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
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
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
Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed met...Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed metal ion environments.Herein,a new synergistic solvent extraction(SSX)system comprised of a novel pyridine analog,N,N-bis(pyridin-2-ylmethyl)dodecan-1-amine(BPMDA),and dinonylnaphthalene sulfonic acid(DNNSA)with tributyl phosphate as phase modifier is introduced.The SSX system demonstrates high extraction performance achieving>90%for Ni and>97%for Co in a singlestage extraction process,with high selectivity.Under optimal conditions,the selectivity sequence is observed as Co^(2+)(>97%)>Ni^(2+)(>90%)>Mn^(2+)(<20%)>Fe^(3+)(<10%)>Mg^(2+)(<5%)>Al^(3+)(<2%)>Ca^(2+)(<1%).Spectroscopic analysis evidences the preferential binding of BPMDA with Ni and Co in the presence of DNNSA,concurrently achieving a significant reduction in the co-extraction of Fe(Ⅲ)and Al.The selective complexation of Ni and Co using the SSX system offers a highly efficient and selective approach for their extraction,with promising potential for applications in recovery-based processes.展开更多
Polyvinyl chloride is the most widely used general-purpose plastic and plays a vital role in various industries.Mercury-based catalysts severely limit the green sustainability of industry.Non-metallic carbon materials...Polyvinyl chloride is the most widely used general-purpose plastic and plays a vital role in various industries.Mercury-based catalysts severely limit the green sustainability of industry.Non-metallic carbon materials are very promising alternatives in acetylene hydrochlorination,but their stability remains a challenge of major concern at present.Based on the principle of green chemistry,structurally tunable and defect-rich carbon materials were synthesized by hydrothermal carbonization and pyrolysis using glucose as carbon source and m-phenylenediamine as nitrogen source and cross-linking agent.Experimental characterization and density functional theory confirmed that pyridinic N was the main active site.The introduction of N not only regulated the formation of the hierarchically porous structure of the carbon material,but also increased the adsorption of HCl and decreased the adsorption strength of C_(2)H_(2).The synergistic effect of high N content and porous structure significantly enhanced the catalytic performance of the catalysts in acetylene hydrochlorination.The C_(2)H_(2)conversion was maintained at around98%after 100 h under the reaction conditions(T=220°C,GHSV(C_(2)H_(2))=30 h^(-1),V_(HCl)/VC_(2)H_(2)=1.15).Thus,the one-pot synthesis process used here is a good benchmark for future catalyst research.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
With the relentless expansion of human economic activities,a substantial increase in CO_(2)emissions has been observed,primarily stemming from the rampant combustion of fossil fuels.This relentless surge has undeniabl...With the relentless expansion of human economic activities,a substantial increase in CO_(2)emissions has been observed,primarily stemming from the rampant combustion of fossil fuels.This relentless surge has undeniably exacerbated global warming and climate change,necessitating urgent measures to mitigate greenhouse gas emissions[1].The conventional CO_(2)separation technologies required the addition of amine-based absorbents,while their applications were limited by the strong corrosivity,toxic volatiles and by-products,and energy-consuming regeneration process.Recent advancements in membrane technology,including polymer thin film composites,metal-organic frameworks,and stacked nanosheets,have exhibited promising CO_(2)/N_(2)separation performances[2,3].However,the challenge of balancing high selectivity with high permeance remains,due to the inherent limitation of reducing thickness of the selective layer below 50–100 nm without introducing detrimental defects.Porous single-layer graphene,with its atomically thin pores,emerges as a promising two-dimensional(2D)material that minimizes diffusion resistance for molecular transport[4].Nevertheless,balancing high selectivity with high permeance has remained a formidable challenge.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
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
Chloromethylation of polystyrene （PS） with two different chloromethylating systems methylal/thionyl chloride and paraformaldehyde/trimethylchlorosilane was studied. Soluble chloromethylated polystyrene with a degree...Chloromethylation of polystyrene （PS） with two different chloromethylating systems methylal/thionyl chloride and paraformaldehyde/trimethylchlorosilane was studied. Soluble chloromethylated polystyrene with a degree of substitution of 89% was obtained. The Conant-Finkelstein reaction on the chloromethylated PS afforded soluble iodomethylated polystyrene with a degree of substitution as high as 96%. The reaction conditions of Minisci were employed to radically pyridinate PS via its iodomethylated derivative. Polyelectrolytes were formed which could be converted to normal polymers by treatment with a 20% aqueous solution of NaOH.展开更多
PVC was subjected to a chemical modification aiming at replacing the chlorine atoms by pyridine groups via a homolytic route. Pyridine groups were peculiarly affixed to the PVC matrix via a carbon-carbon bond rather t...PVC was subjected to a chemical modification aiming at replacing the chlorine atoms by pyridine groups via a homolytic route. Pyridine groups were peculiarly affixed to the PVC matrix via a carbon-carbon bond rather than a carbonnitrogen one. PVC was first iodinated using the Conant-Finkelstein reaction, followed by the application of the homolytic conditions of Minisci to generate pyridinated PVC with a varying degree of substitution. The extent of substitution was not high; the reaction on 30% iodinated PVC afforded a degree of modification no greater than 3%.展开更多
