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1.
Environ Sci Technol ; 58(16): 6868-6877, 2024 Apr 23.
Article in English | MEDLINE | ID: mdl-38593035

ABSTRACT

Bioaerosols play a significant role in the transmission of many infectious diseases, especially in enclosed indoor environments. Ultraviolet (UV) disinfection has demonstrated a high efficacy in inactivating microorganisms suspended in the air. To develop more effective and efficient UV disinfection protocols, it is necessary to evaluate and optimize the effectiveness of UV disinfection against aerosolized bacteria and viruses across the entire UV spectrum. In this study, we evaluated the performance of UV disinfection across the UV spectrum, ranging from 222 to 365 nm, against aerosolized bacteria and viruses, including Escherichia coli, Staphylococcus epidermidis, Salmonella enterica, MS2, P22, and Phi6. Six commonly available UV sources, including gas discharge tubes and light-emitting diodes with different emission spectra, were utilized, and their performance in terms of inactivation efficacy, action spectrum, and energy efficiency was determined. Among these UV sources, the krypton chloride excilamp emitting at a peak wavelength of 222 nm was the most efficient in inactivating viral bioaerosols. A low-pressure mercury lamp emitting at 254 nm performed well on both inactivation efficacy and energy efficiency. A UV light-emitting diode emitting at 268 nm demonstrated the highest bacterial inactivation efficacy, but required approximately 10 times more energy to achieve an equivalent inactivation level compared with that of the krypton chloride excilamp and low-pressure mercury lamp. This study provides insights into UV inactivation on bioaerosols, which can guide the development of effective wavelength-targeted UV air disinfection technologies and may significantly help reduce bioaerosol transmission in public areas.

2.
J Hazard Mater ; 460: 132419, 2023 Oct 15.
Article in English | MEDLINE | ID: mdl-37651931

ABSTRACT

In recent years, shorter-chain fluorinated compounds have been manufactured as alternatives to legacy per- and polyfluoroalkyl substances (PFAS) after a global ban on some long-chain PFAS. This study is the first to investigate the degradability of emerging PFAS by an electrochemical plug flow reactor (EPFR). Ten different emerging PFAS, representing classes of fluorotelomer alcohol, perfluoroalkyl ether carboxylate, polyfluoroalkyl ethersulfonic acids, perfluoroalkyl ether/polyether carboxylates, perfluoroether sulfonate, N-alkyl perfluoroalkylsulfonamido carboxylate, fluoroalkyl phosphonic acid, and perfluoro alkane sulfonamide were investigated. The process kinetics was performed. The degradation of parent compounds increased with increasing retention time (RT). At 45.2 min of RT, the degradation of parent compounds ranged between 68%-100% with a current density of 17.2 mA/cm2. A linear increase in pseudo-first order rate constants was observed for all PFAS with increasing current density from 5.7 to 28.7 mA/cm2 (R2 > 0.91). The effect of pH, natural organic matter, and bicarbonate on the degradation, defluorination, and fluorine mass balance are reported. Alkaline pH (11) caused a decrease in degradation for all PFAS. While the presence of natural organic matter (NOM) significantly decreased the degradation and defluorination processes, the presence of bicarbonate at all studied concentrations (25, 50, and 100 mg/L) did not affect the process efficiency. The defluorination reduced to 34% from 81% with 15 mg/L NOM. The unknown/undetected fluorine fraction also increased in the presence of 15 mg/L NOM indicating the formation of NOM-PFAS complexes. Additionally, C2-C8 perfluoro carboxylic acids (PFCAs), one perfluoro sulfonic acid (PFSA), two H-PFCAs, and 4:2 fluorotelomer sulfonate (FTS) were identified as degradation byproducts in suspect screening. The electrical energy per order for PFAS ranged between 1.8 and 19.4 kWh/m3. This study demonstrates that emerging types of PFAS can potentially be degraded using an EPFR with relatively low electrical energy requirements.

