JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
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IF 10.319
Shuangqin Chen,Mai Li,Qingmin Ji,Tao Feng,Si Lan,KeFu Yao
Fe-based metallic glasses (Fe–MGs) are potential candidate catalysts for advanced oxidation processes (AOPs) for recalcitrant organic pollutant degradation. However, industrial wastewater and natural contaminated sites usually contain abundant inorganic ions, like the chloride ion (Cl − ), which significantly affect AOPs, but their influence on MG-activated AOPs still remains unclear. Through the study of three commonly used oxidants, hydrogen peroxide (H 2 O 2 ), peroxydisulfate (PDS), and peroxymonosulfate (PMS), the effect of Cl − on the FeSiB-catalyzed process of degradation of the typical azo dye Orange II was investigated. Evidence indicates that the addition of Cl − resulted in the monotonous inhibition of the degradation process when the H 2 O 2 /FeSiB and PDS/FeSiB systems were employed, but promoted effect was detected with the PMS/FeSiB system, which is different from the previously observed dual effect of Cl − . It is closely relative with FeSiB induced unique variety of degradation pathways, including radicals, non-radicals ( 1 O 2 ), and direct reduction degradation. Moreover, the presence of Cl − significantly affected the systems’ absorbable organic halogen content and the amount of Fe leached into the solution. The results of this work will provide essential references for Fe-based MG used as AOP catalysts in field applications and the development of advanced MGs with excellent adaptability to complex environments.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2022
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IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 27
·40734-40744
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IF 5.19
Zhu Bo,Xu Jiangyan,Xu Zhihui,Wu Meisheng,Jiang Hongmei
A facile soft-template solvent thermal strategy was developed to prepare mesoporous carbon–silica composite (MMCS) by using furfuryl alcohol (FA) as carbon precursor, Pluronic copolymer P123 as template, hydrated iron nitrate as iron source, and teraethylorthosilicate as silicon source and it was applied for the removal of methyl orange (MO). The as-synthesized MMCS with abound of hydrophilic groups processed a high specific surface area, large pore volume, and good magnetic response. With the increased amount of FA, the surface area and functional groups increased, promoting the adsorption effect. The maximum adsorption capacity of MO on MMCS can be high to 113.1 mg g −1 at pH 4 with 150 mg L −1 initial MO concentration. The adsorption isotherm, kinetic, and thermodynamics were all studied and the results showed the adsorption process well fitted Langmuir adsorption isotherm and pseudo-second-order model. Additionally, it was shown that the adsorption process could not be interfered by the co-existence of PO 4 3− , NO 3 − , CO 3 2− , SO 4 2− , and real water matrix. And the proposed adsorbent can remove MO in three practical water samples with satisfied removal rates ranging from 92.8 to 99.8%. Thus, the MMCS prepared in this study could be utilized as an alternative adsorbent for the removal of methyl orange from practical aqueous solution.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Linjie Wang,Qing Jin,Youlin Xiang,Lu Gan,Lijie Xu,Ying Wu,Xingyu Fang,Haiqin Lu,Shuguang Han,Juqing Cui
Spinel structured Co x Mn 3-x O 4 nanoparticles embedded carbon composites (Co x Mn 3-x O 4 -C) were rationally designed and prepared using Co/Mn bimetallic metal organic frameworks (MOFs) as the template. The Co x Mn 3-x O 4 -C represented prominent bisphenol A (BPA) degradation capability by activating peroxymonosulfate (PMS), in which Co 1.5 Mn 1.5 O 4 -C exhibited the highest BPA degradation efficiency. Specifically, Co 1.5 Mn 1.5 O 4 -C (0.1 g/L) could completely degrade 0.1 mM of BPA within 3 min, which was better than many previous reported catalysts. Moreover, the Co 2+ leaching was limited in the Co 1.5 Mn 1.5 O 4 -C/PMS system. It was revealed that hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) were the main active species in the reaction system, which dominated a dual pathway mechanism for BPA degradation. Furthermore, the Co 1.5 Mn 1.5 O 4 -C could maintain its performance in a variety of water matrices with promising recyclability. This study encourages the rational design and preparation of high-efficient catalysts by employing tunable MOFs precursors for refractory organic pollutant degradation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yu Li,Jiemin Chen,Jie Zhong,Bin Yang,Zequn Yang,Kaimin Shih,Yong Feng
