Journal of Energy Chemistry最新文献

Towards circular batteries: A water-soluble, recyclable, self-healing binder for aqueous-processed sulfur cathodes 迈向循环电池：一种水溶性、可回收、自愈的粘合剂，用于水处理的硫阴极

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-02-03 DOI: 10.1016/j.jechem.2026.01.030

Yuchuan Ren , Qian Xue , Liqiang Lu , Canhuang Li , Guanjie Li , Nikolay Kardjilov , Ingo Manke , Jiaqi Zhao , Xuan Lu , Jing Yu , Guifang Zeng , Xiaoyu Bi , Shengnan Zhang , Armando Berlanga-Vázquez , Chen Huang , Xuede Qi , Xueqiang Qi , Jordi Arbiol , Yan Lu , Guoqiang Tan , Andreu Cabot

Sulfur cathodes have attracted considerable attention due to their potential for high energy density and cost-effectiveness. However, their limited stability, in part stemming from volume changes during cycling and the dissolution and migration of metal polysulfides, has hindered their commercialization. Binders play a critical role in preventing electrode delamination, while potentially contributing additional functionalities, such as trapping polysulfides. In this work, we introduce an aqueous-processable sulfur cathode binder composed of polyvinyl alcohol (PVA) and polyethylene glycol (PEG). Multiple hydrogen bonding interactions provided by the PVA/PEG binder hydrogen-bond network enhance metal-ion diffusion and trap polysulfides, thereby reducing their dissolution. Additionally, microcracks generated during the cycling can be healed by the dynamic hydrogen-bond network. Thereby, in lithium-sulfur cells, PVA/PEG-based cathodes exhibit an ultralow per-cycle capacity fade of 0.0023% over 600 cycles at 1C, and deliver up to 677 mAh/g in lean-electrolyte pouch cells (E/S = 4 µL/mg), retaining 99% of the initial capacity after 100 cycles at 0.1C in pouch cell. Theoretical calculations and molecular dynamics simulations confirm the superior adsorption energy and repairability of the PVA/PEG binder, reinforcing its ability to stabilize the cathode. Additionally, PVA/PEG-based cathodes exhibit excellent flame retardancy, support eco-friendly and closed-loop recycling due to the binder’s water solubility, which allows for easy electrode material reutilization.

硫阴极由于其高能量密度和成本效益的潜力而引起了人们的广泛关注。然而，它们有限的稳定性，部分源于循环过程中的体积变化和金属多硫化物的溶解和迁移，阻碍了它们的商业化。粘合剂在防止电极分层方面起着至关重要的作用，同时还具有潜在的附加功能，例如捕获多硫化物。本文介绍了一种由聚乙烯醇（PVA）和聚乙二醇（PEG）组成的可水加工硫阴极粘结剂。PVA/PEG粘结剂氢键网络提供的多重氢键相互作用增强了金属离子的扩散并捕获了多硫化物，从而减少了它们的溶解。此外，循环过程中产生的微裂纹可以通过动态氢键网络修复。因此，在锂硫电池中，PVA/ peg基阴极在1C下的600次循环中表现出0.0023%的超低每循环容量衰减，并且在稀薄电解质袋状电池（E/S = 4 μ L/mg）中提供高达677 mAh/g的容量，在0.1C的袋状电池中进行100次循环后保持99%的初始容量。理论计算和分子动力学模拟证实了PVA/PEG粘合剂优越的吸附能和可修复性，增强了其稳定阴极的能力。此外，PVA/ peg基阴极具有优异的阻燃性，由于粘合剂的水溶性，支持环保和闭环回收，这使得电极材料易于再利用。

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引用次数: 0

Controlling the dynamic structural changes of catalysts for COx hydrogenation 控制COx加氢催化剂的动态结构变化

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-30 DOI: 10.1016/j.jechem.2026.01.042

Hangjie Li , Jun Bao , Xiaodong Yi , Peipei Zhang , Shuangqin Zeng , Junyi Zhang , Haisheng Liu , Xionghou Gao , Qinghe Yang , Hai Wang , Liang Wang

Hydrogenation of CO and CO₂ (CO_x) into value-added chemicals and fuels is a central process for the sustainable utilization of carbon resources, where the dynamic structural changes of the catalysts play a crucial role in determining catalytic performances. This review summarizes recent progress in regulating catalyst dynamic changes to achieve efficient CO_x hydrogenation. We highlight the crucial role of promoters in tuning the electronic and/or geometric structures of active sites, discuss the influence of supports in stabilizing metal nanoparticles, and emphasize the importance of reaction atmosphere engineering in suppressing or directing catalyst surface restructuring. These strategies efficiently modulate the catalyst dynamics, either by stabilizing the catalyst against undesirable restructuring or by harnessing dynamic restructuring to generate new active sites. As a result, enhanced activity, improved selectivity, and prolonged catalyst durability can be achieved. We anticipate that these concepts and insights discussed in this review will provide valuable guidance for the rational design of highly efficient catalysts for CO_x hydrogenation.

