CHEMOSPHERE
·
2023
·
IF 8.8
Jiahao Liang,He Liu,Mengyao Zou,Xueqin Tao,Jiangmin Zhou,Zhi Dang,Guining Lu
Polybrominated diphenyl ethers (PBDEs) as a typical brominated flame retardant (BFR) have attracted worldwide attention due to the high environmental risk and resistance to conventional remediation processes. In this study, thermally activated persulfate (TAP) process was applied to degrade 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47), which is the most toxic and representative PBDEs in e-waste dismantling sites. Impact factors such as PDS dosage, heating temperature, and initial pH were evaluated. Results showed that BDE-47 can be 100% degraded within 180 min under the condition of PDS:BDE-47 = 1000:1, 60 °C, and pH = 7. Quenching experiments combined with EPR analysis further proved the important role of SO 4 ·− in oxidating BDE-47. According to high-resolution mass spectrometry (HRMS) analysis, only one oxidation product of low toxicity was detected during the oxidation process. Theoretical calculations further revealed that the oxidation process mainly involved radical attack at C–Br bond, cleavage of C–Br bond, and fission of ether bond, and HSO 4 · may also play an important role in BDE-47 degradation in TAP system. In addition, TAP system exhibited universality as all selected PBDE congeners can be degraded, and the degradation rate of PBDEs was greatly affected by the number of substituted Br atoms in a negative trend. Overall, these findings indicate that TAP can be applied as an effective method for removal of PBDEs, and we provide a new insight for the practical application of TAP technology in BDE-47 degradation from experimental and theoretical aspects.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinhao Wang,Zhaokun Xiong,Hongle Shi,Zelin Wu,Bingkun Huang,Heng Zhang,Peng Zhou,Zhicheng Pan,Wen Liu,Bo Lai
Rationally regulating reaction mechanisms in Fenton-like reactions by tuning the properties of catalysts is of great significance, but still challenging. Herein, we synthesized various active center size-dependent catalysts to realize the switching of reaction mechanisms and pollutant degradation routes in peroxymonosulfate (PMS) activation systems. The results illustrated that the reaction mechanism transformed from radical oxidation (51.64%) to nonradical oxidation (89.92%) with the decrease of active center size from nanoparticle (Co NP -NC) to single atom (Co SA -NC). The evolution of reactive species switched the degradation intermediates and pathway of sulfisoxazole (SIZ). The generation of singlet oxygen ( 1 O 2 ) in Co SA -NC/PMS tends to selectively attack electron-rich site of SIZ, while reaction between radicals and SIZ prefers non-selective oxidation in Co NP -NC/PMS system. Besides, the toxicity tests indicated that the conversion from non-selective to selective oxidation resulted in lower toxicity of effluent after reaction, which can further reduce environmental risks of effluent.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Tianyao Shen,Xiaojing Wang,Jiaqin Li,Peng Xu,Chunyan Yang,Peng Wang,Guangshan Zhang
Antibiotics in surface water adversely affect food safety and aquatic ecosystem, which hinder biological water treatment , and advanced oxidation technology (AOPs) is of great significance. This study achieved nitroimidazole antibiotic metronidazole (MNZ) removal in a dielectric barrier discharge plasma (DBDP) process. A ternary Bi 2 Mn 4 O 10 /NiF (BMON) was synthesized via microwave-assistant to enhance the DBDP process. Compared with Bi 2 Mn 4 O 10 , BMON has a more stable structure with lower ion dissolution but higher oxygen vacancy (Vö) content. The DBDP process generates active species, and O 2 ⋅ − acts as an intermediate in forming 1 O 2 ⋅ − to degrade MNZ through multipath. The cycle of lattice oxygen (O L )/O 2 and M n+ /M (n−1)+ maintain the charge balance on the BMON surface, during which the transformation of Vö and 1 O 2 improve the catalytic efficiency. Furthermore, MNZ possible degradation pathways were proposed by DFT calculations and ESI-QTOF-MS detection. The DBDP/BMON process exhibited great potential for heterogeneous catalytic in nitroimidazole antibiotic degradation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Minzi Liao,Shengxi Zhao,Kai Wei,Hongwei Sun,Lizhi Zhang
