Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent yea...Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent years.The primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical performance.This technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling path.This review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode materials.It encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical properties.Furthermore,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and sustainability.Based on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.展开更多
Background This paper presents an intelligent path planner for lifting tasks by tower cranes in highly complex environments,such as old industrial plants that were built many decades ago and sites used as tentative st...Background This paper presents an intelligent path planner for lifting tasks by tower cranes in highly complex environments,such as old industrial plants that were built many decades ago and sites used as tentative storage spaces.Generally,these environments do not have workable digital models and 3 D representations are impractical.Methods The current investigation introduces the use of cutting edge laser scanning technology to convert real environments into virtualized versions of the construction sites or plants in the form of point clouds.The challenge is in dealing with the large point cloud datasets from the multiple scans needed to produce a complete virtualized model.The tower crane is also virtualized for the purpose of path planning.A parallelized genetic algorithm is employed to achieve intelligent path planning for the lifting task performed by tower cranes in complicated environments taking advantage of graphics processing unit technology,which has high computing performance yet low cost.Results Optimal lifting paths are generate d in several seconds.展开更多
Metal halide perovskite solar cells(PSCs)have made substantial progress in power conversion efficiency(PCE)and stability in the past decade thanks to the advancements in perovskite deposition methodology,charge transp...Metal halide perovskite solar cells(PSCs)have made substantial progress in power conversion efficiency(PCE)and stability in the past decade thanks to the advancements in perovskite deposition methodology,charge transport layer(CTL)optimization,and encapsulation technology.Solution-based methods have been intensively investigated and a 25.7% certified efficiency has been achieved.Vacuum vapor deposition protocols were less studied,but have nevertheless received increasing attention from industry and academia due to the great potential for large-area module fabrication,facile integration with tandem solar cell architectures,and compatibility with industrial manufacturing approaches.In this article,we systematically discuss the applications of several promising vacuum vapor deposition techniques,namely thermal evaporation,chemical vapor deposition(CVD),atomic layer deposition(ALD),magnetron sputtering,pulsed laser deposition(PLD),and electron beam evaporation(e-beam evaporation)in the fabrication of CTLs,perovskite absorbers,encapsulants,and connection layers for monolithic tandem solar cells.展开更多
The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties.As the perovskite material dimensionality is reduced to exploit the quantum confinement effe...The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties.As the perovskite material dimensionality is reduced to exploit the quantum confinement effects,the disruption to the perovskite lattice,often with insulating organic ligands,raises new questions on the charge diffusion properties.Herein,we report direct imaging of>1μm exciton diffusion lengths in CH3NH3PbBr3 perovskite nanocrystal(PNC)films.Surprisingly,the resulting exciton mobilities in these PNC films can reach 10±2cm^(2)V^(-1) s^(-1),,which is counterintuitively several times higher than the carrier mobility in 3D perovskite films.We show that this ultralong exciton diffusion originates from both efficient inter-NC exciton hopping(via Forster energy transfer)and the photon recycling process with a smaller yet significant contribution.Importantly,our study not only sheds new light on the highly debated origins of the excellent exciton diffusion in PNC films but also highlights the potential of PNCs for optoelearonic applications.展开更多
Electrochemically producing formate by oxidizing methanol is a promising way to add value to methanol.Noble metal-based electrocatalysts,which have been extensively studied for the methanol oxidation reaction,can cata...Electrochemically producing formate by oxidizing methanol is a promising way to add value to methanol.Noble metal-based electrocatalysts,which have been extensively studied for the methanol oxidation reaction,can catalyze the complete oxidation of methanol to carbon dioxide,but not the mild oxidation to formate.As a result,exploring efficient and earth-abundant electrocatalysts for formate production from methanol is of interest.Herein,we present the electro-oxidation of methanol to formate,catalyzed by iron-substituted lanthanum cobaltite(LaCo_(1-x)Fe_(x)O_(3)).The Fe/Co ratio in the oxides greatly influences the activity and selectivity.This effect is attributed to the higher affinity of Fe and Co to the two reactants:CH3OH and OH,respectively.Because a balance between these affinities is favored,LaCo_(0.5)Fe_(0.5)O_(3) shows the highest formate production rate,at 24.5 mmol h^(-1) g_(oxide)^(-1),and a relatively high Faradaic efficiency of 44.4%in a series of(LaCo_(1-x)Fe_(x)O_(3))samples(x=0.00,0.25,0.50,0.75,1.00)at 1.6 V versus a reversible hydrogen electrode.展开更多
