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单壁碳纳米管负载的Pt-Ru双金属超纳米催化剂用于在温和条件下由甲胺硼烷甲醇解制氢

Single-walled carbon nanotube supported Pt-Ru bimetallic superb nanocatalyst for the hydrogen generation from the methanolysis of methylamine-borane at mild conditions.

作者信息

Sogut Eda Gokirmak, Acidereli Hilal, Kuyuldar Esra, Karatas Yasar, Gulcan Mehmet, Sen Fatih

机构信息

Chemistry Department, Faculty of Science, Van Yüzüncü Yıl University, Zeve Campus, 65080, Van, Turkey.

Sen Research Group, Biochemistry Department, Faculty of Arts and Science, Dumlupınar University, Evliya Çelebi Campus, 43100, Kütahya, Turkey.

出版信息

Sci Rep. 2019 Oct 31;9(1):15724. doi: 10.1038/s41598-019-52182-w.

Abstract

Several metal nanoparticle based catalysts have been synthesized for catalyzing the hydrogen production process by hydrolysis of methylamine-borane (MeAB). However, there was only one study that catalyzes the producing of hydrogen via the methanolysis of MeAB, and it was carried out by our research group. For this reason, in this work, a new catalyst system entitled by single-walled carbon nanotube (SWCNT) supported bimetallic platinum-ruthenium nanoparticles were developed and called as PtRu@SWCNT. These NPs were characterized by several techniques (XRD, XPS, Raman, and TEM), and they were performed for the methanolysis of MeAB with high catalytic activity. The prepared PtRu@SWCNT NPs were also tested in the methanolysis of MeAB at different parameters including different temperatures, catalyst and substrate concentrations, and reusability performance. Experimental results revealed that the new PtRu@SWCNT NPs had excellent catalytic activity and reusability for removing of hydrogen from the methanolysis of MeAB at ambient conditions. According to the obtained data, the turnover frequency is 136.25 mole H/mole PtRu × min, and the activation energy (Ea) is 17.29 kJ/mole. More than 99% of conversion was observed at room temperature.

摘要

已经合成了几种基于金属纳米颗粒的催化剂,用于催化甲胺硼烷(MeAB)水解制氢过程。然而,仅有一项研究是关于通过MeAB甲醇解制氢的,且该研究由我们的研究团队进行。因此,在本工作中,开发了一种名为单壁碳纳米管(SWCNT)负载双金属铂钌纳米颗粒的新型催化剂体系,称为PtRu@SWCNT。这些纳米颗粒通过多种技术(XRD、XPS、拉曼光谱和TEM)进行了表征,并对其在MeAB甲醇解反应中表现出的高催化活性进行了研究。制备的PtRu@SWCNT纳米颗粒还在不同参数(包括不同温度、催化剂和底物浓度以及可重复使用性能)下进行了MeAB甲醇解反应测试。实验结果表明,新型PtRu@SWCNT纳米颗粒在环境条件下对MeAB甲醇解制氢具有优异的催化活性和可重复使用性。根据所得数据,周转频率为136.25摩尔H/摩尔PtRu×分钟,活化能(Ea)为17.29 kJ/摩尔。在室温下观察到转化率超过99%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6a85/6823424/22341bef15c1/41598_2019_52182_Fig1_HTML.jpg

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