Graphene–carbon 2D heterostructures with hierarchically-porous P,N-doped layered architecture for capacitive deionization

Exploring a new-family of carbon-based desalinators to optimize their performances beyond the current commercial benchmark is of significance for the development of practically useful capacitive deionization (CDI) materials. Here, we have fabricated a hierarchically porous N,P-doped carbon-graphene 2D heterostructure (denoted NPC/rGO) by using metal-organic framework (MOF)-nanoparticle-driven assembly on graphene oxide (GO) nanosheets followed by stepwise pyrolysis and phosphorization procedures. The resulting NPC/rGO-based CDI desalinator exhibits ultrahigh deionization performance with a salt adsorption capacity of 39.34 mg g^-1 in a 1000 mg L^-1 NaCl solution at 1.2 V over 30 min with good cycling stability over 50 cycles. The excellent performance is attributed to the high specific surface area, high conductivity, favorable meso-/microporous structure together with nitrogen and phosphorus heteroatom co-doping, all of which are beneficial for the accommodation of ions and charge transport during the CDI process. More importantly, NPC/rGO exhibits a state-of-the-art CDI performance compared to the commercial benchmark and most of the previously reported carbon materials, highlighting the significance of the MOF nanoparticle-driven assembly strategy and graphene-carbon 2D heterostructures for CDI applications.