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Towards practical Li-ion full batteries with glass anodes 使用玻璃阳极开发实用的全锂离子电池
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-29 DOI: 10.1016/j.nanoen.2024.109950
Kai Zheng , Lanxiang Chen , Zhitao Shan , Jiayan Zhang , Chengwei Gao , Yuanzheng Yue , Yanfei Zhang

Vanadium (V)-based glasses have recently garnered considerable attention as promising anode materials for lithium-ion batteries (LIBs) due to their abundance of Li+ storage sites, neglectable volume expansion upon lithiation/delithiation, and facile preparation. However, the inherently low electronic conductivity and relatively low energy density of V-based glass anodes hinder its application in full LIBs. In this work, we tackled this challenge by optimizing the chemical composition of the V-based glass anode to achieve high-performance half and full cells. We investigated the impact of partially substituting B2O3 for P2O5 in 50V2O5-(50-x)P2O5-xB2O3 (mol%) (VPB) glass series on its structure and electrochemical performances. The glass with 30 mol% B2O3 (VPB30 glass) was found to deliver the highest electronic conductivity, an enhanced reversible capacity of 470 mA h g−1 at 1 A g−1 after 500 cycles, and an excellent rate capability. The optimized performances were ascribed to the boosted lithium-ion diffusivity and the increased lithium storage sites. We assembled a full cell by coupling a VPB30 glass anode with a LiCoO2 cathode to test its cycling performance. The VPB30//LiCoO2 cell exhibits the required power density, and hence, high practicality. Our work implied the practical application of glass anodes in high-performance LIBs.

钒(V)基玻璃作为锂离子电池(LIB)的阳极材料,因其具有丰富的 Li+ 储存位点、在锂化/退锂化过程中可忽略的体积膨胀以及易于制备等优点,最近引起了广泛关注。然而,V 基玻璃阳极固有的低电子电导率和相对较低的能量密度阻碍了它在全锂离子电池中的应用。在这项工作中,我们通过优化 V 基玻璃阳极的化学成分来应对这一挑战,从而实现高性能的半电池和全电池。我们研究了在 50V2O5-(50-x)P2O5-xB2O3 (mol%) (VPB) 玻璃系列中用 B2O3 部分替代 P2O5 对其结构和电化学性能的影响。研究发现,含 30 mol% B2O3 的玻璃(VPB30 玻璃)具有最高的电子电导率,在 1 A g-1 的条件下循环 500 次后,可逆容量可提高到 470 mA h g-1,并且具有出色的速率能力。性能的优化归功于锂离子扩散率的提高和锂存储点的增加。我们通过将 VPB30 玻璃阳极与钴酸锂阴极耦合组装成一个完整的电池,以测试其循环性能。VPB30//LiCoO2 电池达到了所需的功率密度,因此具有很高的实用性。我们的工作意味着玻璃阳极在高性能锂电池中的实际应用。
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引用次数: 0
Novel ultrastable 2D MOF/MXene nanofluidic membrane with ultralow resistance for highly efficient osmotic power harvesting 具有超低电阻的新型超稳定二维 MOF/MXene 纳米流体膜,可用于高效渗透动力收集
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.nanoen.2024.109924
Wen-Hung Lin , Ting-Yi Huang , Chi-Han Bai , Cheng-Hsuan Hung , Chia-An Lung , Wen-Hsin Hung , Kalon Gopinadhan , Li-Hsien Yeh

