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WATER RESEARCH · 2024 · IF 11.4

A universal model to predict yields of THMs and HAAs based on UV–Visible absorption spectra

Yang Deng,Shansheng Mo,Gregory V. Korshin,Mingquan Yan

Differential absorption spectroscopy (DAS) quantifies changes in the UV–Visible absorbance of dissolved organic matter (DOM) caused by reactions of its chromophores. As a result of its precision and sensitvity, DAS serves as a powerful tool for characterizing the formation of disinfection by-products (DBPs) in generated in DOM chlorination reactions. However, the nonlinear relationship between the intensity of DAS and DBP concentrations as well as the need to develop site-specific fitting parameters limit its practical applications. This study investigated the physico-chemical nature of DAS of chlorinated DOM through experimental measurements and theoretical calculations. Results of this study provide molecular-level evidence that electrophilic substitution reactions involving DOM reactive sites result in the emergence of DAS feaures ascribed to the "fast" chromophores. The ring opening in the cyclic enones-like structures which can be present either in the original DOM or are generated as intermediates in its chlorination, leads to the emergence of DAS features associated with the "slow" chromophores and high yields of DBPs. The kinetic study of chlorination of real waters reveals a strong linear relationship (R 2 > 0.91) between ln([DBP]) and the long-wavelength (λ > 325 nm) parameter of the DAS, notably (ln(-DA 350 )). This relationship varies among different water sources due to the differences in the heterogeneity of Band A 3 whose maximum is near 350 nm. Band A 3 is one of the Gaussian bands that comprise the overall UV–Visible spectrum of DOM. A new function ( f ( − D A 350 ) f(−DA350) ) is proposed in this study to quantify DBP formation. This function, which is determined by the Band A 3 's area, allows establishing a universal linear relationship between f ( − D A 350 ) f(−DA350) and ln([THMs]), as well as f ( − D A 350 ) f(−DA350) and ln([HAAs]), across various water sources. The findings of this study will stimulate further development of spectroscopy-based DBP monitoring technology for monitoring and optimization of water disinfection processes.

CAS / MDL: 99-96-7 123-31-9
研究领域: 环境科学 · 分析化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Catalytical dehalogenation of HAAs through electrolysis on VB12-modified electrode: kinetics, intermediates, and mechanisms

Xiaoyan Ma,Kunming Wei,Hongwei Liu,Qi Zheng,Wenqing Cao,Liang Zhang,Liangjie Tang,Stefanos Giannakis,Jing Deng,Su Jiang,Daniel L. Gallagher,Andrea M. Dietrich

Haloacetic acids (HAAs) are prevalently occurred in drinking water after disinfection by chlorine or chloramine, classified as the non-volatile and thermally stable disinfection byproducts (DBPs). To minimize the existed HAAs, catalytical electrolysis based on effective cathode was employed. Dehalogenation of HAAs were improved by vitamin B12 (VB12) coating on the stainless steel (SS), iron, copper, and aluminum electrodes. The VB12/SS composite electrode proved to be the optimal for the synergistic effect of VB12 and metal substrate on the DCAA degradation. Target chloro-, bromo-, and iodo-HAAs were catalytically decomposed, and their dehalogenation efficiency and mechanistic pathway were compared. The results show that HAAs electrolytic dehalogenation rates were significantly related with both the degree of halogenation (tri > di > mono) and the halogen atomic weight (I > Br > Cl). Dehalogenation of HAAs follows a first-order kinetic model, and kinetic variations were well described by a linear model. The logarithm base 10 of the dehalogenation rate constant k was proportional to its HAA molecular weight: log 10 (k) =0.00237 MW -0.85. The intermediate dehalogenation products were identified as less-halogenated acetic acids, and the final were acetic acid and halide ions. No mineralization occurred according to carbon conservation analysis. ESR detection and quenching experiments confirmed that HAAs dehalogenation was mainly an indirect reduction mediated by atomic H*. The synergistic effect between atomic H* and VB12 occurred through the electron transfer. This comparative study of various HAAs dehalogenation provides a mechanism of dehalogenation and a predictive linear model for electrolysis of HAAs.

