APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Yujie Cao,Tianran Sheng,Jinfei Mei,Peng Qian,Deqian Huang,Liangquan Sheng,Guoping Sheng
Herein, peroxymonosulfate (PMS)-like Fenton oxidation catalyst (DR-Vo-Co 3 O 4 ) with rich oxygen vacancies and carved flower-like structures were constructed using Co 3 O 4 as precursor via deep reduction strategy. DR-Vo-Co 3 O 4 could activate PMS to achieve almost 100% degradation of sulfadiazine (SD) within 1 min with ultra-high efficiency, possessing a degradation rate constant ( k ) value as high as 5.9 ± 0.2 min −1 , which was 86 and 5 times higher than the unreduced and reported maximum, respectively. Furthermore, the catalytic system showed unparalleled reactivity towards 14 different types of contaminants, with the maximum k value even exceeding 20 min −1 . The carved flower-like structure of DR-Vo-Co 3 O 4 catalysts not only facilitated PMS adsorption, but also provided more reaction sites for PMS activation. Meanwhile, rich oxygen vacancies could effectively tune the DR-Vo-Co 3 O 4 surface electronic state to further accelerate charge transfer, significantly enhancing PMS oxidation efficiency. Catalytic mechanism analysis revealed that 1 O 2 and O 2 •− played a dominant role in contaminant degradation.
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CHEMOSPHERE
·
2022
·
IF 8.943
Xuechun Yang,Xiaoyi Zhang,Xinwei Chen,Xiaoying Gao,Yunjia Liu,Jinlan Weng,Shenghong Yang,Tian Gui,Xiangshu Chen,Rusong Zhao,Jian Liu
Achieving both rapid adsorption rate and high adsorption capacity for bisphenol micropollutants from aquatic systems is critical for efficient adsorbents in water remediation . Here, we elaborately prepared three nitrogen-rich triazine-based porous polymers (NTPs) with similar geometric configurations and nitrogen contents (41.70–44.18 wt%) while tunable BET surface areas and micropore volumes in the range of 454.7–536.3 m 2 g −1 and 0.20–0.84 cm 3 g −1 , respectively. It was systematically revealed that the synergy of hydrogen bonding, π−π electron-donor-acceptor interaction, and micropore preservation promoted the rapid (within 5 min) and high capacity adsorption of bisphenols by NTPs. Particularly, microporous-dominated NTPs-3 with the highest micro-pore volume (0.84 cm 3 g −1 ) displays remarkable adsorption capacity towards bisphenol A as evidenced by the adsorption capacity of 182.23 mg g −1 . A simple column filter constructed by NTPs-3 also expressed good dynamic adsorption and regeneration capacity. This work provided new insight into the rational design and engineering of nitrogen-rich porous polymers for the remediation of micropollutant wastewater.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
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IF 8.025
Peng Xie,Wang Zhang,Wugao Wu,Zhuanglin Shen,Mingliang Wang,Yuxiao Lai,Yantao Chen,Zhongfan Jia
A mediation strategy can effectively overcome the low reaction activity of enzymes with nonspecific substrates. In this study, we demonstrated how phenol compounds can mitigate the substrate limitation of HRP in catalytic degradation of various organic pollutants. In a classical HRP/H 2 O 2 system, phenol and natural phenolic compounds (4-HBA & pHBA), exhibited up to over 100-fold enhancement in eliminating organic dyes and persistent antibiotics while the loading is only 2–5 wt%. A combination of molecular modelling, docking and frontier orbital energy analysis was employed to elucidate the catalytic performance and mechanism. We revealed that (1) generating phenoxyl radicals required the proximity of mediators to the HRP active centre, and (2) the subsequent efficient radical transfer to pollutants was determined by the large energy gap between the SOMO energy of phenoxyl radicals and the HOMO energy of phenols. When considering phenols as pollutants, we showed a synergistic effect on catalytic degradation of phenols, dyes, and tetracycline with a removal efficiency of 71–92 %. Overall, this work not only demonstrates that phenoxyl mediators can overcome the lower efficiency and substrate-specificity limitations of the HRP/H 2 O 2 system but also revealed their structure-mediation relationship, implying great potential in the biodegradation of diverse pollutants and their mixtures.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yabin Li,Jingyao Qi,Jimin Shen,Pengwei Yan,Jing Kang,Binyuan Wang,Shuyu Wang,Jinxiang Zuo,Zhonglin Chen