Due to the emergence of various new infectious(viral/bacteria)diseases,the remote surveillance of infected persons has become most important,especially if hospitals need to isolate infected patients to prevent the spr...Due to the emergence of various new infectious(viral/bacteria)diseases,the remote surveillance of infected persons has become most important,especially if hospitals need to isolate infected patients to prevent the spreading of pathogens to health care personnel.Therefore,we develop a remote health monitoring system by integrating a stretchable asymmetric supercapacitor(SASC)as a portable power source with sensors that can monitor the human physical health condition in real-time and remotely.An abnormal body temperature and breathing rate could indicate a person’s sickness/infection status.Here we integrated FePS3@graphene-based strain sensor and SASC into an all-in-one textile system and wrapped it around the abdomen to continuously monitor the breathing cycle of the person.The real body temperature was recorded by integrating the temperature sensor with the SASC.The proposed system recorded physiological parameters in real-time and when monitored remotely could be employed as a screening tool for monitoring pathogen infection status.展开更多
The evaluation of the intrinsic activity of catalysts is the most basic in searching energy-and cost-efficient catalyst materials for various applications.The accurate determination of the intrinsic activity is essent...The evaluation of the intrinsic activity of catalysts is the most basic in searching energy-and cost-efficient catalyst materials for various applications.The accurate determination of the intrinsic activity is essential for identifying efficient catalysts.While a huge number of studies of electrocatalysis for various applications have been reported,the effects of electrode loading on the apparent intrinsic activity obtained experimentally have been rarely discussed.With a high mass loading on the electrode,not all the catalyst surfaces can be electrochemically active because not all the surfaces can be wetted by the electrolyte.The loading also affects the transport of electrons over the electrode as well as the transport of ions in the electrolyte,and thus affects the kinetics.These lead to the derivations of the apparent intrinsic activity from the real intrinsic activity.Herein,for better understanding the derivations,we evaluate and discuss the effects of electrode mass loading using oxygen evolution reaction as an example.展开更多
We present an optical and photoelectron spectroscopic study to elucidate the interfacial electronic properties of organic-inorganic semiconductor heterojunctions formed in a kinetically blocked heptazethrene triisopro...We present an optical and photoelectron spectroscopic study to elucidate the interfacial electronic properties of organic-inorganic semiconductor heterojunctions formed in a kinetically blocked heptazethrene triisopropylsilyl ethynylene (HZ-TIPS) and its homologue,octazethrene (OZ-TIPS) on an all-inorganic perovskite cesium lead bromide (CsPbBr3) surface.The photoluminescence behavior of the underlying perovskites upon differing molecular doping conditions was examined.It turns out that the charge transfer dynamics of thermally-evaporated OZ-TIPS molecule exhibited a faster average lifetime than that of the HZ-TIPS case suggesting the importance of the biradical state in the former molecule.An interfacial dipole was formed at the interface due to the competing interaction between the dispersion force of the bulky TIPS-substituent group and the attractive van der Waals interaction at the first few layers.Photoemission spectroscopy of the physisorbed HZ-TIPS shows chemical shifts,which indicates electron transfer from HZ-TIPS molecules to the CsPbBr3 perovskite single crystal.In contrast,the adsorbed OZ-TIPS molecular layer on CsPbBr3 demonstrates the opposite trend indicating a hole transfer process.The average molecular orientation as determined by near edge X-ray absorption fine structure (NEXAFS) suggests that the HZ-TIPS molecular plane is generally lifted with respect to the perovskite surface.We suggest that the nature of the closed-shell electronic ground state of HZ-TIPS could contribute to the formation of interfacial dipole at the molecule/perovskite interface.展开更多