3.
Heliyon ; 9(5): e16450, 2023 May.
Article in English | MEDLINE | ID: mdl-37305481

ABSTRACT

Photocatalytic degradation of organic pollutants in water using graphitic carbon nitride and persulfate under visible light (g-C3N4/PS system) has been studied. Here, we demonstrate augmentation of photocatalytic degradation of Acetaminophen (AAP) using hydrothermally treated g-C3N4 and PS under 400 nm LED irradiation (HT-g-C3N4/PS system). A pseudo-first-order rate constant (kobs, 0.328 min-1) for degradation of AAP using HT-g-C3N4/PS system was determined to be 15 times higher compared to g-C3N4/PS system (kobs, 0.022 min-1). HT-g-C3N4 showed a higher surface area (81 m2/g) than g-C3N4 (21 m2/g). Photocurrent response for HT-g-C3N4 was higher (1.5 times) than g-C3N4. Moreover, Nyquist plot semicircle for HT-g-C3N4 was smaller compared to g-C3N4. These results confirm effective photoelectron-hole separation and charge-transfer in HT-g-C3N4 compared to g-C3N4. AAP degradation using HT-g-C3N4/PS system was significantly inhibited with O2.- and h+ scavengers compared to 1O2,SO4.- and HO. scavengers. ESR results revealed O2.- formation in HT-g-C3N4/PS system. Moreover, photocurrent measurements reveal AAP oxidation by h+ of HT-g-C3N4 was effective than g-C3N4. HT-g-C3N4 was reused for five cycles in HT-g-C3N4/PS system. Augmented photocatalytic degradation of AAP by HT-g-C3N4/PS system compared to g-C3N4/PS is attributed to effective photoelectron hole separation of HT-g-C3N4 that generates O2.- and h+ for oxidation of pollutant. Importantly, electrical energy per order (EEO) was 7.2 kWh m-3 order-1. kobs for degradation of AAP in simulated groundwater and tap water were determined as 0.029 and 0.035 min-1, respectively. Degradation intermediates of AAP were proposed. AAP ecotoxicity against marine bacteria Aliivibrio fischeri was completely removed after treatment by HT-g-C3N4/PS system.

4.
Chemosphere ; 327: 138540, 2023 Jun.
Article in English | MEDLINE | ID: mdl-36996925

ABSTRACT

As the primary inorganic by-product species of ClO2, chlorite is believed to have negative toxicological effects on human health and therefrom greatly limits the wide application of ClO2 in water treatment. The synergistic trimethoprim (TMP) removal concerning degradation efficiency, energy consumption and disinfection by-products (DBPs) formation in the UV activated chlorite process accompanied by the simultaneously elimination of chlorite was comprehensively evaluated. UV/chlorite integrated process removed TMP far more rapidly than UV (1.52%) or chlorite (3.20%) alone due to the endogenous radicals (Cl•, ClO• and •OH), the contributing proportions of which were 31.96%, 19.20% and 44.12%. The second-order rate constants of TMP reaction with Cl•, ClO• and •OH were determined to be 1.75 × 1010, 1.30 × 109 and 8.66 × 109 M-1 s-1. The effects of main water parameters including chlorite dosage, UV intensity, pH as well as water matrixes (nature organic matter, Cl- and HCO3-) were examined. kobs obeyed the order as UV/Cl2>UV/H2O2≈UV/chlorite>UV, and the cost ranking via electrical energy per order (EE/O, kWh m-3 order-1) parameter was UV/chlorite (3.7034) > UV/H2O2 (1.1625) >UV/Cl2 (0.1631). The operational scenarios can be optimized to achieve the maximum removal efficiencies and the minimum energy costs. The destruction mechanisms of TMP were proposed by LC-ESI-MS analysis. The overall weighted toxicity in subsequent disinfection was assessed as UV/Cl2>UV/chlorite > UV, the values of which in post-chlorination were 6.2947, 2.5806 and 1.6267, respectively. Owing to the vital roles of reactive chlorine species (RCS), UV/chlorite displayed far higher TMP degradation efficiency than UV, and concurrently presented much less toxicity than UV/Cl2. In an effort to determine the viability of the promising combination technology, this study was devoted to reduce and reuse chlorite and synchronously realize the contaminants degradation efficiently.


Subject(s)
Water Pollutants, Chemical , Water Purification , Humans , Disinfection , Hydrogen Peroxide , Trimethoprim , Ultraviolet Rays , Halogenation , Chlorine , Water Pollutants, Chemical/analysis , Oxidation-Reduction
5.
J Environ Sci (China) ; 126: 656-667, 2023 Apr.
Article in English | MEDLINE | ID: mdl-36503791

ABSTRACT

As an active metabolite of venlafaxine and emerging antidepressant, O-desmethylvenlafaxine (ODVEN) was widely detected in different water bodies, which caused potential harm to human health and environmental safety. In this study, the comparative work on the ODVEN degradation by UV (254 nm) and UV-LED (275 nm) activated sodium percarbonate (SPC) systems was systematically performed. The higher removal rate of ODVEN can be achieved under UV-LED direct photolysis (14.99%) than UV direct photolysis (4.57%) due to the higher values of photolysis coefficient at the wavelength 275 nm. Significant synergistic effects were observed in the UV/SPC (80.38%) and UV-LED/SPC (53.57%) systems and the former exhibited better performance for the elimination of ODVEN. The degradation of ODVEN all followed the pseudo-first-order kinetics well in these processes, and the pseudo-first-order rate constant (kobs) increased with increasing SPC concentration. Radicals quenching experiments demonstrated that both ·OH and CO3·- were involved in the degradation of ODVEN and the second-order rate constant of ODVEN with CO3·- (1.58 × 108 (mol/L)-1 sec-1) was reported for the first time based on competitive kinetic method. The introduction of HA, Cl-, NO3- and HCO3- inhibited the ODVEN degradation to varying degrees in the both processes. According to quantum chemical calculation, radical addition at the ortho-position of the phenolic hydroxyl group was confirmed to be the main reaction pathways for the oxidation of ODVEN by ·OH. In addition, the oxidation of ODVEN may involve the demethylation, H-abstraction, OH-addition and C-N bond cleavage. Eventually, the UV-LED/SPC process was considered to be more cost-effective compared to the UV/SPC process, although the UV/SPC process possessed a higher removal rate of ODVEN.


