ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2019
·Vol. 27
·期 1
·812-822
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IF 2.914
Xu Suyun,Yan Ning,Cui Minghao,Liu Hongbo
In this study, ozone-oxidation was used to treat synthetic chemical plating solution containing Cu(II)/Ni(II)-EDTA solution to realize the purpose of decomplexation. The effects of solution pH, initial concentration of Cu(II)/Ni(II)-EDTA, the molar ratio of EDTA to Cu(II)/Ni(II), and the coexistence of Cu(II)/Ni(II) on their removal efficiencies were investigated. The degradation of EDTA-Cu(II) and EDTA-Ni(II) were mainly attributed to OH oxidation, and the removal rates of Cu(II)/Ni(II) depend on the complete decomplexation. The removal rates of Cu(II) and Ni(II) was affected by the pH of solution, and the optimal pH was found to be 7–9; nevertheless, their removal rates can still be up to 90% even in acidic pHs of 3~5. When the molar ratio of EDTA to Cu(II)/Ni(II) increased from 1:1 to 3:1, the kinetics of metal ion removal rate declined from 0.0788 and 0.1139 min -1 to 0.0250 and 0.0271 min -1 . The synergistic effect was found in the Cu(II)/Ni(II) blended system due to the higher catalytic capability and the lower complexation affinity toward EDTA for Ni(II). In summary, ozone oxidation can be considered as an effective technology to realize the complete decomplexation of Cu(II)/Ni(II)-EDTA that contained in chemical plating industry wastewater.
Graphical Abstract
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Hao Zhu,Wencheng Ma,Hongjun Han,Chunyan Xu,Yuxing Han,Weiwei Ma
Ozonation of pyridine and indole was investigated both in aqueous solution and biologically pretreated coal gasification wastewater (BPCGW). Experimental results showed that the removal of indole was hardly affected by pH value. Direct reaction rate constant of ozone with pyridine increased from 0.18 M −1 s −1 (protonated pyridine) to 3.03 M −1 s −1 (molecular pyridine), and that with molecular indole was 8.6 × 10 5 M −1 s −1 . Seven and five transformation intermediates were observed for pyridine and indole, respectively. Ozonation pathways were proposed as hydroxylation, opening and cleavage of the aromatic ring. It was found that ammonia nitrogen (NH 3 N) increased by 3.3 mg L −1 in ozone process, suggesting the broken of the C N bonds of pyridine, indole and other N-heterocyclic compounds. In terms of biochemical oxygen demand to chemical oxygen demand (BOD 5 /COD), toxicity and resazurin dehydrogenase activity (DHA), the biodegradability was improved after ozone treatment , indicating the possibility of ozone combined with biosystem for the treatment of BPCGW. The results of gas chromatograph and mass spectrometry (GC-MS) indicated that primary products during first 10 min might lead to the obstinate toxicity, which was further proved by US Environmental Protection Agency (US-EPA) test. This study would assist in obtaining a better understanding of the application of ozonation pretreatment in BPCGW.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yang Zong,Wenjie Ji,Yu Xie,Deli Wu
The mineralization of organic pollutant by O 3 is prone to be restricted by the accumulative production of oxalate (OA) that is recalcitrant to the attack of hydroxyl radical ( OH). Herein, it was interestingly found that the presence of 0.5 mM Ni(II) enhanced the mineralization efficiency of EDTA by O 3 under alkaline conditions by 22.8%, with the promoting effect of Ni(II) augmented as the increasing loading of Ni(II). Based on the results from scavenging experiment, chemical probe detection and XPS characterization, it was verified that except for the commonly recognized reactive oxidants (i.e., OH and O 3 ) in EDTA mineralization, the overlooked Ni(III) species (i.e., NiOOH) also played an indispensable role in enhancing the mineralization of EDTA. The Ni(III) species was formed via the oxidation of decomplexed Ni(II) by OH and in turn collaborated with OH to decompose EDTA. More importantly, the generated Ni(III) species exerted higher affinity towards OH and O 3 -resistent oxalate, hence elevating EDTA mineralization. This study elucidated the significant role of Ni(III) species in promoting the mineralization efficiency of EDTA, and also proposed a new insight into elevating the treatment performance of ozonation via the collaborative oxidation mechanism-co-mediated by OH and Ni(III) species.
