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High-entropy alloys for hydrogen storage, separation, and detection: Recent progress and prospects 用于储氢、分离和检测的高熵合金:最新进展与展望
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-11-28 DOI: 10.1016/j.esci.2025.100506
Jiaxi Liu , Pengru Huang , Yongpeng Xia , Yanping Liu , Yumei Luo , Huanzhi Zhang , Yongjin Zou , Hailiang Chu , Gaixia Zhang , Shuhui Sun , Sergey P. Verevkin , Sergey V. Vostrikov , Lixian Sun , Fen Xu , Zongwen Liu , Hongge Pan
As a pivotal clean energy carrier with promising efficiency, environmental friendliness, and sustainability, hydrogen stands at the forefront of the global energy technology revolution. However, achieving the efficient storage, easy separation, and trace detection of hydrogen remain critical challenges. High-entropy alloys (HEAs) have garnered attention because of their remarkable attributes, including high stability, single-phase reversibility, and a wide tunable range of composition and electronic structure. Commencing with a succinct background overview, we explore the pivotal role of theoretical methods in designing the phase structure and ensuring the stability of HEAs, focusing especially on diverse element types and contents. We then present a summary of prevalent methods for preparing HEAs, followed by a detailed examination of recent advances in their hydrogen-related properties, encompassing hydrogen storage, separation, and detection. Finally, we look at the existing challenges and offer perspectives on the trajectory of future research and applications in this promising technological domain.
氢作为一种重要的清洁能源载体,具有高效、环保和可持续性等特点,站在全球能源技术革命的前沿。然而,实现氢的高效储存,易于分离和痕量检测仍然是关键的挑战。高熵合金(HEAs)因其高稳定性、单相可逆性、广泛的成分和电子结构可调范围等特点而备受关注。从简单的背景概述开始,我们探讨了理论方法在设计相结构和确保HEAs稳定性方面的关键作用,特别是关注不同元素类型和含量。然后,我们总结了制备HEAs的流行方法,然后详细研究了HEAs的氢相关特性的最新进展,包括氢的储存、分离和检测。最后,我们展望了现有的挑战,并对这一前景广阔的技术领域的未来研究和应用轨迹提出了展望。
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引用次数: 0
A review of advanced SOFCs and SOECs: Materials, innovative synthesis, functional mechanisms, and system integration 先进SOFCs和socs:材料、创新合成、功能机制和系统集成
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-08-14 DOI: 10.1016/j.esci.2025.100460
Peng Feng , Kuan Yang , Xuanyou Liu , Jiujun Zhang , Zhi-Peng Li
Solid oxide fuel cells (SOFCs) and solid oxide electrolysis cells (SOECs) are next-generation energy conversion technologies that have attracted widespread attention due to their high efficiency, fuel flexibility, and environmental friendliness. The reversible reaction processes of the two can achieve power generation and energy storage in one device. This paper provides an extensive overview of the latest developments in the field of SOFCs and SOECs, including types, material synthesis, mechanism research, and system integration. First, we introduce the classification of current SOFCs/SOECs according to their different supports and conducting ions. Then, we summarize the synthesis methods and optimization strategies for key materials, including the latest developments in electrolytes, electrodes, and interconnects. Subsequently, the electrochemical mechanisms, including ion transport, electron conduction, electrochemical reaction kinetics, and interfacial phenomena, are analyzed in depth. This paper also outlines challenges and strategies for system integration, such as thermal management, fluid dynamics, and mechanical stress control. Through comprehensive analysis, this review aims to provide researchers with a holistic perspective and guidance for the future development of SOFCs and SOECs. We close by discussing the main challenges and future research directions for further promoting the commercialization and large-scale development of these technologies.
