RSC Advances
·
2021
·Vol. 11
·期 39
·24065-24071
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IF 3.361
Min Feng,Shaohua Wen,Xiaofang Chen,Die Deng,Xiupei Yang,Run Zhang
Hydroquinone (HQ) is poorly degradable in the ecological environment and is highly toxic to human health even at a low concentration. The colorimetric method has the advantages of low cost and fast analysis, which provides the possibility for simple and rapid detection of HQ. In this work, a new colorimetric method has been developed for HQ detection based on a peroxidase-like catalyst, α-Fe2O3@CoNi. This sweetsop-like α-Fe2O3@CoNi catalyst enables H2O2 to produce hydroxyl (˙OH), leading to the oxidization of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxTMB. In the presence of HQ, the blue oxTMB is reduced to colorless, which allows for colorimetric detection of HQ in water samples. This method has been validated by detecting HQ in water samples with high selectivity, rapid response, broad detection range (0.50 to 30 μM), and low detection limit (0.16 μM).
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Journal of Chemistry
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2021
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IF 2.506
Renjie Zhou,Gui Chen,Yuejun Ouyang,Hairui Ni,Nonglin Zhou,Bailin Xiang
Using MOF-5 as a template, the porous carbon (MDPC-600) possessing high specific surface area was obtained after carbonization and acid washing. After MDPC-600 was loaded with Cu ions, the catalyst Cu/MDPC-600 was acquired by heat treatment under nitrogen atmosphere. The catalyst was characterized by X-ray powder diffraction (XRD), N2 physical adsorption (BET), field emission electron microscope (SEM), energy spectrum, and transmission electron microscope (TEM). The results show that the Cu/MDPC-600 catalyst prepared by using MOF-5 as the template has a very high specific surface area, and Cu is uniformly supported on the carrier. The catalytic hydrogen peroxide oxidation reaction of phenol hydroxylation was investigated and exhibits better catalytic activity and stability in the phenol hydroxylation reaction. The catalytic effect was best when the reaction temperature was 80°C, the reaction time was 2 h, and the amount of catalyst was 0.05 g. The conversion rate of phenol was 47.6%; the yield and selectivity of catechol were 37.8% and 79.4%, respectively. The activity of the catalyst changes little after three cycles of use.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Jihong Xu,Peisheng Zhou,Penghui Shi,Yulin Min,Qunjie Xu
Concern about nitrogen-doped carbon materials for pollutant removal via nonradical pathway is mounting. In this study, graphite carbon nitride (g-C 3 N 4 ) was transformed into a high nitrogen-doped three-dimensional carbon material (N-CM) through the “metal template method”. The synthesized N-CM showed high efficiency in removing 2,4-dichlorophenol (2,4-DCP) via the activation of peroxymonosulfate (PMS). Under neutral condition, 2,4-DCP (0.2 g/L) was completely eliminated with 0.3 g/L PMS and 0.1 g/L N-CM900 in 30 min. Initial pH value, inorganic anions, and cycle experiments were selected to explore the availability of N-CM900/PMS. In addition, 1 O 2 dominated 2,4-DCP oxidation (about 60–70%), while the remaining 30–40% was contributed by the mediated electron transfer and N-CM-PMS*. Mechanism investigation suggested that graphitic nitrogen, the electron-rich ketonic groups and defects play a pivotal role in peroxymonosulfate activation . Combined with byproducts analysis, small-molecule acids, H 2 O and CO 2 were predominant. Overall, this study unveils a novel direction for the design of high nitrogen-doped carbon materials and improves the understanding of the coexistence of multiple mechanisms in the activation of PMS by nitrogen-doped carbon materials.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Qing Zhang,Yi Zhai,Fumin Wang,Xubin Zhang,Guojun Lv,Yongkui Liu,Mengyue Li,Mengyao Li
