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Table of Content
01 December 2024, Volume 40 Issue 6
Previous Issue
Contents
Chemical Research in Chinese Universities Vol.40 No.6 June 2024
2024, 40(6): 0-0.
Abstract
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Unveiling the Mechanism of Glycerol Oxidation to Lactic Acid on Pt/Sn-MFI Zeolite: an
In situ
Solid-state NMR Study
SHEN Xueyuan, QI Guodong, LIANG Jiawei, WANG Ruichen, XU Jun, DENG Feng
2024, 40(6): 935-942. doi:
10.1007/s40242-024-4168-4
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Heterogeneous glycerol (GLY) oxidation offers a promising route for the production of lactic acid (LA), a key monomer in biodegradable bioplastics. However, the specific reaction pathways remain poorly understood. This study presents a mechanistic investigation of GLY oxidation to LA using Pt/Sn-MFI catalysts. Characterizations
via
DR-UV-Vis spectroscopy,
119
Sn NMR, and TEM reveal the formation of zeolite framework Sn and well-dispersed Pt nanoparticles in Pt/Sn-MFI. The Lewis acidity of framework Sn in MFI zeolite is confirmed through
31
P NMR probe techniques. GLY conversion and LA selectivity correlate strongly with framework Sn concentration and the presence of Pt nanoparticles.
In situ
13
C solid-state NMR experiments, complemented by two-dimensional
13
C correlation NMR, allow real-time monitoring of GLY conversion and identification of various mobile and rigid (surface-adsorbed) species. Results indicate that GLY preferentially transforms to LA
via
a dihydroxyacetone (DHA) intermediate, facilitated by the Pt-Sn synergistic effect. However, accumulation of surface-adsorbed LA on Sn sites promotes consecutive oxidation of GLY to glyceric acid, tartaric acid, and ultimately CO
2
.
Review
Synthesis and Utilization of MXene/MOF Hybrid Composite Materials
JI Houqiang, LIU Yuxin, DU Guangyu, HUANG Tianyu, ZHU Ying, SUN Yangyang, PANG Huan
2024, 40(6): 943-963. doi:
10.1007/s40242-024-4179-1
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Metal-organic frameworks (MOFs) are crystalline porous architectures formed by the coordination of organic ligands with metal ions or clusters. MOFs are notable for their vast surface area, abundant active sites, high porosity, and tunable properties. However, their application in energy storage and catalysis is impeded by limited conductivity and chemical stability. A promising approach to mitigating these constraints is the integration of MOFs with other functional or conductive materials. MXenes, with their distinctive layered structure, exceptional electrical conductivity, and rich surface functional groups, provide numerous advantages when combined with MOFs. This review encapsulates the synthesis methodologies of MXene/MOF composites and explores their applications across various domains, including lithium-ion batteries, supercapacitors, lithium-sulfur batteries, zinc-ion batteries, electrocatalysts, and photocatalysts.
Articles
Design and Synthesis of Bismuth-based Metal-Organic Frameworks for Photothermal Energy Conversion
WANG Rui, WANG Ziyu, YIN Qi, LIU Haixiong, LIU Tianfu, CAO Rong
2024, 40(6): 964-969. doi:
10.1007/s40242-024-4037-1
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Template effect of the solvents plays a key role in metal-organic frameworks (MOFs) synthesis. In addition, Bi
3+
has a flexible and changeable coordination configuration, which is conducive to the construction of structurally diverse MOFs. Herein, we demonstrate that these features can be integrated into two stable bismuth-based porphyrin MOFs (named PFC-100 and PFC-101) with a wide range of light absorption. Further studies demonstrate that PFC-101 with weaker interactions of adjacent porphyrin planes achieves 22.2% photothermal conversion efficiency (PTCE), 1.5-fold higher than that of PFC-100 (14.3%) under 660 nm irradiation. This study may shed light on the impact of solvent templates on the synthesis of bismuth-based MOFs, not only enriching the MOFs library but also broadening the horizon of their potential applications.
Rh-loaded High-entropy Oxide for Efficiently Catalyzing the Reverse Water-Gas Shift Reaction
WANG Ke, ZHANG Rui, WANG Huilin, ZHANG Lingling, WANG Zijian, WANG Xiao, SONG Shuyan, ZHANG Hongjie
2024, 40(6): 970-977. doi:
10.1007/s40242-024-4079-4
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Establishing efficient CO
2
hydrogenation technology based on the reverse water-gas shift (RWGS) reaction can effectively alleviate environmental problems while providing high-value-added products. The development of suitable advanced supports is the key to improving the catalytic activity and selectivity. Herein, we designed and synthesized a new type of spinel-phase high entropy oxides [(FeCrMnAlGa)
3
O
4-
x
, FMG], which exhibited remarkable RWGS performance after loading small-size Rh nanoparticles. The CO yield was as high as 145.5 μmol
CO
·g
cat
-1
·s
-1
at 380 ℃ and the CO selectivity was nearly 100%. Moreover, the catalyst retained over 95% of the initial activity after 25 h of continuous catalyzing. Experimental and structural studies reveal that the FMG support has elemental synergy and high-entropy stability, which affect the Rh dispersion and oxygen vacancy generation, in turn achieving superior catalytic performance.
Dark-vacuole Bodies Studying by High-resolution Label-free Microscopy Assisted with Fluorescence Technology
LIU Xiangyu, ZHANG Jinrui, XU Haijiao, SHAO Lina, WANG Hongda
2024, 40(6): 978-986. doi:
10.1007/s40242-024-3271-x
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The intracellular logistics system, consisting of vesicles, plays a crucial role in cellular transport. However, there is a lack of research on the types and functions of intracellular vesicles, and new technologies are needed for further investigation. Recently, researchers have discovered a new subcellular structure known as Dark-vacuole bodies. The composition, function, and potential synergy with other organelles of these Dark-vacuole bodies remain unclear. In this study, we utilized the high-resolution label-free Fourier ptychographic microscopy, developed by our research group, along with fluorescence confocal technology, to study and analyze Dark-vacuole bodies. Our findings provide evidence of the influence of Dark-vacuole bodies on the morphology, distribution, movement, and cell cycle of living cells. Specifically, we analyzed the effects of drug induced stimulation of lipid drops and endosomes, promotion of cell endocytosis, and induction of cellular senescence on Dark-vacuole bodies. Our results indicate that Dark-vacuole bodies show little correlation with lipid drops and endocytosis vesicles, but are significantly associated with late endosomes. Furthermore, cellular senescence leads to a significant increase in the number and size of Dark-vacuole bodies. This study serves as a foundation for further confirming the nature of Dark-vacuole bodies as new organelles.
