JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Xiuru Yang,Zhi Chen,Wan Zhao,Chunxi Liu,Xiaoxiao Qian,Wenya Chang,Tao Sun,Cai Shen,Guoying Wei
Porous-hydrangea x%BiOBr/BiOI n-n heterojunction with ordered morphology was successfully prepared through a simple solvothermal process using Bi(NO 3 ) 3 ·5H 2 O, KBr, BiOI, and ethylene glycol as the precursors. The prepared x%BiOBr/BiOI (x = 2, 5, 10, 15 mol ratio) n-n heterojunctions exhibit enhanced photodegradation properties during treatment of tetracycline hydrochloride (TC-HCl) under visible light irradiation. The highest efficiency at optimized x = 5 is 1.3-, 1.7- and 1.3-fold higher than that of the pristine BiOI, BiOBr, and commercial titanium dioxide (P25), respectively. The improved photocatalytic performance was assigned to the optimized charge-separation properties of n-n heterojunction. However, over-loading of BiOBr upon BiOI may restrain the access of light to BiOI, which could limit the light absorption. The active species have been investigated by trapping experiments and it was found that holes (h + ) and superoxide radicals (∙O 2 - ) were mainly responsible for the photodegradation of TC-HCl. Additionally, the structure and activity relationship were systemically investigated, and the formation of n-n heterojunction is discussed accordingly. The photodegradation of TC-HCl is proved to be a complete mineralization process and the reaction mechanism is also proposed.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Lvxia Zhang,Hui Ouyang,Dan Zhang,Zhifeng Fu
Novel cobalt-based metal-organic frameworks (Co MOFs) were synthesized by a facile “controlled synthesis” strategy. The MOFs displayed superior catalytic performance on the chemiluminescent (CL) reaction between N -(4-aminobutyl)- N -ethylisoluminol (ABEI) and H 2 O 2 . UV–vis absorption, CL spectrum, ESR, and radical scavenger experiments were conducted for clarifying the catalytic mechanism of Co MOFs. All results revealed that Co MOFs can accelerate decomposition of H 2 O 2 and production of OH • , O 2 • − as well as 1 O 2 radicals. The rapid reaction between these reactive oxygen species and ABEI resulted in the generation of ABEI-ox∗. The excited-state oxidation product emitted a very intensive CL signal with a maximal emission wavelength of 430 nm as it returned to the ground state. To explore their application potential in CL assay, Co MOFs were used as powerful CL reaction catalyst for establishing a very sensitive method for immunoassay of aflatoxin B 1 . The detection range was 0.05–60 ng mL −1 , and the limit of detection was 4.3 pg mL −1 . The result for detecting herbal medicine samples demonstrates the acceptable reliability of the Co MOFs-based CL immunoassay. The proof-of-principle work verifies the application potential of Co MOFs on boosting intensive CL signal, and meets the demand for high sensitivity in various bioassay fields.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Zhixiang Cui,Jixin Lin,Jiahui Wu,Jiaqi Yu,Junhui Si,Qianting Wang
The development of high-efficiency and low-cost oxygen evolution reaction (OER) electrocatalysts has attracted increasing research attention. Herein, we report a novel nanocomposite of N-doped CoP nanoparticles embedded in porous carbon nanofibers (N–CoP@NPCNFs) synthesized using zeolitic imidazolate framework-67 (ZIF-67)@Polyacrylonitrile (PAN) nanofibers (ZIF-67@PNFs) as the precursor through carbonization, oxidation and phosphidation with N-doping. The fabricated N 1 –CoP@NPCNFs-900 shows outstanding electrocatalytic properties for OER due to a synergistic effect between the carbon nanofibers and the N-doped CoP nanoparticles. It exhibits a low overpotential of only 266 mV at 10 mA cm −2 , a small Tafel slope of 70 mV dec −1 and excellent durability for OER in 1.0 M KOH. Therefore, the obtained N 1 –CoP@NPCNFs-900 is promising for application as a high-efficiency and low-cost OER electrocatalyst.