Two-dimensional (2D) materials have shown great potential in harvesting osmotic power due to their high membrane selectivity, but the high resistance from tortuous pathways of 2D nanofluidic membranes still impedes the further improvement in output performance. Here, we report an innovative 2D MXCT (MXene/Cu-TCPP) lamellar membrane with ultralow resistance for highly efficient osmotic power generation. The incorporation of 2D Ti3C2Tx MXene with rich functional groups not only resolves the water-stability issue of 2D metal-organic framework (MOF) Cu-TCPP, but provides large surface charges for selective ion transport. The orderly sub-2 nm framework channels of Cu-TCPP provide much shorter permeation pathways for fast ion transport, thus endowing the MXCT membrane with ultralow resistance. Consequently, the MXCT membrane reaches an ultrahigh power output of ∼8.29 W/m2 by mixing seawater and river water, which is ∼275 % higher than that of the pristine MXene membrane. Additionally, it outperforms all the reported single-layer 2D nanosheet-based osmotic power generators under the same experimental conditions in terms of output power and internal resistance (9 kΩ). This work presents a reliable strategy for stabilizing 2D Cu-TCPP MOF in electrolytes, opening new avenues for designing promising 2D nanofluidic membranes for efficient blue energy harvesting and ionic devices.

二维(2D)材料因其高膜选择性而在收集渗透动力方面显示出巨大潜力,但二维纳米流体膜的曲折路径所产生的高阻力仍然阻碍着输出性能的进一步提高。在此,我们报告了一种具有超低阻力的创新型二维 MXCT(MXene/Cu-TCPP)层状膜,可用于高效渗透发电。含有丰富官能团的二维 Ti3C2Tx MXene 不仅解决了二维金属有机框架(MOF)Cu-TCPP 的水稳定性问题,还为选择性离子传输提供了大量表面电荷。Cu-TCPP 2 纳米以下的有序框架通道为快速离子传输提供了更短的渗透路径,从而使 MXCT 膜具有超低电阻。因此,MXCT 膜在混合海水和河水后可达到 8.29 W/m2 的超高功率输出,比原始 MXene 膜高出 275%。此外,在相同的实验条件下,它的输出功率和内阻(9 kΩ)均优于所有已报道的基于单层二维纳米片的渗透发电装置。这项研究提出了在电解质中稳定二维铜-TCPP MOF 的可靠策略,为设计用于高效蓝色能量收集和离子装置的前景广阔的二维纳米流体膜开辟了新途径。
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引用次数: 0
Boosting the intercalation reaction of FeOF-based cathode toward highly reversible lithium storage 促进基于 FeOF 正极的插层反应,实现高度可逆的锂存储
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.nanoen.2024.109944
Yechao Lin , Yufan Xia , Haosheng Li , Xuan Zhang , Huiling Liu , Youchen Hao , Hongge Pan , Mi Yan , Yinzhu Jiang

FeOF as an intercalation-conversion cathode features a high theoretical capacity toward high energy density lithium-ion batteries (LIBs). However, the inadequate intercalation process and poor reversibility of redox reaction deteriorate its practical capacity and cycling stability. Herein, a S-substitution strategy in FeOF (FeOF-S) is proposed to boost the intercalation reaction and enhance the reaction kinetics, achieving a record-high capacity of 668 mAh g−1 at 0.05 A g−1 and a long cycling stability up to 1500 cycles at 0.5 A g−1. Under this strategy, the Li+ intercalation energy of FeOF-S is remarkably reduced in thermodynamics, promoting the intercalation capacity to 230 mAh g−1 which is 50% higher than that of FeOF. Furthermore, a nearly zero band gap with superior electronic conduction is achieved in FeOF-S, leading to excellent rate capability with much enhanced pseudo-capacitance contribution. This work presents new insights into the regulation of thermodynamics and kinetics toward the boosted electrochemical performance of conversion-type electrodes for high energy density LIBs.