Understanding Fatigue Failure in Binary Rubber Blends: Role of Crack Initiation and Propagation
PAN Lijia, WANG Yuge, WEI Lai, SUN Zhaoyan
2024, 40(6): 987-993. doi:
10.1007/s40242-024-4001-0
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Under cyclic loading conditions, the breakdown of rubber products is mainly caused by the formation and spread of cracks. This study focuses on understanding how cracks initiate and grow during the fatigue failure of blended rubber. We prepared composite materials by blending bio-mimetic rubber (BMR) and butadiene rubber (BR) in different mass ratios and evaluated their resistance to crack initiation and propagation. Our results indicate a clear trend: as the BR content increases, crack initiation in blended rubber is inhibited, while crack propagation is enhanced. This shift leads to a change in the primary factor influencing fatigue fracture from crack initiation to crack propagation. Additionally, we observed that the fatigue life of the rubber blend initially increases and then decreases as the BMR content rises, indicating a critical threshold when the mass ratio of BMR to BR is comparable. By closely examining the materials using a scanning electron microscope (SEM) and image analysis, we confirmed that before the threshold, crack initiation is the dominant factor in fatigue failure, while after the threshold, crack propagation takes over. This study provides valuable insights into the mechanisms behind fatigue failure in rubber blends, contributing to a better understanding of this important material behavior.
Label-free Super-resolution Microscopy for Long-term Monitoring the Dynamic Interactions of Cellular Organelles
SHAO Lina, SUN Minglu, ZHANG Jinrui, XU Haijiao, YANG Hui, LI Hongru, WANG Huili, CUI Zongqiang, LI Dayu, WANG Hongda
2024, 40(6): 994-1003. doi:
10.1007/s40242-024-4006-8
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The ideal method for imaging living cells is one that allows for long-term, label-free observation in real-time with super-resolution capabilities. Such a method would overcome the drawbacks of phototoxicity and photobleaching associated with fluorescence labeling microscopy. Fourier ptychography is a promising label-free imaging technique that surpasses the diffraction limit of conventional microscopy while avoiding issues related to fluorescent labeling. However, previous Fourier ptychography microscopy (FPM) systems lacked high spatiotemporal resolution, preventing real-time observation of subcellular organelle structures in living cells. To address this limitation, we have developed a high-speed super-resolution microscope based hemispherical digital illumination (HDI) device. This system utilizes 61 light-emitting diodes (LEDs) to provide high-angle illumination with a numerical aperture (NA) of 0.98. By employing a 40×/0.6 NA objective lens, we have achieved lateral resolutions of around 150 nm, enabling us to capture images at a speed of over
1
Hz with the field of view measuring 118×118 μm
2
. HDI-FPM allows for the monitoring of various cellular processes, such as vesicular transportation, mitochondrial fusion and division, as well as cell-cell fusion over a duration of 4 h. The development of HDI-FPM represents a significant advancement in label-free imaging of living cells. It offers a comprehensive understanding of the mechanisms underlying cellular activities.
Potassium Promoted Ferrocene/Graphene for Ammonia Synthesis
CHEN Ziquan, YE Yihan, PAN Xiulian, BAO Xinhe
2024, 40(6): 1004-1010. doi:
10.1007/s40242-024-4019-3
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Innovation of catalysts for mild condition ammonia synthesis promotes the carbon neutrality. Herein we report that ferrocene supported on reduced graphene oxide (rGO) and promoted by alkali metal K is active catalyzing NH
3
synthesis from N
2
/H
2
mixture. It exhibits a NH
3
formation rate of 0.1 μmol
NH
3
·
g
c
-1
·h
-1
at 190 ℃ and increases by one order of magnitude to 2.1 μmol
NH
3
·
g
c
-1
·h
-1
at 230 ℃ and under 0.1 MPa. By contrast, both rGO promoted by K and ferrocene supported on rGO without K promotion are almost inactive under the same conditions. Density functional theory calculations validate the essential role of K promoter for facilitating the adsorption of N
2
at the coordination unsaturated iron sites in the cyclopentadienylidene form. This finding could guide further development of metal complex catalysts for mild condition ammonia synthesis.
Multifunctional Liquid Metal Active Material for Wound Repair and Motion Monitoring
via
Free Radical Polymerization Assembly
WEI Zheng, WAN Sikang, JIA Bo, CHENG Wenhao, LI Ming, CHEN Jing, LIU Yawei, ZHANG Hongjie, LIU Kai, WANG Fan
2024, 40(6): 1011-1022. doi:
10.1007/s40242-024-4195-1
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Bacterial infections and excessive oxidative stress seriously hinder the healing of skin wounds. Traditional wound dressings can only serve as physical barriers and lack active molecules essential for actively promoting wound healing. Herein, an antibacterial and antioxidant liquid metal inorganic active material is developed for wound repair through
in situ
polymerization of chitosan/acrylic acid precursor solution initiated by tannic acid-coated liquid metal nanoparticles, without extra initiators and ultraviolet (UV) light. The tannic acid component enables the inorganic active material to exhibit antioxidant property, which can remove 90% of free radicals and relieve cellular oxidative stress. The chitosan component endows the inorganic active material with antibacterial property, effectively inhibiting the growth of
Staphylococcus aureus
and
Escherichia coli
(killing ratio: 90%).
In vivo
experiment demonstrates that this inorganic active material can promote the healing of
Staphylococcus aureus
-infected wound, achieving a closure rate of 98.16% on the 9th day. Meanwhile, this inorganic active material exhibits good electrical conductivity, enabling timely and stable monitoring of human joint movements. This work offers a simple strategy for developing multifunctional inorganic active material, which holds great potential for wound repair and motion monitoring.
Prussian Blue Nanoparticles with High Oxidase-like Activity for Simultaneous Detection of Ascorbic Acid and Alkaline Phosphatase in Real Samples
TANG Zeng, LAI Yue, LU Hao, XIA Yi, JIANG Xue, XIONG Xiaoli, XIAO Ting
2024, 40(6): 1023-1032. doi:
10.1007/s40242-024-3239-x
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Prussian blue nanoparticles (PB NPs) have exhibited favorable anti-inflammatory effects in animal models, and have been proved to mimic three antioxidant enzymes: peroxidase, catalase, and superoxide dismutase. Whereas the oxidase-like activity of PB NPs has not been demonstrated. In this work, PB NPs with outstanding oxidase-like activity were demonstrated by virtue of the colorimetric substrate
o
-phenylenediamine (OPD). Interestingly, based on the oxidase-like activity, PB NPs can also catalytically oxidize vitamin B
1
(VB
1
) to strongly fluorescent product in the physiological environment without the addition of other oxidants. Considering that VB
1
has no toxicity and carcinogenicity comparing with OPD, a novel PB NPs-VB
1
fluorescent sensor was further developed for simple, nontoxic, and rapid detection of ascorbic acid (AA) in foods and alkaline phosphatase (ALP) in human serum samples by taking advantage of the reduction of PB NPs to Prussian White by AA or enzymatic hydrolysate of ALP and ascorbic acid 2-phosphate (AA2P), leading to the decrease of fluorescence intensity. The extremely low detection limits of 44 nmol/L for AA and 72 mU/L for ALP as well as the excellent applicability in real samples were both obtained. Therefore, we envision that such a novel fluorescent probe would be potentially applied in the food analysis and clinic diagnosis fields.
