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Interfacial Zn ion capture and desolvation engineering for high-performance Zn metal anode 用于高性能锌金属阳极的界面锌离子捕获和脱溶工程
IF 6.2 3区 材料科学 Pub Date : 2024-06-10 DOI: 10.1016/j.flatc.2024.100695
Jianyu Chen , Tian Kang , Fanlai Zhang , Xudong Chen , Xiaoshi Wang , Yanwen Ma , Jin Zhao

The uneven surface of planar zinc (Zn) metal anodes fundamentally reduces the electrochemical reversibility of aqueous Zn metal batteries due to dendritic growth. Herein, an interphase protection layer engineering is formed on the surface of the Zn metal anode through a solution-processed coating method. This interesting carbon layer, composed of carbon nanoparticles obtained from outer flame-derived candle soot (OFCS), exhibits excellent Zn ion capturing and storage capabilities, effectively reducing the accumulation of charge density on the Zn metal surface, providing a homogeneous Zn ion flux and inducing even Zn metal deposition. The OFCS@Zn can promote the desolvation of [Zn(H2O)6]2+ through strong interaction with Zn ions, mitigating corrosion and hydrogen evolution reactions. The multifunctional integration of the OFCS layer synergistically induces uniform Zn metal plating and inhibits side reactions. Consequently, in the OFCS @Zn | OFCS @Zn symmetric-cell tests, high-rate performance and deep charge/discharge capabilities are demonstrated. The OFCS@Zn anode-based pouch cell exhibits a high discharge capacity of 156.2 mAh g-1 and maintains a significant capacity retention rate of 95.4 % for 200 cycles at the current density of 1 A g-1, indicating its potential for enhanced battery stability and efficiency.

由于树枝状生长,平面锌(Zn)金属阳极凹凸不平的表面从根本上降低了水溶液锌金属电池的电化学可逆性。在这里,通过一种溶液加工涂层方法,在锌金属阳极表面形成了一种相间保护层工程。这种有趣的碳层由从外焰烛烟(OFCS)中获得的碳纳米颗粒组成,具有出色的锌离子捕获和存储能力,可有效降低锌金属表面的电荷密度积累,提供均匀的锌离子通量,并诱导锌金属均匀沉积。OFCS@Zn 能通过与 Zn 离子的强相互作用促进 [Zn(H2O)6]2+ 的脱溶,缓解腐蚀和氢演化反应。OFCS 层的多功能集成协同诱导了均匀的锌金属镀层,并抑制了副反应。因此,在 OFCS @Zn | OFCS @Zn 对称电池测试中,显示出了高倍率性能和深度充放电能力。基于 OFCS@Zn 阳极的袋式电池显示出 156.2 mAh g-1 的高放电容量,并且在 1 A g-1 的电流密度下循环 200 次仍能保持 95.4% 的显著容量保持率,这表明它具有提高电池稳定性和效率的潜力。
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引用次数: 0
Exploiting in-plane anisotropy in Ta2NiSe5 spanning near to mid-infrared photodetection 利用 Ta2NiSe5 的面内各向异性实现近红外至中红外光探测
IF 6.2 3区 材料科学 Pub Date : 2024-06-07 DOI: 10.1016/j.flatc.2024.100694
Shicong Hou , Shi Zhang , Kening Xiao , Yunduo Zhang , Yuanfeng Wen , Libo Zhang , Xuguang Guo

Miniaturized and stabilized polarization-sensitive mid-Infrared photodetectors at room temperature are indispensable in fields ranging from medical diagnostics to military surveillance in the next-generation on-chip polarimeters. Emerging two-dimensional materials offer a promising avenue to fulfill these requirements, facilitated by their ease of integration onto complex structures, inherent in-plane anisotropic crystal structures that enhance polarization sensitivity, and robust quantum confinement effects that enable superior photodetection performance at room temperature. Here, we report the systematic investigation of polarization-dependent infrared photoresponse based on Ta2NiSe5, revealing significant anisotropy photocurrent with excellent stability at room temperature. Significantly, a large anisotropic ratio of Ta2NiSe5 ensures the polarization sensitivity achieves a ratio of 1.23 at 1550 nm. Moreover, at 4.6 μm, the device exhibits a peak photocurrent response of 1.16 A/W along the armchair orientation, with an anisotropy ratio of approximately 3.3. These findings not only enhance our understanding of the photophysical mechanisms in two-dimensional materials but also guide the optimization of photodetector design for enhanced performance.

