ANALYTICAL CHEMISTRY
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2022
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IF 8.008
Kai Niu,Pengcheng Sun,Jiping Chen,Xianbo Lu
Due to the fascinating properties such as high porosity, large surface areas, and tunable chemical components, metal–organic frameworks (MOFs) have emerged in many fields including catalysis, energy storage, and gas separation. However, the intrinsic electrical insulation of MOFs severely restricts their application in electrochemistry. Here, we synthesize a series of 2D conductive MOFs (cMOFs) through tuning the structure with atomic precision using simple hydrothermal methods. Various electroactive probes are used to reveal the structure–property relationships in 2D cMOFs. Then, we demonstrate the first exploration and implementation of 2D cMOFs toward the construction of electrochemical biosensors. In particular, the biosensor based on Cu3(tetrahydroxy-1,4-quinone)2 [Cu3(THQ)2] displays a remarkably improved electrocatalytic performance at a much lower potential. The mechanism study reveals the essential role of charge-transfer interactions between the dense catalytic sites of Cu3(THQ)2 and analytes. Furthermore, the Cu3(THQ)2-based biosensor demonstrates robust anti-interference capability, good stability, fast response speed, and an ultralow detection limit for paraoxon. These promising results indicate the great potential of cMOFs in biomedical, food safety, and environmental sensing applications.
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PubMed
高影响因子
Journal of Cleaner Production
·
2023
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IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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Journal of Energy Chemistry
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2023
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IF 13.1
Baoyu Wang,Peng Zhou,Ximing Yan,Hu Li,Hongguo Wu,Zehui Zhang
In this work, a dual-size MOF-derived Co catalyst (0.2Co 1-NPs @NC) composed of single atoms (Co 1 ) and highly dispersed nanoparticles (Co NPs) was prepared by in-situ Zn evaporation for the high-performance conversion of lignin-derived o- methoxyphenols (lignin oil) to cyclohexanols (up to 97% yield) via cascade demethoxylation and dearomatization. Theoretical calculations elaborated that the dual-size Co catalyst exhibited a cooperative effect in the selective demethoxylation process, in which the Co NPs could initially dissociate hydrogen at lower energies while Co 1 remarkably facilitated the cleavage of the C Ar − OCH 3 bond. Moreover, the intramolecular hydrogen bonds formed in the o -methoxy-containing phenols were found to result in a decrease in the bond energy of the C Ar − OCH 3 bond, which was more prone to be activated by the dual-size Co sites. Notably, the pre-hydrogenated intermediate (e.g., 2-methoxycyclohexanol from guaiacol) is difficult to undergo demethoxylation, indicating that the selective C Ar − OCH 3 bond cleavage is a prerequisite for the synthesis of cyclohexanols. The 0.2Co 1-NPs @NC catalyst was highly recyclable with a neglect decline in activity during five consecutive cycles. This cooperative catalytic strategy based on the metal size effect opens new avenues for biomass upgrading via enhanced C O bond cleavage of high selectivity.
