Journal of Energy Chemistry最新文献_第4页

Plasma-engineered interfacial built-in electric fields in wood-templated heterostructures for synergistic bifunctional electrocatalysis 等离子体工程界面内置电场在木模板异质结构协同双功能电催化

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-27 DOI: 10.1016/j.jechem.2025.12.037

Chang Liu, Guijuan Wei, Zaixing Zheng, Xixia Zhao, Xin Zhao, Honglei Chen

Realizing the multi-species adsorption in electrocatalysis requires precise control of interfacial electronic structures at heterojunctions, yet this remains a fundamental challenge under industrial operational conditions. Here, we develop a gradient plasma nano-engineering strategy to construct Ru-Ni@Ni₂P heterostructures within hierarchically porous P-doped carbonized wood (PCW) monoliths. This approach simultaneously achieves plasma-induced phase transformation/phosphidation and the creation of a continuous built-in electric field (BIEF) at the heterointerface. Ultraviolet photoelectron spectroscopy and Kelvin probe force microscopy confirm that a work function difference of 0.15 eV drives spontaneous electron transfer from Ru-Ni to Ni₂P, generating a robust BIEF with a 42.3 mV potential gradient. This BIEF induces a synergistic optimization of the adsorption energetics for multiple reactive species (H and HMF). Specifically, the catalyst achieves an ultralow hydrogen evolution overpotential (96 mV at 100 mA cm⁻²) with near-ideal ΔG_H* (0.04 eV), and concurrently drives efficient HMF oxidation at 1.35 V (100 mA cm⁻²), 230 mV below the oxygen evolution potential, via an optimized reaction pathway (HMF → HMFCA → FFCA → FDCA). The native wood microstructure and plasma-sculpted nanoarrays ensure efficient mass transport and BIEF-enhanced bubble repulsion, yielding exceptional durability. This work establishes a general paradigm based on interfacial electric field programming within sustainable scaffolds and offers a transformative platform for energy-efficient electrochemical refining and hydrogen production.

实现电催化中的多物质吸附需要精确控制异质结的界面电子结构，但在工业操作条件下，这仍然是一个基本的挑战。在这里，我们开发了一种梯度等离子体纳米工程策略，在分层多孔p掺杂碳化木材（PCW）单体中构建Ru-Ni@Ni2P异质结构。这种方法同时实现了等离子体诱导的相变/磷化，并在异质界面处产生了连续的内置电场（BIEF）。紫外光电子能谱和开尔文探针力显微镜证实，0.15 eV的功函数差驱动了Ru-Ni向Ni2P的自发电子转移，产生了42.3 mV电位梯度的强劲BIEF。该BIEF诱导了多种反应物质（H和HMF）吸附能量的协同优化。具体而言，该催化剂在接近理想的ΔGH* (0.04 eV)条件下实现了超低析氢过电位（96 mV, 100 mA cm−2），同时通过优化的反应途径（HMF→HMFCA→FFCA→FDCA），在低于析氧电位230 mV的1.35 V （100 mA cm−2）下实现了HMF的高效氧化。原生木材微结构和等离子体雕刻的纳米阵列确保了有效的质量传输和bief增强的气泡排斥，产生了卓越的耐久性。这项工作建立了一个基于可持续支架内界面电场规划的通用范例，并为节能电化学精炼和制氢提供了一个变革性的平台。

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引用次数: 0

Bifunctional crosslinking-induced structural engineering towards improved sodium storage in pitch-derived hard carbon 改善沥青衍生硬碳中钠储存的双功能交联诱导结构工程

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-04 DOI: 10.1016/j.jechem.2025.12.048

Yanqing Wu , Ying Mo , Wang Zhou , Liqiang Ouyang , Biao Zheng , Guoku Liu , Hui Liu , Aiping Hu , Yan Duan , Wenbin Zhong , Jilei Liu

