Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Siyuan Diao,Lili Meng,Lanlan Feng
The application of peroxymonosulfate (PMS)-based advanced oxidation processes , facilitated by the incorporation of metal-deposited MoS 2 catalyst, has attracted considerable interest in recent years within the scientific community. Nevertheless, investigating the structure-performance relationship between MoS 2 and deposited metal still presents a formidable challenge, yet a highly desirable pursuit. In this study, a Cu-MoS 2 single-atom catalyst (SAC) was successfully synthesized by a photo-deposition method, wherein Cu ions were deposited on the MoS 2 surface. The Cu-MoS 2 /PMS system exhibits exceptional degradation performance for tetracycline (TC), with a removal efficiency reaching 96% at 60 min. Furthermore, the density functional theory (DFT) is applied to investigate the coordination microenvironment of the catalyst by depositing of Cu. Experimental and theoretical calculations results exhibit that, on one hand, the introduction of Cu decreases the adsorption energy barrier and enhances the adsorption capacity of the catalyst for PMS. On the other hand, the abundant presence of Cu on the surface of the MoS 2 facilitates an accelerated transfer of electron , availing the formation of reactive oxygen species (ROS) via the distinct pathway: MoS 2 → transition metal → PMS. Concurrently, the synergistic interaction between Mo and Cu expedites rapid valence evolution of Mo 4+ /Mo 5+ /Mo 6+ and Cu + /Cu 2+ , thereby further enhancing the PMS activation. Hence, adjusting the coordination microenvironment of the catalyst represents a promising strategy for enhancing the catalytic activity.
研究领域:
环境科学
·
催化材料
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Ruyao Chen,Haiyue Zhang,Yuming Dong,Haifeng Shi
In the metal-based peroxymonosulfate (PMS) activation process, the sluggish surface redox cycle of metal ions generally hampered the efficiency of PMS activation for pollutant removal. Herein, Co-doped CuWO 4 /BN quantum dots (CW/Co/BNQDs) photocatalysts were developed to realize Cu 2+ /Cu + and Co 2+ /Co 3+ dual ions redox cycles for PMS activation, which would facilitate the tetracycline (TC) removal. CW/4Co/2BNQDs could degrade 94.8% TC within 30 min in PMS/Vis system, and the apparent rate constant of CW/4Co/2BNQDs was 2.7 times and 1.2 times higher than those of CW and CW/4Co, respectively. The improved TC degradation performance could be attributed to the synergetic effect between BNQDs and dual redox cycles. X-ray photoelectron spectroscopy (XPS) spectra of samples before and after the reaction demonstrated that BNQDs were beneficial for accelerating the Cu 2+ /Cu + and Co 2+ /Co 3+ redox cycles in CW/4Co/2BNQDs, further boosting the activation of PMS in TC degradation. Experiments of different radical scavengers revealed that the SO 4 ·− /·OH/h + / 1 O 2 reactive species participated in the PMS activation for the TC degradation process. The possible TC degradation pathway and intermediate toxicity were detailed investigated. In addition, CW/4Co/2BNQDs exhibited outstanding photocatalytic activity over five consecutive cycles, which illustrated that it was supposed to be a reliable PMS activator over antibiotic elimination for practical application. And this work shed new light on constructing dual redox cycles for efficient PMS activation.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Fu Xingyu,Chang Shufang,Sun Xiaoqin
