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Comprehensive Insights on MXene-Based TENGs: from Structures, Functions to Applications. 对基于 MXene 的 TENGs 的全面了解:从结构、功能到应用。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202404872
Shengwu Deng, Wasim Akram, Xiaorui Ye, Lizi Zhang, Yang Yang, Si Cheng, Jian Fang

The rapid advancement of triboelectric nanogenerators (TENGs) has introduced a transformative approach to energy harvesting and self-powered sensing in recent years. Nonetheless, the untapped potential of TENGs in practical scenarios necessitates multiple strategies like material selections and structure designs to enhance their output performance. Given the various superior properties, MXenes, a kind of novel 2D materials, have demonstrated great promise in enhancing TENG functionality. Here, this review comprehensively delineates the advantages of incorporating MXenes into TENGs, majoring in six pivotal aspects. First, an overview of TENGs is provided, stating their theoretical foundations, working modes, material considerations, and prevailing challenges. Additionally, the structural characteristics, fabrication methodologies, and family of MXenes, charting their developmental trajectory are highlighted. The selection of MXenes as various functional layers (negative and positive triboelectric layer, electrode layer) while designing TENGs is briefed. Furthermore, the distinctive advantages of MXene-based TENGs and their applications are emphasized. Last, the existing challenges are highlighted, and the future developing directions of MXene-based TENGs are forecasted.

近年来,三电纳米发电机(TENGs)的快速发展为能量收集和自供电传感带来了一种变革性方法。然而,由于三电纳米发电机在实际应用中的潜力尚未得到充分挖掘,因此有必要采取多种策略(如材料选择和结构设计)来提高其输出性能。MXenes 是一种新型二维材料,具有各种优越性能,因此在增强 TENG 功能方面大有可为。在此,本综述从六个关键方面全面阐述了在 TENG 中加入 MXenes 的优势。首先,综述了 TENG 的理论基础、工作模式、材料考虑因素和主要挑战。此外,还重点介绍了 MXenes 的结构特点、制造方法和家族,并描绘了其发展轨迹。此外,还简要介绍了在设计 TENGs 时选择 MXenes 作为各种功能层(三电负极层和正极层、电极层)的情况。此外,还强调了基于二氧化二烯烃的 TENG 的独特优势及其应用。最后,强调了现有的挑战,并预测了基于 MXene 的 TENGs 的未来发展方向。
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引用次数: 0
Stepwise Curing Induced All-Stretchable Thermoelectric Generator of High Power Density. 逐步固化诱导的高功率密度全拉伸热电发生器。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202406662
Daegun Kim, Myeong-Eun Kim, Hoimin Kim, Jaehoon Lee, Jiyun Lee, Hansol Lee, Dongki Lee, Nae-Eung Lee, Boseok Kang

In this study, a wearable and highly stretchable organic thermoelectric (TE) generator with a notable power density is developed. A highly stretchable and solution-processable TE/electrode pattern is realized by stepwise-curing elastomeric and conducting network. Significant advances in the TE or electrical properties are obtained for these stretchable patterns through post-activation treatment, which creates long-range charge transport pathways without degrading pre-established elastomeric networks. The TE and electrode patterns are solution-processed to a stretchable template, so that all-stretchable TE generator is realized. The fabricated TE generator maintains 90% of its maximum TE power output at 40% stretching stress and shows a stable TE power output after 200 stretching cycles. The TE generator maintains its stretchability in highly densified patterns, as the highly stretchable TE/electrode patterns enable good stretchability with little aid of the stretchable template. So, the TE generator has a high power density of 0.32 nW cm-2 K-2, one of the highest values among stretchable TE generators to date.