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Chemosensors
·
2022
·Vol. 11
·期 1
·27
·
IF 4.229
Meili Liu,Liuheng Xue,Qinghua Feng,Yingsha Wang,Jia Liu,Shouting Zhang,Wenping Hu
The Co3O4hollow dodecahedron (Co3O4@CN) was prepared by calcining ZIF-67 in N2and then air atmosphere. In the Co3O4@CN compound material, Co3O4nanoparticles (Co3O4NPs) are anchored in the carbon skeleton, solving the aggregation problem of Co3O4NPs. Because Co3O4@CN retains the porous structure of ZIF-67, and the presence of Co2+and Co3+favors electron transfer between the enzyme substrates, it has excellent peroxidase-like (POD-like) activity. Enzymatic kinetic tests show that Co3O4@CN has approximately six times more affinity for TMB than HRP and the maximal reaction rate is approximately three times that of HRP. The cholesterol sensor was constructed with Co3O4@CN, and its linear range was 20-1000 μM, and the detection limit was 14.33 μM. The application of Co3O4@CN to the detection of human serum cholesterol will be a valuable research direction.Keywords:Co3O4@CN compound material;peroxidase-like activity;cholesterol sensor
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yin Lu,Jiamei Liu,Wenqian Zhao,Kan Zhang
The frequent fire accidents and sustainable development concerns have called for more durable and safer flame retardant polymeric materials produced from natural renewable resources. Herein, we successfully developed a molecular design strategy by incorporating oxazine ring substituents into bio-benzoxazine monomers to achieve highly thermally stable and intrinsically flame retardant thermosets. The polybenzoxazine derived from a small-molecule bio-benzoxazine resin, 3-(furan-2-ylmethyl)-3,4-dihydro-2 H -benzo[ e ] [1] , [3] oxazine ( PH-fa ), was found to reveal a very high glass transition temperature of 317 °C. However, it was thermally unstable during the polymerization process and easy to ignite without self-extinguishing characteristic. 9,10-Dihydro-9-oxa-10-phosphaphenathrene-10-oxide (DOPO) was incorporated into PH-fa to obtain an oxazine ring substituted bio-benzoxazine ( PH-fa-[4]DOPO ) possessing non-ignitable capability, which reached the V-0 rating of UL-94 test. Unfortunately, a trade-off between the thermal stability and flame retardancy was discovered through the DOPO modification. Further incorporating renewable benzaldehyde into PH-fa -[4] DOPO generated a 2,4-substituted bio-benzoxazine ( PH-fa-[2]ph[4]DOPO ) with ideally enhanced flame retardancy as well as remained higher thermal stability. These results highlight the utility of sustainable molecular design and provide molecular-level insights into roles of oxazine ring substituents in thermal and fire-related properties of polybenzoxazines, as well as a new angle for the design of non-ignitable and high-performance bio-thermosets based on benzoxazine chemistry.
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TALANTA
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2022
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IF 6.556
Mengzhen Ren,Yujie Zhang,Lanlan Yu,Lingbo Qu,Zhaohui Li,Lin Zhang
Nanozyme with the merit of excellent and adjustable catalytic activity, outstanding stability and low cost is a promising alternative for natural enzymes widely applied in a variety of fields. In the present study, a new two-dimensional cobalt-based MOF nanocomposite designated as MVCM@β-CD was synthesized. Combined with the strategies of increasing the ratio of Co(Ⅲ)/Co(Ⅱ) and modifying with small molecule β-cyclodextrin (β-CD), MVCM@β-CD displayed remarkably enhanced oxidase-mimicking activity, which was attributed to synergistic effect from large surface area of two dimensional Co-MOF nanosheet , numerous exposed active sites, high-proportioned trivalence of cobalt and regulating action of β-cyclodextrin. The addition of aminophenol isomers inhibited the catalytic oxidation process, resulting in different color change of the solution and UV–Vis absorption behaviors, based on which a sensitive ratiometric colorimetry for m -aminophenol ( m -Ap) and a simple colorimetric p -aminophenol ( p -Ap) detection method were developed with the detection limit of 0.16 μM and 1.01 μM, respectively. This method realized the colorimetric differentiation of aminophenol isomers, which provided a simple, accurate and low-cost approach for visual discrimination without complicated instrument and procedure, especially appropriate for on-site detection.