The versatile nature of organic conjugated materials renders their flawless integration into a diverse family of optoelectronic devices with light-harvesting,photodetection,or light-emitting capabilities.Classes of ma...The versatile nature of organic conjugated materials renders their flawless integration into a diverse family of optoelectronic devices with light-harvesting,photodetection,or light-emitting capabilities.Classes of materials that offer the possibilities of two or more distinct optoelectronic functions are particularly attractive as they enable smart applications while providing the benefits of the ease of fabrication using low-cost processes.Here,we develop a novel,multi-purpose conjugated small molecule by combining boron-azadipyrromethene(aza-BODIPY)as electron acceptor with triphenylamine(TPA)as end-capping donor units.The implemented donor–acceptor–donor(D–A–D)configuration,in the form of TPA-azaBODIPY-TPA,preserves ideal charge transfer characteristics with appropriate excitation energy levels,with the additional ability to be used as either a charge transporting interlayer or light-sensing semiconducting layer in optoelectronic devices.To demonstrate its versatility,we first show that TPA-azaBODIPY-TPA can act as an excellent hole transport layer in methylammonium lead triiodide(MAPbI3)-based perovskite solar cells with measured power conversion efficiencies exceeding 17%,outperforming control solar cells with PEDOT:PSS by nearly 60%.Furthermore,the optical bandgap of 1.49 eV is shown to provide significant photodetection in the wavelength range of up to 800 nm where TPA-azaBODIPY-TPA functions as donor in near-infrared organic photodetectors(OPDs)composed of fullerene derivatives.Overall,the established versatility of TPA-azaBODIPY-TPA,combined with its robust thermal stability as well as excellent solubility and processability,provides a new guide for developing highly efficient multi-purpose electronic materials for the next-generation of smart optoelectronic devices.展开更多
基金National Research Foundation Singapore and National Environment Agency Singapore,Grant/Award Number:CTRL-2023-1D-01。
文摘Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent years.The primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical performance.This technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling path.This review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode materials.It encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical properties.Furthermore,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and sustainability.Based on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.
文摘Background This paper presents an intelligent path planner for lifting tasks by tower cranes in highly complex environments,such as old industrial plants that were built many decades ago and sites used as tentative storage spaces.Generally,these environments do not have workable digital models and 3 D representations are impractical.Methods The current investigation introduces the use of cutting edge laser scanning technology to convert real environments into virtualized versions of the construction sites or plants in the form of point clouds.The challenge is in dealing with the large point cloud datasets from the multiple scans needed to produce a complete virtualized model.The tower crane is also virtualized for the purpose of path planning.A parallelized genetic algorithm is employed to achieve intelligent path planning for the lifting task performed by tower cranes in complicated environments taking advantage of graphics processing unit technology,which has high computing performance yet low cost.Results Optimal lifting paths are generate d in several seconds.
基金financial support of the National Key Research and Development Program of China(2022YFB3803304)The project supported by Tsinghua University Initiative Scientific Research Program(20221080065,20223080044)+9 种基金National Natural Science Foundation of China(No.21872080)State Key Laboratory of Power System and Generation Equipment(Nos.SKLD21Z03 and SKLD20M03)The Chinese Thousand Talents Program for Young Professionals,State Grid Corporation of China,National Bio Energy Co.,Ltd.Grant Number 52789922000DChina Huaneng Group Co.,Ltd.,and grant no.HNKJ20-H88financial support of the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation programme(Grant agreement No.834431)the Spanish Agencia estatal de investigacion(AEI)Grant PDC2021-121317-I00funded by MCIN/AEI/10.13039/501100011033by the“European Union NextGenerationEU/PRTR”the support from the Energy Materials and Surface Sciences Unit of the Okinawa Institute of Science and Technology Graduate Universitythe support from the National Natural Science Foundation of China(No.52232008).
文摘Metal halide perovskite solar cells(PSCs)have made substantial progress in power conversion efficiency(PCE)and stability in the past decade thanks to the advancements in perovskite deposition methodology,charge transport layer(CTL)optimization,and encapsulation technology.Solution-based methods have been intensively investigated and a 25.7% certified efficiency has been achieved.Vacuum vapor deposition protocols were less studied,but have nevertheless received increasing attention from industry and academia due to the great potential for large-area module fabrication,facile integration with tandem solar cell architectures,and compatibility with industrial manufacturing approaches.In this article,we systematically discuss the applications of several promising vacuum vapor deposition techniques,namely thermal evaporation,chemical vapor deposition(CVD),atomic layer deposition(ALD),magnetron sputtering,pulsed laser deposition(PLD),and electron beam evaporation(e-beam evaporation)in the fabrication of CTLs,perovskite absorbers,encapsulants,and connection layers for monolithic tandem solar cells.
