3-Methylthio-5-hydroxy-1,2,4-triazine(1c)reacted with substituted benzenesulfonyl chloride to give 3-methylthio-5-oxy-1,2,4-triazin-6-yl pyridinium betaine(4)in anhydrous pyridine.But when NaOH/H_2O/CH_3COCH_3 or NaOH...3-Methylthio-5-hydroxy-1,2,4-triazine(1c)reacted with substituted benzenesulfonyl chloride to give 3-methylthio-5-oxy-1,2,4-triazin-6-yl pyridinium betaine(4)in anhydrous pyridine.But when NaOH/H_2O/CH_3COCH_3 or NaOH/CH_3OH were used as reactant and solvent,3-methylthio-4-substituted benzenesulfonyl-5-oxo-6-hydroxy-1,4,5,6-tetrahydro-1,2,4-triazine(6)or 1-tosyl-3-methylthio-5-oxo-6-methyloxy-1,4,5,6-tetrahydro-1,2,4-triazine(7)was obtained respectively.The above reactions show anomalous properties of nucleophilic attack on 6-carbon in 1,2,4-triazine ring.展开更多
Six fully optimized structures of the aza-calix[2]arene[2]-triazines/RDX supramo-lecular complexes have been obtained at the DFT-B3LYP/6-311＋＋G＊＊ level,and the corresponding intermolecular interactions have been i...Six fully optimized structures of the aza-calix[2]arene[2]-triazines/RDX supramo-lecular complexes have been obtained at the DFT-B3LYP/6-311＋＋G＊＊ level,and the corresponding intermolecular interactions have been investigated using the B3LYP,mPWPW91 and MP2 methods at the 6-311＋＋G＊＊ level,respectively.The natural bond orbital（NBO） and atoms in molecules（AIM） analyses have been performed to reveal the origin of interactions.To our interest,the result indicates that the strongest interaction is up to-22.34 kJ/mol after basis set superposition error（BSSE） and zero point energy（ZPE） correction at the MP2/6-311＋＋G＊＊ level.Furthermore,the intermolecular interactions between aza-calix[2]arene[2]-triazines with the substituted amidos and RDX are stronger than those of other complexes.Thus,the complexes with amidos can be used as the candidates to increase the stability of explosive and eliminate the explosive wastewater.展开更多
Introduction 4,6-Diamino-1,2-dihydro-2,2-dimethyl-1-substituted-1,3,5-triazines (Ⅰ) are dihydrofolate reductase(DHFR) inhibitors, hence they possess the inhibition to the growth of bacteria and cancer cells. Baker’s...Introduction 4,6-Diamino-1,2-dihydro-2,2-dimethyl-1-substituted-1,3,5-triazines (Ⅰ) are dihydrofolate reductase(DHFR) inhibitors, hence they possess the inhibition to the growth of bacteria and cancer cells. Baker’s antifolate (Ⅱ) has shown promise as an antitumor agertt in clinical trials. The study of the structure-activity relationships of I shows that the inhibition to vertebrate DHFR is significantly influenced by the hydrophobicity of 1-substituent, i.e., the stronger the hydrophobicity of the 1-substituent, the more potent the inhibition of the compound to vertebrate DHFR.展开更多
Highly porous nitrogen-doped carbon materials were synthesized by the carbonization of a low-cost porous covalent triazine polymer, PCTP-3, which had been synthesized by the AlClcatalyzed FriedelCrafts reaction of rea...Highly porous nitrogen-doped carbon materials were synthesized by the carbonization of a low-cost porous covalent triazine polymer, PCTP-3, which had been synthesized by the AlClcatalyzed FriedelCrafts reaction of readily available monomers. The nature of the bond and structure of the resulting materials were confirmed using various spectroscopic methods, and the effects of KOH activation on the textural properties of the porous carbon materials were also examined. The KOH-activated porous carbon（aPCTP-3c） materials possessed a high surface area of 2271 mgand large micro/total pore volumes of 0.87/0.95 cmg, respectively, with narrower micropore size distributions than the porous carbon prepared without activation（PCTP-3c）. The aPCTP-3c exhibited the best COuptakes of 284.5 and 162.3 mg gand CHuptakes of 39.6 and 25.9 mg gat 273 and 298 K/1 bar, respectively, which are comparable to the performance of some benchmark carbon materials under the same conditions. The prepared materials exhibited high CO/Nselectivity and could be regenerated easily.展开更多
