JOURNAL OF CHEMICAL SCIENCES
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2021
·Vol. 133
·期 2
·1-8
·
IF 1.573
Fu Guiyu,Weng Huanyuan,Lai Zhuzhi,Lin Zhengzhong,Huang Zhiyong
A rare earth complex Eu(MAA) 3 Phen was prepared with methacrylic acid and o -phenanthroline as ligands under mild conditions. The complex has a fluorescence emission centered at 618 nm with a half-peak width of 15 nm. Since the emission peak of the complex matches the absorption peak of malachite green (MG), the fluorescence of the complex will be quenched by MG through the fluorescence resonance energy transfer effect. The fluorescence testing conditions for MG were optimized based on fluorescence intensity and fluorescence quenching efficiency. The FRET efficiency was calculated to be 0.21. Under the optimal conditions, the response time was only 5 min. Compared with sulfonamides, chloramphenicol and other banned fishery drugs, the complex exhibited the highest quenching efficiency to MG. The linear range was 0.5–20 μmol L −1 , and the detection limit was 117.29 nmol L −1 (3σ/S, n = 9). This complex was used to detect MG residue in aquaculture water, and the recoveries were between 96.10% and 98.76%, indicating that the prepared fluorescent probe could be used for the rapid detection of MG in aquaculture water. Graphical abstract
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Xiaoling Lei,Ziyi Deng,Yanbo Zeng,Shisi Huang,Yiwen Yang,Hailong Wang,Longhua Guo,Lei Li
A novel composite of conductive metal organic framework and molecularly imprinted poly (ionic liquid) (CMOF-MIPIL) was prepared for highly sensitive detection of bisphenol A (BPA). Ni-based CMOFs with various organic ligands, i.e., 2,3,6,7,10,11-hexaiminotriphenylene, hexa-aminobenzene, and 2,3,6,7,10,11-hexahydroxytriphenylene were synthesized. The electrochemical properties of the obtained Ni-based CMOFs were investigated. The results demonstrated that Ni 3 (HITP) 2 had the highest conductivity and largest effective surface area. CMOF-MIPIL was then prepared with Ni 3 (HITP) 2 as supporter, BPA as template, and ILs as monomer and cross-linker. Under optimal conditions, CMOF-MIPIL sensor exhibited a linear range of BPA detection from 0.005 to 5.0 μM. The detection limit was 4.0 nM. Compared with MIPIL, Ni 3 (HITP) 2 , and CMOF-NIPIL-based sensors, the performance of this sensor for BPA detection was superior due to the excellent conductivity and the presence of specific recognition sites. In addition, CMOF-MIPIL sensor had excellent selectivity for BPA. The proposed assay was used for detection of BPA in environmental water samples, plastic bottle and fresh liquid milk samples with success.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Dong Liu,Chunling Li,Tianjun Ni,Ranpeng Gao,Jiayu Ge,Fengquan Zhang,Weidong Wu,Jinliang Li,Qian Zhao
Currently, the photo-Fenton oxidation has been increasingly studied in the domain of contaminant elimination. However, the lack of active sites and the slow charge migration in the catalytic process, still limit its practical application. 3D/0D hybrids offer a better opportunity for improving photo-Fenton activity due to their high charge mobility and increased number of catalytic sites, which is highly desirable but remains a large challenge. Herein, 3D interconnected porous g-C 3 N 4 hybridized with Fe 2 O 3 QDs (FCN) was developed and exhibited a porous structure and large specific areas. A large number of active sites and rapid charge separation/migration were achieved by the loading of ultrasmall Fe 2 O 3 QDs on the surface of g-C 3 N 4 . Moreover, the high charge mobility of this material promoted the fast conversion of Fe 3+ to Fe 2+ , resulting in the optimum synergistic effect between the photocatalytic and Fenton oxidation processes. Thus, the FCN catalysts exhibited excellent photo-Fenton oxidation activity towards the decomposition of organic contaminants (such as phenol, 2,4-dibromophenol, 2,4,6-trichlorophenol, rhodamine B and methyl orange). In addition, the roles of active species in the photo-Fenton oxidation reaction were also studied, and the results imply that the hydroxyl radicals played the most important role in the degradation of organic contaminants.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2021
·
IF 4.952
Li Li,Yafan Zhao,Jiaqi Li,Lanzhen Ban,Lina Yang,Shengnan Wang,Lijie Zhu,Hong Song,He Liu
Soy hull insoluble dietary fiber (SHIDF) extracted from soybean water-soluble polysaccharides enzymatically is a good carbon source for the growth of gut microbiota. Genomics, co-precipitation and proteomics analyses were used to investigate adhesion behavior of the gut microbiota toward SHIDF in vitro. After gut microbiota fermentation, the content of total and reducing sugars decreased with increasing fermentation time, but the content of NH 3 –N first increased and then decreased, and gas was produced mainly during 8–16 h. The structure and abundance of the gut microbiota were regulated after fermentation. Proliferation of beneficial bacteria increased, particularly Lactobacillus and Bifidobacterium . The adhesion of Lactobacillus plantarum and Bifidobacterium longum to SHIDF increased gradually with increasing adhesion time. The adhesion of two probiotics to IDF first increased and then decreased with increasing bacterial age (6, 12, 24, and 36 h). SDS, EDTA, bile salts, trypsin and proteinase K in the adhesion environment affected probiotic adhesion to SHIDF to a certain extent. Lactobacillus plantarum and Bifidobacterium longum showed significant differences in adhesion membrane proteins after SHIDF treatment. The 30S ribosomal protein S21 and GAPDH (glyceraldehyde 3-phosphate dehydrogenase), a surface protein involved in intestinal adhesion, were found to be significantly upregulated through label free proteomic analysis.
