Photogeneration of singlet oxygen catalyzed by hexafluoroisopropanol for selective degradation of dyes
Jia Han,
Lei Wang,
Wenjin Cao,
Qinqin Yuan,
Xiaoguo Zhou,
Shilin Liu,
Xue-Bin Wang
Affiliations
Jia Han
Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China
Lei Wang
Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China
Wenjin Cao
Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA
Qinqin Yuan
Department of Chemistry, Anhui University, Hefei, Anhui 230601, P.R. China
Xiaoguo Zhou
Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China; Corresponding author
Shilin Liu
Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P.R. China
Xue-Bin Wang
Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA 99352, USA; Corresponding author
Summary: Singlet oxygen (1O2) shows great potential for selective degradation of dyes in environmental remediation of wastewater. In this study, we showcased that 1O2 can be effectively generated from an anion complex composed of deprotonated hexafluoroisopropanol anion ([HFIP-H]‒) with hydroperoxyl radical (⋅HO2) via ultraviolet (UV) photodetachment. Electronic structure calculations and cryogenic negative ion photoelectron spectroscopy unveil critical proton transfer upon complex formation and electron ejection, effectively photoconverting prevalent triplet ground state 3O2 to long-lived excited 1O2, stabilized by nearby HFIP. Inspired by this spectroscopic study, a novel “photogeneration” strategy is proposed to produce 1O2 with the incorporation of atmospheric O2 and HFIP, acting as a catalyst. Conceptually, the designed catalytic cycle upon UV irradiation and electron injection is able to achieve different degradations of dye molecules in a controllable fashion from decolorization to complete mineralization, shedding new light on potential water purification.
