Polymers
·
2023
·Vol. 15
·期 8
·1918
·
IF 5
Rui Zhou,Wusong Xu,Peisen Liu,Shangyuan Zhao,Gang Xu,Qizhong Xiong,Weifeng Zhang,Chaochun Zhang,Xinxin Ye
Phosphorus is one of the important metabolic elements for living organisms, but excess phosphorus in water can lead to eutrophication. At present, the removal of phosphorus in water bodies mainly focuses on inorganic phosphorus, while there is still a lack of research on the removal of organic phosphorus (OP). Therefore, the degradation of OP and synchronous recovery of the produced inorganic phosphorus has important significance for the reuse of OP resources and the prevention of water eutrophication. Herein, a novel FeOOH-loaded aminated polyacrylonitrile fiber (PANAF-FeOOH) was constructed to enhance the removal of OP and phosphate. Taking phenylphosphonic acid (PPOA) as an example, the results indicated that modification of the aminated fiber was beneficial to FeOOH fixation, and the PANAF-FeOOH prepared with 0.3 mol L−1Fe(OH)3colloid had the best performance for OP degradation. The PANAF-FeOOH efficiently activated peroxydisulfate (PDS) for the degradation of PPOA with a removal efficiency of 99%. Moreover, the PANAF-FeOOH maintained high removal capacity for OP over five cycles as well as strong anti-interference in a coexisting ion system. In addition, the removal mechanism of PPOA by the PANAF-FeOOH was mainly attributed to the enrichment effect of PPOA adsorption on the fiber surface’s special microenvironment, which was more conducive to contact with SO4•−and •OH generated by PDS activation. Furthermore, the PANAF-FeOOH prepared with 0.2 mol L−1Fe(OH)3colloid possessed excellent phosphate removal capacity with a maximal adsorption quantity of 9.92 mg P g−1. The adsorption kinetics and isotherms of the PANAF-FeOOH for phosphate were best depicted by pseudo-quadratic kinetics and a Langmuir isotherm model, showing a monolayer chemisorption procedure. Additionally, the phosphate removal mechanism was mainly due to the strong binding force of iron and the electrostatic force of protonated amine on the PANAF-FeOOH. In conclusion, this study provides evidence for PANAF-FeOOH as a potential material for the degradation of OP and simultaneous recovery of phosphate.Keywords:polyacrylonitrile fiber;FeOOH;activate peroxydisulfate;organic phosphorus;adsorption
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
CHEMOSPHERE
·
2022
·
IF 8.943
Chen Chen,Lu-Lu Zhou,Yu-Nuo Huang,Wei-Kang Wang,Juan Xu
Biochar has been developed to activate persulfate for wastewater treatment due to its carbon essence, easily-available and low-cost. Efficiently active sites and interfacial electron transfer are highly desired for peroxydisulfate (PDS) activation. In this study, boronic ester structure and defect degree of boron-doped biochar are confirmed as activate sites to improve PDS activation. The performance of pollutants degradation is proven to have structure-activity relationships with both activate sites. Moreover, boron-doped biochar exhibits higher stability and oxidation potential by forming the surface-confined complex, promoting electron transfer from pollutants to complex. The optimized boron-doped biochar has the advantages of adapting to a broad pH range (2.9–10.0), strong resistance to Cl − and organic matters, a low activation energy of 11.22 kJ mol −1 , and achieving the decomposition of practical dyeing wastewater. Our work provides a promising approach to regulating the interfacial catalytic sites of biochar by doping heteroatom for PDS activation in practical wastewater treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Wang Yangyang,Xu Jianfeng,Wang Xiaoshu,Li Tongtong,Zhang Gen,Yan Zheng,Liu Jiancong,Wang Lei
The background value of iron in red soil is superior, primarily absorbed and homogeneously encapsulated in harvested biomass. However, this property on the high-value utilization of bionic iron-encapsulated biomass remains unknown. In this study, special biochar (Fe@BC) was obtained from this kind of biomass by one-step pyrolysis method, which was further used to activate peroxydisulfate (PDS) and degrade 2,4-dichlorophenol (2,4-DCP). The results showed that Fe3O4 was formed and homogeneously embedded in biochar at 500oC. Comparing to catalysts prepared by impregnation pyrolysis (Fe/BC), Fe@BC exhibited excellent degradation performance (90.9%, k = 0.0037 min−1) for 2,4-DCP. According to the free radicals quenching studies, hydroxyl radicals (·OH) and superoxide radicals (·O2−) were the dominant reactive oxygen species (ROS) in Fe@BC/PDS system. Importantly, a PDS adsorption model was established, and the electron transport and PDS activation in the core-shell structure were demonstrated by DFT calculations. Therefore, this study could supply a high-performance catalyst and significant implications for high-value biomass utilization in red soil.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Qin Yin,Haihong Yan,Yu Liang,Haiyan Wang,Pingzhou Duan,Bo Lai
