LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversio...LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversion via anodic oxidation reaction of direct borohydride fuel cells(DBFCs).However,the realization of practical hydrogen applications heavily depends on the effective synthesis of high-purity LiBH_(4) and recycling of the spent fuels(LiBO_(2)·xH_(2)O).The present work demonstrates a convenient and high-efficiency solvent-free strategy for regenerating LiBH_(4) with a maximum yield close to 80%,by retrieving its by-products with MgH_(2) as a reducing agent under ambient conditions.Besides,the hydrogen released from the regeneration course can completely compensate the demand for consumed MgH_(2).The isotopic tracer method reveals that the hydrogen stored in LiBH_(4) comes from both MgH_(2) and coordinated water bound to LiBO_(2).Here,the expensive MgH_(2) can be substituted with the readily available and cost-effective MgH_(2)-Mg mixtures to simplify the regeneration route.Notably,LiBH_(4) catalyzed by CoCl_(2) can stably supply hydrogen to proton exchange membrane fuel cell(PEMFC),thus powering a portable prototype vehicle.By combining hydrogen storage,production and utilization in a closed cycle,this work offers new insights into deploying boron-based hydrides for energy applications.展开更多
Mg-based materials have been intensively studied for hydrogen storage applications due to their high energy density up to 2600 Wh/kg or 3700 Wh/L.However,the Mg-based materials with poor kinetics and the necessity for...Mg-based materials have been intensively studied for hydrogen storage applications due to their high energy density up to 2600 Wh/kg or 3700 Wh/L.However,the Mg-based materials with poor kinetics and the necessity for a high temperature to achieve 0.1 MPa hydrogen equilibrium pressure limit the applications in the onboard storage in Fuel cell vehicles(FCVs).Over the past decades,many methods have been applied to improve the hydriding/dehydriding(H/D)kinetics of Mg/MgH 2 by forming amorphous or nanosized particles,adding catalysts and employing external energy field,etc.However,which method is more effective and the intrinsic mechanism they work are widely differing versions.The hydrogenation and dehydrogenation behaviors of Mg-based alloys analyzing by kinetic models is an efficient way to reveal the H/D kinetic mechanism.However,some recently proposed models with physical meaning and simple analysis method are not known intimately by researchers.Therefore,this review focuses on the enhancement method of kinetics in Mg-based hydrogen storage materials and introduces the new kinetic models.展开更多
Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthe...Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthesis of perovskite nanostructures have been made towards potential device applications.The engineering of their band structures holds great promise in the rational tuning of the electronic and optical properties of perovskite nanostructures,which is one of the keys to achieving efficient and multifunctional optoelectronic devices.In this article,we summarize recent advances in band structure engineering of perovskite nanostructures.A survey of bandgap engineering of nanostructured perovskites is firstly presented from the aspects of dimensionality tailoring,compositional substitution,phase segregation and transition,as well as strain and pressure stimuli.The strategies of electronic doping are then reviewed,including defect-induced self-doping,inorganic or organic molecules-based chemical doping,and modification by metal ions or nanostructures.Based on the bandgap engineering and electronic doping,discussions on engineering energy band alignments in perovskite nanostructures are provided for building high-performance perovskite p-n junctions and heterostructures.At last,we provide our perspectives in engineering band structures of perovskite nanostructures towards future low-energy optoelectronics technologies.展开更多
Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devi...Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devices.At present work,the hydrogen generation properties of MgLi-graphite composites were evaluated for the first time.The MgLi-graphite composites with different doping amounts of expanded graphite(abbreviated as EG hereinafter)were synthesized through ball milling and the hydrogen behaviors of the composites were investigated in chloride solutions.Among the above doping systems,the 10 wt.%EG-doped MgLi exhibited the best hydrogen performance in MgCl_(2)solutions.In particular,the 22 h-milled MgLi-10 wt.%EG composites possessed both desirable hydrogen conversion and rapid reaction kinetics,delivering a hydrogen yield of 966 mL H_(2)g^(-1)within merely 2 min and a maximum hydrogen generation rate of 1147 mL H_(2)min^(-1)g^(-1),as opposed to the sluggish kinetics in the EG-free composites.Moreover,the EG-doped MgLi showed superior air-stable ability even under a 75 RH%ambient atmosphere.For example,the 22 h-milled MgLi-10 wt.%EG composites held a fuel conversion of 89%after air exposure for 72 h,rendering it an advantage for Mg-based materials to safely store and transfer in practical applications.The similar favorable hydrogen performance of MgLi-EG composites in(simulate)seawater may shed light on future development of hydrogen generation technologies.展开更多
