With tunable local electronic environment,high mass density of MN4sites,and ease of preparation,metal-organic conjugated coordinative polymer(CCP) with inherent electronic conductivity provides a promising alternative...With tunable local electronic environment,high mass density of MN4sites,and ease of preparation,metal-organic conjugated coordinative polymer(CCP) with inherent electronic conductivity provides a promising alternative to the well-known M-N-C electrocatalysts.Herein,the coordination reaction between Cu^(2+)and 1,2,4,5-tetraaminobenzene(TAB) was conducted on the surface of metallic Cu nanowires,forming a thin layer of CuN4-based CCP(Cu-TAB) on the Cu nanowire.More importantly,interfacial transfer of electrons from Cu core to the CuN4-based CCP nanoshell was observed within the resulting CuTAB@Cu,which was found to enrich the local electronic density of the CuN4sites.As such,the CuTAB@Cu demonstrates much improved affinity to the*COOH intermediate formed from the rate determining step;the energy barrier for C-C coupling,which is critical to convert CO_(2)into C2products,is also decreased.Accordingly,it delivers a current density of-9.1 mA cm^(-2)at a potential as high as 0.558 V(vs.RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol.This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN4-based CCPs for efficient electroreduction of CO_(2).展开更多
Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient gratin...Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient grating. Two major compo- nents are resolved in the dynamics of Rh6G＋. The first component, with a lifetime τTPIET = 140 fs-260 fs, is attributed to PIET from the phenyl ring to the xanthene plane. The IVR process occurring in the range ZIVR = 3.3 ps-5.2 ps is much slower than the first component. The PIET and IVR processes occurring in the excited state of Rh6G＋ are quantitatively determined, and a better understanding of the relationship between these processes is obtained.展开更多
The modulation of electrical properties of MoS_2 has attracted extensive research interest because of its potential applications in electronic and optoelectronic devices.Herein,interfacial charge transfer induced elec...The modulation of electrical properties of MoS_2 has attracted extensive research interest because of its potential applications in electronic and optoelectronic devices.Herein,interfacial charge transfer induced electronic property tuning of MoS_2 are investigated by in situ ultraviolet photoelectron spectroscopy and x-ray photoelectron spectroscopy measurements.A downward band-bending of MoS_2-related electronic states along with the decreasing work function,which are induced by the electron transfer from Cs overlayers to MoS_2,is observed after the functionalization of MoS_2 with Cs,leading to n-type doping.Meanwhile,when MoS_2 is modified with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane(F_4-TCNQ),an upward band-bending of MoS_2-related electronic states along with the increasing work function is observed at the interfaces.This is attributed to the electron depletion within MoS_2 due to the strong electron withdrawing property of F_4-TCNQ,indicating p-type doping of MoS_2.Our findings reveal that surface transfer doping is an effective approach for electronic property tuning of MoS_2 and paves the way to optimize its performance in electronic and optoelectronic devices.展开更多
Dicarboxylic acids have a wide range of applications in the polymer industry to construct valuable materials.Photocatalysis has recently emerged as an efficient and sustainable strategy to generate dicarboxylic acids....Dicarboxylic acids have a wide range of applications in the polymer industry to construct valuable materials.Photocatalysis has recently emerged as an efficient and sustainable strategy to generate dicarboxylic acids.However,photocatalytic dicarboxylation with CO_(2) is mainly limited to unsaturated bonds,and the dicarboxylation of C-C single bonds still remains a challenge.Herein,we report a photocatalytic dicarboxylation of C-C single bonds in strained rings with CO_(2) units via consecutive photo-induced electron transfer(ConPET).It is also the first photocatalytic reductive ring-opening reaction of cyclobutanes.Notably,this transition-metal-free protocol exhibits good functional group tolerance,broad substrate scope,facile scalability,and easy product derivatizations.Moreover,diacids can easily be derivatized to mainchain liquid crystalline polyesters.展开更多