The title compound 4-oxo-1,2,4-triazino[4,5-a]benzimidazole（C9H6N4O,Mr = 186.18） has been synthesized and structurally characterized by IR,NMR and single-crystal X-ray diffraction. The crystal belongs to monoclinic,...The title compound 4-oxo-1,2,4-triazino[4,5-a]benzimidazole（C9H6N4O,Mr = 186.18） has been synthesized and structurally characterized by IR,NMR and single-crystal X-ray diffraction. The crystal belongs to monoclinic,space group P21/c,with a = 9.1530（18） ,b = 7.2260（14）,c = 12.604（3） ,β = 106.92（3） ,V = 797.5（3）A^3,Z = 4,Dc = 1.551 g/cm^3,λ（MoKa） = 0.71073,F（000） = 384,μ（MoKa） = 0.109 mm^-1,the final R = 0.0632 and wR = 0.1095. A total of 1444 unique reflections were collected,of which 767 with I 〉 2σ（I） were observed. The structure of the title compound is planar. In packing,the molecules are intersected to each other to form chains along three dimensions,together by intermolecular N-H…O and C-H…N hydrogen bonds. The whole structure is further stabilized by π…π interaction between two adjacent tricyclic ring systems,with the centroid-to-centroid distance of 3.369（4） A.展开更多
Solar‐driven CO_(2)conversion to precious fossil fuels has been proved to become a potential way to decrease CO_(2)with producing renewable fuels,which mainly relies on photocatalysts with efficient charge separation...Solar‐driven CO_(2)conversion to precious fossil fuels has been proved to become a potential way to decrease CO_(2)with producing renewable fuels,which mainly relies on photocatalysts with efficient charge separation.In this work,a metal free heterostructure of covalent triazine framework(CTF)and graphite carbon nitride(g‐C_(3)N_(4),abbreviated as CN)is applied in the CO_(2)photoreduction for the first time.Detailed characterization methods such as photoluminescence(PL)and time‐resolved PL(TR‐PL)decay are utilized to reveal the photo‐induced carries separating process on g‐C_(3)N_(4)/CTF(CN/CTF)heterostructure.The introduced CTF demonstrated a great boosting photocatalytic activity for CN,bringing about the transform rates of CO_(2)to CO reaching 151.1μmol/(g·h)with a 30 h stabilization time,while negligible CH_(4)was detected.The optimal CN/CTF heterostructure could more efficiently separate charges with a lower probability of recombination under visible light irradiation,which made the photoreduction efficiency of CO_(2)to CO be 25.5 and 2.5 times higher than that of CTF and CN,respectively.This investigation is expected to offer a new thought for fabricating high‐efficiency photocatalyst without metal in solar‐energy‐driven CO_(2)reduction.展开更多
Carbon super-heterostructures with high nitrogen contents from the covalent hybrid precursors of covalent triazine frameworks(CTFs)and zeolitic imidazolic frameworks(ZIFs)are scarcely explored because of CTF's ord...Carbon super-heterostructures with high nitrogen contents from the covalent hybrid precursors of covalent triazine frameworks(CTFs)and zeolitic imidazolic frameworks(ZIFs)are scarcely explored because of CTF's ordered structure and toxic superacid that dissolves or destabilizes the metal nodes.To solve this problem,herein,we report a straightforward two-step pathway for the covalent