研究领域:
环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Shan Jiang,Xiuyu Liu,Zehai Wang,Lin Zhou,Zhiqian Meng,Xinyi Wang,Guoning Chen,Shuangfei Wang,Yan Jiang
Lignocellulose nanopaper (LNP) assembled from lignocellulose nanofibrils (LCNFs) is an emerging eco-friendly structural material applicable to a variety of fields. Lignin serves as a crucial functional component in the LNP matrix; however, it negatively affects the interfacial hydrogen-bonding behaviors among LCNFs and consequently the inferior mechanical performance of LNP. In this study, a mild ozone-oxidation strategy was used to modify lignin macromolecules in situ without significant degradation of carbohydrate polymers (i.e., cellulose and hemicellulose) in LCNFs whereupon the interfacial hydrogen-bond energy was dramatically improved in the assembly and deformation process of LNP as validated by molecular dynamics simulation. Consequently, the lignin-modified LNP exhibited significantly enhanced tensile strength (from 83 to 140 MPa) and toughness (from 1.9 to 7.1 J/m3), which even surpassed those of conventional cellulose nanopaper. Benefiting from the well-preserved lignocellulosic structure, lignin-modified LNP maintained its inherent favorable water and thermal stability and intriguing optical performance, which supported our developed LNP to be a multifunctional structural material for diversified fields, for example, flexible electronic applications. Additionally, the estimated production cost for our developed LNP was approximately half of that for conventional cellulose nanopaper due to its significantly lower resource inputs such as the material, water, and energy. Overall, our study provides a site-specific macromolecular modulation strategy for the economically and environmentally feasible fabrication of high-performance lignocellulosic nanomaterials toward advanced structural applications.
研究领域:
材料科学
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林业工程
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环境科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
·
IF 7.864
Qian-Yuan Wu,Lu-Lin Yang,Xin-Yang Zhang,Wen-Long Wang,Yao Lu,Ye Du,Yun Lu,Hong-Ying Hu
Ammonia (NH4+) and hydrogen peroxide (H2O2) have been widely used to inhibit bromate formation during ozonation. However, organic byproducts can also pose a risk under these conditions. During bromate inhibition, the influence of NH4+ and H2O2 on organic byproducts and their toxicity should be elucidated. Our study found that NH4+ suppressed organic bromine, but might result in increased toxicity. Adding 0.5 mg/L of NH4+–N substantially increased both the formation of cytotoxicity and genotoxicity (DNA double-strand breaks) of organic byproducts from 0.6 to 1.6 mg-phenol/L, and from 0.3 to 0.8 μg-4-NQO/L (0.5 mg/L Br–, 5 mg/L O3). NH4+ decreased bromate, but increased the overall toxicity of the integrated byproducts (organic byproducts and bromate). Organic nitrogen measurements and 15N isotope analysis showed enhanced incorporation of nitrogen into organic matter when NH4+ and Br– coexisted during ozonation. NH4+ decreased the formation of brominated acetonitriles, but enhanced the formation of brominated nitromethanes and brominated acetamides. These brominated nitrogenous byproducts were partially responsible for this increase in toxicity. Different from ammonia, H2O2 could reduce both bromate and the toxicity of organic byproducts. In the presence of 0.5 mg/L Br– and 10 mg/L O3, adding H2O2 (0.5 mM) substantially suppressed bromate, cytotoxicity formation and genotoxicity formation by 88%, 63% and 67%. This study highlights that focusing on bromate control with NH4+ addition might result in higher toxicity. Efforts are needed to effectively control the toxicities of bromate and organic byproducts simultaneously.