研究领域: 环境科学 · 化学工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2012 · IF 3.286

Factors affecting THMs, HAAs and HNMs formation of Jin Lan Reservoir water exposed to chlorine and monochloramine

Huachang Hong,Yujing Xiong,Mengyong Ruan,Fanglei Liao,Hongjun Lin,Yan Liang

The formations of THMs, HAAs, and HNMs from chlorination and chloramination of water from Jinlan Reservoir were investigated in this study. Results showed that monochloramine rather than chlorine generally resulted in lower concentration of DBPs, and the DBPs formation varied greatly as the treatment conditions changed. Specifically, the yields of THMs, HAAs and HNMs all increased with the high bromide level and high disinfectant dose both during chlorination and chloramination. The longer reaction time had a positive effect on the formation of THMs, HAAs and HNMs during chlorination and HNMs during chloramination. However, no time effect was observed on the formation of THMs and HAAs during chloramination. An increase in pH enhanced the levels of THMs and HNMs upon chlorination but reduced levels of HNMs upon chloramination. As for the THMs in chloramination and HAAs in chlorination and chloramination, no obvious pH effect was observed. The elevated temperature significantly increased the yields of THMs during chlorination and HNMs during chloramination, but has no effect on THMs and HAAs yields during chloramination. In the same temperature range, the formation of HAAs and HNMs in chlorination showed a first increasing and then a decreasing trend. In chloramination study, addition of nitrite markedly increased the formation of HNMs but had little impact on the formation of THMs and HAAs. While in chlorination study, the presence of high nitrite levels significantly reduced the yields of THMs, HAAs and HNMs. Range analysis revealed that the bromide and disinfectant levels were the major factors affecting THMs, HAAs and HNMs formation, in both chlorination and chloramination. Finally, comparisons of the speciation of mono-halogenated, di-halogenated, tri-halogenated HAAs and HNMs between chlorination and monochloramination were also conducted, and factors influencing the speciation pattern were identified.

CAS / MDL: 78-75-1
研究领域: 环境科学 · 公共卫生
✓ 已验证 产品关联 DOI PubMed 高影响因子
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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

THMs, HAAs and NAs production from culturable microorganisms in pipeline network by ozonation, chlorination, chloramination and joint disinfection strategies

Xiaochao Duan,Xiaobin Liao,Jianfei Chen,Shuguang Xie,Huan Qi,Fei Li,Baoling Yuan

Disinfection is an indispensable process to inactivate pathogens , while unexpected disinfection by-products (DBPs) would also be formed between the reaction of residual disinfectants and microorganisms in the water distribution system (WDS). However, there are few studies referring to the formation of DBPs and DBPs-associated toxicity under various disinfection methods based on microorganisms in the real WDS. In addition, the main contributors of bacterial communities or components that generate DBPs are unclear. In this study, the formation of trihalomethanes (THMs), halo-acetic acids (HAAs), nitrosamines (NAs) from culturable microorganisms in pipeline network by ozonation(O 3 ), chlorination (Cl 2 ), chloramination (NH 2 Cl) and joint disinfection methods were compared, meanwhile, their calculated toxicities under different oxidation scenarios were also discussed. Moreover, 16S ribosomal ribonucleic acid (rRNA) gene sequencing was used to identify the main microbial communities . The results demonstrated that THMs and HAAs increased with increasing disinfectant dosages, while the quantity of NAs (mainly nitroso dimethylamine (NDMA)) was not significantly related to disinfectant dosages for each disinfection strategy. Chloroform (TCM) and dichloroacetic acid (DCAA) were the dominant THMs and HAAs species, respectively. NDMA existed in the samples before disinfections, which may due to the metabolic activity of microorganisms. Pre-O 3 increased THMs formation during subsequent Cl 2 and NH 2 Cl treatment. However, pre-O 3 effectively reduced HAAs produced by subsequent chlorination. O 3 /Cl 2 disinfection had the highest DBPs formation potential (DBPFP) (883.6 nM), while its calculated toxicity was similar to that in Cl 2 disinfection treatment. Pseudomonas was the most abundant bacterial genus in biofilm of WDS pipeline. This study can aid in an optimal disinfection strategy for water treatment plants to reduce the toxicity of DBPs caused by biomass in pipelines and ensure water quality safety.

研究领域: 环境科学 · 微生物学
✓ 已验证 DOI PubMed 高影响因子
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ACS Applied Nano Materials · 2022 · IF 6.14

Giant Carrier Mobility in Graphene with Enhanced Shubnikov–de Haas Quantum Oscillations: Implications for Low-Power-Consumption Device Applications

Ying Zhang,Shasha Wang,Guojing Hu,Haoliang Huang,Bo Zheng,Yuehui Zhou,Yan Feng,Xiang Ma,Junfeng He,Yalin Lu,Meng Gu,Yu-Lun Chueh,Guorui Chen,Bin Xiang

Graphene devices are susceptible to the surrounding environment. For example, the substrate in contact with graphene influences the device performance because the carriers are confined in two-dimensional (2D) atomic thickness. However, 2D van der Waals dielectric materials used as an interface modifier can provide a path to improve the device quality. In this paper, we report enhanced mobility of up to 540 000 cm2 V–1 s–1 in monolayer graphene sandwiched between two layers of a CrOCl insulator through a dielectric shielding effect. The Shubnikov–de Haas quantum oscillation is also observed with the amplitude linearly decreasing with increasing temperature, consistent with the standard Lifshitz–Kosevich theory. More strikingly, this oscillation persists to a temperature as high as 100 K because of this enhanced mobility. Our work paves a way to improve the mobility of graphene and realize the nontrivial quantum states at high temperatures for the exploration of low-power-consumption device applications in electronics.