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ACS ES&T Engineering
·
2020
·
IF 0
Yuxian Wang,Nuo Ren,Jiaxin Xi,Ya Liu,Tao Kong,Chunmao Chen,Yongbing Xie,Xiaoguang Duan,Shaobin Wang
High-performance and robust catalysts act as core drivers for advanced oxidation technologies for decontamination of water resources. In this study, we used a facile strategy to prepare magnetic and N-doped carbon nanotubes with cobalt encapsulation (Co–N@CNTs) to catalyze ozone for decomposition of aqueous organic pollutants. By regulating the thermal conditions during the synthesis, the derived Co–N@CNTs manifested maneuvered adsorption capabilities. The embedded Co nanoparticles (NPs) not only afforded carbon nanotubes with a magnetic property but also significantly boosted catalytic ozonation due to the synergistic coupling of the Co interface and N-doped graphitic layer. Formation of such a coordinating structure accelerated electron transfer at the interface and increased the conductivity of surface carbon to coordinate a redox reaction. Density functional theory (DFT) calculations and experimental evidence confirmed that cobalt coupled with graphene with pyridinic N dopants was the most favorable structure, which remarkably enhanced ozone adsorption and its dissociation to generate reactive oxygen species (ROS). Intriguingly, the catalytic ozonation underwent different nonradical regimes dependent on the molecular structures of target organics. In terms of ROS, surface-adsorbed atomic oxygen (*Oad) was responsible for degradation of oxalic acid, while phenolics were primarily degraded by O3 molecules and singlet oxygen (1O2). This study provides a cost-efficient and recyclable carbocatalyst for wastewater decontamination and new insights into the structure–functional relationships in carbon-based advanced oxidation processes.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 18
·7652-7664
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IF 3.553
Gao Ailin,Chen Shuju,Zhao Shuai,Zhang Guangfa,Cui Jian,Yan Yehai
In this work, mechanically strong and electrically conductive poly( N , N -dimethylacrylamide) (PDMAA)/pristine graphene (GR) nanocomposite hydrogel was synthesized by directly dispersing pristine GR into N , N -dimethylacrylamide (DMAA) monomers, which have been commonly used to prepare polymeric hydrogel as reactive monomers. Results showed that the introduction of GR nanosheets as physical cross-linking and its cooperation with organic cross-linker N , N -methylene bisacrylamide (BIS) were found to efficiently improve the mechanical strength, dimensional homogeneity of pore structure, thermal and electrical conductivity of resultant PDMAA hydrogels. More importantly, the intrinsic interaction between DMAA monomer and GR was systematically analyzed by ultraviolet–visible (UV–Vis) spectrophotometer, nuclear magnetic resonance ( 1 H NMR) and rheological test for the first time. These studies help us understand the formation mechanism of PDMAA hydrogel when graphene was added, as well as the fundamental parameters that govern the properties of hydrogels.
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FOOD CHEMISTRY
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2021
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IF 7.514
Jing Li,Kunpeng Gao,Francesco Secundo,Xiangzhao Mao
Chitin, one of the most abundant renewable biopolymers on Earth, is commercially available from crustacean wastes. One critical step in converting chitin to high-value products is its degradation by chitinolytic enzymes to N -acetyl- d -glucosamine (GlcNAc), which plays a significant role in functional food and pharmaceutical industries. Here, we cloned and biochemically characterized two novel β - N -acetylglucosaminidases named SvNag2557 (family-84) and SvNag4755 (family-3) from Streptomyces violascens ATCC 27968. Both SvNag2557 and SvNag4755 exhibited strict substrate specificity toward N -acetyl chitooligosaccharides with GlcNAc as the sole product. Thus, a one-pot production for pure GlcNAc from chitin by an enzyme cocktail reaction was further developed. Under the co-action of an endo-type chitinase SaChiA4 and SvNag2557 (mass ratio 1:2), the final conversion rates of colloidal chitin and ionic liquid pretreated chitin to GlcNAc were 80.2% and 73.8% with GlcNAc purities of 99.7% and 96.8%, respectively.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Dongju Fu,ZiYue Zhu,Jianjun Chen,Liqiang Ye,XinRui Song,XieRong Zeng
