ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 47
·71721-71730
·
IF 5.19
Huang Wenjun,Li Sichao,Wang Hongbin,Cui Peng,Xu Haomiao,Cheng Can,Qu Zan,Yan Naiqiang
Oxidation–reduction-absorption based on sulfite is a promising process for simultaneous removal of NO x and SO 2 . However, excessive oxidation of sulfite and competitive absorption between NO x and SO 2 limit its application. A matching strategy between antioxidants and alkaline agents has been proposed to solve these problems and enhance the absorption process. The comparison results of inhibitors showed that hydroquinone exhibited long-term high-efficiency inhibition of S(IV) (SO 3 2- /HSO 3 - ) oxidation. The comparison of alkaline agents showed that the Na 2 SO 3 solution with heterogeneous mixture of MgO and hydroquinone exhibited better absorption performance than that with other combinations. The absorption amounts of NO x in 0.15 mol/L Na 2 SO 3 50 mL solution added 0.1% hydroquinone (HQ) with 0.09 mol/L MgO were 2.24 mmol, which improved 5 times than that without additives. In addition, studies on the influence of pH showed that the pH of MgO mixture could be stabilized at 9–10 for a long time, while the pH of Na 2 CO 3 mixture decreased faster. Further studies suggested that the hydration of MgO resulted in the solution with MgO keeping high pH. This is also the main reason why the combination of MgO and hydroquinone is superior to the combination of Na 2 CO 3 and hydroquinone in desulfurization and denitration performance.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zhiyuan Ning,Xiangqian Tan,Qian Wei,Yue Liu,Ruigang Wang,He Guo,Jingyu Ren,Qiuling Ma,Jian Zhou,Tiecheng Wang
A nanoconfinement strategy was employed to encapsulate iron species within carbon nanotubes (Fe-CCNTs) in this study, enabling rapid degradation of sulfadiazine (SDZ) through sulfite (S(IV)) activation. The Fe-CCNTs catalyst enhanced the generation of reactive species during the S(IV) activation process. Nearly complete SDZ degradation was achieved within 10 min, with a reaction rate constant 1.8 times higher than that of the non-confined system. Fe-CCNTs shifted the mechanism from a radical pathway (SO 4 • − and •OH) to a non-radical pathway ( 1 O 2 and Fe IV =O), thereby improving SDZ degradation efficiency. The nanoconfinement effect increased the local charge density, accelerating electron transfer and promoting the formation of reactive species. This system exhibited strong catalytic performance, high reusability, and resistance to interference. Furthermore, the Fe-CCNTs/S(IV) treatment reduced the abundance of intestinal pathogenic bacteria and the toxicity of byproducts. The Fe-CCNTs/S(IV) system offers a promising and low-toxicity solution for antibiotic removal in water treatment.
研究领域:
环境科学
·
纳米技术
·
催化
·
水处理
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
AQUA-Water Infrastructure Ecosystems and Society
·
2024
·Vol. 73
·期 5
·930-944
·
IF 2.1
Ye Miaomiao,Song Lei,Chen Peng,Li Kexin,Zheng Kai,Zhang Tuqiao,Liu Xiaowei
View large Download slide View large Download slide Close modal The S(IV)–Fe(II)/PM pretreatment has demonstrated preliminary potential as an effective ultrafiltration (UF) pretreatment technology. However, a comprehensive understanding of its impact on UF membrane fouling control and the dynamic evolution of membrane fouling during prolonged operation is still lacking. In this study, a relatively prolonged fouling experiment was conducted. Results revealed that the S(IV)–Fe(II)/PM pretreatment exhibited superior performance over Al(III) coagulation pretreatment in mitigating the transmembrane pressure difference and addressing both reversible and irreversible membrane fouling. The application of a cluster analysis method to classify membrane fouling evolution stages further confirmed that S(IV)–Fe(II)/PM pretreatment effectively decelerated the rate of membrane fouling evolution. The surface cake layer of UF membranes pretreated with S(IV)–Fe(II)/PM exhibited greater looseness and smoothness. It also showed better results than Al(III) coagulation pretreatment in reducing the accumulation of organic foulants, controlling the Si content and reducing the total microorganisms and live microorganisms in the UF feed water. Variance Partitioning Analysis indicated that the combined contribution of organic, inorganic, and biological foulants was the most significant for UF membranes after S(IV)–Fe(II)/PM pretreatment (50.4%) and UF membranes after Al(III) coagulation pretreatment (70.2%). These findings underscore the efficacy of S(IV)–Fe(II)/PM pretreatment in controlling UF membrane fouling under prolonged operation. S(IV)/Fe(II)/PM pretreatment efficiently mitigated UF membrane fouling during long-term operation. S(IV)/Fe(II)/PM pretreatment yielded a long uncontaminated stage and accelerated contaminated stage. S(IV)/Fe(II)/PM pretreatment suppressed the contribution of organic–inorganic–biological composite fouling.