研究领域:
环境科学
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毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Yu Xie,Shuhan Peng,Yong Feng,Deli Wu
The degradation of carboxylic acid has been identified as one of the rate-determining steps in the mineralization of organic pollutants by ozonation . In this study, Ce(III)-doped graphitic carbon nitride (Ce–CN) composites with different Ce(III) contents were synthesized and used as catalysts for the ozonation of oxalate. The morphology and structure of the Ce–CN were comprehensively characterized using various techniques such as SEM, XRD , FTIR , and XPS. The results show that the structure of g-C 3 N 4 provided an ideal site for the accommodation of Ce(III) and thus facilitated the formation of surface hydroxyl groups. With 2.5%Ce–CN as a catalyst, the degradation efficiency of oxalate was increased by 47.1% after reaction for 30 min. The decomposition of ozone was accelerated in the presence of Ce–CN. Hydroxyl radicals were recorded by electron spin resonance and identified as the major actives species. Under the catalysis of 2.5%Ce–CN, the production of hydroxyl radicals was increased by 40%. The Ce(III) and surface hydroxyl groups that distributed uniformly on the surface of Ce–CN were speculated as the dual catalytic sites for the complexation of oxalate and activation of ozone, respectively. Ce–CN had a high stability and reutilization capability. It is proposed that a complex was formed between surface Ce(III) and oxalate, and this complex could be more easily attacked by the surrounding ozone and hydroxyl radicals than free oxalate. As oxalate is a typical recalcitrant carboxylic acid, the findings from this study are expected to promote the application of ozonation in the removal of organic pollutants.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Junqi Cheng,Zhitao Han,Jiawei Li,Xinxiang Pan
Previous work proposed a one-stage wet scrubbing in situ combined with O3 oxidation for simultaneous removal of NO and SO2 from flue gas, and the results showed that wet scrubbing combined in situ with O3 injection could effectively improve O3 oxidant utilization efficiency. In this work, a follow-up research work was carried out to further explore the synergistic effect of dual oxidants of NaClO in the liquid phase and O3 in gas phase. The synergistic effects of O3/NO molar ratio and NaClO concentration in the circulating scrubbing solution on NOx removal performance was investigated systematically. The results showed that when molar ratio of O3/NO was 0.5 and NaClO concentration was 25 mM, NO could be oxidized completely and averaged NOx removal efficiency exceeded 70%. NOx concentrations in outlet gas and anion compositions in the scrubbed solution were analyzed, and the possible reaction paths of wet scrubbing NaClO solution in situ with O3 injection in denitration process were also discussed. When the solution pH was around 6, a relative balance between NOx oxidation and absorption might be achieved, resulting in a high NOx removal efficiency. The temperature of inlet flue gas imposed little impact on NOx removal efficiency due to the quick and efficient cooling effect by wet scrubbing. The increase of initial SO2 concentration led to a slight increase of NOx removal efficiency from 70 to 73.5%. A complete removal of SO2 could be achieved, but coexisting SO2 in flue gas would consume NaClO oxidant and shorten the reaction duration.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2024
·
IF 5.3
Yuwen Deng,Zaili Xiong,Jijun Guo,Bingzhi Liu,Meirong Zeng,Zhandong Wang,Zhongyue Zhou,Wenhao Yuan,Fei Qi
Elucidating the oxidation chemistry of polycyclic aromatic hydrocarbons (PAHs) aids in understanding the degradation reaction processes of PAHs, as well as their competitive roles in PAH growth. In this work, ozone-assisted oxidation of indene , the smallest prototype PAH molecule, was investigated in an atmospheric jet stirred reactor at 400–550 K. Ab initio quantum chemistry calculations were conducted to characterize the oxidation kinetics of indene and interpret the experimental observations. Fingerprint oxidation products including 2-(2-oxoethyl) benzoic acid, 2-(formylmethyl) benzaldehyde , 1,2-indanedione and 1-indanone were identified by synchrotron vacuum ultraviolet photoionization mass spectrometry . The initial C 9 H 8 O 3 adduct resulting from O 3 -addition to indene exhibits high instability and is primarily detected as 2-(2-oxoethyl)benzoic acid following ozonolysis reactions. Minor amounts of vinylhydroperoxide were also observed as isomeric products of the C 9 H 8 O 3 adduct. Theoretical calculations indicate that indene ozonolysis is highly structure-dependent, where the conformation of the C 9 H 8 O 3 adduct determines the configuration of the resulting Criegee intermediates (CI). The distinctive reaction pathways introduced by the bifunctionalized characteristics of indene-derived large CIs are emphasized in this study. syn -Configuration CI features more conversion pathways compared to anti -CI due to the interaction between CI functionality and the neighboring aldehyde group, among which the bicyclic ring-closure reaction yielding secondary ozonide is most favored. The dioxirane intermediates generated from anti -CIs can undergo the Crossed Acid-forming channel to yield the target acid products, which provides an alternative way for dioxirane conversion. Further theoretical analyses demonstrate that ozonolysis is not the exclusive mechanism for indene oxidation under O 3 -assisted conditions. Instead, it is accompanied by low-temperature reactions initiated by OH/O 2 , leading to key products such as 2-(formylmethyl) benzaldehyde and 1-indanone. The present work aims to unravel the elusive chemistry involved in the O 3 -initiated oxidation of indene, providing new insights into the distinctive kinetics introduced by large bifunctionalized CIs in the ozonolysis of structurally similar PAHs.
