Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water spl...Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water splitting.In this study,we constructed a superior Ti-doped hematite photoanode(TiFeO)by employing SnOx as an electron transfer mediator,partially oxidized graphene(pGO)as a hole transfer mediator,and molecular Co cubane as a water oxidation catalyst.The Co/pGO/TiFeO/SnO_(x)integrated system achieves a photocurrent density of 2.52 mA cm^(-2) at 1.23 VRHE,which is 2.4 times higher than bare photoanode(1.04 mA cm^(-2)),with operational stability up to 100 h.Kinetic measurements indicate that pGO can promote charge transfer from TiFeO to the Co cubane catalyst.In contrast,SnOx reduces charge recombination at the interface between TiFeO and the fluorinated tin oxide substrate.In-situ infrared spectroscopy shows the formation of an O–O bonded intermediate during water oxidation.This study highlights the crucial role of incorporating dual charge-transfer mediators into photoelectrodes for efficient solar energy conversion.展开更多
Theoretical calculations serve as an effective method for determining plasma temperatures within planetary atmospheres.To simulate plasma temperature,a comprehensive implementation of the energy equation is used,which...Theoretical calculations serve as an effective method for determining plasma temperatures within planetary atmospheres.To simulate plasma temperature,a comprehensive implementation of the energy equation is used,which is governed by five terms:conductivity,heating,cooling,adiabatic expansion,and advection.The derivations mentioned are strongly dependent on the collision cross section between electrons and other particles(e.g.,neutrals,ions).It is notable that the momentum transfer cross sections between electrons and neutrals have been updated in recent decades.However,the widely used momentum average collision cross sections between electrons and neutrals,derived from the momentum transfer cross sections,are collected in studies dating back nearly half a century.Therefore,it becomes imperative to revise the momentum average collision cross sections relevant to astrophysical contexts,based on the latest studies.In this study,we summarize the momentum average collision cross sections of 13 species common in planetary atmospheres:H,H_(2),He,O,CH_(4),H_(2)O,CO,N_(2),O_(2),Ar,CO_(2),N_(2)O,and NO_(2).All results are derived from the latest studies concerning the electron-neutral collision cross section and are compared with previous studies.Furthermore,we present a comparison of the derived total electron-neutral collision frequency at Mars between this study and previous studies.Prominent differences in the total electron-neutral collision frequency between this and prior studies support the significance of updating the momentum average collision cross section between electrons and neutrals in studying the planetary atmospheres.展开更多
The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow...The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow charge transfer dynamics and severe charge recombination at the interface.Herein,a novel“killing two birds with one stone”approach was discovered by employing CoPi as an interface mediator,which shifts its charge transfer behavior from conventional hole storage or passivation to hole transporter.The optimized BiVO_(4)/CoPi/FeOOH photoanode achieves a noteworthy photocurrent density of 5.4 mA/cm^(2) and exhibits long term stability(13 h).The dynamic analysis and electrochemical characterization reveal that CoPi can rapidly and directly transfer more photogenerated holes to the surface of OEC in comparison to traditional slow holes transfer behavior,resulting in highly efficient interface charge separation.Interestingly,the strong interfacial interactions can also be extended to OEC/electrolyte interface,specifically by promoting the surface reaction dynamics.Moreover,this innovative approach of altering behavior of CoPi can also be utilized to design other photoanodes,like BiVO_(4)/CoPi/NiOOH,aimed at efficient PEC water splitting.This finding affords a smart strategy to develop highly efficient and stable photoelectrodes for water splitting.展开更多
Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sust...Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.展开更多
The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising c...The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.展开更多
Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been...Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been extensively studied for diagnosing malignancy and stroke.In recent years,the emerging exploration of chemical exchange saturation transfer magnetic resonance imaging for detecting pathological changes in neurodegenerative diseases has opened up new possibilities for early detection and repetitive scans without ionizing radiation.This review serves as an overview of chemical exchange saturation transfer magnetic resonance imaging with detailed information on contrast mechanisms and processing methods and summarizes recent developments in both clinical and preclinical studies of chemical exchange saturation transfer magnetic resonance imaging for Alzheimer’s disease,Parkinson’s disease,multiple sclerosis,and Huntington’s disease.A comprehensive literature search was conducted using databases such as PubMed and Google Scholar,focusing on peer-reviewed articles from the past 15 years relevant to clinical and preclinical applications.The findings suggest that chemical exchange saturation transfer magnetic resonance imaging has the potential to detect molecular changes and altered metabolism,which may aid in early diagnosis and assessment of the severity of neurodegenerative diseases.Although promising results have been observed in selected clinical and preclinical trials,further validations are needed to evaluate their clinical value.When combined with other imaging modalities and advanced analytical methods,chemical exchange saturation transfer magnetic resonance imaging shows potential as an in vivo biomarker,enhancing the understanding of neuropathological mechanisms in neurodegenerative diseases.展开更多
文摘Regulating the interfacial charge transfer is pivotal for elucidating the kinetics of engineering the interface between the light-harvesting semiconductor and the substrate/catalyst for photoelectrocatalytic water splitting.In this study,we constructed a superior Ti-doped hematite photoanode(TiFeO)by employing SnOx as an electron transfer mediator,partially oxidized graphene(pGO)as a hole transfer mediator,and molecular Co cubane as a water oxidation catalyst.The Co/pGO/TiFeO/SnO_(x)integrated system achieves a photocurrent density of 2.52 mA cm^(-2) at 1.23 VRHE,which is 2.4 times higher than bare photoanode(1.04 mA cm^(-2)),with operational stability up to 100 h.Kinetic measurements indicate that pGO can promote charge transfer from TiFeO to the Co cubane catalyst.In contrast,SnOx reduces charge recombination at the interface between TiFeO and the fluorinated tin oxide substrate.In-situ infrared spectroscopy shows the formation of an O–O bonded intermediate during water oxidation.This study highlights the crucial role of incorporating dual charge-transfer mediators into photoelectrodes for efficient solar energy conversion.
基金the National Natural Science Foundation of China through Grants 42261160643,42441806,42241114,and 42304166supported by the open project funded by the Key Laboratory of Geospace Environment,Chinese Academy of Sciences,University of Science and Technology of China.
文摘Theoretical calculations serve as an effective method for determining plasma temperatures within planetary atmospheres.To simulate plasma temperature,a comprehensive implementation of the energy equation is used,which is governed by five terms:conductivity,heating,cooling,adiabatic expansion,and advection.The derivations mentioned are strongly dependent on the collision cross section between electrons and other particles(e.g.,neutrals,ions).It is notable that the momentum transfer cross sections between electrons and neutrals have been updated in recent decades.However,the widely used momentum average collision cross sections between electrons and neutrals,derived from the momentum transfer cross sections,are collected in studies dating back nearly half a century.Therefore,it becomes imperative to revise the momentum average collision cross sections relevant to astrophysical contexts,based on the latest studies.In this study,we summarize the momentum average collision cross sections of 13 species common in planetary atmospheres:H,H_(2),He,O,CH_(4),H_(2)O,CO,N_(2),O_(2),Ar,CO_(2),N_(2)O,and NO_(2).All results are derived from the latest studies concerning the electron-neutral collision cross section and are compared with previous studies.Furthermore,we present a comparison of the derived total electron-neutral collision frequency at Mars between this study and previous studies.Prominent differences in the total electron-neutral collision frequency between this and prior studies support the significance of updating the momentum average collision cross section between electrons and neutrals in studying the planetary atmospheres.
基金the National Natural Science Foundation of China(Nos.22202126,52273186,51873100,and 62105194)San Qin Scholars Innovation Teams in Shaanxi Province,China,International Joint Research Center of Shaanxi Province for Photoelectric Materials Science,and International Science and Technology Cooperation Project of Shaanxi Province,China(No.2021KW-20).
