A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficie...A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.展开更多
The tumor microenvironment(TME)significantly influences cancer evolution and therapeutic efficacy.Targeting biofunctional molecules to the TME has long been appreciated as a means of raising local drug concentrations ...The tumor microenvironment(TME)significantly influences cancer evolution and therapeutic efficacy.Targeting biofunctional molecules to the TME has long been appreciated as a means of raising local drug concentrations and reducing systemic toxicities.The booming nanotechnology field has realized the importance of cathepsin B to derive a variety of intelligent enzyme-responsive nanosized drug delivery systems(nanoDDS)to improve treatment responses and clinical outcomes.In this tutorial review,after introducing the molecular structure and physiological/pathological functions of cathepsin B,the outstanding achievements of cathepsin B-responsive nanoplatforms in the precise diagnosis,targeted therapy,and synergistic theranostics of malignant tumors are systematically described.Finally,the challenges of enzyme-substrate incompatibility,low diagnostic sensitivity,mass production and biocompatibility of multifunctional nanoDDS are considered in order to successfully promote them to clinical applications.展开更多
Compared to the widely used carbon-centered radicals,N-radicals have been relatively unexplored owing to the lack of practical and convenient production methods.Over the past few years,benefitting from the resurgence ...Compared to the widely used carbon-centered radicals,N-radicals have been relatively unexplored owing to the lack of practical and convenient production methods.Over the past few years,benefitting from the resurgence of reliable and controllable radical chemistry,N-radicals have been produced via thermal decomposition,oxidants,metal salts,or electrocatalysis.Therefore,numerous N-radical enabled cyclization of 1,n-enynes methods have been developed,providing a versatile and concise synthetic platform for the preparation of complex cyclic systems and natural products containing elaborate ring frameworks.In this review,we will summarize recent advances in the promising field of radical chemistry focusing on the production methods of N-radicals and their cyclization patterns,associated mechanisms,unmet challenges,and future opportunities.展开更多
Five new coumarin amide derivatives were synthesized with coupling reagent,the structures of which were characterized by IR,1H NMR,13C NMR,MS and element analysis.Their spectral properties were studied in dichlorometh...Five new coumarin amide derivatives were synthesized with coupling reagent,the structures of which were characterized by IR,1H NMR,13C NMR,MS and element analysis.Their spectral properties were studied in dichloromethane,in N,N-dimethylformamide（DMF） and in solid state.Solvent polarity has less influence on the UV-Vis maximum absorption at about 430 nm.The maximum emission wavelengths change from 464 nm to 474 nm in dichloromethane,from 476 nm to 482 nm in DMF and from 521 nm to 548 nm in solid state,respectively.The fluorescence intensities of compounds 8 and 9 were extremely strong in solvents or in solid state.Compounds 8 and 9 exhibited high fluorescenct quantumn yields in solution compared to compounds 4 ＂7.The fluorescence lifetimes of all the compounds in solvents were measured.展开更多
Oil dispersible suspension concentrates are safe,green,and environmentally friendly formulations.Problems such as layering,pasting,and bottoming are frequently encountered during the production,storage,and transportat...Oil dispersible suspension concentrates are safe,green,and environmentally friendly formulations.Problems such as layering,pasting,and bottoming are frequently encountered during the production,storage,and transportation process.Polyisobutylene succinimide functions as a dispersant and exhibits great potential to improve the physical stability of the oil dispersible suspension concentrate.From a microscopic perspective,the sorption characteristics of the polyisobutylene succinimide dispersant T151 on penoxsulam particle surfaces were comprehensively evaluated with XPS,FTIR,and SEM.The T151 adsorption procedure complied with a pseudo-second-order kinetic adsorption model,and it was a kind of physical sorption with an Ea of 22.57 kJ⋅mol^(−1).The T151 sorption model was consistent with the Langmuir isotherm.The adsorption process was spontaneous and followed by an entropy increase.TheΔH^(θ)of dispersant T151 on the surface of penoxsulam particles was 31.59 kJ⋅mol^(−1).The adsorption procedure was endothermic,and the primary force was hydrogen bonding.The XPS results showed that the F and S electronic peaks at the penoxsulam interface decreased,and that the C electronic peak increased significantly after the adsorption of dispersant T151,indicating the adsorption on the surface of penoxsulam particles.The results of this study provide a vital theoretical basis for the application of polyisobutylene succinimide dispersants in oil dispersible suspension systems.展开更多
