A pairwise/sandwich-like assembly consisting of a TaO3 nanomesh and reduced graphene oxide for a pelletized self-supported cathode towards high-areal-capacity Li-S batteries
A pairwise/sandwich-like assembly consisting of a TaO3 nanomesh and reduced graphene oxide for a pelletized self-supported cathode towards high-areal-capacity Li-S batteries
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由 TaO3 纳米网和还原氧化石墨烯组成的成对/三明治状组件，用于高面积容量锂硫电池的粒状自支撑阴极
DOI：
10.1039/d2ta07139h
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发表时间：
2022
影响因子：
11.9
通讯作者：
Sasaki Takayoshi
中科院分区：
文献类型：
--
作者：
Wang Chenhui;Sakai Nobuyuki;Ebina Yasuo;Suehara Shigeru;Kikuchi Takayuki;Tang Daiming;Ma Renzhi;Sasaki Takayoshi
锂硫电池作为一种极具发展前景的储能技术受到了广泛的关注。然而，由于硫的负荷和利用率低，导致这些电池的实际能量密度较差，阻碍了它们的广泛应用。在这里，我们展示了一种分子成对/三明治状的氧化石墨烯/氧化石墨烯组装，它可以成球成一个自持阴极，以提高硫的负载和利用率。这种独特的双/三明治状异质结构是通过自组装的溶液过程产生的，并通过x射线衍射分析/模拟和TEM观察进行了鉴定。分子尺度的异质结构通过与导电还原氧化石墨烯结合，最大限度地发挥了陶3纳米网的吸引力特征：晶体开放通道、极性Ta-O键、刘易斯酸表面和大量暴露的活性位点。结果表明，该异质结构具有Li+的快速转移、对多硫化物的有效约束以及对多硫化物锂转化和Li2S均匀沉积的高催化活性，从而提高了硫的利用率。因此，用这些自支撑阴极组装的Li-S电池在2 mA cm - 2时获得了10.5 mA h cm - 2的高面容量。这种制造具有高负载粉末状活性材料的电极的通用策略可应用于各种储能系统，如碱金属电池，促进其实际应用。
Lithium–sulfur (Li–S) batteries have attracted considerable attention as a promising energy storage technology. However, the low loading and utilization of sulfur result in the poor practical energy density of these batteries, which has hindered their extensive application. Herein, we demonstrate the fabrication of a molecular pairwise/sandwich-like assembly of TaO3/rGO, which can be pelletized into a self-supported cathode to improve sulfur loading and utilization. This unique pairwise/sandwich-like heterostructure of TaO3/rGO was produced through a solution process via self-assembly and identified by X-ray diffraction analysis/simulation and TEM observations. The molecular-scale heterostructure maximizes attractive features of the TaO3 nanomesh: crystalline open channels, polar Ta–O bonds, Lewis acid surfaces and largely exposed active sites, by combining with electrically conductive rGO. As a result, the heterostructure exhibited fast Li+ transfer, effective confinement of polysulfides and high catalytic activity for the conversion of lithium polysulfides and uniform deposition of Li2S, thereby contributing to high sulfur utilization. Consequently, the Li–S batteries assembled with these self-supported cathodes achieved a high areal capacity of 10.5 mA h cm−2 at 2 mA cm−2. This versatile strategy of fabricating electrodes with a high loading of powder-like active materials can be applied to various energy storage systems, such as alkali metal batteries, promoting their practical application.