Highly Sensitive Ethanol Gas Sensor Based on Ag Nanoparticles Decorated In
2
O
3
ZHANG Susu, ZHANG Meng, GUO Ying
2024, 40(6): 1033-1040. doi:
10.1007/s40242-024-3244-0
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Ag nanoparticle decorated In
2
O
3
composites for high sensitivity and high selectivity detection of ethanol were prepared by hydrothermal and annealing methods. The effects of Ag content on the sensing properties of Ag decorated In
2
O
3
sensors were also investigated. It was found that all Ag decorated In
2
O
3
sensors exhibited better sensing performance in terms of sensitivity and selectivity compared to pure In
2
O
3
sensors. By optimizing the addition amount of Ag, the 7%-Ag/In
2
O
3
sensor showed the highest response to ethanol (35.6
vs
. 100 ppm, ppm=parts per million), which was about seven times higher than that of the pure In
2
O
3
sensor at 270 ℃. The improved performance of the Ag-In
2
O
3
composite sensor can be attributed to the catalytic effect of silver and the Schottky barrier formed at the Ag-In
2
O
3
interface.
Metal Acetylacetonates as Robust Catalysts for the Synthesis of Oxazolidinone from CO
2
and Aziridine Under Atmospheric Pressure
LI Bohan, GONG Yujie, LOU Huimin, WEI Yujuan, GUO Liping, WANG Hongmei, ZHANG Zulei, LI Lei
2024, 40(6): 1041-1049. doi:
10.1007/s40242-024-3253-z
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Metal acetylacetonates, a type of readily synthesized or commercially available metal complex, were demonstrated to be robust catalysts for the synthesis of oxazolidinone from CO
2
and aziridine under condition of atmospheric pressure and mild temperature, exhibiting high chemo- and regio-selectivity. Tetrabutylammonium halides were employed as cocatalysts in the reaction, and it was believed that the reaction activity was influenced by a balance of anions’ two abilities, namely their nucleophilicity in ring-opening of aziridines and their leaving capacity in ring-closing of intermediate carbamate salts to form oxazolidinones. Notably, higher nucleophilicity of these anions resulted in increased formation of dimers, which served as by-products of the reaction. The study of mechanism suggested that there should be an alternative pathway involving CO
2
derivative acting as a nucleophile during the ring-opening process, and this pathway could not be ignored when conventional nucleophiles, such as tetrabutylammonium halides are absent.
Study on Antibacterial and Biocompatibility of Thermally Crosslinked Polyvinylpyrrolidone Nanofiber Iodine Complexes
XU Dejun, HE Liu, ZENG Fudong, LIU Bo, MA Jinli, HAN Dongmei, YANG Qingbiao, DU Jianshi
2024, 40(6): 1050-1059. doi:
10.1007/s40242-024-3262-y
Abstract
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Polyvinylpyrrolidone-iodine (PVP-I) complexes are widely used in the medical and health field due to its strong antimicrobial properties and good biocompatibility, but their water solubility negates the possibility to be used as a wound dressing. In this work, the problem of PVP dissolving in water was solved by the method of thermally crosslinking, and it was found that the thermally crosslinked PVP nanofiber heated at 170 ℃ for 6 h had good liquid absorption capacity, stability and good fiber morphology. In addition, the thermally crosslinked PVP nanofiber is complexed with I
2
to endow it with excellent antibacterial properties. It has been demonstrated to have good biocompatibility through cytotoxicity and hemolysis experiments, which provides the possibility for it to be a dressing for the treatment of infectious wounds.
Reproductive Toxicities of Tetradecyltrimethylammonium Chloride and Tetradecyltrimethylammonium Bromide on
Caenorhabditis elegans
over Four Consecutive Generations
ZHANG Jing, DING Ruoqi, YU Zhenyang
2024, 40(6): 1060-1067. doi:
10.1007/s40242-024-3266-7
Abstract
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)
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Quaternary ammonium compounds (QACs) become emerging pollutants and their toxicities earn increasing attention. So far, their reproductive toxicities were poorly investigated, and their effects over generations were even less explored. In the present study, reproductive toxicities of two QACs,
i.e.
, tetradecyltrimethylammonium chloride (TTAC) and tetradecyltrimethylammonium bromide (TTAB) were studied on
Caenorhabditis elegans
with a consecutive exposure over four generations (from F1 to F4). The effects of TTAC on total and initial reproduction showed stimulation and inhibition, which oscillated from F1 to F4. The effects of TTAB on the total reproduction commonly showed stimulation over generations with the greatest stimulation in F2, and it inhibited the initial reproduction but stimulated the reproduction duration. Further exploration demonstrated that TTAC and TTAB significantly disturbed the levels of spermatocyte protein 8 (SPE8), sperm transmembrane protein 9 (SPE9), vitellogenin (Vg), major sperm protein (MSP) and ephrin receptor protein tyrosine kinase (VAB-1) and the expressions of
vab-1, ceh-18, set-2, met-2
and
mes-4
. Such disturbances demonstrated that both QACs impacted the reproductive processes
via
oocyte meiosis, gonadal support and germline development. Notably, the effects of TTAC and TTAB in parents were connected with those in the offspring, which highlighted the roles of reproduction in connecting generations. In addition, different effects between TTAC and TTAB demonstrated the anionic influences on the QACs’ toxicities.
Nano-crystallites Imine-based Copper(II) Complexes as Mimetics for Copper Oxidase Proteins: Synthesis, Characterization, DFT and Oxidase Mimicking Activity
ALHADHRAMI Abdulrahman, RAMADAN Abd El-Motaleb, FATHY Ahmed
2024, 40(6): 1068-1081. doi:
10.1007/s40242-024-3273-8
Abstract
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Three tridentate imine ligands containing N
2
S donors were synthesized
via
Schiff condensation between derivatives of both amino triazine and 2-carbonyl pyridine. The reaction of these ligands with CuCl
2
in a molar ratio of 1:1 provides three Cu(II) complexes with the general formula [CuL
n
·Cl
2
]. Analytical, electrical, magnetic, and spectroscopic studies were used to assign the molecular formulae of these metallic chelates. Density function theory (DFT) calculations confirmed the structural analysis results obtained from spectroscopic studies. The various characterization techniques used demonstrated the penta-coordinated slightly distorted square pyramidal structure for the present Cu(II) complexes
1
,
2
, and
3
. Measurements of cyclic voltammetry were done in methanol to define the electrochemical behavior of the current Cu(II) complexes. The biomimetics of catechol oxidase (C.O.) and phenoxazinone synthase (PHS) have been studied in the aerobic oxidation of some phenolic substrates, such as 3,5-di-tert-butylcatechol (3,5-DTBCH
2
) and
ortho
-aminophenol (
o
-APH
3
). The three candidate oxidase mimetics showed promising activity in the order
3
>
1
>
2
. The catalytic activity related to the structural properties of existing oxidase mimetics was discussed. The driving force (-Δ
G
°) controlling the redox reactions of the present biomolecules was calculated from the redox data of Cu(II) complexes
1
,
2
, and
3
. The potential catalytic reaction pathway for the oxidation of the studied phenolic substrates was discussed.