hybridization of disordered CTF(d–CTF)–ZIF composites via preincorporation of an imidazole(IM)linker into ordered CTFs,followed by the imidazole-site-specific covalent growth of ZIFs.Direct carbonization of these synthesized d–CTF−IM−ZIF hybrids results in unique hollow carbon super-heterostructures with ultrahigh nitrogen content(>18.6%),high specific surface area(1663m^(2)g^(−1)),and beneficial trace metal(Co/Zn NPs)contents for promoting the redox pseudocapacitance.As proof of concept,the obtained carbon super-heterostructure(Co–Zn–NC_(SNH)–800)is used as a positive electrode in an asymmetric supercapacitor,demonstrating a remarkable energy density of 61Wh kg^(−1)and extraordinary cyclic stability of 97%retention after 30,000 cycles at the cell level.Our presynthetic modifications of CTF and their covalent hybridization with ZIF crystals pave the way toward new design strategies for synthesizing functional porous carbon materials for promising energy applications.展开更多
探究秦川牛宰后成熟过程中线粒体Tu翻译延长因子(mitochondrial Tu translation elongation factor,TUFM)表达对肉的持水性影响。以秦川牛背最长肌为研究对象,测定4℃不同成熟时间下的pH值、贮藏损失、离心损失、蒸煮损失、水分分布、...探究秦川牛宰后成熟过程中线粒体Tu翻译延长因子(mitochondrial Tu translation elongation factor,TUFM)表达对肉的持水性影响。以秦川牛背最长肌为研究对象,测定4℃不同成熟时间下的pH值、贮藏损失、离心损失、蒸煮损失、水分分布、肌原纤维蛋白等指标变化情况,测定不同成熟时间(0、96、192 h)下TUFM表达量及其含量、Beclin1蛋白表达量。结果显示:在秦川牛宰后成熟期间,肌原纤维蛋白发生降解,TUFM的表达量与Beclin1蛋白表达量和牛肉的持水性存在密切关系,其中蛋白质组学测定的TUFM表达量变化与TUFM含量变化趋势一致,Beclin1蛋白表达量、贮藏损失、离心损失、蒸煮损失整体均呈先上升后下降趋势,pH值呈先下降后上升趋势;Pearson相关性分析表明,牛背最长肌中TUFM表达量与低场核磁共振峰面积比P_(2b)、Beclin1蛋白表达量呈极显著正相关(P<0.01),与贮藏损失、离心损失、蒸煮损失呈显著正相关(P<0.05),与P_(21)呈极显著负相关(P<0.01),与P_(22)呈显著负相关(P<0.05),与pH值无显著相关性(P>0.05)。通过蛋白质组学鉴定出23种与TUFM相关的差异蛋白,通过基因本体论、京都基因与基因组百科全书通路分析发现,差异蛋白可通过多种途径参与能量代谢,进而介导细胞自噬;对差异蛋白和持水性指标进行Pearson相关性分析发现,有5种差异蛋白(ATP5F1D、EEF1A2、GSPT1、NDUFB5、SUCLG1)与持水性指标具有显著相关性(P<0.05、P<0.01)。分析可知,包括TUFM在内,共6种蛋白主要通过能量代谢和氧转运等途径正向或负向影响细胞自噬,从而影响肉的持水性。展开更多
New fluorine substituted 6-(5’-fluoro-2’-triphenylphosphiniminophenyl) 3-thioxo-1,2,4-triazin-5 (2H, 4H) one (2) was obtained via Wittig’s reaction of the corresponding 6-(5’-fluoro-2’-amino-phenyl)-3-thioxo-1,2,...New fluorine substituted 6-(5’-fluoro-2’-triphenylphosphiniminophenyl) 3-thioxo-1,2,4-triazin-5 (2H, 4H) one (2) was obtained via Wittig’s reaction of the corresponding 6-(5’-fluoro-2’-amino-phenyl)-3-thioxo-1,2,4-triazinone (1). Behavior of compound 2 towards alkylating agents and/or oxidizing agents was studied were, N-hydroxyl (3), Mannich base (4,5), S-alkyl (6,7,8) and thiazolo [3,2-b][1,2,4] triazinones (10-14) and or 3-disulfide (18), 3-sulfonic acid 19 and 1,2,4-triazin-3,5-Dionne (20) derivatives obtained. Structures of the new products are established by elemental and spectral data. The new targets obtained screened as Molluscicidalagents against Biomophlaria Alexandrina snails responsible for Bilharziasis diseases, in compare with Baylucide as standard drug.展开更多
In this work, a 2D covalent triazine-based framework was prepared by using 1,3-dicyanobenzo[c]thiophene（DCBT） as monomer to effectively capture CO. The resulting CTF-DCBT was characterized by FT-IR, XPS, PXRD, eleme...In this work, a 2D covalent triazine-based framework was prepared by using 1,3-dicyanobenzo[c]thiophene（DCBT） as monomer to effectively capture CO. The resulting CTF-DCBT was characterized by FT-IR, XPS, PXRD, elemental analysis, SEM, TEM, and Nadsorption-desorption.The results indicate that CTF-DCBT is partially crystalline and has ultramicropore（6.5 A?） as well as high heteroatom contents（11.24 wt% and 12.61 wt% for N and S, respectively）. In addition, the BET surface area and total pore volume of