High-performance white light-emitting diodes (WLEDs) hold great potential for the next-generation backlight display applications.However,achieving highly efficient and stable WLEDs with wide-color-gamut has remained a...High-performance white light-emitting diodes (WLEDs) hold great potential for the next-generation backlight display applications.However,achieving highly efficient and stable WLEDs with wide-color-gamut has remained a formidable goal.Reported here is the first example of pure red narrow bandwidth emission triangular CQDs (PR-NBE-T-CQDs) with photoluminescence peaking at 610 nm.The PR-NBE-T-CQDs synthesized from resorcinol show high quantum yield (QY) of 72% with small full width at half maximum of 33 nm.By simply controlling the reaction time,pure green (PG-) NBE-T-CQDs with high QY of 75% were also obtained.Highly efficient and stable WLEDs with wide-color-gamut based on PR- and PG-NBE-T-CQDs was achieved.This WLED showed a remarkable wide-color gamut of 110% NTSC and high power efficiency of 86.5 lumens per Watt.Furthermore,such WLEDs demonstrate outstanding stability.This work will set the stage for developing highly efficient,low cost and environment-friendly WLEDs based on CQDs for the next-generation wide-color gamut backlight displays.展开更多
Oral drug delivery,which requires surviving the harsh environment in the gastrointestinal(Gl)tract and penetrating the intestinal epithelium,has not bee n achieved using simple formulatio n nan oparticles(NPs).Medici ...Oral drug delivery,which requires surviving the harsh environment in the gastrointestinal(Gl)tract and penetrating the intestinal epithelium,has not bee n achieved using simple formulatio n nan oparticles(NPs).Medici nal natural products(MNPs)have bee n widely used in traditi onal medicine for disease management through oral consumption.However,most pharmacologically active compounds within MNPs do not have the properties suitable for oral applicatio ns.We hypothesize that some MNPs contain n atural nano materials that can convert those compounds into oral formulations by forming NPs.After screening 66 MNPs,we identified five classes of small molecules that form NPs,many of which are capable of efficient drug encapsulation and Gl penetration.We show that one of them,dehydrotrametenolic acid(DTA),is capable of mediating oral delivery for effective disease treatment.We determined that DTA NPs assemble through hydrogen bonding and penetra怕the Gl tract via apical sodium-depe ndent bile acid tran sporter.Our study reveals a no vel class of single comp orient,small molecule-assembled NPs for oral drug delivery,and suggests a n ovel approach to modernizi ng MNPs through nano material discovery.展开更多
With practical electrocatalytic hydrogen production frequently involving the splitting of water in various pH media,there is an urgent need but still a technical challenge to develop low-cost,highly active,and stable ...With practical electrocatalytic hydrogen production frequently involving the splitting of water in various pH media,there is an urgent need but still a technical challenge to develop low-cost,highly active,and stable electrocatalysts for pH-universal hydrogen evolution reaction(HER).We report herein the adoption of a hydrothermal reaction combined with a post gas-phase doping strategy to fabricate P-doped NiCo_(2)Se_(4) hollow nanoneedle arrays on carbon fiber paper(i.e.,P-NiCo_(2)Se_(4)/CFP).Notably,the optimal arrays(P8.71-NiCo_(2)Se_(4)/CFP)can afford an outstanding pH-universal HER performance,with an overpotential as low as 33,57,and 69 mV at 10 mA·cm^(−2) and corresponding Tafel slopes down to 52,61,and 72 mV·dec^(−1) in acidic,alkaline,and neutral media,respectively,outperforming most state-of-the-art nonprecious catalysts and even the commercial Pt/C catalyst in both neutral and alkaline media at large current densities.Impressively,P_(8.71-)NiCo_(2)Se_(4)/CFP also displays good durability toward long-time stability testing in harsh acidic and alkaline electrolytes.Experimental and theoretical studies further reveal that the doping of P atoms into NiCo_(2)Se_(4) can simultaneously optimize its H*adsorption/desorption energy,water adsorption energy,and water dissociation energy by adjusting the local electronic states of various active sites,thus accelerating the rate-determining step of HER in different pH media to endow P-NiCo_(2)Se_(4) with an outstanding pH-universal HER performance.This work provides atomic-level insights into the roles of active sites in various electrolysis environments,thereby shedding new light on the rational design of highly efficient pH-universal nonprecious catalysts for HER and beyond.展开更多
