厚的铝），我们降低了MPCC与正极材料之间的接触电阻。使用碳包覆Al-PET （C@Al-PET）作为CC， 6.0 ah石墨/LiCoO2袋状电池具有显著提高的快速充电能力和循环稳定性，通过多物理场模拟确定了其均匀化的电位分布和电极利用率。最重要的是，含有C@Al-PET CC的电池仍然可以通过严酷的冲击测试，有望在具有优越安全性的高速率lib中应用。

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引用次数: 0

Balancing reactant adsorption for ultra-stable electrocatalytic methanol oxidation reaction 超稳定电催化甲醇氧化反应中平衡反应物吸附

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-16 DOI: 10.1016/j.esci.2025.100430

Yang Liu , Ruyan Wu , Yongzhen Jin , Jiaye Dong , Hongju Li , Jianhui Wang

The practical application of the electrocatalytic methanol oxidation reaction (EMOR) has long been hindered by the lack of active and stable catalysts. Herein, we report a unique dealloyed PtMn catalyst on carbon cloth (d-PtMn/CC) characterized by a compressively strained Pt surface and a Mn concentration-gradient core. This d-PtMn/CC catalyst demonstrates EMOR activity that is 7–14 times higher than that of conventional Pt/CC catalysts in all-pH electrolytes, while exhibiting exceptional resistance to catalytic poisoning over a broad potential range of 0.4–1.2 V vs. reversible hydrogen electrode (RHE). When employed in direct methanol fuel cells, it achieves 111.6 mW cm⁻² for over 10 h at ultralow 0.59 mg_Pt cm⁻², substantially outperforming commercial Pt/C catalysts. Comparative analyses of adsorbed reactants/intermediates revealed that imbalanced adsorption of reactants on the catalyst surface is the primary cause of EMOR poisoning. The d-PtMn/CC catalyst, benefiting from surface compressive strain and ligand effects, maintains balanced reactant adsorption over the wide potential range, thereby achieving ultra-stable EMOR performance. These findings not only resolve the longstanding controversy regarding EMOR poisoning mechanism but also identify the effectiveness of the “ligand + surface strain” strategy in DMFCs, facilitating its practical applications.

由于缺乏活性稳定的催化剂，电催化甲醇氧化反应（EMOR）的实际应用一直受到阻碍。在此，我们报道了一种独特的碳布合金PtMn催化剂（d-PtMn/CC），其特征是压缩应变的Pt表面和Mn浓度梯度的核心。这种d-PtMn/CC催化剂的EMOR活性比传统Pt/CC催化剂在全ph电解质中的EMOR活性高7-14倍，同时与可逆氢电极（RHE）相比，在0.4-1.2 V的宽电位范围内表现出优异的抗催化中毒能力。当用于直接甲醇燃料电池时，它在超低0.59 mgPt cm - 2下达到111.6 mW cm - 2超过10小时，大大优于商用Pt/C催化剂。吸附反应物/中间体的对比分析表明，反应物在催化剂表面的不平衡吸附是EMOR中毒的主要原因。d-PtMn/CC催化剂得益于表面压缩应变和配体效应，在较宽的电位范围内保持平衡的反应物吸附，从而实现超稳定的EMOR性能。这些发现不仅解决了长期以来关于EMOR中毒机制的争议，而且确定了“配体+表面应变”策略在dmfc中的有效性，为其实际应用提供了便利。

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引用次数: 0

Understanding the electro-chemo-mechanics of lithium metal anodes 了解锂金属阳极的电化学力学

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-16 DOI: 10.1016/j.esci.2025.100429

Quan Wu , Elin Dufvenius Esping , Marita Afiandika , Shizhao Xiong , Aleksandar Matic

Lithium metal batteries (LMBs) are candidates for next-generation energy storage due to their potential to increase energy density. However, the nonuniform electrodeposition of Li during cycling, plus the growth of Li dendrites and the side reactions between Li metal and the electrolyte, hinder the practical deployment of LMBs. The plating/stripping behavior of Li is an electro-chemo-mechanical process, and gaining a thorough understanding of its mechanisms is a cornerstone of LMB development. In this review, the current understanding of electro-chemo-mechanical processes on Li metal anodes is systematically summarized from the perspectives of Li plating/stripping in liquid- and solid-state electrolytes, the important role of the solid–electrolyte interphase, and the methodologies for understanding the electro-chemo-mechanics of the Li metal anode. The aim is to promote the development of LMBs through the optimization of Li metal anodes, which is based on understanding the fundamental processes occurring during electrochemical plating and stripping.

