APPLIED CATALYSIS B-ENVIRONMENTAL
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2015
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IF 7.435
Shenyu Lan,Ya Xiong,Shuanghong Tian,Jinxi Feng,Tianyao Xie
A new insight into the degradation of CuEDTA with UV/H 2 O 2 was performed. It was found that the degradation was an UV-enhanced self-catalytic process with two main stages. The first was the induction stage in which cupric ions were produced in CuEDTA degradation with UV photolysis or/and H 2 O 2 oxidation . The second was the photo-catalytic degradation stage in which CuEDTA was oxidized by UV-enhanced cupric ion-based Fenton process. The degradation efficiency reached as high as 82.2% during 18 min, being 37.4 times higher than the efficiency sum of single H 2 O 2 oxidation and single UV photolysis. The enhancement effect can be contributed to the synergetic interaction between H 2 O 2 , cupric ion and UV, specially, to the excellent photo-activity of copper-peroxide intermediates. One of them was identified to be CuO 2 by analysis of its CE-C 4 D electropherograms, UV–vis adsorption spectra, FT-IR spectra, Raman spectra, especially XPS spectra. The enhancement mechanism was experimentally confirmed to be due to the acceleration of Cu(II)-to-Cu(I) transform by the photolysis of copper-peroxide intermediates, leading to the increasing CuEDTA degradation.
研究领域:
环境科学
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化学工程
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Qiong-Qiong Ren,Jing Wu,Wen-Chao Zhang,Chang Wang,Xin Qin,Guo-Chang Liu,Zhen-Xin Li,Yi Yu
Single-walled carbon nanotubes (SWCNTs), horseradish peroxidase (HRP), and 1-butyl-3-methylimidazolium tetrafluoroborate (BMIM·BF 4 ) were employed to construct a cellular H 2 O 2 sensor based on direct electron transfer. At a working potential of −0.35 V, HRP-BMIM·BF 4 /SWCNTs/CFUME showed a dynamic range of up to 10.2 μM with a low detection limit of 0.13 μM (S/N = 3) and a high sensitivity of 4.25 A/M cm 2 . The apparent Michaelis-Menten constant ( K m,app ) was estimated to be as low as 15.4 μM, which suggested that HRP molecules entrapped in the BMIM·BF 4 and SWCNTs immobilized at the carbon fiber ultramicroelectrode maintained a very high affinity. Because of the extremely small dimension and low working potential, HRP-BMIM·BF 4 /SWCNTs/CFUME enabled direct amperometric real-time monitoring of H 2 O 2 in HeLa cells treated with the anticancer drug, camptothecin, without requiring complex data processing and extra surface coatings to prevent interference. HRP-BMIM·BF 4 /SWCNTs/CFUME testing clearly showed that the H 2 O 2 level significantly increased in HeLa cells under camptothecin stress. When HeLa cells were cultured in medium without camptothecin, the H 2 O 2 level remained stable during the whole measurement process. These results indicate that HRP-BMIM·BF 4 /SWCNTs/CFUME could be a powerful tool for real-time investigation of cellular H 2 O 2 level, especially under anticancer drug stress. This method could provide in-depth insights regarding the occurrence, development, and apoptosis of tumors.
研究领域:
分析化学
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生物医学
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肿瘤学
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高影响因子
Royal Society Open Science
·
2019
·Vol. 6
·期 12
·
IF 2.515
Yan Wang,Hui-qiang Li,Li-ming Ren
The electro-Fenton (EF) process was applied to treat mother liquor of gas field wastewater (ML-GFW). The Fe-Fe electrodes were used and H2O2 was added to the EF system. Effect of initial pH on chemical oxygen demand (COD) removal efficiency, specific electrical energy consumption (SEEC), specific electrode plate consumption (SEPC) and organic matter removal mechanism was investigated. The results showed that COD removal efficiency reached the maximum (71.9%) at initial pH of 3 after reaction for 3 h. Besides, considering with the SEEC and SEPC, pH of 3 was also the best choice, at which SEEC was 4.7 kW h kgCOD−1, SEPC was 0.82 kgFe kgCOD−1. Organic matter removal was achieved by two ways: oxidation and flocculation, and oxidation played a major role. With the analysis of GC-MS, the possible degradation pathways of the representative contaminants in the ML-GFW were given.
