SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yang Zong,Wenjie Ji,Yu Xie,Deli Wu
The mineralization of organic pollutant by O 3 is prone to be restricted by the accumulative production of oxalate (OA) that is recalcitrant to the attack of hydroxyl radical ( OH). Herein, it was interestingly found that the presence of 0.5 mM Ni(II) enhanced the mineralization efficiency of EDTA by O 3 under alkaline conditions by 22.8%, with the promoting effect of Ni(II) augmented as the increasing loading of Ni(II). Based on the results from scavenging experiment, chemical probe detection and XPS characterization, it was verified that except for the commonly recognized reactive oxidants (i.e., OH and O 3 ) in EDTA mineralization, the overlooked Ni(III) species (i.e., NiOOH) also played an indispensable role in enhancing the mineralization of EDTA. The Ni(III) species was formed via the oxidation of decomplexed Ni(II) by OH and in turn collaborated with OH to decompose EDTA. More importantly, the generated Ni(III) species exerted higher affinity towards OH and O 3 -resistent oxalate, hence elevating EDTA mineralization. This study elucidated the significant role of Ni(III) species in promoting the mineralization efficiency of EDTA, and also proposed a new insight into elevating the treatment performance of ozonation via the collaborative oxidation mechanism-co-mediated by OH and Ni(III) species.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
RADIATION PHYSICS AND CHEMISTRY
·
2021
·
IF 2.858
Zhuhao Huo,Siqi Wang,Qi Zou,Haiyang Shao,Gang Xu
Atenolol (ATE) is one of the most frequently detected persistent emerging pollutants in wastewater. The performance of electron beam irradiation (EB) in decomposition and mineralization of ATE in aqueous solutions was evaluated. The results showed the radiolytic degradation of ATE was efficient with a degradation rate of 97% for 100 mg L −1 under 5 kGy. The degradation kinetic nicely followed pseudo first-order kinetic model. The effect of saturated solutions of N 2 O, O 2 , N 2 , and tert -butanol were studied, which elucidated that • OH played a major role and • H and e − aq played a minor role in ATE degradation. The presence of NO 2 − , NO 3 − , CO 3 2− , Cl − and fulvic acid significantly affected the degradation of ATE. The degradation of ATE was seriously inhibited in municipal wastewater compared with surface water and ultrapure water. The TOC removal efficiency of ATE by electron beam alone was relative low about 3% in 10 kGy, which was improved to 20% combining with 10 mM K 2 S 2 O 8 due to reaction between SO 4 •− radical and intermediates. The main radiolytic degradation pathways of ATE involved breakage of the ether bond in branched chain, cleavage of the isopropyl group and the carboxamide group, and attack to the aromatic ring by • OH radical. The potential active sites probed by Fukui function and Dual descriptor were consistent with the results of intermediates. This study envisaged a promising strategy to treat wastewater containing recalcitrant contaminants.
研究领域:
环境科学
·
放射化学
·
水处理工程
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Hongwei Luo,Ying Cheng,Yifeng Zeng,Kai Luo,Dongqin He,Xiangliang Pan
Despite the previous success of MoS 2 /Fe 2+ /PMS process in detoxifying organic micropollutants, the drawback of requiring a narrow range of working pH limits its practical application. In this study, a class of commercial MoS 2 nanoparticles was introduced as a co-catalyst to facilitate the PMS activation by Fe 3+ ion. Results showed that the MoS 2 /Fe 3+ /PMS system over a wide range of pH values (3.0–9.0) achieved above 90% of removal efficiency for seven pollutants (chloramphenicol, tetracycline, ciprofloxacin, benzoic acid , rhodamine B, sulfadiazine, and bisphenol A) within 60 min of reaction time. The addition of MoS 2 greatly accelerated the reduction of Fe 3+ to Fe 2+ and the decomposition of PMS, thereby resulting in increased mineralization efficiency of pollutants. The generation of Mo 6+ ion and Mo 6+ peroxo-complexes also contributed to the promoting effect. Both sulfate (SO 4 − ) and hydroxyl ( OH) radicals were identified in MoS 2 /Fe 3+ /PMS system but SO 4 − was the dominant reactive oxidant. Chloride ion (Cl − ) showed an enhanced effect on degradation, while bicarbonate ion (HCO 3 − ) showed an inhibitory effect. Economic analysis was conducted by using an electrical energy per order (EE/O) approach. The above research findings suggest that the MoS 2 /Fe 3+ /PMS system is a promising oxidation technology owing to its efficient removal of various pollutants over a wide pH range.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jun Zhang,Songying Qu