Mass loading and potential plateau are the two most important issues of potassium(K)-ion batteries(KIBs),but they have long been ignored in previous studies.Herein,we report a simple and scalable method to fabricate a...Mass loading and potential plateau are the two most important issues of potassium(K)-ion batteries(KIBs),but they have long been ignored in previous studies.Herein,we report a simple and scalable method to fabricate acidized carbon clothes(A-CC)as high mass loading(13.1 mg cm−2)anode for KIBs,which achieved a reversible areal-specific capacity of 1.81 mAh cm−2 at 0.2 mA cm−2.Besides,we have proposed the concept of“relative energy density”to reasonably evaluate the electrochemical performance of the anode.According to our calculation method,the A-CC electrode exhibited an ultrahigh relative energy density of 46 Wh m−2 in the initial charge process and remained at 40 Wh m−2 after 50 cycles.Furthermore,we performed the operando Raman spectroscopy(ORS)to investigate the K-ion storage mechanism.We believe that our work might provide a new guideline for the evaluation of anode performance,thereby,opening an avenue for the development of commercial anode.展开更多
High-performance infrared(IR)photodetectors made by low dimensional materials promise a wide range of applications in communication,security and biomedicine.Moreover,light-harvesting effects based on novel plasmonic m...High-performance infrared(IR)photodetectors made by low dimensional materials promise a wide range of applications in communication,security and biomedicine.Moreover,light-harvesting effects based on novel plasmonic materials and their combinations with two-dimensional(2 D)materials have raised tremendous interest in recent years,as they may potentially help the device complement or surpass currently commercialized IR photodetectors.Graphene is a particularly attractive plasmonic material because graphene plasmons are electrically tunable with a high degree of electromagnetic confinement in the mid-infrared(mid-IR)to terahertz regime and the field concentration can be further enhanced by forming nanostructures.Here,we report an efficient mid-IR room-temperature photodetector enhanced by plasmonic effect in graphene nanoresonators(GNRs)/graphene heterostructure.The plasmon polaritons in GNRs are size-dependent with strong field localization.Considering that the size and density of GNRs are controllable by chemical vapor deposition method,our work opens a cost-effective and scalable pathway to fabricate efficient IR optoelectronic devices with wavelength tunability.展开更多
The d-band centers of catalysts have exhibited excellent performance in various reactions.Among them,the enhanced catalytic reaction is considered a crucial way to power dynamics and reduce the“shuttle”effect in pol...The d-band centers of catalysts have exhibited excellent performance in various reactions.Among them,the enhanced catalytic reaction is considered a crucial way to power dynamics and reduce the“shuttle”effect in polysulfide conversions of lithium-sulfur batteries.Here,we report two-dimensional-shaped tungsten borides(WB)nanosheets with d-band centers,where the d orbits of W atoms on the(001)facets show greatly promoting the electrocatalytic sulfur reduction reaction.As-prepared WB-based Li-S cells exhibit excellent electrochemical performance for Li-ion storage.Especially,it delivers superior capacities of 7.7 mAh/cm^(2) under the 8.0 mg/cm^(2) sulfur loading,which is far superior to most other electrode catalysts.This study provides insights into the d-band centers as a promising catalyst of twodimensional boride materials.展开更多
The ultrafast monitoring of deoxyribonucleic acid(DNA)dynamic structural changes is an emerging and rapidly growing research topic in biotechnology.The existing optical spectroscopy used to identify different dynamica...The ultrafast monitoring of deoxyribonucleic acid(DNA)dynamic structural changes is an emerging and rapidly growing research topic in biotechnology.The existing optical spectroscopy used to identify different dynamical DNA structures lacks quick response while requiring large consumption of samples and bulky instrumental facilities.It is highly demanded to develop an ultrafast technique that monitors DNA structural changes with the external stimulus or cancer-related disease scenarios.Here,we demonstrate a novel photonic integrated graphene-optofluidic device to monitor DNA structural changes with the ultrafast response time.Our approach is featured with an effective and straightforward design of decoding the electronic structure change of graphene induced by its interactions with DNAs in different conformations using ultrafast nanosecond pulse laser and achieving refractive index sensitivity of~3×10^(−5) RIU.This innovative technique for the first time allows us to perform ultrafast monitoring of the conformational changes of special DNA molecules structures,including G-quadruplex formation by K+ions and i-motif formation by the low pH stimulus.The graphene-optofluidic device as presented here provides a new class of label-free,ultrafast,ultrasensitive,compact,and cost-effective optical biosensors for medical and healthcare applications.展开更多
基金This work was financially supported by the National Natural Science Foundation of China Projects(Nos.51771075)the National Key R&D Program of China(No.2018YFB1502101)+2 种基金the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.NSFC51621001)by the Project Supported by Nat-ural Science Foundation of Guangdong Province of China(2016A030312011)Shao acknowledges support from Macao Science and Technology Development Fund(FDCT)(Project No.:0062/2018/A2 and 0019/2019/AGJ).
