Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 14, Issue 1, Pages 654-667Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c17406
Keywords
bismuth oxychalcogenide; UV light; PFAS; coordination elements; photocarriers' internal access
Funding
- National Natural Science Foundation of China [22076092]
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This study investigated the bridging ability of bismuth oxychalcogenide for constructing an effective photocarrier pathway to PFOA, showing outstanding photocatalytic activity of Bi2O2Se with a broad pH adaptability. The results provide new insights for the development of Se-coordinated catalysts.
The destruction of perfluorooctanoic acid (PFOA) from outside was inhibited by the barrel spiral barrier, but the construction of the photocatalyst-PFOA complex provided a direct attack on photogenerated reactive species (RSs). Here, we investigated the bridging ability of bismuth oxychalcogenide (Bi2O2X) for constructing an effective photocarrier pathway to PFOA. The experimental results and DFT calculations showed that a more intense internal access of Bi2O2Se was built via the terminal carboxylate tail, and the weaker electrostatic interaction of Bi-Se bonds helped realize the smaller band gap and slower recombination of photocarriers, thereby inhibiting the invalid annihilation of holes with H2O and facilitating the transformation of electrons to O-2(-center dot). The pseudo-first-order rate coefficient (k(obs)) was 2 and 4 times higher than Bi2O2S and TiO2, respectively, showing the outstanding photocatalytic activity of Bi2O2Se. A broad pH (4-8) adaptability of Bi2O2 Se was observed for defluorination, especially in alkali condition. This new understanding may inspire the development of Se-coordinated catalysts.
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