Journal of Energy Chemistry最新文献_第7页

Chemically interlinked and ionically conductive sulfonated graphene framework enabling fully integrated silicon anodes for high-performance Li-ion batteries 化学互连和离子导电磺化石墨烯框架，使高性能锂离子电池完全集成硅阳极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-22 DOI: 10.1016/j.jechem.2025.12.026

Yuanyuan Yu , Yuanqi Kang , Jiadeng Zhu , Junhua Zhang , Mengjin Jiang

Silicon (Si) anodes offer an ultrahigh theoretical capacity but face two major barriers to commercialization: severe structural degradation caused by significant volume changes and sluggish ion transport kinetics due to the discontinuous ionic conductance of conventional binders. To address these challenges, we develop a fully integrated Si anode using sulfonated graphene (SG) as a dual-functional ion-conductive and mechanical reinforcing framework within a conventional carboxymethyl cellulose/styrene-butadiene rubber (CMC/SBR) binder. Thermally activated reactions during electrode fabrication establish covalent sulfonate ester bonds between SG and CMC, elastic carboxylate crosslinks between SBR and CMC, and chemical anchoring between the binders and Si particles, which are all further reinforced by hydrogen bonding. This multi-bonding network not only dissipates mechanical stress and maintains electronic connectivity via embedded C65 carbon but also significantly enhances Li⁺ transport through high intrinsic ionic conductivity of SG, facilitating the formation of a stable solid electrolyte interphase (SEI). The resulting Si@CMC/SBR/SG anode delivers a high initial capacity of 3513.2 mAh g⁻¹ and retains 77% capacity after 500 cycles at 2 A g⁻¹. It achieves 762 mAh g⁻¹ at 4 A g⁻¹ and practical areal capacities exceeding 4 mAh cm⁻². Full-cell tests with NCM811 cathodes confirm 86.2% capacity retention after 100 cycles. This work demonstrates a pragmatic and scalable integration paradigm for durable, high-energy-density Si anodes.

硅（Si）阳极提供了超高的理论容量，但面临商业化的两个主要障碍：由于显着的体积变化引起的严重结构降解和由于传统粘合剂的不连续离子电导导致的离子传输动力学缓慢。为了解决这些挑战，我们开发了一种完全集成的硅阳极，使用磺化石墨烯（SG）作为双功能离子导电和机械增强框架，在传统的羧甲基纤维素/丁苯橡胶（CMC/SBR）粘合剂中。在电极制作过程中，热激活反应在SG和CMC之间建立了共价磺酸酯键，在SBR和CMC之间建立了弹性羧酸交联，在粘合剂和Si颗粒之间建立了化学锚定，这些都通过氢键进一步加强。这种多键网络不仅可以通过嵌入的C65碳来消散机械应力并保持电子连接，还可以通过SG的高固有离子电导率显著增强Li+的传输，促进稳定固体电解质界面（SEI）的形成。由此产生的Si@CMC/SBR/SG阳极提供3513.2 mAh g - 1的高初始容量，并在2 a g - 1下循环500次后保持77%的容量。它在4a1g - 1时达到762 mAh g - 1，实际面积容量超过4mah cm - 2。使用NCM811阴极的全电池测试确认100次循环后容量保持率为86.2%。这项工作展示了一种实用的、可扩展的集成范例，用于耐用、高能量密度的硅阳极。

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引用次数: 0

Unlocking high-rate MXenes as lithium-ion battery anodes via Σ7 coincidence site lattice grain boundaries 通过Σ7重合点晶格晶界解锁高速率MXenes作为锂离子电池阳极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-19 DOI: 10.1016/j.jechem.2025.12.023

