CONSTRUCTION AND BUILDING MATERIALS
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2019
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IF 4.046
Jianfeng Ma,Yazhuo Shang,Changjun Peng,Honglai Liu,Shuzhen Zheng,Hongxia Zhao,Shuai Qi,Qianping Ran
Air content can greatly affect the properties of concrete, therefore, the development of high efficient air-entraining agents is important. In this work, novel phosphate-modified polymers with different aryl substitutions were synthesized and used as highly efficient air-entraining agents. The structure of polymers was characterized by 1 H NMR and IR spectra. The foamability and foam stability of the different polymeric surfactants were tested in solutions. Surfactants with large steric hindrance, such as APP-6, showed superior performance of foamability and foam stability. In view of the excellent foamability properties of synthesized polymers in aqueous solution, the application of these polymers used in cement mortar as air-entraining agents were also evaluated for practical application. The surface tension, theoretical calculation and dynamic light scattering test for these polymeric surfactants were also studied. The synthetic aryl-polyether-phosphate surfactants showed higher surface activity, foamability, foam stability, and air-entraining performance compared with commercial air-entraining agent.
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ACS Applied Materials & Interfaces
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2019
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IF 8.456
Sixuan Wu,Hongliang Tan,Caihong Wang,Jinhong Wang,Shouri Sheng
Coordination polymers (CPs) as fascinating materials have been explored in a number of fields due to their diverse properties. In this work, we demonstrate the feasibility of CPs in the facile fabrication of multifunctional composites for establishing an immunoassay. To this end, a zinc(II)-based CP (ZnCP) with adenine as a bridge ligand was employed to integrate with alkaline phosphatase (ALP) and anticarcinoembryonic antigen (anti-CEA) antibody, which produces ALP/anti-CEA@ZnCPs. Benefiting from the adaptive inclusion property of ZnCPs, the integrated ALP and anti-CEA can maintain their original catalytic activity and capture ability to target antigen, respectively. This allows the ALP/anti-CEA@ZnCPs to be a detection antibody for performing an immunoassay. Meanwhile, ZnCP as a host can effectively protect the loaded ALP and anti-CEA against harsh environments. On this basis, by using iron(II)-phenanthroline complex as a signal amplifier, a colorimetric immunoassay for CEA detection was developed, and a low detection limit of 21.1 pg/mL has been achieved. This immunoassay was successfully applied to determine CEA levels in serum samples with good recovery and precision. We believe that this study can not only provide a new method for CEA detection but also open up a new way for the rational design and fabrication of multifunctional composites.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Yi Xiao,Zeqing He,Renshan Wang,Xueqin Tao,Benxia Li
Notwithstanding intensive research in recent decades, the conspicuous restrictions in photocatalysts still remain as low utilization of visible light, poor charge transfer/separation, and insufficient surface active sites. Designing semiconductor heterostructures as photocatalysts is a promising approach to enhance the photocatalytic efficiency for degrading organic pollutants. In this work, a novel WO 3 /BiOCl p–n heterostructure photocatalyst with optimal molar ratio was successfully fabricated by growing BiOCl nanosheets on WO 3 nanofibers through the electrospinning method followed with a solvothermal process. The optical properties and photoelectrochemical tests indicated that the WO 3 /BiOCl heterostructures possess high ability of photogenerated charge separation. The photocatalytic performance of the as-obtained materials was assessed by the degradations of rhodamine B (RhB) and phenol in water under visible light. Compared with pure WO 3 nanofibers and BiOCl nanosheets, the WO 3 /BiOCl heterostructure catalysts showed improved photocatalytic efficiencies, and the apparent rate constant of RhB degradation is 0.259 min −1 on the optimal WO 3 /BiOCl(2) sample, which is about 2.3 times that of pure BiOCl (0.113 min −1 ). The roles of different active species in the photocatalytic system were determined by active-species-eliminating experiments, revealing that the photogenerated holes play a leading function in the degradation of organic pollutants. The enhanced photocatalysis of WO 3 /BiOCl(2) heterostructures results from the joint effect of high activity of BiOCl nanosheets, anti-agglomeration of WO 3 nanofibers, and well-matched straddling band-structures for charge separation. This photocatalyst presents great potential in the removal of organic pollutants from aquatic environment.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yu Xie,Lin Gu,Shun Mao,Deli Wu,Jinhong Fan
Tetracycline antibiotics (TCs) are broad-spectrum antibiotics widely used in the prevention and treatment of human and poultry diseases, which can be frequently detected in natural water, soils and sediments. In this study, tetracycline was used as a model pollutant to investigate the performance and mechanism of ferrous sulfide in the removal of aqueous tetracycline antibiotics. Fe(II) species on the surface were proved to be crucial active sites of adsorption and reduction. S(-II) species couldn’t degrade tetracycline directly, but it promoted the circle of Fe(III)/Fe(II) as the other electron donor. Dissolve oxygen and pH of solution were crucial factors in transformation of mineral surface. Combined with the SEM, XPS and XRD analysis of the minerals before and after the reaction, it was found that the generated hydroxides were good to improve the mass transfer because the appearance of Fe(III) species reduced the electrostatic repulsion by changing pH zpc of the mineral surface. As a strong oxidant, The addition of Cr(VI) promoted the degradation of tetracycline under acidic conditions, but inhibited the degradation under medium alkaline conditions. The LC-MS analysis shown the degradation pathway of tetracycline is a process of gradually removing the electron-withdrawing group. Comparing to the higher mass-to-charge ratio of intermediate products from oxidative degradation, the removal of tetracycline was inferred to be reduction because the mass-to-charge ratio of the intermediate only decreased gradually in this study. The degradation pathway was to gradually remove the electron-withdrawing group according to the electrophilic ability.
