Ultralow loading of engineered palladium nanoclusters in polymeric membranes for high permeability hydrogen separation
摘要
Palladium (Pd) has exceptional H2 adsorption capacity and has been used as an adsorptive filler in mixed matrix membranes (MMMs) to enhance H2 separation performance. However, a high Pd loading (20 wt%–60 wt%) is impractical due to cost. In this study, highly dispersed Pd nanoclusters are confined within the channels of mesoporous silica nanoparticles (MSNs), largely improving Pd atom utilization for facilitating H2 transport while greatly reducing Pd loading content. MMMs prepared by mixing Pd@MSN with polybenzimidazole matrix, corresponding to a very low Pd loading of 0.6 wt%–3.0 wt%, exhibit much improved H2/CO2 separation performance. Specifically, an MMM containing only 2.5 wt% Pd shows mixed-gas separation performance of 302.6 barrer of H2 permeability and 16.3 of H2/CO2 selectivity at 120 °C, largely surpassing the latest 150 °C upper bound. Our work demonstrates the enormous potential for applying Pd-based MMMs in gas separation by reducing noble metal loading by nearly two orders of magnitude.