The recycling of biochar for wastewater treatment has attracted much attention due to the persistent increase of organic waste. Recently, it has been demonstrated that nitrogen (N)-doping biochar has high catalytic activity, however, the role of exogenous N and the reaction mechanism are not yet clear. In this study, biochar was manufactured from cyanobacteria from Lake Dianchi via thermal pyrolysis and decorated with N atoms to enhance its catalytic performance in peroxydisulfate (PDS) activation. The optimal synthesis of C/N = 1:2 (CN12) with high N loading, large specific area, and excellent electron transfer rate was achieved. A comprehensive study of the mechanism was conducted by integrating selective ESR, radical scavenging experiment, and electrochemical measurements, which demonstrated that the degradation of TC includes free radical and nonradical pathways. The formation of 1 O 2 and surficial reactive complexes derived from PDS performs a crucial role by attacking the adsorbed TC molecules. It is proved that N-doping accelerates the electron transfer between TC and PDS by increasing electrochemical specific area and mediation of a metastable CN12/PDS complex. Moreover, N-containing functional groups such as graphitic N, pyridinic-N and C O/C C/C N functional groups strengthened the nonradical pathway mediated by sp 2 defects. The influence of an alkaline environment indicates that electrostatic interaction between TC and CN12 determines the adsorption capacity and formation of surface reactive complexes. This study helps to understand the mechanism of an algal biochar catalyst for PDS activation and degradation of organic pollutants, and proposes a new approach for solid waste recycling.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Cai-Wu Luo,Liang Jiang,Sen-Ping Mao,Chao Xie,Deng-Gao Huang,Tian-Jiao Jiang
The metal-nitrogen-carbon materials are considered as ideal candidates for activating peroxydisulfate (PDS) to remove organic pollutants in wastewater. However, the bimetallic oxides supported g-C 3 N 5 with nitrogen vacancies (Nvs) is little reported. In this work, a novel CuMn/g-C 3 N 5 -Nvs composite was fabricated by a simple method and then applied for the activation of PDS to degrade tetracycline (TC). A series of characterization results revealed that the the bimetallic CuMn oxides was successfully loaded onto the surface of g-C 3 N 5 , enriching catalytic active sites and forming more Nvs. The preparation of catalyst and related reaction conditions were systematically evaluated. The results showed that the degradation efficiency of TC by CuMn/g-C 3 N 5 -Nvs was 21 and 46 times higher than that of CuMnO x and g-C 3 N 5 . This enhancement was attributed to the synergistic effect among Cu and Mn ions, and Nvs in the CuMn/g-C 3 N 5 -Nvs. Furthermore, this catalyst exhibited a good stability. The quenching and electron spin resonance experiments confirmed that the TC removal was occurred through the co-existence of radical and non-radical pathways. Additionally, the biological toxicity tests demonstrated that its toxicity significantly decreased after treatment by the CuMn/g-C 3 N 5 -Nvs/PDS system. Overall, this work provided a feasible approach for constructing the composite containing Nvs and highlighted the potential treating process for environmental remediation.
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
Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Fang-Lan Geng,Hai-Yuan Chi,Hua-Chao Zhao,Jin-Quan Wan,Jian Sun
Fe-based metal-organic frameworks (MOFs) show high activity toward the activation of peroxodisulfate (PDS) for the removal of organic micropollutants (OMPs) in wastewater treatment. However, there is a phenomenon of Fe ion dissolution in the Fe-based MOFs’ active PDS system, and the reasons and influencing factors that cause Fe ion dissolution are poorly understood. In this study, we synthesized four types of Fe-based MOFs and confirmed their crystal structure through characterization. All types of Fe-based MOFs were found to activate PDS and form sulfate radicals (SO 4 − ), which effectively remove OMPs in wastewater. During the process of Fe-based MOFs activating PDS for CIP removal, activated species, oxidant reagent, and pH negatively impact the stability performance of the MOFs’ structure. The coordination bond between Fe atom and O atom can be attacked by water molecules, free radicals, and H + , causing damage to the crystal structure of MOFs. Additionally, Fe (II)-MOFs exhibit the best stability performance, due to the enhanced bond energy of the coordination bond in MOFs by the F ligands. This study summarizes the influencing factors of Fe-based MOFs’ damage during PDS activation processes, providing new insights for the future development of Fe-based MOFs.
