Disinfection byproducts and halogen-specific total organic halogen speciation in chlorinated source waters – The impact of iopamidol and bromide Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Nana Osei B. Ackerson, Hannah K. Liberatore, Michael J. Plewa, Susan D. Richardson, Thomas A. Ternes, Stephen E. Duirk Abstract This study investigated the speciation of halogen-specific total organic halogen and disinfection byproducts (DBPs) upon chlorination of natural organic matter (NOM) in the presence of iopamidol and bromide (Br−). Experiments were conducted with low bromide source waters with different NOM characteristics from Northeast Ohio, USA and varied spiked levels of bromide (2–30 μmol/L) and iopamidol (1–5 μmol/L). Iopamidol was found to be a direct precursor to trihalomethane (THM) and haloacetic acid formation, and in the presence of Br− favored brominated analogs. The concentration and speciation of DBPs formed were impacted by iopamidol and bromide concentrations, as well as the presence of NOM. As iopamidol increased the concentration of iodinated DBPs (iodo-DBPs) and THMs increased. However, as Br− concentrations increased, the concentrations of non-brominated iodo- and chloro-DBPs decreased while brominated-DBPs increased. Regardless of the concentration of either iopamidol or bromide, bromochloroiodomethane (CHBrClI) was the most predominant iodo-DBP formed except at the lowest bromide concentration studied. At relevant concentrations of iopamidol (1 μmol/L) and bromide (2 μmol/L), significant quantities of highly toxic iodinated and brominated DBPs were formed. However, the rapid oxidation and incorporation of bromide appear to inhibit iodo-DBP formation under conditions relevant to drinking water treatment. Graphical abstract

Water quality induced corrosion of stainless steel valves during long-term service in a reverse osmosis system Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Xiyan Xu, Shuming Liu, Ying Liu, Kate Smith, Xiaoting Wang, Junyu Li, Ziqing Ma, Zhangqing Wang, Yong Cui Abstract The current study analyzes the contribution of 10 water quality parameters (including pH, turbidity, conductivity, total dissolved solids (TDS), hardness, total organic carbon (TOC), alkalinity, calcium ions, chlorides and sulfates) to corrosion extent of stainless steel valves taken from different locations in a reverse osmosis system of a reclaimed water plant. The valves were in service for 5 years. Raman spectroscopy and X-ray photoelectron spectroscopy analyses are conducted to quantify corrosion products on different valves under various water quality conditions. On that basis, bivariate and multivariate regression analyses between the 10 water quality parameters and the corrosion extent of valve specimens (represented by metal loss percentage (MLP) values) are carried out to check the contribution of those water quality parameters to MLP. The results indicate that the proportions of metal oxides as corrosion products vary according to the corrosion extent of the valves. Although no linear correlation is found, all 10 water quality parameters except for pH show a significant positive correlation with the MLP values of the valve specimens. Moreover, results of multivariate regression suggest that the variation of MLP can be explained by turbidity, TDS, TOC and sulfates. A positive contribution of turbidity, TDS and TOC to MLP is observed, whereas the contribution of sulfates is negative. The results from the current work help to identify the reasons for water quality-induced failure of stainless steel equipment in RO systems. Graphical abstract

Kitchen waste valorization through a mild-temperature pretreatment to enhance biogas production and fermentability: Kinetics study in mesophilic and thermophilic regimen Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Agata Gallipoli, Camilla M. Braguglia, Andrea Gianico, Daniele Montecchio, Pamela Pagliaccia Abstract Biowaste valorization through anaerobic digestion is an attractive option to achieve both climate protection goals and renewable energy production. In this paper, a complete set of batch trials was carried out on kitchen waste to investigate the effects of mild thermal pretreatment, temperature regimen and substrate/inoculum ratio. Thermal pretreatment was effective in the solubilisation of macromolecular fractions, particularly carbohydrates. The ability of the theoretical methodologies in estimating hydrogen and methane yields of complex substrates was evaluated by comparing the experimental results with the theoretical values. Despite the single batch configuration, a significant initial hydrogen production was observed, prior to methane yield. Main pretreatment effect was the gain in hydrogen production; the extent was highly variable according to the other parameters values. High hydrogen yields, up to 113 mL H2/g VSfed, were related to the prompt transformation of soluble sugars. Thermophilic regimen resulted, as expected, in faster digestions (up to 78 mL CH4/gVS/day) and sorted out pH inhibition. The relatively low methane yields (342–398 mL CH4/g VSfed) were the result of the consistent lignocellulosic content and low lipid content. Thermal pretreatment proved to be a promising option for the enhancement of hydrogen production in food waste dark fermentation. Graphical abstract

