CHEMOSPHERE
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2019
·
IF 5.108
Longjun Rao,Yunfei Yang,Likun Chen,Xiudan Liu,Haixiang Chen,Yuyuan Yao,Wentao Wang
The development of highly efficient and green catalytic oxidation process based on peroxymonosulfate (PMS) activation has been identified to be a significant yet challenging objective in the environmental catalysis field. A simple, environmentally benign and highly effective catalytic oxidation system was innovatively constructed by coupling NaBO 2 and PMS for the removal of Acid Red 1. The catalytic mechanism in the NaBO 2 /PMS system was elucidated by electron paramagnetic resonance (EPR) combined with several radical capture reagents (ascorbic acid, methanol, tert -butyl alcohol, ethanol and l -histidine). The experimental results indicated that singlet oxygen ( 1 O 2 ) severed as the predominant reactive oxygen species (ROS) rather than the HO or during the catalytic oxidation process, at variance with the reported radical pathway in the Co 2+ /PMS system. Inspiringly, p -benzoquinone ( p -BQ) as a trapping agent in most advanced oxidation process could be turned into the positive one in the NaBO 2 /PMS system, achieving a nearly 3-times enhancement in terms of the rate constant for AR1 removal. More interestingly, sodium chloride (NaCl) presented the same enhancement effect as p -benzoquinone due to generation of hypochlorous acid (HOCl) and more 1 O 2 , which was completely different from the reported. This study develops a highly efficient green oxidation process and opens up a new insight in the remediation of contaminated water .
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ACS Applied Bio Materials
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2019
·
IF 0
Lin Xiong,Mengyao Zhao,Yong Fan,Shangfeng Wang,Yanling Yang,Xiaomin Li,Dongyuan Zhao,Fan Zhang
An ultraviolet (UV) filter is the core component of sunscreen and protects skin from various photo damages. Current UV filters are hampered by skin penetration, poor photostability, photocatalytic generation of harmful reactive oxygen species (ROS), and potential environmental risks. In this work, manganese dioxide nanoclusters were developed as an eco-friendly UV filter by a facile two-step synthesis, using colloid silica as support under ambient conditions. These nanoclusters show a better UV-shielding profile than commercial titanium dioxide nanoparticles and capability to scavenge various ROS. They can be easily incorporated by a sunscreen formula and demonstrate an excellent skin photoprotection performance both in vitro and in vivo.
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Journal of Physical Chemistry C
·
2019
·
IF 4.309
Zenghe Li,Xuejie Chen,Xu Teng,Chao Lu
The formation of hydroxylated intermediates is the first step in the persulfate-based advanced oxidation processes (AOPs) and depends directly on the oxidation degree of recalcitrant pollutants. Therefore, the monitoring of hydroxylated intermediates plays a vital role in persulfate-based AOPs for evaluating the oxidation degree and understanding the degradation mechanism. In this work, based on the attractive amplification of luminol chemiluminescence (CL) signals by hydroxylated intermediates, we developed a rapid, sensitive, and simple CL-based method to monitor hydroxylated intermediate (i.e., 3,5-diethyl-1,4-benzenediol) generated in persulfate-based AOPs of 1,2-divinylbenzene (DVB). The possible mechanism of the proposed CL system was that hydroxylated intermediates could be oxidized by persulfate in alkaline solution to form superoxide anion radicals and thus lead to an increase in the luminol CL. Finally, the proposed CL system was successfully applied in monitoring hydroxylated intermediates generated during persulfate-based AOPs under different degradation conditions, whose validity and reliability were verified by liquid chromatography–mass spectrometry (LC-MS) and Fourier-transform infrared spectroscopy (FT-IR). The generality of the proposed CL system was verified by monitoring hydroxylated intermediates generated in persulfate-based AOPs of methylbenzene and benzoic acid. These results suggested that this present CL system provided a promising indicator for monitoring hydroxylated intermediates in persulfate-based AOPs.
