ENVIRONMENTAL RESEARCH
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2021
·
IF 6.498
Lingxiao Xue,Lijing Hao,Hui Ding,Rui Liu,Dan Zhao,Jianfeng Fu,Mengling Zhang
Glyphosate , a common broad-spectrum herbicide, is a serious environmental pollutant that causes a significant threat to humans. Hence, there is a pressing task to remove glyphosate from the environment. Here, we report an excellent Fe 3 Ce 1 O x catalyst synthesized via the one-step co-precipitation method for activating peroxymonosulfate (PMS) to degrade glyphosate at 25 °C. As a result, glyphosate is completely degraded with a high degradation rate of 400 mg L −1 ·h −1 , and the TOC and TN removals are 85.6% and 80.8%, respectively. As proven by systematic characterizations, the Fe–Ce synergistic effect plays a significant role in promoting PMS activation . The main reactive oxygen species for glyphosate oxidation are surface-bound SO 4 − · and ·OH, produced by activating PMS by electron transfer between Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ of Fe 3 Ce 1 O x . In light of the products determined, the possible degradation process of glyphosate is also speculated: C–N and C–P bonds of glyphosate molecules are attacked to form aminomethylphosphonic acid (AMPA) and orthophosphate (PO 4 3− ) by surface-bound SO 4 − · and ·OH that continuously mineralize and dephosphorylate AMPA to generate small molecules and inorganic ions, such as H 2 O and PO 4 3− . The results of this work suggest that Fe 3 Ce 1 O x /PMS could provide a potential candidate for efficiently removing organic compounds containing nitrogen or phosphorus from wastewater.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yiwei Li,Yaohong Ma,Eric Lichtfouse,Jin Song,Rui Gong,Jinheng Zhang,Shuo Wang,Leilei Xiao
Para-Nitrophenol ( p -nitrophenol) is a common industrial pollutant occurring widely in water bodies, yet actual monitoring methods are limited. Herein we proposed a fully electrochemically in situ synthesized graphene-polyarginine composite functionalized screen printed electrode, as a novel p-nitrophenol sensing platform. The electrode was characterized by morphologic, spectrometric and electrochemical techniques. p -nitrophenol in both pure aqueous solution and real water samples was tested. Results show a detection limit as low as the nanomolar level, and display a linear response and high selectivity in the range of 0.5–1250 μM. Molecular simulation reveals a detailed synergy between graphene and poly-arginine. The preferable orientation of nitrophenol molecules on the graphene interface in the presence of poly-arginine induces H- and ionic binding. This sensor is an ideal prototype for p -nitrophenol quantification in real waters.
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高影响因子
MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 8
·1-8
·
IF 5.833
Hu Cong Yi,Jiang Zhong Wei,Huang Cheng Zhi,Li Yuan Fang
Based on the laccase-mimicking activity of Cu 2+ -modified University of Oslo (UiO) metal–organic framework (UiO-67-Cu 2+ ), we developed a colorimetric sensor array for distinguishing a series of phenols with different number and position of substituted hydroxyl group (-OH) and different substituent group on the benzene ring, including phenol, catechol, quinol, resorcinol, pyrogallol, phloroglucinol, o -chlorophenol, o -aminophenol, and o -nitrophenol. The highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) energy levels of phenolic compounds were obtained by theoretical calculation. The results show that the lower the LUMO energy level, the easier the chromogenic reaction occurs. The UiO-67-Cu 2+ -catalyzed phenol chromogenic reaction showed a good linearity in the range from 0.1 to 200 μM with limit of detection approximately 61 nM. Through the detection of phenol in tap water and river water, the recovery rate and RSD ( n = 3) were calculated as 94.1~103% and 1.0~3.3, respectively, showing good recovery, reliable results, and outstanding stability. Therefore, the proposed colorimetric sensor array will have a great potential for the detection of phenols in the environment. Graphical abstract
Schematic presentation of a simple and sensitive colorimetric strategy based on the laccase-mimicking activity of Cu 2+ -modified UiO-type metal–organic framework (MOFs, Uio-67-Cu 2+ ) to distinguish phenols with analogous structures.
