Materials Advances
·
2021
·Vol. 3
·期 1
·272-281
·
IF 0
J. Cheng,P. Ganesan,Z. Wang,M. Zhang,G. Zhang,N. Maeda,J. Matsuda,M. Yamauchi,B. Chi,N. Nakashima
Perovskite oxides with a low cost and high catalytic activity are considered as suitable candidates for the oxygen evolution reaction (OER)/oxygen reduction reaction (ORR), but most of them favour only either the ORR or the OER. Besides, their underlying catalytic mechanisms are subject of an ongoing debate. Herein, La0.8Sr0.2CoO3−δ (LSC) was selected as a base perovskite oxide for doping different elements into its B-site to fabricate four different La0.8Sr0.2Co0.8M0.2O3−δ (LSCM; M = Ni, Fe, Mn, and Cu) perovskite oxides. Among the catalysts tested with and without multi-walled carbon nanotubes (MWNTs), La0.8Sr0.2Co0.8Fe0.2O3−δ (LSCF) outperformed any other catalysts in terms of both OER and ORR activity. The OER/ORR activity enhancement with LSCF is also discussed based on spectroscopic and microscopic analyses and lattice oxygen transportation.
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Molecular Catalysis
·
2021
·
IF 5.062
Guoliang Gao,Huangze Yu,Xue Lu Wang,Ye-Feng Yao
The alloy catalyst formed by transition metal and a small amount of noble metal has become the most promising substitute for M-based ( M = Pt, Pd, Ru, Rh) catalyst. However, due to the direct exposure of the metal core to the electrolyte, it is vulnerable to corrosion and oxidation, which in turn reduces the catalytic stability and is becoming a major obstacle to sustainable hydrogen production. The present work addresses this issue by developing a one-step immersion-adsorption-pyrolysis strategy for synthesizing FeM alloy nanoparticles with N-doped carbon coatings (FeM@CN) for use as electrocatalysts in the HER. The deliberately designed metal-organic framework material was used as the precursor of catalyst synthesis to achieve the carbon coatings and simultaneously the heteroatom in-situ doping for the alloy nanoparticles. The optimal FePt@CN demonstrates excellent catalytic stability and HER activity in an acidic electrolyte medium. The reactions obtain a small overpotential of 28 mV to achieve current densities of 10 mA cm −2 , which are comparable to a high-performance commercial Pt/C electrocatalyst with a much higher Pt loading. The FeRu@CN also demonstrates an outstanding performance with an overpotential of only 18 mV to achieve a current density of 10 mA cm −2 in an alkaline medium.
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Frontiers in Cellular and Infection Microbiology
·
2020
·
IF 4.123
Ali Md Kaisar,Zhen Gong,Nzungize Lambert,Stojkoska Andrea,Duan Xiangke,Li Chunyan,Duan Wei,Xu Junqi,Xie Jianping
The Mycobacterium (M.) tuberculosis comprising proline–glutamic acid (PE) subfamily proteins associate with virulence, pathogenesis, and host-immune modulations. While the functions of most of this family members are not yet explored. Here, we explore the functions of “PE only” subfamily member PE31 (Rv3477) in virulence and host-pathogen interactions. We have expressed the M. tuberculosis PE31 in non-pathogenic Mycobacterium smegmatis strain (Ms_PE31) and demonstrated that PE31 significantly altered the cell facet features including colony morphology and biofilm formation. PE31 expressing M. smegmatis showed more resistant to the low pH, diamide, H2O2 and surface stress. Moreover, Ms_PE31 showed higher intracellular survival in macrophage THP-1 cells. Ms_PE31 significantly down-regulated the production of IL-12p40 and IL-6, while up-regulates the production of IL-10 in macrophages. Ms_PE31 also induced the expression of guanylate-binding protein-1 (GBP-1) in macrophages. Further analysis demonstrates that Ms_PE31 inhibits the caspase-3 activation and reduces the macrophages apoptosis. Besides, the NF-κB signaling pathway involves the interplay between Ms_PE31 and macrophages. Collectively, our finding identified that PE31 act as a functionally relevant virulence factor of M. tuberculosis.