The effects of 2-[p-(Dimethylamino)styryl] pyridine methiodide(DSPM)on slow response action potential(SRAP)and slow inward current(Isi) of guinea pig papillary muscles were studied by intracellular microelectrodes and...The effects of 2-[p-(Dimethylamino)styryl] pyridine methiodide(DSPM)on slow response action potential(SRAP)and slow inward current(Isi) of guinea pig papillary muscles were studied by intracellular microelectrodes and voltage clamp techniques.The APA and V_(max) of SRAP induced by high K￣+were decreased after 50 min of perfusion with DSPM solu- tion. Isi was suppressed from a peak value of8.8± 1.6μA to 5.7± 1.8μA, The results indicated that DSPM has a selective blocking effect on calcium channel.展开更多
Simultaneous pyridine biodegradation and nitrogen removal were successfully achieved in a sequencing batch reactor（SBR） based on aerobic granules. In a typical SBR cycle, nitritation occurred obviously after the maj...Simultaneous pyridine biodegradation and nitrogen removal were successfully achieved in a sequencing batch reactor（SBR） based on aerobic granules. In a typical SBR cycle, nitritation occurred obviously after the majority of pyridine was removed, while denitrification occurred at early stage of the cycle when oxygen consumption was aggravated. The effect of several key operation parameters, i.e., air flow rate, influent NH4~＋-N concentration,influent p H and pyridine concentration, on nitritation, pyridine degradation and total nitrogen（TN） removal, was systematically investigated. The results indicated that high air flow rate had a positive effect on both pyridine degradation and nitritation but a negative impact of overhigh air flow rate. With the increase of NH4~＋ dosage, both nitritation and TN removal could be severely inhibited. Slightly alkaline condition, i.e., pH 7.0–8.0, was beneficial for both pyridine degradation and nitritation. High pyridine dosage often resulted in the delay of both pyridine degradation and nitritation. Besides, extracellular polymeric substances production was affected by air flow rate, NH4~＋ dosage, pyridine dosage and p H.In addition, high-throughput sequencing analysis demonstrated that Bdellovibrio and Paracoccus were the dominant species in the aerobic granulation system. Coexistence of pyridine degrader, nitrification related species, denitrification related species, polymeric substances producer and self-aggregation related species was also confirmed by highthroughput sequencing.展开更多
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.
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supported by the National Natural Science Foundation of China(22278407,22001147,21922814,22138012,22178349)CAS Project for Young Scientists in Basic Research(YSBR-038)+2 种基金the Ministry of Science and Technology of China(2021YFC2901500)Excellent Member in Youth Innovation Promotion Association,Chinese Academy of Sciences(Y202014)Shandong Energy Institute(SEI U202306).
文摘Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed metal ion environments.Herein,a new synergistic solvent extraction(SSX)system comprised of a novel pyridine analog,N,N-bis(pyridin-2-ylmethyl)dodecan-1-amine(BPMDA),and dinonylnaphthalene sulfonic acid(DNNSA)with tributyl phosphate as phase modifier is introduced.The SSX system demonstrates high extraction performance achieving>90%for Ni and>97%for Co in a singlestage extraction process,with high selectivity.Under optimal conditions,the selectivity sequence is observed as Co^(2+)(>97%)>Ni^(2+)(>90%)>Mn^(2+)(<20%)>Fe^(3+)(<10%)>Mg^(2+)(<5%)>Al^(3+)(<2%)>Ca^(2+)(<1%).Spectroscopic analysis evidences the preferential binding of BPMDA with Ni and Co in the presence of DNNSA,concurrently achieving a significant reduction in the co-extraction of Fe(Ⅲ)and Al.The selective complexation of Ni and Co using the SSX system offers a highly efficient and selective approach for their extraction,with promising potential for applications in recovery-based processes.
基金supported by the Tianchi Innovation Leading Talent Development Fund(No.CZ002710)in Xinjiangthe Taishan Scholars Program of Shandong Province(No.tsqn202103051)+4 种基金the Project of Science and Technology Development of Yantai City(No.2023JCYJ073)Natural science foundation of Shandong province(No.ZR2023MB064)special funds for over provincial level leading talent of Yantai citythe Start-Up Foundation for High-level Professionals of Shihezi University(No.RCZK201932)Tianshan Talents Training Program of Xinjiang(Science and Technology Innovation Team,No.2022TSYCTD0021)。
文摘Polyvinyl chloride is the most widely used general-purpose plastic and plays a vital role in various industries.Mercury-based catalysts severely limit the green sustainability of industry.Non-metallic carbon materials are very promising alternatives in acetylene hydrochlorination,but their stability remains a challenge of major concern at present.Based on the principle of green chemistry,structurally tunable and defect-rich carbon materials were synthesized by hydrothermal carbonization and pyrolysis using glucose as carbon source and m-phenylenediamine as nitrogen source and cross-linking agent.Experimental characterization and density functional theory confirmed that pyridinic N was the main active site.The introduction of N not only regulated the formation of the hierarchically porous structure of the carbon material,but also increased the adsorption of HCl and decreased the adsorption strength of C_(2)H_(2).The synergistic effect of high N content and porous structure significantly enhanced the catalytic performance of the catalysts in acetylene hydrochlorination.The C_(2)H_(2)conversion was maintained at around98%after 100 h under the reaction conditions(T=220°C,GHSV(C_(2)H_(2))=30 h^(-1),V_(HCl)/VC_(2)H_(2)=1.15).Thus,the one-pot synthesis process used here is a good benchmark for future catalyst research.