The construction of crosslinking structures in pitch-derived carbons is essential for disrupting intrinsic π-π stacking and achieving high performance sodium-ion batteries. However, the structural collapse caused by the pyrolysis-oxidation kinetic mismatch and the challenge of rational crosslinker selection remain significant obstacles. Herein, we introduce a bifunctional crosslinking agent that simultaneously accelerates oxidative ring-opening and reinforces covalent network formation, thereby overcoming the kinetic imbalance between oxidation and pyrolysis. Specifically, 3, 4, 9, 10-perylenetetracarboxylic dianhydride (PTCDA) not only promotes generating oxygen-free radicals due to the low bond energy of its C–O bonds but also reacts with oxygen-containing functional groups in oxidized pitch to form covalent linkages, thereby further increasing crosslinking density. Consequently, the resulting hard carbons exhibit expanded interlayer spacing (d₀₀₂) and a defect-rich hierarchical porous structure. This gives rise to high reversible capacity (328.32 mAh g⁻¹), excellent rate capability (171.54 mAh g⁻¹ at 400 mA g⁻¹), and outstanding cycling stability (93.4% capacity retention after 200 cycles at 40 mA g⁻¹). Moreover, its practical feasibility is demonstrated in full cells. This work establishes a robust paradigm for developing next-generation hard carbon anodes by synergistically optimizing the bonding configuration of precursors, pore architecture, and carbon framework, while offering deep mechanistic insight into the pitch crosslinking process.

在沥青衍生碳中构建交联结构对于破坏本征π-π堆积和实现高性能钠离子电池至关重要。然而，由热解氧化动力学失配引起的结构崩溃和合理选择交联剂的挑战仍然是重要的障碍。本文介绍了一种双功能交联剂，该交联剂可以同时加速氧化开环和加强共价网络的形成，从而克服氧化和热解之间的动力学不平衡。具体来说，3,4,9,10 -苝四羧酸二酐（PTCDA）由于其C-O键的键能较低，不仅能促进氧自由基的生成，还能与氧化沥青中的含氧官能团反应形成共价键，从而进一步提高交联密度。因此，所得到的硬碳表现出扩大的层间距（d002）和富含缺陷的分层多孔结构。这产生了高可逆容量（328.32 mAh g - 1），出色的倍率容量（171.54 mAh g - 1, 400 mA g - 1），以及出色的循环稳定性（在40 mA g - 1下200次循环后，容量保持率为93.4%）。并在全电池中验证了其实际可行性。这项工作通过协同优化前驱体、孔隙结构和碳框架的键合配置，为开发下一代硬碳阳极建立了一个强大的范例，同时为节距交联过程提供了深入的机制见解。

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引用次数: 0

Solid additive-mediated modulation of donor and acceptor aggregation for regulating phase separation in efficient all-polymer solar cells 固体添加剂介导的供体和受体聚集调节高效全聚合物太阳能电池的相分离

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-06 DOI: 10.1016/j.jechem.2025.12.042

Zhenmin Zhao , Yuanxian Liang , Hua Tang , Jiancheng Zhong , Chenxi Cao , Yuanyuan Qin , Hongxiang Li , Liang Bai , Wei Pang , Guanlin Chen , Safakath Karuthedath , Zhipeng Kan

By tuning the active layer morphology with additives, the power conversion efficiency (PCE) of all-polymer solar cells (all-PSCs) has surpassed 19%. However, the distinct aggregation behaviors of donors and acceptors often pose limitations to further performance enhancements. Herein, we introduce a novel solid additive, biphenyl (BPE), to simultaneously modulate the morphologies of both donor and acceptor materials. Characterized by its strong crystallinity and excellent compatibility with the acceptor material, BPE effectively increases the aggregation of the donor while reducing that of the acceptor. Therefore, the blend film processed with BPE achieves superior phase separation, resulting in a reduced trap density and lower energetic disorder, which culminates in an optimum PCE of 18.5% with an open-circuit voltage of 942 mV in binary devices composed of PBQx-TCl: PY-IT. Moreover, when BPE was used to selectively modulate the acceptor phase using a pseudo-planar heterojunction (PPHJ) active layer, a PCE of 17.4% was achieved, highlighting the effectiveness of enhancing the solubility of the acceptor phase in fabricating all-PSCs based on PPHJ. Our findings underscore the role of BPE-based additives in optimizing active layer phase separation, thereby facilitating the solution-processable fabrication of highly efficient all-PSCs.