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高影响因子
FUEL
·
2022
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IF 8.035
Tao Liu,Zhipeng Tian,Weijie Zhang,Bowen Luo,Libin Lei,Chao Wang,Jianping Liu,Riyang Shu,Ying Chen
Selective hydrodeoxygenation (HDO) of phenolic compounds derived from the pyrolysis lignin-oil to desired products is a promising route in the high-value utilization of biomass-derived products. Cyclohexanol, as one of the important chemical materials, is an intermediate of catalytic HDO of guaiacol. Controllable selective HDO is conducted to improve the cyclohexanol selectivity over RuFe bimetallic catalyst prepared by ethylene glycol reduction method in this work. 99.99% guaiacol conversion and 81.35% cyclohexanol selectivity are obtained over optimized 2Ru2.5Fe/Al 2 O 3 -EG catalyst, which is better than those over 2Ru/Al 2 O 3 -EG catalyst. The mild catalyst preparation method gives it a high dispersion and uniform distribution of Ru and Fe species on the support. Various characterizations have proved that the intimate contact between Ru and Fe 2 O 3 species contributes to the improvement of cyclohexanol selectivity. Partial blockage of Ru sites by Fe 2 O 3 species slightly reduces the hydrogen adsorption capacity while the addition of Fe helps enhancing the hydrogenolysis of C-OMe bond. The reciprocal effect facilitates the removal of methoxyl groups and hinders the dehydroxylation of cyclohexanol to cyclohexane. Besides, other phenolic compounds and pyrolysis lignin-oil as substrates also show good selective HDO reactivity to corresponding alkyl cyclohexanols, implying potential application in the transformation from lignin-oil to high-value products.
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Food Chemistry-X
·
2023
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IF 6.1
Shi-Kang Chen,Hai-Feng Lin,Xin Wang,Yi Yuan,Jun-Yi Yin,Xiao-Xiao Song
In this study, ten pea ( Pisum sativum L.) varieties were compared in their nutrient composition, phenolic compounds, antioxidant properties and their diversity were deciphered by multivariate analysis of correlation analysis and principal component analysis (PCA). The ten pea cultivars are rich in nutrients with different contents in lipid (0.57 to 3.52%), dietary fiber (11.34 to 16.13%), soluble sugar (17.53 to 23.99%), protein (19.75 to 26.48%) and starch (32.56 to 48.57%). Through the UPLC-QTOF-MS and HPLC-QQQ-MS/MS analysis, the ethanol extracts of ten peas mainly included 12 kinds of phenolic substances and showed good antioxidant activities on the 1,1-Diphenyl-2-picrylhydrazyl (DPPH) radical scavenging, ferric reducing antioxidant power (FRAP) and oxygen radical absorbance capacity (ORAC). The phenolic content and protocatechuic acid showed a positive correlation with antioxidant capacity. All results provide theoretical basis for the development and rational application of different varieties of peas and their related products.
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Environmental Science-Nano
·
2022
·Vol. 10
·期 2
·476-488
·
IF 9.473
Xiaolei Zhang,Bin Liu,Tao Wei,Zongming Liu,Jinkai Li
Micromotors, which combine nanotechnology with autonomous movement, have attracted extensive interest in the field of environmental monitoring and remediation. However, it is still a challenge to develop a facile method to prepare a multifunctional micromotor for simultaneously detecting and removing organic pollutants from water. Herein, we report a novel magnetically controllable Janus micromotor with peroxidase-like activity for simultaneous colorimetric detection and degradation of hydroquinone (HQ). Such polyethylene glycol (PEG) modified Janus micromotor was composed of calcined manganese(II) acetate modified Fe3O4@polyacrylic acid (PAA) and ferric oxide (Fe3O4) nanoparticles. The obtained Janus micromotors (P-FM JMMs) have a unique asymmetric structure and exhibit autonomous motion with a maximum speed of 95.2 ± 3.02 μm s−1 in the presence of 100 mM H2O2. Combining the advantages of autonomous motion and superior peroxidase-like activity, P-FM JMMs as effective micromotors were established for dynamic sensitive colorimetric detection of HQ with a detection limit of 0.0923 μM and rapid degradation of HQ via excellent Fenton-like activity in water. In addition, such Janus micromotors also could achieve effective magnetic recovery to reduce water pollution. The strategy provides a new insight for the future multifunctional task allocation of micromotors on demand.