文摘LiBH_(4) has been considered as one of the most promising energy storage materials with its ultrahigh hydrogen capacity,which can supply hydrogen through hydrolysis process or realize hydrogen-to-electricity conversion via anodic oxidation reaction of direct borohydride fuel cells(DBFCs).However,the realization of practical hydrogen applications heavily depends on the effective synthesis of high-purity LiBH_(4) and recycling of the spent fuels(LiBO_(2)·xH_(2)O).The present work demonstrates a convenient and high-efficiency solvent-free strategy for regenerating LiBH_(4) with a maximum yield close to 80%,by retrieving its by-products with MgH_(2) as a reducing agent under ambient conditions.Besides,the hydrogen released from the regeneration course can completely compensate the demand for consumed MgH_(2).The isotopic tracer method reveals that the hydrogen stored in LiBH_(4) comes from both MgH_(2) and coordinated water bound to LiBO_(2).Here,the expensive MgH_(2) can be substituted with the readily available and cost-effective MgH_(2)-Mg mixtures to simplify the regeneration route.Notably,LiBH_(4) catalyzed by CoCl_(2) can stably supply hydrogen to proton exchange membrane fuel cell(PEMFC),thus powering a portable prototype vehicle.By combining hydrogen storage,production and utilization in a closed cycle,this work offers new insights into deploying boron-based hydrides for energy applications.
基金H.Shao acknowledges the Macao Science and Technol-ogy Development Fund(FDCT)for funding(project no.118/2016/A3 and 0062/2018/A2)and this work was also par-tially supported by a Start-Up Research Fund from the Uni-versity of Macao(SRG2016-00088-FST)+5 种基金Q.Li also thanks the financial support from the National Natural Science Foun-dation of China(51671118)Young Elite Scientists Sponsor-ship Program by CAST(2017QNRC001)the“Chenguang”Program from the Shanghai Municipal Education Commission(17CG42)Science and Technology Committee of Shanghai(16520721800)the Program for Professor of Special Ap-pointment(Eastern Scholar)by Shanghai Municipal Educa-tion Commission(No.TP2015040).。
文摘Mg-based materials have been intensively studied for hydrogen storage applications due to their high energy density up to 2600 Wh/kg or 3700 Wh/L.However,the Mg-based materials with poor kinetics and the necessity for a high temperature to achieve 0.1 MPa hydrogen equilibrium pressure limit the applications in the onboard storage in Fuel cell vehicles(FCVs).Over the past decades,many methods have been applied to improve the hydriding/dehydriding(H/D)kinetics of Mg/MgH 2 by forming amorphous or nanosized particles,adding catalysts and employing external energy field,etc.However,which method is more effective and the intrinsic mechanism they work are widely differing versions.The hydrogenation and dehydrogenation behaviors of Mg-based alloys analyzing by kinetic models is an efficient way to reveal the H/D kinetic mechanism.However,some recently proposed models with physical meaning and simple analysis method are not known intimately by researchers.Therefore,this review focuses on the enhancement method of kinetics in Mg-based hydrogen storage materials and introduces the new kinetic models.