锂金属电池（lmb）由于具有提高能量密度的潜力，成为下一代储能系统的候选者。然而，循环过程中锂的电沉积不均匀，加上锂枝晶的生长和锂金属与电解质之间的副反应，阻碍了lmb的实际部署。锂的电镀/剥离行为是一个电化学-机械过程，深入了解其机制是LMB发展的基石。本文从液态和固态电解液中镀/剥离锂、固-电解质界面的重要作用以及理解锂金属阳极电化学力学的方法等方面，系统地总结了目前对锂金属阳极电化学力学过程的认识。目的是在了解电化学镀和剥离过程的基本过程的基础上，通过优化锂金属阳极来促进lmb的发展。

引用次数: 0

Heterointerface photo-electron effect in VO2(B)/V2O5 nanocomposite under long-wave infrared illumination for high-temperature microbolometers 高温微热计用长波红外照明下VO2(B)/V2O5纳米复合材料的异质界面光电子效应

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-09 DOI: 10.1016/j.esci.2025.100428

Jeongeun Mo , Haeri Park , Seungwan Woo , Donghee Park , Jeong Min Baik , Won Jun Choi

This study introduces a VO₂(B)/V₂O₅ nanocomposite thin film, fabricated via low-temperature sputtering (< 300 °C), as a high-performance thermistor material at high temperatures up to 125 °C for long-wave infrared (LWIR) microbolometers. By incorporating V₂O₅ into the VO₂(B) matrix and optimizing the heterointerface, the composite achieves a high temperature coefficient of resistance (TCR) of 2.19 (−/K) at room temperature and 1.19 (−%/K) at 125 °C. The synergistic properties of conductive VO₂(B) and insulating V₂O₅ enhance interfacial charge transfer, electron density, and thermal stability. Structural and compositional analyses confirm that oxygen vacancies and optimized band alignment play key roles in improving conductivity and photo-response. The microbolometers exhibit exceptional responsivity (2.3 kV/W) and fast response times (∼0.72 ms) at elevated temperature of 125 °C, highlighting the VO₂(B)/V₂O₅ nanocomposite as a robust and reliable material for LWIR detection in outdoor applications.

本研究介绍了一种通过低温溅射（< 300°C）制备的VO2(B)/V2O5纳米复合薄膜，作为长波红外（LWIR）微辐射热计在高达125°C高温下的高性能热敏电阻材料。通过将V2O5加入到VO2(B)基体中并优化异质界面，复合材料的高温电阻系数（TCR）在室温下为2.19(−%/K)，在125℃时为1.19（−%/K）。导电VO2(B)和绝缘V2O5的协同特性增强了界面电荷转移、电子密度和热稳定性。结构和成分分析证实，氧空位和优化的能带排列在提高电导率和光响应方面发挥了关键作用。微辐射热计在125°C的高温下表现出优异的响应性（2.3 kV/W）和快速响应时间（~ 0.72 ms），突出了VO2(B)/V2O5纳米复合材料作为户外应用中LWIR检测的坚固可靠的材料。

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引用次数: 0

Manganese-containing electrocatalysts for sustainable acidic oxygen evolution 可持续酸性析氧的含锰电催化剂

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-02 DOI: 10.1016/j.esci.2025.100427

Wenqi Jia, Licheng Miao, Xuejie Cao, Xiaojie Chen, Ting Jin, Fangyi Cheng, Lifang Jiao, Jun Chen

Proton exchange membrane water electrolysis (PEMWE) is recognized as an advanced technology for green hydrogen production and renewable energy conversion. However, the prohibitive cost and limited availability of precious-metal catalysts for the oxygen evolution reaction (OER) hamper its industrial application, and it is imperative to reduce the precious-metal loading by incorporating other elements or exploring alternative materials. Given the low cost and abundant reserves, manganese (Mn)-related catalysts have garnered increasing attention. This review systematically summarizes the progress of Mn-containing catalysts for acidic OER. Initially, we present an overview of fundamental characteristics and OER performance, especially the excellent stability, of Mn oxides. Then, we introduce the modulating effect of Mn in terms of the support, electronic structure, reaction mechanism, and surface reconstruction, followed by an analysis of the advancement of Mn-containing catalysts in PEMWE. Finally, the unresolved issues and future research directions for Mn-containing catalysts in acidic OER are critically discussed.

