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Designing mesostructured iron (II) fluorides with a stable in situ polymer electrolyte interface for high-energy-density lithium-ion batteries 为高能量密度锂离子电池设计具有稳定原位聚合物电解质界面的介结构铁 (II) 氟化物
Q1 ELECTROCHEMISTRY Pub Date : 2024-02-01 DOI: 10.1016/j.esci.2023.100188
Lidong Sun , Yong Wang , Lingchen Kong , Shaoshan Chen , Cong Peng , Jiahui Zheng , Yu Li , Wei Feng

As high-energy cathode materials, conversion-type metal fluorides provide a prospective pathway for developing next-generation lithium-ion batteries. However, they suffer from severe performance decay owing to continuous structural destruction and active material dissolution upon cycling, which worsen at elevated temperatures. Here, we design a novel FeF2 cathode with in situ polymerized solid-state electrolyte systems to enhance the cycling ability of metal fluorides at 60 ​°C. Novel FeF2 with a mesoporous structure (meso-FeF2) improves Li+ diffusion and relieves the volume change that typically occurs during the alternating conversion reactions. The structural stability of the meso-FeF2 cathode is strengthened by an in situ polymerized solid-state electrolyte, which prevents the pulverization and ion dissolution that are inevitable for conventional liquid electrolytes. Under the double action of this in situ polymerized solid-state electrolyte and the meso-FeF2's mesoporous structure, the active material maintains an intact SEI layer and part of the mesoporous structure after long charge–discharge cycling, showing excellent cycling stability at high temperatures.

作为高能正极材料,转换型金属氟化物为开发下一代锂离子电池提供了一条前景广阔的途径。然而,由于在循环过程中结构持续破坏和活性材料溶解,它们的性能衰减严重,在温度升高时情况更加恶化。在此,我们设计了一种新型 FeF2 阴极,并采用原位聚合固态电解质系统,以增强金属氟化物在 60 °C 下的循环能力。具有介孔结构(meso-FeF2)的新型 FeF2 改善了 Li+ 的扩散,缓解了通常在交替转换反应中发生的体积变化。原位聚合固态电解质增强了介孔 FeF2 阴极的结构稳定性,防止了传统液态电解质不可避免的粉碎和离子溶解现象。在这种原位聚合固态电解质和介质 FeF2 的介孔结构的双重作用下,活性材料在长时间充放电循环后仍能保持完整的 SEI 层和部分介孔结构,在高温下表现出优异的循环稳定性。
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引用次数: 0
Neighboring effect in single-atom catalysts for the electrochemical carbon dioxide reduction reaction 电化学二氧化碳还原反应中单原子催化剂的邻近效应
Q1 ELECTROCHEMISTRY Pub Date : 2024-02-01 DOI: 10.1016/j.esci.2023.100140
Hon Ho Wong , Mingzi Sun , Tong Wu , Cheuk Hei Chan , Lu Lu , Qiuyang Lu , Baian Chen , Bolong Huang

Although single-atom catalysts (SACs) have attracted enormous attention for their applications in the electrochemical reduction of CO2 (CO2RR) due to their extraordinary catalytic activity and well-defined active centers, neighboring effects and their influence on the electrochemical performance of SACs have not been well investigated. In this review, we present a summary of the neighboring effects on SACs for the CO2RR process, where the surrounding atoms not only induce electronic modulation of the metal atom but also participate in the CO2RR. Both theoretical and experimental studies have pointed out that the neighboring sites of the anchored metal center can provide second active/adsorption locations during the catalytic process, enhancing CO2RR performance tremendously. This review supplies advanced insights into the significant roles and impacts of neighboring effects on the catalytic process, which also benefit the development of advanced SACs to achieve efficient electrocatalysis.