An efficient procedure for the selective preparation of hydroxy-,carbonyl-and acetal-containing 2-pyrrolidinones has been developed through radical cyclization of 1,6-dienes initiated byα-C(sp3)-H functionalization o...An efficient procedure for the selective preparation of hydroxy-,carbonyl-and acetal-containing 2-pyrrolidinones has been developed through radical cyclization of 1,6-dienes initiated byα-C(sp3)-H functionalization of alcohols.This protocol could be conducted at catalyst-free conditions at relatively low temperature(80℃)by employing commercially available tert-butyl peroxybenzoate(TBPB)as the oxidant.展开更多
A new 1D coordination polymer,{[Mn2（4＇,4-hbc）4（4＇,4-Hhbc）2（H2O）]·H2O}n（4＇,4-Hhbc=4＇-hydroxyl-biphenyl-4-carboxylic acid）,has been hydrothermally synthesized and struc-turally characterized by elementa...A new 1D coordination polymer,{[Mn2（4＇,4-hbc）4（4＇,4-Hhbc）2（H2O）]·H2O}n（4＇,4-Hhbc=4＇-hydroxyl-biphenyl-4-carboxylic acid）,has been hydrothermally synthesized and struc-turally characterized by elemental analysis,IR spectroscopy and single-crystal X-ray diffraction.The crystal belongs to the monoclinic system,space group C2/c with a=52.421（10）,b=7.5388（15）,c=16.478（3）,β=106.12（3）°,V=6256（2）3,Z=4,C78H62Mn2O21,Mr=1445.16,Dc=1.534g/cm3,μ（MoKα）=0.490mm-1,F（000）=2992,R=0.0764 and wR=0.2006 for 2984 observed reflections with I2σ（I）.X-ray diffraction analyses reveal that the title compound is a one-dimensional infinite chain,in which the MnⅡ atom adopts a distorted octahedral geometry coordinated by four 4＇,4-hbc ligands,one 4＇,4-Hhbc ligand and one water molecule.Furthermore,the luminescent property of title compound was investigated.展开更多
Proteases have a fundamental role in maintaining physiological homeostasis,but their dysregulation results in severe activity imbalance and pathological conditions,including cancer onset,progression,invasion,and metas...Proteases have a fundamental role in maintaining physiological homeostasis,but their dysregulation results in severe activity imbalance and pathological conditions,including cancer onset,progression,invasion,and metastasis.This striking importance plus superior biological recognition and catalytic performance of proteases,combining with the excellent physicochemical characteristics of nanomaterials,results in enzyme-activated nano-drug delivery systems(nanoDDS)that perform theranostic functions in highly specific response to the tumor phenotype stimulus.In the tutorial review,the key advances of protease-responsive nanoDDS in the specific diagnosis and targeted treatment for malignancies are emphatically classified according to the effector biomolecule types,on the premise of summarizing the structure and function of each protease.Subsequently,the incomplete matching and recognition between enzyme and substrate,structural design complexity,volume production,and toxicological issues related to the nanocomposites are highlighted to clarify the direction of efforts in nanotheranostics.This will facilitate the promotion of nanotechnology in the management of malignant tumors.展开更多
In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental li...In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental limitations to accelerate rational catalyst design.Hence,significant efforts have been made to perform ML to accelerate calculation and aid electrocatalyst design for CO_(2) reduction.This review discusses recent applications of ML to discover,design,and optimize novel electrocatalysts.First,insights into ML aided in accelerating calculation are presented.Then,ML aided in the rational design of the electrocatalyst is introduced,including establishing a data set/data source selection and validation of descriptor selection of ML algorithms validation and predictions of the model.Finally,the opportunities and future challenges are summarized for the future design of electrocatalyst for CO_(2) reduction with the assistance of ML.展开更多
