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2021 Volume 40 Issue 10
2021, 40(10): 1253-1264
doi: 10.14102/j.cnki.0254–5861.2011–3147
Abstract:
We have designed and synthesized a family of dinuclear cyanido-bridged complexes [PY5Me2Ru(μ-CN)Ru(dppe)CpMen][PF6]2 (PY5Me2 = 2, 6-bis (1, 1-bis (2-pyridyl)ethyl) pyridine, Cp = cyclopentadienyl, n = 0, 2[PF6]2; n = 1, 3[PF6]2; n = 5, 4[PF6]2) by using a mononuclear complex [PY5Me2Ru(μ-CN)][PF6] (1) as the precursor. All the three complexes have been fully characterized by including single-crystal X-ray diffraction analysis. The one-electron oxidation complexes 23+, 33+ and 43+ obtained in situ all show a MMCT absorption band in the visible range. The MMCT energy increases as the redox potential of the N-terminal fragments decreases, and the redox potential decreases as the number of methyl groups on the cyclopentadiene of the cyanido-nitrogen coordinated Ru metal increases, supported by the TDF/TDDFT calculations.
We have designed and synthesized a family of dinuclear cyanido-bridged complexes [PY5Me2Ru(μ-CN)Ru(dppe)CpMen][PF6]2 (PY5Me2 = 2, 6-bis (1, 1-bis (2-pyridyl)ethyl) pyridine, Cp = cyclopentadienyl, n = 0, 2[PF6]2; n = 1, 3[PF6]2; n = 5, 4[PF6]2) by using a mononuclear complex [PY5Me2Ru(μ-CN)][PF6] (1) as the precursor. All the three complexes have been fully characterized by including single-crystal X-ray diffraction analysis. The one-electron oxidation complexes 23+, 33+ and 43+ obtained in situ all show a MMCT absorption band in the visible range. The MMCT energy increases as the redox potential of the N-terminal fragments decreases, and the redox potential decreases as the number of methyl groups on the cyclopentadiene of the cyanido-nitrogen coordinated Ru metal increases, supported by the TDF/TDDFT calculations.
2021, 40(10): 1265-1270
doi: 10.14102/j.cnki.0254–5861.2011–3149
Abstract:
Two pyrazole-based zinc(II) metal-organic frameworks, [(Zn4(PDC)2(BDC)(H2O)2]n (compound 1, PDC = 1H-pyrazole-3, 5-dicarboxylic acid, BDC = benzene-1, 4, -dicarboxylic acid) and [(Zn3(PDC)2(BPY)3(H2O)2]n (compound 2, BPY = 4, 4-bipyridine), were synthesized and characterized by X-ray diffraction, elemental analysis, thermogravimetric analysis, infrared and fluorescence spectroscopy. Compound 1 crystallizes in space group Pna21 with a = 14.325(3), b = 10.004(2), c = 16.454(3) Å, V = 2357.8(8) Å3, Z = 4, Mr = 821.83, Dc = 2.298 g·cm-3, F(000) = 1608, GOOF = 1.163, the final R = 0.0218 and wR = 0.0686 for 5150 observed reflections with I > 2σ(I). Compound 2 crystallizes in monoclinic space group C2/c with a = 17.034(2), b = 11.6313(9), c = 11.7608(13) Å, V = 2034.9(4) Å3, Z = 2, Mr = 1006.91, Dc = 1.643 g·cm-3, F(000) = 1020, GOOF = 1.084, the final R = 0.0320 and wR = 0.0768 for 2435 observed reflections with I > 2σ(I).
Two pyrazole-based zinc(II) metal-organic frameworks, [(Zn4(PDC)2(BDC)(H2O)2]n (compound 1, PDC = 1H-pyrazole-3, 5-dicarboxylic acid, BDC = benzene-1, 4, -dicarboxylic acid) and [(Zn3(PDC)2(BPY)3(H2O)2]n (compound 2, BPY = 4, 4-bipyridine), were synthesized and characterized by X-ray diffraction, elemental analysis, thermogravimetric analysis, infrared and fluorescence spectroscopy. Compound 1 crystallizes in space group Pna21 with a = 14.325(3), b = 10.004(2), c = 16.454(3) Å, V = 2357.8(8) Å3, Z = 4, Mr = 821.83, Dc = 2.298 g·cm-3, F(000) = 1608, GOOF = 1.163, the final R = 0.0218 and wR = 0.0686 for 5150 observed reflections with I > 2σ(I). Compound 2 crystallizes in monoclinic space group C2/c with a = 17.034(2), b = 11.6313(9), c = 11.7608(13) Å, V = 2034.9(4) Å3, Z = 2, Mr = 1006.91, Dc = 1.643 g·cm-3, F(000) = 1020, GOOF = 1.084, the final R = 0.0320 and wR = 0.0768 for 2435 observed reflections with I > 2σ(I).