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CATALYSIS TODAY
·
2018
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IF 4.667
Imtyaz Hussain,Yongqing Zhang,Mingyu Li,Shaobin Huang,Waseem Hayat,Liangming He,Xiaodong Du,Guoqiang Liu,Meimei Du
In this study, magnetic BiFeO 3 nanoparticles (BFO MNPs) were successfully synthesized by simple sole-gel method. The BFO MNPs catalyst was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), x-ray photoelectron spectroscopy (XPS) and Fourier transform infrared (FT-IR) techniques. The prepared catalyst was used to activate persulfate (PS) to generate sulfate radicals (SO4 − ) for the enhanced degradation of aniline from aqueous solution. It was found that BFO MNPs showed high catalytic activity toward PS decomposition for the degradation of aniline. The degradation efficiency of aniline (0.5 mM) was 100% within 120 min using initial dosage of 0.5 g/L BFO MNPs and concentration of 5 mM persulfate. Even at neutral pH (7.0), aniline was efficiently degraded in BFO MNPs /PS system. The effects of reaction parameters such as initial pH, PS concentration and dosage of BFO MNPs were investigated. The radical scavenging and electron paramagnetic resonance (EPR) results showed that sulfate radicals (SO4 − ) and hydroxyl radicals ( OH) were generated by the activation of PS with BFO MNPs for the degradation of aniline. The stability of catalyst was tested by means of successive reuse cycles. The results revealed that BiFeO 3 catalyst exhibited high reusability and stability in degrading aniline through PS activation .
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PHOTOCHEMISTRY AND PHOTOBIOLOGY
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2018
·Vol. 94
·期 4
·650-658
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IF 2.214
Rong Liu,Yonggang Zhang
Photoelectrocatalytic (PEC) system greatly improves the migration of photoexcited charges, retards the fast recombination of electron-hole and increases the lifetime of photogenerated holes. In this article, we constructed a novel PEC system to degrade berberine chloride form (BCF). XRD patterns indicated aging time was an important condition for the crystal type of TiO 2, and the best proportion of anatase/rutile was 80/20. The band gap energy of the TiO 2 was 3.01 eV. We demonstrated that a synergistic effect existed between photocatalysis (PC) and electrocatalysis (EC). Besides, we discussed the influence of pH, current density, the amount of catalyst and initial BCF concentration on the degradation of BCF. Electron spin resonance (ESR) through spin trap 5, 5-dimethyl-1-pyrroline-N-oxide (DMPO) and the scavenging experiments suggested that the reactive oxygen species (ROS) were superoxide radicals ( ), hydroxyl radicals (·OH) and sulfate radical ( ) in PEC system. Furthermore, we compared the two pathway of formation DMPO-SO 4 adducts and found that was the most major oxidized species in degrading BCF. We proposed a plausible reaction mechanism. Intriguingly, even under lower current and weaker light conditions, the PEC process maintained its effectiveness, demonstrating the feasibility of the PEC approach.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Qiang Guo,Hui Li,Qian Zhang,Yanlin Zhang
In recent years, the frequent eutrophication of water bodies around the world has led to the accumulation of microcystins (MC-LR) in water bodies, causing great harm to humans and aquatic organisms. In this study, a Z-scheme Ag 3 PO 4 /NG/PI composite photocatalyst was fabricated by using silver orthophosphate, nitrogen-doped graphene and polyimide for photocatalytic degradation of MC-LR under visible light irradiation. The structure, morphology and optical properties of Ag 3 PO 4 /NG/PI were characterized by XRD, SEM, TEM, XPS, FT-IR, BET, and UV–vis DRS. The degradation ratio of MC-LR by Ag 3 PO 4 /NG/PI photocatalysts was higher (up to 94.4%) than that of pure Ag 3 PO 4 for MC-LR degradation within 10 h under visible light irradiation, and the kinetic constant over Ag 3 PO 4 /NG/PI was ∼7 times of pure Ag 3 PO 4 . Based on the results of Liquid Chromatography–Mass Spectrometry (LC–MS), the possible degradation pathways of MC-LR were proposed. Photoelectrochemistry measurement (the photocurrent response, electrochemical impedance spectroscopy and Mott-Schottky plots), radical trapping experiment, electron spin resonance test, PL spectroscopy and analysis of band gap have revealed that the photocatalysis of Ag 3 PO 4 /NG/PI follows the Z-scheme mechanism, which can not only promote the separation and migration of photogenerated carriers to reduce re-combination, but also maintain a strong redox capacity. Meanwhile, the stability of Ag 3 PO 4 /NG/PI photocatalyst is greatly improved because the photogenerated electrons (e − ) of Ag 3 PO 4 are migrated to NG to suppress the photo-corrosion of Ag 3 PO 4 .