固体氧化物燃料电池(SOFCs)和固体氧化物电解电池(SOECs)是新一代能源转换技术,因其高效、燃料灵活性和环境友好性而受到广泛关注。两者的可逆反应过程可以在一个装置中实现发电和储能。本文综述了SOFCs和soec领域的最新进展,包括类型、材料合成、机理研究和系统集成。首先,我们介绍了当前sofc / soec根据其不同的支持和导电离子的分类。然后,我们总结了关键材料的合成方法和优化策略,包括电解质、电极和互连的最新进展。随后,深入分析了离子传递、电子传导、电化学反应动力学和界面现象等电化学机理。本文还概述了系统集成的挑战和策略,如热管理、流体动力学和机械应力控制。通过综合分析,本文旨在为SOFCs和soec的未来发展提供一个整体的视角和指导。最后,我们讨论了进一步促进这些技术的商业化和大规模开发的主要挑战和未来的研究方向。
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引用次数: 0
Nonequilibrium carriers trigger hydrogen spillover for the highly efficient semihydrogenation of alkynes under ambient conditions 非平衡载流子引发氢溢出,在环境条件下实现了高效的炔烃半加氢反应
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-10-09 DOI: 10.1016/j.esci.2025.100481
Aonan Zhu , Ning Zhao , Yue Mao , Ling Yang , Ji Qi , Taghrid S. Alomar , Najla AlMasoud , Wei Xie
Facile reactant dissociation and weakly bound intermediates are essential for achieving both efficient and selective catalysis. However, these two factors are inherently interconnected, making their simultaneous optimization particularly challenging. Herein, we propose a decoupling strategy to circumvent this limitation and demonstrate it using a novel antenna-reactor catalyst constructed with single atom and plasmonic nanoparticles. By combining in situ surface-enhanced Raman spectroscopy with density functional theory calculations, we reveal that nonequilibrium carriers significantly enhance hydrogen dissociation at Pd single-atom sites. Subsequently, these active hydrogen atoms spillover to adjacent Au surfaces, facilitating more favorable alkyne hydrogenation and alkene desorption processes. Consequently, the Pd SAC-Au photocatalyst exhibits remarkable catalytic performance, achieving a turnover frequency value of 3964 molC=C molPd1 h−1 and demonstrating 99.99% conversion of phenylacetylene with 90% selectivity toward styrene under mild reaction conditions (298 K, 101.3 kPa). This approach offers a novel pathway to overcome traditional catalytic trade-off, highlighting the potential for designing high-performance single-atom catalysts for chemical reactions.
容易的反应物解离和弱结合的中间体是实现高效和选择性催化的必要条件。然而,这两个因素本质上是相互关联的,使得它们的同时优化特别具有挑战性。在此,我们提出了一种解耦策略来绕过这一限制,并使用一种由单原子和等离子体纳米粒子构成的新型天线反应器催化剂来证明它。通过将原位表面增强拉曼光谱与密度泛函理论计算相结合,我们发现非平衡载流子显著增强了Pd单原子位点的氢解离。随后,这些活性氢原子溢出到相邻的金表面,促进更有利的炔加氢和烯烃脱附过程。因此,Pd - SAC-Au光催化剂表现出优异的催化性能,在温和的反应条件下(298 K, 101.3 kPa),转换频率值为3964 molC=C molPd−1 h−1,苯乙炔转化率为99.99%,苯乙烯选择性为90%。这种方法为克服传统的催化权衡提供了一种新的途径,突出了设计用于化学反应的高性能单原子催化剂的潜力。
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引用次数: 0
Multi-rare-earth alloy nanoparticles from binary to septenary for electrocatalytic semi-hydrogenation of acetylene 用于乙炔电催化半加氢的二元至七元稀土合金纳米颗粒
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-09-23 DOI: 10.1016/j.esci.2025.100477
Cheng Yang , Huawei Li , Senyao Meng , Yaqin Hou , Ping Wang , Jiasai Yao , Jiarui Yang , Zechao Zhuang , Tianbao Zhang , Rui Tan , Dingsheng Wang , Zhenxing Li
The controllable synthesis of palladium-based multi-rare-earth alloy nanomaterials via chemical methods poses a considerable challenge, owing to the low reduction potential and high oxophilicity of rare earth (RE) elements. Herein, a series of Pd-RE alloy nanoparticles, from binary to septenary alloy, is newly designed and synthesized through the single atom-enhanced chemical potential method. This synthetic strategy utilizes a single atom to effectively enhance the chemical potential of a rare earth atom, which thermodynamically favors the synthesis of a Pd-RE alloy. Using this general chemical synthesis method, we successfully synthesized 22 kinds of Pd-RE alloy nanoparticles, including 4 kinds of Pd-RE high-entropy alloy nanoparticles. The ErPd3 catalyst demonstrated outstanding electrocatalytic performance in acetylene hydrogenation: electron-enriched Pd sites facilitated acetylene adsorption and activation, while the incorporated Er effectively suppressed the competing hydrogen evolution reaction, thereby significantly enhancing the utilization efficiency of H∗. This work establishes a general strategy for designing Pd-RE alloy nanomaterials.
