Enhanced Photocatalytic CO2 Reduction Performance via Photothermal-Magnetic Synergistic Effects for Solar Fuel Production
ACS SUSTAINABLE CHEMISTRY & ENGINEERING(2024)
摘要
Photocatalytic CO2 reduction with naturally abundant H2O as the proton source has attracted widespread concern for its environmental and sustainable advantages. Nevertheless, the high recombination rate of photogenerated electron-hole pairs leads to unsatisfactory solar-to-chemical energy conversion efficiency. In this work, we proposed and validated a strategy that photothermal-magnetic synergistically promotes the separation of photogenerated carriers, as well as their transport, leading to boosted photocatalytic performance. A paramagnetic Z-scheme ZnFe2O4/TiO2 heterojunction was fabricated, and its performance in CO2 reduction was examined under concentrated full-spectrum light illumination with an applied external magnetic field. The built-in electric field of the Z-scheme heterojunction improved the dynamic properties of electron-hole pairs. At the same time, the thermal effect induced by infrared light played a crucial role in promoting CO2 conversion. Importantly, the applied external magnetic field further suppressed the recombination of charge carriers via Lorentz force, magnetoresistance, and spin-polarization effects. As a result, the assistance of a magnetic field significantly increased the yields of CO, CH4, and H-2 in comparison to the absence of a magnetic field, with maximum enhancements of 25.3, 29.6, and 62.9%, respectively. Moreover, the excessive heating due to the higher concentrated ratio may induce magnetic disorder within the material, potentially reducing the magnetic field's ability to facilitate carrier transport. The photothermal-magnetic synergy mechanism was systematically explored. Our work has presented a new approach in which photothermal-magnetic effects synergistically contribute to solar fuel production.
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关键词
photothermal catalysis,CO2 reduction,magnetic field,charge separation,solar fuels
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