Here we investigated the synergetic multiple free radicals (atomic hydrogen (H*), superoxide anion (•O 2 − ), and hydroxyl radicals (•OH)) in enhancing removal efficiencies of the halogen organic pollutants , such as p-chlorophenol (4-CP). A TiO 2 photoanode and a palladium and carbon layer co-modified Cu/Cu 2 O/CuO (Cu x O@C/Pd) photocathode were combined to construct a photoelectrocatalytic platform that enabled the synchronous production of multiple free radicals. It was found that the conversion and mineralization rates of 4-CP were up to ∼0.044 min −1 and ∼71.3% respectively, representing an increase of ∼4.3 times and ∼2.1 times compared to conventional •OH mediated oxidation . Theoretical calculations and experiments indicated that the conversion barrier of 4-CP was significantly reduced through the redox synergies of H* and •OH and the simultaneous nucleophilic-electrophilic addition of •O 2 − effectively inhibited the accumulation of benzoquinone intermediates. This work is beneficial for the study and application of advanced oxidation processes mediated by multiple free radicals.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Xukai Li,Weirui Chen,Yiming Tang,Laisheng Li
Fe-MCM-48 catalyst with a three-dimensional cubic pore structure was directly synthesized via a hydrothermal method, and the mineralization efficiency of diclofenac (DCF) in the catalytic ozonation process (Fe-MCM-48/O 3 ) was assessed. X-ray diffraction (XRD), N 2 adsorption desorption, transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) characterizations revealed that Fe existed in the framework of MCM-48, and Fe-MCM-48 possessed a large surface area and a highly ordered cubic mesoporous structure, which could accelerate reactants and products diffusion. Regarding mineralization efficiency, the addition of Fe-MCM-48 significantly improved total organic carbon (TOC) removal, and approximately 49.9% TOC were removed through the Fe-MCM-48/O 3 process at 60 min, which was 2.0 times higher than that in single ozonation. Due to this catalyst's superior structure, Fe-MCM-48 showed the better catalytic activity compared with Fe-MCM-41 and Fe loaded MCM-48 (Fe/MCM-48, Fe existed on the surface of MCM-48). DCF removal in the Fe-MCM-48/O 3 process was primarily based on ozone direct oxidation. The improvement of mineralization efficiency was attributed to the function of generated hydroxyl radicals (•OH), which indicated that the presence of Fe-MCM-48 accelerated ozone decomposition . Moreover, the negatively charged surface of Fe-MCM-48 and the proper pH value of the DCF solution played an essential role in OH generation.
研究领域:
环境科学
·
催化材料
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiaoying Chen,Run Zhuan,Jianlong Wang
In this study, the degradation of norfloxacin was investigated by ionizing radiation combined with Fenton-like oxidation in order to enhance the degradation and mineralization of norfloxacin. The result showed that the removal efficiency of norfloxacin was 100%, 81.8%, 64.5%, 51.9%, and 45.6% at 0.4 kGy radiation when its concentration was 5, 10, 20, 30, and 40 mg/L. Norfloxacin could be completely degraded over pH range of 3.06–10.96 at 2 kGy radiation. The presence of inorganic anions had obvious influence on the degradation of norfloxacin, which decreased from 89.4% to 59.0%, 76.9%, 86.9%, 88.7% and 83.9% in the presence of 10 mmol/L CO 3 2– , HCO 3 – , NO 3 – , SO 4 2 – , Cl – , HPO 4 2 – . The removal efficiency of norfloxacin decreased from 100% to 11.8%, 27.6% and 89.3% in the presence of peptone, glucose, and humic acid . The addition of Fenton-like catalysts, such as magnetite and goethite , could improve the mineralization ratio of norfloxacin because they could decompose hydrogen peroxide generated during the radiation process, to form hydroxyl radicals , leading to the enhancement of removal efficiency of norfloxacin. Finally, the intermediate products of norfloxacin degradation were analyzed by ultra-performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-QTOF), and the degradation pathway was proposed.