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INTERNATIONAL JOURNAL OF CHEMICAL KINETICS
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2021
·Vol. 54
·期 2
·71-80
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IF 1.462
Yufei Yang,Yadong Zhang
In this work, a HPW/ZSM-5 catalyst was prepared by impregnating phosphotungstic acid (HPW) with carrier ZSM-5 zeolite and characterized by XRD, SEM, N 2 adsorption/desorption isotherm, NH 3 -TPD, and FT-IR techniques. The catalytic performance of HPW/ZSM-5 was investigated by using the decomposition reaction of cyclohexylbenzene-1-hydroperoxide (CHBHP) to phenol and cyclohexanone. The conversion rate of CHBHP was up to 97.28%. In addition, the reusability test exhibited that the high durability HPW/ZSM-5 as the conversion rate of CHBHP only decreased by 3.11% after five runs. The kinetic study of the decomposition reaction indicated it was a primary reaction. The apparent activation energy of the decomposition reaction was 102.39 kJ·mol –1 in the temperature range of 45–60℃. All results indicate that the HPW/ZSM-5 catalyst has good performance and promising applications in acid catalyzed organic chemistry.
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CHINESE JOURNAL OF POLYMER SCIENCE
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2021
·Vol. 39
·期 12
·1528-1537
·
IF 3.603
Song Guang-Xing,Miao Teng-Fei,Cheng Xiao-Xiao,Ma Hao-Tian,He Zi-Xiang,Zhang Wei,Zhang Zheng-Biao,Zhu Xiu-Lin
In this contribution, we utilized surface-initiated atom transfer radical polymerization (SI-ATRP) to prepare organic-inorganic hybrid core/shell silica nanoparticles (NPs), where silica particles acted as cores and polymeric shells (PAzoMA*) were attached to silica particles via covalent bond. Subsequently, chiroptical switch was successfully constructed on silica NPs surface taking advantage of supramolecular chiral self-assembly of the grafted side-chain Azo-containing polymer (PAzoMA*). We found that the supramolecular chirality was highly dependent on the molecular weight of grafted PAzoMA*. Meanwhile, the supramolecular chirality could be regulated using 365 nm UV light irradiation and heating-cooling treatment, and a reversible supramolecular chiroptical switch could be repeated for over five cycles on silica NPs surface. Moreover, when heated above the glass transition temperature ( T g ) of PAzoMA*, the organic-inorganic hybrid nanoparticles (SiO 2 @PAzoMA* NPs) still exhibited intense DRCD signals. Interestingly, the supramolecular chirality could be retained in solid film for more than 3 months. To conclude, we have prepared an organic-inorganic hybrid core/shell chiral silica nanomaterial with dynamic reversible chirality, thermal stability and chiral storage functions, providing potential applications in dynamic asymmetric catalysis, chiral separation and so on.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
·
IF 3.764
Lei Zhang,Yuanyuan Feng,Linlin Li,Xiaofang Guo,Wei Du,Songbo Wang,Jun Xiang,Penggao Cheng,Na Tang
Novel Fe–enzyme complexes featuring magnetic nanoparticles (MNPs) embedded in/on enzymes in situ were fabricated for high-efficiency catalysis and separation. Fe(III) was immobilized on the inside or surface of an enzyme by metal coordination interactions and dopamine polymerization; after that, the MNPs were formed around Fe ions induced by aqueous NH3 solution. The as-prepared complexes could function as catalysts in their free state and then be separated and collected by a magnetic field after the catalytic reaction. The formation mechanism and catalytic activity of the complexes were investigated to evaluate their performance. The proposed strategy produces complexes mainly composed of the enzyme (ca. 77 wt %) and MNPs (ca. 23 wt %), and the preparation process is controllable under mild conditions to retain enzyme activity. The complex could effectively avoid the problem of steric hindrance encountered in the use of many carriers during catalysis, and the device space and mixing energy for mixing were further conserved for carrier weight inducement. This approach may open a facile and general way to prepare MNP–biomacromolecule complex with efficient load.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yihao Li,Lu Jiang,Rui Wang,Pingxiao Wu,Juan Liu,Shanshan Yang,Jiahao Liang,Guining Lu,Nengwu Zhu
In this paper, Phenol , 4-Chlorophenol (4-CP), 2,4-Dichlorophenol (2,4-DCP) and 2,4,6-Trichlorophenol (2,4,6-TCP) were selected as model pollutants to explore the oxidant mechanism by ferrate (Fe(VI)). The reactions between ferrate (1000 μM) and four phenolic compounds (100 μM) were conformed to the second-order reaction kinetics at pH 9.2, and the order of k obs followed as: k 4-CP (129 M −1 s −1 ) > k 2,4-DCP (96 M −1 s −1 ) > k 2,4,6-TCP (44 M −1 s −1 ) > k Phenol (12 M −1 s −1 ). Meanwhile, the degradation rates of all four compounds by Fe(VI) increased with increased pH (3.1–9.2). A total of 14 degradation products were identified by Liquid chromatography-Time-of-Flight-Mass Spectrometry (LC-TOF-MS), and two pathways including hydroxylation of benzene ring and substitution of chlorine atom were proposed. Hydroxyl radicals , played a vital role during the degradation of phenolic compounds. Moreover, density functional theory calculations were used to explore the degradation mechanisms. The results showed that the hydroxyl radical was more favorable to substitute chlorine atom than hydrogen atom , and the substitution on ortho-position was more favorable than para-position for all four compounds. The findings of this study could greatly improve our understanding on the degradation mechanism of chlorophenol-like compounds by Fe(VI) for environmental remediation.