Sulfur(S)-doped graphene sheets were prepared by a facile electrochemical method, which effectively combined exfoliation of graphite and in situ S doping of graphene together. The metal-free S-doped graphene sheets ex...Sulfur(S)-doped graphene sheets were prepared by a facile electrochemical method, which effectively combined exfoliation of graphite and in situ S doping of graphene together. The metal-free S-doped graphene sheets exhibit high electrocatalytic activity, long-term stability, and excellent tolerance to cross-over effects of methanol in alkaline media for the oxygen reduction reaction(ORR), indicating that these S-doped graphene sheets possess great potential for a substitute for Pt-based catalysts in fuel cells.展开更多
As a new type of nanomaterial,carbon dots(CDs)have been recognized as a versatile nanoplatform with enormous potential for biomedical and optoelectronic applications because of low cytotoxicity,photostability,biocompa...As a new type of nanomaterial,carbon dots(CDs)have been recognized as a versatile nanoplatform with enormous potential for biomedical and optoelectronic applications because of low cytotoxicity,photostability,biocompatibility and versatility in addition to their tunable photoluminescence.In this review,we aim at updating the latest research on preparation,optoelectronic and chemical properties of CDs as well as their biomedical and optoelectronic applications.We highlight the applications of CDs for stem cell imaging,cell nucleus imaging,two-photon fluorescence imaging,tumor diagnosis and therapy and their optoelectronic applications including light-emitting diodes(LEDs),solar cells and electrocatalysis.Furthermore,we also discuss current challenges and breakthroughs on machine-learning-driven synthesis of CDs as well as nucleic acid detection with an eye towards the future.Finally,we hope that this review will give further impulses to target-oriented research on CDs for biomedical and optoelectronic applications.展开更多
Two-dimensional(2D)atomically thin quantum dots(QDs)possess extraordinary electrical and optical properties.However,fabricating high quality 2D QDs via a universal and reliable technique remains a challenge.Here,we re...Two-dimensional(2D)atomically thin quantum dots(QDs)possess extraordinary electrical and optical properties.However,fabricating high quality 2D QDs via a universal and reliable technique remains a challenge.Here,we report a simple strategy to prepare high quality,monolayer single crystal 2D QDs via ultrathin cutting 2D bulk single crystals by ultramicrotome,followed by an exfoliation process.The as-prepared 2D QDs have pristine surface,high quality,high monolayer yield and high photoluminescence quantum yield(the highest photoluminescence quantum yield of WS2 is18%),which can be used as promising,low toxic,biocompatible,and good cell-permeability fluorescent labeling agents for in vitro imaging.展开更多
In the version of this article originally published,Figs.2(d)and 3(a),and Figs.S3 and S6 in the Electronic Supplementary Material(ESM)were incorrect.The corrected images are shown below.
In recent years,carbon dots(CDs),including carbon nanodots,carbonized polymer dots,carbon quantum dots,and graphene quantum dots have attracted a mounting interest as readily accessible,nontoxic,and relatively inexpen...In recent years,carbon dots(CDs),including carbon nanodots,carbonized polymer dots,carbon quantum dots,and graphene quantum dots have attracted a mounting interest as readily accessible,nontoxic,and relatively inexpensive carbon-based nanomaterials.Yet,despite intense research for a number of years,a unifying picture is still lacking to clarify the exact definition,clear chemical structure,and unique optical properties of this family of nanomaterials.In this review,we systematically summarize the recent development of CDs from molecular design to related properties of excited states as well as their applications in optoelectronic devices and biology.We point out the current challenges,including exploring precise synthesis,clarifying the structure-property relationship,and regulating singlet and triplet states of fluorescence,phosphorescence,and delayed fluorescence.Moreover,the structural optimization of optoelectronic devices,tumor targeting mechanism,selective imaging,and drug delivery of CDs are also highlighted.We hope that the information provided in this review will inspire more exciting research on CDs from a brand-new perspective and promote practical application of CDs in multiple directions of current and future research.展开更多
基金supported by the National Natural Science Foundation of China (NSFC)(Nos.21573019 and 21872010)the Major Research Plan of the National Natural Science Foundation of China (No.21233003)the Fundamental Research Funds for the Central Universities.
