Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn ...Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.展开更多
Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highq...Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.展开更多
Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite format...Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite formation,high interfacial resistance,and deleterious interfacial reactions caused by solid-solid contact between electrode and electrolyte have hindered the commercialization of SSLBs.Thus,in this review,the state-of-the-art developments in the rational design of solid-state electrolyte and their progression toward practical applications are reviewed.First,the origin of interface instability and the sluggish charge carrier transportation in solid-solid interface are presented.Second,various strategies toward stabilizing interfacial stability(reducing interfacial resistance,suppressing lithium dendrites,and side reactions)are summarized from the physical and chemical perspective,including building protective layer,constructing 3D and gradient structures,etc.Finally,the remaining challenges and future development trends of solidstate electrolyte are prospected.This review provides a deep insight into solving the interfacial instability issues and promising solutions to enable practical high-energy-density lithium metal batteries.展开更多
Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling sta...Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling stability of WO_(3)-based aqueous ECBs is currently unsatisfactory due to the repeated phase transition during the redox process and the corrosion by acidic electrolytes.Herein,we present a titanium-tungsten oxide alloy(Ti-WO_(3))with controllable morphology and crystal phase synthesized by a facile hot injection method to overcome the challenges.In contrast to conventional monoclinic WO_(3),the Ti-WO_(3)nanorods can stably maintain their cubic crystal phase during the redox reaction in an acidic electrolyte,thus leading to dramatically enhanced response speed and cycling stability,Specifically,when working in a well-matched hybrid Al^(3+)/Zn^(2+)aqueous electrolyte,our phasetransition-free cubic Ti-WO_(3)exhibits an ultra-high cycling stability(>20000 cycles),fast response speed(3,95 s/4,65 s for bleaching/coloring),as well as excellent discharge areal capacity of 214.5 mA h m^(-2),We further fabricate a fully complementa ry aqueous electrochromic device,for the first time,using a Ti-WO_(3)/Prussian blue device architecture.Remarkably,the complementary ECB shows>10000 stable operation cycles,attesting to the feasibility of our Ti-WO_(3)for practical applications.Our work validates the significance of inhibiting the phase transitions of WO_(3)during the electrochromic process for realizing highly cyclable aqueous ECB,which can possibly provide a generalized design guidance for other high-quality metallic oxides for electrochemical applications.展开更多
The High Altitude Detection of Astronomical Radiation(HADAR)experiment,which was constructed in Tibet,China,combines the wide-angle advantages of traditional EAS array detectors with the high-sensitivity advantages of...The High Altitude Detection of Astronomical Radiation(HADAR)experiment,which was constructed in Tibet,China,combines the wide-angle advantages of traditional EAS array detectors with the high-sensitivity advantages of focused Cherenkov detectors.Its objective is to observe transient sources such as gamma-ray bursts and the counterparts of gravitational waves.This study aims to utilize the latest AI technology to enhance the sensitivity of HADAR experiments.Training datasets and models with distinctive creativity were constructed by incorporating the relevant physical theories for various applications.These models can determine the type,energy,and direction of the incident particles after careful design.We obtained a background identification accuracy of 98.6%,a relative energy reconstruction error of 10.0%,and an angular resolution of 0.22°in a test dataset at 10 TeV.These findings demonstrate the significant potential for enhancing the precision and dependability of detector data analysis in astrophysical research.By using deep learning techniques,the HADAR experiment’s observational sensitivity to the Crab Nebula has surpassed that of MAGIC and H.E.S.S.at energies below 0.5 TeV and remains competitive with conventional narrow-field Cherenkov telescopes at higher energies.In addition,our experiment offers a new approach for dealing with strongly connected,scattered data.展开更多
On February 6, 2023, the doublet earthquake including two main shocks with magnitudes M_(W)7.8 and M_(W)7.5, occurred near the western side of the East Anatolian Fault at the southeast boundary of the Anatolian Platea...On February 6, 2023, the doublet earthquake including two main shocks with magnitudes M_(W)7.8 and M_(W)7.5, occurred near the western side of the East Anatolian Fault at the southeast boundary of the Anatolian Plateau in Turkey. Based on the WGM2012 Bouguer gravity anomaly data and the Etopo1topography data, this study first introduced a joint inversion of admittance and coherence functions and used the Bayesian optimal parameter estimation method to obtain the effective elastic thickness Teand loading ratio F of the lithosphere for various tectonic units in the Anatolian Plateau. Secondly, we discussed the characteristics and influencing factors of the lithospheric mechanical strength and analyzed its relationship with seismic activity. The lithospheric mechanical strength of the Anatolian Plateau showed clear lateral heterogeneity and a "weak-strong-weak" spatial pattern from east to west,reflecting various tectonic processes. At last, the strong seismic activity was found where the lithospheric strength was low in the Anatolian Plate. We also incorporated GPS strain rate and other results to investigate the tectonic background and primary causes of the M_(W)7.8 and M_(W)7.5 doublet earthquakes in Turkey. The results have a good insight into urban safety design in the Turkish region, including postdisaster rehabilitation, earthquake hazard assessment, and loss reduction.展开更多
Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the ...Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.展开更多
基金supported by the National Key Research and Development Program of China(2022YFE0206300)the National Natural Science Foundation of China(22209047,U21A2081,22075074)+2 种基金Natural Science Foundation of Hunan Province(2020JJ5035)Hunan Provincial Department of Education Outstanding Youth Project(23B0037)Macao Science and Technology Development Fund(Macao SAR,FDCT-0096/2020/A2).
