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Central composite rotatable design for non-convex optimization of removal efficiency of hydroxychloroquine in an electrochemical cell

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Abstract

Hydroxychloroquine sulfate (HCQ), an against-COVID-19 drug, is a dangerous organic compound in wastewater. In this study, 0.6 L of an HCQ solution (50 mg L−1) was electro-oxidized in a batch electrochemical cell (BEC) with two boron-doped diamond (BDD) electrodes. The optimal operating conditions were established by DoE-driven non-convex constrained optimization. A central composite rotatable design (CCRD) was applied to model the chemical oxygen demand (COD) removal efficiency and to evaluate the influence of current density (j): 10–120 mA cm−2, initial pH: 2–12, and stirring speed (Ω): 400–600 rpm. Experimental results were modeled by a reduced third-order polynomial function having a determination coefficient (R2), root mean square error (RMSE), mean square error (MSE), and coefficient of variation (C.V.) of 0.9906, 0.0460, 0.0021, and 3.72%, respectively. This validates the predictive capacity of the fitted model and the efficiency of the employed electro-oxidation process. The optimal operating vector was j = 46.36 mA cm−2, pH0 = 12.04, and Ω = 584 rpm within 5 h of reaction time, attaining a maximum COD removal efficiency of 85.55% with an energy consumption of 1.24 kW h L−1 and a total operating cost of 0.067 USD$ L−1. Also, a total organic carbon removal of 52.5% was achieved. Additionally, mathematical models were established to fit the temporary profiles of HCQ degradation, COD, and TOC removal. The estimated apparent kinetic constants (kapp) were 1.21 h−1, 0.26 h−1, and 2.65 mg L−1 h−1, respectively. Finally, it was concluded that the assessed electrochemical process could help mineralizing wastewater containing HCQ.

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Abbreviations

a :

Electrode surface (cm2)

ANOVA:

Analysis of variance

BDD:

Boron-doped diamond

BEC:

Batch electrochemical cell

C :

Concentration (mg L−1)

CCD:

Central composite design

CCRD::

Central composite rotatable design

COD:

Chemical oxygen demand (mg L−1)

C.V.:

Coefficient of variation (%)

EC:

Total energy consumption (kW h)

E:

Electricity used (kW h)

F-value:

Ratio of the mean square’s treatment to the mean squares error

GWE:

Global warming potential

HCQ:

Hydroxychloroquine

j :

Current density (mA cm−2)

i :

Current intensity (µA)

K :

Factor number

k :

Kinetic constant (h−1)

m :

Mass of electrolyte (kg)

MSE:

Mean square error

OH● :

Hydroxyl radical

OC:

Operating cost (USD$)

pH:

Power of hydrogen (dimensionless)

p-value::

Probability of getting a result at least as extreme as the one that was observed

P :

Supplier catalog nominal power (kW h)

RMSE:

Root mean square error

R2 :

Determination coefficient

t :

Electrolysis time (h)

TOC:

Total organic carbon (mg L−1)

T :

Temperature (°C)

U :

Mean voltage cell (V)

V :

Volume treated (L)

VIFs:

Variance inflation factor

x :

Encrypted independent variables

α :

Rotatability (1.68)

γ :

Values of the coefficient of the polynomial equation

Δ:

Increased

ξ :

Electricity price (USD$ (kW h)−1)

Ω:

Stirred speed (rpm)

η :

Efficiency (%)

ϕ :

Electrolyte price (USD$ kg−1)

Adj:

Adjusted

app:

Apparent

Elec:

Electrode

Model:

Model

M:

Mineralization

Pred:

Predicted

Pump:

Recirculation pump

Stirred:

Magnetic stirred

Tr:

Treated

i :

Number of independent variables

0:

Initial

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Acknowledgements

The support of Derek Joe Brockett, an English professor at Universidad del Mar, is acknowledged for his support in correcting the English writing of this work. Finally, authors would like to thank the staff of the environmental and investigation laboratories for dedicating their time and effort to facilitate the materials to conduct this research work.

Funding

The authors are grateful to Universidad del Mar for providing financial support for the research project CUP: 2II2104. Also, the authors (A.R.-M., E.P.-R., and R.N.) are grateful to the Mexican Council of Science and Technology (CONAHCyT) for the financial support through the Investigators National System program (SNII). Similarly, D.V.-H. thank CONAHCyT-Mexico for providing scholarship No. 809459 for his master’s studies.

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  1. Research Laboratories, Universidad del Mar-Campus Puerto Ángel, Ciudad Universitaria, Col. El Faro, Puerto Ángel, San Pedro Pochutla, 70902, México

    Alejandro Regalado-Méndez, Daniel Vásquez-Hernández & Ever Peralta-Reyes

  2. Chemical Engineering Laboratory, Joint Centre for Research on Sustainable Chemistry, UAEM-UNAM, Universidad Autónoma del Estado de México, Km 14.5 Toluca-Atlacomulco Road, Toluca, 50200, México

    Reyna Natividad

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  1. Alejandro Regalado-Méndez
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  2. Daniel Vásquez-Hernández
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  3. Reyna Natividad
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  4. Ever Peralta-Reyes
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Correspondence to Alejandro Regalado-Méndez or Ever Peralta-Reyes.

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Regalado-Méndez, A., Vásquez-Hernández, D., Natividad, R. et al. Central composite rotatable design for non-convex optimization of removal efficiency of hydroxychloroquine in an electrochemical cell. J Solid State Electrochem (2024). https://doi.org/10.1007/s10008-024-05962-y

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