作为一种插层转换阴极,FeOF 对高能量密度锂离子电池(LIB)具有很高的理论容量。然而,不充分的插层过程和氧化还原反应的可逆性较差,降低了其实际容量和循环稳定性。本文提出了一种在 FeOF(FeOF-S)中进行 S 取代的策略,以促进插层反应并增强反应动力学,在 0.05 A g-1 的条件下实现了 668 mAh g-1 的创纪录高容量,在 0.5 A g-1 的条件下实现了高达 1500 次循环的长循环稳定性。在这种策略下,FeOF-S 的锂+插层能量在热力学上显著降低,使插层容量达到 230 mAh g-1,比 FeOF 高出 50%。此外,FeOF-S 实现了接近零的带隙和卓越的电子传导,从而具有出色的速率能力,并大大提高了伪电容贡献。这项研究就如何调节热力学和动力学以提高高能量密度 LIB 转换型电极的电化学性能提出了新的见解。
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引用次数: 0
Post-treatment optimization for silver nanowire networks in transparent droplet-based TENG sensors 基于透明液滴的 TENG 传感器中银纳米线网络的后处理优化
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.nanoen.2024.109940
Onuralp Cakir , Doga Doganay , Murathan Cugunlular , Melih Ogeday Cicek , Onur Demircioglu , Sahin Coskun , Husnu Emrah Unalan

Transparent conducting electrodes (TCEs) serve as essential components in various devices, including smart windows, thin film heaters, and sensors. Historically, indium tin oxide (ITO) thin films have served as the primary TCE material. However, the scarcity of indium in the Earth’s crust and costly vacuum-based deposition processes have prompted researchers to seek alternatives. While silver nanowire (Ag NW) networks have emerged as the leading candidate for TCEs among various alternatives, the presence of polyvinyl pyrrolidone (PVP) layer surrounding Ag NWs often leads to substantial contact resistances at the junction areas. Given the diverse characteristics of Ag NWs, including length, diameter, PVP thickness, and deposition methods, the efficacy of a specific post-treatment method on the same Ag NW batch remained unknown. This work collected effective post-treatment methods from existing literature and innovatively developed in-house approaches to optimize the treatment of Ag NW networks. Following post-treatment, the resulting electrodes exhibited a 70 % reduction in sheet resistance, with only a marginal 1 % decrease in optical transmittance. The optical figure of merit (FoM) for the optimized networks showed a remarkable five-fold improvement, rising from 66 to 305. The optimized Ag NW networks were then utilized as current collectors in water droplet-based TENG sensors, showcasing the device's effectiveness in pH and chemical concentration sensing. The fabricated TENG recorded peak Voc and Isc values of 22 V and 370 nA, respectively. Furthermore, we developed a sensor-integrated device capable of gauging the incident droplets’ pH level, signaling acid rain safety. In addition, the droplets activate a large-area Ag NW-based transparent thin film heater. Rapid defogging and defrosting capabilities of the heater was also demonstrated. The device holds the potential to be applied to the side-view mirrors of cars, providing an anti-fogging display for a significantly safer journey.

透明导电电极(TCE)是智能窗户、薄膜加热器和传感器等各种设备的重要组成部分。一直以来,铟锡氧化物(ITO)薄膜是主要的 TCE 材料。然而,地壳中铟的稀缺性和昂贵的真空沉积工艺促使研究人员寻找替代品。在各种替代品中,银纳米线(Ag NW)网络已成为 TCE 的主要候选材料,但银纳米线周围聚乙烯吡咯烷酮(PVP)层的存在往往会导致交界处产生巨大的接触电阻。考虑到 Ag NWs 的不同特性,包括长度、直径、PVP 厚度和沉积方法,特定的后处理方法对同一批 Ag NWs 的功效仍是未知数。这项工作从现有文献中收集了有效的后处理方法,并创新性地开发了内部方法来优化 Ag NW 网络的处理。经过后处理后,所得电极的片电阻降低了 70%,而光学透射率仅略微降低了 1%。优化网络的光学优越性(FoM)显著提高了五倍,从 66 提高到 305。优化后的银纳米线网络被用作基于水滴的 TENG 传感器的集流器,展示了该器件在 pH 值和化学浓度传感方面的有效性。所制造的 TENG 记录的峰值 Voc 和 Isc 值分别为 22 V 和 370 nA。此外,我们还开发了一种集成传感器的装置,能够测量入射液滴的 pH 值,从而发出酸雨安全信号。此外,液滴还能激活基于 Ag NW 的大面积透明薄膜加热器。加热器的快速除雾和除霜功能也得到了验证。该装置有望应用于汽车的侧视镜,提供防雾显示,大大提高行车安全。
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引用次数: 0
Corrigendum to “High-bandwidth self-powered vibration sensors based on triboelectric particle-surface interactions” [Nano Energy 119 (2024) 109060] 基于三电粒子-表面相互作用的高带宽自供电振动传感器"[纳米能源 119 (2024) 109060] 更正
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.nanoen.2024.109935
Shanshi Gao , Guang Li , Shuying Wu , Teresa X. Cheng , Zhao Sha , Shuai He , Shuhua Peng , Chun H. Wang
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引用次数: 0
A highly efficient self-powered variable impendence system 高效的自供电可变阻抗系统
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.nanoen.2024.109942
Jie Chen , Ruilong Guo , Wei Zhao , Mei Chen , Jian Hu , Xingwei Wang , Fei Wu , Hengyu Guo