Photocatalysis-peroxymonosulfate (PMS) activation system is regarded as a promising strategy for antibiotic degradation. Herein, a type-II SnS 2 /NiFe LDH heterojunction assembled by nanosheets was constructed to realize the dual modulation of photogenerated carrier directional migration and PMS activation sites. The intimate and large coupled interface facilitated the charge separation and transfer. And the optimization of the electronic structure in the heterojunction enabled good visible light absorption capacity. Benefiting from the construction of type-II heterojunction, the Fe 2+ /Fe 3+ and Ni 2+ /Ni 3+ redox cycles in SnS 2 /NiFe LDH had been greatly improved, which further promoted the PMS activation. The constructed heterojunction achieved excellent metronidazole (MNZ) degradation performance (93.9% removal within 30 min) via PMS activation-assisted photocatalysis under visible light irradiation, which was greatly enhanced compared to the control conditions of photocatalysis without PMS (3.5%) or without light irradiation (78.1%). It also demonstrated excellent stability and functioned well across a wide pH range (3–11). The quenching experiments revealed that ·OH and h + were the main reactive species for MNZ oxidation. The mechanism analysis further confirmed that the transfer of photogenerated carriers was consistent with the type-II mode. This study is expected to provide new insights into design and application of type-II heterojunction in PMS activation for efficient wastewater treatment. Graphical abstract
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ke Li,Yibing Sun,Jiawei Zhou,Xinyue Zhang,Hongchao Li,Zhichao Yang
The combination of transition metal oxides with carbon-based materials is a promising strategy for constructing efficient catalysts for peroxymonosulfate (PMS) activation to degrade aqueous organic contaminants. However, the complex heterostructure of the composites often hinders the identification of the actual reactive species responsible for pollutant degradation. In this study, we integrate Mn 3 O 4 into N-doped graphite (NG) to elucidate the mechanisms involved in the Mn-NG composite mediated PMS activation process. The Mn-NG/PMS system shows excellent performance in oxidizing bisphenol A (BPA) over a wide pH range (3.4 to 9.4) and in the presence of co-existing substrates. Mn sites in Mn 3 O 4 are responsible for the activation of PMS, and the NG matrix enhances the dispersion of Mn in the Mn-NG composite. Multiple experimental results indicate that free radicals (i.e., hydroxyl radicals (HO • ) and sulfate radicals (SO 4 •− )) are not generated, and surface reactive Mn(IV) is proposed as the primary reactive species for BPA oxidation. This study provides new insights into understanding the role of Mn oxides in carbon-based composites in PMS activation for degradation of organic pollutants.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Bing Zhang,Bo Wang,Heli Tang,Qingjie Li,Wenxin Shi
In this study, an innovative ferric tetrasulfide/peroxymonosulfate (Fe 3 S 4 /PMS) pre-oxidation system was integrated into an aerobic granular membrane bioreactor (AGMBR) to alleviate membrane fouling. The role and underlying mechanisms associated with solution pH was also investigated. The results demonstrated that under optimal conditions (pH 6.0, 0.2 g/L Fe 3 S 4 , and 2.0 mM PMS), pre-oxidation treatment significantly reduced the total membrane fouling resistance by 98 % and shifted the fouling mechanism from cake layer fouling to pore blocking fouling. Moreover, pre-oxidation treatment at pH 6.0 enhanced the energy barrier between foulants-membrane and foulants-foulants, thereby alleviating membrane fouling. The key reactive oxygen species were identified as •OH, SO 4 • – , and 1 O 2 with contributions of 7.03 %, 46.62 %, and 22.38 %, respectively. Furthermore, phosphates significantly inhibited the performance of Fe 3 S 4 /PMS oxidation system for mitigating membrane fouling; however, decreasing solution pH alleviated this inhibition effect. Additionally, an inhibiting effect on coating metal oxide or hydroxide on catalyst surface was observed along with variation in surface charge properties of Fe 3 S 4 when pH was decreased to 6.0, which further promoted activation of PMS for mitigating membrane fouling. This study provides a robust theoretical foundation for employing Fe 3 S 4 /PMS pre-oxidation in AGMBR to alleviate membrane fouling issues which represents an important engineering advancement.