Yifan Wu , Zhongyong Zhang , Shangquan Zhao , Bin Huang , Neng Li , Naigen Zhou

Grain boundaries (GBs), particularly Σ7 coincidence site lattice (CSL) defects experimentally observed in MXenes, significantly influence their performance as lithium-ion battery (LIB) anodes. This work systematically investigates the impact of Σ7 GBs on MXene electrochemical properties, with a focus on rate capability. The results indicated that Σ7 GB formation is thermodynamically favored in Ti₂C, Nb₂C, and Mo₂C MXenes compared to other M₂C compositions, with stability further enhanced by oxygen and sulfur surface functionalization. These GBs induce substantial geometric distortions that reduce surface charge localization while enhancing electrical conductivity in Ti₂CO₂. The altered electronic structure at GB sites weakens lithium adsorption strength without promoting lithium dendrite formation. Furthermore, diffusion kinetics calculations reveal significantly reduced lithium diffusion barriers at Σ7 GBs in Ti₂C, Mo₂C, and Mo₂CS₂ compared to pristine materials. Mechanistic analysis attributes this enhancement to diminished charge localization at GB regions, which generates a “charge pool” effect—a zone of uniformly distributed free charge observed in Ti₂C and Mo₂C. This charge pool not only facilitates ultra-low lithium diffusion barriers (as low as 11 meV in M₂C at 0.1 V vs. Li⁺/Li) but also enhances potential responsiveness of diffusion kinetics. Our findings establish the intentional introduction of Σ7 GBs as an effective strategy for designing high-rate MXene anodes. This work provides fundamental insights into GB-enhanced electrochemical mechanisms in 2D materials, offering crucial theoretical guidance for the design of high-rate anode materials.

MXenes中晶界（GBs），特别是Σ7重合点阵（CSL）缺陷，对其作为锂离子电池（LIB）阳极的性能有显著影响。这项工作系统地研究了Σ7 gb对MXene电化学性能的影响，重点是速率能力。结果表明，与其他M2C组分相比，在Ti2C、Nb2C和Mo2C MXenes中Σ7 GB的形成在热力学上更有利，并且通过氧和硫的表面官能化进一步增强了稳定性。这些gb诱导了大量的几何畸变，减少了表面电荷的局部化，同时增强了Ti2CO2中的导电性。GB位电子结构的改变削弱了锂的吸附强度，但没有促进锂枝晶的形成。此外，扩散动力学计算表明，与原始材料相比，Ti2C， Mo2C和Mo2CS2中Σ7 gb的锂扩散屏障显著降低。机理分析将这种增强归因于GB区域电荷局域化的减弱，这产生了“电荷池”效应——在Ti2C和Mo2C中观察到一个均匀分布的自由电荷区。这种电荷池不仅有利于超低锂扩散势垒（与Li+/Li相比，0.1 V时M2C的锂离子扩散势垒低至11 meV），而且还增强了扩散动力学的潜在响应性。我们的研究结果确立了有意引入Σ7 gb作为设计高速率MXene阳极的有效策略。这项工作为二维材料中gb增强的电化学机制提供了基本的见解，为设计高速率阳极材料提供了重要的理论指导。

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引用次数: 0

Synergistic pinning and piezoelectric effects in CNT/BaTiO3 network for SiO-based anodes toward ultra-stable lithium batteries 超稳定锂电池用碳纳米管/BaTiO3阳极网络的协同钉钉和压电效应

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-19 DOI: 10.1016/j.jechem.2025.12.025

Feng Sun , Anjun Hu , Junmei Han , Shenghai Xin , Zhihui Ma , Youwei Wang , Jianbin Li , Qi Wan , Ruidie Tang , Shaofei Wu , Xuanhui Qu , Ping Li