The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy b...The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER.In this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor.The RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water dissociation.This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.展开更多
This paper reviews the recent progress in the electron transfer and interfacial behavior of redox proteins. Significant achievements in the relevant fields are summarized including the direct electron transfer between...This paper reviews the recent progress in the electron transfer and interfacial behavior of redox proteins. Significant achievements in the relevant fields are summarized including the direct electron transfer between proteins and electrodes, the thermodynamic and kinetic properties, catalytic activities and activity regulation of the redox proteins. It has been demonstrated that the electrochemical technique is an effective tool for protein studies, especially for probing into the electron transfer and interfacial behavior of redox proteins.展开更多
Constructing step-scheme(S-scheme)heterojunctions can considerably facilitate separation and transfer of photocarriers,as well as promote strong redox ability.The interface resistance of heterojunctions immediately af...Constructing step-scheme(S-scheme)heterojunctions can considerably facilitate separation and transfer of photocarriers,as well as promote strong redox ability.The interface resistance of heterojunctions immediately affects photocarrier separation and determines the photocatalytic activity.Herein,we constructed a novel Bi OBr/Ni_(2)P/g-C_(3)N_(4) heterojunction using Ni_(2)P as a novel electron bridge to reduce the interfacial resistance of photocarriers between Bi OBr and g-C3N4.The as-prepared 10% BiOBr/Ni2P/g-C_(3)N_(4) sample exhibited outstanding visible-light photocatalytic performance for methyl orange and rhodamine B removal,with degradation efficiencies of 91.4% and 98.9%,respectively.The excellent photocatalytic activity of Bi OBr/Ni_(2)P/g-C_(3)N_(4) was mainly attributed to the synergistic effects of the Ni2P cocatalyst and S-scheme heterojunction,which not only reduced the interface resistance but also retained the strong redox potential of the photocarriers.In addition,the formation of the S-scheme system was supported by active oxygen species investigation,current-voltage curves,and density functional theory calculations.This work provides a guideline for the design of highly efficient S-scheme photocatalysts with transition metal phosphates as electron bridges to improve photocarriers separation.展开更多
A number of electron donors, acceptors and diads containing xanthene dyes were sythesized. When the dyes were excited, the rate constants and the efficiencies of the intermolecular and intramolecular photo-induced ele...A number of electron donors, acceptors and diads containing xanthene dyes were sythesized. When the dyes were excited, the rate constants and the efficiencies of the intermolecular and intramolecular photo-induced electron transfer reactions were determined and calculated. It is found that the photo-induced electron transfer reactions occurred between xanthene dyes and many, including very weak donors or acceptors. The rate constants of intermolecular reactions were controlled by diffusion, and influenced by the reactant concentrations. The laser flash experiments showed that for low reactant concentrations, this kind of reactions took place mainly via the triplet excited state of the dyes. If different electric charges exist with dyes and donors/acceptors, there will be static quenching of the dyes’ fluorescence. The intramolecular electron transfer reactions are independent of the solution concentrations, and they may directly proceed via the singlet excited state of the dyes effectively.展开更多
Integrating heterogeneous interface through nanostructure design and interfacial modification is essential to realize strengthened interfacial polarization relaxation in electromagnetic wave absorption.However,an in-d...Integrating heterogeneous interface through nanostructure design and interfacial modification is essential to realize strengthened interfacial polarization relaxation in electromagnetic wave absorption.However,an in-depth comprehension of the interfacial polarization behavior at hetero-junction/interface is highly desired but remains a great challenge.Herein,a Mott-Schottky heterojunction consisting of honeycomb-like porous N-doped carbon confined CoP nanoparticles(CoP@HNC)is designed to elevate the interfacial polarization strength.Simultaneously,corresponding electron migration and redistribution between the heterointerface of defective carbon and CoP nanoparticles are revealed.The