Electrodes that have high desalting capacity, fast desalting rates and stable desalination performance are needed in capacitive deionization (CDI) technologies for water security. Herein, confined interfacial self-assembly of lignin-based graphene-like carbon (GC) precursors in Ti3C2-MXene interlayers was developed for forming GC/MXene composites. The formation of GC was generated in-situ by KHCO3-assisted pyrolytic carbonization which leads to exfoliation of multilayered MXene thereby forming GC/MXene heterostructures having strong interfacial interactions. GC/MXene exhibited tremella-like nanosheets morphology, accompanied by the formation of a TiO2 phase at the interface of GC and MXene hybridization, which confirmed formation of a heterostructure. Crystallographic phase identification of GC/MXene showed the exfoliation of MXene. GC/MXene had an ultra-negative surface charge of −39.3 mV, making it favorable for application as a cathode for Na+ removal. The GC/MXene heterostructure had high desalting capacity (54.2 mg g−1), high desalting rate (2.7 mg g−1 min−1), and stable cycling performance (90 % SAC retention after 30 cycles). The interfacial self-assembly strategy developed in this work is expected to enable green synthesis routes for graphene/MXene-based composite materials that allow construction of 2D/2D heterostructures for multilayer MXene and their analogues.
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