Silicon dioxide (SiO) is regarded as a promising anode candidate for high-energy-density lithium-ion batteries (LIBs) owing to its superior theoretical specific capacity. However, SiO anodes encounter substantial challenges, including substantial volume expansion and persistent growth of a thick solid electrolyte interphase (SEI). In this work, a composite conductive network with dual pinning and piezoelectric effects is proposed, which is cleverly designed to improve the electrochemical reaction kinetics of the electrode. Within the proposed network architecture, single-walled carbon nanotubes (CNTs) serve as fast electronic conductors and structural protective layers, forming a three-dimensional (3D) coating network on the surface of SiO particles. Barium titanate (BTO) nanoparticles are anchored at the nodes of the CNT network through the formation of rigid anchor points, dispersing stress throughout the network. Concurrently, mechanical stress induced by electrochemical reactions prompts BTO to generate a local electric field, facilitating Li⁺ transport. Consequently, the developed anode (SiO@PCB) demonstrates remarkable electrochemical performance in LIBs, exhibiting a capacity retention rate of 94% even after 500 cycles at 1 A g⁻¹. Furthermore, a capacity retention of 71.6% is demonstrated by SiO@PCB anode after 1000 cycles at 5 C in sulfide-based all-solid-state LIBs using an NCM83 cathode. This composite conductive network structure provides an effective guidance plan for achieving interface stability and long-term lithium storage of Si-based anodes.

二氧化硅（SiO）由于其优越的理论比容量，被认为是高能量密度锂离子电池（LIBs）极有前途的阳极候选材料。然而，SiO阳极面临着巨大的挑战，包括大量的体积膨胀和厚固体电解质界面（SEI）的持续生长。在这项工作中，提出了一种具有双钉钉和压电效应的复合导电网络，该网络的设计巧妙地改善了电极的电化学反应动力学。在提出的网络结构中，单壁碳纳米管（CNTs）作为快速电子导体和结构保护层，在SiO颗粒表面形成三维（3D）涂层网络。钛酸钡（BTO）纳米颗粒通过形成刚性锚点锚定在碳纳米管网络的节点上，在整个网络中分散应力。同时，电化学反应引起的机械应力促使BTO产生局部电场，有利于Li+的输运。因此，开发的阳极（SiO@PCB）在锂离子电池中表现出卓越的电化学性能，即使在1 a g−1下循环500次后，其容量保持率仍为94%。此外，在使用NCM83阴极的硫化物基全固态锂电池中，SiO@PCB阳极在5℃下循环1000次后，其容量保持率为71.6%。这种复合导电网络结构为实现硅基阳极的界面稳定性和锂的长期存储提供了有效的指导方案。

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引用次数: 0

Plasma promotion of CO2 methanation at low temperature: Validation of nonthermal effect on large-scale biogas upgrading 低温等离子体促进CO2甲烷化：大规模沼气升级的非热效应验证

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-19 DOI: 10.1016/j.jechem.2025.12.022

Wenjun Zhang , Takehisa Mimbu , Dae-Yeong Kim , Shinya Furukawa , Hyun-Ha Kim , Tomohiro Nozaki

Methanation of CO₂ in biogas offers an efficient and sustainable pathway compared to the carbon sources from carbon capture and utilization/storage (CCU/CCS) technologies, as it avoids a separate CO₂ capture step. Moreover, CO₂ from biogas combustion does not need to be recycled, owing to the carbon-neutral nature of biogas as a renewable energy source. Herein, we report biogas methanation using plasma catalysis for the first time in a packed-bed dielectric barrier discharge (DBD) reactor over 6 wt%-Ni/γ-Al₂O₃. The total gas flow rate reached up to 3000 mL min⁻¹ (CH₄/CO₂ = 60/40, CO₂/H₂ = 1/4), representing a large-scale study. The respective contributions of nonthermal plasma and methanation reaction heat were clarified. We observed that plasma-generated reactive species—vibrationally excited CO₂ and plasma-derived atomic hydrogen (PDAH)—play a crucial role. These species enhance CH₄ yield at low temperature and decrease reaction onset temperature (T_ON) compared to thermal catalysis. Also, pseudo-autonomous operation was confirmed at a total gas flow of 3000 mL min⁻¹ and DBD power of 11 W with CO₂ conversion of 77%, CH₄ selectivity >98%, and energy efficiency of 75%. Moreover, pulsed CH₄ injection experiments demonstrated that they endow the reaction system with the ability to withstand external disturbances, such as fluctuation of CH₄ content in biogas. These results demonstrate the feasibility and high efficiency of plasma-catalyzed biogas methanation. Moreover, a high flexibility of DBD makes it particularly suitable for upgrading decentralized or stranded biogas resources.

