ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 30
·42921-42930
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IF 0
Ye Miaomiao,Luo Ziyi,Jin Wen,Wang Xingyuan,Zhang Tuqiao,Liu Xiaowei
The viewpoints on whether high concentrations of chloride ion (Cl − ) promote or inhibit the oxidation activity of activated persulfates are still inconclusive. Furthermore, the degradation of organic pollutants by the persulfates in the presence of high Cl − concentrations without any activation medium has not yet been studied. In this work, the efficiency and mechanism of degradation of organic pollutants such as carbamazepine (CBZ), sulfadiazine (SDZ), and phenol (PN) by Cl − -activated PMS (denoted as Cl − /PMS) were investigated. Results showed that Cl − could effectively activate PMS for the complete removal of CBZ, SDZ, and PN with reaction kinetic constants of 0.4516 min −1 , 0.01753 min −1 , and 0.06805 min −1 , respectively. Parameters such as PMS dose, Cl − concentration, solution pH, and initial concentrations of organic pollutants that affect the degradation efficiencies of the Cl − /PMS process were optimized. Unlike conventional activated persulfates, it was confirmed that the free chlorine was the main active species in the Cl − /PMS process. Finally, the degradation by-products of CBZ and SDZ as well as their toxicity were detected, and a possible degradation pathway for CBZ and SDZ was proposed. Though higher toxic chlorinated by-products were generated, the Cl − /PMS process was still an efficient oxidation method for the removal of organic pollutants in aqueous solutions which contain high concentrations of Cl − .
研究领域:
环境科学
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化学工程
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产品关联
DOI
PubMed
CHEMOSPHERE
·
2019
·
IF 5.108
Shizong Wang,Jianlong Wang
Carbon-based materials have been studied as metal-free catalyst for persulfate activation. At present, the activation performance of carbon materials for persulfate is usually characterized by the removal efficiency of organic pollutants. However, the kinetics of persulfate activation by carbon materials has not been investigated. In this study, the kinetics of peroxymonosulfate (PMS) activation by reduced graphene oxide (RGO) and sludge-derived biochar (BC) were investigated. The experimental results showed that the kinetics of PMS activation followed the two-phase kinetic model (fast phase (a 1 ) and slow phase (a 2 )). In the absence of organic pollutants, the a 1 and a 2 were calculated to be 0.320 and 0.0471 min −1 for BC, respectively, and 0.322 and 0.0850 min −1 for RGO, respectively. Based on the characterization of BC and RGO, it can be concluded that the fast phase was mainly due to the formation of surface-bound active species. Competitive adsorption between PMS and targeted pollutants decreased the kinetic constant for the first phase (a 1 ) and the kinetic constant for the second phase (a 2 ) for both BC and RGO. The value of a 1 and a 2 increased for BC after the addition of phenol, due to the enhanced PMS activation by surface adsorbed phenol. The increase of phenol concentration decreased slightly the value of a 1 and a 2 . The increase of PMS concentration increased significantly the value of a 1 and a 2 . The decrease of a 1 and a 2 in repeated use of carbon materials could be due to the decrease of oxygen-containing functional groups and defect intensity.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 32
·49267-49278
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IF 5.19
Peng Huan,Chen Rong,Tao Ningyao,Xiao Yangyi,Li Chenxing,Zhang Tuqiao,Ye Miaomiao
Activation of peroxymonosulfate (PMS) by Fe 2+ is a green oxidation process for degradation of organic contaminants. However, the formation of iron mud and low PMS utilization lead to the decreased oxidation efficiency. In this work, commercial MoS 2 particles were used as the catalyst for boosting the Fe 2+ /PMS process for carbamazepine (CBZ) removal. The CBZ removal efficiency by the MoS 2 /Fe 2+ /PMS process was significantly enhanced, increasing to 6.5 times that of the Fe 2+ /PMS process. The Fe 3+ was reduced to Fe 2+ by the exposed Mo 4+ on the surface of MoS 2 , leading to the enhanced PMS utilization rate and increased Fe 2+ concentration. The relative intensity of DMPO-HO• and DMPO- SO 4 – • followed the order of MoS 2 /PMS < Fe 2+ /PMS < MoS 2 /Fe 2+ /PMS, also suggesting the enhanced oxidation activity with the addition of MoS 2 in the process of Fe 2+ /PMS. The commercial MoS 2 had good stability shown by the CBZ removal efficiency remaining almost unchanged during 8-time cycling use. Finally, a possible CBZ degradation pathway was proposed for helping understand the oxidation mechanism of the MoS 2 /Fe 2+ /PMS process.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
