Pyridine-based agrochemical products have become the most commercially successful in the 21st century.About half of the agrochemicals with pyridine scaffold were released,registered or invented only in the current mil...Pyridine-based agrochemical products have become the most commercially successful in the 21st century.About half of the agrochemicals with pyridine scaffold were released,registered or invented only in the current millennium.Some of them have a unique structure and previously unknown modes of action.The literature provides examples of the use of the pyridine ring in pesticides for reducing the dosage of the active ingredient,hence to take care of the environment due to their increased efficacy,overcoming the pest resistance,and also makes it possible to create patentable structures by dodging the parent patent,which sometimes leads to a change in the spectrum of activity of the compounds.The newest 13 substances registered by the ISO from January 2021 to June 2024,and not reviewed previously are considered.展开更多
The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions durin...The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions during cycling.Electrolyte additive modification is considered one of the most effective and simplest methods for solving the aforementioned problems.Herein,the pyridine derivatives(PD)including 2,4-dihydroxypyridine(2,4-DHP),2,3-dihydroxypyridine(2,3-DHP),and 2-hydroxypyrdine(2-DHP),were em-ployed as novel electrolyte additives in ZnSO_(4)electrolyte.Both density functional theory calculation and experimental findings demonstrated that the incorporation of PD additives into the electrolyte effectively modulates the solvation structure of hydrated Zn ions,thereby suppressing side reactions in AZIBs.Ad-ditionally,the adsorption of PD molecules on the zinc anode surface contributed to uniform Zn deposi-tion and dendrite growth inhibition.Consequently,a 2,4-DHP-modified Zn/Zn symmetrical cell achieved an extremely long cyclic stability up to 5650 h at 1 mA cm^(-2).Furthermore,the Zn/NH_(4)V_(4)O_(10)full cell with 2,4-DHP-containing electrolyte exhibited an outstanding initial capacity of 204 mAh g^(-1),with a no-table capacity retention of 79%after 1000 cycles at 5 A g^(-1).Hence,this study expands the selection of electrolyte additives for AZIBs,and the working mechanism of PD additives provides new insights for electrolyte modification enabling highly reversible zinc anode.展开更多
The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Cova...The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.展开更多
A series of cyclopropane-1,1-diamide derivatives containing imidazo[1,2-a]pyridine were synthesized.The inhibitory effects of these compounds on FLT3-ITD kinase and their anti-proliferative activities against two acut...A series of cyclopropane-1,1-diamide derivatives containing imidazo[1,2-a]pyridine were synthesized.The inhibitory effects of these compounds on FLT3-ITD kinase and their anti-proliferative activities against two acute myeloid leukemia cell lines expressing FLT3-ITD were evaluated.With focused on the different substitutions of imidazo[1,2-a]pyridine,a preliminary exploration of the structure-activity relationship was conducted for 22 compounds.The results revealed that most compounds exhibited certain inhibitory effects on FLT3-ITD kinase with IC_(50) values below 0.5μmol·L^(-1).Among them,N-(4-fluorophenyl)-N-(4-(7-((2-morpholinoethyl)carbamoyl)imidazo[1,2-a]pyridine-3-carbonyl)phenyl)cyclopropane-1,1-dicarboxamide(12a)demonstrated the most potent FLT3-ITD kinase inhibitory activity and the strongest anti-proliferative effect on the MV4-11 and MOLM-13 cell lines expressing FLT3-ITD with IC50 values of 0.06 and 0.2μmol·L^(-1),respectively.Moreover,compound 12a did not exhibit anti-proliferative activity against cell lines without FLT3 mutations,such as THP-1,HCT-116,A549,HepG2,K562,and MCF-7,and it displayed non-cytotoxicity towards normal human renal tubular epithelial cells(HK-2),human liver progenitor cells(HepaRG),and HEK293(human embryonic kidney cells).Although 12a exhibits inferior inhibitory activity against FLT3-ITD kinase and anti-tumor cell proliferation compared to C abozantinib in this study,it can provide a reference for further research into FLT3-ITD inhibitors.展开更多
Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal s...Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.展开更多
A direct Michael addition reaction between imidazo[1,2-a]pyridines andα,β-unsaturated ketones using acidic alumina as a C(sp3)—H acid catalyst has been developed.The abundant C(sp3)—H acid sites(Al^(3+))on the aci...A direct Michael addition reaction between imidazo[1,2-a]pyridines andα,β-unsaturated ketones using acidic alumina as a C(sp3)—H acid catalyst has been developed.The abundant C(sp3)—H acid sites(Al^(3+))on the acidic alumina surface effectively activate the carbonyl group ofα,β-unsaturated ketones,significantly enhancing the electrophilicity of theβ-carbon and thereby facilitating selective alkylation at the C3 position of imidazo[1,2-a]pyridines.This method demonstrates excellent functional group compatibility,mild reaction conditions,low reagent costs,and operational simplicity,providing a novel strategy for the efficient synthesis of alkylated imidazo[1,2-a]pyridine derivatives.展开更多