基金support from Australian Research Council (ARC, FT150100450, IH150100006 and CE170100039)support from the MCATM and the FLEET+1 种基金the support from Shenzhen Nanshan District Pilotage Team Program (LHTD20170006)support from Guangzhou Science and Technology Program (Grant No. 201804010322)
文摘Metal halide perovskite nanostructures have emerged as low-dimensional semiconductors of great significance in many fields such as photovoltaics,photonics,and optoelectronics.Extensive efforts on the controlled synthesis of perovskite nanostructures have been made towards potential device applications.The engineering of their band structures holds great promise in the rational tuning of the electronic and optical properties of perovskite nanostructures,which is one of the keys to achieving efficient and multifunctional optoelectronic devices.In this article,we summarize recent advances in band structure engineering of perovskite nanostructures.A survey of bandgap engineering of nanostructured perovskites is firstly presented from the aspects of dimensionality tailoring,compositional substitution,phase segregation and transition,as well as strain and pressure stimuli.The strategies of electronic doping are then reviewed,including defect-induced self-doping,inorganic or organic molecules-based chemical doping,and modification by metal ions or nanostructures.Based on the bandgap engineering and electronic doping,discussions on engineering energy band alignments in perovskite nanostructures are provided for building high-performance perovskite p-n junctions and heterostructures.At last,we provide our perspectives in engineering band structures of perovskite nanostructures towards future low-energy optoelectronics technologies.
基金financially supported by the National Natural Science Foundation of China Projects(Nos.51771075)the National Key R&D Program of China(No.2018YFB1502101)+1 种基金the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.NSFC51621001)the Project Supported by Natural Science Foundation of Guangdong Province of China(2016A030312011)
文摘Hydrolysis of Mg-based materials is considered as a potential means of safe and convenient real-time control of H_(2)release,enabling efficient loading,discharge and utilization of hydrogen in portable electronic devices.At present work,the hydrogen generation properties of MgLi-graphite composites were evaluated for the first time.The MgLi-graphite composites with different doping amounts of expanded graphite(abbreviated as EG hereinafter)were synthesized through ball milling and the hydrogen behaviors of the composites were investigated in chloride solutions.Among the above doping systems,the 10 wt.%EG-doped MgLi exhibited the best hydrogen performance in MgCl_(2)solutions.In particular,the 22 h-milled MgLi-10 wt.%EG composites possessed both desirable hydrogen conversion and rapid reaction kinetics,delivering a hydrogen yield of 966 mL H_(2)g^(-1)within merely 2 min and a maximum hydrogen generation rate of 1147 mL H_(2)min^(-1)g^(-1),as opposed to the sluggish kinetics in the EG-free composites.Moreover,the EG-doped MgLi showed superior air-stable ability even under a 75 RH%ambient atmosphere.For example,the 22 h-milled MgLi-10 wt.%EG composites held a fuel conversion of 89%after air exposure for 72 h,rendering it an advantage for Mg-based materials to safely store and transfer in practical applications.The similar favorable hydrogen performance of MgLi-EG composites in(simulate)seawater may shed light on future development of hydrogen generation technologies.
基金supports from the National Natural Science Foundation of China(51702056 and 51772135)the Ministry of Education of China(6141A02022516),China Postdoctoral Science Foundation(2017M622902 and 2019T120790)+1 种基金funding from the University of Macao(SRG2016-00092-IAPME,MYRG2018-00079-IAPME,and MYRG2019-00115IAPME)the Science and Technology Development Fund,Macao SAR(FDCT081/2017/A2,FDCT0059/2018/A2,and FDCT009/2017/AMJ).
文摘Mass loading and potential plateau are the two most important issues of potassium(K)-ion batteries(KIBs),but they have long been ignored in previous studies.Herein,we report a simple and scalable method to fabricate acidized carbon clothes(A-CC)as high mass loading(13.1 mg cm−2)anode for KIBs,which achieved a reversible areal-specific capacity of 1.81 mAh cm−2 at 0.2 mA cm−2.Besides,we have proposed the concept of“relative energy density”to reasonably evaluate the electrochemical performance of the anode.According to our calculation method,the A-CC electrode exhibited an ultrahigh relative energy density of 46 Wh m−2 in the initial charge process and remained at 40 Wh m−2 after 50 cycles.Furthermore,we performed the operando Raman spectroscopy(ORS)to investigate the K-ion storage mechanism.We believe that our work might provide a new guideline for the evaluation of anode performance,thereby,opening an avenue for the development of commercial anode.
