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Metal-Organic Framework-Based Materials for Zinc-Halogen (Br2, I2) Batteries: Mechanisms and Performance 锌卤素(Br2, I2)电池的金属有机骨架材料:机理和性能
IF 12 Pub Date : 2026-02-17 DOI: 10.1002/cnl2.70125
Muhammad Saad Bhatti, Hassan Akhtar, Muhammad Sufyan Javed, Jiantao Zai, Muhammad Awais Nawaz, Aqsa Ibrahim, Tayyaba Najam, Muhammad Altaf Nazir, Syed Shoaib Ahmad Shah

Zinc–bromine and zinc–iodine batteries have been widely regarded as promising systems for large-scale energy storage, yet their practical application is currently hampered by slow redox reactions, low efficiency due to the shuttle effect, and zinc dendrite growth. In this review, we overview the contribution of metal–organic frameworks (MOFs) and MOF-derived materials to overcoming these drawbacks. Two typical strategies are presented: assembling pristine MOFs as selective porous barriers to confine polyhalides and MOF-templated carbon materials, including single-atom catalysts for enhanced conductivities and fast charge transfer. We show that pristine MOFs exhibit interesting selectivity properties but rarely meet the required chemical stability in acidic electrolytes. However, MOF-based carbons are more stable and conductive, but their performance requires careful regulation of synthesis conditions to maintain active sites. Overall, it seems most promising to develop bifunctional hosts that are conductive carbon frameworks embedded with single-atom metal sites, which both trap adsorbed halogen species and catalyze their decomposition. This review highlights the critical developments required to progress from promising electrochemical data in the laboratory to practical high-capacity battery electrodes.

锌-溴电池和锌-碘电池被广泛认为是一种有前景的大规模储能系统,但它们的实际应用目前受到氧化还原反应缓慢、穿梭效应导致的效率低下以及锌枝晶生长的阻碍。在这篇综述中,我们概述了金属有机框架(mof)和mof衍生材料在克服这些缺点方面的贡献。提出了两种典型的策略:组装原始mof作为选择性多孔屏障来限制多卤化物和mof模板碳材料,包括单原子催化剂来增强电导率和快速电荷转移。我们发现原始mof表现出有趣的选择性,但在酸性电解质中很少满足所需的化学稳定性。然而,mof基碳更稳定和导电,但它们的性能需要仔细调节合成条件以保持活性位点。总的来说,似乎最有希望开发双功能宿主,即嵌入单原子金属位的导电碳框架,既能捕获吸附的卤素物种,又能催化它们的分解。这篇综述强调了从实验室中有前途的电化学数据到实际的高容量电池电极所需的关键发展。
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引用次数: 0
Green Hydrogen for Maritime Decarbonization 绿色氢用于海洋脱碳
IF 12 Pub Date : 2026-02-15 DOI: 10.1002/cnl2.70128
Chunjing Li, Wenwen Guo, Jingqiang Wang

In pursuit of global carbon neutrality, maritime shipping with high CO2 emissions confronts an urgent imperative deep decarbonization. Green hydrogen is a zero-carbon fuel produced through water electrolysis by renewable energy sources, which is emerging as a promising solution for maritime decarbonization owing to its high energy density and versatile application potential. Here, it provides a systematic overview of the technological feasibility of green hydrogen for maritime shipping, encompassing its current application status and key challenges. It analyzes recent advances in green hydrogen production, storage, transportation, and infrastructure development, while exploring the enabling roles of policy support, technological innovation, and international collaboration. Despite facing substantial barriers in cost, technology, and infrastructure, green hydrogen boasts enormous decarbonization potential and occupies an indispensable strategic position in the global carbon neutrality agenda.

