Suzhou Nano Institute of Supercapacitor Electrode Materials Based on Two-dimensional Single Crystal Nanosheets

Since the Yangshao Culture (5000–3000 BC), ancient Chinese people living in the Yellow River Basin began to use natural layered materials to create pottery, such as bowls, plates, and vessels. This early innovation marked the beginning of the Neolithic Age and represented a significant step in human history—being the first time that humans intentionally used layered materials to create new objects. Over time, with further research into these materials, more advanced layered compounds were discovered and applied, including graphite, montmorillonite, layered sulfides, and layered metal hydroxides. Among these, layered metal hydroxides are anionic layered compounds, typically composed of transition metals like cobalt, nickel, and iron. Like other lamellar materials, they can be exfoliated into monolayer structures with a thickness of just about 1 nanometer. Due to their large surface area, these two-dimensional materials show great potential in electrochemical applications, such as supercapacitors. However, the high surface energy of these 2D materials often leads to self-stacking during electrode preparation, which significantly hinders their practical use in electrochemical systems. To address this challenge, researchers at the Institute of Nanotechnology and Nano-Bionics, Chinese Academy of Sciences, and Suzhou University, led by Qi Jian, developed a novel method for preparing a full two-dimensional supercapacitor electrode. By utilizing the surface charge for intercalation and assembly of heterogeneous materials, they successfully avoided the "self-stacking" issue. The team first used the electrostatic interaction between graphene oxide and monolayer cobalt hydroxide to achieve self-assembly of two-dimensional materials, resulting in high-performance supercapacitor electrodes. Their findings were published in *Chem. Commun.* (2011) and *Langmuir* (2012). Further work focused on improving the electrochemical performance of supercapacitors by adjusting the interlayer spacing of α-phase layered cobalt hydroxide using small molecule ligands. They successfully created cobalt hydroxide layers with spacing of 1.6, 0.7, and 0.09 nm, and studied how these variations affected capacitor activity. This research was published in *Adv. Funct. Mater.* (2013). In subsequent studies, the team observed a phase transition during the exfoliation of α-phase cobalt hydroxide, leading to the successful synthesis of single-layer β-phase cobalt hydroxide with a thickness of only ~1 nm. The yield of this process was nearly 100%. They then fabricated a composite electrode by self-assembling reduced graphene oxide with the β-phase cobalt hydroxide nanosheets, which demonstrated excellent supercapacitor performance. This work was published in *ACS Nano* (DOI: 10.1021/nn500386u). These studies were supported by several key projects, including the National Natural Science Foundation of China (21004076), the “973” Major Research Plan (2013CB933000), and the Key Deployment Project of the Chinese Academy of Sciences (KJZD-EW-M01-3).

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