研究领域:
化学动力学
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环境科学
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量子化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Wanzhen Zhong,Wencong Hao,Shuhao Liang,Xinshenghui Zhu,Siyi Luo,Weiqiang Tan,Zongliang Zuo,Kangshuai Lin,Dongdong Ren
Polyethylene glycols (PEG) are widely employed and frequently detected in wastewater, and between 0.5 and 68 mg L −1 of PEG were found in river water and seawater. It puts significant pressure on COD treatment of the water environment. Nevertheless, PEG is not easily broken down by biological processes, and other treatment methods include drawbacks such as membrane blockage and stringent pH requirements. Ozone oxidation technology can overcome these drawbacks, but low ozone utilization and higher catalytic costs limit the industrialization of the technology to some extent. In this research, discarded copper slag was used as an in situ iron donator, and modified into a catalyst for ozone catalytic oxidation, which achieved lower costs and waste reuse. Based on the Response Surface Methodology simulation and experimental tests, to achieve the greatest catalytic performance, the copper slag was calcined at 710 °C for 3.5 h. Under optimal conditions, with the introduction of CS-710,3.5 to ozone oxidation, the removal rate of PEG was improved from 79.27 % to 97.40 % in 10 min with an initial PEG concentration of 20 mg L −1 . In addition, the COD removal rate was increased by 18.3 % and the first-order rate constant (k) was 2.66 times higher than that of the individual ozone system. After 10 cycles of reuse, the removal rate still reached 73.8 %, indicating the catalyst's good stability. The concentration of Pb and Zn dissolved was 1.6 and 4.4 μg L −1 , respectively, sufficient to meet Environmental quality standards for surface water (GB 3838-2002, China). Thus, the safety of the catalyst is proven. The reaction process based on the free radical mechanism, according to density functional theory (DFT), CS-710,3.5 enhanced the conversion of ozone to OH, O− 2, and 1 O 2 , and hastened the degradation of PEG. Despite taking a while to mineralize fully, PEG was effective in breaking down macromolecules into smaller ones. As such, it can be regarded as a successful PEG pretreatment technique.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xixi Chen,Hai Yang,Chaktong Au,Shuanghong Tian,Ya Xiong,Yu Chang
Reduction of potential carcinogenic bromate formation is a big challenge for the application of ozone in the treatment of Br − -containing wastewater. Three CeO 2 nanocrystals individually with exposed (1 0 0), (1 1 0), and (1 1 1) facets were prepared and adopted as catalysts for the ozonation of Br − containing wastewater. It is found that faceted CeO 2 greatly inhibited the bromate formation and simultaneously enhanced the pollutant removal. The catalytic activity follows the order of (1 0 0) > (1 1 0) > (1 1 1). In the presence of CeO 2 (1 0 0), there is 71.4 ± 2.9% of sulfamethoxazole (SMZ) degradation (only 24.9 ± 1.8% in ozone alone). Moreover, the generation of bromate was reduced by 29.6%, 38.8%, 52.4%, 66.4%, respectively, when the initial Br − concentration is 1.0, 2.0, 34.0, 65.0 mg L −1 . Meanwhile, the antibacterial-active groups in most of the identified intermediates were destroyed and much lower biotoxicity of the treated wastewater is observed. The good reducibility and Lewis acidity of CeO 2 (1 0 0) favors the activation of ozone and the redox cycle of ceria. DFT calculations show that ozone facilely dissociates into surface O and O 2 through interaction with the (1 0 0) facet. It is demonstrated that O 2 − , its derivatives (i.e. OH and 1 O 2 ) and surface O are generated and get involved in SMZ degradation. It is noted that O 2 − also functions as a key reductant to convert Ce 4+ to Ce 3+ which reduce HBrO/BrO − and BrO 3 − to Br − and therefore inhibit the formation of bromate. These results indicate that CeO 2 (1 0 0) catalyzed ozonation is a promising advanced oxidation process for the treatment of Br-containing wastewater, and crystal facet engineering is an efficient strategy to enhance the catalytic performance.
