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Double-ligand Fe, Ru catalysts: A novel route for enhanced H2 production from Formic Acid
International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2020-05-16 , DOI: 10.1016/j.ijhydene.2020.04.215
M. Solakidou , M. Theodorakopoulos , Y. Deligiannakis , M. Louloudi

Catalytic Ru- or Fe-complexes bearing two ligands L1, L2, where L1 = phosphine and L2 = Schiff-base ligand, present remarkable H2 production efficiency from Formic Acid (FA) than their single-ligand counterparts. The optimum L1RuL2 and L1FeL2 catalysts were obtained using a phosphine = P(CH2CH2PPh2)3 (or PP3) as L1 and a Schiff-base ligand (abbreviated Lγ herein) as L2, while the using of amino functionalized nanoparticle H2N@SiO2 as cocatalyst further promotes the H2 production efficiency. In long term stability experiments [RuPP3Lγ]/H2N@SiO2 and [FePP3Lγ]/H2N@SiO2 achieve a total TONs >17,367 and >29,372 respectively without deactivation. Thermodynamic and spectroscopic data reveal a common catalytic mechanism for both Fe and Ru based systems, involving synergism between L1, L2 in order to promote the rate-limiting steps. The present work is the first example of “double-ligand catalyst” concept as a novel route for high-efficiency, HCOOH dehydrogenation catalysts, which can be operative for either noble-metal or earth-abundant metals.



中文翻译:

双配体铁,钌催化剂:提高甲酸生产H 2的新途径

带有两个配体L1,L2(其中L1 =膦和L2 = Schiff碱配体)的催化Ru-或Fe复合物,与单配体相比,甲酸(FA)的H 2生产效率显着提高。使用膦= P(CH得到最佳L1RuL2和L1FeL2催化剂2 CH 2 P博士23(或PP 3)作为L1和席夫碱配体(简写大号γ本文中)为L2,而使用氨基的功能化的纳米颗粒H 2 N @ SiO 2作为助催化剂进一步提高了H 2的生产效率。在长期稳定性实验中[RuPP 3 Lγ ] / H 2 N - [的SiO 2和[FePP 3大号γ ] / H 2 N - [的SiO 2共实现吨> 17367和分别> 29372无失活。热力学和光谱数据揭示了基于Fe和Ru的系统的共同催化机理,涉及L1,L2之间的协同作用以促进限速步骤。目前的工作是“双配体催化剂”概念的第一个实例,它是高效的HCOOH脱氢催化剂的新颖途径,可用于贵金属或富稀土金属。

更新日期:2020-05-16
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