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Sustainable Degradation of Acetaminophen by a Solar-Powered Electro-Fenton Process - A Green and Energy-Efficient Approach

MetadataDetails
Publication Date2025-08-20
JournalProcesses
AuthorsSonia Herrera-ChĂĄvez, Silvia GutiĂ©rrez‐Granados, Miguel A. Sandoval, Enric Brillas, MartĂ­n Pacheco‐Álvarez
InstitutionsUniversidad de Guanajuato, Tecnológico Nacional de México
Citations1
AnalysisFull AI Review Included

This study validates the Solar Photo-Electro-Fenton (SPEF) process using Boron-Doped Diamond (BDD) electrodes as a highly efficient and sustainable technology for degrading acetaminophen (ACTP).

  • Superior Performance: SPEF demonstrated a clear efficiency hierarchy (SPEF > EF > EO), achieving up to 97% ACTP removal and 78% Chemical Oxygen Demand (COD) reduction within 90 minutes.
  • Energy Efficiency: SPEF exhibited significantly enhanced energy efficiency, requiring only ~0.052 kWh per gram of COD removed (gCOD-1), highlighting its cost-effectiveness.
  • Synergistic Mechanism: The high performance is attributed to the synergistic action of BDD anodic oxidation, homogeneous electro-Fenton reactions, and natural solar UV irradiation, which continuously regenerates the Fe2+ catalyst.
  • Optimal Conditions: Optimization via Box-Behnken design identified the optimal conditions: 60 mA cm-2 current density, 10 mg L-1 initial ACTP concentration, and 60-90 minutes electrolysis time.
  • Reaction Kinetics: The degradation followed pseudo-first-order kinetics, with a maximum rate constant (Kc) of 0.0865 min-1 under optimized SPEF conditions.
  • Degradation Pathway: HPLC confirmed the transient formation of Phenol and Catechol, indicating a pathway involving hydroxylation, aromatic ring cleavage, and subsequent oxidation to low-molecular-weight carboxylic acids.
  • Sustainability: The use of natural solar radiation makes SPEF a viable, environmentally friendly alternative for treating pharmaceutical contaminants, particularly in regions with high solar availability.
ParameterValueUnitContext
Optimal ACTP Removal (SPEF)97%Achieved in 60 min (10 mg L-1 ACTP)
Optimal COD Reduction (SPEF)78%Achieved in 90 min (10 mg L-1 ACTP)
Specific Energy Consumption (SEC)0.052kWh gCOD-1Calculated after 90 min treatment
Optimal Current Density (j)60mA cm-2Maximized radical generation rate
Optimal Initial ACTP Conc. (C0)10mg L-1Used for maximum fractional removal
Optimal Fe2+ Dosage0.05mmol L-1Used in EF and SPEF processes
Optimal pH3.0-Maintained using H2SO4
Supporting Electrolyte Conc.0.05MNa2SO4
Solar UV-A Irradiation Intensity30-35W/m2Natural sunlight (300-400 nm)
Maximum Kinetic Constant (Kc)0.0865min-1Pseudo-first-order rate (optimized SPEF)
Current Efficiency Index (ICE)3.2-Measured after 90 min treatment
Electrode Lifespan Estimate (BDD)782hMedian lifetime at 10-50 mA cm-2
  1. Electrochemical Cell Setup: Experiments were performed in a 250 mL stirred-tank reactor, continuously stirred at 60 rpm, with constant oxygen supply via an air pump.
  2. Electrode Materials and Configuration:
    • EO: BDD (anode) / Graphite (cathode).
    • EF/SPEF: BDD (anode) / BDD (cathode).
    • Interelectrode distance was maintained at approximately 2 cm.
  3. Chemical Environment: Solutions were prepared using ultrapure water, maintained at pH 3.0 (adjusted with H2SO4), and utilized 0.05 M Na2SO4 as the supporting electrolyte. Ferrous sulfate (FeSO4·7H2O) was added for Fenton processes (0.05 mmol L-1).
  4. Solar Irradiation Source: SPEF trials were conducted outdoors during the summer of 2023, utilizing natural UV radiation (300-400 nm) measured by a Kipp & Zonen CUV 5 radiometer (30-35 W/m2).
  5. Process Optimization: A three-level Box-Behnken experimental design (RSM) was used to model and optimize the degradation rate constant (Kc) based on three independent variables: electrolysis time (30-90 min), initial ACTP concentration (10-30 mg L-1), and applied current density (20-60 mA cm-2).
  6. Analytical Techniques:
    • ACTP concentration was monitored by UV-Vis spectrophotometry (243 nm) and High-Performance Liquid Chromatography (HPLC) using a Zorbax SB-C18 column (isocratic method, 50:50 acetonitrile:water).
    • Mineralization was quantified by Chemical Oxygen Demand (COD) assays (Standard Methods 5220D).
    • Intermediate products (Phenol, Catechol) were identified via HPLC.