Mineralogical characteristics and photocatalytic properties of natural sphalerite from China Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Can Shen, Xiangping Gu, Bin Yang, Dexian Zhang, Zhilin Wang, Zhengxiang Shu, Jeffrey Dick, Anhuai Lu Abstract Different natural sphalerites have a range of photocatalytic properties that can potentially be exploited for environmental remediation purposes. To develop value in the exploitation of sphalerite, samples were collected from 19 ore deposits in China and characterized for their mineralogical and photocatalytic properties. X-ray diffraction (XRD) and electron probe micro analysis (EPMA) measurements indicated that all the natural sphalerites from various localities crystallized in cubic phases with various chemical compositions. The substitution of Fe for Zn ranged from 0.235% to 14.826% by weight, Mn from 0.004% to 4.868%, Cu from 0.009% to 5.529% and Cd from 0.133% to 1.576%. As Fe became more abundant, the color of natural sphalerite darkened, becoming almost black; and higher Fe content was associated with stronger visible light absorption. Photoluminescence spectra showed emission mainly related to S-vacancies and progressively decreasing fluorescence intensity with increasing Fe content. Tests of the photocatalytic degradation of methyl orange indicated that the sample with the highest Cd content but moderate Fe content had the highest photocatalytic activity. Specifically, the degradation of Methyl Orange (30 mg/L) attained 82.11% efficiency under visible light irradiation for 4 hr of natural sphalerite with 4.262% Fe and 1.576% Cd. Overall, the Fe content in sphalerite was found to contribute to the visible light absorption ability and the recombination rate of photo-generated electrons and holes, while substitution by Cd was observed to have a greater effect on the photocatalytic properties. These findings provide a scientific basis for the profitable utilization of base metal resources like sphalerite. Graphical abstract

Mn2NiO4 spinel catalyst for high-efficiency selective catalytic reduction of nitrogen oxides with good resistance to H2O and SO2 at low temperature Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Fengyu Gao, Xiaolong Tang, Honghong Yi, Shunzheng Zhao, Wenjuan Zhu, Yiran Shi Abstract Mn–Ni oxides with different compositions were prepared using standard co–precipitation (CP) and urea hydrolysis-precipitation (UH) methods and optimized for the selective catalytic reduction of nitrogen oxides (NOx) by NH3 at low temperature. Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH (with Mn:Ni molar ratio of 2:1) catalysts showed almost identical selective catalytic reduction (SCR) catalytic activity, with about 96% NOx conversion at 75°C and ~99% in the temperature range from 100 to 250°C. X-ray diffraction (XRD) results showed that Mn(2)Ni(1)Ox-CP and Mn(2)Ni(1)Ox-UH catalysts crystallized in the form of Mn2NiO4 and MnO2–Mn2NiO4 spinel, respectively. The latter gave relatively good selectivity to N2, which might be due to the presence of the MnO2 phase and high metal–O binding energy, resulting in low dehydrogenation ability. According to the results of various characterization methods, it was found that a high density of surface chemisorbed oxygen species and efficient electron transfer between Mn and Ni in the crystal structure of Mn2NiO4 spinel played important roles in the high-efficiency SCR activity of these catalysts. Mn(2)Ni(1)Ox catalysts presented good resistance to H2O or/and SO2 with stable activity, which benefited from the Mn2NiO4 spinel structure and Eley-Rideal mechanism, with only slight effects from SO2. Graphical abstract

