Shao Zhihui, Li Yang, Liu Chenguang, Ai Wenying, Luo Shu-Ping, Liu Qiang
Center of Basic Molecular Science (CBMS), Department of Chemistry, Tsinghua University, Beijing, 100084, China.
State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou, 310014, China.
Nat Commun. 2020 Jan 30;11(1):591. doi: 10.1038/s41467-020-14380-3.
The development of cost-effective, sustainable, and efficient catalysts for liquid organic hydrogen carrier systems is a significant goal. However, all the reported liquid organic hydrogen carrier systems relied on the use of precious metal catalysts. Herein, a liquid organic hydrogen carrier system based on non-noble metal catalysis was established. The Mn-catalyzed dehydrogenative coupling of methanol and N,N'-dimethylethylenediamine to form N,N'-(ethane-1,2-diyl)bis(N-methylformamide), and the reverse hydrogenation reaction constitute a hydrogen storage system with a theoretical hydrogen capacity of 5.3 wt%. A rechargeable hydrogen storage could be achieved by a subsequent hydrogenation of the resulting dehydrogenation mixture to regenerate the H-rich compound. The maximum selectivity for the dehydrogenative amide formation was 97%.
开发用于液体有机氢载体系统的具有成本效益、可持续且高效的催化剂是一个重要目标。然而，所有已报道的液体有机氢载体系统都依赖于使用贵金属催化剂。在此，建立了一种基于非贵金属催化的液体有机氢载体系统。锰催化甲醇与N,N'-二甲基乙二胺脱氢偶联形成N,N'-(乙烷-1,2-二基)双(N-甲基甲酰胺)，以及逆氢化反应构成了一个理论储氢容量为5.3 wt%的储氢系统。通过对所得脱氢混合物进行后续氢化以再生富氢化合物，可以实现可再充电储氢。脱氢酰胺形成的最大选择性为97%。
