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Discovery of a new phase transition and high-valent redox mechanism in Fe-substituted Na2Mn3O7 铁取代Na2Mn3O7新相变及高价氧化还原机制的发现
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.nanoen.2026.111737
Hugh Barrett Smith , Bachu Sravan Kumar , Anirudh Adavi , Willem Vanmoerkerke , Ming Lei , Tong Wu , Jorge Moncada , Hui Zhong , Jianming Bai , Adrian Hunt , Iradwikanari Waluyo , Eli Stavitski , Loza F. Tadesse , Iwnetim Iwnetu Abate
Sodium-ion batteries are a promising lower-cost alternative to lithium-ion batteries, but further improvements in electrochemical performance are required. One strategy to increase capacity is to enable reversible high-valent cationic and anionic redox in layered cathode materials; however, this is typically accompanied by structural degradation. Here, we elucidate the mechanism by which Fe-doped Na2Mn3O7, featuring ordered transition metal-vacancies, achieves reversible high-valent redox. Using Mössbauer spectroscopy, soft X-ray absorption spectroscopy (XAS), and in-situ hard XAS, we demonstrate reversible high-valent cationic redox involving both Fe and Mn while in-situ Raman confirms the absence of local structural degradation associated with oxygen redox. Combining in-situ X-ray diffraction with theoretical calculations, we further identify a previously unreported global phase transition from the P1̅ to the P21/c space group during electrochemical cycling and develop a physical model describing this structural evolution. These results provide insights for structurally stable layered sodium transition metal oxide cathodes with reversible high-valent redox.
钠离子电池是一种很有前途的低成本锂离子电池替代品,但电化学性能还需要进一步改进。提高容量的一种策略是在层状阴极材料中实现可逆的高价阳离子和阴离子氧化还原;然而,这通常伴随着结构退化。在这里,我们阐明了具有有序过渡金属空位的fe掺杂Na2Mn3O7实现可逆高价氧化还原的机制。利用Mössbauer光谱,软x射线吸收光谱(XAS)和原位硬XAS,我们证明了铁和锰的可逆高价阳离子氧化还原,而原位拉曼证实了不存在与氧氧化还原相关的局部结构降解。结合原位x射线衍射和理论计算,我们进一步确定了电化学循环过程中从P1′s到P21/c空间群的全局相变,并建立了描述这种结构演变的物理模型。这些结果为具有可逆高价氧化还原的结构稳定的层状过渡金属氧化物钠阴极提供了见解。
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引用次数: 0
Molecular engineering of weak intermolecular interactions for regulating solvation and interface in cyclic ether electrolytes enabling robust lithium metal batteries 调节循环醚电解质溶剂化和界面的弱分子间相互作用的分子工程,实现坚固的锂金属电池
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.nanoen.2026.111744
Qujiang Sun , Bowen Yang , Di Zhang , Zhaojin Li , Qiujun Wang , Fei Yuan , Ranran Li , Huilan Sun , Yeguo Zou , Yu Qiao , Bo Wang
Lithium metal anodes are pivotal for pursuing high-energy-density lithium-ion batteries, yet persistent challenges including dendrite-induced safety risks, incompatibility with conventional ester electrolytes, and poor low-temperature performance hinder their practical deployment. Herein, a solvation chemistry modulation strategy via weak intermolecular interactions in tetrahydrofuran (THF)-based electrolytes is proposed, employing a low-melting-point solvent 1, 1, 2, 2-tetrafluoroethyl-2, 2, 2-trifluoroethyl ether (TFTFE) as a diluent. We found that the weak intermolecular interactions (i.e., dipole-dipole interaction, anion-dipole interaction) can effectively weaken Li+-THF interaction within the solvation structure, facilitating Li+ desolvation kinetics and achieving 99.3 % Li plating/stripping Coulombic efficiency. The optimized electrolyte endows the 50 μm-Li || LiFePO4 full cell to maintain stable cycling over 500 cycles with 115 mAh g−1 at 5.0 C, while maintaining 95.7 % capacity retention over 100 cycles even at −20°C. This work highlights the significance of weak interactions in fine-tuning electrolyte properties, and also paving innovative approaches for developing compatible electrolytes towards low-temperature and fast-charging lithium metal batteries.
