SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Shizong Wang,Jun Hu,Jianlong Wang
In this study cobalt sulfides (Co 9 S 8 ) coated on the nitrogen and sulfur co-doped graphene (Co 9 S 8 @S-N-RG) was firstly prepared and used for degradation of antibiotic sulfamethoxazole (SMX). The results showed that SMX could be completely degraded by Co 9 S 8 @S-N-RG-activated peroxymonosulfate (PMS) within 20 min with its mineralization efficiency of 38.7%. The SMX degradation rate followed pseudo first-order kinetics with kinetic constant of 0.377 min −1 that was higher than that induced by Co 9 S 8 , N-RG, S-N-RG and Co 9 S 8 @S-RG, indicating Co 9 S 8 @S-N-RG had superior catalytic activity . Co 9 S 8 @S-N-RG can activate PMS to produce sulfate radicals and hydroxyl radicals , while sulfate radicals played major role. Co 9 S 8 participated in PMS activation in which Co 2+ was involved in sulfate radicals formation, while sulfur species facilitated the conversion of Co 3+ to Co 2+ . In addition, carbon defects, C O, pyridinic N and pyrrolic N also contributed to PMS activation.The superior catalytic activity was attributed to the synergistic effect of Co 9 S 8 and S-N-RG. This study could provide an efficient and stable PMS activator, and insight into the PMS activation mechanism by Co 9 S 8 @S-N-RG.
研究领域:
环境科学
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化学工程
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材料科学
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2022
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IF 8.943
Xinyu Liu,Jianlong Wang
The selective oxidation of ammonia to dinitrogen gas in some special wastewater is of paramount significance, but still a challenge. In this study, chlorine radical (Cl•)-mediated oxidation process was developed to realize the selective oxidation of NH 4 + -N to N 2 , in which Cl• was generated in Co 2+ /peroxymonosulfate (PMS)/chloridion (Cl − ) system. The effect of various operational parameters on the efficiency and selectivity of ammonia oxidation to N 2 was investigated, such as PMS concentration, Co 2+ concentration, Cl − concentration and pH value. The experiment results showed that Cl•-mediated NH 4 + -N oxidation reaction exhibited high NH 4 + -N removal efficiency and considerable selectivity to N 2 in the range of pH from 2.0 to 6.5. The removal efficiency of NH 4 + -N was 90.39%, and the selectivity of NH 4 + -N to N 2 achieved up to 97.16%. The possible mechanism for high efficient and selective oxidation of NH 4 + -N to N 2 was tentatively proposed. The process developed in this study could provide a novel technology for the treatment and selective oxidation of ammonium in some special types of ammonium-containing wastewater.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Bingxuan Ji,Muhammad Bilal Asif,Zhenghua Zhang
Membrane distillation (MD) has demonstrated its efficacy for seawater desalination, which prompted researchers to investigate its performance for the treatment of surface water containing natural organic matter (NOM). However, membrane fouling remains a significant technological constraint in the acceptability and implementation of MD modules. Herein, for the first time, a photothermally-activated PMS pre-treatment process is coupled to a direct contact (DC)-MD module for effective membrane fouling control. Photothermally-activated PMS (2 mM) pre-treatment achieved 69 % of UV 254 removal and 30.9 % of dissolved organic carbon removal and allowed stable operation of the DCMD without any reduction in water permeance vs 50 % reduction obtained without the pretreatment step. The analysis of NOM fractions after pre-treatment using Parallel Factor Analysis and molecular weight distribution indicated changes in NOM composition, which facilitated membrane fouling control. The photothermally-activated PMS pre-treatment seems to alleviate membrane fouling by limiting the foulant-membrane interaction, which was observed to result in the formation of the fouling layer containing aromatic proteins, microbial byproducts-like substances, and inorganic ( e.g., calcium) foulants. Finally, characterization of the used MD membranes revealed that the MD membrane properties could be kept unchanged by the photothermally-activated PMS pre-treatment step, thereby making the integrated DCMD system sustainable and attractive for widespread applications.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Yiwu Tang,Jin Kang,Min Wang,Chongyue Jin,Jiayun Liu,Mei Li,Siyan Li,Zhilin Li
In this work, FeVO 4 nanorods were successfully synthesized and employed as peroxymonosulfate (PMS) activators for oxytetracycline (OTC) degradation. The obtained FeVO 4 nanorods exhibited excellent catalytic performance for PMS activation because of the synchronous transformations of Fe 3+ /Fe 2+ , V 5+ /V 4+ and Fe 3+ /V 4+ , and abundant adsorbed oxygen (O ads ). Almost 100% of OTC can be decomposed via FeVO 4 activating PMS in 40 min and the reaction rate constant (k) was 0.1073 min −1 , being 5.65 times of commercial Co 3 O 4 (0.0219 min −1 ). Meanwhile, FeVO 4 exhibited a good stability and reusability. In addition, the impacts of experimental parameters (catalysts and PMS dosage, temperature, pH, and co-existing anions) on OTC degradation were detected in detail. It was proved that •O 2 − , •OH and 1 O 2 were generated and the contribution role in OTC degradation followed the sequence” •OH > 1 O 2 ≈ •O 2 − . The possible mechanism of PMS activation by FeVO 4 was deeply explored and the OTC degradation pathway was deduced according to the detected degradation intermediates. This study develops one new environmental-friendly, low cost, high efficiency and stable PMS activator for the efficient removal of antibiotics.
