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Currently, there is strong interest in carbon capture and absorption as a means of reducing carbon dioxide emissions and combating climate change. Unfortunately, the current and traditional methods to achieve such goals are not economical, because they require a huge absorption- desorption plant with high investment and operating costs and high recycle rates of chemical absorbers. In this paper, we propose a novel CO2 capture method combining dimethyl carbonate as a physical solvent and polydimethylsiloxane (PDMS)/TiO2 nanocomposite as a desorption membrane. The effects of TiO2 concentration, feed temperature, and permeate pressure on the pervaporation process for CO2 capture were studied. Results showed that the addition of TiO2 nanoparticles (up to 5 wt %) resulted in 3.61 kg/m(2).h flux and 44.68 selectivity of the membrane. The presence of TiO2 nanoparticles in the PDMS membrane not only increased the performance of membrane's but also reduced (about 72%) energy consumption. To corroborate our experimental findings, a simple simulation was conducted by Gaussian 09. The modeling results demonstrated that the incorporation of TiO2 nanoparticles to the PDMS led to favorable absorption of CO, compared with the composite one. These results indicate a novel and promising method to capture CO2 effectively and economically for industrial purposes.