Seasonal variation and sources of derivatized phenols in atmospheric fine particulate matter in North China Plain Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Yang Yang, Xingru Li, Rongrong Shen, Zirui Liu, Dongsheng Ji, Yuesi Wang Abstract Qualitative and quantitative analyses of derivatized phenols in Beijing and in Xinglong were performed from 2016 to 2017 using gas chromatography-mass spectrometry. The results showed substantially more severe pollution in Beijing. Of the 14 compounds detected, the total average concentration was 100 ng/m3 in Beijing, compared with 11.6 ng/m3 in Xinglong. More specifically, concentration of nitro-aromatic compounds (NACs) (81.9 ng/m3 in Beijing and 8.49 ng/m3 in Xinglong) was the highest, followed by aromatic acids (14.6 ng/m3 in Beijing and 2.42 ng/m3 in Xinglong) and aromatic aldehydes (3.62 ng/m3 in Beijing and 0.681 ng/m3 in Xinglong). In terms of seasonal variation, the highest concentrations were found for 4-nitrocatechol in winter in Beijing (79.1 ± 63.9 ng/m3) and 4-nitrophenol in winter in Xinglong (9.72 ± 8.94 ng/m3). The analysis also revealed diurnal variations across different seasons. Most compounds presented higher concentrations at night in winter because of the decreased boundary layer height and increased heating intensity. While some presented higher levels during the day, which attributed to the photo-oxidation process for summer and more biomass burning activities for autumn. Higher concentrations appeared in winter and autumn than in spring and summer, which resulted from more coal combustions and adverse meteorological conditions. The significant correlations among NACs indicated similar sources of pollution. Higher correlations presented within each subgroup than those between the subgroups. Good correlations between levoglucosan and nitrophenols, nitrocatechols, nitrosalicylic acids, with correlation coefficients (r) of 0.66, 0.69 and 0.69, respectively, indicating an important role of biomass burning among primary sources. Graphical abstract

Role of glycine on sulfuric acid-ammonia clusters formation: Transporter or participator Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Danfeng Li, Dongping Chen, Fengyi Liu, Wenliang Wang Abstract Glycine (Gly) is ubiquitous in the atmosphere and plays a vital role in new particle formation (NPF). However, the potential mechanism of its on sulfuric acid (SA) - ammonia (A) clusters formation under various atmospheric conditions is still ambiguous. Herein, a (Gly)x·(SA)y·(A)z (z ≤ x + y ≤ 3) multicomponent system was investigated by using density functional theory (DFT) combined with Atmospheric Cluster Dynamics Code (ACDC) at different temperatures and precursor concentrations. The results show that Gly, with one carboxyl (–COOH) and one amine (–NH2) group, can interact strongly with SA and A in two directions through hydrogen bonds or proton transfer. Within the relevant range of atmospheric concentrations, Gly can enhance the formation rate of SA-A-based clusters, especially at low temperature, low [SA], and median [A]. The enhancement (R) of Gly on NPF can be up to 340 at T = 218.15 K, [SA] = 104, [A] = 109, and [Gly] = 107 molecules/cm3. In addition, the main growth paths of clusters show that Gly molecules participate into cluster formation in the initial stage and eventually leave the cluster by evaporation in subsequent cluster growth at low [Gly], it acts as an important “transporter” to connect the smaller and larger cluster. With the increase of [Gly], it acts as a “participator” directly participating in NPF. Graphical abstract

Agglomeration and removal characteristics of fine particles from coal combustion under different turbulent flow fields Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Zongkang Sun, Linjun Yang, Hao Wu, Xin Wu Abstract Turbulent agglomeration is a promising pretreatment technology for improving the removal of fine particles in industrial flue gas, which can improve the particle removal effect of dust removal equipment safely and economically. However, due to the complexity of turbulence mechanisms, the relationship between turbulent flow fields and the agglomeration of fine particles is not known with precision, resulting a weak promotion effect for particle removal with this pretreatment technology. In this work, three kinds of turbulent agglomerators were constructed to investigate the agglomeration and removal characteristics of fine particles under different turbulent flow fields. The results demonstrated that the turbulent agglomerator with small-scale and three-dimensional vortexes in the flow field had the best effect in improving the agglomeration and removal of fine particles. Two kinds of agglomeration modes in turbulent agglomeration were proposed, one being agglomeration between fine particles in the vortex area, and the other the capture of fine particles by coarse particles. Furthermore, the motion trajectory, relative velocity and residence time of fine particles of different sizes in different flow fields were calculated by numerical simulation to investigate the interaction mechanism of particle agglomeration and turbulent flow fields. The results showed that a flow field with small-scale and three-dimensional vortexes can reduce the Stokes number (StK) and the relative velocity of particles of different sizes, and extend their residence time in a turbulent flow field, so as to obtain a better agglomeration effect for fine particles. Graphical abstract

