PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2022
·Vol. 119
·期 30
·e2202682119
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IF 12.779
Mingjie Huang,Yu-Sheng Li,Chuan-Qi Zhang,Chao Cui,Qing-Qing Huang,Mengkai Li,Zhimin Qiang,Tao Zhou,Xiaohui Wu,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS)–based advanced oxidation processes (AOPs) have shown a great potential for pollutant degradation, but their feasibility for large-scale water treatment application has not been demonstrated. Herein, we develop a facile coprecipitation method for the scalable production (∼10 kg) of the Cu-Fe-Mn spinel oxide (CuFeMnO). Such a catalyst has rich oxygen vacancies and symmetry-breaking sites, which endorse it with a superior PMS-catalytic capacity. We find that the working reactive species and their contributions are highly dependent on the properties of target organic pollutants. For the organics with electron-donating group (e.g., -OH), high-valent metal species are mainly responsible for the pollutant degradation, whereas for the organics with electron-withdrawing group (e.g., -COOH and -NO2), hydroxyl radical (•OH) as the secondary oxidant also plays an important role. We demonstrate that the CuFeMnO–PMS system is able to achieve efficient and stable removal of the pollutants in the secondary effluent from a municipal wastewater plant at both bench and pilot scales. Moreover, we explore the application prospect of this PMS-based AOP process for large-scale wastewater treatment. This work describes an opportunity to scalably prepare robust spinel oxide catalysts for water purification and is beneficial to the practical applications of the heterogeneous PMS-AOPs.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Yingqing Guo,Zhenyu Jin,Xiaolu Li,Feng Wang,Yuanyuan Yan,Leiyu Feng
Water pollution caused by antibiotic abuse has become an urgent environmental problem. In this study, nitrogen-doped carbon materials which were prepared with reindeer manure via a thermal annealing method (shortened as DF X , X representing the thermal temperature) were applied to the removal of tetracycline hydrochloride (TH) in wastewater. According to the results, the DF700 material had the best adsorption ability, and could catalyze the degradation of TH by potassium persulfate (PS). At the initial concentration of 35 mg/L, about 69.8% of TH could be removed within two hours after the catalytic oxidation . The material characterization showed that DF700, which was doped with 2.4% nitrogen atoms , had a large specific surface area and mesoporous structures, resulting in excellent adsorption and catalytic properties. Furthermore, the degradation reaction by PS over the nitrogen-doped carbon materials was confirmed a nonradical oxidation process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Amina,Qumber Abbas,Awais Shakoor,Mu Naushad,Balal Yousaf
Calcium peroxide (CaO₂) and persulfate (PS) dual oxidant system is an innovative in-situ chemical oxidation (ISCO) technique for the restoration of contaminated groundwater. Several field applications also confirm its efficacy in remediating the groundwater, however, published articles are rarely present. In this work, the performance of the CaO₂/PS system was examined for the degradation of sulfamethoxazole (SMX) in the SMX polluted soil and water. Results indicated that SMX could be efficiently degraded with CaO₂ and PS (2 g/L dosages for each oxidant) around neutral pH (7), and 95.8% pollutant removed after 36 h of reaction time. The removal efficiency of SMX improved as the concentrations of CaO₂ and PS were increased. Moreover, SMX removal was significantly decreased with the increase of initial solution pH. This dual oxidant system at 30 °C was also used for the remediation of SMX (10 mg/kg) spiked soil. Soil degradation experiment was performed at 150 rpm of shaking speed using soil slurry (soil/water; 1/1 ratio) at pH 7. Dual oxidant dosage was kept at 2 g/L CaO₂ and 2 g/L PS. The results showed that this dual oxidant system is also very efficient for the antibiotics SMX degradation in the soil system. Overall, an insight knowledge and practical information gained from this work will help in the treatment of SMX contaminated soil and water as well as wastewater with CaO₂/PS dual oxidant system.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qiulian Yang,Jian Ke,Haitao Li,Wei Huang,Dong Wang,Yanhua Liu,Jianqiu Chen,Ruixin Guo
