Copper oxide nanowires with varying oxidation states are prepared and their activity for water oxidation is studied. The nanowires with a CuO phase are found to be the most active, and their degree of crystallinity is...Copper oxide nanowires with varying oxidation states are prepared and their activity for water oxidation is studied. The nanowires with a CuO phase are found to be the most active, and their degree of crystallinity is important in achieving efficient water oxidation. For the crystalline CuO nanowires in a weakly basic Na2CO3 electrolyte, a Tafel slope of 41 mV/decade, an overpotential of approximately 500 mV at - 10 mA/crn2 (without compensation for the solution resistance), and a faradaic efficiency of nearly 100% are obtained. This electrode maintains a stable current for over 15 lx The low overpotential of 500 mV at 10 mA/cm2, small Tafel slope, long-term stability, and low cost make CuO one of the most promising catalysts for water oxidation. Moreover, the evolution of the CuO nanowire morphology over time is studied by electron microscop)-revealing that the diffusion of Cu ions from the interior of the nanowires to their surface causes the aggregation of individual nanowires over time. However, despite this aggregation, the current density remains nearly constant, because the total electrochemically active surface area of CuO does not change.展开更多
Knowledge in thermal and electric transport through grain boundary(GB)is crucial for designing nanostructured thermoelectric materials,where the transport greatly depends on GB atomistic structure.In this work,we empl...Knowledge in thermal and electric transport through grain boundary(GB)is crucial for designing nanostructured thermoelectric materials,where the transport greatly depends on GB atomistic structure.In this work,we employ machine learning(ML)techniques to study the relationship between silicon GB structure and its thermal and electric boundary conductance(TBC and EBC)calculated by Green’s function methods.We present a robust ML prediction model of TBC covering crystalline–crystalline and crystalline–amorphous interfaces,using disorder descriptors and atomic density.We also construct high-accuracy ML models for predicting both TBC and EBC and their ratio,using only small data of crystalline GBs.We found that the variations of interatomic angles and distance at GB are the most predictive descriptors for TBC and EBC,respectively.These results demonstrate the robustness of the black-box model and open the way to decouple thermal and electrical conductance,which is a key physical problem with engineering needs.展开更多
To retrieve the fuel debris in Fukushima Daiichi Nuclear Power Plants(1F),it is essential to infer the fuel debris distribution.In particular,the molten metal spreading behavior is one of the vital phenomena in nuclea...To retrieve the fuel debris in Fukushima Daiichi Nuclear Power Plants(1F),it is essential to infer the fuel debris distribution.In particular,the molten metal spreading behavior is one of the vital phenomena in nuclear severe accidents because it determines the initial condition for further accident scenarios such as molten core concrete interaction(MCCI).In this study,the fundamental molten metal spreading experiments were performed with different outlet diameters and sample amounts to investigate the effect of the outlet for spreading-solidification behavior.In the numerical analysis,the moving particle full-implicit method(MPFI),which is one of the particle methods,was applied to simulate the spreading experiments.In the MPFI framework,the melting-solidification model including heat transfer,radiation heat loss,phase change,and solid fraction-dependent viscosity was developed and implemented.In addition,the difference in the spreading and solidification behavior due to the outlet diameters was reproduced in the calculation.The simulation results reveal the detailed solidification procedure during the molten metal spreading.It is found that the viscosity change and the solid fraction change during the spreading are key factors for the free surface condition and solidified materials.Overall,it is suggested that the MPFI method has the potential to simulate the actual nuclear melt-down phenomena in the future.展开更多
Ta3N5 is regarded as a promising photocatalyst for solar water splitting because of its excellent visible light absorption characteristics and simple composition.Conventional Ta3N5 photocatalysts prepared from oxide p...Ta3N5 is regarded as a promising photocatalyst for solar water splitting because of its excellent visible light absorption characteristics and simple composition.Conventional Ta3N5 photocatalysts prepared from oxide precursors typically comprise aggregated polycrystalline particles with defects and grain boundaries that reduce the water oxidation activity of the material.In the present work,well-dispersed Ta3N5 nanoparticulate single crystals were synthesized via a mild nitridation process using pure Ta metal nanopowder or Ta nanopowder mixed with NaCl.The resulting high-quality Ta3N5 nanoparticles,after loading with an oxygen evolution cocatalyst,exhibited impressively high photocatalytic performance during O_(2)evolution from a sacrificial AgNO3 solution,with an apparent quantum yield of 9.4%at 420 nm.Our findings suggest a new approach to the facile fabrication of nanostructured single-crystal photocatalysts for efficient solar water splitting,based on the use of metal nanopowders.展开更多