As promising high-temperature proton exchange membranes,phosphoric acid(PA)doped polybenzimidazole(PBI)membranes still face challenges,including excessive PA leaching and limited long-term stability.The preparation of...As promising high-temperature proton exchange membranes,phosphoric acid(PA)doped polybenzimidazole(PBI)membranes still face challenges,including excessive PA leaching and limited long-term stability.The preparation of mixed matrix membranes(MMMs)has emerged as a viable strategy to address these limitations,which can combine the excellent mechanical properties of polymers with the structural advantages of porous fillers.Among various filler materials,nitrogen-containing porous organic polymers(POPs)have shown particular promise because of their excellent compatibility with polymers.Therefore,in this work,a new pyridine-based POP called Py-POP was synthesized.Py-POP was mixed with commercial poly[2,2′-(p-oxidiphenylene)-5,5′-benzimidazole](OPBI)to prepare MMMs.Theoretical calculations indicate that the pyridine groups exhibit strong interactions with PA,significantly enhancing both PA retention and proton conduction efficiency.Remarkably,the PA retention rate of the composite membrane doped with 10 wt%Py-POP is 77.2%at 80/40%RH,which is much higher than that of the OPBI(62.7%).Furthermore,the membrane achieves an outstanding proton conductivity of 0.173 S cm^(-1)at 180℃,which is 4.2 times higher than that of the OPBI membrane.The peak power density of the composite membrane can achieve 915.1 mW cm^(-2) and remains at 891.5 mW cm^(-2) after 80 cycles of testing at 180℃.展开更多
Abundant efforts have been devoted to improving the efficiency of organic light-emitting diodes(OLEDs),however,approaches to control the device efficiency roll-off are still extremely limited,especially in nondoped bl...Abundant efforts have been devoted to improving the efficiency of organic light-emitting diodes(OLEDs),however,approaches to control the device efficiency roll-off are still extremely limited,especially in nondoped blue OLEDs.In this work,three blue emitters(TAT,TAMT and TAMT-CN)with"hot exciton"properties are designed and synthesized based on[1,2,4]triazolo[1,5-a]pyridine(TP)as a regulating unit as well as anthracene-triphenylamine(An-TPA)as the chromophore.By adjusting the linkage mode and modifying the TP unit,the excited state properties,carrier transfer abilities,horizontal orientation,and device efficiency roll-off were precisely controlled.Among these materials,emitters that directly connect the fused TP unit exhibit balanced charge-transporting ability,higher photoluminescent quantum yield and improved horizontal orientation,resulting in better electroluminescence(EL)performance in non-doped blue OLEDs.As a result,non-doped blue OLEDs exhibit excellent performance with external quantum efficiencies of over 6%,brightness of over 30,000 cd/m2and EL peaks of around 476 nm.More importantly,the device based on TAMT-CN exhibits an ultra-low efficiency roll-off of 2.97%at a high brightness of10,000 cd/m2.The accessible molecular unit and feasible design strategy in this work are of great significance for designing highly efficient and ultra-low efficiency roll-off non-doped blue OLEDs.展开更多
A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible ...A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible N-(pyridyl)amides could be converted into the products featuring a diverse set of functional groups.The sustainable methodology was successfully applied to the late-stage functionalization of natural products and drugs.展开更多
Designing highly effective cathodic catalysts that can efficiently generate H_(2)O_(2)in situ and promptly convert it to hydroxyl radicals(·OH)poses a significant challenge within the heterogeneous electro-Fenton...Designing highly effective cathodic catalysts that can efficiently generate H_(2)O_(2)in situ and promptly convert it to hydroxyl radicals(·OH)poses a significant challenge within the heterogeneous electro-Fenton(EF)systems.Herein,we fabricate a bifunctional core-shell catalyst featuring Co^(0)species encapsulated within N,P-codoped carbon shells through a hydrothermal-pyrolysis strategy,utilizing bamboo shoots as biomass-derived precursors.Density functional theory(DFT)calculations elucidate that the protonation of pyridinic nitrogen modifies the adsorption energy of the OOH*intermediate,positioning it optimally at the peak(3.81 eV)on the twoelectron oxygen reduction reaction(2e-ORR)volcano plot,thereby significantly boosting H_(2)O_(2)production.Moreover,the Co^(0)species embedded within the catalyst function as electron donors,catalyzing the activation of H_(2)O_(2)to produce·OH by efficiently facilitating the transfer of electrons to Fe^(3+).Consequently,the synthesized catalyst exhibits a minimum electron transfer number of 2.06 and a maximum H_(2)O_(2)selectivity of 97.4%.Moreover,the degradation for the methylene blue solution exceeds 95%within 15 min,with only an 11.3%reduction in degradation efficiency after 180 min of continuous operation(9 cycles).This bifunctional catalyst design provides valuable insights that can accelerate the development of EF-based degradation systems.展开更多