在下一代片上偏振计中,室温下微型化和稳定的偏振敏感中红外光探测器在从医疗诊断到军事监控等领域都是不可或缺的。新兴的二维材料易于集成到复杂的结构中,固有的面内各向异性晶体结构可提高偏振灵敏度,强大的量子约束效应可在室温下实现卓越的光电探测性能,因此为满足这些要求提供了一条大有可为的途径。在此,我们报告了基于 Ta2NiSe5 的偏振依赖性红外光响应的系统研究,揭示了显著的各向异性光电流,并在室温下具有出色的稳定性。值得注意的是,Ta2NiSe5 的各向异性比很大,确保了其偏振灵敏度在 1550 纳米波长达到 1.23。此外,在 4.6 μm 波长处,该器件沿 armchair 方向显示出 1.16 A/W 的峰值光电流响应,各向异性比约为 3.3。这些发现不仅加深了我们对二维材料光物理机制的理解,还为优化光电探测器设计以提高性能提供了指导。
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引用次数: 0
Interface engineering in LGPS-type solid-state electrolytes for all-solid-state lithium batteries 全固态锂电池 LGPS 型固态电解质的界面工程学
IF 6.2 3区 材料科学 Pub Date : 2024-06-06 DOI: 10.1016/j.flatc.2024.100693
Shuai Jian , Hongda Li , Xiaobo Jia , Dailin Zhong , Boran Tao , Xiong He , Guofu Wang , Haixin Chang

As key components of next-generation battery energy storage systems, solid-state batteries have attracted widespread attention. Li10GeP2S12 (LGPS)-type solid-state electrolytes (SSEs) are favored by researchers owing to their excellent ionic conductivity and potential high-temperature stability. However, the poor interface between LGPS-type SSEs and electrodes has seriously hindered the commercialization of LGPS all-solid-state lithium batteries. This review introduces the structure and Li-ion conduction mechanisms of LGPS-type SSEs and discusses the challenges related to LGPS-type SSEs/electrode interfaces, along with strategies for overcoming these challenges. To improve the interface compatibility, researchers have developed feasible methods for improving and optimizing LGPS-type SSEs. The review concludes with potential research directions and prospects of future LGPS all-solid-state lithium batteries.

作为下一代电池储能系统的关键部件,固态电池已引起广泛关注。Li10GeP2S12(LGPS)型固态电解质(SSE)因其优异的离子导电性和潜在的高温稳定性而受到研究人员的青睐。然而,LGPS 型固态电解质与电极之间的界面不良严重阻碍了 LGPS 全固态锂电池的商业化。本综述介绍了 LGPS 型固态锂电池的结构和锂离子传导机制,并讨论了与 LGPS 型固态锂电池/电极界面相关的挑战以及克服这些挑战的策略。为了提高界面兼容性,研究人员开发了改进和优化 LGPS 型 SSE 的可行方法。综述最后介绍了未来 LGPS 全固态锂电池的潜在研究方向和前景。
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引用次数: 0
A novel and promising Penta-Octa-Based silicon carbide semiconductor 一种新型、前景广阔的五辛基碳化硅半导体
IF 6.2 3区 材料科学 Pub Date : 2024-06-05 DOI: 10.1016/j.flatc.2024.100691
José A. S. Laranjeira , Nicolas F. Martins , Pablo A. Denis , Julio R. Sambrano

Penta-octa-graphene (POG) consists of pentagonal and octagonal carbon rings, hosting type-I and type-II Dirac line nodes due to its sp2 and sp3 mixed bonds. Inorganic analogs of 2D carbon lattices have increased the potential applications and changed the main properties of carbon-based structures. Therefore, this work proposes penta-octa-graphene based on silicon carbide using DFT simulations. With a cohesive energy of −5.22 eV/atom, POG-Si5C4 is energetically viable in comparison with other silicon carbide-based monolayers. Phonon dispersion analysis confirms the POG-Si5C4 dynamical stability. MD simulations demonstrate that this new monolayer can withstand temperatures up to 1020 K. Electronic analysis indicates it is a semiconductor with an indirect band gap transition of 2.02 eV. The mechanical properties exhibit anisotropy, with Young’s modulus ranging from 38.65 to 99.47 N/m and an unusual negative Poisson’s ratio of −0.09. The band edge alignment suggests that POG-Si5C4 holds potential for hydrogen generation through photocatalytic water splitting. This research opens possibilities for designing inorganic penta-octa-based structures and provides insights for future experimental and theoretical studies focused on exploring and optimizing advanced silicon-carbide 2D materials.

