Influence of the Metal Ion on the Electrocatalytic Hydrogen Production by a Thiosemicarbazone Palladium Complex

被引：26

作者：

Straistari, Tatiana ^{[1
,2
]}

Hardre, Renaud ^{[1
]}

Massin, Julien ^{[1
]}

Attolini, Mireille ^{[1
]}

Faure, Bruno ^{[1
]}

Giorgi, Michel ^{[3
]}

Reglier, Marius ^{[1
]}

Orio, Maylis ^{[1
]}

机构：

[1] Aix Marseille Univ, CNRS, Cent Marseille, ISm2, Marseille, France

[2] Moldavian Acad Sci, Inst Chem, 3 Acad Str, MD-2028 Kishinev, Moldova

[3] Aix Marseille Univ, CNRS, Federat Chim, Spectropole, Marseille, France

来源：

EUROPEAN JOURNAL OF INORGANIC CHEMISTRY | 2018年 / 20-21期

关键词：

Palladium; Redox chemistry; Quantum chemistry; Electrocatalysis; Hydrogen evolution reaction; DENSITY-FUNCTIONAL THEORY; TRANSITION-METAL; CORRELATION-ENERGY; IRON HYDROGENASE; HARTREE-FOCK; BASIS-SETS; EVOLUTION; WATER; APPROXIMATION; REDUCTION;

D O I：

10.1002/ejic.201800120

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

We describe the synthesis and characterization of a new mononuclear palladium complex (PdL) based on a thiosemicarbazone ligand. X-ray diffraction data collected on single crystals reveal that the complex is a neutral mononuclear entity with symmetric square-planar geometry around the metal center. The complex exhibits an electrocatalytic behavior for proton reduction in DMF solvent using trifluoroacetic acid (TFA) as a proton source. Gas analysis under controlled electrocatalytic conditions during 4 h at a pool mercury working electrode showed a moderate production of dihydrogen. By combining experimental techniques to theoretical calculations, the results are analyzed and compared to those obtained for the previously reported NiL complex in an effort to rationalize the influence of the metal center on the catalytic performance of PdL to mediate hydrogen evolution.

引用

页码：2259 / 2266

页数：8

共 52 条

[1] The Trivalent Copper Complex of a Conjugated Bis-dithiocarbazate Schiff Base: Stabilization of Cu in Three Different Oxidation States [J].