Cr(III)-organic complexes removal from wastewater is challenging to decompose the complexes without producing toxic Cr(VI). Herein we demonstrated that oxalated zero-valent iron (Ox-ZVI) could one-step decomplex 95.4% of Cr(III)-EDTA with 94.2% removal of total Cr and 60.5% removal of TOC without generating Cr(VI) at pH 6.0. Ox-ZVI with FeC 2 O 4 shell preferred to adsorb and activate O 2 to produce more reactive species than ZVI with iron oxide shell, while the generated 1 O 2 could selectively break the Cr-O and Cr-N bond to precisely decomplex Cr(III)-EDTA without producing Cr(VI). The released Cr(III) was in-situ precipitated on the surface of ZVI in Cr(OH) 3 form. Interestingly, •OH preferred the effective degradation of the released EDTA ligand to the oxidation of the chelated Cr(III) at pH 6.0. This study offers a green and facile method for the Cr(III)-organic complexes treatment, and also sheds light on the importance of reactive species adjustment for the precise pollutant control.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Wenjun Zhu,Shuai Zhang,Xiaohua Zuo,Xin Li,Xiangyi Deng,Guanghui Wang,Deng Ding,Chunlei Wang,JunTao Yan,Xiaobo Wang
The magnetic CuFeO 2 anchored on nitrogen-doped porous carbon (CuFeO 2 /NC) hybrid catalysts were further synthesized via hydrothermal reaction without the addition of a chemical reductant. The systematic CuFeO 2 /NC with larger specific surface areas (SSAs) and abundant active sites exhibited strong adsorption ability and great catalytic performance towards activating peroxymonosulfate (PMS) for sulfamethoxazole (SMX) removal. It was noted that 18 mg/L SMX was completely removed after 40 min of pre-adsorption and 30 min of oxidative degradation in CuFeO 2 /NC and PMS system. The degradation rate constant ( k ) was calculated by fitting as 0.166 min −1 , being about 7.9 times that in the CuFeO 2 and PMS system (0.021 min −1 ). The SO 4 · - ,·OH, and 1 O 2 as the dominant reactive oxygen species (ROSs) contributed to sulfamethoxazole degradation. The N species, active oxygen and the redox cycles of Cu(Ⅱ)/Cu(Ⅰ) and Fe(Ⅲ)/Fe(Ⅱ) were confirmed to play a vital role in the activation of PMS for the generation of ROSs. Based on the LC-MS analysis, the possible degradation routes of SMX in the PMS activation system by CuFeO 2 /NC were proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Siqi Tong,Dan Chen,Xinbai Jiang,Zhixiang Xu,Xiaodong Liu,Jinyou Shen
A novel composite biochar synthesized from Fenton sludge (FS) and sewage sludge (SS) was employed to catalyze persulfate for the removal of 1-H-1,2,4-triazole (TZ). The optimized conditions for the synthesis and operating process were identified through response surface methodology as follow: SS/FS mass ratio = 5:1, catalyst dosage = 0.9 g L −1 and PDS concentration = 0.5 g L −1 . The removal efficiencies of TZ, TOC and organic nitrogen were found to be as high as 97.6%, 80.33% and 100%, respectively, with the addition of Fe 3 O 4 -doped biochar in persulfate catalytic system. Besides, Fe 3 O 4 -doped biochar exhibited superior stability and tolerance to wide range of pH (2–12), temperature (15–45 °C) and co-existing substrate. The reactive oxygen species, which resulted in the catalytic degradation of TZ followed the order of SO 4 ∙− > ∙OH > O 2 ∙− > 1 O 2 , were identified by electron spin resonance and quenching tests. It demonstrated that the radical pathway accomplished with non-radical pathway contributed to the enhanced degradation of TZ, which was further identified by electrochemical experiments. Moreover, the possible degradation pathway of TZ was ascertained and proposed through DFT calculation and LC-MS analysis. These findings illustrated that the novel magnetic biochar would be a promising persulfate catalyst for the treatment of refractory organic matters. In addition, it also provided a new alternative method for the resource utilization of FS and SS.