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 the National Natural Science Foundation of China(22122602,22376071,22161142005)the Foundation of State Key Laboratory of Coal Combustion,China.
文摘With the relentless expansion of human economic activities,a substantial increase in CO_(2)emissions has been observed,primarily stemming from the rampant combustion of fossil fuels.This relentless surge has undeniably exacerbated global warming and climate change,necessitating urgent measures to mitigate greenhouse gas emissions[1].The conventional CO_(2)separation technologies required the addition of amine-based absorbents,while their applications were limited by the strong corrosivity,toxic volatiles and by-products,and energy-consuming regeneration process.Recent advancements in membrane technology,including polymer thin film composites,metal-organic frameworks,and stacked nanosheets,have exhibited promising CO_(2)/N_(2)separation performances[2,3].However,the challenge of balancing high selectivity with high permeance remains,due to the inherent limitation of reducing thickness of the selective layer below 50–100 nm without introducing detrimental defects.Porous single-layer graphene,with its atomically thin pores,emerges as a promising two-dimensional(2D)material that minimizes diffusion resistance for molecular transport[4].Nevertheless,balancing high selectivity with high permeance has remained a formidable challenge.
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℃.
文摘Chloromethylation of polystyrene （PS） with two different chloromethylating systems methylal/thionyl chloride and paraformaldehyde/trimethylchlorosilane was studied. Soluble chloromethylated polystyrene with a degree of substitution of 89% was obtained. The Conant-Finkelstein reaction on the chloromethylated PS afforded soluble iodomethylated polystyrene with a degree of substitution as high as 96%. The reaction conditions of Minisci were employed to radically pyridinate PS via its iodomethylated derivative. Polyelectrolytes were formed which could be converted to normal polymers by treatment with a 20% aqueous solution of NaOH.
文摘PVC was subjected to a chemical modification aiming at replacing the chlorine atoms by pyridine groups via a homolytic route. Pyridine groups were peculiarly affixed to the PVC matrix via a carbon-carbon bond rather than a carbonnitrogen one. PVC was first iodinated using the Conant-Finkelstein reaction, followed by the application of the homolytic conditions of Minisci to generate pyridinated PVC with a varying degree of substitution. The extent of substitution was not high; the reaction on 30% iodinated PVC afforded a degree of modification no greater than 3%.
文摘The effects of 2-[p-(Dimethylamino)styryl] pyridine methiodide(DSPM)on slow response action potential(SRAP)and slow inward current(Isi) of guinea pig papillary muscles were studied by intracellular microelectrodes and voltage clamp techniques.The APA and V_(max) of SRAP induced by high K￣+were decreased after 50 min of perfusion with DSPM solu- tion. Isi was suppressed from a peak value of8.8± 1.6μA to 5.7± 1.8μA, The results indicated that DSPM has a selective blocking effect on calcium channel.
基金supported by the Natural Science Foundation of Jiangsu Province for Distinguished Young Scholars (No. BK20170038)the Natural Science Foundation of Jiangsu Province (No. BK20151485)the National Natural Science Foundation of China (Nos. 51478225 and 51778294)
文摘Simultaneous pyridine biodegradation and nitrogen removal were successfully achieved in a sequencing batch reactor（SBR） based on aerobic granules. In a typical SBR cycle, nitritation occurred obviously after the majority of pyridine was removed, while denitrification occurred at early stage of the cycle when oxygen consumption was aggravated. The effect of several key operation parameters, i.e., air flow rate, influent NH4~＋-N concentration,influent p H and pyridine concentration, on nitritation, pyridine degradation and total nitrogen（TN） removal, was systematically investigated. The results indicated that high air flow rate had a positive effect on both pyridine degradation and nitritation but a negative impact of overhigh air flow rate. With the increase of NH4~＋ dosage, both nitritation and TN removal could be severely inhibited. Slightly alkaline condition, i.e., pH 7.0–8.0, was beneficial for both pyridine degradation and nitritation. High pyridine dosage often resulted in the delay of both pyridine degradation and nitritation. Besides, extracellular polymeric substances production was affected by air flow rate, NH4~＋ dosage, pyridine dosage and p H.In addition, high-throughput sequencing analysis demonstrated that Bdellovibrio and Paracoccus were the dominant species in the aerobic granulation system. Coexistence of pyridine degrader, nitrification related species, denitrification related species, polymeric substances producer and self-aggregation related species was also confirmed by highthroughput sequencing.
