MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Zhao Mu,Hao Chen,Xiao Feng,Tengfeng Xie,Dejun Wang,Yanhong Lin
Photocatalytic coupled SO 4 •- based advanced oxidation processes (SR-AOPs) are considered as an advanced wastewater treatment technology for degrading pollutants. In this work, Co-doped g-C 3 N 4 (CCN) photocatalysts were successfully designed for activation of permonosulfate (PMS) under visible light to efficiently degrade tetracycline (TC). The CCN photocatalyst exhibited enhanced degradation efficiency, removing 95.9 % of TC within 20 min, with a much higher degradation rate constant (0.1354 min -1 ) than that of the photocatalytic system (0.0090 min -1 ) and the SR-AOPs system (0.0538 min -1 ). The separation and transport properties of photogenerated carriers were probed with the assistance of measurements including surface photovoltage and photoluminescence. The results showed that the introduction of Co promoted the effective separation of photogenerated charges in CCN, which accelerated the Co 3+/2+ cycle and realized the efficient activation of PMS. Overall, this study provides a new strategy for the development of efficient photocatalytic activation of PMS for rapid degradation of organic pollutants.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
LANGMUIR
·
2026
·
IF 4.4
Pengfei Zhang,Hao Zhang,Xin Yan,Hongji Zhang,Xiangchao Zhang,Chunfang Du
It is crucial to achieve the valid treatment and reuse of solid waste coal gangue (CG). This work extracted Al and Fe elements from solid waste coal gangue (CG) for the synthesis of layered double hydroxides (NiAlFe-LDHs), which were then converted to layered oxides (LDOs) via calcination to activate peroxymonosulfate (PMS) for rhodamine B (RhB) degradation. NiAlFe-LDOs/SiO2 was also synthesized utilizing leached CG (SiO2) as an inorganic support through thermal treatment of NiAlFe-LDH/SiO2 under an air atmosphere. Due to the different structures and physicochemical properties, NiAlFe-LDOs and NiAlFe-LDOs/SiO2 displayed different removal performance toward organic pollutants. LDO-400 exhibited an outstanding RhB degradation efficiency of about 96% within 20 min in the PMS activation system, and it also showed excellent cycling stability with about 82% degradation efficiency after the eighth cycle. The toxicity of RhB and its degradation intermediates was simulated via ECOSAR software to evaluate the environmental safety of the degradation process. For practical application, LDO@sodium alginate (SA) gel beads were synthesized and employed in a fixed-bed reactor, which maintained a degradation efficiency exceeding 90% after 96 h of continuous operation. Other than the excellent RhB degradation efficiency of LDO-400, LDO/SiO2-400 showed a more remarkable adsorption efficiency of 95% toward tetracycline hydrochloride (TC, 50 mg·L–1) within 40 min compared with LDO-400 (54%) and SiO2 (7%). This work not only provides an effective strategy for aquatic pollutant removal but also realizes the comprehensive utilization of CG as an inorganic non-metallic raw material.
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PubMed
高影响因子
ADVANCED POWDER TECHNOLOGY
·
2026
·Vol. 37
·期 7
·105314
·
IF 4.5
Lin Li,Kaiyun Yang,Zhan Ding,Chang Liu
Spodumene is often associated with albite, and their similar physicochemical properties render conventional collectors ineffective for achieving selective flotation separation. This study introduces a Fe 2+ /PMS Fenton-like system to selectively enhance the adsorption of NaOL onto the spodumene surface, thereby enlarging the floatability difference between the two minerals and enabling their separation. Single-mineral flotation tests demonstrated that under optimal conditions (pH 9, NaOL dosage 8 × 10 -4 mol/L, and Fe 2+ /PMS dosage 2 × 10 -4 mol/L with a Fe 2+ :PMS molar ratio of 1:3), the recoveries of spodumene and albite were 92.37% and 8.64%, respectively. Flotation experiments on an artificial mixed mineral (spodumene:albite = 1:3) yielded a spodumene concentrate with a Li 2 O grade of 6.73% and a recovery of 88.17%. The separation mechanism was elucidated through contact angle measurements, atomic force microscopy (AFM), zeta potential analysis, electron paramagnetic resonance (EPR), and X-ray photoelectron spectroscopy (XPS). The results indicate that the Fe 2+ /PMS system selectively generates reactive oxygen species (SO 4 • − and •OH) on the spodumene surface. These species oxidize Fe 2+ to Fe 3+ , leading to the adsorption of more Fe 3+ species on spodumene which subsequently act as active sites for oleate anion adsorption. In contrast, the system exhibited a comparatively minor effect on the albite surface. This work provides a novel reagent approach and a theoretical foundation for the flotation separation of spodumene from albite.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