研究领域:
环境科学
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废水处理
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Yingshi Zhu,Shan Qiu,Fengxia Deng,Fang Ma,Yanshi Zheng
In this work, nitrogen-doped cathodes for high H 2 O 2 production and sulfathiazole (STZ) degradation in electro-Fenton (EF) systems were prepared by the carbonization of three carbon/nitrogen-enriched precursors. Among the cathodes elaborated from different precursors, the one using 1h-1,2,4-triazole-3,5-diamine as the precursor showed the best oxygen reduction reaction (ORR) ability with the normalized H 2 O 2 accumulation of 9.49 ± 0.03 mg L −1 h −1 cm −2 compared to the other two N-containing cathodes. The enhanced H 2 O 2 accumulation was attributed to the high electroactive surface area and pyrrolic N (60.45%) content. Regarding reactive oxygen species in the absence of Fe 2+ , aside from the H 2 O 2 , O 2 − and 1 O 2 were identified using spectroscopic techniques and chemical probes. As a result, a degradation and mineralization efficiency of 98.25 ± 0.14% and 70.57 ± 0.27% of STZ were attained in the 180-min treatment, mainly coming from the homogeneous OH from classical Fenton , anodic OH on BDD anode and direct/indirect oxidation of O 2 − and 1 O 2 . In addition, the plausible degradation pathway of STZ was proposed based on the density functional theory (DFT) combined with experimental data derived by ultra-performance liquid chromatography tandem mass spectrometry (UPLC-MS/MS). The frontier orbital theory and Fukui function theoretically suggested the vulnerable sites of STZ for different active species including OH, O 2 − and 1 O 2 . This study provides a new strategy for improving the ORR process and analyzing the generation and conversion of reactive oxygen species in the EF process.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
Scientific Reports
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2016
·Vol. 6
·期 1
·1-11
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IF 5.228
Xiang Wei,Zhang Beiping,Zhou Tao,Wu Xiaohui,Mao Juan
This study demonstrated the synergistic degradation of 4-chlorophenol (4-CP) achieved in a magnetic field (MF) enhanced zero-valent iron (ZVI)/H 2 O 2 Fenton-like (FL) system and revealed an interesting correlative dependence relationship between MF and the pristine iron oxides layer (Fe x O y ) on ZVI particles. First, a comparative investigation between the FL and MF-FL systems was conducted under different experimental conditions. The MF-FL system could suppress the duration of initial lag degradation phase one order of magnitude in addition of the significant enhancement in overall 4-CP degradation. Monitoring of intermediates/products indicated that MF would just accelerate the Fenton reactions to produce hydroxyl radical more rapidly. Evolutions of simultaneously released dissolved iron species suggested that MF would not only improve mass-transfer of the initial heterogeneous reactions, but also modify the pristine ZVI surface. Characterizations of the specific prepared ZVI samples evidenced that MF would induce a special evolution mechanism of the ZVI particles surface depending on the existence of Fe x O y layer. It comprised of an initial rapid point dissolution of Fe x O y and a following pitting corrosion of the exposed Fe 0 reactive sites, finally leading to appearance of a particular rugged surface topography with numerous adjacent Fe 0 pits and Fe x O y tubercles.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
Environmental Science-Nano
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2021
·Vol. 8
·期 11
·3138-3152
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IF 8.131
Weirui Chen,Hengxi He,Ruini Zou,Yidan Chen,Xukai Li,Jing Wang,Yiming Tang,Laisheng Li
In this study, CeOx with different exposed facets was prepared to investigate their potential effect on activating the peroxone reaction (H2O2/O3) and breaking through the restriction of solution pH on peroxone. By controlling the concentration of hydroxide, cube CeOx with a (100) facet, rod CeOx with a (110) facet and octahedron CeOx with a (111) facet were prepared by the hydrothermal precipitation method, and they all promoted heterogeneous peroxone for oxalic acid (OA) under acidic conditions. The catalytic activity of CeOx was highly related to their surface oxygen vacancies (OVs) and the interfacial electron transfer process. Both experiments and theoretical calculations showed that CeOx with different exposed facets activated peroxone in different ways and (111) CeOx possessed better activity than (100) or (110) CeOx. The low efficiencies of (100) and (110) CeOx were due to their inefficient use of H2O2 to reduce surface Ce4+ and their large energy gap to generate surface peroxide (OVs-OOH). (111) CeOx was stable with surface-adsorbed H2O2, and the rich electrons at OVs could be donated to H2O2 and generate OVs-OOH, which then triggered O3 decomposition into hydroxyl radical (˙OH) and superoxide radical (˙O2−). These electron migration processes depended on the electron-donating ability of the OVs rather than solution pH, therefore, still greater amounts of reactive species were generated under acidic conditions. The flexibility of the (111) CeOx/H2O2/O3 process was further investigated for removing 20 kinds of pharmaceuticals. The synergy effect of (111) CeOx/O3 and H2O2 varied with the structure of the pharmaceuticals.
