Abstract
ABSTRACT
The accumulation of microplastic waste has raised growing environmental concerns, motivating the development of sustainable strategies for plastic‐to‐fuel conversion. Here, we report a platinum single‐atom catalyst anchored on distorted graphitic carbon nitride (Pt
1
/CN) for efficient photocatalytic microplastics photoreforming. Unlike conventional planar g‐C
3
N
4
models, the locally distorted heptazine framework introduces off‐plane coordination environments that enable unconstrained Pt─N coordination and promote electronic flexibility. X‐ray absorption spectroscopy reveals Pt─N coordination associated with distorted heptazine units, where distortion‐induced charge localization enhances interfacial electron transfer to Pt sites. In situ measurements under light irradiation further confirm efficient charge transfer at the Pt
1
/CN interface. Among various microplastics, polyethylene terephthalate (PET) exhibits the highest hydrogen evolution rate of 533.18 µmol·g
−1
·h
−1
, attributed to alkaline‐assisted ester bond cleavage. Density functional theory calculations demonstrate that Pt single atoms facilitate hydrogen evolution by lowering H
+
reaction barrier and stabilizing key intermediates. This work elucidates the structure–activity relationship of Pt
1
in polymeric semiconductors and establishes a framework‐level design strategy for electronic flexibility in photocatalytic plastic‐to‐fuel conversion.