Subject(s)
Phenols , Humans , Desvenlafaxine Succinate , Venlafaxine Hydrochloride , Photolysis
6.
Sci Total Environ ; 859(Pt 1): 160256, 2023 Feb 10.
Article in English | MEDLINE | ID: mdl-36402311

ABSTRACT

Ultraviolet light-emitting diodes (UV LEDs) have shown ability to inactivate microorganisms and viruses in water. The unique characteristic of the UV-LEDs' diversity in wavelengths ranging from UV-C, UV-B, and UV-A, allows for wavelengths to be combined in different manners for polychromatic irradiation. Previous studies reported no synergy from simultaneous or sequential UV-C and UV-B as well as UV-C or UV-B followed by UV-A irradiation. However, synergy was reported for UV-A followed by UV-C or UV-B irradiation on various microorganisms. Nevertheless, no clear ground has been reached on whether to adopt single UV-C wavelengths or UV-A followed by UV-C LED, irradiation on inactivation of microorganisms and viruses in water. Therefore, this work evaluates the disinfection efficacy of single UV-C as well as UV-A followed by UV-C LED irradiation on Escherichia coli, Bacillus spizizenii spores and MS2 bacteriophage in water. The UV-C wavelengths were represented by 267 and 278 nm UV LEDs, and UV-A by 368 nm UV LEDs. In this study, E. coli was highly susceptible to UV radiation followed by B. spizizenii spores, and lastly MS2. Repair following UV inactivation was only observed in E. coli. The synergistic effect found in both E. coli, and B. spizizenii spores was attributed to the different inactivation mechanisms of the UV-C and UV-A wavelengths. In both single UV-C, and UV-A followed by UV-C LED irradiations, single 267 nm UV-C LED showed higher inactivation efficacy. Meanwhile, single 278 nm UV-C LED showed higher efficacy in terms of suppression of repair, and electrical energy consumption. Using single UV-C LEDs in a water disinfection system cuts down on related extra costs by avoiding combined wavelengths while still attaining better levels of microorganism inactivation, repair suppression and electrical energy consumption. These findings are applicable for the design and implementation of UV LED water disinfection systems.


Subject(s)
Ultraviolet Rays , Water Purification , Levivirus , Escherichia coli/radiation effects , Water , Water Microbiology , Disinfection
7.
Photochem Photobiol Sci ; 22(1): 185-193, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36181659

ABSTRACT

The impact of light modulation on the decolorization of Acid Orange 7 (AO7) in aqueous solution was examined in this paper. A fixed bed batch photocatalytic reactor with a flat plate geometry, irradiated by 240 white-light LEDs, was used. A successful transfer of visible active photocatalyst (N-TiO2) in powder form on a polystyrene (PS) transparent plate was realized. The structured photocatalyst was characterized through SEM-EDX, Raman and UV-DRS analyses, evidencing the formation of a coating of N-TiO2 in the anatase phase, with a band-gap energy of 2.5 eV, and almost uniform distribution on the PS surface. Different LED dimming techniques, with fixed and variable duty-cycle values, were tested, and four types of light modulation were compared: fixed duty cycle (constant irradiation), sinusoidal variable duty cycle (sinusoidal variable irradiation), triangular variable duty cycle (triangular variable irradiation), and square wave variable duty cycle (square wave variable irradiation). The resulting responsiveness/efficiency of the LED versus the current intensity was evaluated, and the stability of the photocatalyst activity and the influence of optimized irradiation waveforms were examined in the decolorization of 400 mL of 10 ppm AO7 solution. The sinusoidal modulation, with current between 50 and 100 mA and 10 s as the period, shows the highest value of the apparent pseudo-first-order kinetic constant, resulting equal to 0.0044 min-1, at parity of total transmitted photons. An energy saving with the application of sinusoidal irradiation is highlighted with respect to the literature.