Achieving carbon neutrality is an essential part of responding to climate change caused by the deforestation and over-exploitation of natural resources that have accompanied the development of human society.The carbon...Achieving carbon neutrality is an essential part of responding to climate change caused by the deforestation and over-exploitation of natural resources that have accompanied the development of human society.The carbon dioxide reduction reaction(CO_(2)RR)is a promising strategy to capture and convert carbon dioxide(CO_(2))into value-added chemical products.However,the traditional trial-and-error method makes it expensive and time-consuming to understand the deeper mechanism behind the reaction,discover novel catalysts with superior performance and lower cost,and determine optimal support structures and electrolytes for the CO_(2)RR.Emerging machine learning(ML)techniques provide an opportunity to integrate material science and artificial intelligence,which would enable chemists to extract the implicit knowledge behind data,be guided by the insights thereby gained,and be freed from performing repetitive experiments.In this perspective article,we focus on recent ad-vancements in ML-participated CO_(2)RR applications.After a brief introduction to ML techniques and the CO_(2)RR,we first focus on ML-accelerated property prediction for potential CO_(2)RR catalysts.Then we explore ML-aided prediction of catalytic activity and selectivity.This is followed by a discussion about ML-guided catalyst and electrode design.Next,the potential application of ML-assisted experimental synthesis for the CO_(2)RR is discussed.展开更多
of main observation and conclusion Genkwadane F-I(1-4),four new diterpenes,along with four known ones(5-8),were isolated from the flower buds of D.genkwa.The structures including absolute configurations of 1-4 were de...of main observation and conclusion Genkwadane F-I(1-4),four new diterpenes,along with four known ones(5-8),were isolated from the flower buds of D.genkwa.The structures including absolute configurations of 1-4 were determined based on the analysis of NMR and ECD calculations.All compounds were evaluated for their cytotoxicities against MCF-7 and Hep3B cell lines,among which compounds 3 and 4 showed significant activities.Compound 4 exhibited the most potent activity with IC50 values of 1.33μM against MCF-7,and the IC50 values of compound 3 against MCF-7 and Hep3B were 5.54μM and 8.73μM;respectively.Further studies by Hoechst 33258 staining and Annexin V/PI analysis demonstrated that compounds 3 and 4 could induce apoptosis to exhibit anti-tumor activities.展开更多
N-Methyl-2-（4-N,N-diphenylaminophenyl）fulleropyrrolidine and N-methyl-2-（4-di-p-tolylaminophenyl）fulleropyrrolidine were synthesized via the 1,3-dipolar cycloaddition reactions under microwave irradiation. The mol...N-Methyl-2-（4-N,N-diphenylaminophenyl）fulleropyrrolidine and N-methyl-2-（4-di-p-tolylaminophenyl）fulleropyrrolidine were synthesized via the 1,3-dipolar cycloaddition reactions under microwave irradiation. The molecular structures were identified and characterized by MS, UV-Vis, FT-IR, ^1H NMR and fluorescence spectra. Photoinduced intramolecular electron transfer process from C60 moiety to triphenylamine moiety have been studied by nanosecond laser flash photolysis. The optimized structure and the distribution of the frontier molecular orbitals for C60-TPA were obtained by using DFT method at B3LYP/6-31G（d） level. The results indicated that the intramolecular photoinduced electron transfer could occur in these compounds, which were in excellent agreement with the nanosecond transient absorption spectra observed experimentally in polar solvent. The electronic spectrum of the compound C60-TPA was studied by ZINDO method on the basis of the optimized geometrics, which was essentially consistent with experimental values.展开更多
[60]Fullerenes attached with piperidinodithiocarboxylate dyad （1） and 7-chloro-1,2,3,4-tetrahydrophenazine （2） were efficiently synthesized through Diels-Atder cycloaddition with dienes. The physical properties of...[60]Fullerenes attached with piperidinodithiocarboxylate dyad （1） and 7-chloro-1,2,3,4-tetrahydrophenazine （2） were efficiently synthesized through Diels-Atder cycloaddition with dienes. The physical properties of the triplet states of these compounds, in which strong electron acceptor moieties were covalently attached to C60 cores, were investigated by nanosecond laser flash photolysis. The excited triplet states in benzonitrite have been evaluated by observing the transient absorption bands in the near-IR region. The HOMO and LUMO were calculated by semiempirical methods AM1, which could predict the intramolecular photoinduced electron transfer in 1 and 2, and the nanosecond transient absorption spectra observed experimentally in solution were in excellent agreement with the calculated ones.展开更多