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CARBON
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2018
·
IF 7.082
Yanbin Wang,Man Liu,Xu Zhao,Di Cao,Tao Guo,Bo Yang
Sulfate radicals and/or hydroxyl radicals (SO 4 − ∙ or ∙OH) have been generally demonstrated as the primary oxidative species in the activation of peroxymonosulfate (PMS). Recently, the role of singlet oxygen ( 1 O 2 ) on the degradation of pollutants has attracted increasing research attention. In this study, boron-doped ordered mesoporous carbon (B-OMC) was prepared and used to activate PMS for the removal of bisphenol A (BPA). Compared with the pristine OMC, the catalytic activity of B-OMC was greatly increased, which resulted from the enhanced adsorption capacity for BPA and the increased catalytic activity for PMS activation. On the one hand, B doping promoted the BET surface area and pore size of OMC; on the other hand, Lewis acid sites were introduced on the surface of OMC and acted as catalytic sites for PMS activation. Influencing factors, such as PMS concentration, catalysts dosage, reaction temperature and initial pH, on the removal of BPA were investigated. Combining the results of radical quenching experiments with electron spin resonance , it was verified that superoxide radical (O 2 − ·) and 1 O 2 instead of SO 4 − ∙ and ∙OH were the dominated oxidative species in B-OMC-PMS system. Electrochemical analysis demonstrated that the boron doping benefited from the electron transfer from B-OMC to PMS.
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TALANTA
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2018
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IF 4.244
Jingjing Guo,Yan Wang,Min Zhao
Ferrous(II) phosphate nanoflowers (Fe 3 (PO 4 ) 2 ·8H 2 O NFs) were synthesized by a facial co-precipitation method. The structure, composition and morphology were characterized by XRD, EDX , element mapping and FESEM . The as-prepared Fe 3 (PO 4 ) 2 ·8H 2 O NFs exhibited excellent intrinsic peroxidase-like activity. Steady-state kinetic studies showed that Fe 3 (PO 4 ) 2 ·8H 2 O NFs exhibited stronger affinities with 3,3,5,5-tetramethylbenzidine (TMB) and H 2 O 2 as the substrates compared with the natural horseradish peroxidase (HRP) and the catalytic constant ( k cat ) value was even higher than HRP and other reported nanomaterial based peroxidase mimics. The investigation of the catalytic mechanism by cyclic voltammetry , fluorescence spectroscopy and ESR displayed the catalytic activity of Fe 3 (PO 4 ) 2 ·8H 2 O NFs originated from the generation of •OH. The Fe 3 (PO 4 ) 2 ·8H 2 O NFs also exhibited higher robustness and better storage stability than HRP. Then, a Fe 3 (PO 4 ) 2 ·8H 2 O NFs-based colorimetric platform was developed to determine H 2 O 2 and glucose. The linear range of H 2 O 2 and glucose was as broad as 1 × 10 −5 –2.5 mM and 8 × 10 −4 –1.2 mM, and the detection limit (LOD) was as low as 5 nM and 35 nM, respectively. This simple assay offered a highly sensitive and specific strategy for H 2 O 2 and glucose determination, which had been successfully utilized for real sample analysis with good reproducibility and accuracy.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 9
·4167-4178
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IF 9.931
Siyi Guo,Yongrong Jiang,Liuyi Li,Xiangdong Huang,Zanyong Zhuang,Yan Yu
Despite extensive efforts dedicated to researching two-dimensional (2D) transition metal oxides (TMOs), significant challenges still remain to simplify their synthesis and improve the activity and reusability of these materials. In this work, we prepared a 2D Cu-containing layered double oxide (CuLDO) under mild conditions. Only via stirring LDO in diluted Cu solution at room temperature could ion exchange between Mg in LDO and Cu ions from that solution allow fixing of Cu onto the surfaces of LDO nanosheets with good dispersion at a high density. The obtained CuLDO was then annealed to give CuOx-rich nanosheets (denoted as c-CuLDO), which maintained a thin thickness of 5–9 nm with a flowers-like architecture thanks to the structural memory of the source materials. The excellent morphology of CuOx-based nanosheets helped to avoid the restacking of nanosheets. Such a c-CuLDO outperformed many other reported Cu-based nanomaterials as a catalyst in phenol degradation (k = 0.335 min−1) because c-CuLDO could efficiently activate persulfate to generate abundant amounts of sulfate radical (SO4˙−). Furthermore, the catalytic activity of used c-CuLDO could be restored by a simple hydrothermal treatment. The developed chemistry could also be used to remove copper ions from wastewater, generating value-added Cu-based nanomaterials and eliminating waste at the same time. The current results may inspire the design of novel low dimensional nanomaterials that are difficult to synthesize directly by conventional bottom-up strategies.
