Advanced treatment of digested restaurant wastewater using a combination of anaerobic/oxic unit, Fenton, and a biological aerated filter in pilot-scale treatment

doi:10.21203/rs.3.rs-1840491/v1

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Advanced treatment of digested restaurant wastewater using a combination of anaerobic/oxic unit, Fenton, and a biological aerated filter in pilot-scale treatment

https://doi.org/10.21203/rs.3.rs-1840491/v1

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Biological treatment is the most economical and practical wastewater treatment method; however, for highly concentrated organic wastewater, such as digested restaurant wastewater, a single biological treatment method does not meet the discharge requirements. An anaerobic/oxic-Fenton-biological aerated filter (A/O-Fenton-BAF) system was employed to treat digested restaurant wastewater with a high concentration of organic compounds in a pilot-scale experiment. The degradation process and mechanism of chemical oxygen demand (COD), total nitrogen (TN), NH₄⁺-N, NO₃⁻-N, and dissolved organic nitrogen (DON) in each stage of the process were analyzed. Gas chromatography-mass spectrometry and fluorescence spectrum characteristics were also studied. The average removal rate of both COD and NH₄⁺-N in the entire process was 98%. The removal rates of COD, TN, NH₄⁺-N, and DON reached 78.5%, 66.0%, 95.3%, and 51% using the A/O unit. Although Fenton was ineffective in the removal of nitrogenous organic and inorganic substances, the fluorescence spectra and GC-MS showed that the nitrogen-containing organic compounds of macromolecules were transformed into small molecules after the Fenton reaction and could be removed by the BAF unit. The removal rate of DON was up to 24.3% in the Fenton + BAF process, which reduced the TN concentration in the effluent. The dominant species in all biological processes were nitrifying and organic matter-decomposing bacteria. This study provides key data for the design of a full-scale system for treating digested restaurant wastewater.

digested restaurant wastewater

Fenton process

nitrogen

COD

A/O

BAF

China has built more than a dozen cities with a population of tens of millions owing to rapid urbanization. Furthermore, large agglomerations of urban residents have resulted in the expansion of the catering industry of these cities, which is growing by approximately 18% per year, twice as fast as the gross domestic product. This sudden growth has triggered complex environmental problems mainly pertaining to kitchen waste. According to statistics, the annual output of kitchen waste in China is about 1.2 × 10⁹ t, and the trend of rapid growth is maintained (Gao et al. 2022). To manage the ensuing large amounts of kitchen waste, China has designated several pilot cities to focus on the harmless treatment of kitchen waste resources for the centralized treatment of kitchen waste. A large amount of kitchen wastewater is generated after solid–liquid separation and the removal of high chemical oxygen demand (COD), salinity, ammonia nitrogen, and oil and grease from most of the oils and fats (Kaushik et al. 2015; Joonveob et al. 2016; Geng and Wang 2019). Currently, most kitchen wastewater is treated by anaerobic digestion; however, the digested wastewater still contains high COD concentrations, NH₄⁺-N, and total nitrogen (TN). Although some studies have been conducted on environmental pollution control for the treatment of restaurant wastewater or digested wastewater, such as membrane bioreactor, anaerobic digestion, electroflocculation, and advanced oxidation technologies (Wang et al. 2014; Feng et al. 2016; Zhu et al. 2019), there are still technical limitations on how to treat such large-scale digested restaurant wastewater cost-effectively and harmlessly.

Digested restaurant wastewater contains high concentrations of organic matter, nitrogen, and phosphorus, which can be easily degraded by microorganisms. Hence, biological nitrogen- and phosphorus-removal processes, such as anaerobic/oxic (A/O) and biological aerated filter (BAF), are the most simple and effective methods to treat digested restaurant wastewater (Zeng et al. 2018; Gabarró et al. 2019; Gao et al. 2017). Such processes have the advantages of low operational costs, low susceptibility to sludge filamentous expansion, strong resistance to shock loading, and ease of automation and management. In our preliminary experiments, we attempted to achieve discharge standards of digested restaurant wastewater using only biological treatment, especially when TN concentrations are high; however, the results were not encouraging.