The monoaminotrinitro iron phthalocyanine(FeMATNPc)is used to connect with isonicotinic acid(INA)for amide bonding and axial coordination to synthetic a unique catalyst FeMATNPc-INA,which is loaded in polyacrylonitril...The monoaminotrinitro iron phthalocyanine(FeMATNPc)is used to connect with isonicotinic acid(INA)for amide bonding and axial coordination to synthetic a unique catalyst FeMATNPc-INA,which is loaded in polyacrylonitrile(PAN)nanofibers by electrospinning.The introduction of INA destroys theπ-πconjugated stack structure in phthalocyanine molecules and exposes more active sites.The FeMATNPc-INA structure is characterized by X-ray photoelectron spectroscopy and UV-visible absorption spectrum,and the FeMATNPcINA/PAN structure is characterized by Fourier transform infrared spectroscopy and X-ray diffraction.The FeMATNPc-INA/PAN can effectively activate peroxymonosulfate(PMS)to eliminate carbamazepine(CBZ)within 40 minutes(PMS 1.5 mmol/L)in the dark.The effects of catalyst dosage,PMS concentration,pH and inorganic anion on the degradation of CBZ are investigated.It has been confirmed by electron paramagnetic resonance,gas chromatography–mass spectroscopy and free radical capture experiments that the catalytic system is degraded by·OH,SO4^(·-)and Fe(IV)=O are the major active species,the singlet oxygen(^(1)O_(2))is the secondary active species.The degradation process of CBZ is analyzed by ultra-high performance liquid chromatography-mass spectrometry and the aromatic compounds have been degraded to small molecular acids.展开更多
Sb-based materials exhibit considerable potential for sodium-ion storage owing to their high theoretica capacities.However,the bulk properties of Sb-based materials always result in poor cycling and rate performances....Sb-based materials exhibit considerable potential for sodium-ion storage owing to their high theoretica capacities.However,the bulk properties of Sb-based materials always result in poor cycling and rate performances.To overcome these issues,pyridine-regulated Sb@InSbS_(3)ultrafine nanoplates loaded on reduced graphene oxides(Sb@InSbS_(3)@rGO)were designed and synthesized.During the synthesis process,pyridine was initially adopted to coordinate with In^(3+),and uniformly dispersed In_(2)S_(3)ultrafine nanoplates on reduced graphene oxide were generated after sulfidation.Next,partial In^(3+)was exchanged with Sb^(3+),and Sb@InSbS_(3)@rGO was obtained by using the subsequent annealing method.The unique structure of Sb@InSbS_(3)@rGO effectively shortened the transfer path of sodium ions and electrons and provided a high pseudocapacitance.As the anode in sodium-ion batteries,the Sb@InSbS_(3)@rGO electrode demonstrated a significantly higher reversible capacity better stability(445 m Ah·g^(-1)at 0.1 A·g^(-1)after 200 cycles and 212 mAh·g^(-1)at 2 A·g^(-1)after 1200 cycles),and superior rate(210 mAh·g^(-1)at 6.4 A·g^(-1))than the electrode without pyridine(355 mAh·g-1at 0.1 A·g-1after 55 cycles and 109 mAh·g^(-1)at 2 A·g^(-1)after 770 cycles)Furthermore,full cells were assembled by using the Sb@InSbS_(3)@rGO as anode and Na_(3)V_(2)(PO_(4))_(3)as cathode which demonstrated good cycling and rate performances and exhibited promising application prospects.These results indicate that adjusting the microstructure of electrode materials through coordination balance is A·good strategy for obtaining high-capacity,high-rate,and longcycle sodium storage performances.展开更多
Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,...Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.展开更多
The reactivity and stability of seventeen (17) imidazo [1,2-a]pyridine N-acylhydrazone derivatives were investigated using density functional theory at the B3LYP/6-31+ G (d, p) level. Analysis of the molecular electro...The reactivity and stability of seventeen (17) imidazo [1,2-a]pyridine N-acylhydrazone derivatives were investigated using density functional theory at the B3LYP/6-31+ G (d, p) level. Analysis of the molecular electrostatic potential (MEP) and determination of the dual descriptor revealed that in most cases, the nitrogen atoms of the 6-πelectron conjugation, the oxygen, and the sulfur atom are nucleophilic site. Chemical reactivity of the compounds was assessed through analysis of frontier molecular orbitals (HOMO and LUMO), energy gap (Δℰ), chemical hardness (η), and the softness (S). Consequently, the compound 9e exhibited the lowest reactivity, least electron donating, and the highest stability. This comprehensive study offers valuable insights into the chemical behavior of these derivatives, crucial for further exploration and potential applications.展开更多
The three-component reaction of aromatic aldehyde,malononitrile and aliphatic amine in a mixed solvent of methanol and water exhibited very interesting molecular diversity and gave the derivatives of polysubstituted N...The three-component reaction of aromatic aldehyde,malononitrile and aliphatic amine in a mixed solvent of methanol and water exhibited very interesting molecular diversity and gave the derivatives of polysubstituted N-methyldihydropyridines,2-dialkylaminopyridines and 2-methoxypyridines as main products according to the structure of aliphatic amines used.展开更多
Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this ...Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this research,we propose a“self‐assembly‐template”method to prepare B,N codoped porous carbon(BN‐C)with a nanosandwich structure and abundant pyridinic N‐B species.The nanosandwich structure can increase powder density and cycle stability by constructing a stable solid electrolyte interphase film,shortening the Li^(+) diffusion pathway,and accommodating volume expansion during repeated charging/discharging.The abundant pyridinic N‐B species can simultaneously promote the adsorption/desorption of Li^(+)/PF_(6)^(−) and reduce the diffusion barrier.The BN‐C electrode showed a high lithium‐ion storage capacity of above 1140 mAh g^(−1) at 0.05 A g^(−1) and superior stability(96.5% retained after 2000 cycles).Moreover,owing to the synergistic effect of the nanosandwich structure and pyridinic N‐B species,the assembled symmetrical BN‐C//BN‐C full cell shows a high energy density of 234.7Wh kg^(−1),high power density of 39.38 kW kg−1,and excellent cycling stability,superior to most of the other cells reported in the literature.As the density functional theory simulation demonstrated,pyridinic N‐B shows enhanced adsorption activity for Li^(+) and PF_(6)^(−),which promotes an increase in the capacity of the anode and cathode,respectively.Meanwhile,the relatively lower diffusion barrier of pyridinic N‐B promotes Li^(+) migration,resulting in good rate performance.Therefore,this study provides a new approach for the synergistic modulation of a nanostructure and an active site simultaneously to fabricate the carbon electrode material in energy storage devices.展开更多
A rapid and simple procedure for synthesis of 2,6-di（naphthalene thioureido carbamino）pyridine fluorescine anion acceptor by the reaction between pyridine-2,6-dicarbohydrazide obtained from 2,6-dimethylpyridine afte...A rapid and simple procedure for synthesis of 2,6-di（naphthalene thioureido carbamino）pyridine fluorescine anion acceptor by the reaction between pyridine-2,6-dicarbohydrazide obtained from 2,6-dimethylpyridine after three-step reaction and 1-napbthyl isothiocyanate is described, and all reactions could be carried out under microwave heating condition.展开更多
A new kind of aromatic diamine monomer containing pyridine unit,2,6-bis[4-(4-aminophenoxy)phenoxy]pyridine(BAPP),was synthesized in three steps,using hydroquinone as starting material.A novel pyridine-containing polyi...A new kind of aromatic diamine monomer containing pyridine unit,2,6-bis[4-(4-aminophenoxy)phenoxy]pyridine(BAPP),was synthesized in three steps,using hydroquinone as starting material.A novel pyridine-containing polyimide was prepared from the resulting diamine BAPP with 4,4 -oxydiphthalic anhydride(ODPA) via a conventional two-step thermal imidization method.The resulting polyimide exhibits excellent solubility,film-forming capability and high thermal resistance.展开更多
This research took 2,6-dimethylpyridine as raw materials under microwave irradiation to syntheses pyridine 2,6-dicarboxylic acid by adding oxidation potassium permanganate. However, there are lots of factors affecting...This research took 2,6-dimethylpyridine as raw materials under microwave irradiation to syntheses pyridine 2,6-dicarboxylic acid by adding oxidation potassium permanganate. However, there are lots of factors affecting the yield including the amount of potassium permanganate and sulfuric acid, reaction time, power, 2,6-dimethylpyridine dosage. We made the further research, using orthogonal experiment to find the optimal process conditions. Thus our research changed the synthesis process from a traditional method to a new type of microwave technology.展开更多
文摘Pyridine-based agrochemical products have become the most commercially successful in the 21st century.About half of the agrochemicals with pyridine scaffold were released,registered or invented only in the current millennium.Some of them have a unique structure and previously unknown modes of action.The literature provides examples of the use of the pyridine ring in pesticides for reducing the dosage of the active ingredient,hence to take care of the environment due to their increased efficacy,overcoming the pest resistance,and also makes it possible to create patentable structures by dodging the parent patent,which sometimes leads to a change in the spectrum of activity of the compounds.The newest 13 substances registered by the ISO from January 2021 to June 2024,and not reviewed previously are considered.
基金supported by the Key Science and Technol-ogy Program of Henan Province(No.232102241020)the Ph.D.Research Startup Foundation of Henan University of Science and Technology(No.400613480015)+1 种基金the Postdoctoral Research Startup Foundation of Henan University of Science and Technology(No.400613554001)the Natural Science Foundation of Henan Province(242300420021).