本研究开发了一种具有显著功率密度的可穿戴、高拉伸有机热电(TE)发电机。通过逐步固化弹性体和导电网络,实现了一种高度可拉伸和可溶液加工的 TE/电极图案。通过活化后处理,这些可拉伸图案的 TE 或电气性能有了显著提高,在不破坏预先建立的弹性体网络的情况下,建立了长距离电荷传输通道。TE 和电极图案经溶液处理后成为可拉伸模板,从而实现了全拉伸 TE 发生器。制成的 TE 发生器在 40% 的拉伸应力下能保持 90% 的最大 TE 功率输出,并在 200 次拉伸循环后显示出稳定的 TE 功率输出。该 TE 发生器在高密度化模式下仍能保持其拉伸性,因为高拉伸性 TE/电极模式只需拉伸模板的少量辅助就能实现良好的拉伸性。因此,该 TE 发生器的功率密度高达 0.32 nW cm-2 K-2,是迄今为止可拉伸 TE 发生器中功率密度最高的产品之一。
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引用次数: 0
Oxygen Vacancies Regulated S-Scheme Charge Transport Route in BiVO4-OVs/g-C3N4 Heterojunction for Enhanced Photocatalytic Performance. 增强光催化性能的 BiVO4-OVs/g-C3N4 异质结中的氧空位调控 S 型电荷传输路线
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202405551
Kangrui Su, Lingcheng Zheng, Mei Liu, Juan Gao, Zeyu Shi, Changzhao Chen, Yang Li, Jie He, Mao Peng

Oxygen vacancies (OVs) are widely considered as active sites in photocatalytic reactions, yet the crucial role of OVs in S-scheme heterojunction photocatalysts requires deeper understanding. In this work, OVs at hetero-interface regulated S-scheme BiVO4-OVs/g-C3N4 photocatalysts are constructed. The Fermi-level structures of BiVO4 and g-C3N4 lead to a redistribution of charges at the heterojunction interface, inducing an internal electric field at the interface, which tends to promote the recombination of photogenerated carriers at the interface. Importantly, the introduction of OVs induces defect electronic states in the BiVO4 bandgap, creating indirect recombination energy level that serves as crucial intermediator for photogenerated carrier recombination in the S-scheme heterojunction. As a result, the photocatalytic degradation rate on Rhodamine B (RhB) and tetracyclines (TCs) for the optimal sample is 10.7 and 11.8 times higher than the bare one, the photocatalytic hydrogen production rate is also improved to 558 µmol g-1 h-1. This work shows the importance of OVs in heterostructure photocatalysis from both thermodynamic and kinetic aspects and may provide new insight into the rational design of S-scheme photocatalysts.

人们普遍认为氧空位(OVs)是光催化反应中的活性位点,但对于 OVs 在 S 型异质结光催化剂中的关键作用还需要更深入的了解。在这项工作中,我们构建了异质界面上的 OV 调节 S 型 BiVO4-OVs/g-C3N4 光催化剂。BiVO4 和 g-C3N4 的费米级结构导致电荷在异质结界面重新分布,从而在界面上产生内电场,这往往会促进光生载流子在界面上重组。重要的是,OV 的引入诱导了 BiVO4 带隙中的缺陷电子态,产生了间接重组能级,成为 S 型异质结中光生载流子重组的关键中介。因此,最佳样品对罗丹明 B(RhB)和四环素(TCs)的光催化降解率分别是裸样品的 10.7 倍和 11.8 倍,光催化产氢率也提高到 558 µmol g-1 h-1。这项研究从热力学和动力学两方面说明了 OVs 在异质结构光催化中的重要性,为合理设计 S 型光催化剂提供了新的思路。
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引用次数: 0
Exploring Pyrazine-Based Organic Redox Couples for Enhanced Thermoelectric Performance in Wearable Energy Harvesters. 探索吡嗪基有机氧化还原偶联剂,提高可穿戴式能量收集器的热电性能。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202407622
Chia-Yu Lee, Ching-Chieh Hsu, Chia-Hsin Wang, U-Ser Jeng, Shih-Huang Tung, Chi-Chang Hu, Cheng-Liang Liu

Thermoelectric generators (TEGs) based on thermogalvanic cells can convert low-temperature waste heat into electricity. Organic redox couples are well-suited for wearable devices due to their nontoxicity and the potential to enhance the ionic Seebeck coefficient through functional-group modifications.  Pyrazine-based organic redox couples with different functional groups is comparatively analyzed through cyclic voltammetry under varying temperatures. The results reveal substantial differences in entropy changes with temperature and highlight 2,5-pyrazinedicarboxylic acid dihydrate (PDCA) as the optimal candidate. How the functional groups of the pyrazine compounds impact the ionic Seebeck coefficient is examined, by calculating the electrostatic potential based on density functional theory. To evaluate the thermoelectric properties, PDCA is integrated in different concentrations into a double-network hydrogel comprising poly(vinyl alcohol) and polyacrylamide. The resulting champion device exhibits an impressive ionic Seebeck coefficient (Si) of 2.99 mV K-1, with ionic and thermal conductivities of ≈67.6 µS cm-1 and ≈0.49 W m-1 K-1, respectively. Finally, a TEG is constructed by connecting 36 pieces of 20 × 10-3 m PDCA-soaked hydrogel in series. It achieves a maximum power output of ≈0.28 µW under a temperature gradient of 28.3 °C and can power a small light-emitting diode. These findings highlight the significant potential of TEGs for wearable devices.

