Harnessing Ionic Power from Equilibrium Electrolyte Solution via Photoinduced Active Ion Transport through van‐der‐Waals‐Like Heterostructures

Abstract Nanofluidic ion transport through van der Waals heterostructures, composed of two or more types of reconstructed 2D nanomaterials, gives rise to fascinating opportunities for light‐energy harvesting, due to coupling between the optoelectronic properties of the layered constituents and ion transport in between the atomic layers. Here, a photoinduced active ion transport phenomenon through transition metal dichalcogenides (TMDs)‐based van‐der‐Waals‐like multilayer heterostructures is reported for harnessing ionic power from equilibrium electrolyte solution. The binary heterostructure comprises sequentially stacked 2D‐WS₂ and 2D‐MoS₂ multilayers with sub‐1 nm interlayer spacing. Upon visible‐light illumination, a net ionic flow is initiated through the Janus membrane, suggesting a directional cationic transport from WS₂ to MoS₂ part. The transport mechanism is explained in terms of a photovoltaic effect due to type II band alignment of WS₂/MoS₂ heterostructures. The driving mechanism can be generally applied to a variety of heterogeneous TMD membranes with type II semiconductor heterojunctions. In equilibrium ionic solutions, the maximum ionic photoresponse approaches ≈21 µA cm^–2 and ≈45 mV under one sun equivalent excitation. Under optimized conditions, the harvested power density reaches 2 mW m^–2. The proof‐of‐concept demonstration of photonic‐to‐ionic power generation within angstrom‐scale confinement anticipates potential for light‐controlled ionic circuits, artificial photosynthesis, and biomimetic energy conversion.