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Journal of Materials Chemistry A
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2019
·Vol. 7
·期 37
·21149-21156
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IF 10.733
Juan Bai,Hao Huang,Fu-Min Li,Yue Zhao,Pei Chen,Pu-Jun Jin,Shu-Ni Li,Hong-Chang Yao,Jing-Hui Zeng,Yu Chen
As an alternative pathway for present nitrogen fixation methods, the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions represents an attractive approach for sustainable and economic development of chemistry and biology. In this work, we synthesize bimetallic RhCu ultrathin nanoflake nanoaggregates (RhCu-BUNNs) with atomic thickness by a facile hydrothermal method. For the NRR, bimetallic RhCu-BUNNs exhibit better electrocatalytic activity than monometallic Rh ultrathin nanoflake nanoaggregates (Rh-UNNs) because the introduction of Cu can effectively weaken the competitive hydrogen evolution reaction (HER), which can achieve a high NH3 yield rate (95.06 μg h−1 mgcat−1) at −0.2 V potential. Density functional theory (DFT) calculations suggest that the introduction of Cu can effectively lower the energy demand in the *NN reductive process, resulting in NRR activity enhancement. Meanwhile, RhCu-BUNNs also show excellent electrocatalytic activity and selectivity for the glycerol oxidation reaction (GOR). For the electrochemical NH3 production, the sluggish anodic oxygen evolution reaction (OER) increases the overall electrolysis voltage. Herein, we replace the anodic OER with the GOR to assist the NRR using a bifunctional RhCu-BUNN electrocatalyst. Specifically, only 1.2 V whole voltage is required for electrochemical NH3 production in the presence of glycerol, accompanied by the generation of valuable glyceraldehyde at the anode. This work may provide a promising pathway to obtain both NH3 and valuable organic chemicals with high efficiency and low cost.
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CARBOHYDRATE POLYMERS
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2019
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IF 6.044
Shuangyu Xiong,Luminita Marin,Lian Duan,Xinjian Cheng
Nitroaromatic compounds, especially 2, 4, 6-trinitrophenol, have strong biological toxicity and explosive risks, so the detection of 2, 4, 6-trinitrophenol exhibit importantly practical and scientific significance. In this work, three fluorescence functionalized chitosan CNS 3 , CNS 4 and CNS 5 were prepared using chitosan as matrix. When 2, 4, 6-trinitrophenol (TNP) and/or p-nitrophenol (4-NP) was present in spot, these fluorescent chitosan sensors produced notable fluorescence quenching. It renders the chitosan sensing ability to detect TNP and 4-NP selectively and sensitively. The sensing mechanism is investigated as well. When introduced electron-rich moieties to the fluorescent chitosan, the sensitive detecting ability could be obtained. Excellent recognition ability could reach as low as 0.28 μM. The fluorescence fictionalization cause slight influence to the gel performance of chitosan.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Ying Liu,Wei Miao,Xian Fang,Yulin Tang,Deli Wu,Shun Mao
The development of metal-free catalysts with high activity and stability for persulfate activation draws increasing attention due to their promising performance and environmental benignity. Herein, hierarchically porous nitrogen (N)-doped carbon (N C) with merits of highly-dispersed nitrogen, large surface area and controllable structure is synthesized. The as-prepared N C exhibits outstanding performance for peroxydisulfate activation in the degradation of diverse organic pollutants, as well as a wide working pH range of 3–10. Impressively, an annealing strategy can regulate C O and graphitic N contents in N C and their quantitative correlations with the reaction rate constants reveal that the C O and graphitic N in N C are active sites. Furthermore, peroxydisulfate activation by N C involves with three pathways in which the contribution from radicals (SO 4 − , OH) are comparatively weak and non-radical pathways including singlet oxygen ( 1 O 2 ) and electron transfer are dominant. The contribution of 1 O 2 is diminishing with delay of reaction while the electron transfer shows the opposite trend. Besides, good recycling performance is achieved by facile re-annealing of N C. This work provides new insights into the reaction mechanism of persulfate catalysis and can guide future catalyst development in advanced oxidation process.