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
Journal of Water Process Engineering
·
2020
·
IF 3.465
Xuerui Bai,Maiqian Nie,Zhenjun Diwu,Hongyun Nie,Yan Wang
Pseudomonas stutzeri N2 and Rhodococcus qingshengii FF were combined to enhance phenol degradation, and the interaction mechanism of microorganisms was investigated. The cells in the culture of mixed strain degrading 1000 mg/L phenol exhibited a rapid growth and proliferation, and the maximum cell density of mixed strain was 34.6 ± 0.3% and 60.8 ± 0.2% higher than the single strain N2 and strain FF respectively. The degradation of phenol by mixed strain was completed within 24 h, and the phenol mineralization efficiency was up to 84.9 ± 0.4%. In addition, two ring-cleavage products of catechol accumulating from the culture of mixed strain were markedly reduced. Through the analysis of intermediates and functional groups, the enhanced phenol degradation by mixed strain was found to mainly depend on the synergistic effect of strain N2 served as an oxidant and strain FF acted as a reductant. Based on the synergic mechanism, the mixed strain might be used as a promising bacterial agent for removing phenolic compounds from the industrial wastewater.
研究领域:
环境生物学
·
微生物学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 19
·28525-28537
·
IF 0
Qiu Rui,Chen Aiyin,Zhang Peng,Tang Xuejiao,Wang Cuiping,Sun Hongwen
Herein, novel catalysts of Fe-containing zeolite-A (Fe/zeolite-A) were synthesized by exchanging iron ions into zeolite-A framework, and short-chain organic acids (SCOAs) were employed as chelating agents. Reactive Brilliant Blue KN-R (KN-R) was used as a model pollutant to evaluate the performance of these catalysts based on the heterogeneous Fenton reaction. The results showed that Fe-OA/3A, which applied zeolite-3A as the supporter and oxalic as the chelating agent, presented the most prominent KN-R decolorization efficiency. Under the initial pH of 2.5, 0.4 mM KN-R could be totally decolorized within 20 min. However, the mineralization efficiency of KN-R was only 58.2%. Therefore, anthraquinone dyes were introduced to modify zeolite-3A. As a result, the mineralization efficiency of KN-R was elevated to 92.7% when using Alizarin Violet (AV) as the modifier. Moreover, the modified catalysts exhibited excellent stability, the KN-R decolorization efficiency could be maintained above 95.0% within 20 min after operating for nine cycles. The mechanism revealed that the Fe(II)/Fe(III) cycle was accelerated by AV-modified catalyst thus prompting the KN-R decolorization in Fenton-like system. These findings provide new insights for preparing catalysts with excellent activity and stability for dye wastewater treatment.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yawei Feng,Hao Li,Lili Ling,Sa Yan,Donglai Pan,Hao Ge,Hexing Li,Zhenfeng Bian
The introduction of a piezoelectric field has been proven a promising method to enhance photocatalytic activity by preventing photoelectron–hole recombination. However, the formation of a piezoelectric field requires additional mechanical force or high-frequency ultrasonic baths, which limits its potential application on industrial scale. Therefore, it is of great practical significance to design the catalyst that can harvest the discrete energy such as the fluid mechanical energy to form the electric field. Herein, PZT/TiO2 catalyst with a core–shell configuration was prepared by a simple coating method. By collecting the mechanical energy of water, an internal piezoelectric field was induced. Under 800 rpm stirring, transient photocurrent measured on PZT/TiO2 electrode is about 1.7 times higher than that of 400 rpm. Correspondingly, the photocatalytic degradation rate and mineralization efficiency of RhB, BPA, phenol, p-chlorophenol much improved, showing the promoting effect of piezoelectric field generated directly from harvesting the discrete fluid mechanical energy.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xubin Qian,Kefu Peng,Lei Xu,Shaoyu Tang,Weilai Wang,Min Zhang,Junfeng Niu
