Formation of metallacarboxylic acids through Hieber base reaction. A density functional theory study

被引：1

作者：

Ahmad, Shahbaz ^{[1
]}

Berry, Elisabeth A. ^{[1
]}

Boyle, Conor H. ^{[1
]}

Hudson, Christopher G. ^{[1
]}

Ireland, Oliver W. ^{[1
]}

Thompson, Emily A. ^{[1
]}

Buhl, Michael ^{[1
]}

机构：

[1] Univ St Andrews, Sch Chem, St Andrews KY16 9ST, Fife, Scotland

来源：

JOURNAL OF MOLECULAR MODELING | 2019年 / 25卷 / 02期

关键词：

Homogeneous catalysis; Water gas shift reaction; Hieber base reaction; Density functional theory; GAS-SHIFT REACTION; HYDROGEN-PRODUCTION; HOMOGENEOUS CATALYSIS; RUTHENIUM CARBONYL; AB-INITIO; MECHANISMS; COMPLEXES; ENERGY; IRON; APPROXIMATION;

D O I：

10.1007/s00894-018-3915-1

中图分类号：

Q5 [生物化学]; Q7 [分子生物学];

学科分类号：

071010 ; 081704 ;

摘要：

Using density functional theory (B97-D/ECP2/PCM//RI-BP86/ECP1 level), we have studied the effects of ligand variation on OH- uptake by transition-metal carbonyls (Hieber base reaction), i.e., LnM(CO)+OH-[LnM(CO2H)](-), M=Fe, Ru, Os, L=CO, PMe3, PF3, py, bipy, Cl, H. The viability of this step depends notably on the nature of the co-ligands, and a large span of driving forces is predicted, ranging from G=-144kJ/mol to +122kJ/mol. Based on evaluation of atomic charges from natural population analysis, it is the ability of the co-ligands to delocalize the additional negative charge (through their -acidity) that is the key factor affecting the driving force for OH- uptake. Implications for the design of new catalysts for water gas shift reaction are discussed.

引用

页数：8

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