Subject(s)
Light , Titanium , Titanium/chemistry , Azo Compounds/chemistry , Catalysis
8.
Chemosphere ; 309(Pt 1): 136534, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36210593

ABSTRACT

In this study, a ternary layered double hydroxide containing Zn, Co, and Fe transition metals (ZnCoFe LDH) was developed using a co-precipitation procedure. The as-synthesized photocatalyst was evaluated for its performance in the degradation of methylene blue (MB) under visible light irradiation. The effects of various process conditions including photocatalyst dosage, pollutant concentration, pH, lamp distance, and lamp power were investigated. The ZnCoFe LDH achieved approximately 74% photodegradation efficiency owing to the narrow bandgap of 2.14 eV. The Langmuir-Hinselwood rate constants were calculated as 1.17 min-1 and 3.55 min-1 for photolysis by LED lamp alone and for photocatalysis by LED/ZnCoFe LDH, respectively. The photocatalytic ability of the LDH was attributed to the generation of radical species like •OH and O2•-. The photocatalytic degradation intermediates of MB were determined by GC-MS analysis. The catalyst retained its performance throughout seven reuse cycles with only a 4.17% reduction in removal efficiency. The energy per order EEO of the ZnCoFe/LED process in 180 min treatment time was determined as 5.41 kWh.m-3. order-1. This study shows that ZnCoFe LDH has sufficient activity and photostability for long-term application in photocatalytic water treatment.


Subject(s)
Environmental Pollutants , Water Purification , Methylene Blue , Hydroxides , Light , Catalysis
9.
Sci Total Environ ; 844: 157162, 2022 Oct 20.
Article in English | MEDLINE | ID: mdl-35798102

ABSTRACT

The binding between water components (dissolved organic matters, anions and cations) and pharmaceuticals influences the migration and transformation of pollutants. Herein, the impact of water matrices on drug degradation, as well as the electrical energy demands during UV, UV/catalysts, UV/O3, UV/H2O2-based, UV/persulfate and UV/chlorine processes were systemically evaluated. The enhancement effects of water constituents are due to the powerful reactive species formation, the recombination reduction of electrons and holes of catalyst and the catalyst regeneration; the inhibition results from the light attenuation, quenching effects of the excited states of target pollutants and reactive species, the stable complexations generation and the catalyst deactivation. The transformation pathways of the same pollutant in various AOPs have high similarities. At the same time, each oxidant also can act as a special nucleophile or electrophile, depending on the functional groups of the target compound. The electrical energy per order (EEO) of drugs degradation may follow the order of EEOUV > EEOUV/catalyst > EEOUV/H2O2 > EEOUV/PS > EEOUV/chlorine or EEOUV/O3. Meanwhile, it is crucial to balance the cost-benefit assessment and toxic by-products formation, and the comparison of the contaminant degradation pathways and productions in the presence of different water matrices is still lacking.


Subject(s)
Water Pollutants, Chemical , Water Purification , Chlorine , Hydrogen Peroxide/chemistry , Kinetics , Oxidation-Reduction , Pharmaceutical Preparations , Ultraviolet Rays , Water , Water Pollutants, Chemical/analysis , Water Purification/methods
10.
Environ Pollut ; 308: 119673, 2022 Sep 01.
Article in English | MEDLINE | ID: mdl-35760199

ABSTRACT

Antibiotics are emerging contaminants in aquatic environments which pose serious risks to the ecological environment and human health. Advanced oxidation processes (AOPs) based on ultraviolet (UV) light have good application prospects for antibiotic degradation. As new and developing UV-AOPs, UV/chlorine and derived UV/chloramine processes have attracted increasing attention due to the production of highly reactive radicals (e.g., hydroxyl radical, reactive chlorine species, and reactive nitrogen species) and also because they can provide long-lasting disinfection. In this review, the main reaction pathways of radicals formed during the UV/chlor (am)ine process are proposed. The degradation efficiency, influencing factors, generation of disinfection by-products (DBPs), and changes in toxicity that occur during antibiotic degradation by UV/chlor (am)ine are reviewed. Based on the statistics and analysis of published results, the effects caused by energy consumption, defined as electrical energy per order (EE/O), increase in the following order: UV/chlorine < UV/peroxydisulfate (PDS)< UV/H2O2 < UV/persulfate (PS) < 265 nm and 285 nm UV-LED/chlorine (EE/O). Some inherent problems that affect the UV/chlor (am)ine processes and prospects for future research are proposed. The use of UV/chlor (am)ine AOPs is a rich field of research and has promising future applications, and this review provides a theoretical basis for that.


