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CHEMICAL ENGINEERING JOURNAL · 2014 · IF 4.058

Enhanced decolorization of Orange G in a Fe(II)-EDDS activated persulfate process by accelerating the regeneration of ferrous iron with hydroxylamine

Donghui Han,Jinquan Wan,Yongwen Ma,Yan Wang,Mingzhi Huang,Yangmei Chen,Dongya Li,Zeyu Guan,Ying Li

Oxidative decolorization of Orange G (OG) in Fe(II)/(S,S)-ethylenediamine-N,N′-disuccinic acid (EDDS)/persulfate (PS) process was investigated. Hydroxylamine was combined to accelerate the Fe(II) recovery for improvement of PS activation. Effects of the reagents dosage, pH, and hydroxylamine adding mode were evaluated in batch experiments. All the decolorization experiments were performed at 25   °C within 180   min and with initial OG concentration ranging from 0.25 to 2.5   mM. The results indicated that EDDS decreased the Fe(II) accessibility to 11.9% at the molar ratio of EDDS/Fe(II)   =   1/1 and could improve the OG decolorization by slowing down the Fe(II) depletion rate. The addition of hydroxylamine was effective in further enhancement of the oxidative ability and 98% OG decolorization was obtained rapidly with only 50.6% PS decomposition when hydroxylamine/Fe(II)   =   8/5. The combination of EDDS and hydroxylamine could expand the effective pH range up to 7. The hydroxylamine adding mode also played a significant role and OG decolorization efficiency was 49.4%, 67.7% and 70.7% when adding times was 1, 3 and 5, respectively. In addition, under the condition of PS/Fe(II)/hydroxylamine   =   5/10/16, OG suffered incomplete decolorization up to 71.8% due to the insufficient PS dosage, while a decline of OG decolorization was observed as well when PS/Fe(II)/hydroxylamine   =   80/10/16 because of the intensive consumption of hydroxylamine and hydroxyl radicals ( OH) by excessive PS. The radicals characterization via electron spin resonance (ESR) technique was also conducted and the results indicated hydroxyl radicals were the predominant oxidative species in studied processes.

研究领域: 环境科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2016 · IF 4.836

Study on enhanced degradation of atrazine by ozonation in the presence of hydroxylamine

Jingxin Yang,Ji Li,Wenyi Dong,Jun Ma,Jie Cao,Tingting Li,Jiayin Li,Jia Gu,Pingxin Liu

Degradation of atrazine (ATZ) by ozonation in the presence of hydroxylamine (HA) was experimentally investigated in this study. The results showed approximately 80% of ATZ was degraded by ozonation in the presence of HA, while only 20% was degraded by ozonation alone. The obvious inhibition of the ATZ degradation by tert -butanol suggested the enhanced ATZ degradation by ozone/HA was primarily attributed to OH. The OH yield was determined to be 25.8%. Additionally, the optimum HA dosage for the ATZ degradation was 4   μM, when the ozone dosage was 20   μM. The effects of pH, bicarbonate and temperature on ATZ degradation by ozone/HA were investigated in details. Most importantly, the enhanced ATZ degradation by ozonation in the presence of HA was still observed in real water especially at acidic pHs. Furthermore, the potential mechanism of OH formation during the reaction of ozone with HA was proposed herein. Nine products were identified by UPLC/Q-TOF-MS system. The ATZ degradation involved dealkylation, dechlorination-hydroxylation and olefination. The evolutions of the concentrations of three available transformation products including deethylatrazine, deisopropylatrazine and deethyldeisopropylatrazine in ozone/HA were evaluated and compared with that in ozonation alone.

研究领域: 环境科学 · 化学
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CHEMOSPHERE · 2020 · IF 5.778

Degradation of chloramphenicol by α-FeOOH-activated two different double-oxidant systems with hydroxylamine assistance

Fu He,Wencheng Ma,Dan Zhong,Yixing Yuan

The pipe deposits from water distribution network are iron-wastes, which could be used as a catalyst of advanced oxidation processes (AOPs). This paper prepared one main composition (α-FeOOH) of pipe deposits and compared the difference of chloramphenicol (CAP) degradation by α-FeOOH-activated hydrogen peroxide/persulfate and α-FeOOH-activated hydrogen peroxide/peroxymonosulfate with hydroxylamine assistance. Several key affecting factors were investigated. The results revealed that the double-oxidant system has a synergy effect in CAP degradation process. The hydroxyl radicals were identified as the predominant radicals in two different degradation processes via electron paramagnetic resonance (EPR) technique. The possible degradation pathways and products were confirmed by liquid chromatography-mass spectrometry (LC-MS). This study provided a theoretic research for pollutant removal by taking full advantage of pipe deposits and advance the development of water quality security in water distribution network in future.