锂金属阳极是追求高能量密度锂离子电池的关键,但枝晶引发的安全风险、与传统酯电解质的不相容性以及低温性能差等持续存在的挑战阻碍了其实际应用。本文采用低熔点溶剂1,1,2,2 -四氟乙基- 2,2,2 -三氟乙醚(TFTFE)作为稀释剂,提出了一种基于四氢呋喃(THF)电解质中弱分子间相互作用的溶剂化化学调制策略。研究发现,弱分子间相互作用(即偶极子-偶极子相互作用、阴离子-偶极子相互作用)可以有效地减弱Li+-THF在溶剂化结构中的相互作用,促进Li+脱溶动力学,实现99.3%的Li电镀/剥离库仑效率。优化后的电解质可使50 μm-Li || LiFePO4全电池在5.0℃下以115 mAh g-1保持500次循环稳定,即使在-20℃下也能保持95.7%的容量保持。这项工作强调了弱相互作用在微调电解质特性中的重要性,也为开发低温快速充电锂金属电池的兼容电解质铺平了创新途径。
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引用次数: 0
Sequential kinetic control of in-situ polymerization enables a graded solid electrolyte interphase for ultra-stable separator-free solid-state lithium metal batteries 原位聚合的顺序动力学控制实现了超稳定无分离器固态锂金属电池的梯度固体电解质界面
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.nanoen.2026.111743
Meng Wang, Huangxuanyu Yang, Yewen Li, Zhaoyuan Ding, Ruiping Liu
Precise regulation of the solid electrolyte interphase (SEI) is paramount yet challenging for developing high-performance solid-state lithium-metal batteries. Herein, we report a stepwise, kinetically controlled in-situ polymerization strategy that decouples the construction of a mechanical scaffold from the formation of an ion-conducting network within a single, integrated process. This approach begins with rapid UV-curing to form a liquid crystal polymer scaffold, which effectively localizes electrolyte precursors at the electrode interface. This scaffold then guides a subsequent slow cationic polymerization. This spatiotemporal control over the reaction environment is key to forming a robust, inorganic-rich (LiF/Li2CO3) gradient SEI. The obtained separator-free semi-interpenetrating network electrolyte not only achieves desirable bulk properties, including high ionic conductivity (6.22 × 10⁻4 S cm⁻1), a high Li+ transference number (0.81), and a wide electrochemical window (5.1 V vs. Li/Li+), but also, and more critically, achieves substantially improved interfacial stability compared to its thermally polymerized counterpart. The tailored interface enables ultra-stable lithium plating/stripping, evidenced by Li||Li symmetric cells cycling for over 2480 h under low polarization. Furthermore, LiFePO4||Li full cells demonstrate outstanding cycling stability, retaining 97 % of their initial capacity after 340 cycles. This work establishes sequential, photopolymerization-driven kinetic control as a powerful paradigm for designing next-generation solid-state batteries with precisely engineered and highly stable interfaces.
