ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 35
·83545-83557
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IF 5.8
Xiong Yehan,Zhou Ting,Bao Jianguo,Du Jiangkun,Faheem Muhammad,Luo Liting
Fenton-like oxidation processes are widely used to degrade recalcitrant organic pollutants, but are limited by narrow application pH and low reaction efficiency. This study investigated the synchronous activation of H 2 O 2 and persulfate (PDS) by sulfidated zero valent iron (S-nZVI) in ambient conditions for Fenton-like oxidation of bisphenol S (BPS), an estrogenic endocrine-disrupting chemical. The activation of S-nZVI induced H 2 O 2 or PDS could be greatly enhanced with the assistance of PDS and H 2 O 2 , respectively, even across a wide range of pH value (3–11). The first-order rate constant of S-nZVI/H 2 O 2 /PDS, S-nZVI/PDS and S-nZVI/H 2 O 2 systems was found to be 0.2766 min −1 , 0.0436 min −1 , and 0.0113 min −1 , respectively. A significant synergy between H 2 O 2 and PDS was achieved when the PDS-H 2 O 2 molar ratio was above 1:1, and where sulfidation promoted iron corrosion and decreased solution pH were observed in the S-nZVI/H 2 O 2 /PDS system. Radical scavenging experiments and electron paramagnetic resonance (EPR) investigations suggest that both SO 4 •− and • OH were generated and that • OH played a crucial role in BPS removal. Furthermore, four BPS degradation intermediates were detected and three degradation pathways were proposed in line with the HPLC-Q-TOF–MS analysis. This study demonstrated that compared to the traditional Fenton-like system, the S-nZVI/H 2 O 2 /PDS system could be a more efficient, advanced oxidation technology capable of being used across a broad pH range for emerging pollutants’ degradation.
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
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Yabin Li,Jingyao Qi,Jimin Shen,Pengwei Yan,Jing Kang,Binyuan Wang,Shuyu Wang,Jinxiang Zuo,Zhonglin Chen
Peroxymonosulfate (PMS)-based advanced oxidation processes are perceived as a novel strategy for water purification. However, designing an efficient catalyst with a low metal leaching rate remains challenging. Here, under palygorskite (PAL) mediation, 16%-CoCu 0.4 Fe 1.6 O 4 @PAL (16%-CCFO@PAL) was constructed, exhibiting ample oxygen vacancies (V O ) and low metal leakage. The V O was confirmed by systematic characterizations and theoretical calculations. The catalyst showed the efficient catalytic capacity for PMS by dual-path (i.e., metal sites and V O ) activation. Large amounts of SO 4 •- , •OH, and 1 O 2 were produced, greatly destroying bisphenol S (BPS). BPS removal was greater than 99% within 25 min in the 16%-CCFO@PAL/PMS system. At the metal sites, PMS was activated under the synergistic effects of Co(II)/Co(III), Fe(II)/Fe(III), and Cu(I)/Cu(II) pairs and electron transfer. In addition to metal sites, the V O was also an activation center for PMS, which mainly captured the O I atom in [H-O I -O II -SO 3 ] - , donating an electron to O I and promoting SO 4 •- generation. The interfacial reaction mechanism was explored by in situ tests, and a dual-path activation mechanism was proposed. This work provides a new perspective for V O -assisted PMS activation for water treatment.
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
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 10
·103504
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IF 3.9
Lu Chen,Qibin Tao,Lin Wang,Hao Lan,Qizhou Dai
In this study, a lead dioxide electrode co-modified with carbon microspheres and neodymium (CMS-Nd-PbO2) was prepared. The structural morphology and electrochemical properties of the four electrodes, PbO2, CMS-PbO2, Nd-PbO2, and CMS-Nd-PbO2, were compared by field emission scanning electron microscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, cyclic voltammetry, and electrochemical impedance, respectively. The results showed that the prepared CMS-Nd-PbO2 electrode had higher surface denseness and higher electrode activity. Based on the accelerated lifetime experiment, the actual working life of four electrodes was studied, and the CMS-Nd-PbO2 electrode had a relatively long lifetime, increased 24.60% compared with the PbO2 electrode. The influencing parameters of electrochemical degradation of bisphenol S (BPS) by CMS-Nd-PbO2 electrode, the ability of different electrodes to generate hydroxyl radicals, reaction mechanism, and the possible BPS degradation pathways were also discussed. Further, the safety of the prepared electrode was evaluated. Under the optimal parameters, the removal rate of BPS and chemical oxygen demand (COD) were 96.49% and 51.84%, respectively. The dissolved lead ion concentration in the solution after electrochemical oxidation was lower than the WHO standard. The CMS-Nd-PbO2 electrode showed promising applications in the degradation of emerging contaminants wastewater.