Subject(s)
Water Pollutants, Chemical , Water Purification , Anti-Bacterial Agents , Chlorine , Disinfection/methods , Humans , Hydrogen Peroxide , Oxidation-Reduction , Ultraviolet Rays , Water Pollutants, Chemical/analysis , Water Purification/methods
11.
Water Res ; 217: 118442, 2022 Jun 15.
Article in English | MEDLINE | ID: mdl-35429888

ABSTRACT

Antidepressants are released into the aquatic environment because of their incomplete removal from wastewater treatment plants. In the present work, we investigated the photochemical degradation of a commonly prescribed antidepressant, namely sertraline, in aqueous matrices. The molar absorption coefficient of sertraline at 254 nm and at various pH values in the range from 4.0 to 9.0 was 444±65 L•mol-1•cm-1, while the quantum yield of its direct photolysis under UVC radiation (λ = 254 nm) was (1.7±0.1) × 10-2 mol∙einstein-1 (i.e., both values were relatively low). Next, we investigated the photochemical degradation of sertraline under UVC radiation in the presence of hydrogen peroxide, H2O2 (i.e., UVC/H2O2) or persulfate ions, S2O82- (i.e., UVC/PS). Several parameters were studied, such as the initial concentrations of the oxidants, solution pH, and the composition of the aqueous matrix (experiments were carried out in aqueous phosphate buffers, in synthetic wastewater, as well as in synthetic fresh and hydrolyzed human urine). It was found that, in all aqueous matrices, the photochemical degradation of sertraline followed pseudo first-order kinetics. The values of the observed pseudo first-order rate constants in the UVC/H2O2 and UVC/PS processes were from one to three orders of magnitude higher than the corresponding value in the UVC process. The UVC/PS process was more efficient than the UVC/H2O2 process, either in aqueous phosphate buffer solutions or in synthetic wastewaters, despite the comparable reactivity of sertraline towards hydroxyl and sulfate radicals. However, both processes resulted in partial mineralization of the compound after prolonged irradiation. In the UVC/H2O2 process, there was an optimum H2O2 concentration which depended on the aqueous matrix, while in the UVC/PS process, there was an almost linear increase in treatment efficiency as a function of PS concentration, at least in the range of concentrations studied in the present work. Solution pH in the range from 6.0 to 9.0 had a relatively negligible effect on treatment performance for both processes. In synthetic urine matrices, despite the reduction in reaction rate (the observed pseudo first-order rate constants were reduced by approximately one to two orders of magnitude), the photochemical degradation of sertraline proceeded to a relatively satisfactory degree. Finally, the calculations of the electrical energy per order and the associated cost showed that the UVC/H2O2 and UVC/PS processes are cost-efficient and suitable for full-scale applications.


Subject(s)
Hydrogen Peroxide , Water Pollutants, Chemical , Antidepressive Agents , Humans , Hydrogen Peroxide/chemistry , Kinetics , Oxidation-Reduction , Phosphates , Sertraline , Ultraviolet Rays , Wastewater , Water , Water Pollutants, Chemical/chemistry
12.
Sci Total Environ ; 832: 154804, 2022 Aug 01.
Article in English | MEDLINE | ID: mdl-35341856

ABSTRACT

The oil sands industry generates large volumes of oil sands process water (OSPW). There is an urgent need for OSPW treatment to reduce process water inventories and to support current reclamation approaches. This study discusses how efficient ozone (O3)-based combined advanced oxidation processes (AOPs), including hydrogen peroxide (H2O2) and UV-C, are at achieving mineralization while reducing the toxicity arising from such organic components as naphthenic acids (NAs) in OSPW. The results showed that the dissolved organic carbon (DOC) removals of 45%, 84%, 84% and 98%, obtained after 90-min treatments with O3, O3/H2O2, UVC/O3 and UVC/O3/H2O2, respectively, at a production rate of 6 g/L·h O3 were considerably higher than at lower O3 production rates. The acute toxicity on Vibrio fischeri was significantly reduced by all the treatments, which explains the high percentages of NA removal (up to 99% as confirmed by UPLC-QTOF-HRMS.) Mineralization (expressed as DOC removal) was highest with UVC/O3/H2O2 at ca. 2 mg C/L in the treated effluent, which means that it could be used as cooling/boiling process water in bitumen upgrading units. However, considering the energy demand of the treatments tested, the treatment using O3/H2O2 was found to be the most realistic for large-scale applications.


