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Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1372-4

摘要：

• The MCNZVI is prepared as an interesting material for PS activation.

关键词： MCNZVI     Core-shell structure     Reactive Black 5     Persulfate     Mechanism    

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Comparison of exogenous degrader-enhanced bioremediation with low-dose persulfate oxidation for polycyclic

《环境科学与工程前沿（英文）》 2023年 第17卷 第11期 doi: 10.1007/s11783-023-1733-x

摘要： Polycyclic aromatic hydrocarbon (PAH)-contaminated soils are usually complex and characterized by a lack of nutrition and soil salinization, resulting in difficulties in soil remediation. In this study, bioaugmentation with a PAH-degrading Bacillus PheN7 (BA) and low-dose persulfate oxidation (PS), along with natural biodegradation, were utilized to remediate alkaline PAH-contaminated soil. The soil used in the study had a pH of 9.35, and the total PAH content was 568.8 ± 31.0 mg/kg dry soil. After 42 d of remediation, the degradation efficiency of PAHs was 96.72% and 93.88% using persulfate oxidation and bioaugmentation, respectively, whereas 38.66% of PAHs were degraded in natural attenuation (NA). Bacillus was the dominant genera throughout the process of bioremediation with the relative abundance of 79.3% on day 42 in the BA system, whereas, Alcanivorax was enriched and became the dominant genera in PS systems. In the meantime, PAH degradation genes were detected with remarkably higher level in the BA system than in PS system during the remediation. In addition to the degradation of contaminants, persulfate oxidation promotes microbial bioremediation efficiency mainly by lowering the pH to neutral and increasing the active phosphorus content in the soil. Microbial species and ecological niches were less reduced in the PS system than in the BA system. Collectively, persulfate oxidation had a better impact on the soil microbiome and is more suitable for long-term soil health than bioaugmentation through PheN7 addition.

关键词： Bioaugmentation     Low-dose persulfate oxidation     Polycyclic aromatic hydrocarbon     Remediation    

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Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic

Minhui XU,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 438-446 doi: 10.1007/s11783-015-0798-6

摘要： The thermally activated persulfate (PS) degradation of carbon tetrachloride (CT) in the presence of formic acid (FA) was investigated. The results indicated that CT degradation followed a zero order kinetic model, and was responsible for the degradation of CT confirmed by radical scavenger tests. CT degradation rate increased with increasing PS or FA dosage, and the initial CT had no effect on CT degradation rate. However, the initial solution pH had effect on the degradation of CT, and the best CT degradation occurred at initial pH 6. Cl had a negative effect on CT degradation, and high concentration of Cl displayed much strong inhibition. Ten mmol·L promoted CT degradation, while 100 mmol·L inhibited the degradation of CT, but promoted CT degradation in the presence of FA. The measured Cl concentration released into solution along with CT degradation was 75.8% of the total theoretical dechlorination yield, but no chlorinated intermediates were detected. The split of C-Cl was proposed as the possible reaction pathways in CT degradation. In conclusion, this study strongly demonstrated that the thermally activated PS system in the presence of FA is a promising technique in in situ chemical oxidation (ISCO) remediation for CT contaminated site.

关键词： persulfate     carbon tetrachloride     thermal activation     formic acid     carbon dioxide radical anion    

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Integration of microbial reductive dehalogenation with persulfate activation and oxidation (Bio-RD-PAO

《环境科学与工程前沿（英文）》 2022年 第16卷 第2期 doi: 10.1007/s11783-021-1457-8

摘要：

•Bio-RD-PAO can effectively and extensively remove organohalides.

关键词： Bio-RD-PAO     Microbial reductive dehalogenation     Persulfate     Organohalide respiration     Complete attenuation    

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Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1581-1592 doi: 10.1007/s11705-023-2327-7

摘要： Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al2O3, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including SO4•‒, OH •, and O2•‒) and singlet oxygen (1O2) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al2O3 promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

关键词： Cu–Al bimetallic oxides     mesoporous silica spheres     peroxydisulfate     bisphenol A    

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Decomposition of perfluorooctanoic acid by microwave-activated persulfate: Effects of temperature, pH

Yuchi LEE, Shanglien LO, Jeff KUO, Chinghong HSIEH

《环境科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 17-25 doi: 10.1007/s11783-011-0371-x

摘要： Microwave-hydrothermal treatment of persistent and bioaccumulative perfluorooctanoic acid (PFOA) in water with persulfate ( ) has been found effective. However, applications of this process to effectively remediate PFOA pollution require a better understanding on free-radical scavenging reactions that also take place. The objectives of this study were to investigate the effects of pH (pH= 2.5, 6.6, 8.8, and 10.5), chloride concentrations (0.01–0.15 mol·L ), and temperature (60°C, 90°C, and 130°C) on persulfate oxidation of PFOA under microwave irradiation. Maximum PFOA degradation occurred at pH 2.5, while little or no degradation at pH 10.5. Lowering system pH resulted in an increase in PFOA degradation rate. Both high pH and chloride concentrations would result in more scavenging of sulfate free radicals and slow down PFOA degradation. When chloride concentrations were less than 0.04 mol·L at 90°C and 0.06 mol·L at 60°C, presence of chloride ions had insignificant impacts on PFOA degradation. However, beyond these concentration levels, PFOA degradation rates reduced significantly with an increase in chloride concentrations, especially under the higher temperature.

