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2021 Volume 84 Issue 1
2021, 84(1): 2-9, 30
Abstract:
Traditional supported metal catalysts are prone to sintering under high temperature environments or after long hours of work. This irreversible process will result in a significant reduction of the active sites of the catalysts, which will cause the catalysts to be severely deactivated. Therefore, it is often necessary to update the catalysts in time to meet the needs of industrial production, but this will greatly increase production costs. Unlike traditional supported metal catalysts, the central metal atom of single-atom catalysts (SACs) can form strong bonds with heteroatoms (N, O, S, etc.), thereby effectively inhibiting metal sintering. Based on the characteristics of single-atom catalysts, we can prepare ultra-stable single-atom catalysts that are resistant to sintering and high temperature to deal with special industrial catalytic environments. This paper summarizes the progress in the synthesis and application of anti-sintering ultra-stable single-atom catalysts in recent years, and provides references for the research in the field of single-atom catalysis.
Traditional supported metal catalysts are prone to sintering under high temperature environments or after long hours of work. This irreversible process will result in a significant reduction of the active sites of the catalysts, which will cause the catalysts to be severely deactivated. Therefore, it is often necessary to update the catalysts in time to meet the needs of industrial production, but this will greatly increase production costs. Unlike traditional supported metal catalysts, the central metal atom of single-atom catalysts (SACs) can form strong bonds with heteroatoms (N, O, S, etc.), thereby effectively inhibiting metal sintering. Based on the characteristics of single-atom catalysts, we can prepare ultra-stable single-atom catalysts that are resistant to sintering and high temperature to deal with special industrial catalytic environments. This paper summarizes the progress in the synthesis and application of anti-sintering ultra-stable single-atom catalysts in recent years, and provides references for the research in the field of single-atom catalysis.
2021, 84(1): 10-15
Abstract:
The facile conversion of H2O or CO2 into chemical fuels (such as H2, CO) via semiconductor quantum dots (QDs) artificial photosynthesis is considered as an effective way to solve the energy and environmental crisis. Due to the unique photophysical and photochemical properties (e.g., excellent light absorption capacity, adjustable energy band structure, multi-exciton generation, abundant surface active sites, etc.), QDs have received much attention in the field of artificial photosynthesis in recent years. Here, we summarize our recent advances in chemical conversions via artificial photosynthesis using semiconductor QDs, and also provide prospects of future studies.
The facile conversion of H2O or CO2 into chemical fuels (such as H2, CO) via semiconductor quantum dots (QDs) artificial photosynthesis is considered as an effective way to solve the energy and environmental crisis. Due to the unique photophysical and photochemical properties (e.g., excellent light absorption capacity, adjustable energy band structure, multi-exciton generation, abundant surface active sites, etc.), QDs have received much attention in the field of artificial photosynthesis in recent years. Here, we summarize our recent advances in chemical conversions via artificial photosynthesis using semiconductor QDs, and also provide prospects of future studies.
2021, 84(1): 16-20
Abstract:
Reactive oxygen species (ROS) play vital roles in photocatalytic selective oxidation reactions. Researchers fabricate variety of materials to optimize their ROS generation, which enhances the efficiency of corresponding photocatalytic reactions and facilitates the future green industrialization process. This review summarizes common ROS generation along with their photocatalytic mechanisms, and the testing methods of different ROS are also introduced. This paper provides new thoughts for optimizing photocatalytic reactions.
Reactive oxygen species (ROS) play vital roles in photocatalytic selective oxidation reactions. Researchers fabricate variety of materials to optimize their ROS generation, which enhances the efficiency of corresponding photocatalytic reactions and facilitates the future green industrialization process. This review summarizes common ROS generation along with their photocatalytic mechanisms, and the testing methods of different ROS are also introduced. This paper provides new thoughts for optimizing photocatalytic reactions.
2021, 84(1): 21-30
Abstract:
Methanol is considered as an excellent hydrogen carrier (the gravimetric hydrogen density over 12.5%). The "methanol-hydrogen" energy system has been proposed in aiming at solving the H2 transportation and storage problem, one of the major bottleneck problems in hydrogen application, and promoting the utilization of hydrogen energy in large scale. How to generate hydrogen from methanol efficiently and selectively has been one of the vital components in the methanol-H2 system. In this review, the recent progresses and challenges in the catalysis for hydrogen production from methanol are introduced in detail. We discuss the advantages and economic rationality of storing and releasing hydrogen into/from methanol. The methods of catalytic hydrogen evolution from methanol along with the structure and mechanism of representative hydrogen production catalysts are also reviewed in details. We anticipate this perspective to provide references for the catalytic studies of methanol-H2 energy system and promote the development of suitable catalysts for the potential large scale H2 production in the near future.
