Unraveling Defect-Dependent Conductivity-Type Switching in CuFe2O4 for Enhanced Photoelectrocatalytic Reduction of Benzaldehyde
Yen-Chun Huang, Manoj Kumar Mohanta, Jun-Lin Fong, Abdul M. Reyes, Sebastian E. Reyes-Lillo, Chang-Ming Jiang
TL;DR
A defect-engineered CuFe2O4 photocathode enables efficient and sustainable benzaldehyde reduction under mild conditions using photoelectrocatalysis.
Contribution
A defect-tuned CuFe2O4 photocathode enables direct PEC reduction of benzaldehyde with high efficiency and low energy input.
Findings
Oxygen-rich annealing stabilizes copper vacancies and enhances hole concentration in CuFe2O4.
The optimized photocathode achieves a benzyl alcohol production rate of 2.57 μmol/h with 51.3% Faradaic efficiency.
The PEC method reduces the required applied potential by ~1 V compared to traditional electrocatalytic methods.
Abstract
Photoelectrocatalytic (PEC) reduction provides a sustainable route for upgrading biomass-derived feedstocks with reduced energy requirements, yet remains largely unexplored beyond hydrogen evolution and CO2 reduction due to the scarcity of stable photocathodes. Here, we report a defect-engineered CuFe2O4 photocathode that enables directly quantified PEC reduction of benzaldehyde to benzyl alcohol using a single-component, earth-abundant oxide. By controlling annealing temperature and oxygen partial pressure, CuFe2O4 is systematically tuned from n-type to p-type conductivity. Electrochemical measurements, X-ray and ultraviolet photoelectron spectroscopy, and first-principles defect calculations collectively show that oxygen-rich annealing conditions suppress deep donor-type oxygen vacancies while stabilizing shallow acceptor-type copper vacancies, resulting in enhanced hole concentration…
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Taxonomy
TopicsCO2 Reduction Techniques and Catalysts · Advanced Photocatalysis Techniques · Catalysis for Biomass Conversion