由于稀土元素的低还原电位和高亲氧性,通过化学方法可控合成钯基多稀土合金纳米材料面临相当大的挑战。本文采用单原子增强化学势法,设计并合成了从二元合金到七元合金的一系列Pd-RE合金纳米颗粒。该合成策略利用单个原子有效地增强稀土原子的化学势,这在热力学上有利于Pd-RE合金的合成。利用这种通用的化学合成方法,我们成功地合成了22种Pd-RE合金纳米颗粒,其中包括4种Pd-RE高熵合金纳米颗粒。ErPd3催化剂在乙炔加氢过程中表现出优异的电催化性能:富含电子的Pd位点促进了乙炔的吸附和活化,而加入的Er有效地抑制了竞争性析氢反应,从而显著提高了H *的利用效率。本研究为钯稀土合金纳米材料的设计提供了一个总体思路。
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引用次数: 0
Noble metal-free single-atom electrocatalysts and reactor engineering for enhanced hydrogen peroxide generation via two-electron oxygen reduction reaction 无贵金属单原子电催化剂及通过双电子氧还原反应增强过氧化氢生成的反应器工程
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-07-25 DOI: 10.1016/j.esci.2025.100456
Jingqin Ji , Hui Wang , Yanlan Zhao , Yan Wang , Kaifeng Wang , Yuexin Cui , Ridha Djellabi , Chuan Xia , Xu Zhao , Xiangming He
The generation of hydrogen peroxide (H2O2), a compound with diverse applications, via the two-electron (2e) oxygen reduction reaction (ORR) has garnered extensive attention in both laboratory research and industrial settings. The integration of non-noble metals such as Co, Fe, Ni, Zn, Mn, Mo, or Bi into nitrogen-doped carbon (M–N–C) matrices with defined structures and active metal center sites has emerged as a promising approach for fabricating electrocatalysts for the ORR. This review uncovers the latest advancements in the development of noble metal-free single-atom electrocatalysts (M–N–C SAECs) and electrochemical reactors aimed at enhancing and stabilizing H2O2 production from the 2e ORR. Firstly, the review explores the basics of the ORR for H2O2 production and the impact of electrochemical conditions. Subsequently, the synthesis strategies and characterization methods of various M–N–C SAECs are examined in depth. In addition, the structural attributes of both conventional and altered M–N–C SAECs are meticulously investigated, and the importance of engineering and optimizing reactors to elevate H2O2 yields is highlighted. This review identifies the challenges and technological hurdles in bridging the gap between laboratory-scale research and practical, real-world applications.
过氧化氢(H2O2)是一种应用广泛的化合物,通过双电子(2e−)氧还原反应(ORR)生成过氧化氢(H2O2)在实验室研究和工业环境中都得到了广泛的关注。将Co, Fe, Ni, Zn, Mn, Mo或Bi等非贵金属整合到具有明确结构和活性金属中心位置的氮掺杂碳(M-N-C)基体中,已成为制造ORR电催化剂的一种有前途的方法。本文综述了无贵金属单原子电催化剂(M-N-C saec)和旨在提高和稳定2e - ORR产生H2O2的电化学反应器的最新进展。首先,综述了ORR生产H2O2的基本原理和电化学条件的影响。随后,深入研究了各种M-N-C saec的合成策略和表征方法。此外,本文还详细研究了常规和改进型M-N-C saec的结构特性,并强调了提高H2O2产率的工程和优化反应器的重要性。这篇综述指出了在弥合实验室规模研究和实际应用之间的差距方面面临的挑战和技术障碍。
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引用次数: 0
Scalable and universal synthesis of hierarchical organic/carbon composites towards practical organic batteries 面向实用有机电池的分级有机/碳复合材料的可扩展和通用合成
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-09-17 DOI: 10.1016/j.esci.2025.100474
Xing Wu , Huiling Peng , Lei Zhang , Yaheng Geng , Zehao Yu , Mengjiao Li , Yuhong Nie , Zichao Yan , Mingshan Han , Yuxiang Hu , Zhiqiang Zhu