·
IF 12.2
Zhou Yang,Feng Yuqing,Wen Rui,Huang Qiping,Guo Qin,Lu Xixin,Han Bin,Xie Haijiao,Ma Jinxing,Jiang Jin,Ma Jun,Gao Yuan
Balancing degradation efficiency with environmental sustainability
remains a critical challenge for permanganate (Mn(VII))-based oxidation
processes in environmental remediation. In this study, we report a
novel system initiated by low-dose Mn(VII) dosage (2 μM) in
combination with peroxymonosulfate (PMS), enabling efficient removal
of emerging contaminants exemplified by bisphenol A (BPA), especially
under alkaline conditions (e.g., pH 10). Notably, distinct from conventional
radical or nonradical activation mechanisms, we identified a previously
unrecognized Mn(VII) regeneration process in the Mn(VII)/PMS system,
as supported by a series of complementary evidence from radical quenching
experiments, stopped-flow spectroscopy, DFT calculations, and kinetic
modeling. The in situ generated Mn(VI) from the reaction of Mn(VII)
and BPA was demonstrated to act as the key intermediate, which was
subsequently reoxidized by PMS via a multihydrogen-bonded complex
back to Mn(VII). This Mn(VI)/Mn(VII) interconversion, reported here
for the first time, not only effectively enhanced contaminant degradation
but also significantly improved Mn(VII) utilization efficiency. These
findings broaden the mechanistic understanding of Mn(VII)-based systems
beyond traditional free radical- and Mn(III)/Mn(V)-driven pathways
and open new insights for developing efficient and environmentally
benign water treatment technologies.
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PubMed
高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Jing Zhang,Zhi Song,Boxia Liu,Dongxu Han,Xiayan Zhang,Jialu Liu,Yeqiong Huang,Chuhan Xing
Prussian blue analogues (PBAs) show potential in pollutant degradation, but are often limited by crystal structure regulation and insufficient exposure of active sites. In this study, Bi doping was used to synergistically optimize the crystal structure and electronic environment of CuFe-PBA and construct an efficient CuFe-Bi-3 catalyst for peroxymonosulfate (PMS) activated degradation of tetracycline (TC). The introduction of Bi induces crystal plane reconstruction, enhances the Cu 2+ /Cu + and Fe 3+ /Fe 2+ cycles, and increases the exposure of active sites. The TC degradation rate of CuFe-Bi-3 increased from 72.2 % to 92.1 % within 80 min, and the reaction rate constant increased from 0.01133 to 0.02631 min −1 . Mechanistic studies have shown that Bi regulation promotes the directional generation and utilization of 1 O 2 , constructing a synergistic oxidation pathway dominated by non-free radicals. A comprehensive comparison of EPR signals for various reactive oxygen species showed that the 1 O 2 signal was the strongest, significantly higher than O 2 •- , •OH and SO 4 •- . The system has good stability in various water qualities and a wide pH range, and toxicity assessment also shows that it can effectively reduce the toxicity of degradation products. This study provides theoretical support and application reference for the structure-electronic regulation of PBAs catalysts and Bi doping to construct an environmentally friendly and efficient PMS activation system in a complex water environment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Guanhan Chen,Hongjie Wang,Wenyi Dong,Wenhui Ding,Feifei Wang,Zilong Zhao,Yuxiong Huang
Cobalt oxide (Co 3 O 4 ) activated peroxymonosulfate (PMS) system was extensively studied due to its excellent catalytic performance. However, the relatively high cobalt (Co 2+ ) leaching (up to 2 mg/L) would pose high ecotoxicological risks. Herein, we identified the existence of Co(OH) 2 on the surface of Co 3 O 4 were the major source of Co 2+ leaching in the Co 3 O 4 activated PMS system. Furthermore, the Co 2+ leaching was effectively suppressed by converting Co(OH) 2 to Co 3 O 4 via pyrolysis treatment. In addition, reduced graphene oxide (rGO) was engaged to enhance the degradation performance of antibiotics in the Co 3 O 4 activated PMS system. The oxygen functionalities of rGO would catalyze PMS to generate sulfate radicals (SO 4 − ) and trigger the non-radical pathway of singlet oxygen ( 1 O 2 ). We have achieved outstanding catalytic performance for carbamazepine (CAZ) degradation with low Co 2+ leaching, as CAZ (5 mg/L) could be completely degraded in 30 min. Combining experimental investigation and theoretical calculation, we also revealed the degradation pathways and mechanisms that CAZ would be oxidized and detoxified by 1 O 2 and SO 4 − . We have provided a simple approach to inhibit the Co 2+ leaching and enhance the catalytic performance of Co 3 O 4 activated PMS system for the effective control of antibiotics.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Dong Guo,Yongqiang Wang,Chen Chen,Jiaqi He,Meilin Zhu,Jie Chen,Conglu Zhang
