APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Shizong Wang,Jianlong Wang
This study prepared the carbon-supported cobalt catalyst (Co-C-X) for activating peroxymonosulfate (PMS), and investigated the effect of co-pyrolysis temperature of graphitic carbon nitride (g-C 3 N 4 ) and vitamin B 12 on the catalytic activity. It was found that with the increase of co-pyrolysis temperature, the catalytic activity of Co-C-X increased, due to the different coordination structures of cobalt. At 500 °C (Co-C-500), cobalt existed as CoO; while it was single atom Co at 600 °C (Co-C-600); and small size CoO at 700 °C (Co-C-700). Co-C-X could activate PMS to produce hydroxyl radicals, sulfate radicals, high-valent cobalt-oxo and singlet oxygen, which depended on the pyrolysis temperature. Although Co-C-700 had the highest catalytic activity, the leaching cobalt was also highest (3.23 mg/L), compared with that of Co-C-500 (0.27 mg/L) and Co-C-600 (0.14 mg/L). Co-C-600 had fast degradation for atrazine, nitrobenzene , bisphenol A, phenol and 4-chlorophenol, which also had wide pH range and high tolerance to inorganic ions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Mengke Li,Zhiguo He,Hui Zhong,Wei Sun,Liang Hu,Mengqi Luo
A novel ternary composite catalyst (FeOOH/Fe 2 O 3 /(Fe 0.67 Mn 0.33 )OOH ) directly prepared from electrolytic manganese residue was applied for terpineol degradation in this study. The reaction system could remove 76.8% of chemical oxygen demand (COD) from simulated water containing terpineol (100 mg/L), while the degradation process could be accelerated under alkaline condition (84.6% at pH 9.0). The degradation performances of Fe 2 O 3 , FeOOH and (Fe 0.67 Mn 0.33 )OOH indicated that the in-situ formed (Fe 0.67 Mn 0.33 )OOH riched in oxygen vacancies (O V ) could promote the PMS activation activity of catalyst mainly ascribed by enhancing interfacial electron transfer . The · OH was the primary active radical, the production of which was favored by the metal−OH. This ternary composite catalyst had anti-jamming ability toward most common ions. Further, this system also displayed an outstanding degradation ability for actual mineral processing wastewater (93.2% COD removal). The developed system expanded the horizon for the high-value utilization of metallurgical slag and the treatment of refractory organic pollutants in mineral processing wastewater.
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高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Xiwen Liu,Penghui Shao,Shanshan Gao,Zhaoyu Bai,Jiayu Tian
Benzoquinone (BQ) is of great significance for enhancement of contaminants degradation in the homogeneous oxidation system of peroxymonosulfate (PMS). However, the role of BQ in the heterogeneous activation of PMS for contaminants oxidation is still not clear. Herein, this work reported that the addition of BQ into the Fe 3 S 4 /PMS system could effectively enhance the degradation and mineralization of bisphenol A (BPA). Mechanistic study uncovered that the BQ and PMS would form active complexes (BQ-PMS*) on the surface of Fe 3 S 4 and the excited BQ-PMS* can oxidize the BPA. To be specific, the electron of BPA was extracted by BQ-PMS* and then transfer to the surface of Fe 3 S 4 . The surface electron can induce the change of valence state of S and Fe elements, which can trigger the degradation of BPA and inhibit the decomposition of BQ itself. To the best of our knowledge, it is the first time to unveil the positive role of BQ in the heterogeneous activation of PMS, which may shed new light on the establishment of high-efficient PMS-based oxidation technology for remediation of organic pollutant.