Dislocation-mediated plasticity in inorganic semiconductors and oxides has attracted increasing research interest because of the promising mechanical and functional properties tuned by dislocations.In this study,we in...Dislocation-mediated plasticity in inorganic semiconductors and oxides has attracted increasing research interest because of the promising mechanical and functional properties tuned by dislocations.In this study,we investigated the effects of light illumination on the dislocation-mediated plasticity in hexagonal wurtzite ZnO,a representative third-generation semiconductor material.A(0001)45o off sample was specially designed to preferentially activate the basal slip on(0001)plane.Three types of nanoindentation tests were performed under four different light conditions(550 nm,334 nm,405 nm,and darkness),including low-load(60μN)pop-in tests,high-load(500μN)nanoindentation tests,and nanoindentation creep tests.The maximum shear stresses at pop-in were found to approximate the theoretical shear strength regardless of the light conditions.The activation volume at pop-ins was calculated to be larger in light than in darkness.Cross-sectional transmission electron microscope images taken from beneath the indentation imprints showed that all indentation-induced dislocations were located beneath the indentation imprint in a thin-plate shape along one basal slip plane.These indentation-induced dislocations could spread much deeper in darkness than in light,revealing the suppressive effect of light on dislocation behavior.An analytical model was adopted to estimate the elastoplastic stress field beneath the indenter.It was found that dislocation glide ceased at a higher stress level in light,indicating the increase in the Peierls barrier under light illumination.Furthermore,nanoindentation creep tests showed the suppression of both indentation depth and creep rate by light.Nanoindentation creep also yielded a larger activation volume in light than in darkness.展开更多
The spread of data-driven materials research has increased the need for systematically designed materials property databases.However,the development of polymer databases has lagged far behind other material systems.We...The spread of data-driven materials research has increased the need for systematically designed materials property databases.However,the development of polymer databases has lagged far behind other material systems.We present RadonPy,an open-source library that can automate the complete process of all-atom classical molecular dynamics(MD)simulations applicable to a wide variety of polymeric materials.Herein,15 different properties were calculated for more than 1000 amorphous polymers.The MD-calculated properties were systematically compared with experimental data to validate the calculation conditions;the bias and variance in the MD-calculated properties were successfully calibrated by a machine learning technique.During the high-throughput data production,we identified eight amorphous polymers with extremely high thermal conductivity(>0.4 W∙m^(–1)∙K^(–1))and their underlying mechanisms.Similar to the advancement of materials informatics since the advent of computational property databases for inorganic crystals,database construction using RadonPy will promote the development of polymer informatics.展开更多
基金the National Science and Technology Support Program of China (Grant No. 2012BAC19B07)the National Natural Science Foundation of China (Grant No. 41190084)+1 种基金the Ministry of Science and Technology of China (MOST) (Grant No. 2013FY111400)CREST Project of Japan Science and Technology Agency
文摘Copper oxide nanowires with varying oxidation states are prepared and their activity for water oxidation is studied. The nanowires with a CuO phase are found to be the most active, and their degree of crystallinity is important in achieving efficient water oxidation. For the crystalline CuO nanowires in a weakly basic Na2CO3 electrolyte, a Tafel slope of 41 mV/decade, an overpotential of approximately 500 mV at - 10 mA/crn2 (without compensation for the solution resistance), and a faradaic efficiency of nearly 100% are obtained. This electrode maintains a stable current for over 15 lx The low overpotential of 500 mV at 10 mA/cm2, small Tafel slope, long-term stability, and low cost make CuO one of the most promising catalysts for water oxidation. Moreover, the evolution of the CuO nanowire morphology over time is studied by electron microscop)-revealing that the diffusion of Cu ions from the interior of the nanowires to their surface causes the aggregation of individual nanowires over time. However, despite this aggregation, the current density remains nearly constant, because the total electrochemically active surface area of CuO does not change.
