Mirshafiee Faezeh, Rezaei Mehran
School of Chemical, Petroleum and Gas Engineering, Iran University of Science and Technology (IUST), Tehran, Iran.
Sci Rep. 2024 Apr 26;14(1):9659. doi: 10.1038/s41598-024-60428-5.
In this study, a series of cobalt-based spinel ferrites catalysts, including nickel, cobalt, zinc, and copper ferrites, were synthesized using the sol-gel auto-combustion method followed by a chemical reduction process. These catalysts were employed for accelerating hydrogen generation via the sodium borohydride hydrolysis process. A continuous stirred tank reactor was used to perform catalytic reactor tests. All samples were subjected to analysis using XRD, FESEM, EDX, FTIR, and nitrogen adsorption-desorption techniques. The results revealed that the cobalt-based copper ferrite sample, Co/Cu-Ferrite, exhibited superior particle distribution, and porosity characteristics, as it achieved a high hydrogen generation rate of 2937 mL/min.g. In addition, the higher electrical donating property of Cu-Ferrite which leads to the increase in the electron density of the cobalt active sites can account for its superior performance towards hydrolysis of NaBH. Using the Arrhenius equation and the zero-order reaction calculation, activation energy for the sodium borohydride hydrolysis reaction on the Co/Cu-Ferrite catalyst was determined to be 18.12 kJ/mol. This low activation energy compared to other cobalt-based spinel ferrite catalysts confirms the catalyst's superior performance as well. Additionally, the outcomes from the recycling experiments revealed a gradual decline in the catalyst's performance after each cycle during 4 repetitive cycles. The aforementioned properties render the Co/Cu-Ferrite catalyst an efficient catalyst for hydrogen generation through NaBH hydrolysis.
在本研究中,采用溶胶-凝胶自燃烧法并结合化学还原过程,合成了一系列钴基尖晶石铁氧体催化剂,包括镍铁氧体、钴铁氧体、锌铁氧体和铜铁氧体。这些催化剂用于通过硼氢化钠水解过程加速氢气生成。使用连续搅拌釜式反应器进行催化反应器测试。所有样品均采用X射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、能谱分析(EDX)、傅里叶变换红外光谱(FTIR)和氮吸附-脱附技术进行分析。结果表明,钴基铜铁氧体样品Co/Cu-铁氧体表现出优异的颗粒分布和孔隙率特性,其氢气生成速率高达2937 mL/min·g。此外,铜铁氧体较高的给电子性能导致钴活性位点的电子密度增加,这可以解释其对硼氢化钠水解的优异性能。利用阿伦尼乌斯方程和零级反应计算,确定Co/Cu-铁氧体催化剂上硼氢化钠水解反应的活化能为18.12 kJ/mol。与其他钴基尖晶石铁氧体催化剂相比,这种低活化能也证实了该催化剂的优异性能。此外,循环实验结果表明,在4次重复循环中,每次循环后催化剂的性能逐渐下降。上述特性使Co/Cu-铁氧体催化剂成为通过硼氢化钠水解制氢的高效催化剂。