研究领域:
环境工程
·
水处理技术
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Weijie Hua,Yong Kang,Huixin Yuan
The effective and rapid treatment of emerging pollutants in water is an essential solution to the pollution of water environment. The emerging pollutant-malachite green (MG) wastewater was treated using pulsed discharge plasma on water surface system (WSP) combining Fe 2+ /PMS. Compared with WSP alone, the addition of 125 μM Fe 2+ and 0.5 mM peroxymonosulfate (PMS) in WSP could enhance the degradation efficiency and energy efficiency of MG by 32.8% and 9.7% respectively, with the synergistic factor of up to 2.056. UV–Vis absorption spectra and mineralization further demonstrated the synergistic effect. When the peak voltage and air flow rate were 22 kV and 0.7 L/min, the degradation efficiency and kinetic constant of MG could reach 97.9% and 0.259 min −1 , respectively. MG degradation with high conductivity (1000 μS/cm) by WSP + Fe 2+ /PMS not only exhibited the better purification effect, but also could maintain the faster reaction rate. The active species involved in the degradation of MG in WSP + Fe 2+ /PMS system were mainly ·OH, SO 4 · − , O 2 · − and e* − . Furthermore, H 2 O 2 and O 3 also have a certain oxidizing effect on MG. Cl − , SO 4 2− , HCO 3 − and humic acid (HA) could inhibit MG degradation to some extent, but still removed more than 80% of MG in water. The WSP + Fe 2+ /PMS reaction system was suitable for the treatment of other emerging pollutants in water. The results of LC-MS analysis revealed that the N-demethylation reaction and decomposition of conjugated structure were the important pathways for MG degradation. The H 2 O 2 and acidic liquid environment provided by WSP laid the foundation for the formation of Fenton, and the introduced Fe 2+ could fully undergo the Fenton and activation reaction with H 2 O 2 and a small amount of PMS in the liquid phase, which enhanced the generation of active species, especially · OH.
研究领域:
环境科学
·
水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jiajun Liu,Xionghao Zhang,Junda Li,Yi Feng,Li Feng,Shuai Han,Tingyu Pan,Taiheng Zhang,Shenyu Wu,Zijie Ke,Bingzhi Liu,Huaili Zheng
In this study, an advanced oxidation process with E/Ce(IV) synergistic PMS (E/Ce(IV)/PMS) was established for the efficient removal of Reactive Blue 19 (RB19). The catalytic oxidation performance of different coupling systems was examined and the synergistic effect of E/Ce(IV) with PMS in the system was substantiated. The oxidative removal of RB19 in E/Ce(IV)/PMS was excellent, achieving a removal efficiency of 94.47% and a reasonable power consumption (EE/O value was 3.27 kWh·m −3 ). The effect of pH, current density, Ce(IV) concentration, PMS concentration, initial RB19 concentration and water matrix on the removal efficiency of RB19 were explored. Additionally, quenching and EPR experiments showed that the solution contains different radicals such as SO 4 ·− , HO∙ and 1 O 2 , where 1 O 2 and SO 4 ·− played key roles, but HO∙ just acted a weaker role. Ce ion trapping experiment confirmed that Ce(IV) was involved in the reaction process and played a major role (29.91%). RB19 was subject to three possible degradation pathways, and the intermediate products displayed well biochemical properties. To conclude, the degradation mechanism of RB19 was explored and discussed. In the presence of current, E/Ce(IV)/PMS performed a rapid Ce(IV)/Ce(III) cycle, continuously generating strong catalytic oxidation Ce(IV), The reactive radicals derived from the decomposition of PMS, in conjunction with Ce(IV) and direct electro-oxidation, efficiently destroyed the molecular structure of RB19 and showed an efficient removal rate.