基金This work was partially supported by JST-CREST(Grant No.JPMJCR21O2).
文摘Knowledge in thermal and electric transport through grain boundary(GB)is crucial for designing nanostructured thermoelectric materials,where the transport greatly depends on GB atomistic structure.In this work,we employ machine learning(ML)techniques to study the relationship between silicon GB structure and its thermal and electric boundary conductance(TBC and EBC)calculated by Green’s function methods.We present a robust ML prediction model of TBC covering crystalline–crystalline and crystalline–amorphous interfaces,using disorder descriptors and atomic density.We also construct high-accuracy ML models for predicting both TBC and EBC and their ratio,using only small data of crystalline GBs.We found that the variations of interatomic angles and distance at GB are the most predictive descriptors for TBC and EBC,respectively.These results demonstrate the robustness of the black-box model and open the way to decouple thermal and electrical conductance,which is a key physical problem with engineering needs.
文摘To retrieve the fuel debris in Fukushima Daiichi Nuclear Power Plants(1F),it is essential to infer the fuel debris distribution.In particular,the molten metal spreading behavior is one of the vital phenomena in nuclear severe accidents because it determines the initial condition for further accident scenarios such as molten core concrete interaction(MCCI).In this study,the fundamental molten metal spreading experiments were performed with different outlet diameters and sample amounts to investigate the effect of the outlet for spreading-solidification behavior.In the numerical analysis,the moving particle full-implicit method(MPFI),which is one of the particle methods,was applied to simulate the spreading experiments.In the MPFI framework,the melting-solidification model including heat transfer,radiation heat loss,phase change,and solid fraction-dependent viscosity was developed and implemented.In addition,the difference in the spreading and solidification behavior due to the outlet diameters was reproduced in the calculation.The simulation results reveal the detailed solidification procedure during the molten metal spreading.It is found that the viscosity change and the solid fraction change during the spreading are key factors for the free surface condition and solidified materials.Overall,it is suggested that the MPFI method has the potential to simulate the actual nuclear melt-down phenomena in the future.
基金supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization(NEDO).Part of this work was conducted at the Advanced Characterization Nanotechnology Platform of the University of Tokyo,supported by the“Nanotechnology Platform”of the Ministry of Education,Culture,Sports,Science and Technology(MEXT),Japan(No.JPMXP09A-19-UT-0023).
文摘Ta3N5 is regarded as a promising photocatalyst for solar water splitting because of its excellent visible light absorption characteristics and simple composition.Conventional Ta3N5 photocatalysts prepared from oxide precursors typically comprise aggregated polycrystalline particles with defects and grain boundaries that reduce the water oxidation activity of the material.In the present work,well-dispersed Ta3N5 nanoparticulate single crystals were synthesized via a mild nitridation process using pure Ta metal nanopowder or Ta nanopowder mixed with NaCl.The resulting high-quality Ta3N5 nanoparticles,after loading with an oxygen evolution cocatalyst,exhibited impressively high photocatalytic performance during O_(2)evolution from a sacrificial AgNO3 solution,with an apparent quantum yield of 9.4%at 420 nm.Our findings suggest a new approach to the facile fabrication of nanostructured single-crystal photocatalysts for efficient solar water splitting,based on the use of metal nanopowders.
