Two-dimensional transition metal dichalcogenides(TMDs)show great promise for developing the next generation of electronic and optoelectronic devices.However,most TMDs have n-type or n-dominant bipolar characteristics,...Two-dimensional transition metal dichalcogenides(TMDs)show great promise for developing the next generation of electronic and optoelectronic devices.However,most TMDs have n-type or n-dominant bipolar characteristics,and this severely limits their potential for being designed as multi-functional heterostructures.Recently,thermal annealing has been reported as an easy means of p-doping TMDs,but the mechanism remains ambiguous,thereby preventing reliable outcomes and it becoming a mature doping technology for TMDs.Here,the mechanism of thermal annealing for p-doping a 2D selenide is investigated thoroughly,revealing the key role of the catalytic effect of nano-thick gold electrodes in achieving p-doping.As an example,2D SnSe_(2)with a fairly high electron density of∼10^(18)cm^(−3)is used,and its electrical performance is greatly enhanced after thermal annealing when 30-nm-thick gold electrodes are deposited.The results of performing XPS and Auger electron spectroscopy on samples before and after annealing show that the p-doping effect is due to the oxidation of selenide atoms,during which the gold acts as a critical catalytic element.This method is also shown to be valid for other 2D selenides including WSe_(2)and MoSe_(2),and the present findings offer new avenues for enriching the electrical properties of 2D selenides by means of annealing.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silico...Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silicon^([1,2]).As a repre-sentative TMD and a promising 2D channel material for high-performance,scalable p-type transistors,tungsten diselenide(WSe_(2))has attracted considerable academic and industrial interest for its potential in advanced complementary metal−oxide−semiconductor(CMOS)logic technology and in extending Moore’s Law^([3−7]).展开更多
Two-dimensional material has been widely investigated for potential applications in sensor and flexible electronics.In this work,a self-powered flexible humidity sensing device based on poly(vinyl alcohol)/Ti_(3)C_(2)...Two-dimensional material has been widely investigated for potential applications in sensor and flexible electronics.In this work,a self-powered flexible humidity sensing device based on poly(vinyl alcohol)/Ti_(3)C_(2)Tx(PVA/MXene)nanofibers film and monolayer molybdenum diselenide(MoSe2)piezoelectric nanogenerator(PENG)was reported for the first time.The monolayer MoSe_(2)-based PENG was fabricated by atmospheric pressure chemical vapor deposition techniques,which can generate a peak output of 35 mV and a power density of42 mW m^(-2).The flexible PENG integrated on polyethylene terephthalate(PET)substrate can harvest energy generated by different parts of human body and exhibit great application prospects in wearable devices.The electrospinned PVA/MXene nanofiber-based humidity sensor with flexible PET substrate under the driven of monolayer MoSe_(2) PENG,shows high response of~40,fast response/recovery time of 0.9/6.3 s,low hysteresis of 1.8%and excellent repeatability.The self-powered flexible humidity sensor yields the capability of detecting human skin moisture and ambient humidity.This work provides a pathway to explore the high-performance humidity sensor integrated with PENG for the self-powered flexible electronic devices.展开更多
The rapid development of two-dimensional(2D)transition-metal dichalcogenides has been possible owing to their special structures and remarkable properties.In particular,palladium diselenide(PdSe_(2))with a novel penta...The rapid development of two-dimensional(2D)transition-metal dichalcogenides has been possible owing to their special structures and remarkable properties.In particular,palladium diselenide(PdSe_(2))with a novel pentagonal structure and unique physical characteristics have recently attracted extensive research inter-est.Consequently,tremendous research progress has been achieved regarding the physics,chemistry,and electronics of PdSe_(2).Accordingly,in this review,we recapitulate and summarize the most recent research on PdSe_(2),including its structure,properties,synthesis,and appli-cations.First,a mechanical exfoliation method to obtain PdSe_(2) nanosheets is introduced,and large-area synthesis strate-gies are explained with respect to chemical vapor deposition and metal selenization.Next,the electronic and optoelectronic properties of PdSe_(2) and related hetero-structures,such as field-effect transistors,photodetectors,sensors,and thermoelec-tric devices,are discussed.Subsequently,the integration of systems into infrared image sensors on the basis of PdSe_(2) van der Waals heterostructures is explored.Finally,future opportunities are highlighted to serve as a general guide for physicists,chemists,materials scientists,and engineers.Therefore,this com-prehensive review may shed light on the research conducted by the 2D material community.展开更多