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Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 30
·6459-6468
·
IF 5.344
Xiaodan Zhang,Yuwan Lu,Qiumeng Chen,Yuming Huang
A self-templated strategy was adopted to design hollow Co3O4/MO3 (M = Mo, W) mixed-metal oxides via the Mo or W doping of ZIF-67, and subsequent pyrolysis under an atmosphere of air at a low temperature of 450 °C. The hollow Co3O4/MO3 (M = Mo, W) mixed-metal oxides displayed tunable oxidase-like and peroxidase-like activities able to efficiently catalyze the oxidation of TMB to generate a deep blue color in the absence or presence of H2O2. Relative to that of the un-doped Co3O4, the oxidase mimic activity of the Mo-doped Co3O4 increased to 1.3 to 2.1-fold, while its peroxidase mimic activity increased to 7.1 to 19.9-fold, depending on different Mo doping amounts. The oxidase mimic activity of the W-doped Co3O4 increased to 2.1 to 2.3-fold, while its peroxidase mimic activity increased to 4.8 to 5.9-fold, depending on the different W doping amounts. The Mo- and W-doped Co3O4 nanohybrid exhibited both higher O2 and H2O2 activating capability, and their H2O2 activating capacity was superior to the O2 activating capability. Furthermore, the Mo- and W-doped Co3O4 nanohybrids exhibited similar O2 activating abilities, while the Mo-doped one displayed a higher H2O2 activating capability than the W-doped one. The discrepant peroxidase-like nature of Mo- and W-doped Co3O4 nanohybrids is likely attributed to their different catalytic mechanisms. The peroxidase-like activity of Mo-doped Co3O4 is highly related to the ˙OH free radical, while that of W-doped Co3O4 is likely ascribed to the electron transfer between TMB and H2O2. The Km values of Co3O4/MoO3 for TMB and H2O2 were 0.0352 mM and 0.134 mM, which were 3.2- and 1.9-fold lower than that of pure Co3O4, respectively. A Co3O4/MoO3-based colorimetric platform was developed for the determination of H2O2 in the 0.1–200 μM range, with a limit of detection of 0.08 μM (3σ). Based on the thiocholine (TCh) inhibition of the excellent peroxidase-like activity of Co3O4/MoO3 and the TCh generation via acetylcholinesterase (AChE) catalyzed hydrolysis of acetylthiocholine chloride (ATCh), the colorimetric platform was extended to screen AChE activity and its inhibitor.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2023
·
IF 4.3
Jian Yang,Yuen Muk Fung,Peng Wu,Yuan Li,Xiang Liu,Kui Zhang
Photoluminescence (PL) was the core of carbon nano dots (CDs). However, there were different opinions about origin of the PL. Also, the cause for enhanced PL performance via nitrogen doping was still obscure occasionally. However, the fluorophore certification provided an easier understanding on the PL and the surface group ascertainment facilitated nitrogen doping on CDs via surface modification. Imaginably, if CDs were purified in the first place discussions on the PL would be more convincing. Herein, CDs were obtained by hydrothermal treatment on glucose solution and were purified successively via an extraction of ethyl acetate (represented with gCDs). Nitrogen doping was accomplished successfully via the reaction between amine of m -phenylenediamine and the carboxyl of gCDs (the product was represented with N-gCDs). That realized the notable red-shift of the emission with remarkable enhancement of fluorescence quantum yield. Experiments revealed that aldehyde was the fluorophore and C = C bonds constructed the fluorescent skeleton of gCDs or N-gCDs, which were also supported by ab initio calculations on the fluorescent models for gCDs and N-gCDs. Cellular imaging experiment indicated N-gCDs could penetrate cytomembrance of MCF-7 successfully and stained cytoplasm and nucleus effectively during the cell cultivation, which excelled several nitrogen-doped CDs in this aspect.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiwen Tao,Zhengguang Zhang,Zheng Li,Shuangsheng Xiong,Shengmei Wang,Faming Gao,Chen Wang,Li Hou
Potassium-ion batteries (PIBs) have become the desirable alternatives for lithium-ion batteries (LIBs) originating from abundant reserves and appropriate redox potential, while the considerable radius size of K+ leading to poor reaction kinetics and huge volume expansion limits the practical application of PIBs. Hybridization of transition-metal phosphides and carbon substrates can effectively optimize the obstacles of poor conductivity, sluggish kinetics, and huge volume variation. Thus, the peapod-like structural MxPy@BNCNTs (M = Fe, Co, and Ni) composites as anode materials for PIBs were synthesized through a facile strategy. Notably, the unique architecture of B/N codoped carbon nanotube array as fast ion/electron transfer pathways effectively improves the electronic conductivity of composites. The MxPy nanoparticles (NPs) are encapsulated in BNCNTs with an amorphous carbon layer (5–10 nm), which discernibly alleviate the volume changes during potassiation/depotassiation. In conclusion, the composites show a commendable cycling performance, possessing reversible capacities of 111, 152, and 122 mA h g–1 after 1000 cycles at 1.0 A g–1 with a negligible capacity loss for FeP@BNCNT, CoP/Co2P@BNCNT, and Ni2P@BNCNT electrodes, respectively. Especially, after 1000 cycles at 2.0 A g–1, the CoP/Co2P@BNCNT electrode still possesses a capacity of 87.9 mA h g–1, demonstrating excellent rate performance and long-term life. This work may offer an innovative and viable route to construct a stable architecture for solving the issue of poor stability of TMP-based anodes at a high current density.