Treatment of organic contaminants in waste acid via electrochemical oxidation process has drawn sustained attention. Inspired by the electro-generation of persulfate from homogeneous sulfate (SO 4 2- ) in waste acid and the catalytic activity of heterogeneous tourmaline, this study aimed to investigate the feasibility of in-situ persulfate electro-generation and activation via utilizing homogeneous–heterogeneous hybrid catalysts system (SO 4 2- /tourmaline) for organic contaminants removal in high chemical oxygen demand (COD) sulfate-containing waste acid. p -Aminodiphenylamine (RT-Base) was selected as a model organic contaminant to explore the mechanism of electrolysis/SO 4 2- /tourmaline system. No RT-Base was detected after 60 min reaction in electrolysis/SO 4 2- /tourmaline system. The formation of • OH and SO 4 •− in electrolysis/SO 4 2- /tourmaline system made contributions to the RT-Base degradation. Degradation intermediates of RT-Base were identified and possible degradation pathway was proposed. Additionally, the application of electrolysis/SO 4 2- /tourmaline system in treating the real RT-Base waste acid, which contained high COD and SO 4 2- , was explored. Results showed that the COD removal rate was 67.94% under the optimal conditions, and the electrolysis/SO 4 2- /tourmaline system could enhance the biodegradability of RT-Base waste acid. Furthermore, the electrolysis/SO 4 2- /tourmaline system followed by the activated sludge process achieved a high COD removal efficiency (99.09%). Microbial DNA analysis suggested that Bacteroidetes, Proteobacteria, and Actinobacteria were the dominant bacterial phyla in the activated sludge; and metabolism was the predominant microbial function. In-situ electro-generation of persulfate/SO 4 •− for organics degradation achieved efficient utilization of waste sulfate. Electrochemical oxidation process with activated sludge process as a post-treatment showed great potential in the treatment of organics in high-sulfate waste acid.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Ze-Wei Ma,Wen-Rong Li,Jing-Yue Zhang,Wen-Xin Yang,Shaozao Tan,Ji-Ye Cai,Sui-Ping Deng
Effective photosensitizers (PSs) are at the heart of the key role of photo-driven antibacterial therapy. However, relative high temperature required for bactericidal activity, stimulating at multiple wavelengths, and multi-step synthesis of the photothermal and photodynamic agents challenge their applications in antibacterial treatment. In this study, silver nanoparticles (AgNPs) functionalized by kaempferol (Kae) are implanted into Prussian blue (PB) to construct photo-responsive nanocubes (AgPB) by a simple synthetic process. The as-synthesized AgPB nanocomposites were found to have an average size of ∼140 nm, and the particle size range of the loaded-AgNPs was 5–15 nm. The structure of AgPB was characterized, and the photothermal and photodynamic evaluation of antibacterial activity of AgPB was investigated under single 808 nm near-infrared (NIR) light. By adjusting the doping ratio of AgNPs, the band gap can be tuned from 2.78 to 2.56 eV to further enhance the photothermal conversion of AgPB and its ability to generate reactive oxygen species (ROS). When compared with AgPB without NIR illumination, in vitro antibacterial studies by usingEscherichia coliandStaphylococcus aureusshowed that AgPB under 808 nm NIR light could rapidly heat up to 50 °C, enhance the formation of ROS, and promote the ion release amount of Fe2+, Fe3+, and Ag+ to increase oxidative stress, leading to inhibition of bacterial proliferation significantly. BothE. coliandS. aureuswere completely killed within 10 min. Moreover, the biofilm formation was remarkably inhibited, and the eradication ratio againstE. coliandS. aureusbiofilms was 69.73 and 60.01%, respectively. In addition, the hemolytic activity test proved that AgPB had good biocompatibility. The results showed that AgPB with triple bactericidal modalities could expand the application of PSs and serve as a promising nanocomposite for antibacterial therapy.