通过添加添加剂调节活性层形态，全聚合物太阳能电池的功率转换效率（PCE）超过19%。然而，供体和受体不同的聚合行为往往会限制进一步的性能增强。在此，我们引入了一种新的固体添加剂，联苯（BPE），以同时调节供体和受体材料的形态。BPE具有很强的结晶度和与受体材料良好的相容性，可以有效地增加供体的聚集，同时降低受体的聚集。因此，在PBQx-TCl: PY-IT组成的二元器件中，用BPE加工的共混膜实现了优异的相分离，从而降低了陷阱密度，降低了能量无序，最终达到了最佳PCE为18.5%，开路电压为942 mV。此外，当BPE利用伪平面异质结（PPHJ）活性层选择性调制受体相时，PCE达到17.4%，突出了增强受体相溶解度在基于PPHJ制备全pscs中的有效性。我们的研究结果强调了基于bpe的添加剂在优化活性层相分离中的作用，从而促进了高效全psc的溶液可加工制造。

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引用次数: 0

Unveiling the valid active site of copper nano-electrocatalysts by surface reconstruction for enhanced nitrate reduction to ammonia 通过表面重构揭示铜纳米电催化剂的有效活性位点，促进硝酸还原为氨

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-12 DOI: 10.1016/j.jechem.2026.01.001

Jiewen Liu , Susu Duan , Ankang Chen , Xuan Liu , Chuanjin Tian , Nan Gao , Yongming Sui , Bo Zou

Electrochemical conversion of nitrate (NO₃⁻) to ammonia (NH₃) is a prospective way to balance the nitrogen cycle for the environment. Currently, the actual active phase of copper-based materials as nitrate reduction reaction (NO₃⁻RR) catalysts is controversial. Herein, the surface-reconstructed copper nanowires (Cu NWs-SR) with excellent antioxidant properties are proposed to build efficient active sites to promote the NO₃⁻RR, revealing the key role of Cu (111) crystal planes. The electrochemical test results show an average NO₃⁻ conversion of 95% over an ultra-wide NO₃⁻ concentration range (20–500 mM), with NH₃ selectivity of 94% and Faraday efficiency (FE) of 96%, respectively. The catalyst demonstrated high stability of over 100 h, achieving a FE of 93% at a current density of approximately 300 mA cm⁻², with a yield rate of 17.6 mg h⁻¹ cm⁻¹. In situ electrochemical characterization and density functional theory calculations reveal that the reconstructed Cu (111) crystal planes serve as active sites to promote the NO₃⁻RR, while suppressing the hydrogen evolution reaction (HER). This study is valuable in revealing the origin of the active phase of Cu-based catalysts over NO₃⁻RR, which contributes to the catalytic performance across a wide range of NO₃⁻ concentrations.

硝酸盐（NO3−）的电化学转化为氨（NH3）是平衡环境氮循环的一种有前景的途径。目前，铜基材料作为硝酸还原反应（NO3−RR）催化剂的实际活性相存在争议。本文提出了具有优异抗氧化性能的表面重构铜纳米线（Cu NWs-SR），以构建有效的活性位点促进NO3−RR，揭示了Cu（111）晶体平面的关键作用。电化学测试结果表明，在超宽NO3−浓度范围（20 ~ 500 mM）内，NO3−的平均转化率为95%，NH3选择性为94%，法拉第效率（FE）为96%。该催化剂表现出100 h以上的高稳定性，在约300 mA cm−2的电流密度下，FE达到93%，产率为17.6 mg h−1 cm−1。原位电化学表征和密度泛函理论计算表明，重构的Cu（111）晶面是促进NO3−RR的活性位点，同时抑制析氢反应（HER）。这项研究揭示了cu基催化剂在NO3 - RR上的活性相的起源，这有助于在广泛的NO3 -浓度范围内的催化性能。

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引用次数: 0

MBenes on the rise: progress, prospects, and multifunctional applications MBenes的崛起：进展、前景和多功能应用

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-08 DOI: 10.1016/j.jechem.2025.11.058

Guodong Zou , Hengyuan Zhang , Sen Li , Yu Zhang , Zhongchen Fang , Jinyu Li , Zhibo Xu , Tianyue Zhang , Yangyang Wang , Carlos Fernandez , Qiuming Peng