Organic electrode materials with renewability, environmental benignity, and structural tunability have attracted increasing attention for lithium-ion batteries, but their practical application is hindered by low mass loadings (< 2 mg cm−2) and inadequate areal capacities (< 0.5 mAh cm−2), primarily due to low electronic conductivity and sluggish ion diffusion. Here, we address these limitations by introducing a scalable spray-drying method to synthesize hierarchical organic/carbon composites. By using lithium terephthalate (Li2TP), carbon nanotubes (CNTs), and polyvinylpyrrolidone as precursors, we fabricate Li2TP-H, a composite featuring Li2TP nanoparticles (∼20 nm) assembled into microspheres with 3D CNTs networks. This hierarchical design ensures efficient ion and electron transport, yielding a high capacity retention of 91.6% (from 298 to 273 mAh g−1) when increasing mass loading from 2 to 43 mg cm−2. The resulting areal capacity of 11.7 mAh cm−2 ranks among the highest reported for organic electrodes. Moreover, the methodology is extendable to other carboxylate-based compounds, with all derivatives exhibiting enhanced performance under a high-mass-loading of 10 mg cm−2. This work provides a new paradigm for developing high-areal-capacity organic electrodes, representing a pivotal step toward commercializing organic battery technologies.
具有可再生性、环境友好性和结构可调性的有机电极材料越来越受到锂离子电池的关注,但其实际应用受到低质量负载(< 2mg cm - 2)和面积容量(< 0.5 mAh cm - 2)的阻碍,主要是由于电子电导率低和离子扩散缓慢。在这里,我们通过引入一种可扩展的喷雾干燥方法来合成分层有机/碳复合材料来解决这些限制。通过使用对苯二甲酸锂(Li2TP)、碳纳米管(CNTs)和聚乙烯吡咯烷酮作为前体,我们制备了Li2TP- h,这是一种将Li2TP纳米颗粒(~ 20 nm)组装成具有3D碳纳米管网络的微球的复合材料。这种分层设计确保了高效的离子和电子传输,当质量负载从2增加到43 mg cm - 2时,产生91.6%的高容量保留(从298到273 mAh g - 1)。所得的面积容量为11.7 mAh cm−2,是有机电极中最高的。此外,该方法可扩展到其他羧酸基化合物,所有衍生物在10 mg cm−2的高质量负载下表现出增强的性能。这项工作为开发高面积容量有机电极提供了一个新的范例,代表了有机电池技术商业化的关键一步。
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引用次数: 0
Inspired by green corrosion chemistry and wastewater remediation: A high-performance Zn anode with locally gradient microstructures 受绿色腐蚀化学和废水修复启发:一种具有局部梯度微结构的高性能锌阳极
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-07-29 DOI: 10.1016/j.esci.2025.100459
Bing Wu , Weihao Song , Jiaying Peng , Qing Ma , Masatsugu Fujishige , Morinobu Endo , Jin Niu , Feng Wang
Driven by the new energy industry’s rapid growth, surging demand for lithium/zinc raw materials has accelerated polymetallic ore mining. Cadmium ions (Cd2+), as co-existing heavy metal pollutants in smelting wastewater, pose environmental challenges while inspiring innovative solutions. This work introduces a green corrosion approach achieving > 99% removal of Cd2+, Pb2+, and Cu2+ via Zn foil functionalization. During controlled corrosion, Cd2+ are directly reduced to metallic Cd by Zn, while generated Zn2+ form Zn5(OH)8Cl2⋅H2O (ZCH) nanosheet arrays in situ. A gelatin-assisted low-temperature pyrolysis then converts these products into a carbon/Cd/zinc oxide (ZO-Cd-GC) multilayer on Zn foil, which creates a local gradient in Zn anode properties: enhanced zincophilicity, improved Zn2+ desolvation, and suppressed hydrogen evolution from electrolyte to anode. The resulting Zn@ZO-Cd-GC anode enables uniform electron/ion transport, fast kinetics, suppressed side reactions, and dendrite-free deposition. Symmetric cells with this anode exhibit an ultra-long lifetime exceeding 6000 h at 2 mA cm−2/1 mAh cm−2 and stable operation without short-circuiting at 20 mA cm−2. A Zn@ZO-Cd-GC||NH4V4O10 pouch cell delivers a high discharge capacity and maintains stability over 2000 cycles at 33.75 mA cm−2.
