Catalysis Group, Department of Chemistry, Indian Institute of Technology Indore, Khandwa Road, Simrol, Indore, Madhya Pradesh 453552, India.
Inorg Chem. 2022 Mar 21;61(11):4618-4626. doi: 10.1021/acs.inorgchem.1c03529. Epub 2022 Mar 8.
Efficient catalytic systems based on arene-Ru(II) complexes bearing bis-imidazole methane-based ligands were developed to achieve additive-free hydrogen generation from formaldehyde and paraformaldehyde in water. Our findings inferred the influential role of bis-imidazole methane ligands in the observed catalytic performance of the studied catalysts. Among the screened complexes, [(η--cymene)RuCl()]Cl () ( = 4,4'-((2-methoxyphenyl)methylene)bis(2-ethyl-5-methyl-1-imidazole) outperformed others to generate hydrogen gas from paraformaldehyde in water with an exceptionally high turnover number (TON) of >20,000. A detailed mechanistic pathway for hydrogen gas generation from formaldehyde has been proposed on the basis of identified several crucial catalytic intermediate species involved in the hydrogen production process.
开发了基于芳基-Ru(II)配合物的高效催化体系，该配合物带有双咪唑甲烷基配体，可在水中实现甲醛和多聚甲醛的无添加剂制氢。我们的研究结果推断出双咪唑甲烷配体在研究催化剂的观察到的催化性能中具有重要作用。在所筛选的配合物中，[(η--环戊二烯)RuCl()]Cl ()（ = 4,4'-((2-甲氧基苯基)亚甲基)双(2-乙基-5-甲基-1-咪唑)）在水中从多聚甲醛中生成氢气的表现优于其他配合物，其周转数（TON）超过 20,000。基于鉴定出的几个参与制氢过程的关键催化中间物种，提出了从甲醛生成氢气的详细机理途径。