Homodimeric prodrug-based self-assembled nanoparticles,with carrier-free structure and ultrahigh drug loading,is drawing more and more attentions.Homodimeric prodrugs are composed of two drug molecules and a pivotal l...Homodimeric prodrug-based self-assembled nanoparticles,with carrier-free structure and ultrahigh drug loading,is drawing more and more attentions.Homodimeric prodrugs are composed of two drug molecules and a pivotal linkage.The influence of the linkages on the self-assembly,in vivo fate and antitumor activity of homodimeric prodrugs is the focus of research.Herein,three docetaxel(DTX)homodimeric prodrugs are developed using different lengths of diselenide bond-containing linkages.Interestingly,compared with the other two linkages,the longest diselenide bond-containing linkage could facilitate the self-delivery of DTX prodrugs,thus improving the stability,circulation time and tumor targeting of prodrug nanoassemblies.Besides,the extension of linkages reduces the redox-triggered drug release and cytotoxicity of prodrug nanoassemblies in tumor cells.Although the longest diselenide bond-containing prodrug nanoassemblies possessed the lowest cytotoxicity to 4T1 cells,their stable nanostructure maintained intact during circulation and achieve the maximum accumulation of DTX in tumor cells,which finally“turned the table”.Our study illustrates the crucial role of linkages in homodimeric prodrugs,and gives valuable proposal for the development of advanced nano-DDS for cancer treatment.展开更多
In recent years,emerging two-dimensional(2D)platinum diselenide(PtSe2)has quickly attracted the attention of the research community due to its novel physical and chemical properties.For the past few years,increasing r...In recent years,emerging two-dimensional(2D)platinum diselenide(PtSe2)has quickly attracted the attention of the research community due to its novel physical and chemical properties.For the past few years,increasing research achievements on 2D PtSe2 have been reported toward the fundamental science and various potential applications of PtSe2.In this review,the properties and structure characteristics of 2D PtSe2 are discussed at first.Then,the recent advances in synthesis of PtSe2 as well as their applications are reviewed.At last,potential perspectives in exploring the application of 2D PtSe2 are reviewed.展开更多
Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables R...Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables ReSe_(2)have an important application in optoelectronic devices.Here,we report the thickness-dependent exciton relaxation dynamics of mechanically exfoliated few-layer ReSe_(2)flakes by using time-resolved pump–probe transient transmission spectroscopies.The results reveal two thickness-dependent relaxation processes of the excitons.The fast one correlates with the exciton formation(i.e.,the conversion of hot carriers to excitons),while the slow one is attributed to the exciton recombination dominated by defect-assisted exciton trapping besides photon emission channel.The decrease of scattering probability caused by defects leads to the increase of fast lifetime with thickness,and the increase of slow lifetime with thickness is related to the trap-mediated exciton depopulation induced by surface defects.Polarization-dependent transient spectroscopy indicates the isotropic exciton dynamics in the two-dimensional(2D)plane.These results are insightful for better understanding of excitonic dynamics of ReSe_(2)materials and its application in future optoelectronic and electronic devices.展开更多
Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,contro...Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,controllable preparation of tantalum diselenide(TaSe2)remains challenging,which has hindered the exploration on its application in HER.Herein,we develop a facile method named surface-assisted chemical vapor transport(SACVT)for controllable synthesis of TaSe2 plates and nanobelts,by regulating the molar ratio of selenium to tantalum and reaction temperature.Unique quasi-arrays and self-supported structure help TaSe2 nanobelt own more active sites and higher ability of charge transfer,so it is superior to TaSe2 plate in electrocatalytic HER.Interestingly,they both exhibit the ability to optimize their morphologies upon cycling for dramatically improved and robust electrocatalytic performance.The selfoptimized structures can increase the effective active surface by exposing more active sites on the basal-planes and edges,shorten the interlayer electron-transfer pathways at a thinned domain,and accelerate the charge transfer,which mainly derive from high basal-plane activity and weak interaction between layers of metallic TaSe2.This work provides a reliable way for controllable synthesis of different TaSe2 structures,motivating further efforts to explore new high-efficiency catalysts in the large family of metallic TMDs for electrochemical energy conversion.展开更多