Peroxymonosulfate (PMS)-based advanced oxidation processes are perceived as a novel strategy for water purification. However, designing an efficient catalyst with a low metal leaching rate remains challenging. Here, under palygorskite (PAL) mediation, 16%-CoCu 0.4 Fe 1.6 O 4 @PAL (16%-CCFO@PAL) was constructed, exhibiting ample oxygen vacancies (V O ) and low metal leakage. The V O was confirmed by systematic characterizations and theoretical calculations. The catalyst showed the efficient catalytic capacity for PMS by dual-path (i.e., metal sites and V O ) activation. Large amounts of SO 4 •- , •OH, and 1 O 2 were produced, greatly destroying bisphenol S (BPS). BPS removal was greater than 99% within 25 min in the 16%-CCFO@PAL/PMS system. At the metal sites, PMS was activated under the synergistic effects of Co(II)/Co(III), Fe(II)/Fe(III), and Cu(I)/Cu(II) pairs and electron transfer. In addition to metal sites, the V O was also an activation center for PMS, which mainly captured the O I atom in [H-O I -O II -SO 3 ] - , donating an electron to O I and promoting SO 4 •- generation. The interfacial reaction mechanism was explored by in situ tests, and a dual-path activation mechanism was proposed. This work provides a new perspective for V O -assisted PMS activation for water treatment.
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CARBON
·
2022
·
IF 11.307
Bin Li,Biao Ma,Mengying Wei,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Qing Xia,Wenchao Peng
Recycle of the spent lithium-ion batteries (LIBs) can reuse the toxic heavy metals for the synthesis of useful materials. In this study, the cobalt metal is obtained by recycling the cathodes of spent LIBs, which is then used as cobalt source for the synthesis of highly porous Co-NC composites. Attributing to the addition of EDTA-2Na and NaNO 3 as chelate agent and activation agent respectively, very large surface areas (>3700 m 2 /g) and highly porous structure can be achieved. These composites can activate peroxymonosulfate (PMS) effectively for the degradation of bisphenol A (BPA) in aqueous solution. The optimized Co-NC/PMS system also shows good performance in a wide pH range and great tolerance to different inorganic ions and NOMs. Radical scavenging experiments and EPR results prove that 1 O 2 is the only functional reactive oxidation species (ROS) for BPA degradation. A generation route of PMS – *OH – *O – 1 O 2 for 1 O 2 is also simulated and proved by DFT calculation. This work provides a novel way to synthesize effective catalysts for PMS activation from the environmental wastes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Xiao-Qiu Lin,Jia-Mei You,Ling-Yu Meng,Naoko Yoshida,Jing-Long Han,Cong-Ju Li,Ai-Jie Wang,Zhi-Ling Li
Tetrabromobisphenol A (TBBPA), a hazardous and persistent flame retardant , has been widely detected in the natural aquatic system. The acceleration of reductive debromination (rate-limiting process) is vital during the decomposition and detoxification of TBBPA. This study achieved superior TBBPA electrochemical reductive debromination performance by nano Pd doped Ni foam electrode (4.8 times higher than Ni foam electrode). The optimal TBBPA reductive debromination performance was obtained under −1.2 V of cathode potential, 1.2 wt% of Pd loading, 10 mg L −1 of TBBPA and 100 mM of Na 2 SO 4 as the electrolyte solution. UPLC-QTOF-MS verified that Br atoms in TBBPA were removed sequentially to form bisphenol A as the major product. Most TBBPA was reductively debrominated by atomic H* through indirect hydrodebromination, evidenced by the atomic H* quenching test. The higher solution conductivity and appropriate TBBPA concentration would contribute to the debromination efficiency. Excessive H 2 generation whether by over negative potential or H atom richness electrolyte largely disturbed the reaction process and restricted the debromination. The improved generation of reductant (H*) ads Pd was the most significant, while excessive Pd loading would make aggregation and limit the debromination efficiency. The study confirmed the optimization strategies of conditions for Pd/Ni foam electrode and revealed the related function mechanism for stimulating TBBPA electrochemical reduction, giving suggestions for the efficient removal of TBBPA in the aquatic environment.