CTF-DCBT are 500 m/g and 0.26 cm/g, respectively. CTF-DCBT possesses excellent thermal stability（450 °C） and chemical stability towards boiling water, 4 M HCl, and 1 M Na OH.The COadsorption capacity of CTF-DCBT is 37.8 cm/g at 1 bar and 25 °C. After six adsorption-desorption cycles, there is no obvious loss of COuptake observed. Due to the ultramicropore and high heteroatom contents, CTF-DCBT has high isosteric heats of adsorption for COand high selectivities of COover Nand CH. At 25 °C, the CO/Nand CO/CHselectivities are 112.5 and 10.3, respectively, which are higher than those of most POFs. Breakthrough curves indicate that CTF-DCBT could effectively separate CO/Nand CO/CHmixtures.展开更多
The crystal structure of the title compound 3-phenyl-6-（4-methylphenyl）-1,2,4- triazolo[4,3-b]-1,2,4-triazine （C17H13N5, Mr = 287.32） was synthesized and determined by singlecrystal X-ray diffraction. It belongs t...The crystal structure of the title compound 3-phenyl-6-（4-methylphenyl）-1,2,4- triazolo[4,3-b]-1,2,4-triazine （C17H13N5, Mr = 287.32） was synthesized and determined by singlecrystal X-ray diffraction. It belongs to monoclinic, space group P21/c, with α = 11.4038（18）, b = 11.7675（18）, c = 11.0904（18） A, β = 108.439（7）°, V = 1411.9（4） A^3, Z = 2, Dc = 1.352 g/cm^3, p = 0.085 mm^-1, F（000） = 600, R = 0.0445 and wR = 0.1041 for 2888 unique reflections with 1501 observed ones （I 〉20（I））. In the crystal structure, the triazine moiety is almost coplanar with the triazole ring, and the largest deviation for atom C（4） is -0.026 A. The intermolecular hydrogen bond in the crystal lattice plays an important role in stabilizing the structure.展开更多
[Pb（TPT）（μ-I）2PbI2（μ-I）2Pb（TPT）] 1 （TPT is the abbreviation of 3,5,6-tris（2- pyridyl）-1,2,4-triazine ligand） has been synthesized and characterized by elemental analysis, IR, J H- NMR spectroscopy and st...[Pb（TPT）（μ-I）2PbI2（μ-I）2Pb（TPT）] 1 （TPT is the abbreviation of 3,5,6-tris（2- pyridyl）-1,2,4-triazine ligand） has been synthesized and characterized by elemental analysis, IR, J H- NMR spectroscopy and studied by thermal and electrochemical properties as well as X-ray crystallography. The single-crystal X-ray data show two different kinds of Pb2＋ ions in 1 with coordination numbers of six, Pbl = PbI6, and five, Pb2 = PbN312, with holodirected and hemidirected coordination spheres, respectively. The supramolecular features in 1 are negotiated through the weak but directional Pb...I, C-H...N and C-H...I interactions and aromatic π-π stacking interactions.展开更多
The title compounds,C9H13ClN6O2S 1 and C15H17ClN6O2S 2,were synthesized and structurally characterized by elemental analysis,IR,1H NMR spectra and single-crystal X-ray diffraction.Compound 1 is in the monoclinic syste...The title compounds,C9H13ClN6O2S 1 and C15H17ClN6O2S 2,were synthesized and structurally characterized by elemental analysis,IR,1H NMR spectra and single-crystal X-ray diffraction.Compound 1 is in the monoclinic system,space group P21/c with a=13.7711（5）,b=10.3883（4）,c=9.7623（2）,V=1344.47（8）3,Dc=1.506 g/cm3,C9H13ClN6O2S,Mr=304.76,F（000）=632,μ=0.448 mm-1,Z=4,S=1.084,R=0.0497 and wR=0.1328 for 2640 unique reflections（Rint=0.0787） with 2089 observed ones（I2σ（I））.Compound 2 belongs to the monoclinic system,space group P21/n with a=8.3828（5）,b=14.5285（7）,c=14.2456（4）,V=1729.74（14）3,Dc=1.462 g/cm3,C15H17ClN6O2S,Mr=380.86,F（000）=792,μ=0.364 mm-1,Z=4,S=1.057,R=0.0598 and wR=0.1582 for 3384 unique reflections（Rint=0.0469） with 2833 observed ones（I2σ（I））.Compounds 1 and 2 are homologues and stabilized by intermolecular and intramolecular hydrogen bonds.Moreover,compound 2 containing C（2）–H（2）…π（thiazole） interaction is more stable than 1.展开更多
