Pd-N to Pd-O rearrangement for a carbamate synthesis from carbon dioxide and methane: a density functional and ab initio molecular dynamics metadynamics study.

Abstract

We investigated the key step of Pd-N to Pd-O rearrangement from a model catalytic cycle for the activation of carbon dioxide and methane with static quantum chemical calculations and metadynamics simulation. Our calculations show that different bottlenecks appear in the catalytic cycle but that the investigated rearrangement of the Pd-N to Pd-O bounded complex has a barrier ΔG(#)/ΔF(#) of approximately 20 kJ mol⁻¹ and is therefore accessible at ambient reaction conditions.

Cite this paper

@article{Dio2011PdNTP, title={Pd-N to Pd-O rearrangement for a carbamate synthesis from carbon dioxide and methane: a density functional and ab initio molecular dynamics metadynamics study.}, author={Philipp J. di Dio and Marc Br{\"{u}ssel and Kilian Mu{\~n}iz and Rupashree Shyama Ray and Stefan Zahn and Barbara Kirchner}, journal={Angewandte Chemie}, year={2011}, volume={50 37}, pages={A40-5} }