在追求全球碳中和的过程中,二氧化碳排放量高的海运面临着迫切需要的深度脱碳。绿色氢是一种利用可再生能源通过水电解生产的零碳燃料,由于其高能量密度和广泛的应用潜力,正成为海洋脱碳的一种有前景的解决方案。在这里,它提供了一个系统的概述绿色氢用于海运的技术可行性,包括其目前的应用现状和主要挑战。报告分析了绿色氢气生产、储存、运输和基础设施发展方面的最新进展,同时探讨了政策支持、技术创新和国际合作的促进作用。尽管面临成本、技术和基础设施方面的巨大障碍,但绿色氢具有巨大的脱碳潜力,在全球碳中和议程中占有不可或缺的战略地位。
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引用次数: 0
Thermoplasmonic Response of Non-Noble Metal Core–Shell Nanostructures for Solar Energy Harvesting 用于太阳能收集的非贵金属核壳纳米结构热等离子体响应
IF 12 Pub Date : 2026-02-15 DOI: 10.1002/cnl2.70124
Jiarong Lv, Xiaofeng Kang, Feng Wang, Shengjie Bai, Shaohua Shen, Ya Liu

Core–Shell plasmonic nanostructures are drawing significant interest for its multifunctionality in light-harvesting; however, the mechanisms of the structure–performance relationship of non-noble metal materials are not yet fully elucidated. Here, finite element method (FEM) is employed to simulate the thermoplasmonic performance of X@Fe2O3(X = Bi, Ni, Co, Al) core–shell nanoparticles and analyze the influence of interparticle spacing and shell thickness on thermoplasmonic behavior with different structures. With Fe2O3 shell, monomers exhibit strong plasmonic features within visible regions and resonances peak redshift as shell thickness increases, and certain shell thickness can enhance the intensity of the resonances peak. Longitudinally polarized dimers exhibit strong interparticle coupling, resulting in pronounced field-heat hotspot alignment that promotes efficient light-to-heat conversion. Conversely, transverse polarization causes spatial decoupling between electromagnetic and thermal responses. The simulation results indicate that for 100 nm nanoparticles, maximum absorption efficiency does not always correspond to peak temperature response, underscoring the need to consider both spectral and spatial factors in thermoplasmonic design. This study provides important insight into the potential of non-noble metal-based core–shell nanostructures for solar energy harvesting.

核壳等离子体纳米结构因其在光捕获中的多功能性而引起了人们的极大兴趣;然而,非贵金属材料的结构-性能关系机理尚未完全阐明。本文采用有限元方法模拟了X@Fe2O3(X = Bi, Ni, Co, Al)核壳纳米粒子的热等离子体性能,分析了不同结构下粒子间距和壳层厚度对热等离子体行为的影响。在Fe2O3壳层中,单体在可见区表现出强烈的等离子体特征,共振峰随壳层厚度的增加而红移,一定的壳层厚度可以增强共振峰的强度。纵向极化二聚体表现出强烈的粒子间耦合,导致明显的场-热热点对准,促进有效的光-热转换。相反,横向极化导致电磁和热响应之间的空间解耦。模拟结果表明,对于100 nm的纳米颗粒,最大吸收效率并不总是与峰值温度响应相对应,这表明在热等离子体设计中需要同时考虑光谱和空间因素。这项研究为非贵金属基核壳纳米结构在太阳能收集方面的潜力提供了重要的见解。
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引用次数: 0
Non-Equilibrium Construction of Layered Ruddlesden–Popper La2NiO4 Porous Nanosheets for Efficient Urea Electrooxidation 层状Ruddlesden-Popper La2NiO4多孔纳米片用于高效尿素电氧化的非平衡结构
IF 12 Pub Date : 2026-02-15 DOI: 10.1002/cnl2.70132
Mingjie Wang, Hanyuan Zhang, Jiao Dai, Bohao Chang, Kaisi Liu, Weilin Xu, Yujie Ma, Jun Wan

