Experimental evidence for the influence of charge on the adsorption capacity of carbon dioxide on charged fullerenes

Abstract

We show, with both experiment and theory, that adsorption of $C{O}_2$ is sensitive to charge on a capturing model carbonaceous surface. In the experiment we dope superfluid helium droplets with $C_{60}$ and $C{O}_2$ and expose them to ionising free electrons. Both positively and negatively charged $C_{60}(C{O}_2{)}_n^{+/-}$ cluster ion distributions are observed with a high-resolution mass spectrometer and these show remarkable and reproducible anomalies in intensities that are strongly dependent on the charge. The highest adsorption capacity is seen with $C_{60}^{+}$. Complementary density functional theory calculations and molecular dynamics simulations provided insight into the nature of the interaction of charged $C_{60}$ with $C{O}_2$ as well as trends in the packing of $C_{60}^{+}$ and $C_{60}^{-}$. The quadrupole moment of $C{O}_2$ itself was seen to be decisive in determining the charge dependence of the observed adsorption features. Our findings are expected to apply to adsorption of $C{O}_2$ by charged surfaces in general.

References in corpus (1)

• Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory