Journal of Central South University
·
2021
·Vol. 28
·期 5
·1279-1290
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IF 1.716
Zhang Guang-ji,Tang Fei-ying,Wang Li-qiang,Yang Wen-jie,Liu You-nian
Transition metal sulfides (TMSs)-based materials have been extensively investigated as effective non-noble catalysts for various applications. However, the exploration of TMSs-based catalysts for hydrogenation of nitro compounds is limited. Herein, CoS x /NC catalysts were prepared by solvothermal sulfurization of ZIF-67, followed by high-temperature annealing (300–600 °C) under NH 3 atmosphere. It was found that the structures and compositions of the as-prepared CoS x /NC can be readily tuned by varying the annealing temperature. Particularly, CoS x /NC-500, which possesses higher degree of S defects and larger specific surface areas, can achieve high conversion, selectivity and stability for catalytic reduction of nitro compounds into amines under mild reaction conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xin Liu,Peng Xu,Qi Fu,Runhan Li,Chenxi He,Wenxuan Yao,Lei Wang,Shiqi Xie,Zhiyi Xie,Qiulai He,John C. Crittenden
Zero − valent copper activated peroxymonosulfate (Cu(0)/PMS) system had widely studied for degrading contaminant due to being highly efficient. However, the weak reactivity and easy dismutation of Cu(I) in acid condition restrained its efficiency. In our study, ferric ion (Fe(III)) significantly enhanced Cu(0)/PMS system for acetaminophen degradation and total organic carbon removal. Multiple reactive oxidants including Fe(IV), Cu(III) and hydroxyl radical (•OH) were generated in the Fe(III)/Cu(0)/PMS system. In the Fe(III)/Cu(0)/PMS system, Cu(0) generated Cu(I) by hydrogen corrosion and PMS oxidation, and then Fe(III) reacted with Cu(I) and Cu(0) producing Fe(II). At the same time, PMS reduced Cu(II) to Cu(I), and Cu(I) reacted with oxygen with forming hydrogen peroxide (H 2 O 2 ). Finally, both Cu(I) and Fe(II) induced H 2 O 2 and PMS producing reactive oxidants, and meanwhile H 2 O 2 was formed by the reaction of Fe(IV) and •OH. Thereinto, Fe(IV) and •OH made main contribution on the degradation of acetaminophen, while Fe(IV), Cu(III) and •OH were responsible for orange II degradation. Common water matrix including sulfate ion, nitrate ion and carbonate ion had inapparent impact on acetaminophen degradation, but chloride ion and humic acid limited slightly the degradation of acetaminophen. There had a good degradation of acetaminophen in tap water, lake water and well water with the Fe(III)/Cu(0)/PMS system. Adjusting the final reaction solution to pH 8.0 and subsiding, the discharge of total copper was within the II-level environmental quality standards for surface water in China (1 mg/L). The study might provide a new and promising idea based on Cu(0) activated PMS system for enhanced degradation of contaminants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Jibo Dou,Jie Cheng,Zhijiang Lu,Ziqi Tian,Jianming Xu,Yan He
In this study, N/B co-doped biochars were employed as metal-free activators of peroxydisulfate (PDS) for tetracycline degradation, more importantly, the roles of dopants and the relative contribution of radical vs nonradical oxidations were comprehensively investigated. Integrating with electron paramagnetic resonance and kinetics calculations, we showed that co-doping N and B into biochars not only boosted the catalytic activity but also switched the radical PDS-activated process into the electron transfer-dominated nonradical process. Compared with pristine biochar/PDS systems (22%), the nonradical contribution of N/B co-doped biochar/PDS systems increased to 59%, exhibiting outstanding stability and selectivity. Galvanic oxidation tests and theoretical simulations unveiled that doped biochars as conductive tunnels accelerate the potential difference-driven electron transfer from the highest occupied molecular orbital of pollutants to the lowest unoccupied molecular orbital of PDS due to the lower energy gap. This study provided new insights into the critical role of heteroatom-doped carbocatalysts in PDS nonradical activation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Huiming Xiang,Naiyun Gao,Xian Lu,Yuanquan Xiang,Wenhai Chu
