JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Meesam Ali,Muhammad Tariq,Yong Sun,Jingyao Huang,Xiaogang Gu,Sana Ullah,Muhammad Asif Nawaz,Zhengyuan Zhou,Ali Shan,Muhammad Danish,Shuguang Lyu
Carbonaceous materials (CMs) have been applied extensively for enhancing the catalytic performance of environmental catalysts, however, the self-catalytic mechanism of CMs for groundwater remediation is rarely investigated. Herein, we unveiled the catalytic ability of various CMs via Fe(III) reduction through polyvinyl alcohol-coated calcium peroxide nanoparticles (PVA@nCP) for trichloroethylene (TCE) removal. Among selected CMs (graphite (G), biochar (BC) and activated carbon (AC)), BC and AC showed enhancement of TCE removal of 89% and 98% via both adsorption and catalytic degradation. BET and SEM analyses showed a higher adsorption capacity of AC (27.8%) than others. The generation of solution-Fe(II) and surface-Fe(II) revealed the reduction of Fe(III) on CMs-surface. The role of O-containing groups was investigated by the FTIR technique and XPS quantified the 52% and 57% surface-Fe(II) in BC and AC systems, respectively. EPR and quenching tests confirmed that both solution and surface-bound species (HO•, O 2 − • and 1 O 2 ) contributed to TCE degradation. Acidic pH condition encouraged TCE removal and the presence of HCO 3 − negatively affected TCE removal than other inorganic ions. Both schemes (PVA@nCP/Fe(III)/BC and PVA@nCP/Fe(III)/AC) exhibited promising results in the actual groundwater, surfactant-amended solution, and removal of other chlorinated-pollutants, opening a new direction towards green environmental remediation for prolonged benefits.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Guanjun Wang,Dongdong Ge,Lu Bai,Yanting Dong,Chang Bian,Jiajia Xu,Nanwen Zhu,Haiping Yuan
Sludge dewatering , as one of the most important steps of sludge treatment , can facilitate transportation and improve disposal efficiency by reducing the volume of sludge . This study investigated the effects of electrolysis-activated persulfate oxidation on improving sludge dewaterability. The results indicated that the sludge capillary suction time (CST) and water content of dewatered sludge cake (Wc) reduced from 93.7 s and 87.8% to 9.7 s and 68.3% respectively at the optimized process parameters: electrolysis voltage of 40 V, electrolysis time of 20 min, and 1.2 mmol/g TS S 2 O 8 2− . Correlation analysis revealed that the enhancement of sludge dewaterability was closely associated with the increased floc size and zeta potential , decreased protein content in three-layers extracellular polymeric substances (EPS) and viscosity ( R = −0.868, p = 0.002; R = −0.703, p = 0.035; R ≥ 0.961, p < 0.001; R = 0.949, p < 0.001). Four protein fluorescence regions in EPS were analyzed by three-dimensional excitation-emission matrix parallel factor (3D-EEM-PARAFAC). The protein secondary structure was changed after the treatment, and the reduction of α-helix/(β-sheet + random coil) indicated that more hydrophobic sites were exposed. Analysis by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR) and rheological test demonstrated that the hydrophilic functional groups of the sludge were decreased and the sludge mobility was significantly enhanced after the treatment with electrolysis-activated persulfate oxidation. Moreover, bound water was converted to free water during SO 4 · − and ·OH generated by electrolysis-activated persulfate degraded EPS and attacked sludge cells. Meanwhile, scanning electron microscopy (SEM) images revealed that the treated sludge formed porous channel structures, which promoted the flowability of the water. These findings provide a new insight based on electrolysis-activated persulfate oxidation in sludge treatment for enhancing sludge dewaterability.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Chunxiang Wan,Yuzhen Pan,Zhen Chen,Jinglu Hu,Zhe Zhang,Yawen Sun,Wei Ma