Urea electrooxidation offers a low-voltage pathway for hydrogen production while simultaneously addressing nitrogen-cycle remediation, yet its multi-step mechanism is kinetically hindered by sluggish C–N bond cleavage and the accumulation of strongly adsorbed intermediates. Conventional nickel-based oxides suffer from limited exposure of Ni–O active sites and slow charge redistribution, restricting overall catalytic turnover. In this study, a microwave shock strategy was developed to construct two-dimensional porous La2NiO4 nanosheets with a well-defined Ruddlesden–Popper (n = 2) layered structure. The ultrafast non-equilibrium synthesis generates transient supersaturation and controlled gas evolution, promoting the formation of open interlayer channels and abundant oxygen vacancies. This architecture enhances mixed ionic–electronic transport and facilitates rapid proton-coupled electron transfer during urea oxidation, yielding a low onset potential, high mass activity, and excellent durability. Mechanistic analysis reveals that the coexistence of Ni2+/Ni3+ redox couples and oxygen defects strengthens Ni 3d–O 2p hybridization, narrows the band gap, and accelerates charge redistribution. The results establish a structure–defect–activity correlation for layered nickelates and show that microwave-induced non-equilibrium synthesis provides a versatile route for designing metastable oxides. This work advances the understanding of structure-driven electrocatalysis and offers a strategic framework for future energy–environment catalytic technologies.

尿素电氧化提供了一种低压制氢途径,同时解决了氮循环修复问题,但其多步骤机制受到缓慢的C-N键裂解和强吸附中间体积累的动力学阻碍。传统的镍基氧化物暴露于Ni-O活性位点有限,电荷再分配缓慢,限制了整体催化周转。在这项研究中,采用微波冲击策略构建了具有明确定义的Ruddlesden-Popper (n = 2)层状结构的二维多孔La2NiO4纳米片。超快非平衡合成产生了瞬态过饱和,控制了气体演化,促进了开放层间通道和丰富氧空位的形成。这种结构增强了混合离子-电子传递,促进了尿素氧化过程中质子耦合电子的快速转移,产生了低起始电位、高质量活性和优异的耐久性。机理分析表明,Ni2+/Ni3+氧化还原对和氧缺陷的共存增强了Ni 3d-O - 2p杂化,缩小了带隙,加速了电荷的再分配。结果建立了层状镍酸盐的结构-缺陷-活性相关性,并表明微波诱导非平衡合成为设计亚稳氧化物提供了一种通用的途径。这项工作促进了对结构驱动电催化的理解,并为未来的能源-环境催化技术提供了一个战略框架。
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引用次数: 0
Optimization of Light-Management Strategies in All-Perovskite Four-Terminal Tandem Solar Cells: Efficiency Enhancement and Optical Loss Analysis 全钙钛矿四端串联太阳能电池光管理策略的优化:效率提高和光损耗分析
IF 12 Pub Date : 2026-02-15 DOI: 10.1002/cnl2.70126
Zhaosheng Xia, Yeqiang Yan, Xingang Ren, Bo Wu, Rida Ahmed, Gang Wang, Xiaoyan Zhao, Hong Zhang, Hui Wang, Zhixiang Huang

All-perovskite four-terminal tandem solar cells offer a promising platform for high-efficiency photovoltaics due to their electrical independence and flexible subcell optimization. However, optical losses such as interfacial reflection and parasitic absorption limit device performance. In this study, a systematic light-management optimization framework was established, and multiphysics simulations were employed to reveal how perovskite layer thickness, intermediate light-coupling layer (ILCL) materials and thickness, and top cell structural inversion collaboratively regulate light distribution, electromagnetic field phase, and transmission and reflection characteristics. Optimizing the perovskite layer thickness balances light absorption between subcells, increasing the power conversion efficiency (PCE) from 25.0% to 26.1%. Further introduction of the ILCL with phase-control design enhances optical coupling, raising the PCE to 28.10%. Numerical simulations indicate that top cell structural inversion effectively suppresses long-wavelength reflection and enhances bottom cell absorption, resulting in a simulated PCE of 33.73%, approaching the theoretical limit predicted by a semiempirical model guided by experimental data. Quantitative analysis based on admittance and phase matching elucidates the optical mechanisms, providing generalizable guidance for the design of multijunction photovoltaic devices. These results demonstrate that a unified light-management strategy not only systematically enhances device performance but also provides deep insights into the optical physics of all-perovskite tandem solar cells.