研究领域:
环境科学
·
水处理工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sitao Wang,Zhijie Liu,Bolun Pang,Yuting Gao,Santu Luo,Qiaosong Li,Hailan Chen,Michael G Kong
Antibiotics are widely used to treat or prevent infectious diseases in human and veterinary medicine. Excessive residues in the aquatic environment lead to increasingly prominent antibiotic pollution; therefore, it is urgent to develop sustainable strategies for rapidly degrading antibiotics. In this study, a highly synergetic effect for norfloxacin (NOR) remediation is achieved by coupling underwater bubble plasma formation with a Fe (III)–S (IV) system due to the efficient utilization of reactive species in chain reactions. The degradation rate using synergetic approach can reach 76.4% within 50 min discharge, and further increases significantly to 94.4% after 5 h post-discharge. The effects of pulsed peak voltage and Fe (III)/S (IV) dosage on NOR removal are characterized. The existence of hydroxyl radicals ( • OH) and sulfate radicals (SO 4 •− ) are proved by electron spin resonance spectrometer (ESR) during degradation. Furthermore, radical scavenger experiments demonstrate that • OH and SO 4 •− play a crucial role in degradation. Underwater bubble plasma provides the oxic and acidic liquid environment for the Fe (III)–S (IV) system to accelerate the self-perpetuating chain reactions. These reactions not only introduce SO 4 •− and generate more • OH during plasma-on, but also induce their regeneration and further prolong the degradation process during plasma-off through plasma-generated effects. Finally, the degradation intermediates of NOR are identified, and a possible degradation pathway is proposed. The possible contribution weight of each approach on the degradation rate is speculated. These new findings offer promising applications for developing a technology with real potential for the treatment of organic compounds in industrial wastewater treatment.
研究领域:
环境科学
·
化学工程
·
等离子体化学
·
污水处理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Tong Liu,Zhican Xie,Peng Zhou,Zhaokun Xiong,Heng Zhang,Zhicheng Pan,Yang Liu,Bo Lai
Transition metal activation of sulfite (S(IV)) is a promising wastewater treatment technology . In this study, the activation of potassium pyrosulfite (PPS) with ferric iron (Fe 3+ ) is proposed firstly to degrade carbamazepine (CBZ). PPS has the advantages of low cost, non-toxicity and acidic solution, which makes it unnecessary to adjust the pH. The results showed that the Fe 3+ cycle was realized during the reaction process, and the degradation trend of CBZ was consistent with the formation rate of Fe 2+ and the decay rate of S(IV). Moreover, oxygen (O 2 ) plays a decisive role in the system and was the initiator of free radical chain reactions. The existence of sulfite radical (SO 3 •− ), sulfate radical (SO 4 •− ) and hydroxyl radicals (HO • ) in Fe 3+ /PPS system was proved by electron paramagnetic resonance (EPR), quenching experiments and terephthalic acid (TA) photoluminescence probing technique. The contribution of SO 4 •− and OH • to the removal of CBZ in Fe 3+ /PPS system is 64% and 35%, respectively. In addition, intermediates of CBZ were identified by Liquid Chromatography–Tandem Mass Spectrometry (LC–MS/MS) and possible removal pathways were also proposed. Finally, the effects of PPS concentration, Fe 3+ concentration, initial pH, anions and humic acid (HA) were also investigated.