The application of Zinc oxide has drawn great attention in bacterial inhibition and contaminant degradation field in recent years. The internal structure and the morphology of the material was characterized by XRD , XPS , SEM , TEM. The dopant of 1 wt% graphene oxide（GO） and 30 wt% Al 2 O 3 shows excellent piezocatalytic and antibacterial ability. Application potential of the material is investigated by the degradation of RhB and the inhibition of Bacillus. It is found that the RhB solution can be degraded 92.5% by ZA-GO in 15 min, while ZnO can degrade 64.2%. It shows superior catalytic behavior in successive experiments of degradation of RhB without obvious decrease in efficiency. The quenching experiment combined with ESR spectrum demonstrate that both •O 2 - and •OH radicals were generated, while •OH did the most damage. Bacterial inhibition tests have also proven that the generation of reactive oxygen species cause the bacteria inactivated. In this work, a novel composite ZnO-Al 2 O 3 /GO has been successfully prepared based on mechanical synthesis method. Graphene oxide has higher mechanical strength and higher specific surface area. Zn ions doping carbon materials not only increases its stability, but also promotes its conductivity. The doping of Al atoms effectively reduce the work function of ZnO. Graphene oxide together with alumina coordinate the band gap of piezoelectric materials ZnO and the catalytic reaction efficiency was dramatically enhanced. What’s more, this work provides a facile approach eliminated the use of solvents and organic reagents, ensuring greater environmental safety. The novel zinc oxide matrix composites are depicted as a promising candidate to be used as intelligent antibacterial agent and alleviate environmental pollution.
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Advanced Healthcare Materials
·
2021
·Vol. 10
·期 18
·2100518
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IF 9.933
Xingyi Xu,Rongyuan Zhang,Xianfeng Yang,Yao Lu,Zhongmin Yang,Mingying Peng,Zhijun Ma,Ju Jiao,Lihua Li
Triple-negative breast cancer (TNBC) exhibits aggressive behavior and high levels of metastasis owing to its complex heterogeneous structure and lack of specific receptors. Here, tumor cell membrane (CM)-coated bismuth/manganese oxide nanoparticles (NPs) with high indocyanine green (ICG) payload up to 50.6 wt% (mBMNI NPs) for targeted TNBC therapy are constructed. The extra-high drug load Bi@Bi 2 O 3 @MnO x NPs (honey-comb like structure) are formed by Kirkendall effect and electrostatic attraction. After modified with CM, they can home into tumor sites precisely, where they respond to internal overexpressed glutathione (GSH), releasing Mn 2+ for chemodynamic therapy (CDT) with GSH depletion, while H 2 O 2 degrades into O 2 enabling relief of tumor hypoxia. In response to external near-infrared irradiation, mBMNI NPs intelligently generate vigorous heat and single oxygen ( 1 O 2 ) for photothermal therapy (PTT) and photodynamic therapy (PDT) owing to high load. Importantly, O 2 production and GSH consumption during the internal response reinforce external PDT, while the heat generated through PTT during the external response promotes internal CDT. The honeycomb-like structure with high ICG load and mutual reinforcement between internal and external response results in excellent therapeutic effects against TNBC.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Zhuofan Huang,Qintie Lin,Nan Cai,Qingsong Weng,Jingwei Xu,Shuchai Gan,Chao Chen,Quanfa Zhong,Hengyi Fu,Yuejie Xia,Pengran Guo
In this study, CuO/HNTs were applied to activate persulfate (PS) to firstly degrade and mineralize TCS. The morphology, crystal structure, specific surface and surface composition were characterized by SEM, TEM, BET, XRD and XPS. The experimental parameters were optimized with 0.2 g/L CuO/HNTs and 2 mM PS. TCS was totally removed in 180 min under optimized conditions. The mechanism study using the quenching reaction, EPR, XPS and electrochemistry demonstrated that even radical reactions (•OH and O 2 •- ) pathway existed; the nonradical mechanism ( 1 O 2 and surface electron transport) was dominant to the efficient TCS degradation. Using FT-ICR MS, the degradation intermediates were identified, and transformation pathways were proposed. The degradation intermediate studies indicated that TCS began to break from the aromatic ring containing monochlorine, and the Cl functional group was gradually substituted. CO 2 and H 2 O were generated with breaking of ether bonds. The toxicity of the solution was also evaluated by the survival rate of the luminescent bacteria, and the toxicity of the solution decreased overall. A stability study showed that CuO/HNTs retained good crystal structure and degradation efficiency even after 5 cycles.