基于热电解质电池的热发电机(TEG)可以将低温废热转化为电能。有机氧化还原偶具有无毒性以及通过官能团修饰提高离子塞贝克系数的潜力,因此非常适合用于可穿戴设备。 我们在不同温度下通过循环伏安法对具有不同官能团的吡嗪基有机氧化还原偶进行了比较分析。结果显示,熵的变化随温度的变化存在很大差异,并突出显示 2,5-吡嗪二羧酸二水合物(PDCA)是最佳候选物质。通过基于密度泛函理论计算静电势,研究了吡嗪化合物的官能团如何影响离子塞贝克系数。为了评估热电特性,将不同浓度的 PDCA 整合到由聚(乙烯醇)和聚丙烯酰胺组成的双网水凝胶中。由此产生的冠军装置表现出令人印象深刻的离子塞贝克系数(Si),为 2.99 mV K-1,离子导电率和导热率分别为 ≈67.6 µS cm-1 和 ≈0.49 W m-1 K-1。最后,通过串联 36 块 20 × 10-3 m PDCA 浸透水凝胶,构建了一个 TEG。在 28.3 °C 的温度梯度下,它的最大功率输出≈0.28 µW,可为一个小型发光二极管供电。这些发现凸显了 TEG 在可穿戴设备方面的巨大潜力。
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引用次数: 0
Elucidating siRNA Cellular Delivery Mechanism Mediated by Quaternized Starch Nanoparticles. 阐明季铵化淀粉纳米颗粒介导的 siRNA 细胞递送机制
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202405524
Eliz Amar-Lewis, Limor Cohen, Ramesh Chintakunta, Chen Benafsha, Yael Lavi, Riki Goldbart, Tamar Traitel, Levi A Gheber, Joseph Kost

Starch-based nanoparticles are highly utilized in the realm of drug delivery taking advantage of their biocompatibility and biodegradability. Studies have utilized Quaternized starch (Q-starch) for small interfering RNA (siRNA) delivery, in which quaternary amines enable interaction with negatively charged siRNA, resulting in self-assembly complexation. Although reports present numerous applications, the demonstrated efficacy is nonetheless limited due to undiscovered cellular mechanistic delivery. In this study, a deep dive into Q-starch/siRNA complexes' cellular mechanism and kinetics at the cellular level is revealed using single-particle tracking and cell population level using imaging flow cytometry. Uptake studies depict the efficient cellular internalization via endocytosis while a significant fraction of complexes' intracellular fate is lysosome. Utilizing single-particle tracking, it is found that an average of 15% of cellular detected complexes escape the endosome which holds the potential for the integration in the cytoplasmatic gene silencing mechanism. Additional experimental manipulations (overcoming endosomal escape) demonstrate that the complex's disassembly is the rate-limiting step, correlating Q-starch's structure-function properties as siRNA carrier. Structure-function properties accentuating the high affinity of the interaction between Q-starch's quaternary groups and siRNA's phosphate groups that results in low release efficiency. However, low-frequency ultrasound (20 kHz) application may have induced siRNA release resulting in faster gene silencing kinetics.