The synthesis of Vis-light driven catalysts with high photocatalytic performance and efficient activation of persulfate requires new strategies. Herein, a multistage structural tuning graphitic carbon nitride co-modified by Co, S (pg-C 3 N 4 /Co 3 O 4 /CoS) was synthesized for the first time through in-situ template method and microwave sulfurization treatment. A photocatalysis-PMS oxidation coupling system was also proposed. The results showed that the introduction of cobalt could improve the photocatalysis and PMS activation efficiency of the graphitic carbon nitride. Further sulfurization treatment could generate more active sites for PMS activation and increase the interlayer distance of carbon nitride to broaden the absorption range of Vis-light. Density functional theory (DFT) calculations indicated the migration of electrons from carbon nitride to CoS promoted the recycling of Co 3+ /Co 2+ . In the coupling system, BPF 50 mL (30 mg L -1 ) was degraded by 99% in 10 min with 0.1 g L -1 catalyst and 0.32 mmol L -1 PMS. The degradation rate was 4 times faster than that of pure PMS system under visible light. Notably, BPF was effectively mineralized and TOC removal rate reached 90%. The stability and recycling experiments showed that pg-C 3 N 4 /Co 3 O 4 /CoS maintained high catalytic performance under complex matrix and multiple cycles, and could be quickly separated and recovered due to the magnetic Co 3 O 4 . This work will provide a new strategy for the development of multi performance catalytic materials, and the proposed photocatalysis-PMS coupling system has huge potential for the wastewater treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yuan Zhang,Kangping Cui,Xueyan Liu,Minshu Cui,Xing Chen,Yuchao Tang,Haiyang Li
Metal-based catalyst could be used for efficient peroxymonosulfate (PMS) activation, but inevitably suffered from metal ion leaching. Metal-free graphitic carbon nitride (g-C 3 N 4 ) materials that can activate PMS are more conducive for practical water treatment. In this study, g-C 3 N 4 with both N-defects and P-doping (CN-NP) was synthesized, which mainly produce singlet oxygen ( 1 O 2 ), and 97 % of 4-CP (4-Chlorophenol) was removed by CN-NP/PMS/Vis reaction system within 60 min. The active species was identified by quenching experiments and electron spin resonance (ESR) tests, and the origin of mainly active species was further verified by the concentration change of PMS during the reaction. It was verified by experiments and theoretical calculations that the introduction of N-defects led to the separation of photoinduced electron-hole pairs and improved photocatalytic activity. Notably, density functional theory (DFT) revealed that both N-defects and P-doping are electron-deficient sites, and P-doping acts as the main PMS adsorption site to promote the loss of electrons from PMS to generate 1 O 2 . In addition, the catalysts developed in this research were anticipated to be applied in real wastewater treatment, contributing to further comprehend the mechanisms of element doping and defect modification in g-C 3 N 4 activating PMS, and providing new insights for the design of PMS-activating catalysts.
研究领域:
环境科学
·
材料科学
·
催化
·
水处理
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yiyang Ma,Hongjie Wang,Xiaofan Lv,Dongbin Xiong,Haijiao Xie,Zhenghua Zhang
Peroxymonosulfate (PMS)-induced advanced oxidation processes hold great promise for the in-depth treatment of many challenging pollutants. Herein, three-dimensional ordered mesoporous Co 3 O 4 (3D OM-Co 3 O 4 ) was synthesized with a KIT-6 template to boost PMS activation for the rapid removal of a target pollutant of ranitidine (RAN). At the optimal conditions, 3D OM-Co 3 O 4 achieved the RAN removal efficiency of 99.2% and the RAN mineralization efficiency of 63.7% within 7 min. PMS activation by 3D OM-Co 3 O 4 involved simultaneous non-radical and radical pathways, with the latter accounting for 73.2% of the total RAN removal efficiency. Density functional theory calculations demonstrated that compared with Co 3 O 4 nanoparticles, the adsorption energy of PMS molecules bonded to 3D OM-Co 3 O 4 was increased from −0.213 eV to −0.297 eV due to its ordered mesoporous structure. The regeneration of 3D OM-Co 3 O 4 by a reduction treatment indicated that its catalytic stability was associated with rapid charge transfer between the Co(III)/Co(II) redox couple. The possible degradation pathways revealed the oxidation behavior of RAN in the 3D OM-Co 3 O 4 /PMS heterogeneous system. This study provides a new perspective for the mechanism of PMS-induced heterogeneous catalytic oxidation and a novel method for enhancing the synergistic effect between Co 3 O 4 nanoparticles.
