CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaoyi Zhang,Rongqing Chen,Xiaoying Gao,Jinlan Weng,Yunjia Liu,Tian Gui,Shenghong Yang,Dunqing Wang,Xiangshu Chen,Jian Liu
Cyclodextrin-based porous polymers have become a kind of promising adsorbents for the remediation of wastewater by virtue of their sustainability and economic potential. The acquisition of aforementioned adsorbents commonly requires elaborate preparation procedures which involve organic solvent, catalyst, inert atmosphere, or long reaction time. Herein, a facile and scalable solid-state mechanochemical approach was developed to afford reticular β-cyclodextrin polyurethanes (CDPUs) in a short time (2 h) without any organic solvents and catalysts at ambient conditions. Various diisocyanates can be used as coupling agents to link β-CD molecules into CDPUs relying on the driving force of ball milling. CDPUs-based composites can be also successfully synthesized via a “one-pot” mechanochemical reaction. The afforded CDPUs exhibit nearly the same physiochemical characteristics as those synthesized in solvents or with the assistance of catalyst. CDPUs have numerous accessible active adsorption sites, including β-CD cavities, bridging urethane groups, dangling amino groups, and aromatic rings. Owing to the accessible porosities and abundant adsorption sites, CDPUs exhibited rapid adsorption rate and high adsorption capacity towards phenolic micropollutants. CDPUs can maintain adsorption efficiency in a wide pH range, ionic strength, and humic acid. There is no significant decrease of adsorption efficiency for more than eight regeneration cycles, indicating their suitability for practical water treatment. This solid-state mechanochemical synthesis method for reticular CD-based polymers paves a new insight into green preparation of adsorbents and their sustainable use for the practical remediation of micropollutant wastewater.
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 11
·1-13
·
IF 3.061
Xu Jingmei,Meng Lingxin,Shi Qingyuan,Ren Qiang,Wang Zhe
In this study, sulfonated poly (ether ketone sulfone)s polymers with long sulfonic acid alkyl side chains and amino groups were prepared by free radical and polycondensation reaction. Poly (ether ketone)s with carboxyl groups were used for macromolecule crosslinking agent to prepare cross-linked membranes by amidation reaction. This series of membranes were characterized by FT-IR and 1 H NMR. Meanwhile, cross-linked composite membranes possessed excellent mechanical properties, methanol resistance performance and thermal stability. The highest proton conductivity of 0.096 S cm −1 was observed for APD-3/CP at 80 °C. The range of methanol permeation coefficients for the prepared membranes (2.89 × 10 −7 cm 2 s −1 —4.95 × 10 −7 cm 2 s −1 ) was far lower as compared to that of Nafion 117 (24.1 × 10 −7 cm 2 s −1 ). The results of morphology, swelling ratio and proton conductivity showed that the hydrophilic-hydrophobic phase separation structure effectively improved the properties of the membrane namely water uptake, dimensional stability and proton conductivity. Long-side chains functionalized cross-linked sulfonated poly (ether ketone sulfone)s proton exchange membranes had good candidate for application in fuel cells.
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ANALYST
·
2022
·Vol. 147
·期 24
·5655-5662
·
IF 5.227
Ying Zhou,Ruichun Li,Guomei Zhang,Yan Zhang,Caihong Zhang,Shaomin Shuang
Metal–organic frameworks (MOFs) have emerged as interesting nanomaterials owing to their large surface area, high porosity, tunable pore architecture and easy functionalization. However, an inferior electrical conductivity hinders their application in electrochemical sensing. In this paper, gold–palladium alloy/UiO-66-NH2/graphene (AuPd/UiO-66-NH2/GN) composites were synthesized by loading alloys on the surfaces of MOFs and then attaching them to the graphene surface. The addition of metal nanoparticles and graphene enhanced the electron transfer ability of MOFs. Then, composites were used to modify a glassy carbon electrode (GCE) to construct a sensitive dopamine (DA) electrochemical sensor. The developed sensor manifested two linear relationships in lower concentration ranges and in higher concentration ranges with a 0.21 × 10−6 mol L−1 low detection limit (3σ/k) under optimal conditions. The results certified that the constructed sensor had high selectivity, excellent reproducibility and good stability, and had been used successfully for DA detection in actual human serum samples.
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PubMed
高影响因子
ACS ES&T Water
·
2022
·
IF 0
Yi Zhou,Xia Li,Xinyu Chen,Jian Lu,Yanbo Zhou
Manganese dioxide (MnO2) is often used to treat pollutants in water owing to its high oxidative activity. Bisulfite (BS) as an activator can promote the degradation efficiency of MnO2. However, the mechanism of different crystalline MnO2 in the presence of BS is still controversial. The oxidation performance of the tunnel type (α-MnO2, β-MnO2) and the two-dimensional lamellar type (δ-MnO2) in the presence of BS was investigated. β-MnO2/BS exhibited the highest oxidative activity under optimal conditions. The bisphenol A (BPA) oxidation kinetic constant of β-MnO2/BS (0.737 min–1) was 6 and 2.3 times higher than that of δ-MnO2/BS and α-MnO2/BS, respectively. The mineralization efficiency of BPA reached 80.05% within 15 min, owing to the high content of Mn(IV) in β-MnO2. BS could rapidly reduce β-MnO2 to produce a high concentration of Mn(III). Soluble Mn(III) directly participates in the BPA oxidation, and the surface Mn(III) can react with the surface adsorbed oxygen molecules (Oad) to generate superoxide radicals (O2•–) to promote the deep mineralization of target contaminants. Moreover, the β-MnO2/BS system can efficiently oxidate various phenolic organic pollutants even in natural water. This research can provide new insights for better understanding of the oxidation process of different crystalline-phase MnO2/BS.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Menglu Xu,Yibing Zhang,Huaqin Yin,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Co-ZFO@Mn-CN with 1 O 2 and O 2 •− as main reactive oxygen species was synthesized for catalytic ozonation , which could efficiently degrade organic pollutants . EPR and XPS analysis indicated that lattice doping of Co induced formation of abundant of OVs, which could provide localized electrons for O 3 activation with the generation of HO 2 • /O 2 •− . 1 O 2 and H 2 O 2 were produced by the recombination of HO 2 • /O 2 •− . DFT calculation demonstrated that H 2 O 2 was deprotonated to generate HOO − , which preferred to form HOO-Mn-N X bonds with Co-ZFO@Mn-CN. Under the attack of O 3 , HOO-Mn-N X bonds were broken with the generation of HO 2 • and HO 3 • /O 3 •− , not only accelerating 1 O 2 production for organics degradation but also avoiding Mn(Ⅱ) sites oxidation . Combining advantages of OVs and HOO-Mn-N X , Co-ZFO@Mn-CN achieved 70–100% mineralization for different organic pollutants . Thus, this work provided a simple and efficient way for enhancing the utilization of O 3 by the synergistic effect of OVs and HOO-Mn-N X bonds, also improving ROS transformation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Weijie Yang,Kailong Sun,Jun Wan,Yang-Ai Ma,Yu Wang,Lin Liu,Bicheng Zhu,Feng Fu
Solar-driven activation of molecular oxygen (O 2 ) offers an appealing strategy to realize aerobic oxidation catalysis at room temperature, while the efficiency of photocatalytic O 2 activation is severely limited by lacking O 2 adsorption sites and poor carrier utilization. Herein, an efficient Ni 2 P/Bi 3 O 4 Br-OVs heterojunction is firstly proposed to overcome the limitation by the dual-site design of oxygen vacancies (OVs) and on Ni 2 P cocatalyst. By the joint observations from spectroscopic measurements and theoretical simulations, the introduction of OVs and Ni 2 P on Bi 3 O 4 Br nanosheets can not only optimize the light absorption, facilitate the separation and transfer of photogenerated charge carrier through the S-scheme mechanism, but also provide active sites for effective adsorption and activation of oxygen molecules, thereby contributing to highly efficient generation of •O 2 − radicals. Benefiting from the more oxidative active species of •O 2 − and h + , the Ni 2 P/Bi 3 O 4 Br-OVs photocatalyst achieves near-unity conversion rate and selectivity in aerobic oxidation of sulfide to sulfoxide, and it also exhibits outstanding photoactivity in the aerobic degradation of phenolic pollutants under visible light. This study showcases a feasible O 2 activation approach by defect and heterojunction engineering, and provides a new perspective for designing high-performance photocatalysts in the field of aerobic oxidation catalysis.