CNTs-promoted Co-Cu Catalyst for Efficient Synthesis of Cinnamyl Alcohol from Hydrogenation of Cinnamaldehyde
DONG Xin, LIU Cheng, ZHOU Zhaohui
2024, 40(6): 1082-1087. doi:
10.1007/s40242-024-4007-7
Abstract
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)
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With types of in-house-synthesized multi-walled carbon nanotubes (CNTs), highly active CNT-promoted Co-Cu catalysts, symbolized as Co
i
Cu
j
-
x
%CNTs (mass fraction) were prepared by the co-precipitation method from nitrate salts of the corresponding metallic components. Their catalytic performances for the cinnamyl alcohol synthesis from the hydrogenation of cinnamaldehyde were studied and compared with the corresponding CNT-free coprecipitated catalyst of Co
i
Cu
j
mixed oxide. It was shown that the appropriate incorporation of a minor amount of the CNTs into Co
i
Cu
j
oxide could significantly increase the catalytic activity for cinnamyl alcohol synthesis. Under the pressure of 5.0 MPa, the highest yield of cinnamyl alcohol reaches 94.4% with selectivity of 98.7% for the catalyst Co
2
-Cu
1
-10.0%CNTs. The addition of an appropriate amount of CNT can promote the highly dispersed catalyst and promote the recovery of the catalyst. The results show that carbon nanotube is an excellent accelerator, and its properties for unique hydrogen absorption play important roles in promoting the synthesis of cinnamyl alcohol.
ZIF-8/MS Hybrid Sponge
via
Secondary Growth for Efficient Removal of Pb(II) and Cu(II)
BIAN Hang, LI Peng, MA Yu, LIU Lin, LI Dong, ZHANG Ning
2024, 40(6): 1088-1095. doi:
10.1007/s40242-024-4009-5
Abstract
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)
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In recent years, the surge in industrialization and urbanization has led to the release of a significant amount of heavy metal ions into water. These ions, when present in drinking water, can enter the human body and cause irreversible health problem. Metal-organic frameworks (MOFs) have drawn considerable attention for their outstanding ability to remove these heavy metal ions. However, MOF powders tend to aggregate in water, reducing their adsorption efficiency and potentially leading to secondary environmental pollution. In this regard, the development of MOF composites that are highly adsorptive, recyclable, and maintain stable dispensability in water is crucial for heavy metal ions removal. Herein, the
in situ
growth of zeolitic imidazolate framework (ZIF-8) on melamine sponge (MS) using a secondary growth method is reported. The resultant composite sponges exhibit high efficiency in adsorbing Pb(II) and Cu(II) from water and maintain good reusability. These findings offer a promising method in efficiently eliminating Pb(II) and Cu(II) from aqueous solutions.
A Concise, Practical Chiral Resolution Approach of Racemic (
E
)-4,4-Dimethyl-1-(4-nitrophenyl) pent-1-en-3-ol to Its both Enantiomers
via
Strategy of Diastereomeric Ester Formation and Crystallization Using both
N
-Boc-
D
- and
N
-Boc-
L
-phenylglycines as Chiral Auxiliaries
JIANG Shanshan, YUAN Jia, QIN Yanlan, LUO Ying, JIN Zhengsheng, ZHAO Guilong, TI Huihui
2024, 40(6): 1096-1105. doi:
10.1007/s40242-024-4011-y
Abstract
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)
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Chiral secondary alcohols are an important class of functionalities commonly seen in drugs and other bioactive compounds. In an ongoing drug discovery program in our laboratories, a nitro-bearing racemic allylic secondary alcohol (±)-
1
was discovered as a promising drug candidate, and in the following preclinical studies, a concise, reliable, practical synthetic approach to its both enantiomers with high optical purities was greatly needed. In the present study, we developed a chiral resolution approach of (±)-
1
to its both enantiomers,
i. e.
, (+)-
1
and (-)-
1
,
via
the strategy of diastereomeric ester formation and crystallization using both
N
-Boc-
D
- and
N
-Boc-
L
-phenylglycines as chiral auxiliaries. The absolute configurations of all the four key intermediates were unambiguously determined by single-crystal X-ray diffraction, providing a solid foundation for the stereochemistry of the present study. The two enantiomers were obtained in high optical purities. This approach is characterized by scalability and practicality and is envisaged to enable the chiral resolution of other racemic secondary alcohols, especially those with labile groups, such as NO
2
and olefinic C=C bond.
Electrocatalytic Hydrogen Evolution by Binuclear Metal (M=Co, Fe, Mn) Xanthine Bridged Bis-corrole
XU Shiyin, CEN Jinghe, YANG Gang, SI Liping, XIAO Xinyan, LIU Haiyang
2024, 40(6): 1106-1115. doi:
10.1007/s40242-024-4013-9
Abstract
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)
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Three binuclear metal (M=Co, Fe, Mn) xanthine bridged bis-corrole complexes were synthesized and investigated as electrocatalysts for the hydrogen evolution reaction (HER). All the prepared metal bis-corrole catalysts exhibited good HER performance when using acetic acid (AcOH), trifluoroacetic acid (TFA) and
p
-toluenesulfonic acid (TsOH) as proton sources. The catalytic HER activities followed an order of Co bis-corrole (
1
)> Fe bis-corrole (
2
)> Mn bis-corrole (
3
) and complex
1
exhibited a significantly lower overpotential at -270 mV (in TsOH). Furthermore, complex
1
may go EECC and EECEC pathways in organic solvents (E: electron transfer step, C: proton coupling) and exhibit an HER activity with a turnover frequency (TOF) of 85 h
-1
and a Faraday efficiency of 94% when using water as proton source.
Prussian Blue Analogue Derived N-Doped Graphitic Carbon Wrapped Iron-Cobalt Nanoparticles as Recyclable Heterogeneous Catalysts for Friedel-Crafts Acylation
LEI Zhenyu, SUN Honglei, DONG Zhehan, SUN Shuaishuai, BI Chongyao, ZHAN Junling, WU Lin, JIA Mingjun
2024, 40(6): 1116-1126. doi:
10.1007/s40242-024-4020-x
Abstract
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)
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The rational design of efficient heterogeneous catalysts for Friedel-Crafts acylation reactions is highly desirable for meeting the need for the industrial production of various aromatic ketone compounds and biomass-derived chemicals. Herein, we reported that graphitic carbon wrapped FeCo bimetallic nanoparticles confined in nitrogen-doped carbon nanotubes, which were prepared by pyrolysis of FeCo-based Prussian blue analogue and melamine
via
a two-stage programmed heating procedure, exhibited excellent catalytic activity and recyclability for the acylation of aromatic compounds with acyl chlorides. The oxidized bimetallic species embedded in the external graphitic carbon shell should be the main active sites for the acylation reaction. The graphitic carbon shell and the carbon nanotube could provide effective protection on the active metal species against leaching through multiple interactions, leading to the formation of a highly active and durable heterogeneous catalyst for the acylation reaction.