研究领域:
环境科学
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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
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IF 8.6
Weibao Liu,Ying Yang,Yunhe Li,Yuerong Zhou,Ce Wang,Yingtang Zhou,Jiangwei Shang,Xiuwen Cheng
The preparation of sulfate-based advanced oxidation catalysts is usually both complex and expensive. In this study, natural manganese sand enriched with oxygen vacancies was prepared by NaBH 4 reduction of natural manganese sand for activating peroxymonosulfate (PMS) to remove carbamazepine (CBZ). 70% of carbamazepine was degraded at 120 min when natural manganese sand enriched with oxygen vacancies and PMS were dosed at 0.4 g/L and 0.3 g/L respectively, and the reaction rate constant of the natural manganese sand system with rich oxygen vacancies was 7 times that of the common system. The mineralization of total organic carbon (TOC) reached 41.9%. Combined EPR and radical quenching assays revealed that degradation of pollutants relied on the involvement of free radicals and non-free radicals, in which singlet oxygen was dominant. The XPS results showed that the redox cycles of Fe 3+ /Fe 2+ and Mn 4+ /Mn 3+ /Mn 2+ promoted the generation of free radicals. Density functional theory results also showed that the energy required for PMS to adsorb on natural manganese sand with many oxygen vacancies was decreased, and the O O bond was elongated, which was beneficial to the catalytic reaction. According to LC-MS and Fukui function, the degradation route of CBZ was predicted, and the toxicity of the breakdown products was calculated. The research provides a reference for introducing oxygen vacancies in natural catalysts to improve degradation performance for “green (source) to green (application)”.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Arabian Journal of Chemistry
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2023
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IF 6
Aijing Li,Xinpeng Chen,Ping Yao,Jun Zhang,Tieling Xing,Guoqiang Chen
In this work, polydopamine (PDA) was used to facilitate the reduction of silver nitrate (AgNO 3 ) to silver nanoparticles (AgNPs) and the simultaneous loading on waste silk fabrics (PDA-SF/AgNPs). The removal activity of the obtained composite PDA-SF/AgNPs on different dyes in the presence of hydrogen peroxide (H 2 O 2 ) and potassium peroxymonosulfate (PMS) was compared. The effects of reaction temperature, H 2 O 2 /PMS dosage, dye concentration, composite dosage, electrolyte concentration and time in two catalyst systems on the dye removal were discussed. The results showed the dye removal of Telon Red A2R reached 81% and 95% in 30–50 min in PDA-SF/AgNPs-H 2 O 2 and PDA-SF/AgNPs-PMS system, respectively. Quenching experiments demonstrated that ·OH, ·O 2 – and SO 4 - · were produced during the degradation process, and the possible degradation pathway of Telon Red A2R were analyzed by HPLC-MS. In addition, the kinetic study indicated that the removal of dye followed quasi-second-order adsorption kinetics. These findings suggest that fabric-based composites have great potential and applications in catalysis and treatment of wastewater.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
CHEMICAL PHYSICS LETTERS
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2025
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IF 3.1
Ying He,Lidan Ding,Jiabin Zhou,Dan Liu,Ying Zhang
In this study, Fe 2 O 3 /Bi 2 O 3 p-n heterojunction photocatalysts were fabricated to remove tetracycline (TC). The Fe 2 O 3 /Bi 2 O 3 /Vis/PMS system achieved the complete degradation of TC within 80 min, with a reaction rate constant of 0.0553 min −1 , which was 34.5 and 5.8 times higher than individual photocatalytic process and PMS-AOPs, respectively. This superior catalytic performance of Fe 2 O 3 /Bi 2 O 3 is primarily attributed to two key aspects. Firstly, forming a heterojunction promotes efficient segregation of photogenerated electron–hole pairs, wherein holes (h + ) directly activate PMS. Secondly, PMS simultaneously functioned as an electron acceptor to generate SO₄• − , accelerating the Fe 3+ /Fe 2+ redox cycle while inhibiting electron-hole recombination. This study confirmed the dual advantages of enhanced radical generation through PMS-assisted photocatalysis synergistic effects and improved charge separation via heterojunction engineering.