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CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Shengda Wang,Hanqing Jiang,Ronghua Yu,Shenghui Lou,Li Ma,Jie Liu,Tao Tang
A series of epoxy resins containing aromatic imine are synthesized via the Duff reaction by using various bisphenols, which show significantly reduced heat release capacity (HRC) and total heat release (THR) after curing. Compared to diglycidyl ether bisphenol A/4,4-diaminodiphenyl methane (DGEBA/DDM), the HRC and THR of phenolphthalein-based epoxy resin containing aromatic imine/DDM (BPP-E/DDM) are reduced by 87% (464 J/g K vs 58 J/g K) and 62% (30.2 kJ/g vs 11.4 kJ/g), respectively. Furthermore, the BPP-E/DDM exhibits a UL-94 V-0 rating (1.6 mm) and a limiting oxygen index of 48% (3.2 mm). Compared to DGEBA/DDM in the cone calorimeter test, the peak heat release rate, THR, peak smoke produce rate, and total smoke production of BPP-E/DDM were reduced by 91% (1006 kW/m2vs 87 kW/m2), 51% (89 MJ/m2vs 44 MJ/m2), 89% (0.36 m2/s vs 0.09 m2/s), and 79% (38 m2vs 8 m2), respectively. The influences of aromatic imine and the chemical structures between two benzene rings in the bisphenols on HRC and THR of the resultant epoxy thermosets are investigated. The mechanism studies show that the presence of aromatic imine in the epoxy resins completely changes the decomposition process to generate the products containing aromatic N-heterocycle, which contributes greatly to the improved char-forming ability and flame retardancy. Meanwhile the thermosets bearing carbonyl, 3-phthalidylene, and sulfonyl between two benzene rings in the bisphenols show better char-forming ability and flame retardancy among the resultant epoxy resins containing aromatic imine, due to more polycyclic aromatic hydrocarbons produced in the condensed phase.
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高影响因子
BIODEGRADATION
·
2022
·Vol. 34
·期 1
·73-81
·
IF 3.731
Gu Chen,Liang Jinxuan,Liu Ming,Rui Jianliang,Shi Jiyan,Yu Yanming,Zhang Xuwang
Bisphenol A (BPA) has been widely used in the manufacture of polymeric materials. BPA is regarded as an endocrine disrupting chemical, posing a great threat to the public health. In this study, a bacterial strain LM-1, capable of utilizing BPA as the sole carbon and energy source under aerobic conditions, was originally isolated from an activated sludge sample. The isolate was identified as Pseudomonas sp. based on 16S rRNA gene sequence analysis. Strain LM-1 was able to completely degrade 25–100 mg/L BPA within 14–24 h, and it also exhibited high capacity for BPA degradation at a range of pH (6.0–8.0). (NH 4 ) 2 SO 4 and NH 4 NO 3 were the suitable nitrogen sources for its growth and BPA biodegradation, and the BPA degradation could be accelerated when exogenous carbon sources were introduced as the co-substrates. Metal ions such as Zn 2+ , Cu 2+ , and Ni 2+ could considerably suppress the growth of strain LM-1 and BPA degradation. According to the analysis of liquid chromatography coupled to Q-Exactive high resolution mass spectrometry, hydroquinone, p -hydroxybenzaldehyde, and p -hydroxybenzoate were the predominate metabolites in the BPA biodegradation and the degradation pathways were proposed. This study is important for assessment of the fate of BPA in engineered and natural systems and possibly for designing bioremediation strategies.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mengxiang Ye,Chao Zhang,Zhenzhen Liu,Huaimeng Li,Zhen Fu,Haimin Zhang,Guozhong Wang,Yunxia Zhang
Extensive utilization and excessive accumulation of bisphenol A (BPA) has posed a serious threat to the whole ecosystem, necessitating the rational design of metal-based catalysts capable of complete mineralization of BPA via electrochemical oxidation. Considering the shortage of metals resources and ever-increasing generation of electronic waste (e-waste), converting e-waste into high-performance catalysts is highly expected to offer an economical and feasible means to achieve the degradation of BPA. To this end, CuAu bimetallic catalysts are in situ electro-codeposited on the carbon cloth (CC) support with the waste central processing unit (CPU) leachate as electrolyte. Significantly, the recovered CuAu/CC composites can be directly applied as an efficient electrocatalyst for the decontamination of BPA via the electro-Fenton process. The electrocatalytic activities of the fabricated CuAu/CC electrodes can be regulated by tuning the reduction potentials during electro-deposition process. Under the optimized operational conditions, 99.5 % of BPA (50 mg/L) is removed within 120 min at a constant cathodic potential of −1.0 V (vs Ag/AgCl) in the CuAu/CC-mediated electro-Fenton system, accompanied by 64.2 % of total organic carbon (TOC) removal, highlighting a satisfactory performance of the BPA electrochemical oxidation. In addition, the proposed CuAu/CC electrode material can be facilely regenerated and reused for at least ten cycles without significant decline in BPA removal efficiency. Our work offers valuable guidance for upcycling of bimetallic alloy catalysts from e-waste and further application in electrochemical decontamination of organic pollutants, achieving the innovative target of “using waste to treat waste.”