MBenes, an emerging family of two-dimensional (2D) transition metal borides, have attracted considerable interest owing to their tunable electronic structures, rich physicochemical properties, and broad application potential. In recent years, extensive research efforts have led to the development of diverse synthetic strategies and a rapidly expanding range of applications across multiple disciplines. Although several excellent reviews have summarized the progress of MBenes from specific perspectives, a comprehensive review that innovatively categorizes their synthesis methods, unique properties, and functional applications remains absent. To address this gap, this review provides a thorough overview of the synthesis, structural attributes, distinctive properties, and diverse applications of MBenes. Beginning with a critical evaluation of synthesis methodologies, the review highlights advances in etching and delamination techniques, along with their impacts on material morphology and structure. It further examines the electronic structure and surface chemistry of MBenes to elucidate their physicochemical and mechanical properties. Subsequently, the key performance metrics of MBenes are comprehensively surveyed in applications spanning energy storage and conversion, physical devices, sensors, water purification, and biomedical fields. Finally, the review discusses persistent challenges such as scalable synthesis and defect control, and suggests promising future research directions, including green synthesis routes, machine learning-assisted optimization, and the integration of multifunctional devices. By positioning MBenes as a versatile platform for interdisciplinary innovation, this work aims to provide foundational insights that will guide the development of next-generation 2D materials.

MBenes是一类新兴的二维（2D）过渡金属硼化物，由于其具有可调谐的电子结构、丰富的物理化学性质和广泛的应用潜力而引起了人们的广泛关注。近年来，广泛的研究工作导致了多种合成策略的发展，并迅速扩大了跨学科的应用范围。虽然有一些优秀的综述从特定的角度总结了MBenes的进展，但对其合成方法、独特性质和功能应用进行创新分类的全面综述仍然缺乏。为了弥补这一空白，本文综述了MBenes的合成、结构属性、独特性质和各种应用。从对合成方法的批判性评价开始，综述强调了蚀刻和分层技术的进展，以及它们对材料形态和结构的影响。进一步研究了MBenes的电子结构和表面化学，以阐明其物理化学和机械性能。随后，对MBenes在能源存储和转换、物理设备、传感器、水净化和生物医学领域的应用中的关键性能指标进行了全面调查。最后，综述讨论了可扩展合成和缺陷控制等持续存在的挑战，并提出了有希望的未来研究方向，包括绿色合成路线，机器学习辅助优化和多功能设备集成。通过将MBenes定位为跨学科创新的多功能平台，这项工作旨在提供指导下一代2D材料开发的基础见解。

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引用次数: 0

Ta3N5-based solar-driven water splitting with broadband visible-light absorption 基于ta3n5的太阳能驱动水分解与宽带可见光吸收

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2025-12-27 DOI: 10.1016/j.jechem.2025.12.035

Ying Luo , Hui Yang , Yaru Lei , Kuo Liu , Zheng Wang

Tantalum nitride (Ta₃N₅), a semiconductor photocatalyst with a narrow bandgap and suitable band positions, exhibits broad absorption across the visible light spectrum and a theoretical solar energy conversion efficiency of up to 15.9%, demonstrating significant potential in photocatalytic overall water splitting. This review systematically summarizes recent advances in Ta₃N₅-based photocatalytic overall water splitting, focusing on strategies for enhancing performance through bulk and surface modifications. Key aspects discussed include synthesis methods design, doping strategies, morphology control, surface functionalization, and heterostructure construction. These approaches collectively aim to address critical challenges in practical applications, such as the reduction of bulk defects, suppression of charge recombination, and enhancement of surface reaction kinetics, thereby mitigating severe charge recombination and activity stability issues. Finally, future research directions and development prospects for Ta₃N₅-based photocatalysts are discussed, aiming to provide theoretical guidance and technical references for the design of highly efficient and stable Ta₃N₅-based photocatalytic systems.