文摘The poor reversibility and stability of Zn anodes greatly restrict the practical application of aqueous Zn-ion batteries(AZIBs),resulting from the uncontrollable dendrite growth and H_(2)O-induced side reactions during cycling.Electrolyte additive modification is considered one of the most effective and simplest methods for solving the aforementioned problems.Herein,the pyridine derivatives(PD)including 2,4-dihydroxypyridine(2,4-DHP),2,3-dihydroxypyridine(2,3-DHP),and 2-hydroxypyrdine(2-DHP),were em-ployed as novel electrolyte additives in ZnSO_(4)electrolyte.Both density functional theory calculation and experimental findings demonstrated that the incorporation of PD additives into the electrolyte effectively modulates the solvation structure of hydrated Zn ions,thereby suppressing side reactions in AZIBs.Ad-ditionally,the adsorption of PD molecules on the zinc anode surface contributed to uniform Zn deposi-tion and dendrite growth inhibition.Consequently,a 2,4-DHP-modified Zn/Zn symmetrical cell achieved an extremely long cyclic stability up to 5650 h at 1 mA cm^(-2).Furthermore,the Zn/NH_(4)V_(4)O_(10)full cell with 2,4-DHP-containing electrolyte exhibited an outstanding initial capacity of 204 mAh g^(-1),with a no-table capacity retention of 79%after 1000 cycles at 5 A g^(-1).Hence,this study expands the selection of electrolyte additives for AZIBs,and the working mechanism of PD additives provides new insights for electrolyte modification enabling highly reversible zinc anode.
基金supported by the National Natural Science Foundation of China(Nos.22375031,22202037,22472023)the Fundamental Research Funds for the Central Universities(Nos.2412023YQ001,2412023QD019,2412024QD014)+1 种基金supported by grants from the seventh batch of Jilin Province Youth Science and Technology Talent Lifting Project(No.QT202305)Science and Technology Development Plan Project of Jilin Province,China(No.20240101192JC)。
文摘The light-driven CO_(2)reduction reaction(CO_(2)RR)to CO is a very effective way to address global warming.To avoid competition with water photolysis,metal-free gas-solid CO_(2)RR catalysts should be investigated.Covalent organic frameworks(COFs)offer a promising approach for CO_(2)transformation but lack high efficiency and selectivity in the absence of metals.Here,we have incorporated a pyridine nitrogen component into the imine-COF conjugated structure(Tp Pym).This innovative system has set a record of producing a CO yield of 1565μmol g^(-1)within 6 h.The soft X-ray absorption fine structure measurement proves that Tp Pym has both better conjugation and electron cloud enrichment.The electronic structure distribution delays the charge-carrier recombination,as evidenced by femtosecond transient absorption spectroscopy.The energy band diagram and theoretical calculation show that the conduction-band potential of Tp Pym is lower and the reduction reaction of CO_(2)to CO is more likely to occur.
文摘A series of cyclopropane-1,1-diamide derivatives containing imidazo[1,2-a]pyridine were synthesized.The inhibitory effects of these compounds on FLT3-ITD kinase and their anti-proliferative activities against two acute myeloid leukemia cell lines expressing FLT3-ITD were evaluated.With focused on the different substitutions of imidazo[1,2-a]pyridine,a preliminary exploration of the structure-activity relationship was conducted for 22 compounds.The results revealed that most compounds exhibited certain inhibitory effects on FLT3-ITD kinase with IC_(50) values below 0.5μmol·L^(-1).Among them,N-(4-fluorophenyl)-N-(4-(7-((2-morpholinoethyl)carbamoyl)imidazo[1,2-a]pyridine-3-carbonyl)phenyl)cyclopropane-1,1-dicarboxamide(12a)demonstrated the most potent FLT3-ITD kinase inhibitory activity and the strongest anti-proliferative effect on the MV4-11 and MOLM-13 cell lines expressing FLT3-ITD with IC50 values of 0.06 and 0.2μmol·L^(-1),respectively.Moreover,compound 12a did not exhibit anti-proliferative activity against cell lines without FLT3 mutations,such as THP-1,HCT-116,A549,HepG2,K562,and MCF-7,and it displayed non-cytotoxicity towards normal human renal tubular epithelial cells(HK-2),human liver progenitor cells(HepaRG),and HEK293(human embryonic kidney cells).Although 12a exhibits inferior inhibitory activity against FLT3-ITD kinase and anti-tumor cell proliferation compared to C abozantinib in this study,it can provide a reference for further research into FLT3-ITD inhibitors.
文摘Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.
文摘A direct Michael addition reaction between imidazo[1,2-a]pyridines andα,β-unsaturated ketones using acidic alumina as a C(sp3)—H acid catalyst has been developed.The abundant C(sp3)—H acid sites(Al^(3+))on the acidic alumina surface effectively activate the carbonyl group ofα,β-unsaturated ketones,significantly enhancing the electrophilicity of theβ-carbon and thereby facilitating selective alkylation at the C3 position of imidazo[1,2-a]pyridines.This method demonstrates excellent functional group compatibility,mild reaction conditions,low reagent costs,and operational simplicity,providing a novel strategy for the efficient synthesis of alkylated imidazo[1,2-a]pyridine derivatives.
基金the Natural Science Foundation of Gansu Province(No.24JRRA391).