Advanced oxidation processes offer considerable advantages for the degradation of highly concentrated organic wastewater (Klavarioti et al. 2009; Sirés et al. 2014; Li et al. 2022). In 1894, a French scientist, Fenton, presented a novel process—known as the Fenton process—for analyzing reduced organic substances and oxidants. H₂O₂ decomposes under the catalytic effect of Fe²⁺ to produce -OH, which oxidizes and decomposes organic matter into intermediates with lower molecular weight through electron transfer and other pathways. Furthermore, Fe²⁺ is oxidized to Fe³⁺ to produce flocculation precipitation, which can remove a large amount of organic matter. The Fenton process, as an advanced oxidation technology, is widely used in the deep treatment of organic wastewater because of its simple operation and rapid reaction time (Wookeun et al. 2015). In practical engineering, a small amount of the Fenton reagent is often used for the pretreatment of industrial wastewater to partially oxidize the hard-to-degrade organic substances in the wastewater and change their biochemical properties, solubility, and coagulation performance for subsequent treatment (Bae et al. 2015; Li et al., 2016; Wu et al. 2017).

Based on previous studies, a combined A/O-Fenton-BAF process was developed in this study. The aim of this study was to effectively reduce nutrients, such as nitrogen and phosphorus, in the wastewater and improve the effluent water quality. The performance of the combined process for COD and ammonia nitrogen removal from digested restaurant wastewater was investigated, and the organic constituents in each section were identified using gas chromatography-mass spectrometry (GC-MS) and excitation–emission matrix (EEM). Functional bacterial populations in A/O and BAF reactors were analyzed to investigate the biological characteristics in the combined process. The results of the present study can provide an engineering perspective for the treatment of digested municipal restaurant wastewater.

Wastewater and inoculated activated sludge

The wastewater used in the present study comprised mixed liquor that was discharged from an anaerobic digestion tank in a kitchen waste treatment plant in Changsha, Hunan Province (South China). The general characteristics of the raw wastewater were as follows: COD, 3000–8000 mg·L^− 1; NH₄⁺-N, 600–1500 mg·L^− 1; TN, 1200–2000 mg·L^− 1; and pH, 7.0–8.2. The activated sludge inoculated in the pilot A/O unit and BAF unit was also obtained from the aeration tank of the same waste treatment plant.

Experimental system

The pilot-scale unit consisted of process units such as a raw water storage tank, A/O unit (8.9 m³), BAF unit (0.5 m³), Fenton reactor, and discharge tank with supporting piping and electrical control devices. The configuration of the pilot-scale unit is shown in Fig. 1 and the set of equipment used for pilot testing is shown in Fig. 2. The flow rate of the A/O was 40 L/h and the hydraulic retention time of A/O and BAF was 9 d and 10 h, respectively. The dissolved oxygen (DO) in value A and O and the BAF unit was approximately 0.3–0.5, 1.5–2.5, and 3.0–5.0 mg/L, respectively.

Analytical methods

The pilot unit was operated for 6 months, and the influent and effluent waters of each functional unit were regularly collected, analyzed, and tested during the stabilization period. The DO and pH of wastewater in the reactor were recorded daily using a portable DO/pH meter (HQ20; Hach, Loveland, USA). The COD was measured using a COD speed measuring device (CTL-12; Huatong Inc., Chengde, China). The NH₄⁺-N concentration was measured using a spectrophotometer (8453; Agilent, Palo Alto, USA) according to Messler’s reagent spectrometry. The TN and NO₃⁻N concentrations were measured using alkaline potassium persulfate-UV spectrophotometry and phenol two sulfonic acid photometric method (State Environmental Protection Administration of China 2002), respectively. Dissolved organic nitrogen (DON) was calculated by subtracting total inorganic nitrogen content (TIN) from TN content (Kong et al. 2016).

Process set-up

Anaerobic/oxic set-up

First, 9 m³ of sludge was inoculated in the A/O process. As the inoculated activated sludge was obtained from the kitchen waste treatment plant, undiluted original wastewater was fed into the A/O unit. The flow rate was 21 L/h, A/O temperature was 25°C, and sludge reflux ratio was 100%. The COD, MLSS, SV, and SVI of the A/O system were monitored, and the microbial growth phase in the reactor was investigated. When the effluent COD was stable and activated sludge was normal, the startup process lasted 30 d.