研究领域: 凝聚态物理 · 纳米电子学 · 量子材料 · 低功耗电子学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Formation of DBPs during chlorination of antibiotics and control with permanganate/bisulfite pretreatment

Hailan Wang,Weiye Shi,Defang Ma,Yanan Shang,Yan Wang,Baoyu Gao

Antibiotics are widespread in water and wastewater, which could react with chlorine to produce disinfection byproducts (DBPs) during disinfection process. Activation of permanganate by bisulfite generates a permanganate/bisulfite (PM/BS) ultra-fast oxidation system, which exhibits more complete oxidation of refractory organics than conventional advanced oxidation processes. This study explored the formation and speciation of trihalomethanes (THMs), haloacetic acids (HAAs), haloacetonitriles, haloketones and trichloronitromethane during chlorination of antibiotics (chloramphenicol, ciprofloxacin and sulfamerazine), as well as the impact of Br - Br- . PM/BS pre-oxidation was further applied to control DBP formation from antibiotics. Only THMs and HAAs were quantifiable. Trichloromethane was dominant in THMs. HAAs derived from ciprofloxacin and sulfamerazine were mostly constituted by monochloroacetic acid, while trichloroacetic acid was dominate in chlorinated chloramphenicol. Sulfamerazine exhibited the highest DBP formation potential (DBPFP), of which trihalomethane formation potential (THMFP) was 997.14 ± 13.96 μg L −1 and haloacetic acid formation potential (HAAFP) was 3767.86 ± 325.09 μg L −1 . Chloramphenicol had very low THMFP, but high HAAFP (1560.29 ± 56.55 μg L −1 ), which was six times higher than that of ciprofloxacin. Adding Br - Br- increased DBPFP and yields of brominated species. PM/BS pre-oxidation (KMnO 4 /HSO 3 − was 1.0/2.5 mM/mM) significantly reduced the DBPFP and chlorine reactivity, and inhibited the utilization of bromine into DBPs with the presence of Br - Br- . After PM/BS treatment, over 50% of the ciprofloxacin in real drug manufacturing wastewater were degraded, and the THMFP decreased by about 50%. Overall. PM/BS process is a promising advanced oxidation technology for antibiotic wastewater treatment and control of DBP formation.

CAS / MDL: 127-79-7
研究领域: 环境科学 · 水处理 · 高级氧化过程
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FOOD CHEMISTRY · 2022 · IF 9.231

Electrophilic components from Xiaoheiyao (rhizomes of Inula nervosa Wall.) alleviate the production of heterocyclic aromatic amines via creatinine inhibition

Xiang-Rong Cheng,Jia-Hui Ma,Issoufou Amadou,Wei Zhao,Yu-Yao Chen,Chen-Xi Zhang,Bin Guan

Xiaoheiyao is the rhizome of Inula nervosa Wall., a traditional spice and medicinal herb in China. In this study, the creatinine inhibitor from Xiaoheiyao extract and also the effects and mechanism on the production of heterocyclic aromatic amines (HAAs) were investigated. Xiaoheiyao extract inhibited the total contents of seven detected HAAs in grilled beef patties, particularly aminoimidazole-azaarenes (AIAs) in a dose-dependent manner, reaching a maximum inhibition rate of 62% for total HAAs and 73% for AIAs. The most effective subfraction of Xiaoheiyao extract (IER80) contained abundant potential creatinine inhibitors, as revealed by immobilized creatinine probe, HPLC and UPLC-MS/MS analyses. Moreover, electrophilic p -coumaric acid derivatives were discovered from IER80 by feature based molecular networking. p -Coumaric acid was demonstrated to inhibit the contents of total HAAs and AIAs in grilled beef patties and model system. Quantitative analyses of the precursor and intermediates of AIAs in model system revealed that p -coumaric acid mainly affected the generation of AIAs by inhibiting creatinine.

