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Emergence of electrochemical catalytic activity via an electrochemical-probe on defective transition metal dichalcogenide nanosheets 通过电化学探针在有缺陷的过渡金属二卤化物纳米片上发现电化学催化活性
Pub Date : 2024-02-27 DOI: 10.1063/5.0175653
A. Kumatani, H. Ogawa, T. Endo, J. Lustikova, H. Ida, Y. Takahashi, Y. Miyata, Y. Ikuhara, H. Shiku, Y. Wakayama
Two-dimensional transition metal dichalcogenides (2D TMDs) have shown exceptional electrochemical catalytic activity for the efficient generation of hydrogen through electrochemical water splitting. In the case of molybdenum disulfide (MoS2), a prominent member of 2D TMDs, the electrochemically active sites primarily reside at the edges, while the basal plane, which constitutes the majority of the MoS2 structure, remains relatively inactive. In this study, we aimed to activate the inert sites of the basal plane with some defective structure for hydrogen evolution reaction (HER) by employing an electrochemical-probe in combination with voltage sweeping. The initiation of HER at these previously inactive sites was visualized and confirmed using scanning electrochemical cell microscopy (SECCM). Our findings reveal that the enhanced HER activity originates from surface defects induced by the probing process.
二维过渡金属二掺杂物(2D TMDs)在通过电化学水分离高效制氢方面表现出了卓越的电化学催化活性。二硫化钼(MoS2)是二维 TMD 的重要成员,其电化学活性位点主要位于边缘,而构成 MoS2 结构大部分的基底面则相对不活跃。在本研究中,我们旨在通过电化学探针结合电压扫描,激活基底面上具有某些结构缺陷的惰性位点,使其发生氢进化反应(HER)。使用扫描电化学细胞显微镜(SECCM)观察并确认了在这些先前不活跃的位点上启动氢进化反应的过程。我们的研究结果表明,HER 活性的增强源于探测过程诱发的表面缺陷。
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引用次数: 0
Solar energy harvesting using new broadband metamaterial solar absorbers for generation of heat 利用新型宽带超材料太阳能吸收器收集太阳能以产生热量
Pub Date : 2024-01-31 DOI: 10.1063/5.0179924
Vivek Khichar, Nader Hozhabri, A. R. Koymen
We have designed and fabricated TiN/SiO2/TiN–HfO2-based new metamaterial microstructures as an absorber of the visible wavelength, in the range of 400–700 nm, with exceptionally high absorption efficiency (>96%) for solar energy harvesting purposes and generation of heat upon absorption of electromagnetic energy. The finite element method-based COMSOL Multiphysics software simulations were used to optimize the structural parameters of the microstructures and visualize the electric field and electromagnetic power loss distribution in the structure. An optimized 2D unit cell of the structure consists of a 4 μm × 160 nm TiN base on a glass substrate covered with a 70 nm thick SiO2 film. A periodic structure of TiN straps (each 90 nm thick and 2 μm wide) is deposited over the SiO2. The straps are capped with a 40 nm thick layer of high-temperature dielectric HfO2 with a periodicity of 4 µm. This unit is symmetric along the other dimension and is repeated periodically along the horizontal direction. Similar optimized parameters were used for 7, 10, and 100 µm periodic structures to investigate the effect of grating structure pitch on the absorption of light. Although these microstructures were optimized for the visible light spectrum, they show absorption efficiency of >92% when integrated over a broadband wavelength spectrum ranging from 400 to 1200 nm. The experimental data show excellent agreement with the simulated results. We observe less than 5% difference between experimental and simulated absorption efficiencies for the investigated microstructures. Furthermore, we should emphasize that, to the best of our knowledge, this is the first study to experimentally report the light to heat conversion in metamaterials with micron-range size patterned structures.
我们设计并制造了基于 TiN/SiO2/TiN-HfO2 的新型超材料微结构,作为可见光波长(400-700 nm)范围内的吸收器,具有极高的吸收效率(>96%),可用于太阳能收集目的,并在吸收电磁能后产生热量。基于有限元法的 COMSOL Multiphysics 软件模拟用于优化微结构的结构参数,并直观显示结构中的电场和电磁功率损耗分布。该结构的优化二维单元由一个 4 μm × 160 nm 的 TiN 基底组成,基底位于玻璃衬底上,上面覆盖着一层 70 nm 厚的 SiO2 薄膜。二氧化硅上沉积有周期性结构的 TiN 带(每条厚 90 nm,宽 2 μm)。这些带子上覆盖着一层 40 纳米厚、周期为 4 微米的高温介电质 HfO2。该单元沿另一维度对称,并沿水平方向周期性重复。类似的优化参数也用于 7、10 和 100 µm 周期结构,以研究光栅结构间距对光吸收的影响。虽然这些微结构是针对可见光光谱进行优化的,但在波长范围为 400 至 1200 纳米的宽带光谱中,它们的吸收效率大于 92%。实验数据与模拟结果非常吻合。我们观察到,所研究的微结构的实验吸收效率与模拟吸收效率相差不到 5%。此外,我们需要强调的是,据我们所知,这是首次通过实验报告具有微米级尺寸图案结构的超材料中的光热转换。
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引用次数: 0
Three-dimensional network of graphene for electrochemical capacitors and capacitive deionization 用于电化学电容器和电容式去离子的三维石墨烯网络
Pub Date : 2024-01-31 DOI: 10.1063/5.0177677
Hongda Zhu, Dingfei Deng, Chiwei Xu, Xuebin Wang, Xiangfen Jiang
Supercapacitors, as high-performance energy storage devices, have garnered extensive research interest. Furthermore, capacitive deionization technology based on a supercapacitor has emerged as a crucial solution to tackling issues of freshwater scarcity and seawater pollution. However, their power density and cycling lifespan remain constrained by electrode materials. In recent years, 3D network graphene materials have gained prominence as an ideal choice due to their unique porous structure, high specific surface area, and excellent conductivity. This review summarizes the preparation methods of 3D network graphene materials, including techniques like chemical vapor deposition, graphene oxide reduction, and foaming methods. It also discusses their applications and the ongoing research advancements in supercapacitor energy storage and capacitive deionization. Ultimately, this review offers researchers an understanding and outlook on the application of 3D network graphene materials in supercapacitor energy storage and capacitive deionization.