As an efficient mechanical energy harvester, the triboelectric-electromagnetic hybrid generator (TEHG) stands as a cornerstone in self-powered systems. Nevertheless, significant impedance disparities between triboelectric nanogenerators (TENGs) and electromagnetic generators (EMGs) often hamper systems’ energy utilization efficiency, attributed to impedance mismatch at the load. Here, a variable impedance strategy is proposed, aimed at maximizing the utilization of mechanical energies converted by TEHG. This approach capitalizes on electronic components with dynamic impedance from GΩ to kΩ in response to OFF-ON state transitions, thus matching the impedance of TENG and EMG. Experimentally, an ultraviolent gas discharge tube (UV-GDT) is integrated into the self-powered variable impedance system. Operated at 240 rpm, the TEHG-driven UV-GDT extracts energy amounting to 1304.27 mJ with an 87.5 % utilization efficiency. These metrics outperform the situation where UV-GDT is individually powered by either EMG (0 mJ, 0 %) or TENG (18.24 mJ, 60.7 %). Furthermore, the mechanical energy-activated UV system demonstrates promise for sterilization, curing, and photo-chemical reactions. This variable impedance strategy resolves the impendence mismatch between TEHG and load, more importantly, provides a valuable guideline for developing hybrid generator systems with enhanced energy utilization efficiency.

作为一种高效的机械能收集器,三电-电磁混合发电机(TEHG)是自供电系统的基石。然而,由于负载阻抗不匹配,三电纳米发电机(TENG)和电磁发电机(EMG)之间存在明显的阻抗差异,往往会影响系统的能量利用效率。本文提出了一种可变阻抗策略,旨在最大限度地利用 TEHG 转换的机械能。这种方法利用电子元件的动态阻抗从 GΩ 到 kΩ,以响应关-开状态转换,从而匹配 TENG 和 EMG 的阻抗。实验中,自供电可变阻抗系统集成了一个紫外气体放电管(UV-GDT)。TEHG 驱动的 UV-GDT 在 240 rpm 的转速下工作,可提取 1304.27 mJ 的能量,利用效率为 87.5%。这些指标均优于由 EMG(0 mJ,0 %)或 TENG(18.24 mJ,60.7 %)单独为 UV-GDT 供电的情况。此外,机械能激活的紫外线系统在灭菌、固化和光化学反应方面也大有可为。这种可变阻抗策略解决了 TEHG 与负载之间的阻抗失配问题,更重要的是,它为开发具有更高能量利用效率的混合发电机系统提供了宝贵的指导。
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引用次数: 0
Solar water evaporation-induced long-term locomotion of self-propelled soft robots 太阳能水蒸发诱导自走式软体机器人长期运动
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.nanoen.2024.109938
Ruoyu Sun , Chuang Liu , Jing Zhao , Qiangqiang Sun , Jiliang Mo , Zhongrong Zhou