基金We acknowledged Dr.Pio John S.Buenconsejo from the Facility for Analysis Characterization Testing and Simulation(FACTS),Nanyang Technological University,Singapore,for help with GI5AXS measurements.This research/project was supported by Nanyang Technological University under its start-up grants(M4080514,M4081630)the Ministry of Education under its AcRF Tier 1 grant(RG91/19)and Tier 2 grants(MOE2016-T2-1-034,MOE2017-T2-1-001,and MOE2017-T2-2-002)+1 种基金the National Research Foundation(NRF)Singapore under its NRF Investigatorship(NRF-NRFI-2018-04)Competitive Research Programme(NRF-CRP14-2014-03).
文摘The outstanding optoelectronic performance of lead halide perovskites lies in their exceptional carrier diffusion properties.As the perovskite material dimensionality is reduced to exploit the quantum confinement effects,the disruption to the perovskite lattice,often with insulating organic ligands,raises new questions on the charge diffusion properties.Herein,we report direct imaging of>1μm exciton diffusion lengths in CH3NH3PbBr3 perovskite nanocrystal(PNC)films.Surprisingly,the resulting exciton mobilities in these PNC films can reach 10±2cm^(2)V^(-1) s^(-1),,which is counterintuitively several times higher than the carrier mobility in 3D perovskite films.We show that this ultralong exciton diffusion originates from both efficient inter-NC exciton hopping(via Forster energy transfer)and the photon recycling process with a smaller yet significant contribution.Importantly,our study not only sheds new light on the highly debated origins of the excellent exciton diffusion in PNC films but also highlights the potential of PNCs for optoelearonic applications.
基金This research was supported by the National Research Foundation,Prime Minister's Office,Singapore,under its Campus for Research Excellence and Technological Enterprise(CREATE)programThe work was partially supported by a Singapore Ministry of Education Tier 1 grant(2019-T1-002-125)and Tier 2 grant(MOE-T2EP10220-0001).
文摘Electrochemically producing formate by oxidizing methanol is a promising way to add value to methanol.Noble metal-based electrocatalysts,which have been extensively studied for the methanol oxidation reaction,can catalyze the complete oxidation of methanol to carbon dioxide,but not the mild oxidation to formate.As a result,exploring efficient and earth-abundant electrocatalysts for formate production from methanol is of interest.Herein,we present the electro-oxidation of methanol to formate,catalyzed by iron-substituted lanthanum cobaltite(LaCo_(1-x)Fe_(x)O_(3)).The Fe/Co ratio in the oxides greatly influences the activity and selectivity.This effect is attributed to the higher affinity of Fe and Co to the two reactants:CH3OH and OH,respectively.Because a balance between these affinities is favored,LaCo_(0.5)Fe_(0.5)O_(3) shows the highest formate production rate,at 24.5 mmol h^(-1) g_(oxide)^(-1),and a relatively high Faradaic efficiency of 44.4%in a series of(LaCo_(1-x)Fe_(x)O_(3))samples(x=0.00,0.25,0.50,0.75,1.00)at 1.6 V versus a reversible hydrogen electrode.
基金the project Advanced Functional Nanorobots (Reg.no.CZ.02.1.01/0.0/0.0/15_003/0000444 financed by the EFRR)for support.
文摘Due to the emergence of various new infectious(viral/bacteria)diseases,the remote surveillance of infected persons has become most important,especially if hospitals need to isolate infected patients to prevent the spreading of pathogens to health care personnel.Therefore,we develop a remote health monitoring system by integrating a stretchable asymmetric supercapacitor(SASC)as a portable power source with sensors that can monitor the human physical health condition in real-time and remotely.An abnormal body temperature and breathing rate could indicate a person’s sickness/infection status.Here we integrated FePS3@graphene-based strain sensor and SASC into an all-in-one textile system and wrapped it around the abdomen to continuously monitor the breathing cycle of the person.The real body temperature was recorded by integrating the temperature sensor with the SASC.The proposed system recorded physiological parameters in real-time and when monitored remotely could be employed as a screening tool for monitoring pathogen infection status.