2021, 40(10): 1271-1276
doi: 10.14102/j.cnki.0254–5861.2011–3135
Abstract:
A new quaternary metal thiophosphate, Cs2Ga3PS8, in triclinic P\begin{document}$ \overline 1 $\end{document}
A new quaternary metal thiophosphate, Cs2Ga3PS8, in triclinic P
2021, 40(10): 1277-1283
doi: 10.14102/j.cnki.0254–5861.2011–3150
Abstract:
In this paper, two cocrystals 1 and 2 with the same chemical composition [L1.L2] (L1 = bis(4΄-pyridyl)-TTF, L2 = 4, 4΄-diiodophenyl) were synthesized by slow diffusion with different solvent systems. Cocrystals 1 and 2 were characterized by single-crystal X-ray and the purity of these two cocrystals was confirmed by PXRD data. The photocurrent responses of these two cocrystals were also tested. Only cocrystal 1 could generate photocurrent signal when exposed to light. From the crystal structure analysis, the possible reason may come from the different biphenyl conformations in L2.
In this paper, two cocrystals 1 and 2 with the same chemical composition [L1.L2] (L1 = bis(4΄-pyridyl)-TTF, L2 = 4, 4΄-diiodophenyl) were synthesized by slow diffusion with different solvent systems. Cocrystals 1 and 2 were characterized by single-crystal X-ray and the purity of these two cocrystals was confirmed by PXRD data. The photocurrent responses of these two cocrystals were also tested. Only cocrystal 1 could generate photocurrent signal when exposed to light. From the crystal structure analysis, the possible reason may come from the different biphenyl conformations in L2.
2021, 40(10): 1284-1290
doi: 10.14102/j.cnki.0254–5861.2011–3158
Abstract:
The target compound IV (C20H21N) was synthesized through four-step reactions and structurally determined by single-crystal X-ray diffraction. The crystal of compound IV is in the orthorhombic system, space group Fdd2 with a = 41.178(19), b = 30.389(8), c = 4.8182(17) Å, β = 90°, C20H21N, Mr = 275.38, Dc = 1.213 g/cm3, V = 6029(4) Å3, Z = 16, F(000) = 2368, µ(MoKa) = 0.527 mm-1, T = 240(2) K, 2200 independent reflections with 1233 observed ones (I > 2σ(I)), R = 0.1285 and wR = 0.2589 with GOF = 1.050 (R = 0.2058 and wR = 0.3055 for all data). A one-dimensional interaction model of the title compound was formed by one kind of π-π interactions between the two phenyl rings of the adjacent molecules at upper and lower levels. The inhibition to the strand transfer process of HIV-1 integrase of the target compound was also evaluated.
The target compound IV (C20H21N) was synthesized through four-step reactions and structurally determined by single-crystal X-ray diffraction. The crystal of compound IV is in the orthorhombic system, space group Fdd2 with a = 41.178(19), b = 30.389(8), c = 4.8182(17) Å, β = 90°, C20H21N, Mr = 275.38, Dc = 1.213 g/cm3, V = 6029(4) Å3, Z = 16, F(000) = 2368, µ(MoKa) = 0.527 mm-1, T = 240(2) K, 2200 independent reflections with 1233 observed ones (I > 2σ(I)), R = 0.1285 and wR = 0.2589 with GOF = 1.050 (R = 0.2058 and wR = 0.3055 for all data). A one-dimensional interaction model of the title compound was formed by one kind of π-π interactions between the two phenyl rings of the adjacent molecules at upper and lower levels. The inhibition to the strand transfer process of HIV-1 integrase of the target compound was also evaluated.