尽管单原子催化剂(SACs)因其非凡的催化活性和明确的活性中心在二氧化碳电化学还原(CO2RR)中的应用而备受关注,但邻近效应及其对 SACs 电化学性能的影响尚未得到很好的研究。在本综述中,我们总结了在 CO2RR 过程中 SAC 的邻近效应,在 CO2RR 过程中,周围的原子不仅会引起金属原子的电子调制,而且还会参与 CO2RR。理论和实验研究都指出,在催化过程中,锚定金属中心的邻位可以提供第二活性/吸附位置,从而大大提高 CO2RR 的性能。本综述提供了关于邻位效应在催化过程中的重要作用和影响的先进见解,这也有利于开发先进的 SACs 以实现高效电催化。
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引用次数: 0
Managing the lifecycle of perovskite solar cells: Addressing stability and environmental concerns from utilization to end-of-life 管理过氧化物太阳能电池的生命周期:解决从使用到报废的稳定性和环境问题
Q1 ELECTROCHEMISTRY Pub Date : 2024-01-25 DOI: 10.1016/j.esci.2024.100243
Hee Jung Kim , Gill Sang Han , Hyun Suk Jung

Perovskite solar cells (PSCs) have shown remarkable advancements and achieved impressive power conversion efficiencies since their initial introduction in 2012. However, challenges regarding stability, quality, and sustainability must be addressed for their successful commercial use. This review analyses the recent studies and challenges related to the operating life and end-of-life utilization of PSCs. Strategies to enhance the stability and mitigate the toxic Pb leakage in operational and recycling approaches of discarded PSCs post their end-of-life are examined to establish a viable and sustainable PSC industry. Additionally, future research directions are proposed for the advancements in the PSC industry. The goal is to ensure high efficiency as well as economic and environmental sustainability throughout the lifecycle of PSCs.

自 2012 年首次问世以来,过氧化物太阳能电池(PSC)取得了显著的进步,并实现了令人印象深刻的功率转换效率。然而,要想成功实现商业应用,必须解决稳定性、质量和可持续性方面的挑战。本综述分析了有关 PSC 运行寿命和报废利用的最新研究和挑战。研究了在使用中提高稳定性和减少有毒铅泄漏的策略,以及报废后废弃 PSC 的回收方法,以建立一个可行且可持续发展的 PSC 产业。此外,还提出了未来的研究方向,以推动 PSC 产业的发展。目标是确保高效率以及在整个 PSC 生命周期内的经济和环境可持续性。
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引用次数: 0
Playdough-like carbon electrode: A promising strategy for high efficiency perovskite solar cells and modules 橡皮泥状碳电极:高效率过氧化物太阳能电池和模块的可行策略
Q1 ELECTROCHEMISTRY Pub Date : 2023-12-10 DOI: 10.1016/j.esci.2023.100221
Aodong Zhu , Lin Chen , Ao Zhang , Chenpu Zhu , Xinxin Zhang , Jie Zhong , Fuzhi Huang , Yi-Bing Cheng , Junyan Xiao

Carbon-based perovskite solar cells (C-PSCs) are promising candidates for large-scale photovoltaic applications due to their theoretical low cost and high stability. However, the fabrication of high-performance C-PSCs with large-area electrodes remains challenging. In this work, we propose a novel playdough-like graphite putty as top electrode in the perovskite devices. This electrode with soft nature can form good contact with the hole-transporting layer and the conductive substrate at room temperature by a simple pressing technique, which facilitates the fabrication of both small-area devices and perovskite solar modules. In this preliminary research, the corresponding small devices and modules can achieve efficiencies of 20.29% (∼0.15 ​cm2) and 16.01% (∼10 ​cm2), respectively. Moreover, we analyze the limitations of the optical and electrical properties of this playdough-like graphite electrode on the device performance, suggesting a direction for further improvement of C-PSCs in the future.

碳基过氧化物太阳能电池(C-PSCs)理论上成本低、稳定性高,是大规模光伏应用的理想候选材料。然而,制造具有大面积电极的高性能 C-PSC 仍然具有挑战性。在这项工作中,我们提出了一种新型的橡皮泥状石墨腻子作为过氧化物器件的顶部电极。这种电极具有柔软的特性,通过简单的压制技术就能在室温下与空穴传输层和导电基板形成良好的接触,从而方便了小面积器件和过氧化物太阳能模块的制造。在这项初步研究中,相应的小型器件和模块的效率分别达到了 20.29% (∼0.15 cm2) 和 16.01% (∼10 cm2)。此外,我们还分析了这种橡皮泥状石墨电极的光学和电学特性对器件性能的限制,为今后进一步改进 C-PSC 指明了方向。
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引用次数: 0
Photoelectric-driven conductive composite ionogel patch for effective wound healing 用于伤口有效愈合的光电驱动导电复合离子凝胶贴片
Q1 ELECTROCHEMISTRY Pub Date : 2023-12-10 DOI: 10.1016/j.esci.2023.100223
Xingkai Ju , Jiao Kong , Guohua Qi , Shuping Hou , Bo Wang , Xingkang Diao , Shaojun Dong , Yongdong Jin