固体电解质间相(SEI)的精确调控对于高性能固态锂金属电池的开发是至关重要的,但也是具有挑战性的。在此,我们报告了一种逐步的、动态控制的原位聚合策略,该策略将机械支架的构建与离子传导网络的形成在一个单一的、集成的过程中解耦。这种方法从快速紫外线固化开始,形成液晶聚合物支架,有效地将电解质前体定位在电极界面。然后,这个支架引导随后的缓慢阳离子聚合。这种对反应环境的时空控制是形成坚固的、无机丰富的(LiF/Li2CO3)梯度SEI的关键。所获得的无分离器半互穿网络电解质不仅具有理想的体积特性,包括高离子电导率(6.22 × 10⁻4 S cm⁻1),高Li+转移数(0.81)和宽电化学窗口(5.1 V vs. Li/Li+),而且更重要的是,与热聚合的电解质相比,界面稳定性大大提高。量身定制的界面实现了超稳定的锂电镀/剥离,证明了Li||Li对称电池在低极化下循环超过2480小时。此外,LiFePO4||Li充满电池表现出出色的循环稳定性,在340次循环后保持了97%的初始容量。这项工作建立了顺序的、光聚合驱动的动力学控制,作为设计具有精确设计和高度稳定界面的下一代固态电池的有力范例。
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引用次数: 0
High-sulfur-doped cathodes enable efficient chloride conversion in rechargeable Na-Cl2 batteries 高硫掺杂阴极使可充电Na-Cl2电池中的氯离子高效转化
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-20 DOI: 10.1016/j.nanoen.2026.111745
Yiming Sun , Guanzhong Ma , Zihui Liu , Xinru Wei , Chenyu Ma , Wenting Feng , Xinghao Zhang , Han Wang , Xiaowei Zhang , Peiqi Liu , Debin Kong , Linjie Zhi
Rechargeable metal-chlorine (Li/Na-Cl2) batteries are regarded as promising contenders for novel energy storage devices due to their exceptionally high energy density and broad operating temperature range. However, their practical application is severely constrained by the slow conversion and insufficient supply of chlorine species during redox reactions, resulting in short cycle lifetimes when Na-Cl2 batteries undergo repeated charge-discharge cycles at high specific capacities. To achieve Na-Cl2 batteries with high cut-off capacity, we hereby report for the first time the introduction of dual heteroatoms N and S into graphene via rapid Joule heating thermal shock. By leveraging nitrogen's preferential deposition to alter graphene's local electronic effects, we synthesise highly S-doped graphene materials. This doping induces charge redistribution on the carbon surface. This enables the doped S to fully exhibit its high catalytic activity, achieving efficient conversion of Cl2 to NaCl. Consequently, the secondary Na-Cl2 battery utilising high S-rGO demonstrates significantly enhanced output capacity, achieving a discharge capacity of 3000 mAh g−1 at 1.5 A g−1. This study demonstrates the efficacy of heteroatom engineering in modulating C/Cl interactions and enhancing the performance of Li/Na-Cl2 batteries.
可充电金属-氯(Li/Na-Cl2)电池因其超高的能量密度和较宽的工作温度范围而被认为是新型储能装置的有力竞争者。然而,由于Na-Cl2电池在高比容量下反复充放电循环,其实际应用受到氧化还原反应过程中转换缓慢和氯气供应不足的严重制约。为了实现具有高截止容量的Na-Cl2电池,我们在此首次报道通过快速焦耳加热热冲击将双杂原子N和S引入石墨烯。通过利用氮的优先沉积来改变石墨烯的局部电子效应,我们合成了高s掺杂的石墨烯材料。这种掺杂引起碳表面的电荷重新分布。这使得掺杂的S充分发挥了其高催化活性,实现了Cl2到NaCl的高效转化。因此,利用高S-rGO的二次Na-Cl2电池显示出显着增强的输出容量,在1.5 a g−1下实现3000 mAh g−1的放电容量。本研究证明了杂原子工程在调节C/Cl相互作用和提高Li/Na-Cl2电池性能方面的有效性。
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引用次数: 0
Low-power and non-volatile multi-level synaptic weight update characteristics in self-selecting Nb2O5/CeO2 memristor crossbar array for in-memory computing system 内存计算系统中自选Nb2O5/CeO2忆阻交叉栅阵列的低功耗、非易失性多层次突触权更新特性
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111739
Kitae Park , Hanju Ko , Peter Hayoung Chung , Jiyeon Ryu , Sola Moon , Tae-Sik Yoon