The atomic geometry, structure stability, electronic and magnetic properties of VSe2 were systematically investigated based on the density functional theory（DFT）. Varying from 3D to 2D four VSe2 structures, bulk 2H-...The atomic geometry, structure stability, electronic and magnetic properties of VSe2 were systematically investigated based on the density functional theory（DFT）. Varying from 3D to 2D four VSe2 structures, bulk 2H-VSe2 and 1T-VSe2, monolayer H-VSe2 and T-VSe2 are all demonstrated as thermodynamically stable by lattice dynamic calculations. More interestingly, the phase transition temperature is dramatically different due to the lattice size. Finally, owing to different crystal structures, H-VSe2 is semimetallic whereas T-VSe2 is totally metallic and also they have different magnetic moments. Our main argument is that being exfoliated from bulk to monolayer, 2H-VSe2 transforms to T-VSe2, accompanied by both semimetallic-metallic transition and dramatic magnetic moment variation. Our calculations provide a novel structure phase transition and an efficient way to modulate the electronic structure and magnetic moment of layered VSe2, which suggests potential applications as high-performance functional nanomaterial.展开更多
Two-way shape memory polymeric aerogels(2W-SMPAs),with the ability to undergo reversible shape deformation in response to external stimuli,have extensive application in diverse fields such as actuators,sensors,robotic...Two-way shape memory polymeric aerogels(2W-SMPAs),with the ability to undergo reversible shape deformation in response to external stimuli,have extensive application in diverse fields such as actuators,sensors,robotics,and other relevant domains.In this study,we introduce a novel approach for fabricating a 2W-SMPA material based on liquid crystal elastomers(LCEs)incorporating dynamic diselenide bonds.The aerogel exhibits liquid crystal phases,excellent compressibility and shape stability,and the mesogens are uniaxial-oriented along the stretching direction.By capitalizing on the dynamic diselenide bonds,the LCEbased aerogel demonstrated remarkable reprogrammability,weldability,and recyclability through thermal reorganization.The shape-programmed aerogel sample exhibits reversible shrinking deformation during the heating and cooling cycles,ultimately achieving a maximum shrinkage ratio of 26.1%.Moreover,the LCE-based aerogel's porous structure and monodomain orientation effectively enable the adsorption of the photothermal dye DR1 and facilitated the reversible photothermal-induced shape deformation when exposed to 520 nm light irradiation.These findings reveal the potential application of this innovative LCE-based aerogel material,enabled by dynamic diselenide bonds,in various areas including control devices,soft actuators,and other diverse fields.展开更多
An intramolecular selenocyclizations of olefins mediated by a commercially available hypervalent iodine(Ⅲ) reagent,PhIO,was developed.This method provided access to a wide range of selenenylated heterocycles under am...An intramolecular selenocyclizations of olefins mediated by a commercially available hypervalent iodine(Ⅲ) reagent,PhIO,was developed.This method provided access to a wide range of selenenylated heterocycles under ambient conditions.The striking advantages of this protocol over all previous methods include mild reaction conditions,easy operation,good yields,high levels of functional group compatibility,large-scale application and suitability for the late-stage functionalization of complex molecules of biological importance.展开更多
A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethyls...A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethylsilyl chloride under mild conditions. Presumably, the diselenides are cleaved by Sm/TMSCI system to form selemde anions, which then undergo SN2＇ substitution of Baylis-Hillman adducts to produce the （Z）-allyl selenides.展开更多
A facile and efficient electrochemical method for sustainable constructing both selanyl phenanthrenes and selanyl polycyclic heteroaromatics(32 examples,71%-97%yields)through the radical annulation of 2-alkynyl biaryl...A facile and efficient electrochemical method for sustainable constructing both selanyl phenanthrenes and selanyl polycyclic heteroaromatics(32 examples,71%-97%yields)through the radical annulation of 2-alkynyl biaryls and 2-heteroaryl-substituted alkynyl benzenes with diselenides at ambient temperature under additive-,chemical oxidant-,catalyst-free and mild conditions was established.展开更多
The Se-Se bond in diaryl diselenides was reduced by Zn/ZrCl4 system to produce selenide anions, which react with acyl chlorides or acid anhydrides to afford selenoesters in THF under mild and neutral conditions.
