Knörr Pascal, Lentz Nicolas, Albrecht Martin
Department of Chemistry, Biochemistry & Pharmaceutical Sciences, University of Bern Freiestrasse 3 3012 Bern Switzerland
Catal Sci Technol. 2023 Jul 17;13(19):5625-5631. doi: 10.1039/d3cy00512g. eCollection 2023 Oct 2.
A new ruthenium complex containing a pyridylidene amine-based NNN ligand was developed as a catalyst precursor for formic acid dehydrogenation, which, as a rare example, does not require basic additives to display high activity (TOF ∼10 000 h). Conveniently, the complex is air-stable, but sensitive to light. Mechanistic investigations using UV-vis and NMR spectroscopic monitoring correlated with gas evolution profiles indicate rapid and reversible protonation of the central nitrogen of the NNN ligand as key step of catalyst activation, followed by an associative step for formic acid dehydrogenation.
一种含有基于亚胺吡啶胺的NNN配体的新型钌配合物被开发为甲酸脱氢的催化剂前体，这是一个罕见的例子，即不需要碱性添加剂就能表现出高活性（TOF ∼10 000 h⁻¹）。方便的是，该配合物在空气中稳定，但对光敏感。使用紫外可见光谱和核磁共振光谱监测并与气体释放曲线相关联的机理研究表明，NNN配体中心氮的快速可逆质子化是催化剂活化的关键步骤，随后是甲酸脱氢的缔合步骤。