Self-propelled soft robots have attracted extensive attention because of their unique application in exploring dangerous and complex environments that are unsuitable for human beings. However, these soft robots require cyclical chemical stimulation or external power and have short locomotion times, which limits their practical applications. It remains challenging to create self-propelled soft robots exhibiting long-term locomotion. Here, we couple an active hydrogel with a solar absorbing coating to realize self-propelled soft robots with long-term locomotion. The active hydrogel can move freely on the water surface by continuously establishing asymmetric surface tension through dynamic wetting. The sunlight absorbers promote water evaporation inside the self-propelled soft robot to delay or even disrupt the swelling equilibrium of the hydrogel, thus establishing dynamic balance between water absorption and evaporation. In this way, the locomotion time of this self-propelled soft robot under constant light irradiation equivalent to 1 sun (1 kW/m2) is 6.5 times higher than that of active hydrogel reported previously. Owing to the enhanced locomotion time through solar water evaporation water, this self-propelled soft robot is expected to be applied to oil pollution exploration, cargo transportation, and debris cleaning in small water areas.

自走式软体机器人因其在探索不适合人类的危险和复杂环境方面的独特应用而受到广泛关注。然而,这些软体机器人需要周期性的化学刺激或外部动力,且运动时间较短,这限制了它们的实际应用。要制造出具有长期运动能力的自推进软体机器人仍然是一项挑战。在这里,我们将活性水凝胶与太阳能吸收涂层结合起来,实现了具有长期运动能力的自推进软机器人。活性水凝胶通过动态润湿不断建立非对称表面张力,从而在水面上自由移动。阳光吸收剂促进自走式软机器人内部的水分蒸发,延缓甚至破坏水凝胶的溶胀平衡,从而在吸水和蒸发之间建立动态平衡。这样,在相当于 1 个太阳(1 kW/m2)的恒定光照射下,这种自走式软机器人的运动时间是之前报道的活性水凝胶的 6.5 倍。由于通过太阳能蒸发水提高了运动时间,这种自走式软机器人有望应用于油污勘探、货物运输和小水域的杂物清理。
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引用次数: 0
Fe-NiO/MoO2 and in-situ reconstructed Fe, Mo-NiOOH with enhanced negatively charges of oxygen atoms on the surface for salinity tolerance seawater splitting 表面氧原子负电荷增强的 Fe-NiO/MoO2 和原位重构的 Fe、Mo-NiOOH,用于耐盐性海水分离
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.nanoen.2024.109921
Shiyu Qin , Zhan Zhao , Jianpeng Sun , Zisheng Zhang , Xiangchao Meng

Seawater electrolysis is a promising technique for H2 production on a large scale. However, the electrocatalytic activity and stability will be deteriorated as the increase of salt concentrations which happened in the seawater splitting. Herein, through the electrodeposition and rapid Joule heating method, the Fe-NiO/MoO2 heterostructure is designed as a highly active bifunctional electrocatalyst. During the OER possess, Fe-NiO/MoO2 is reconstructed to the Fe, Mo-NiOOH with Fe and Mo co-doping. Based on the theoretical analysis, more electrons were transferred to the O atoms on the surface of Fe, Mo-NiOOH, thereby forming a more negatively charged surface. Moreover, that surface is found to repel Cl ions while enriching H2O molecules to form a thin water layer on Fe, Mo-NiOOH surface based on molecule dynamics (MD) simulation, thereby improving the anti-corrosion capacity of Fe, Mo-NiOOH. The reconstructed Fe, Mo-NiOOH achieved an overpotential of 399 mV at 1000 mA cm−2 in alkaline seawater, and the increase of overpotential for Fe, Mo-NiOOH was about 0.02 V at 500 mA cm−2 from 0 M to 3 M NaCl in 1 M KOH electrolyte. For the HER, Fe-NiO/MoO2 achieved an overpotential of 169 mV and 417 mV at 100 and 1000 mA cm−2 in alkaline seawater, respectively, and the increase of overpotential for Fe-NiO/MoO2 was about 0 mV at 500 mA cm−2 from 0 M to 3 M NaCl in 1 M KOH electrolyte. This work sheds fresh light into the development of efficient electrocatalysts for salinity tolerance seawater splitting.