The reduction of diacyl diselenides by samarium diiodide led to the production ofsamarium acylselenolates, which reacted with a,β-unsaturated esters or nitriles to give β-selenoesters or selenonitriles under mild an...The reduction of diacyl diselenides by samarium diiodide led to the production ofsamarium acylselenolates, which reacted with a,β-unsaturated esters or nitriles to give β-selenoesters or selenonitriles under mild and neutral conditions.展开更多
A novel diselenide-containing crown ether(BC7Se_(2))was fabricated,which can polymerize to form cyclic oligomers through intermolecular dynamic covalent reaction by irradiation of visible light.The size and distributi...A novel diselenide-containing crown ether(BC7Se_(2))was fabricated,which can polymerize to form cyclic oligomers through intermolecular dynamic covalent reaction by irradiation of visible light.The size and distribution of oligomers are related to the monomer concentration.The decomposition reaction of oligomers is controlled by topology and solvents.Furthermore,potassium cation can inhibit the polymerization of BC7Se_(2)and accelerate the decomposition of oligomers.展开更多
KBr or NaCl is found to be a good catalyst in Se-Se bond cleavage of diselenides in the present of the oxidant mCPBA.The electrophilic addition of the in situ generated reactive electrophilic selenium species PhSeX（X...KBr or NaCl is found to be a good catalyst in Se-Se bond cleavage of diselenides in the present of the oxidant mCPBA.The electrophilic addition of the in situ generated reactive electrophilic selenium species PhSeX（X = Br,Cl） to alkenes in AcOH provides a convenient access to 2-acetoxy-1-selenides.Compared with other catalysts,KBr or NaCl is less expensive and more environment-friendly.展开更多
Organoseleniums are a class of compounds attracting attention across the globe owing to their Glutathione peroxidase(GPx)mimicry,which confers on them a strong antioxidant activity.Diphenyl diselenide(DPDS)is an Organ...Organoseleniums are a class of compounds attracting attention across the globe owing to their Glutathione peroxidase(GPx)mimicry,which confers on them a strong antioxidant activity.Diphenyl diselenide(DPDS)is an Organoselenium whose GPx mimetic property has been suggested to rely on the oxidation of non-protein or protein thiols critical to the activities of some sulfhydryl enzymes.This study,therefore investigated the GPx mimic/antioxidant property of DPDS as well as the role of thiols of two key sulfhydryl enzymes,cerebral Na^(+)/K^(+)-ATPase(sodium pump)and hepatic delta-aminolevulinic acid dehydratase(δ-ALAD)in the GPx mimicry of DPDS.Albino Wistar rats were euthanized,and the liver and brain were removed and used to assay for the effect of DPDS on lipid peroxidation induced by two prooxidants[Fe2^(+)(10μM)and H2O2,(1 mM)]as well as the activities of the sulfhydryl enzymes.The results revealed that DPDS profoundly(P<0.05)counteracted Fe2^(+)and H2O2-induced lipid peroxidation in the rats’hepatic and cerebral tissues.Furthermore,the results of assay systems for lipid peroxidation and sodium pump revealed that DPDS inhibited Na^(+)/K^(+)-ATPase and lipid peroxidation in the brain tissue homogenates in the same reaction system.A similar result was obtained in the assay system for lipid peroxidation and hepaticδ-ALAD as DPDS simultaneously inhibited the enzyme’s activity and lipid peroxidation.This suggests that the GPx mimetic property of DPDS may be linked to the enzymes’loss of activity,which further validates the suggestions that the enzymes’inhibition,as well as the antioxidant action of DPDS,rely on the oxidation of critical thiols of the enzymes.However,the GPx mimicry of DPDS should be investigated in the presence of thiol-blocking or oxidizing agents in biological systems in order to further ascertain the role of protein thiols.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.52075385 and 12034001)the National Key R&D Program(Grant No.2018YFA0307200)the 111 Project(Grant No.B07014).
文摘Two-dimensional transition metal dichalcogenides(TMDs)show great promise for developing the next generation of electronic and optoelectronic devices.However,most TMDs have n-type or n-dominant bipolar characteristics,and this severely limits their potential for being designed as multi-functional heterostructures.Recently,thermal annealing has been reported as an easy means of p-doping TMDs,but the mechanism remains ambiguous,thereby preventing reliable outcomes and it becoming a mature doping technology for TMDs.Here,the mechanism of thermal annealing for p-doping a 2D selenide is investigated thoroughly,revealing the key role of the catalytic effect of nano-thick gold electrodes in achieving p-doping.As an example,2D SnSe_(2)with a fairly high electron density of∼10^(18)cm^(−3)is used,and its electrical performance is greatly enhanced after thermal annealing when 30-nm-thick gold electrodes are deposited.The results of performing XPS and Auger electron spectroscopy on samples before and after annealing show that the p-doping effect is due to the oxidation of selenide atoms,during which the gold acts as a critical catalytic element.This method is also shown to be valid for other 2D selenides including WSe_(2)and MoSe_(2),and the present findings offer new avenues for enriching the electrical properties of 2D selenides by means of annealing.