文摘High-performance white light-emitting diodes (WLEDs) hold great potential for the next-generation backlight display applications.However,achieving highly efficient and stable WLEDs with wide-color-gamut has remained a formidable goal.Reported here is the first example of pure red narrow bandwidth emission triangular CQDs (PR-NBE-T-CQDs) with photoluminescence peaking at 610 nm.The PR-NBE-T-CQDs synthesized from resorcinol show high quantum yield (QY) of 72% with small full width at half maximum of 33 nm.By simply controlling the reaction time,pure green (PG-) NBE-T-CQDs with high QY of 75% were also obtained.Highly efficient and stable WLEDs with wide-color-gamut based on PR- and PG-NBE-T-CQDs was achieved.This WLED showed a remarkable wide-color gamut of 110% NTSC and high power efficiency of 86.5 lumens per Watt.Furthermore,such WLEDs demonstrate outstanding stability.This work will set the stage for developing highly efficient,low cost and environment-friendly WLEDs based on CQDs for the next-generation wide-color gamut backlight displays.
基金This work was supported by NIH(Nos.NS095817(J.Z.)and 18TPA34170180(J.Z.))the National Natural Science Foundation of China(NSFC)(Nos.31770614(C.M.),21233003(L.F.),and 21573019(L.F.)).
文摘Oral drug delivery,which requires surviving the harsh environment in the gastrointestinal(Gl)tract and penetrating the intestinal epithelium,has not bee n achieved using simple formulatio n nan oparticles(NPs).Medici nal natural products(MNPs)have bee n widely used in traditi onal medicine for disease management through oral consumption.However,most pharmacologically active compounds within MNPs do not have the properties suitable for oral applicatio ns.We hypothesize that some MNPs contain n atural nano materials that can convert those compounds into oral formulations by forming NPs.After screening 66 MNPs,we identified five classes of small molecules that form NPs,many of which are capable of efficient drug encapsulation and Gl penetration.We show that one of them,dehydrotrametenolic acid(DTA),is capable of mediating oral delivery for effective disease treatment.We determined that DTA NPs assemble through hydrogen bonding and penetra怕the Gl tract via apical sodium-depe ndent bile acid tran sporter.Our study reveals a no vel class of single comp orient,small molecule-assembled NPs for oral drug delivery,and suggests a n ovel approach to modernizi ng MNPs through nano material discovery.
基金supported by the National Natural Science Foundation of China(Nos.21872011 and 21273020).
文摘With practical electrocatalytic hydrogen production frequently involving the splitting of water in various pH media,there is an urgent need but still a technical challenge to develop low-cost,highly active,and stable electrocatalysts for pH-universal hydrogen evolution reaction(HER).We report herein the adoption of a hydrothermal reaction combined with a post gas-phase doping strategy to fabricate P-doped NiCo_(2)Se_(4) hollow nanoneedle arrays on carbon fiber paper(i.e.,P-NiCo_(2)Se_(4)/CFP).Notably,the optimal arrays(P8.71-NiCo_(2)Se_(4)/CFP)can afford an outstanding pH-universal HER performance,with an overpotential as low as 33,57,and 69 mV at 10 mA·cm^(−2) and corresponding Tafel slopes down to 52,61,and 72 mV·dec^(−1) in acidic,alkaline,and neutral media,respectively,outperforming most state-of-the-art nonprecious catalysts and even the commercial Pt/C catalyst in both neutral and alkaline media at large current densities.Impressively,P_(8.71-)NiCo_(2)Se_(4)/CFP also displays good durability toward long-time stability testing in harsh acidic and alkaline electrolytes.Experimental and theoretical studies further reveal that the doping of P atoms into NiCo_(2)Se_(4) can simultaneously optimize its H*adsorption/desorption energy,water adsorption energy,and water dissociation energy by adjusting the local electronic states of various active sites,thus accelerating the rate-determining step of HER in different pH media to endow P-NiCo_(2)Se_(4) with an outstanding pH-universal HER performance.This work provides atomic-level insights into the roles of active sites in various electrolysis environments,thereby shedding new light on the rational design of highly efficient pH-universal nonprecious catalysts for HER and beyond.