Non-filamentary valence change memory (VCM)-type memristors are considered the promising candidates as artificial synapses for in-memory computing systems to achieve high energy-efficient computing due to their analog or multi-level conductance change for training operations. However, their poor retention properties originating from unintended diffusion of redistributed oxygen ions limit their application only to the training operation, because the inference operation requires non-volatile retention of updated weights. In this study, non-volatile retention with multi-level synaptic weight update characteristics is demonstrated in non-filamentary bi-layered memristor with cerium oxide (CeO2) and niobium oxide (Nb2O5), i.e., Nb2O5/CeO2, where CeO2 acts as switching layer and Nb2O5 serves as an oxygen ion-holding layer. Due to their high oxygen-ion conductivity and active oxygen-ion exchange property, the memristor enables polarity-dependent, linear, and symmetric analog conductance changes as weight updates, while operating stably at low power with a current range of 0.5–500 nA at + 1.5 V or below. Notably, the device exhibits long-term retention of updated weights enabling discrimination of multi-level states via stably holding oxygen ions in Nb2O5 layer. In addition, by employing Nb2O5/CeO2 bi-layered structure, it achieves self-selecting characteristics from asymmetric Schottky contacts at oxide/electrode interfaces as well as high non-linearity ratio in half-bias operation scheme, which minimizes write disturbance and sneak current in selector-free crossbar array architecture. Using the obtained weight update characteristics, pattern recognition accuracy is simulated to be 96.6 % for MNIST handwritten patterns using CrossSim program. These linear, symmetric, and analog non-volatile conductance change with low power consumption as well as self-selecting behaviors of bi-layered Nb2O5/CeO2 memristor crossbar array confirms the potential of the proposed device to be applicable to integrated in-memory computing systems that implement both efficient training and inference operations.
非丝状价变存储器(VCM)型记忆电阻器由于具有模拟或多级电导变化的特性,被认为是内存计算系统中实现高能效计算的人工突触的有希望的候选人。然而,由于再分布氧离子的意外扩散,它们的保留性能很差,这限制了它们仅在训练操作中的应用,因为推理操作需要更新权重的非易失性保留。在本研究中,以氧化铈(CeO2)和氧化铌(Nb2O5)为材料的非丝状双层记忆电阻器,即Nb2O5/CeO2中,CeO2作为开关层,Nb2O5作为氧离子保持层,证明了具有多级突触权更新特性的非挥发性保留。由于其高氧离子电导率和活性氧离子交换特性,该忆阻器可以随着重量的更新实现极性依赖、线性和对称的模拟电导变化,同时在+1.5 V或更低的低功率下稳定工作,电流范围为0.5-500 nA。值得注意的是,该器件通过稳定地保持Nb2O5层中的氧离子,能够长期保留更新的权重,从而能够区分多层次状态。此外,通过采用Nb2O5/CeO2双层结构,实现了氧化物/电极界面不对称肖特基接触的自选择特性和半偏置操作方案的高非线性比,从而最大限度地减少了无选择器交叉棒阵列结构中的写入干扰和潜流。利用得到的权值更新特征,利用CrossSim程序对MNIST手写模式进行模式识别,准确率达到96.6%。这些线性、对称和模拟的非易失性电导变化具有低功耗和自选择行为的双层Nb2O5/CeO2忆阻交叉棒阵列证实了所提出的器件适用于实现高效训练和推理操作的集成内存计算系统的潜力。
{"title":"Low-power and non-volatile multi-level synaptic weight update characteristics in self-selecting Nb2O5/CeO2 memristor crossbar array for in-memory computing system","authors":"Kitae Park ,&nbsp;Hanju Ko ,&nbsp;Peter Hayoung Chung ,&nbsp;Jiyeon Ryu ,&nbsp;Sola Moon ,&nbsp;Tae-Sik Yoon","doi":"10.1016/j.nanoen.2026.111739","DOIUrl":"10.1016/j.nanoen.2026.111739","url":null,"abstract":"<div><div>Non-filamentary valence change memory (VCM)-type memristors are considered the promising candidates as artificial synapses for in-memory computing systems to achieve high energy-efficient computing due to their analog or multi-level conductance change for training operations. However, their poor retention properties originating from unintended diffusion of redistributed oxygen ions limit their application only to the training operation, because the inference operation requires non-volatile retention of updated weights. In this study, non-volatile retention with multi-level synaptic weight update characteristics is demonstrated in non-filamentary bi-layered memristor with cerium oxide (CeO<sub>2</sub>) and