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silicon^([1,2]).As a repre-sentative TMD and a promising 2D channel material for high-performance,scalable p-type transistors,tungsten diselenide(WSe_(2))has attracted considerable academic and industrial interest for its potential in advanced complementary metal−oxide−semiconductor(CMOS)logic technology and in extending Moore’s Law^([3−7]).
基金supported by the National Natural Science Foundation of China(51777215)National Natural Science Foundation of China(51775306)+1 种基金Beijing Municipal Natural Science Foundation(4192027)the Graduate Innovation Fund of China University of Petroleum(YCX2020097)。
文摘Two-dimensional material has been widely investigated for potential applications in sensor and flexible electronics.In this work,a self-powered flexible humidity sensing device based on poly(vinyl alcohol)/Ti_(3)C_(2)Tx(PVA/MXene)nanofibers film and monolayer molybdenum diselenide(MoSe2)piezoelectric nanogenerator(PENG)was reported for the first time.The monolayer MoSe_(2)-based PENG was fabricated by atmospheric pressure chemical vapor deposition techniques,which can generate a peak output of 35 mV and a power density of42 mW m^(-2).The flexible PENG integrated on polyethylene terephthalate(PET)substrate can harvest energy generated by different parts of human body and exhibit great application prospects in wearable devices.The electrospinned PVA/MXene nanofiber-based humidity sensor with flexible PET substrate under the driven of monolayer MoSe_(2) PENG,shows high response of~40,fast response/recovery time of 0.9/6.3 s,low hysteresis of 1.8%and excellent repeatability.The self-powered flexible humidity sensor yields the capability of detecting human skin moisture and ambient humidity.This work provides a pathway to explore the high-performance humidity sensor integrated with PENG for the self-powered flexible electronic devices.
基金H.L.acknowledges the National Key Research and Development Program of China(2017YFB0405400)from the Ministry of Science and Technology(MOST)of Chinathe Natural Science Foundation for Distinguished Young Scientist of Shandong Province(Grant No.JQ201814)+6 种基金We thank the Project of“20 items of University”of Jinan(2018GXRC031)W.Z thanks Taishan Scholars Project Special Funds(tsqn201812083)and NSFC(No.52022037)The authors show their gratitude to the National Natural Science Foundation of China(NSFC grant No.51802113,51802116)the Natural Science Foundation of Shandong Province,China(grant No.ZR2019BEM040,ZR2018BEM015)M.H.R.thanks the National Science Foundation China(NSFC,Project 52071225)the National Science Center and the Czech Republic under the ERDF program“Institute of Environmental Technology-Excellent Research”(No.CZ.02.1.01/0.0/0.0/16_019/0000853)the Sino-German Research Institute for support(Project No.GZ 1400).
文摘The rapid development of two-dimensional(2D)transition-metal dichalcogenides has been possible owing to their special structures and remarkable properties.In particular,palladium diselenide(PdSe_(2))with a novel pentagonal structure and unique physical characteristics have recently attracted extensive research inter-est.Consequently,tremendous research progress has been achieved regarding the physics,chemistry,and electronics of PdSe_(2).Accordingly,in this review,we recapitulate and summarize the most recent research on PdSe_(2),including its structure,properties,synthesis,and appli-cations.First,a mechanical exfoliation method to obtain PdSe_(2) nanosheets is introduced,and large-area synthesis strate-gies are explained with respect to chemical vapor deposition and metal selenization.Next,the electronic and optoelectronic properties of PdSe_(2) and related hetero-structures,such as field-effect transistors,photodetectors,sensors,and thermoelec-tric devices,are discussed.Subsequently,the integration of systems into infrared image sensors on the basis of PdSe_(2) van der Waals heterostructures is explored.Finally,future opportunities are highlighted to serve as a general guide for physicists,chemists,materials scientists,and engineers.Therefore,this com-prehensive review may shed light on the research conducted by the 2D material community.