Subject(s)
Ozone , Water Pollutants, Chemical , Water Purification , Carboxylic Acids , Hydrogen Peroxide , Oil and Gas Fields , Water , Water Pollutants, Chemical/analysis , Water Purification/methods
13.
Chemosphere ; 287(Pt 2): 132099, 2022 Jan.
Article in English | MEDLINE | ID: mdl-34509761

ABSTRACT

Photocatalytic activation of peroxymonosulfate (PMS) by graphitic carbon nitride (g-C3N4) is emerging as a sulfate radical anion based advanced oxidation process (S-AOP) for degradation of organic pollutants. Importantly, photocatalytic activation of PMS by g-C3N4 is energy intensive as light irradiation requires high electrical energy. Here, we studied activation of PMS by g-C3N4 under 400 nm light emitting diode (LED) irradiation (g-C3N4/PMS/400-LED system) for degradation of Acid Orange 7 (AO7). LED array having optical emission maximum around 400 nm (FWHM = 16 nm), with electrical input power of 1.54 W (14 V and 110 mA) was used for irradiation. Pseudo-first order rate constant (kobs) value for degradation of AO7 by g-C3N4/PMS/400-LED system was determined to be 0.094 min-1. O2·-, SO4·- were revealed by radical scavenging and ESR investigations. kobs value in simulated ground and real tap water were determined to be 0.068 min-1 and 0.063 min-1, respectively. g-C3N4 was stable, and reused four times without any significant loss in its photocatalytic activity. Importantly, electrical energy per order (EEO) for degradation of AO7 by g-C3N4/PMS/400-LED system was determined to be 24.51 kWh m-3 order-1. In contrast, the EEO value for the degradation of AO7 by g-C3N4 activated PMS under visible light irradiation (>400 nm), using conventional xenon lamp, (g-C3N4/PMS/Vis-Xe system) was found to be very high as 2702 kWh m-3 order-1. Thus, the study highlights, LED irradiation source is promising for the development of energy efficient g-C3N4 photocatalytic activation of PMS for removal of organic pollutants.


Subject(s)
Conservation of Energy Resources , Peroxides , Azo Compounds , Benzenesulfonates , Light
14.
Chemosphere ; 279: 130876, 2021 Sep.
Article in English | MEDLINE | ID: mdl-34134436

ABSTRACT

Conventional wastewater treatment processes cannot effectively remove dissolved organic nitrogen (DON) and soluble non-reactive phosphorus (sNRP), which can pose regulatory compliance challenges for total nitrogen and total phosphorus discharges. Moreover, DON and sNRP are not easily recoverable for beneficial reuse as part of the waste to resource paradigm. Conversion of DON and sNRP to more readily removable dissolved inorganic nitrogen (DIN) and soluble reactive phosphorus (sRP), respectively, will help meet stringent nutrient limits and facilitate nutrient recovery. In this study, electro-oxidation (EO) was evaluated for conversion of four DON compounds to DIN and five sNRP compounds to sRP. EO was more efficient and provided higher extents of conversion of the recalcitrant nutrient fractions compared to a more traditional advanced oxidation process, UV/H2O2. Direct electron transfer was likely the dominant oxidation mechanism for EO-based DON and sNRP conversion, with DON being more recalcitrant. Among the DON compounds tested, greater availability of primary amine (C-N bonds) yielded greater conversion compared to compounds with fewer primary amine or those with secondary amine (C-N-C bond). Among the sNRP compounds tested, those with P-O-C bonds (organic sNRP) converted more readily than those with P-O-P bonds (inorganic sNRP), presumably because cleavage of the latter bond requires greater energy. Using 30 min of EO treatment, the highest DON and sNRP compound conversion was 11.7 ± 0.09% for urea and 31.1 ± 0.75% for beta-glycerol phosphate. A similar extent of EO-based conversion of DON (6.41 ± 1.5%) and sNRP (32.7 ± 3.3%) was observed in real wastewater.


Subject(s)
Phosphorus , Water Purification , Hydrogen Peroxide , Nitrogen/analysis , Wastewater
15.
Chemosphere ; 273: 129377, 2021 Jun.
Article in English | MEDLINE | ID: mdl-33517114

ABSTRACT

In-situ water treatment can be accomplished using electrochemical treatments such as electrocoagulation (EC), which generates coagulants, and electrooxidation (EO), which generates oxidants (e.g., free chlorine and reactive oxygen species) via electrolysis using boron-doped diamond electrodes. In sequential EC-EO, EC can remove oxidant scavengers present in dissolved organic carbon (DOC), thereby improving the efficacy of downstream oxidation via EO. This study evaluated sequential EC-EO (and each process independently for comparison) for mitigating the trace organic compounds (TOrCs) acyclovir (ACY), trimethoprim (TMP), and benzyldimethyldecylammonium chloride (BAC-C10) in model groundwaters and surface waters. EO-only removed greater than 70% of ACY and TMP but negligible BAC-C10 in model groundwaters. In model surface waters, EO-only removed ∼55-75% BAC-C10, but had less removal for ACY and TMP (∼20-55%), primarily due to DOC interference. Sequential-EC-EO was investigated to better gauge the potential process improvement due to the addition of EC ahead of EO. EC removed 74 ± 7% DOC from model surface water and improved downstream EO treatment relative to EO-only by a factor of 3.4 for ACY, 1.7 for TMP, and 1.4 for BAC-C10. When treating model groundwater, EC-EO resulted in no improvement compared to EO-only for ACY and TMP. BAC-C10 removal was attributed to the particle separation step between EC and EO rather than electrochemical inputs. EO-only treatment was more energy efficient for model groundwater compared to model surface waters based on electrical energy per order (EEO) values. Sequential EC-EO further improved the energy efficiency for treating model river water.


