High ion selectivity and permeability, as two contradictory aspects for the membrane design, highly hamper the development of osmotic energy harvesting technologies. Metal–organic frameworks (MOFs) with ultra‐small and high‐density pores and functional surface groups show great promise in tackling these problems. Here, we propose a facile and mild cathodic deposition method to directly prepare crack‐free porphyrin MOF membranes on a porous anodic aluminum oxide for osmotic energy harvesting. The abundant carboxyl groups of the functionalized porphyrin ligands together with the nanoporous structure endows the MOF membrane with high cation selectivity and ion permeability, thus a large output power density of 6.26 W m−2 is achieved. The photoactive porphyrin ligands further lead to an improvement of the power density to 7.74 W m−2 upon light irradiation. This work provides a promising strategy for the design of high‐performance osmotic energy harvesting systems.

Biological ion pumps with two separate gates can actively transport ions against the concentration gradient. Developing an artificial nanofluidic device with multiple responsive sites is of great importance to improve its controllability over ion transport to further explore its logic function and mimic the biological process. Here, we propose an electrochemical polymerization method to fabricate electrochemically switchable doublegate nanofluidic devices. The ion transport of the double-gate nanofluidic device can be in situ and reversibly switched among four different states. The logic function of this nanofluidic device is systematically investigated by assuming the gate state as the input and the transmembrane ionic conductance as the output. A biomimetic electrochemical ion pump is then established by alternately applying two different specific logic combinations, realizing an active ion transport under a concentration gradient. This work would inspire further studies to construct complex logical networks and explore bioinspired ion pump systems.

High ion selectivity and permeability, as two contradictory aspects for the membrane design, highly hamper the development of osmotic energy harvesting technologies. Metal-organic frameworks (MOFs) with ultra-small and high-density pores and functional surface groups show great promise in tackling these problems.Here, we propose a facile and mild cathodic deposition method to directly prepare crack-free porphyrin MOF membranes on a porous anodic aluminum oxide for osmotic energy harvesting. The abundant carboxyl groups of the functionalized porphyrin ligands together with the nanoporous structure endows the MOF membrane with high cation selectivity and ion permeability, thus a large output power density of 6.26 W m À 2 is achieved. The photoactive porphyrin ligands further lead to an improvement of the power density to 7.74 W m À 2 upon light irradiation. This work provides a promising strategy for the design of high-performance osmotic energy harvesting systems.

The unique ion-transport properties in nanoconfined pores enable nanofluidic devices with great potential in harvesting osmotic energy. The energy conversion performance could be significantly improved by the precise regulation of the “permeability–selectivity” trade-off and the ion concentration polarization effect. Here, we take the advantage of electrodeposition technique to fabricate a Janus metal–organic framework (J-MOF) membrane that possesses rapid ion-transport capability and impeccable ion selectivity. The asymmetric structure and asymmetric surface charge distribution of the J-MOF device can suppress the ion concentration polarization effect and enhance the ion charge separation, exhibiting an improved energy harvesting performance. An output power density of 3.44 W/m2 has been achieved with the J-MOF membrane at a 1000-fold concentration gradient. This work provides a new strategy for fabricating high-performance energy-harvesting devices.

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