Kinetics of the thermal decomposition of thermally reduced graphene oxide treated with a pulsed high-frequency discharge in hydrogen atmosphere

Pub Date : 2024-05-01 DOI:10.1063/10.0025619
M. Barabashko, M. Drozd, A. V. Dolbin, R. M. Basnukaeva, N. А. Vinnikov
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Abstract

Thermal stability and the kinetics of thermal decomposition of the thermally reduced graphene oxide (TRGO) treated by a pulsed high-frequency discharge in a hydrogen atmosphere have been studied. The modified Hummers method was used for obtaining the initial graphite oxide from graphite powder. Thermal exfoliation of the graphene oxide powder has been done in vacuum conditions with a heating rate of 5–7 degrees per minute to a temperature of 300 °С. TRGO has been treated by pulsed high-frequency discharge in a hydrogen atmosphere for partial graphene hydrogenation (chemical addition of atomic hydrogen) that leads to structural changes in the carbon planes and formation of C–H sp3 bonds. The thermogravimetry analysis measurements of the mass loss have been carried from room temperature to 1000 °C in a nitrogen atmosphere with a nitrogen flow rate of 20 mL/min and different heating rates: 50, 75 100, 125, 150, and 200 K/min, respectively. Kissinger’s multiple heating rate method has been used to determine the activation energy for decomposing substances. Activation energies Ea1, Ea2, and Ea3 equal 28, 50, and 148 kJ/mol, respectively, have been compared with the energies of the activation of thermal defunctionalization of multiwalled carbon nanotubes (MWCNTs). The activation energy Ea3 = 148 kJ/mol is close to that of the thermal decomposition of anhydride functional groups in MWCNT. The value of Ea2 = 50 kJ/mol indicates the presence of the keto and hydroxy acid’s function groups on TRGO. Activation energy Ea1 = 28 kJ/mol related with all other groups including the lighter C–H bonds that destructed due to dehydrogenation of the TRGO. Obtained experimental results are useful for further proposing the kinetic model of the mechanism of the most probable reaction of TRGO decomposition.
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在氢气环境中用脉冲高频放电处理热还原氧化石墨烯的热分解动力学
研究了在氢气环境中通过脉冲高频放电处理的热还原氧化石墨烯(TRGO)的热稳定性和热分解动力学。从石墨粉中获取初始氧化石墨时采用了改进的 Hummers 法。氧化石墨烯粉末的热剥离是在真空条件下进行的,加热速度为每分钟 5-7 度,温度为 300 °С。TRGO 在氢气环境中通过脉冲高频放电进行部分石墨烯氢化(原子氢的化学添加)处理,从而导致碳平面的结构变化和 C-H sp3 键的形成。在氮气环境中,以 20 mL/min 的氮气流速和不同的加热速率,从室温到 1000 °C 进行了质量损失的热重分析测量:加热速率分别为 50、75 100、125、150 和 200 K/分钟。基辛格的多重加热速率法被用来测定分解物质的活化能。活化能 Ea1、Ea2 和 Ea3 分别等于 28、50 和 148 kJ/mol,并与多壁碳纳米管(MWCNT)的热解官能化活化能进行了比较。活化能 Ea3 = 148 kJ/mol 与 MWCNT 中酸酐官能团热分解的活化能接近。Ea2 = 50 kJ/mol 的值表明 TRGO 上存在酮和羟基酸官能团。活化能 Ea1 = 28 kJ/mol 与所有其他基团有关,包括因 TRGO 脱氢而破坏的较轻的 C-H 键。获得的实验结果有助于进一步提出 TRGO 最可能分解反应的动力学机理模型。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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