全钙钛矿四端串联太阳能电池由于其电独立性和灵活的亚电池优化,为高效光伏发电提供了一个有前途的平台。然而,界面反射和寄生吸收等光学损耗限制了器件的性能。本研究建立了系统的光管理优化框架,并采用多物理场模拟揭示了钙钛矿层厚度、中间光耦合层(ILCL)材料和厚度以及顶电池结构反演如何协同调节光分布、电磁场相位以及传输和反射特性。优化钙钛矿层厚度平衡亚电池之间的光吸收,将功率转换效率(PCE)从25.0%提高到26.1%。进一步引入相位控制设计的ILCL增强了光耦合,将PCE提高到28.10%。数值模拟表明,顶胞结构反演有效抑制了长波反射,增强了底胞吸收,模拟PCE为33.73%,接近实验数据指导下半经验模型预测的理论极限。基于导纳和相位匹配的定量分析阐明了多结光电器件的光学机理,为多结光电器件的设计提供了可推广的指导。这些结果表明,统一的光管理策略不仅系统地提高了器件性能,而且为全钙钛矿串联太阳能电池的光学物理提供了深刻的见解。
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引用次数: 0
Quantitative Phase Tuning and Interlayer Anchoring Stabilize Biphasic High-Entropy Cathodes for Sodium-Ion Batteries 定量相位调谐和层间锚定稳定钠离子电池双相高熵阴极
IF 12 Pub Date : 2026-02-11 DOI: 10.1002/cnl2.70129
Hao Liu, Yanfu Tong, Qin Cui, Pengyun Liu, Tonghui Cai, Yongpeng Cui, Zhi Liu, Xuejin Li, Wei Xing

The development of layered oxide cathodes for sodium-ion batteries is hindered by irreversible phase transitions and substantial volume changes at high voltages. While P2/O3 biphasic structures can mitigate these issues, achieving precise control over phase composition and understanding the underlying stabilization mechanisms remain challenging. Herein, we propose a synergistic regulation strategy integrating cationic potential design and thermal processing optimization. Using a high-entropy layered oxide Na0.75Ni0.29Zn0.05Cu0.06Mn0.6-xTixO2 as a model, we establish a quantitative correlation between Ti4+ content and the P2/O3 phase ratio, achieving continuous tuning from 0% to 100% O3 phase. Further refinement via calcination temperature yields an optimal P2:O3 ratio of 72.7:27.3. This optimally designed cathode delivers a high-rate capability (76.2 mAh g−1 at 5 A g−1) and superior cycling stability (77.5% capacity retention after 200 cycles). Operando XRD and DFT calculations reveal an “interlayer anchoring mechanism” at the phase boundary, where strong ionic bonding (e.g., Ti-O) suppresses transition metal layer sliding, guiding a highly reversible phase evolution and reducing the volume change to 7.6%, significantly lower than that of the single-phase counterpart (12.7%). This work provides a quantitative “composition–process–phase–performance” design principle for advanced biphasic cathode materials.

在高压条件下,不可逆的相变和大量的体积变化阻碍了钠离子电池层状氧化物阴极的发展。虽然P2/O3双相结构可以缓解这些问题,但实现对相组成的精确控制和了解潜在的稳定机制仍然具有挑战性。在此,我们提出了一种结合阳离子电位设计和热加工优化的协同调节策略。以高熵层状氧化物Na0.75Ni0.29Zn0.05Cu0.06Mn0.6-xTixO2为模型,建立了Ti4+含量与P2/O3相比之间的定量相关性,实现了O3相从0%到100%的连续调谐。通过煅烧温度进一步细化,得到最佳的P2:O3比为72.7:27.3。这种优化设计的阴极提供了高倍率容量(5ag - 1时76.2 mAh g - 1)和卓越的循环稳定性(200次循环后77.5%的容量保持)。Operando XRD和DFT计算揭示了相边界处的“层间锚定机制”,其中强离子键(例如Ti-O)抑制了过渡金属层的滑动,引导了高度可逆的相演变,并将体积变化降低到7.6%,明显低于单相对应的12.7%。这项工作为先进的双相阴极材料提供了定量的“成分-工艺-相位-性能”设计原则。
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引用次数: 0
Graphene–Based Two-Dimensional Nanomaterials: From Scalable Synthesis, Interfacial Mechanism to Emerging Biomedical Applications 基于石墨烯的二维纳米材料:从可扩展合成、界面机制到新兴的生物医学应用
IF 12 Pub Date : 2026-02-05 DOI: 10.1002/cnl2.70121
Shi Li, Sijie Xia, Xingchang Ma, Liang Du, Yian Li, Zuwu Tang, Zhenzeng Wu, Wei Zhang