Hierarchical Fe-doped MFI/MCM-41 composites (Fe-HMZs) were one-pot hydrothermal synthesized by partial transformation strategy using conventional CTAB as a dual-functional template. The hierarchical Fe-doped MFI/MCM-41 composites possess ordered mesopores and crystallized MFI structure. The effect of addition amount of NaOH and CTAB as well as the type of the alkali source on the formation of hierarchical Fe-MFI/MCM-41 composites have been investigated in detail. In addition, the temperature-gradient treatment plays the vital roles in the formation of MFI and the possible formation mechanism has been proposed. The obtained hierarchical Fe-HMZ-40 sample exhibits outstanding catalytic performance for phenol hydroxylation and 48% of phenol conversion as well as 89% of dihydroxybenzene selectivity could be achieved, which are ascribed to the more accessible active sites endowed by the significant diffusion ability of ordered mesopores. Compared with Fe-MCM-41 sample, the hydrothermal stability is improved because of the presence of MFI structure.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Chuankun Yin,Qianna Xia,Jiao Zhou,Bowen Li,Yu Guo,Aimal Khan,Xiaoxia Li,Aihua Xu
The development of efficient and eco-friendly Mn-based catalysts for peroxymonosulfate (PMS) activation and revealing the mechanism are highly desired for pollutants removal in wastewater. In this study, a ternary mullite oxide YMn 2 O 5 (YMO) was synthesized for bisphenol A (BPA) degradation in the presence of PMS for the first time. Combined with XPS, EPR and TG, abundant surface labile oxygen species (O lab ) with a ratio of 39.7% were identified in the mullite materials, which was higher than that for α-, β-, γ- and δ-MnO 2 . YMO also exhibited higher interfacial conductivity and stronger interactions among the catalyst, PMS and BPA than other MnO 2 . Superior performance in BPA degradation was observed with YMO, and O lab was suggested as the main active sites, for the normalized first-order rate constant was linearly dependent on the ratio of the oxygen species. Chemical quenching experiments, EPR and open circuit potential suggested that the degradation of BPA was mainly caused by the direct electron transfer process through the reactive O lab -PMS complexes. The influence of YMO concentration, PMS concentration, solution pH, different anions and reaction temperature was thoroughly studied. Moreover, the intermediates were identified and the possible degradation pathways were proposed. This work demonstrated that mullite oxide YMO with enriched O lab species can be used as eco-friendly catalysts for efficient PMS activation to remove recalcitrant organic compounds in wastewater.
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Theranostics
·
2021
·
IF 11.556
Yiliang Wang,Weisheng Luo,Lianzhou Huang,Ji Xiao,Xiaowei Song,Feng Li,Yuying Ma,Xiaohui Wang,Fujun Jin,Ping Liu,Yexuan Zhu,Kaio Kitazato,Yifei Wang,Zhe Ren
Microglia are the primary cellular source of type I interferons (I-IFNs) in the brain upon neurotropic virus infection. Although the I-IFN-based antiviral innate immune response is crucial for eliminating viruses, overproduction led to immune disorders. Therefore, the relatively long-lasting I-IFNs must be precisely controlled, but the regulatory mechanism for the innate antiviral response in microglia remains largely unknown. Long non-coding RNAs (lncRNAs) are being recognized as crucial factors in numerous diseases, but their regulatory roles in the innate antiviral response in microglia are undefined. Methods: The high-throughput RNA sequencing was performed to obtain differentially expressed lncRNAs (DELs) in primary microglia infected with or without the neurotropic herpes simplex virus type 1 (HSV-1). We selected four DELs ranked in the top 15 in basic level and their fold change induced by HSV-1, i.e., FPKM HSV-1 /FPKM Cells .We subsequently found a key lncRNA affecting the innate antiviral response of microglia significantly. We next used dual-luciferase reporter assays, bioinformatical tools, and truncation mutants of both lncRNA and targeted proteins to elucidate the downstream and upstream mechanism of action of lncRNA. Further, we established microglia-specific knock-in (KI) mice