研究领域:
环境科学
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材料科学
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化学
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高影响因子
Journal of Energy Chemistry
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2026
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IF 15.6
Bo Wang,Xiaorui Huang,Wei Li,Wenjun Chen,Junwei Zhuo,Yongyi Li,Shuanglong Li,Huiyang Xu,Junyu Huang,Zimo Wang
In this work, we synthesize an unprecedented five-component high-entropy phthalocyanine framework (HE-MPcF), a new molecular framework fundamentally distinct from conventional monometallic or simple polymetallic phthalocyanines. We unambiguously validate that the prominent configurational entropy effect, rather than trivial metal synergism widely reported in ordinary multi-metal phthalocyanines, acts as the core driving force to modulate the intrinsic electronic and catalytic properties of the framework. The entropy-triggered disordered spatial distribution of five types of metal centers constructs continuous gradient electronic states and extensive built-in electric fields throughout the skeleton, which enables ultrafast charge separation and drastically inhibits unfavorable electron-hole recombination. Benefiting from this unique entropy-mediated structural and electronic regulation, the optimized two-electron oxygen reduction pathway is achieved, delivering efficient and highly selective photocatalytic H 2 O 2 evolution in pure water without sacrificial agents. Under visible-light irradiation, the HE-MPcF exhibits an outstanding H 2 O 2 production rate of 4183µmol g −1 h −1 together with a selectivity of 78%. Multiple in situ spectroscopic measurements, synchrotron characterizations, and density functional theory theoretical calculations jointly corroborate the entropy-dominated catalytic mechanism. This work establishes an entropy-engineering strategy for designing phthalocyanine framework photocatalysts, provides a platform to explore high-entropy effects in molecular catalysis, and offers guidance for developing sustainable photocatalysts for environmental energy conversion. By revealing why entropy engineering is essential for overcoming the intrinsic limitations of conventional phthalocyanine photocatalysts, how high-entropy molecular frameworks regulate charge dynamics and reaction pathways, and what new design principles they offer for selective H 2 O 2 photosynthesis, this work advances the fundamental understanding and practical development of molecular photocatalysis. A high-entropy phthalocyanine framework with multi-metal M–N 4 sites enables efficient sacrificial-agent-free photocatalytic H 2 O 2 production in pure water via synergistic 2e − oxygen reduction reaction (ORR) and 2e − water oxidation reaction (WOR) pathways. Download: Download high-res image (199KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Jiaqiao Yuan,Zhan Ding,Xiang Gong,Anmei Yu,Shuming Wen,Shaojun Bai
Efficient treatment of residual xanthate from tailing wastewater has attracted soaring interesting recently. Herein, effect of activated H 2 O 2 by natural ilmenite (FeTiO 3 ) as a catalyst on sodium butyl xanthate (SBX) degradation was systematically investigated. More than 98 % SBX degradation efficiency was achieved by the method under optimal conditions (a natural pH = 8.7, [FeTiO 3 ] 0 = 4.0 g/L, [H 2 O 2 ] 0 = 2.0 mM, and [SBX] 0 = 40.0 mg/L), and chemical oxygen demand (COD) removal rate was 85.41 %. Kinetic studies indicated that SBX degradation efficiency in FeTiO 3 -H 2 O 2 system conformed with a pseudo first order kinetic equation. Also, comparative experiments indicated that this system degraded SBX was superior to the H 2 O 2 alone and FeTiO 3 alone systems. Reactive oxygen species (ROS) were determined by quenching experiments and electron paramagnetic resonance (EPR) tests, suggesting that OH and O 2 − were the primary reactive radicals in FeTiO 3 -H 2 O 2 system. Cycling experiments and leaching metal ion tests suggested that FeTiO 3 still exhibited high catalytic activity and excellent stability after five times of recycling. Finally, possible degradation pathways and mechanism of SBX in this system were proposed. Consequently, this study promotes the application of natural iron-based minerals as a catalyst in wastewater treatment, and provides new insights into the effective treatment of organic pollutants in tailing wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Liyuan Wu,Chenjing Hou,Xin Wang,Pengpeng Guo,Xiaoran Zhang,Yi Jin,Yongwei Gong,Xudan Chen,Haiyan Li
The presence of chloride ions (Cl − ) in dye wastewater can hinder the peroxymonosulfate (PMS) oxidation and lead to the abundant production of toxic adsorbable organic halogens (AOX). In this study, we investigate the detailed influence of Cl − on Rhodamine B (RhB) removal and its mechanism, and propose a potential pathway for 1 O 2 -dominated systems to inhibit AOX formation. The concentration of Cl − has a dual effect on the degradation of RhB, with low concentrations inhibiting and high concentrations promoting. Further studies have revealed that Cl − significantly impact the generation and transformation of reactive oxygen species (ROSs). EPR capturing, quenching tests, and molecular probe experiments indicate that as the Cl − concentration increases, the concentration of SO 4 − , OH and their contribution to the degradation of RhB gradually decrease, 1 O 2 slightly increase and then decrease, while HClO and chlorine radicals increase linearly. Additionally, the catalyst plays a crucial role in inhibiting AOX formation and improving the mineralization of RhB. On the one hand, introducing catalysts can alter the proportion of ROSs production. On the other hand, the in-situ generation of H 2 O 2 on the catalyst surface, through O 2 adsorption at sulfur vacancies sites, consumes the produced HClO, thereby inhibiting the formation of AOX. This study proposed a new insight into the mechanism for effective reduction of AOX content for 1 O 2 dominated non-radical PMS activation under saline water.