研究领域: 环境科学 · 水处理工程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2018 ·Vol. 25 ·期 16 ·15733-15742 · IF 2.8

Enhanced effect of EDDS and hydroxylamine on Fe(II)-catalyzed SPC system for trichloroethylene degradation

Fu Xiaori,Dionysiou Dionysios D.,Brusseau Mark L.,Zaman Waqas Qamar,Zang Xueke,Lu Shuguang,Qiu Zhaofu,Sui Qian

This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •− ) in the three systems. A gradual increasing contribution of O 2 •− to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl − concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO • oxidation and O 2 •− reaction was proposed.

研究领域: 环境科学 · 化学工程
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2017 ·Vol. 24 ·期 31 ·24318-24326 · IF 2.741

Enhanced effect of HAH on citric acid-chelated Fe(II)-catalyzed percarbonate for trichloroethene degradation

Fu Xiaori,Brusseau Mark L.,Zang Xueke,Lu Shuguang,Zhang Xiang,Farooq Usman,Qiu Zhaofu,Sui Qian

This work demonstrates the impact of hydroxylamine hydrochloride (HAH) addition on enhancing the degradation of trichloroethene (TCE) by the citric acid (CA)-chelated Fe(II)-catalyzed percarbonate (SPC) system. The results of a series of batch-reactor experiments show that TCE removal with HAH addition was increased from approximately 57 to 79% for a CA concentration of 0.1 mM and from 89 to 99.6% for a 0.5 mM concentration. Free-radical probe tests elucidated the existence of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •- ) in both CA/Fe(II)/SPC and HAH/CA/Fe(II)/SPC systems. However, higher removal rates of radical probe compounds were observed in the HAH/CA/Fe(II)/SPC system, indicating that HAH addition enhanced the generation of both free radicals. In addition, increased contribution of O 2 •- in the HAH/CA/Fe(II)/SPC system compared to the CA/Fe(II)/SPC system was verified by free-radical scavengers tests. Complete TCE dechlorination was confirmed based on the total mass balance of the released Cl − species. Lower concentrations of formic acid were produced in the later stages of the reaction for the HAH/CA/Fe(II)/SPC system, suggesting that HAH addition favors complete TCE mineralization. Studies of the impact of selected groundwater matrix constituents indicate that TCE removal in the HAH/CA/Fe(II)/SPC system is slightly affected by initial solution pH, with higher removal rates under acidic and near neutral conditions. Although HCO 3 − was observed to have an adverse impact on TCE removal for the HAH/CA/Fe(II)/SPC system, the addition of HAH reduced its inhibitory effect compared to the CA/Fe(II)/SPC system. Finally, TCE removal in actual groundwater was much significant with the addition of HAH to the CA/Fe(II)/SPC system. The study results indicate that HAH amendment has potential to enhance effective remediation of TCE-contaminated groundwater.

研究领域: 环境科学 · 化学工程
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Chemosensors · 2021 ·Vol. 9 ·期 12 ·335 · IF 3.398

Paper-Based Vapor Detection of Formaldehyde: Colorimetric Sensing with High Sensitivity

Chenglong Liao,Miao Zhang,Nan Gao,Qingyun Tian,Jiangfan Shi,Shuai Chen,Chuanyi Wang,Ling Zang

We report on a novel colorimetric sensor system for highly sensitive detection of formaldehyde (FA) in the gas phase. The sensor is constructed with paper towel as a substrate coated with the sulfuric acid salt of hydroxylamine ((NH2OH)2·H2SO4) together with two pH indicators, bromophenol blue and thymol blue. Upon exposure to FA, the hydroxylamine will react with the absorbed FA to form a Schiff base (H2C=N-OH), thus releasing a stoichiometric amount of sulfuric acid, which in turn induces a color change of the pH indicator. Such a color change was significantly enriched by incorporating two pH indicators in the system. With the optimized molar ratio of the two pH indicators, the color change (from brown to yellow, and to red) could become so dramatic as to be visible to the eye depending on the concentration of FA. In particular, under 80 ppb of FA (the air quality threshold set by WHO) the color of the sensor substrate changes from brown to yellow, which can even be envisioned clearly by the naked eyes. By using a color reader, the observed color change can be measured quantitatively as a function of the vapor concentration of FA, which produces a linear relationship as fitted with the data points. This helps estimate the limit of detection (LOD), to be 10 ppb under an exposure time of 10 min, which is much lower than the air quality threshold set by WHO. The reported sensor also demonstrates high selectivity towards FA with no color change observed when exposed to other common chemicals, including solvents and volatile organic compounds. With its high sensitivity and selectivity, the proposed paper-based colorimetric sensor thus developed can potentially be employed as a low-cost and disposable detection kit that may find broad application in detecting FA in indoor air and many other environments.Keywords:vapor detection;formaldehyde;colorimetric;paper-based sensor;hydroxylamine

