ENVIRONMENTAL POLLUTION
·
2020
·
IF 6.793
Yuanyuan Peng,Wenhua Tong,Yi Xie,Wanrong Hu,Yonghong Li,Yongkui Zhang,Yabo Wang
Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation have attracted increasing attention in recent years for organic pollutants removal . Herein, we put forward a facile method to form cobalt phosphide/carbon composite for PMS activation. Combining impregnation approach with pyrolysis treatment enabled the formation of Co 2 P/biochar composites using baker’s yeast and Co 2+ as precursors. The as-synthesized products exhibited excellent catalytic activity for sulfamethoxazole (SMX) degradation over the pH range 3.0–9.0 b y activating PMS. For example, 100% of SMX (20 mg L −1 ) removal was achieved in 20 min with catalyst dosage of 0.4 g L −1 and PMS loading of 0.4 g L −1 . Near zero Co 2+ leaching was observed during catalytic reaction, which remarkably lowered the toxic risk of transition metal ion in water. Meanwhile, the reusability of catalyst could be attained by thermal treatment. SMX degradation intermediates were identified by liquid chromatography-mass spectrometry (LC-MS), which facilitated the proposal of possible SMX degradation pathways. Ecological Structure Activity Relationships (ECOSAR) analysis indicated that SMX degradation intermediates may not pose ecological toxicity to the environment. Further investigation verified that Co 2 P/biochar composites could set off PMS activation not only for the degradation of SMX but also for other sulfonamides. In this study, we not only developed a facile method of utilizing environmental-benign biomass for transition metal phosphide/carbon composite formation, but also achieved highly efficient antibiotic elimination by PMS-based AOP.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Murtaza Ali,Jun-Hu Cheng,Da-Wen Sun
This study investigated the effect of plasma-activated liquid (PAL) including plasma-activated water (PAW) and plasma-activated buffer solution (PABS) for the reduction of chlorothalonil (CTL) and thiram (THM) pesticide residues on tomato fruit. Results revealed that the PAL obtained by using atmospheric air as the feed gas, CTL residues were decreased to 85.3% and 74.2% and THM residues decreased to 79.47 and 72.21% after treatments with PAW 10 and PABS 10 , respectively, and increasing the activation time caused a significant reduction in fungicide residues. In addition, CTL and THM residues were also decreased while increasing the activation time of PAL using Ar/O 2 as the feed gas, the concentrations of the CTL residues were decreased to 75.07 and 69.89% for PAW 10 and PABS 10 , respectively and THM residues decreased to 65.89 and 61.91% for PAW 10 and PABS 10 , respectively. Oxidation-reduction potential (ORP) and electrical conductivity (EC) were increased significantly after plasma treatment, while pH values of both solutions were decreased significantly with activation time. NO 3 − and NO 2 − concentrations of PAW increased significantly, while for PABS, NO 3 − concentration decreased but NO 2 − , with increasing the plasma activation time. Additionally, washing with PAW and PABS caused no notable negative impact on tomato fruit. Results confirmed that PAL treatments showed a significant reduction of CTL and THM fungicide residues ( p < 0.05) in tomato without affecting the quality.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 12
·1-7
·
IF 5.479
Li Shuhuai,Ma Xionghui,Pang Chaohai,Tian Hai,Xu Zhi,Yang Yan,Lv Daizhu,Ge Huilin
A fluorometric assay is described for the determination of Cd(II) in environmental and agricultural samples. It is making use of a molecularly imprinted polymer (MIP) and aptamer as dual recognition units, while carbon quantum dots (co-doped with sulphur and nitrogen) and gold nanoparticles (SN-CQD/Au) act as the fluorophores. The aptamer-modified MIP was placed on an SN-CQD/Au-modified indium tin oxide glass electrode. Cd(II) was detected with high selectivity by the recognition sites of the aptamer in the MIP. Fluorescence, with excitation/emission peaks at 370/430 nm, is quenched by Cd(II). Response is linear in the 20 pM to 12 nM concentration range. The detection limit is 1.2 pM. The sensor is selective for Cd(II), and recoveries from spiked waters, soils and vegetables real-world samples range between 82.1 and 113.9%.