Developing the high biosafety, effective and wearable devices for fast wound healing is highly desired but remains a challenge. Here, we propose a “win–win co-operation” strategy to potentiate effective skin wound healing at the wound site by constructing robust and ecofriendly composite patch under opto-electric stimulation. The wearable patch is composed of ionic gel doped with Ti3C2Tx (MXene), which possesses good photothermal response to kill the bacteria via effective inhibition of the expression of inflammatory factors, preventing wound infection. Importantly, the composite ionogel patch is capable of providing green and on-demand electrical stimulation for wound site, guiding cell migration and proliferation by improved bioenergy and expression up-regulation of growth factor. In mice wound models, the treatment group healed ∼31% more rapidly. Mechanistically, the wearable devices could enable visual and real-time supervising treatment effect due to their good transmittance. The proposed strategy would be promising for future clinical treatment of wound healing.

开发生物安全性高、有效且可穿戴的快速伤口愈合设备是人们的殷切期望,但仍是一项挑战。在此,我们提出了一种 "双赢合作 "策略,通过构建光电刺激下的坚固且环保的复合贴片,促进伤口部位皮肤伤口的有效愈合。该可穿戴贴片由掺杂 Ti3C2Tx(MXene)的离子凝胶组成,具有良好的光热反应,可通过有效抑制炎症因子的表达来杀灭细菌,防止伤口感染。重要的是,复合离子凝胶贴片能够为伤口部位提供绿色、按需的电刺激,通过改善生物能和上调生长因子的表达来引导细胞迁移和增殖。在小鼠伤口模型中,治疗组的愈合速度提高了 31%。从机理上讲,由于可穿戴设备具有良好的透光性,因此可以直观、实时地监督治疗效果。所提出的策略在未来的伤口愈合临床治疗中将大有可为。
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引用次数: 0
Phase engineering of Pd–Te nanoplates via potential energy trapping 通过势能捕获实现 Pd-Te 纳米板的相工程
Q1 ELECTROCHEMISTRY Pub Date : 2023-11-08 DOI: 10.1016/j.esci.2023.100209
Mengjun Wang , Jun Jia , Hao Yan , Guang Li , Qiming Hong , Yuzheng Guo , Yong Xu , Xiaoqing Huang

Phase modulation of noble metal alloys (NMAs) is critically important in nanoscience since the distinct atomic arrangements can largely determine their physicochemical properties. However, the precise modulation of NMAs is formidably challenging, because thermodynamically stable phases are generally preferential compared to those metastable ones. Herein, we proposed a potential energy trapping strategy for phase modulation of Pd–Te alloys with solvents. Thereinto, ethylene glycol can increase the energy barrier for both Pd leaching and Te introduction, forming metastable Pd20Te7 phase. Inversely, N, N-dimethylformamide is unable to trap metastable phase, inducing the phase evolution to thermodynamically stable PdTe phase, and the precise phase modulation was realized including Pd20Te7, PdTe and PdTe2 phases. The Pd–Te alloys displayed phase-dependent formic acid oxidation catalytic performance with PdTe phase showing the best. This work proposes a strategy for creating metastable phase with potential energy trap, which may deepen the understanding of phase engineering for noble metal-based nanocrystals.