氮化钽（Ta3N5）是一种半导体光催化剂，具有窄带隙和合适的能带位置，在可见光光谱中具有广泛的吸收，理论太阳能转换效率高达15.9%，在光催化整体水分解方面具有重要的潜力。本文系统总结了基于ta3n5的光催化整体水分解的最新进展，重点介绍了通过体修饰和表面修饰来提高性能的策略。讨论的关键方面包括合成方法设计、掺杂策略、形貌控制、表面功能化和异质结构的构建。这些方法共同旨在解决实际应用中的关键挑战，例如减少体缺陷，抑制电荷重组，增强表面反应动力学，从而减轻严重的电荷重组和活性稳定性问题。最后讨论了ta3n5基光催化剂未来的研究方向和发展前景，旨在为设计高效稳定的ta3n5基光催化体系提供理论指导和技术参考。

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引用次数: 0

Engineering dual-salt hybrid-solvation electrolytes with moderate coordination: enabling low-temperature kinetics and high-voltage stability in lithium batteries 工程双盐混合溶剂化电解质与适度协调：使低温动力学和高压稳定性的锂电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-19 DOI: 10.1016/j.jechem.2026.01.019

Jiayue Peng , Yuwei Li , Canfu Zhang , Saisai Qiu , Shijie Cheng , Jia Xie

The widespread adoption of lithium-metal batteries (LMBs) faces a critical challenge: the absence of electrolytes that can simultaneously withstand low-temperature and high-voltage operating conditions. To address this fundamental limitation, we introduce a mechanistically guided electrolyte design strategy based on a molecularly engineered hybrid-solvation structure combined with a synergistic dual-salt system. Our approach uniquely employs a fluorinated solvent mixture—comprising fluoroethylene carbonate (FEC) and moderately coordinating fluorinated ethyl acetate (TFEA)—to reconfigure the Li⁺ solvation environment. This tailored solvation sheath facilitates anion participation and achieves an optimal balance between contact ion pairs (CIP) and aggregates (AGG), thereby significantly lowering the Li⁺ desolvation energy barrier. Furthermore, the incorporation of a LiFSI-LiClO₄ dual-salt formulation works in concert to construct highly conductive LiF-rich interphases on both electrodes: a stable solid-electrolyte interphase (SEI) on the Li anode and a robust cathode-electrolyte interphase (CEI) under high voltages. As a result, Li||NCM811 cells exhibit excellent cycling stability from room temperature to −20 °C, together with high capacity retention at high discharge rates (up to 3 C) under a moderate charging rate (0.5 C) and stable operation up to 4.7 V, substantially outperforming conventional single-salt electrolytes. This work establishes a transferrable solvation-interphase design paradigm that links coordination chemistry to interfacial stability, advancing LMBs toward practical, high-energy, wide-temperature deployment.

锂金属电池（lmb）的广泛应用面临着一个严峻的挑战：缺乏能够同时承受低温和高压操作条件的电解质。为了解决这一基本限制，我们引入了一种基于分子工程混合溶剂化结构结合协同双盐系统的机械引导电解质设计策略。我们的方法独特地采用了一种含氟溶剂混合物——包括氟乙烯碳酸酯（FEC）和适度配位的氟乙酸乙酯（TFEA）——来重新配置Li+溶剂化环境。这种定制的溶剂化鞘有利于阴离子的参与，并实现了接触离子对（CIP）和聚集体（AGG）之间的最佳平衡，从而显著降低了Li+的脱溶能垒。此外，结合LiFSI-LiClO4双盐配方协同工作，在两个电极上构建高导电性富liff界面：锂阳极上稳定的固体电解质界面（SEI）和高压下稳健的阴极电解质界面（CEI）。因此，Li||NCM811电池在室温至- 20°C范围内表现出优异的循环稳定性，在中等充电率（0.5 C）下，在高放电率（高达3 C）下保持高容量，在高达4.7 V下稳定运行，大大优于传统的单盐电解质。这项工作建立了一种可转移的溶剂-界面设计范式，将配位化学与界面稳定性联系起来，推动lmb向实用、高能、宽温度的方向发展。

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引用次数: 0

In-situ lithiated dry-processed graphite electrodes for “intercalation-conversion” lithium-sulfur batteries 用于“插层转换”锂硫电池的原位锂化干法石墨电极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-28 DOI: 10.1016/j.jechem.2026.01.025

Xiaoyu Jin , Xiaoqun Qi , Lei Zhao , Shuai Huang , Jie Ji , Dan Yang , Fengyi Yang , Ruining Jiang , Yunhui Huang , Long Qie