Processes
·
2022
·Vol. 10
·期 5
·941
·
IF 3.352
Yixin Lu,Yujie Liu,Chenghan Tang,Jiao Chen,Guo Liu
The degradation effect of heat/peroxymonosulfate (PMS) on atrazine (ATZ) is studied. The results show that the heat/PMS degradation for ATZ is 96.28% at the moment that the phosphate buffer (PB) pH, temperature, PMS dosage, ATZ concentration, and reaction time are 7, 50 °C, 400 μmol/L, 2.5 μmol/L, and 60 min. A more alkaline PB is more likely to promote the breakdown of ATZ through heat/PMS, while the PB alone has a more acidic effect on the PMS than the partially alkaline solution.HO•andSO4−•coexisted within the heat/PMS scheme, and ATZ quantity degraded byHO•andSO4−•in PB with pH = 7, pH = 1.7~1.HCO3−makes it difficult for heat/PMS to degrade ATZ according to inorganic anion studies, whileCl−andNO3−accelerate the degradation and the acceleration effect ofNO3−is more obvious. The kinetics of ATZ degradation via heat/PMS is quasi-first-order. Ethanol (ETA) with the identical concentration inhibited ATZ degradation slightly more thanHCO3−, and both of them reduced the degradation rates of heat/PMS to 7.06% and 11.56%. The addition ofCl−andNO3−increased the maximum rate of ATZ degradation by heat/PMS by 62.94% and 189.31%.Keywords:heat activation;PMS;atrazine;degradation mechanism;kinetics
研究领域:
环境科学
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化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Ming Zhu,Daqin Guan,Zhiwei Hu,Hong-Ji Lin,Chien-Te Chen,Hwo-Shuenn Sheu,Shaobin Wang,Jing Zhou,Wei Zhou,Zongping Shao
Synergistic effects are often used in catalyst design for many environmental/energy applications, however, the mechanism and a molecular-level structure to exert maximal synergy effects in catalyzing advanced oxidation processes (AOPs) in wastewater remediation are still unknown. Here, by designing a model perovskite family R BaCo 2 O 6- δ ( R = lanthanides) with Co 4+ in octahedral coordination (Co4+ oct) and Co 3+ in pyramidal coordination (Co3+ pyr), we ambitiously confirm the unique synergy of unsaturated (Co3+ pyr) and metallic (Co4+ oct) Co sites for efficient peroxymonosulfate (PMS) activation. Combined X-ray adsorption spectra and theoretical calculations strongly demonstrate that Co3+ pyr and Co4+ oct synergistically contribute to PMS adsorption and O O bond cleavage, and facilitate Co 3+ /Co 4+ redox cycle for radical generation. With appropriate ratio and ordered distribution of Co3+ pyr/Co4+ oct, the Gd 0.5 La 0.5 BaCo 2 O 5.75 exhibits remarkable catalytic activity for pollutant degradation, outperforming all previously reported Co 4+ -related oxides. This work may inspire rational design of efficient metal oxide catalysts.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
FARADAY DISCUSSIONS
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2024
·
IF 3.3
Wandong Zhao,Jin Lu
We describe a single-molecule electrochemical imaging strategy to study the electrocatalytic (EC') mechanism. Using the fluorescent molecule ATTO647N at extremely low concentrations as the substrate, we confirmed its catalytic reduction to a nonfluorescence form in the presence of the mediator phenazine methosulfate (PMS) by imaging and counting fluorescent molecules. Conventional electrochemical current in cyclic voltammetry would not have allowed us to infer the existence of an EC’ process or the PMS-mediated ATTO647N reduction. Additionally, we observed shifts in the catalytic reduction potential of ATTO647N at various mediator concentrations, which agree with the theoretical predictions by Savéant. Our work offers a new perspective on connecting single-molecule EC’ behaviors with the conventional ensemble EC’ mechanism, both practically and theoretically.