淀粉基纳米粒子具有生物相容性和生物可降解性,因此在给药领域得到了广泛应用。研究利用季铵盐化淀粉(Q-starch)来递送小干扰 RNA(siRNA),季胺能与带负电荷的 siRNA 相互作用,从而产生自组装复合物。虽然报告中介绍了许多应用,但由于细胞递送机制尚未被发现,因此所展示的功效有限。在本研究中,我们利用单颗粒追踪技术和成像流式细胞术,深入研究了 Q 淀粉/siRNA 复合物在细胞水平上的细胞机制和动力学。吸收研究表明,Q-淀粉/siRNA 复合物可通过内吞作用高效内化细胞,而复合物在细胞内的命运有很大一部分是溶酶体。利用单颗粒追踪技术,研究发现平均有 15%的细胞检测到的复合物逃逸出内质体,这为整合到细胞质基因沉默机制中提供了可能。其他实验操作(克服内质体逃逸)表明,复合物的分解是限制速度的一步,这与 Q 淀粉作为 siRNA 载体的结构功能特性相关。结构-功能特性表明,Q-淀粉的季铵盐基团与 siRNA 的磷酸基团之间的高亲和力相互作用导致释放效率较低。然而,低频超声(20 千赫)的应用可能会诱导 siRNA 的释放,从而加快基因沉默的动力学过程。
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引用次数: 0
Corrigendum to "Plasma-Engineering of Oxygen Vacancies on NiCo2O4 Nanowires with Enhanced Bifunctional Electrocatalytic Performance for Rechargeable Zinc-Air Battery". 镍钴氧化物纳米线上的氧空位等离子工程增强了可充电锌-空气电池的双功能电催化性能》的更正。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202404107
He Li, Jihao Wang, Tim Tjardts, Igor Barg, Haoyi Qiu, Martin Müller, Jan Krahmer, Sadegh Askari, Salih Veziroglu, Cenk Aktas, Lorenz Kienle, Jan Benedikt
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引用次数: 0
Closed-Loop Recycling of Wearable Electronic Textiles. 可穿戴电子纺织品的闭环回收。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202407207
Marzia Dulal, Shaila Afroj, Md Rashedul Islam, Minglonghai Zhang, Yadie Yang, Hong Hu, Kostya S Novoselov, Nazmul Karim

Wearable electronic textiles (e-textiles) are transforming personalized healthcare through innovative applications. However, integrating electronics into textiles for e-textile manufacturing exacerbates the rapidly growing issues of electronic waste (e-waste) and textile recycling due to the complicated recycling and disposal processes needed for mixed materials, including textile fibers, electronic materials, and components. Here, first closed-loop recycling for wearable e-textiles is reported by incorporating the thermal-pyrolysis of graphene-based e-textiles to convert them into graphene-like electrically conductive recycled powders. A scalable pad-dry coating technique is then used to reproduce graphene-based wearable e-textiles and demonstrate their potential healthcare applications as wearable electrodes for capturing electrocardiogram (ECG) signals and temperature sensors. Additionally, recycled graphene-based textile supercapacitor highlights their potential as sustainable energy storage devices, maintaining notable durability and retaining ≈94% capacitance after 1000 cycles with an areal capacitance of 4.92 mF cm⁻2. Such sustainable closed-loop recycling of e-textiles showcases the potential for their repurposing into multifunctional applications, promoting a circular approach that potentially prevents negative environmental impact and reduces landfill disposal.

可穿戴电子纺织品(电子纺织品)正在通过创新应用改变个性化医疗保健。然而,由于混合材料(包括纺织纤维、电子材料和组件)需要复杂的回收和处理过程,将电子元件集成到纺织品中以制造电子纺织品加剧了快速增长的电子废物(电子垃圾)和纺织品回收问题。本文首次报道了可穿戴电子纺织品的闭环回收利用,通过对石墨烯基电子纺织品进行热解,将其转化为类似石墨烯的导电回收粉末。然后,利用可扩展的垫干涂层技术复制了石墨烯基可穿戴电子纺织品,并展示了其作为可穿戴电极捕捉心电图(ECG)信号和温度传感器的潜在医疗应用。此外,回收的石墨烯基纺织品超级电容器突显了其作为可持续储能设备的潜力,在 1000 次循环后仍能保持显著的耐用性和≈94% 的电容,其面积电容为 4.92 mF cm-2。电子纺织品的这种可持续闭环回收利用展示了将其重新用于多功能应用的潜力,促进了一种循环方法,有可能防止对环境的负面影响并减少垃圾填埋处理。
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引用次数: 0
Electrokinetic Analysis-Driven Promotion of Electrocatalytic CO Reduction to n-Propanol. 电动分析驱动的电催化一氧化碳还原成正丙醇的促进作用。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202406345
Yaqin Yan, Kunhao Liu, Chao Yang, Yangshen Chen, Ximeng Lv, Cejun Hu, Lijuan Zhang, Gengfeng Zheng