2021, 40(10): 1291-1297
doi: 10.14102/j.cnki.0254–5861.2011–3176
Abstract:
A π-conjugated optical functional organic compound comprising an electron donor (D) and acceptor (A) was synthesized. The crystal structure was determined through single-crystal X-ray diffraction analysis. It crystallizes in monoclinic, space group P21 with a = 9.6610(5), b = 8.9093(4), c = 26.303(1) Å, β = 96.262(4)°, V = 2250.5(2) Å3, Z = 4, Dc = 1.220 Mg/m3, F(000) = 872, Μr = 413.50, μ = 0.072 mm-1, the final R = 0.0569 and wR = 0.1700 for 8976 observed reflections with I > 2σ(I). Optical properties were studied in detail through theoretical calculation and experimental study. The result reveals that the compound exhibits excellent fluorescence performance and it can be compatible in the cytoplasm of NIH/3T3 cells, showing potential in fluorescence microscopy bioimaging.
A π-conjugated optical functional organic compound comprising an electron donor (D) and acceptor (A) was synthesized. The crystal structure was determined through single-crystal X-ray diffraction analysis. It crystallizes in monoclinic, space group P21 with a = 9.6610(5), b = 8.9093(4), c = 26.303(1) Å, β = 96.262(4)°, V = 2250.5(2) Å3, Z = 4, Dc = 1.220 Mg/m3, F(000) = 872, Μr = 413.50, μ = 0.072 mm-1, the final R = 0.0569 and wR = 0.1700 for 8976 observed reflections with I > 2σ(I). Optical properties were studied in detail through theoretical calculation and experimental study. The result reveals that the compound exhibits excellent fluorescence performance and it can be compatible in the cytoplasm of NIH/3T3 cells, showing potential in fluorescence microscopy bioimaging.
2021, 40(10): 1298-1308
doi: 10.14102/j.cnki.0254–5861.2011–3126
Abstract:
HDAC8 is an important target for the treatment of many cancers and other diseases. To develop potent and selective HDAC8 inhibitors, molecular docking and molecular dynamics (MD) simulations were employed for investigation of the mechanism of HDAC8 inhibitions containing hydroxamic acid group. Compound 1 with high activity and compound 2 with low activity were selected for comparative study. Compound 1 formed a stronger chelation with Zn ion and was more stable in the HDAC8 pocket than compound 2. Residues HIS-180, ASP-178, ASP-267, and GLY-140 played a critical role in securing the position of compound 1. Both the head and tail of compound 1 formed strong hydrogen bonds with ASP-178, facilitating the ZBG of compound 1 close to the Zn ion so that they formed permanent chelation during the simulation period. The Cap group of the compounds with branch and long chains was advantageous to form interaction with active pocket opening. What's more, based on the results of this study, three innovative recommendations for the design of highly active HDAC8 inhibitors were presented, which will be useful for the development of new HDAC8 inhibitors.
HDAC8 is an important target for the treatment of many cancers and other diseases. To develop potent and selective HDAC8 inhibitors, molecular docking and molecular dynamics (MD) simulations were employed for investigation of the mechanism of HDAC8 inhibitions containing hydroxamic acid group. Compound 1 with high activity and compound 2 with low activity were selected for comparative study. Compound 1 formed a stronger chelation with Zn ion and was more stable in the HDAC8 pocket than compound 2. Residues HIS-180, ASP-178, ASP-267, and GLY-140 played a critical role in securing the position of compound 1. Both the head and tail of compound 1 formed strong hydrogen bonds with ASP-178, facilitating the ZBG of compound 1 close to the Zn ion so that they formed permanent chelation during the simulation period. The Cap group of the compounds with branch and long chains was advantageous to form interaction with active pocket opening. What's more, based on the results of this study, three innovative recommendations for the design of highly active HDAC8 inhibitors were presented, which will be useful for the development of new HDAC8 inhibitors.