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JOURNAL OF SOLUTION CHEMISTRY
·
2023
·Vol. 52
·期 7
·762-789
·
IF 1.2
Li Min,Zhang Xiaocheng,Yu Yingmin,Liu Lanmu
The extractive distillation was used to separate ethylbenzene and m-xylene. After the solvent screening, 1,2,4-trichlorobenzene was chosen as the extractive solvent. The vapor–liquid equilibrium (VLE) of binary mixtures of m-xylene, ethylbenzene, and 1,2,4-trichlorobenzene was measured at 101.33 kPa. The measurements were taken with a modified Rose equilibrium still. The Wisniak’s test was used to assess the thermodynamic consistency of the VLE experimental results. To obtain the binary interaction parameters, the binary VLE experimental data were correlated with the NRTL, Wilson, and UNIQUAC activity coefficient models. The results showed that three models all fit the experimental values of three binary systems well, and the ternary VLE data of m-xylene + ethylbenzene + 1,2,4-trichlorobenzene were estimated using Aspen Plus V11 based on these model parameters. The experimental data agree well with the estimation values generated from three models. Finally, the effect of 1,2,4-trichlorobenzene as an extractant was analyzed, and it is proved to have a good influence on the separation of ethylbenzene from mixed xylenes by extractive distillation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kangyu Liu,Bingzhang Shao,Haichao Liu,Jinlong He,Aiguo Zheng,Genghong Li,Bo Zheng,Zeyang Li,Wei Liu,Xuefeng Li,Baoning Zong
Antibacterial monomers are prerequisites for synthesizing antibacterial polymers, especially during the current COVID-19 pandemic. Dimethyl-protected cyclic lysine (DMCL) is a promising functional monomer for nylon-6 based self-cleaning antibacterial polymers. However, the production of DMCL still faces formidable challenges, such as harsh reaction conditions and low catalyst activities. In this study, we developed a Pd/ m -Al 2 O 3 -Si catalyst, which exhibited high efficiency in converting α -amino- ε -caprolactam ( α -ACL) to DMCL, affording a yield of as high as 97.1% at 100 °C and 1 MPa H 2 . The lack of Brönsted acid sites on the catalyst surface facilitated the formation of DMCL and suppressed undesirable hydrolysis or cracking by-products from the lactam-based reactant. The recycled experiments showed that Pd/ m -Al 2 O 3 -Si performed excellent stability and physical strength with essentially no damage to its microspheres after the reaction. The nylon‑6 copolymers produced from the as-synthesized DMCL exhibited similar structure and thermal stability with pure nylon-6, showing great potential in synthesizing the self-cleaning antibacterial polymers. This work provides a sustainable and efficient method for producing DMCL and other lysine-based antibacterial monomers, showing a great prospect for the utilization of bio-based chemicals in synthesizing functional polymers.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2018
·
IF 3.927
Yi Yang,Huiping Zhang,Ying Yan
A novel microfibers entrapped carbon-nanotube composite catalyst with iron loaded (MF-CNT-Fe 2 O 3 ) was develop followed by fixed bed catalytic wet peroxide oxidation (CWPO) of m-cresol. Firstly, the microfibers entrapped carbon-nanotube composite (MF-CNT) support was prepared by wet lay-up papermaking process and sintering process and the entrapment ratio of support was evaluated. Then active components were loaded on support by metal organic chemical vapor deposition (MOCVD) method. Characterizations were carried out including Field-Emission Scanning Electron Microscope (FE-SEM), Energy Dispersive Spectroscopy (EDS), N 2 adsorption–desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H 2 -Temperature-Programmed Reduction (H 2 -TPR) and Thermogravimetric Analysis (TG), respectively. At last, catalytic activity was tested. Results showed that the best entrapment ratio (72.5%) occurred when stirring time was 9.5 min and the mass ratio of CNTs to stainless steel fibers was 6:3. Characterization results illustrated that advanced three-dimensional network was formed in the microfibers composites and catalysts performed high thermal stability. CNTs were successfully entrapped in the fibers and iron components were uniformly dispersed on supports. CWPO results showed that MF-CNT-Fe 2 O 3 catalysts prepared by MOCVD performed better than by impregnation method. Additionally, MF-CNT-Fe 2 O 3 catalysts could perform high CWPO activity (m-cresol conversion highest at 99% and TOC conversion highest at 42%, respectively). Little iron loss was observed in all treated effluents.