The crystal structure of 3-（5-amino-4-ethoxycarbonyl-3-methylthio-l-H-pyrazolyl）-5-phenyl- 1,2,4-triazine （C16H16N6O2S, Mr = 356.41） has been determined by single-crystal X-ray diffraction. It belongs to monoclini...The crystal structure of 3-（5-amino-4-ethoxycarbonyl-3-methylthio-l-H-pyrazolyl）-5-phenyl- 1,2,4-triazine （C16H16N6O2S, Mr = 356.41） has been determined by single-crystal X-ray diffraction. It belongs to monoclinic, space group P2（1/c） with a = 16.961（14）, b = 7.297（6）, c = 13.857（11）A^°, β = 109.803（13）°, V = 2237（2）A^°3, Z = 4, Dc = 1.467 g/cm^3,μ = 0.225 mm^-1, F（000） = 744, R=0.0477 and wR = 0.1156 for 2847 unique reflections with 1713 observed ones （I 〉2σ（I））. X-ray analysis reveals that there exist both intra- and intermolecular hydrogen bonds in the crystal lattice.展开更多
Herein,a novel direct Z-scheme photocatalyst was accomplished by hybridization of 0D MoS2 quantum dots(MSQDs)and 3D honeycomb-like conjugated triazine polymers(CTP)(namely,CTP-MSQD).The unique 0D/3D hierarchical struc...Herein,a novel direct Z-scheme photocatalyst was accomplished by hybridization of 0D MoS2 quantum dots(MSQDs)and 3D honeycomb-like conjugated triazine polymers(CTP)(namely,CTP-MSQD).The unique 0D/3D hierarchical structure significantly enhanced the exposure of active sites and light harvesting property,while the formed p-n junction enabled the direct strong interface coupling without the necessity of any mediators.The optimized CTP-MSQD3 exhibited continuously increased visible-light-driven photocatalytic activity and strong durability both in Cr(VI)reduction and H2 evolution,featured a rate of 0.069 min^(-1) and 1070μmol/(hr•g),respectively,which were 8 times than those of pure 3D-CTP(0.009 min^(−1) and 129μmol/(hr•g)).We believe that this work provides a promising photocatalyst system that combines a 0D/3D hierarchical structure and a Z-scheme charge flow for efficient and stable photocatalytic conversion.展开更多
基金Director of the project supported by National Natural Science foundation of China.
文摘3-Methylthio-5-hydroxy-1,2,4-triazine(1c)reacted with substituted benzenesulfonyl chloride to give 3-methylthio-5-oxy-1,2,4-triazin-6-yl pyridinium betaine(4)in anhydrous pyridine.But when NaOH/H_2O/CH_3COCH_3 or NaOH/CH_3OH were used as reactant and solvent,3-methylthio-4-substituted benzenesulfonyl-5-oxo-6-hydroxy-1,4,5,6-tetrahydro-1,2,4-triazine(6)or 1-tosyl-3-methylthio-5-oxo-6-methyloxy-1,4,5,6-tetrahydro-1,2,4-triazine(7)was obtained respectively.The above reactions show anomalous properties of nucleophilic attack on 6-carbon in 1,2,4-triazine ring.
文摘Six fully optimized structures of the aza-calix[2]arene[2]-triazines/RDX supramo-lecular complexes have been obtained at the DFT-B3LYP/6-311＋＋G＊＊ level,and the corresponding intermolecular interactions have been investigated using the B3LYP,mPWPW91 and MP2 methods at the 6-311＋＋G＊＊ level,respectively.The natural bond orbital（NBO） and atoms in molecules（AIM） analyses have been performed to reveal the origin of interactions.To our interest,the result indicates that the strongest interaction is up to-22.34 kJ/mol after basis set superposition error（BSSE） and zero point energy（ZPE） correction at the MP2/6-311＋＋G＊＊ level.Furthermore,the intermolecular interactions between aza-calix[2]arene[2]-triazines with the substituted amidos and RDX are stronger than those of other complexes.Thus,the complexes with amidos can be used as the candidates to increase the stability of explosive and eliminate the explosive wastewater.