在新能源产业快速增长的带动下,锂/锌原料需求激增,加速了多金属矿开采。镉离子(Cd2+)作为冶炼废水中共存的重金属污染物,在激发创新解决方案的同时,也给环境带来了挑战。这项工作介绍了一种绿色腐蚀方法,通过锌箔功能化实现了99%的Cd2+, Pb2+和Cu2+的去除。在控制腐蚀过程中,Cd2+被Zn直接还原为金属Cd,而Zn2+则在原位形成Zn5(OH)8Cl2⋅H2O (ZCH)纳米片阵列。然后明胶辅助低温热解将这些产物转化为锌箔上的碳/Cd/氧化锌(ZO-Cd-GC)多层,从而在锌阳极性能上产生局部梯度:增强亲锌性,改善Zn2+的脱溶,抑制氢从电解质向阳极的析出。由此产生的Zn@ZO-Cd-GC阳极能够实现均匀的电子/离子传输,快速动力学,抑制副反应和无枝晶沉积。具有这种阳极的对称电池在2 mA cm - 2/1 mAh cm - 2下具有超过6000小时的超长寿命,并且在20 mA cm - 2下稳定运行而不短路。Zn@ZO-Cd-GC||NH4V4O10袋电池提供高放电容量,并在33.75 mA cm−2下保持超过2000次循环的稳定性。
{"title":"Inspired by green corrosion chemistry and wastewater remediation: A high-performance Zn anode with locally gradient microstructures","authors":"Bing Wu ,&nbsp;Weihao Song ,&nbsp;Jiaying Peng ,&nbsp;Qing Ma ,&nbsp;Masatsugu Fujishige ,&nbsp;Morinobu Endo ,&nbsp;Jin Niu ,&nbsp;Feng Wang","doi":"10.1016/j.esci.2025.100459","DOIUrl":"10.1016/j.esci.2025.100459","url":null,"abstract":"<div><div>Driven by the new energy industry’s rapid growth, surging demand for lithium/zinc raw materials has accelerated polymetallic ore mining. Cadmium ions (Cd<sup>2+</sup>), as co-existing heavy metal pollutants in smelting wastewater, pose environmental challenges while inspiring innovative solutions. This work introduces a green corrosion approach achieving &gt; 99% removal of Cd<sup>2+</sup>, Pb<sup>2+</sup>, and Cu<sup>2+</sup> via Zn foil functionalization. During controlled corrosion, Cd<sup>2+</sup> are directly reduced to metallic Cd by Zn, while generated Zn<sup>2+</sup> form Zn<sub>5</sub>(OH)<sub>8</sub>Cl<sub>2</sub>⋅H<sub>2</sub>O (ZCH) nanosheet arrays <em>in situ</em>. A gelatin-assisted low-temperature pyrolysis then converts these products into a carbon/Cd/zinc oxide (ZO-Cd-GC) multilayer on Zn foil, which creates a local gradient in Zn anode properties: enhanced zincophilicity, improved Zn<sup>2+</sup> desolvation, and suppressed hydrogen evolution from electrolyte to anode. The resulting Zn@ZO-Cd-GC anode enables uniform electron/ion transport, fast kinetics, suppressed side reactions, and dendrite-free deposition. Symmetric cells with this anode exhibit an ultra-long lifetime exceeding 6000 h at 2 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup> and stable operation without short-circuiting at 20 mA cm<sup>−2</sup>. A Zn@ZO-Cd-GC||NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> pouch cell delivers a high discharge capacity and maintains stability over 2000 cycles at 33.75 mA cm<sup>−2</sup>.</div></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"6 2","pages":"Article 100459"},"PeriodicalIF":36.6,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146039158","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Crystallization modulation in perovskite light-emitting diodes 钙钛矿发光二极管的结晶调制
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-09-29 DOI: 10.1016/j.esci.2025.100478
Aqiang Liu , Jifeng Yuan , Yongge Yang , Hong Lian , Yuwei Guo , Xuyong Yang , Wojciech Pisula , Shuanglong Wang
Recent developments in perovskite light-emitting diodes (PeLEDs) have been driven by strategies for modulating crystallization that precisely control nucleation, growth, and crystal structures. This review provides a multi-scale perspective on perovskite crystallization by integrating knowledge-driven theories with data-driven insights to propel the development of PeLEDs. We first outline classical nucleation and growth models, establishing the theoretical foundations of crystallization dynamics. We then examine state-of-the-art in situ characterization techniques, highlighting their unparalleled capacity to resolve spatiotemporal crystallization processes. A systematic discussion follows on the critical role of crystallization modulation, including film morphology tuning, crystal structure control, and preferred orientation management—three key factors for optimizing optoelectronic properties. Finally, we explore persistent challenges and emerging opportunities in crystallization design. By bridging theoretical frameworks with experimental advancements, this work aims to refine crystallization control for high-performance and stable PeLEDs.