五八角石墨烯(POG)由五角形和八角形碳环组成,由于其 sp2 和 sp3 混合键,可承载 I 型和 II 型狄拉克线节点。二维碳晶格的无机类似物增加了碳基结构的潜在应用并改变了其主要特性。因此,本研究利用 DFT 模拟提出了基于碳化硅的五-八石墨烯。POG-Si5C4 的内聚能为 -5.22 eV/原子,与其他基于碳化硅的单层相比,在能量上是可行的。声子色散分析证实了 POG-Si5C4 的动态稳定性。电子分析表明它是一种间接带隙转变为 2.02 eV 的半导体。其机械性能表现出各向异性,杨氏模量从 38.65 牛米到 99.47 牛米不等,泊松比为-0.09。带边排列表明,POG-Si5C4 具有通过光催化水分裂产生氢的潜力。这项研究为设计基于五八面体的无机结构提供了可能性,并为未来重点探索和优化先进碳化硅二维材料的实验和理论研究提供了启示。
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引用次数: 0
MXene-based nanocomposite for electrochemical hydrogen evolution reaction: Experimental and theoretical advances 用于电化学氢进化反应的 MXene 基纳米复合材料:实验和理论进展
IF 6.2 3区 材料科学 Pub Date : 2024-06-05 DOI: 10.1016/j.flatc.2024.100692
Agam Pamungkas , Fida N. Rahmani , Fariz Ikramullah , St Mardiana , Grandprix T.M. Kadja

MXene’s outstanding performance in driving the Hydrogen Evolution Reaction (HER) has attracted significant interest. The HER involves hydrogen generation by electrolyzing water. It is widely recognized that hydrogen represents a renewable and future-oriented alternative energy source that is currently receiving significant attention. On the other hand, MXenes also have a crucial function as catalysts, elevating the pace and effectiveness of chemical reactions. Moreover, their properties make them essential in diverse fields, contributing to advancements in energy storage, sensing technology, and catalysis for improved reactions. Herein, we highlighted MXene nanocomposite materials from synthesized to utilization in HER reaction both experimentally and theoretically. Various MXene-based nanocomposites, which consist of monomer, carbon, and oxide that can be used in hydrogen evolution reactions, are also elaborated in detail. Ultimately, we concluded this review with the future prospect of MXenes in electrochemical HER.

MXene 在驱动氢进化反应(HER)方面的出色性能引起了人们的极大兴趣。氢进化反应包括通过电解水产生氢气。氢是一种可再生的、面向未来的替代能源,目前正受到广泛关注。另一方面,二氧化二烯还具有催化剂的重要功能,可加快化学反应的速度并提高其效率。此外,它们的特性还使其在多个领域发挥着重要作用,有助于推动能源储存、传感技术和催化反应的改进。在本文中,我们从实验和理论两方面重点介绍了 MXene 纳米复合材料从合成到在 HER 反应中的应用。我们还详细阐述了各种基于 MXene 的纳米复合材料,它们由单体、碳和氧化物组成,可用于氢进化反应。最后,我们总结了 MXene 在电化学 HER 中的未来前景。
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引用次数: 0
Tailoring tin sulfide electrocatalyst with petroleum coke derived reduced graphene oxide for overall water splitting 利用石油焦衍生的还原氧化石墨烯定制硫化锡电催化剂,实现整体水分离
IF 6.2 3区 材料科学 Pub Date : 2024-05-31 DOI: 10.1016/j.flatc.2024.100689
Chandan Kumar , Thangjam Ibomcha Singh , Pinky Saharan , Ashish Gupta , Jogender Singh , Mandeep Singh , S.R. Dhakate