The practical applications of lithium-sulfur (Li-S) batteries are limited by the safety risks and rapid capacity loss attributed to Li-metal anodes. “Intercalation-conversion” Li-S batteries using prelithiated graphite anodes offer a safer, more practical alternative—but their progress is largely impeded by the complex graphite prelithiation process. Here, we report an in situ lithiation approach by stacking dry-processed graphite electrodes featuring simple fabrication, structural stability, and high-loading capability, onto Li-metal foil in the cells, accomplished during the initial discharge–charge process. The intimate contact within the hybrid Li-Graphite anode ensures efficient Li-ion transport, enabling complete stripping of the lithium metal and in situ lithiation of Graphite. This facilitates the subsequent intercalation chemistry at the anode and conversion chemistry at the cathode. With this configuration, by optimizing the N/P ratio, we achieve 100% utilization of lithium metal and highly reversible Li-ion intercalation/deintercalation. The proposed “intercalation-conversion” Li-S batteries exhibit significantly prolonged cycle life, achieving more than 15 times longer lifespan compared with conventional Li-S batteries. This strategy offers a versatile solution for the applications of battery systems employing Li-free cathodes.

锂硫电池的实际应用受到锂金属阳极的安全风险和快速容量损失的限制。使用预锂化石墨阳极的“插层转换”锂电池提供了一种更安全、更实用的替代方案，但其进展在很大程度上受到复杂的石墨预锂化过程的阻碍。在这里，我们报告了一种原位锂化方法，通过将具有简单制作，结构稳定和高负载能力的干加工石墨电极堆叠在电池中的锂金属箔上，在初始充放电过程中完成。混合锂-石墨阳极内部的紧密接触确保了高效的锂离子传输，实现了锂金属的完全剥离和石墨的原位锂化。这有利于随后在阳极的插层化学和在阴极的转化化学。在这种配置下，通过优化N/P比，我们实现了100%的锂金属利用率和高度可逆的锂离子插入/脱嵌。所提出的“插层转换”锂- s电池具有显着延长的循环寿命，与传统锂- s电池相比，寿命延长了15倍以上。该策略为采用无锂阴极的电池系统的应用提供了一个通用的解决方案。

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引用次数: 0

Stabilizing high-voltage operation of layered oxide cathodes through ionic interdiffusion-triggered surface reinforcement for sodium-ion batteries 通过离子互扩散触发的钠离子电池表面强化来稳定层状氧化物阴极的高压运行

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-14 DOI: 10.1016/j.jechem.2026.01.007

Guohu Chen , Yundian Ya , Yan Li , Guangpeng He , Yuyu Chen , Wenwei Wu , Xuehang Wu

O3-type Ni/Mn-based layered oxides have shown promise for application in sodium ion batteries (SIBs), due to their ability to achieve high energy density at increased upper cut-off voltages through the synergistic cationic/anionic redox reactions. However, a series of interfacial side reactions usually leads to rapid capacity/voltage decay. Herein, we propose a surface reinforcement approach to enable stable 4.5 V high-voltage cycling of O3-type layered oxides. Through thermally induced ionic interdiffusion, Zn(H₂PO₄)₂ acts as a surface reinforcement initiator, enabling the simultaneous achievement of triple effects: elimination of residual alkali, construction of surface coating, and implementation of surface doping. Zn²⁺ doping constructs a special Zn–O–Na/vacancy configuration, enhancing oxygen redox reaction reversibility by increasing non-bonding O 2p states and improving ionic/electronic transport. Additionally, the cubic-structured Na₃₋₂_xZn_xPO₄ (NZP) nanolayer facilitates rapid Na⁺ transfer, restrains lattice oxygen release, and alleviates electrolyte decomposition during cycling. This surface reinforcement treatment diminishes localized asynchronous structural evolution and simplifies the phase transition process during cycling. The surface-reinforced O3-type Na_0.9Cu_0.12Ni_0.33Mn_0.4Ti_0.15O₂ exhibits superior cycling stability (76.8% vs. 48.4% capacity retention over 200 cycles at 100 mA g⁻¹) and rate capability (88.2 vs. 43.1 mAh g⁻¹ at 2000 mA g⁻¹) compared to the pristine counterpart at 4.5 V. This work presents a new approach to fortify the surface structure for developing high-voltage stable layered oxide cathode materials for SIBs.