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Journal of Materials Chemistry B
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2021
·Vol. 9
·期 37
·7686-7697
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IF 6.331
Jingmei Guo,Yue Xu,Miaodeng Liu,Jian Yu,Hongye Yang,Wenlong Lei,Cui Huang
The validity and biocompatibility of irrigating agents are imperative for the success of root canal therapy. The imperfections in the currently available irrigants highlight the fact that more advanced technologies and strategies are required for complete disinfection in endodontic treatments. In the present study, a Fenton reaction-enhanced antimicrobial sonodynamic therapy (SDT) platform was fabricated for root canal disinfection. Firstly, mesoporous silica nanoparticles (MSNs) were synthesized, grafted with an amino group and then conjugated with sonosensitizer protoporphyrin IX (PpIX). Iron ions were then anchored (M@P-Fe) to initiate a Fenton reaction. Nanoparticle characterization by size and zeta potential measurements, scanning electron microscopy, transmission electron microscopy and thermogravimetric analysis confirmed that the platform was successfully developed. Reactive oxygen species (ROS) generation assessment, methylene blue degradation and electron spin resonance assays illustrated upon ultrasound (US) irradiation, that augmented ROS, can be produced by US activated PpIX and iron mediated Fenton reactions from low concentration H2O2 (0.01%). In vitro anti-Enterococcus faecalis efficacy was demonstrated by growth curve and colony forming unit measurements. Confocal laser scanning microscopy and scanning electron microscopy observations illustrated the effectiveness of the platform on in situ biofilm eradication in root canal. Owing to the stronger oxidizing capability and short lifetime of ROS, the Fenton reaction-enhanced SDT can induce detrimental oxidative damage to bacteria upon activation of US while avoiding nonspecific toxicity to cells, which was verified by cytotoxicity evaluations using CCK-8 assay and morphology observation of MC3T3-E1 cells. Compared to commonly used NaClO, this nanoplatform displayed desirable anti-bacterial, anti-biofilm abilities and better biocompatibility. These results highlight that the integrated M@P-Fe + US + H2O2 platform is a promising candidate for US enhanced root canal irrigation and disinfection.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiaona Dong,Xiaoxue Yang,Sheng Hua,Ziqian Wang,Tianming Cai,Canlan Jiang
The continuous accumulation of triphenyl phosphate (TPHP) in soil poses a potential threat to human health. Persulfate-based advanced oxidation processes (SR-AOPs) are promising soil remediation technologies. Naturally occurring soil constituents could interact with persulfate (PS) during soil remediation by SR-AOPs. However, the production and transformation of reactive oxygen species (ROS) by synthetic reactions between PS and different soil constituents, as well as their roles in the pollutants degradation, are still largely unknown. This study systematically investigated the generation of ROS and their roles in degradation of TPHP in soil constituents activated PS process and in soil constituents-heat (50 °C) co-activated PS process. Comprehensive studies including ROS identification, electron paramagnetic resonance analysis, and ROS-generated model systems were carried out. An appreciable degradation rate of TPHP (~21.9%) in soil-PS system and the significant discrepancy in degradation rate (69.0–97.0%) in heat-soil-PS systems with three different soils suggested that soil constituents exhibited complex effects on the activation of PS. The Fe/Mn-minerals in soil effectively activated PS and facilitated TPHP degradation. Specially, the iron redox cycle (Fe(II) ↔ Fe(III)) plays a key role in ROS generation. Small molecular soil organic matter (SOM) rapidly consumed the produced ROS which led to their mineralization, while the remaining macromolecular SOM became more hydrophilic by interaction with ROS. SO 4 •− , •OH, and 1 O 2 played major roles directly in TPHP degradation, while O 2 •− could not degrade TPHP directly but might promote TPHP degradation by reducing Fe(III)- to Fe(II)-minerals or converting to other ROS. This study provides new and deeper insights into the interaction between PS and soil constituents and their roles in organic pollutant degradation in contaminated soil using SR-AOPs.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2021