As a metal-free semiconductor,graphitic carbon nitride(g-C3N4)has received extensive attention due to its high stability,nontoxicity,facile and low-cost synthesis,appropriate band gap in the visible spectral range and...As a metal-free semiconductor,graphitic carbon nitride(g-C3N4)has received extensive attention due to its high stability,nontoxicity,facile and low-cost synthesis,appropriate band gap in the visible spectral range and wide availability of resources.The dimensions of g-C3N4 can influence the regime of the confinement of electrons,and consequently,g-C3N4 with various dimensionalities shows different properties,making them available for many stimulating applications.Although there are some reviews focusing on the synthesis strategy and applications of g-C3N4,there is still a lack of comprehensive review that systemically summarises the synthesis and application of different dimensions of g-C3N4,which can provide an important theoretical and practical basis for the development of g-C3N4 with different dimensionalities and maximises their potential in diverse applications.By reviewing the latest progress of g-C3N4 studies,we aim to summarise the preparation of g-C3N4 with different dimensionalities using various structural engineering strategies,discuss the fundamental bottlenecks of currently existing methods and their solution strategies,and explore their applications in energy and environmental applications.Furthermore,it also puts forward the views on the future research direction of these unique materials.展开更多
基金supported by Sichuan Science and Technology Program(No.2023NSFSC0101)the 2024 Provincial platform project of Chengdu Normal University(No.GNFZ202404)+1 种基金Natural Science Foundation of Shandong Province(No.ZR2021MB065)National Natural Science Foundation of China(No.22101237)。
文摘A convenient photocatalytic multi-component reaction of alkenes,quinoxalin-2(1H)-ones,and diazo compounds has been developed in the presence of water.A number of ester-containing quinoxalin-2(1H)-ones could be efficiently obtained in moderate to good yields at room temperature.This metal-free visiblelight-driven tandem reaction was conducted through proton-coupled electron transfer(PCET)process using water as the hydrogen donor and 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as the photocatalyst.
基金the National Natural Science Foundation of China(Nos.81903662,51903201)China Postdoctoral Science Foundation Grant(Nos.2019M661057,2019M653660)+5 种基金the Applied Basic Research Programs of Shanxi Province(No.201901D211347)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(No.2019L0428)the Startup Foundation for Doctors of Shanxi Province(No.SD1827)Natural Science Foundation of Shaanxi Province(No.2020JQ-086)College Students’Innovation and Entrepreneurship Training Program(No.SJ201910698121)the Startup Foundation for Doctors of Shanxi Medical University(No.XD1824)。
文摘The tumor microenvironment(TME)significantly influences cancer evolution and therapeutic efficacy.Targeting biofunctional molecules to the TME has long been appreciated as a means of raising local drug concentrations and reducing systemic toxicities.The booming nanotechnology field has realized the importance of cathepsin B to derive a variety of intelligent enzyme-responsive nanosized drug delivery systems(nanoDDS)to improve treatment responses and clinical outcomes.In this tutorial review,after introducing the molecular structure and physiological/pathological functions of cathepsin B,the outstanding achievements of cathepsin B-responsive nanoplatforms in the precise diagnosis,targeted therapy,and synergistic theranostics of malignant tumors are systematically described.Finally,the challenges of enzyme-substrate incompatibility,low diagnostic sensitivity,mass production and biocompatibility of multifunctional nanoDDS are considered in order to successfully promote them to clinical applications.
文摘Compared to the widely used carbon-centered radicals,N-radicals have been relatively unexplored owing to the lack of practical and convenient production methods.Over the past few years,benefitting from the resurgence of reliable and controllable radical chemistry,N-radicals have been produced via thermal decomposition,oxidants,metal salts,or electrocatalysis.Therefore,numerous N-radical enabled cyclization of 1,n-enynes methods have been developed,providing a versatile and concise synthetic platform for the preparation of complex cyclic systems and natural products containing elaborate ring frameworks.In this review,we will summarize recent advances in the promising field of radical chemistry focusing on the production methods of N-radicals and their cyclization patterns,associated mechanisms,unmet challenges,and future opportunities.