niobium oxide (Nb<sub>2</sub>O<sub>5</sub>), i.e., Nb<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub>, where CeO<sub>2</sub> acts as switching layer and Nb<sub>2</sub>O<sub>5</sub> serves as an oxygen ion-holding layer. Due to their high oxygen-ion conductivity and active oxygen-ion exchange property, the memristor enables polarity-dependent, linear, and symmetric analog conductance changes as weight updates, while operating stably at low power with a current range of 0.5–500 nA at + 1.5 V or below. Notably, the device exhibits long-term retention of updated weights enabling discrimination of multi-level states via stably holding oxygen ions in Nb<sub>2</sub>O<sub>5</sub> layer. In addition, by employing Nb<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> bi-layered structure, it achieves self-selecting characteristics from asymmetric Schottky contacts at oxide/electrode interfaces as well as high non-linearity ratio in half-bias operation scheme, which minimizes write disturbance and sneak current in selector-free crossbar array architecture. Using the obtained weight update characteristics, pattern recognition accuracy is simulated to be 96.6 % for MNIST handwritten patterns using CrossSim program. These linear, symmetric, and analog non-volatile conductance change with low power consumption as well as self-selecting behaviors of bi-layered Nb<sub>2</sub>O<sub>5</sub>/CeO<sub>2</sub> memristor crossbar array confirms the potential of the proposed device to be applicable to integrated in-memory computing systems that implement both efficient training and inference operations.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111739"},"PeriodicalIF":17.1,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001568","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interface-engineered mixed-dimensional GaS/GaN heterojunction for low-noise ultraviolet photodetector and imaging 用于低噪声紫外探测器和成像的界面工程混合维GaS/GaN异质结
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111738
Yutian Lin , Wenfeng Li , Siyu Zhou , Zexin Dong , Zhiyuan Zhang , Yuqing Yang , Ying Yu , Ping Liu , Xingfu Wang , Zhihong Zhu
Interface engineering is an effective strategy for enhancing the performance of optoelectronic devices. In this work, we develop a reliable interface modulation approach specifically for III-nitride materials by fabricating low-dark-current GaS/GaN heterojunction ultraviolet (UV) photodetectors (PDs) with controlled polarity and dimensionality, thereby improving both responsivity and detectivity. Compared with Ga-polar devices, the N-polar heterojunction PDs exhibit markedly superior performance: the responsivity increases from 1.13 mA/W to 143 mA/W, the specific detectivity improves from 3.4 × 108 Jones to 6.58 × 1010 Jones, and the linear dynamic range is enhanced from 19 to 50 dB. Simulation results of the two heterojunction interfaces reveal that these performance enhancements arise from a stronger built-in electric field in the N-polar heterojunction, which facilitates more efficient separation of photogenerated electron-hole pairs. Furthermore, we investigate the potential of these devices for low-noise UV optical imaging, enabled by their low dark current and ultra-low NEP. Overall, this work demonstrates an effective strategy for tuning the performance of III-nitride heterojunctions and highlights their strong potential for low-noise UV detection applications.
