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Research Article

Probing reaction pathways for H2O-mediated HCHO photooxidation at room temperature

Weiwei Shao1,2,§, Xiaodong Li1,2,§, Xiaolong Zu1,2, Liang Liang1,2, Yang Pan1,2, Junfa Zhu1,2, Chengming Wang1,2, Yongfu Sun1,2( ), Yi Xie1,2( )
Hefei National Laboratory for Physical Sciences at Microscale, National Synchrotron Radiation Laboratory, Hefei Science Center of CAS, University of Science and Technology of China, Hefei 230026, China
Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China
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Abstract

Photooxidation provides a promising strategy for removing the dominant indoor pollutant of HCHO, while the underlying photooxidation mechanism is still unclear, especially the exact role of H2O molecules. Herein, we utilize in-situ spectral techniques to unveil the H2O-mediated HCHO photooxidation mechanism. As an example, the synthetic defective Bi2WO6 ultrathin sheets realize high-rate HCHO photooxidation with the assistance of H2O at room temperature. In-situ electron paramagnetic resonance spectroscopy demonstrates the existence of •OH radicals, possibly stemmed from H2O oxidation by the photoexcited holes. Synchrotron-radiation vacuum ultraviolet photoionization mass spectroscopy and H218O isotope-labeling experiment directly evidence the formed •OH radicals as the source of oxygen atoms, trigger HCHO photooxidation to produce CO2, while in-situ Fourier transform infrared spectroscopy discloses the HCOO* radical is the main photooxidation intermediate. Density-functional-theory calculations further reveal the •OH formation process is the rate-limiting step, strongly verifying the critical role of H2O in promoting HCHO photooxidation. This work first clearly uncovers the H2O-mediated HCHO photooxidation mechanism, holding promise for high-efficiency indoor HCHO removal at ambient conditions.

Keywords

room temperaturemechanistic studyH2O-mediatedHCHO photooxidation

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Nano Research
Volume 14 Issue 5,
May 2021
Pages 1471-1478
DOI: 10.1007/s12274-020-3205-y
Cite this article:
Shao W, Li X, Zu X, et al. Probing reaction pathways for H2O-mediated HCHO photooxidation at room temperature. Nano Research, 2021, 14(5): 1471-1478. https://doi.org/10.1007/s12274-020-3205-y
Topics:
Density functional theoryElectron spin resonance spectroscopyFourier transform infrared spectroscopyIndium compoundsMass spectrometryPhotocatalysis

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Received: 31 August 2020
Revised: 27 September 2020
Accepted: 15 October 2020
Published: 13 November 2020
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature
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