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JOURNAL OF SEPARATION SCIENCE
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2018
·Vol. 41
·期 16
·3318-3327
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IF 2.415
Ming Zhong,Yan-Hong Wang,Lu Wang,Rui-Qing Long,Chun-Lin Chen
A novel type of magnetic molecularly imprinted polymer was prepared for the selective enrichment and isolation of chelerythrine from Macleaya cordata (Willd) R. Br . The magnetic molecularly imprinted polymers were prepared using functional Fe 3 O 4 @SiO 2 as a magnetic support, chelerythrine as template, methacrylic acid as functional monomer, and ethylene glycol dimethacrylate as cross-linker. Density functional theory at the B3LYP/6-31G (d, p) level with Gaussian 09 software was applied to calculate the interaction energies of chelerythrine, methacrylic acid and the complexes formed from chelerythrine and methacrylic acid in different ratios. The structural features and morphology of the synthesized polymers were characterized by using Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, and vibration sample magnetometry. Adsorption experiments revealed that the magnetic molecularly imprinted polymers possessed rapid kinetics, high selectivity, and a higher binding capacity (7.96 mg/g) to chelerythrine than magnetic molecularly non-imprinted polymers (2.36 mg/g). The adsorption process was in good agreement with the Langmuir adsorption isotherm and pseudo-second-order kinetics models. Furthermore, the magnetic molecularly imprinted polymers were successfully employed as adsorbents for the extraction and enrichment of chelerythrine from Macleaya cordata (Willd) R. Br . The results indicated that the magnetic molecularly imprinted polymers were suitable for the selective adsorption of chelerythrine from complex samples such as natural medical plants.
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ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Dequan Chi,Fei Liu,Haining Na,Jing Chen,Chuncheng Hao,Jin Zhu
With a high melting temperature and good crystallization ability, poly(neopentyl glycol 2,5-furandicarboxylate) (PNF), a polyester derived from bio-based 2,5-furandicarboxylic acid and neopentyl glycol, has been proposed and proved to be a promising hard segment for the development of novel bio-based thermoplastic poly(ether-ester) elastomer (TPEE). The resulting TPEE, namely PNF–PTMG, has high performance comparable to the petroleum-based counterpart PBT–PTMG (i.e., Hytrel, Dupont). Among all of the existing polyesters derived from bio-based 2,5-furandicarboxylic acid (FDCA), PNF has perfectly balanced properties, namely, a high melting temperature of 200 °C and a good crystallization ability to easily grow medium to large-size crystalline spherulites. Characterizations based on dynamic mechanical analysis and small-angle X-ray scattering suggest that there are two domains in PNF–PTMG, the crystalline PNF and a mixture of amorphous PNF and PTMG. These two domains form microphase separation induced mainly by the crystallization of PNF. By adjusting the PTMG soft segment from 30 to 60 wt%, PNF–PTMG shows a melting temperature, tensile modulus (E), and elongation at the break (εb) ranging from 180 to 134 °C, 738 to 56 MPa, and 38 to 1089%, respectively. More importantly, the shape recovery ratios increase from 57 to 90% at 200% strain when the amount of PTMG increases from 50 to 70 wt%, indicating excellent elastic property. These results indicate that PNF is an excellent hard segment to serve as a strong physical cross-link so that PNF–PTMG is able to display high performance comparable to extensively commercialized PBT–PTMG.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Gaoyuan Long,Jiafeng Ding,Lihong Xie,Runze Sun,Mengxia Chen,Yanfang Zhou,Xiuying Huang,Gaorui Han,Yajun Li,Weirong Zhao