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PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Xuan Chen,Jie Zhou,Hanwen Yang,Hui Wang,Huanxuan Li,Shengji Wu,Wei Yang
Refractory organic pollutant effluent has led to severe water pollution . In this study, magnetic Co–N-doped carbon hybrid catalysts (Co-NC- x ) were fabricated using a facile cation exchange combined pyrolysis and self-reduction technique to activate peroxymonosulfate (PMS) for rehabilitation of the water environment. Factors affecting the catalytic activity of the Co-NC-850 were comprehensively examined. 100% of RhB degradation efficiency within 20 min was achieved in the Co-NC-850/PMS system at the optimum conditions ( C 0 = 80 mg L −1 , catalyst loading 0.025 g L −1 , PMS concentration 0.8 mM, native pH and 25 °C). The electron paramagnetic resonance measurements and competitive quenching tests demonstrated that a sulfate radical (SO 4 • - ) and singlet oxygen ( 1 O 2 ) account for RhB degradation in the Co-NC-850/PMS system, and 1 O 2 contributed ~86.2% to RhB removal. The synergistic effect of Co 0 nanoparticles (NPs) and NC on Co-NC-850 might induce a predominant non-radical route to trigger PMS activation for RhB degradation. Direct oxidation of O 2 • - by a hydroxyl radical (•OH) might be the crucial process for forming 1 O 2 . Magnetic response and successive cycles verified that Co-NC-850 has superior separable performance and reusability. This innovative magnetic Co-NC-850 hybrid catalyst for PMS activation delivered vast potential for disintegration of refractory organic contaminants .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Zhiyan Huang,Pingxiao Wu,Chenhui Liu,Meiqing Chen,Shanshan Yang,Zhi Dang,Nengwu Zhu
Understanding the origin of high activity of graphene layers encapsulated Fe-N-C catalysts in Fenton-like reaction is critical, but still challenging for developing catalysts with high activity and durability. Therefore, we prepared a highly active Fe-N-C catalyst (Fe x Mn y -Fe@NCs) containing FeN 4 coordination to activate peroxymonosulfate (PMS) toward 4-aminobenzoic acid ethyl ester (ABEE) degradation, and revealed the multiple catalytic reaction sites by investigating the composition and the structure of the catalyst. The relationship between the catalytic degradation performance and multiple catalytic reaction sites was performed on the basis of both experiments and density functional theory (DFT) calculations. The catalytic performance of Fe 2 Mn 1 -Fe@NCs was found to show optimal catalytic degradation performance. Pyrrolic N served as adsorption site as well as singlet oxygen generation site to promote the catalytic degradation. Fe-pyridinic N-C acted as hydroxyl radical and sulfate radical generation site. Both singlet oxygen and superoxide radical were dominated the catalytic reaction. The insight achieved from this study may be further applied to other Fe-N-C catalysts design and further efficient organic pollution remediation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ying Cao,Wei Qiu,Yumeng Zhao,Juan Li,Jin Jiang,Yi Yang,Su-Yan Pang,Guanqi Liu
The frequent detection of chloramphenicol (CAP) in wastewater and surface water gives rise to concerns on its fatal myelosuppression and aplastic anemia. Recently, the combination of ozone and peroxymonosulfate (O 3 /PMS) has received wide attention in removing pollutants due to the multiple oxidants (i.e., O 3 , hydroxyl radicals ( OH) and sulfate radicals (SO 4 − )) existed therein. This study showed that O 3 /PMS could effectively degrade CAP under various conditions. The second-order rate constant of CAP with O 3 , OH and SO 4 − was 0.291 ± 0.005 , 2.27 ( ± 0.03 ) × 10 9 and 1.02 ± 0.02 × 10 8 M - 1 s - 1 , respectively. The degradation efficiency of CAP was significantly enhanced as PMS concentration or pH increased. Bicarbonate (HCO 3 − ) at concentration of 5 mM slightly inhibited CAP degradation at pH 7. Chloride (Cl − ) at concentration of 0.5 mM enhanced CAP removal at pH 7, while this enhancement gradually weakened as Cl − concentration further increased. The degradation efficiency of CAP first increased with increasing natural organic matter (NOM) concentrations (0.1–0.3 mg/L), while it was completely suppressed at higher NOM concentrations (0.5 mg/L). Four degradation products in total of CAP were identified in O 3 -based processes (i.e., O 3 , O 3 /TBA, O 3 /H 2 O 2 , O 3 /PMS and O 3 /PMS/ tert -butyl alcohol (TBA) systems. Besides, these transformation products by OH, SO 4 − and/or O 3 were also distinguished. Finally, the impact of O 3 /PMS pre-oxidation on the formation of dichloroacetamide (DCAcAm) from CAP during post-chlorination process was investigated. Compared with the traditional O 3 and O 3 /H 2 O 2 processes, O 3 /PMS pre-oxidation generally led to the least generation of DCAcAm under similar conditions, where SO 4 − rather than OH was conducive to relieve the formation of DCAcAm. Moreover, the presence of NOM obviously alleviated the formation of DCAcAm by O 3 /PMS pre-oxidation.
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高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
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IF 7.963
Shiyin Zhao,Yangke Long,Xuehua Shen,Shubin Wang,Yiping Su,Xuanjun Zhang,Zuotai Zhang
Peroxymonosulfate (PMS)-based Fenton-like reactions are widely used for wastewater remediation. Metal-free carbonaceous activators can avoid the secondary pollution caused by metal leaching but often suffer from insufficient activity due to limited active centers and mass transfer barriers. Here, we prepared a series of heteroatom (N, S, F)-doped, highly porous carbonaceous materials (UC- X , X = N, S, F) by pyrolyzing UiO-66 precursors assembled by various organic ligands. Density functional theory calculations showed that the heteroatoms modulated the electronic structures of the carbon plane. UC- X exhibited significantly enhanced PMS activation capability compared with the undoped counterpart, in the efficiency order of UC-N > UC-S > UC-F > UC. UC-N (calcined at 1000°C) showed the best PMS activation, exceeding that of commonly used carbocatalysts. The prominent performance of UC-N originated from its unique porous structure and homogeneously dispersed graphitic N moieties. Trapping experiments and electron spin resonance showed a nonradical degradation pathway in the UC-N/PMS system, through which organics were oxidized by donating electrons to UC-N/PMS* metastable complexes. This work not only reports a universal way to access high-performance, metal-free PMS activators but also provides insight into the underlying mechanism of the carbon-activated PMS process.