文摘As promising high-temperature proton exchange membranes,phosphoric acid(PA)doped polybenzimidazole(PBI)membranes still face challenges,including excessive PA leaching and limited long-term stability.The preparation of mixed matrix membranes(MMMs)has emerged as a viable strategy to address these limitations,which can combine the excellent mechanical properties of polymers with the structural advantages of porous fillers.Among various filler materials,nitrogen-containing porous organic polymers(POPs)have shown particular promise because of their excellent compatibility with polymers.Therefore,in this work,a new pyridine-based POP called Py-POP was synthesized.Py-POP was mixed with commercial poly[2,2′-(p-oxidiphenylene)-5,5′-benzimidazole](OPBI)to prepare MMMs.Theoretical calculations indicate that the pyridine groups exhibit strong interactions with PA,significantly enhancing both PA retention and proton conduction efficiency.Remarkably,the PA retention rate of the composite membrane doped with 10 wt%Py-POP is 77.2%at 80/40%RH,which is much higher than that of the OPBI(62.7%).Furthermore,the membrane achieves an outstanding proton conductivity of 0.173 S cm^(-1)at 180℃,which is 4.2 times higher than that of the OPBI membrane.The peak power density of the composite membrane can achieve 915.1 mW cm^(-2) and remains at 891.5 mW cm^(-2) after 80 cycles of testing at 180℃.
基金the financial support from the National Natural Science Foundation of China(Nos.52273187 and 51973107)the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2019(No.GDUPS2019)。
文摘Abundant efforts have been devoted to improving the efficiency of organic light-emitting diodes(OLEDs),however,approaches to control the device efficiency roll-off are still extremely limited,especially in nondoped blue OLEDs.In this work,three blue emitters(TAT,TAMT and TAMT-CN)with"hot exciton"properties are designed and synthesized based on[1,2,4]triazolo[1,5-a]pyridine(TP)as a regulating unit as well as anthracene-triphenylamine(An-TPA)as the chromophore.By adjusting the linkage mode and modifying the TP unit,the excited state properties,carrier transfer abilities,horizontal orientation,and device efficiency roll-off were precisely controlled.Among these materials,emitters that directly connect the fused TP unit exhibit balanced charge-transporting ability,higher photoluminescent quantum yield and improved horizontal orientation,resulting in better electroluminescence(EL)performance in non-doped blue OLEDs.As a result,non-doped blue OLEDs exhibit excellent performance with external quantum efficiencies of over 6%,brightness of over 30,000 cd/m2and EL peaks of around 476 nm.More importantly,the device based on TAMT-CN exhibits an ultra-low efficiency roll-off of 2.97%at a high brightness of10,000 cd/m2.The accessible molecular unit and feasible design strategy in this work are of great significance for designing highly efficient and ultra-low efficiency roll-off non-doped blue OLEDs.
基金financial support from the National Natural Science Foundation of China(No.82003585)the Program for Science&Technology Innovation Talents in Universities of Henan Province(No.24HASTIT069)+5 种基金the Technical Innovation Team of Henan Normal University(No.2022TD03)the Special Project for Fundamental Research in University of Henan Province(No.23ZX009)the Henan Science and Technology Program(No.232102310364)the Key Project of Henan Educational Committee(No.22A150041)Excellent Youth Foundation of Henan Scientific Committee(No.222300420012)the Young Core Instructor Training Program of Xinyang Agriculture and Forestry University(2023)。
文摘A transition-metal-and oxidant-free amination/cyclization reaction to access 1,2,4-triazolo[1,5-a]pyridines was realized in water by using amino diphenylphosphinate as amino source.A broad array of readily accessible N-(pyridyl)amides could be converted into the products featuring a diverse set of functional groups.The sustainable methodology was successfully applied to the late-stage functionalization of natural products and drugs.
基金financially supported by the National Natural Science Foundation of China(Nos.52402249 and 52302288)the China Postdoctoral Science Foundation(No.2021M690930)+1 种基金the Key Scientific Research Project of Henan Province Higher Education of China(Nos.23A430005 and 24A430023)Songshan Lake Materials Laboratory(SLAB)grant(No.260842082)
文摘Designing highly effective cathodic catalysts that can efficiently generate H_(2)O_(2)in situ and promptly convert it to hydroxyl radicals(·OH)poses a significant challenge within the heterogeneous electro-Fenton(EF)systems.Herein,we fabricate a bifunctional core-shell catalyst featuring Co^(0)species encapsulated within N,P-codoped carbon shells through a hydrothermal-pyrolysis strategy,utilizing bamboo shoots as biomass-derived precursors.Density functional theory(DFT)calculations elucidate that the protonation of pyridinic nitrogen modifies the adsorption energy of the OOH*intermediate,positioning it optimally at the peak(3.81 eV)on the twoelectron oxygen reduction reaction(2e-ORR)volcano plot,thereby significantly boosting H_(2)O_(2)production.Moreover,the Co^(0)species embedded within the catalyst function as electron donors,catalyzing the activation of H_(2)O_(2)to produce·OH by efficiently facilitating the transfer of electrons to Fe^(3+).Consequently,the synthesized catalyst exhibits a minimum electron transfer number of 2.06 and a maximum H_(2)O_(2)selectivity of 97.4%.Moreover,the degradation for the methylene blue solution exceeds 95%within 15 min,with only an 11.3%reduction in degradation efficiency after 180 min of continuous operation(9 cycles).This bifunctional catalyst design provides valuable insights that can accelerate the development of EF-based degradation systems.