The use of cocatalyst in Fenton-like reactions has been demonstrated as a reliable approach to improve their efficiency via accelerating the circulation of Fe 3+ /Fe 2+ . In this study, we for the first time used natural pyrite (FeS 2 ) as a Fenton-like cocatalyst to improve the reactivity of Fe 3+ instead of the widely investigated molybdenum disulfide that releases potential harmful molybdenum ions. The presence of FeS 2 significantly improved the degradation of sulfamethoxazole (SMX) by Fe 3+ -peroxymonosulfate (PMS); near complete removal of SMX by FeS 2 -Fe 3+ -PMS was achieved, while no obvious removal of SMX by Fe 3+ -PMS was noticed. Meanwhile, the surface area-normalized rate constant of SMX degradation by FeS 2 -Fe 3+ -PMS was more than 18 times higher than that by MoS 2 -Fe 3+ -PMS. FeS 2 -Fe 3+ -PMS worked effectively in a wide range of pH values from 3.0 to 10.0. Although hydroxyl radicals, sulfate radicals, superoxide anion radicals, and singlet oxygen were recorded by electron paramagnetic resonance spectroscopy, only sulfate radicals were mainly responsible for the degradation. Sulfide ions were identified as one of the intermediates, but the reactive species generated by their interaction with PMS did not contribute to the degradation. FeS 2 had a good stability by continually accelerating the circulation of Fe 3+ /Fe 2+ . The findings from this study reveal a highly efficient cocatalyst for Fenton-like reactions.
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高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Yanzhuo Zhang,Mengqi Xu,Rui He,Jing Zhao,Wei Kang,Jinghua Lv
Because of the increasingly widespread contamination of antibiotics, the preparation of biochar by heteroatom doping to further improve the catalytic degradation efficiency of antibiotics has become a major focus of research. In this study, N-doped (NBC), S-doped (SBC), and NS-doped (NSBC) moso bamboo biochar were obtained at preparation temperatures of 300–700 °C. The concentration of environmentally persistent free radicals (EPFRs) in all biochars peaked when the preparation temperature was 500 °C: 2.45 × 10 19 spins·g −1 (BC), 9.23 × 10 19 spins·g −1 (NBC), 6.10 × 10 19 spins·g −1 (SBC), and 4.36 × 10 19 spins·g −1 (NSBC). After heteroatom doping, EPFR species were more abundant, and the distribution of three types of EPFRs (oxygen-centered (g > 2.0040), carbon-centered (g < 2.0030), and carbon-centered radicals with oxygen atom free radicals (2.0030 < g < 2.0040) varied with the preparation temperature. In the process of antibiotic degradation, both NBC and SBC increased the degradation rate of antibiotics, whereas NSBC reduced the degradation rate. Compared with the degradation rate of antibiotics of biochar (79.86%), the degradation rate of antibiotics by NBC, SBC, and NSBC via PMS activation was 92.23%, 88.86%, and 70.97% on average in 30 min, respectively. The greatest contributors to the catalytic degradation were SO 4 •- , followed by 1 O 2 , •OH, and O 2 •- . EPFRs and 1 O 2 might be the main contributors to the free radical and non-free radical pathways. The enhancement of EPFRs following the N doping or S doping of biochar is the key factor underlying PMS activation. Therefore, changes in the structure of biochar can better activate PMS to produce reactive oxygen species-degrading antibiotics. The mineralization rate of antibiotics by BC, NBC, SBC, and NSBC was 42.12%, 47.06%, 44.99%, and 39.01%, respectively. This means that a small portion of the antibiotics was completely decomposed into CO 2 , H 2 O, and inorganic substances after degradation. Cyclic experiments showed that heteroatom-doped biochar had higher reusability, and the degradation rate decreased less than 15%.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jixiang Xu,Yi Wang,Jun Wan,Lei Wang
In this work, carbon-doped CoMn 2 O 4 /Mn 3 O 4 (C-CoMnO) composite catalyst were prepared via calcining solvothermal product of Mn 2+ , Co 2+ , and 2-methylimidazole in air. The catalytic performance of activating peroxymonosulfate (PMS) for ciprofloxacin (CIP) degradation was discussed. The results showed that the 0.1 g L −1 C-2CoMnO could effectively activate PMS, resulting in 96.18% CIP was degraded within 60 min. The corresponding total organic carbon removal ratio and apparent rate constant were 81.33% and 0.043 min −1 , respectively. The influencing factors, such as Co/Mn molar ratios, calcination temperature, PMS concentration, solution pH, and coexisting ions were explored. The optimal catalytic system exhibited good recycling performance, wide pH adaptation and high resistance to salt interference. SO 4 ⋅ − , ⋅OH, and ⋅O 2 − -based radicals, as well as 1 O 2 and surface complexes-based nonradicals were participated in CIP degradation. The CIP degradation pathways were proposed. Density functional theory calculations (DFT) indicated that PMS was more easily activated via Co/Mn synergism. The doped carbon was also contributed to PMS activation via facilitating electron transfer. This study may shed light toward the synergistic effect of metal oxides in PMS activation.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Hui Yang,Chaonan Tao,Lincai Peng,Junhua Zhang,Liang He,Huai Liu
