4.6 Article

Bismuth single atom supported CeO2 nanosheets for oxidation resistant photothermal reverse water gas shift reaction

期刊

CATALYSIS SCIENCE & TECHNOLOGY
卷 12, 期 18, 页码 5559-5564

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00771a

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资金

  1. Hebei Natural Science Foundation [B2022201090, B2021201074, B2021201034]
  2. Hebei Provincial Department of Science and Technology [216Z4303G]
  3. Hebei Education Department [BJ2019016, QN2022059]
  4. Hebei University [521100311, DXK202109]
  5. State Key Laboratory of Catalysis in DICP [N-21-05]
  6. Advanced Talents Incubation Program of Hebei University [521000981248, 521000981377, 8012605]
  7. Scientific Research Foundation of Hebei Agricultural University [YJ201939]

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This study synthesized Bi single atoms supported by CeO2 nanosheets using the soft template method, and achieved high activity and oxidation resistance for photothermal reverse water gas shift reaction (RWGS). Experimental and calculation results showed that the Bi single atoms maintained their +3 valence state and had a low energy barrier for RWGS, leading to high activity and oxidation resistance. The addition of BiOx/CeO2 catalyst in a photothermal system significantly increased the CO generation rate, and there was no inactivation during intermittent air oxidation, which is crucial for the industrialization of photothermal RWGS.
Photothermal reverse water gas shift reaction (RWGS) is one of the most essential green technologies for CO2 utilization. However, the intermittent photothermal RWGS makes all catalysts inactive due to air oxidation. Therefore, investigating new catalysts with high activity and oxidation resistance simultaneously is imperative for the industrialization of photothermal RWGS, which has not yet been realized. Here, Bi single atoms supported by CeO2 nanosheets are synthesized via the soft template method, which showed high activity and stability for RWGS under air corrosion at 400 degrees C, revealing unprecedented oxidation resistance. Experiments and first principles calculation confirm that the Bi single atoms kept their +3 valence state during RWGS and have a low energy barrier for RWGS, thus leading to high activity and oxidation resistance for RWGS. When loading BiOx/CeO2 in a Ti2O3 based photothermal system, a CO generation rate of 31.00 mmol g(-1) h(-1) was achieved under 3 sun units of irradiation, 4 times higher than the state of the art of solar driven RWGS under 20 sun units of irradiation. Moreover, there is still no inactivation of BiOx/CeO2 in intermittent air oxidation, which can directly promote the industrialization of photothermal RWGS.

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