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
APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Peixun Zhai,Haibo Liu,Fuwei Sun,Tianhu Chen,Xuehua Zou,Hanlin Wang,Ziyang Chu,Can Wang,Meng Liu,Dong Chen
As a natural and environmentally friendly adsorbent, palygorskite (Pal) has been approved to be excellent for the adsorption of dyes . However, the spent Pal is difficult to be regenerated through normal desorption methods, and thus, becoming a solid waste. In this study, methylene blue (MB) was adsorbed by Pal, and the MB absorbed on palygorskite (MP) was carbonized at different temperatures. The carbonized MP (CMP) was used for peroxydisulfate (PDS) activation to degrade bisphenol A (BPA). The effects of carbonization temperature, pH values, PDS concentration, and catalysts dosage on BPA degradation were investigated. The results show that the MP carbonized at 800 °C (CMP800) has the best activation performance due to the high degree of carbon defectivity and high specific surface area. The CMP800 can effectively degrade BPA over a wide pH range from 3 to 9 and is extremely resistant to the effects of various anions, such as Cl − , NO 3 − , HCO 3 − , and H 2 PO 4 − . Based on quenching experiments, electron spin resonance (ESR), and electrochemical analysis results, a non-radical pathway involving electron transfer from BPA to PDS is responsible for the degradation of pollutants. Moreover, the CMP800 has a high total organic carbon (TOC) removal efficiency of 83%, high stability in three cycles, and low PDS consumption. This study demonstrates the feasibility of the treatment and utilization of the waste Pal, which also provides a carbon-based activator for the activation of PDS to degrade organic contaminants .
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Mengjiao Pei,Keyan Li,Xiangyang Li,Chunshan Song,Xinwen Guo
Iron phthalocyanine/carbon nitride (FePc/CN) heterojunction nanosheets were prepared by a facile calcination strategy, which exhibited superior ability of peroxydisulfate (PDS) activation toward degradation of tetracycline (TC) assisted by visible light. The removal rate of high-concentration TC (50 mg L–1) over FePc/CN-6 reached 97% within 40 min, with the degradation rate constant of 4.4 and 9.2 times those of CN and FePc, respectively. The excellent catalytic performance of FePc/CN-6 could be attributed to the synergistic effect between photocatalysis and PDS activation. The construction of the FePc/CN-6 heterojunction with an intimate interface via π–π conjugation inhibited the aggregation of FePc, promoted charge separation and transfer, and broadened the response range of visible light. As a result, the highly dispersed Fe active sites as well as more available photogenerated electrons and holes enhanced the PDS activation and the photodegradation. EPR spin-trapping tests and radical quenching experiments confirmed the role of multiple active species in the TC removal. The effects of temperature, pH, coexisting anions, and water sources on the removal rate of TC were investigated. FePc/CN-6 also displayed good potential in actual wastewater treatment. This work not only provides insight into design and preparation of efficient and stable catalysts for PDS activation but also establishes a promising catalytic oxidation system for the green remediation of actual wastewater.
研究领域:
环境科学
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 13
·5345-5358
·
IF 3.5
Zhang Min,Deng Xingping,Yang Hua,Ding Yao,Ran Longzheng,Zhang Liang
Abstract Sulfonamides are detected in various water environments and threaten aquatic ecosystems. To remove sulfonamides, many previous studies have focused on preparing metal–organic framework-derived carbon materials (MOFs-CMs) applied in persulfate activation. In this study, Fe-based MOFs derived from porous carbon materials were obtained by facile one-pot hydrothermal and pyrolysis. The catalyst can overcome passivation in alkaline environments and showed a high peroxydisulfate (PDS) activation performance. Unlike traditional modifications, ZnO was added during the synthesis process to control the morphology characteristics of the catalyst. FeZn–MOF-CMs in this study displayed a high sulfadiazine removal efficiency of 99.6% in alkaline conditions, and exhibited high resistance to common anions and organic matter. The surface morphology could be controlled by different amounts of ZnO additions and the free radical pathway was the main mechanism in the PDS system. This study provides a facile synthesis method for the preparation of porous carbon materials from Fe-based MOFs. 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
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Zhendong Yu,Jiachen Ma,Jinlan Dai,Shiyu He,Xiaoyi Huang,Yuancai Lv,Yifan Liu,Chunxiang Lin,Junfeng Chen,Minghua Liu
In this study, a bimetallic composite catalyst (Co–Fe@C) was fabricated with calcination at high temperature (800 °C) by using Co-MIL-101 (Fe) as the precursor. The characterization results showed that the resulted Co–Fe@C composite mainly consisted of carbon, FeCo alloys, Fe 3 O 4 , Co 3 O 4 and FeO, and owned evident magnetism. In addition, the Co–Fe@C was employed to activate the peroxydisulfate (PDS) to degrade a representative organic pollutant ( p -arsanilic acid, p -ASA) and the main factors were optimized, which involved 0.2 g L −1 of catalyst dosage, 1.0 g L −1 of PDS dosage and 5.0 of initial pH. Under the optimal condition, Co–Fe@C/PDS system could completely degrade p -ASA (20 mg L −1 ) in 5 min. In the Co–Fe@C/PDS system, SO 4 − · , Fe(IV) and ·OH were the main species during p -ASA degradation. Under the attack of these species, p -ASA was first decomposed into phenols and then transformed into the organics acids and finally mineralized into CO 2 and H 2 O through a series of reactions like hydroxylation, dearsenification, deamination and benzene ring opening. Importantly, most of the released inorganic arsenic species (93.40%) could be efficiently adsorbed by the catalyst.
