Alptekin Oznur, Sen Betul, Savk Aysun, Ercetin Umran, Mustafov Sibel Demiroglu, Fellah Mehmet Ferdi, Sen Fatih
Department of Mechanical Engineering, Faculty of Engineering, Dumlupınar University, Evliya Çelebi Campus, 43100, Kütahya, Turkey.
Sen Research Group, Department of Biochemistry, Faculty of Art and Science, Dumlupınar University, Evliya Çelebi Campus, 43100, Kütahya, Turkey.
Sci Rep. 2020 Apr 29;10(1):7215. doi: 10.1038/s41598-020-64221-y.
In this study, the effects of silica-based gold-nickel (AuNi@SiO) nanohybrid to the production of hydrogen from dimethylamine borane (DMAB) were investigated. AuNi@SiO nanohybrid constructs were prepared as nanocatalysts for the dimethylamine borane dehydrogenation. The prepared nanohybrid structures were exhibited high catalytic activity and a stable form. The resulting nanohybrid, AuNi@SiO as a nanocatalyst, was tested in the hydrogen evolution from DMAB at room temperature. The synthesized nanohybrids were characterized using some analytical techniques. According to the results of the characterization, it was observed that the catalyst was in nanoscale and the gold-nickel alloys showed a homogenous distribution on the SiO surface. After characterization, the turn over frequency (TOF) of nanohybrid prepared for the production of hydrogen from dimethylamine was calculated (546.9 h). Also, the prepared nanohybrid can be used non-observed a significant decrease in activity even after the fifth use, in the same reaction. In addition, the activation energy (E) of the reaction of DMAB catalyzed AuNi@SiO nanohybrid was found to be 16.653 ± 1 kJmol that facilitated the catalytic reaction. Furthermore, DFT-B3LYP calculations were used on the AuNi@SiO cluster to investigate catalyst activity. Computational results based on DFT obtained in the theoretical part of the study support the experimental data.
在本研究中，研究了二氧化硅基金纳米镍（AuNi@SiO）杂化材料对二甲胺硼烷（DMAB）制氢的影响。制备了AuNi@SiO纳米杂化结构作为二甲胺硼烷脱氢的纳米催化剂。所制备的纳米杂化结构表现出高催化活性和稳定形态。将所得的纳米杂化物AuNi@SiO作为纳米催化剂，在室温下对其从DMAB析氢进行了测试。使用一些分析技术对合成出的纳米杂化物进行了表征。根据表征结果，观察到催化剂处于纳米尺度，并且金镍合金在SiO表面呈现均匀分布。表征之后，计算了用于二甲胺制氢的纳米杂化物的周转频率（TOF）（546.9 h⁻¹）。此外，所制备的纳米杂化物在相同反应中即使在第五次使用后也未观察到活性有显著下降。另外，发现AuNi@SiO纳米杂化材料催化的DMAB反应的活化能（E）为16.653±1 kJmol⁻¹，这促进了催化反应。此外，对AuNi@SiO团簇进行了密度泛函理论（DFT）-B3LYP计算以研究催化剂活性。在该研究的理论部分基于DFT获得的计算结果支持了实验数据。