CO和CO2 （COx）加氢转化为增值化学品和燃料是碳资源可持续利用的核心过程，其中催化剂的动态结构变化对催化性能起着至关重要的作用。本文综述了调节催化剂动态变化以实现高效COx加氢的研究进展。我们强调了促进剂在调节活性位点的电子和/或几何结构方面的关键作用，讨论了支撑剂在稳定金属纳米粒子方面的影响，并强调了反应气氛工程在抑制或指导催化剂表面重组方面的重要性。这些策略有效地调节催化剂动力学，要么通过稳定催化剂以防止不良的重组，要么通过利用动态重组来产生新的活性位点。因此，可以提高活性，提高选择性，延长催化剂的耐用性。我们期望本文所讨论的这些概念和见解将为合理设计高效的COx加氢催化剂提供有价值的指导。

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引用次数: 0

Multi-electron redox chemistry in phosphate cathodes for aqueous zinc batteries 含水锌电池磷酸盐阴极的多电子氧化还原化学

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.032

Ruifu Li, Hongsheng Han, Huihua Li, Huang Zhang

Aqueous zinc-ion batteries (AZIBs) are emerging as a viable option for grid-scale energy storage, but their energy density is currently capped by the limitations of conventional cathode materials. While phosphate-based cathodes, due to their high operational voltage and exceptional structural stability, represent a step forward, their capacity remains constrained by single-electron redox processes. This review advocates multi-electron redox chemistry as the crucial pathway to overcome this limitation. Focusing on vanadium-based phosphates with their multiple accessible oxidation states, we examine key challenges including low electronic conductivity, vanadium dissolution, and evaluate advanced strategies such as defect engineering and elemental doping. By showcasing recent advances in NASICON-type and related structures capable of multi-electron redox reactions, we outline a roadmap for developing next-generation phosphate cathodes, laying the groundwork for the development of high-performance AZIBs.

水锌离子电池（azib）正在成为电网规模储能的可行选择，但其能量密度目前受到传统阴极材料的限制。虽然磷酸盐基阴极由于其高工作电压和特殊的结构稳定性，代表了一个进步，但它们的容量仍然受到单电子氧化还原过程的限制。本文认为多电子氧化还原化学是克服这一限制的关键途径。关注钒基磷酸盐具有多种可达氧化态，我们研究了包括低电子导电性，钒溶解在内的关键挑战，并评估了诸如缺陷工程和元素掺杂等先进策略。通过展示nasicon型和能够进行多电子氧化还原反应的相关结构的最新进展，我们概述了开发下一代磷酸盐阴极的路线图，为高性能azib的开发奠定了基础。

引用次数: 0

Electrocatalytic ammonium nitrate synthesis through integrating nitric oxide redox reactions over porphyrinic metal–organic frameworks 在卟啉金属-有机框架上整合一氧化氮氧化还原反应的电催化硝酸铵合成

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.029

Yi Tan , Xiaokang Chen , Jian Yuan , Guan Sheng , Wei-Qiao Deng , Ghim Wei Ho , Hao Wu

The conversion of nitric oxide (NO), a gaseous pollutant with an intermediate nitrogen oxidation state, into value-added ammonium nitrate (NH₄NO₃) via redox processes offers a sustainable alternative to conventional disposal methods, which are hampered by competing pathways that yield undesirable byproducts. Herein, we decouple the synthesis of NH₄NO₃ into electrochemical NO oxidation (NOOR) and reduction (NORR) by employing H-terminated and Cu-metallated porphyrinic metal–organic framework catalysts (H-PMOF and Cu-PMOF, respectively), leveraging their tailored coordination environments and varied NO adsorption configurations. The H-PMOF favors O-atom adsorption via hydrogen bonding, whereas the Cu-PMOF strengthens N-atom adsorption through CuN interactions. They promote NOOR to NO₃⁻ and NORR to NH₄⁺, respectively, achieving greater Faradaic efficiencies and yield rates compared to their respective counterparts. When integrated in one electrolyzer, they enable direct synthesis of NH₄NO₃ by generating 662.4 µmol of NO₃⁻ and 409.5 µmol of NH₄⁺ hourly. Molecular dynamics simulations reveal differences in adsorption modes, while computational results identify the rate-determining dehydrogenation (*HNO₃ → *NO₃ for NOOR) and hydrogenation steps (*NO → *NHO for NORR), with both catalysts exhibiting reduced energy barriers. This work presents a strategy for directing NO redox reactions through coordination engineering, paving the way for sustainable nitrogen valorization.