2021, 40(10): 1309-1316
doi: 10.14102/j.cnki.0254–5861.2011–3159
Abstract:
A highly selective iron ions fluorescent probe based on the benz(c)acridine-1, 2, 3-triazole derivatives was produced by multi-step reactions. 1-(7-Benz[c]acridinyl)-4-(4-methylphenyl)-1, 2, 3-triazole (4a), C26H18N4, was structurally determined by single-crystal X-ray diffraction. It crystallizes in the trigonal system, space group R-3 with a = 36.230(10), b = 36.230(10), c = 7.993(3) Å, β = 90°, V = 9086(6) Å3, Z = 18, Dc = 1.271 g/cm3, F(000) = 3636, μ = 0.602 mm-1, the final R = 0.0865 and wR = 0.1619 for 3951 observed reflections (I > 2σ(I)). X-ray analysis indicated that all four rings of benz(c)acridine are in the same plane, and the 1, 2, 3-triazole ring and the corresponding linked benzene (C(1)–C(6)–C(7)–C(8)–C(9)–N(1)) are approximately perpendicular with a dihedral angle of 106.5°. The crystal packing of the compound was stabilized by two weak interactions between C(11)–H(10)···N(4) and C(18)–H(18)···N(1). In fluorescence spectra studies, compound 4c was exhibited good selectivity and sensitivity towards iron ions in DMSO: mops buffer solution. Furthermore, 4c was successfully used for imaging iron ions in living HeLa cervical cancer cells.
A highly selective iron ions fluorescent probe based on the benz(c)acridine-1, 2, 3-triazole derivatives was produced by multi-step reactions. 1-(7-Benz[c]acridinyl)-4-(4-methylphenyl)-1, 2, 3-triazole (4a), C26H18N4, was structurally determined by single-crystal X-ray diffraction. It crystallizes in the trigonal system, space group R-3 with a = 36.230(10), b = 36.230(10), c = 7.993(3) Å, β = 90°, V = 9086(6) Å3, Z = 18, Dc = 1.271 g/cm3, F(000) = 3636, μ = 0.602 mm-1, the final R = 0.0865 and wR = 0.1619 for 3951 observed reflections (I > 2σ(I)). X-ray analysis indicated that all four rings of benz(c)acridine are in the same plane, and the 1, 2, 3-triazole ring and the corresponding linked benzene (C(1)–C(6)–C(7)–C(8)–C(9)–N(1)) are approximately perpendicular with a dihedral angle of 106.5°. The crystal packing of the compound was stabilized by two weak interactions between C(11)–H(10)···N(4) and C(18)–H(18)···N(1). In fluorescence spectra studies, compound 4c was exhibited good selectivity and sensitivity towards iron ions in DMSO: mops buffer solution. Furthermore, 4c was successfully used for imaging iron ions in living HeLa cervical cancer cells.
2021, 40(10): 1317-1327
doi: 10.14102/j.cnki.0254–5861.2011–3171
Abstract:
Based on CiteSpace software, big data bibliometrics analysis was carried out on the keywords of papers of photocatalytic materials published in 2020. Tracking the hotspots and directions can help young scholars to understand the latest progress. In the Web of Sciences, 4147 related papers were searched with "photocatalytic materials" as the main topic. Cluster analysis showed that the hotspots were g-C3N4, Mxene and metal-organic frameworks (MOF) and titanium dioxide (TiO2).
Based on CiteSpace software, big data bibliometrics analysis was carried out on the keywords of papers of photocatalytic materials published in 2020. Tracking the hotspots and directions can help young scholars to understand the latest progress. In the Web of Sciences, 4147 related papers were searched with "photocatalytic materials" as the main topic. Cluster analysis showed that the hotspots were g-C3N4, Mxene and metal-organic frameworks (MOF) and titanium dioxide (TiO2).
2021, 40(10): 1328-1336
doi: 10.14102/j.cnki.0254–5861.2011–3173
Abstract:
Traditional adsorbents are normally suffered from a low adsorption capacity that has a finite saturated adsorption capacity. We reported herein a hierarchical self-growing porous calcium silicate hydrate (CSH) that uses biowaste as the precursor and is highly efficient in wastewater purification. In the process of phosphorus removal, CSH can react with phosphorus in water and grow into the hydroxyapatite (HAP). The generation of HAP further increases the active sites while maintains the porous structure of pristine CSH. Subsequently, the HAP could conduct the efficient extraction of Pb2+ from wastewater based on the ion exchange between Ca2+ and Pb2+. Clearly, the CSH structure has self-growing structure using the pollutants as the building blocks, not only achieving high adsorption capacity for pollutants, but also maintaining the hierarchically porous structure that supports the high efficiency in the next cycling. We provide here an intriguing pathway to tackle bottleneck of the traditional adsorbents, i.e., a finite saturated adsorption capacity.
