Bioinspired Bifunctional MOF Synergizing Superhydrophobicity‐Photothermal Adsorption via Narrow‐Bandgap Engineering for On‐Demand Oil Remediation

The design of dual-mode remediation platforms using flexible metal-organic frameworks (MOFs) to synergize superhydrophobicity and broadband photothermal activity remains a fundamental challenge for programmable solar-driven oil/water separation in spill remediation. A cactus-inspired nanoneedle-architected CuTCNQ MOF (TCNQ = tetracyanoquinodimethane) is developed through bandgap engineering and self-assembly, synergizing intrinsic superhydrophobicity with a narrow bandgap (E_g = 0.36 eV). The passive CuTCNQ@CM membrane achieves gravity-driven oil/water separation (99.53 ± 0.29% efficiency, 84.22 ± 3.82 kL·m^-2·h^-1 flux), retaining 98.26% performance after 20 cyclic separation tests, where ultralong 1D nanostructures amplify surface roughness and capillary forces through synergistic wettability enhancement and separation kinetics optimization. In parallel, the active CuTCNQ@PU system exhibits 98.96% broadband solar absorption (200-2500 nm) and a high solar-thermal conversion efficiency (STCE) of 93.64%, rapidly heating to 90.6 °C under 1-sun irradiation to reduce crude oil viscosity by 98.93%, enabling ultrafast adsorption (84.1 ± 2.3 g·g^-1 capacity, 436.7 ± 23.5 g·g^-1·min^-1 rate). The design pioneers dual-mode superhydrophobicity-bandgap MOFs by unifying passive/active functionalities through nanostructuring. The scalable synthesis, combined with sunlight-triggered adsorption, delivers an uninterrupted remediation platform-passively treating bulk spills and actively addressing viscous residues via light-controlled synergy, advancing energy-efficient environmental technologies.