一氧化氮（NO）是一种具有中间氮氧化态的气态污染物，通过氧化还原过程将其转化为增值硝酸铵（NH4NO3），为传统的处理方法提供了一种可持续的替代方案，传统的处理方法受到产生不良副产物的竞争途径的阻碍。本文采用h端金属卟啉型和cu金属卟啉型金属有机骨架催化剂（分别为H-PMOF和Cu-PMOF），利用其定制的配位环境和不同的NO吸附构型，将NH4NO3的合成解耦为电化学NO氧化（NOOR）和还原（NORR）。H-PMOF有利于通过氢键吸附o原子，而Cu-PMOF则通过CuN相互作用增强n原子的吸附。它们分别将NOOR转化为NO3 -和NORR转化为NH4+，与它们各自的对应物相比，实现了更高的法拉第效率和产率。当集成在一个电解槽中时，它们可以通过每小时产生662.4µmol NO3−和409.5µmol NH4+来直接合成NH4NO3。分子动力学模拟揭示了吸附模式的差异，而计算结果确定了脱氢速率（NOOR为*HNO3→*NO3）和加氢步骤（NORR为*NO→*NHO），两种催化剂都表现出降低的能垒。这项工作提出了一种通过配位工程指导NO氧化还原反应的策略，为可持续的氮增值铺平了道路。

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引用次数: 0

Vacancy-single-atom dual regulation unlocking lattice-oxygen activation pathway driving a leap in alkaline overall water-splitting performance 空位-单原子双调控解锁晶格-氧激活途径，推动碱性整体水分解性能的飞跃

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.024

Yun Zhao, Xianju Leng, Jiaqian Guan, Wentao Ding, Yu Zhu, Sheng Han, Jibo Jiang

Activating lattice oxygen to directly participate in the oxygen evolution reaction (OER) has emerged as a highly efficient strategy to overcome conventional catalytic bottlenecks, while the dynamic switching of reaction pathways is influenced by electronic structure modulation that induces lattice oxygen activation. Using NiFe Prussian blue analogues (PBAs) as a model platform, this study proposes a vacancy-single atom synergistic strategy that couples cyanide vacancies (V_CN) with Ru single atoms. Experiments demonstrate that pristine NiFe PBA rapidly reconfigures into NiFeOOH upon potential application, following the conventional adsorbed species evolution mechanism (AEM). Following synergistic design, the lattice oxygen-mediated pathway (LOM) is activated, with electrochemical metrics indicating substantially enhanced performance. The resulting Ru-PBA-V_CN/MX material simultaneously functions as both cathode and anode, exhibiting a low cell voltage of 1.53 V at a current density of 10 mA cm⁻². Density functional theory (DFT) calculations further elucidate that the dual modification tunes the electronic structure, compressing the free-energy barrier of the OER rate-determining step to 1.64 eV, while simultaneously weakening the *OH/*OOH linear-scaling constraint, thereby enabling stable release of lattice oxygen. This synergistic effect overcomes the inherent linear proportional limitations of AEM, providing a novel blueprint for designing high-performance LOM catalysts.

