Abstract

A new generation of "molecular basket" sorbents (MBS) has been developed by the optimum combination of the nanoporous material and CO2/H2S-philic polymer sorbent to increase the accessible sorption sites for CO2 capture from flue gas (Postdecarbonization), and for CO2 and H2S separation from the reduced gases, such as synthesis gas, reformate (Predecarbonization), natural gas, coal/biomass gasification gas, and biogas. The sorption capacity of 140 mg of CO2/g of sorb was achieved at 15 kPa CO2 partial pressure, which shows superior performance in comparison with other known sorbents. In addition, an exceptional dependence of MBS sorption performance on temperature for CO2 and H2S was found and discussed at a molecular level via the computational chemistry approach. On the basis of the fundamental understanding of MBS sorption characteristics, an innovative sorption process was proposed and demonstrated at the laboratory scale for removing and recovering CO2 and H2S, respectively, from a model gas. The present study provides a new approach for development of the novel CO2/H2S sorbents and may have a major impact on the advance of science and technology for CO2/H2S capture and separation from various gases.