与碳捕集与利用/封存（CCU/CCS）技术相比，沼气中二氧化碳的甲烷化提供了一种高效和可持续的途径，因为它避免了单独的二氧化碳捕集步骤。此外，由于沼气作为可再生能源的碳中性特性，沼气燃烧产生的二氧化碳不需要再循环利用。在此，我们首次报道了等离子体催化沼气甲烷化在填充床介质阻挡放电（DBD）反应器中使用6 wt%-Ni/γ-Al2O3。总气量高达3000 mL min - 1 (CH4/CO2 = 60/40, CO2/H2 = 1/4)，为大规模研究。澄清了非热等离子体和甲烷化反应热各自的贡献。我们观察到等离子体产生的反应物质-振动激发CO2和等离子体衍生的原子氢(PDAH) -起着至关重要的作用。与热催化相比，这些物质提高了低温下CH4的产率，降低了反应起始温度。同时，在总气量为3000 mL min - 1、DBD功率为11 W、CO2转化率为77%、CH4选择性为98%、能效为75%的条件下，模拟自主运行。此外，脉冲CH4注入实验表明，它们赋予反应体系抵御外部干扰的能力，如沼气中CH4含量的波动。这些结果证明了等离子体催化沼气甲烷化的可行性和高效性。此外，DBD的高度灵活性使其特别适合于升级分散或搁浅的沼气资源。

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引用次数: 0

In situ/operando characterization of dynamic processes in lithium metal anodes 锂金属阳极动态过程的原位/操作表征

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-19 DOI: 10.1016/j.jechem.2025.12.024

Ben Su , Sida Huo , Lei Chai , Yue Wang , Meng Li , Anbin Zhou , Jingyi Qiu , Wendong Xue

Lithium metal anodes, with high theoretical capacity and low reduction potential, are widely regarded as the ideal solution to overcome the energy-density limits of current batteries. However, uncontrolled Li dendrite growth, repeated rupture and reconstruction of solid electrolyte interphase (SEI), and irreversible side reactions severely impede their commercial viability. A deep understanding of these complex failure mechanisms and their intrinsic links to electrochemical performance is essential to surmount these challenges. Conventional ex situ techniques only provide static snapshots and may distort transient information. In contrast, in situ/operando characterization enables real-time observation of electrochemical, structural, and chemical evolution under realistic conditions, offering dynamic insights inaccessible to ex situ analyses. Here, a comprehensive review of in situ/operando characterization techniques is presented, focusing on the revelation of dynamic processes in lithium metal anodes, including first, real-time visualization approaches for monitoring lithium nucleation, growth, dissolution, and spatial distribution; second, chemical/structural/property probes for probing SEI formation, evolution, and related changes; third, trackers of active Li consumption for quantitative discrimination of lithium species and resolution of gas-release. The principles, applicability, and limitations of each method are systematically elucidated. Finally, the perspectives on current technical bottlenecks are provided, and a roadmap for future research is outlined, aiming to bridge the gap between fundamental studies and the practical engineering of high-energy-density lithium metal batteries.

锂金属阳极具有较高的理论容量和较低的还原电位，被广泛认为是克服当前电池能量密度限制的理想方案。然而，不受控制的锂枝晶生长、固体电解质界面（SEI）的反复破裂和重建以及不可逆的副反应严重阻碍了它们的商业可行性。深入了解这些复杂的失效机制及其与电化学性能的内在联系对于克服这些挑战至关重要。传统的非原位技术只能提供静态快照，可能会扭曲瞬态信息。相比之下，原位/operando表征可以在现实条件下实时观察电化学、结构和化学演变，提供非原位分析无法获得的动态见解。本文对原位/operando表征技术进行了全面回顾，重点介绍了锂金属阳极的动态过程，包括用于监测锂成核、生长、溶解和空间分布的实时可视化方法；二是化学/结构/性质探针，用于探测SEI的形成、演化及相关变化；三是活性锂消耗跟踪器，用于锂种类的定量判别和气体释放的解决。系统地阐述了每种方法的原理、适用性和局限性。最后，对当前的技术瓶颈进行了展望，并概述了未来的研究路线图，旨在弥合高能量密度锂金属电池的基础研究与实际工程之间的差距。