A fluorescence sensor composed of a molecularly imprinted polymer and an aptamer as a dual identification system for Cd 2+ coupled with and carbon quantum dots (co-doped with sulphur and nitrogen) and gold nanoparticles (SN-CQDs/Au) as fluorescent element that can detect Cd 2+ with high selectivity by a dual-recognition mechanism.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Bin Han,Wenbin Li,Yang Shen,Ruifang Li,Mengyi Wang,Zhijia Zhuang,Yikai Zhou,Tao Jing
The extensive use of antibiotics leading to the rapid spread of antibiotic resistance poses high health risks to humans, but to date there is still lack of an on-site detection method of SA residues. In this study, we integrated radical polymerization using sodium p-styrenesulfonate as a functional monomer and the self-polymerization of dopamine to prepare double-system imprinted polymers (DIPs) using sulfonamide antibiotics as templates. We found that the DIPs were semi-interpenetrating polymer networks and introduction of poly(dopamine) improved the selectivity of the imprinted cavities as well as the conductivity. The selectivity and sensitivity of the sensor using DIPs were much higher than those using single-system MIPs. This sensor could determine sulfonamides in complex samples in the presence of structural analogues. The linear range was from 0.01 to 10.00 μmol L −1 with a detection limit of 4.00 nmol L −1 . Furthermore, based on the highly selective DIPs and statistics analysis, this method could be used for simultaneous analysis of 4 sulfonamide types in real samples with an accuracy of 94.87 %. This work provides a strategy to improve the selectivity and sensitivity of MIPs based-sensor that can serve as tool for the simultaneous analysis of antibiotic residues in environment samples.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Honghong Lyu,Pin Li,Jingchun Tang,Weixin Zou,Pengfei Wang,Bin Gao,Lin Dong
Synergy between adsorption and photocatalysis provides an ideal green technology to treat antibiotic pollution in water. In this study, single-atom Mn anchored on N-doped graphene oxide (Mn-NGO) was synthesized for enhanced adsorptive-photocatalytic removal of aqueous sulfanilamide (SNM) and the corresponding mechanisms were revealed. The Mn-NGO had better performance of SNM degradation and TOC removal than GO and NGO. Density functional theory (DFT) calculation showed that the electrons of d-orbital (Mn) and p-orbital (N) upgraded the electronic structures of GO of the Mn-NGO to interact with amino and aromatic rings of SNM, increasing the adsorption and polarizing of SNM. Furthermore, more hydroxyl and superoxide radicals were observed on Mn-NGO, leading to the generation of key reaction intermediates of 2-aminohydroquinone and benzenesulfonic and thus subsequently opening loops and mineralizing SNM. In addition, Mn-NGO effectively removed SNM in different types of water systems (e.g., lake water, tap water, and deionized water) through synergistic adsorption-photocatalytic degradation.
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Natural Product Communications
·
2020
·
IF 0.468
Qiushan Zhang,Jin Shao,Tong Zhao,Lei He,Huiping Ma,Linlin Jing
In the present study, the antioxidant property of 4 flavones (moslosooflavone, wogonin, isowogonin, and norwogonin) was evaluated using 6 different assays: 1,1-diphenyl-2-picrylhydrazyl (DPPH·), superoxide (O2 •−), and nitric oxide (NO) radical scavenging assays, ferrous iron chelation, reducing power, and total antioxidant capacity. The 4 flavones exhibited antioxidant activities with decreasing order as norwogonin > isowogonin >> wogonin> moslosooflavone. The present results demonstrated that norwogonin and isowogonin exhibited excellent antioxidant activity, which was mainly based on the presence of C-8 hydroxyl group.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Zhang Rong,Li Chuan,Cui Huilin,Wang Yanbo,Zhang Shaoce,Li Pei,Hou Yue,Guo Ying,Liang Guojin,Huang Zhaodong,Peng Chao,Zhi Chunyi
Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of nitrate reduction under acidic conditions is rarely reported. In this work, we demonstrate the potential of TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity for selective and rapid nitrate reduction to ammonia under acidic conditions. Hybridized with iron phthalocyanine, the resulting catalyst displays remarkably improved efficiency toward ammonia formation owing to the enhanced nitrate adsorption, suppressed hydrogen evolution and lowered energy barrier for the rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed with high open-circuit voltage of 1.99 V and power density of 91.4 mW cm –2 . Further, the environmental sulfur recovery can be powered by above hybrid battery and the hydrazine-nitrate fuel cell can be developed for simultaneously hydrazine/nitrate conversion and electricity generation. This work demonstrates the attractive potential of acidic nitrate reduction for ammonia electrosynthesis and broadens the field of energy conversion.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 12
·5059-5070
·
IF 1.6
Guo Zifang,Zhang Yang,Jiao Limin,Li Yifan,Lin Zijian,Du Xiangyi,Zhao Xing,Gao Xuan,Yu Guobing,Liu Chunyu,Lin Mingzhang