基金This work was supported by China Postdoctoral Innovative Talents Support Program(no.BX20190219)China Postdoctoral Science Foundation(no.2019M661134)National Natural Science Foundation of China(no.81872816).
文摘Homodimeric prodrug-based self-assembled nanoparticles,with carrier-free structure and ultrahigh drug loading,is drawing more and more attentions.Homodimeric prodrugs are composed of two drug molecules and a pivotal linkage.The influence of the linkages on the self-assembly,in vivo fate and antitumor activity of homodimeric prodrugs is the focus of research.Herein,three docetaxel(DTX)homodimeric prodrugs are developed using different lengths of diselenide bond-containing linkages.Interestingly,compared with the other two linkages,the longest diselenide bond-containing linkage could facilitate the self-delivery of DTX prodrugs,thus improving the stability,circulation time and tumor targeting of prodrug nanoassemblies.Besides,the extension of linkages reduces the redox-triggered drug release and cytotoxicity of prodrug nanoassemblies in tumor cells.Although the longest diselenide bond-containing prodrug nanoassemblies possessed the lowest cytotoxicity to 4T1 cells,their stable nanostructure maintained intact during circulation and achieve the maximum accumulation of DTX in tumor cells,which finally“turned the table”.Our study illustrates the crucial role of linkages in homodimeric prodrugs,and gives valuable proposal for the development of advanced nano-DDS for cancer treatment.
基金This work is supported by the Science and Technology Innovation Commission of Shenzhen(JCYJ20190808142415003)National Natural Science Foundation of China(Grant Nos.61905161,61875138,and 61961136001)the Shenzhen Nanshan District Pilotage Team Program(LHTD20170006).
文摘In recent years,emerging two-dimensional(2D)platinum diselenide(PtSe2)has quickly attracted the attention of the research community due to its novel physical and chemical properties.For the past few years,increasing research achievements on 2D PtSe2 have been reported toward the fundamental science and various potential applications of PtSe2.In this review,the properties and structure characteristics of 2D PtSe2 are discussed at first.Then,the recent advances in synthesis of PtSe2 as well as their applications are reviewed.At last,potential perspectives in exploring the application of 2D PtSe2 are reviewed.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12074202,12174207,and 11974190)the Natural Science Foundation of Tianjin City(Grant Nos.20JCQNJC00020 and 22JCYBJC00390)。
文摘Rhenium diselenide(ReSe_(2))has gathered much attention due to its low symmetry of lattice structure,which makes it possess in-plane anisotropic optical,electrical as well as excitonic properties and further enables ReSe_(2)have an important application in optoelectronic devices.Here,we report the thickness-dependent exciton relaxation dynamics of mechanically exfoliated few-layer ReSe_(2)flakes by using time-resolved pump–probe transient transmission spectroscopies.The results reveal two thickness-dependent relaxation processes of the excitons.The fast one correlates with the exciton formation(i.e.,the conversion of hot carriers to excitons),while the slow one is attributed to the exciton recombination dominated by defect-assisted exciton trapping besides photon emission channel.The decrease of scattering probability caused by defects leads to the increase of fast lifetime with thickness,and the increase of slow lifetime with thickness is related to the trap-mediated exciton depopulation induced by surface defects.Polarization-dependent transient spectroscopy indicates the isotropic exciton dynamics in the two-dimensional(2D)plane.These results are insightful for better understanding of excitonic dynamics of ReSe_(2)materials and its application in future optoelectronic and electronic devices.
