Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
Airless tires are essential for enhancing the safety,reliability,and convenience of maintenance of electric bicycles.Polyurethane(PU)is considered a promising candidate for such applications owing to its versatile pro...Airless tires are essential for enhancing the safety,reliability,and convenience of maintenance of electric bicycles.Polyurethane(PU)is considered a promising candidate for such applications owing to its versatile properties.However,their use is limited by insufficient heat resistance and excessive dynamic heat generation under cyclic loading.In this study,star-shaped trifunctional polypropylene glycerol(PPG3)was incorporated into conventional poly(tetramethylene glycol)(PTMG)and 4,4'-methylenediphenyl diisocyanate(MDI)-based systems to construct microporous star-shaped casting polyurethanes(SCPU),with water serving as a green foaming agent.Unlike conventional small-molecule trifunctional crosslinkers that create junctions within hard segment domains,PPG3 introduces long flexible arms between the hard segments,anchoring the crosslinking points at its molecular core.The large steric hindrance of PPG3 effectively suppresses soft segment crystallization and lowers the degree of microphase separation,whereas the crosslinked network restricts chain mobility,thereby reducing dynamic heat generation.These structural features also enhance the heat resistance,yielding a softening temperature of 183℃,which is 30.9%higher than that of polyurethane without PPG3.When applied to airless tires by casting SCPU into rubber treads,the fabricated hybrid airless tires achieved a rolling distance of over 3000 km under a load of 65 kg at 25km/h without structural failure,satisfying practical performance requirements.This strategy offers a simple,solvent-free,and environmentally friendly process,underscoring the potential of SCPU for scalable production of high-performance airless tires.展开更多
Air cathodes with high electrocatalytic activity are vital for developing H2/O_(2) proton exchange membrane fuel cells(PEMFC)and Zn-air batteries.However,the state-of-the-art air cathodes suffer from either limited ca...Air cathodes with high electrocatalytic activity are vital for developing H2/O_(2) proton exchange membrane fuel cells(PEMFC)and Zn-air batteries.However,the state-of-the-art air cathodes suffer from either limited catalytic activity or high cost,which thus hinder their applications.Herein,we designed ZIF-8 derived nitrogen and atomic iron dual-doped porous carbon nanocubes as high-quality catalysts for ORR,through a novel gas-doping approach.The porous carbon nanocubic architecture and abundant Fe-Nxactive species endow ZIF-8 derived single atomic iron catalyst(PCN-A@Fe SA)with superior catalytic activity,and surpass Pt/C and a majority of the reported catalysts.Both XAS and DFT calculations suggest that Fe2+N4 moieties are the main active centers that are favorable for oxygen affinity and OH*intermediate desorption,which can result in promising catalytic performance.Most importantly,PCNA@Fe SA can achieve power density of 514 m W cm^(-2) as cathodic catalyst in a PEMFC and discharge peak power density of 185 m W cm^(-2) in an alkaline Zn-air battery.The outstanding performance is derived from both the high specific surface area and high-density of iron single atom in nitrogen doped nanocubic carbon matrix.展开更多
The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and telluriu...The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and tellurium(Te)have shown promising hole mobilities,the instability under ambient conditions of bP and relatively low hole mobility of Te remain as daunting issues.Here we report the growth of high-quality Te nanobelts on atomically flat hexagonal boron nitride(h-BN)for high-performance p-type field-effect transistors(FETs).Importantly,the Te-based FET exhibits an ultrahigh hole mobility up to 1370 cm^(2) V^(−1) s^(−1) at room temperature,that may lay the foundation for the future high-performance p-type 2D FET and metal-oxide-semiconductor(p-MOS)inverter.The vdW h-BN dielectric substrate not only provides an ultra-flat surface without dangling bonds for growth of high-quality Te nanobelts,but also reduces the scattering centers at the interface between the channel material and the dielectric layer,thus resulting in the ultrahigh hole mobility.展开更多
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金financially supported by the National Natural Science Foundation of China(No.52303063)Hubei Provincial Department of Education Guided Scientific Research Project(No.B2024056)。
文摘Airless tires are essential for enhancing the safety,reliability,and convenience of maintenance of electric bicycles.Polyurethane(PU)is considered a promising candidate for such applications owing to its versatile properties.However,their use is limited by insufficient heat resistance and excessive dynamic heat generation under cyclic loading.In this study,star-shaped trifunctional polypropylene glycerol(PPG3)was incorporated into conventional poly(tetramethylene glycol)(PTMG)and 4,4'-methylenediphenyl diisocyanate(MDI)-based systems to construct microporous star-shaped casting polyurethanes(SCPU),with water serving as a green foaming agent.Unlike conventional small-molecule trifunctional crosslinkers that create junctions within hard segment domains,PPG3 introduces long flexible arms between the hard segments,anchoring the crosslinking points at its molecular core.The large steric hindrance of PPG3 effectively suppresses soft segment crystallization and lowers the degree of microphase separation,whereas the crosslinked network restricts chain mobility,thereby reducing dynamic heat generation.These structural features also enhance the heat resistance,yielding a softening temperature of 183℃,which is 30.9%higher than that of polyurethane without PPG3.When applied to airless tires by casting SCPU into rubber treads,the fabricated hybrid airless tires achieved a rolling distance of over 3000 km under a load of 65 kg at 25km/h without structural failure,satisfying practical performance requirements.This strategy offers a simple,solvent-free,and environmentally friendly process,underscoring the potential of SCPU for scalable production of high-performance airless tires.