BAF set-up

BAF startup was performed simultaneously with the A/O system startup. Inoculated activated sludge was the same as that in the A/O system. After 7 d of aeration, water was continuously fed in the BAF, and the flow rate was gradually increased (5, 10, and 15 L/h). After 18 d, the inlet water flow rate was adjusted to 20 L/h, and the aeration rate was 173 L/h. After 40 d, the COD and nitrogen removal rate remained stable, and the microscopic examination showed rotifers, nematodes, clostridia, and a small amount of filamentous bacteria.

Fenton experiments

Fenton performance has been mainly investigated according to variations in the initial pH, concentration of H₂O₂ and Fe²⁺, and reaction time (Li et al. 2016; Xu et al. 2017). In this study, an L₁₆(4⁴) orthogonal experiment was designed, and the results were analyzed. Thereafter, a single-factor test was conducted. The optimal reaction conditions were as follows: H₂O₂ concentration, 100 mg/L; Fe²⁺ concentration, 300 mg/L; initial pH, 5; and reaction time, 60 min.

Determination and analysis of microbial community structure

Sludge was obtained from the A/O and BAF systems of the pilot plant, and the sludge used as a comparison sample was also obtained from the aeration tank in the combined kitchen wastewater treatment station. All samples were transported on dry ice to Biotech Bioengineering (Shanghai) Co. for characterizing the variations in microbial communities using Illumina Miseq sequencing. The total DNA was extracted and amplified using an OMEGA kit (Omega Bio-Tek, Norcross, GA, USA). The primers used for polymerase chain reaction were fused with the V3–V4 universal primers of the Miseq sequencing platform. The V3–V4 region of the 16S rRNA genes was amplified using primer pair 5´-ACTCCTACGGGAGGCAGCAG-3´ and 5´-GGAC-TACHVGGGTWTCTAAT-3´.

Gas chromatography-mass spectrometry

The organic compounds in the waters were analyzed using electron impact gas chromatography-mass spectrometry (EI-GC-MS7890A/5977C; Agilent, Palo Alto, USA; EI mode at 70 eV). The GC conditions were as follows: inlet temperature, 280°C; gas interface temperature, 250°C; carrier gas flow rate, 1.5 mL/min; injection volume, 1 µL; and shunt ratio, 1:1. Samples were heated initially at 40°C, maintained for 4 min, and then heated to 270°C at a rate of 10°C/min and maintained for 20 min. The samples were then heated to 290°C at a rate of 10°C/min and maintained for 10 min. The MS conditions were as follows: ion source temperature, 230°C; quadrupole temperature, 150°C; EI ionization, 70 eV; and full scan, 35–550 da.

Spectrum analysis

3DMM fluorescence spectroscopy was employed to measure the concentrations of organic compounds using a Hitachi F-4600 fluorescence spectrometer (F-4600; Hitachi, Ltd, Tokyo, Japan). All samples were tested with the subsequent scanned emission wavelength (Em) range of 220–500 nm and the excitation wavelength (Ex) range of 200–500 nm with a step size of 10 nm; the scanning speed of the spectrum was 12,000 nm/min and the bandwidth of emission and excitation was 5 nm.

Process operation analysis

COD removal performance

When the system was stably operated, the combined process was operated for 134 d according to the set operating conditions; the activated sludge performance of the system was stable, and the effluent quality was relatively stable (Fig. 3). The COD in the influent of the pilot plant fluctuated between 3600 and 7400 mg/L, with an average concentration of 5568 mg/L. The average COD in the effluent was 121 mg/L, which satisfied the concentration limit of the Comprehensive Wastewater Discharge Standard of China (COD concentration < 150 mg/L), and the COD in some periods was < 100 mg/L. The average COD removal rate reached 98%.

The COD decreased from an average of 5568 to 1195 mg/L (Fig. 4). The highest COD removal efficiency was achieved in the A/O unit, with a removal rate of approximately 78.5%. Furthermore, the COD-removal rates were 69.8% and 66.3% in the Fenton and BAF units, respectively. According to the degradation effect of COD during the process shown in Fig. 4, the strong oxidation effect of the Fenton process resulted in high COD removal in the BAF unit. This combined process can accomplish wastewater treatment goals more effectively than a single biological treatment process.