Metal chalcogenides like Tin sulfide (SnS2) presents as viable alternative electrocatalysts for alkaline water splitting (AWS) due to their huge abundance, stability, and environment friendly nature. However, insufficient exposed active sites and poor conductivity severely impede its large-scale applications. In this work, an in-situ hybridization of hexagonal SnS2 with intercalation of reduced graphene oxide nanosheets (TS-rGOx) overcomes the problem of SnS2 stacking. It further enhances the interlayer spacing thereby boosting the number of active sites. The resulting TS-rGOx exhibited excellent oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) activities demanding low overpotential of 313 mV and 196.2 mV at 20 mA/cm2 with long term durability upto 60 h, which can be attributed to enhanced interlayer spacing of SnS2, abundant active sites and higher conductivity resulting from the in-situ hybridization and intercalation of rGO nanosheets. This work opens a prospect towards the design and application of efficient SnS2 based heterostructured electrocatalyst for AWS.

硫化锡(SnS2)等金属卤化物因其大量存在、稳定性和环境友好性,可作为碱性水分离(AWS)的替代电催化剂。然而,活性位点暴露不足和导电性差严重阻碍了其大规模应用。在这项研究中,六方 SnS2 与还原氧化石墨烯纳米片(TS-rGOx)的原位杂化克服了 SnS2 堆叠的问题。它进一步增强了层间间距,从而增加了活性位点的数量。在 20 mA/cm2 的条件下,TS-rGOx 表现出卓越的氧进化反应(OER)和氢进化反应(HER)活性,过电位分别为 313 mV 和 196.2 mV,长期耐久性可达 60 h,这归因于 rGO 纳米片的原位杂交和插层增强了 SnS2 的层间距、丰富的活性位点和更高的导电性。这项工作为设计和应用基于 SnS2 的高效 AWS 异质结构电催化剂开辟了前景。
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引用次数: 0
Electrodeposition of Au nanoparticles on ITO/PDAC/2H-MoS2 electrode for sensitive determination of bisphenol-A 在 ITO/PDAC/2H-MoS2 电极上电沉积金纳米粒子,用于灵敏测定双酚-A
IF 6.2 3区 材料科学 Pub Date : 2024-05-27 DOI: 10.1016/j.flatc.2024.100690
Fernando H. O. Alves , Marcos A. Gross , Marco A. Souza , Marcelo A. Pereira-da-Silva , Leonardo G. Paterno

Exfoliated 2H-MoS2 holds a promising future for various electrochemical applications. Nevertheless, its electrical conductivity and electrocatalytic efficiency are limited, restricting its standalone use. To address this limitation, this study proposes the electrochemical deposition of gold nanoparticles on layer-by-layer films of poly(diallyl dimethylammonium) hydrochloride interspersed with exfoliated 2H-MoS2, previously assembled on ITO substrate. This modified electrode, denoted as ITO/PDAC/2H-MoS2/Au, was assessed for its effectiveness in the voltametric detection of bisphenol-A (BPA). The optimal electrode architecture demonstrated a linear BPA detection range (0.9 µM-19 µM; R2 > 0.99), with a limit of detection of 23 nM. Notably, the electrochemical deposition was effective on both bare and film modified ITO substrates. However, it was on the ITO/PDAC/2H-MoS2/Au electrode that BPA detection achieved a reasonable level of sensitivity. During electrodeposition, superficial Mo(IV) is oxidized to Mo(VI) while sulfur vacancies are generated. These defect sites enhance the electrochemical activity of 2H-MoS2 and play a pivotal role in nucleating, growing, and immobilizing gold nanoparticles, which collectively enhance the sensor’s performance.