Ultraviolet combined monochloramine (UV/NH 2 Cl) process is a promising advanced oxidation process (AOP) to remove organic micropollutants effectively through the generation of various reactive species e.g., hydroxyl radicals (HO • ), reactive chlorine species (RCS), and reactive nitrogen species (RNS). This study investigated the kinetics, transformation pathways, DBPs formation, and toxicity alternation in the degradation of sulfamethazine (SMT). Based on the calculation of degradation kinetic models, RNS was proved to be the most important reactive species in the degradation of SMT in UV/NH 2 Cl. The contribution of RNS, HO • and RCS were approximately 56.6%, 38.8%, and 4.5%, respectively. With the NH 2 Cl dosage increased from 100 to 800 µmol L -1 , degradation rate increased from 37% to 73% in 10 min. Significantly alternation was not observed with the changing of pH. Natural organic matter (NOM) remarkably inhibited the degradation rate to 48.6% and 32.8% in the presence of 1 and 2 mg L -1 NOM. Degradation reactions of SMT in UV/NH 2 Cl system primarily comprised of hydroxylation, nitrosation, and ring opening reactions. The total theoretical toxicity of degradation system increased in the first 20 min and decreased eventually. Comparing with UV/free chlorine (UV/Cl 2 ) process, less disinfection by-products (DBPs) generated in UV/NH 2 Cl treatment. Thus, the theoretical toxicity of DBPs formed in UV/NH 2 Cl was much lower than UV/Cl 2 . Within 40 min degradation, the theoretical toxicity value reached maximum at pH 7.1 due to the mass production of dicloroacetonitrile (DCAN). Bromide ions (10 µmol L -1 ) significantly promoted the formation of brominated DBPs especially dibromoacetonitrile (DBAN). This study provided insight into the important role of RNS in the SAs’ transformation in UV/NH 2 Cl process and reference to benefits and disadvantages when selecting the process for disinfection in drinking water treatment.
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Reaction Chemistry & Engineering
·
2021
·Vol. 7
·期 3
·590-598
·
IF 4.239
Runzhe Liang,Xiaonan Duan,Jisong Zhang,Zhihong Yuan
In recent years, self-optimization strategies have been gradually utilized for the determination of optimal reaction conditions owing to their high convenience and independence from researchers' experience. However, most self-optimization algorithms still focus on homogeneous reactions or simple heterogeneous reactions. Investigations on complex heterogeneous gas–liquid–solid reactions are rare. Based on the Nelder–Mead simplex method and Bayesian optimization, this work proposes a reaction optimization framework for optimizing complex gas–liquid–solid reactions. Three gas–liquid–solid reactions including the hydrogenations of nitrobenzene, 3,4-dichloronitrobenzene, and 5-nitroisoquinoline are investigated, respectively. Reaction parameters (temperature, hydrogen pressure, liquid flow rate, and gas flow rate) are optimized. Compared with the traditional OVAT method, the proposed Bayesian based optimization algorithm exhibits remarkable performance with higher yields (0.998, 0.991 and 0.995, respectively) and computational efficiency.