研究领域:
电化学
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催化反应动力学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Meiling Wu,Yang Tao,Yuwei Liu,Sanying Hou,Tiyang Xiao,Qing Fu,Guowen Peng,Lang Shi
In this study, Fe/N co-doped graphene-like honeycomb porous carbon (Fe-NC)was produced and used for the activating PMS to degrade TC. The Fe-NC catalyst has shown high activity in the TC degradation by activated PMS, with an efficiency of up to 94 % in 30 min. while the blank catalyst without N and Fe doping exhibited the lowest performance with 47.3 % TC degradation. Moreover, other operational factors of Fe-NC catalysts were also investigated to evaluate its catalytic activity. The burst experiments and electron paramagnetic resonance (EPR) experiments demonstrated that free radical paths (O 2 ·- ) and non-free radical paths ( 1 O 2 ) coexist inside the Fe-NC/PMS system. The experiment results and degradation mechanism analysis revealed that N species(Pyridine N, Graphite N,Fe-N x ) and iron species (Fe0) were possible to be the active species of catalysts. Furthermore, Fe-NC/PMS system was investigated for possible pathway of TC degradation by liquid mass spectrometry (LC-MS), and the presence of intermediates was analyzed for toxicity magnitude by ECOSAR software.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 6
·15377-15391
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IF 5.19
Wang Junwei,Zhang Di,Nie Fan,Zhang Ruixue,Fang Xiaojie,Wang Yaxin
MnO 2 , as a representative manganese-based catalyst with many kinds of crystal forms, has been widely used to activate PMS. However, the role of morphological scale and crystal structures on the catalytic capability of MnO 2 still lacks further study. In this study, four different crystal forms of MnO 2 (α-MnO 2 , β-MnO 2 , γ-MnO 2 , and δ-MnO 2 ) are succeeded in being fabricated via hydrothermal processes and evaluated by activating PMS for the removal of Reactive Yellow X-RG, typical azo dye. Experiment results indicate that α-MnO 2 with a one-dimensional structure exhibits the best catalytic performance among the four as-prepared MnO 2 , which can be attributed to its broadest crystal interplanar distance (0.692), the highest portion of Mn (III)/Mn (IV) (4.194), and lowest value of average oxidation state AOS (2.696). Correlation analysis confirms that interplanar distance is the most relative factor with the catalytic activity of MnO 2 among the three studied factors ( R 2 = 0.99715). Meanwhile, the morphological scale structure of α-MnO 2 can also account for its highest catalytic ability among the four as-prepared MnO 2 , including its large specific area and advantageous one-dimensional nanostructure. Furthermore, according to the response surface methodology, when the dosage of PMS is 2.369 g/L, the dosage of α-MnO 2 is 0.991 g/L, and the initial dye concentration is 1025 mg/L, the maximum removal rate of Reactive Yellow X-RG is up to 97.38%. Graphical abstract
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Haoran Song,Linxia Yan,Yuwei Wang,Jin Jiang,Jun Ma,Changping Li,Gang Wang,Jia Gu,Peng Liu
In this study, a comparison between electrochemically activated peroxomonosulfate (PMS) and peroxydisulfate (PDS) using carbon anodes was conducted for the first time. PMS activation was achieved using graphite (GR) and multi-walled carbon nanotube (MWCNT) anodes, which significantly promoted the degradation of organic pollutants sulfamethoxazole (SMX). The radical probing and scavenging experiments demonstrated that SO 4 − was the dominant reactive species (64.93% relative contribution ratio). By contrast, nonradical oxidation accounted for 95.79% relative contribution ratio to organic pollutants degradation in electrochemically activated PDS process under the identical conditions. The structure difference between PDS ( − O 4 S-SO 4 − ) and PMS (HO-SO 4 − ) led to their various reactivities. The electrochemically activated PMS molecule (PMS*, acting as nonradical oxidation) had higher reactivity and lower stability than electrochemically activated PDS molecule (PDS*, acting as nonradical oxidation), thus to quickly decomposed to SO 4 − . Interestingly, electrochemically activated PMS (radical oxidation system) exhibited stronger resistance towards water background components than PDS (nonradical oxidation system), being suitable to treat the complicated water and wastewater containing various ions and organic compounds.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 6