关键词： microwave     perfluorooctanoic acid     pH     persulfate     chloride ions     perfluorocarboxylic acids    

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Efficient photodegradation of phenol assisted by persulfate under visible light irradiation via a nitrogen-doped

Yan Cui, Zequan Zeng, Jianfeng Zheng, Zhanggen Huang, Jieyang Yang

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1125-1133 doi: 10.1007/s11705-020-2012-z

摘要： To realize the utilization of visible light and improve the photocatalytic efficiency of organic pollutant degradation in wastewater, a nitrogen-doped titanium-carbon composite (N-TiO /AC) prepared by sol-gel methods was applied in the photodegradation of phenol assisted by persulfate under visible light irradiation (named N-TiO /AC/PS/VIS). The results show that a synergistic effect exists between visible-light photocatalysis and persulfate activation. Compared with TiO /PS/VIS, the phenol degradation rate was found to be observably improved by 65% in the N-TiO /AC/PS/VIS system. This significant increase in degradation rate was mainly attributed to the following two factors: 1) The N and C doping can change the crystal structure of TiO , which extends the TiO absorption wavelength range to the visible light region. 2) As an electron acceptor, PS can not only prevent electrons and holes from recombining with each other but can also generate strong oxidizing radicals such as ∙SO and ∙OH to accelerate the reaction dynamics. The process of phenol degradation was found to be consistent with the Langmuir pseudo-first-order kinetic model with an apparent rate constant of 1.73 min . The N-TiO /AC/PS/VIS process was proven to be a facile method for pollutant degradation with high pH adaptability, excellent visible-light utilization and good application prospects.

关键词： N-TiO2/AC     visible light     photocatalysis     persulfate activation     phenol    

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Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 460-469 doi: 10.1007/s11705-022-2224-5

摘要： Nitric oxide being a major gas pollutant has attracted much attention and various technologies have been developed to reduce NO emission to preserve the environment. Advanced persulfate oxidation technology is a workable and effective choice for wet flue gas denitrification due to its high efficiency and green advantages. However, NO absorption rate is limited and affected by mass transfer limitation of NO and aqueous persulfate in traditional reactors. In this study, a rotating packed bed (RPB) was employed as a gas–liquid absorption device to elevate the NO removal efficiency (ηNO) by aqueous persulfate ((NH4)2S2O8) activated by ferrous ethylenediaminetetraacetate (Fe2+-EDTA). The experimental results regarding the NO absorption were obtained by investigating the effect of various operating parameters on the removal efficiency of NO in RPB. Increasing the concentration of (NH4)2S2O8 and liquid–gas ratio could promoted the oxidation and absorption of NO while the ηNO decreased with the increase of the gas flow and NO concentration. In addition, improving the high gravity factor increased the ηNO and the total volumetric mass transfer coefficient (KGα) which raise the ηNO up to more than 75% under the investigated system. These observations proved that the RPB can enhance the gas–liquid mass transfer process in NO absorption. The correlation formula between KGα and the influencing factors was determined by regression calculation, which is used to guide the industrial scale-up application of the system in NO removal. The presence of O2 also had a negative effect on the NO removal process and through electron spin resonance spectrometer detection and product analysis, it was revealed that Fe2+-EDTA activated (NH4)2S2O8 to produce •SO4–, •OH and •O2–, played a leading role in the oxidation of NO, to produce NO3– as the final product. The obtained results demonstrated a good applicable potential of RPB/PS/Fe2+-EDTA in the removal of NO from flue gases.

关键词： rotating packed bed     Fe2+-EDTA     sulfate radical     hydroxyl radical     NO removal efficiency    

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Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

Qishi LUO

《环境科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 188-194 doi: 10.1007/s11783-013-0544-x

摘要： The oxidation of aqueous monochlorobenzene (MCB) solutions using thermally- activated persulfate has been investigated. The influence of reaction temperature on the kinetics of MCB oxidation was examined, and the Arrenhius Equation rate constants at 20°C, 30°C, 40°C, 50°C, and 60°C for MCB oxidation performance were calculated as 0, 0.001, 0.002, 0.015, 0.057 min , which indicates that elevated temperature accelerated the rate. The most efficient molar ratio of persulfate/MCB for MCB oxidation was determined to be 200 to 1 and an increase in the rate constants suggests that the oxidation process proceeded more rapidly with increasing persulfate/MCB molar ratios. In addition, the reactivity of persulfate in contaminated water is partly influenced by the presence of background ions such as Cl , , , and . Importantly, a scavenging effect in rate constant was observed for both Cl and but not for other ions. The effective thermally activated persulfate oxidation of MCB in groundwater from a real contaminated site was achieved using both elevated reaction temperature and increased persulfate/MCB molar ratio.