钙钛矿发光二极管(PeLEDs)的最新发展是由精确控制成核、生长和晶体结构的调制结晶策略驱动的。本文通过将知识驱动的理论与数据驱动的见解相结合,为钙钛矿结晶的发展提供了一个多尺度的视角。我们首先概述了经典的成核和生长模型,建立了结晶动力学的理论基础。然后,我们研究了最先进的原位表征技术,突出了其无与伦比的解决时空结晶过程的能力。系统地讨论了结晶调制的关键作用,包括薄膜形态调谐、晶体结构控制和优选取向管理,这是优化光电性能的三个关键因素。最后,我们探讨了结晶设计中持续存在的挑战和新出现的机遇。通过将理论框架与实验进展相结合,这项工作旨在改进高性能和稳定的ped的结晶控制。
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引用次数: 0
Two-dimensional polymeric metal phthalocyanines with anion fluxing and Li-ion-conducting properties for lithium metal full batteries 具有阴离子通量和锂离子导电性能的二维聚合物金属酞菁用于锂金属电池
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-10-01 DOI: 10.1016/j.esci.2025.100480
Jun Su Kim , Yoonbin Kim , Sang Ha Baek , Yonggoon Jeon , Suhwan Kim , Won Il Kim , Dong Wook Kim , Hongdae Lee , Shengyang Huang , Hyun Chul Kim , Jeongyeon Lee , Yong Min Lee , Atsuo Yamada , Jungwon Park , Ho Seok Park
Herein, we report the molecular engineering of anion-fluxing polymeric metal phthalocyanines (MTPs) by controlling the types of metal centers and incorporating lithiophilic linkers to achieve ultrastable Li metal batteries. Spectroscopic characterization, cryogenic transmission electron microscopy, and computational simulations demonstrate that the Co–N4 sites of Co in the incorporated MTP (CoTP) facilitate the local accumulation and directional flux of TFSI anions, inducing the formation of uniform, dense LiF-rich solid electrolyte interphases. As a result of this interfacial chemistry, symmetric cells with CoTP@CC–Li exhibited outstanding cycling stability, exceeding 2500 h at 1 mA cm−2 and 1 mAh cm−2. CoTP@CC–Li||LiFePO4 full cells operated stably for over 600 cycles under fast charge/discharge conditions, with a high-mass-loading cathode of 20 mg cm−2. CoTP@CC–Li||LiFePO4 pouch cells demonstrated stable cyclability under demanding practical conditions, including a low N/P ratio of 2.5, high cathode mass loading (23.53 mg cm−2), and lean electrolyte usage (5 g Ah−1). Furthermore, CoTP@CC-enabled anode-free full cells achieved exceptional stability over 500 cycles, even under stringent conditions (NCM811 mass loading of 20 mg cm−2 and lean electrolyte usage of 3 g Ah−1). These results highlight the effectiveness of the anion-flux interfacial engineering strategy for enabling stable and reversible Li deposition under demanding conditions.
