Abstract
Highly permeable and selective membranes are crucial for energy-efficient gas separation. Two-dimensional (2D) graphitic carbon nitride (g-C(3)N(4)) has attracted significant attention due to its unique structural characteristics, including ultra-thin thickness, inherent surface porosity, and abundant amine groups. However, the interfacial defects caused by poor compatibility between g-C(3)N(4) and polymers deteriorate the separation performance of membrane materials. In this study, amino-functionalized g-C(3)N(4) nanosheets (CN@PEI) was prepared by a post-synthesis method, then blended with the polymer Pebax to fabricate Pebax/CN@PEI mixed matrix membranes (MMMs). Compared to g-C(3)N(4), MMMs with CN@PEI loading of 20 wt% as nanofiller exhibited a CO(2) permeance of 241 Barrer as well as the CO(2)/CH(4) and CO(2)/N(2) selectivity of 39.7 and 61.2, respectively, at the feed gas pressure of 2 bar, which approaches the 2008 Robeson upper bound and exceeded the 1991 Robeson upper bound. The Pebax/CN@PEI (20) membrane showed robust stability performance over 70 h continuous gas permeability testing, and no significant decline was observed. SEM characterization revealed a uniform dispersion of CN@PEI throughout the Pebax matrix, demonstrating excellent interfacial compatibility between the components. The increased free volume fraction, enhanced solubility, and higher diffusion coefficient demonstrated that the incorporation of CN@PEI nanosheets introduced more CO(2)-philic amino groups and disrupted the chain packing of the Pebax matrix, thereby creating additional diffusion channels and facilitating CO(2) transport.