界面工程是提高光电器件性能的有效策略。在这项工作中,我们通过制造具有可控极性和尺寸的低暗电流GaS/GaN异质结紫外(UV)光电探测器(pd),开发了一种专门针对iii -氮化物材料的可靠界面调制方法,从而提高了响应性和探测性。与ga极性器件相比,n极性异质结器件表现出明显的性能优势:响应度从1.13 mA/W提高到143 mA/W,比探测率从3.4 × 108 Jones提高到6.58 × 1010 Jones,线性动态范围从19提高到50 dB。两个异质结界面的仿真结果表明,这些性能的增强是由于n极异质结中更强的内置电场,这有助于更有效地分离光生电子-空穴对。此外,我们还研究了这些器件在低噪声紫外光学成像方面的潜力,这些器件具有低暗电流和超低NEP。总的来说,这项工作展示了一种有效的策略来调整iii -氮化物异质结的性能,并突出了它们在低噪声紫外检测应用中的强大潜力。
{"title":"Interface-engineered mixed-dimensional GaS/GaN heterojunction for low-noise ultraviolet photodetector and imaging","authors":"Yutian Lin ,&nbsp;Wenfeng Li ,&nbsp;Siyu Zhou ,&nbsp;Zexin Dong ,&nbsp;Zhiyuan Zhang ,&nbsp;Yuqing Yang ,&nbsp;Ying Yu ,&nbsp;Ping Liu ,&nbsp;Xingfu Wang ,&nbsp;Zhihong Zhu","doi":"10.1016/j.nanoen.2026.111738","DOIUrl":"10.1016/j.nanoen.2026.111738","url":null,"abstract":"<div><div>Interface engineering is an effective strategy for enhancing the performance of optoelectronic devices. In this work, we develop a reliable interface modulation approach specifically for III-nitride materials by fabricating low-dark-current GaS/GaN heterojunction ultraviolet (UV) photodetectors (PDs) with controlled polarity and dimensionality, thereby improving both responsivity and detectivity. Compared with Ga-polar devices, the N-polar heterojunction PDs exhibit markedly superior performance: the responsivity increases from 1.13 mA/W to 143 mA/W, the specific detectivity improves from 3.4 × 10<sup>8</sup> Jones to 6.58 × 10<sup>10</sup> Jones, and the linear dynamic range is enhanced from 19 to 50 dB. Simulation results of the two heterojunction interfaces reveal that these performance enhancements arise from a stronger built-in electric field in the N-polar heterojunction, which facilitates more efficient separation of photogenerated electron-hole pairs. Furthermore, we investigate the potential of these devices for low-noise UV optical imaging, enabled by their low dark current and ultra-low NEP. Overall, this work demonstrates an effective strategy for tuning the performance of III-nitride heterojunctions and highlights their strong potential for low-noise UV detection applications.</div></div>","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"149 ","pages":"Article 111738"},"PeriodicalIF":17.1,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001582","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing the stability of lattice oxygen and thermotolerance in LiNi0.83Co0.12Mn0.05O2 cathodes through surface-to-bulk modulation for superior electrochemical performance 通过表面-体调制提高LiNi0.83Co0.12Mn0.05O2阴极的晶格氧稳定性和耐热性,获得优异的电化学性能
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111742
Hangyu Zhang , Yanxue Wu , Xijun Xu , Fangkun Li , Yongxin Kuang , Zheng Li , Yizhong Guo , Jingwei Zhao , Zhiyuan Zeng , Jun Liu , Yanping Huo
LiNixCoyMn1−x−yO2 (x > 0.8) are the most promising cathodes for lithium-ion batteries (LIBs) due to their high energy density. However, its practical applications are significantly hindered by an unstable cathode-electrolyte interface (CEI) and the oxidation of lattice oxygen under high voltage and elevated temperature conditions. Herein, a dual-function collaborative strategy integrating Li5GaO4 (LGO) coating with Ga doping is implemented for LiNi0.83Co0.12Mn0.05O2 (G-NCM83). Due to the synergistic effect of surface-to-bulk engineering, this G-NCM83 achieves an impressive capacity retention rate of 88.9 % after 400 cycles at 1 C and attains 179.8 mAh g−1 after 200 cycles at 1 C under 60 ℃. The coated LGO layer can avoid the side reaction between G-NCM83 and the electrolyte, thus resulting in a stable CEI. Furthermore, multiscale characterizations verified that this dual-function collaborative strategy greatly stabilizes lattice oxygen and impedes Li/Ni cation mixing of G-NCM83, thus enhancing thermal shock tolerance from 25 to 500 °C. Density functional theory (DFT) calculation further validates that this modified G-NCM83 endows rapid Li+/electron transfer, mitigates HF erosion, and increases the formation energy of oxygen vacancies. This strategy integrates surface engineering and lattice modulation to reinforce lattice oxygen stability and suppress irreversible layered-spinel-rocksalt phase transitions, thereby enhancing the Thermotolerance of LiNi0.83Co0.12Mn0.05O2.