Methanol is considered as an excellent hydrogen carrier (the gravimetric hydrogen density over 12.5%). The "methanol-hydrogen" energy system has been proposed in aiming at solving the H2 transportation and storage problem, one of the major bottleneck problems in hydrogen application, and promoting the utilization of hydrogen energy in large scale. How to generate hydrogen from methanol efficiently and selectively has been one of the vital components in the methanol-H2 system. In this review, the recent progresses and challenges in the catalysis for hydrogen production from methanol are introduced in detail. We discuss the advantages and economic rationality of storing and releasing hydrogen into/from methanol. The methods of catalytic hydrogen evolution from methanol along with the structure and mechanism of representative hydrogen production catalysts are also reviewed in details. We anticipate this perspective to provide references for the catalytic studies of methanol-H2 energy system and promote the development of suitable catalysts for the potential large scale H2 production in the near future.
2021, 84(1): 31-39
Abstract:
Suzuki cross-coupling reaction has been widely recognized as one of the most effective methods for the construction of C-C bonds and plays an important role in medicine, dye and electronics industry. In recent years, with the rapid development of photocatalytic technology and green organic synthetic chemistry, the use of renewable solar photocatalytic Suzuki cross-coupling reaction can not only solve energy and environmental problems, but also can obtain high yield of biphenyl compound at room temperature, so it has attracted the widespread attention of scientists. Compared with the homogeneous photocatalyst, the heterogeneous photocatalyst with advantages of good chemical stability and convenient recovery and recycling has become the key research object of photocatalytic Suzuki cross-coupling reaction. In this review, the basic principle of Suzuki cross-coupling reaction photocatalyzed by heterogeneous catalyst is summarized, and a series of researches on the preparation method, catalytic performance and recyclability of heterogeneous catalyst in photocatalytic Suzuki cross-coupling reaction are introduced.
Suzuki cross-coupling reaction has been widely recognized as one of the most effective methods for the construction of C-C bonds and plays an important role in medicine, dye and electronics industry. In recent years, with the rapid development of photocatalytic technology and green organic synthetic chemistry, the use of renewable solar photocatalytic Suzuki cross-coupling reaction can not only solve energy and environmental problems, but also can obtain high yield of biphenyl compound at room temperature, so it has attracted the widespread attention of scientists. Compared with the homogeneous photocatalyst, the heterogeneous photocatalyst with advantages of good chemical stability and convenient recovery and recycling has become the key research object of photocatalytic Suzuki cross-coupling reaction. In this review, the basic principle of Suzuki cross-coupling reaction photocatalyzed by heterogeneous catalyst is summarized, and a series of researches on the preparation method, catalytic performance and recyclability of heterogeneous catalyst in photocatalytic Suzuki cross-coupling reaction are introduced.
2021, 84(1): 40-46
Abstract:
Aptamers are short oligonucleotide molecules (ssDNA or RNA) screened from in vitro synthesized oligonucleotide libraries by exponential enrichment ligand phylogenetic technique (SELEX). Aptamers can bind to target molecules specifically by folding into specific spatial structures. Compared with antibodies, aptamers have a great deal of advantages, such as high affinity, easy modification, low cost, easy synthesis and low immunogenicity, which can be used for the research of cancer biomarkers, such as cells, proteins, tissues and growth factors. As a new method for cancer diagnosis, they have broad application prospects in molecular diagnosis. In this paper, the application of aptamers in the diagnosis of lung cancer, gastric cancer, colorectal cancer, breast cancer and prostate cancer in recent years is reviewed, and the role of aptamers as molecular probes from cell detection to serum detection is clarified.
Aptamers are short oligonucleotide molecules (ssDNA or RNA) screened from in vitro synthesized oligonucleotide libraries by exponential enrichment ligand phylogenetic technique (SELEX). Aptamers can bind to target molecules specifically by folding into specific spatial structures. Compared with antibodies, aptamers have a great deal of advantages, such as high affinity, easy modification, low cost, easy synthesis and low immunogenicity, which can be used for the research of cancer biomarkers, such as cells, proteins, tissues and growth factors. As a new method for cancer diagnosis, they have broad application prospects in molecular diagnosis. In this paper, the application of aptamers in the diagnosis of lung cancer, gastric cancer, colorectal cancer, breast cancer and prostate cancer in recent years is reviewed, and the role of aptamers as molecular probes from cell detection to serum detection is clarified.