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引用次数: 0

A nano-island surface architecture that unlocks synergistic kinetic and stability enhancements in P2-type sodium-ion battery cathodes 一种纳米岛表面结构，解锁了p2型钠离子电池阴极的协同动力学和稳定性增强

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-17 DOI: 10.1016/j.jechem.2025.12.021

Yu Huang , Gui Chu , Mao Wang , Kehan Li , Tongen Lin , Lili Wang , Yongqi Sun , Kui Li , Xiaobo Zhu

P2-type layered oxides are promising cathodes for sodium-ion batteries, yet their practical application is hindered by structural instability and parasitic interfacial reactions. Conventional surface coatings face a fundamental trade-off, where protective layers inevitably introduce additional Na⁺ transport paths and barriers. Here, we overcome this limitation by designing a multifunctional Nd-rich nano-island heterostructure on the P2-type cathode surface. Driven by a large lattice mismatch, this non-continuous architecture creates a thermodynamically stable interface where chemically rooted, electronically conductive nano-islands enhance charge transfer, while inter-island channels maintain open pathways for rapid Na⁺ diffusion. Theoretical calculations reveal that the heterostructure improves surface conductivity and anchors lattice oxygen via strong Nd–O bonds. Experimentally, in situ XRD confirms the mitigation of the detrimental P2-O2 phase transition by a buffering Z-phase and the recovery of lattice parameters upon discharge, while depth-resolved ToF-SIMS validates the formation of a thin, compact, and inorganic-rich cathode-electrolyte interphase that reduces interfacial side reactions. Consequently, the engineered cathode demonstrates exceptional rate performance (90 mA h g⁻¹ at 20 C), outstanding cycling stability (85.8 % retention over 200 cycles), and demonstrated potential in practical pouch cell configurations.

p2型层状氧化物是一种很有前途的钠离子电池阴极材料，但其实际应用受到结构不稳定性和寄生界面反应的阻碍。传统的表面涂层面临着一个基本的权衡，其中保护层不可避免地引入额外的Na+传输路径和屏障。在这里，我们通过在p2型阴极表面设计多功能富nd纳米岛异质结构来克服这一限制。在大晶格失配的驱动下，这种非连续结构创造了一个热力学稳定的界面，其中化学扎根的电子导电纳米岛增强了电荷转移，而岛间通道保持了Na+快速扩散的开放途径。理论计算表明，异质结构提高了表面导电性，并通过强Nd-O键锚定晶格氧。实验中，原位XRD证实了缓冲z相减缓了有害的P2-O2相变，并在放电时恢复了晶格参数，而深度分辨ToF-SIMS证实了薄、致密、富无机的阴极电解质界面相的形成，减少了界面副反应。因此，该工程阴极表现出优异的倍率性能（20℃下90 mA h g−1），出色的循环稳定性（200次循环保持率85.8%），并在实际的袋状电池配置中显示出潜力。

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引用次数: 0

Synergistic engineering of the electric double layer and solid electrolyte interphase by a trace glutamate-derived additive for stable aqueous zinc-ion batteries 用微量谷氨酸衍生添加剂对稳定水锌离子电池双电层和固体电解质界面的协同工程

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-17 DOI: 10.1016/j.jechem.2025.12.019

Dongyin Liu , Yuanjun Zhang , Yuhao Wu , Xiaoyang Zheng , Guanyao Wang , Hua-Kun Liu , Shi-Xue Dou , Chao Wu