基金Supported by the National Natural Science Foundation of China
文摘Introduction 4,6-Diamino-1,2-dihydro-2,2-dimethyl-1-substituted-1,3,5-triazines (Ⅰ) are dihydrofolate reductase(DHFR) inhibitors, hence they possess the inhibition to the growth of bacteria and cancer cells. Baker’s antifolate (Ⅱ) has shown promise as an antitumor agertt in clinical trials. The study of the structure-activity relationships of I shows that the inhibition to vertebrate DHFR is significantly influenced by the hydrophobicity of 1-substituent, i.e., the stronger the hydrophobicity of the 1-substituent, the more potent the inhibition of the compound to vertebrate DHFR.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(grant number:2015042434)the support by the Korea Research Fellowship Program(grant number:2017H1D3A1A02013620)
文摘Highly porous nitrogen-doped carbon materials were synthesized by the carbonization of a low-cost porous covalent triazine polymer, PCTP-3, which had been synthesized by the AlClcatalyzed FriedelCrafts reaction of readily available monomers. The nature of the bond and structure of the resulting materials were confirmed using various spectroscopic methods, and the effects of KOH activation on the textural properties of the porous carbon materials were also examined. The KOH-activated porous carbon（aPCTP-3c） materials possessed a high surface area of 2271 mgand large micro/total pore volumes of 0.87/0.95 cmg, respectively, with narrower micropore size distributions than the porous carbon prepared without activation（PCTP-3c）. The aPCTP-3c exhibited the best COuptakes of 284.5 and 162.3 mg gand CHuptakes of 39.6 and 25.9 mg gat 273 and 298 K/1 bar, respectively, which are comparable to the performance of some benchmark carbon materials under the same conditions. The prepared materials exhibited high CO/Nselectivity and could be regenerated easily.
基金sponsored by the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry
文摘The title compound 4-oxo-1,2,4-triazino[4,5-a]benzimidazole（C9H6N4O,Mr = 186.18） has been synthesized and structurally characterized by IR,NMR and single-crystal X-ray diffraction. The crystal belongs to monoclinic,space group P21/c,with a = 9.1530（18） ,b = 7.2260（14）,c = 12.604（3） ,β = 106.92（3） ,V = 797.5（3）A^3,Z = 4,Dc = 1.551 g/cm^3,λ（MoKa） = 0.71073,F（000） = 384,μ（MoKa） = 0.109 mm^-1,the final R = 0.0632 and wR = 0.1095. A total of 1444 unique reflections were collected,of which 767 with I 〉 2σ（I） were observed. The structure of the title compound is planar. In packing,the molecules are intersected to each other to form chains along three dimensions,together by intermolecular N-H…O and C-H…N hydrogen bonds. The whole structure is further stabilized by π…π interaction between two adjacent tricyclic ring systems,with the centroid-to-centroid distance of 3.369（4） A.
文摘Solar‐driven CO_(2)conversion to precious fossil fuels has been proved to become a potential way to decrease CO_(2)with producing renewable fuels,which mainly relies on photocatalysts with efficient charge separation.In this work,a metal free heterostructure of covalent triazine framework(CTF)and graphite carbon nitride(g‐C_(3)N_(4),abbreviated as CN)is applied in the CO_(2)photoreduction for the first time.Detailed characterization methods such as photoluminescence(PL)and time‐resolved PL(TR‐PL)decay are utilized to reveal the photo‐induced carries separating process on g‐C_(3)N_(4)/CTF(CN/CTF)heterostructure.The introduced CTF demonstrated a great boosting photocatalytic activity for CN,bringing about the transform rates of CO_(2)to CO reaching 151.1μmol/(g·h)with a 30 h stabilization time,while negligible CH_(4)was detected.The optimal CN/CTF heterostructure could more efficiently separate charges with a lower probability of recombination under visible light irradiation,which made the photoreduction efficiency of CO_(2)to CO be 25.5 and 2.5 times higher than that of CTF and CN,respectively.This investigation is expected to offer a new thought for fabricating high‐efficiency photocatalyst without metal in solar‐energy‐driven CO_(2)reduction.