2021, 84(1): 47-52
Abstract:
Indole is a compound widely found in nature, having a variety of biological activities like antitumor, antioxidant and antibacterial. The introduction of different substituents at the 3-position on the indole ring for structural modification and transformation has always been a drug research hotspot. In this article the related literature in recent years were summarized, and the antitumor activities of 3-substitution indole derivatives with the different heterocycle substituents such as pyrazoles and pyrazolines, diazoles and triazoles, cyclization with 2-position were reviewed in order to provide a theoretical basis for the development of highly active antitumor drugs.
Indole is a compound widely found in nature, having a variety of biological activities like antitumor, antioxidant and antibacterial. The introduction of different substituents at the 3-position on the indole ring for structural modification and transformation has always been a drug research hotspot. In this article the related literature in recent years were summarized, and the antitumor activities of 3-substitution indole derivatives with the different heterocycle substituents such as pyrazoles and pyrazolines, diazoles and triazoles, cyclization with 2-position were reviewed in order to provide a theoretical basis for the development of highly active antitumor drugs.
2021, 84(1): 53-57
Abstract:
The display technology based on high color purity light sources has the characteristics of wide achievable color gamut, good color saturation and high contrast ratio, which can bring people better visual experience. In recent years, the development of narrow bandwidth light sources is receiving more and more attentions. Here, three typical light-emitting polymers were selected to construct polymer light-emitting electrochemical cells (PLEC), and a distributed Bragg reflector (DBR) and Al thin film were used as cavities to narrow the emission spectra. The results showed that the bandwidth of the emitted light from the red, green and blue PLECs dramatically narrowed down to 10, 11 and 8 nm, respectively, and the color purity has been greatly improved. The acquisition of such high color purity light sources is expected to significantly promote the development of next-generation display technology.
The display technology based on high color purity light sources has the characteristics of wide achievable color gamut, good color saturation and high contrast ratio, which can bring people better visual experience. In recent years, the development of narrow bandwidth light sources is receiving more and more attentions. Here, three typical light-emitting polymers were selected to construct polymer light-emitting electrochemical cells (PLEC), and a distributed Bragg reflector (DBR) and Al thin film were used as cavities to narrow the emission spectra. The results showed that the bandwidth of the emitted light from the red, green and blue PLECs dramatically narrowed down to 10, 11 and 8 nm, respectively, and the color purity has been greatly improved. The acquisition of such high color purity light sources is expected to significantly promote the development of next-generation display technology.
2021, 84(1): 58-62
Abstract:
This paper introduces a simple method to synthesize[Cu2(bipy)2(H2P2O7)(OH)2]·7H2O binuclear copper water cluster complex. The crystal structure analysis indicated that seven crystal waters form a two-dimensional water cluster polymer[(H2O)7]n, and the water cluster then forms a strong hydrogen bond with the hydroxyl group in the core structure. The structure of the whole complex resembles a dragonfly. Through the research of this kind of water cluster polymer, it is helpful for improving the modelling of some of the unexplained properties of water and better understanding the structure and behaviour of water molecules in chemical and biological process.
This paper introduces a simple method to synthesize[Cu2(bipy)2(H2P2O7)(OH)2]·7H2O binuclear copper water cluster complex. The crystal structure analysis indicated that seven crystal waters form a two-dimensional water cluster polymer[(H2O)7]n, and the water cluster then forms a strong hydrogen bond with the hydroxyl group in the core structure. The structure of the whole complex resembles a dragonfly. Through the research of this kind of water cluster polymer, it is helpful for improving the modelling of some of the unexplained properties of water and better understanding the structure and behaviour of water molecules in chemical and biological process.
2021, 84(1): 63-68
Abstract:
Naphthalene diimide (NDI) compounds are widely used in organic field effect transistors (OFETs) and organic solar cells (OSCs) due to their good planarity and strong ability to accept electrons. However, there are fewer high-mobility n-type and bipolar NDI-based semiconductor materials. Based on this, we design and synthesize two NDI derivative containing selenium heterocycle. By introducing 1, 2-diselenobenzene and 1, 2-diselonaphthalene groups, the energy level is effectively regulated and two narrow band gap naphthalene diimide derivatives are obtained. Through solution spin coating method, the field effect transistor devices with bottom gate and bottom contact of two materials are prepared. Both of them show n-type semiconductor characteristics in air, and their electron mobilities reach 1×10-3cm2·V-1·s-1 (4) and 5×10-3cm2·V-1·s-1 (5) respeetively when annealed at 120℃. At the same time, the annealing process of the film has been studied by atomic force microscope and X-ray diffraction.