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
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Tian Wang,Xufang Qian,Dongting Yue,Xuan Yan,Hiromi Yamashita,Yixin Zhao
Perovskite oxides ABO 3 with unique structure showed promising performance on persulfates activation. Previous research works mainly focused on Co-based or rare earth metal (La, Sr)-based perovskite oxides for peroxymonosulfate (PMS) activation. Here, we firstly studied perovskite CaMnO 3 metal oxide composed with the low cost and eco-friendly Ca and Mn elements for PDS activation. Perovskite CaMnO 3 metal oxide achieve the superior catalytic activity for reactive oxygen species generation than the regular Mn oxides (β-MnO 2 and Mn 2 O 3 ) and other types Ca x Mn y O z (spinel-type CaMn 2 O 4 and Ca 2 MnO 4 ) solid solution due to the tolerance of Mn multivalence and defects in the perovskite structure and the excellent Mn 3+ /Mn 4+ redox capacity in CaMnO 3 . The CaMnO 3 /PDS system could be applied at a wide pH range from 4 to 12, and exhibited better performance in basic conditions. Different active species including SO 4 − , OH reactive radicals and singlet oxygen 1 O 2 were found and responsible for effective pollutants degradation. Our study shows eco-friendly perovskites possess great potential in the refractory organic pollutants removal by catalytic activation of PDS.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CARBON
·
2025
·
IF 11.6
Bowen Yang,Longhui Zheng,Zhiwen Cheng,Maohong Fan,Jiming Hao,Qiang Ma
Phenol-polluted water poses significant risks, inflicting serious harm on both aquatic and terrestrial organisms. While Fenton and Fenton-like processes have been widely employed in wastewater treatment, their effectiveness is hindered by a major limitation: the sluggish cycle of Fe(III)/Fe(II). This slow cycle has become the Achilles' Heel of these methods, preventing their broader application. In this study, graphene oxide (GO) was introduced to facilitate the generation of Fe(II) from Fe(III), enhancing peroxydisulfate (PDS) activation for pollutant degradation. The Fe(III)/GO/PDS system demonstrated effective pollutant degradation capability with 100 % treatment efficiency (phenol = 10 mg L −1 , GO = 50 mg L −1 , Fe(III) = 0.2 mM, PDS = 1 mM, and initial pH of 3). The radical-mediated oxidation mechanism was proposed based on radical scavenger effects, oxidation products, and electron paramagnetic resonance spectra. The conversion of methyl phenyl sulfoxide (PMSO) to methyl phenyl sulfone (PMSO 2 ) indicated the formation of Fe(IV) in Fe(III)/GO/PDS system. To reveal degradation rules for multiple substrates, eighteen molecular descriptors were calculated using density functional theory (DFT) and correlated them with degradation rate constants ( k ). BO n , E B3LYP , and F (−) x emerged as significant parameters in this relationship. The Fe(III)/GO/PDS system demonstrated excellent reusability during the first five runs, effectively treating contaminants. However, its performance was hindered by kinetic retardation when certain anions, such as phosphate and bicarbonate, were present. These findings contribute to both scientific understanding and technical development of persulfate activation via the Fe(III)/Fe(II) cycle using carbonaceous materials, particularly for environmental remediation applications.
研究领域:
环境科学
·
化学工程
✓ 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）