4.2 Article

Mechanistic Insight into the Heterogeneous Electro-Fenton/Sulfite Process for Ultraefficient Degradation of Pollutants over a Wide pH Range

Journal

ACS ES&T WATER
Volume 1, Issue 7, Pages 1637-1647

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsestwater.1c00123

Keywords

electro-Fenton; sulfite; iron-carbon catalyst; carbamazepine; pH application range

Funding

  1. National Key R&D Pro gram International Cooperation Project [2021YFE0106500]
  2. National Natural Science Foundation of China [21773129, 21976096, 21811530274]
  3. Tianjin Science and Technology Program [19PTZWHZ00050]
  4. Tianjin Development Program for Innovation and Entrepreneurship
  5. Tianjin Postgraduate Students Research and Innovation Project [2019YJSB075]
  6. Fundamental Research Funds for the Central Universities, Nankai University

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The study synthesized an iron-carbon catalyst to expand the pH application range to 7 in the EF/sulfite process, significantly increasing the rate constant for carbamazepine degradation. Results demonstrated the applicability of the process to different pollutants and its enhancement of various catalysts.
Electro-Fenton (EF) has received widespread attention in terms of water decontamination in advanced oxidation processes but still has the bottlenecks of a narrow pH (similar to 3) application range and a slow rate of reduction of the iron ion to sustain high treatment efficiency. Herein, an iron-carbon catalyst was synthesized to develop a heterogeneous EF/sulfite (hetero-EF/sulfite) process, which expanded the pH application range to 7 and increased the rate constant of carbamazepine (CBZ) degradation 10.74 times compared with that of the hetero-EF process. The catalyst was systematically characterized; important process factors such as the applied current, initial pH, and CBZ, catalyst, and sulfite dosage were investigated, and a possible degradation mechanism and a possible pathway were proposed. The quenching experiments and electron paramagnetic resonance test revealed the existence of active species such as (OH)-O-center dot, SO4 center dot-, O-2(center dot-), O-1(2), and their mutual transformation, in which (OH)-O-center dot and O-2(center dot-) were dominant. This work also verified the suitability of the hetero-EF/sulfite for different pollutants, and its universal enhancement for different heterogeneous and homogeneous catalysts. This modified EF process expands the pH application range and enables the co-generation and transformation of free radicals, which has broad prospects for application in the effective degradation of organic pollutants for water purification.

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