Traditional adsorbents are normally suffered from a low adsorption capacity that has a finite saturated adsorption capacity. We reported herein a hierarchical self-growing porous calcium silicate hydrate (CSH) that uses biowaste as the precursor and is highly efficient in wastewater purification. In the process of phosphorus removal, CSH can react with phosphorus in water and grow into the hydroxyapatite (HAP). The generation of HAP further increases the active sites while maintains the porous structure of pristine CSH. Subsequently, the HAP could conduct the efficient extraction of Pb2+ from wastewater based on the ion exchange between Ca2+ and Pb2+. Clearly, the CSH structure has self-growing structure using the pollutants as the building blocks, not only achieving high adsorption capacity for pollutants, but also maintaining the hierarchically porous structure that supports the high efficiency in the next cycling. We provide here an intriguing pathway to tackle bottleneck of the traditional adsorbents, i.e., a finite saturated adsorption capacity.
2021, 40(10): 1337-1345
doi: 10.14102/j.cnki.0254–5861.2011–3146
Abstract:
Scintillator is a material that converts high-energy rays into visible light, and has great applications in high-energy physics, medical imaging, and security inspections. As a type of scintillator, scintillation glass has the advantages of low cost, high stability, controllable shape, and ability to be prepared on a large scale. In this paper, a traditional fusion quenching method was used to prepare a cerium-terbium co-doped glass. The green characteristic light of Tb ion was observed at 543 nm. Moreover, through the doping sensitization of Ce ions, the luminescence of Tb was successfully enhanced. The material has high X-ray response sensitivity, complete stability and strong X-ray emission intensity. We use a simple X-ray imaging platform for imaging, and the results show that our glass has a spatial resolution of 7.0 lp/mm.
Scintillator is a material that converts high-energy rays into visible light, and has great applications in high-energy physics, medical imaging, and security inspections. As a type of scintillator, scintillation glass has the advantages of low cost, high stability, controllable shape, and ability to be prepared on a large scale. In this paper, a traditional fusion quenching method was used to prepare a cerium-terbium co-doped glass. The green characteristic light of Tb ion was observed at 543 nm. Moreover, through the doping sensitization of Ce ions, the luminescence of Tb was successfully enhanced. The material has high X-ray response sensitivity, complete stability and strong X-ray emission intensity. We use a simple X-ray imaging platform for imaging, and the results show that our glass has a spatial resolution of 7.0 lp/mm.
2021, 40(10): 1346-1356
doi: 10.14102/j.cnki.0254–5861.2011–3153
Abstract:
Designing efficient electrocatalysts for efficient hydrogen evolution is extremely desired but challenging. Herein, we report a facile MOF-assisted strategy to synthesize the hierarchical hollow spherical NiRu-C nanohybrid with closely packed rod-like bulges on the surface. Benefited from the more exposed active sites of NiRu-C nanohybrid and the efficient electron/mass transport in its unique hierarchical hollow spherical nanostructure, the optimized nanohybrid showed excellent performance for alkaline hydrogen evolution with ultralow overpotentials, which are much superior to those of Pt/C and the overwhelming majority of reported electrocatalysts. The interpretation of the reaction mechanism was further discussed with DFT calculations. Our research may provide a guidance for the development of advanced electrocatalysts with controlled morphology and excellent performance for future energy applications.
Designing efficient electrocatalysts for efficient hydrogen evolution is extremely desired but challenging. Herein, we report a facile MOF-assisted strategy to synthesize the hierarchical hollow spherical NiRu-C nanohybrid with closely packed rod-like bulges on the surface. Benefited from the more exposed active sites of NiRu-C nanohybrid and the efficient electron/mass transport in its unique hierarchical hollow spherical nanostructure, the optimized nanohybrid showed excellent performance for alkaline hydrogen evolution with ultralow overpotentials, which are much superior to those of Pt/C and the overwhelming majority of reported electrocatalysts. The interpretation of the reaction mechanism was further discussed with DFT calculations. Our research may provide a guidance for the development of advanced electrocatalysts with controlled morphology and excellent performance for future energy applications.
2021, 40(10): 1357-1364
doi: 10.14102/j.cnki.0254–5861.2011–3154
Abstract:
It is very hard to obtain uniformly dispersed conductive polymer nanocomposites because of the accumulation tendency of nanomaterials. In current work, the aramid nanofiber/silver nanowire composite film was prepared by mixing evenly through the solution and then vacuum filtration. The composite film exhibited desirable physical properties such as high tensile strength (121 MPa), outstanding electrical conductivity (652 S·cm-1), and thermal conductivity (0.12 W·m-1·K-1). These endow our aramid nanofiber/silver nanowire composite film with possible applications in infrared stealth and harsh environments.
