The effect of basic pH and carbonate ion on the mechanism of photocatalytic destruction of cylindrospermopsin
Abstract
This study investigated the mechanistic effects of basic pH and the presence of high carbonate concentration on the TiO2 photocatalytic degradation of the cyanobacterial toxin cylindrospermopsin (CYN). High-performance liquid chromatography combined with quadrupole time-of-flight electrospray ionization tandem mass spectrometry (LC/Q-TOF-ESI-MS) was employed for the identification of reaction byproducts. The reaction pathways were proposed based on the identified degradation byproducts and radical chemistry. In high pH system (pH = 10.5) similar reaction byproducts as those in neutral pH system were identified. However, high pH appeared to inhibit sulfate elimination with less sulfate elimination byproducts detected. In the presence of carbonate in the photocatalytic process, hydroxyl radical reaction would be largely inhibited since carbonate ion would react with hydroxyl radical to form carbonate radical. The second order rate constant of carbonate radical with CYN was estimated to be 1.4 × 10(8) M(-1)s(-1), which is much smaller than that of hydroxyl radical. However, the more significant abundance of carbonate radical in the reaction solution strongly contributed to the transformation of CYN. Carbonate radical has higher reaction selectivity than hydroxyl radical and hence, played a different role in the photocatalytic reaction. It would promote the formation of byproduct m/z 420.12 which has not been identified in the other two studied photocatalytic systems. Besides, the presence of carbonate ion may hinder the removal of toxicity originated from uracil moiety due to the low reaction activity of carbonate radical with uracil moiety in CYN molecule. This work would further support the application of photocatalytic technologies for CYN treatment and provide fundamental information for the complete assessment of CYN removal by using TiO2 photocatalysis process.
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Release of the H atom from the radical cation and subsequent rearrangement forms a carbon-centered radical.
“The release of the H atom from this species and a subsequent rearrangement forms a carbon-centered radical [54,58].”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [58]
CO3·- accepts an electron from an electron-rich center to form radical cations.
“CO3 ·-accept an electron from the electron-rich center to form radical cations.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [58]
H abstraction can also form a carbon-centered radical.
“The H abstraction can also form a carbon-centered radical.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [58]
CO3·- is highly selective towards electron-rich moieties such as -NH2, -OH (especially phenols), and aromatic rings.
“The highly selective nature of the CO3 ·-makes it more selective towards electron-rich moieties such as -NH2, -OH (especially phenols), and aromatic rings.”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [58]
For CYN and HPyBr, the number of intermediates detected in the presence of carbonate ions was less than that detected in the pure photocatalytic process, especially sulfate group elimination byproducts.
“A similar tendency was reported for CYN and hexylpyridinium bromide (HPyBr). The number of intermediates detected in the presence of carbonate ions was less than that detected in the pure photocatalytic process, especially sulfate group elimination byproducts [58].”
From Advanced Oxidation Processes for Degradation of Water Pollutants—Ambivalent Impact of Carbonate Species: A Review (2023) · cites this paper as [58]
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- Authors
- Zhang, G., He, X., Nadagouda, M. N., E. O'Shea, K., & Dionysiou, D. D.
- Affiliations
- University of Cincinnati (US)
- Corresponding author
- Dionysiou, Dionysios D.
- Venue
- Water Research
- Publisher
- Elsevier BV
- Published
- 2015-04
- Volume
- 73
- Pages
- 353-361
- ISSN
- 0043-1354 (ISSN-L)
- OpenAlex
- W2018643296
- Cited by
- 128
- References
- 65
- Citations by year
- 2026: 9 · 2025: 13 · 2024: 13 · 2023: 12 · 2022: 17 · 2021: 18 · 2020: 13 · 2019: 12 · 2018: 5 · 2017: 5 · 2016: 8 · 2015: 3
- FWCI
- 4.64
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Water Research (publishedVersion)
- PubMed (publishedVersion)
- Funders
- U.S. Department of Agriculture (58-3148-1-152)
- China Scholarship Council (CSC) Scholarships (2009617129)
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Environmental Science › Environmental Chemistry › Aquatic Ecosystems and Phytoplankton Dynamics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › TiO2 Photocatalysis and Solar Cells
- Keywords
- cylindrospermopsin, TiO2 photocatalysis, cyanotoxins, carbonate radical, hydroxyl radicals, pH effect, degradation by-products, reaction mechanism, water treatment
- MeSH terms
- Cyanobacteria Toxins, Alkaloids, Bacterial Toxins, Carbonates, Chromatography, High Pressure Liquid, Hydrogen-Ion Concentration, Photolysis, Titanium, Uracil, Waste Disposal, Fluid, Water Pollutants, Chemical, Tandem Mass Spectrometry
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