It remains a challenging task for the efficient conversion of carbohydrates to value-added chemicals at concentrated feedstock solution. In this contribution, the acid-catalyzed processing of high-concentration C5/C6 sugars (180 g/L) in the ethylene glycol (EG) solvent system was investigated, and prominent discrepancy was noticed between C5 and C6 sugars. A large amount of liquefied products was achieved in the concentrated C6 sugars EG solution, whereas the main products in the case of C5 sugars were found to be solid humins. The reaction mechanism studies revealed that EG can shelter fructose and reaction intermediates (5-hydroxymethylfurfural and levulinic acid) from the cross-polymerization and self-etherification reactions, thereby reducing the generation of solid humins during the fructose liquidation process. However, in the case of xylose, the copolymerization between EG and furfural (FF) generates a solid resin, thus rendering a high solid product yield. Moreover, the produced FF–EG resin was found to be a polymer with high molecular weight formed by connecting the furan ring and the alkyl structure through an ether bond. This finding provides insights into the acid-catalyzed conversion of concentrated C5/C6 sugars in EG, facilitating rationally designed processes for the valorization of concentrated carbohydrates.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Shan Xue,Zhilin Xie,Xiaoyu Ma,Yinqi Xu,Shiyu Zhang,Qina Jia,Rui Wan,Haisheng Tao
Carbon-based catalyst-activated persulfate-driven advanced oxidation processes (AOPs) have received great attention for wastewater treatment . Herein, a magnetic Fe-doped activated carbon (FeC 2 O 4 /AC) was successfully prepared via a conventional method using FeC 2 O 4 as an iron source and Zoysia sinica as biomass. FeC 2 O 4 /AC was characterized and used to activate peroxymonosulfate (PMS) for Rhodamine B (RhB) degradation. The influence of various factors on RhB removal was evaluated, including initial pH, temperature, coexisting ions, RhB concentration, PMS concentration and catalyst dosage. Under the optimized condition, the removal efficiency of FeC 2 O 4 /AC for RhB (300 mg/L) reached up to 97% within 150 min. Radical scavenging results and EPR experiments confirm that singlet-oxygen ( 1 O 2 ) was confirmed as the main active species in the degradation of RhB in the FeC 2 O 4 /AC/PMS system. More importantly, the possible route of 1 O 2 generation was revealed: the synergistic effect of Fe species and the activated carbon acts as a crucial part in promoting the PMS activation and contributing to the generation of 1 O 2 . The reaction rate constant ( k obs ) of FeC 2 O 4 /AC is about 7.4 times that of pure AC, and the excellent leaching rate of Fe 2+ (<0.09%) proves that this material is an excellent catalyst. This research on the development of Fe-doped activated carbon with high activity and high stability has profound implications for the effective treatment of organic wastewater.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Li Chen,Tahir Maqbool,Ghazanfar Nazir,Congyu Hou,Yulong Yang,Jianning Guo,Xihui Zhang
Endocrine disrupting compounds (EDCs) in the aquatic systems are of growing concerns that could undermine drinking water safety. In this study, manganese (III) oxide (Mn 2 O 3 ) based catalytic ceramic membrane (CCM) was developed for the activation of peroxymonosulfate (PMS), and its applicability has been tested in degrading the ten different EDCs (including bisphenol analogs (BPs)) in drinking water. The CCMs were synthesized at different calcination temperatures i.e., 850, 950, and 1150 °C. Optimal performance of CCMs/PMS was achieved at a higher degree of calcination. The CCMs/PMS has shown a potential to effectively degrade the EDCs at higher concentrations (mg/L) to trace levels (ng/L). The CCMs/PMS system adopted a non-radical pathway of degrading the EDCs through the extensive generation of singlet oxygen ( 1 O 2 ), as confirmed using quenching experiments and electron paramagnetic resonance (EPR) spectroscopy. 1 O 2 -based oxidation process showed special selectivity for the decontamination of phenols and bisphenols. The long-term performance of CCMs/PMS showed good stability in degradation of the EDCs in drinking water, also with efficient mineralization (TOC removal >55%) and negligible release of Mn (0.004 wt%Mn/min). CCMs/PMS system also showed high potential in improving water quality by reducing the disinfection byproducts (DBPs) formation potential, highest recorded for bromodichloromethane (CHCl 2 Br, 100%) and lowest for dichloroacetic acids (TCAA, ∼50%). The study provided a highly efficient catalytic ceramic membrane based advanced oxidation process (AOPs) for effective degradation multiple of EDCs in drinking water, and the findings of this work can be a baseline for full-scale water treatment applications.