LiNixCoyMn1−x−yO2 (x >; 0.8)由于其高能量密度而成为锂离子电池(LIBs)最有前途的阴极。然而,阴极-电解质界面(CEI)的不稳定以及晶格氧在高压和高温条件下的氧化严重阻碍了其实际应用。在此基础上,对LiNi0.83Co0.12Mn0.05O2 (G-NCM83)材料实现了Li5GaO4 (LGO)涂层与Ga掺杂的双功能协同策略。由于表面-体工程的协同效应,该g - ncm83在1 ℃下循环400次后的容量保持率达到88.9 %,在1 ℃下60℃下循环200次后的容量保持率达到179.8 mAh g−1。涂覆的LGO层可以避免G-NCM83与电解质之间的副反应,从而获得稳定的CEI。此外,多尺度表征证实,这种双功能协同策略极大地稳定了晶格氧,阻碍了G-NCM83的Li/Ni阳离子混合,从而提高了25至500°C的热冲击耐冲击性。密度泛函理论(DFT)进一步验证了改性后的G-NCM83具有快速的Li+/电子转移,减轻HF侵蚀,提高氧空位的形成能。该策略将表面工程和晶格调制相结合,增强了晶格氧稳定性,抑制了不可逆层状尖晶石-岩盐相变,从而提高了LiNi0.83Co0.12Mn0.05O2的耐热性。
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引用次数: 0
Isopropylammonium doping enhances efficiency and stability of triple-cation perovskite solar cells via effective intrinsic lattice modulation 异丙铵掺杂通过有效的本征晶格调制提高三阳离子钙钛矿太阳能电池的效率和稳定性
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111740
Xiang Li , Zhen-Jie Guan , Pan Luo , Xue-yin Sun , Li Yang , Jian-Tang Jiang , Yang Li , Wen-zhu Shao , Liang Zhen
Despite remarkable advances in efficiency, perovskite solar cells (PSCs) still suffer from critical stability issues arising from halide vacancies and ion migration induced by intrinsic lattice defects. Herein, an effective doping strategy to enhance intrinsic stability is introduced. Guided by density functional theory calculations, isopropylammonium (IPA+) is identified and incorporated into the perovskite lattice. IPA doping effectively reduces bulk defects and suppresses non-radiative recombination, while simultaneously disrupting ion migration pathways and inhibiting ion migration. As a result, the IPA-doped device achieves a power conversion efficiency (PCE) of 23.3 % and an open-circuit voltage of 1.214 V, ranking among the highest reported for single-junction PSCs with a bandgap of ∼1.63 eV. Moreover, the doped devices exhibit exceptional stability, retaining over 96 % of their initial PCE after 960 h of dark storage (ISOS-D-1), over 94 % after 288 h of thermal aging at 65 ℃ (ISOS-D-2), about 93 % after 288 h of thermal cycling, and 74 % after 288 h of continuous light soaking (ISOS-L-1). This study highlights the synergy between computational prediction and experimental validation, offering a new compositional design strategy for intrinsically stabilizing perovskite materials.