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INDUSTRIAL CROPS AND PRODUCTS
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2022
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IF 6.449
Xinyu Lu,Xiaoli Gu
Lignin, commonly treated as a waste from industrial or agricultural/forestry activities, can be used as a sustainable alternative of fossil phenol to fabricate lignin-based epoxy resins. In this study, the cured samples of lignin-based epoxy resins were prepared after curing process, and their combustion behaviors were investigated by thermogravimetric analysis coupled with Fourier transform infrared spectrometer (TG-FTIR) and cone calorimeter test. Results showed that these as-prepared epoxy thermosets (containing 0%, 5%, and 10% lignin) contained a higher LOI (limited oxygen index) value compared to others commercial resins reported in previous literature. Furthermore, they were all self-extinguishing materials during the first burning process, which was primarily contributed to their high-compactness crosslinking structure. Lignin addition would cause a negative effect on the thermomechanical properties of cured samples due to the decrease of crosslinking density, while better excellent gaseous inhibition and charring capacity can be obtained after lignin addition. This study presented an effective strategy to incorporate lignin into epoxy resin system via chemical crosslinking using glyoxal in place of formaldehyde as a green crosslinking agent to improve the combustion behaviors via reducing smoke releasing and increasing char formation, which was also beneficial for lignin valorization.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2022
·
IF 6.056
Yue Sun,Lin Zhou,Xiao Shan,Tiantian Zhao,Meirong Cui,Wenqian Hao,Binbin Wei
Polygonatum is a medicinal and edible homologous food, for which nine steaming and nine drying (SAD-9) is the most used processing method. The processed polygonatum not only changes its components, but also causes the fluctuation of metabolites in vivo . UPLC-QTOF/MS (Ultraperformance liquid chromatography-Quadrupole time of flight mass spectrometry) was employed to analyze the changes in components and the plasma untargeted metabolomics, thus, the differences in vitro of three groups of polygonatum (Raw Polygonatum, RP; two steaming and two drying, SAD-2; nine steaming and nine drying, SAD-9) and their effects on metabolic fluctuations in vivo were revealed. Results showed that the components, such as protein, fat, polysaccharide, flavonoids, saponins and isoflavones changed after processing. Moreover, 4 types of Lysophosphatidylcholines, the major differential metabolites, were highly expressed in rats’ plasma of SAD-9 group. Furthermore, through network pharmacological analysis, it was found that liquiritigenin and 4′,5-dihydroxyflavone activated PLA2 type enzymes to promote the production of lysophosphatidylcholine, and the processing method of SAD-9 was conducive to the role of these two components. These findings indicated the dissimilarity of components and metabolic profiles of polygonatum under different processing times, and revealed the advantages of SAD-9 processing methods.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Dazhen Xiong,Yang Wang,Huihui Ma,Lige Lu,Qian Zhang,Yunlei Shi,Yang Zhao,Jianji Wang
5-Hydroxymethylfurfural (HMF) is a key biobased platform compound for the production of high-value chemicals and fuels. However, separation and purification of HMF is currently the bottleneck for HMF production. In this work, a novel class of temperature-responsive deep eutectic solvent (DES)–water systems have been explored to selectively separate HMF from reaction mixtures. The fructose dehydration reaction was conducted in homogeneous DES–H2O systems, and then, the produced HMF was migrated to the DES-rich phase while the unreacted fructose was retained in the H2O-rich phase upon cooling. Thus, selective separation of HMF was realized. It was found that water–water and DES–DES interactions predominate over DES–water interactions during cooling, thus resulting in upper critical solution temperature phase separation. Under optimal conditions, the partition coefficient and separation factor of HMF could reach up to 78 and 609, respectively, which is about 5 and 13 times those reported in ionic liquid-based aqueous biphasic systems. Furthermore, HMF could be removed from the DES-rich phase, giving a high recovery efficiency of 69%, which is much higher than the best value reported in the literature. At the same time, DES was regenerated and reused in the next process, and no obvious decrease in partition coefficient of HMF was observed after six cycles.
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