JOURNAL OF SUPERCRITICAL FLUIDS
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2017
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IF 2.991
Chenyu Wang,Wei Zhu,Miao Gong,Ying Su,Yujie Fan
Dewatered sewage sludge was treated with H 2 O 2 and/or Ni in supercritical water in a high-pressure autoclave (400 °C, 23 MPa, 60 min). The combined application of H 2 O 2 and Ni was more effective than applying each separately for hydrogen production and for inhibiting the formation of polycyclic aromatic hydrocarbons (PAHs). The hydrogen yield (0.79–1.28 mol/kg organic matter) of combined additives with different Ni:H 2 O 2 ratios was 21% to 35% higher than the calculated value of the hydrogen yield from the mixture. The Ni:H 2 O 2 ratio affected the ring number composition of PAHs (proportion of 4–6 ring PAHs increased from 13% to 44% with increasing Ni:H 2 O 2 ratio) considerably, but had little effect on the concentration of PAHs. The mechanisms of the Ni/H 2 O 2 additive were also investigated from the viewpoint of combined action and intermediates. Overall, the method developed herein has the potential to promote hydrogen production in an environmentally compatible manner.
研究领域:
环境科学
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能源工程
·
催化化学
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MICROCHIMICA ACTA
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2018
·Vol. 185
·期 2
·1-8
·
IF 5.705
Chen Ying-Chu,Hsu Jui-Hung,Hsu Yu-Kuei
This study introduces a two-step method for the deposition of branched silver nanowires (AgNWs) on fluorine-doped tin oxide (FTO) glass. This material serves as both an active surface-enhanced Raman-scattering (SERS) substrate and as an enzyme-free electrochemical sensor for H 2 O 2 . This dual functionality is systematically studied. The AgNWs as the main trunk were first deposited on FTO by spray-coating. Silver branches were then electrochemically produced on the preformed NWs. Scanning electron microscopy, X-ray diffraction and X-ray photoelectron spectrometry were employed to characterize morphology, composition and microstructure. SERS experiments show that the branched AgNW/FTO substrate exhibits excellent performance in detecting 4-aminothiophenol at an ultra-low concentration of 0.1 fM. Simultaneously, this material displays an excellent electrocatalytic response to H 2 O 2 reduction at a concentration as low as 1 μM. The sensor has a rapid response and two linear analytical ranges that extend from 0.25 to 300 μM, and from 0.3 to 2.6 mM of H 2 O 2 , respectively. The ultrahigh sensitivity and satisfactory reproducibility highlights the merit of this hierarchical AgNW dendritic structure for sensing applications.
Branched silver nanowires can serve as both an active surface-enhanced Raman scattering substrate and as an electrochemical sensor for H 2 O 2 . This dual functionality is systematically investigated.
研究领域:
材料科学
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分析化学
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WATER RESEARCH
·
2018
·
IF 7.051
Tongcai Liu,Kai Yin,Chengbin Liu,Jinming Luo,John Crittenden,Weiqiu Zhang,Shenglian Luo,Qunying He,Yongxiu Deng,Hui Liu,Danyu Zhang
Oxcarbazepine (OXC) is ubiquitous in the aqueous environment. And due to its ecotoxicological effects and potential risks to human, an effective way to eliminate OXC from aqueous environment has aroused public concerns in recent years. Radical-based reactions have been shown to be an efficient way for OXC destruction, but the reactions of OXC with reactive oxygen species (ROS) and carbonate radical (CO 3 •− ) are still unclear. In this study, we focused the degradation of OXC and ROS, CO 3 •− generation mechanism, and their roles in OXC degradation via UV and UV/H 2 O 2 . The triplet state of oxcarbazepine ( 3 OXC ∗ ) was found to play an important role in OXC degradation via UV. And hydroxyl radicals ( • OH) and singlet oxygen ( 1 O 2 ) were found to be the dominant ROS in OXC degradation. Superoxide radical (O 2 •− ) did not react with OXC directly, but it may react with intermediate byproducts. Generation of CO 3 •− played a positive role on OXC degradation for both UV and UV/H 2 O 2 . In addition to • OH, 3 OXC* also contribute to CO 3 •− production. The second-order rate constants of OXC with • OH and CO 3 •− were 1.7 × 10 10 M −1 s −1 and 8.6 × 10 7 M −1 s −1 , respectively. Potential OXC degradation mechanisms by • OH were proposed and included hydroxylation, α-ketol rearrangement, and benzylic acid rearrangement. Compared with non-selective • OH, the reactions involving CO 3 •− are mainly electron transfer and hydrogen abstraction. And the acute toxicity of OXC was lower after UV/H 2 O 2 and UV/H 2 O 2 /HCO 3 − treatments, which was confirmed by luminescent bacterial assay ( Vibrio fischeri bacterium).