基金Ministry of Trade,Industry&Energy of Korea,Grant/Award Number:RS‐2022‐00155717National Research Foundation of Korea,Grant/Award Numbers:2020H1D3A1A04081472,2022M3J1A1054323。
文摘Carbon super-heterostructures with high nitrogen contents from the covalent hybrid precursors of covalent triazine frameworks(CTFs)and zeolitic imidazolic frameworks(ZIFs)are scarcely explored because of CTF's ordered structure and toxic superacid that dissolves or destabilizes the metal nodes.To solve this problem,herein,we report a straightforward two-step pathway for the covalent hybridization of disordered CTF(d–CTF)–ZIF composites via preincorporation of an imidazole(IM)linker into ordered CTFs,followed by the imidazole-site-specific covalent growth of ZIFs.Direct carbonization of these synthesized d–CTF−IM−ZIF hybrids results in unique hollow carbon super-heterostructures with ultrahigh nitrogen content(>18.6%),high specific surface area(1663m^(2)g^(−1)),and beneficial trace metal(Co/Zn NPs)contents for promoting the redox pseudocapacitance.As proof of concept,the obtained carbon super-heterostructure(Co–Zn–NC_(SNH)–800)is used as a positive electrode in an asymmetric supercapacitor,demonstrating a remarkable energy density of 61Wh kg^(−1)and extraordinary cyclic stability of 97%retention after 30,000 cycles at the cell level.Our presynthetic modifications of CTF and their covalent hybridization with ZIF crystals pave the way toward new design strategies for synthesizing functional porous carbon materials for promising energy applications.
文摘New fluorine substituted 6-(5’-fluoro-2’-triphenylphosphiniminophenyl) 3-thioxo-1,2,4-triazin-5 (2H, 4H) one (2) was obtained via Wittig’s reaction of the corresponding 6-(5’-fluoro-2’-amino-phenyl)-3-thioxo-1,2,4-triazinone (1). Behavior of compound 2 towards alkylating agents and/or oxidizing agents was studied were, N-hydroxyl (3), Mannich base (4,5), S-alkyl (6,7,8) and thiazolo [3,2-b][1,2,4] triazinones (10-14) and or 3-disulfide (18), 3-sulfonic acid 19 and 1,2,4-triazin-3,5-Dionne (20) derivatives obtained. Structures of the new products are established by elemental and spectral data. The new targets obtained screened as Molluscicidalagents against Biomophlaria Alexandrina snails responsible for Bilharziasis diseases, in compare with Baylucide as standard drug.
基金supported by the National Key R&D Program of China(2016YFB0600901)the Natural Science Foundation of China(grant nos.21536001 and 21606007)
文摘In this work, a 2D covalent triazine-based framework was prepared by using 1,3-dicyanobenzo[c]thiophene（DCBT） as monomer to effectively capture CO. The resulting CTF-DCBT was characterized by FT-IR, XPS, PXRD, elemental analysis, SEM, TEM, and Nadsorption-desorption.The results indicate that CTF-DCBT is partially crystalline and has ultramicropore（6.5 A?） as well as high heteroatom contents（11.24 wt% and 12.61 wt% for N and S, respectively）. In addition, the BET surface area and total pore volume of CTF-DCBT are 500 m/g and 0.26 cm/g, respectively. CTF-DCBT possesses excellent thermal stability（450 °C） and chemical stability towards boiling water, 4 M HCl, and 1 M Na OH.The COadsorption capacity of CTF-DCBT is 37.8 cm/g at 1 bar and 25 °C. After six adsorption-desorption cycles, there is no obvious loss of COuptake observed. Due to the ultramicropore and high heteroatom contents, CTF-DCBT has high isosteric heats of adsorption for COand high selectivities of COover Nand CH. At 25 °C, the CO/Nand CO/CHselectivities are 112.5 and 10.3, respectively, which are higher than those of most POFs. Breakthrough curves indicate that CTF-DCBT could effectively separate CO/Nand CO/CHmixtures.
基金The project was supported by the NNSFC (20572057) and NSF of Shandong Province (Y2006B011)
文摘The crystal structure of the title compound 3-phenyl-6-（4-methylphenyl）-1,2,4- triazolo[4,3-b]-1,2,4-triazine （C17H13N5, Mr = 287.32） was synthesized and determined by singlecrystal X-ray diffraction. It belongs to monoclinic, space group P21/c, with α = 11.4038（18）, b = 11.7675（18）, c = 11.0904（18） A, β = 108.439（7）°, V = 1411.9（4） A^3, Z = 2, Dc = 1.352 g/cm^3, p = 0.085 mm^-1, F（000） = 600, R = 0.0445 and wR = 0.1041 for 2888 unique reflections with 1501 observed ones （I 〉20（I））. In the crystal structure, the triazine moiety is almost coplanar with the triazole ring, and the largest deviation for atom C（4） is -0.026 A. The intermolecular hydrogen bond in the crystal lattice plays an important role in stabilizing the structure.