significant difference in the work function on both sides of heterogeneous interface boosts the interfacial polarization in high frequency region.Furthermore,the relevant spectroscopic characterizations demonstrate that electron spontaneously migrates from CoP to N-doped carbon at the heterointerface,thereby contributing to the accumulation of electron on defective carbon side and the distribution of hole on CoP side.Impressively,benefitting from the synergistic effects of three-dimensional porous conductive carbon skeleton,foreign N heteroatoms,special CoP nanoparticles,and the resultant CoP/N-doped carbon Mott-Schottky heterojunction,the CoP@HNC exhibits remarkable electromagnetic wave absorption performances with minimum reflection loss up to−60.8 dB and the maximum effective absorption bandwidth of 4.96 GHz,which is superior to most of recently reported transition metal phosphides microwave absorbing composites.The present work opens a new avenue for designing heterogeneous interface to realize strengthened microwave absorption capability and also reveals the in-depth influence of interface structure on electromagnetic wave absorption.展开更多
Electron donors(EDs)are widely used to improve the H 2 production performance of Schottky junction photocatalysts,but the functions of EDs are still unknown from the perspective of electron transfer dy-namics.Herein,P...Electron donors(EDs)are widely used to improve the H 2 production performance of Schottky junction photocatalysts,but the functions of EDs are still unknown from the perspective of electron transfer dy-namics.Herein,Pt nanocluster-decorated CdS nanorod is successfully prepared to construct a typical CdS/Pt Schottky junction.Pt nanoclusters with a diameter of∼2 nm are deposited on the surface of CdS nanorods by in situ photoreduction at sub-zero temperature.The CdS/Pt photocatalyst using lactic acid shows a higher H_(2)production rate of 4762μmol g^(-1)h^(-1)compared to that using methanol,tri-ethanolamine,and glycerol.To understand the cause,the dynamics of photogenerated carriers in CdS/Pt photocatalysts during ED-assisted H_(2)production are revealed by femtosecond transient absorption spec-troscopy.Among the four organic EDs,lactic acid enables the fastest electron transfer rate of 1.8×10^(9)s^(-1)and the highest electron transfer efficiency of 76%at the CdS/Pt interface due to the most efficient hole consumption.This work sheds light on the importance of efficient interfacial electron transfer for im-proving the photocatalytic performance of Schottky junction photocatalysts.展开更多
Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the e...Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the electronic states efficiently for intrinsic activity improvement.Here,we report a co-phosphorization approach to construct a VPO_(4)-Ni_(2)P heterostructure on nickel foam with strongly chemical binding,wherein phosphate acts as electronic modifier for Ni_(2)P electrocatalyst.Profiting from the interfacial interaction,it is uncovered that electron shifts from Ni_(2)P to VPO_(4)to render valence increment in Ni species.Such an electronic manipulation rationalizes the chemical affinities of various oxygen intermediates in OER pathway,giving a substantially reduced energy barrier.As a result,the advanced VPO_(4)-Ni_(2)P heterostructure only requires an overpotential of 289 mV to deliver a high current density of 350 mA/cm^(2)for OER in alkaline electrolyte,together with a Tafel slope as low as 28 mV/dec.This work brings fresh insights into interfacial engineering for advanced electrocatalyst design.展开更多
The evolution of membrane-type electronics has facilitated the development of stick-and-play systems,which confer diverse electrical functions to various planar or arbitrary curvilinear surfaces.The stick-and-play con...The evolution of membrane-type electronics has facilitated the development of stick-and-play systems,which confer diverse electrical functions to various planar or arbitrary curvilinear surfaces.The stick-and-play concept is based on the development of thin electronic devices in a printable format and their subsequent transfer to target surfaces.The development of this technology requires control of the interfacial adhesion of the electronic prints for retrieval from a carrier and transfer to the target surface.First,we discuss the transfer printing for membrane-type electronics,starting from an overview of materials available for flexible substrates,transfer printing of electronic prints for retrieval,and assembly for further integration.Second,we explain the stick-and-play concept based on fabricated membrane-type electronics;"stick" and “play"refer to the transfer of electronic devices and the performance of their electronic functions,respectively.In particular,we broadly survey various methods based on micro/nanostructures,including gecko-inspired,interlocking,cephalopod-sucker-inspired,and cilia structures,which can be employed to stick-and-play systems for enhancing interfacial adhesion with complex target surfaces under dynamic and wet conditions.Finally,we highlight the stick-and-play system application of micro/nanostructures for skin-attachable biomedical electronics,e-textiles,and environmental monitoring electronics.展开更多