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IF 6.291
Guomin Geng,Yanhui Gao,Zhitong Zhang,Kangqi Gao,Wenyu Zhang,Jianjun Song
Developing monolithic carbon-based catalyst with low cost, easy separation and high performance to degrade pollutants via PMS activation is crucial. In this work, a series of novel monolithic Me-CA catalysts based on biomass derived carbon aerogel were prepared by hydrothermal method using waste watermelon peel as raw material. Co-CA catalyst showed excellent performance to activate PMS for 2, 4-DCP degradation in different temperature and different water matrices. Different pollutants, such as ciprofloxacin (CIP), bisphenol A (BPA), and 2, 4-dichlorophenoxyacetic acid (2, 4-D) could also be removed in the Co-CA/PMS system. As expected, Co-CA could be easily separated from degraded solution, and show high stability and reusability for PMS activation with a lower cobalt leaching. Based on the results of the quenching tests, electron paramagnetic resonance (EPR) spectra, Chronoamperometric test (i-t curves) and electro-chemical impedance spectroscopy (EIS), the PMS activation mechanism was proposed. The phytotoxicity assessment determined by germination situation of mung bean indicated that PMS activation could eliminate the hazards of 2, 4-D. Therefore, this study provides a low cost, efficient and environmental-friendly monolithic biomass carbon aerogel catalyst for different pollutants degradation , which further advances monolithic catalyst for practical wastewater treatment .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Congyu Wang,Zepeng Rao,Asad Mahmood,Xiao Wang,Yan Wang,Xiaofeng Xie,Jing Sun
In the process of photocatalytic oxidation (PCO), titanium dioxide (TiO 2 ) shows excellent capabilities. However, when TiO 2 is used to remove volatile organic compounds (VOCs), there are some drawbacks including weak adsorption of gaseous contaminants, insufficient utilization of sunlight, and rapid recombination of photogenerated carriers. Herein, a TiO 2 -based ternary heterogeneous photocatalyst, g-C 3 N 4 /Ag-TiO 2 , was successfully fabricated to photodegrade gaseous acetaldehyde (one of the representatives of oxygenated VOCs) under visible light. Among the various samples, the g-C 3 N 4 /50 wt% Ag-TiO 2 exhibited an excellent photocatalytic activity , which was 5.8 times of bare TiO 2 . The mineralization efficiency of acetaldehyde was also increased by 3.7 times compared to bare TiO 2 . The substantial improvement in the PCO performance of the ternary system can be associated with the good adsorption to acetaldehyde gas and light-harvesting capability, as well as improved charge separation process. The application of Langmuir-Hinshelwood kinetic model suggested that relative humidity played a significant role in the VOCs degradation. Also, the photodegradation of gaseous acetaldehyde primarily occurred on the catalysts surface. Based on several characterizations, i.e., UV–vis spectroscopy, photoluminescence spectrum, photocurrent spectroscopy and electron spin-resonance test, a suitable degradation mechanism is proposed. This study provides a novel ternary photocatalyst with improved photocatalytic performance and stability, which can be used for the low-concentration VOCs abatement in the indoor environment.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Yanan Qin,Junmei Luo,Qingda An,Zuoyi Xiao,Jingai Hao,Yao Tong,Shangru Zhai
