Photodegradation of pharmaceutical compounds in partially nitritated wastewater during UV irradiation

Priya I Hora, Paige J Novak, Bill Arnold

Research output: Contribution to journalArticle

Abstract

The first step of an anaerobic ammonia oxidation (anammox) system is typically the formation of nitrite (NO2-) via partial nitritation, which can generate hydroxyl radical (OH) when irradiated with ultraviolet (UV) light. This study demonstrated that the presence of nitrite in buffer and wastewater matrices during medium-pressure UV irradiation (at λ ≥ 220 or ≥ 280 nm) enhanced the degradation of select pharmaceutical compounds of different therapeutic classes (atenolol, carbamazepine, fluoxetine, and trimethoprim). Total pharmaceutical removals in a wastewater matrix irradiated at λ ≥ 280 for 120 minutes were 47% for trimethoprim, 50% for carbamazepine, 60% for atenolol, and 57% for fluoxetine at fluences of 58.6 mEi m-2 (2033.1 mJ cm-2). When irradiated at λ ≥ 220 for 60 minutes, removals were 52% for trimethoprim, 56% for carbamazepine, 69% for atenolol, and 90% for fluoxetine at fluences of 634.7 mEi m-2 (23:969.2 mJ cm-2). Reaction with OH accounted for ∼78-90% of pharmaceutical removal at λ ≥ 280 nm. Although direct photolysis did contribute to target compound removal for irradiation with λ ≥ 220 nm, much of the light was absorbed in the buffer and wastewater matrices, and reaction with OH accounted for ∼70-93% of pharmaceutical removal. Quencher experiments with isopropanol confirmed the importance of reaction with OH as the main contributor to pharmaceutical removal. para-Chlorobenzoic acid was used as a probe to estimate steady-state OH concentrations, which averaged 8.58 × 10-15 M for both matrices at λ ≥ 280 nm and 3.50 × 10-14 M for both matrices at λ ≥ 220 nm. Nitrosamines were formed and accumulated during the UV treatment step, however, concomitant with their direct photochemical destruction. Presence of the pharmaceutical micro-pollutants studied, such as the secondary-amine containing atenolol and fluoxetine, did not elevate nitrosamine formation.

Original languageEnglish (US)
Pages (from-to)897-909
Number of pages13
JournalEnvironmental Science: Water Research and Technology
Volume5
Issue number5
DOIs
StatePublished - May 1 2019

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Photodegradation
photodegradation
Drug products
irradiation
Wastewater
drug
Irradiation
wastewater
matrix
Nitrosamines
nitrite
Photolysis
hydroxyl radical
photolysis
removal
Ammonia
Amines
ammonia
probe
oxidation