研究领域: 环境科学 · 分析化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Salting-out extraction of acetoin from fermentation broths using hydroxylammonium ionic liquids as extractants

Yan Li,Jian-Ying Dai,Zhi-Long Xiu

The salting-out extraction (SOE) systems based on ionic liquids (ILs) have attracted extensive attention in the separation of bio-based products, in which imidazolium ILs were widely studied. However, the high cost and toxicity have hindered their further industrial application. Hydroxylammonium ILs have the characteristics of cheap raw material, simple synthesis process and low toxicity, but are rarely used in the SOE systems. In this work, five hydroxylammonium ILs (2 cations and 4 carboxylate anions) were synthesized and used in SOE of bio-chemicals. The phase forming abilities of ILs with K 3 PO 4 and H 2 O were affected by the hydrophilicity of anions and cations. With the increase of carbon chain length, phase forming abilities of ILs increased, while the temperature had little influence. The partition behaviors of acetoin, ILs and 2,3-butandiol, and the selectivity of acetoin to organic acids were investigated and compared at different concentrations of ethanolammonium butyrate (EOAB) and K 3 PO 4 . In a SOE system consisted of 6% EOAB-38% K 3 PO 4 (w/w), the recovery of acetoin, IL and 2,3-butandiol was 92.7%, 76.0% and 86.0%, respectively, and the selectivity of acetoin to lactic acid and acetic acid was 16.46 and 3.85, respectively. The ATR-IR spectra showed the hydrogen bonds formed between acetoin and O-H, N-H, –COO – of hydroxylammonium IL played an important role in the efficient extraction of acetoin from fermentation broths.

CAS / MDL: 513-86-0 7778-53-2
研究领域: 生物化工 · 化学工程
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CHEMISTRY-A EUROPEAN JOURNAL · 2023 ·Vol. 29 ·期 38 ·e202300969 · IF 4.3

Toughening Hydrogels by Forming Robust Hydrazide-Transition Metal Coordination Complexes

Huaqiang Ju,Qing Li Zhu,Min Zuo,Songmiao Liang,Miao Du,Qiang Zheng,Zi Liang Wu

Graphical Tough hydrogels were developed by forming robust hydrazide-Zn 2+ coordination complexes. The mechanical properties of the resultant gels exhibited a notable temperature dependence and thus a good shape-memory ability due to the dynamic nature of coordination bonds. The reactive amine group of the hydrazide enables facile surface modification and functionalization based on Schiff's base reactions. Energy dissipation based on dynamic fracture of metal ligands is an effective way to toughen hydrogels for specific applications in biomedical and engineering fields. Exploration of new kinds of metal-ligand coordinates with robust bonding strength is crucial for the facile synthesis of tough gels. Here a hydrogel toughening strategy based on the formation of robust coordination complexes between the hydrazide ligands and zinc ions is reported. The resultant hydrogels exhibit high strength and toughness at room temperature. Their mechanical properties show temperature dependence due to the dynamic nature of coordination bonds. In addition, the amine group of hydrazides in the gel matrix provides a reactive site for Schiff's base reaction, enabling surface modification without influence on overall mechanical performances of the gel. The hydrazide ligands are easy to synthesize and can coordinate very well with several transition metals. Such a metal-ligand coordination should be suitable to develop tough soft materials with versatile applications.

研究领域: 材料科学 · 生物医学工程
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Applied Catalysis O: Open · 2024 · IF 0

Direct amination of toluene with hydroxylamine to produce toluidine over vanadium catalysts

Jiayuan Nie,Pengyu Yin,Qiusheng Yang,Zhihui Li,Yanji Wang,Xiaoshu Ding,Dongsheng Zhang

In this study, metallic vanadium was used as catalysts for direct amination of toluene with hydroxylamine to produce toluidine under mild conditions. High toluene conversion and toluidine selectivity were obtained, corresponding to 87.62% and 96.45% respectively. Additionally, thermodynamic and kinetic calculations were carried out. It was concluded that the reaction was dominated by kinetics, with the distribution of three products being para > ortho > meta. The computational and experimental results indicated that the amination process involves an amino radical mechanism.