研究领域:
环境科学
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材料化学
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催化
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水处理技术
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DOI
高影响因子
Journal of Water Process Engineering
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2024
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IF 6.3
Mei Dong,Kuilong Liu,Guoqiang Song,Guiping Ma
In this study, MOF-on-MOF hybrids were successfully synthesized by interfacial growth method using CoZn-ZIF as guest MOF and MIL-101(Fe) as host MOF, and then employed as heterogeneous catalysts to activate peroxymonosulfate (PMS) in the degradation of dyes. The hybrids exhibited different morphologies depending on the Co/Zn ratios (10/0, 10/2, 10/10, and 2/10), all of which displayed exceptional catalytic performance. Notably, the hybrid with a Co/Zn ratio of 10/2 showed the highest degradation rate of MB, reaching 100 % removal within 3 min with a k obs value of 452.75 Lg −1 min −1 based on the pseudo-second-order kinetic model. Through EPR characterization and scavenging experiments, it was determined that the degradation of dyes occurred through a combination of radical (SO 4 •-, •OH)and non-radical ( 1 O 2 ) pathways, with 1 O 2 and SO 4 •- playing prominent roles. Various factors such as Co/Zn ratio, catalyst dosage, PMS concentration, initial pH, temperature, and MB solution concentration were systematically investigated to understand their influence on the catalytic performance. Furthermore, the influence of inorganic ions, humic acid (HA), and the reusability and stability of the catalyst was evaluated, demonstrating its potential for practical applications. Overall, this research provides valuable insights into the design and application of MOF-based catalysts for environmental remediation processes.
研究领域:
环境科学
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催化
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材料科学
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化学工程
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meng Liu,Yu Liu,Qiuyu Chen,Xiaoping Li,Lanxuan Wen,Xiaobao Chen,Dahu Ding,Gen Wang,Yingxin Zhao,Yang Chen,Rongzhi Chen
Inherent defects in carbon material serve as an important way to enhance peroxymonosulfate (PMS) activity, however, the mechanism that activates PMS has always been ambiguous. Herein, the pyrolysis of straw with Prussian blue nanoparticles to prepare CoFe 2 O 4 /C (Carbon) was applied to analyze the mechanism of defective amorphous-C catalyzed activation of PMS. Amorphous-C structural defects increased the specific surface area of CoFe 2 O 4 /C (from 44.19 to 108.73 m 2 /g) with triggered electronic rearrangement, resulting in more PMS adsorption. CoFe 2 O 4 /C ensured the supply of low-valent metals (≡Co 2+ and ≡Fe 2+ ) simultaneously introduced a large number of surface oxygen-containing functional groups, which facilitated free radical generation. The structural defects enhanced electron transfer contributing to the direct oxidative degradation of BPA. Thus, 100 % removal of 450 µM BPA was achieved within 40 min attributed to the combined effect of catalyst-mediated ∙OH, 1 O 2, and electron transfer. Furthermore, the CoFe 2 O 4 /C/PMS system for BPA degradation exhibited universal pH suitability (4 ∼ 10) and low metal leaching (452.10 and 19.53 μg/L for Co and Fe, respectively). This study constructs systematic support for proposing the catalytic mechanism of carbon intrinsic defects activated PMS.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
ACS Catalysis
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2021
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IF 13.084
Lipeng Wu,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Herein, a series of Co@N–C materials are synthesized using nitrates (LiNO3, NaNO3, and KNO3) as templates to control the preferential growth of the cobalt (200) facet. Co@N–C–X (X = LiNO3, NaNO3, and KNO3) exhibit excellent activities and long-term stabilities for Fenton-like degradation of bisphenol A (BPA) with peroxymonosulfate (PMS) as an oxidant. The texture coefficient (TC) is used to investigate the relationship between the Co facets and their catalytic activities, and a linear relation is built between the TC of Co(200) and the reaction rate constant (k). Co(200) is therefore the most active facet for PMS activation, while nitrates can promote the preferential growth of the Co(200) facet. Moreover, the Co(200) facet is more stable against leaching and can achieve more quick transformation between Co2+/Co3+. Quenching tests, electron paramagnetic resonance spectra, and electrochemical tests show that singlet oxygen (1O2) plays the dominant role for BPA degradation. Density functional theory verifies that Co nanoparticles coated with a graphitic nitrogen-doped carbon layer have the best activity for PMS activation. This work first proposes the strategy of using nitrates to control the preferential growth of Co facets and reveals the relationship between the TC value and k, thus attracting great interest in the environmental field.
