1. Efficient singlet oxygen nanogenerator with low-spin iron for selective contaminant decontamination.
- Author
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Jiang, Jingjing, Niu, Shu, Liu, Shengda, Zhang, Hao, Liu, Yansong, Sun, Tongze, Shi, Donglong, Zhao, Bowen, Yan, Ge, Huo, Mingxin, Zhou, Dandan, and Dong, Shuangshi
- Subjects
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REACTIVE oxygen species , *IRON , *CARBON content of water , *WATER purification , *DECONTAMINATION (From gases, chemicals, etc.) , *WASTEWATER treatment , *IONIZATION energy - Abstract
[Display omitted] • Efficient 1O 2 nanogenerator was precisely constructed by regulating Fe spin state. • Low spin-state Fe induced nonradical conversion from H 2 O 2 to 1O 2. • The 1O 2 -dominated system selectively removed low ionization potential contaminants. • Stable Fh/BiOI transformed high-toxic contaminant into low-toxic products. • Fh/BiOI exhibited excellent mineralization performance towards secondary effluent. The hydrogen peroxide (H 2 O 2)-based photo-Fenton-like was a promising technology for the generation of singlet oxygen (1O 2), which was highly desirable in water purification. However, the yield of 1O 2 in traditional radical system was low due to the radical competition. Targeted construction of the non-radical system could solve the above issue, but it has been a challenge. In this study, we targetedly regulated the Fe spin state to efficiently generate 1O 2 in a nonradical path. The experimental and theoretical results demonstrated that low-spin FeIII enhanced H 2 O 2 adsorption, directly extracted electrons from H 2 O 2 to Fe center, and rapidly cleaved O–H bond to accelerate the recombination of *OOH with H 2 O 2 for efficient 1O 2 generation. This unique nonradical process differed obviously from the traditional radical pathway for 1O 2 generation. The developed 1O 2 -dominant 50Fh/BiOI/H 2 O 2 /vis system degraded 98.4% of TCH, which was higher than that in •OH-dominant Fh/H 2 O 2 /vis system (84.2%) and it had excellent resistance to various substances, including inorganic ions, dissolved organic matter and real water matrix (tap water and secondary effluent). This study enhanced our understanding of spin-state-dependent photo-Fenton-like reaction and inspired the targeted development of a new-generation selective wastewater treatment technology. [ABSTRACT FROM AUTHOR]
- Published
- 2023
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