Aqueous zinc-ion batteries (AZIBs) have garnered considerable attention as promising candidates for next-generation energy storage systems due to their inherent advantages. However, AZIBs have also constantly encountered interfacial challenges arising from the structure of the electric double layer (EDL) and the composition of the solid electrolyte interphase (SEI), fundamentally limiting their reversibility and cycling stability. Herein, we propose a novel trace additive strategy employing tetrasodium glutamate diacetate (TGD) to simultaneously reconstruct the EDL and form a stable SEI on the zinc anode surface. TGD molecules could preferentially adsorb on the zinc anode surface, which could displace water molecules from the inner Helmholtz plane (IHP) to reconstruct a water-deficient EDL and suppress hydrogen evolution reactions/water-induced parasitic reactions. Moreover, the adsorbed TGD molecules could also be involved in the formation of a stable organic–inorganic hybrid SEI, effectively stabilizing the anode/electrolyte interface, reducing interfacial impedance and facilitating uniform zinc deposition. Consequently, the symmetric cells deliver an outstanding cycling life of over 4800 h at 1 mA cm⁻² and 1 mA h cm⁻², and Zn||Cu cells achieve a high average Coulombic efficiency of 99.64 % for up to 2250 cycles. The Zn||PANI full cell with TGD-based electrolyte retains 91.32 % capacity after 2000 cycles at 3 A g⁻¹. These findings highlight TGD-based interface engineering as a viable strategy for high-performance AZIBs.

水性锌离子电池（azib）由于其固有的优点，作为下一代储能系统的有前途的候选者，已经引起了相当大的关注。然而，azib也不断遇到来自双电层（EDL）结构和固体电解质界面相（SEI）组成的界面挑战，从根本上限制了它们的可逆性和循环稳定性。在此，我们提出了一种新的微量添加剂策略，使用谷氨酸四钠（TGD）来同时重建EDL并在锌阳极表面形成稳定的SEI。TGD分子可以优先吸附在锌阳极表面，取代内部亥姆霍兹面（IHP）中的水分子，重建缺水EDL，抑制析氢反应/水诱导寄生反应。此外，吸附的TGD分子还可以参与形成稳定的有机-无机杂化SEI，有效地稳定阳极/电解质界面，降低界面阻抗，促进均匀的锌沉积。因此，对称电池在1ma cm - 2和1ma h cm - 2下的循环寿命超过4800小时，而Zn||Cu电池在2250次循环中实现了99.64%的平均库仑效率。采用tgd基电解质的Zn||PANI全电池在3ag−1下循环2000次后容量保持在91.32%。这些发现强调了基于tgd的界面工程是高性能azib的可行策略。

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引用次数: 0

Regulating solvation chemistry via co-solvent electrolyte for ultralow-temperature aqueous zinc-ion batteries 用助溶剂电解质调节超低温锌离子电池的溶剂化化学

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-17 DOI: 10.1016/j.jechem.2025.12.020

Jintao Qi , Yahan Meng , Apeng Li , Ze Xu , Xiang Li , Lei Yang , Mingming Wang , Pengfei Gao , Shaoming Huang

Aqueous zinc-ion batteries (AZIBs) hold great promise for large-scale energy storage due to their safety, low cost, and environmental compatibility. However, AZIBs face severe challenges, including cathode dissolution and anode dendrite growth, while their reliability under extreme conditions is limited by electrolyte instability. Electrolyte additives, especially organic molecule additives, provide an effective and cost-efficient strategy to address these issues. Herein, we report a novel nontoxic, green, low-cost, and water-miscible organic molecule additive used as a co-solvent, which synergistically reconstructs the solvation structure of Zn²⁺ and disrupts the strong bonding among H₂O molecules by modulating the electrostatic interactions among Zn²⁺, H₂O, and ClO₄⁻, suppressing water-induced side reactions and lowering the freezing point of the electrolyte, thereby optimizing Zn ion migration and deposition behavior. Consequently, Zn||Zn batteries exhibit excellent performance at ambient temperature (25 °C) and can still achieve over 2500 h of cycling life at a low temperature of −40 °C. It is worth noting that Zn||Zn batteries can also operate stably under the ultra-low temperature condition of −60 °C. Additionally, the co-solvent electrolyte suppresses the dissolution of vanadium-based cathodes under low-rate conditions, enabling Zn||VO₂ batteries to maintain a high capacity retention of 91 % after 600 cycles at 0.5 A g⁻¹ under ambient temperature (25 °C). Furthermore, at −40 °C, the Zn||VO₂ battery can operate for over 1000 h at a current density of 0.1 A g⁻¹. This work provides a new strategy for constructing high-performance AZIBs over a wide temperature range.