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Food Bioscience
·
2022
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IF 5.318
Caixing Pan,Heping Cui,Khizar Hayat,Xiaoming Zhang,Chi-Tang Ho
This research elucidated the reason of flavor deficiency during the thermal degradation of glutamic acid (Glu)-galactose (Gal) Amadori rearrangement product (GG-ARP) and the solution. The flavor formation from GG-ARP during the thermal degradation was investigated. Compared to the volatile compounds in Glu-Gal Maillard reaction products (GG-MRP), pyrazines in the volatile compounds derived from GG-ARP were restrained. The disadvantage in evolution asynchrony and content sufficiency of α -dicarbonyl compounds and Glu in the GG-ARP model limited the pyrazines formation. With the addition of Gal, the asynchronous effect was further exacerbated, and the furans in the GG-ARP-Gal model (956.81 μg/L, 120 °C, 60 min) were more significantly dominant among the volatile flavor compounds than in the GG-ARP model (454.98 μg/L, 120 °C, 60 min), while the pyrazines were still missing. Whereas, the extra-added Glu in the GG-ARP model could offset the deficiency of amino acids growth after α -dicarbonyl formation and promote the formation of pyrazines (74.47 μg/L, 120 °C, 60 min). Meanwhile, the formation of diketones (92.96 μg/L, 120 °C, 60 min) was promoted. The addition of Glu enhanced both milk-like and baking flavor of the GG-ARP system simultaneously. Formulated GG-ARP-Glu mixture was proposed to promisingly achieve the controlled formation of process flavors for baked foods with both desirable milk-like and baking scent.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Wei Li,Wei Li,Kuanchang He,Longxiang Tang,Qian Liu,Kui Yang,Yi-Di Chen,Xin Zhao,Kai Wang,Hui Lin,Sihao Lv
Cobalt-based catalysts have been widely explored in the degradation of organic pollutants based on peroxymonosulfate (PMS) activation. Herein, we report an MXene nano-Co 3 O 4 co-catalyst enriched with oxygen vacancies (O v ) and steadily fixed in nickel foam (NF) plates, which is used as an efficient and stable PMS activator for the removal of 1,4-dioxane (1,4-D). Ti originating from MXene was doped into the Co 3 O 4 crystal, generating large amounts of O v , which could provide more active sites to enhance PMS activation and facilitate the transformation of Co 2+ and Co 3+ , causing a high stability. As a result, the 1,4-D removal efficiency of the NF/MXene-Co 3 O 4 /PMS system ( k app : 2.41 min −1 ) was about four times higher than that of the NF/Co 3 O 4 /PMS system ( k app : 0.62 min −1 ). In addition, singlet oxygen was the predominant reactive oxygen species . Notably, the 1,4-D removal of the NF/MXene-Co 3 O 4 /PMS system was over 95% after 20 h operation in the single-pass filtration mode with only 3.72% accumulative Co leaching, showing excellent stability and reusability of NF/MXene-Co 3 O 4 . This work provides a defect engineering strategy to design a robust and stable catalytic system for water treatment , which expands the application of MXene in the field of environmental remediation.
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高影响因子