研究领域:
环境科学
·
毒理学
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ACS Sustainable Chemistry & Engineering
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2017
·
IF 5.951
Enmin Zong,Xiaohuan Liu,Lina Liu,Jifu Wang,Pingan Song,Zhongqing Ma,Jie Ding,Shenyuan Fu
Effective utilization of abundant industrial lignin has growingly attracted much attention besides potential environmental issues. Although chemical graft polymerization modification is one facile strategy for extending its applications, it remains an intractable challenge to select a highly efficient initiation system. We herein have attempt to understand the CaCl2–H2O2 system in initiating the graft polymerization of acrylic monomers onto acetic acid lignin (AAL) and biobutanol lignin (BBL). The initiation system is found to be highly efficient and selective, as proved by the successful graft of polyacrylates onto them, and a possible mechanism is also proposed. Thermal analysis shows that the graft modification results in a higher glass transition temperature and higher thermal stability of lignin. The graft modification make both AAL and BBL become more hydrophobic than before modification. Moreover, adding a small amount of lignin-graft-polyacrylate can considerably improve the UV blocking capability in addition to the reinforcing effect on polylactic acid. This work offers a novel, highly effective, and selective free radical initiation system for functionalizing lignin.
研究领域:
材料科学
·
化学工程
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuehua Shi,Tao Liu,Zhaoyang Wang,Xiaolong Zhao,Leyong Zeng
Nanocatalytic medicine was attracting considerable attention, owing to the specific treatment by the intrinsic chemical reactions within tumors. However, the insufficient hydrogen peroxide (H 2 O 2 ) and unsuitable pH value limited its application. Herein, a tumor microenvironment (TME) responsive multifunctional nanoprobe with self-accelerating cascade catalysis (MPB@CeO 2 -GOx) was developed for enhanced catalytic therapy, in which ultrasmall cerium oxide (CeO 2 ) and glucose oxidase (GOx) were modified on mesoporous Prussian blue (MPB). The developed MPB@CeO 2 @-GOx nanoprobes exhibited the dual-nanozyme activity of catalase (CAT) and peroxidase (POD), by which the O 2 and hydroxyl radical (·OH) were generated by Ce 4+ and Ce 3+ . Moreover, the sufficient O 2 promoted the glucose consumption of GOx , and the generated H 2 O 2 and gluconic acid further enhanced the catalytic therapy by reducing pH value, by which ·OH yield increased by 26.21%. In addition, the photothermal effect of MPB also significantly improved the POD activity of CeO 2 . Compared with MPB@CeO 2 , the cell survival reduced from 20.8% to 3.8%, and the tumor growth was completely inhibited. Therefore, by self-supplying O 2 /H 2 O 2 and reducing pH value, the developed MPB@CeO 2 -GOx nanoprobes with self-accelerating cascade reactions achieved PTT and enhanced catalytic therapy against breast cancer.