It is very hard to obtain uniformly dispersed conductive polymer nanocomposites because of the accumulation tendency of nanomaterials. In current work, the aramid nanofiber/silver nanowire composite film was prepared by mixing evenly through the solution and then vacuum filtration. The composite film exhibited desirable physical properties such as high tensile strength (121 MPa), outstanding electrical conductivity (652 S·cm-1), and thermal conductivity (0.12 W·m-1·K-1). These endow our aramid nanofiber/silver nanowire composite film with possible applications in infrared stealth and harsh environments.
2021, 40(10): 1365-1371
doi: 10.14102/j.cnki.0254–5861.2011–3168
Abstract:
In the industry, cheap and stable electrocatalysts are eagerly expected for hydrogen evolution reaction (HER) at a high current density. Two-component electrochemical catalysts with integrated multiple interfaces seem to be an expedient strategy to enhance the inherent electronic structure of hybrid electrocatalysts and optimize the catalytic ability. In this work, we report an active tungsten carbide and nickel hydroxide (WC/Ni(OH)2) electrocatalyst seamlessly synthesized on the substrate of W foil. Ni(OH)2 trends to adsorb OHad and WC can effectively adsorb Had. Prompted by the synergistic effect, the ability of the catalyst manifests an effective HER kinetics with an overpotential of 475 mV (vs. RHE) at a high current density of 1000 mA/cm2 in 1 M KOH. Moreover, due to its self-supported construction, the catalyst presents reliable long-term stability with no obvious active property loss after 8000 cycles and 50 hours of operation in an alkaline solution.
In the industry, cheap and stable electrocatalysts are eagerly expected for hydrogen evolution reaction (HER) at a high current density. Two-component electrochemical catalysts with integrated multiple interfaces seem to be an expedient strategy to enhance the inherent electronic structure of hybrid electrocatalysts and optimize the catalytic ability. In this work, we report an active tungsten carbide and nickel hydroxide (WC/Ni(OH)2) electrocatalyst seamlessly synthesized on the substrate of W foil. Ni(OH)2 trends to adsorb OHad and WC can effectively adsorb Had. Prompted by the synergistic effect, the ability of the catalyst manifests an effective HER kinetics with an overpotential of 475 mV (vs. RHE) at a high current density of 1000 mA/cm2 in 1 M KOH. Moreover, due to its self-supported construction, the catalyst presents reliable long-term stability with no obvious active property loss after 8000 cycles and 50 hours of operation in an alkaline solution.
2021, 40(10): 1372-1378
doi: 10.14102/j.cnki.0254–5861.2011–3178
Abstract:
In this study, an efficient catalyst Ag@g-C3N4 nanocomposite was successfully synthesized through a simple green reaction, and the characterizations through XRD, FTIR, SEM, BET and XPS were also studied. The activities of Ag@g-C3N4 were investigated toward the reduction of 4-nitrophenol to their corresponding aminophenol compounds in the presence of excess NaBH4 as a reducing agent. The Ag@g-C3N4 nanocomposites exhibited high catalytic activities, in which a 92.2% 4-nitrophenol conversion in 10 min and the apparent rate constant Kapp = 264.27×10-3 min-1 were obtained. The as-prepared Ag@g-C3N4 nanocomposites showed great potential in catalytically inducing the reduction of 4-nitrophenol, which makes them economically and energy conservation attractive from industrial waste water treatment.
In this study, an efficient catalyst Ag@g-C3N4 nanocomposite was successfully synthesized through a simple green reaction, and the characterizations through XRD, FTIR, SEM, BET and XPS were also studied. The activities of Ag@g-C3N4 were investigated toward the reduction of 4-nitrophenol to their corresponding aminophenol compounds in the presence of excess NaBH4 as a reducing agent. The Ag@g-C3N4 nanocomposites exhibited high catalytic activities, in which a 92.2% 4-nitrophenol conversion in 10 min and the apparent rate constant Kapp = 264.27×10-3 min-1 were obtained. The as-prepared Ag@g-C3N4 nanocomposites showed great potential in catalytically inducing the reduction of 4-nitrophenol, which makes them economically and energy conservation attractive from industrial waste water treatment.
