Skip to content

Chlorpyrifos removal - Nb/boron-doped diamond anode coupled with solid polymer electrolyte and ultrasound irradiation

MetadataDetails
Publication Date2020-10-09
JournalJournal of Environmental Health Science and Engineering
AuthorsAndrea Luca Tasca, Davide Clematis, Marco Panizza, Sandra Vitolo, Monica Puccini
InstitutionsUniversity of Pisa, University of Genoa
Citations9
AnalysisFull AI Review Included
  • Novel Reactor Design: A sono-electrochemical reactor was developed utilizing a Niobium/Boron-Doped Diamond (Nb/BDD) anode coupled with a Solid Polymer Electrolyte (SPE) (NafionÂź N324) to degrade Chlorpyrifos (CP).
  • High Removal Efficiency: Anodic oxidation alone achieved up to 89.28% CP removal in 30 minutes at a low current intensity (0.1 A), demonstrating superior performance compared to previously reported methods for low-conductivity solutions.
  • SPE Success: The SPE membrane successfully facilitated the electrochemical process in low-conductivity aqueous media (initial CP concentration: 0.56 ”g L-1), overcoming a major limitation of conventional electro-oxidation.
  • Degradation Pathway: CP degradation proceeds via oxidation and hydrolysis, generating 3,5,6-trichloro-2-pyridinol (TCP) and O,O-Diethyl O-(3,5,6-trichloropyridin-2-yl) phosphate (OCP) as primary intermediates.
  • Sonication Ineffectiveness: Ultrasound irradiation (40 kHz) did not enhance CP removal efficiency and significantly increased the specific energy consumption (up to 26x), indicating that mass transport limitations near the anode surface were the dominant kinetic constraint.
  • Future Potential: The BDD/SPE technology is highly promising for the remediation of emerging pollutants (pharmaceuticals, pesticides) in low-conductivity industrial streams and for in-situ groundwater treatment, offering a sludge-free oxidation alternative.
ParameterValueUnitContext
Anode MaterialNb/Boron-Doped Diamond (BDD)N/AHigh hydroxyl radical generation
Cathode MaterialTi/RuO2 meshN/AUsed for hydrogen evolution
Electrolyte TypeNafionÂź N324N/ASolid Polymer Electrolyte (SPE)
Electrode Dimensions3.5 x 7.5cmActive surface area
Electrode Gap0.15mmDistance between anode and cathode
Initial CP Concentration0.56 ± 0.005”g L-1Low concentration test solution
Current Intensities Tested0.1 and 0.5AGalvanostatic operation
Sonication Frequency40kHzUltrasonic irradiation
Max CP Removal (0.1 A, 30 min)89.28%Sonication Off
Min Specific Energy Consumption8.68·10-6kWh ”g-1 removed0.1 A, 10 min, Sonication Off
Max Specific Energy Consumption2.33·10-3kWh ”g-1 removed0.5 A, 30 min, Sonication On
Stirring Rate550rpmVertical stirrer mixing
Operating Temperature20°CAmbient conditions
  1. Reactor Configuration: Experiments were conducted in a single-compartment electrochemical cell using a Nb/BDD anode and a Ti/RuO2 mesh cathode, separated by a NafionÂź N324 Solid Polymer Electrolyte (SPE) membrane.
  2. Electrolysis Conditions: Trials were performed under galvanostatic control (0.1 A and 0.5 A) for 30 minutes at 20 °C and natural pH, powered by an AMEL 2055 potentiostat/galvanostat.
  3. Mixing and Pre-treatment: Solutions were continuously mixed at 550 rpm. Electrodes were pre-sonicated for 30 minutes at 1 A prior to each assay to ensure surface cleanliness.
  4. Sono-Electrolysis Coupling: Sonication was applied using a SONICA 2200 ultrasonic device operating at 40 kHz during coupled trials.
  5. Extraction and Analysis: Samples were collected at defined intervals, stored in the dark at 4 °C, and extracted using rotary evaporation with a cyclohexane/ethylacetate mixture (1:1).
  6. Quantification: CP and its metabolites (TCP, OCP) were quantified using a Shimadzu GC-MS-TQ8040 equipped with a crossbond diphenyl dimethyl polysiloxane SH-Rxi-5 ms column.
  • Advanced Oxidation Processes (AOPs): Integration of BDD anodic oxidation into tertiary water treatment facilities to achieve high mineralization rates for persistent organic pollutants (POPs) and emerging contaminants.
  • Low-Conductivity Wastewater Treatment: Specialized remediation systems for industrial streams (e.g., pharmaceutical manufacturing, chemical synthesis) characterized by low ionic strength, where traditional electrochemical methods fail.
  • Solid Polymer Electrolyte (SPE) Systems: Development of compact, energy-efficient electrochemical cells utilizing SPE technology for decentralized or mobile water purification units, eliminating the need for added supporting electrolytes.
  • Diamond Electrode Supply: Increased demand for high-performance, stable Nb/BDD electrodes for industrial electrochemical applications requiring robust hydroxyl radical generation and resistance to passivation.
  • In-Situ Groundwater Remediation: Application of BDD/SPE reactors for the direct treatment of contaminated groundwater containing pesticides (like Chlorpyrifos) and personal care products, offering a sludge-free, in-situ solution.