Carbon dioxide hydrogenation to formate catalyzed by highly active Ru-tris (pyrazolyl)methane complexes

被引：0

作者：

Kostera, Sylwia ^{[1
]}

Gobbo, Alberto ^{[2
]}

Guelfi, Massimo ^{[2
]}

Zacchini, Stefano ^{[3
]}

Manca, Gabriele ^{[1
]}

Marchetti, Fabio ^{[2
]}

Gonsalvi, Luca ^{[1
]}

机构：

[1] Ist Chim Composti Organometall ICCOM, Consiglio Nazl Ric CNR, Via Madonna Piano 10, I-50019 Florence, Italy

[2] Univ Pisa, Dept Chem & Ind Chem, Via G Moruzzi 13, I-56124 Pisa, Italy

[3] Univ Bologna, Dept Ind Chem Toso Montanari, Via P Gobetti 85, I-40129 Bologna, Italy

来源：

JOURNAL OF CATALYSIS | 2025年 / 450卷

关键词：

CO2; hydrogenation; Ruthenium complexes; Tris(pyrazolyl)methane; Homogeneous catalysis; Mechanistic studies; LOW-PRESSURE HYDROGENATION; DEFINED IRON CATALYST; CO2; HYDROGENATION; FORMIC-ACID; HOMOGENEOUS HYDROGENATION; REVERSIBLE HYDROGENATION; COORDINATION CHEMISTRY; METAL-COMPLEXES; RUTHENIUM; LIGANDS;

D O I：

10.1016/j.jcat.2025.116231

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

In the quest for novel, active ruthenium(II) complexes for homogeneous catalytic CO2 hydrogenation to formate, a small library of cationic Ru(kappa 3-tpm) complexes [tpm = tris(pyrazolyl)methane] bearing different ancillary ligands were tested under various reaction conditions, with and without the addition of a Lewis acid co-catalyst. Under optimized conditions (80 bar, 120 degrees C) and in the presence of LiOTf, TONs > 54000 were obtained in single batch runs with the complex [RuCl(kappa(3)-tpm)(PPh3)(CH3CN)]Cl (1). Mechanistic studies using NMR spectroscopy and DFT calculations were also carried out to elucidate key steps and the energies associated with the reaction pathway, which allowed for the proposal of a catalytic mechanism.

引用

页数：17

共 95 条

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