研究领域: 食品科学 · 药理学 · 化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Food Bioscience · 2024 · IF 4.8

Effect of tea extracts on heterocyclic aromatic amines and advanced glycation end products in roasting Eleutheronema Tetradactylum and lipid-mediated inhibition mechanism analysis

Ruichun Wang,Songyi Lin,Junbo Chu,Yi Yuan,Simin Zhang

Eleutheronema Tetradactylum is commercially important marine fish and a fixture at tables. However, nonnegligible hazardous substances, such as heterocyclic aromatic amines (HAAs) and advanced glycation end products (AGEs), generates along during thermal processing. Herein, we determined HAAs and two representative AGEs, Nε-carboxyethyl-lysine (CEL) and Nε-carboxymethyl-lysine (CML) formation in roasted Eleutheronema Tetradactylum , and proposed inhibitory method of tea polyphenol to effectively reduce HAAs, CML and CEL, which caused 51.23, 46.72, 24.06 and 35.48 percentage reduction of Norharman, Harman, CML and CEL, respectively, led IQ, 8-MeIQx below detected limitation. Precursors (amino acids, creatin(in)e, glucose and glyoxal), lipid oxidation, fatty acid analysis and further nontargeted lipidomic approaches are attempted to reveal the inhibition mechanism. This work develops a new method to minimize HAAs and AGEs in Eleutheronema Tetradactylum , provide a comprehensive interpretation of inhibition mechanism by tea polyphenols, which is helpful to food manufacturers for healthier fish production.

研究领域: 食品科学 · 营养学 · 生物化学 · 毒理学 · 化学
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CHEMOSPHERE · 2023 · IF 8.8

Overlooked inorganic DBPs in trichloroisocyanuric acid (TCCA) disinfected indoor swimming pool: Evidences from concentration, cytotoxicity, and human health risk

Jiafu Li,Jingsi Chen,Zhiyong Hu,Xinyu Li,Mei Li,Yuan Wang,Zengli Zhang,Xiaojun Liang

Trichloroisocyanuric acid (TCCA) is a popular disinfectant for swimming pools in China. However, the occurrence and importance of regulated disinfection byproducts (DBPs) in TCCA-disinfected swimming pools are less understood. This study analyzed 12 regulated DBPs (4 trihalomethanes (THMs), 5 haloacetic acid (HAAs), bromate , chlorate, and chlorite) in 85 swimming pool water samples and 17 input tap water samples from one swimming pool for 17 days continuously. Considering water temperature, pH, free chlorine, total chlorine, and urea, most of swimming pool water samples were within the water quality limits for China. Total concentrations of THMs, HAAs, and inorganic DBPs of 20.4–42.2, 82.0–229, and 100–729 μg/L in the swimming pool, and 16.6–28.3, 8.2–12.8, and 64.4–95.6 μg/L in the tap water, indicating inorganic DBPs are the dominant swimming pool and drinking water pollutants. Cancer risk values of regulated DBPs in swimming pools and input tap water are 2.7E-05 and 8.1E-05, respectively, and exceed the US EPA's threshold (1.0E-06). The non-cancer risk is below the US EPA's threshold. Following TCCA disinfection, the concentration and calculated cytotoxicity of regulated DBPs had a 3.6-fold and 1.9-fold increase, respectively. Inorganic DBPs contribute to the calculated concentration and cancer risks of DBPs in swimming pools and tap water at sufficient concentrations warranting regulation. This study provides data on 12 regulated DBPs in TCCA-disinfected indoor swimming pools, highlighting the importance of inorganic DBPs from evidences of concentration, cytotoxicity, and cancer risk for the first time.

研究领域: 环境科学 · 公共卫生 · 水质 · 毒理学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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FOOD CONTROL · 2021 · IF 5.548

Inhibitory effect and mechanism of various fruit extracts on the formation of heterocyclic aromatic amines and flavor changes in roast large yellow croaker (Pseudosciaena crocea)

Meng Li,Songyi Lin,Ruichun Wang,Duo Gao,Zhijie Bao,Dong Chen,Yue Tang,Na Sun,Simin Zhang

The large yellow croaker ( Pseudosciaena crocea ) is one of the most commercially important marine fish in China and is a fixture at Chinese tables. Herein, we determined the formation of heterocyclic aromatic amines (HAAs) in roasted yellow croaker and evaluated the inhibitory effect of natural fruits extracts (blueberry extract, acerola cherry extract and grape seed extract) on the formation of HAAs in roast yellow croaker. All the three fruit extracts treatments minimize the amount of HAAs and the addition of blueberries extracts is the most effective approach on reducing the total HAAs content, which caused a signification reduction of 94.85% and 71.15% of the Norhaman and PhIP content, respectively, led IQ, 8-MeIQX, 4,8-DiMeIQX below the detected limitation, compared to the control group. Furthermore, antioxidant index of fruits extracts, precursors (free amino acids, creatine, creatinine and glucose) of HAAs, lipid and protein oxidation, flavor changes are evaluated to determine the mechanism and physical/chemical changes of fruit extracts on the formation of HAAs. This research develops a new method to minimize the amount of HAAs, which is helpful to food manufacturers for the production of healthier yellow croaker products and may be applicable to various meat systems.

CAS / MDL: 497-19-8
研究领域: 食品科学 · 营养学 · 化学 · 生物化学
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