关键词： persulfate     monochlorobenzene     advanced oxidation process    

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过硫酸盐诱导的缺陷氮化碳中三配位氮（N3C）空位增强光催化产过氧化氢 Article

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

《工程（英文）》 2023年 第25卷 第6期   页码 214-221 doi: 10.1016/j.eng.2021.12.016

摘要：

近年来，原位光催化可持续过氧化氢合成技术受到越来越多的关注。其中石墨氮化碳（g-C3N4）被认为是最有前途的合成过氧化氢的光催化剂之一；并且，在g-C3N4中引入氮空位已被证明是提高其光催化活性的有效策略。然而，由于g-C3N4中不同类型的氮空位对光催化活性的影响方式不同，氮空位的光催化作用机制尚不清楚。在此，本文提出了一种简便的过硫酸钠共晶聚合方法，制备了具有丰富三配位氮空位（N3C）的g-C3N4。这种类型的氮空位在g-C3N4光催化产过氧化氢的研究中尚未得到重视。本研究的结果表明，在g-C3N4中引入N3C空位可以成功地拓宽光吸收范围，抑制光激发电荷的重组，增强O2的吸附和活化。富含N3C空位的g-C3N4的光催化过氧化氢产量是原始g-C3N4的4.5倍。本研究提出了在g-C3N4中引入N3C空位的新策略，为开发光催化产过氧化氢的活性催化剂提供了一种新方法。

关键词： 氮化碳     N3C空位     过氧化氢     光催化     过硫酸盐    

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Preparation and characterization of SO42-/TiO2 and S2O82-/TiO2 catalysts

MA Xuedan, GUO Daishi, JIANG Qizhong, MA Zifeng, MA Zhengfei, YE Weidong, LI Chunbo

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 45-49 doi: 10.1007/s11705-007-0009-5

摘要： Nanosized solid superacids SO/TiO and SO/TiO, as well as MCM-41-supported SO/ZrO, were prepared. Their structures, acidities, and catalytic activities were investigated and compared using XRD, N adsorption-desorption, and in situ FTIR-pyridine adsorption, as well as an evaluation reaction with pseudoionone cyclization. The results showed that SO/TiO and SO/TiO possess not only nanosized particles with diameters <7.0 nm, a BET surface greater than 140 cm/g and relatively regular mesostructures with pores around 4.0 nm, but also a pure anatase phase and strong acidity. Different from the Lewis acid nature of SO/ZrO/MCM-41, SO/TiO and SO/TiO exhibit mainly Br¢nsted acidities. The strongest Br¢nsted acid sites were produced on SO/TiO promoted with HSO, while Lewis acid sites on SO/TiO even stronger than those on SO/ZrO/MCM-41 were generated when persulfate solution was used as sulfating agent. Because of their distinct acid natures, SO/TiO and SO/TiO exhibited catalytic activities for the cyclization of pseudoionone that were much higher than that of SO/ZrO/MCM-41. It can be concluded that the existence of more Br¢nsted acid sites was favorable for proton participation in the cyclization reaction.

关键词： exhibit     Different     persulfate     adsorption-desorption     catalytic    

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标题 作者 时间 类型 操作

Preparation of nZVI embedded modified mesoporous carbon for catalytic persulfate to degradation of reactive

期刊论文

Comparison of exogenous degrader-enhanced bioremediation with low-dose persulfate oxidation for polycyclic

期刊论文

Degradation of carbon tetrachloride in thermally activated persulfate system in the presence of formic

Minhui XU,Xiaogang GU,Shuguang LU,Zhouwei MIAO,Xueke ZANG,Xiaoliang WU,Zhaofu QIU,Qian SUI

期刊论文

Integration of microbial reductive dehalogenation with persulfate activation and oxidation (Bio-RD-PAO

期刊论文

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

期刊论文

Decomposition of perfluorooctanoic acid by microwave-activated persulfate: Effects of temperature, pH

Yuchi LEE, Shanglien LO, Jeff KUO, Chinghong HSIEH

期刊论文

Efficient photodegradation of phenol assisted by persulfate under visible light irradiation via a nitrogen-doped

Yan Cui, Zequan Zeng, Jianfeng Zheng, Zhanggen Huang, Jieyang Yang

期刊论文

Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate

期刊论文

Oxidative treatment of aqueous monochlorobenzene with thermally-activated persulfate

Qishi LUO

期刊论文

过硫酸盐诱导的缺陷氮化碳中三配位氮（N3C）空位增强光催化产过氧化氢

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

期刊论文

Preparation and characterization of SO42-/TiO2 and S2O82-/TiO2 catalysts

MA Xuedan, GUO Daishi, JIANG Qizhong, MA Zifeng, MA Zhengfei, YE Weidong, LI Chunbo

期刊论文