The electrocatalytic carbon dioxide or carbon monoxide reduction reaction (CO2RR or CORR) features a sustainable method for reducing carbon emissions and producing value-added chemicals. However, the generation of C3 products with higher energy density and market values, such as n-propanol, remains highly challenging, which is attributed to the unclear formation mechanism of C3+ versus C2 products. In this work, by the Tafel slope analysis, electrolyte pH correlation exploration, and the kinetic analysis of CO partial pressure fitting, it is identified that both n-propanol and C2 products share the same rate-determining step, which is the coupling of two C1 intermediates via the derivation of the Butler-Volmer equation. In addition, inspired by the mechanistic study, it is proposed that a high OH concentration and a water-limited environment are beneficial for promoting the subsequent *C2-*C1 coupling to n-propanol. At 5.0 m [OH-], the partial current density of producing n-propanol (jn-propanol) reached 45 mA cm-2, which is 35 and 1.3 times higher than that at 0.01 m [OH-] and 1.0 m [OH-], respectively. This study provides a comprehensive kinetic analysis of n-propanol production and suggests opportunities for designing new catalytic systems for promoting the C3 production.

电催化二氧化碳或一氧化碳还原反应(CO2RR 或 CORR)是减少碳排放和生产高附加值化学品的可持续方法。然而,生成能量密度和市场价值更高的 C3 产物(如正丙醇)仍然极具挑战性,原因在于 C3+ 与 C2 产物的形成机理尚不清楚。在这项工作中,通过塔菲尔斜率分析、电解质 pH 值相关性探索和 CO 分压拟合动力学分析,确定了正丙醇和 C2 产物具有相同的速率决定步骤,即通过推导 Butler-Volmer 方程耦合两个 C1 中间体。此外,受机理研究的启发,有人提出高浓度的 OH─ 和限水环境有利于促进随后的 *C2-*C1 与正丙醇的偶联。在 5.0 m [OH-] 条件下,生成正丙醇的部分电流密度(jn-propanol)达到 45 mA cm-2,分别是 0.01 m [OH-] 和 1.0 m [OH-] 条件下的 35 倍和 1.3 倍。这项研究对正丙醇的生产提供了全面的动力学分析,并为设计新的催化体系以促进 C3 的生产提供了机会。
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引用次数: 0
PAD4 Inhibitor-Loaded Layered Double Hydroxide Nanosheets as a Multifunctional Nanoplatform for Photodynamic Therapy-Mediated Tumor Metastasis Treatment. PAD4抑制剂负载的层状双氢氧化物纳米片作为光动力疗法介导的肿瘤转移治疗的多功能纳米平台
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202404211
Rong Chen, Tingting Hu, Yu Lu, Shuqing Yang, Min Zhang, Chaoliang Tan, Ruizheng Liang, Yuji Wang

Photodynamic therapy (PDT) is demonstrated to be effective in inducing antitumor immune responses for tumor metastasis treatment. However, tumor hypoxia, inferior tissue penetration of light, and low singlet oxygen (1O2) quantum yield significantly hamper the efficacy of PDT, thus weakening its immune function. Moreover, PDT-mediated neutrophil extracellular traps (NETs) formation can further reduce the therapeutic effectiveness. Herein, the use of defect-rich CoMo-layered double hydroxide (DR-CoMo-LDH) nanosheets as a carrier to load a typical peptidyl arginine deiminase 4 inhibitor, i.e., YW4-03, to construct a multifunctional nanoagent (403@DR-LDH) for PDT/immunotherapy, is reported. Specifically, 403@DR-LDH inherits excellent 1O2 generation activity under 1550 nm laser irradiation and improves the half-life of YW4-03. Meanwhile, 403@DR-LDH plus 1550 nm laser irradiation can stimulate immunogenic cell death to promote the maturation of dendric cells and activation/infiltration of T cells and significantly downregulate H3cit protein expression to inhibit NETs formation, synergistically promoting the antitumor metastasis effect. Taken together, 403@DR-LDH can kill cancer cells and inhibit tumor growth/metastasis under 1550 nm laser irradiation. Single-cell analysis indicates that 403@DR-LDH can regulate the ratio of immune cells and immune-related proteins to improve the tumor immune microenvironment, showing strong efficacy to inhibit the tumor growth, metastasis, and recurrence.

