Unveiling the role of Atomic-Level “Pump-Driven” effect in MoS2/MnO2 for facilitating directional charge transfer in hybrid capacitive deionization

In addressing the limitations imposed by the inherently low electronic conductivity and substantial ion transfer resistance of transition metal oxides (TMOs) in hybrid capacitive deionization (HCDI) applications, this study delineates a pioneering approach through the fabrication of a MoS2/MnO2 heterostructure, leveraging manganese dioxide (MnO2) as a model system. The investigation underscores the essentiality of constructing high-quality interfaces to act as conduits for directional charge flow, a critical but formidable challenge for enhancing desalination efficacy in electrode materials. By harnessing an atomistic “pump-driven” mechanism, the MoS2/MnO2 heterostructure demonstrably facilitates the promotion of desalination processes, underscored by the establishment of a potent local electric field (IEF) aimed at commanding charge dynamics. Empirical and computational analyses coalesce to unveil the preferential electron transfer from MoS2 to MnO2, a phenomenon precipitated by charge redistribution. This orchestrated charge flow not only augments electronic and ionic transfer efficiencies but also emboldens the MoS2/MnO2 heterostructure with enhanced desalination capabilities. The results show that MoS2/MnO2 demonstrates superior HCDI performance compared to MnO2 in a 500 mg L-1 NaCl solution at 1.2 V, with SRC of 33.21 mg g−1 and SRR of 1.50 mg g−1 min−1. The elucidation of this charge-guided dynamic, achieved through meticulous manipulation of the electronic microstructure and the IEF at the atomic scale, presents a novel paradigm for material science. This research presents an innovative approach for realizing robust charge-guided dynamics through the deliberate manipulation of the electronic microstructure and IEF of materials, employing an atomic-level “pump-driven” effect. This strategy opens new avenues for extending these principles to a broad array of advanced materials.