Direct polyethylene photoreforming to high-energy-density
C2 fuels under mild conditions is of great significance
and
still faces a huge challenge, which is partly attributed to the extreme
instability of *CH2CH2 adsorbed on the traditional
catalysts with single catalytic sites. Herein, charge-asymmetrical
dual sites are designed to boost the adsorption of *CH2CH2 for direct polyethylene photoreforming into C2 fuels under normal temperature and pressure. As a prototype,
the synthetic Zr-doped CoFe2O4 quantum dots
with charge-asymmetrical dual metal sites realize direct polyethylene
photoreforming into acetic acid, with 100% selectivity of liquid fuel
and the evolution rate of 1.10 mmol g–1 h–1, outperforming those of most previously reported photocatalysts
under similar conditions. In situ X-ray photoelectron
spectra, density-functional-theory calculations, and control experiments
reveal the charge-asymmetrical Zr–Fe dual sites may act as
the predominate catalytic sites, which can simultaneously bond with
the *CH2CH2 intermediates for the following
stepwise oxidation to form C2 products.