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RSC Advances
·
2022
·Vol. 12
·期 37
·24088-24100
·
IF 4.036
Yan Wang,Tao Gan,Jingyu Xiu,Ganghua Liu,Haiming Zou
Solid waste resource utilization and the treatment of wastewater are two important aspects in environmental protection. Here, biochar (BC) derived from municipal sewage sludge has been combined with ZnFe2O4 to form the photocatalyst ZnFe2O4/biochar (ZnFe/BC), and it was used to degrade sulfadiazine (SDZ) in the presence of peroxymonosulfate (PMS) under visible (Vis) light irradiation in an internal loop-airlift reactor (ALR). The surface morphology and structure of ZnFe/BC have been characterized by X-ray diffraction (XRD), scanning electron microscopy equipped with an attachment for energy-dispersive spectroscopy (SEM-EDS), X-ray photoelectron spectroscopy (XPS), and UV-Vis diffuse reflectance spectroscopy (UV-Vis DRS). ZnFe/BC displays outstanding photocatalytic performance and reusability. After four reuse cycles of ZnFe/BC in the Vis/ZnFe/BC/PMS system, the SDZ degradation rate and efficiency still reached 0.082 min−1 and 99.05%, respectively. Reactive species in this system included free radicals SO4˙−, ˙OH, and ˙O2−, as well as non-radicals 1O2, e−, and h+, as established from the results of chemical quenching experiments and electron paramagnetic resonance (EPR) analyses. Moreover, a mechanism of action of the Vis/ZnFe/BC/PMS system for SDZ degradation was proposed. The acute toxicity of the reaction solution towards Photobacterium phosphoreum T3 spp. in the Vis/ZnFe/BC/PMS process increased during the first 40 min and then decreased, illustrating that Vis/ZnFe/BC/PMS provided an effective and safe method for the removal of SDZ.
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Environmental Technology & Innovation
·
2022
·
IF 7.758
Yu-Xiang Shi,Lei Li,Da-Mao Xu,Rong-Bing Fu
In this study, inorganic and organic radicals generated from a thermally activated peroxyacetic acid (PAA) system were used to degrade pentachlorophenol (PCP) in contaminated soils. In addition, the effects of various operating parameters on PCP removal were fully considered, including reaction temperature, PAA dosage, initial pH and natural organic matter (NOM). The experimental results showed that PCP was more easily degraded under the conditions that temperature was higher than 40 °C and near neutral pH, and PAA dosage was more than 750 mM/kg. In contrast, humic acid (HA) exhibited a significant inhibitory impact on PCP degradation. The results from the chemical quenching and electron para-magnetic resonance (EPR) experiments further indicated that in the PAA system, HO• has much better degradation ability for PCP than 1 O 2 . Moreover, the degradation of PCP was dominated by R-O• radicals, including CH 3 C(O)O• and CH 3 C(O)OO•. Besides, the potential degradation pathways of PCP by PAA system were investigated, based on the degradation intermediates and the density functional theory (DFT) calculation. The present study results indicated that the combined process of PAA and heat treatment has a significantly high efficiency in the degradation of chlorobenzenes in soils. This study is the first to use thermally activated PAA for soil remediation without the use of other chemicals as activators, and provides a novel, efficient and economical technique for the remediation of actual chlorinated hydrocarbon contaminated sites.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Wenli Yao,Mingzhe Li,Changduo Sun,Yanlong Liu,Mengling Ma,Fengjuan Chen,Lei Zhou,Yian Zheng
Removal of perfluorinated compounds (PFCs) from the environment is a major challenge due to their refractory, persistent and bioaccumulative properties. In this study, trace Co coupled via Co–P coordination and tourmaline (TM) doped g-C 3 N 4 was fabricated (marked as Co/TM/g-C 3 N 4 ) and used as the catalyst for activating peroxymonosulfate (PMS) to remove emerging PFOA under visible light irradiation. Several affecting parameters were systematically investigated, inlcuding Co/TM/g-C 3 N 4 dosage, PMS concentration, initial pH, as well as coexisting Cl − , HC O 3 − , H 2 P O 4 − , N O 3 − and humic acid . Under the conditions of 0.5 g/L Co/TM/g-C 3 N 4 , 2.5 g/L PMS and pH 3.0, the developed synergistic system had the ability for 81.11% removal of PFOA within 4 h, 67.64% removal after the fourth run, and also could be effectively applied in actual water bodies. During the degradation process , π-π*, N–C N and graphite N played the vital role, with the final defluorination rate of 31.12% at 4 h. Free radical quenching and quantitative analysis, as well as electron paramagnetic resonance was used to verify the free radical and non-free radical pathways for PFOA removal, with the findings that S O 4 • − (2.61 μM at 1 h), •OH (0.067 μM at 4 h), O 2 • − , h + , and O 1 2 were involved with possible time-dependent. By liquid chromatography-mass spectrometry analysis, the short-chain intermediates of C3–C7 were proposed and identified. From this study, trace Co coupled and TM doped g-C 3 N 4 demonstrated higher catalytic potential to activate PMS for visible-light synergistic PFOA removal, with the expectation of achieving a cleaner water environment for human beings.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Xinyu Hu,Juntao Wang,Jing Wang,Yao Deng,Huidi Zhang,Tao Xu,Wenlei Wang