Naphthalene diimide (NDI) compounds are widely used in organic field effect transistors (OFETs) and organic solar cells (OSCs) due to their good planarity and strong ability to accept electrons. However, there are fewer high-mobility n-type and bipolar NDI-based semiconductor materials. Based on this, we design and synthesize two NDI derivative containing selenium heterocycle. By introducing 1, 2-diselenobenzene and 1, 2-diselonaphthalene groups, the energy level is effectively regulated and two narrow band gap naphthalene diimide derivatives are obtained. Through solution spin coating method, the field effect transistor devices with bottom gate and bottom contact of two materials are prepared. Both of them show n-type semiconductor characteristics in air, and their electron mobilities reach 1×10-3cm2·V-1·s-1 (4) and 5×10-3cm2·V-1·s-1 (5) respeetively when annealed at 120℃. At the same time, the annealing process of the film has been studied by atomic force microscope and X-ray diffraction.
2021, 84(1): 69-74, 95
Abstract:
Silicon carbide quantum dots (QDs) were prepared by a controllable chemical etching method. The original SiC powders synthesized by self propagating high temperature synthesis (SHS) were corroded by a mixture of hydrofluoric acid and nitric acid. Then, the aqueous phase SiC QDs were obtained by ultrasonic cavitation and high-speed centrifugal chromatography. The effects of preparation parameters on the photoluminescence intensity, emission wavelength spectra and particle size of QDs were studied. The results showed that the composition and ratio of the etchant are the main factors affecting the photoluminescence intensity of QDs, while the ultrasonic vibration time and the centrifugal high gravity coefficient of the chromatographic clipping have an effect on the photoluminescence intensity to a certain extent. The main factors affecting the optical properties of the two factors are the shift of the characteristic emission wavelength, the half peak width, the size of the quantum dots and the particle size distribution uniformity. In addition, in the process of adjusting the composition of the etchant, it is found that replacing part of nitric acid in the original etchant with an appropriate amount of analytically pure sulfuric acid will not only change the photoluminescence intensity of QDs, but also coupled with new functional groups sulfhydryl except carboxyl and hydroxyl groups on the surface.
Silicon carbide quantum dots (QDs) were prepared by a controllable chemical etching method. The original SiC powders synthesized by self propagating high temperature synthesis (SHS) were corroded by a mixture of hydrofluoric acid and nitric acid. Then, the aqueous phase SiC QDs were obtained by ultrasonic cavitation and high-speed centrifugal chromatography. The effects of preparation parameters on the photoluminescence intensity, emission wavelength spectra and particle size of QDs were studied. The results showed that the composition and ratio of the etchant are the main factors affecting the photoluminescence intensity of QDs, while the ultrasonic vibration time and the centrifugal high gravity coefficient of the chromatographic clipping have an effect on the photoluminescence intensity to a certain extent. The main factors affecting the optical properties of the two factors are the shift of the characteristic emission wavelength, the half peak width, the size of the quantum dots and the particle size distribution uniformity. In addition, in the process of adjusting the composition of the etchant, it is found that replacing part of nitric acid in the original etchant with an appropriate amount of analytically pure sulfuric acid will not only change the photoluminescence intensity of QDs, but also coupled with new functional groups sulfhydryl except carboxyl and hydroxyl groups on the surface.
2021, 84(1): 75-80
Abstract:
La-MOFs adsorbents were fabricated by hydrothermal method, and the structure and morphology of prepared La-MOFs adsorbents were analyzed by scanning electron microscope, fourier transform infrared spectroscopy, X-ray powder diffraction and N2 adsorption-desorption isotherms. The La-MOFs adsorbents were woolen spherical structure with the most pore size of 15.84 nm and specific surface area of 16.95 m2/g and lanthanum fluoride crystals were formed after adsorption of fluoride ions. The effects of parameters, such as mass ratio of lanthanum nitrate and 2-aminoterephthalic acid, reaction temperature and time, etc. on fluoride adsorption by the La-MOFs adsorbents were investigated. When LN/AA=4:3, DMF reaction temperature 130℃, reaction time 24 h and methanol reaction temperature 120℃, the adsorption capacity of La-MOFs reaches the maximum value of 43.1 mg/g. The pseudo-second-order has been found suitable for describing the kinetics process of the fluoride ions absorption on the La-MOFs adsorbent while the net rate can thus be sequentially controlled in a multi-stage condition. The fitness of adsorption data by Freundlich model was superior to Langmuir model. The adsorption process is an exothermic reaction, and increasing the temperature is beneficial to the adsorption process.
