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一种环境可持续的超声辅助石墨烯剥离方法及其与聚苯胺的纳米复合用于超级电容器应用。

An environmentally sustainable ultrasonic-assisted exfoliation approach to graphene and its nanocompositing with polyaniline for supercapacitor applications.

作者信息

A P Chandni, Vattapparambil Chandran Suchitra, Narayanan Binitha N

机构信息

Department of Chemistry, University of Calicut, Calicut University (PO), Malappuram DT, Kerala - 673635, India.

Department of Chemistry, University of Calicut, Calicut University (PO), Malappuram DT, Kerala - 673635, India.

出版信息

Ultrasonics. 2025 Jan;145:107482. doi: 10.1016/j.ultras.2024.107482. Epub 2024 Sep 29.

Abstract

In the present work, a green high-yielding method for the preparation of graphene is introduced via ultrasonic-assisted liquid phase exfoliation (LPE) of graphite in a green solvent medium, since the common preparation method of graphene via graphite oxide is hazardous. A high concentration of 3.2 mg/ml graphene is achieved here in a comparatively short duration of 3 h ultrasonication. By using a mixed solvents strategy (acetophenone and isopropyl alcohol, 1:19 V/V), surface energy requirements needed for the exfoliation of graphite are satisfied here with acetophenone, where isopropyl alcohol further facilitated the exfoliation via non-conventional CH-π and OH-π interactions. Turbostratic graphene in high-yield (16 %) in a simple means of ultrasonic assisted LPE is the added attraction of the present procedure. The less-defective structure of graphene, its few-layered turbostratic nature, and edge functionalization of the sheets are evident from the material characterization via Raman spectroscopy, XRD, TEM-SAED, and XPS analyses. Here, we report a combination of the attractive conducting polymer polyaniline (PANI) with the as-prepared graphene for supercapacitor applications, where the PANI/graphene nanocomposites with different aniline concentrations (PANI1.125/G, PANI4.5/G, and PANI9/G) have been prepared via in-situ polymerization of aniline in the graphene dispersion. The structure and morphology of the nanocomposites are investigated using different characterization techniques which revealed that the molecular structure of the PANI is retained in the nanocomposites even with a strong interaction with graphene. FESEM and TEM images revealed the good coverage of graphene sheets with PANI that limit the volume change of PANI during the repeated charge-discharge processes. Electrochemical studies showed that PANI4.5/G has the highest specific capacitance of 126.16 mF/cm at a current density of 1 mA/cm, resulting from the perfect combination of the pseudocapacitance behavior of the PANI along with the electrical double layer capacitance of graphene. A symmetric supercapacitor device is also fabricated with PANI4.5/G, which showed the highest areal capacitance of 116.38 mF/cm similar to that with three-electrode studies and also good cycling stability with 87 % capacitance retention in the specific capacitance after 6000 cycles. It also exhibited an energy density of 16 µWh/cm (0.29 Wh/kg) and a power density of 3.99 mW/cm (72.72 W/kg).

摘要

在本工作中,介绍了一种绿色高产制备石墨烯的方法,即通过在绿色溶剂介质中对石墨进行超声辅助液相剥离(LPE),因为通过氧化石墨烯制备石墨烯的常用方法具有危险性。在此,通过3小时的超声处理,在相对较短的时间内实现了3.2毫克/毫升的高浓度石墨烯。通过使用混合溶剂策略(苯乙酮和异丙醇,体积比1:19),苯乙酮满足了石墨剥离所需的表面能要求,而异丙醇通过非常规的CH-π和OH-π相互作用进一步促进了剥离。以简单的超声辅助LPE方法高产率(16%)制备的乱层石墨烯是本方法的额外吸引力。通过拉曼光谱、XRD、TEM-SAED和XPS分析对材料进行表征,石墨烯结构缺陷较少、具有少层乱层性质以及片层边缘功能化的特点显而易见。在此,我们报道了将具有吸引力的导电聚合物聚苯胺(PANI)与所制备的石墨烯结合用于超级电容器应用,其中通过在石墨烯分散体中原位聚合苯胺制备了不同苯胺浓度的PANI/石墨烯纳米复合材料(PANI1.125/G、PANI4.5/G和PANI9/G)。使用不同的表征技术研究了纳米复合材料的结构和形态,结果表明即使与石墨烯有强烈相互作用,PANI的分子结构仍保留在纳米复合材料中。FESEM和TEM图像显示PANI对石墨烯片层有良好的覆盖,这限制了PANI在反复充放电过程中的体积变化。电化学研究表明,在电流密度为1毫安/平方厘米时,PANI4.5/G具有最高比电容126.16毫法/平方厘米,这是由于PANI的赝电容行为与石墨烯的双电层电容完美结合所致。还使用PANI4.5/G制作了对称超级电容器器件,其表现出与三电极研究相似的最高面积电容116.38毫法/平方厘米,并且在6000次循环后比电容保持率为87%,具有良好的循环稳定性。它还表现出16微瓦/平方厘米(0.29瓦/千克)的能量密度和3.99毫瓦/平方厘米(72.72瓦/千克)的功率密度。

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