基金support from the National Key Research&Development Program(No.2016YFA0201902,2018YFA0703200)Shenzhen Nanshan District Pilotage Team Program(LHTD20170006)+4 种基金National Natural Science Foundation of China(61974099 and 61604102,51773041,61890940)Shanghai Committee of Science and Technology in China(18ZR1404900)Natural Science Research Project for Anhui Universities(Grant No.KJ2019A0596)Youth Project of Provincial Natural Science Foundation of Anhui(Grant No.2008085QF319)Australian Research Council(ARC,FT150100450 and IH150100006)。
文摘High-performance infrared(IR)photodetectors made by low dimensional materials promise a wide range of applications in communication,security and biomedicine.Moreover,light-harvesting effects based on novel plasmonic materials and their combinations with two-dimensional(2 D)materials have raised tremendous interest in recent years,as they may potentially help the device complement or surpass currently commercialized IR photodetectors.Graphene is a particularly attractive plasmonic material because graphene plasmons are electrically tunable with a high degree of electromagnetic confinement in the mid-infrared(mid-IR)to terahertz regime and the field concentration can be further enhanced by forming nanostructures.Here,we report an efficient mid-IR room-temperature photodetector enhanced by plasmonic effect in graphene nanoresonators(GNRs)/graphene heterostructure.The plasmon polaritons in GNRs are size-dependent with strong field localization.Considering that the size and density of GNRs are controllable by chemical vapor deposition method,our work opens a cost-effective and scalable pathway to fabricate efficient IR optoelectronic devices with wavelength tunability.
基金supported by the National Natural Science Foundation of China(Nos.61904080,22205101)the Natural Science Foundation of Jiangsu Province(No.BK20190670)+5 种基金the Natural Science Foundation of Colleges and Universities in Jiangsu Province(No.19KJB530008)the Macao Young Scholars Program(No.AM2020005)the High-Performance Computing Cluster(HPCC)of Information and Communication Technology Office(ICTO)at University of Macao,Science and Technology Development Fund,Macao SAR(Nos.0191/2017/A3,0041/2019/A1,0046/2019/AFJ,0021/2019/AIR)University of Macao(Nos.MYRG2017-00216-FST and MYRG2018-00192-IAPME),FDCT Funding Scheme for Postdoctoral Researchers(No.0026/APD/2021)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the UEA funding,and Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110994).
文摘The d-band centers of catalysts have exhibited excellent performance in various reactions.Among them,the enhanced catalytic reaction is considered a crucial way to power dynamics and reduce the“shuttle”effect in polysulfide conversions of lithium-sulfur batteries.Here,we report two-dimensional-shaped tungsten borides(WB)nanosheets with d-band centers,where the d orbits of W atoms on the(001)facets show greatly promoting the electrocatalytic sulfur reduction reaction.As-prepared WB-based Li-S cells exhibit excellent electrochemical performance for Li-ion storage.Especially,it delivers superior capacities of 7.7 mAh/cm^(2) under the 8.0 mg/cm^(2) sulfur loading,which is far superior to most other electrode catalysts.This study provides insights into the d-band centers as a promising catalyst of twodimensional boride materials.
基金from the National Natural Science Foundation of China(21874096,21575095,51602305,61604102 and 61875139)the 111 Project,and the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)+2 种基金the China Postdoctoral Science Foundation(2018M633118)Shenzhen Nanshan District Pilotage Team Program(LHTD20170006)Australian Research Council(ARC,FT150100450,IH150100006 and CE170100039).Q.Bao acknowledges support from the Australian Research Council(ARC)Centre of Excellence in Future Low-Energy Electronics Technologies(FLEET).
文摘The ultrafast monitoring of deoxyribonucleic acid(DNA)dynamic structural changes is an emerging and rapidly growing research topic in biotechnology.The existing optical spectroscopy used to identify different dynamical DNA structures lacks quick response while requiring large consumption of samples and bulky instrumental facilities.It is highly demanded to develop an ultrafast technique that monitors DNA structural changes with the external stimulus or cancer-related disease scenarios.Here,we demonstrate a novel photonic integrated graphene-optofluidic device to monitor DNA structural changes with the ultrafast response time.Our approach is featured with an effective and straightforward design of decoding the electronic structure change of graphene induced by its interactions with DNAs in different conformations using ultrafast nanosecond pulse laser and achieving refractive index sensitivity of~3×10^(−5) RIU.This innovative technique for the first time allows us to perform ultrafast monitoring of the conformational changes of special DNA molecules structures,including G-quadruplex formation by K+ions and i-motif formation by the low pH stimulus.The graphene-optofluidic device as presented here provides a new class of label-free,ultrafast,ultrasensitive,compact,and cost-effective optical biosensors for medical and healthcare applications.