Journal
ADVANCED ENERGY MATERIALS
Volume 11, Issue 12, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202002783
Keywords
Fe‐ based catalysts; layered double hydroxide; photothermal catalysis; value‐ added hydrocarbons
Categories
Funding
- National Key Projects for Fundamental Research and Development of China [2018YFB1502002, 2017YFA0206904, 2017YFA0206900]
- National Natural Science Foundation of China [51825205, 51772305, 21871279, 21802154, 21902168]
- Beijing Natural Science Foundation [2191002, 2182078, 2194089]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Royal Society-Newton Advanced Fellowship [NA170422]
- International Partnership Program of Chinese Academy of Sciences [GJHZ1819, GJHZ201974]
- Central China Normal University [2019YBZZ025, 6300-30101202001]
- K. C. Wong Education Foundation
- Youth Innovation Promotion Association of the Chinese Academy of Sciences
- Energy Education Trust of New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology
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A series of novel Fe-based catalysts with different chemical compositions were successfully fabricated through hydrogen reduction, with Fe-500 exhibiting outstanding activity for CO2 photothermal conversion under UV-Vis irradiation. The density functional theory calculations improved the C-C coupling ability, enhancing the selectivity to C2+ products.
The solar-driven conversion of CO2 into carbon-based fuels and other valuable chemical feedstocks is actively being pursued as an approach for curbing greenhouse gas emissions. Herein, a series of novel Fe-based catalysts with different chemical compositions are successfully fabricated through the hydrogen reduction of MgFeAl-layered double hydroxide nanosheets at temperatures from 300 to 700 degrees C. The catalysts obtained are denoted herein as Fe-x, where x is the reduction temperature in celsius. Fe-500 offers outstanding activity for the photothermal conversion of CO2 to C2+ hydrocarbons under ultraviolet-visible (UV-Vis) irradiation (CO2 conversion 50.1%, C2+ selectivity 52.9%). Characterization studies using X-ray diffraction, extended X-ray absorption fine structure, Mossbauer spectroscopy, and high-resolution transmission electron microscopy determine that the Fe-500 catalyst is comprised of Fe and FeOx nanoparticles on a MgO-Al2O3 mixed metal oxide support. Density functional theory calculations establish that heterostructures consisting of partially oxidized metallic Fe nanoparticles improve the C-C coupling ability of CO2 hydrogenation intermediates, thus enhancing the selectivity to C2+ products. This work introduces a novel photothermal hydrogenation strategy for converting CO2 into valuable chemicals and also opens new avenues toward the development of related solar energy utilization schemes.
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