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International Journal of Environmental Research and Public Health
·
2022
·Vol. 19
·期 15
·9437
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IF 4.614
Qianli Guo,Xianhu Qi,Jian Zhang,Bo Sun
Aqueous complexes of Mn(III) ion with ligands exist in various aquatic systems and many stages of water treatment works, while HSO3−is a common reductant in water treatment. This study discloses that their encounter results in a process that oxidizes organic contaminants rapidly. Pyrophosphate (PP, a nonredox active ligand) was used to prepare the Mn(III) solution. An approximate 71% removal of carbamazepine (CBZ) was achieved by the Mn(III)/HSO3−process at pH 7.0 within 20 s, while negligible CBZ was degraded by Mn(III) or HSO3−alone. The reactive species responsible for pollutant abatement in the Mn(III)/HSO3−process were SO4•−and HO•. The treatment efficiency of the Mn(III)/HSO3−process is highly related to the dosage of HSO3−because HSO3−acted as both the radical scavenger and precursor. The reaction of Mn(III) with HSO3−follows second-order reaction kinetics and the second-order rate constants ranged from 7.5 × 103to 17 M−1s−1under the reaction conditions of this study, suggesting that the Mn(III)/HSO3−process is an effective process for producing SO4•−. The pH and PP:Mn(III) ratio affect the reactivity of Mn(III) towards HSO3−. The water background constituents, such as Cl−and dissolved organic matter, induce considerable loss of the treatment efficiency in different ways.Keywords:Mn(III);bisulfite;advanced oxidation processes;sulfate radical;micropollutant abatement
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BIOMEDICAL CHROMATOGRAPHY
·
2022
·Vol. 36
·期 11
·e5454
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IF 1.911
Yong Zhang,Kaifang Wei,Litao Wang,Guihua Gao
In this work, MIL-53(Al), as an inorganic “filler” component, was embedded in polyvinylidene difluoride (PVDF) and polystyrene-block-polybutadiene (SBS) matrices to prepare two mixed-matrix membranes (MMMs), using a simpler method than that previously reported. The PVDF and SBS membranes retained much of the properties of PVDF, SBS, and native MIL-53(Al). The prepared MMMs were then placed in a vortex-stirred sample solution to develop a membrane solid-phase extraction method to extract estrogens and parabens, which were determined by high-performance liquid chromatography with fluorescence detection. The extraction efficiencies of the two membranes were compared, with the PVDF membrane exhibiting superior performance. In addition, the PVDF membrane was more freestanding and flexible, and its preparation method was also more facile and simple. The extraction conditions were optimized, and the analytical method showed low limits of detection (0.005–0.18 ng/mL), good linearity, and high accuracy, with recoveries ranging from 90.7% to 102.5%. As a result, this membrane solid-phase extraction method indicated its potential for application in aqueous sample pretreatment. For metal–organic framework–based MMM used in this method, in addition to being durable, freestanding, mechanically stable, and possessing a large area, it should also exhibit high metal–organic framework incorporation, good flexibility, and appropriate thickness and weight.
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JOURNAL OF BIOCHEMICAL AND MOLECULAR TOXICOLOGY
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2022
·Vol. 36
·期 9
·e23120
·
IF 3.568
Jun-Heng Jiao,Lei Gao,Wen-Long Yong,Zhong-Yun Kou,Zhi-Qiang Ren,Rui Cai,Gui-Yan Chu,Wei-Jun Pang
Bisphenol A (BPA), as a widely used plasticizer, is easily absorbed by animals and humans. It has certain toxic effects on various tissues, including liver, heart, kidney, testis, and ovary. The toxic effects of BPA on animal reproduction have aroused widespread concern, but its regulatory mechanism and antidote in female animals estrus cycle remain unclear. In this study, the results displayed that BPA destroyed the normal estrus cycle of mice through decreasing the levels of progesterone and estradiol. Furthermore, BPA significantly increased the levels of oxidative stress, autophagy, and apoptosis in ovaries and granulosa cells. Interestingly, we found that the natural antioxidant resveratrol rescued estrus disorder and impaired estradiol secretion, reduced the abnormal reactive oxygen species accumulation, autophagy, and apoptosis in BPA exposed ovarian tissues. Moreover, transmission electron microscopy showed that resveratrol reduced BPA-induced autophagic vesicles formation and flow cytometry showed that resveratrol inhibited the increase of apoptotic cells induced by BPA on granulosa cells. Therefore, the supplement of resveratrol could restore BPA-induced estrus disorder by protecting ovarian granulosa cells. Overall, resveratrol is a potential drug to alleviate BPA-induced estrous cycle disorders and ovarian damage.