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ADVANCED POWDER TECHNOLOGY
·
2023
·
IF 5.2
Tingting Mao,Qihui Ding,Qian Shan,Xiaochen Chang,Wei Wu
In this paper, a magnetic ferrosoferric oxide/two-dimensional molybdenum disulfide (Fe 3 O 4 /2D-MoS 2 ) composite material was successfully prepared by combining liquid phase exfoliation and in-situ liquid phase co-precipitation methods with scalable and facile characteristics and applied to catalyze the degradation of tetracycline (TC) during the peroxymonosulfate-based advanced oxidation processes (PMS-AOPs), which is a typical and widely used antibiotic. The morphology and crystallinity of the composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction, respectively. And its BET surface area was tested by N 2 adsorption and desorption curves. For the PMS-AOPs, the effects of iron loading, different systems, initial concentration of pollutants, dosage of the composites, concentration of peroxymonosulfate (PMS) and solution initial pH on the removal of TC were researched in details. The results showed that it could reach 89.0% degradation efficiency within 90 min for 50 mg/L TC with the as-prepared composites as catalyst, showing good catalytic performances. In addition, the mechanisms of the reaction were deduced by quenching experiments and X-ray photoelectron spectroscopy analysis. It was turned out that the as-synthsized material has a broad applying prospect in PMS-AOPs.
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Journal of Cleaner Production
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2023
·
IF 11.1
Jiaqi Bu,Hongru Jiang,Tianhao Li,Chengyun Zhou,Shian Zhong
A laboratory-scale electrochemical reaction tank was self-designed for the degradation of sulfamethoxazole (SMZ). Coupling electrocatalysis (EC) with personoxysulfate (PMS) and chloride ion (Cl − ), the degradation system of EC + PMS + Cl was established. The degradation efficiency of the EC + PMS + Cl system for SMZ (10 mg/L) reached 100% within 20 min, and the degradation process of SMZ conforms to the first-order kinetics. EC + PMS + Cl system also has good degradation efficiency for other organic pollutants or polysaccharide wastewater (real wastewater) from coriolus versicolor. The electrochemical performance test shows that TiO 2 /RuO 2 –IrO 2 electrode not only has a good chlorine evolution effect but also has good stability. •OH and active chlorine play a major role in the degradation system. Theoretical calculation (DFT) and XPS analyses confirm that the RuO 2 –IrO 2 site as an active center activates PMS and Cl − into active oxygen and active chlorine, and the TiO 2 site as an active center activates molecular oxygen into active oxygen. The results of liquid chromatography and mass spectrometry (LC-MS) and Toxicity Estimation Software Tool (TEST) showed that the water quality of SMZ after 20 min of degradation was almost harmless. Therefore, this research work will provide a new vision for the electrocatalytic degradation of organic wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Chen Wang,Huanran Liu,Peng Sun,Jingjing Cai,Mingxing Sun,Haijiao Xie,Guoqing Shen
Single-atom dispersed catalysts (SACs) have gained considerable attention in organic contaminants remediation due to their superior reactivity and stability. However, the complex and costly synthesis processes limit their practical applications in environmental protection. Herein, a facile and cost-effective single-atom iron catalyst (Fe-SA/NC) anchored on nitrogen-doped porous carbon was first fabricated by using waste biomass as a carbon source. The Fe-SA/NC catalyst exhibited outstanding performance with a high turnover frequency of 1.72 min −1 toward antibiotics degradation via peroxymonosulfate activation . ECOSAR program and algae growth experiments demonstrated that the byproducts produced during the sulfamethoxazole degradation process were not detrimental to the aquatic environment. Radical quenching and electron paramagnetic resonance experiments revealed that Fe-SA/NC remarkably promoted 1 O 2 production in PMS-assisted reaction, and thus 1 O 2 contributed as much as 78.77% to sulfamethoxazole degradation. As indicated by experiment and density functional theory (DFT) calculations, FeN 2 O 2 configuration serves as the active site. DFT calculations further presented the most rational generation route of 1 O 2 as PMS→OH* →O* → 1 O 2 . We also designed Fe-SA/NC embedded spherical pellets for contaminants elimination at the device level. This study offers new insights into the synthesis of SACs from waste biomass and their practical application in environmental remediation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Haoyu Luo,Yi Wan,Jie Li,Yuhao Cai,Zhi Dang,Hua Yin