Protonated Mesoporous Aluminosilica Nanospheres Boosting Aza-Michael Cyclization and Diels-Alder Reaction
LI Baoyan, MENG Jingjing, LI Yingding, JIANG Lingxia, CHENG Tanyu, LIU Guohua
2024, 40(6): 1127-1133. doi:
10.1007/s40242-024-4033-5
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Mesoporous aluminosilica hollow nanospheres were prepared easily, which possess very strong acid site. The heterogeneous catalyst can be utilized in both intramolecular aza-Michael addition cyclization and intermolecular Diels-Alder reaction. The catalyst could be easily recovered and reused. Furthermore, the catalyst could be used in continuous flow chemistry for the uninterrupted synthesis of 2,3-dihydroquinolin-4(1
H
)-ones, which disclosed the potential application of the present solid catalyst in both academic and industrial syntheses. In addition, the catalyst could be recovered and reused at least 7 times without obvious loss of activity.
Differential Antibacterial Effects of Chiral Co
3
O
4
SUN Jia, SONG Shanshan, GUO Caoyu, LIU Liqiang, SUN Maozhong, KUANG Hua, XU Chuanlai, GUO Lingling
2024, 40(6): 1134-1140. doi:
10.1007/s40242-024-4036-2
Abstract
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With the global spread of antimicrobial resistance, it is imperative to satisfy the need to develop novel antibacterial agents. Here, we synthesized chiral Co
3
O
4
nanoparticles (NPs) with obvious bactericidal effects. It was found that the circular dichroism (CD) spectra of
L
-Co
3
O
4
NPs and
D
-Co
3
O
4
NPs exhibited perfect mirror image inversion. Specifically, the survival rate of primary uterine fibroblast (PCS) cells reached above 90% by co-culturing with chiral Co
3
O
4
NPs. Besides, the chiral Co
3
O
4
NPs showed obvious killing ability on Gram-positive (
Staphylococcus aureus
) and Gram-negative (
Escherichia coli
O157:H7) bacteria both
in vitro
and
in vivo
. Particularly,
D
-Co
3
O
4
NPs showed better antibacterial activity. Mechanistic studies confirmed that the level of reactive oxygen species level generated by
D
-Co
3
O
4
NPs was higher than that of
L
-Co
3
O
4
NPs. Overall, the synthesized
D
-Co
3
O
4
NPs have the potential to become a kind of novel antibacterial nanomaterials.
Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis
FAN Yiwen, WANG Yang, WANG Huijuan, CHEN Yuzhen, LI Zhibo
2024, 40(6): 1141-1150. doi:
10.1007/s40242-024-4044-2
Abstract
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Multiple metal sites doped in metal-organic frameworks (MOFs) are essential for their promising application in cascade reactions. However, precision synthesis of tetrametallic MOFs with total coordination and regular shapes is challenging due to the different coordination abilities of four metal ions. Herein, a series of tetrametallic MOFs (
t
-MOFs) with four regular morphologies is successfully constructed by regulating the metal ratio, amount of morphologic modulating reagent or growth time. The
t
-MOFs can be flexibly oxidized to afford porous metal oxides (M
x
Co
3
O
4
, M=CuZnNi) under air or reduced to carbon-encapsulated CuCoNi under H
2
/Ar for different reactions to maximize the value-in-use of MOFs. In particular, the
t
-MOF@M
x
Co
3
O
4
obtained upon the surface oxidation of
t
-MOF well integrates the Lewis-base sites from MOF core with photothermal oxidation activity from M
x
Co
3
O
4
shell. The hybrid effectively catalyzes the cascade reaction of styrene oxidation coupling Knoevenagel condensation under visible light. Thus, the by-product, benzaldehyde, is successfully converted to easily separated benzylidene malononitrile to finally obtain pure styrene epoxide (SO). In M
x
Co
3
O
4
, Ni species afford good photothermal effect, Cu and Co species provide catalytic activity, and Zn species increase SO selectivity. The host-object coordination and the synergy among objects may greatly boost more complex reactions in the future.
Organic-free, Ultrafast Synthesis of K-CHA Nano-aggregates with Various Morphologies and Their Adsorption Performances
CHU Kailiang, WANG Yaquan, LIU Wenrong, BU Lingzhen, HUANG Yitong, GUO Niandong, QU Liping, SANG Juncai, LI Yaoning, SU Xuemei, ZHANG Xian
2024, 40(6): 1151-1159. doi:
10.1007/s40242-024-4045-1
Abstract
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K-Chabazite (K-CHA) zeolites were synthesized with an ultrafast procedure through an eco-friendly and cost-effective “one-pot” method. By solely employing colloidal silica and aluminum hydroxide in the K
+
/Sr
2+
system without the assistance of seeds, fluorides or organic structure as directing agents, the K-CHA nano-aggregates were successfully synthesized in a few hours. The crystallization behavior of the gels with different SiO
2
/Al
2
O
3
molar ratios (SARs) was investigated using X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray fluorescence (XRF),
27
Al and
29
Si magic angle spinning nuclear magnetic resonance (MAS NMR), Fourier-transform infrared spectra (FTIR), UV-Raman characterizations. As the nucleation rates were changed with the SARs, three kinds of K-CHA nano-aggregates, namely, hamburger-, disk- and walnut-shaped, were obtained. A possible formation mechanism of the K-CHA nano-aggregates was proposed. Additionally, the walnut-shaped sample with an SAR of 7 possessed the largest pore volume and specific surface area, resulting in the highest methane adsorption capacity. Furthermore, it exhibited a CH
4
/N
2
selectivity of more than 3 under relative pressures ranging from 0 to 0.6. This work offers guidance for modifying the stacking modes of other nano-sized zeolites.
Improving the Stability and Efficiency of Perovskite Solar Cells by Controlling the Crystallization Active Layer with Binary Anti-solvent
CHEN Diandian, Hari Bala, ZHANG Bowen, ZHAO Zhiyong, ZHAO Yunpeng, CHENG Fei, WEN Yingjie
2024, 40(6): 1160-1170. doi:
10.1007/s40242-024-4049-x
Abstract
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In this study, a hybrid anti-solvent treatment was used to prepare high-quality MA
0.9
FA
0.1
PbI
3
perovskite film, and perovskite solar cells (PSCs) with carbon counter electrodes of high stability and high efficiency were fabricated. Different ratios of chlorobenzene (CB) and toluene (TL) were utilized as binary anti-solvent, and dropwise addition was initiated within spin-coating perovskite film. By optimizing the ratio of CB and TL, the formation process of perovskite film was effectively controlled and the crystallinity and coverage of the perovskite film were improved. The carbon electrode PSCs composed of MA
0.9
FA
0.1
PbI
3
film treated with anti-solvent exhibited a maximum power conversion efficiency (PCE) of 12.21% under air atmosphere conditions, which was higher than that of the PSCs of MA
0.9
FA
0.1
PbI
3
film without anti-solvent treatment. Finally, PSCs showed that the device still exhibits 90% of the initial efficiency after being stored in the air for 100 d, which shows excellent stability.