光动力疗法(PDT)被证明能有效诱导抗肿瘤免疫反应,用于治疗肿瘤转移。然而,肿瘤缺氧、光的组织穿透性较差以及单线态氧(1O2)量子产率较低等因素严重影响了光动力疗法的疗效,从而削弱了其免疫功能。此外,PDT 介导的中性粒细胞胞外捕获物(NETs)的形成会进一步降低治疗效果。本文报道了利用富含缺陷的 CoMo 层状双氢氧化物(DR-CoMo-LDH)纳米片作为载体,载入典型的肽基精氨酸脱氨酶 4 抑制剂 YW4-03,从而构建出一种用于光透射/免疫疗法的多功能纳米试剂(403@DR-LDH)。具体而言,403@DR-LDH 在 1550 nm 激光照射下具有优异的 1O2 生成活性,并改善了 YW4-03 的半衰期。同时,403@DR-LDH 加 1550 纳米激光照射可刺激免疫原性细胞死亡,促进树突细胞的成熟和 T 细胞的活化/浸润,并显著下调 H3cit 蛋白的表达,抑制 NETs 的形成,协同促进抗肿瘤转移作用。综上所述,403@DR-LDH 可在 1550 纳米激光照射下杀死癌细胞并抑制肿瘤生长/转移。单细胞分析表明,403@DR-LDH 可调节免疫细胞和免疫相关蛋白的比例,改善肿瘤免疫微环境,对抑制肿瘤生长、转移和复发具有很强的功效。
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引用次数: 0
Revealing the Role of Ruthenium on the Performance of P2-Type Na0.67Mn1-xRuxO2 Cathodes for Na-Ion Full-Cells. 揭示钌对 Na 离子全电池 P2 型 Na0.67Mn1-xRuxO2 阴极性能的作用。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-10-02 DOI: 10.1002/smll.202406332
Emine Altin, Iqra Moeez, Eunji Kwon, Ali Hussain Umar Bhatti, Seungho Yu, Kyung Yoon Chung, Muhammad Arshad, Messaoud Harfouche, Murat Buldu, Sebahat Altundag, Fatih Bulut, Sevda Sahinbay, Serdar Altin, Mehmet Nurullah Ates

Herein, P2-type layered manganese and ruthenium oxide is synthesized as an outstanding intercalation cathode material for high-energy density Na-ion batteries (NIBs). P2-type sodium deficient transition metal oxide structure, Na0.67Mn1-xRuxO2 cathodes where x varied between 0.05 and 0.5 are fabricated. The partially substituted main phase where x = 0.4 exhibits the best electrochemical performance with a discharge capacity of ≈170 mAh g-1. The in situ X-ray Absorption Spectroscopy (XAS) and time-resolved X-ray Diffraction (TR-XRD) measurements are performed to elucidate the neighborhood of the local structure and lattice parameters during cycling. X-ray photoelectron spectroscopy (XPS) revealed the oxygen-rich structure when Ru is introduced. Density of States (DOS) calculations revealed the Fermi-Level bandgap increases when Ru is doped, which enhances the electronic conductivity of the cathode. Furthermore, magnetization calculations revealed the presence of stronger Ru─O bonds and the stabilizing effect of Ru-doping on MnO6 octahedra. The results of Time-of-flight secondary-ion mass spectroscopy (TOF-SIMS) revealed that the Ru-doped sample has more sodium and oxygenated-based species on the surface, while the inner layers mainly contain Ru-O and Mn-O species. The full cell study demonstrated the outstanding capacity retention where the cell maintained 70% of its initial capacity at 1 C-rate after 500 cycles.

本文合成了 P2 型层状锰和钌氧化物,作为高能量密度钠离子电池(NIBs)的一种出色的插层阴极材料。制备了 P2- 型缺钠过渡金属氧化物结构 Na0.67Mn1-xRuxO2 阴极,其中 x 在 0.05 和 0.5 之间变化。x = 0.4 的部分取代主相表现出最佳的电化学性能,放电容量≈170 mAh g-1。原位 X 射线吸收光谱(XAS)和时间分辨 X 射线衍射(TR-XRD)测量阐明了循环过程中局部结构和晶格参数的邻域。X 射线光电子能谱 (XPS) 揭示了引入 Ru 时的富氧结构。状态密度(DOS)计算显示,当掺入 Ru 时,费米级带隙增大,从而增强了阴极的电子导电性。此外,磁化计算表明,Ru─O 键的存在更强,掺杂 Ru 对 MnO6 八面体具有稳定作用。飞行时间二次离子质谱(TOF-SIMS)的结果表明,掺杂 Ru 的样品表面有更多的钠和含氧物种,而内层则主要含有 Ru-O 和 Mn-O 物种。全电池研究表明,该电池具有出色的容量保持能力,在 1 C 速率下循环 500 次后,其容量仍保持在初始容量的 70%。
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引用次数: 0
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