A theoretical study is presented on the CO2 activation. From quantum chemical point of view, in what extent and how we can understand and evaluate the level of activation of this molecule is studied. We propose a way to characterize the activation order of magnitude, providing an index. Taking the state of CO2 molecule in dilute gas phase or in vacuum as a reference state, the activated states in electronic structure (wave functions) as well as in geometrical change are described by measuring the degree of modifications relative to the reference state.The DFT calculations are performed to visualize this degree of activation as a function of the environmental effect on CO2; gas phase, liquid phase (especially as a function of pH), and coordination on transition metals. To rationalize thus defined theoretical evaluation method, we compared the calculated indexes with various spectroscopic data such as IR, UV absorption, and NMR.Then we applied the theoretical evaluation method of the CO2 activation degree to understand experimental reactions, especially on our CO2 reduction (1). Typical demonstration of this study has been presented by the reduction in hydrothermal condition with bulk transition metals. In this situation neither precious metals nor sophisticated transition metal complexes are used, nevertheless a considerably high efficiency (more than 60%) of conversion to useful organic compounds is obtained. We believe this theoretical characterization to measure the magnitude of the CO2 activation provides an insight for further design of experimental processes.

Activation of the CO<sub>2</sub> molecules, a theoretical study

246th National Meeting (2013)

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Activation of the CO2 molecules, a theoretical study

Activation of the CO₂ molecules, a theoretical study