质子交换膜电解（PEMWE）是公认的绿色制氢和可再生能源转化的先进技术。然而，贵金属析氧催化剂的高昂成本和有限的可用性阻碍了其工业应用，通过加入其他元素或探索替代材料来减少贵金属的负载是势在必行的。锰（Mn）催化剂由于成本低、储量丰富而越来越受到人们的关注。本文系统地综述了酸性OER中含锰催化剂的研究进展。首先，我们概述了锰氧化物的基本特性和OER性能，特别是优异的稳定性。然后，从载体、电子结构、反应机理和表面重构等方面介绍了Mn的调制作用，并对含Mn催化剂在PEMWE中的研究进展进行了分析。最后，对酸性OER中含锰催化剂存在的问题和未来的研究方向进行了批判性的讨论。

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引用次数: 0

Engineering bimetallic cluster architectures: Harnessing unique “remote synergy effect” between Mn and Y for enhanced electrocatalytic oxygen reduction reaction 工程双金属簇结构：利用Mn和Y之间独特的“远程协同效应”增强电催化氧还原反应

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-01 DOI: 10.1016/j.esci.2024.100332

Yijian Song , Chao Han , Weijie Li , Xiufeng Yi , Qing Liao , Ji Zhou , Yaqin Zhou , Yitao Ouyang , Yingping Zhang , Qingqing Zheng , Anqiang Pan

Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance. Compared to single-atom catalysts, those incorporating both single atoms and clusters exhibit superior catalytic activity. However, the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood. In this study, we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method. Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect, thereby reducing energy barriers and enhancing the reaction kinetics. Additionally, the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N₃ coordination structures, resulting in excellent oxygen reduction reaction (ORR) performance. Consequently, the MnY/NC catalyst demonstrated a half-wave potential (E₁/₂) of 0.90 V and maintained stability in 0.1 M KOH, outperforming both Mn/NC and Pt/C. This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems, effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the “remote synergy effect” in heterogeneous catalysis.

将单个原子和簇整合到一个统一的催化系统中代表了一种提高催化性能的新策略。与单原子催化剂相比，那些结合单原子和簇的催化剂表现出更好的催化活性。然而，这些系统的共同构建及其催化效果的机制仍然具有挑战性且知之甚少。在这项研究中，我们通过简单的两步烧结法合成了一种具有MnY簇和Mn单原子的Mn - n - c催化剂。Y掺杂通过独特的协同效应促进了Mn簇的形成，优化了Mn的d带中心，从而降低了能垒，提高了反应动力学。此外，Y单原子的给电子能力促进了不饱和Mn-N₃配位结构的形成，从而获得了优异的氧还原反应（ORR）性能。因此，MnY/NC催化剂的半波电位（E₁/ 2）为0.90 V，在0.1 M KOH下保持稳定性，优于Mn/NC和Pt/C。这项工作强调了稀土金属在过渡金属中掺杂的潜力，可以创建稳定的单原子和簇体系，有效地利用它们的协同效应来获得卓越的催化性能，并验证了多相催化中“远程协同效应”的概念。

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引用次数: 0

Anode optimization strategies for zinc–air batteries 锌空气电池阳极优化策略

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-01 DOI: 10.1016/j.esci.2024.100309

Ruo-Bei Huang , Meng-Yin Wang , Jian-Feng Xiong , Hua Zhang , Jing-Hua Tian , Jian-Feng Li

With issues of energy security and environmental crisis intensifying, we urgently need to develop energy storage systems with high energy density and high safety. Zinc–air batteries have attracted extensive attention for their energy density, safety, and low cost, but problems with the zinc anode—such as hydrogen evolution, corrosion, passivation, dendrite proliferation, and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life; these remain the key obstacles hindering the batteries’ further development. In this review paper, we briefly describe the reaction mechanism of zinc–air batteries, then summarize the strategies for solving the key issues in zinc anodes. These approaches are divided into three aspects: structural designs for the zinc anode; interface engineering; and electrolyte selection and optimization. We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.

