Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect.Herein,an innovative method was developed to synthesize C-doped Pd interstiti...Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect.Herein,an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant.Elaborate characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate ions.The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation.The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm^(-2),i.e.,2.4 and 2.6 times of Pd,respectively.DFT calculations revealed that interstitial doping with C atoms induced differentiation of Pd sites.The strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance.This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.展开更多
Near infrared(NIR)fluorescence imaging guided photodynamic therapy(PDT)is a technique which has been developed in many clinical trials due to its advantage of real-time optical monitoring,specific spatiotemporal selec...Near infrared(NIR)fluorescence imaging guided photodynamic therapy(PDT)is a technique which has been developed in many clinical trials due to its advantage of real-time optical monitoring,specific spatiotemporal selectivity,and minimal invasiveness.For this,photosensitizers with NIR fluorescence emission and high^(1)O_(2)generation quantum yield are highly desirable.Herein,we designed and synthesized a"donor-acceptor"(D-A)structured semiconductor polymer(SP),which was then wrapped with an amphiphilic compound(Pluronic■F127)to prepare water-soluble nanoparticles(F-SP NPs).The obtained F-SP NPs exhibit good water solubility,excellent particle size stability,strong absorbance at deep red region,and strong NIR fluorescent emission characteristics.The maximal mass extinction coe±cient and fluorescence quantum yield of these F-SPs were calculated to be 21.7 L/(g·cm)and 6.5%,respectively.Moreover,the^(1)O_(2)quantum yield of 89%for F-SP NPs has been achieved under 635 nm laser irradiation,which is higher than Methylene Blue,Ce6,and PpIX.The outstanding properties of these F-SP NPs originate from their unique D-A molecular characteristic.This work should help guide the design of novel semiconductor polymer for NIR fluorescent imaging guided PDT applications.展开更多
The power co nversion efficiency(PCE)of OFQx-T:PC_(71)BM blend films reaches 7.59%.On this basis,ternary organic solar cells(OSCs)were fabricated with ITIC or PTB7-Th as the third component.The ternary OSCs with 50 wt...The power co nversion efficiency(PCE)of OFQx-T:PC_(71)BM blend films reaches 7.59%.On this basis,ternary organic solar cells(OSCs)were fabricated with ITIC or PTB7-Th as the third component.The ternary OSCs with 50 wt%ITIC in acceptors exhibits an enhanced efficiency,from 7.59%to 8.17%.Also,the PCE of ternary OSCs with 50 wt%PTB7-Th in donors achieves 8.72%,which is 13%higher than that of binary OSCs.The PCE improvement of two ternary OSCs is mainly due to the increase of short-circuit current density(J_(SC)),which can be attributed to the complementary absorption spectra and improved film morphology.This work suggests that the selection of an appropriate third component plays a critical role in improving the PCE of ternary OSCs.展开更多
Visual object recognition in humans and nonhuman primates is achieved by the ventral visual pathway(ventral occipital-temporal cortex,VOTC),which shows a well-documented object domain structure.An on-going question is...Visual object recognition in humans and nonhuman primates is achieved by the ventral visual pathway(ventral occipital-temporal cortex,VOTC),which shows a well-documented object domain structure.An on-going question is what type of information is processed in the higher-order VOTC that underlies such observations,with recent evidence suggesting effects of certain visual features.Combining computational vision models,fMRI experiment using a parametric-modulation approach,and natural image statistics of common objects,we depicted the neural distribution of a comprehensive set of visual features in the VOTC,identifying voxel sensitivities with specific feature sets across geometry/shape,Fourier power,and color.The visual feature combination pattern in the VOTC is significantly explained by their relationships to different types of response-action computation(fight-or-flight,navigation,and manipulation),as derived from behavioral ratings and natural image statistics.These results offer a comprehensive visual feature map in the VOTC and a plausible theoretical explanation as a mapping onto different types of downstream response-action systems.展开更多
基金the financial support from the National Natural Science Foundation of China(51904191)the Overseas High-level Talents Foundation of Shenzhen。
文摘Light-metalloid-atom-doped Pd interstitial nanoalloy is promising candidate for electrocatalysis because of the favorable electronic effect.Herein,an innovative method was developed to synthesize C-doped Pd interstitial nanoalloy using palladium acetate both as metal precursor and C dopant.Elaborate characterizations demonstrated that C atoms were successfully doped into the Pd lattice via self-catalytic decomposition of acetate ions.The as-synthesized C-doped Pd catalysts showed excellent activity and durable stability for formic acid electrooxidation.The mass activity and specific activity at 0.6 V of C-doped Pd were approximately 2.59 A/mg and 3.50 mA cm^(-2),i.e.,2.4 and 2.6 times of Pd,respectively.DFT calculations revealed that interstitial doping with C atoms induced differentiation of Pd sites.The strong noncovalent interaction between the Pd sites and the key intermediates endowed Pd with high-selectivity to direct routes and enhanced CO tolerance.This work presents a sites-differentiation strategy for metallic catalysts to improve the electrocatalysis.