研究领域:
环境科学
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电化学工程
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Yi Ren,Chao Liu,Naiwen Li,Bo Lai,Jun Li
In this study, a new Fenton-like catalyst was developed through incorporating iron and copper in polymeric graphitic carbon nitride (FeCu/CN) for catalytic activity and reusability enhancement. With theoretical Fe/Cu ratio of 7:3 (Fe 7 Cu 3 /CN) and pH of 5, the bimetallic catalyst system showed a pseudo-first-order rate constant of 0.07294 min −1 for bisphenol S (BPS) degradation, which was near double the sum of values in monometallic catalyst systems. Moreover, the new catalyst showed much better performance for reuse, BPS removal of which catalyzed system decreased from 98.0 % to 87.3 % after five cycles used. Comparatively, BPS removal declined from 69.5 % to 45.0 % in Fe/CN catalyzed system. Characterization results indicate the superiority of Fe 7 Cu 3 /CN for Fenton-like catalysis is mainly attributed to the intrinsic advantage of CN support, Fe(II) formation, copper catalysis, and synergistic effect between iron and copper. Furthermore, hydroxyl radicals were determined as the main species for pollutant degradation, and their accumulation was monitored. The destruction pathways of BPS were analyzed by detection of degradation intermediates, and the results further confirm the main active species of hydroxyl radicals. Moreover, the new Fenton-like system also exhibited good performance for different pollutant removal and real wastewater treatment. This study provided a new catalyst with superior catalytic activity and favorable reusability, and also sheds new light on supported bimetallic catalyst development.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Yi Ren,Jing Zhang,Chenghan Ji,Shu Wang,Lu Lv,Weiming Zhang
In this study, a new catalyst was fabricated by pyrolysis under nitrogen atmosphere with MIL-53(Fe) as the precursor, and was applied to catalyze Fenton-like process. Effects of calcination temperature and pH on decontamination performance, and stability of materials were investigated. Under optimal conditions (calcination temperature of 500 °C and pH of 5.0), the new Fenton-like system remained low iron leaching , and achieved high pseudo-first-order rate constant of 0.0251 min −1 for bisphenol S (BPS) removal, which is much higher than those in MIL-53(Fe), and nano-Fe 3 O 4 catalyzed Fenton-like systems. The superiority of the new catalyst for Fenton-like catalysis was attributed to high specific surface area, as well as formed Fe(II), coordinatively unsaturated iron center and the Fe-O/Fe-C compounds based on the analyses of characterizations. Furthermore, main active species for BPS degradation was identified as hydroxyl radicals , and total hydroxyl radical generation was determined by trapping experiments. The degradation pathways of BPS were also proposed by intermediates monitoring. Moreover, this catalyst showed good potential for practical application, according to the evaluation of reuse, different pollutants degradation , and BPS removal in real wastewater . We believe this study developed a new catalyst with high catalytic activity , high stability and wide application scope, and also sheds light on further development of metal-organic frameworks for Fenton-like catalysis.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Ya Zeng,Lingfeng Qin,Sijie Tian,Caicheng Long,Taiping Qing,Peng Zhang,Bo Feng
Cobalt-based multiphase catalysts can effectively activate peroxymonosulfate (PMS) and degrade organic pollutants. However, their practical application faces critical challenges, including insufficient exposure of active sites, slow reaction kinetics, and cobalt ion leaching, which collectively reduce catalytic efficiency and sustainability. Although there have been attempts to improve the catalytic efficiency through structural modifications such as core-shell structure or porous design, these strategies are still difficult to optimize the active site exposure and cobalt ion stability simultaneously. To overcome these limitations, here we propose a novel triple-shell yolk@shell architecture (3YS-Co@NC) constructed via a stepwise strategy involving crystal extension growth, selective etching, and calcination. The optimized nanoreactor degraded 100 % of bisphenol S (BPS) within 12 min with a rate constant (0.342 min −1 ) 9.5-, 2.34-, and 1.49-fold higher than solid nanoparticles (Co@NC), single-shell (1YS-Co@NC), and double-shell (2YS-Co@NC) counterparts, respectively. Notably, the TOC removal rate of 3YS-Co@NC reached 71 %, surpassing those of 1YS-Co@NC (53 %), 2YS-Co@NC (65 %), and Co@NC (21 %). The enhanced performance results from (i) the yolk@shell structure providing nanoreaction cavities and abundant active sites, and (ii) the robust Co 0 /Co 2+ /Co 3+ redox cycling. Quenching experiments and EPR analysis revealed that SO 4 •- and •OH dominated PMS activation, while O 2 •- played an auxiliary role. In contrast, 1 O 2 exhibited negligible contribution. LC/MS analysis identified key degradation intermediates, and the ECOSAR model predicted reduced biotoxicity of these products. This study not only promotes the development of advanced oxidation processes, but also provides a new insight into the design of cobalt-based catalysts.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jiali Peng,Hongyu Zhou,Wen Liu,Zhimin Ao,Haodong Ji,Yang Liu,Shijun Su,Gang Yao,Bo Lai
In this study, natural chalcopyrite (NCP) was employed in the activation of peroxymonosulfate (PMS) for bisphenol S (BPS) degradation. Firstly, the NCP catalyst was characterized via X-ray diffraction (XRD), scanning electron microscopy and energy dispersive spectroscopy (SEM-EDS) techniques. Then, several key parameters such as catalyst dosage, PMS dosage and initial pH were investigated in NCP/PMS system. Furthermore, the transformation of various free radicals (SO 4 •− , • OH and O 2 •− ) with the changes of initial pH were investigated by quenching experiments and electron spin resonance (ESR) study. Also, sulfur species cycling of copper and iron species were investigated via exogenous Cu 2+ and Fe 3+ addition experiments and X-ray photoelectron spectroscopy (XPS) analysis, the result indicated that sulfur species promoted Fe 3+ /Fe 2+ and Cu 2+ /Cu + cycles on the NCP surface. Furthermore, thirteen major degradation intermediates of BPS were detected by UPLC-QTOF-MS/MS and density functional theory (DFT) method was used to illustrate possible reaction pathways of BPS. Finally, a reasonable reaction mechanism of NCP/PMS system for BPS degradation was proposed on the basis of the comprehensive analysis. In brief, this work helps to provide useful information for the application of natural metallic sulfide minerals in treatment of contaminated waters.
研究领域:
环境科学
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化学工程
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分析化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）