随着能源安全和环境危机的加剧，我们迫切需要开发高能量密度、高安全性的储能系统。锌空气电池因其能量密度、安全性和低成本而受到广泛关注，但锌阳极的析氢、腐蚀、钝化、枝晶扩散和变形等问题导致锌空气电池库仑效率低、循环寿命短；这些仍然是阻碍电池进一步发展的主要障碍。本文简要介绍了锌-空气电池的反应机理，总结了锌阳极中关键问题的解决策略。这些方法分为三个方面：锌阳极的结构设计；接口工程;以及电解液的选择与优化。最后对锌空气电池锌阳极的改进提出了今后的研究方向。

引用次数: 0

Re-understanding and mitigating hydrogen release chemistry toward reversible aqueous zinc metal batteries 重新理解和减轻氢释放化学的可逆水性锌金属电池

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-01 DOI: 10.1016/j.esci.2024.100330

Bo Liu , Zhibin Xu , Cong Wei , Zixuan Zhu , Yanyan Fang , Xin Lei , Ya Zhou , Chongyang Tang , Shiyi Ni , Hongge Pan , Gongming Wang

Interfacial H₂ release severely limits the reversibility and feasibility of aqueous Zn metal batteries for large-scale energy storage. Different from the conventional perception that H₂ release mainly originates from the competition between hydrogen evolution reaction and Zn plating process, we herein surprisingly find that non-negligible H₂ is also generated during stripping due to the accelerated chemical corrosion of the newly exposed Zn surface. To address this issue, we systematically screened the organic additives with different molecular structures and functional groups. Interestingly, a positive correlation between the adsorption strength of additives and the ability to inhibit the interfacial hydrogen release is found. Taking cysteamine (MEA) as a model additive, a gradient solid electrolyte interphase (SEI) is in situ formed at the Zn surface, acting as a chemical “barrier” to isolate interfacial water molecules from electrode surface consequently enable a higher Coulombic efficiency (> 99.5%, 4000 cycles) compared with that of MEA-free electrolyte (98.1%, 189 cycles). This work provides a new understanding of the interfacial hydrogen release mechanism and the criteria for selecting additives for aqueous Zn metal anodes.

界面H2释放严重限制了水锌金属电池大规模储能的可逆性和可行性。与以往认为氢气释放主要来源于析氢反应和镀锌过程的竞争不同，我们惊奇地发现，在汽提过程中，由于新暴露的锌表面的化学腐蚀加速，也会产生不可忽略的氢气。为了解决这一问题，我们系统地筛选了具有不同分子结构和官能团的有机添加剂。有趣的是，添加剂的吸附强度与抑制界面氢释放的能力呈正相关。以半胱胺（MEA）为模型添加剂，在Zn表面原位形成梯度固体电解质界面相（SEI），作为化学“屏障”将界面水分子与电极表面隔离，从而获得更高的库仑效率(>；99.5%， 4000次循环)，而无mea电解质的回收率为98.1%，189次循环。这项工作为界面氢释放机理和选择锌金属阳极添加剂的标准提供了新的认识。

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引用次数: 0

Probing a solid electrolyte interphase layer with sub-nanometer pores using redox mediators 利用氧化还原介质探测具有亚纳米孔的固体电解质间相层

IF 42.9 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-05-01 DOI: 10.1016/j.esci.2024.100351

Ximei Lv , Jie Liu , Chenkun Li , Fengjiao Yu , Dengji Xiao , Shulin Zhao , Yuping Wu , Yuhui Chen

The solid electrolyte interphase (SEI) layer is crucial for lithium-ion batteries and has a significant impact on the electrochemical performance of negative electrodes, particularly for conversion-type materials with large volume changes and metallic lithium anode. However, the SEI layer has not yet been well understood. In this work, we used redox mediators of various sizes to probe the SEI layer that formed in carbonate-based electrolytes. The SEI layer has diffusion channels that allow the mediators smaller than benzoquinone (5.7 Å) to pass, suggesting that lithium ions have to partially de-solvate to pass through. Additionally, due to partial desolvation, the diffusion coefficient in the diffusion channels was higher than that in the bulk electrolytes. Both lithium salts and solvents influenced the size and areal density of channels. Herein, we aim to enhance comprehension of SEI structure and provide a method to study porous SEI layers using mediators, which can be extended to other electrochemical systems.

固体电解质间相（SEI）层对锂离子电池至关重要，对负极的电化学性能有重要影响，特别是对于体积变化大的转换型材料和金属锂阳极。然而，人们还没有很好地理解SEI层。在这项工作中，我们使用不同尺寸的氧化还原介质来探测碳酸盐基电解质中形成的SEI层。SEI层具有扩散通道，允许比苯醌（5.7 Å）小的介质通过，这表明锂离子必须部分去溶剂化才能通过。此外，由于部分脱溶，扩散通道中的扩散系数高于散装电解质中的扩散系数。锂盐和溶剂都影响通道的大小和面密度。本文旨在增强对SEI结构的理解，并提供一种利用介质研究多孔SEI层的方法，该方法可扩展到其他电化学体系。

引用次数: 0

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