基金Support of this investigation by Payame Noor University
文摘[Pb（TPT）（μ-I）2PbI2（μ-I）2Pb（TPT）] 1 （TPT is the abbreviation of 3,5,6-tris（2- pyridyl）-1,2,4-triazine ligand） has been synthesized and characterized by elemental analysis, IR, J H- NMR spectroscopy and studied by thermal and electrochemical properties as well as X-ray crystallography. The single-crystal X-ray data show two different kinds of Pb2＋ ions in 1 with coordination numbers of six, Pbl = PbI6, and five, Pb2 = PbN312, with holodirected and hemidirected coordination spheres, respectively. The supramolecular features in 1 are negotiated through the weak but directional Pb...I, C-H...N and C-H...I interactions and aromatic π-π stacking interactions.
基金Supported by the NNSFC (No 20672073)Shanghai Key Laboratory of Thulium Functional Materials (07d222303)
文摘The title compounds,C9H13ClN6O2S 1 and C15H17ClN6O2S 2,were synthesized and structurally characterized by elemental analysis,IR,1H NMR spectra and single-crystal X-ray diffraction.Compound 1 is in the monoclinic system,space group P21/c with a=13.7711（5）,b=10.3883（4）,c=9.7623（2）,V=1344.47（8）3,Dc=1.506 g/cm3,C9H13ClN6O2S,Mr=304.76,F（000）=632,μ=0.448 mm-1,Z=4,S=1.084,R=0.0497 and wR=0.1328 for 2640 unique reflections（Rint=0.0787） with 2089 observed ones（I2σ（I））.Compound 2 belongs to the monoclinic system,space group P21/n with a=8.3828（5）,b=14.5285（7）,c=14.2456（4）,V=1729.74（14）3,Dc=1.462 g/cm3,C15H17ClN6O2S,Mr=380.86,F（000）=792,μ=0.364 mm-1,Z=4,S=1.057,R=0.0598 and wR=0.1582 for 3384 unique reflections（Rint=0.0469） with 2833 observed ones（I2σ（I））.Compounds 1 and 2 are homologues and stabilized by intermolecular and intramolecular hydrogen bonds.Moreover,compound 2 containing C（2）–H（2）…π（thiazole） interaction is more stable than 1.
基金The project was supported by the NNSFC (No. 20572057) and NSF of Shandong Province (No. Y2003B01)
文摘The crystal structure of 3-（5-amino-4-ethoxycarbonyl-3-methylthio-l-H-pyrazolyl）-5-phenyl- 1,2,4-triazine （C16H16N6O2S, Mr = 356.41） has been determined by single-crystal X-ray diffraction. It belongs to monoclinic, space group P2（1/c） with a = 16.961（14）, b = 7.297（6）, c = 13.857（11）A^°, β = 109.803（13）°, V = 2237（2）A^°3, Z = 4, Dc = 1.467 g/cm^3,μ = 0.225 mm^-1, F（000） = 744, R=0.0477 and wR = 0.1156 for 2847 unique reflections with 1713 observed ones （I 〉2σ（I））. X-ray analysis reveals that there exist both intra- and intermolecular hydrogen bonds in the crystal lattice.
基金supported by the Zhejiang Provincial Natural Science Foundation of China (No. LR21E080001)the National Natural Science Foundation of China (Nos. 21876156, 52000158, 22076168)+1 种基金the Zhejiang Provincial Ten Thousand Talent Program (No. 2018R52013)the Key Research and Development Plan of Zhajiang Province (No. 2021C03176)
文摘Herein,a novel direct Z-scheme photocatalyst was accomplished by hybridization of 0D MoS2 quantum dots(MSQDs)and 3D honeycomb-like conjugated triazine polymers(CTP)(namely,CTP-MSQD).The unique 0D/3D hierarchical structure significantly enhanced the exposure of active sites and light harvesting property,while the formed p-n junction enabled the direct strong interface coupling without the necessity of any mediators.The optimized CTP-MSQD3 exhibited continuously increased visible-light-driven photocatalytic activity and strong durability both in Cr(VI)reduction and H2 evolution,featured a rate of 0.069 min^(-1) and 1070μmol/(hr•g),respectively,which were 8 times than those of pure 3D-CTP(0.009 min^(−1) and 129μmol/(hr•g)).We believe that this work provides a promising photocatalyst system that combines a 0D/3D hierarchical structure and a Z-scheme charge flow for efficient and stable photocatalytic conversion.