Graphene–based porous two-dimensional (2D) materials are pivotal for advanced health, yet their translation faces three intertwined bottlenecks: scalable synthesis, quantifiable biological risks, and cradle-to-grave sustainability. Emerging paradigms now focus on developing green, surface–engineered porous nanomaterials that simultaneously display high biocompatibility, minimal cytotoxicity, and potent anticoagulant activity, enabling seamless deployment across in vitro diagnostics, targeted drug delivery, antimicrobial coatings, photothermal and gene therapies, and multimodal bioimaging. For the first time in a decade of numerous reviews on graphene's biomedical applications, this review focuses specifically on porous graphene two-dimensional materials. It systematically addresses three intertwined challenges and their solutions: controllable synthesis, biological risks, and full-lifecycle sustainability. We specifically highlight state-of-the-art functionalization strategies for porous nanomaterial preparation (e.g., mechanical exfoliation, chemical vapor deposition, oxidation–reduction, liquid-phase exfoliation, electrochemical exfoliation and SiC epitaxial growth method), alongside their potential risks to the human body, particularly interface mechanism with cell membranes, deoxyribonucleic acid (DNA), proteins, enzymes, cells, tissues, and organs. Current limitations and future research directions are critically discussed, emphasizing the role as a sustainable porous 2D nanomaterial platform. Beyond addressing healthcare challenges, high–performing graphene–based 2D nanomaterials unlock transformative opportunities for next-generation technologies.

基于石墨烯的多孔二维(2D)材料对于先进的健康至关重要,但其转化面临三个相互交织的瓶颈:可扩展的合成、可量化的生物风险和从摇篮到坟墓的可持续性。新兴的范例现在专注于开发绿色,表面工程多孔纳米材料,同时显示高生物相容性,最小的细胞毒性和强大的抗凝活性,能够无缝部署在体外诊断,靶向药物输送,抗菌涂层,光热和基因治疗,以及多模态生物成像。在十年来对石墨烯生物医学应用的众多评论中,这是第一次特别关注多孔石墨烯二维材料。它系统地解决了三个相互交织的挑战及其解决方案:可控合成、生物风险和全生命周期可持续性。我们特别强调了多孔纳米材料制备的最先进的功能化策略(例如,机械剥落,化学气相沉积,氧化还原,液相剥落,电化学剥落和SiC外延生长方法),以及它们对人体的潜在风险,特别是与细胞膜,脱氧核糖核酸(DNA),蛋白质,酶,细胞,组织和器官的界面机制。讨论了目前的局限性和未来的研究方向,强调了作为可持续多孔二维纳米材料平台的作用。除了解决医疗保健方面的挑战,高性能石墨烯基二维纳米材料还为下一代技术带来了变革机遇。
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引用次数: 0
Coordinated Solvation and Interphase Regulation by Sodium p-Aminobenzenesulfonate for Long-Life Aqueous Zinc-Ion Batteries 对氨基苯磺酸钠对长寿命锌离子电池的协同溶剂化和间相调节
IF 12 Pub Date : 2026-02-03 DOI: 10.1002/cnl2.70123
Jiangtao Tong, Yitong Wang, Yuhua Wang, Haijun Zhang, Jianxin Li, Denglei Zhu, Yao Guo, Xiaojing Bai, Chaojun Cui