Enhanced phosphate removal using zirconium hydroxide encapsulated in quaternized cellulose Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Shuoxun Dong, Qinghua Ji, Yili Wang, Huijuan Liu, Jiuhui Qu Abstract Zirconium-based materials are efficient adsorbent for aqueous phosphate removal. However, current zirconium-based materials still show unsatisfied performance on adsorption capacity and selectivity. Here, we demonstrate a zirconium hydroxide encapsulated in quaternized cellulose (QC–Zr) for the selective phosphate removal. Zirconium hydroxide nanoparticles were simultaneously generated in situ with the QC framework and firmly anchored in the three-dimensional (3D) cross-linked cellulose chains. The maximum P adsorption capacity of QC–Zr was 83.6 mg P/g. Furthermore, the QC–Zr shows high P adsorption performance in a wide pH range, generally due to the electrostatic effects of quaternized cellulose. The enhanced adsorption of P was also achieved in the presence of competing anions (including Cl−, NO3−, SO42−, SO44−) and humic acid (HA) even at a molar ratio up to 20 levels. The column adsorption capacity of QC–Zr reached 4000 bed volumes (BV) at EBCT = 0.5 min as the P concentration decreased from 2.5 to 0.5 mg/L. Mechanism study revealed that both –N+(CH3)3 groups and zirconium hydroxide were involved in phosphate adsorption via electrostatic interactions between –N+(CH3)3 and phosphate, and the formation of zirconium hydrogen phosphate (Zr(HPO4)x). The 31P nuclear magnetic resonance (NMR) study implied that P surface–precipitated and inner–sphere complexed with zirconium hydroxide at a ratio of 3:1. Graphical abstract

Novel synthesis of aluminum hydroxide gel-coated nano zero-valent iron and studies of its activity in flocculation-enhanced removal of tetracycline Publication date: March 2020 Source: Journal of Environmental Sciences, Volume 89 Author(s): Xiangyu Wang, Binbin Zhang, Jun Ma, Ping Ning Abstract A newly designed aluminum hydroxide gel-coated nanoscale zero-valent iron (AHG@NZVI) with enhanced activity and dispersibility of NZVI was successfully synthesized. The AHG@NZVI composite was synthesized via control of the surface AHG content. AHG@NZVI-1, AHG@NZVI-2 and AHG@NZVI-3 were prepared under centrifugal mixing speeds of 1000, 2000 and 4000 r/min, respectively. The activity of AHG@NZVI was evaluated by its tetracycline (TC) removal efficiency. The effects of AHG content, pH value, reaction temperature, and presence of competitive anions on TC removal were investigated. TC could be removed by both adsorption and chemical reduction on AHG@NZVI-2 (centrifugal speed 2000 r/min) in a short time with high removal efficiency (≥98.1%) at the optimal conditions. Such excellent performance can be attributed to a synergistic interaction between aluminum hydroxide gel and NZVI: (1) AHG could enhance the stability and dispersity of NZVI; (2) aluminum hydroxide gel could absorb a certain amount of TC and Fe2+/Fe3+, which facilitated the mass transfer of TC onto the NZVI surface, resulting in acceleration of the reduction rate of TC by the AHG@NZVI composite; and (3) AHG-Fe2+/Fe3+ could absorb a certain amount of TC by flocculation. The kinetics of TC removal by AHG@NZVI composite was found to follow a two-parameter pseudo-first-order model. The presence of competitive anions slightly inhibited the activity of AHG@NZVI systems for TC removal. Overall, this study provides a promising alternative material and environmental pollution management option for antibiotic wastewater treatment. Graphical abstract