All‐solid‐state supercapacitors are known for their safety, stability, and excellent cycling performance. However, their limited voltage window results in lower energy density, restricting their widespread application in practical scenarios. Therefore, in this work, CC/MoO3@Ti3C2Tx negative electrode and Mo1Al1‐MnO2/CC positive electrode materials are synthesized and prepared by electrochemical deposition co‐coating and one‐step hydrothermal methods, respectively, and assembled into an asymmetric supercapacitor (ASC) device based on the two electrode materials. The study reveals that the surface capacitances of the positive and negative electrodes are 1685.5 mF cm−2 and 1134.98 mF cm−2 correspondingly, with potential windows of both as high as 1.1 V. Surprisingly, the potential window of the all‐solid‐state supercapacitor assembled based on the two electrodes reaches 2.2 V, and the energy density reaches 0.44 m W h cm−2, which is much higher than the performance indicators based on similar electrodes. The resulting excellent performance parameters are mainly attributed to the efficient synergy between the pseudo‐capacitance effect of the MoO3 film and the high electrical conductivity of the Ti3C2Tx sheets, as well as the great improvement of the intrinsic electron mobility and ion diffusion channel stability of MnO2 by Mo and Al bimetallic doping.

中文翻译：

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协调宽电压窗口和高能量密度，实现非对称全固态超级电容器


全固态超级电容器以其安全性、稳定性和出色的循环性能而闻名。然而，它们的电压窗口有限，导致能量密度较低，限制了它们在实际场景中的广泛应用。因此，本工作分别通过电化学沉积共涂层和一步水热法合成并制备了 CC/MoO3@Ti3C2Tx负极和 Mo1Al1-MnO2/CC 正极材料，并基于这两种电极材料组装成不对称超级电容器 （ASC） 器件。研究表明，正极和负极的表面电容分别为 1685.5 mF cm-2 和 1134.98 mF cm-2，电位窗均高达 1.1 V。令人惊讶的是，基于两个电极组装的全固态超级电容器的电位窗达到 2.2 V，能量密度达到 0.44 m W h cm-2， 这远高于基于类似电极的性能指标。由此产生的优异性能参数主要归因于 MoO3 薄膜的赝电容效应与 Ti3C2Tx 片材的高导电性之间的有效协同作用，以及 Mo 和 Al 双金属掺杂对 MnO2 的本征电子迁移率和离子扩散通道稳定性的极大改善。