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高影响因子
FUEL
·
2021
·
IF 6.609
Mingqiang Chen,Jingjing Shi,Yishuang Wang,Zhiyuan Tang,Zhonglian Yang,Jun Wang,Han Zhang
Highly efficient conversion of lignin to value-added liquid fuel or phenol monomers has attracted widespread attentions. The W-Ni-Mo/SEP trimetallic catalyst was firstly prepared and used for lignin catalytic depolymerization (LCD) under supercritical ethanol, which significantly ameliorated the problem of complex product compositions and poor cycle-stability in Mo/SEP. Characterization results confirmed that doping W and Ni metals led to the transformation of metallic oxide phases, and then increased oxygen vacancies (O V ), enhanced the metal-support interaction, and lowered acid site content. The experimental results revealed that W-Ni-Mo/SEP yielded 39.56% of lignin oil (LO) with 32.37 MJ/kg of HHV at 280 °C for 4 h. The selectivity to guaiacol and ethoxyphenol monomer was remarkably increased as compare with Mo/SEP. Furthermore, the W-Ni-Mo/SEP catalyst exhibited unique cycle stability and produced LO even increased to 41.41% after five LCD cycles. The possible reaction paths of lignin converted to guaiacol and ethoxyphenol over W-Ni-Mo/SEP were proposed. Brønsted-acid site promoted the self-activation of ethanol to form aliphatic products. The higher O V preferentially adsorbed phenol-intermediates containing dual oxygens and activated direct dealkylation to obtain guaiacol. The lower Lewis-acid site promoted the demethylation of methoxy in side-chains of phenol-intermediates and then interacted with free ethyl groups to form ethoxyphenol.
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ENVIRONMENTAL TECHNOLOGY
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2021
·
IF 3.247
Binchao Lu,Liang Wang,Xin Zheng,Zhongce Hu,Zhiyan Pan
Environmental contamination by 4-chlorophenol (4-CP) is a major concern. Photosynthetic bacteria have the ability to biodegrade 4-CP under dark aerobic conditions. In this study, we found that using different carbon sources (i.e. glucose, sodium acetate, sodium propionate sucrose, and malic acid) as co-metabolic substrates accelerated the biodegradation of 4-CP, and this acceleration was especially pronounced in the glucose treatment. A maximum degradation rate of 96.99% was reached under a concentration of 3.0 g·L−1 after 6 days of culture. The optimum conditions were pH 7.5, a temperature of 30°C, and a rotation speed of 135 rpm. The biodegradation of 4-CP was achieved at a range of salinities (0–3.0% NaCl, w/v). The biodegradation kinetics agreed with the Haldane model, and the kinetic constants were rmax = 0.14 d−1, Km = 33.9 mg·L−1, and Ki = 159.6 mg·L−1. Additionally, the coexistence of phenol or 2,4-dichlorophenol (2, 4-DCP) had a certain impact on the degradation of 4-CP under dark aerobic conditions. When the coexisting phenol concentration reached 100 mg·L−1, the maximum degradation rate of 4-CP reached 90.20%. The degradation rate of 4-CP decreased as the concentration of coexisting 2, 4-DCP increased.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Xinyao Zou,Chao Ma,Ang Li,Zhan Gao,Zulipiya Shadike,Kun Jiang,Junliang Zhang,Zhen Huang,Lei Zhu
Electrochemical conversion of CO2 to the syngas hybrid with the Fischer–Tropsch (FT) process is a promising way to produce synthetic fuels from renewable energy sources. The product distribution in liquid hydrocarbons produced by FT synthesis has strong dependence on the CO/H2 ratio of the syngas feedstock. Herein, we demonstrated the feasibility of tuning the CO/H2 ratio at a wide range by developing nanoparticle-assisted Ni–Co binary single-atom catalysts for electrocatalytic production of syngas. By controlling the elemental proportion of Ni–Co in the composite catalysts, electrochemical reduction of CO2 to syngas with a tunable CO/H2 ratio from 0.3 to 27.6 was achieved. For the binary catalysts with a Ni–Co ratio of 1:1, the CO/H2 ratio maintains at 1.3–1.5 in a broad potential range from −0.59 to −0.83 V versus reversible hydrogen electrode (RHE) and the total current density reaches ∼32.2 mA/cm2 at −1.0 V versus RHE. The promotion effect of nanoparticles on Ni–Co single-atom catalysts was validated by partial removal of nanoparticles and further density functional theory (DFT) calculations. As revealed by DFT calculations, nanoparticles incorporated in single-atom sites take essential roles in facilitating the adsorption of CO2 and the formation of *COOH. The origin of CO2RR and hydrogen evolution reaction reactivities can be identified as Ni–N4 and Co–N4 single-atom sites, respectively. The dual active sites allow the facile control of the CO/H2 ratio of electrochemical converted syngas, and it will be beneficial to downstream production of diverse chemicals.