to investigate the role of lncRNA in vivo . Results: We identified a long intergenic non-coding RNA, linc-AhRA, involved in regulating the innate antiviral response in murine microglia. linc-AhRA is activated by aryl hydrocarbon receptor (AhR) and restricts I-IFN production in microglia upon neurotropic herpesvirus infection and innate immune stimulation. Mechanistically, linc-AhRA binds to both tripartite motif-containing 27 (TRIM27) and TANK-binding kinase 1 (TBK1) through its conserved 117nt fragment as a molecular scaffold to enhance TRIM27-TBK1 interaction. This interaction facilitates the TRIM27-mediated ubiquitination of TBK1 and results in ubiquitin-proteasome-dependent degradation of TBK1. Consequently, linc-AhRA suppresses I-IFN production through facilitating TBK1 degradation and limits the microglial innate immune response against neurotropic herpesvirus infection. Microglia-specific KI of linc-AhRA mice shows a weakened antiviral immune response upon neurotropic herpesvirus challenge due to a reduction of TBK1 in microglia. Conclusion: Our findings indicate that linc-AhRA is a negative regulator of I-IFN production in microglia to avoid excessive autoimmune responses. These findings uncover a previously unappreciated role for lncRNA conserved fragments in the innate antiviral response, providing a strong foundation for developing nucleotide drugs based on conserved functional fragments within lncRNAs.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yi Jia,Yi-Gang Ji,Qi Xue,Fu-Min Li,Guang-Tao Zhao,Pu-Jun Jin,Shu-Ni Li,Yu Chen
The nitrate electroreduction reaction (NO3–-ERR) is an efficient and green approach for nitrate remediation, which requires a highly active and selective electrocatalyst. In this work, porous and amorphous cobalt phosphide nanoshuttles (CoP PANSs) are successfully synthesized by using Mg2+ ion-doped calcium carbonate nanoshuttles (Mg-CaCO3 NSs) as the initial reaction precursor via precipitation transformation and a high-temperature phosphidation strategy. Various physical characterizations show that CoP PANSs have porous architecture, amorphous crystal structure, and big surface area. Electrochemical measurements reveal for the first time that CoP PANSs have outstanding electroactivity for NO3–-ERR in a neutral electrolyte. At an applied potential of −0.5 V vs reversible hydrogen electrode, CoP PANSs can achieve a high Faraday efficiency (94.24 ± 2.8%) and high yield rate (19.28 ± 0.53 mg h–1 mgcat–1) for ammonia production, which exceeds most reported values at various electrocatalysts for NO3–-ERR. Thus, the present result indicates that cobalt phosphide nanomaterials have promising application for NO3–-ERR.
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高影响因子
FUEL
·
2021
·
IF 6.609
Mingxing Zhao,Jun Hu,Shiliang Wu,Liu Yang,Xue An,Peng Yuan,Ping Lu
Cyclohexanols, promising oxygenated fuel additives and value-added chemicals, can be obtained by hydrodeoxygenation (HDO) of lignin-derived phenolics. Here, an N-doped bimetallic RuCoN x /NC catalyst was facilely prepared for HDO by direct pyrolysis of chitin impregnated with precursors of Ru and Co. Characterization of RuCoN x /NC with N 2 sorption, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and NH 3 temperature-programmed desorption (NH 3 -TPD) reveal that the metallic particles of electron-deficient Ru species and electron-enriched Co species were uniformly anchored on the micro-mesoporous N-doped carbon matrix with high dispersion and nano-scale size. The abundant accessible active sites and continuous spillover of H from Ru to Co make RuCoN x /NC an excellent HDO catalyst. 4-Propylguaiacol, a typical phenolic compound from lignin degradation, was hydrodeoxygenated into 92% 4-propylcyclohexanol over RuCoN x /NC at 210 ℃. With temperature increasing, propylcyclohexane became the major product, possessing 95% selectivity at 280 °C after 6 h. Reusability tests show that RuCoN x /NC can be recycled four times without the loss of conversion and initial selectivity. HDO of other phenolic compounds confirms the general applicability of RuCoN x /NC.