海水电解是一种很有前途的大规模生产 H2 的技术。然而,海水电解过程中盐浓度的增加会导致电催化活性和稳定性的降低。本文通过电沉积和快速焦耳加热的方法,设计了一种高活性双功能电催化剂--Fe-NiO/MoO2 异质结构。在拥有 OER 的过程中,Fe-NiO/MoO2 被重构为 Fe、Mo-NiOOH,并掺杂了 Fe 和 Mo。根据理论分析,更多的电子转移到了 Fe、Mo-NiOOH 表面的 O 原子上,从而形成了带负电荷更多的表面。此外,根据分子动力学(MD)模拟发现,该表面在排斥 Cl- 离子的同时,还富集了 H2O 分子,在 Fe, Mo-NiOOH 表面形成了一层薄薄的水层,从而提高了 Fe, Mo-NiOOH 的抗腐蚀能力。重构后的 Fe, Mo-NiOOH 在碱性海水中 1000 mA cm-2 的过电位为 399 mV,而在 1 M KOH 电解液中,从 0 M NaCl 到 3 M NaCl,Fe, Mo-NiOOH 在 500 mA cm-2 的过电位增加了约 0.02 V。在碱性海水中,Fe-NiO/MoO2 在 100 和 1000 mA cm-2 条件下的过电位分别为 169 mV 和 417 mV,而在 1 M KOH 电解液中,Fe-NiO/MoO2 在 500 mA cm-2 条件下,从 0 M NaCl 到 3 M NaCl 的过电位增加约为 0 mV。这项工作为开发耐盐性海水分离的高效电催化剂提供了新的启示。
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引用次数: 0
Hybridized triboelectric-electromagnetic nanogenerators for efficient harvesting of wave energy for self-powered ocean buoy 为自供电海洋浮标高效收集波浪能的三电-电磁混合纳米发电机
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-26 DOI: 10.1016/j.nanoen.2024.109929
Chengzhuo Zhang , Shaohui Yang , Xianggang Dai , Yongqiang Tu , Zhichang Du , Xiaobo Wu , Yan Huang , Jianyu Fan , Zhanyong Hong , Tao Jiang , Zhong Lin Wang

Triboelectric nanogenerators (TENGs) have been widely used in energy harvesting from low-frequency, irregular motions due to their unique characteristics and excellent electromechanical conversion efficiency. Harvesting ocean energy to build a marine Internet of Things (MIoTs) has become an important research field for TENGs. However, the output power density of TENGs must be further enhanced for promoting their practical applications, by effective means such as the coupling of TENGs and electromagnetic generators (EMGs). Herein, we report a triboelectric-electromagnetic hybrid nanogenerator (TEH-NG) for self-powered ocean buoy to harvest water wave energy efficiently for the first time. The buoy consists of a self-engineered wave energy converter for converting wave energy into simple turbomachinery energy through the pressure difference created by the relative motion, and a TEH-NG for converting the turbomachinery energy into electrical energy. The TENG delivers an average output power of 3.40 mW (with power density of 141.7 W m−3), and the EMG achieves an average power of 0.04 W (with power density of 400.0 W m−3). The excellent performance of the TEH-NG makes it a potential candidate for constructing the MIoTs to achieve distributed marine environmental monitoring networks.