本文报道了通过控制金属中心的类型和加入亲锂连接剂来实现阴离子通量聚合金属酞菁(MTPs)的分子工程,以实现超稳定的锂金属电池。光谱表征、低温透射电镜和计算模拟表明,Co在掺杂MTP (CoTP)中的Co - n4位点促进了TFSI阴离子的局部积累和定向通量,诱导形成均匀、致密的富liff固体电解质界面。由于这种界面化学,含有CoTP@CC -Li的对称电池表现出出色的循环稳定性,在1ma cm - 2和1mah cm - 2下超过2500小时。CoTP@CC -Li ||LiFePO4全电池在快速充放电条件下稳定运行超过600次,阴极质量负载为20 mg cm−2。CoTP@CC -Li ||LiFePO4袋电池在苛刻的实际条件下表现出稳定的可循环性,包括低N/P比2.5,高阴极质量负载(23.53 mg cm−2)和低电解质使用量(5 g Ah−1)。此外,CoTP@CC-enabled无阳极全电池即使在严格的条件下(NCM811质量负载为20 mg cm - 2,贫电解质使用量为3 g Ah - 1),也能在500次循环中实现卓越的稳定性。这些结果强调了阴离子通量界面工程策略在苛刻条件下实现稳定可逆锂沉积的有效性。
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引用次数: 0
Multi-site passivation agent for efficient tandem solar cells: Simultaneously suppressing defect recombination in NiOx surface, perovskite buried interface, and silicon edge 高效串联太阳能电池的多位点钝化剂:同时抑制NiOx表面、钙钛矿埋藏界面和硅边缺陷的复合
IF 36.6 Q1 ELECTROCHEMISTRY Pub Date : 2026-03-01 Epub Date: 2025-09-11 DOI: 10.1016/j.esci.2025.100471
Xinru Wang , Mengqi Li , Lijie Yu , Bingbing Chen , Mengnan Cui , Haishun Gao , Xueliang Yang , Xuning Zhang , Jianhui Chen
Wide-band gap perovskites combined with silicon (Si) in tandem solar cells offer a cost-effective path to industrialization. However, surface recombination at the buried interface of perovskite solar cells (PSCs) and the edge surface of Si solar cells affects their efficiency and stability. Herein, we design a multi-site passivation agent to simultaneously suppress defect recombination in hole transfer layer (HTL) surface, perovskite buried interface, and Si edge for efficient tandem solar cells. The increased ratio of Ni3+/Ni2+ reduces the nickel oxide (NiOx)/perovskite interface reaction and improves the conductivity of the NiOx HTL. The reconstructed underlayer is more propitious to the perovskite deposition, which releases the residual strain, resulting in the enhancement of the efficiency and stability of PSCs. Moreover, the multi-site passivation agent presents a distinctive passivation effect for edge surface of Si solar cells. Power conversion efficiencies (PCEs) of 21.95% and 20.01% are obtained at opaque and semitransparent PSCs, respectively. Additionally, a four-terminal tandem solar cell exhibits a PCE of 31.02% with +1.19%abs PCE increase for bottom cell by edge surface passivation. Overall, this work provides a simple and multi-site surface defect passivation strategy for obtaining high-efficiency and stable perovskite and perovskite tandem solar cells.
宽带隙钙钛矿与硅(Si)相结合的串联太阳能电池为产业化提供了一条经济有效的途径。然而,钙钛矿太阳电池(PSCs)的埋藏界面和硅太阳电池的边缘表面的表面复合影响了它们的效率和稳定性。在此,我们设计了一种多位点钝化剂,可以同时抑制高效串联太阳能电池的空穴转移层(HTL)表面、钙钛矿埋藏界面和Si边缘的缺陷重组。Ni3+/Ni2+的增加减少了氧化镍(NiOx)/钙钛矿界面反应,提高了NiOx HTL的导电性。重构后的衬底层更有利于钙钛矿沉积,从而释放残余应变,提高了聚苯乙烯复合材料的效率和稳定性。此外,多位点钝化剂对硅太阳电池的边缘表面表现出明显的钝化效果。在不透明和半透明的PSCs上,功率转换效率分别为21.95%和20.01%。此外,四端串联太阳能电池的PCE为31.02%,底部电池的PCE增加了+1.19%。总的来说,这项工作为获得高效稳定的钙钛矿和钙钛矿串联太阳能电池提供了一种简单的多位点表面缺陷钝化策略。
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