文摘The coupling of photoanode(Pho)and oxygen evolution catalyst(OEC)is an ideal approach to enhance the photoelectrochemical(PEC)activity.Nevertheless,the anticipated photocurrent density has not been reached due to slow charge transfer dynamics and severe charge recombination at the interface.Herein,a novel“killing two birds with one stone”approach was discovered by employing CoPi as an interface mediator,which shifts its charge transfer behavior from conventional hole storage or passivation to hole transporter.The optimized BiVO_(4)/CoPi/FeOOH photoanode achieves a noteworthy photocurrent density of 5.4 mA/cm^(2) and exhibits long term stability(13 h).The dynamic analysis and electrochemical characterization reveal that CoPi can rapidly and directly transfer more photogenerated holes to the surface of OEC in comparison to traditional slow holes transfer behavior,resulting in highly efficient interface charge separation.Interestingly,the strong interfacial interactions can also be extended to OEC/electrolyte interface,specifically by promoting the surface reaction dynamics.Moreover,this innovative approach of altering behavior of CoPi can also be utilized to design other photoanodes,like BiVO_(4)/CoPi/NiOOH,aimed at efficient PEC water splitting.This finding affords a smart strategy to develop highly efficient and stable photoelectrodes for water splitting.
基金financially supported by the Key Research and Development Program of Heilongjiang Province(No.2024ZXJ03C06)National Natural Science Foundation of China(No.52476192,No.52106237)+1 种基金Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)Technology Project of China Datang Technology Innovation Co.,Ltd(No.DTKC-2024-20610).
文摘Pulsed dynamic electrolysis(PDE),driven by renewable energy,has emerged as an innovative electrocatalytic conversion method,demonstrating significant potential in addressing global energy challenges and promoting sustainable development.Despite significant progress in various electrochemical systems,the regulatory mechanisms of PDE in energy and mass transfer and the lifespan extension of electrolysis systems,particularly in water electrolysis(WE)for hydrogen production,remain insufficiently explored.Therefore,there is an urgent need for a deeper understanding of the unique contributions of PDE in mass transfer enhancement,microenvironment regulation,and hydrogen production optimization,aiming to achieve low-energy consumption,high catalytic activity,and long-term stability in the generation of target products.Here,this review critically examines the microenvironmental effects of PDE on energy and mass transfer,the electrode degradation mechanisms in the lifespan extension of electrolysis systems,and the key factors in enhancing WE for hydrogen production,providing a comprehensive summary of current research progress.The review focuses on the complex regulatory mechanisms of frequency,duty cycle,amplitude,and other factors in hydrogen evolution reaction(HER)performance within PDE strategies,revealing the interrelationships among them.Finally,the potential future directions and challenges for transitioning from laboratory studies to industrial applications are proposed.
基金financial support from 2024 Domestic Visiting Scholar Program for Teachers'Professional Development in Universities(Grant No.FX2024022)National Natural Science Foundation of China(Grant No.61904043)。
文摘The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.
基金supported by The University of Hong Kong,China(109000487,109001694,204610401,and 204610519)National Natural Science Foundation of China(82402225)(to JH).
文摘Chemical exchange saturation transfer magnetic resonance imaging is an advanced imaging technique that enables the detection of compounds at low concentrations with high sensitivity and spatial resolution and has been extensively studied for diagnosing malignancy and stroke.In recent years,the emerging exploration of chemical exchange saturation transfer magnetic resonance imaging for detecting pathological changes in neurodegenerative diseases has opened up new possibilities for early detection and repetitive scans without ionizing radiation.This review serves as an overview of chemical exchange saturation transfer magnetic resonance imaging with detailed information on contrast mechanisms and processing methods and summarizes recent developments in both clinical and preclinical studies of chemical exchange saturation transfer magnetic resonance imaging for Alzheimer’s disease,Parkinson’s disease,multiple sclerosis,and Huntington’s disease.A comprehensive literature search was conducted using databases such as PubMed and Google Scholar,focusing on peer-reviewed articles from the past 15 years relevant to clinical and preclinical applications.The findings suggest that chemical exchange saturation transfer magnetic resonance imaging has the potential to detect molecular changes and altered metabolism,which may aid in early diagnosis and assessment of the severity of neurodegenerative diseases.Although promising results have been observed in selected clinical and preclinical trials,further validations are needed to evaluate their clinical value.When combined with other imaging modalities and advanced analytical methods,chemical exchange saturation transfer magnetic resonance imaging shows potential as an in vivo biomarker,enhancing the understanding of neuropathological mechanisms in neurodegenerative diseases.