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ACS Applied Materials & Interfaces
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2018
·
IF 8.097
Da Wang,Haodan Xu,Jun Ma,Xiaohui Lu,Jingyao Qi,Shuang Song
Novel single-crystal hexagonal MnTiO3 nanosheets with exposed {0001} facets have been synthesized via a simple one-pot hydrothermal method using NaOH as a mineralizer and tetraethylammonium hydroxide (TEAH) as a morphology controller. The intermediate morphologies of MnTiO3 nanostructures such as nanoparticles, nanowires, nanorods, and nanodiscs are trapped kinetically by adjusting the synthesis conditions. This approach enables us to elucidate the growth mechanisms of MnTiO3 nanosheets based on the tetraethylammonium cation adsorption abilities on different MnTiO3 crystal facets combined with density functional theory calculations. Dissolution and recrystallization processes are involved during the MnTiO3 crystallization. The surface-controlled MnTiO3 has been found to be effective as a catalyst for ozonation in the degradation of 4-chlorophenol (4-CP). Within typical experimental conditions (catalyst dosage = 0.3 g L–1, [4-CP]0 = 50 mg L–1, [O3] = 20 mg L–1, gas flow = 0.1 L min–1, pH 6.8, and T = 293 K), the total organic carbon (TOC) removal efficiency of 4-CP in catalytic ozonation with well-structured MnTiO3 (MnTiO3-180-10 sample) was 76.3% after 60 min, compared with only 22.1 and 38.5% TOC removal in the absence of catalyst and with uncontrolled MnTiO3 (MnTiO3-no TEAH sample), respectively. Benefiting from the high exposure percentage of {0001} facet, mixed-valences of manganese, surface hydroxyl groups, and the enrichment Lewis acid sites provided by Mn and Ti, the morphology-controlled MnTiO3 nanosheets can be applied as heterogeneous catalytic ozonation catalysts which exhibit excellent pollutant degradation. We anticipate that MnTiO3 can be a promising candidate material for the application in remediation of organic pollutants in water.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Amina,Xiongyuan Si,Kang Wu,Youbin Si,Balal Yousaf
In this study, a modified Fenton system using calcium peroxide (CaO 2 ) powder, as an effective source of hydrogen peroxide (H 2 O 2 ), for the degradation of sulfamethoxazole (SMX) in aqueous solution was investigated. Our results indicated that degradation of SMX in Fe(II)-EDTA catalyzed CaO 2 system was readily more efficient than in Fe(II) catalyzed CaO 2 system. The SMX degradation efficiency was found maximum at pH 6.0 and SMX degradation was suppressed as the initial solution pH was increased. Nevertheless overall removal efficiency in this system was favorable near to neutral pH. In addition, it was observed that the higher bicarbonates (HCO 3 − ) contents had a considerable scavenging ability to SMX degradation while low concentration exhibited auspicious role. The presence of chlorides (Cl − ), nitrates (NO 3 − ), sulfates (SO 4 2− ), and humic acid (HA) could improve SMX removal in this Fenton-like system. Furthermore, chemical probe and radical scavenging activity confirmed the formation of hydroxyl (HO ) and superoxide (O 2 − ) radicals, and also described that the SMX degradation was predominantly due to the HO -induced oxidative destruction. Electron paramagnetic resonance (EPR) studies for different systems, different pH values and different reaction times were carried out to determine the HO radical intensities. EPR results showed that HO intensities were higher in Fe(II)-EDTA catalyzed CaO 2 system, at pH 6.0 and at 90 s reaction time, respectively. Intermediate products of SMX were identified and possible mechanism of SMX degradation was suggested. In conclusion, this work provided comprehensive knowledge for the use of Fe(II)-EDTA catalyzed CaO 2 system for remediation of SMX contaminated sites.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Yi Li,Suge Zhang,Yugui Han,Shanshan Cheng,Wenping Hu,Jingjing Han,Yanan Li
Ciprofloxacin (CIP) is a pervasive ecosystematic contaminant which is classified as highly effective broad-spectrum antibiotic. In this work, CIP was degraded by a self-prepared ternary Ce 3 ZrFe 4 O 14-x /CF composite cathode (x referred to oxygen vacancies) undergoing the heterogeneous electrocatalytic process. The influences of operating parameters such as pH, applied current and loading capacity, were estimated by removing efficiency. Compared with the pure carbon felt (CF), 3.8 wt% Ce 3 ZrFe 4 O 14-x /CF composite cathode showed the efficient degradation of CIP in broad pH range 3.0–6.0 with 100 mA. The degradation rates reached more than 98.0% at the wide pH range in 3 h, even reached 100% at pH = 3. The results indicated that the Ce 3 ZrFe 4 O 14-x /CF composite emerged a brilliant electrocatalysis in enhancing oxygen active species with converting reactions in Ce 4+ ↔Ce 3+ and Fe 3+ ↔Fe 2+ . For further understanding the ternary Ce 3 ZrFe 4 O 14-x /CF composite electrode, we used SEM, BET, TEM, XRD, XPS, TOC , HPLC–MS, EPR, CV and EIS to characterize and analyze. Also, it was deemed as a prospective cathode to accomplish industrialization for CIP degradation, based on lower energy consumption and wide pH range.
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