贵金属合金(NMAs)的相调制在纳米科学中至关重要,因为不同的原子排列在很大程度上决定了它们的物理化学特性。然而,由于热力学上稳定的相通常优于可稳定的相,因此对 NMAs 进行精确调制极具挑战性。在此,我们提出了一种利用溶剂对钯碲合金进行相调节的潜在能量捕获策略。其中,乙二醇可增加钯浸出和碲引入的能垒,形成铂碲合金的 "陨落 "相 Pd20Te7。相反,N, N-二甲基甲酰胺无法捕获逸散相,从而诱导相演化为热力学稳定的 PdTe 相,并实现了包括 Pd20Te7、PdTe 和 PdTe2 相在内的精确相调制。Pd-Te 合金显示出与相有关的甲酸氧化催化性能,其中 PdTe 相的性能最佳。这项工作提出了一种利用势能陷阱创建可转移相的策略,可加深对贵金属基纳米晶体相工程的理解。
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引用次数: 0
A plasmonic S-scheme Au/MIL-101(Fe)/BiOBr photocatalyst for efficient synchronous decontamination of Cr(VI) and norfloxacin antibiotic 用于高效同步净化六价铬和诺氟沙星抗生素的等离子体 S 型 Au/MIL-101(Fe)/BiOBr 光催化剂
Q1 ELECTROCHEMISTRY Pub Date : 2023-11-02 DOI: 10.1016/j.esci.2023.100208
Shijie Li , Kexin Dong , Mingjie Cai , Xinyu Li , Xiaobo Chen

Present photocatalysts for the synchronous cleanup of pharmaceuticals and heavy metals have several drawbacks, including inadequate reactive sites, inefficient electron–hole disassociation, and insufficient oxidation and reduction power. In this research, we sought to address these issues by using a facile solvothermal-photoreduction route to develop an innovative plasmonic S-scheme heterojunction, Au/MIL-101(Fe)/BiOBr. The screened-out Au/MIL-101(Fe)/BiOBr (AMB-2) works in a durable and high-performance manner for both Cr(VI) and norfloxacin (NOR) eradication under visible light, manifesting up to 53.3 and 2 times greater Cr(VI) and NOR abatement rates, respectively, than BiOBr. Remarkably, AMB-2's ability to remove Cr(VI) in a Cr(VI)-NOR co-existence system is appreciably better than in a sole-Cr(VI) environment; the synergy among Cr(VI), NOR, and AMB-2 results in the better utilization of photo-induced carriers, yielding a desirable capacity for decontaminating Cr(VI) and NOR synchronously. The integration of MOF-based S-scheme heterojunctions and a plasmonic effect contributes to markedly reinforced photocatalytic ability by increasing the number of active sites, augmenting the visible-light absorbance, boosting the efficient disassociation and redistribution of powerful photo-carriers, and elevating the generation of reactive substances. We provide details of the photocatalytic mechanism, NOR decomposition process, and bio-toxicity of the intermediates. This synergistic strategy of modifying S-scheme heterojunctions with a noble metal opens new horizons for devising excellent MOF-based photosystems with a plasmonic effect for environment purification.

目前用于同步净化药物和重金属的光催化剂存在几个缺点,包括反应位点不足、电子-空穴解离效率低以及氧化和还原能力不足。在这项研究中,我们试图利用一种简便的溶热-光诱导路线来开发一种创新的等离子体 S 型异质结 Au/MIL-101(Fe)/BiOBr,从而解决这些问题。筛选出的金/MIL-101(Fe)/BiOBr(AMB-2)可在可见光下持久、高效地消除六价铬和诺氟沙星(NOR),其六价铬和 NOR 的消除率分别是 BiOBr 的 53.3 倍和 2 倍。值得注意的是,AMB-2 在六价铬-NOR 共存系统中去除六价铬的能力明显优于在单一六价铬环境中;六价铬、NOR 和 AMB-2 之间的协同作用使光诱导载体得到了更好的利用,从而产生了同步去除六价铬和 NOR 的理想能力。基于 MOF 的 S 型异质结与等离子体效应相结合,增加了活性位点的数量,提高了可见光吸收率,促进了强力光载体的有效解离和再分配,并提高了反应物质的生成,从而显著增强了光催化能力。我们详细介绍了光催化机理、NOR 分解过程以及中间产物的生物毒性。这种用贵金属修饰 S 型异质结的协同策略为设计出具有质子效应、用于环境净化的卓越 MOF 基光电系统开辟了新天地。
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引用次数: 0
Molecular engineering of self-assembled monolayers for highly utilized Zn anodes 用于高利用率锌阳极的自组装单层分子工程学
Q1 ELECTROCHEMISTRY Pub Date : 2023-10-19 DOI: 10.1016/j.esci.2023.100205
Lei Zhang , Jin Xiao , Xilin Xiao , Wenli Xin , Yaheng Geng , Zichao Yan , Zhiqiang Zhu