o3型Ni/ mn基层状氧化物在钠离子电池（sib）中有着广阔的应用前景，因为它们能够在更高的截止电压下通过协同的阳离子/阴离子氧化还原反应获得高能量密度。然而，一系列的界面副反应通常会导致容量/电压的快速衰减。在此，我们提出了一种表面强化方法来实现o3型层状氧化物稳定的4.5 V高压循环。通过热诱导离子相互扩散，Zn(H2PO4)2作为表面增强引发剂，可以同时达到消除残碱、构建表面涂层和实现表面掺杂的三重效果。Zn2+掺杂构建了一种特殊的Zn-O-Na /空位构型，通过增加o2p非键态和改善离子/电子输运来增强氧氧化还原反应的可逆性。此外，立方结构的Na3−2xZnxPO4 （NZP）纳米层促进了Na+的快速转移，抑制了晶格氧的释放，减轻了循环过程中电解质的分解。这种表面强化处理减少了局部的异步结构演变，简化了循环过程中的相变过程。表面增强的o3型Na0.9Cu0.12Ni0.33Mn0.4Ti0.15O2在100 mA g−1下200次循环时的容量保持率为76.8%比48.4%，在2000 mA g−1下的倍率容量为88.2比43.1 mAh g−1。本工作为开发高电压稳定层状氧化阴极材料提供了一种强化表面结构的新方法。

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引用次数: 0

Simultaneously boosting ionic conductivity, Li+ transference number and oxidative stability in solid polymer electrolytes via ionic coordination regulation 同时通过离子配位调控提高固体聚合物电解质的离子电导率、Li+转移数和氧化稳定性

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-05-01 Epub Date: 2026-01-28 DOI: 10.1016/j.jechem.2026.01.022

Guoyong Xue , Jie Lu , Yulu He , Ruilong Liu , Qiuyi Zhang , Nannan Qin , Chenji Hu , Fuqiang Huang , Liwei Chen

Achieving simultaneous improvement in ionic conductivity, Li⁺ transference number, and high-voltage stability remains an intractable challenge in the development of solid polymer electrolytes (SPEs) for all-solid-state lithium batteries (ASSLBs). Here, we report a multi-functional borate-crosslinked polymer electrolyte (dubbed PVBA) designed through integrated molecular engineering. The PVBA SPE matrix incorporates three polar coordination motifs (CO, COC and SO) to establish a multidimensional Li⁺ conduction network via synergistic ion–dipole interactions. Concurrently, the electron-deficient boron centers serve as Lewis acid sites to immobilize anions. In addition, electron-withdrawing sulfone groups enhance oxidative resistance by lowering the highest occupied molecular orbital (HOMO) energy level. This design enables PVBA SPE to deliver a high ionic conductivity of 1.18 mS cm⁻¹, a Li⁺ transference number of 0.81, and an electrochemical stability window exceeding 5.4 V. When paired with high-voltage cathodes, such as LiCoO₂ and LiNi_0.8Co_0.1Mn_0.1O₂, the PVBA SPE-based ASSLB exhibits stable cycling under high cut-off voltage of 4.6 V vs. Li⁺/Li at 2C, significantly outperforming state-of-the-art SPE-based counterparts. This work establishes a new design strategy for overcoming the intrinsic limitations of SPEs toward next-generation energy storage systems.

在全固态锂电池（ASSLBs）用固体聚合物电解质（spe）的开发过程中，如何同时提高离子电导率、Li+转移数和高压稳定性仍然是一个棘手的挑战。本文报道了一种通过集成分子工程设计的多功能硼酸交联聚合物电解质（简称PVBA）。PVBA SPE矩阵包含三个极性配位基序（CO， COC和SO），通过协同离子偶极子相互作用建立了多维Li+传导网络。同时，缺电子硼中心作为路易斯酸位点固定阴离子。此外，吸电子砜基团通过降低最高已占据分子轨道（HOMO）能级来增强抗氧化性。该设计使PVBA SPE能够提供1.18 mS cm−1的高离子电导率，0.81的Li+转移数和超过5.4 V的电化学稳定窗口。当与LiCoO2和LiNi0.8Co0.1Mn0.1O2等高压阴极配合使用时，PVBA基于spe的ASSLB在4.6 V的高截止电压下与Li+/Li在2C时表现出稳定的循环，显著优于最先进的基于spe的ASSLB。这项工作建立了一种新的设计策略，以克服spe对下一代储能系统的内在限制。

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