La-MOFs adsorbents were fabricated by hydrothermal method, and the structure and morphology of prepared La-MOFs adsorbents were analyzed by scanning electron microscope, fourier transform infrared spectroscopy, X-ray powder diffraction and N2 adsorption-desorption isotherms. The La-MOFs adsorbents were woolen spherical structure with the most pore size of 15.84 nm and specific surface area of 16.95 m2/g and lanthanum fluoride crystals were formed after adsorption of fluoride ions. The effects of parameters, such as mass ratio of lanthanum nitrate and 2-aminoterephthalic acid, reaction temperature and time, etc. on fluoride adsorption by the La-MOFs adsorbents were investigated. When LN/AA=4:3, DMF reaction temperature 130℃, reaction time 24 h and methanol reaction temperature 120℃, the adsorption capacity of La-MOFs reaches the maximum value of 43.1 mg/g. The pseudo-second-order has been found suitable for describing the kinetics process of the fluoride ions absorption on the La-MOFs adsorbent while the net rate can thus be sequentially controlled in a multi-stage condition. The fitness of adsorption data by Freundlich model was superior to Langmuir model. The adsorption process is an exothermic reaction, and increasing the temperature is beneficial to the adsorption process.
2021, 84(1): 81-89
Abstract:
Quinoline hydrazone and quinoline acylhydrazone compounds had been found to have a wide range of biological activities. In this paper, 29 unreported 4-(2-aryl) quinoline arylhydrazone and aroylhydrazone compounds were designed and synthesized, and the inhibitory effects of these compounds on protein tyrosine phosphatase (PTP 1B) were tested by light absorption detection method. The results showed that quinoline hydrazone compounds have a significant enzyme inhibitory effect on PTP 1B. At the concentration of 20 μg/mL, 21 as-synthesized compounds have an inhibition rate of over 80% for PTP 1B. Among them, compound 6q has the best inhibitory rate of 97.98%. Therefore, these compounds have the potential to regulate metabolism, and provide a certain research basis for the development of new anti-diabetes and anti-tumor drugs.
Quinoline hydrazone and quinoline acylhydrazone compounds had been found to have a wide range of biological activities. In this paper, 29 unreported 4-(2-aryl) quinoline arylhydrazone and aroylhydrazone compounds were designed and synthesized, and the inhibitory effects of these compounds on protein tyrosine phosphatase (PTP 1B) were tested by light absorption detection method. The results showed that quinoline hydrazone compounds have a significant enzyme inhibitory effect on PTP 1B. At the concentration of 20 μg/mL, 21 as-synthesized compounds have an inhibition rate of over 80% for PTP 1B. Among them, compound 6q has the best inhibitory rate of 97.98%. Therefore, these compounds have the potential to regulate metabolism, and provide a certain research basis for the development of new anti-diabetes and anti-tumor drugs.
2021, 84(1): 90-95
Abstract:
Taking natural product naringenin as raw material, it was etherified with α-bromoacetophenone, 4-chloro-α-bromoacetophenone, 1-(2-bromoethyl)-indole-3-formaldehyde and α-bromoacetone respectively. Then the intermediate products were subjected to oximation reaction with hydroxylamine hydrochloride and methoxyamine hydrochloride to obtained eight polyoxime naringin derivatives 6~13. Their structures were determined by IR, NMR and HR-MS. The cytotoxic activities of the target compounds were evaluated against SGC-7901 by MTT method in vitro. The results showed that the compounds 10 and 12 display distinct antiproliferative activity against SGC-7901 with the values of IC50 16.4 and 15.3 μmol/L, respectively.
Taking natural product naringenin as raw material, it was etherified with α-bromoacetophenone, 4-chloro-α-bromoacetophenone, 1-(2-bromoethyl)-indole-3-formaldehyde and α-bromoacetone respectively. Then the intermediate products were subjected to oximation reaction with hydroxylamine hydrochloride and methoxyamine hydrochloride to obtained eight polyoxime naringin derivatives 6~13. Their structures were determined by IR, NMR and HR-MS. The cytotoxic activities of the target compounds were evaluated against SGC-7901 by MTT method in vitro. The results showed that the compounds 10 and 12 display distinct antiproliferative activity against SGC-7901 with the values of IC50 16.4 and 15.3 μmol/L, respectively.