NH₄⁺-N removal performance

The influent NH₄⁺-N concentration of the pilot plant fluctuated between 660 and 1280 mg/L, with an average concentration of 943 mg/L. The average concentration of effluent NH₄⁺-N was 12.6 mg/L after treatment (Fig. 5). which met the most stringent standard of the combined wastewater discharge standard of China (NH₄⁺-N concentration < 15 mg/L). However, it was > 15 mg/L on days 105–125, which may be because of the increase in the activated sludge temperature during operation. Days 105–125 were within the highest average summer temperature period, during which the water temperature of the A/O unit reached 35–37°C. The high temperature reduced the activity and proliferation rate of nitrifying bacteria and decreased the NH₄⁺-N-removal rate. The NH₄⁺-N-removal rate quickly increased again to a stable state after the adjustment of device temperature.

Nitrogen-removal process

The change in the concentration of N along the process is shown in Fig. 6. The average concentrations of NH₄⁺-N, DON, and NO₃⁻-N, which comprised the TN, were 943, 777, and 10 mg/L, respectively. In the A/O unit, the average effluent NH₄⁺-N concentration was 44.5 mg/L, and the average NH₄⁺-N-removal rate was 95.3%. The degradation of DON in the A/O unit mainly occurred in the A tank, with a removal rate of 51%, and DON removal in the O-tank was not evident. There was 66% TN removal in the A/O unit. As the main process of TN removal, the A/O unit released NH₄⁺-N into the atmosphere as nitrogen through nitrification and denitrification, whereas incompletely denitrified NH₄⁺-N remained in the water as NO₃⁻-N. Total nitrogen was composed of DON and NO₃⁻-N in the A/O effluent. The NO₃⁻-N concentration in the A/O effluent reached 315.6 mg/L, which may have been owing to incomplete denitrification with insufficient organic carbon in the A/O unit. After the Fenton process, the concentrations of DON, NO₃⁻-N, and TN decreased slightly, which showed that the Fenton process did not effectively remove nitrogenous organic and inorganic substances.

The average concentration of NH₄⁺-N in the effluent of the BAF unit was 12.6 mg/L. Both TN and DON concentrations decreased substantially in the effluent compared to those measured for the influent. This may be because of the strong oxidation effect of Fenton, which changed the structure of nitrogenous organic matter and converted it to substances suitable for biochemical treatment to be removed by BAF. Although the NO₃⁻-N concentration in the BAF effluent was reduced, it still reached 234 mg/L, accounting for 92.5% of the effluent TN. The DON accounted for 6% of the effluent TN.

Microbial population diversity analysis

High-throughput sequencing of microorganisms in the A/O anoxic zone, aerobic zone, and BAF reactor using the Miseq platform yielded 2252, 3133, and 3712 operational taxonomic units, respectively (Table 1), and the coverage indices of the three samples were 95%, 96%, and 96%, respectively. The results indicated that the bacterial library created using this high-throughput sequencing technology contained most bacteria in the system, and the sequencing results represented the actual situation of the samples. Ace and Chao indices were used to estimate the abundance of microbial populations; higher values indicated a higher abundance of microbial populations. The Shannon and Simpson indices were used to estimate the microbial diversity in the samples. Higher Shannon values indicated lower diversity of microbial populations and a larger proportion of dominant microorganisms in the total biomass. A comparison of the Shannon and Simpson indices of each bio-tank (Table 1) revealed that the microbial diversity results were similar for the A tank and O tank. Furthermore, the microbial diversity in the BAF unit was higher than that in the A/O unit.

Table 1

Species abundance and diversity of microbial communities in the A/O and BAF units
Sample	OTU	Shannon	Ace	Chao1	Coverage	Simpson
A tank	2252	4.58	19581.07	10033.84	0.95	0.05
O tank	3133	4.45	44991.82	20515.31	0.96	0.05
BAF	3712	5.39	41597.33	23076.76	0.96	0.02

OUT, operational taxonomic unit; BAF, biological aerated filter; A/O, anaerobic/oxic