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Jiannan Chen,Xiuhua Xia,Peizhen Li,Hang Yu,Yunfei Xie,Yahui Guo,Weirong Yao,He Qian,Yuliang Cheng
Natural N and S co-doped carbon dots (NSCDs) were synthesized via hydrothermal synthesis using food-derived crawfish shells as green precursors. The relationship between quantum yield (QY) and protein content of six crawfish shells treated with different alkalis was investigated. The synthesized NSCDs displayed a large QY of 18.57 %, which was higher than most of the chitin-derived CDs. Due to the oxidation of hydroxyl radicals, adding H 2 O 2 and horseradish peroxidase (HRP) quenched the fluorescence of NSCDs, resulting in a detection limit (LOD) of 1.25 μM for H 2 O 2 . The addition of pentachlorophenol (PCP) was supposed to consume part of the hydroxyl radicals and protect NSCDs from being oxidized. Accordingly, a facile and rapid “off–on” fluorescence sensor was developed to detect PCP with a LOD of 2.30 μM. Further, the method described was successfully used to detect PCP in three real samples.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yujun Ju,Jianwei Zhang,Qinyu Cai,Zhengze Zhang,Yan Zhao,Jianguo Cui,Ruien Hou,Yi Wei,Zhiqiang Liang,Fengjuan Chen
Polluted water caused by antibiotics leads to serious risks to human health and ecosystem. Rapidly and efficiently treating antibiotic pollutions to make it safe is urgently needed for environmental protection and public health. Herein, we report that ZIF-67 derived nano-cube Co 3 O 4 as model catalysts were immobilized in the rotary-angle three-dimensional (3D) printed multilayer reduced graphene oxide/carbon nanotubes (Co 3 O 4 /R-rGO/CNTs) membrane for the highly efficient degradation of antibiotic pollutants through sulfate radical-based advanced oxidation process (SR-AOP). The macropores in the designed Co 3 O 4 /R-rGO/CNTs membrane are distributed in a rotationally staggered arrangement, which increases the opportunity for contaminant contact with the catalyst. The micro-cellular structures formed by the freeze-casting treatment in Co 3 O 4 /R-rGO/CNTs membrane provide abundant anchor sites for catalysts as-well-as plentiful active sites for catalytic reactions. The degradation efficiency of the designed membrane toward aureomycin hydrochloride (CTC) reached 99.3% at a flux rate of 636.9 L m −2 h −1 , which is increased by 100% comparing with the traditional 3D printing membrane with vertical macroporous arrays. This strategy put forward a new idea for the efficient degradation of antibiotic pollutants and has great application prospects in the field of environmental remediation.
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Symmetry-Basel
·
2022
·Vol. 14
·期 11
·2293
·
IF 2.94
Fuchong Li,Wei Liu,Yang Gao,Li Tian,Junhong Guo,Jinfeng Cui,Baoping Yang
Organic fluorescent materials are widely applied in different important fields, such as light-emitting display, explosive detection, molecular imprinting, and so on, because of their low cost, easy functionalization, and large-scale fabrication. In this work, we designed and synthesized a new kind of organic fluorescent polysulfate composite material through post-sulfonation sulfur-fluorine exchange polymerization (a new kind of click chemistry) by symmetric molecular. Sulfur-fluorine exchange polymerization: symmetrical structure SO2F−R1−SO2F molecular reacted with symmetrical OH−R2−OH molecular through nucleophilic reaction in the presence of inorganic base. The polysulfate material was further modified by ClSO3H to get PSE−SO3H materials. Tb3+was highly dispersed on PSE−SO3H to afford organic-inorganic hybrid fluorescent materials through the conventional coordination chemistry method. The emission wavelength of the organic-inorganic hybrid fluorescent polymer PSE−SO3H−Tb3+was between 475 and 685 nm, the quantum yield reached 1.18%, and fluorescence lifetime lasted for 730.168 us, with the pure green light emission and long light-emitting lifetime. The fluorescence film was prepared through phase transformation method by the fluorescent polymer material PSE−SO3H−Tb3+. The film has the strong stability property in different pH conditions (pH 1~13). Thus, this kind of organic fluorescent polysulfate composite material may have certain prospects application in terms of detection and luminescence in extreme chemical environments in the future.Keywords:polysulfate material;rare earth matal;Tb3+;fluorescence;polymer;symmetric molecular;stepwise polymerization
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危险品化学品经营许可证（带存储）