研究领域:
环境科学
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催化
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材料科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Ye Du,Wen-Long Wang,Zhi-Wei Wang,Chang-Jie Yuan,Ming-Qi Ye,Qian-Yuan Wu
Byproduct formation (chlorate, bromate, organic halogen, etc.) during sulfate radical (SO4•–)-based processes like ultraviolet/peroxymonosulfate (UV/PMS) has aroused widespread concern. However, hypohalous acid (HOCl and HOBr) can form via two-electron transfer directly from PMS, thus leading to the formation of organic halogenated byproducts as well. This study found both PMS alone and UV/PMS can increase the toxicity to mammalian cells of wastewater, while the UV/H2O2 decreased the toxicity. Cytotoxicity of two wastewater samples increased from 5.6–8.3 to 15.7–29.9 mg-phenol/L, and genotoxicity increased from 2.8–3.1 to 5.8–12.8 μg 4-NQO/L after PMS treatment because of organic halogen formation. Organic halogen formation from bromide rather than chloride was found to dominate the toxicity increase. The SO4•–-based process UV/PMS led to the formation of both organic halogen and inorganic bromate and chlorate. However, because of the very low concentration (<20 μg/L) and relatively low toxicity of bromate and chlorate, contributions of inorganic byproducts to toxicity increase were negligible. PMS would not form chlorate and bromate, but it generated a higher concentration of total organic halogen, thus leading to a more toxic treated wastewater than UV/PMS. UV/PMS formed less organic halogen and toxicity because of the destruction of byproducts by UV irradiation and the removal of byproduct precursors. Currently, many studies focused on the byproducts bromate and chlorate during SO4•–-based oxidation processes. This work revealed that the oxidant PMS even needs more attention because it caused higher toxicity due to more organic halogen formation.
研究领域:
环境科学
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毒理学
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水处理
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化学工程
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
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2025
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IF 4.9
Xinping Wu,Mengting Liu,Hongyao Zhao,Danhong Shang,Yanyun Wang,Feng Zeng,Jialing Shen,Jianming Pan,Xiang Liu,Yiyan Song,Fu Yang
Widespread industrial application of bisphenol A (BPA) has produced large amounts of contaminated wastewater, and its accumulation in the environment has threatened human health. In this study, MnOOH nanorods were deposited with the polydopamine layer containing incorporated Co precursor, which was derived to obtain carbon shell confined Co 3 O 4 onto Mn 2 O 3 nanorods. The controlled calcination temperature was optimized to improve the active state of metal species. Carbon shells mediate the electronic interactions between Co 3 O 4 and Mn 2 O 3 , triggering more Co(II/III) redox cycles and an enhanced fraction of Mn(III) along with more oxygen vacancies in Mn 2 O 3 . In addition, more pyridinic N species were generated in the carbon shell of Mn@C/Co-600, affording better affinity to the polar contaminants and peroxymonosulfate (PMS). Therefore, these characters in Mn@C/Co-600 caused the accelerated reaction cycles in the PMS activation and BPA degradation. Compared with other catalysts, Mn@C/Co-600 showed the highest degradation efficiency of bisphenol A (BPA) with the rate constant of 0.827 min −1 , which was up to 30 times higher than that of Mn@C/Co-Cl-600 (0.027 min −1 ). The anions interference effect on BPA degradation follows the order of Cl − (0.925 min −1 )
研究领域:
环境科学
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材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）