基金supported by National Natural Science Foundation of China (No.22006136)。
文摘The monoaminotrinitro iron phthalocyanine(FeMATNPc)is used to connect with isonicotinic acid(INA)for amide bonding and axial coordination to synthetic a unique catalyst FeMATNPc-INA,which is loaded in polyacrylonitrile(PAN)nanofibers by electrospinning.The introduction of INA destroys theπ-πconjugated stack structure in phthalocyanine molecules and exposes more active sites.The FeMATNPc-INA structure is characterized by X-ray photoelectron spectroscopy and UV-visible absorption spectrum,and the FeMATNPcINA/PAN structure is characterized by Fourier transform infrared spectroscopy and X-ray diffraction.The FeMATNPc-INA/PAN can effectively activate peroxymonosulfate(PMS)to eliminate carbamazepine(CBZ)within 40 minutes(PMS 1.5 mmol/L)in the dark.The effects of catalyst dosage,PMS concentration,pH and inorganic anion on the degradation of CBZ are investigated.It has been confirmed by electron paramagnetic resonance,gas chromatography–mass spectroscopy and free radical capture experiments that the catalytic system is degraded by·OH,SO4^(·-)and Fe(IV)=O are the major active species,the singlet oxygen(^(1)O_(2))is the secondary active species.The degradation process of CBZ is analyzed by ultra-high performance liquid chromatography-mass spectrometry and the aromatic compounds have been degraded to small molecular acids.
基金supported by the National Natural Science Foundation of China(Nos.42007138,51772082 and 51804106)the Natural Science Foundation of Hunan Province(No.2023JJ10005).
文摘Sb-based materials exhibit considerable potential for sodium-ion storage owing to their high theoretica capacities.However,the bulk properties of Sb-based materials always result in poor cycling and rate performances.To overcome these issues,pyridine-regulated Sb@InSbS_(3)ultrafine nanoplates loaded on reduced graphene oxides(Sb@InSbS_(3)@rGO)were designed and synthesized.During the synthesis process,pyridine was initially adopted to coordinate with In^(3+),and uniformly dispersed In_(2)S_(3)ultrafine nanoplates on reduced graphene oxide were generated after sulfidation.Next,partial In^(3+)was exchanged with Sb^(3+),and Sb@InSbS_(3)@rGO was obtained by using the subsequent annealing method.The unique structure of Sb@InSbS_(3)@rGO effectively shortened the transfer path of sodium ions and electrons and provided a high pseudocapacitance.As the anode in sodium-ion batteries,the Sb@InSbS_(3)@rGO electrode demonstrated a significantly higher reversible capacity better stability(445 m Ah·g^(-1)at 0.1 A·g^(-1)after 200 cycles and 212 mAh·g^(-1)at 2 A·g^(-1)after 1200 cycles),and superior rate(210 mAh·g^(-1)at 6.4 A·g^(-1))than the electrode without pyridine(355 mAh·g-1at 0.1 A·g-1after 55 cycles and 109 mAh·g^(-1)at 2 A·g^(-1)after 770 cycles)Furthermore,full cells were assembled by using the Sb@InSbS_(3)@rGO as anode and Na_(3)V_(2)(PO_(4))_(3)as cathode which demonstrated good cycling and rate performances and exhibited promising application prospects.These results indicate that adjusting the microstructure of electrode materials through coordination balance is A·good strategy for obtaining high-capacity,high-rate,and longcycle sodium storage performances.
文摘Three coordination polymers[Mn(epda)(2,2'⁃bipy)(H_(2)O)](1),[Mn(epda)(phen)](2),and[Co_(2)(epda)2(bpe)2(H_(2)O)_(4)]·5H_(2)O(3)(H2epda=5⁃ethyl⁃pyridine⁃2,3⁃dicarboxylic acid,2,2'⁃bipy=2,2'⁃bipyridine,phen=phenanthroline,bpe=1,2⁃bis(4⁃pyridyl)ethylene)were synthesized by solvothermal reactions and characterized by single⁃crystal X⁃ray diffraction,thermogravimetric analyses,IR spectroscopy and elemental analysis.1 displays a 1D chain struc⁃ture,and these chains are joined by O-H…O hydrogen bonding andπ⁃πstacking interactions to generate a 2D layer structure.2 displays a 2D layer structure,and adjacent layers are generated 3D architecture throughπ⁃πstacking interactions.3 displays a 1D chain structure,and adjacent chains are generated double layer structure through O-H…O hydrogen bonding.The fluorescent properties of 1 and 3 indicate that they can potentially be used as a luminescent sensor.1 was highly selective and sensitive towards o⁃nitrophenol through different detection mechanisms,however,3 was highly selective and sensitive towards 2,4,6⁃trinitrophenol.In addition,the magnetic behavior of 2 has also been investigated.CCDC:2172533,1,2355773,2,2355774,3.