A new fluorescent probe （BPbl） for Pb^2＋ has been synthesized, where diethanolamine （receptor） is linked with 4,4-difluoro-4- bora-3a, 4a-diaza-s-indacene （BODIPY） （fluorophore） via a methylene group （spacer...A new fluorescent probe （BPbl） for Pb^2＋ has been synthesized, where diethanolamine （receptor） is linked with 4,4-difluoro-4- bora-3a, 4a-diaza-s-indacene （BODIPY） （fluorophore） via a methylene group （spacer）. The absorption （496 nm） and emission （505 nm） wavelengths are in visible range. The fluorescence quantum yields of the lead-free and lead-bound states of BPb1 in acetonitrile are 0.013 and 0.693, respectively. The large chelation enhanced fluorescence effect （CHEF） with Pb^2＋ can be explained by the blocking of the photoinduced electron transfer （PET） process.展开更多
The interracial electron transfer （IET） dynamics of single CdSe core/multilayer shell （CdS2MLZnCdS1MLZnSIML） quantum dots （QDs） on the （110） surface of a futile TiO2 single crystal and TiO2 nanoparticles have ...The interracial electron transfer （IET） dynamics of single CdSe core/multilayer shell （CdS2MLZnCdS1MLZnSIML） quantum dots （QDs） on the （110） surface of a futile TiO2 single crystal and TiO2 nanoparticles have been compared. The fluorescence decay rates of single QDs on TiO2 are faster than those on glass, an insulating substrate, due to lET from the QDs to TiO2. Whereas the average IET rates are similar for QDs on the single crystal and nanoparticles, the distribution of lET rates is much broader in the latter, indicating a broad distribution of QD adsorption sites on the TiO2 nanoparticles.展开更多
基金The National Key Research and Development Program of China(2021YFA1502000 and 2022YFA1505300)the National Natural Science Foundation of China (22288102, 22072124)+1 种基金support from Beijing Synchrotron Radiation Facility (1W1B, BSRF)China Scholarship Council for the financial support。
文摘With tunable local electronic environment,high mass density of MN4sites,and ease of preparation,metal-organic conjugated coordinative polymer(CCP) with inherent electronic conductivity provides a promising alternative to the well-known M-N-C electrocatalysts.Herein,the coordination reaction between Cu^(2+)and 1,2,4,5-tetraaminobenzene(TAB) was conducted on the surface of metallic Cu nanowires,forming a thin layer of CuN4-based CCP(Cu-TAB) on the Cu nanowire.More importantly,interfacial transfer of electrons from Cu core to the CuN4-based CCP nanoshell was observed within the resulting CuTAB@Cu,which was found to enrich the local electronic density of the CuN4sites.As such,the CuTAB@Cu demonstrates much improved affinity to the*COOH intermediate formed from the rate determining step;the energy barrier for C-C coupling,which is critical to convert CO_(2)into C2products,is also decreased.Accordingly,it delivers a current density of-9.1 mA cm^(-2)at a potential as high as 0.558 V(vs.RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol.This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN4-based CCPs for efficient electroreduction of CO_(2).
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21003033 and 21203047)the Guangxi Provincial Natural Science Foundation,China(Grant Nos.2012GXNSFBA053012 and 2014GXNSFAA118019)the Research Foundation of Education Bureau of Guangxi Zhuang Autonomous Region,China(Grant No.ZD2014127)
文摘Photo-induced intramolecular electron transfer （PIET） and intramolecular vibrational relaxation （IVR） dynamics of the excited state of rhodamine 6G （Rh6G＋） in DMSO are investigated by multiplex transient grating. Two major compo- nents are resolved in the dynamics of Rh6G＋. The first component, with a lifetime τTPIET = 140 fs-260 fs, is attributed to PIET from the phenyl ring to the xanthene plane. The IVR process occurring in the range ZIVR = 3.3 ps-5.2 ps is much slower than the first component. The PIET and IVR processes occurring in the excited state of Rh6G＋ are quantitatively determined, and a better understanding of the relationship between these processes is obtained.