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Nano Research
·
2021
·Vol. 14
·期 11
·4304-4313
·
IF 8.897
Zhai Yi,Wang Fumin,Zhang Xubin,Lv Guojun,Wu Yuzhou,Jiang Tao,Zhang Qing,Li Mengyue,Li Mengyao,Liu Yongkui
How to directionally design the hollow zeolite via a green route is of great significance. Here, we successfully synthesized the hollow Fe-silicate-1 encapsulated ultra-small Fe 2 O 3 nanoparticles (2.5 nm) with higher yield (85.2%) by mother liquid than traditional dissolution-recrystallization for the first time, which was achieved by precisely regulating the number and distribution of defects in zeolite and cleverly utilizing the TPAOH and nuclei in mother liquor. The effects of synthetic temperature, synthetic period and addition amount of parent zeolite on the formation of hollow zeolite have been investigated and the effect of synthetic conditions on the defects in parent zeolite has been also firstly quantified. The corresponding formation mechanism has been proposed. The abundant inner defects provided by the zeolite synthesized at 130 °C for 1 day and large amount of TPAOH remaining in mother liquid are conducive to the formation of hollow zeolite. Meanwhile, both parent zeolite and nuclei (4-, 5-member rings and structure units) in mother liquid obtained at 130 °C play the crucial roles in enhancing the zeolite yield. Notably, Fe 2 O 3 nanoparticles could decompose into small fragments by the interaction with nuclei in mother liquid. Partial ultra-small Fe 2 O 3 nanoparticles would be encapsulated in cavity and the rest could be inserted in the zeolite framework, which is significantly different from the conventional dissolution-recrystallization mechanism. The obtained encapsulated catalyst shows the superior catalytic performance and stability in phenol and tetracycline degradation reactions.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 7
·077517
·
IF 4.316
Ziyu Zhao,Jialun Luo,Simon Tricard,Jihua Zhao,Qiangming Wang,Jian Fang
The development of effective and accurate catechol (CC) electrochemical sensors is critical for environment and life health perspectives. A facile pyrolysis of 2D bimetallic (Zn/Co) zeolitic imidazolate framework (Zn/Co-ZIF-L) was employed to prepare Zn and Co nanoparticles encapsulated in N-doped porous carbon (Zn/Co@NPC). Prussian blue (PB) was synthesized in situ via the co-precipitation of ferricyanide ([Fe(CN)6]3−) and iron (II) ion originated from the reduction of Fe3+ by Zn/Co@NPC and then served as the main active substance of CC detection. The morphology and composition of the final composite Zn/Co@NPC-PB were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and X-ray powder diffraction (XRD). The Zn/Co@NPC-PB modified glass carbon electrode (GCE) exhibits two concentration linear ranges of 4.13 μM − 1.08 mM (R2 = 0.999) and 1.08 mM−11.82 mM (R2 = 0.999) for CC electrochemical detection with a limit of detection 1.05 μM (S/N = 3). At the same time, the Zn/Co@NPC-PB/GCE shows great selectivity to electrochemical oxidation behavior of CC in presence of 20 folds dihydroxybenzene interferents such as hydroquinone and resorcinol. Furthermore, it showed a long-term stability and near 100% recovery for the detection of a real sample in Yellow River water.
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ACS ES&T Engineering
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2021
·
IF 0
Cong Wang,Shao-Yi Jia,You Han,Yang Li,Yong Liu,Hai-Tao Ren,Song-Hai Wu,Xu Han
Enzymatic polymerization of phenolic contaminants to polyphenolics by H2O2 is an effective method to turn phenolic wastes to useful polymers. However, the sensitivities and the high costs of enzymes always limit their applications in the long-run treatment of industrial wastewater. In this study, a highly efficient CuO-persulfate (PS) system is reported to be a promising candidate for enzyme–H2O2 and shows high reactivity to polymerize various phenolic contaminants to polymers under alkaline conditions with the ratio of PS/phenolics less than 2.0. Compared with the generally accepted mechanism that the oxidizing species of SO4•– and ·OH generated during PS activation primarily contribute to the oxidation of various organic contaminants, quenching experiments, EPR (electron paramagnetic resonance) analysis and DFT calculations in this study indicate that PS is activated on CuO via a nonradical pathway under alkaline conditions, and the O–O bond in PS is moderately elongated from 1.45 to 1.58 Å. The inversely linear relationship between log kobs and BDEO–H values of various phenolics in the Hammett plot confirms H-abstraction from various phenolics under alkaline conditions. DFT calculations further reveal the formation of phenolic radicals after the activated PS abstracts H from phenolic −OH, followed by subsequent polymerization of phenoxyl radicals to polyphenolics. Characterizations of the oxidation products confirm that more than 80% phenolic contaminants have been transformed to polyphenolics. This study provides a new alternative for recovering various phenolic contaminants from industrial wastewater.