It is paramount important to design and explore excellent bifunctional oxygen electrocatalysts to conquer or weaken the shortcomings encountered by Zinc-air batteries at present. Herein, a novel N -doped hollow carbon tubes modified by uniform NiCo 2 O 4 nanocrystals ( N -HCTs@NiCo 2 O 4 ), has been developed as an extremely efficient bifunctional catalyst. The hollow structure of N -HCTs possesses a large specific surface area of 610.60 cm g −1 which provides abundant active N -dopant sites for the oxygen reduction reaction, whereas the NiCo 2 O 4 nanocrystals serve as the positive phase for the oxygen evolution reaction. It is found that the efficient bifunctional activity is obtained by establishing a coupling interface between N -HCTs and NiCo 2 O 4 . The N -HCTs@NiCo 2 O 4 composite has a half-wave potential of 0.81 V toward ORR and the overpotential of 330 mV at a current density of 10 mA cm −2 toward OER as compared with noble metal catalysts. The N -HCTs@NiCo 2 O 4 as the cathode catalyst for Zinc-air batteries exhibits superior peak power density (150 mW cm −2 ), specific capacity up to 779 mAh g −1 , and good stability even after 100 h of cyclic charge/discharge cycles N -HCTs@NiCo 2 O 4 has good prospects for practical applications of non-precious metal catalysts in the cathode of Zinc-air batteries.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 136
·期 20
·47473
·
IF 2.188
Xiaoning Wang,Yacheng Xing,Xihui Zhao,Quan Ji,Yanzhi Xia,Xiaomei Ma
To seek adsorptive hydrogels with high stability, poly(N,N-dimethylacrylamide) (PDMAM)-based hydrogels were fabricated employing vinylated chitosan as a macro-crosslinker. The prepared hydrogels achieves a maximum compressive stress above 11 MPa (98% strain), a maximum tensile strength, and fracture elongation of 0.037 MPa and 929%. The recovery ratios after three consecutive compressions (90% strain) and 1 h's resting (600% stretch) exceed 94% and 85%, respectively. The optimal adsorption effect (>90% removal efficiency) is achieved at pH 3 and 318 K in 2.5 h using hydrogels crosslinked by 9.77 wt % chitosan. The kinetic study indicates that the experimental data fit to the pseudo-second-order kinetic model better. The adsorption isotherm fits to the Freundlich model, indicating nonhomogeneous adsorption of the dyes on the hydrogels. Most adsorbed dyes are desorbed in 2 h at pH 10 and 318 K, both adsorption/desorption efficiencies exceed 90% after five adsorption–desorption cycles, confirming reusability of the hydrogels. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47473.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
·
IF 6.434
Genming Li,Wenbo Zhao,Muyuan Chai,Yanhong Li,Qingming Jia,Yuan Chen
In the present work, liquid-liquid phase-change absorption of SO 2 was investigated using N , N -dimethylcyclohexylamine (DMCHA) as an absorbent, and high boiling liquid paraffin (LP) as a solvent to reduce volatilization of the absorbent. The homogenous solution was split into two immiscible phases upon SO 2 loading. The phase-change mechanism was attributed to the polarity variation of DMCHA before and after absorption by forming the charge-transfer complex DMCHA·SO 2 . The viscosity of the lower phase reached a maximum value of 24.5 mPa s at the absorption capacity of 1 mol SO 2 /mol DMCHA, and the viscosity of the corresponding upper phase was 46.4 mPa s. Both are lower than the reported viscosity of most ionic liquids. This solution exhibited extremely high mass selectivity of SO 2 /CO 2 with a value of 626. The mass absorption capacity was founded to be 1.19 g SO 2 /g DMCHA at 1 atm, which is comparable with the highest reported mass absorption capacity. At low partial pressure, the absorption capacity still reached 0.78 g/g at 0.1 atm, 0.43 g/g at 0.02 atm and 0.27 g/g at 0.001 atm. Furthermore, DMCHA could be completely regenerated in 10 min via microwave heating. All the results indicated this phase-change solution is a promising candidate for SO 2 capture.