激活晶格氧直接参与析氧反应（OER）已成为克服传统催化瓶颈的一种高效策略，而诱导晶格氧活化的电子结构调制影响了反应途径的动态切换。本研究以NiFe普鲁士蓝类似物（PBAs）为模型平台，提出了一种空位-单原子协同策略，将氰化物空位（VCN）与Ru单原子偶联。实验表明，原始的NiFe PBA在潜在的应用中迅速重新配置为NiFeOOH，遵循传统的吸附物种进化机制（AEM）。在协同设计之后，晶格氧介导途径（LOM）被激活，电化学指标表明性能显著增强。得到的Ru-PBA-VCN/MX材料同时作为阴极和阳极，在电流密度为10 mA cm - 2时显示出1.53 V的低电池电压。密度泛函理论（DFT）计算进一步阐明，双重修饰调整了电子结构，将OER速率决定步骤的自由能势垒压缩到1.64 eV，同时减弱了*OH/*OOH线性标度约束，从而实现了晶格氧的稳定释放。这种协同效应克服了AEM固有的线性比例限制，为设计高性能LOM催化剂提供了新的蓝图。

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引用次数: 0

A versatile route to tailor-made catalysts via molten salt-assisted synthesis for catalytic conversion 通过熔盐辅助合成用于催化转化的定制催化剂的通用路线

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.021

Shasha Gao , Jinteng Guan , Rui Zhang , Feifei Mao , Dong Guo , Chaolong Wang , Gonglei Shao

Amidst global energy transition and carbon neutrality initiatives, the development of high-performance catalysts to address energy and environmental challenges has become imperative. Molten salt-assisted synthesis (MSAS) offers a novel and robust route for catalyst preparation. It overcomes the critical drawbacks of conventional methods, such as limited mass transfer in solid-phase synthesis and constrained thermodynamics in wet-chemical processes. By harnessing high-temperature ion-mediated effects and dynamic interfacial regulation mechanisms, MSAS establishes a pragmatic paradigm for the precise synthesis of catalysts. In this review, we first outline the physicochemical properties of diverse molten salt systems, examine the molten salt system selection criteria and the theoretical mechanism basis for synthesizing catalysts via MSAS. Then recent advances in various MSAS-derived catalysts and their applications in electrochemical energy conversion are systematically reviewed. Finally, current challenges and future prospects for MSAS in catalyst design are comprehensively discussed. The systematic assessments and insights presented herein not only deepen the understanding of MSAS, but also bridge theoretical knowledge and practical design for novel, high-performance electrocatalysts.

在全球能源转型和碳中和倡议的背景下，开发高性能催化剂以应对能源和环境挑战已势在必行。熔盐辅助合成（MSAS）为催化剂的制备提供了一条新颖、可靠的途径。它克服了传统方法的关键缺陷，如固相合成中的有限传质和湿化学过程中的受限热力学。通过利用高温离子介导效应和动态界面调节机制，MSAS为精确合成催化剂建立了实用范例。本文首先概述了不同熔盐体系的物理化学性质，探讨了熔盐体系的选择标准以及通过MSAS法合成催化剂的理论机理基础。然后系统地综述了近年来各种msas衍生催化剂的研究进展及其在电化学能量转换中的应用。最后，全面讨论了MSAS在催化剂设计中面临的挑战和未来前景。本文提出的系统评估和见解不仅加深了对MSAS的理解，而且为新型高性能电催化剂的理论知识和实际设计架起了桥梁。

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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 : 2026-01-28 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

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 : 2026-01-28 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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引用次数: 0

A reactor design approach to address the high-loading paradox in high-energy-density flow batteries 解决高能量密度液流电池高负荷悖论的反应器设计方法

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.020

Xinyue Liu, Yuwei Chen, Weicheng Wu, Zijian Guan, Jiankang Yang, Yunxuan Li, Mingyue Zhou, Xingying Lan

Redox targeting-based flow batteries (RTFBs), which integrate high-capacity solid materials, hold immense promise for breaking the energy density ceiling of conventional flow batteries. However, this promise has been severely hindered by a persistent “high-loading paradox,” where increasing the solid material loading paradoxically diminishes its utilization, preventing meaningful performance gains. Here, we overturn the long-standing assumption that this is an intrinsic material limitation. We demonstrate that the paradox is, in fact, a solvable macroscopic transport problem. By introducing a rational, hydrodynamics-driven reactor engineering paradigm, we successfully shatter this performance barrier. Our optimized architecture eradicates flow stagnation zones, enabling uniform solid–liquid contact and unlocking the full potential of the active material. This strategy achieved an unprecedented simultaneous high solid loading of 0.88 kg L⁻¹ and an outstanding utilization of 83%, resolving the paradox. Consequently, a Zn-PB hybrid flow battery delivered a record-high energy density of 111.6 Wh L⁻¹. This work demonstrates macro-scale reactor engineering as a powerful and previously overlooked design dimension for the [Fe(CN)₆]³⁻-PB electrolyte system, offering a new approach for redox-targeting systems to unlock the true performance of solid-state materials in next-generation, high-energy-density flow batteries.

