Boddien Albert, Gartner Felix, Mellmann Dorthe, Sponholz Peter, Junge Henrik, Laurenczy Gábor, Beller Matthias
Leibniz-Institut für Katalyse e.V., Universität Restock, Albert Einstein Str. 29a, D-18059 Restock, Germany.
Chimia (Aarau). 2011;65(4):214-8.
Formic acid, containing 4.4 wt% of hydrogen, is a non-toxic liquid at ambient temperature and therefore an ideal candidate as potential hydrogen storage material. Formic acid can be generated via catalytic hydrogenation of CO2 or bicarbonate in the presence of an amine with suitable ruthenium catalysts. In addition selective dehydrogenation of formic acid amine adducts can be carried out at ambient temperatures with either ruthenium phosphine catalyst systems as well as iron-based catalysts. In detail we obtained with the [RuCl2(benzene)]2/dppe catalyst system a remarkable TON of 260,000 at room temperature. Moreover applying Fe3(CO)12 together with tribenzylphosphine and 2,2':6',2"-terpyridine under visible light irradiation a TON of 1266 was obtained, which is the highest activity known to date for selective dehydrogenation of formic acid applying non-precious metal catalysts.
甲酸含氢量为4.4 wt%，在环境温度下是一种无毒液体，因此是潜在储氢材料的理想候选物。甲酸可通过在合适的钌催化剂存在下，使二氧化碳或碳酸氢盐与胺进行催化氢化反应生成。此外，甲酸胺加合物的选择性脱氢反应可在环境温度下，使用钌膦催化剂体系或铁基催化剂进行。具体而言，使用[RuCl2(苯)]2/二苯基膦催化剂体系，在室温下我们获得了高达260,000的显著吨摩尔数（TON）。此外，在可见光照射下，将Fe3(CO)12与三苄基膦和2,2':6',2"-三联吡啶一起使用，获得了1266的TON，这是迄今为止已知的使用非贵金属催化剂进行甲酸选择性脱氢反应的最高活性。
