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Delocalization Effect Promoted the Indoor Air Purification via Directly Unlocking the Ring-Opening Pathway of Toluene

  • Wenqiang Qu
    Wenqiang Qu
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    More by Wenqiang Qu
  • Penglu Wang
    Penglu Wang
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    More by Penglu Wang
  • Min Gao
    Min Gao
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
    More by Min Gao
  • Jun-ya Hasegawa
    Jun-ya Hasegawa
    Institute for Catalysis, Hokkaido University, Sapporo, Hokkaido 001-0021, Japan
  • Zhi Shen
    Zhi Shen
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    More by Zhi Shen
  • Qing Wang
    Qing Wang
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    More by Qing Wang
  • Ruomei Li
    Ruomei Li
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    More by Ruomei Li
  • , and 
  • Dengsong Zhang*
    Dengsong Zhang
    International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, People’s Republic of China
    *Telephone: +86-21-66137152. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2020, 54, 15, 9693–9701
Publication Date (Web):June 29, 2020
https://doi.org/10.1021/acs.est.0c02906
Copyright © 2020 American Chemical Society
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Abstract

The ring-opening process was generally considered as the rate-determining step for aromatic volatile organic compound photocatalytic degradation. A sophisticated and intensive degradation pathway is critical to the poor removal efficiency and low mineralization. In the present contribution, we successfully tailored and identified the ring-opening pathway of toluene elimination by electron delocalization in a borocarbonitride photocatalyst. By means of modulation of the dopant coordination configuration and electron geometry in the catalyst, the lone electrons of carbon transform into delocalized counterparts, sequentially elevating the interaction between the toluene molecules and photocatalyst. The aromatic ring of toluene can be attacked directly in the effect of electron delocalization without engendering additional intermediate species, significantly facilitating the removal and mineralization of toluene. This unprecedented route-control strategy alters the aromatic-ring-based reaction behavior from toluene to CO2 and paves a way to purify the refractory pollutants from the top design.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.0c02906.

  • Characterization, DFT calculations, O2-TPD, photoelectrochemical measurements, EPR experiment, XRD patterns of samples (Figures S1 and S6), TEM and HRTEM images of BCN and BCN-C (Figures S2–S5 and S19), TG–MS signals of the gaseous components (Figure S7), XPS spectra of BCN and BCN-C (Figure S8), EPR spectra samples with different carbon contents (Figure S9), schematic illustration of the carbon-doping process (Figure S10), optical images (Figure S11), transient photocurrent response (Figure S12), valence-band XPS spectra (Figure S13), Mott–Schottky plots (Figure S14), chemical kinetic constant (Figure S15), N2 adsorption–desorption isotherms and BET surface area data (Figure S18), toluene-TPD–MS profiles (Figure S20), oxygen-TPD profiles (Figure S21), EPR spectra of DMPO–O2 (Figure S22), in situ DRIFTS spectra (Figures S23–S25), GC–MS profiles of toluene degradation (Figures S26 and S27) over BCN and BCN-C, gas toluene oxidation behavior of BCN-C and BCN with different carbon contents (Figure S16), degradation performance of BCN-C and C3N4 toward gas toluene (Figure S17), degradation performance of gas benzene (Figure S28) on BCN-C and BCN, atom percentage (Table S1), detailed bond information (Tables S2–S4) of BCN and BCN-C, recent works reported for photocatalytic degradation toward toluene (Table S5), and assigned species of corresponding bands for in situ DRIFTS spectra (Table S6) (PDF)

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