尽管钙钛矿太阳能电池(PSCs)在效率方面取得了显著进步,但由于卤化物空位和固有晶格缺陷引起的离子迁移,PSCs的稳定性仍然存在关键问题。本文介绍了一种有效的增强本征稳定性的掺杂策略。在密度泛函理论计算的指导下,异丙基铵(IPA+)被识别并纳入钙钛矿晶格中。IPA掺杂有效地减少了体缺陷,抑制了非辐射重组,同时破坏了离子迁移途径,抑制了离子迁移。因此,ipa掺杂器件的功率转换效率(PCE)为23.3% %,开路电压为1.214 V,是目前报道的带隙为1.63 eV的单结PSCs中最高的。此外,掺杂器件表现出优异的稳定性,在960 h的暗储存(iso - d -1)后,其初始PCE保持在96 %以上,在65℃热老化288 h后保持在94 %以上(iso - d -2),在288 h的热循环后保持在93 %左右,在288 h的连续光浸泡(iso - l -1)后保持在74 %以上。本研究强调了计算预测和实验验证之间的协同作用,为钙钛矿材料的本质稳定提供了一种新的成分设计策略。
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引用次数: 0
Corrigendum to “Recent progress of halide perovskites for thermoelectric application” [Nano Energy 94 (2022) 106949] “热电应用卤化物钙钛矿的最新进展”[Nano Energy 94(2022) 106949]的勘误表
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111734
Yingzhi Zhou , Jing Wang , Dongxiang Luo , Dehua Hu , Yonggang Min , Qifan Xue
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引用次数: 0
Potassium-induced trap state passivation for high-efficiency antimony selenide solar cells 高效硒化锑太阳能电池的钾诱导阱态钝化
IF 17.1 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-19 DOI: 10.1016/j.nanoen.2026.111741
Xiaoyang Liang , Qiwei Chang , Liangliang Zhang , Anming Mo , Bingxin Yang , Xinzhou Lu , Ying Wang , Wei Dang , Takhir M. Razykov , Yingnan Guo , Yaohua Mai , Zhiqiang Li
Antimony selenide (Sb2Se3) thin-film solar cells have shown remarkable progress over the past decade, yet their power conversion efficiency (PCE) remains hindered by substantial bulk and interface defects. Herein, we develop a potassium fluoride post-deposition treatment (KF-PDT) strategy to concurrently passivate deep-level defects in the bulk and on the surface of Sb2Se3 thin films. The incorporated potassium introduces shallow acceptor levels, enhancing p-type conductivity and increasing the free carrier density, while effectively suppressing deep-level defect concentrations and associated non-radiative recombination. Moreover, the KF-PDT process modulates surface states-particularly at grain boundaries-thereby improving charge carrier transport and collection. As a result, the KF-PDT-treated Sb2Se3 solar cell achieves a champion efficiency of 10.10 %, corresponding to a 17 % relative improvement over the control device (8.64 %). This study presents a simple but robust approach for mitigating defects in Sb2Se3 photovoltaics, accelerating their development toward commercial viability.
硒化锑(Sb2Se3)薄膜太阳能电池在过去十年中取得了显著的进展,但其功率转换效率(PCE)仍然受到大量体积和界面缺陷的阻碍。在此,我们开发了一种氟化钾沉积后处理(KF-PDT)策略,可以同时钝化Sb2Se3薄膜体和表面的深层缺陷。加入的钾引入了浅受体水平,增强了p型电导率,增加了自由载流子密度,同时有效地抑制了深能级缺陷浓度和相关的非辐射重组。此外,KF-PDT工艺调节了表面状态,特别是在晶界处,从而改善了载流子的传输和收集。结果,kf - pdt处理的Sb2Se3太阳能电池达到了10.10 %的冠军效率,相对于控制装置(8.64 %)提高了17 %。本研究提出了一种简单但强大的方法来减轻Sb2Se3光伏电池的缺陷,加速其商业可行性的发展。
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Nano Energy
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