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
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ying Yang,Hua Li,Yilong Hou,Ce Wang,Kangyi Zhang,Zhihao Man,Jiangwei Shang,Xiuwen Cheng
Antibiotics that permeate aquatic environments present significant risks to both ecosystems and human health. In this study, we employed the techniques of room temperature aqueous solution precipitation to fabricate ZIF-67 derivatives, and established a Co 3 O 4 /CeO 2 /O 3 /PMS (Co-Ce/OP) system. Furthermore, a 10 mg/L Levofloxacin (LEF) solution could reach rapid degradation (97.2%) and effective mineralization (40.4%) under specific conditions. Subsequent investigations identified the primary active substances, intermediates, and reaction mechanism in the Co-Ce/OP system. Evidence from Electron Paramagnetic Resonance (EPR) and quenching experiments indicates that SO 4 · - , OH·, O 2 · - and 1 O 2 contribute to the degradation process. Applying High Performance Liquid Chromatography-Mass Spectrometry (HPLC-MS), we discovered that the principal degradation mechanisms for LEF encompass the cleavage and subsequent loss of the piperazine, quinolone, and morpholine rings, in addition to decarboxylation and defluorination reactions. Besides, we studied the acute toxicity, bioconcentration factor, developmental toxicity, and mutagenicity of LEF and its intermediate products. Our findings reveal a notable reduction in the toxicity of the intermediate products relative to LEF. Later experiment demonstrates that the degradation rate of LEF sustains above 90% after five cycles of reactions, indicative that the catalyst has excellent recyclability and stability. Furthermore, this study employed experiments across four different natural water matrices, demonstrating the system's considerable potential for effective application within authentic aquatic settings.
研究领域:
环境科学
·
材料科学
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yinan Chen,Qi Peng,Chengwen Song,Yuanlu Xu,Zaijin You,Xinfei Fan
Despite the membrane technology as an efficient method for treating emulsified oily wastewater, the issue of membrane fouling remains an enormous challenge during extended operation. Hence, a unique self-assembled method was proposed to clean membrane fouling for oil/water (O/W) separation, where the tannic acid/iron (TA/Fe) coating layer improved hydrophilicity and doped with iron nanoparticles to activate peroxymonosulfate (PMS) for removing of the irreversible oil fouling. The TA/Fe coating, which contained phenolic hydroxyl groups, rendered the modified membrane superhydrophilic and underwater oleophobic properties to resist membrane surface oil droplets. The iron nanoparticles/TA/polyvinylidene fluoride (FeNPs/TA/PVDF) achieved notable permeation flux of 1571.13 L m −2 h −1 and 1490 L m −2 h −1 in O/W mixture and oil-in-water emulsion (liquid paraffin as oil phase), respectively. Meanwhile, the membrane exhibited a distinguished oil removal rate, surpassing 98 % for various emulsions (e.g. N-hexane, isooctane, soybean oil). Notably, in the pollution and cyclic experiments, the regeneration water flux of FeNPs/TA/PVDF increased from 71.7 % of pristine PVDF to 91.5 % after final modification, which proved the enhancement of the membrane anti-oil-fouling capability through the deposition of the hydrophilic coating. Moreover, after catalytic cleaning, the water permeation flux of FeNPs/TA/PVDF could reach approximately 90 % of its original value. Obviously, we observed that FeNPs/TA/PVDF exhibited a high regenerative capacity during the PMS-assisted catalytic cleaning process, where the radical and nonradical pathways coexisted. Generally, the research offered a simple approach to creating functional membranes suitable for efficient O/W separation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2025
·Vol. 36
·期 19
·195602
·
IF 2.8
Qing Sun,Jiao Yan,Jiale Yu,Xiaofang Hu,Jian Zhang,Jiawei Sheng
In this study, the core-shell nanostructure of magnesium reinforced cobalt silicate@13X was synthesized by a two-step reaction using zeolite 13X as the initial silicate material and carrier, and the organic pollutant metronidazole was degraded by activating PMS. It was found that 6CoMg-13X had excellent and stable catalytic performance on PMS activation, with a degradation rate of 99.7% in 5 min and a removal rate of more than 99.4% after 5 cycles. Under hydrothermal conditions, 13X gradually dissolved into silicate anion under the action of urea, while Co2+ and Mg2+ reacted on 13X surface to form ultra-thin core-shell nanostructures. The calcination process further improves the stability of the catalyst while reducing