Efficient charge separation remains a key challenge limiting the photocatalytic performance of metal–organic frameworks (MOFs). In a recent advance, Huang et al. developed an ultrathin 2D/2D MOF-based S-scheme heterojunction to overcome this limitation. By exfoliating Cu-TCPP and Cd-TBAPy MOFs into few-layer nanosheets and assembling them via pH-controlled electrostatic attraction, they formed an intimate face-to-face metal–organic layer (MOL) interface with a built-in electric field. A suite of characterizations confirmed an S-scheme band alignment that promotes directional charge transfer and maintains strong redox potentials. The optimized Cu/Cd-MOL achieved an H2 evolution rate of 1342 μmol h−1 g−1, whereas a Cu/Ni-MOL variant reached 2027 μmol h−1 g−1 with a 2.75% apparent quantum yield. This study provides a general strategy for constructing ultrathin MOF heterostructures with accelerated charge kinetics for efficient solar-to-hydrogen conversion.
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2026 The Author(s). EcoEnergy published by John Wiley & Sons Australia, Ltd on behalf of China Chemical Safety Association.