Subject(s)
Drinking Water , Water Pollutants, Chemical , Water Purification , Diamond , Electrocoagulation , Electrodes , Oxidation-Reduction , Waste Disposal, Fluid , Water Pollutants, Chemical/analysis
16.
Chem Eng J ; 398: 125570, 2020 Oct 15.
Article in English | MEDLINE | ID: mdl-32508521

ABSTRACT

The UV-induced advanced oxidation processes (AOPs, including UV/Cl2, UV/NH2Cl, UV/ClO2 and UV/H2O2 ) degradation kinetics and energy requirements of iopamidol as well as DBPs-related toxicity in sequential disinfection were compared in this study. The photodegradation of iopamidol in these processes can be well described by pseudo-first-order model and the removal efficiency ranked in descending order of UV/Cl2  > UV/H2O2  > UV/NH2Cl > UV/ClO2  > UV. The synergistic effects could be attributed to diverse radical species generated in each system. Influencing factors of oxidant dosage, UV intensity, solution pH and water matrixes (Cl- , NH4 + and nature organic matter) were evaluated in detail. Higher oxidant dosages and greater UV intensities led to bigger pseudo-first-order rate constants (Kobs) in these processes, but the pH behaviors exhibited quite differently. The presence of Cl- , NH4 + and nature organic matter posed different effects on the degradation rate. The parameter of electrical energy per order (EE/O) was adopted to evaluate the energy requirements of the tested systems and it followed the trend of UV/ClO2  > UV > UV/NH2Cl > UV/H2O2  > UV/Cl2 . Pretreatment of iopamidol by UV/Cl2 and UV/NH2Cl clearly enhanced the production of classical disinfection by-products (DBPs) and iodo-trihalomethanes (I-THMs) during subsequent oxidation while UV/ClO2 and UV/H2O2 exhibited almost elimination effect. From the perspective of weighted water toxicity, the risk ranking was UV/NH2Cl > UV/Cl2 > UV > UV/H2O2 > UV/ClO2 . Among the discussed UV-driven AOPs, UV/Cl2 was proved to be the most cost-effective one for iopamidol removal while UV/ClO2 displayed overwhelming advantages in regulating the water toxicity associated with DBPs, especially I-THMs. The present results could provide some insights into the application of UV-activated AOPs technologies in tradeoffs between cost-effectiveness assessment and DBPs-related toxicity control of the disinfected waters containing iopamidol.

17.
Water Res ; 173: 115581, 2020 Apr 15.
Article in English | MEDLINE | ID: mdl-32058153

ABSTRACT

This study provided an overview of established and emerging nanomaterial (NM)-enabled processes and devices for water disinfection for both centralized and decentralized systems. In addition to a discussion of major disinfection mechanisms, data on disinfection performance (shortest contact time for complete disinfection) and energy efficiency (electrical energy per order; EEO) were collected enabling assessments firstly for disinfection processes and then for disinfection devices. The NM-enabled electro-based disinfection process gained the highest disinfection efficiency with the lowest energy consumption compared with physical-based, peroxy-based, and photo-based disinfection processes owing to the unique disinfection mechanism and the direct mean of translating energy input to microbes. Among the established disinfection devices (e.g., the stirred, the plug-flow, and the flow-through reactor), the flow-through reactor with mesh/membrane or 3-dimensional porous electrodes showed the highest disinfection performance and energy efficiency attributed to its highest mass transfer efficiency. Additionally, we also summarized recent knowledge about current and potential NMs separation and recovery methods as well as electrode strengthening and optimization strategies. Magnetic separation and robust immobilization (anchoring and coating) are feasible strategies to prompt the practical application of NM-enabled disinfection devices. Magnetic separation effectively solved the problem for the separation of evenly distributed particle-sized NMs from microbial solution and robust immobilization increased the stability of NM-modified electrodes and prevented these electrodes from degradation by hydraulic detachment and/or electrochemical dissolution. Furthermore, the study of computational fluid dynamics (CFD) was capable of simulating NM-enabled devices, which showed great potential for system optimization and reactor expansion. In this overview, we stressed the need to concern not only the treatment performance and energy efficiency of NM-enabled disinfection processes and devices but also the overall feasibility of system construction and operation for practical application.