基金Supported by the Science & Research Program of Guangdong Province,China(No.C80017)
文摘Five new coumarin amide derivatives were synthesized with coupling reagent,the structures of which were characterized by IR,1H NMR,13C NMR,MS and element analysis.Their spectral properties were studied in dichloromethane,in N,N-dimethylformamide（DMF） and in solid state.Solvent polarity has less influence on the UV-Vis maximum absorption at about 430 nm.The maximum emission wavelengths change from 464 nm to 474 nm in dichloromethane,from 476 nm to 482 nm in DMF and from 521 nm to 548 nm in solid state,respectively.The fluorescence intensities of compounds 8 and 9 were extremely strong in solvents or in solid state.Compounds 8 and 9 exhibited high fluorescenct quantumn yields in solution compared to compounds 4 ＂7.The fluorescence lifetimes of all the compounds in solvents were measured.
基金This work was funded by the Foundation(No.LJ2020030)from the Project of the Education Department of Liaoning Province,China.
文摘Oil dispersible suspension concentrates are safe,green,and environmentally friendly formulations.Problems such as layering,pasting,and bottoming are frequently encountered during the production,storage,and transportation process.Polyisobutylene succinimide functions as a dispersant and exhibits great potential to improve the physical stability of the oil dispersible suspension concentrate.From a microscopic perspective,the sorption characteristics of the polyisobutylene succinimide dispersant T151 on penoxsulam particle surfaces were comprehensively evaluated with XPS,FTIR,and SEM.The T151 adsorption procedure complied with a pseudo-second-order kinetic adsorption model,and it was a kind of physical sorption with an Ea of 22.57 kJ⋅mol^(−1).The T151 sorption model was consistent with the Langmuir isotherm.The adsorption process was spontaneous and followed by an entropy increase.TheΔH^(θ)of dispersant T151 on the surface of penoxsulam particles was 31.59 kJ⋅mol^(−1).The adsorption procedure was endothermic,and the primary force was hydrogen bonding.The XPS results showed that the F and S electronic peaks at the penoxsulam interface decreased,and that the C electronic peak increased significantly after the adsorption of dispersant T151,indicating the adsorption on the surface of penoxsulam particles.The results of this study provide a vital theoretical basis for the application of polyisobutylene succinimide dispersants in oil dispersible suspension systems.
基金the National Natural Science Foundation of China(No.21801142)the Natural Science Foundation of Zhejiang Province(No.LQ18B020002)+1 种基金the Ningbo Municipal Natural Science Foundation(No.2019A610021)the Hunan Provincial NaturalScience Foundation of China(No.2019JJ20008)for financial support。
文摘An efficient procedure for the selective preparation of hydroxy-,carbonyl-and acetal-containing 2-pyrrolidinones has been developed through radical cyclization of 1,6-dienes initiated byα-C(sp3)-H functionalization of alcohols.This protocol could be conducted at catalyst-free conditions at relatively low temperature(80℃)by employing commercially available tert-butyl peroxybenzoate(TBPB)as the oxidant.
基金supported by the Natural Science Foundation of Guangdong Province (7300449)
文摘A new 1D coordination polymer,{[Mn2（4＇,4-hbc）4（4＇,4-Hhbc）2（H2O）]·H2O}n（4＇,4-Hhbc=4＇-hydroxyl-biphenyl-4-carboxylic acid）,has been hydrothermally synthesized and struc-turally characterized by elemental analysis,IR spectroscopy and single-crystal X-ray diffraction.The crystal belongs to the monoclinic system,space group C2/c with a=52.421（10）,b=7.5388（15）,c=16.478（3）,β=106.12（3）°,V=6256（2）3,Z=4,C78H62Mn2O21,Mr=1445.16,Dc=1.534g/cm3,μ（MoKα）=0.490mm-1,F（000）=2992,R=0.0764 and wR=0.2006 for 2984 observed reflections with I2σ（I）.X-ray diffraction analyses reveal that the title compound is a one-dimensional infinite chain,in which the MnⅡ atom adopts a distorted octahedral geometry coordinated by four 4＇,4-hbc ligands,one 4＇,4-Hhbc ligand and one water molecule.Furthermore,the luminescent property of title compound was investigated.