基金supported by the Beijing Natural Science Foundation(2172027)the Tsinghua University Initiative Scientific Research Program+3 种基金the National Natural Science Foundation of China(21802154)the Fund of Key Laboratory of Advanced Materials of Ministry of Education(2018AML05)the Foundation of Director of the Technical Institute of Physics and Chemistry of CASthe Youth Innovation Promotion Association of the CAS(2019026)
文摘Metallic layered transition metal dichalcogenides(TMDs)nanomaterials based on Group 5 transition metals are attracting substantial interests as alternative catalysts for hydrogen evolution reaction(HER).However,controllable preparation of tantalum diselenide(TaSe2)remains challenging,which has hindered the exploration on its application in HER.Herein,we develop a facile method named surface-assisted chemical vapor transport(SACVT)for controllable synthesis of TaSe2 plates and nanobelts,by regulating the molar ratio of selenium to tantalum and reaction temperature.Unique quasi-arrays and self-supported structure help TaSe2 nanobelt own more active sites and higher ability of charge transfer,so it is superior to TaSe2 plate in electrocatalytic HER.Interestingly,they both exhibit the ability to optimize their morphologies upon cycling for dramatically improved and robust electrocatalytic performance.The selfoptimized structures can increase the effective active surface by exposing more active sites on the basal-planes and edges,shorten the interlayer electron-transfer pathways at a thinned domain,and accelerate the charge transfer,which mainly derive from high basal-plane activity and weak interaction between layers of metallic TaSe2.This work provides a reliable way for controllable synthesis of different TaSe2 structures,motivating further efforts to explore new high-efficiency catalysts in the large family of metallic TMDs for electrochemical energy conversion.
基金Funded by the National Natural Science Foundation of China(No.11547115)the Science Research Foundation for Ph D of Liaoning Province(No.201501091)
文摘The atomic geometry, structure stability, electronic and magnetic properties of VSe2 were systematically investigated based on the density functional theory（DFT）. Varying from 3D to 2D four VSe2 structures, bulk 2H-VSe2 and 1T-VSe2, monolayer H-VSe2 and T-VSe2 are all demonstrated as thermodynamically stable by lattice dynamic calculations. More interestingly, the phase transition temperature is dramatically different due to the lattice size. Finally, owing to different crystal structures, H-VSe2 is semimetallic whereas T-VSe2 is totally metallic and also they have different magnetic moments. Our main argument is that being exfoliated from bulk to monolayer, 2H-VSe2 transforms to T-VSe2, accompanied by both semimetallic-metallic transition and dramatic magnetic moment variation. Our calculations provide a novel structure phase transition and an efficient way to modulate the electronic structure and magnetic moment of layered VSe2, which suggests potential applications as high-performance functional nanomaterial.
基金the National Natural Science Foundation of China(No.22325501,21971037,52173109).
文摘Two-way shape memory polymeric aerogels(2W-SMPAs),with the ability to undergo reversible shape deformation in response to external stimuli,have extensive application in diverse fields such as actuators,sensors,robotics,and other relevant domains.In this study,we introduce a novel approach for fabricating a 2W-SMPA material based on liquid crystal elastomers(LCEs)incorporating dynamic diselenide bonds.The aerogel exhibits liquid crystal phases,excellent compressibility and shape stability,and the mesogens are uniaxial-oriented along the stretching direction.By capitalizing on the dynamic diselenide bonds,the LCEbased aerogel demonstrated remarkable reprogrammability,weldability,and recyclability through thermal reorganization.The shape-programmed aerogel sample exhibits reversible shrinking deformation during the heating and cooling cycles,ultimately achieving a maximum shrinkage ratio of 26.1%.Moreover,the LCE-based aerogel's porous structure and monodomain orientation effectively enable the adsorption of the photothermal dye DR1 and facilitated the reversible photothermal-induced shape deformation when exposed to 520 nm light irradiation.These findings reveal the potential application of this innovative LCE-based aerogel material,enabled by dynamic diselenide bonds,in various areas including control devices,soft actuators,and other diverse fields.
基金supported by the Natural Science Foundation of Jiangsu Province (No.BK20170439)Science and Technology Plan Projects of Nantong (Nos.JC2019102 and JC2020072)。
文摘An intramolecular selenocyclizations of olefins mediated by a commercially available hypervalent iodine(Ⅲ) reagent,PhIO,was developed.This method provided access to a wide range of selenenylated heterocycles under ambient conditions.The striking advantages of this protocol over all previous methods include mild reaction conditions,easy operation,good yields,high levels of functional group compatibility,large-scale application and suitability for the late-stage functionalization of complex molecules of biological importance.
基金Project (No. 2004C21032) supported by the Key Technologies R &D Program of Zhejiang Province, China
文摘A simple and convenient procedure for stercoselective synthesis of （Z）-allyl selenides has been developed by a one-pot reaction of diselenides with Baylis-Hillman adducts in the presence of samarium metal-trimethylsilyl chloride under mild conditions. Presumably, the diselenides are cleaved by Sm/TMSCI system to form selemde anions, which then undergo SN2＇ substitution of Baylis-Hillman adducts to produce the （Z）-allyl selenides.