水锌离子电池（azib）由于其安全、低成本和环境兼容性，在大规模储能方面具有很大的前景。然而，azib面临着严峻的挑战，包括阴极溶解和阳极枝晶生长，而其在极端条件下的可靠性受到电解质不稳定性的限制。电解质添加剂，特别是有机分子添加剂，为解决这些问题提供了一种有效且经济的策略。本文报道了一种新型无毒、绿色、低成本、水可混溶的有机分子添加剂作为助溶剂，通过调节Zn2+、H2O和ClO4−之间的静电相互作用，抑制水诱导的副反应，降低电解质的冰点，从而协同重建Zn2+的溶剂化结构，破坏H2O分子之间的强键，从而优化Zn离子的迁移和沉积行为。因此，锌电池在环境温度（25°C）下表现出优异的性能，并且在- 40°C的低温下仍然可以实现超过2500 h的循环寿命。值得注意的是，Zn||锌电池在−60℃的超低温条件下也能稳定运行。此外，在低倍率条件下，共溶剂电解质抑制了钒基阴极的溶解，使Zn||VO2电池在环境温度（25°C）下，在0.5 a g−1下循环600次后保持91%的高容量保持率。此外，在−40°C下，Zn||VO2电池可以在0.1 a g−1的电流密度下工作超过1000小时。这项工作为在宽温度范围内构建高性能azib提供了一种新的策略。

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引用次数: 0

Sustainable biopolymer hydrogel electrolytes for electrochromics: Materials, mechanisms, and roadmaps to next-generation smart technologies 用于电致变色的可持续生物聚合物水凝胶电解质：材料、机制和下一代智能技术的路线图

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-16 DOI: 10.1016/j.jechem.2025.12.014

Pramod V. Rathod, Pooja V. Chavan, Hern Kim

Biopolymer-based hydrogel electrolytes are rapidly emerging as sustainable alternatives for electrochromic devices (ECDs) due to their environmental compatibility, tunable ionic conductivity, and mechanical flexibility. Recent advances leverage renewable biopolymers such as cellulose, chitosan, and alginate, along with their nanostructured derivatives, to create dynamic hydrogel matrices with optimized ionic transport and multifunctional properties. This review comprehensively details the evolution of biopolymer hydrogel electrolytes in ECDs by emphasizing structure-performance relationships, including molecular design, crosslinking chemistry, and interfacial engineering for enhanced electro-optical properties. However, despite notable progress, several critical bottlenecks remain: limited long-term operational stability under varying humidity and temperature, susceptibility to water evaporation and drying, narrow electrochemical voltage windows, and challenges in scaling for large-area device integration. These issues currently hinder their widespread deployment relative to synthetic counterparts. We critically analyze recent strategies to overcome these limitations, such as scalable fabrication techniques and adaptive encapsulation methods, aiming to accelerate material innovation and device performance optimization. Furthermore, the review highlights the expanding application scope of biopolymer-based ECDs, including adaptive smart windows, wearable biosensors, and sustainable display technologies. By integrating achievements with current challenges, this work offers a balanced roadmap toward durable, high-performance, and environmentally responsible electrochromic systems based on next-generation biopolymer hydrogels.