Subject(s)
Nanostructures , Water Purification , Disinfection , Electrodes , Hydrodynamics , Water
18.
J Hazard Mater ; 362: 238-245, 2019 01 15.
Article in English | MEDLINE | ID: mdl-30240998

ABSTRACT

The emergence of micropollutants into our aquatic resources is regarded as an issue of increasing environmental concern. To protect the aquatic environment against further contamination with micropollutants, treatment with advanced oxidation processes (AOPs) is put forward as a promising technique. In this work, an innovative AOP based on electrical discharges in a continuous-flow pulsed dielectric barrier discharge (DBD) reactor with falling water film over activated carbon textile is examined for its potential application in water treatment. The effect of various operational parameters including feed gas type, gas flow rate, water flow rate and power on removal and energy efficiency has been studied. To this end, a synthetic micropollutant mixture containing five pesticides (atrazine, alachlor, diuron, dichlorvos and pentachlorophenol), two pharmaceuticals (carbamazepine and 1,7-α-ethinylestradiol), and 1 plasticizer (bisphenol A) is used. While working under optimal conditions, energy consumption was situated in the range 2.42-4.25 kW h/m³, which is about two times lower than the economically viable energy cost of AOPs (5 kW h/m³). Hence, the application of non-thermal plasma could be regarded as a promising alternative AOP for (industrial) wastewater remediation.

19.
Water Res ; 139: 118-131, 2018 08 01.
Article in English | MEDLINE | ID: mdl-29631187

ABSTRACT

This study provides an overview of established processes as well as recent progress in emerging technologies for advanced oxidation processes (AOPs). In addition to a discussion of major reaction mechanisms and formation of by-products, data on energy efficiency were collected in an extensive analysis of studies reported in the peer-reviewed literature enabling a critical comparison of various established and emerging AOPs based on electrical energy per order (EEO) values. Despite strong variations within reviewed EEO values, significant differences could be observed between three groups of AOPs: (1) O3 (often considered as AOP-like process), O3/H2O2, O3/UV, UV/H2O2, UV/persulfate, UV/chlorine, and electron beam represent median EEO values of <1 kWh/m3, while median energy consumption by (2) photo-Fenton, plasma, and electrolytic AOPs were significantly higher (EEO values in the range of 1-100 kWh/m3). (3) UV-based photocatalysis, ultrasound, and microwave-based AOPs are characterized by median values of >100 kWh/m3 and were therefore considered as not (yet) energy efficient AOPs. Specific evaluation of 147 data points for the UV/H2O2 process revealed strong effects of operational conditions on reported EEO values. Besides water type and quality, a major influence was observed for process capacity (lab-vs. pilot-vs. full-scale applications) and, in case of UV-based processes, of the lamp type. However, due to the contribution of other factors, correlation of EEO values with specific water quality parameters such as UV absorbance and dissolved organic carbon were not substantial. Also, correlations between EEO and compound reactivity with OH-radicals were not significant (photolytically active compounds were not considered). Based on these findings, recommendations regarding the use of the EEO concept, including the upscaling of laboratory results, were derived.


Subject(s)
Waste Disposal, Fluid/methods , Water Pollutants, Chemical/chemistry , Water Purification/methods , Oxidation-Reduction , Wastewater/chemistry
20.
Water Res ; 109: 207-216, 2017 Feb 01.
Article in English | MEDLINE | ID: mdl-27889622

ABSTRACT

A dual-wavelength UV-C LED unit, emitting at peaks of 260 nm, 280 nm, and the combination of 260|280 nm together was evaluated for its inactivation efficacy and energy efficiency at disinfecting Escherichia coli, MS2 coliphage, human adenovirus type 2 (HAdV2), and Bacillus pumilus spores, compared to conventional low-pressure and medium-pressure UV mercury vapor lamps. The dual-wavelength unit was also used to measure potential synergistic effects of multiple wavelengths on bacterial and viral inactivation and DNA and RNA damage. All five UV sources demonstrated similar inactivation of E. coli. For MS2, the 260 nm LED was most effective. For HAdV2 and B. pumilus, the MP UV lamp was most effective. When measuring electrical energy per order of reduction, the LP UV lamp was most efficient for inactivating E. coli and MS2; the LP UV and MP UV mercury lamps were equally efficient for HAdV2 and B. pumilus spores. Among the UV-C LEDs, there was no statistical difference in electrical efficiency for inactivating MS2, HAdV2, and B. pumilus spores. The 260 nm and 260|280 nm LEDs had a statistical energy advantage for E. coli inactivation. For UV-C LEDs to match the electrical efficiency per order of log reduction of conventional LP UV sources, they must reach efficiencies of 25-39% or be improved on by smart reactor design. No dual wavelength synergies were detected for bacterial and viral inactivation nor for DNA and RNA damage.


Subject(s)
Disinfection , Escherichia coli , Humans , Levivirus , Ultraviolet Rays , Water Purification
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