基金funded by the National Natural Science Foundation of China(81903662,81860630 and 51903201)China Postdoctoral Science Foundation(2019M661057 and 2019M653660)+2 种基金Natural Science Foundation of Shaanxi Province(2020JQ-086,China)the Natural Science Foundation of Jiangxi(20181BAB205087,China)the Key Project of Jiangxi(20192ACB70012,China)
文摘Proteases have a fundamental role in maintaining physiological homeostasis,but their dysregulation results in severe activity imbalance and pathological conditions,including cancer onset,progression,invasion,and metastasis.This striking importance plus superior biological recognition and catalytic performance of proteases,combining with the excellent physicochemical characteristics of nanomaterials,results in enzyme-activated nano-drug delivery systems(nanoDDS)that perform theranostic functions in highly specific response to the tumor phenotype stimulus.In the tutorial review,the key advances of protease-responsive nanoDDS in the specific diagnosis and targeted treatment for malignancies are emphatically classified according to the effector biomolecule types,on the premise of summarizing the structure and function of each protease.Subsequently,the incomplete matching and recognition between enzyme and substrate,structural design complexity,volume production,and toxicological issues related to the nanocomposites are highlighted to clarify the direction of efforts in nanotheranostics.This will facilitate the promotion of nanotechnology in the management of malignant tumors.
基金ANU Futures Scheme,Grant/Award Number:Q4601024National Natural Science Foundation of China,Grant/Award Number:22078054+1 种基金Australian Research Council,Grant/Award Number:DP190100295China Scholarship Council(CSC)Program。
文摘In the past decades,machine learning(ML)has impacted the field of electrocatalysis.Modern researchers have begun to take advantage of ML‐based data‐driven techniques to overcome the computational and experimental limitations to accelerate rational catalyst design.Hence,significant efforts have been made to perform ML to accelerate calculation and aid electrocatalyst design for CO_(2) reduction.This review discusses recent applications of ML to discover,design,and optimize novel electrocatalysts.First,insights into ML aided in accelerating calculation are presented.Then,ML aided in the rational design of the electrocatalyst is introduced,including establishing a data set/data source selection and validation of descriptor selection of ML algorithms validation and predictions of the model.Finally,the opportunities and future challenges are summarized for the future design of electrocatalyst for CO_(2) reduction with the assistance of ML.
基金gratefully express gratitude to all parties who have contributed toward the success of this project,both financially and technically,especially the S&T Innovation 2025 Major Special Programme(Grant No.2018B10022)the Ningbo Commonweal Programme(Grant No.2022S122)funded by the Ningbo Science and Technology Bureau,China,as well as the UNNC FoSE Faculty Inspiration Grant,China+1 种基金the support from the Ningbo Municipal Key Laboratory on Clean Energy Conversion Technologies(2014A22010)as well as the Zhejiang Provincial Key Laboratory for Carbonaceous Wastes Processing and Process Intensification Research funded by the Zhejiang Provincial Department of Science and Technology(2020E10018)support from the ANU Futures Scheme(Q4601024).
文摘Achieving carbon neutrality is an essential part of responding to climate change caused by the deforestation and over-exploitation of natural resources that have accompanied the development of human society.The carbon dioxide reduction reaction(CO_(2)RR)is a promising strategy to capture and convert carbon dioxide(CO_(2))into value-added chemical products.However,the traditional trial-and-error method makes it expensive and time-consuming to understand the deeper mechanism behind the reaction,discover novel catalysts with superior performance and lower cost,and determine optimal support structures and electrolytes for the CO_(2)RR.Emerging machine learning(ML)techniques provide an opportunity to integrate material science and artificial intelligence,which would enable chemists to extract the implicit knowledge behind data,be guided by the insights thereby gained,and be freed from performing repetitive experiments.In this perspective article,we focus on recent ad-vancements in ML-participated CO_(2)RR applications.After a brief introduction to ML techniques and the CO_(2)RR,we first focus on ML-accelerated property prediction for potential CO_(2)RR catalysts.Then we explore ML-aided prediction of catalytic activity and selectivity.This is followed by a discussion about ML-guided catalyst and electrode design.Next,the potential application of ML-assisted experimental synthesis for the CO_(2)RR is discussed.