超级电容器作为高性能的储能设备,已经引起了广泛的研究兴趣。此外,基于超级电容器的电容式去离子技术已成为解决淡水匮乏和海水污染问题的重要解决方案。然而,其功率密度和循环寿命仍然受到电极材料的限制。近年来,三维网络石墨烯材料因其独特的多孔结构、高比表面积和优异的导电性而成为一种理想的选择。本综述总结了三维网络石墨烯材料的制备方法,包括化学气相沉积、氧化石墨烯还原和发泡法等技术。综述还讨论了石墨烯在超级电容器储能和电容式去离子方面的应用和正在取得的研究进展。最终,这篇综述让研究人员了解并展望了三维网络石墨烯材料在超级电容器储能和电容式去离子中的应用。
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引用次数: 0
Transforming scalable synthesis of graphene aerosol gel material toward highly flexible and wide-temperature tolerant printed micro-supercapacitors 将可扩展合成的石墨烯气溶胶凝胶材料转化为高柔性、宽温差印刷微型超级电容器
Pub Date : 2024-01-25 DOI: 10.1063/5.0186302
Kh M Asif Raihan, S. Sahoo, T. Nagaraja, Shusil Sigdel, Brice Lacroix, Christopher M. Sorensen, Suprem R. Das
The ever-growing demand for portable, bendable, twistable, and wearable microelectronics operating in a wide temperature range has stimulated an immense interest in the development of solid-state flexible energy storage devices using scalable fabrication technology. Herein, we developed additively manufactured graphene aerosol gel-based all-solid-state micro-supercapacitors (MSCs) via inkjet printing with functioning temperature in the range from −15 to +70 °C and exhibiting a super-stable and reliable electrochemical performance using interdigitated finger electrodes and PVA/H3PO4 solid-state electrolyte. The graphene aerosol gel was obtained using a scalable single step synthesis method from a gas phase precursor using a detonation process, producing a nanoscale shell type structure. The fabricated graphene aerosol gel-based solid-state MSC achieved a volumetric capacitance of 376.63 mF cm−3 (areal capacitance of 76.23 μF cm−2) at a constant current of 0.25 μA and demonstrated exceptional cyclic stability (∼99.6% of capacitance retention) over 10 000 cycles. To exploit the mechanical strength of the as-fabricated graphene aerosol gel-based solid-state MSC, its supercapacitive performance was scrutinized under various bending and twisting angles and the results showed excellent mechanical flexibility. Furthermore, to study the electrochemical performance of the as-fabricated graphene aerosol gel solid-state MSC in stringent surroundings, a broad temperature dependent supercapacitive analysis was performed as stated above. The electrochemical results of the as-fabricated graphene aerosol gel based all-solid-state MSC exhibit a highly potential route to develop scalable and authentic future miniaturized energy storage devices for IoT based smart electronic appliances.
对可在宽温度范围内工作的便携式、可弯曲、可扭转和可穿戴微电子的需求日益增长,激发了人们对利用可扩展制造技术开发固态柔性储能器件的极大兴趣。在此,我们通过喷墨打印技术开发了基于石墨烯气溶胶凝胶的添加式制造全固态微型超级电容器(MSCs),其工作温度范围为 -15 ℃ 至 +70 ℃,并使用相互咬合的指状电极和 PVA/H3PO4 固态电解质表现出超稳定和可靠的电化学性能。石墨烯气溶胶凝胶采用可扩展的单步合成法,从气相前驱体中通过引爆工艺获得,产生纳米级壳型结构。在 0.25 μA 的恒定电流下,制成的基于石墨烯气溶胶凝胶的固态 MSC 的体积电容达到 376.63 mF cm-3(等效电容为 76.23 μF cm-2),并在 10,000 次循环中表现出卓越的循环稳定性(电容保持率为 99.6%)。为了利用所制备的石墨烯气溶胶凝胶固态 MSC 的机械强度,研究人员对其在各种弯曲和扭转角度下的超级电容性能进行了仔细研究,结果表明其具有出色的机械柔韧性。此外,为了研究制备的石墨烯气溶胶凝胶固态 MSC 在严格环境下的电化学性能,如上所述进行了广泛的温度依赖性超级电容分析。基于气溶胶凝胶的全固态石墨烯气溶胶固态 MSC 的电化学结果表明,为基于物联网的智能电子设备开发可扩展、可靠的未来微型化储能设备提供了一条极具潜力的途径。
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引用次数: 0
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