Stabilizing the Zn anode under high utilization rates is highly applauded yet very challenging in aqueous Zn batteries. Here, we rationally design a zincophilic short-chain aromatic molecule, 4-mercaptopyridine (4Mpy), to construct self-assembled monolayers (SAMs) on a copper substrate to achieve highly utilized Zn anodes. We reveal that 4Mpy could be firmly bound on the Cu substrate via Cu–S bond to form compact and uniform SAMs, which could effectively isolate the water on the electrode surface and thus eliminate the water-related side reactions. In addition, the short-chain aromatic ring structure of 4Mpy could not only ensure the ordered arrangement of zincophilic pyridine N but also facilitate charge transfer, thus enabling uniform and rapid Zn deposition. Consequently, the Zn/4Mpy/Cu electrode not only enables the symmetric cell to stably cycle for over 180 ​h at 10 ​mA ​cm−2 under a high depth-of-discharge of 90%, but also allows the MnO2-paired pouch cell to survive for 100 cycles under a high Zn utilization rate of 78.8%. An anode-free 4Mpy/Cu||graphite cell also operates for 150 cycles without obvious capacity fading at 0.1 ​A ​g−1. This control of interfacial chemistry via SAMs to achieve high utilization rates of metal anodes provides a new paradigm for developing high-energy metal-based batteries.

在高利用率下稳定锌阳极备受赞誉,但在水性锌电池中却极具挑战性。在这里,我们合理地设计了一种亲锌短链芳香族分子--4-巯基吡啶(4Mpy),在铜基底上构建自组装单层(SAM),以实现高利用率的锌阳极。我们发现,4Mpy 可通过 Cu-S 键牢固地结合在铜基板上,形成紧凑均匀的 SAM,从而有效隔离电极表面的水,消除与水相关的副反应。此外,4Mpy 的短链芳环结构不仅能确保亲锌吡啶 N 的有序排列,还能促进电荷转移,从而实现均匀、快速的锌沉积。因此,Zn/4Mpy/Cu 电极不仅能使对称电池在 10 mA cm-2 的条件下以 90% 的高放电深度稳定循环超过 180 小时,还能使 MnO2 对袋电池在 78.8% 的高锌利用率下存活 100 个循环。无阳极的 4Mpy/Cu||| 石墨电池也能在 0.1 A g-1 的条件下运行 150 个循环,且无明显的容量衰减。这种通过 SAMs 控制界面化学以实现金属阳极高利用率的方法为开发高能量金属基电池提供了一种新的范例。
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引用次数: 0
Realizing a dendrite-free metallic-potassium anode using reactive prewetting chemistry 利用活性预湿化学实现无树枝状突起的金属钾阳极
Q1 ELECTROCHEMISTRY Pub Date : 2023-10-04 DOI: 10.1016/j.esci.2023.100201
Lu-Kang Zhao , Xuan-Wen Gao , Qinfen Gu , Xiaochen Ge , Zhimin Ding , Zhaomeng Liu , Wen-Bin Luo

Potassium metal batteries (PMBs) have become a paramount alternative energy storage technology to lithium-ion batteries, due to their low cost and potential energy density. However, uncontrolled dendrite growth interferes with the stability of the interfacial anode, leading to significant capacity degradation and safety hazards. Herein, a facile reactive prewetting strategy is proposed to discourage dendrite growth by constructing a functional KF/Zn-rich hybrid interface layer on K metal. The KF/Zn@K anode design functions like an interconnected paddy field, stabilizing the anode interface through the preferential redistribution of K+ flux/electrons, continuous transport paths, and enhanced transport dynamics. As anticipated, symmetrical batteries exhibit an extended cycling lifetime of over 2000 ​h, with reduced voltage hysteresis at 0.5 ​mA ​cm−2 and 0.5 mAh cm−2. Furthermore, when the KF/Zn@K anode is applied to full batteries coupled with PTCDA, a boosted reversible capacity of 61.6 mAh g−1 at 5 ​C is present over 3000 cycles. This interfacial control creates rational possibilities for constructing high-efficiency, stable K metal anodes.