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CHEMOSPHERE
·
2022
·
IF 8.943
Prosper Kwame Klu,Hao Zhang,Muhammad Abdul Nasir Khan,Chaohai Wang,Junwen Qi,Xiuyun Sun,Jiansheng Li
Developing new catalysts for efficient degradation of micropollutants in water is of significant importance in advanced oxidation processes (AOPs). Herein, TiO 2 /C coated Co 3 O 4 nanocages (Co 3 O 4 @TiO 2 /C) were synthesized and their performance on micropollutants degradation was evaluated. Specifically, cobalt-based Zeolitic imidazolate framework (ZIF-67) coated by a thin layer of titanium species and polydopamine (PDA) was used as a precursor for the preparation of Co 3 O 4 @TiO 2 /C by two-step calcination. The catalytic performance of peroxymonosulfate (PMS) activation towards the degradation of organic pollutants was investigated by using atrazine (ATZ) and Bisphenol A (BPA) as typical micropollutants. The efficiency and the effect of TiO 2 /C shell on the as-synthesized catalyst were analyzed by comparing Co 3 O 4 derived from ZIF-67 and Co 3 O 4 /C derived from ZIF-67/PDA. ATZ degradation results showed that the Co 3 O 4 @TiO 2 /C catalyst was the most efficient for catalytic oxidation when 99.5% of ATZ was removed within 4 min, which is 57.5% and 74.6% faster than that of Co 3 O 4 @C and Co 3 O 4 , respectively. The enhanced performance of Co 3 O 4 @TiO 2 /C is attributed to their unique nanocages structure and improved specific surface area. The catalysis mechanisms and ATZ degradation pathways were presented based on the results of electron paramagnetic resonance (EPR), XPS, and LC-MS analysis. Our results might have added to the design of heterogeneous catalysts of large surface area for efficient PMS activation in AOPs.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 39
·e52858
·
IF 3.057
Xiankun Wu,Chang-an Xu,Mangeng Lu,Kunxin Wang,Zhao Li,Hui Yang
To explore high thermal properties, low dielectric constant and loss for copper clad laminates, poly(phenylene oxide) (PPE) with different end groups (allyl and epoxide groups) were successfully prepared. Firstly, low molecular weight polyphenylene ether was synthesized using the redistribution method. Then the polyphenylene ether thermosetting polymers by modifying their terminal hydroxyl groups were reported and their fundamental materials properties were compared. Through property tests and data analyses, it was found that PPE with vinyl end groups had the best performances, especially high glass transition temperature (about 230°C), the thermal conductivity was 0.32–0.38 Wm −1 K −1 , low dielectric constant (about 2.5) and low dielectric loss (about 4.4 × 10 −3 ). The possible reason was that the main chain of polyphenylene ether contains non-polar crosslinkable group (CC). In a word, through properties comparison of thermosets of PPE, the results demonstrated that the materials of all systems were suitable for using as printed circuit boards.
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Food Analytical Methods
·
2022
·Vol. 15
·期 12
·3468-3478
·
IF 3.498
Li Junkui,Zuo Min,Zhang Wen,Zou Xiaobo,Sun Zongbao
The use of gutter oil in cooking, which poses a serious threat to human health, has attracted increasing attention in recent years. Capsaicin, existing in chili peppers, is used to identify gutter oil. Here, in order to detect capsaicin fast and accurately for gutter oil discrimination, we introduce a hybrid method to detect capsaicin based on a diazo coupling reaction and surface-enhanced Raman scattering (SERS) technology. A diazo coupling reaction is applied to the composite of p-aminothiophenol (4-ATP) and capsaicin, and the product, azo dye, is adopted as the SERS probe. Gold nanorods (Au NRs) are prepared using the seed-mediated growth method and utilized as the SERS substrate. The Au–S bond between the azo dye and the Au NRs has a powerful ability to spontaneously capture target molecules on the sensing interface. The production of the diazo coupling reaction is proven with an ultraviolet–visible (UV–vis) absorption spectrum. As-synthesized Au NRs are characterized with a UV–vis absorption spectrum, transmission electron microscope, and SERS. Significantly improved SERS peaks were observed at 1114 and 1392 cm −1 , showing this method can be used to detect capsaicin and identify gutter oil. In a broad range of 10 −11 ~ 10 −4 M, the log-linear relationship between SERS intensity and capsaicin concentration is well established, with a detection limit of 3.24 × 10 −12 M.
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