To avoid large energy input during crystallization from TBAB solutions, the solid TBAB hydrates were directly used for carbon capture in this work. The CO2 adsorption and release process of TBAB center dot 38H(2)O hydrate were measured by in situ Raman and macroscopic method. Results showed that TBAB center dot 38H(2)O hydrates converted to nCO(2)center dot TBAB center dot 38H(2)O hydrate with no significant structural change. TBAB center dot 38H(2)O hydrate had a relatively large CO2 storage capacity where 1 volume of hydrate could store 122 volumes of standard CO2 at 278 K, 2 MPa. Increasing pressure could greatly enhance the kinetics of CO2 adsorption and total CO2 storage. In the CO2 release process, nCO(2)center dot TBAB center dot 38H(2)O hydrate did not release all of the trapped CO2 molecules. Forty to seventy percent of the trapped CO2 could not be released within 600 min. The good stability of 5(12) cages was suggested to allow nCO(2)center dot TBAB center dot 38H(2)O hydrate to hold a certain amount of CO2 at atmospheric pressure. The slow diffusion of CO2 in hydrate phase was also thought to be the controlling step of CO2 release. Increasing the temperature and the specific surface area of hydrate particles would be helpful to strengthen the CO2 release.