基金supported by the National Natural Science Foundation of China(21073018)the Major Research Plan of the National Natural Science Foundation of China(21233003)the Fundamental Research Funds for the Central Universities,Key Laboratory of Theoretical and Computational Photochemistry
文摘Sulfur(S)-doped graphene sheets were prepared by a facile electrochemical method, which effectively combined exfoliation of graphite and in situ S doping of graphene together. The metal-free S-doped graphene sheets exhibit high electrocatalytic activity, long-term stability, and excellent tolerance to cross-over effects of methanol in alkaline media for the oxygen reduction reaction(ORR), indicating that these S-doped graphene sheets possess great potential for a substitute for Pt-based catalysts in fuel cells.
基金the National Natural Science Foundation of China(NSFC 21573019,21872010)the Fundamental Research Funds for the Central Universities(2020NTST11)We also acknowledge the support from Key Laboratory of Radiopharmaceuticals and Key Laboratory of Theoretical and Computational Photochemistry,Ministry of Education.
文摘As a new type of nanomaterial,carbon dots(CDs)have been recognized as a versatile nanoplatform with enormous potential for biomedical and optoelectronic applications because of low cytotoxicity,photostability,biocompatibility and versatility in addition to their tunable photoluminescence.In this review,we aim at updating the latest research on preparation,optoelectronic and chemical properties of CDs as well as their biomedical and optoelectronic applications.We highlight the applications of CDs for stem cell imaging,cell nucleus imaging,two-photon fluorescence imaging,tumor diagnosis and therapy and their optoelectronic applications including light-emitting diodes(LEDs),solar cells and electrocatalysis.Furthermore,we also discuss current challenges and breakthroughs on machine-learning-driven synthesis of CDs as well as nucleic acid detection with an eye towards the future.Finally,we hope that this review will give further impulses to target-oriented research on CDs for biomedical and optoelectronic applications.
基金This work was supported by the National Natural Science Foundation of China(21573253)the National Key Research and Developmet Program of China(2017YFA0204700)the Strategic Priority Research Programme of the Chinese Academy of Sciences(XDB12010000).
文摘Two-dimensional(2D)atomically thin quantum dots(QDs)possess extraordinary electrical and optical properties.However,fabricating high quality 2D QDs via a universal and reliable technique remains a challenge.Here,we report a simple strategy to prepare high quality,monolayer single crystal 2D QDs via ultrathin cutting 2D bulk single crystals by ultramicrotome,followed by an exfoliation process.The as-prepared 2D QDs have pristine surface,high quality,high monolayer yield and high photoluminescence quantum yield(the highest photoluminescence quantum yield of WS2 is18%),which can be used as promising,low toxic,biocompatible,and good cell-permeability fluorescent labeling agents for in vitro imaging.
文摘In the version of this article originally published,Figs.2(d)and 3(a),and Figs.S3 and S6 in the Electronic Supplementary Material(ESM)were incorrect.The corrected images are shown below.
基金National Natural Science Foundation of China,Grant/Award Numbers:21573019,21872010National Key Research and Development Program of China,Grant/Award Number:2019YFE0112200FundamentalResearch Funds for the Central Universities,Grant/Award Number:2020NTST11。
文摘In recent years,carbon dots(CDs),including carbon nanodots,carbonized polymer dots,carbon quantum dots,and graphene quantum dots have attracted a mounting interest as readily accessible,nontoxic,and relatively inexpensive carbon-based nanomaterials.Yet,despite intense research for a number of years,a unifying picture is still lacking to clarify the exact definition,clear chemical structure,and unique optical properties of this family of nanomaterials.In this review,we systematically summarize the recent development of CDs from molecular design to related properties of excited states as well as their applications in optoelectronic devices and biology.We point out the current challenges,including exploring precise synthesis,clarifying the structure-property relationship,and regulating singlet and triplet states of fluorescence,phosphorescence,and delayed fluorescence.Moreover,the structural optimization of optoelectronic devices,tumor targeting mechanism,selective imaging,and drug delivery of CDs are also highlighted.We hope that the information provided in this review will inspire more exciting research on CDs from a brand-new perspective and promote practical application of CDs in multiple directions of current and future research.