基金This research was supported by the National Nature Science Foundation of China(Nos.81872766,81673324,81573319)the Foundation(L2015518)from the Project of Education Departmentof Liaoning Province of China,the Project of Innovation Team(LT2015027)of Liaoning and the Liaoning province Natural Science Foundation of China(201602705).
文摘of main observation and conclusion Genkwadane F-I(1-4),four new diterpenes,along with four known ones(5-8),were isolated from the flower buds of D.genkwa.The structures including absolute configurations of 1-4 were determined based on the analysis of NMR and ECD calculations.All compounds were evaluated for their cytotoxicities against MCF-7 and Hep3B cell lines,among which compounds 3 and 4 showed significant activities.Compound 4 exhibited the most potent activity with IC50 values of 1.33μM against MCF-7,and the IC50 values of compound 3 against MCF-7 and Hep3B were 5.54μM and 8.73μM;respectively.Further studies by Hoechst 33258 staining and Annexin V/PI analysis demonstrated that compounds 3 and 4 could induce apoptosis to exhibit anti-tumor activities.
基金Project supported by the National Natural Science Foundation of China （Nos. 20231020 and 20471020）.
文摘N-Methyl-2-（4-N,N-diphenylaminophenyl）fulleropyrrolidine and N-methyl-2-（4-di-p-tolylaminophenyl）fulleropyrrolidine were synthesized via the 1,3-dipolar cycloaddition reactions under microwave irradiation. The molecular structures were identified and characterized by MS, UV-Vis, FT-IR, ^1H NMR and fluorescence spectra. Photoinduced intramolecular electron transfer process from C60 moiety to triphenylamine moiety have been studied by nanosecond laser flash photolysis. The optimized structure and the distribution of the frontier molecular orbitals for C60-TPA were obtained by using DFT method at B3LYP/6-31G（d） level. The results indicated that the intramolecular photoinduced electron transfer could occur in these compounds, which were in excellent agreement with the nanosecond transient absorption spectra observed experimentally in polar solvent. The electronic spectrum of the compound C60-TPA was studied by ZINDO method on the basis of the optimized geometrics, which was essentially consistent with experimental values.
基金Project supported by the National Natural Science Foundation of China （Nos. 20231020, 20471020）.
文摘[60]Fullerenes attached with piperidinodithiocarboxylate dyad （1） and 7-chloro-1,2,3,4-tetrahydrophenazine （2） were efficiently synthesized through Diels-Atder cycloaddition with dienes. The physical properties of the triplet states of these compounds, in which strong electron acceptor moieties were covalently attached to C60 cores, were investigated by nanosecond laser flash photolysis. The excited triplet states in benzonitrite have been evaluated by observing the transient absorption bands in the near-IR region. The HOMO and LUMO were calculated by semiempirical methods AM1, which could predict the intramolecular photoinduced electron transfer in 1 and 2, and the nanosecond transient absorption spectra observed experimentally in solution were in excellent agreement with the calculated ones.
基金supported by an Australian Research Council(ARC)Future Fellowship(No.FT160100195)G.H.J.acknowledges the support from the Australian Research Council(ARC)Discovery Early Career Researcher Award(ARC DECRA)(Project ID:DE160100589)Q.H.acknowledges the technical support of Beijing NBET Technology Co.,Ltd.
文摘As a metal-free semiconductor,graphitic carbon nitride(g-C3N4)has received extensive attention due to its high stability,nontoxicity,facile and low-cost synthesis,appropriate band gap in the visible spectral range and wide availability of resources.The dimensions of g-C3N4 can influence the regime of the confinement of electrons,and consequently,g-C3N4 with various dimensionalities shows different properties,making them available for many stimulating applications.Although there are some reviews focusing on the synthesis strategy and applications of g-C3N4,there is still a lack of comprehensive review that systemically summarises the synthesis and application of different dimensions of g-C3N4,which can provide an important theoretical and practical basis for the development of g-C3N4 with different dimensionalities and maximises their potential in diverse applications.By reviewing the latest progress of g-C3N4 studies,we aim to summarise the preparation of g-C3N4 with different dimensionalities using various structural engineering strategies,discuss the fundamental bottlenecks of currently existing methods and their solution strategies,and explore their applications in energy and environmental applications.Furthermore,it also puts forward the views on the future research direction of these unique materials.