文摘Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced specific capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modification of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.
基金funded by the UM’s research funds(MYRG2020-00283-IAPME,MYRG2022-00266-IAPME,and MYRG-GRG2023-00224-IAPME-UMDF)the Science and Technology Development Fund,Macao SAR(FDCT 0006/2021/AKP,FDCT 0096/2020/A2,0013/2021/AMJ,and 0082/2022/A2)City University of Hong Kong(Project No.9020002)
文摘Two-dimensional materials have been widely used to tune the growth and energy-level alignment of perovskites.However,their incomplete passivation and chaotic usage amounts are not conducive to the preparation of highquality perovskite films.Herein,we succeeded in obtaining higher-quality CsPbBr_(3)films by introducing large-area monolayer graphene as a stable physical overlay on top of TiO_(2)substrates.Benefiting from the inert and atomic smooth graphene surface,the CsPbBr_(3)film grown on top by the van der Waal epitaxy has higher crystallinity,improved(100)orientation,and an average domain size of up to 1.22μm.Meanwhile,a strong downward band bending is observed at the graphene/perovskite interface,improving the electron extraction to the electron transport layers(ETL).As a result,perovskite film grown on graphene has lower photoluminescence(PL)intensity,shorter carrier lifetime,and fewer defects.Finally,a photovoltaic device based on epitaxy CsPbBr_(3)film is fabricated,exhibiting power conversion efficiency(PCE)of up to 10.64%and stability over 2000 h in the air.
基金supported by the National Key R&D Program(2022YFE0206400)the National Natural Science Foundation of China(52202256)+4 种基金the Natural Science Foundation of Jiangsu Province of China(BK20220612)the Science and Technology Development Fund,Macao SAR(0096/2020/A2,0013/2021/AMJ,and 0082/2022/A2)the Opening Project of the Key Laboratory of Jiangsu Province for Silk Engineering,Soochow University(KJS2277)the funds from Jiangsu University“Qinglan Project”the Young Elite Scientists Sponsorship Program of the Jiangsu Association for Science and Technology
文摘Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite formation,high interfacial resistance,and deleterious interfacial reactions caused by solid-solid contact between electrode and electrolyte have hindered the commercialization of SSLBs.Thus,in this review,the state-of-the-art developments in the rational design of solid-state electrolyte and their progression toward practical applications are reviewed.First,the origin of interface instability and the sluggish charge carrier transportation in solid-solid interface are presented.Second,various strategies toward stabilizing interfacial stability(reducing interfacial resistance,suppressing lithium dendrites,and side reactions)are summarized from the physical and chemical perspective,including building protective layer,constructing 3D and gradient structures,etc.Finally,the remaining challenges and future development trends of solidstate electrolyte are prospected.This review provides a deep insight into solving the interfacial instability issues and promising solutions to enable practical high-energy-density lithium metal batteries.