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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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JOURNAL OF NANOBIOTECHNOLOGY
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2021
·Vol. 19
·期 1
·1-17
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IF 10.435
Fouad Hatem,Yang Guiying,El-Sayed Ahmed A.,Mao Guofeng,Khalafallah Diab,Saad Mahmoud,Ga’al Hassan,Ibrahim Ezzeldin,Mo Jianchu
Background Despite developments in nanotechnology for use in the pharmaceutical field, there is still a need for implementation of this technology in agrochemistry. In this study, silver nanoparticles (AgNPs) were successfully prepared by a facile and an eco-friendly route using two different ligands, 2ʹ-amino-1,1ʹ:4ʹ,1″-terphenyl-3,3″,5,5″-tetracarboxylic acid (H4L) and 1,3,6,8-tetrakis (p-benzoic acid)-pyrene (TBAPy), as reducing agents. The physiochemical properties of the as-obtained AgNPs were characterized by scanning electron microscopy (SEM), energy-dispersive X-ray (EDX), X-ray diffraction (XRD) and transmission electron microscopy (TEM). The toxicity of H4L–AgNP and TBAPy–AgNP against the brown planthopper (BPH, Nilaparvata lugens) was also measured.Results SEM and TEM analyses demonstrated the formation of quasi-spherical AgNP structures in the presence of H4L and TBAPy. Insecticidal assays showed that TBAPy is less effective against N. lugens, with a median lethal concentration (LC50) of 810 mg/L, while the toxicity of H4L increased and their LC50 reached 786 mg/L 168 h posttreatment at a high concentration of 2000 mg/L. H4L–AgNPs were also highly toxic at a low concentration of 20 mg/L, with LC50 = ~ 3.9 mg/L 168 h posttreatment, while TBAPy–AgNPs exhibited less toxicity at the same concentration, with LC50 = ~ 4.6 mg/L.Conclusion sThese results suggest that the synthesized AgNPs using the two ligands may be a safe and cheaper method compared with chemical insecticides for protection of rice plants from pests and has potential as an effective insecticide in the N. lugens pest management program.
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WATER RESEARCH
·
2021
·
IF 11.236
Zhang Yan,Zongren Dai,Wenxiao Zheng,Zhenchao Lei,Jinwen Qiu,Wenjie Kuang,Weijun Huang,Chunhua Feng
ABSTRACT The treatment of low-concentration ammonium (e.g., <50 mg L −1 ) in highly acidic wastewaters through traditional biological nitrification, physical separation, or chemical stripping remains a huge challenge. Herein, we report that photocatalytic ammonium oxidation using bismuth oxychloride (BiOCl) can successfully occur in Cl − -laden solutions within a pH range of 1.0-6.0. All reactions follow pseudo-zero-order kinetics (with rate constants of 0.27-0.32 mg L −1 min −1 at pH 2.0-6.0 and 0.14 mg L −1 min −1 at pH 1.0), indicating the saturation of reactive species by the reactants. The interlayer is self-oxidized by the valence band holes (VB h + ), resulting in the formation of Cl • and subsequently HClO, which is excited upon UV irradiation to provoke consecutive photoreactions for chlorine radical generation. Compared to the free chlorine, HO • , Cl • , and Cl 2 • − , the ClO • produced using the UV/BiOCl system plays a predominant role in oxidizing ammonium under acidic conditions. BiOCl exhibits good stability because of the compensation of Cl − from solution and maintains high activity under different conditions (i.e., different cations and co-existing anions, temperatures, and initial substrate concentrations). The successful removal of ammonium from real wastewater using the UV/BiOCl system suggests that this is a promising method for treating diluted ammonium under highly acidic conditions.
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Journal of Water Process Engineering
·
2021
·
IF 5.485
Jinxin Lu,Jiaqi Li,Jianye Xu,Huili Tang,Zhen Lv,Erdeng Du,Liping Wang,Mingguo Peng
The UV/chlorine process is a novel light-driven oxidation technique. In this study, norfloxacin (NOR), a typical quinolone contaminant, was degraded by using the UV/chlorine process. The effects of the process parameters were also investigated. The UV/chlorine process was observed to be capable of fully removing NOR in 360 s with a high degradation rate constant of 0.0196 s −1 . NOR degradation was found to be positively correlated with chlorine dose and UV intensity but negatively correlated with ammonia. FMO, MSPA, and CDFT quantum chemical structure analyses reveal the most reactive sites for electrophilic or radical attack are the N6 or N5 atoms in the piperazine ring of the NOR molecule, which are also potential starting reaction sites for the degradation process. Thirteen degradation intermediates were detected and identified by UPLC/Q-TOF HRMS . Three sub-pathways are present during the degradation process, including cleavage and removal of the piperazine ring, transformation and cleavage of the quinolone structure, and chlorination reaction with chlorine active matter (RCS). The full elimination of NOR does not ensure a decrease in acute toxicity. Environmental risks associated with the UV/chlorine process need to be assessed further.