2021, 40(10): 1379-1384
doi: 10.14102/j.cnki.0254–5861.2011–3185
Abstract:
Codoping with Mn+ ions (Mn+ = Li+, Mn2+ and Cu2+) enhanced the blue and red upconversion (UC) emissions in TiO2: Yb3+/Tm3+ nanocrystals under 980 nm excitation. The different effects of Li+, Mn2+ and Cu2+ ions on the phase structures, morphologies and optical characteristics of TiO2: Yb3+/Tm3+ were discussed. The minor shifting in the diffraction peaks at 25.2° was observed for TiO2: Yb3+/Tm3+/Li+, and adding Mn2+ ions remained almost the same position of diffraction peaks, while the introduction of Cu2+ ions resulted in the shift of the diffraction peaks towards the larger angles. TiO2: Yb3+/Tm3+/Li+ and TiO2: Yb3+/Tm3+/Mn2+ nanosheets and the sphere-like TiO2: Yb3+/Tm3+/Cu2+ were observed. The mechanisms for increased UC emissions caused by adding Li+, Mn2+ and Cu2+ ions were attributed to the tailored local environment around Tm3+ ions, efficient energy transition between Mn2+-Yb3+ dimer and Tm3+ ions, and the localized surface plasmon resonance (LSPR) of Cu2+ ions, respectively.
Codoping with Mn+ ions (Mn+ = Li+, Mn2+ and Cu2+) enhanced the blue and red upconversion (UC) emissions in TiO2: Yb3+/Tm3+ nanocrystals under 980 nm excitation. The different effects of Li+, Mn2+ and Cu2+ ions on the phase structures, morphologies and optical characteristics of TiO2: Yb3+/Tm3+ were discussed. The minor shifting in the diffraction peaks at 25.2° was observed for TiO2: Yb3+/Tm3+/Li+, and adding Mn2+ ions remained almost the same position of diffraction peaks, while the introduction of Cu2+ ions resulted in the shift of the diffraction peaks towards the larger angles. TiO2: Yb3+/Tm3+/Li+ and TiO2: Yb3+/Tm3+/Mn2+ nanosheets and the sphere-like TiO2: Yb3+/Tm3+/Cu2+ were observed. The mechanisms for increased UC emissions caused by adding Li+, Mn2+ and Cu2+ ions were attributed to the tailored local environment around Tm3+ ions, efficient energy transition between Mn2+-Yb3+ dimer and Tm3+ ions, and the localized surface plasmon resonance (LSPR) of Cu2+ ions, respectively.
2021, 40(10): 1385-1403
doi: 10.14102/j.cnki.0254–5861.2011–3081
Abstract:
Catalytic conversion of carbon dioxide (CO2) into value-added chemicals is an important and active field in both of the condensed-phase and gas-phase studies. This mini-review summarizes a variety of experimentally identified reactions in the activation and transformation of CO2 by metal species in the gas phase. The use of advanced mass spectrometric instrumentation in conjunction with quantum chemistry calculations can uncover the mechanistic details and determine the vital factors that control the activation of CO2. This review focuses mainly on three topics: the activation of CO2 by (1) bare metal ions and metal oxide species, (2) metal hydrides, and (3) other gas-phase metal species. Emphasis is placed on the latest advances in the hydrogenation of CO2 mediated with metal hydrides. A potential prospect toward the future effort in the activation and transformation of CO2 in gas phase has also been discussed.
Catalytic conversion of carbon dioxide (CO2) into value-added chemicals is an important and active field in both of the condensed-phase and gas-phase studies. This mini-review summarizes a variety of experimentally identified reactions in the activation and transformation of CO2 by metal species in the gas phase. The use of advanced mass spectrometric instrumentation in conjunction with quantum chemistry calculations can uncover the mechanistic details and determine the vital factors that control the activation of CO2. This review focuses mainly on three topics: the activation of CO2 by (1) bare metal ions and metal oxide species, (2) metal hydrides, and (3) other gas-phase metal species. Emphasis is placed on the latest advances in the hydrogenation of CO2 mediated with metal hydrides. A potential prospect toward the future effort in the activation and transformation of CO2 in gas phase has also been discussed.