Cite this

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title = "Photodegradation of pharmaceutical compounds in partially nitritated wastewater during UV irradiation",
abstract = "The first step of an anaerobic ammonia oxidation (anammox) system is typically the formation of nitrite (NO2-) via partial nitritation, which can generate hydroxyl radical (OH) when irradiated with ultraviolet (UV) light. This study demonstrated that the presence of nitrite in buffer and wastewater matrices during medium-pressure UV irradiation (at λ ≥ 220 or ≥ 280 nm) enhanced the degradation of select pharmaceutical compounds of different therapeutic classes (atenolol, carbamazepine, fluoxetine, and trimethoprim). Total pharmaceutical removals in a wastewater matrix irradiated at λ ≥ 280 for 120 minutes were 47{\%} for trimethoprim, 50{\%} for carbamazepine, 60{\%} for atenolol, and 57{\%} for fluoxetine at fluences of 58.6 mEi m-2 (2033.1 mJ cm-2). When irradiated at λ ≥ 220 for 60 minutes, removals were 52{\%} for trimethoprim, 56{\%} for carbamazepine, 69{\%} for atenolol, and 90{\%} for fluoxetine at fluences of 634.7 mEi m-2 (23:969.2 mJ cm-2). Reaction with OH accounted for ∼78-90{\%} of pharmaceutical removal at λ ≥ 280 nm. Although direct photolysis did contribute to target compound removal for irradiation with λ ≥ 220 nm, much of the light was absorbed in the buffer and wastewater matrices, and reaction with OH accounted for ∼70-93{\%} of pharmaceutical removal. Quencher experiments with isopropanol confirmed the importance of reaction with OH as the main contributor to pharmaceutical removal. para-Chlorobenzoic acid was used as a probe to estimate steady-state OH concentrations, which averaged 8.58 × 10-15 M for both matrices at λ ≥ 280 nm and 3.50 × 10-14 M for both matrices at λ ≥ 220 nm. Nitrosamines were formed and accumulated during the UV treatment step, however, concomitant with their direct photochemical destruction. Presence of the pharmaceutical micro-pollutants studied, such as the secondary-amine containing atenolol and fluoxetine, did not elevate nitrosamine formation.",
author = "Hora, {Priya I} and Novak, {Paige J} and Bill Arnold",
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N2 - The first step of an anaerobic ammonia oxidation (anammox) system is typically the formation of nitrite (NO2-) via partial nitritation, which can generate hydroxyl radical (OH) when irradiated with ultraviolet (UV) light. This study demonstrated that the presence of nitrite in buffer and wastewater matrices during medium-pressure UV irradiation (at λ ≥ 220 or ≥ 280 nm) enhanced the degradation of select pharmaceutical compounds of different therapeutic classes (atenolol, carbamazepine, fluoxetine, and trimethoprim). Total pharmaceutical removals in a wastewater matrix irradiated at λ ≥ 280 for 120 minutes were 47% for trimethoprim, 50% for carbamazepine, 60% for atenolol, and 57% for fluoxetine at fluences of 58.6 mEi m-2 (2033.1 mJ cm-2). When irradiated at λ ≥ 220 for 60 minutes, removals were 52% for trimethoprim, 56% for carbamazepine, 69% for atenolol, and 90% for fluoxetine at fluences of 634.7 mEi m-2 (23:969.2 mJ cm-2). Reaction with OH accounted for ∼78-90% of pharmaceutical removal at λ ≥ 280 nm. Although direct photolysis did contribute to target compound removal for irradiation with λ ≥ 220 nm, much of the light was absorbed in the buffer and wastewater matrices, and reaction with OH accounted for ∼70-93% of pharmaceutical removal. Quencher experiments with isopropanol confirmed the importance of reaction with OH as the main contributor to pharmaceutical removal. para-Chlorobenzoic acid was used as a probe to estimate steady-state OH concentrations, which averaged 8.58 × 10-15 M for both matrices at λ ≥ 280 nm and 3.50 × 10-14 M for both matrices at λ ≥ 220 nm. Nitrosamines were formed and accumulated during the UV treatment step, however, concomitant with their direct photochemical destruction. Presence of the pharmaceutical micro-pollutants studied, such as the secondary-amine containing atenolol and fluoxetine, did not elevate nitrosamine formation.

AB - The first step of an anaerobic ammonia oxidation (anammox) system is typically the formation of nitrite (NO2-) via partial nitritation, which can generate hydroxyl radical (OH) when irradiated with ultraviolet (UV) light. This study demonstrated that the presence of nitrite in buffer and wastewater matrices during medium-pressure UV irradiation (at λ ≥ 220 or ≥ 280 nm) enhanced the degradation of select pharmaceutical compounds of different therapeutic classes (atenolol, carbamazepine, fluoxetine, and trimethoprim). Total pharmaceutical removals in a wastewater matrix irradiated at λ ≥ 280 for 120 minutes were 47% for trimethoprim, 50% for carbamazepine, 60% for atenolol, and 57% for fluoxetine at fluences of 58.6 mEi m-2 (2033.1 mJ cm-2). When irradiated at λ ≥ 220 for 60 minutes, removals were 52% for trimethoprim, 56% for carbamazepine, 69% for atenolol, and 90% for fluoxetine at fluences of 634.7 mEi m-2 (23:969.2 mJ cm-2). Reaction with OH accounted for ∼78-90% of pharmaceutical removal at λ ≥ 280 nm. Although direct photolysis did contribute to target compound removal for irradiation with λ ≥ 220 nm, much of the light was absorbed in the buffer and wastewater matrices, and reaction with OH accounted for ∼70-93% of pharmaceutical removal. Quencher experiments with isopropanol confirmed the importance of reaction with OH as the main contributor to pharmaceutical removal. para-Chlorobenzoic acid was used as a probe to estimate steady-state OH concentrations, which averaged 8.58 × 10-15 M for both matrices at λ ≥ 280 nm and 3.50 × 10-14 M for both matrices at λ ≥ 220 nm. Nitrosamines were formed and accumulated during the UV treatment step, however, concomitant with their direct photochemical destruction. Presence of the pharmaceutical micro-pollutants studied, such as the secondary-amine containing atenolol and fluoxetine, did not elevate nitrosamine formation.

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