基金funded by the Science and Technology Development Fund,Macao SAR(File no.0052/2021/AGJ,0027/2023/AMJ,0083/2023/ITP2 and 0107/2023/AFJ)the Multi-Year Research Grants(MYRG2022-00063-IAPME,MYRG-GRG2023-00230-IAPME-UMDF)from the University of Macao+1 种基金the Guangdong Science and Technology Plan(2022A0505020022)the Major Science and Technology Research and Development Project of Jiangxi Province(20223AAE01003)。
文摘Aqueous electrochromic battery(ECB)has shown intense potential for achieving energy storage and saving simultaneously.While tungsten oxide(WO_(3))is the most promising EC material for commercialization,the cycling stability of WO_(3)-based aqueous ECBs is currently unsatisfactory due to the repeated phase transition during the redox process and the corrosion by acidic electrolytes.Herein,we present a titanium-tungsten oxide alloy(Ti-WO_(3))with controllable morphology and crystal phase synthesized by a facile hot injection method to overcome the challenges.In contrast to conventional monoclinic WO_(3),the Ti-WO_(3)nanorods can stably maintain their cubic crystal phase during the redox reaction in an acidic electrolyte,thus leading to dramatically enhanced response speed and cycling stability,Specifically,when working in a well-matched hybrid Al^(3+)/Zn^(2+)aqueous electrolyte,our phasetransition-free cubic Ti-WO_(3)exhibits an ultra-high cycling stability(>20000 cycles),fast response speed(3,95 s/4,65 s for bleaching/coloring),as well as excellent discharge areal capacity of 214.5 mA h m^(-2),We further fabricate a fully complementa ry aqueous electrochromic device,for the first time,using a Ti-WO_(3)/Prussian blue device architecture.Remarkably,the complementary ECB shows>10000 stable operation cycles,attesting to the feasibility of our Ti-WO_(3)for practical applications.Our work validates the significance of inhibiting the phase transitions of WO_(3)during the electrochromic process for realizing highly cyclable aqueous ECB,which can possibly provide a generalized design guidance for other high-quality metallic oxides for electrochemical applications.
文摘The High Altitude Detection of Astronomical Radiation(HADAR)experiment,which was constructed in Tibet,China,combines the wide-angle advantages of traditional EAS array detectors with the high-sensitivity advantages of focused Cherenkov detectors.Its objective is to observe transient sources such as gamma-ray bursts and the counterparts of gravitational waves.This study aims to utilize the latest AI technology to enhance the sensitivity of HADAR experiments.Training datasets and models with distinctive creativity were constructed by incorporating the relevant physical theories for various applications.These models can determine the type,energy,and direction of the incident particles after careful design.We obtained a background identification accuracy of 98.6%,a relative energy reconstruction error of 10.0%,and an angular resolution of 0.22°in a test dataset at 10 TeV.These findings demonstrate the significant potential for enhancing the precision and dependability of detector data analysis in astrophysical research.By using deep learning techniques,the HADAR experiment’s observational sensitivity to the Crab Nebula has surpassed that of MAGIC and H.E.S.S.at energies below 0.5 TeV and remains competitive with conventional narrow-field Cherenkov telescopes at higher energies.In addition,our experiment offers a new approach for dealing with strongly connected,scattered data.
基金funded by the National Natural Science Foundation of China (Grant Nos.U1939205,41974095)the Basic Research Fund of the Institute of Geophysics,China Earthquake Administration (Grant Nos.DQJB21R30)。
文摘On February 6, 2023, the doublet earthquake including two main shocks with magnitudes M_(W)7.8 and M_(W)7.5, occurred near the western side of the East Anatolian Fault at the southeast boundary of the Anatolian Plateau in Turkey. Based on the WGM2012 Bouguer gravity anomaly data and the Etopo1topography data, this study first introduced a joint inversion of admittance and coherence functions and used the Bayesian optimal parameter estimation method to obtain the effective elastic thickness Teand loading ratio F of the lithosphere for various tectonic units in the Anatolian Plateau. Secondly, we discussed the characteristics and influencing factors of the lithospheric mechanical strength and analyzed its relationship with seismic activity. The lithospheric mechanical strength of the Anatolian Plateau showed clear lateral heterogeneity and a "weak-strong-weak" spatial pattern from east to west,reflecting various tectonic processes. At last, the strong seismic activity was found where the lithospheric strength was low in the Anatolian Plate. We also incorporated GPS strain rate and other results to investigate the tectonic background and primary causes of the M_(W)7.8 and M_(W)7.5 doublet earthquakes in Turkey. The results have a good insight into urban safety design in the Turkish region, including postdisaster rehabilitation, earthquake hazard assessment, and loss reduction.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFB3800100 and 2021YFB3800101)the National Natural Science Foundation of China(62004089,U2001217,and U19A2089)+6 种基金the Guangdong Basic and Applied Basic Research Foundation(2019A1515110439,2019B1515120083,and2022A1515011218)the Shenzhen Science and Technology Program(JCYJ20190809150811504 and KQTD2015033110182370)the HKRGC General Research Funds(16312216)the Shenzhen&Hong Kong Joint Research Program(SGLH20180622092406130)the Shenzhen Engineering Research and Development Center for Flexible Solar Cel s Project funding from Shenzhen Development and Reform Committee(2019-126)the Key Fundamental Research Project funding from the Shenzhen Science and Technology Innovation Committee(JCYJ20200109141014474)the Guangdong-Hong Kong-Macao Joint Laboratory(2019B121205001)
文摘Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.