The global detection and potential harm of pharmaceuticals and personal care products (PPCPs) call for the effective decomposition technology. In this study, the modified β-PbO 2 anodes with different hydrophobicity (Ti/SnO 2 -Sb/La-PbO 2 , Ti/SnO 2 -Sb/La-PbO 2 -PTFE and Ti/SnO 2 -Sb/La-PbO 2 -PVDF) were prepared to decompose aqueous PPCPs, i.e. isoniazid, methotrexate, carbamazepine, sulfamethoxazole and ibuprofen. PTFE and PVDF modification improved the physical property, electrochemical property, stability and safety of β-PbO 2 electrode. Moreover, Ti/SnO 2 -Sb/La-PbO 2 -PVDF had the highest oxygen evolution potential (1.95 V vs. SCE), the largest electroactive area (88.85 cm 2 ), the highest HO • production rate (10.44 mM min −1 m −2 ) and the best degradation performance for all the five PPCPs. The hydrophobic surface increased the proportion of free HO • , resulting in higher radical utilization rate and better degradation performance. The excessive hydrophobicity could decrease the degradation performance of PPCPs with high log K ow due to the relatively large hydrophobic force zone. Furthermore, the hydrophobicity enhanced the mineralization (current) efficiency of isoniazid, and its electrochemical degradation mechanism on Ti/SnO 2 -Sb/La-PbO 2 -PVDF was thoroughly proposed. These results demonstrated that Ti/SnO 2 -Sb/La-PbO 2 -PVDF anode exhibited a good application prospect in treating wastewater containing PPCPs.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Weirui Chen,Jinxin Xie,Xukai Li,Laisheng Li
The low efficiency of peroxone (O 3 /H 2 O 2 ) at acidic and neutral pH restrained its application in water purification . To overcome this shortcoming, CeO X @SiO 2 with large surface area, abundant surface oxygen vacancies (V o ), Lewis sites (L sites) and high Ce(III)/Ce(IV) ratio were synthesized to change the traditional electron transfer pathway between O 3 and H 2 O 2 . V o was facile in absorbing H 2 O 2 to form V o -H 2 O 2 and L sites were capable of absorbing O 3 to form L-O 3 . The electron at V o could be donated to V o -H 2 O 2 and generate V o -HO 2 − , which then effectively triggered the decomposition of L-O 3 at CeO X @SiO 2 ’s interface and O 3 in bulk solution. The electron transfer at the solid-liquid interface with the help of Ce 3+ /Ce 4+ redox cycle and V o was pH independent and different from the traditional electron transfer of peroxone reaction. Nitrobenzene (NB) mineralization was promoted to 92.5% in CeO X @SiO 2 -peroxone, but only 63.8% TOC was removed in tradition peroxone process. Moreover, CeO X @SiO 2 -peroxone had a wide pH application range. NB’s degradation in CeO X @SiO 2 -peroxone process followed the co-oxidation mechanism of superoxide free (•O 2 − ) and hydroxyl radical (•OH). The finding of this study could broaden the popularization of peroxone in water treatment and provided a strategy for catalyst design.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Lele Zhou,Zhizhang Shen,Shuibing Wang,Junxian Gao,Lingling Tang,Ji Li,Yuming Dong,Zhenyu Wang,Jinze Lyu
We constructed quantum-scale catalytic regions on the surfaces of TiO 2 nanoparticles by loading TiO 2 quantum dots (QDs) with a two-step method. The removal rate and mineralization efficiency of toluene were measured and then used in evaluating the oxidation performance of the prepared samples. A home-built atmospheric surface photovoltage spectrometer and X-ray photoelectron spectrometer were used in analyzing band alignment across the interface between TiO 2 QD and TiO 2 particle and the transfer of charge carriers at the surface. Results showed that an upward band bending formed from the TiO 2 particle to the TiO 2 QD and promoted the accumulation of holes at the QD side. Moreover, the QD and surrounding substrate TiO 2 formed a quantum-scale catalytic region, improving the reaction probability of electron-hole pairs and corresponding intermediates. The mineralization efficiency of toluene in QD-loaded TiO 2 reached 95.8%. The synthetic method is green and simple, showing potential in scale production and industrial application.
研究领域:
材料科学
·
环境科学
✓ 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）