Computationally Designed 1,2,4-Triazolylidene-Derived N-Heterocyclic Olefins for CO Capture, Activation, and Storage.

In this article, triazolylidene-derived N-heterocyclic olefins (trNHOs) are designed using computational quantum tools, and their potential to promote CO sequestration is tested and discussed in detail. The low barrier heights related to the trNHO-mediated process indicate that the tailored compounds are very promising for fast CO sequestration. The systematic analysis of the presence of distinct substitutes at different N positions of the trNHO ring allows us to rationalize their effect on the carboxylation process and reveal the best N-substituted trNHO systems for CO sequestration and improved trNHO carboxylates for faster CO capture/release.