基金The work was partially supported by the Singapore Ministry of Education Tier 1 Grant(2019-T1-002-125)Dr.S.Sun thanks the funding support from Beijing Natural Science Foundation Program 2212029 and National Natural Science Foundation of China-Youth Science Fund(Grant No.52001009)Dr.Yu thanks the financial support from the National Research Foundation,Prime Minister's Office,Singapore,under its Campus for Research Excellence and Technological Enterprise(CREATE)program。
文摘The evaluation of the intrinsic activity of catalysts is the most basic in searching energy-and cost-efficient catalyst materials for various applications.The accurate determination of the intrinsic activity is essential for identifying efficient catalysts.While a huge number of studies of electrocatalysis for various applications have been reported,the effects of electrode loading on the apparent intrinsic activity obtained experimentally have been rarely discussed.With a high mass loading on the electrode,not all the catalyst surfaces can be electrochemically active because not all the surfaces can be wetted by the electrolyte.The loading also affects the transport of electrons over the electrode as well as the transport of ions in the electrolyte,and thus affects the kinetics.These lead to the derivations of the apparent intrinsic activity from the real intrinsic activity.Herein,for better understanding the derivations,we evaluate and discuss the effects of electrode mass loading using oxygen evolution reaction as an example.
文摘We present an optical and photoelectron spectroscopic study to elucidate the interfacial electronic properties of organic-inorganic semiconductor heterojunctions formed in a kinetically blocked heptazethrene triisopropylsilyl ethynylene (HZ-TIPS) and its homologue,octazethrene (OZ-TIPS) on an all-inorganic perovskite cesium lead bromide (CsPbBr3) surface.The photoluminescence behavior of the underlying perovskites upon differing molecular doping conditions was examined.It turns out that the charge transfer dynamics of thermally-evaporated OZ-TIPS molecule exhibited a faster average lifetime than that of the HZ-TIPS case suggesting the importance of the biradical state in the former molecule.An interfacial dipole was formed at the interface due to the competing interaction between the dispersion force of the bulky TIPS-substituent group and the attractive van der Waals interaction at the first few layers.Photoemission spectroscopy of the physisorbed HZ-TIPS shows chemical shifts,which indicates electron transfer from HZ-TIPS molecules to the CsPbBr3 perovskite single crystal.In contrast,the adsorbed OZ-TIPS molecular layer on CsPbBr3 demonstrates the opposite trend indicating a hole transfer process.The average molecular orientation as determined by near edge X-ray absorption fine structure (NEXAFS) suggests that the HZ-TIPS molecular plane is generally lifted with respect to the perovskite surface.We suggest that the nature of the closed-shell electronic ground state of HZ-TIPS could contribute to the formation of interfacial dipole at the molecule/perovskite interface.
基金Singapore Ministry of Education Academic Research Fund Tier 2,Grant/Award Number:MOE2019-T2-1-085Australian Research Council,Grant/Award Number:FT130101337+1 种基金QUT core funding,Grant/Award Number:QUT/322120-0301/07Australia India Strategic Research Fund,Grant/Award Number:AISRF53820。
文摘The versatile nature of organic conjugated materials renders their flawless integration into a diverse family of optoelectronic devices with light-harvesting,photodetection,or light-emitting capabilities.Classes of materials that offer the possibilities of two or more distinct optoelectronic functions are particularly attractive as they enable smart applications while providing the benefits of the ease of fabrication using low-cost processes.Here,we develop a novel,multi-purpose conjugated small molecule by combining boron-azadipyrromethene(aza-BODIPY)as electron acceptor with triphenylamine(TPA)as end-capping donor units.The implemented donor–acceptor–donor(D–A–D)configuration,in the form of TPA-azaBODIPY-TPA,preserves ideal charge transfer characteristics with appropriate excitation energy levels,with the additional ability to be used as either a charge transporting interlayer or light-sensing semiconducting layer in optoelectronic devices.To demonstrate its versatility,we first show that TPA-azaBODIPY-TPA can act as an excellent hole transport layer in methylammonium lead triiodide(MAPbI3)-based perovskite solar cells with measured power conversion efficiencies exceeding 17%,outperforming control solar cells with PEDOT:PSS by nearly 60%.Furthermore,the optical bandgap of 1.49 eV is shown to provide significant photodetection in the wavelength range of up to 800 nm where TPA-azaBODIPY-TPA functions as donor in near-infrared organic photodetectors(OPDs)composed of fullerene derivatives.Overall,the established versatility of TPA-azaBODIPY-TPA,combined with its robust thermal stability as well as excellent solubility and processability,provides a new guide for developing highly efficient multi-purpose electronic materials for the next-generation of smart optoelectronic devices.