Chlorophenols (CPs) have been considered as a kind of priority environmental pollutants for their potential detrimental effects, and photocatalytic reduction dechlorination tend to be a promising approach to CPs’ removal. In this work, 2,4-dichlorophenol (2,4-DCP) was adopted as the model pollutant of CPs, and a simple mixing and heating method was employed to prepare graphitic carbon nitride and bismuth tungstate (g-C 3 N 4 /Bi 2 WO 6 ) binary photocatalysts. Under UV–vis light irradiation and anoxic atmosphere, the g-C 3 N 4 /Bi 2 WO 6 samples exhibited enhanced photocatalytic activities. The optimal dechlorination rate constant of 2,4-DCP over g-C 3 N 4 /Bi 2 WO 6 (weight ratio 3:7) was 1.13 h −1 , 7.6 and 8.9 times higher than that of pristine g-C 3 N 4 and Bi 2 WO 6 respectively. The enhanced activities originated from the effective suppression of charge recombination and extended spectrum absorption range. Kinetic studies revealed that the dechlorination processes followed the pseudo-first-order model. The photocatalytic mechanism of 2,4-DCP over g-C 3 N 4 /Bi 2 WO 6 was discussed in detail, and based on which, a mediator-free Z-scheme mechanism was proposed. This work extends the application range of g-C 3 N 4 /Bi 2 WO 6 photocatalyst and provides a new insight into environmental remediation.
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ENERGY & FUELS
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2018
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IF 3.024
Da Wang,Yuyang Wang,Xiaoyu Li,Lei Chen,Guangci Li,Xuebing Li
In situ catalytic hydrogenolysis of lignin is an efficient method for lignin valorization. Herein, a novel in situ lignin catalytic hydrogenolysis technique in alkaline aqueous solution over a NiAl alloy catalyst under mild conditions was systematically suited. Ni served as the active phase and could be exposed by etching Al atoms with alkaline aqueous solution. Meanwhile, H2 resources could be in situ generated and easily arrived at the adjacent exposed Ni sites to be activated. The in situ lignin hydrogenolysis system exhibits attractive depolymerization results under mild conditions, with an 86.8% conversion degree and 18.9 wt % yield of aromatic monomers at 220 °C, much higher than the traditional hydrogenolysis method using a commercial Raney Ni catalyst under high pressure external H2. The mechanism studies with lignin model compounds suggest that alkaline aqueous solution could promote the cleavage of C–O–C bonds and hinder the hydrogenation of the benzene ring. In addition, a moderate amount of exposed Ni sites as well as rich active hydrogen species are determinant for efficient lignin depolymerization.
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FUEL PROCESSING TECHNOLOGY
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2018
·
IF 3.956
Congfei Yao,Yucui Hou,Shuhang Ren,Weize Wu,Youan Ji,Hui Liu
To develop a greener method to separate phenols from oils, four kinds of halogen-free zwitterions , including 1-(propyl-3-sulfonate)-triethylaminium (TEA-PS), 1-(propyl-3-sulfonate)-tripropylaminium (TPA-PS), 1-(butyl-4-sulfonate)-triethylaminium (TEA-BS) and 1-(butyl-4-sulfonate)-tripropylaminium (TPA-BS), were designed and synthesized to separate phenols from model oils via forming deep eutectic solvents (DESs) based on the formation of hydrogen bonding between OH group on phenol and the oxygen atom on SO 3 − group of the zwitterions. The effects of time, temperature, dosage of zwitterions, initial phenol content, and structure of zwitterions were investigated. The results show that the extraction process can reach equilibrium within 2 min and the extraction efficiency is not sensitive to temperature. The zwitterions separate well phenol from model oils at room temperature , and the minimum phenol contents follow the order: TEA-PS > TPA-PS > TEA-BS > TPA-BS. The minimum phenol content and the maximum extraction efficiency at 25 °C can reach 4.8 g dm −3 and 98.6%, respectively, by using TPA-BS. All the maximum extraction efficiency can be obtained with n zwitterions : n phenol of less than 0.4, which greatly reduces the dosages of extractants. Importantly, these zwitterions can avoid the introduction of halide ion, which can seriously corrode the process equipment. All these zwitterions can be easily regenerated by an anti-solvent method without an obvious mass loss and a decrease in phenol extraction efficiency. Lastly, the extraction mechanism was studied with FT-IR and the freezing points of DESs indicate that the DESs are formed through hydrogen bonding.
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