基于生物聚合物的水凝胶电解质由于其环境兼容性、可调离子电导率和机械灵活性，正迅速成为电致变色器件（ECDs）的可持续替代品。最近的进展是利用可再生生物聚合物，如纤维素、壳聚糖和海藻酸盐，以及它们的纳米结构衍生物，来创建具有优化离子传输和多功能特性的动态水凝胶基质。本文通过强调结构-性能关系，包括分子设计、交联化学和增强电光性能的界面工程，全面详细介绍了生物聚合物水凝胶电解质在ECDs中的发展。然而，尽管取得了显著进展，但仍存在几个关键瓶颈：在不同湿度和温度下的长期运行稳定性有限，对水分蒸发和干燥的敏感性，狭窄的电化学电压窗，以及在大面积设备集成方面的缩放挑战。这些问题目前阻碍了它们相对于合成对应物的广泛部署。我们批判性地分析了克服这些限制的最新策略，例如可扩展的制造技术和自适应封装方法，旨在加速材料创新和器件性能优化。此外，该综述还强调了基于生物聚合物的ecd的应用范围不断扩大，包括自适应智能窗口、可穿戴生物传感器和可持续显示技术。通过将现有成果与当前挑战相结合，这项工作为基于下一代生物聚合物水凝胶的持久、高性能、环保的电致变色系统提供了一个平衡的路线图。

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引用次数: 0

Layer-dependent ammonia activation on VOx/Cu inverse catalysts VOx/Cu反相催化剂的层依赖氨活化

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2025-12-16 DOI: 10.1016/j.jechem.2025.12.015

Youbin Wu , Dongsen Zhang , Shengdi Zhao , Ruihan Rao , Yingli Liu , Yuanjie Bao , Yan Zhang , Geng Sun , Rentao Mu , Wenpo Shan , Yun Liu , Hong He

Overcoming the kinetic barrier of N–H bond activation in NH₃ remains a central challenge in enabling efficient ammonia decomposition as well as thermocatalytic and electrocatalytic ammonia oxidation. Oxide-on-metal inverse catalysts offer promising opportunities to address this challenge; however, the role of oxide overlayer thickness in governing surface structures and reactivity is still poorly understood. Herein, we have elucidated the layer-dependent atomic structure of vanadium oxide overlayers on Cu(1 1 1) surfaces and its implications for NH₃ adsorption, using a combination of high-resolution scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. Despite sharing the same vanadium oxidation state (V³⁺), VO_x overlayers on Cu(1 1 1) adopt distinct atomic structures depending on the overlayer thickness. A nonlinear correlation is observed between VO_x overlayer thickness and N–H activation capability. The surface-V₂O₃ phase formed by 2–3 VO_x layers exhibits the highest activity, enabling both molecular and dissociative adsorption of NH₃. In contrast, thicker bulk-V₂O₃(0001) (>3 VO_x layers) only shows molecular adsorption without dissociation, while the monolayer VO(1 1 1) surface exhibits negligible NH₃ adsorption. These findings underscore the pivotal influence of oxide overlayer thickness in modulating oxide-on-metal inverse catalyst systems, providing atomic-level insights that can guide the rational design of high-performance catalytic materials for NH₃ activation.

克服NH3中N-H键激活的动力学障碍仍然是实现高效氨分解以及热催化和电催化氨氧化的核心挑战。金属上氧化物反催化剂为解决这一挑战提供了很有希望的机会；然而，氧化层厚度在控制表面结构和反应性中的作用仍然知之甚少。在此，我们利用高分辨率扫描隧道显微镜（STM）、x射线光电子能谱（XPS）和密度泛函理论（DFT）计算，阐明了Cu（11 11）表面氧化钒覆盖层的层依赖原子结构及其对NH3吸附的影响。尽管具有相同的钒氧化态（V3+），但Cu（11 11 1）上的VOx覆盖层根据覆盖层厚度采用不同的原子结构。VOx层厚度与N-H活化能力之间存在非线性相关关系。由2-3层VOx形成的表面- v2o3相表现出最高的活性，可以同时进行NH3的分子吸附和解离吸附。相比之下，较厚的大块v2o3 (0001) （>；3 VOx层）只表现出分子吸附而不解离，而单层VO（11 11）表面对NH3的吸附可以忽略不计。这些发现强调了氧化物覆盖层厚度对调节氧化物-金属逆催化剂体系的关键影响，提供了原子水平的见解，可以指导合理设计用于NH3活化的高性能催化材料。

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引用次数: 0