研究领域:
环境科学
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材料科学
·
化学
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PubMed
高影响因子
CHEMOSPHERE
·
2024
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IF 8.1
Que Wu,Yongqing Zhang,Hong Meng,Xuefeng Wu,Yuqi Liu,Li Li
The non-free radical oxidation pathway (PMS-NOPs) of peroxymonosulfate (PMS) holds significant promise for practical wastewater treatment applications, owing to its low oxidation potential, high PMS utilization rate, and robust anti-interference capability in the degradation of pollutants. A novel activator copper nitrogen co-doped porous biochar (Cu-N-BC) with rich defect edges and functional groups was obtained by adding Cu and N to the biochar matrix generated by sodium alginate through pyrolysis in this study. Under the condition of 1 mM PMS, 30 mg/L activator was used to activate PMS and achieve efficient degradation of 10 mg/L paracetamol (PCT) within 15 min, with a high reaction rate constants (k obs ) of 0.391 min −1 . The activation mechanism of the Cu-N-BC/PMS/PCT system was a non-radical activation pathway with the dominance of singlet oxygen ( 1 O 2 ) and the presence of catalyst-mediated electron transfer. The graphite nitrogen, pyridine nitrogen, and Cu–N coordination introduced by Cu/N co-doping, as well as the carbon skeleton and C O functional group of biochar, were considered active sites that promote the 1 O 2 generation. The Cu-N-BC/PMS system exhibits strong stability, eco-friendliness, effective mineralization, and interference resistance across diverse pH levels (3–11) and interfering ions, including Cl − , H 2 PO 4 − , NO 3 − , SO 4 2− , and humic acid. Remarkably, it efficiently degrades PCT in tap and lake water, achieving a notable 63.73% TOC mineralization rate, with leached copper ions below 0.02 mg/L. This research introduces a novel method for obtaining metal nitrogen carbon activators and enhances understanding of PMS non-radical activation pathways and active sites.
研究领域:
环境科学
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废水处理
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高影响因子
Materials
·
2026
·Vol. 19
·期 1
·169
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IF 3.2
Mingxian Zhang,Jinsong Du,Xuemei Zheng,Aiyuan Ma
The widespread application of Rhodamine B (RhB) poses a serious threat to the aquatic environment. ZnFe2O4, as a catalyst material, can effectively activate persulfate (PMS) and respond to visible light, thus effectively degrading RhB with the joint assistance of sunlight and PMS. This study recovered Fe2O3from high-iron coal gangue through an activating–acid leaching–extracting–back-extracting process and synthesized ZnFe2O4catalysts (CG-ZFO) using coal gangue back-extraction liquid as the Fe source by a hydrothermal method and cetyltrimethylammonium bromide (CTAB)-assisted hydrothermal method. The characterization results of X-ray diffraction (XRD), scanning electron microscopy (SEM), and diffuse reflectance spectroscopy (DRS) showed that the CG-ZFO has a pure crystal phase, and the addition of CTAB can effectively improve the photoelectric performance of the catalyst. The synthesized CG-ZFO can produce a significant synergistic effect with simulated sunlight (SS) and PMS, and the constructed SS/CG-ZFO/PMS system had a good degradation effect on RhB. Based on the conclusions of free radical-quenching experiments, electron paramagnetic resonance (EPR) spectroscopy, and X-ray photoelectron spectroscopy (XPS), the main active species in the SS/CG-ZFO/PMS system was identified as1O2, and the degradation mechanism of RhB was elucidated. CG-ZFO prepared from coal gangue holds promising potential for application in the remediation of organic dye wastewater, and this study also provides a new approach for the resource regeneration of high-iron coal gangue.