研究领域:
环境科学
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催化化学
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理论计算
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Jiangyu Tang,Xiao Wang,Yunfa Wang,Min Shi,Peng Huo,Jianxiang Wu,Qiaoxia Li,Qunjie Xu
The oxygen evolution reaction (OER) serves as a fundamental half–reaction in the electrolysis of water for hydrogen production, which is restricted by the sluggish OER reaction kinetics and unable to be practically applied. The traditional lattice oxygen oxidation mechanism (LOM) offers an advantageous route by circumventing the formation of M-OOH* in the adsorption evolution mechanism (AEM), thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order. Fortunately, the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen, which could be activated by rational band structure design for direct O-O coupling, where the M–O bond maintains its initial bond order. Here, non-bonding oxygen was introduced into NiFe 2 O 4 via annealing in an oxygen-deficient atmosphere. Then, in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons, thereby facilitating the transformation of the redox center from metal to oxygen. LOM based on non-bonding oxygen (LOM NB ) was successfully activated within NiFe 2 O 4 , exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm –2 and excellent durability of stable operation for over 150 h. Additionally, catalysts featuring varying band structures were synthesized for comparative analysis, and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2 p holes are critical prerequisites for triggering and sustaining the LOM NB pathway in transition metal spinel oxides. These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yu Li,Jie Li,Jia Ding,Zirong Song,Bochen Yang,Chuanming Zhang,Baohong Guan
The presence of nanoplastics in drinking water inducing inevitable exposure to human beings has aroused considerable attention. It is worth evaluating the degradation and even mineralization of nanoplastics in drinking water treatment plants designed for guaranteeing drinking water safety. Herein we mainly focus on the decomposition of nano-sized polystyrene plastics by two commonly used disinfection techniques, namely ozonation and chlorination. At recommended dosage for disinfection, ozonation achieves 99.9% molecular weight (MW) degradation and 42.7% mineralization of nano-sized polystyrene plastics in 240 min, while chlorination only attains 7.1% MW degradation and 4.3% mineralization. The overwhelming MW degradation is concentrated in first 30 min with 96.3% for ozonation and 4.2% for chlorination. With the proceeding of ozonation, the surface of nano-sized polystyrene plastics becomes rough and the particle size is decreased, during which the introduction of oxygen-containing groups on the surface of nano-sized polystyrene plastics increases the hydrophilicity of plastics, thus contributing to the further oxidative degradation to produce formic acid, phenol, acetophenone, hydroquinone and other products. However chlorination cannot roughen the surface of nano-sized polystyrene plastics, and only destroys a small amount of C-C bonds in main chain to form shorter chains polymers. This finding shows ozonation other than chlorination is available and effective for degradation of nano-sized polystyrene plastics, indicating that ozonation could be employed as a potential technique to tackle nanoplastics pollution in drinking water treatment plants.
研究领域:
环境科学
·
饮用水处理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）