·期 2
·866-871
·
IF 3.84
Yang Lei,Chuh-Shun Chen,Jia Ai,Heng Lin,Yao-Hui Huang,Hui Zhang
How to effectively activate oxidants like hydrogen peroxide (H2O2), peroxydisulfate (PDS) and peroxymonosulfate (PMS) is the focus of advanced oxidation processes (AOPs). In this study, we have found that PMS can directly decolorize cationic dyes without activation in a wide pH range (2.0–12.0). In addition, the presence of Cl− results in the formation of free available chlorine species and thus improves the degradation efficiency as well as broadening the scope of target pollutants. The first-order rate constant increased by 4.3 times when 2.5 mM Cl− was added as observed by an increase from 0.021 to 0.089 min−1, which further rose to 1.371 min−1 when Cl− was present at a level of 50 mM. Furthermore, it was found that only PMS has such an amazing effect while H2O2 and PDS do not. Radical quenching experiments and electron paramagnetic resonance (EPR) studies show that the decolorization of cationic dyes by PMS does not rely on the formation of sulfate radicals. A plausible mechanism is that cationic dyes (i.e., RhB+) first form a complex with the active component of PMS (HSO5−) owing to their electrical interaction. Subsequently, direct electron transfer from cationic dyes to HSO5− may occur and probably this is responsible for the bleaching of cationic dyes.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Zihao Wan,Minghao Xu,Liang Zhou,Ya Zhang,Xuerui Yang,Sen Lin,Jean-Marc Chovelon,Lei Zhou
In this study, a novel strategy for selectively generating Co(IV)=O species during peroxymonosulfate (PMS) activation was proposed, utilizing an optimized Co 4 Cu 1 -layered double hydroxide (LDH) material with low-coordination and high-spin-state Co sites. The incorporation of Cu(II), influenced by the Jahn-Teller effect, altered the geometry and coordination at Co(III) sites, optimizing the filling of Co 3d orbitals. The Co 4 Cu 1 -LDH/PMS system demonstrated exceptional catalytic activity for degrading emerging contaminants (ECs) across various water matrices, with a high concentration of Co(IV)=O generation. Continuous flow experiments showed an average 97.51 % degradation over 10 hours, indicating significant practical potential. Mechanistically, enhanced performance was attributed to a single electron transfer process and optimized orbital configurations for oxygen ligands at Co(III) sites. This study offers both theoretical insights and practical guidance for developing efficient catalysts targeting Co(IV)=O species in Fenton-like systems.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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IF 5.8
Hongji Chen,Yan Wu,Huiping Xiao,Hongfei Yin,Qian Fei,Chunyu Yuan,Qiuyu Zhao,Yujin Zhang,Yongzheng Zhang,Woonming Lau
Owing to the low conversion efficiency of Fe 3+ to Fe 2+ during the peroxymonosulfate (PMS) activation process, the design of an efficient Fenton-like catalyst is still a challenge. In this work, 0D/2D Co-doped Fe 2 O 3 /g-C 3 N 4 (CNCFO) composite catalysts were constructed for organic pollutant degradation, where the Co-doping not only boosts the conversion efficiency of Fe 3+ to Fe 2+ , but also acts as active site for PMS activation. Among them, CNCFO2 showed excellent catalytic performance, where 96.4% of MO could be degraded within 45 s. X-ray photoelectron spectroscopy (XPS) confirmed that the cobalt doping promoted the cycle of Fe 3+ /Fe 2+ , which was responsible for the enhanced PMS activation. Meanwhile, the good stability and reusability of CNCFO2 itself provide opportunities for its potential practical applications. Based on systematical characterizations, the Z-scheme photo-Fenton mechanism was proposed. This study offers a fresh perspective on the advancement of designing highly efficient Fenton-like catalyst for applications in the field of environmental purification.
研究领域:
环境科学
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催化材料
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）