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MATERIALS RESEARCH BULLETIN
·
2023
·
IF 5.4
Luyao Jin,Xintao Xu,Yanghui Wang,Jiaying Li,Kaihao Fan,Bo Hu,Yi Shen,Xuesong Liu
A series of MnO x /TiO 2 based NO x reduction catalyst was prepared by excessive impregnation method. The catalyst was modified by Ce, W and oxidizing agent H 2 O 2 . Mn-Ce/Ti-H and Mn-Ce-W/Ti-H catalysts exhibit the best low temperature activity (nearly 80% NO x conversion at 155–325 °C) and the widest active temperature range (nearly 80% NO x conversion at 180–420 °C), respectively. Property and structure of the modified catalyst were characterized by XRD, TEM, XPS, H 2 -TPR, NH 3 -TPD, etc. It is found that oxidizing agent H 2 O 2 , as well as the high dispersion and specific surface area, can increase the amount of Mn 4+ , Ce 3+ and active oxygen sites on catalyst surface, and the synergistic interaction between Mn and Ce facilitated redox process of the catalysts. These can improve the low temperature activity of the catalyst by facilitating “fast SCR” reaction. The addition of W increased acidity of the catalyst and improved high temperature catalytic activity of the catalyst.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2023
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IF 6.1
Kunpeng Liu,Nan Wang,Jianhua Li,Fanglin Du,Baorong Hou,Ruiyong Zhang
Electrochemical two-electron water oxidation reaction (2e − WOR) to produce H 2 O 2 has been widely concerned. However, four-electron competition reaction causes the large overpotential and low production rates of 2e − WOR, which restrict its’ development and application. Herein, we prepared N-TiO 2 derived from NH 2 -MIL-125 by the hydrothermal combined with calcination method. We found that N-TiO 2 as photoanode exhibited the well properties of photoelectrocatalysis water oxidation, which gave an overpotential of 630 mV at 1 mA cm −2 . The overpotentials of N-TiO 2 was approximately 130 mV (at 1 mA cm −2 ) lower than NH 2 -MIL-125, and even lower than the previous reported TiO 2 , which may attribute to the increased oxygen vacancy with the calcination process and N doping. In addition, we investigated the degradation performance of the prepared catalysts to degrade methylene blue by photoelctrocatalysis on-site the preparation of H 2 O 2 . It was shown that N-TiO 2 performed high degradation efficiency (∼91%) and excellent stability. The possible mechanism was speculated due to the increased oxygen vacancy and N doping. This work provides a new idea for photoelectrocatalysis water oxidation materials and points out a new way for on-site H 2 O 2 production for direct use.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yanan Dong,Dong Wang,Yingchen Zhu,Qianwen Wang,Guocheng Liu,Qinghua Yan,Yucan Liu,Qinghua Chen,Dong Ma,Guangshan Zhang,Shuaishuai Xin,Yanjun Xin
The self-sufficient heterogeneous photo-Fenton (SH-PF) system was constructed for doxycycline hydrochloride (DOH) degradation with hydroxyapatite (Hap) modified CuFeO 2 (Hap/CuFeO 2 ) composites through H 2 O 2 in-situ production. The modification of Hap could improve the specific surface area, visible-light response, light conversion efficiency, photoelectron lifetime and oxygen vacancies (OVs) of CuFeO 2 , which was conducive to H 2 O 2 production and DOH degradation in SH-PF system. Notably, Hap/CuFeO 2 fabricated with 0.5 g Hap (Hap/CuFeO 2 -0.5) displayed more superior performance for DOH degradation compared to other synthesized catalysts. The Hap/CuFeO 2 -0.5 load and initial solution pH for DOH degradation in SH-PF system were optimized, and the Hap/CuFeO 2 -0.5 had good reusability and stability. The • OH was the main active species for DOH degradation, and the facilitation effect of • O 2 – and photoelectrons on DOH degradation was associated with the H 2 O 2 production in the present work. In addition, the capture of photogenerated holes suppressed the recombination of photogenerated carriers, elevating the production of photoelectrons and thereby enhancing H 2 O 2 production and DOH degradation. The degradation pathways for DOH were proposed and the comprehensive toxicities of DOH were relieved after degradation in SH-PF system.
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Frontiers in Nutrition
·
2023
·
IF 5
Lu Zhang,Chun-yan Peng,Pei-xin Wang,Linju Xu,Jia-hui Liu,Xing Xie,Ling Lu,Zong-cai Tu
Radix Paeonia Alba (RPA) is often used as food and medicine. This study aimed to enrich and identify the antioxidant and hypoglycemic bioactive compounds from RPA. The results indicated that the ethyl acetate fraction (EAF) showed the highest total phenolic content, DPPH, ABTS + scavenging ability, and α-glucosidase inhibition ability (IC 50 = 7.27 μg/ml). The EAF could alleviate H 2 O 2 -induced oxidative stress in HepG2 cells by decreasing the MDA and ROS levels, improving cell apoptosis, increasing the enzyme activity of GPX-Px, CAT, SOD, Na + /K + -ATP, and Ca 2+ /Mg 2+ -ATP, and stimulating T-AOC expression, which also enhanced the glucose uptake of insulin-resistant HepG2 cells. In addition, the EAF significantly reduced the fasting blood glucose level and improved glucose tolerance in diabetic mice. An HPLC-QTOF-MS/MS analysis displayed that procyanidin, digallic acid isomer, methyl gallate, tetragalloylglucose isomer, dimethyl gallic acid, and paeoniflorin were the major compounds in the EAF. These findings are meaningful for the application of the EAF in the medicinal or food industry to prevent and treat oxidative stress and diabetes mellitus.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Lei Zhang,Qimei Li,Jiaqi Zhu,Heng Liu,Xueling Liu,Yi Wang,Guozhi Fan,Yanjun Huang,Likun Li