研究领域:
环境科学
·
催化
·
水处理
·
材料科学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Dongdong Fan,Meihua Hu,Songyuan Li,Pinghua Chen,Hualin Jiang,Xinman Tu,Xibao Li,Xubiao Luo
The efficient activation of peroxymonosulfate for degrading emerging contaminants has become a focal point in recent decades, emphasizing the development of novel materials and efficient strategies for high-performance degradation. This study explores a spatial confinement strategy, where TiO 2 is confined inside carbon nanotubes with Co 3 O 4 loading outside, is performed to prepare the nano-confined composite TiO 2 -in-CNT/Co 3 O 4 . Norfloxacin is chosen as the primary target pollutant, revealing a degradation rate exceeding 97 % within 30 min. The non-radical 1 O 2 species were confirmed to be generated in nano-confined catalyst, but not observed in the control non-confined catalyst. Additionally, the quantity of original radical active species significantly increases in nano-confined catalyst compared to non-confined catalyst. TiO 2 -in-CNT/Co 3 O 4 has excellent reusability and application universality. Wonderful stability is observed in real water and anti-ion interference experiments, highlighting its robust stability. Experimental and DFT calculation results also demonstrate that the spatial confinement strategy prevents nanoparticle aggregation, accelerates electron transfer efficiency, and promotes the cycling of Co 2+ /Co 3+ electron pairs. This work provides insights into the regulation of confined effects in activating PMS and offers a feasible strategy for the synergistic activation of PMS for water environment remediation through a radical and non-radical mixed mechanism.
研究领域:
环境科学
·
材料科学
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Yi Duan,Miaobin Ye,Ye Zou,Haiyan Jiang,Shuai Zhou,Pingli Cai
In this work, cobalt-doped graphitic carbon nitride (Co-CN) was synthesized through a high-temperature calcination method and employed to activate peroxymonosulfate (PMS) for ciprofloxacin (CIP) removal. The experimental outcomes demonstrated that under optimized conditions of 0.5 g/L 0.25Co-CN, 2 mM PMS, an initial solution pH of 7, an initial CIP concentration of 5 mg/L, and at a temperature of 30 °C, the removal efficiency of CIP can reach 99.5 % within 45 min. The kinetics of CIP removal by Co-CN activated PMS are accurately modeled by a bi-exponential decay function, indicating a CIP removal process involving both rapid and slower reaction phases. Furthermore, after five cycles of reuse, the catalyst maintained a respectable removal efficiency of 83.3 % for CIP, with pre- and post-reaction characterizations affirming the excellent reusability and stability of 0.25Co-CN. Quenching experiments and Electron Paramagnetic Resonance (EPR) tests confirmed the predominance role of 1 O 2 in the catalytic degradation mechanism. The Co N 4 active sites within 0.25Co-CN were identified as crucial for adsorption and subsequent degradation of CIP. In this study, a novel kinetics model is proposed for fitting the CIP removal process under the synergistic effect of adsorption and catalysis, which provides new insights into the understanding of the dynamic process of organic pollutant removal.
研究领域:
环境科学
·
催化化学
·
污染控制
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiangdong Zhang,Jian Zhang,Bowen Hou,Xueying Yang,Junlian Ren,Chen Shao
Selective removal of organic pollutants by PMS-activated heterogeneous catalytic system has become one of the commonly used methods, but the adsorption of the catalyst is often ignored in the degradation process. Metal-organic frameworks (MOFs) are often used in the field of environment because of their high porosity and structural diversity/adjustability. However, there are still difficulties in the aggregation and recycling of nanoparticles . This study effectively synthesized the material CuS-PVP@ZIF-67 by using hollow spherical CuS as the carrier of Co-MOF (ZIF-67) to solve these problems. A high concentration of oxytetracycline hydrochloride (OTC) can be successfully adsorbed by electrostatic attraction and π-π interaction, and small amount of PMS may be quickly activated, and the removal rate of OTC is 94.82 % in 20 min. The catalyst used can be easily recovered by suction filtration and has good reusability. In addition, a potential cooperating mechanism for adsorption-PMS activation has additionally been proposed. The degradation pathway of OTC is determined, and the potential harm of intermediate products is analyzed. This work aims to create a heterogeneous catalytic system with significant adsorption and catalytic ability to remove refractory organic contaminants in water.
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高影响因子
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