Aqueous zinc-ion batteries (AZIBs) have garnered considerable attention due to their superior safety, affordability, and eco-friendliness. However, the uncontrolled growth of zinc dendrites and the parasitic hydrogen evolution reaction (HER) severely limit their cycling stability and practical lifespan. In this study, sodium p-aminobenzenesulfonate (SABS) is introduced into ZnSO4-based electrolytes as a functional additive. SABS not only reconstructs the Zn2+ solvation sheath but also forms stable complexes with Zn2+, facilitating the in-situ formation of a robust three-dimensional networked solid electrolyte interphase (SEI) on the zinc anode surface. As a result, Zn||Zn symmetric cells exhibit ultra-stable cycling performance exceeding 2000 h at 1 mA cm−2, while Zn||Cu asymmetric cells maintain over 2000 cycles at 5 mA cm−2 with high Coulombic efficiency. The underlying mechanism of interfacial stabilization and SEI-like interphase formation is further elucidated by combining ex situ structural/chemical characterizations with density functional theory (DFT) calculations. Moreover, the Zn||I2@AC full cell containing SABS additives exhibits excellent specific capacity and long-term cycling performance over a wide range of current densities. This work provides a promising electrolyte additive strategy to enhance the interfacial stability and electrochemical performance of AZIBs through coordinated solvation and interphase regulation.

水性锌离子电池(azib)因其优越的安全性、可负担性和环保性而受到广泛关注。然而,锌枝晶的生长失控和寄生析氢反应严重限制了锌枝晶的循环稳定性和实际使用寿命。本研究将对氨基苯磺酸钠(SABS)作为功能添加剂引入到硫酸锌基电解质中。SABS不仅重建了Zn2+的溶剂化鞘层,而且与Zn2+形成了稳定的配合物,促进了锌阳极表面原位形成坚固的三维网状固体电解质界面(SEI)。结果表明,Zn||Zn对称电池在1 mA cm - 2下的循环性能超过2000 h,而Zn||Cu不对称电池在5 mA cm - 2下的循环性能超过2000 h,具有较高的库仑效率。结合非原位结构/化学表征和密度泛函理论(DFT)计算,进一步阐明了界面稳定和类sei界面形成的潜在机制。此外,含有SABS添加剂的Zn||I2@AC全电池在大电流密度范围内表现出优异的比容量和长期循环性能。本研究提供了一种很有前途的电解质添加剂策略,通过协调的溶剂化和界面调节来提高azib的界面稳定性和电化学性能。
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引用次数: 0
Engineering Cathode–Electrolyte Interphase for High-Performance Li–S Batteries 高性能锂电池的工程阴极-电解液界面
IF 12 Pub Date : 2026-02-03 DOI: 10.1002/cnl2.70122
Anni Ai, Wei Wei, Kaijie Miao, Jiangqi Zhou

Lithium–sulfur (Li–S) batteries exhibit notable advantages, such as lower cost, due to the abundance and affordability of sulfur, coupled with superior gravimetric and volumetric energy densities, ample sulfur reserves, and a reduced environmental footprint. These compelling attributes render Li–S batteries a highly promising energy storage technology, attracting significant global interest. However, their practical deployment is hindered by critical challenges at the cathode–electrolyte interface, including structural degradation (such as heterogeneous Li2S deposition), unstable interphase layers, and the detrimental lithium polysulfides shuttle effect. Addressing these issues requires concerted efforts to optimize both the electrode and interface to improve overall battery performance. This review systematically delineates these interfacial challenges and discusses corresponding mitigation strategies, with emphasis on electrolyte design to form stable cathode–electrolyte interphases, control Li2S deposition behavior, and suppress the shuttle effect through modulation of solid–liquid–solid reaction pathways, their transition to solid–solid conversion routes, and the optimization of solid–solid pathways themselves. Finally, the article offers key perspectives aimed at advancing the fundamental understanding of interfacial phenomena and designing stable battery configurations, with the ultimate goal of stimulating further research and accelerating the commercialization of Li–S batteries.