基金Supported by the National Natural Science Foundation of China (Grant No.22002031)the Natural Science Foundation of Zhejiang Province (Grant No.LY18F010019)the Innovation Project in Hangzhou for Returned Scholar。
文摘The modulation of electrical properties of MoS_2 has attracted extensive research interest because of its potential applications in electronic and optoelectronic devices.Herein,interfacial charge transfer induced electronic property tuning of MoS_2 are investigated by in situ ultraviolet photoelectron spectroscopy and x-ray photoelectron spectroscopy measurements.A downward band-bending of MoS_2-related electronic states along with the decreasing work function,which are induced by the electron transfer from Cs overlayers to MoS_2,is observed after the functionalization of MoS_2 with Cs,leading to n-type doping.Meanwhile,when MoS_2 is modified with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane(F_4-TCNQ),an upward band-bending of MoS_2-related electronic states along with the increasing work function is observed at the interfaces.This is attributed to the electron depletion within MoS_2 due to the strong electron withdrawing property of F_4-TCNQ,indicating p-type doping of MoS_2.Our findings reveal that surface transfer doping is an effective approach for electronic property tuning of MoS_2 and paves the way to optimize its performance in electronic and optoelectronic devices.
基金Financial support is provided by the National Natural Science Foundation of China(No.22225106)Fundamental Research Funds from Sichuan University(No.2020SCUNL102)the Fundamental Research Funds for the Central Universities。
文摘Dicarboxylic acids have a wide range of applications in the polymer industry to construct valuable materials.Photocatalysis has recently emerged as an efficient and sustainable strategy to generate dicarboxylic acids.However,photocatalytic dicarboxylation with CO_(2) is mainly limited to unsaturated bonds,and the dicarboxylation of C-C single bonds still remains a challenge.Herein,we report a photocatalytic dicarboxylation of C-C single bonds in strained rings with CO_(2) units via consecutive photo-induced electron transfer(ConPET).It is also the first photocatalytic reductive ring-opening reaction of cyclobutanes.Notably,this transition-metal-free protocol exhibits good functional group tolerance,broad substrate scope,facile scalability,and easy product derivatizations.Moreover,diacids can easily be derivatized to mainchain liquid crystalline polyesters.
基金supported by the National Natural Science Foundation of China (21721003,22202080 and 22034006)。
文摘The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER.In this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor.The RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water dissociation.This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.
基金support from the National Natural Science Foundation of China (Grant Nos. 90406005 & 20575028) the Program for New Century Excellent Talents in University,the Chinese Ministry of Education (Grant No. NCET-04-0452)
文摘This paper reviews the recent progress in the electron transfer and interfacial behavior of redox proteins. Significant achievements in the relevant fields are summarized including the direct electron transfer between proteins and electrodes, the thermodynamic and kinetic properties, catalytic activities and activity regulation of the redox proteins. It has been demonstrated that the electrochemical technique is an effective tool for protein studies, especially for probing into the electron transfer and interfacial behavior of redox proteins.
文摘Constructing step-scheme(S-scheme)heterojunctions can considerably facilitate separation and transfer of photocarriers,as well as promote strong redox ability.The interface resistance of heterojunctions immediately affects photocarrier separation and determines the photocatalytic activity.Herein,we constructed a novel Bi OBr/Ni_(2)P/g-C_(3)N_(4) heterojunction using Ni_(2)P as a novel electron bridge to reduce the interfacial resistance of photocarriers between Bi OBr and g-C3N4.The as-prepared 10% BiOBr/Ni2P/g-C_(3)N_(4) sample exhibited outstanding visible-light photocatalytic performance for methyl orange and rhodamine B removal,with degradation efficiencies of 91.4% and 98.9%,respectively.The excellent photocatalytic activity of Bi OBr/Ni_(2)P/g-C_(3)N_(4) was mainly attributed to the synergistic effects of the Ni2P cocatalyst and S-scheme heterojunction,which not only reduced the interface resistance but also retained the strong redox potential of the photocarriers.In addition,the formation of the S-scheme system was supported by active oxygen species investigation,current-voltage curves,and density functional theory calculations.This work provides a guideline for the design of highly efficient S-scheme photocatalysts with transition metal phosphates as electron bridges to improve photocarriers separation.