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Entong Ye,Zheng Chen,Yongyong Shi,Dan Zhang,Wenfei Li,Hong Qin,Ziming Luo,Quansheng Wu,Qian Lin,Hongyan Pan,Keliang Wang
Although a high-activity yield of hydrogen peroxide (H 2 O 2 ) can be achieved by direct synthesis from hydrogen and oxygen, developing an extreme catalyst with high activity and stability is still very challenging, which limits its industrial application. Here, we reported a catalyst Pd/SPE with polyelectrolyte membranes SPE as an electronic acceptor to anchor Pd, which achieves H 2 O 2 selectivity of 90.1% and productivity of 5764.4 mmol∙g Pd -1 ∙h −1 . The results of TEM, XRD and ICP-MS, XPS, CO-DRIFT, O 2 -TPD, synchrotron radiation and density functional theory (DFT) simulations reveal that the electrons of Pd are transferred into polyelectrolyte membranes and Pd clusters are strongly chemisorbed on SPE, which is beneficial for O 2 adsorption and inhibits the dissociation of O-O bond, leading to significantly enhanced H 2 O 2 productivity and selectivity.
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Frontiers in Nutrition
·
2023
·
IF 5
Zhang Lu,Deng Mei,Wang Si-yu,Ding Qiao,Liu Jia-hui,Xie Xing,Huang Yun-hong,Tu Zong-cai
Paeoniae Radix Alba (PRA), as a Traditional Chinese Medicine, is widely used in Chinese cuisine due to high health-benefits and nutrition, but the effect of different polarity of solvents on the extraction of antioxidant and hypoglycemic constituents, as well as the major active compounds remain unclear. In this research, 40, 70, and 95% ethanol were firstly applied to extract the polyphenols from PRA, the extraction yields, total phenolics, and total flavonoids content, free radical scavenging ability, α-glucosidase inhibition ability, and anti-glycation ability of extracts were evaluated spectroscopically. The oxidative damage protection, hypoglycemic activity, and alleviation on peripheral nerve damage were evaluated by H2O2-induced HepG2 cells and hyperglycemic zebrafish models. UPLC-QTOF-MS/MS was used to identify the major chemical constituents. The results showed that 40, 70, and 95% ethanol exhibited insignificant difference on the extraction of phenolics and flavonoids from PRA. All extracts showed promising DPPH⋅ and ABTS⋅+ scavenging ability, α-glucosidase inhibition and anti-glycation ability. In addition, PRA extracts could restore the survival rate of HepG2 cells induced by H2O2, and alleviate the oxidative stress by reducing the content of MDA and increasing the levels of SOD, CAT, and GSH-Px. The 70% ethanol extract could also mitigate the blood glucose level and peripheral motor nerve damage of hyperglycemic zebrafish. Thirty-five compounds were identified from 70% ethanol extract, gallotannins, gallic acid and its derivatives, and paeoniflorin and its derivatives were the dominant bioactive compounds. Above results could provide important information for the value-added application of PRA in functional food and medicinal industry.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Zhiwei Zhou,Yanyan Yao,Yanling Yang,Xing Li,Jiawei Ren,Jiangwei Qin
The physicochemical properties of powdered activated carbon (PAC) are important factors affecting its adsorption performance, which is also related to the characteristics of target organic pollutants . In this study, the key indicators affecting the adsorption performance of PAC were identified, and the physicochemical properties of PACs were modified by hydrogen peroxide and/or ultrasound in a targeted manner to improve the adsorption performance. The results indicated the adsorption properties of printing and dyeing secondary effluent organic matter (EfOM) in terms of COD cr and UV absorbance at 254 nm (UV 254 ) positively correlated with mesoporous volume, average pore size and acid group content of PAC. After modification, the mesoporous volume and average pore size of PAC increased, and the number of acidic groups increased, thus enhancing the adsorption efficiency. EfOM removal characteristics showed that PAC preferentially adsorbed unsaturated bonds or aromatic compounds , tryptophan-like proteins, soluble microbial metabolites and low molecular weight fractions below 1 kDa. In addition, the relative contents of specific surface area, pore volume and oxygen-containing functional groups (O-C O, C-OH, C O/O-C-O) of PAC decreased after adsorption, indicating that EfOM adsorption was a physical and chemical process, including pore filling, hydrophobic interaction and chemical bond force interaction. In general, PACs with larger mesoporous volume, average pore size and abundant acid groups possessed good adsorption performance towards EfOM.
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危险品化学品经营许可证（带存储）