文摘The reactivity and stability of seventeen (17) imidazo [1,2-a]pyridine N-acylhydrazone derivatives were investigated using density functional theory at the B3LYP/6-31+ G (d, p) level. Analysis of the molecular electrostatic potential (MEP) and determination of the dual descriptor revealed that in most cases, the nitrogen atoms of the 6-πelectron conjugation, the oxygen, and the sulfur atom are nucleophilic site. Chemical reactivity of the compounds was assessed through analysis of frontier molecular orbitals (HOMO and LUMO), energy gap (Δℰ), chemical hardness (η), and the softness (S). Consequently, the compound 9e exhibited the lowest reactivity, least electron donating, and the highest stability. This comprehensive study offers valuable insights into the chemical behavior of these derivatives, crucial for further exploration and potential applications.
基金Supported by the National Natural Science Foundation of China(No.20972132)
文摘The three-component reaction of aromatic aldehyde,malononitrile and aliphatic amine in a mixed solvent of methanol and water exhibited very interesting molecular diversity and gave the derivatives of polysubstituted N-methyldihydropyridines,2-dialkylaminopyridines and 2-methoxypyridines as main products according to the structure of aliphatic amines used.
基金Jiangsu Key Lab of Biomass Energy and Material,Grant/Award Number:JSBEMS‐202101National Natural Science Foundation of China,Grant/Award Numbers:51902162,51902162+4 种基金National Key R&D Program of China,Grant/Award Number:2022YFB4201904Foundation of Jiangsu Key Lab of Biomass Energy and Material,Grant/Award Number:JSBEM‐S‐202101National Key R&D Program,Grant/Award Number:2022YFB4201904Jiangsu Co‐Innovation Center of Efficient Processing and Utilization of Forest Resources,the International Innovation Center for Forest Chemicals and Materialsanjing Forestry University。
文摘Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this research,we propose a“self‐assembly‐template”method to prepare B,N codoped porous carbon(BN‐C)with a nanosandwich structure and abundant pyridinic N‐B species.The nanosandwich structure can increase powder density and cycle stability by constructing a stable solid electrolyte interphase film,shortening the Li^(+) diffusion pathway,and accommodating volume expansion during repeated charging/discharging.The abundant pyridinic N‐B species can simultaneously promote the adsorption/desorption of Li^(+)/PF_(6)^(−) and reduce the diffusion barrier.The BN‐C electrode showed a high lithium‐ion storage capacity of above 1140 mAh g^(−1) at 0.05 A g^(−1) and superior stability(96.5% retained after 2000 cycles).Moreover,owing to the synergistic effect of the nanosandwich structure and pyridinic N‐B species,the assembled symmetrical BN‐C//BN‐C full cell shows a high energy density of 234.7Wh kg^(−1),high power density of 39.38 kW kg−1,and excellent cycling stability,superior to most of the other cells reported in the literature.As the density functional theory simulation demonstrated,pyridinic N‐B shows enhanced adsorption activity for Li^(+) and PF_(6)^(−),which promotes an increase in the capacity of the anode and cathode,respectively.Meanwhile,the relatively lower diffusion barrier of pyridinic N‐B promotes Li^(+) migration,resulting in good rate performance.Therefore,this study provides a new approach for the synergistic modulation of a nanostructure and an active site simultaneously to fabricate the carbon electrode material in energy storage devices.
文摘A rapid and simple procedure for synthesis of 2,6-di（naphthalene thioureido carbamino）pyridine fluorescine anion acceptor by the reaction between pyridine-2,6-dicarbohydrazide obtained from 2,6-dimethylpyridine after three-step reaction and 1-napbthyl isothiocyanate is described, and all reactions could be carried out under microwave heating condition.
基金support from the Research Foundation of the State Key Laboratory of Applied Organic Chemistry
文摘A new kind of aromatic diamine monomer containing pyridine unit,2,6-bis[4-(4-aminophenoxy)phenoxy]pyridine(BAPP),was synthesized in three steps,using hydroquinone as starting material.A novel pyridine-containing polyimide was prepared from the resulting diamine BAPP with 4,4 -oxydiphthalic anhydride(ODPA) via a conventional two-step thermal imidization method.The resulting polyimide exhibits excellent solubility,film-forming capability and high thermal resistance.
文摘This research took 2,6-dimethylpyridine as raw materials under microwave irradiation to syntheses pyridine 2,6-dicarboxylic acid by adding oxidation potassium permanganate. However, there are lots of factors affecting the yield including the amount of potassium permanganate and sulfuric acid, reaction time, power, 2,6-dimethylpyridine dosage. We made the further research, using orthogonal experiment to find the optimal process conditions. Thus our research changed the synthesis process from a traditional method to a new type of microwave technology.