文摘A number of electron donors, acceptors and diads containing xanthene dyes were sythesized. When the dyes were excited, the rate constants and the efficiencies of the intermolecular and intramolecular photo-induced electron transfer reactions were determined and calculated. It is found that the photo-induced electron transfer reactions occurred between xanthene dyes and many, including very weak donors or acceptors. The rate constants of intermolecular reactions were controlled by diffusion, and influenced by the reactant concentrations. The laser flash experiments showed that for low reactant concentrations, this kind of reactions took place mainly via the triplet excited state of the dyes. If different electric charges exist with dyes and donors/acceptors, there will be static quenching of the dyes’ fluorescence. The intramolecular electron transfer reactions are independent of the solution concentrations, and they may directly proceed via the singlet excited state of the dyes effectively.
基金supported by the National Natural Science Foundation of China(Nos.51872002 and 52172174)Open Project of Provincial and Ministerial Scientific Research Platform,and Fuyang Normal University(No.FSKFKT009D).
文摘Integrating heterogeneous interface through nanostructure design and interfacial modification is essential to realize strengthened interfacial polarization relaxation in electromagnetic wave absorption.However,an in-depth comprehension of the interfacial polarization behavior at hetero-junction/interface is highly desired but remains a great challenge.Herein,a Mott-Schottky heterojunction consisting of honeycomb-like porous N-doped carbon confined CoP nanoparticles(CoP@HNC)is designed to elevate the interfacial polarization strength.Simultaneously,corresponding electron migration and redistribution between the heterointerface of defective carbon and CoP nanoparticles are revealed.The significant difference in the work function on both sides of heterogeneous interface boosts the interfacial polarization in high frequency region.Furthermore,the relevant spectroscopic characterizations demonstrate that electron spontaneously migrates from CoP to N-doped carbon at the heterointerface,thereby contributing to the accumulation of electron on defective carbon side and the distribution of hole on CoP side.Impressively,benefitting from the synergistic effects of three-dimensional porous conductive carbon skeleton,foreign N heteroatoms,special CoP nanoparticles,and the resultant CoP/N-doped carbon Mott-Schottky heterojunction,the CoP@HNC exhibits remarkable electromagnetic wave absorption performances with minimum reflection loss up to−60.8 dB and the maximum effective absorption bandwidth of 4.96 GHz,which is superior to most of recently reported transition metal phosphides microwave absorbing composites.The present work opens a new avenue for designing heterogeneous interface to realize strengthened microwave absorption capability and also reveals the in-depth influence of interface structure on electromagnetic wave absorption.
基金the National Key Research and Development Program of China(Nos.2022YFB3803600 and 2018YFB1502001)National Natural Science Foundation of China(Nos.22238009,51932007,U1905215,52073223,52173065,and 52202375)+2 种基金the Natural Science Foundation of Hubei Province of China(No.2022CFA001)China Postdoctoral Science Foundation(Nos.2021TQ0311 and 2021M702990)International Postdoc-toral Exchange Fellowship Program(No.PC2022051).
文摘Electron donors(EDs)are widely used to improve the H 2 production performance of Schottky junction photocatalysts,but the functions of EDs are still unknown from the perspective of electron transfer dy-namics.Herein,Pt nanocluster-decorated CdS nanorod is successfully prepared to construct a typical CdS/Pt Schottky junction.Pt nanoclusters with a diameter of∼2 nm are deposited on the surface of CdS nanorods by in situ photoreduction at sub-zero temperature.The CdS/Pt photocatalyst using lactic acid shows a higher H_(2)production rate of 4762μmol g^(-1)h^(-1)compared to that using methanol,tri-ethanolamine,and glycerol.To understand the cause,the dynamics of photogenerated carriers in CdS/Pt photocatalysts during ED-assisted H_(2)production are revealed by femtosecond transient absorption spec-troscopy.Among the four organic EDs,lactic acid enables the fastest electron transfer rate of 1.8×10^(9)s^(-1)and the highest electron transfer efficiency of 76%at the CdS/Pt interface due to the most efficient hole consumption.This work sheds light on the importance of efficient interfacial electron transfer for im-proving the photocatalytic performance of Schottky junction photocatalysts.