基于氧化还原靶的液流电池（RTFBs）集成了高容量固体材料，有望突破传统液流电池的能量密度上限。然而，这一前景受到了持续存在的“高负载悖论”的严重阻碍，即增加固体材料负载反而会减少其利用率，从而阻碍了有意义的性能提升。在这里，我们推翻了长期以来的假设，即这是一种内在的物质限制。我们证明了这个悖论实际上是一个可解的宏观输运问题。通过引入一种合理的、流体动力学驱动的反应堆工程范式，我们成功地打破了这一性能障碍。我们优化的结构消除了流动停滞区，实现了均匀的固液接触，释放了活性材料的全部潜力。该策略同时实现了前所未有的高固体载荷0.88 kg L−1和83%的出色利用率，解决了这一矛盾。因此，锌- pb混合液流电池的能量密度达到了创纪录的111.6 Wh L−1。这项工作证明了宏观反应器工程是[Fe(CN)6]3−-PB电解质系统的一个强大的、以前被忽视的设计维度，为氧化还原靶向系统提供了一种新的方法，以解锁下一代高能量密度液流电池中固态材料的真实性能。

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引用次数: 0

Hierarchical catalysis tailoring Li2S2 solid-state dissociation for high-energy lithium-sulfur batteries 分层催化剪裁Li2S2固态解离高能锂硫电池

IF 14.9 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2026-01-28 DOI: 10.1016/j.jechem.2026.01.040

Yu Jiang , Rong Yang , Bailing Jiang , Xin Dong , Hongyu Shang , Kejia Li , Haochen Liu , Yinglin Yan , Jou-Hyeon Ahn

Lithium-sulfur batteries (LSBs) exhibit exceptional theoretical capacity through solid-liquid-solid sulfur conversion in ether-based electrolytes, positioning them as next-generation energy storage candidates. However, their practical implementation faces two fundamental challenges: (1) sluggish redox kinetics arising from the high dissociation energy barrier (>1.5 eV) of insulating Li₂S₂/Li₂S during solid-state conversion, and (2) severe capacity degradation caused by polysulfide shuttling under high sulfur loading. To address these issues, a CoS₂-modified TiS₂-Ti₃C₂T_x heterojunction catalyst (CoS₂@TST) through interfacial engineering was designed. Density functional theory (DFT) calculations reveal that the CoS₂ active sites significantly reduce the Li₂S₂ dissociation barrier to 0.40 eV, while the conductive Ti₃C₂T_x matrix ensures rapid electron transfer. In-situ Raman spectroscopy demonstrates the heterojunction’s dual functionality: TiS₂ chemically anchors lithium polysulfides (LiPSs) and surface functional groups catalyze their conversion, effectively suppressing shuttle effects. The optimized LSBs with CoS₂@TST interlayers achieve an ultralow capacity decay rate of 0.031% per cycle over 500 cycles at 2 C. Notably, under practical conditions of 9.44 mg cm⁻² sulfur loading, the battery delivers an areal capacity of 6.21 mA h cm⁻², representing a critical advancement in balancing energy density and commercial viability.

锂硫电池（lsb）通过在醚基电解质中进行固-液-固硫转化，表现出卓越的理论容量，使其成为下一代储能系统的候选者。然而，它们的实际应用面临着两个根本性的挑战：(1)固态转化过程中绝缘Li2S2/Li2S的高解离能垒（>1.5 eV）导致氧化还原动力学缓慢；(2)高硫负载下多硫穿梭导致严重的容量退化。为了解决这些问题，通过界面工程设计了cos2修饰的TiS2-Ti3C2Tx异质结催化剂（CoS2@TST）。密度泛函理论（DFT）计算表明，CoS2活性位点显著降低Li2S2解离势垒至0.40 eV，而导电Ti3C2Tx矩阵保证了快速的电子转移。原位拉曼光谱证明了异质结的双重功能：TiS2化学锚定锂多硫化物（LiPSs），表面官能团催化其转化，有效抑制穿梭效应。优化后的含有CoS2@TST中间层的LSBs在温度为2℃的500次循环中，每循环的容量衰减率为0.031%。值得注意的是，在9.44 mg cm - 2硫负载的实际条件下，该电池的面容量为6.21 mA h cm - 2，在平衡能量密度和商业可行性方面取得了重要进展。

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引用次数: 0