锂硫(Li-S)电池具有显著的优势,例如成本较低,这是由于硫的丰富和可负担性,再加上优越的重量和体积能量密度,充足的硫储量,以及减少的环境足迹。这些令人信服的特性使Li-S电池成为一种非常有前途的储能技术,吸引了全球的广泛关注。然而,它们的实际部署受到阴极-电解质界面的关键挑战的阻碍,包括结构退化(如非均相Li2S沉积),不稳定的界面层,以及有害的锂多硫化物穿梭效应。解决这些问题需要共同努力,优化电极和接口,以提高整体电池性能。本文系统地描述了这些界面挑战并讨论了相应的缓解策略,重点介绍了通过调节固-液-固反应途径、向固-固转化途径的过渡以及优化固-固途径本身来设计电解质以形成稳定的阴极-电解质界面,控制Li2S沉积行为,抑制穿梭效应。最后,本文提供了关键的观点,旨在促进对界面现象的基本理解和设计稳定的电池配置,最终目标是刺激进一步的研究和加速Li-S电池的商业化。
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引用次数: 0
CeO2-Modified Ni3N as Highly Efficient Bifunctional Electrocatalysts for 5-Hydroxymethylfurfural Oxidation Coupled With Hydrogen Evolution ceo2修饰Ni3N作为5-羟甲基糠醛氧化-析氢高效双功能电催化剂
IF 12 Pub Date : 2026-02-03 DOI: 10.1002/cnl2.70127
Dongyue Cao, Zhuoshen Huang, Yifei Ye, Guangtong Hai, Xiubing Huang

The development of electrocatalysts with excellent water splitting and 5-hydroxymethylfural oxidation reaction (HMFOR) performance can relieve energy challenges and environmental issues. This study constructs a self-supported CeO2-Ni3N/NF composite on nickel foam (NF) through an elemental modification strategy, developing an electrocatalyst with outstanding electrochemical water splitting and HMFOR performance. The modified CeO2 introduces oxygen vacancy defects in Ni3N and optimizes its electronic structure. The reaction mechanism of HMFOR was explored using in situ characterizations, revealing that CeO2 not only promotes the complete reconstruction of Ni3N into active NiOOH species but also enhances charge transfer of the HMFOR process. CeO2 modulates the adsorption of reactant on the Ni active sites, thereby mitigating the reduction in reaction activity caused by competitive adsorption. Additionally, CeO2 reduces the activation energy needed for the intermediate step from *FFCA to *FDCA. By substituting the anodic reaction with HMFOR, the voltage for water splitting can be reduced, while simultaneously generating valuable organic compounds during hydrogen evolution. Specifically, utilizing HMFOR to replace the traditional anodic reaction in water electrolysis only needs 1.43 V to realize 50 mA cm−2, with a Faradaic efficiency (FE) for cathodic hydrogen evolution approaching 100%, a superior HMF conversion rate (93.6%), and FDCA yield (93.4%). This research provides significant insights for designing transition metal-based catalysts with excellent electrolytic water and HMFOR performance.

开发具有优异的水分解和5-羟甲基糠醛氧化反应性能的电催化剂可以缓解能源挑战和环境问题。本研究通过元素改性策略在泡沫镍(NF)上构建了一种自持型CeO2-Ni3N/NF复合材料,开发了一种具有优异电化学水分解和HMFOR性能的电催化剂。改性后的CeO2在Ni3N中引入了氧空位缺陷,优化了Ni3N的电子结构。通过原位表征探索了HMFOR的反应机理,发现CeO2不仅促进Ni3N完全重构为活性NiOOH,而且促进了HMFOR过程的电荷转移。CeO2调节反应物在Ni活性位点上的吸附,从而减轻竞争性吸附引起的反应活性降低。此外,CeO2降低了从*FFCA到*FDCA中间步骤所需的活化能。通过用HMFOR代替阳极反应,可以降低水裂解的电压,同时在析氢过程中生成有价值的有机化合物。具体而言,利用HMFOR取代传统的电解水阳极反应,仅需1.43 V即可实现50 mA cm−2,阴极析氢的法拉第效率(FE)接近100%,HMF转化率(93.6%)和FDCA收率(93.4%)优异。该研究为设计具有优异电解水和HMFOR性能的过渡金属基催化剂提供了重要的见解。
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Carbon Neutralization
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