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Advances in Materials Science and Engineering
·
2021
·
IF 1.726
Wenli Peng,Li Gan,Weihan Li,Shixiong Deng
The development of probes for the testing of the carcinogenic pollutant 2,4,6-trinitrophenol (TNP) is of great importance for environmental protection and human health. In this paper, a new rapid and sensitive fluorescence detection method based on carbon dots (CDs) was designed for the detection of TNP. The CDs were synthesized by simple pyrolysis using citric acid as raw material and characterized by various advanced techniques. The addition of TNP caused a significant turn off in the fluorescence of the CDs. The fluorescence quench intensity and TNP concentration exhibited a good linear correlation in the range of 0–80 μM with a minimum detection limit of 0.48 μM and a related coefficient of 0.994. The analytical method was applied to the determination of trace TNP in river water and tap water with recoveries in the range of 98%–110% and relative standard deviations less than 5%. Importantly, carbon dots functionalized papers (CDFPs) were prepared using the synthesized CDs and successfully applied to the determination of TNP in aqueous solutions, demonstrating the promising application of the method.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
·
IF 3.764
Yaxing Li,Rui Zhang,Xianghai Meng,Ping Ouyang,Haiyan Liu,Chunming Xu,Zhichang Liu
Acid-soluble oil (ASO) was produced during isobutane alkylation catalyzed by chloroaluminate ionic liquids (CAILs). However, the ASO composition characterizations and deactivated CAIL regeneration pathway were not clarified. In this work, a series of characterizations (elemental analysis and infrared, ultraviolet, and mass spectroscopy) were performed to reveal the ASO composition. The result showed that ASO contained numerous conjugated cycloolefins with various alkyl substituents and a few O1–O5 compounds. The activity index (AI) value of fresh CAILs was 1.74 and decreased to 1.18 with the addition of 9.09 wt % ASO because the [Al2Cl7]− anion in CAILs was complexed by C═C and C═O bonds in ASO. The hydrogenation regeneration of deactivated CAILs on the Pd/C catalyst was studied. The AI value of regenerated CAILs increased to 1.45 because unsaturated bonds in ASO were hydrogenated to saturation. Recovery of unsaturated hydrocarbons followed the order benzene > 1-methylcyclopentene > pentamethylcyclopentadiene. This work demonstrated that low ASO recovery was attributed to the partial occupation of the π-electron of unsaturated bonds by the [Al2Cl7]− anion.
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FOOD CHEMISTRY
·
2019
·
IF 5.399
Gaigai Li,Xufeng Meng,Junmin Wang,Qianqian Wang,Junhong Zhou,Chun Wang,Qiuhua Wu,Zhi Wang
In this study, a porous organic polymer (denoted as Car-DMB) was fabricated by a simple one-step crosslinking polymerization of carbazole and p -dimethoxybenzene for the first time. Then the Car-DMB was served as adsorbent of solid phase extraction to enrich triazine herbicides from white gourd, tomato and soybean milk samples prior to their determination by high performance liquid chromatography. Under the optimal conditions, the response linearity was in the range of 0.3–100.0 ng g −1 for white gourds and tomato samples, and 0.5–100.0 ng mL −1 for soybean milk, with the coefficient of determination higher than 0.996. The detection limits were 0.1–0.2 ng g −1 for white gourd and tomato samples, and 0.15–0.3 ng mL −1 for soybean milk. The adsorption mechanism of the Car-DMB for the triazines was attributed to the strong H-bonding and weak π-π interactions. The efficient extraction for several other compounds demonstrated that Car-DMB holds great potential for diverse analysis applications.
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