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
In this paper we describe a convernient method for the synthesis of 3, 6-diphenyl-5-phenylamino-1, 2, 4-triazines in good yields, The unreported triazines were identified by elemental analysis, infrared and mass spectra.
The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalyt...The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center.Therefore,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks.However,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application.Herein,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)ORR.Compared with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by 1000-fold.As a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction pathways.This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR.展开更多
Heterojunction engineering is considered as one of the most effective methods to improve the hydrogen production performance of photocatalysts.In this study,a green,simple and gentle method was used to deposit tiny Ni...Heterojunction engineering is considered as one of the most effective methods to improve the hydrogen production performance of photocatalysts.In this study,a green,simple and gentle method was used to deposit tiny Ni S onto CTF-ES_(200)under xenon lamp irradiation to form heterostructures.The experimental results show that the hydrogen production rate of the synthesized Ni S/CTF-ES_(200)is as high as 22.98mmol g^(-1)h^(-1),showing a higher photocatalytic hydrogen production rate compared to other Ni S-loaded nonmetallic semiconductor materials,which is also much higher than that of pure CTF-ES_(200).The interface electric field(IEF)in this p-n heterojunction leads to an accumulation of photoelectrons on the conduction band of CTF-ES_(200),which makes CTF-ES_(200)to keep a high reductiveness for the hydrogen evolution reaction(HER),and significantly improve the separation efficiency of photoelectrons and holes.Furthermore,XPS and EXAFS data show that an efficient electron transport channel is constructed through the formation of Ni-N bond,which further accelerates the interface carrier transport efficiency.This study provides an effective idea for the preparation of highly efficient heterojunction photocatalysts.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.
文摘In this paper we describe a convernient method for the synthesis of 3, 6-diphenyl-5-phenylamino-1, 2, 4-triazines in good yields, The unreported triazines were identified by elemental analysis, infrared and mass spectra.
基金the financial support by the National Natural Science Foundation of China(Nos.22205124,52172206)Natural Science Foundation of Shandong province(Nos.ZR2021QB070,ZR2023QB110)+2 种基金Basic Research Projects for the Pilot Project of Integrating Science and Education and Industry of Qilu University of Technology(Shandong Academy of Sciences)(Nos.2023PY024,2023PX108)Special Fund for Taishan Scholars Projectthe Development Plan of Youth Innovation Team in Colleges and Universities of Shandong Province。
文摘The high conductivity of electrocatalyst can eliminate the Schottky energy barrier at the interface of heterogeneous phases during an electrocatalytic reaction and accelerate the rapid electron transfer to the catalytic active center.Therefore,the electronic conductivity is a vital parameter for oxygen reduction reaction(ORR).Covalent triazine frameworks(CTFs)have shown great potential application as electrocatalysts in ORR with a merit of the diverse building blocks.However,the intrinsic low conductivity and high impedance of CTFs could be significant setbacks in electrocatalytic application.Herein,CTFs were constructed by introducing F and N co-modification for efficient 2e^(-)ORR.Compared with the pristine CTF,the co-presence of F,N could increase the conductivity obviously by 1000-fold.As a result,F-N-CTF exhibits enhanced catalytic performance of H_(2)O_(2)generation and selectivity towards reaction pathways.This work reveals the importance of conductivity optimization for CTFs and provides guidance for designing high conductivity non-metallic organic semiconductor catalysts for 2e^(-)ORR.
基金financially supported by the National Natural Science Foundation of China(No.22271022)the Science and Technology Development Planning of Jilin Province(No.YDZJ202201ZYTS342)supported by the China Scholarship Council(CSC,No.201802335014)。
文摘Heterojunction engineering is considered as one of the most effective methods to improve the hydrogen production performance of photocatalysts.In this study,a green,simple and gentle method was used to deposit tiny Ni S onto CTF-ES_(200)under xenon lamp irradiation to form heterostructures.The experimental results show that the hydrogen production rate of the synthesized Ni S/CTF-ES_(200)is as high as 22.98mmol g^(-1)h^(-1),showing a higher photocatalytic hydrogen production rate compared to other Ni S-loaded nonmetallic semiconductor materials,which is also much higher than that of pure CTF-ES_(200).The interface electric field(IEF)in this p-n heterojunction leads to an accumulation of photoelectrons on the conduction band of CTF-ES_(200),which makes CTF-ES_(200)to keep a high reductiveness for the hydrogen evolution reaction(HER),and significantly improve the separation efficiency of photoelectrons and holes.Furthermore,XPS and EXAFS data show that an efficient electron transport channel is constructed through the formation of Ni-N bond,which further accelerates the interface carrier transport efficiency.This study provides an effective idea for the preparation of highly efficient heterojunction photocatalysts.