钾金属电池(PMB)因其低成本和潜在的能量密度,已成为锂离子电池的重要替代储能技术。然而,不受控制的枝晶生长会干扰界面阳极的稳定性,导致容量显著下降并带来安全隐患。本文提出了一种简便的反应性预湿策略,通过在 K 金属上构建富含 KF/Zn 的功能性混合界面层来阻止枝晶的生长。KF/Zn@K 阳极设计就像一个相互连接的稻田,通过优先重新分配 K+ 通量/电子、连续传输路径和增强传输动力学来稳定阳极界面。正如预期的那样,对称电池的循环寿命延长了 2000 多小时,在 0.5 mA cm-2 和 0.5 mAh cm-2 时的电压滞后也有所减少。此外,当 KF/Zn@K 阳极与 PTCDA 结合应用于全电池时,在 5 C 条件下,经过 3000 次循环后,可逆容量提高到 61.6 mAh g-1。这种界面控制为构建高效、稳定的 K 金属阳极提供了合理的可能性。
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引用次数: 0
Boosting reversible anionic redox reaction with Li/Cu dual honeycomb centers Li/Cu双蜂窝中心促进可逆阴离子氧化还原反应
Q1 ELECTROCHEMISTRY Pub Date : 2023-10-01 DOI: 10.1016/j.esci.2023.100159
Xiaohui Rong , Dongdong Xiao , Qinghao Li , Yaoshen Niu , Feixiang Ding , Xueyan Hou , Qiyu Wang , Juping Xu , Chenglong Zhao , Dong Zhou , Ruijuan Xiao , Xiqian Yu , Wen Yin , Lin Gu , Hong Li , Xuejie Huang , Liquan Chen , Yong-Sheng Hu

The anionic redox reaction (ARR) is a promising charge contributor to improve the reversible capacity of layered-oxide cathodes for Na-ion batteries; however, some practical bottlenecks still need to be eliminated, including a low capacity retention, large voltage hysteresis, and low rate capability. Herein, we proposed a high-Na content honeycomb-ordered cathode, P2–Na5/6[Li1/6Cu1/6Mn2/3]O2 (P2-NLCMO), with combined cationic/anionic redox. Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry. In addition, advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers, achieving fully active Cu3+/Cu2+ redox and stabilized ARR with interactively suppressed local distortion. With a meticulously regulated charge/discharge protocol, both the cycling and rate capability of P2-NLCMO were significantly improved, demonstrating reasonable capacity and eliminating voltage hysteresis. Overall, this work contributes a well-defined layered oxide cathode with combined cationic/anionic redox towards rational designing advanced Na-ion batteries.

阴离子氧化还原反应(ARR)是提高钠离子电池层状氧化物阴极可逆容量的一种很有前途的电荷贡献者;然而,一些实际的瓶颈仍然需要消除,包括低容量保持率、大电压滞后和低速率能力。在此,我们提出了一种高钠含量的蜂窝状有序阴极,P2–Na5/6[Li1/6Cu1/6Mn2/3]O2(P2-NLCMO),具有阳离子/阴离子复合氧化还原。中子粉末衍射和P2-NLCMO的X射线衍射表明,P2型堆垛具有罕见的P6322对称性。此外,先进的光谱技术和密度泛函理论计算证实了Li/Cu双蜂窝中心之间的协同稳定关系,实现了完全活性的Cu3+/Cu2+氧化还原,并通过相互抑制的局部畸变稳定了ARR。通过精心调节的充电/放电协议,P2-NLCMO的循环能力和倍率能力都得到了显著提高,表现出合理的容量并消除了电压滞后。总的来说,这项工作为合理设计先进的钠离子电池提供了一种具有阳离子/阴离子氧化还原组合的明确的层状氧化物阴极。
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引用次数: 0
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