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International Journal of Peptide Research and Therapeutics
·
2021
·Vol. 27
·期 2
·1343-1350
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IF 1.931
Zhao Yi,Sun Guangming,Yuan Libo,Li Jinlei,Lu Kui
Breast cancer susceptibility gene 1 (BRCA1) is an important tumor suppressor gene in the human which associated with a variety of tumor suppressor genes to inhibit the growth of malignant tumors. Breast cancer is closely related to BRCA1 mutations in humans. Four BRCA1 (856-871) mutants were screened that can interact well with RAD51 (158-180) using computer to simulate mutations at Y 856, R 866 and Q 867. These mutants were synthesized by using Fmoc solid-phase synthesis, and purified by liquid chromatography. According to the results of fluorescence spectroscopy, R866W has the strongest binding ability for the above peptides and RAD51 (158-180). Based on the circular dichroism spectrum results, the sequence of the interaction ability of the above peptides on the secondary structure of RAD51 (158-180) is Y856P, Q867C > Y856P, R866W ≈ R866W > Y856P > BRCA1. All the spectral results show that R866W have the strongest interaction ability with RAD51(158-180).
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Biao Ma,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Yuanzhi Zhu,Wenchao Peng
In this study, a facile atmospheric pressure chemical vapor deposition (CVD) method is used for the synthesis of nitrogen and sulfur co-doped hollow carbon sphere (NSC). Nano-CaCO 3 is used as template for the formation of hollow and highly hierarchical porous carbon structure. The doped percentages of N and S can be easily regulated by changing the ratio of N and S precursors and the deposition temperature. The obtained NSC is highly active for the catalytic oxidation of organic pollutants with peroxymonosulfate (PMS) as oxidant, and the reaction rate constant is 4.5 and 32.7 times faster than the single N or S doped samples, respectively. The PMS activation mechanism is comprehensively investigated by electron paramagnetic resonance (EPR) and radical quenching tests. Superoxide intermediate (O 2 •− ) and singlet oxygen ( 1 O 2 ) play the dominant role for phenol degradation. Moreover, with the introduction of secondary doped S atoms, more O 2 •− are generated for organics degradation. The excellent catalytic activity of NSC should be resulted from the optimized N and S doping percentages and large specific surface area (SSA). The synthesis strategy in this study provides a facile and low-cost synthetic method for heteroatom doped carbon materials and would expand the application of metal-free materials in the environmental remediation field.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wang Jia-Wei,Jiang Long,Huang Hai-Hua,Han Zhiji,Ouyang Gangfeng
The fulfillment of a high quantum efficiency for photocatalytic CO 2 reduction presents a key challenge, which can be overcome by developing strategies for dynamic attachment between photosensitizer and catalyst. In this context, we exploit the use of coordinate bond to connect a pyridine-appended iridium photosensitizer and molecular catalysts for CO 2 reduction, which is systematically demonstrated by 1 H nuclear magnetic resonance titration, theoretical calculations, and spectroscopic measurements. The mechanistic investigations reveal that the coordinative interaction between the photosensitizer and an unmodified cobalt phthalocyanine significantly accelerates the electron transfer and thus realizes a remarkable quantum efficiency of 10.2% ± 0.5% at 450 nm for photocatalytic CO 2 -to-CO conversion with a turn-over number of 391 ± 7 and nearly complete selectivity, over 4 times higher than a comparative system with no additional interaction (2.4%±0.2%). Moreover, the decoration of electron-donating amino groups on cobalt phthalocyanine can optimize the quantum efficiency up to 27.9% ± 0.8% at 425 nm, which is more attributable to the enhanced coordinative interaction rather than the intrinsic activity. The control experiments demonstrate that the dynamic feature of coordinative interaction is important to prevent the coordination occupancy of labile sites, also enabling the wide applicability on diverse non-noble-metal catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yangke Long,Jian Dai,Shiyin Zhao,Shixin Huang,Zuotai Zhang
Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as Co@NC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation , surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation.
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