研究领域:
环境科学
·
废水处理技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tao Luo,Yanan Yuan,Danna Zhou,Liting Luo,Jinjun Li,Feng Wu
In the recent years, sulfite-induced oxidation of various contaminants using oxysulfur radicals (SO 4 − , SO 5 − and SO 3 − ) has been explored to establish novel advanced oxidation processes (AOPs). Although transition metals, such as cupric ions (Cu(II)), have been demonstrated to be capable of activating sulfite (S(IV)), the catalytic mechanism of the specific Cu(II) species is still not very clear. In this work, N-acetyl- para -aminophenol (APAP) was used as a basic substrate to investigate the process, mechanism and stability of the Cu(II)-S(IV) system with low dosages of Cu(II) (0.010 mmol L −1 ) in an alkaline solution (pH 10). The results show that 0.010 mmol L −1 Cu(II) can efficiently activate S(IV) for the oxidation of APAP and other contaminants (e.g., metoprolol, sulfanilamide, aniline, 4-chloroaniline, N,N-dimethylaniline, p -nitrophenol and 3-nitrophenol). Simulation calculations for the distribution of the Cu(II) species and pH-dependence of APAP oxidation in the Cu(II)-S(IV) system showed that Cu(OH) 2 particles are the major active species in the catalysis of S(IV). The surface complexation of S(IV) with the Cu(OH) 2 particles prior to the production of oxysulfur radicals is the basic mechanism of the alkaline Cu(II)-S(IV) system. Radical inhibition with scavengers (ethanol, tert-butyl alcohol or aniline) demonstrates that SO 5 − , SO 4 − and hydroxyl radicals (HO ) are responsible for the contaminant oxidation. Moreover, SO 5 − is believed to be the main active species in the Cu(II)-S(IV) system, which has a second-order rate constant of 2.98 × 10 8 M −1 s −1 with APAP. This work renews our recognition of the Cu(II)-S(IV) system applications and further understanding of the catalytic role of the nascent Cu(OH) 2 particles in the activation of S(IV).
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Jingxin Yang,Yujie Luo,Xianghui Fu,Zijun Dong,Chuan Wang,Hong Liu,Chengchun Jiang
Transition metal catalyzed sulfite auto-oxidation is a promising technology used in water and wastewater treatment for the elimination of contaminants. In the literature, this process has been reported to be efficient only in the presence of oxygen. However, in this study, we unexpectedly found that the degradation of diatrizoate (DTZ) by a system based on the combination of copper ion and sulfite (Cu(II)/S(IV)) reached over 95% under anaerobic conditions , but was considerably retarded under aerobic conditions at pH 7. Furthermore, it was found that Cu(I), generated from the cleavage of the CuSO 3 complex, was the main reactive species responsible for the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions. In fact, the absence of oxygen promoted the accumulation of Cu(I). The concomitant release of the iodide ion with the degradation of DTZ indicated that the anaerobic degradation of DTZ by the Cu(II)/S(IV) system mainly proceeded through the deiodination pathway, which was also confirmed by the detection of deiodinated products. The anaerobic degradation of DTZ was favored at higher initial concentrations of Cu(II) or sulfite in this system. Since the CuSO 3 complex, the precursor of Cu(I), was formed mainly at pH 7, the highest anaerobic degradation of DTZ was achieved at pH 7. An increase in reaction temperature considerably enhanced the degradation of DTZ by the Cu(II)/S(IV) system with an apparent activation energy of 119.4 kJ/mol. The presence of chloride, bicarbonate and humic acid slightly influenced the anaerobic degradation of DTZ. The experiments with real water samples also demonstrated the effectiveness of the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Water
·
2025
·Vol. 17
·期 21
·3100
·
IF 3
Bingyang Wang,Xiaochen Wang,Shuang Liu,Zheng Wang,Fan Bai,Yujie Cheng,Dingkun Lu,Pengchao Xie
In this study, insoluble CaSO3was applied to replace soluble sulfite/bisulfite salt in the Fe(II)-activated sulfite/bisulfite [S(IV)] process for the efficient 2,4,6-tribromophenol (TBP) degradation. CaSO3serves as a low-cost and slow-release source of S(IV), significantly improving S(IV) utilization compared to conventional soluble Na2SO3. The Fe(II)/CaSO3system generated SO4•−and HO•through Fe(II)/Fe(III) redox cycling. Mechanistic studies confirmed SO4•−as the dominant reactive species, selectively attacking C-Br bonds and hydroxyl groups in TBP. Process optimization revealed effective performance under acidic conditions (pH 3.5–4.0) with minimal inhibition by common anions (Cl−, HCO3−). The reactive sites of TBP were identified through Fukui function calculations, and the degradation pathway was elucidated based on LC-MS analysis. Toxicity evaluation indicated reduced ecological risk of degradation intermediates due to debromination and benzene ring cleavage. This work provides a sustainable strategy for efficient TBP removal and detoxification in wastewater treatment with benefiting S(IV) utilization.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Chen-Yan Hu,Xin-Yu Yang,Li-Li Hu,Hao Liu,Jia-Nan Chen,Ling-Mei Gao,Zheng-Yu Dong
