Janus Energy‐Mass Relay Architecture via High‐Entropy Catalysis for Non‐Equilibrium Solar Desalination

ABSTRACT To resolve the thermal‐mass mismatch bottleneck in solar‐driven interfacial evaporation, the study proposes a Janus interface energy‐mass relay integrating high‐entropy alloy oxide (HEAO) nanoparticles with a double‐network hydrogel. The hydrogel acts as an enthalpy modulator, pre‐activating bulk water and blocking conductive heat loss. The top HEAO layer serves as an entropy accelerator, leveraging its active sites and oxygen vacancies to rapidly shear the residual hydrogen bonds of pre‐activated water. In situ XPS and DFT analyses reveal that photo‐induced polarization at HEAO defects injects charge into water anti‐bonding orbitals, stretching the O─H bond to 1.209 Å. Consequently, the evaporator achieves an evaporation rate of 4.02 kg m −2 h −1 under one sun illumination. This work reveals the critical role of cascaded hydration editing in breaking the theoretical limits of interfacial phase transitions.