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在钌夹复合物的催化作用下,无需 pH 值控制或溶剂改变,甲酸盐盐中实现无胺可逆储氢。

Amine-free reversible hydrogen storage in formate salts catalyzed by ruthenium pincer complex without pH control or solvent change.

机构信息

Loker Hydrocarbon Research Institute and Department of Chemistry, University of Southern California, University Park, Los Angeles, CA 90089-1661 (USA), Fax: (+1) 213-740-5087.

出版信息

ChemSusChem. 2015 Apr 24;8(8):1442-51. doi: 10.1002/cssc.201403458. Epub 2015 Mar 30.

DOI:10.1002/cssc.201403458
PMID:25824142
Abstract

Due to the intermittent nature of most renewable energy sources, such as solar and wind, energy storage is increasingly required. Since electricity is difficult to store, hydrogen obtained by electrochemical water splitting has been proposed as an energy carrier. However, the handling and transportation of hydrogen in large quantities is in itself a challenge. We therefore present here a method for hydrogen storage based on a CO2 (HCO3 (-) )/H2 and formate equilibrium. This amine-free and efficient reversible system (>90 % yield in both directions) is catalyzed by well-defined and commercially available Ru pincer complexes. The formate dehydrogenation was triggered by simple pressure swing without requiring external pH control or the change of either the solvent or the catalyst. Up to six hydrogenation-dehydrogenation cycles were performed and the catalyst performance remained steady with high selectivity (CO free H2 /CO2 mixture was produced).

摘要

由于大多数可再生能源(如太阳能和风能)具有间歇性,因此越来越需要进行能量存储。由于电能难以存储,因此通过电化学水分解获得的氢气被提议作为一种能量载体。然而,大量氢气的处理和运输本身就是一个挑战。因此,我们在此提出了一种基于 CO2(HCO3(-))/H2 和甲酸盐平衡的储氢方法。这种无胺且高效的可逆系统(两个方向的产率均>90%)由经过良好定义且可商购的 Ru 夹钳配合物催化。通过简单的压力转换即可触发甲酸盐脱氢,而无需外部 pH 控制,也无需改变溶剂或催化剂。进行了多达六个加氢-脱氢循环,并且催化剂性能保持稳定,具有高选择性(生成不含 CO 的 H2/CO2 混合物)。

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