剥离的 2H-MoS 在各种电化学应用中前景广阔。然而,由于其导电性和电催化效率有限,限制了其单独使用。为了解决这一局限性,本研究提出了一种电化学沉积方法,即在聚二烯丙基二甲基铵盐酸盐与剥离的 2H-MoS 相间的逐层薄膜上沉积金纳米粒子,然后将其组装在 ITO 基底上。这种改性电极被称为 ITO/PDAC/2H-MoS/Au,我们评估了它在伏安法检测双酚 A(BPA)中的有效性。最佳电极结构显示出线性双酚 A 检测范围(0.9 µM-19 µM;R > 0.99),检测限为 23 nM。值得注意的是,电化学沉积在裸ITO基底和薄膜修饰ITO基底上都很有效。不过,只有在 ITO/PDAC/2H-MoS/Au 电极上,双酚 A 检测才达到了合理的灵敏度水平。在电沉积过程中,表层的 Mo(IV) 被氧化成 Mo(VI),同时产生硫空位。这些缺陷位点增强了 2H-MoS 的电化学活性,并在金纳米粒子的成核、生长和固定过程中发挥了关键作用,从而共同提高了传感器的性能。
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引用次数: 0
Investigating and optimizing the variation of selenium infused MoS2 as electrode material for supercapacitor applications 研究和优化超级电容器应用中作为电极材料的渗硒 MoS2 的变化
IF 6.2 3区 材料科学 Pub Date : 2024-05-27 DOI: 10.1016/j.flatc.2024.100688
Pardeep Khichi , Priya Siwach , Latisha Gaba , Vijay Kumar , Jagdish Kumar , Anil Ohlan , Rahul Tripathi

Molybdenum disulfide (MoS2) has been immensely explored for its potential usage in energy storage applications owing to its high theoretical specific capacitance and layered structure. Here, we have investigated the effect of selenium addition in MoS2 forming MoS2(1-x)Se2x alloys and studied their electrochemical performance. Selenization was performed through a simple hydrothermal method. The electrochemical performance of MoS1Se1 was evaluated in a two-electrode configuration. The selenization is found to improve the electrochemical performance of MoS2 and the MoS1Se1 alloy with the optimal S (sulfur) to Se (selenium) ratio of 1:1 exhibits an excellent areal capacitance of 2629.45 mF/cm2 at 1 mA/cm2, with an appreciable specific capacitance of 266.51 F/g at a current density of 0.5 A/g and excellent cycle stability of 81.64 % after 6000 cycles. Along with the experimental findings, Density functional theory calculations were also performed, revealing that the electronic properties of MoSSe systems can be tuned by varying the ratio of S and Se.

二硫化钼(MoS)因其高理论比电容和层状结构而被广泛应用于储能领域。在这里,我们研究了在 MoS 中添加硒形成 MoSSe 合金的效果,并研究了它们的电化学性能。硒化是通过简单的水热法进行的。在双电极配置中对 MoSSe 的电化学性能进行了评估。发现硒化改善了 MoS 的电化学性能,最佳 S(硫)与 Se(硒)比为 1:1 的 MoSSe 合金在 1 mA/cm 的电流密度下显示出 2629.45 mF/cm 的优异等面积电容,在 0.5 A/g 的电流密度下显示出 266.51 F/g 的显著比电容,并且在 6000 次循环后显示出 81.64 % 的优异循环稳定性。除了实验结果之外,我们还进行了密度泛函理论计算,结果表明可以通过改变 S 和 Se 的比例来调整 MoSSe 系统的电子特性。
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引用次数: 0
Seeded growth of PdPtAg-on-Au heterogeneous nanoplates for efficient methanol oxidation Reaction: Interface engineering in quaternary metallic electrocatalysts 用于高效甲醇氧化的 PdPtAg-on-Au 异质纳米板的种子生长 反应:季金属电催化剂的界面工程
IF 6.2 3区 材料科学 Pub Date : 2024-05-21 DOI: 10.1016/j.flatc.2024.100674
Yuanyuan Min , Na Zhao , Yingying Wang , Yanyun Ma , Yiqun Zheng

Interface engineering plays a critical role in the development of high-efficient fuel cell catalysts, as the interfaces across different components can synergistically and substantially accelerate electrocatalysis kinetics, together with improvement in mass transfer and structural stability. In this study, we report a feasible strategy to create PdPtAg-on-Au heterogenous nanoplates (PdPtAg-on-Au HNPs) and validate their structural advantages in electrocatalysis. By limiting the doping of Au nanoplates with Pt/Ag atoms on the surface and subsequently depositing Pd nanodots in a highly scattered pattern, abundant multimetallic interfaces form and enhance the methanol oxidation reaction (MOR) electrocatalytic process. The optimized PdPtAg-on-Au HNPs/C electrocatalysts exhibited superior mass activity, improved reaction kinetics, and long-term durability compared to commercial Pt/C. DFT simulations suggest that the chemical surrounding of the Pd/Pt catalytic active center with AuAg atoms can lower the reaction barrier and CO binding affinity. This work provides a feasible synthetic strategy for preparing multimetallic fuel cell electrocatalysts with advanced control over heterogeneous structures, highlighting the potential of interface engineering in the rational design of electrocatalysts.