The findings support the implementation of BDD-based SPEF technology in several high-value environmental engineering sectors:

  • Pharmaceutical Wastewater Treatment: Direct application for the efficient and cost-effective removal and mineralization of persistent pharmaceutical contaminants (like ACTP) from industrial and hospital effluents.
  • Decentralized Water Remediation Systems: SPEF is highly suitable for deployment in remote or resource-constrained regions, leveraging natural solar energy to reduce operational costs and reliance on complex infrastructure.
  • Advanced Oxidation Reactor Design: The BDD electrode material is critical for high-performance AOPs, offering superior stability and high current density operation necessary for generating adsorbed hydroxyl radicals (BDD(‱OH)).
  • Refractory Organic Mineralization: Used for treating complex industrial wastewaters (e.g., textile, tanning) where stable aromatic intermediates and short-chain carboxylic acids must be fully mineralized to meet strict discharge limits.
  • Sustainable Engineering Solutions: Provides a green technology alternative to conventional chemical or energy-intensive treatments, aligning with sustainable development goals for water quality management.
View Original Abstract

The presence of acetaminophen (ACTP) in aquatic environments has become a significant concern due to its environmental persistence and the potential formation of toxic transformation products. This study systematically compares the performance of three electrochemical advanced oxidation processes (EAOPs), electro-oxidation (EO), electro-Fenton (EF), and solar photo-electro-Fenton (SPEF), for the degradation and mineralization of ACTP in aqueous media using boron-doped diamond (BDD) electrodes. Reactions were conducted under varying operational parameters, including current densities (15-60 mA cm−2), initial ACTP concentrations (10-30 mg L−1), and Fe2+ dosages. In the SPEF system, natural sunlight was utilized as the source of UV-A irradiation (30-35 W m−2). Among the evaluated processes, SPEF exhibited the highest degradation efficiency, achieving up to 97% ACTP removal and 78% chemical oxygen demand (COD) reduction within 90 min. High-performance liquid chromatography (HPLC) analysis identified phenol and catechol as major intermediates, suggesting a degradation pathway involving hydroxylation, aromatic ring cleavage, and subsequent oxidation into low-molecular-weight carboxylic acids. Kinetic modeling revealed pseudo-first-order behavior, with a maximum rate constant of 0.0865 min−1 under optimized conditions determined via Box-Behnken experimental design. Additionally, SPEF demonstrated enhanced energy efficiency (~0.052 kWh gCOD−1) and improved oxidant regeneration under solar radiation, highlighting its potential as an environmentally friendly and cost-effective alternative for pharmaceutical wastewater treatment. These results support the implementation of SPEF as a sustainable strategy for mitigating the environmental impact of emerging contaminants, especially in regions with high solar availability and limited technological resources.

  1. 2012 - Modelling photo-Fenton process for organic matter mineralization, hydrogen peroxide consumption and dissolved oxygen evolution
  2. 2016 - Efficient removal of paracetamol using LaCu1−xMxO3 (M = Mn, Ti) perovskites as heterogeneous Fenton-like catalysts [Crossref]
  3. 2021 - Aluminized surface to improve solar light absorption in open reactors: Application for micropollutants removal in effluents from municipal wastewater treatment plants [Crossref]
  4. 2023 - The occurrence and fate of antibiotics and nonsteroidal anti-inflammatory drugs in water treatment processes: A review
  5. 2019 - Acetaminophen micropollutant: Historical and current occurrences, toxicity, removal strategies and transformation pathways in different environments [Crossref]
  6. 2020 - Removal of Pharmaceutical Contaminants from Aqueous Medium: A State-of-the-Art Review Based on Paracetamol [Crossref]
  7. 2025 - Advanced Oxidation Process-Mediated Removal of Pharmaceuticals from Water: A Review of Recent Advances
  8. 2012 - Degradation of acetaminophen by Fenton and electro-Fenton processes in aerator reactor [Crossref]
  9. 2023 - Development of heterogeneous electro-Fenton process with immobilized FeWO4 catalyst for degradation of tetracycline and crude-oil tank cleaning wastewater [Crossref]
  10. 2011 - Photo-Fenton mineralization of synthetic municipal wastewater effluent containing acetaminophen in a pilot plant [Crossref]