基金financially supported in part by National Key R&D Program of China(Nos.2020YFA0406103,2017YFA0207301)National Natural Science Foundation of China(Nos.21725102,91961106,U1832156,22075267,21803002)+4 种基金Science and Technological Fund of Anhui Province for Outstanding Youth(No.2008085J05)Youth Innovation Promotion Association of CAS(No.2019444)Young Elite Scientist Sponsorship Program by CAST,MOST(No.2018YFA0208603)Users with Excellence Program of Hefei Science Center CAS(No.2020HSC-UE003)Postdoc Matching Fund Scheme of the Hong Kong Polytechnic University(No.1-W144)。
文摘Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the electronic states efficiently for intrinsic activity improvement.Here,we report a co-phosphorization approach to construct a VPO_(4)-Ni_(2)P heterostructure on nickel foam with strongly chemical binding,wherein phosphate acts as electronic modifier for Ni_(2)P electrocatalyst.Profiting from the interfacial interaction,it is uncovered that electron shifts from Ni_(2)P to VPO_(4)to render valence increment in Ni species.Such an electronic manipulation rationalizes the chemical affinities of various oxygen intermediates in OER pathway,giving a substantially reduced energy barrier.As a result,the advanced VPO_(4)-Ni_(2)P heterostructure only requires an overpotential of 289 mV to deliver a high current density of 350 mA/cm^(2)for OER in alkaline electrolyte,together with a Tafel slope as low as 28 mV/dec.This work brings fresh insights into interfacial engineering for advanced electrocatalyst design.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea Government(MSIT)(No.2018R1A2B2005067)and GIST Research Institute(GRI)grant funded by the GIST in 2020.
文摘The evolution of membrane-type electronics has facilitated the development of stick-and-play systems,which confer diverse electrical functions to various planar or arbitrary curvilinear surfaces.The stick-and-play concept is based on the development of thin electronic devices in a printable format and their subsequent transfer to target surfaces.The development of this technology requires control of the interfacial adhesion of the electronic prints for retrieval from a carrier and transfer to the target surface.First,we discuss the transfer printing for membrane-type electronics,starting from an overview of materials available for flexible substrates,transfer printing of electronic prints for retrieval,and assembly for further integration.Second,we explain the stick-and-play concept based on fabricated membrane-type electronics;"stick" and “play"refer to the transfer of electronic devices and the performance of their electronic functions,respectively.In particular,we broadly survey various methods based on micro/nanostructures,including gecko-inspired,interlocking,cephalopod-sucker-inspired,and cilia structures,which can be employed to stick-and-play systems for enhancing interfacial adhesion with complex target surfaces under dynamic and wet conditions.Finally,we highlight the stick-and-play system application of micro/nanostructures for skin-attachable biomedical electronics,e-textiles,and environmental monitoring electronics.
基金support by Shanxi Scholarship Council of China(No.200310)
文摘A new fluorescent probe （BPbl） for Pb^2＋ has been synthesized, where diethanolamine （receptor） is linked with 4,4-difluoro-4- bora-3a, 4a-diaza-s-indacene （BODIPY） （fluorophore） via a methylene group （spacer）. The absorption （496 nm） and emission （505 nm） wavelengths are in visible range. The fluorescence quantum yields of the lead-free and lead-bound states of BPb1 in acetonitrile are 0.013 and 0.693, respectively. The large chelation enhanced fluorescence effect （CHEF） with Pb^2＋ can be explained by the blocking of the photoinduced electron transfer （PET） process.
基金supported by the National Science Foundation (CHE-0848556)the donors of the Petroleum Research Fund of the American Chemical Society (PRF #49286-ND6)
文摘The interracial electron transfer （IET） dynamics of single CdSe core/multilayer shell （CdS2MLZnCdS1MLZnSIML） quantum dots （QDs） on the （110） surface of a futile TiO2 single crystal and TiO2 nanoparticles have been compared. The fluorescence decay rates of single QDs on TiO2 are faster than those on glass, an insulating substrate, due to lET from the QDs to TiO2. Whereas the average IET rates are similar for QDs on the single crystal and nanoparticles, the distribution of lET rates is much broader in the latter, indicating a broad distribution of QD adsorption sites on the TiO2 nanoparticles.