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Foods
·
2021
·Vol. 10
·期 8
·1755
·
IF 4.35
Zhili Sheng,Junmei Liu,Bao Yang
Astragalus membranaceusis a functional food with multiple bioactivities. It presents differentiated health benefits due to origins. Polysaccharides (APS) are the leading bioactive macromolecules ofA. membranaceus, which are highly related to its health benefits. However, the effect of origin on the structural characteristics of APSs remains unclear. In this work, polysaccharides from four origins were isolated and identified by NMR. The results showed APSs of four origins had identical monosaccharide composition and glycosidic linkage. Rhamnogalacturonan II pectins and α-(1→4)-glucan were the dominant polysaccharides. However, the level of methyl ester in pectins varied to a large extent. The molecular weight profiles of APSs were also different. Inner Mongolia APS had the largest percentage of 20–40 kDa polysaccharides. Molecular weight and methyl ester level were two important parameters determining the difference of APSs from four origins. These results were helpful to recognize the origin-related quality ofA. membranaceus.Keywords:glycosidic linkage;monosaccharide composition;NMR;pectin
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Xin Wang,Peike Cao,Kun Zhao,Shuo Chen,Hongtao Yu,Xie Quan
The electro-Fenton reaction is traditionally carried out in a batch or flow-by reactor. However, the electro-Fenton performance is restricted by low utilization efficiency of catalysts, limited contact time of reactants, and the slow mass transfer. In this work, a flow-through heterogeneous electro-Fenton reactor was designed by using absorbent cotton derived three-dimensional carbon fiber network with iron oxide nanoparticles loaded as cathode. This flow-through electro-Fenton system can electrochemically catalyze O 2 molecule to produce ·OH. During the continuous test, the phenol degradation and mineralization efficiency achieved 92.7% and 65.1%, respectively, demonstrating the efficient and stable performance toward pollutant elimination of flow-through electro-Fenton system. Moreover, the flow-through system was demonstrated to be effective in the pH range of 5 ~ 9, and powerful for various refractory organic pollutants degradation including sulfamethoxazole, atrazine and benzoic acid. The high heterogeneous electro-Fenton activity was mainly attributed to the continuous in-situ ·OH generation. This study offers a facile method to construct flow-through heterogeneous electro-Fenton device, which provides a promising technology for wastewater treatment with low cost, high performance and good stability.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yuzhou Xue,Zhenchao Lei,Wenxiao Zheng,Weijian Duan,Liuyi Zhu,Zhang Yan,Chunhua Feng
It is generally known that carbon supports with a large surface area are essential for dispersion of Pd catalysts and adsorption of pollutants (e.g., chlorinated compounds), thus enabling enhanced mass transfer and increased reaction kinetics. However, we demonstrate that, in spite of contributing to achieving highly dispersed Pd nanoparticles , a high-surface-area carbon support favoring fast adsorption of 2,4-dichlorophenol negatively impacts the catalytic activity of Pd. Comparisons of catalytic performance between Pd/activated carbon (AC) catalysts with different mass loadings in a 3D electrochemical dechlorination reactor suggested that Pd(60%)/AC outperformed Pd(10%)/AC, although the latter had smaller Pd catalysts and the amount of Pd was same in these experiments. We found that the dechlorination rate constant was inversely correlated to the adsorption rate constant at Pd loadings from 10% to 60%. We further verified that the use of C 3 N 4 , an optimal carbon support with low surface area that allows good dispersion of Pd nanoparticles (10%), is critical in accelerating the dechlorination reaction kinetics due to the improved accessibility of active sites to the pollutants. This study provides information on how to select optimal supporting materials with desirable features that avoid catalyst aggregation and pre-adsorption of pollutants when the supported Pd catalysts are used as the moveable particle electrodes.
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