cobalt leaching, after calcination, cobalt leaching is only 0.16 mg l−1. In addition, the catalyst had high degradation rates for norfloxacin (NFA), 5-fluorouracil (FLU), tetracycline (TC) and Rhodamine B (RhB), which were 90.29%, 97.36%, 96.24% and 99.69%, respectively. EPR and quenching experiments indicated that SO4‧− and 1O2 are the main active substances in the 6CoMg-13X-PMS system, and ‧OH and ‧O2− also play a certain role in the degradation system. This research provides a feasible solution for developing high performance cobalt-based environmental purification catalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Junmei Luo,Shufeng Bo,Qingda An,Zuoyi Xiao,Haisong Wang,Weijie Cai,Shangru Zhai,Zhongcheng Li
Rational design of ordered catalytic composites with high performance and facile preparation method for environmental remediation still remains a tremendous challenge. For this vision, ordered composites with confined cobalt intercalated N/C layers (Co–N/C) were successfully prepared via carbonizing a mixture of cobalt species, histidine (His) and zirconium-containing SBA-15 (ZS) utilizing a simple non-solvent method. Taking the confinement effect and inherent hydrophilic groups (Si–OH) of mesoporous silica as the foothold, the strong Co 2+ /N or Co 2+ /O coordination (Co 2+ (–COO - or –NH 2 ) 2 and Co 2+ (–O - ) 2 ) and silica/His or His/His adhesive/cohesive interactions endowed the Co-based catalyst with optimal interfacial properties , cycling stability and magnetic separability for degradation of several pollutants (phenol, antibiotics and dyes). The degradation efficiency of Co@NC-ZS-700 for bisphenol A was superior to Co-ZS-700, NC-ZS-700 and Co@NC-SBA-700 due to the flaky structure with confined Co–N/C layers, which could achieve 95.0% within 20 min. In addition, the catalyst could still degrade more than 84.4% bisphenol A after five consecutive reactions. Based on the characterization analysis, tested active species (SO 4 •– , • OH and 1 O 2 ) and degradation products, double-process activation mechanism and degradation pathways were plausibly proposed (radical and non-radical processes). Additionally, various influencing factors, including carbonization temperature, amount of cobalt species, peroxymonosulfate (PMS)/catalyst dosage, pH value, coexisting ions and real water environment, were also systematically studied. This work might pave a feasible way for contaminant treatment utilizing ordered mesoporous silica composites with diffusion promoted channels involved under aqueous systems.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Shuo Wang,Xingrong Li,Hongyao Zhao,Zichen Ma,Danhong Shang,Linzhi Zhai,Xiang Liu,Feng Zeng,Jianming Pan,Yanyun Wang,Fu Yang
Multiphase catalysts with heterointerfaces have shown compelling potential in catalyzing oxidative mineralization of pollutants. In particular, the interfacial electron communication of heterointerfaces is beneficial for activation of reactant molecules through promotive interfacial electron transfer efficiency. In this study, a MnO 2 /CoMn 2 O 4 heterojunction catalyst was constructed for the electron-rich Co centers and abundant redox pairs. Benefiting from the synergistic interaction between cobalt (Co 2+ /Co 3+ ) and manganese (Mn 2+ /Mn 3+ /Mn 4+ ) at the active sites, as well as the electron density difference between the interfaces of the two phases, a significant enhancement of the catalytic activity for peroxymonosulfate (PMS) activation was achieved. Systematic characterization analysis revealed that the catalyst has highly active catalytic sites characterized by electron-rich Co 2+ , and the electron-donating property of the high-electron-density Co 2+ active sites in the A site of spinel CoMn 2 O 4 promotes the efficient transfer of electrons and the rapid generation of reactive oxygen species (ROS) from PMS activation. More exposed catalytic active sites and significantly lower interfacial mass transfer resistance further enhanced the activation performance of the catalysts for bisphenol A degradation by these ROS. The optimal MnO 2 /CoMn 2 O 4 –5 exhibited a optimal BPA degradation activity (86 %, k obs = 0.316 min -1 ) and excellent resistance to anionic interference. The results of free radical quenching experiments indicated that single linear oxygen ( 1 O 2 ) and hydroxyl radical (·OH) were the main active substances for PMS activation and BPA degradation. This study provides meaningful insights into the improvement of heterojunction interfacial systems for catalytic efficiency enhancement and environmental remediation.
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
危险品化学品经营许可证（带存储）