Highly Selective CO
2
Separation on Na-exchanged DNL-6 Synthesized by Utilization of Spent Industrial Catalyst
TANG Yanling, WANG Quanyi, YAN NaNa, ZHANG Xiaosi, YANG Miao, TIAN Peng, LIU Zhongmin
2024, 40(6): 1171-1178. doi:
10.1007/s40242-024-4056-y
Abstract
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Conversion of industrial solid wastes into functional materials has attracted considerable interest, as it can reduce environmental pollution and facilitate the sustainable development of relevant processes. Herein, spent methanol-to-olefins (MTO) industrial catalyst was explored for the synthesis of DNL-6 molecular sieve, a promising SAPO-type adsorbent for CO
2
capture. It was demonstrated that DNL-6 with high purity and crystallinity, and various silica contents can be readily synthesized. Na-exchanged DNL-6 was further prepared using the as-synthesized DNL-6 as the precursor, and its structure was investigated by Rietveld refinement, revealing that Na cations were mainly located in the single 8-rings (S8Rs). Na-DNL-6 with varied silica contents and Na contents were investigated for adsorption studies. Na-DNL-6 with a high Na exchange degree exhibited comparable CO
2
uptake with H-DNL-6 (298 K and 101 kPa), but superior separation selectivity for CO
2
/CH
4
(as high as 1369, 50/50 kPa) and CO
2
/N
2
(∞, 15/85 kPa) owing to the “trapdoor” effect associated with the Na cations sited in the S8Rs. This work provides an eco-friendly approach for the synthesis of efficient silicoaluminophosphate adsorbent for CO
2
capture.
Gas-Liquid Interfacial Deposition Synthesis of Alumina with Large Mesopores
ZHANG Yu, LI Wen-Cui, ZHENG Yuenan, WANG Haowei, WU Fan, ZHANG Wenrui, LU An-Hui
2024, 40(6): 1179-1191. doi:
10.1007/s40242-024-4069-6
Abstract
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)
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The porous structure of alumina is influenced by various factors during the synthesis process. In this study, we proposed a gas-liquid interfacial deposition method, different from conventional liquid-phase reactions, which effectively slows down the precipitation rate, facilitating the investigation of the pore structure and morphology changes of alumina during the synthesis process. Ammonia (NH
3
) and carbon dioxide (CO
2
) generated by the decomposition of inorganic ammonium salts constitute the gas phase, while the aqueous solution of the inorganic aluminum salt serves as the liquid phase. The gas diffuses, contacts, dissolves and reacts with the inorganic aluminum salt solution, constructing a platform for gas-liquid interfacial deposition at the gas-liquid interface. We precisely regulated the critical factors that affected the precipitation rate during the reaction process, such as gas-liquid reaction methods, precipitant types, aluminum salt types, and reaction temperatures, leading to systematic changes in the pore structures of the obtained alumina. After considering the influence of precipitation rate, pH value, and anion types, we found that the fundamental factor affecting pore structure lies in the water content of the precursors. By controlling the phase and crystallinity of the precursors, alumina with a large mesopore size distribution concentrated at 25.3 nm can be obtained.
Synthesis of LSX Using Seed-iteration Approach with High N
2
Adsorption Capacity for Air Separation
HUANG Yitong, WANG Yaquan, LIU Wenrong, BU Lingzhen, QU Liping, CHU Kailiang, GUO Niandong, ZHANG Xian, SU Xuemei, LI Yaoning, SANG Juncai
2024, 40(6): 1192-1200. doi:
10.1007/s40242-024-4073-x
Abstract
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)
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A series of low silica X zeolites (LSX) was synthesized through a seed-iteration approach, based on the seed addition strategy, and then loaded with lithium ions by an ion exchanging method to obtain high N
2
adsorption capacity. These zeolites were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectra (FTIR), thermogravimetric analysis (TGA) and N
2
adsorption-desorption, and the adsorption capacity of N
2
and O
2
was evaluated by the vacuum pressure swing adsorption (VPSA) operation. The results showed that the nucleation period of the synthetic process could be effectively shortened by adding seed; as the seed iterations increased, the specific surface area and pore volume of the zeolites increased; the higher specific surface area and the pore volume, the higher the extent of the N
2
adsorption capacity, with the maximum reaching 28.05 cm
3
/g. However, there were no significant differences in the adsorbed capacity of O
2
by each sample. Therefore, the N
2
/O
2
separation factor also increased gradually with iterations, with the maximum up to 6.61.
Molecular Mechanism of Action of GPR91 Agonists and Antagonists: Insights from Molecular Dynamics Simulation
ZHANG Junjie, LV Lunan, ZHU Haoran, ZHANG Ying, XU Xiaodi, LONG Lanxin, FU Wei
2024, 40(6): 1201-1211. doi:
10.1007/s40242-024-4075-8
Abstract
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)
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G protein-coupled receptor 91 (GPR91) has garnered widespread attention as a prospective therapeutic target for metabolic diseases. However, no structural data for human GPR91 (hGPR91) and detailed molecular mechanism of action (MOA) of GPR91 have been reported, with reported compounds targeting GPR91 limited. In this study, hGPR91 structures were constructed through homology modeling. High-affinity agonist compound
31
and antagonist NF-58-EJ40 were selected for investigation. By molecular dynamics (MD) simulations, we have elucidated MOA of GPR91 agonists and antagonists for the first time. We identified the crucial role of the D174FASSG sequence, the L65
2.46
SVSD
2.50
sequence and the N64
2.45
-W147
4.50
in maintaining GPR91’s inactive state conformation. Agonist binding disrupted constraints mediated by the aforementioned sequence, which led to significant outward movements of transmembrane helixes (TMs) and repositioning of intracellular loop2 (ICL2) and ICL3, thereby forming an expanded cavity for G proteins binding. Furthermore, the pivotal role of the dicarboxylic acid structure of agonists in initiating signal transduction was confirmed. In contrast, antagonist binding stabilized these conformational constraints, resulting in relatively minor movements of TMs that were insufficient to generate a binding cavity large enough to accommodate the G protein. Clarifying MOA of GPR91 agonists and antagonists is crucial for guiding the design of relevant drugs.
Rapid Access to Acylation and Alkylation of
N
-Heteroarenes Using Ester Acetates as Reactants
XU Jianxiong, HUANG Weimin, LI Jizhen
2024, 40(6): 1212-1219. doi:
10.1007/s40242-024-4078-5
Abstract
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)
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The laboratory-abundant and low-toxic ethyl acetate was explored successfully for the first time as acyl group donor for the Minisci-type acylation of quinolines. In this approach, TBAC/K
2
S
2
O
8
(TBAC:
tert
-butylacetyl chloride) system played a important role, and the introduced acyl group was derived from the alkoxyl group moiety of ester acetates. Most
N
-heteroarenes, such as quinoxaline and isoquinoline, etc. were also compatible to this synthetic strategy affording acylated products in high yields. Simultaneously, the C2—H alkylation was realized by accident for 4-quinazolinone. Furthermore, the acylation mechanism was proposed through the chlorine radical abstracting the inactive α-hydrogen of the alkoxyl group.