基金supported by Japan Society for the Promotion of Science KAKENHI(Grant Nos.JP19H05786,JP21H04532,JP21H04618,JP21K20484,JP20H02421,JP22K14143,JP17H01238,and JP17H06094)A.Nakamura and E.Tochigi acknowledge the financial support of JST PRESTO(Grant Nos.JPMJPR199A and JPMJPR1999)X.Fang acknowledges the financial support by the Athene Young Investigator Programme at TU Darmstadt.
文摘Dislocation-mediated plasticity in inorganic semiconductors and oxides has attracted increasing research interest because of the promising mechanical and functional properties tuned by dislocations.In this study,we investigated the effects of light illumination on the dislocation-mediated plasticity in hexagonal wurtzite ZnO,a representative third-generation semiconductor material.A(0001)45o off sample was specially designed to preferentially activate the basal slip on(0001)plane.Three types of nanoindentation tests were performed under four different light conditions(550 nm,334 nm,405 nm,and darkness),including low-load(60μN)pop-in tests,high-load(500μN)nanoindentation tests,and nanoindentation creep tests.The maximum shear stresses at pop-in were found to approximate the theoretical shear strength regardless of the light conditions.The activation volume at pop-ins was calculated to be larger in light than in darkness.Cross-sectional transmission electron microscope images taken from beneath the indentation imprints showed that all indentation-induced dislocations were located beneath the indentation imprint in a thin-plate shape along one basal slip plane.These indentation-induced dislocations could spread much deeper in darkness than in light,revealing the suppressive effect of light on dislocation behavior.An analytical model was adopted to estimate the elastoplastic stress field beneath the indenter.It was found that dislocation glide ceased at a higher stress level in light,indicating the increase in the Peierls barrier under light illumination.Furthermore,nanoindentation creep tests showed the suppression of both indentation depth and creep rate by light.Nanoindentation creep also yielded a larger activation volume in light than in darkness.
基金The numerical calculations were conducted on the five supercomputer systems,Fugaku at the RIKEN Center for Computational Science,Kobe,Japanthe supercomputer at the Research Center for Computational Science,Okazaki,Japan(Project:21-IMS-C126,22-IMS-C125)+7 种基金the supercomputer Ohtaka at the Supercomputer Center,the Institute for Solid State Physics,the University of Tokyo,Tokyo,Japanthe supercomputer TSUBAME3.0 at the Tokyo Institute of Technology,Tokyo,Japanthe supercomputer ABCI at the National Institute of Advanced Industrial Science and Technology,Tsukuba,JapanThis work was supported by the following five grants:a JST CREST(Grant Number JPMJCR19I3 to J.M.and R.Y.)the MEXT as“Program for Promoting Researches on the Supercomputer Fugaku”(Project ID:hp210264 to R.Y.)the Grant-in-Aid for Scientific Research(A)from the Japan Society for the Promotion of Science(19H01132 to R.Y.)the Grant-in-Aid for Scientific Research(C)from the Japan Society for the Promotion of Science(22K11949 to Y.H.)the HPCI System Research Project(Project ID:hp210213 to Y.H.).
文摘The spread of data-driven materials research has increased the need for systematically designed materials property databases.However,the development of polymer databases has lagged far behind other material systems.We present RadonPy,an open-source library that can automate the complete process of all-atom classical molecular dynamics(MD)simulations applicable to a wide variety of polymeric materials.Herein,15 different properties were calculated for more than 1000 amorphous polymers.The MD-calculated properties were systematically compared with experimental data to validate the calculation conditions;the bias and variance in the MD-calculated properties were successfully calibrated by a machine learning technique.During the high-throughput data production,we identified eight amorphous polymers with extremely high thermal conductivity(>0.4 W∙m^(–1)∙K^(–1))and their underlying mechanisms.Similar to the advancement of materials informatics since the advent of computational property databases for inorganic crystals,database construction using RadonPy will promote the development of polymer informatics.