三电纳米发电机(TENGs)因其独特的特性和出色的机电转换效率,已被广泛应用于从低频、不规则运动中收集能量。收集海洋能量以构建海洋物联网(MIoTs)已成为 TENGs 的一个重要研究领域。然而,为促进其实际应用,必须通过有效手段进一步提高 TENGs 的输出功率密度,如将 TENGs 与电磁发电机(EMGs)耦合。在此,我们首次报道了一种用于自供电海洋浮标的三电-电磁混合纳米发电机(TEH-NG),可有效收集水波能。该浮标由一个自行设计的波浪能转换器和一个将涡轮机械能转换成电能的三电-电磁混合纳米发电机组成,前者通过相对运动产生的压力差将波浪能转换成简单的涡轮机械能,后者则将涡轮机械能转换成电能。TENG 的平均输出功率为 3.40 mW(功率密度为 141.7 W m-3),EMG 的平均输出功率为 0.04 W(功率密度为 400.0 W m-3)。TEH-NG 的优异性能使其成为构建 MIoTs 以实现分布式海洋环境监测网络的潜在候选方案。
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引用次数: 0
Heteroatom anchoring to enhance electrochemical reversibility for high-voltage P2-type oxide cathodes of sodium-ion batteries 杂原子锚定增强钠离子电池高电压 P2- 型氧化物阴极的电化学可逆性
IF 16.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-26 DOI: 10.1016/j.nanoen.2024.109925
Kai Liu , Susheng Tan , Xiao-Guang Sun , Qingqing Zhang , Cheng Li , Hailong Lyu , Lianqi Zhang , Bishnu P. Thapaliya , Sheng Dai

P2-type cathode has received extensive attention due to its faster Na+ diffusion and a high theoretical capacity in sodium-ion batteries (SIBs). However, undesirable phase transformations have induced dramatic capacity decay of SIBs during the cycling process. In this study, heteroatom anchoring through Cu/Mg dual doping is introduced into P2-type Na0.67Ni0.33Mn0.67O2 cathode to enhance high-voltage electrochemical reversibility and modulate interfacial Na+ kinetics. The as-prepared Na0.67Ni0.23Mg0.05Cu0.05Mn0.67O2 exhibits an outstanding capacity retention (83.4 % after 2000 cycles at 10 C) and rate performance (73 mAh g−1 at 10 C, accounting for 58.7 % of that at 0.1 C) over the voltage range of 2.5–4.4 V. Intensive explorations further manifest that the modified mechanism of dual-ion doping strategy is attributed to the synergistic coupling effect of a substantial change in Na occupancy distribution and an increase in oxygen vacancy buffer. Thus, the optimized cathode expedites Na+ diffusion and reduces detrimental phase transformation, which favors high-rate performance and long-term cycling stability. This study develops a route to rationally design high-voltage cathode materials for SIBs.

P2- 型阴极在钠离子电池(SIB)中具有更快的 Na+ 扩散速度和更高的理论容量,因此受到广泛关注。然而,在循环过程中,不良的相变会导致 SIB 的容量急剧下降。在本研究中,通过铜/镁双掺杂将杂质原子锚定引入 P2- 型 Na0.67Ni0.33Mn0.67O2 阴极,以提高高压电化学可逆性并调节界面 Na+ 动力学。制备的 Na0.67Ni0.23Mg0.05Cu0.05Mn0.67O2 在 2.5-4.4 V 的电压范围内表现出出色的容量保持率(10 C 下循环 2000 次后为 83.4%)和速率性能(10 C 下为 73 mAh g-1,占 0.1 C 下的 58.7%)。深入探索进一步表明,双离子掺杂策略的改进机制归因于 Na 占位分布的显著变化和氧空位缓冲的增加所产生的协同耦合效应。因此,优化后的阴极加快了 Na+ 扩散,减少了有害的相变,有利于实现高倍率性能和长期循环稳定性。这项研究为合理设计 SIB 的高压阴极材料开辟了一条途径。
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