A DFT Study on the Co-polymerization of CO2 and Ethylene: Feasibility Analysis for the Direct Synthesis of Polyethylene Esters.
The co-polymerization of CO2 with the non-polar monomer ethylene, though highly desirable, still presents a challenge whereas the palladium-catalyzed CO/C2 H4 co-polymerization is well understood. Building on this analogy, the goal of this study was to elucidate the feasibility of developing suitable catalysts for co-polymerizing CO2 with ethylene to polyethylene esters. Computational methods based on density functional theory were hereby employed. In the search for new catalyst lead structures, a closed catalytic cycle was identified for the palladium-catalyzed CO2 /C2 H4 co-polymerization reaction. The computational study on palladium complexes with a substituted anionic 2-[bis(2,4-dimethoxyphenyl)-phosphine]-benzene-2-hydroxo ligand revealed key aspects that need to be considered when designing ligand sets for potential catalysts for the non-alternating co-polymerization of CO2 and ethylene.
CAT Catalytic Center, RWTH Aachen University, Worringerweg 2, 52074, Aachen, Germany.|Lehrstuhl für Technische Chemie und Petrolchemie, Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, 52074, Aachen, Germany.
Verena
V
Moha
CAT Catalytic Center, RWTH Aachen University, Worringerweg 2, 52074, Aachen, Germany.
Daniela
D
Cozzula
Lehrstuhl für Technische Chemie und Petrolchemie, Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, 52074, Aachen, Germany. hoelscher@itmc.rwth-aachen.de.
Markus
M
Hölscher
Lehrstuhl für Technische Chemie und Petrolchemie, Institut für Technische und Makromolekulare Chemie, RWTH Aachen University, Worringerweg 1, 52074, Aachen, Germany.
Walter
W
Leitner
CAT Catalytic Center, RWTH Aachen University, Worringerweg 2, 52074, Aachen, Germany. thomas.mueller@catalyticcenter.rwth-aachen.de.
Thomas E
0000-0002-9126-7653
TE
Müller
D002248:Carbon Monoxide / Q000737:chemistry; D002384:Catalysis; D060326:Chemistry Techniques, Synthetic; D004952:Esters / Q000737:chemistry*; D005030:Ethylenes / Q000737:chemistry*; D005240:Feasibility Studies; D008958:Models, Molecular; D008968:Molecular Conformation; D010165:Palladium / Q000737:chemistry; D020959:Polyethylene / Q000138:chemical synthesis* / Q000737:chemistry*; D058105:Polymerization; D011789:Quantum Theory
D004952:Esters; D005030:Ethylenes; D010165:Palladium; D002248:Carbon Monoxide; D020959:Polyethylene; C036216:ethylene
carbon dioxide; density functional theory; energy profile; palladium catalysis; polyesters