The radiolytic behaviors of aqueous ammonia solutions under γ-ray irradiation were investigated, focusing on several factors, including initial ammonia concentration, absorbed dose, and H 3 BO 3 concentration. The main species including ammonia, H 2 O 2 , nitrogen oxides, and H 2 , were quantitatively analyzed. The results revealed the significant influence of the initial ammonia concentration on the radiolytic behavior of the aqueous ammonia solution. The existence of ammonia in the solution exhibited suppression of the concentrations of H 2 O 2 and O 2 . Furthermore, the radiolysis of aerated aqueous ammonia solution led to the formation of nitrogen oxides (NO 2 − and NO 3 − ). This process was driven by multiple oxidation reactions, in which O 2 and ·OH played crucial roles. Interestingly, the addition of H 3 BO 3 provided protection to ammonia during γ irradiation, while the concentration of H 2 O 2 was increased.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Xia Zhan,Rui Ge,Teng Huo,Juan Lu,Jiding Li
Graphene oxide (GO) membranes exhibit ultrafast water permeation properties, which have been employed in various membrane-based separations including nanofiltration for dye removal from textile wastewater. However, it’s still a great challenge to achieve precise control over the microstructure of GO membranes and obtain ultrathin GO membranes with exceptional separation efficiency and robust membrane structure. Herein, in-situ confined interfacial polymerization (IP) is proposed for fabricating loose polyamide (PA)@GO hybrid membranes with high permeance and dye rejection as well as robust membrane stability. A new diamine of sulfadiazine (SA) with intrinsic hydrophilic and conjugated sulfonamide groups is employed as cross-linker of GO membranes and monomer of PA in IP process, simultaneously. PA is in-situ synthesized in confined GO interlayer via IP process and intercalated into GO interlayer, which enlarges the interlayer spacing of GO membranes gradiently. The combination of hydrophilic PA nanofiltration layer on GO membrane surface and the PA intercalated GO membrane with varying interlayer spacing creates hierarchical transport channels for water molecules, which contributes to the high water permeance. Moreover, the less reactive SA monomer endows PA@GO selective layer with appropriate negative charge and loose transport channels, which contributes to both of high permeance and dye rejection due to Donnon effect and size exclusion effect. The PA@GO hybrid membrane exhibits high permeance of 75.5 L/(m 2 ·h·bar) with TB dye rejection of 99.8 %, and exhibits low NaCl rejection of 11.6 %. Moreover, PA@GO hybrid membrane shows good fouling resistance and long-term stability as well as stable separation performance under harsh conditions. Both of high permeance and dye rejection of PA@GO hybrid membrane suggests that the integration of PA nanofiltration layer and GO membrane via in-situ confined interfacial polymerization can achieve the delicate control over the interlayer channel structure and the physicochemical properties of the membrane surface of GO membranes, which offers a promising method to break through the trade-off effect between permeability and selectivity of GO membranes.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Dongsheng Lu,Tiesen Liu,Jinyu Han,Jiankang Zhao,Hua Wang
Electroreduction of nitrate to ammonia, a potential route for producing ammonia, is still confronted with a great challenge on developing efficient electrocatalysts. In this work, a reduced yolk-shell Co-based oxides (R-Co 3 O 4 ) electrocatalyst with oxygen vacancy-rich Co 3 O 4 and CoO was designed for nitrate reduction . This catalyst presented a nearly 100 % Faradaic efficiency (FE) of ammonia in a low potential from −0.05 to −0.1 V vs. RHE, and a maximum ammonia production rate of 7.25 mg h −1 mg cat. -1 at −0.05 V vs. RHE in 0.1 M KOH + 1000 ppm KNO 3 electrolyte. X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) pattern proved that the content of Co 2+ was dramatically increased in R-Co 3 O 4 . The kinetic correlation experiments and Operando Raman spectra preliminarily manifest that the potential limiting step is the reduction of adsorbed *NO 3 . The density functional theory (DFT) calculations consistently demonstrated that on both oxygen-rich Co 3 O 4 and CoO, the adsorption of key intermediates (*NO 3 , *NO and *NH) are greatly enhanced on the bridge site between two Co 2+ , boosting the nitrate reduction at low over-potential. This work is helpful to design the catalytic material with rich and low-valence sites towards electroreduction of nitrate to ammonia.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Jing Xiao,Jiayuan Tang,Jihong Chen,Lanlan Li,Shu Zhang,Xiaoli Xiong,Zhirong Zou
A facile and portable method was established for the detection of nitrite (NO 2 - ) by a portable gas pressure meter. NO 2 - and sodium cyclamate were reacted specifically under acidic condition, cyclohexene and nitrogen were thus generated, the pressures of reaction bottles were measured by a portable gas pressure meter. The pressures in bottles were increased gradually and proportional to the increase of NO 2 - concentration, the detection of NO 2 - was thus achieved. This method ensured good selectivity for the detection of NO 2 - and avoided interferences from other coexisting ions. In the range of 2–100 mg L −1 (43–2174 μmol L −1 ), the gas pressure was linearly correlated with the NO 2 - concentration, and a limit of detection of 0.65 mg L −1 (14 μmol L −1 ) was obtained. The developed method was further used for NO 2 - detection in water and ham sausage samples, recoveries of 94–106 % were obtained. It is a potential simple, rapid, portable analytical system/method for on-site detection of NO 2 - .
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 43
·e2311585120
·
IF 11.1
Chao-Hai Gu,Song Wang,Ai-Yong Zhang,Chang Liu,Jun Jiang,Han-Qing Yu
Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure–performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure–reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.
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