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ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
·
2019
·Vol. 645
·期 10
·745-751
·
IF 1.337
Xiaofang Li,Yuandong Wu,Dajiang Mei,Thomas Doert
Three new alkali metal transition metal sulfate-oxalates, RbFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O and Cs M (SO 4 )(C 2 O 4 ) 0.5 · H 2 O ( M = Mn, Fe) were prepared through hydrothermal reactions and characterized by single-crystal X-ray diffraction, solid state UV/Vis/NIR diffuse reflectance spectroscopy, infrared spectra, thermogravimetric analysis, and powder X-ray diffraction. The title compounds all crystallize in the monoclinic space group P 2 1 / c (no. 14) with lattice parameters: a = 7.9193(5), b = 9.4907(6), c = 8.8090(6) Å, β = 95.180(2)°, Z = 4 for RbFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O; a = 8.0654(11), b = 9.6103(13), c = 9.2189(13) Å, β = 94.564(4)°, Z = 4 for CsMn(SO 4 )(C 2 O 4 ) 0.5 · H 2 O; and a = 7.9377(3), b = 9.5757(4), c = 9.1474(4) Å, β = 96.1040(10)°, Z = 4 for CsFe(SO 4 )(C 2 O 4 ) 0.5 · H 2 O. All compounds exhibit three-dimensional frameworks composed of [ M O 6 ] octahedra, [SO 4 ] 2– tetrahedra, and [C 2 O 4 ] 2– anions. The alkali cations are located in one-dimensional tunnels.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Wen Li,Kuncan Wang,Junjie Huang,Xiao Liu,Dun Fu,Jiale Huang,Qingbiao Li,Guowu Zhan
Metal–organic frameworks have been exploited as excellent solid precursors and templates for the preparation integrated nanocatalysts with multicomponent and hierarchical structures. Herein, a novel synthetic protocol has been developed to fabricate versatile Zr-based solid solutions (such as ZnO–ZrO2, Co3O4–ZrO2, and CuO–ZrO2) via pyrolysis of Schiff base-modified UiO-66 octahedrons (size <100 nm), which were then utilized as efficient catalysts for CO2 hydrogenation. The Schiff base serves as an effective bridge to dope secondary metal ions into UiO-66 frameworks with controlled amounts of 0.13–8.8 wt %, which are initially hard to achieve. Interestingly, by simply changing the loading metal ions, the selectivity of C1 hydrogenation products can be facilely tuned. For instance, the maximum CO2 conversion of ZnO–ZrO2, Co3O4–ZrO2, and CuO–ZrO2 solid solutions were 5.8, 11.4, and 22.5%, with the main product selectivity of 70% CH3OH, 92.5% CH4, and 86.7% CO, respectively. Moreover, in situ diffuse reflectance infrared Fourier transform spectra characterization reveals that the significant difference in C1 product selectivity is mainly determined by the balance of *HCOO, *CH3O, and *CO intermediate species over the Zr-based solid solutions.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2018
·Vol. 135
·期 23
·46354
·
IF 1.901
Bing Chen,Tingting Li,Zheng Zhang,Sui Wang,Zhiyong Guo,Yufang Hu
A promising strategy to design crosslinked photoluminescent hydrogel (PL hydrogel) is to synthesize the covalently bonded polymer chains by thermal polymerization. A proper ratio of methacrylic acid and m -phenylenediamine was used to prepare the PL hydrogel, and doping with graphene oxide and carboxymethyl chitosan improves the structure of the gel. The green and efficient hydrothermal synthesis realized a high polymerization and a short reaction time. Meanwhile, a series of properties were investigated for several combinations of hydrogels. Ultraviolet spectra, fluorescence spectra, and particle size distributions were used to characterize the PL composites. Scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, thermogravimetric analysis, rheological studies, and stress–strain tests were conducted to characterize the morphology, structure, and performance of the compound hydrogel. The adsorption properties of the PL hydrogel were characterized in adsorption tests. The results indicated that the PL hydrogel exhibited a favorable luminescence property, a certain degree of mechanical strength, and good adsorption performance. The prepared PL hydrogel has potential applications in adsorption and visual detection. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135 , 46354.
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