Synthesis of Anisotropic Silica Nanoparticles
WEI Lili, FAN Yuanqing, LIN Haifeng, CHE Shunai
2024, 40(6): 1220-1226. doi:
10.1007/s40242-024-4092-7
Abstract
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)
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Anisotropic silica nanoparticles (AISNPs) are appealing for various applications due to their greater effective surface area and increased active sites compared to isotropic silica nanoparticles (ISNPs). Herein, we employed a sol-gel method to synthesize AISNPs utilizing the mixture of ethylenediamine (EDA) and 1,3-diaminopropane (1,3-DAP) as both structure-directing agents and catalysts. With increasing EDA:1,3-DAP molar ratio, the samples transitioned from isotropic spherical particles to anisotropic particles with increasing sizes. The synthesis of AISNP with a particle size of ca. 40 nm, average circularity (
e
) of 0.83, fitting ellipse aspect ratio (ar) of 1.18 and percentage of deformed particles of 83.3% was achieved with a molar ratio of EDA:1,3-DAP=7:3. It is speculated that the close proximity of EDA's amine groups facilitates their adsorption on the same primary particle through electrostatic interaction, inhibiting primary particle connections and resulting in spherical seeds that grow into small isotropic particles; the long-distance amine groups of 1,3-DAP connect adjacent particles anisotropically due to the steric hindrance, leading to large anisotropic particles; the mixtures with different EDA/1,3-DAP molar ratios result in different morphologies and sizes by their cooperative effect.
An Electropolymerization (EP)-based Fluorescent Film Probe to Fe
3+
Using Conjugated Polymer as Precursor
TAN Wenjia, MIAO Xin, LI Yan, ZHANG Ming
2024, 40(6): 1227-1232. doi:
10.1007/s40242-024-4093-6
Abstract
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)
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A conjugated polymer
P-M2
with carbazole units as impendent sidechains is used as the electropolymerization (EP) precursor to prepare EP film and realize the coupling reaction between conjugated polymers. Further, the EP film is used as the fluorescent film probe to Fe
3+
, whose limit of detection (LOD) is calculated to be 1.4×10
-7
mol/L. Compared with that of the EP film prepared by small molecule precursor
M2
, the LOD is enhanced ten times. The results are due to both the long conjugation length of
P-M2
and the inherent highly cross-linking network microstructures of
P-M2
EP film. Hereby, this work realizes not only the reaction between conjugated polymers but also a new precursor for the EP method and a promising fluorescent film sensor candidate.
Achieving Enhanced Fire Safety of Polyvinyl Chloride Through Rapid Catalytic Carbonization Using a Triple-effect Flame Retardant of Mg(OH)
2
-ZnO-TiO
2
CAO Heming, SHI Shunli, PENG Hesong, HU Jie, LIAO Sheng, WANG Shuhua, CHEN Chao
2024, 40(6): 1233-1244. doi:
10.1007/s40242-024-4098-1
Abstract
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)
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The concept of catalytic flame retardancy by metal ions is considered an efficient flame-retardant method. However, due to the unclear mechanism, the ambiguity of the reaction process and the unknown properties of the products severely limit its application in composite materials. In view of this, we designed a tri-effect composite flame retardant of Mg(OH)
2
-ZnO-TiO
2
, which not only solves the problem of low flame retardancy efficiency of magnesium hydroxide (MH) but also performs excellently in the evaluation of flame retardancy of polyvinyl chloride (PVC). The limit oxygen index (LOI) increased from 21.5% to 31.1%, and the composite material can be synthesized on a large scale. Through detailed analysis of the condensed phase carbon layer, two different catalytic flame retardant mechanisms were elucidated. This research is expected to provide an important theoretical basis for the development of efficient and environmentally friendly composite flame retardants.
Rapid Synthesis of Boron-MWW Zeolite Through a Solvent-free Strategy
BO Shuang, WANG Tianlong, LV Tianming, WU Huifang, FENG Ziyi, MIAO Lei, FENG Zhaochi, REN Limin, MENG Changgong
2024, 40(6): 1245-1255. doi:
10.1007/s40242-024-4099-0
Abstract
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)
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ERB-1 zeolite emerges as a key bridging material for crafting heteroatom-containing MWW for versatile catalytic applications. In this study, we developed a solvent-free strategy facilitated by high-temperature condition and seed assistance, streamlining the synthesis of ERB-1 zeolite. This novel approach not only significantly reduces the growth time to 12 h compared to the conventional 168-h hydrothermal synthesis but also enhances product yield while minimizing waste generation. Benefiting from the platelet seeds and the grinding force, a distinct non-classical growth pathway, involving nanoparticle attachment, epitaxial growth, anisotropic assembly, and crystallization, was observed in the solvent-free synthesis. Through heteroatom substitution, pillared Sn-MWW was successfully prepared, exhibiting remarkable stability and catalytic performance in the Bayer-Villiger oxidation reaction of 2-adamantanone. Our findings present a simple and cost-effective way for rapid synthesis of MWW zeolite, with implications extending to diverse catalytic applications.
Study on Derivatization and Biological Activity of Natural Product Daidzein
LUO Zeping, PAN Liwei
2024, 40(6): 1256-1265. doi:
10.1007/s40242-024-4102-9
Abstract
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)
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A new class of Daidzein derivatives were developed, and their protective effects on neuronal cells and their mechanisms were examined. The protective effects of Daidzein derivatives against oxygen and glucose deprivation/reoxygenation (OGD/R) injury in HT22 cells were evaluated
via
a Cell Counting Kit 8 (CCK-8) assay. Biomarkers associated with ferroptosis, including changes in reactive oxygen species (ROS), lipid peroxidation, ferrous ion (Fe
2+
), glutathione (GSH), superoxide dismutase (SOD) and malondialdehyde (MDA) levels, were detected
via
fluorescent probes and specific kits. In addition, the protein expression levels of glutathione peroxidase 4 (GPX4), recombinant solute carrier family 7, member 11 (SLC7A11 or xCT) and nuclear Factor 2 (Nrf2) were analyzed
via
Western blotting. The newly synthesized Daidzein derivative outperforms not only its parent compound, especially derivative 3, in improving the viability of OGD/R-treated HT22 cells but also edaravone, a positive control drug. This study further revealed the mechanism of action of derivative 3: reducing the level of ROS and lipid peroxidation induced by OGD/R in HT22 cells, restoring SOD and GSH activities, reducing MDA and Fe
2+
accumulation, and increasing the protein expression of GPX4, xCT and Nrf2. Derivative 3 has significant neuroprotective effects, and its mechanism may involve activating the Nrf2/xCT/GPX4 pathway and inhibiting neuronal ferroptosis. This study provides a new perspective for neuroprotection research and a direction for drug development.
