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水滑石骨架稳定的钌纳米颗粒(Ru/HTaL):用于氨硼烷甲醇解的高效多相催化剂。

Hydrotalcite framework stabilized ruthenium nanoparticles (Ru/HTaL): efficient heterogeneous catalyst for the methanolysis of ammonia-borane.

作者信息

BaĞuÇ İsmail Burak, Yurderİ Mehmet, Saydan KanberoĞlu Gülşah, Bulut Ahmet

机构信息

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

出版信息

Turk J Chem. 2020 Apr 1;44(2):364-377. doi: 10.3906/kim-1910-44. eCollection 2020.

Abstract

Ruthenium nanoparticles stabilized by a hydrotalcite framework (Ru/HTaL) were prepared by following a 2-step procedure comprising a wet-impregnation of ruthenium(III) chloride precatalyst on the surface of HTaL followed by an ammonia-borane (NHBH) reduction of precatalyst on the HTaL surface all at room temperature. The characterization of Ru/HTaL was done by using various spectroscopic and visualization methods including ICP-OES, P-XRD, FTIR, B NMR, XPS, BFTEM, and HRTEM. The sum of the results gained from these analyses has revealed the formation of well-dispersed and highly crystalline ruthenium nanoparticles with a mean diameter of 1.27 ±0.8 nm on HTaL surface. The catalytic performance of Ru/HTaL in terms of activity, selectivity, and stability was investigated in the methanolysis of ammonia-borane (NHBH , AB), which has been considered as one of the most promising chemical hydrogen storage materials. It was found that Ru/HTaL can catalyse methanolysis of AB effectively with an initial turnover frequency (TOF) value of 392.77 min at conversion (>95%) even at room temperature. Moreover, the catalytic stability tests of Ru/HTaL in AB methanolysis showed that Ru/HTaL acts as a highly stable and reusable heterogeneous catalyst in this reaction by preserving more than 95% of its initial activity even at the 5th recycle.

摘要

通过两步法制备了由水滑石骨架稳定的钌纳米颗粒(Ru/HTaL),该方法包括在室温下将氯化钌(III)预催化剂湿浸渍在HTaL表面,然后用氨硼烷(NHBH)还原HTaL表面的预催化剂。通过使用各种光谱和可视化方法对Ru/HTaL进行表征,包括ICP-OES、P-XRD、FTIR、B NMR、XPS、BFTEM和HRTEM。这些分析结果表明,在HTaL表面形成了平均直径为1.27±0.8 nm的分散良好且高度结晶的钌纳米颗粒。在被认为是最有前途的化学储氢材料之一的氨硼烷(NHBH,AB)的甲醇解反应中,研究了Ru/HTaL在活性、选择性和稳定性方面的催化性能。结果发现,即使在室温下,Ru/HTaL也能有效地催化AB的甲醇解反应,初始周转频率(TOF)值为392.77 min,转化率(>95%)。此外,Ru/HTaL在AB甲醇解反应中的催化稳定性测试表明,Ru/HTaL在该反应中是一种高度稳定且可重复使用的多相催化剂,即使在第5次循环时仍能保持其初始活性的95%以上。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/fa7e/7671226/35e4821c9b16/turkjchem-44-364-fig001.jpg

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