Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 295, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120277
Keywords
Half-metal; Erythroid-like; Z-Scheme; Photocatalysis; CO2 conversion
Funding
- National Natural Science Foundation of China [51303083]
- National Natural Science Foundation of China for Excellent Young Scholars [51922050]
- Natural Science Foundation of Jiangsu Province [BK20191293, BK20201120]
- China Postdoctoral Science Foundation [2017m621708]
- Fundamental Research Funds for the Central Universities [30920021123]
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The study developed a hierarchical erythroid-like BiVO4/hm-C4N3 direct Z-Scheme heterojunction, achieving overall photocatalytic CO2 and H2O conversion to CO and O2 without any sacrificial reagent and co-catalyst. The optimized catalyst demonstrated high CO production rate and selectivity.
Photocatalytic overall CO2 and H2O conversion has been very challenging. Herein, a hierarchical erythroid-like BiVO4/hm-C4N3 direct Z-Scheme heterojunction is developed through elaborate template inducement and in-situ polymerization. The superior CO2 capture, activation and charge deliver features are all integrated in reduction site of the Z-Scheme system. The overall photocatalytic CO2 and H2O conversion to CO and O2 are achieved without any sacrificial reagent and co-catalyst. In particular, the optimized BiVO4/hm-C4N3 presents a CO production rate of 40.8 mu mol g-1 h-1 with a selectivity beyond 97 %. DFT calculation and in-situ DRIFTS spectra indicate that the dehydration of *COOH to CO is the rate-determining step. The supplement of proton by H2O oxidation from BiVO4 and the prolonged lifetime of electrons simultaneously contribute to the remarkable decreased reaction barrier. This work provides a new strategy to develop organic half-metal based photocatalyst, and may pave a new way to the target of artificial photosynthesis.
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