Analysis of microbial structures and functional population

The taxonomic distribution at the phylum level is summarized in Fig. 7a. Bacteroidetes, Proteobacteria, Chloroflexi, and Planctomycetes, which are commonly found in biological wastewater treatment systems (Zeng et al. 2018; Zhao 2018; Ji et al. 2019), dominated all three samples. Bacteroidetes members are involved in refractory organic matter catabolism and polysaccharide metabolism (Tang et al. 2017; Huang et al. 2019). Chloroflexi members mainly use carbohydrates in wastewater as nutrient recharge and are also common companion members in anaerobic ammonia oxidation systems. Proteobacteria and Planctomycete members are considered denitrifying functional bacteria (Kragelund et al. 2007; Chen et al. 2013; Reino et al. 2016; Yang et al. 2017; Hester et al. 2018; Torresi et al. 2018). To further explore the evolution of the microbial population, the taxonomic distribution at the class, order, and family levels is summarized in Fig. 7b–d. The abundance and species of the dominant bacteria in the two installations in the A/O process did not differ substantially because of the sludge reflux factor; however, there were some differences in the BAF unit. At the family level, Comamonadaceae, Chitinophagaceae, and Cryomorphaceae were the main microbes in the A/O and BAF units, whereas Anaerolineaceae and Planctomycetaceae were only relatively abundant in the BAF unit. Both bacterial members have a denitrification function. Anaerolineaceae, as a representative family of the green bacterium, have the function of not only denitrification but also degradation of carbohydrates and organic matter (such as amino acids) produced by the decomposition of other bacteria (Li et al. 2009; Chaffron et al. 2010; Han et al. 2019). Here, the analysis of the structural composition of microbial populations revealed that the dominant species in the combined process had the function of degrading COD and TN.

Gas chromatography-mass spectrometry

The samples of raw wastewater and effluent of each unit were analyzed using GC-MS, and the organic composition and change pattern in each unit were obtained as shown in Fig. 8. Fifty-three organic species were detected in the feed water of the A/O unit, comprising several alcohols, ketones, acids, esters, and other long-chain organic compounds as well as aromatic heterocyclic organic compounds and nitrogen-containing heterocyclic compounds, among which p-methyl phenol, as an edible species, was abundant in the kitchen wastewater. After the A/O unit, the COD and nitrogen concentrations substantially decreased. The organic matter in the effluent decreased. Only 12 organics were detected, of which halogenated alkanes, alkanes, and olefins were the most abundant. There was no major change in the type and content of organics in the Fenton effluent; however, the percentage change in organic matter was calculated based on peak areas. Fenton only changed the structure of certain haloalkane organics and may have changed the structure of some halogenated alkane organics. The number of organic substances in the BAF effluent increased to > 20, and some organic substances such as 3-methyl-2-butanone and 2-chloro-2-methylbutane, which were predominant in water, were mostly degraded, and the organic matter of the hexadecane to eicosane series increased. Microbial metabolism in the biological treatment process produces a variety of organic metabolites such as urea, amino acids, DNA, peptides, and fulvic and humic acids (Cowie and Hedges 1992). The increase in organic species in the effluent should be related to abundant microbial metabolic activities in the BAF. These metabolic activities produce low-molecular microbial metabolites.

Excitation–emission matrix fluorescence spectroscopy characteristics

The EEM spectra of the influent and effluent of different units are presented in Fig. 9. The influent had clear peaks A (220–240/320–360 nm) and B (270–285/320–350 nm). In addition, in region C (250–300/425–450 nm), the fluorescence intensity was high, which was similar to that of A; however, no fluorescence peak appeared (Fig. 8a). According to the region division study of the fluorescence spectrum of EEMs, the A peaks may represent the matter generated by low-excitation wavelength tryptophan-like substances such as tyrosine, tryptophan, and aromatic proteins; the B peaks may represent the matter produced by tryptophan-like substances with high excitation wavelengths, such as tryptophan and its analogs and complexine and its analogs; and the C region may relate to the matter produced by the excitation of humic and fulvic acids and their analogs. Figure 8b shows the EEM profile of the A/O effluent, where the A and B peaks representing protein-like substances disappear and the fluorescence is enhanced in the C region. This means that the organic matter in the water changed after A/O biochemical treatment. Figure 8c and d show the EEM profiles of the Fenton and BAF effluents, respectively. The fluorescence intensity decreased after Fenton treatment, whereas the fluorescence was invisible after the BAF unit. This indicates that Fenton effectively changes the structure of protein and humic acid substances and facilitates the subsequent biochemical treatment.