界面工程在高效燃料电池催化剂的开发中起着至关重要的作用,因为不同组分之间的界面可以协同作用,大大加快电催化动力学,同时改善传质和结构稳定性。在本研究中,我们报告了一种制造 PdPtAg-on-Au 异质纳米板(PdPtAg-on-Au HNPs)的可行策略,并验证了其在电催化中的结构优势。通过限制铂/银原子在金纳米板表面的掺杂,然后以高度分散的方式沉积钯纳米点,形成了丰富的多金属界面,增强了甲醇氧化反应(MOR)的电催化过程。与商用 Pt/C 相比,优化的 PdPtAg-on-Au HNPs/C 电催化剂表现出更高的质量活性、更好的反应动力学和长期耐久性。DFT 模拟表明,Pd/Pt 催化活性中心与 AuAg 原子的化学环绕可以降低反应障碍和 CO 结合亲和力。这项工作为制备多金属燃料电池电催化剂提供了一种可行的合成策略,并对异质结构进行了先进的控制,凸显了界面工程在合理设计电催化剂方面的潜力。
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引用次数: 0
Direct laser writing of MnOx decorated laser-induced graphene on paper for sustainable microsupercapacitor fabrication 在纸上直接激光写入氧化锰装饰的激光诱导石墨烯,实现可持续微型超级电容器制造
IF 6.2 3区 材料科学 Pub Date : 2024-05-16 DOI: 10.1016/j.flatc.2024.100672
Rodrigo Abreu , Maykel dos Santos Klem , Tomás Pinheiro , Joana Vaz Pinto , Neri Alves , Rodrigo Martins , Emanuel Carlos , João Coelho

Laser-induced graphene (LIG) on paper is a popular choice for fabricating flexible micro-supercapacitors (MSCs) as it is a simple and sustainable process. However, carbon-based MSC electrodes have limited energy densities. To address this challenge, this study presents a highly reproducible and cost-effective method for decorating manganese oxide (MnOx) on interdigital LIG MSC electrodes, fabricated via a single-step direct laser writing (DLW) process on paper substrates. The paper fibers embedded with MnOx precursors are transformed into graphene through laser processing while reducing the salt, resulting in the formation of MnOx-LIG. The resulting MnOx-LIG-MSC exhibits a specific capacitance of 12.30 mF cm−2 (0.05 mA cm−2) with a 60 % retention at 1000 bending cycles (30°), due to the pseudocapacitive contribution of MnOx. Furthermore, the devices exhibit high electrochemical stability, retaining 190 % of the initial specific capacitance after 10,000 cycles, and a high energy density of 2.6 μWh cm−2 (at a power of 0.109 mW cm−2). The study demonstrates that manganese oxide-based LIG-MSCs have the potential to be used as energy storage devices for portable, low-cost, and flexible paper electronics.

纸上激光诱导石墨烯(LIG)是制造柔性微型超级电容器(MSC)的热门选择,因为它是一种简单且可持续的工艺。然而,碳基 MSC 电极的能量密度有限。为了应对这一挑战,本研究提出了一种具有高度可重复性和成本效益的方法,用于在纸基底上通过单步直接激光写入(DLW)工艺制作的间隙式 LIG MSC 电极上装饰氧化锰(MnO)。嵌入 MnO 前体的纸纤维通过激光加工转化为石墨烯,同时减少盐分,从而形成 MnO-LIG。由于 MnO 的伪电容作用,由此产生的 MnO-LIG-MSC 在 1000 次弯曲循环(30°)中显示出 12.30 mF cm(0.05 mA cm)的比电容和 60% 的保持率。此外,该器件还具有很高的电化学稳定性,在 10000 次循环后仍能保持 190% 的初始比电容,能量密度高达 2.6 μWh cm(功率为 0.109 mW cm)。这项研究表明,基于氧化锰的 LIG-MSCs 有潜力用作便携式、低成本和柔性纸质电子产品的储能器件。
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引用次数: 0
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