In wastewater treatment by persulfate-based advanced oxidation processes (PS-AOPs), electron-deficient aromatic pollutants (EDAPs) are refractory to nonradical pathway. To explore an efficient degradation pathway for EDAPs, Mg x Cu-biochar (BC) (x = 0.5, 1, 1.5) activated peroxydisulfate (PDS) was developed, which could trigger reductive species (•H) to reduce EDAPs first, and subsequently facilitate electron-transfer degradation of reduced intermediates. The roles of Mg-doping in Mg x Cu-BC to promote PDS activation and 2,4-dibromophenol (DBP) degradation were investigated. The mechanisms were then explored via electron paramagnetic resonance (EPR), chemical probes and Density Functional Theory (DFT) calculations. The results showed that Mg-doping improved metal-support interactions (MSIs) of Mg x Cu-BC, inducing •H formation via electron transfer from Cu atoms during PDS activation, which was thermodynamically favorable. The degradation rate of DBP ( k obs , 0.0494 min –1 ) and Br – release (5.35 mg L –1 ) in Mg 1 Cu-BC systems were more 31 and 33 times than that in Cu-BC/PDS system, respectively. The degradation mechanism of •H-enhanced electron transfer processes was that •H attacked one Br group of DBP, and then debrominated intermediates were mineralized by electron transfer processes in the Mg 1 Cu-BC/PDS system. Overall, this study reports a novel pathway in PS-AOPs for selective degradation of EDAPs in wastewaters.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiupeng Yue,Yongping Shan,Wentao Jiao,Kai Shen,Yaping Zhang
Electrokinetic (EK) delivery followed by thermal activated peroxydisulfate (PS) has turned out to be a potential in situ chemical oxidation technology for soil remediation , but the activation behavior of PS in an electrical coupled thermal environment and the effect of direct current (DC) intervention on PS in heating soil has not been explored. In this paper, a DC coupled thermal activated PS (DC-heat/PS) system was constructed to degrade Phenanthrene (Phe) in soil. The results indicated that DC could force PS to migrate in soil, changing the degradation rate-limiting step in heat/PS system from PS diffusion to PS decomposition, which greatly accelerated the degradation rate. In DC/PS system, 1 O 2 was the only reactive species directly detected at platinum (Pt)-anode, confirming that S 2 O 8 2- could not directly obtain electrons at the Pt-cathode to decompose into SO 4 •- . By comparing DC/PS and DC-heat/PS system, it was found that DC could significantly promote the conversion of SO 4 •- and •OH generated by thermal activation of PS to 1 O 2 , which was attributed to the hydrogen evolution caused by DC that destroys the reaction balance in system. It was also the fundamental reason that DC leaded to the reduction of oxidation capacity of DC-heat/PS system. Finally, the possible degradation pathways of phenanthrene were proposed on the basis of seven detected intermediates.
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高影响因子
Processes
·
2023
·Vol. 11
·期 3
·903
·
IF 3.5
Yajie Wang,Xin Dong,Chengfeng Liu,Peng Cheng,Gilles Mailhot
The decolorization of azo dye Orange II using a UVA-Fe3+-PMS-oxalate system was studied. A series of experiments was performed to investigate the effects of several variables, including the pH, PMS dosage, Fe3+concentration, oxalate concentration, and coexisting anions. The results revealed that a lower pH facilitated the decolorization, and relatively high decolorization efficiency (97.5%) could be achieved within 5 min at pH 3.0. The electron paramagnetic resonance (ESR) and radical quenching experiments revealed that SO4•−played a crucial role in the decolorization of Orange II (85.8%),•OH was of secondary importance (9%), and1O2made a small contribution to the decolorization (5.2%). Furthermore, the formation of•OH in the experimental system strongly depended on HO2•/O2•−. These reactive oxidants were able to directly attack the azo bond of the luminescent group in Orange II and initiate the decolorization process. The efficient UVA-Fe3+-PMS-oxalate system showed great application potential in the treatment of wastewater contaminated by azo dyes.Keywords:PMS activation;Orange II;decolorization;UVA irradiation;Fe3+-oxalate complexes
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