A model for the formation and stabilization of charged water clathrates is presented which accounts for observed anomalies in H+(H2O)nion distributions. These anomalies are observed in both ion cluster and neutral expansions and are consistent with the sizes expected for clathrate ions. That the same sizes are observed in both ion cluster and neutral expansions strongly suggests that a rapid ionic process is responsible for their formation. The proposed model is based on the high mobility and bonding effects of the rsquo;rsquo;excessrsquo;rsquo; proton in water. Computer simulations suggest that rsquo;rsquo;excessrsquo;rsquo; proton movement in a water clathrate would be suitable for stabilizing the clathrate structure as well as giving it access to a large number of nearly degenerate proton configurations. The formation of clathrates in charged water clusters of proper size can be ascribed to the following: rapid rsquo;rsquo;excessrsquo;rsquo; proton movement, a strong preference of the H3O+for a 3hyphen;coordinate bonding structure (which is compatible with hydrogen bonding), and finally, relatively slow processes leading to thermal disorder.
展开▼