基金supported by the National Natural Science Foundation of China(NSFC Project Nos.21776104,21476088)the National Key Research and Development Program of China(Project Nos.2016YFB0101201,2017YFB0102900)+1 种基金the Guangdong Provincial Department of Science and Technology(Project No.2015B010106012)the Guangzhou Science,Technology and Innovation Committee(Project Nos.201504281614372,2016GJ006)。
文摘Air cathodes with high electrocatalytic activity are vital for developing H2/O_(2) proton exchange membrane fuel cells(PEMFC)and Zn-air batteries.However,the state-of-the-art air cathodes suffer from either limited catalytic activity or high cost,which thus hinder their applications.Herein,we designed ZIF-8 derived nitrogen and atomic iron dual-doped porous carbon nanocubes as high-quality catalysts for ORR,through a novel gas-doping approach.The porous carbon nanocubic architecture and abundant Fe-Nxactive species endow ZIF-8 derived single atomic iron catalyst(PCN-A@Fe SA)with superior catalytic activity,and surpass Pt/C and a majority of the reported catalysts.Both XAS and DFT calculations suggest that Fe2+N4 moieties are the main active centers that are favorable for oxygen affinity and OH*intermediate desorption,which can result in promising catalytic performance.Most importantly,PCNA@Fe SA can achieve power density of 514 m W cm^(-2) as cathodic catalyst in a PEMFC and discharge peak power density of 185 m W cm^(-2) in an alkaline Zn-air battery.The outstanding performance is derived from both the high specific surface area and high-density of iron single atom in nitrogen doped nanocubic carbon matrix.
基金supported by the financial supports from National Natural Science Foundation of China(Grant No.61904110)Young Teachers’Startup Fund for Scientific Research of Shenzhen University(Grant No.860-000002110426)+2 种基金the funding support from the National Natural Science Foundation of China(52122002)the Start-Up Grant(Project No.9610495)from City University of Hong KongECS scheme(City U 21201821)from the Research Grant Council of Hong Kong。
文摘The lack of stable p-type van der Waals(vdW)semiconductors with high hole mobility severely impedes the step of low-dimensional materials entering the industrial circle.Although p-type black phosphorus(bP)and tellurium(Te)have shown promising hole mobilities,the instability under ambient conditions of bP and relatively low hole mobility of Te remain as daunting issues.Here we report the growth of high-quality Te nanobelts on atomically flat hexagonal boron nitride(h-BN)for high-performance p-type field-effect transistors(FETs).Importantly,the Te-based FET exhibits an ultrahigh hole mobility up to 1370 cm^(2) V^(−1) s^(−1) at room temperature,that may lay the foundation for the future high-performance p-type 2D FET and metal-oxide-semiconductor(p-MOS)inverter.The vdW h-BN dielectric substrate not only provides an ultra-flat surface without dangling bonds for growth of high-quality Te nanobelts,but also reduces the scattering centers at the interface between the channel material and the dielectric layer,thus resulting in the ultrahigh hole mobility.