基金This work was supported by National Natural Science Foundation of China(Nos.61805287 and 62175262)The Open Fund of the State Key Laboratory of Luminescent Materials and Devices(South China University of Technology,No.2021-skllmd-10)+1 种基金The Open Sharing Fund for Large-scale Instruments and Equipment of Central South University(CSUZC202218),Fundamental Research Funds for the Central South Universities(Nos.2020CX021,2020zzts387,and 2020zzts404)Key R&D plan of Hunan Province(No.2022SK2101).
文摘Near infrared(NIR)fluorescence imaging guided photodynamic therapy(PDT)is a technique which has been developed in many clinical trials due to its advantage of real-time optical monitoring,specific spatiotemporal selectivity,and minimal invasiveness.For this,photosensitizers with NIR fluorescence emission and high^(1)O_(2)generation quantum yield are highly desirable.Herein,we designed and synthesized a"donor-acceptor"(D-A)structured semiconductor polymer(SP),which was then wrapped with an amphiphilic compound(Pluronic■F127)to prepare water-soluble nanoparticles(F-SP NPs).The obtained F-SP NPs exhibit good water solubility,excellent particle size stability,strong absorbance at deep red region,and strong NIR fluorescent emission characteristics.The maximal mass extinction coe±cient and fluorescence quantum yield of these F-SPs were calculated to be 21.7 L/(g·cm)and 6.5%,respectively.Moreover,the^(1)O_(2)quantum yield of 89%for F-SP NPs has been achieved under 635 nm laser irradiation,which is higher than Methylene Blue,Ce6,and PpIX.The outstanding properties of these F-SP NPs originate from their unique D-A molecular characteristic.This work should help guide the design of novel semiconductor polymer for NIR fluorescent imaging guided PDT applications.
基金supported by the National Natural Science Foundation of China(No.21506258)Natural Science Foundation of Hunan Province(Nos.2016JJ3134,2017JJ2325)。
文摘The power co nversion efficiency(PCE)of OFQx-T:PC_(71)BM blend films reaches 7.59%.On this basis,ternary organic solar cells(OSCs)were fabricated with ITIC or PTB7-Th as the third component.The ternary OSCs with 50 wt%ITIC in acceptors exhibits an enhanced efficiency,from 7.59%to 8.17%.Also,the PCE of ternary OSCs with 50 wt%PTB7-Th in donors achieves 8.72%,which is 13%higher than that of binary OSCs.The PCE improvement of two ternary OSCs is mainly due to the increase of short-circuit current density(J_(SC)),which can be attributed to the complementary absorption spectra and improved film morphology.This work suggests that the selection of an appropriate third component plays a critical role in improving the PCE of ternary OSCs.
基金by the National Natural Science Foundation of China(31671128,31925020,31700999,31700943,and 31500882)the Changjiang Scholar Professorship Award(T2016031)Fundamental Research Funds for the Central Universities(2017EYT35).
文摘Visual object recognition in humans and nonhuman primates is achieved by the ventral visual pathway(ventral occipital-temporal cortex,VOTC),which shows a well-documented object domain structure.An on-going question is what type of information is processed in the higher-order VOTC that underlies such observations,with recent evidence suggesting effects of certain visual features.Combining computational vision models,fMRI experiment using a parametric-modulation approach,and natural image statistics of common objects,we depicted the neural distribution of a comprehensive set of visual features in the VOTC,identifying voxel sensitivities with specific feature sets across geometry/shape,Fourier power,and color.The visual feature combination pattern in the VOTC is significantly explained by their relationships to different types of response-action computation(fight-or-flight,navigation,and manipulation),as derived from behavioral ratings and natural image statistics.These results offer a comprehensive visual feature map in the VOTC and a plausible theoretical explanation as a mapping onto different types of downstream response-action systems.