研究领域: 有机化学 · 催化化学 · 反应工程
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WATER SCIENCE AND TECHNOLOGY · 2022 ·Vol. 85 ·期 6 ·1813-1823 · IF 2.43

Heterogeneous activation of H2O2/Na2S2O8 with iron ore from water distribution networks for pollutant removal

Zhong Dan,He Fu,Ma Wencheng,Wu Yichuan,Dong Jiaju

In this study, we investigated using the main composition of pipe deposits from water distribution networks as catalyst to activate dual-oxidant H 2 O 2 /Na 2 S 2 O 8 system to produce radicals for perchloroethylene and chloramphenicol removal. According to the results, the degradation efficiency of perchloroethylene by H 2 O 2 /Na 2 S 2 O 8 system was 92.05% within 8 h. Due to the slow conversion between ≡Fe 3+ and ≡Fe 2+ , the hydroxylamine was introduced to reduce reaction time. As for the results, the degradation efficiency of chloramphenicol in the H 2 O 2 /Na 2 S 2 O 8 system with hydroxylamine assistance was 73.31% within 100 min. Meanwhile, several key affecting factors and the kinetic models were investigated. The primary radicals were identified by electron paramagnetic resonance and radical scavenging tests. Eleven degradation products were confirmed by high-resolution liquid chromatography-mass spectrometry. The result of this study provided the theoretical basis for resource utilization of pipe deposits in water treatment in case of emerging contamination events.

研究领域: 环境科学 · 水处理 · 材料化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2023 ·Vol. 30 ·期 32 ·79282-79296 · IF 5.8

Hydroxylamine facilitated catalytic degradation of methylene blue in a Fenton-like system for heat-treatment modified drinking water treatment residues

Zhong Yu,Wan Xiancheng,Lian Xiaoyan,Cheng Wenyu,Ma Xiaoying,Wang Dongtian

Rational treatment of drinking water treatment residues (WTR) has become an environmental and social issue due to the risk of secondary contamination. WTR has been commonly used to prepare adsorbents because of its clay-like pore structure, but then requires further treatment. In this study, a Fenton-like system of H-WTR/HA/H 2 O 2 was constructed to degrade organic pollutants in water. Specifically, WTR was modified by heat treatment to increase its adsorption active site, and to accelerate Fe(III)/Fe(II) cycling on the catalyst surface by the addition of hydroxylamine (HA). Moreover, the effects of pH, HA and H 2 O 2 dosage on the degradation were discussed with methylene blue (MB) as the target pollutant. The mechanism of the action of HA was analyzed and the reactive oxygen species in the reaction system were determined. Combined with the reusability and stability experiments, the removal efficiency of MB remained 65.36% after 5 cycles. Consequently, this study may provide new insights into the resource utilization of WTR. Graphical Abstract

研究领域: 环境科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2025 · IF 7.2

Hydroxylamine enhanced zero-valent copper/persulfate oxidation systems: Rapid corrosion of Cu(0) and reduction of Cu(Ⅱ)

Peng Xu,Jiaqi Feng,Na Li,Jiafan Yao,Guangchao Li,Baolin Hou

Zero-valent copper (Cu(0))-activated peroxodisulfate (PDS) generates reactive oxygen species (ROS) that effectively degrade azo dyes, but its application is limited by low Cu(I) conversion and narrow pH range. To overcome these barriers, this study introduced hydroxylamine (HA) to the Cu(0)/PDS system, boosting its oxidative capacity by accelerating the Cu(I)/Cu(II) redox cycle. Under the optimal conditions, the Cu(0)/PDS/HA system achieved a 78.5 % improvement in the degradation efficiency of orange II (AO7) within 10 min. UV-Vis spectroscopy, electron spin resonance (ESR) analysis, and scavenging experiments confirmed SO 4 •- and • OH as the primary reactive species in the Cu(0)/PDS/HA system, with minimal Cu(III) formation. A Systematic investigation of operational parameters (initial pH, Cu(0) dosage, HA concentration, and PDS concentration) and water matrix components (Cl - , NO 3 - , SO 4 2- , HCO 3 - , and humic acid) revealed their impact on AO7 removal. Furthermore, experiments in real water samples (tap, lake, and river water) validated the practicality of the Cu(0)/PDS/HA system, which was also demonstrated to effectively degrade other common pollutants. In conclusion, the present study provided an efficient strategy to bolster the oxidizing capacity of Cu(0)/PDS system, broadening its application potential for treating refractory organic pollutants.

研究领域: 环境科学 · 化学工程
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