The targeted goal of this work was to treat actual digested restaurant wastewater. Thus, the study had limitations in the choice of process; besides, a stable and efficient process is the primary choice. The pilot experiment of an innovative combination of the combined A/O-Fenton-BAF process operated for six months. Based on the experimental results of the present study, the following conclusions were drawn: First, the combined process exhibited effective removal effect in digested restaurant wastewater. The process operated stably, and when the influent COD and NH₄⁺-N concentrations were 3600–7400 and 660–1280 mg/L, the average effluent COD was 121 mg/L, and the average NH₄⁺-N concentration was < 15 mg/L. Second, the removal rates of COD, TN, NH₄⁺-N, and DON by the A/O unit were 78.5%, 66%, 95.3%, and 51%. Although nitrogenous organic and inorganic substances were not effectively removed by Fenton process, but the fluorescence spectra and GC-MS analysis showed that the nitrogen-containing organic compounds of macromolecules were transformed into small molecules after the Fenton reaction and could be removed by the BAF unit. The maximum-removal rate of DON was 24.3% in the Fenton + BAF process, which reduced the concentration of TN in the effluent. NO₃⁻-N was the main component of TN in the combined process effluent. Third, the microbial analysis of the combined process showed that the dominant species in the biological process were nitrifying and organic matter-decomposing bacteria, which was in good agreement with the pollutant treatment objectives. The increase in DON species in the combination process effluent was related to the abundance of microbial species in the BAF unit, and the metabolites of microorganisms may be the main cause of DON production. The findings of the present study have direct implications in improving the designs of digested municipal restaurant wastewater.

Acknowledgments

This work was supported by the Scientific Research Fund of Hunan Province [Grant number 2021JJ30450] and Hunan Provincial Key Research and Development Program [Grant numbers 2022SK2067 and 2020SK2042]. Author YIN Jiang has received research support from Hunan Normal University.

Funding: This work was supported by the Scientific Research Fund of Hunan Province [Grant number 2021JJ30450] and Hunan Provincial Key Research and Development Program [Grant numbers 2022SK2067 and 2020SK2042]. Author YIN Jiang has received research support from Hunan Normal University.

Competing interests: The authors have no relevant financial or non-financial interests to disclose.

Availability of data and materials: Not applicable.

Author contributions: All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by JIANG Jianghong, TANG Qingchang, and PENG Xin. The first draft of the manuscript was written by YIN Jiang and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

Ethical approval: Not applicable.

Informed consent: Not applicable.

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Advanced treatment of digested restaurant wastewater using a combination of anaerobic/oxic unit, Fenton, and a biological aerated filter in pilot-scale treatment

Status:

Version 1

Abstract

Figures

Introduction

Material And Methods

Wastewater and inoculated activated sludge

Experimental system

Analytical methods

Process set-up

Anaerobic/oxic set-up

BAF set-up

Fenton experiments

Determination and analysis of microbial community structure

Gas chromatography-mass spectrometry

Spectrum analysis

Results And Discussion

Process operation analysis

COD removal performance

NH₄⁺-N removal performance

Nitrogen-removal process

Microbial population diversity analysis

Analysis of microbial structures and functional population

Gas chromatography-mass spectrometry

Excitation–emission matrix fluorescence spectroscopy characteristics

Conclusions

Declarations

References

Status:

Version 1

Advanced treatment of digested restaurant wastewater using a combination of anaerobic/oxic unit, Fenton, and a biological aerated filter in pilot-scale treatment

Status:

Version 1

Abstract

Figures

Introduction

Material And Methods

Wastewater and inoculated activated sludge

Experimental system

Analytical methods

Process set-up

Anaerobic/oxic set-up

BAF set-up

Fenton experiments

Determination and analysis of microbial community structure

Gas chromatography-mass spectrometry

Spectrum analysis

Results And Discussion

Process operation analysis

COD removal performance

NH4+-N removal performance

Nitrogen-removal process

Microbial population diversity analysis

Analysis of microbial structures and functional population

Gas chromatography-mass spectrometry

Excitation–emission matrix fluorescence spectroscopy characteristics

Conclusions

Declarations

References

Status:

Version 1

NH₄⁺-N removal performance