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PubMed
高影响因子
MOLECULES
·
2026
·Vol. 31
·期 16
·2884
·
IF 5.1
Yiqiong Yang,Juan Han,Cui Wang,Pingchuan Yang,Panchen Li,Xiaodong Zhang
MOF-derived catalysts have considerable potential for aqueous contaminant control, but their practical application is often constrained by the aggregation and difficult recovery of powder catalysts. In this study, a self-supportingN-doped Fe/Ni-based monolithic catalyst, denoted N-101-NFF, was fabricated through the in situ growth of an Fe-based MOF precursor on nickel–iron foam followed by pyrolysis. Under the conditions of 50 mg/L chlortetracycline (CTC), 0.08 mmol/L peroxymonosulfate (PMS), and an effective catalyst area of 1 cm2, N-101-NFF degraded 90.3% of CTC within 60 min and maintained a degradation efficiency of 88.6% after five consecutive cycles. Quenching experiments and EPR analysis indicated the involvement of •OH, SO4•−, O2•−, and1O2in CTC degradation. Electrochemical measurements indicated improved interfacial charge-transfer characteristics, while post-reaction XPS analysis revealed changes in the Fe and Ni valence states and surface N- and O-containing groups, supporting the involvement of Fe and Ni redox cycling and these surface functionalities in PMS activation. In a fixed-bed reactor, the system maintained more than 86% CTC removal over 24 h of continuous-flow operation at a CTC feed rate of 200 mL/h. These results highlight the potential of N-101-NFF as a recoverable monolithic catalyst for PMS-based treatment of antibiotic-contaminated water.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Hongyang Liu,Tiancheng Gao,Jian Zhang,Xin Cheng,Zheng Xing,Lina Li,Haina Bai
Constructed MOF-in-LDHs to regulate morphology and anchor active sites. • Ternary metal redox cycles coupled with ETP boosted PMS activation. • Ion resistance and cycling stability enable continuous-flow application. Although the development of catalysts with high activity and stability is still a major problem, advanced oxidation processes based on peroxymonosulfate (PMS-AOPs) show promise for the degradation of antibiotics. In this work, FeCu-LDH with an initial fish-scale embroidered spherical morphology was reconstructed during ZIF-67 growth, forming a unique 3D structure with ZIF-67 nanoparticles confined on lamellar substrates. This structure not only provides ideal anchoring sites for ZIF-67 but also alleviates its self-agglomeration and metal ion leaching via spatial confinement. Under optimized conditions, 2 mg of the catalyst achieved 95.12% norfloxacin (NOR) removal within 30 min; positively charged LDHs stabilized negatively charged PMS, while ZIF-67 Co sites triggered the continual production of reactive oxygen species (ROS). DFT calculations showed ZIF-67/FeCu-LDH efficiently activates PMS by enhancing adsorption and interfacial electron transfer. A continuous-flow reactor with this catalyst maintained >90% NOR removal for 8 h, showing good practical potential. Quenching experiments and EPR confirmed SO 4 ·- , ·OH, ·O 2 − and 1 O 2 generation; electrochemical tests verified the participation of type III electron transfer pathway (ETP(III)), with radical-non-radical coupling promoting NOR degradation. Mechanistically, FeCu-LDH lamellar confinement enhances Fe/Cu/Co redox cycles and accelerates electron transfer, supplying sufficient electrons for PMS activation. This study proposes a potential method for designing MOF-in-LDHs composites, providing a reference for the treatment of water contaminated by antibiotics.
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高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2026
·
IF 7.9
Shengnan Chen,Jun Teng,Jing Deng,Dong Xu,Yaqin Wu,Lei Wang,Hong Wang,Mengyuan Xu,Wenxin Shi
Ultrafiltration (UF), as the heart of third-generation drinking water purification, presents immense potential for water treatment. Nonetheless, inevitable membrane fouling stemming from natural organic matter (NOM) impedes widespread UF application. Thus, the vacuum ultraviolet (VUV, 185 + 254 nm) activated peroxymonosulfate (PMS) process was employed as a UF pretreatment, with the conventional ultraviolet (UV, 254 nm)/PMS process used for comparison. Results demonstrated that VUV/PMS achieved higher steady-state concentrations of HO• (9.97 × 10 −14 M) and SO 4 • − (4.95 × 10 −13 M) than UV/PMS (2.32 × 10 −14 and 2.76 × 10 −13 M), leading to more efficient NOM degradation and molecular weight reduction, thereby achieving greater fouling mitigation. Both pretreatments shifted the dominant fouling mechanism from standard blocking and cake filtration to primarily standard blocking. Although VUV/PMS pretreatment yielded superior UF effluent water quality and fewer disinfection by-products (DBPs) than UV/PMS, it resulted in higher DBPs cytotoxicity due to the increased concentration of highly toxic dichloroacetonitrile. Moreover, increasing pretreatment time and PMS dosage in VUV/PMS further improved performance. In real water, VUV/PMS pretreatment outperformed UV/PMS across multiple critical metrics, including organic contaminant decomposition, membrane fouling alleviation, effluent quality improvement, DBPs generation control, and toxicity reduction. Download: Download high-res image (290KB) Download: Download full-size image
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危险品化学品经营许可证（带存储）