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Molecular Catalysis
·
2021
·
IF 5.062
Junyi Liu,Xianxiang Liu,Qiong Xu,Dulin Yin
A series of highly active and ortho -position selective catalysts based on (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were proposed for the C -methylation of phenol with methanol. The (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were synthesized by coprecipitation method of Fe and V elements and microwave drying. The chemical composition, material structure, acid-base properties, and structure-activity relationship of (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were systematically analyzed by the techniques of XRD, XPS, TEM, N 2 adsorption-desorption, Raman, UV-Vis, ESR, NH 3 /CO 2 -TPD and Pyridine-IR. The (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts have the double advantages of high activity and high stability for the methylation of phenol due to the high BET surface area, large total pore volume, dispersive active sites and enhanced acid-base property. o -cresol and 2,6-xylenol were the main products, and nearly 100% selectivity to the ortho -position of phenol and 90% selectivity to o -cresol were obtained. Furthermore, the (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts possess long lifetime over 2500 h and high activity at a weight hourly space velocity of 1.6 h −1 compared with the microwave-dried α-Fe 2 O 3 catalyst. The doping of vanadium improves the activity and stability of α-Fe 2 O 3 catalyst, which attributes to the modification of catalyst structure, especially the improvement of acid-base centers and oxygen vacancy. Recently the (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts have been stably and efficiently applied in industry for the methylation of phenol.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Mengyue Li,Yi Zhai,Xubin Zhang,Fumin Wang,Guojun Lv,Mengyao Li,Qing Zhang,Yongkui Liu
It is of great significance to develop a novel strategy to synthesize hollow zeolite without using mesoporogens due to its extremely short diffusion length. Ferric nitrate as a common iron source and structure direction agent has been used for synthesizing Fe-doped zeolite. However, the effect of ferric nitrate on the morphology of zeolite has not yet been elaborated. Here, we successfully synthesized hollow MFI zeolite with a framework iron-rich surface by using ferric nitrate as an iron source and seed-assistant strategy. It is the first time to propose that inorganic iron has the hollow structure-directing effect. Herein, by comparatively investigated the effect of iron content on the structure and evolution process of hollow zeolite, a novel crystallization mechanism has been proposed based on the competitive relationship between crystallization and dissolution rates. When the Si/Fe ratio reaches 25, the internal dissolution rate of seeds is faster than the surface crystallization rate of zeolite, the hollow structures are acquired. The obtained Fe-doped hollow zeolite exhibits superior catalytic performance for the reaction of phenol degradation. In this reaction, the higher effectiveness factor (η) close to 1 of Fe-doped hollow zeolite confirmed by calculations indicates its superior mass transferability.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Shi-Lei Ji,Hai-Long Qian,Cheng-Xiong Yang,Xu Zhao,Xiu-Ping Yan
We report a thiol–ene click strategy for the preparation of a novel phenylboronic acid-functionalized covalent organic framework (COF) for selective removal of catechol in aqueous solution. Vinyl-functionalized 2,5-diallyloxyterephthalaldehyde (Da-V) was prepared as a building ligand. Da-V was then condensed with 1,3,5-tris(4-aminophenyl)benzene (Tab) to give a vinyl-functionalized COF DhaTab-V. Subsequently, 4-mercaptophenylboronic acid (4-MPBA) was covalently linked on DhaTab-V via thiol–ene click reaction to give phenylboronic acid-functionalized COF DhaTab-PBA. The adsorption isotherms, energetics and kinetics, and reusability of DhaTab-PBA for the adsorption and removal of catechol from aqueous solution were investigated in detail. This phenylboronic acid-functionalized COF is promising as sorbent for selective removal of catechol from aqueous medium with large adsorption capacity and good reusability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Xiaomeng Dou,Xiao Jiang,Wenzhi Li,Chaofeng Zhu,Qingchuan Liu,Qiang Lu,Xusheng Zheng,Hou-min Chang,Hasan Jameel
Kraft lignin depolymerization to liquid fuels with high yields is crucial to the comprehensive achievement of sustainable and economic feasibility. Herein, we prepared a bimetallic Co-Zn/Off-Al H-beta catalyst through a two-step post synthesis method composed of dealumination and metal incorporation. The bifunctional Co-Zn/Off-Al H-beta catalyst efficiently converted Kraft lignin to liquid fuels, which was attributable to the synergistic effect of Co hydrogen binding sites and Zn Lewis acid sites on H-beta support. Catalytic hydrogenation with Co:Zn = 1:3/Off-Al H-beta catalyst at 320 °C for 24 h gave the highest yield of petroleum ether soluble product (81%, mainly monomers and dimers). Under these conditions, the liquefied lignin gave a higher heating value of 33.3 MJ/kg, which is a significant increase from 26.0 MJ/kg of Kraft lignin. The catalyst stability test showed excellent recyclability. This work provides a paradigm of improving lignin depolymerization efficiency via the combined use of Lewis acid and hydrogenation catalyst.
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