The enhanced degradation mechanism of micropollutants by sulfite (S(IV)) activated permanganate (Mn(VII)/S(IV)) process under different pH conditions were investigated in this study. The Mn(VII)/S(IV) process can significantly promote the degradation of sulfamethoxazole (SMX), ibuprofen (IBU), iohexol (IOX) and acetochlor (ACE). Compared with the permanganate (Mn(VII)) process alone, the degradation efficiency of SMX, IBU, IOX, and ACE in the Mn(VII)/S(IV) process increased by 51.6 %, 38.9 %, 43 % and 78.7 %, respectively. The pH value has a significant impact on the degradation of the four target pollutants. The mechanism of the Mn(VII)/S(IV) process was further explored using SMX as a model pollutant. Hydroxyl radicals (HO•), sulfate radicals (SO 4 •− ), and reactive manganese species (RMnS, Mn(III), and Mn(V)) were detected in the process. HO• plays an important role in the degradation of SMX under acidic conditions. At pH= 7, RMnS is the main reactive species. Under alkaline conditions, SO 4 •− plays an important role in the process. Mn(III) and Mn(V) can also be converted into other manganese species. In addition, the possible degradation pathway of SMX was proposed. This work reveals the important role of pH in the generation and transformation of reactive species, and demonstrates the enormous potential of the Mn(VII)/S(IV) process in controlling micropollutants. Considering the complexity of water matrix, future studies can explore the application of the Mn(VII)/S(IV) process in practical water treatment.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhi Xu,Zi-He Meng,Song-Hai Wu,Shi-Jie Wang,Peng-Yue Zhu,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,Xu Han
Sulfate radical (SO 4 •− ) is always thought to be an important oxidizing species in the metal-sulfite [S(IV)] systems, however, the oxidizing species correlated with the metal species have rarely been mentioned. In this study, the oxidizing species that oxidize arsenite [As(III)] in the Cu(II)-S(IV) system were investigated under alkaline conditions. Kinetic results indicate that complexation between Cu(II) and S(IV) is the pre-requisite to initiate various oxidizing species, followed by internal electron transfer from S(IV) to Cu(II) with the formation of SO 3 •− and the Cu I (SO 3 ) n −2n+1 complexes. Quenching experiments rule out contributions of SO 5 •− , peroxymonosulfate (HSO 5 − , PMS), hydroxyl radical ( • OH), superoxide radical (O 2 •− ) and singlet oxygen ( 1 O 2 ) to As(III) oxidation in the Cu(II)-S(IV) system and indicate that some kinds of peroxo species contribute. On the other side, apart from the oxidizing species such as SO 5 •− , PMS and SO 4 •− generated via a series of reactions between SO 3 •− and O 2 , the Cu I (SO 3 ) n −2n+1 complexes also react with O 2 to form Cu II -O 2 •− -(SO 3 2− ) n superoxo species and Cu III -O 2 2− -(SO 3 2− ) n peroxo species, as revealed by Raman analysis. UV–vis spectrum further confirms the presence of Cu(III) in the Cu(II)-S(IV) system. We therefore suggest that both SO 4 •− and the Cu(III)-peroxo species play important roles in the oxidation of As(III) in the Cu(II)-S(IV) system. This study enriches our understanding on the diversity of oxidizing species in the metal-S(IV) systems under alkaline conditions.
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Zhuoyue Wang,Ji Li,Wei Song,Jingxin Yang,Wenyi Dong,Xiaolei Zhang
Recently, it has been reported that chlorine dioxide (ClO 2 ) and (bi)sulfite/ClO 2 showed excellent performance in micropollutant removal from water; however, the degradation mechanisms and application boundaries of the two system have not been identified. In this study, bisphenol A (BPA) was chosen as the target contaminant to give multiple comparisons of ClO 2 and S(IV)/ClO 2 process regarding the degradation performance of contaminant, generation of reactive species, transformation of products and toxicity variation. Both ClO 2 and S(IV)/ClO 2 can degrade BPA within 3 min. The BPA degradation mechanism was mainly based on direct oxidation in ClO 2 process while it was attributed to radicals (especially SO 4 · - ) generation in S(IV)/ClO 2 process. Meanwhile, the effect of pH and coexisting substances (Cl − , Br − , HCO 3 − and HA) were evaluated. It was found that ClO 2 preferred the neutral and alkaline condition and S(IV)/ClO 2 preferred the acidic condition for BPA degradation. An unexpected speed-up of BPA degradation was observed in ClO 2 process in the presence of Br − , HCO 3 − and HA . In addition, the intermediate products in BPA degradation were identified. Three exclusive products were found in ClO 2 process, in which p-benzoquinone was considered to be the reason of the acute toxicity increase in ClO 2 process.
研究领域:
环境科学
·
化学工程
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）