基金funded by the Scientific Research Fund of Hunan Provincial Education Department(No.22B0435).
文摘A facile and efficient electrochemical method for sustainable constructing both selanyl phenanthrenes and selanyl polycyclic heteroaromatics(32 examples,71%-97%yields)through the radical annulation of 2-alkynyl biaryls and 2-heteroaryl-substituted alkynyl benzenes with diselenides at ambient temperature under additive-,chemical oxidant-,catalyst-free and mild conditions was established.
文摘The Se-Se bond in diaryl diselenides was reduced by Zn/ZrCl4 system to produce selenide anions, which react with acyl chlorides or acid anhydrides to afford selenoesters in THF under mild and neutral conditions.
文摘The reduction of diacyl diselenides by samarium diiodide led to the production ofsamarium acylselenolates, which reacted with a,β-unsaturated esters or nitriles to give β-selenoesters or selenonitriles under mild and neutral conditions.
基金financial support from the National Natural Science Foundation of China(Nos.21901210,21901209,22071196,22007078)Natural Science Foundation of Shaanxi Province of China(No.2019JQ-626)+3 种基金Postdoctoral Innovative Talents Supporting Project of China(No.BX20180255)Key R&D Program of Shaanxi Province(Nos.2019KW-031,2019KW-038)Fundamental Research Funds for the Central Universities(Nos.3102019smxy001,3102018zy051,3102018jcc007,3102017OQD045,3102017OQD040,3102017OQD115,3102019ghxm005)State Key Laboratory of Solidification Processing in NPU(No.SKLSP201817)。
文摘A novel diselenide-containing crown ether(BC7Se_(2))was fabricated,which can polymerize to form cyclic oligomers through intermolecular dynamic covalent reaction by irradiation of visible light.The size and distribution of oligomers are related to the monomer concentration.The decomposition reaction of oligomers is controlled by topology and solvents.Furthermore,potassium cation can inhibit the polymerization of BC7Se_(2)and accelerate the decomposition of oligomers.
文摘KBr or NaCl is found to be a good catalyst in Se-Se bond cleavage of diselenides in the present of the oxidant mCPBA.The electrophilic addition of the in situ generated reactive electrophilic selenium species PhSeX（X = Br,Cl） to alkenes in AcOH provides a convenient access to 2-acetoxy-1-selenides.Compared with other catalysts,KBr or NaCl is less expensive and more environment-friendly.
文摘Organoseleniums are a class of compounds attracting attention across the globe owing to their Glutathione peroxidase(GPx)mimicry,which confers on them a strong antioxidant activity.Diphenyl diselenide(DPDS)is an Organoselenium whose GPx mimetic property has been suggested to rely on the oxidation of non-protein or protein thiols critical to the activities of some sulfhydryl enzymes.This study,therefore investigated the GPx mimic/antioxidant property of DPDS as well as the role of thiols of two key sulfhydryl enzymes,cerebral Na^(+)/K^(+)-ATPase(sodium pump)and hepatic delta-aminolevulinic acid dehydratase(δ-ALAD)in the GPx mimicry of DPDS.Albino Wistar rats were euthanized,and the liver and brain were removed and used to assay for the effect of DPDS on lipid peroxidation induced by two prooxidants[Fe2^(+)(10μM)and H2O2,(1 mM)]as well as the activities of the sulfhydryl enzymes.The results revealed that DPDS profoundly(P<0.05)counteracted Fe2^(+)and H2O2-induced lipid peroxidation in the rats’hepatic and cerebral tissues.Furthermore,the results of assay systems for lipid peroxidation and sodium pump revealed that DPDS inhibited Na^(+)/K^(+)-ATPase and lipid peroxidation in the brain tissue homogenates in the same reaction system.A similar result was obtained in the assay system for lipid peroxidation and hepaticδ-ALAD as DPDS simultaneously inhibited the enzyme’s activity and lipid peroxidation.This suggests that the GPx mimetic property of DPDS may be linked to the enzymes’loss of activity,which further validates the suggestions that the enzymes’inhibition,as well as the antioxidant action of DPDS,rely on the oxidation of critical thiols of the enzymes.However,the GPx mimicry of DPDS should be investigated in the presence of thiol-blocking or oxidizing agents in biological systems in order to further ascertain the role of protein thiols.