A facile and environmentally friendly method to synthesize efficient catalysts for activating peroxymonosulfate (PMS) to degrade contaminants is highly important yet remains challenging. By combining the superiorities of ordered Co/N@ZS and alginate hydrogels, namely regular and stable channels, large specific surface area, outstanding hydrophilicity and unique three-dimensional structure, an excellent recovery and recyclability catalyst, Co 0·6 /N@ZS-SA, exhibited outstanding performance in activating 0.50 g/L PMS for ciprofloxacin degradation (20 mg/L) with a high degradation rate of 82.52%. The effect of diversified influencing parameters, stability and recyclability on the degradation efficiency was systematically investigated. More importantly, the composite hydrogel with excellent recovery and recyclability could still degrade more than 63.4% CIP after three consecutive reactions. In addition, combined EPR analysis and ROS quenching research indicated that HO • , SO 4 •− , O 2 •− and 1 O 2 were generated but CIP degradation dominated by the radical mechanism comprising the yield of SO 4 •− . Besides, the intermediate products were identified by LC-MS analyses to propose the possible degradation pathways.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Danyu Zhang,Kai Yin,Yanhong Tang,Yuanfeng Wei,Haifang Tang,Yi Du,Huiling Liu,Yuqing Chen,Chengbin Liu
Narrow pH application range and tepid reaction kinetics greatly hinder the efficacy of heterogeneous Fenton and electro-Fenton technologies. Herein, a hollow sea-urchin-shaped carbon-anchored single-atom iron (SAFe@HSC) derived from metal organic framework has been developed as a dual-functional electro-Fenton catalyst for O 2 reduction to H 2 O 2 followed by in situ activation to •OH. Benefited by the unique structure and atomically dispersed iron, the electro-Fenton system exhibits fast reaction kinetics in a wide pH range from 3 to 11. For instance, 120.7 mmol g catalyst −1 (7.5 mol g Fe −1 ) H 2 O 2 and 50.7 mmol g catalyst −1 (3.1 mol g Fe −1 ) •OH can be detected simultaneously at 60 min (20 mA cm −2 and pH 7). As a result, the mass kinetic constants of refractory thiamphenicol (TAP) degradation are as high as 4506 min −1 g Fe −1 (pH 3), 4099 min −1 g Fe −1 (pH 5), 4037 min −1 g Fe −1 (pH 7), 2974 min −1 g Fe −1 (pH 9), and 2595 min −1 g Fe −1 (pH 11). The TAP removal efficiency in static flow process achieves nearly 100% within 40 min, showing a high total organic carbon (TOC) removal of 85% in 2 h (pH 7, 20 mA cm −2 , C 0 = 20 mg L −1 , 1.5 mg of catalyst). It is the highest electro-Fenton activity among the reported catalysts for pollutant degradation at pH above 5. Furthermore, the TAP removal keeps 97% and the TOC removal reaches as high as 82.2% in the continuous-flow process ( C 0 = 20 mg L −1 , pH 7, 20 mA cm −2 , flow rate = 2 mL min −1 ). Moreover, only 1.5% Fe is leaked within 6 h. This study develops a highly efficient electro-Fenton catalyst for the treatment of organic wastewater.
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Journal of Cleaner Production
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2021
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IF 9.297
Wuming Xie,Zijun Huang,Fengping Zhou,Yuhui Li,Xiaolin Bi,Qiushi Bian,Shuiyu Sun
The presence of the antibiotics in wastewater and drinking water is causing increasing concern around the world, thereby an advanced sustainable technology needs to be developed to remove the antibiotics from water resources. In this study, Metal-organic frameworks (MOFs) derived zero-valent iron embedded in the carbon matrix structure named FMC is prepared by a direct pyrolysis of Fe-based metal organic framework. FMC is used as a heterogeneous Fenton-like catalyst to degrade amoxicillin (AMX) based on the oxidation and degradation reactions. FMC had the strengthened catalytic performance for amoxicillin elimination with high mineralization efficiency (60.41%), which was evaluated over various experimental conditions. The role of reaction in FMC/H 2 O 2 system was identified, suggesting amoxicillin was eliminated by the attack of hydroxyls radicals (·OH). The carbon structures can facilitate the passage of electrons and boost the contact of zero valent iron and Fe 2+ species on FMC surface with H 2 O 2 , resulting in the accelerated production of ·OH and high removal efficiency of amoxicillin. By defining reactive oxidizing species and degradation intermediates, the plausible degradation pathways of amoxicillin have been inferred. This study revealed that FMC/H 2 O 2 system has high AMX degradation efficiency and decent recyclability .
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