Dithieno[3,2-
c
: 3',2'-
h
][2,6]naphthyridine-4,9(5
H
,10
H
)-dione-based Quinoidal Small Molecules: Synthesis, Properties, and Optoelectronic Applications
SU Yunran, ZHAO Lingxu, ZHANG Shengnan, CHEN Jiawei, LI Yanru, JIANG Ting, LI Jie, JI Deyang, LI Liqiang, FEI Zhuping
2024, 40(6): 1266-1274. doi:
10.1007/s40242-024-4106-5
Abstract
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)
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Amide and imide groups have been widely used in the design of organic semiconductors, and the development of new structure semiconductors based on these functional groups is of great interest to further improve the performance of organic electronic devices. Herein, we designed and synthesized two novel 5,10-dihydrodithieno[3,2-
c
:3',2'-
h
][2,6]naphthyridine-4,9-dione (TVTDA) based quinoidal molecules with different side chains, TVTDA-CN-EH and TVTDA-CN-OD. Both molecules showed the deep lowest unoccupied molecular orbital (LUMO) and the deep highest occupied molecular orbital (HOMO) energy levels and strong absorption in the long wavelength region. Organic field-effect transistors (OFETs) based on TVTDA-CN-EH and TVTDA-CN-OD exhibited unipolar n-type electron transport behavior with mobilities of 0.04 and 0.0064 cm
2
·V
-1
·s
-1
, respectively. TVTDA-CN-EH with shorter alkyl side chains demonstrated better electron transport properties, which is attributed to the larger grain size in the film to facilitate charge transport. Furthermore, organic phototransistors (OPTs) based on TVTDA-CN-EH film showed good photo detection property from red light to near infrared region. Our work provides a new idea for the design and synthesis of organic semiconductors, especially for n-type organic semiconductors with photoresponse in the long wavelength.
Granular Ln-MOF@Activated Carbon Composite for Highly Selective and Sensitive Detection of Cr
3+
Cations
LIU Yuebin, YU Jingran, ZHANG Zhiyu, FENG Jinhua, LIN Weihai, XUE Ming
2024, 40(6): 1275-1281. doi:
10.1007/s40242-024-4107-4
Abstract
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)
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Lanthanide metal-organic frameworks (MOFs) have received special attention due to their unusual coordination characteristics and exceptional luminescence properties, while their development has extremely limited by the cost effective and powder form. Herein, a gentle and facile strategy was developed to create a granular lanthanide MOFs@activated carbon (AC) composite. The obtained granular Tb-BTC@AC composite displays high fluorescent selectivity and sensitivity towards Cr
3+
cations in water with quenching efficiency up to 90.12%, and shows great sensitivity in the range of 10
-5
—10
-4
mol/L with the Stern-Volmer constant of 2.224×10
3
L/mol. Benefited by the high surface area, the abundant self-assembly space was provided for the self-assembling of the Lanthanide MOFs, which leads to promising Cr
3+
cation-recognition ability with low MOF quantity. Also, the large size (with an average diameter of 2 mm) and shaped form of this new composite material reduced the threshold of MOF application.
Investigation of a Novel Atmospheric Pressure Microwave Cold Plasma Torch and Its Characteristics
LI Yarui, BAI Yiwen, YU Dengjie, WANG Rongyao, MU Ying, JIN Wei, YU Bingwen
2024, 40(6): 1282-1289. doi:
10.1007/s40242-024-4112-7
Abstract
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)
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This study proposes a coaxial structure atmospheric pressure microwave cold plasma device that utilizes argon as the main working gas. It achieves stable formation of atmospheric pressure cold plasma jet at low power (<50 W) with a jet length ranging from
1
mm to 32 mm. The paper analyzes the composition of the cold plasma using spectroscopy and investigates its composition changes at different positions along the jet. It also studies the appearance and reaction composition of the plasma filament under different shielding gases. Furthermore, it explores the effects of continuous and modulated microwave power on the length, appearance, and composition of the plasma filament. Finally, it examines the bactericidal effect of the plasma filament on
Escherichia coli
under various gas conditions, providing a foundation for further application research.
Construction of Photo- and Thermo-Responsive Polymer-MOF@Enzyme Composites for Enhancing Its Biocatalytic Performance
TAJWAR Muhammad Ali, ALI Nasir, ZHANG Xiangru, JABEEN Rubina, LIU Yutong, SHANGGUAN Dihua, QI Li
2024, 40(6): 1290-1297. doi:
10.1007/s40242-024-4140-3
Abstract
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)
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Recently, metal-organic framework (MOF)@enzyme composites have attracted increasing research interest. However, the fabrication of polymers-modified MOF@enzyme composites with high bio-catalytic performance remains challenging. Herein, a stimulus-responsive polymer, poly(acrylate-3',3'-dimethyl-6-nitro-spiro-2
H
-1-benzopyran-2,2' indoline-1'-ester-co-
N
-isopropyl acrylamide) (PSPN), was
in-situ
polymerized in UiO-66-NH
2
(UN). The dual-responsive PSPN-UN@
L
-ASNase composites were constructed following
L
-asparaginase (
L
-ASNase) covalently attached to the UN surface. Interestingly, under 365 nm UV irradiation at 45 ℃, the PSP moiety in PSPN underwent a
trans-to-cis
conformational change and the PN moiety in PSPN transferred from a stretched- to a coiled-state, generating a confinement effect that significantly enhanced the bio-catalytic performance of the composites. Compared with free
L
-ASNase, the composites showed a 42.0-folds increase in maximum catalytic reaction velocity. Furthermore, the PSPN-UN@
L
-ASNase composites demonstrated high toxicity for Jurkat leukaemia cells. The stimulus-responsive polymer-MOF@enzyme composites provide a novel avenue for controlled bio-catalysis with great potential for targeted leukaemia therapy.
In silico
Exploration of Inhibition Mechanism of Lianhua Qingwen Formula (LQF) Interaction on SARS-CoV-2 Mpro
XUE Xiaolong, WANG Xin, YE Chenghao, GAO Meina, LI Peng, YU Kunqian, CHEN Guanghui
2024, 40(6): 1298-1310. doi:
10.1007/s40242-024-4150-1
Abstract
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)
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It is well known that the severe epidemic respiratory disease COVID-19 was caused by the novel coronavirus SARS-CoV-2. Lianhua Qingwen Formula (LQF), as a traditional Chinese medicine (TCM) formula, exerts anti-coronavirus activity by suppressing viral replication and activating anti-inflammatory effects. In this work, the unknown molecular inhibition mechanism of LQF ingredients on the main protease (Mpro) of SARS-CoV-2 was investigated. From the screening of pharmacophore model, docking, molecular dynamics (MD) simulations and molecular mechanics Poisson-Boltzmann surface area (MM/PBSA) calculations, it is found that Isoliquiritin apioside, Liquiritin apioside, Forsythoside E, Rutin, and Isoliquiritin possess much larger binding free energies than reference X77. These five hit molecules are characterized by multi-hydroxyl groups, which facilitate the formation of hydrogen bonds with polar amino acid residues at S1' subsite and rationalize their primary binding to Mpro with electrostatic rather than usual van der Waals (vdW) interaction. In addition, the Isoliquiritin apioside, Liquiritin apioside, and Rutin were also identified as potential inhibitors on SARS-CoV Mpro, possessing much larger binding free energies with large electrostatic interaction than that of reference ENB. The present study can not only enrich the scaffolds of Mpro of SARS-CoV family inhibitors, but also provide an idea for the new drug development.
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