In this study, a novel composite bead (MPB-ALG) was prepared by encapsulating H 2 O 2 modified peanut shell-derived biochar (MPB) into alginate matrix through a facile method. The structure and properties of prepared materials were characterized using FTIR , BET, SEM, and XPS . Batch adsorption experiments were performed to compare the Cu(II) adsorption performance of MPB, plain alginate beads (ALG), and MPB-ALG. The effect parameters of the components, solution pH, contact time, initial concentration, and coexisting ions were studied systematically. The results showed that the maximum adsorption capacity of the optimized MPB-ALG-1 (MPB/alginate = 1:1 w/w%) was 117.4 mg g −1 at pH 5, which was much higher than that of MPB (37.4 mg g −1 ). The adsorption kinetics and isotherms data of Cu(II) on MPB-ALG-1 were well described by Elovich kinetic model and Freundlich adsorption isotherm. Compared with plain ALG beads, MPB-ALG-1 exhibited better reusability and anti-interference of coexisting ions. Finally, the adsorption mechanisms of Cu(II) on MPB-ALG-1 beads were revealed by FTIR and XPS analysis. The experimental results demonstrated that MPB-ALG-1 beads can be used as an environmentally friendly and efficient adsorbent for the removal of Cu(II) from wastewater.
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Nano Research
·
2023
·Vol. 16
·期 10
·12106-12115
·
IF 9.9
Wang Siqi,Jin Yao,Ai Wenhui,Wang Xiufeng,Zhang Zhiqing,Zhou Ting,Zhang Guodong,Wang Fang
Unexpected benefits to the catalytic performance of materials often originate from the presence of surface defects. Here, novel D-penicillamine modified molybdenum oxide nanodots, with abundant oxygen vacancy defects, were fabrication by a mild, simple, and cost-effective method. Ultraviolet—visible (UV—Vis) absorption spectra analysis showed that the nanodots had peroxidase-like and catalase-like activities. The reactive oxygen species were probed by electronic paramagnetic resonance technique and spectroscopic methods, demonstrating that the nanodots also had oxidase-like activity. Interestingly, the peroxidase-like activity of nanodots was synergistically enhanced in the presence of ferrous ions or ferric ions. Remarkably, less than nanomolar levels of ferrous ions were required to display this phenomenon, meaning Fenton reagent acted as leverage. Based on this, a sensitive colorimetric and fluorescent dual-mode sensor for alendronate sodium was developed. The linear ranges for colorimetric and fluorescence analysis were 0.2–2.5 and 0.2–2.0 µM, with detection limits of 31.21 and 71.84 nM, correspondingly. The method has a simple large-scale material preparation process with higher sensitivity and shorter reaction time, which can inspire and enlighten the design of nanozyme sensors.
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PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2022
·Vol. 43
·期 2
·491-511
·
IF 3.337
Huang Shaoyong,Huang Quanjia,Gan Jiaming,Li Ting,Wang Lei
In this study, Fe-rich sludge was pretreated by dielectric barrier discharge (DBD) and used as a Fenton catalyst for the degradation of 2,4-dichlorophenoxyacetic acid (2,4-D) in aqueous solution, where hydrogen peroxide was in situ supplied from a glow discharge plasma (GDP) in contact with the solution. Synergistic mechanism of the two plasmas during 2,4-D degradation was explored. The Fe-rich sludge pretreated by H 2 -DBD could significantly accelerate the 2,4-D degradation as it converted Fe(III) in the sludge to the active Fe(II). 2,4-D can be completely removed in the presence of H 2 -DBD pretreated Fe-rich sludge with 25 min of GDP at pH 0 3.0 and catalyst dosage of 1.0 g/L. Quenching experimental studies showed that both ·OH (oxidative degradation) and ·H (reductive dechlorination) were responsible for 2,4-D degradation. Reducing radicals (such as ·R and·H) formed during GDP can continuously reduce the Fe 3+ back to Fe 2+ , which further promoted the degradation and dechlorination of 2,4-D. The results of three consecutive experiments indicated the stability and reusability of catalyst. This study provides a potential method for the recycle of Fe-rich sludge as a novel and cost-effective catalyst for 2,4-D removal from aqueous environments, which is significant for the terminal disposal of Fe-rich sludge. Graphical Abstract
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