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CHEMOSPHERE
·
2018
·
IF 4.427
Jiali Peng,Jianfei Yan,Qixuan Chen,Xia Jiang,Gang Yao,Bo Lai
To enhance the degradation of N, N-dimethylacetamide (DMAC) in aqueous solution, the natural mackinawite (NM) is introduced for catalytic ozonation in this study as it is an environmentally friendly catalyst with low cost and easy availability. The properties of the NM were initially characterized via scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), Fourier Transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Then, impact factors including NM dosage, ozone gas concentration and initial pH were investigated and the optimal conditions (i.e., NM dosage = 3.5 g/L, ozone gas concentration = 300 L/min, initial pH = 6.8) were obtained in NM/O3 process. Besides, the superiority of the NM/O 3 process was confirmed by the experiments that the degradation efficiency of DMAC in the NM/O 3 process (i.e., 95.4%) was much higher than that in the zero-valent iron (ZVI)/O 3 process (i.e., 46.1%) and the synthetic FeS/O 3 process (i.e., 68.6%). Furthermore, the intermediate and possible degradation pathway of DMAC were proposed, and the biological toxicity of the intermediate was subsequently evaluated by the activated sludge . Finally, the mechanism of the NM/O3 process was proposed in this study based on control experiment and radical scavenging experiment. The extraordinary efficiency for DMAC degradation was found to be mainly caused by HO • of the reactive oxygen species (ROS) (i.e., HO • , O 2 •- and H 2 O 2 ) generated in the NM/O 3 process. Therefore, this study confirmed that NM was a high efficient catalyst for degradation the toxic and refractory pollutants in catalytic ozonation system.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 24
·20959-20967
·
IF 2.324
Wu Xiang-Feng,Zhang Chen-Xu,Wang Yu-Duan,Su Jun-Zhang,Zhang Jia-Rui,Feng Yan-Mei,Zhang Mi,Tong Xin,Zhang Wei-Guang,Sun Xiu-Guo
The Ag 2 CrO 4 /SnO 2 n–n type heterojunction has been fabricated by coupling Ag 2 CrO 4 particles with SnO 2 nanorods via an in situ synthetic method. The photocatalytic degradation mechanism of the as-prepared heterojunction has also been discussed. Characterization results revealed that the as-fabricated Ag 2 CrO 4 /SnO 2 composites could reinforce the photo-degradation competencies for rhodamine B dilute solution compared to pure Ag 2 CrO 4 and SnO 2 samples. As the increase in the molar ratios of Ag 2 CrO 4 –SnO 2 , the photocatalytic degradation efficiency appeared to the tendency of first increasing and then decreasing. When it was 4:10, in 90 min, the as-obtained samples possessed the vintage photocatalytic degradation efficiency of 95.8% among of pure SnO 2 , Ag 2 CrO 4 and the as-prepared composites with various molar ratios, respectively. Furthermore, the Ag 2 CrO 4 and SnO 2 were connected via chemical bonds to form the homogenous heterojunction. It could boost the separation and transfer of the photogenerated holes and electrons. In addition, the holes, hydroxyl and superoxide radicals played a major role during the photodegradation process.
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
·
2015
·Vol. 54
·期 8
·1036-1043
·
IF 3.113
Xueteng Cao,Daniel Horák,Zesheng An,Zdeněk Plichta
Nonspecific interaction is a key parameter affecting the efficiency of proteins, nucleic acids or cell separation. Currently, many approaches to introduce antifouling properties to materials have been developed. Among these, surface modification with polymer brushes plays a prominent role. The aim of this study was to synthesize new magnetic microspheres grafted with poly( N,N -dimethylacrylamide) (PDMA) that resist nonspecific protein adsorption. Monodisperse macroporous poly(2-hydroxyethyl methacrylate) (PHEMA) microspheres, 4 μm in size, were synthesized by a multiple swelling polymerization method. To render the microspheres magnetic, iron oxide was precipitated inside the microsphere pores. Functional carboxyl groups, introduced by the hydrolysis of the 2-(methacryloyl)oxyethyl acetate (HEMA-Ac) comonomer, were used to react with propargylamine, followed by coupling of a chain transfer agent via an azide-alkyne click reaction. PDMA was grafted from the PHEMA microspheres using reversible addition-fragmentation chain transfer polymerization (RAFT), resulting in surfaces with more than 81 wt % PDMA attached. The successful modification of the microspheres was confirmed by XPS. The magnetic microspheres grafted with PDMA showed excellent antifouling properties as tested in bovine serum protein solutions. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016 , 54 , 1036–1043
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