Catalytic Hydrogenation of CO2 by Manganese Complexes: Role of π-Acceptor Ligands

被引：42

作者：

Rawat, Kuber Singh ^{[1
]}

Mahata, Arup ^{[1
]}

Choudhuri, Indrani ^{[1
]}

Pathak, Biswarup ^{[1
,2
]}

机构：

[1] Indian Inst Technol IIT Indore, Discipline Chem, Indore 453552, Madhya Pradesh, India

[2] Indian Inst Technol IIT Indore, Discipline Met Engn & Mat Sci, Indore 453552, Madhya Pradesh, India

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2016年 / 120卷 / 30期

关键词：

DENSITY-FUNCTIONAL THERMOCHEMISTRY; CARBON-DIOXIDE HYDROGENATION; LOW-PRESSURE HYDROGENATION; MOLECULAR-ORBITAL METHODS; DEFINED IRON CATALYST; FORMIC-ACID; RUTHENIUM(II)-CATALYZED HYDROGENATION; HETEROLYTIC CLEAVAGE; COMPUTATIONAL DESIGN; MECHANISTIC INSIGHT;

D O I：

10.1021/acs.jpcc.6b05065

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：

We have carried out computational studies on the CO2 hydrogenation reaction catalyzed by three different Mn-based complexes (Mn1, Mn2, and Mn3) to understand the role of sigma-donor (PMe3) and pi-acceptor (CO) character of the ligands. Further, the role of a different set of sigma-donor and pi-acceptor ligands is studied as the studied CO (pi-acceptor and PMe3 (sigma-donor) ligands have the differences not only in electronic properties but also in steric effects. Here, we find that the sigma-donor ligands (PMe3/PH3) favor the hydride transfer, whereas the pi-acceptor ligands (CO/PF3) favor the heterolytic H-2-cleavege. The energy profile diagram shows that the hydride transfer is the rate-determining step when the CO2 hydrogenation reaction is catalyzed by a Mn-complex containing sigma-donor (PMe3/PH3) and pi-acceptor (CO/PF3) ligands.

引用

页码：16478 / 16488

页数：11

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