Chemical instability of graphene oxide following exposure to highly reactive radicals in advanced oxidation processes

The rapidly increasing and widespread use of graphene oxide (GO) as catalyst supports, requires further understanding of its chemical stability in advanced oxidation processes (AOPs). In this study, UV/H₂O₂ and UV/persulfate (UV/PS) processes were selected to test the chemical instability of GO in terms of their performance in producing highly reactive hydroxyl radicals (^[rad]OH) and sulfate radicals (SO₄^[rad]−), respectively. The degradation intermediates were characterized using UV–visible absorption spectra (UV–vis), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), Raman spectroscopy, and matrix-assisted laser desorption and ionization time-of-flight mass spectrometry (MALDI-TOF-MS). Experimental data indicate that UV/PS process was more effective in enhancing GO degradation than the UV/H₂O₂ system. The overall oxygen-containing functionalities (e.g. C–O, C[dbnd]O and O–C[dbnd]O groups) dramatically declined. After radical attack, sheet-like GO was destructed into lots of flakes and some low-molecular-weight molecules were detected. The results suggest GO is most vulnerable against SO₄^[rad]− radical attack, which deserves special attention while GO acts as a catalyst support or even as a catalyst itself. Therefore, stability of GO and its derivatives should be carefully assessed before they are applied to SO₄^[rad]−-based AOPs.