In this work, a high-energy β electron beam was applied to promote the generation and directional inward migration of surface oxygen defects. The valence band potential changed to a high potential due to the transfer of surface oxygen vacancies on BiVO 4 /Bi 2 O 3−x . Interface oxygen vacancies have significant advantages in inducing the formation of oxygen vacancy levels and reducing the band gap energy. Surface oxygen vacancy and vacancy levels can prevent the recombination of photogenerated carriers. The electrons enriched in the surface oxygen vacancies can remarkably activate PMS with O−O bonds to degrade ciprofloxacin (CIP). The degradation kinetic constant and CIP mineralization rate of BiVO 4 /Bi 2 O 3−x -450/PMS were 2.09 and 1.51 times higher than those of BiVO 4 /Bi 2 O 3−x /PMS, respectively. BiVO 4 /Bi 2 O 3−x -450 with a lower relative content of surface oxygen vacancies (24.70%) exhibited a stronger activation ability. Obviously, the change of band structure caused by interface oxygen vacancies is the reason for increasing photoactivation efficiency of PMS.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Mei-Mei Wang,Li-Juan Liu,Jia-Rui Xi,Ying Ding,Peng-Xi Liu,Liang Mao,Bing-Jie Ni,Wei-Kang Wang,Juan Xu
The presence of oxygen vacancies (OVs) promotes persulfate activation. However, rational modulation of OVs without compromising the inherent structure of catalysts is challenging. Herein, novel OVs-enriched hollow ZnCo 2 O 4 nanocages are synthesized based on a bimetallic ZIF-67@ZIF-8 precursor for efficient peroxydisulfate (PDS) activation. The incorporation of Zn into the lattice of Co 3 O 4 boosts the number of OVs in the catalysts while preserving the morphology of Co 3 O 4 nanocages derived from metal-organic framework (MOFs) templates. As a result, the degradation rate of organic pollutants such as bisphenol A is improved by over 20 times in the developed PDS activation system. OVs promote the formation of a surface-activated complex from PDS onto the catalyst surface, which can subsequently deprive electrons from pollutants. The developed PDS activation system is resistant to Cl − , NO 3 − and humic acid at environmental concentrations. This system adapts to selectively degrade organic pollutants with low ionic potential, and shows applicable potential in practical packaging wastewater treatment. The decreased catalytic performance of catalysts during utilization can be recovered with a facile thermal treatment. Our work constructs OV active sites on Co 3 O 4 nanocages while preserving their original structural superiorities, providing a new strategy to functionalize MOF-derived materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Wenwei Feng,Hui Lin,Andac Armutlulu,Jie Chen,Rui Liu,Ruzhen Xie,Bo Lai
A novel eco-friendly vanadium-mediated Magnéli phase titanium suboxide (V@Ti 4 O 7 ) was fabricated via ball-milling-vacuum sintering method. The presence of V improved the stability and electrochemical performance of Ti 4 O 7 , which significantly promoted the activation of persulfate (PS) for superior degradation of organic pollutant ciprofloxacin (CIP). The results show that V doping significantly facilitated the electron transfer process and enhanced the oxygen evolution potential. The redox cycle of V 3+ /V 4+ and V 4+ /V 5+ endows the electrode with high stability and enriched catalytic active sites for PS activation , which allows for 89.11% CIP removal after the 8 th reuse. Scavenging experiments and electron paramagnetic resonance (EPR) results revealed the contribution of reactive oxidant species (i.e., SO 4 − , OH and 1 O 2 ) for efficient CIP degradation in the E-V@Ti 4 O 7 -PS system, in which, OH was the dominant reactive species accounting for 53.09 % of CIP removal, resulting in efficient CIP mineralization (TOC > 86.51%). The results of this study provide a better understanding of the relationship between the nature of anode and electro-activation of PS, which can facilitate the electrode design and optimization of E-PS reactors.
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