Relationship between the activity for photocatalytic H_(2)O overall splitting(HOS)and the electron occupancy on d orbits of the active component in photocatalysts shows volcanic diagram,and specially the d^(10)electro...Relationship between the activity for photocatalytic H_(2)O overall splitting(HOS)and the electron occupancy on d orbits of the active component in photocatalysts shows volcanic diagram,and specially the d^(10)electronic configuration in valley bottom exhibits inert activity,which seriously fetters the development of catalytic materials with great potentials.Herein,In d^(10)electronic configuration of In_(2)O_(3)was activated by phosphorus atoms replacing its lattice oxygen to regulate the collocation of the ascended In 5p-band(Inɛ5p)and descended O 2p-band(Oɛ2p)centers as efficient active sites for chemisorption to*OH and*H during forward HOS,respectively,along with a declined In 4d-band center(Inɛ4d)to inhibit its backward reaction.A stable STH efficiency of 2.23%under AM 1.5 G irradiation at 65°C has been obtained over the activated d^(10)electronic configuration with a lowered activation energy for H_(2)evolution,verified by femtosecond transient absorption spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations of dynamics.These findings devote to activating d^(10)electronic configuration for resolving the reaction energy barrier and dynamical bottleneck of forward HOS,which expands the exploration of high-efficiency catalytic materials.展开更多
High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inhere...High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.展开更多
Many ＂rich - connected＂ topologies with multiple parallel paths between smwers have been proposed for data center networks recently to provide high bisection bandwidth, but it re mains challenging to fully utilize t...Many ＂rich - connected＂ topologies with multiple parallel paths between smwers have been proposed for data center networks recently to provide high bisection bandwidth, but it re mains challenging to fully utilize the high network capacity by appropriate multi- path routing algorithms. As flow-level path splitting may lead to trafl＇ic imbalance between paths due to flow- size difference, packet-level path splitting attracts more attention lately, which spreads packets from flows into multiple available paths and significantly improves link utilizations. However, it may cause packet reordering, confusing the TCP congestion control algorithm and lowering the throughput of flows. In this paper, we design a novel packetlevel multi-path routing scheme called SOPA, which leverag- es OpenFlow to perform packet-level path splitting in a round- robin fashion, and hence significantly mitigates the packet reordering problem and improves the network throughput. Moreover, SOPA leverages the topological feature of data center networks to encode a very small number of switches along the path into the packet header, resulting in very light overhead. Compared with random packet spraying （RPS）, Hedera and equal-cost multi-path routing （ECMP）, our simulations demonstrate that SOPA achieves 29.87%, 50.41% and 77.74% higher network throughput respectively under permutation workload, and reduces average data transfer completion time by 53.65%, 343.31% and 348.25% respectively under production workload.展开更多
Using the method of Picus and Beer invariants, general expressions are obtained for the total intensity I and the degree of circular polarization Рcirc.of the luminescence of GaAs-type semiconductors with the partici...Using the method of Picus and Beer invariants, general expressions are obtained for the total intensity I and the degree of circular polarization Рcirc.of the luminescence of GaAs-type semiconductors with the participation of shallow acceptor levels in a longitudinal magnetic field H. Special cases are analyzed depending on the value and direction of the magnetic field strength, as well as on the constants of the g-factor of the acceptor g1,g2and the conduction band electron ge. In the case of a strong magnetic field H// [100], [111], [110], a numerical calculation of the angular dependence of the quantities I and Рcirc.was performed for some critical values of g2/g1, at which Рcirc.exhibits a sharp anisotropy in the range from −100% to +100%, and the intensity of the crystal radiation along the magnetic field tends to a minimum value.展开更多
文摘Relationship between the activity for photocatalytic H_(2)O overall splitting(HOS)and the electron occupancy on d orbits of the active component in photocatalysts shows volcanic diagram,and specially the d^(10)electronic configuration in valley bottom exhibits inert activity,which seriously fetters the development of catalytic materials with great potentials.Herein,In d^(10)electronic configuration of In_(2)O_(3)was activated by phosphorus atoms replacing its lattice oxygen to regulate the collocation of the ascended In 5p-band(Inɛ5p)and descended O 2p-band(Oɛ2p)centers as efficient active sites for chemisorption to*OH and*H during forward HOS,respectively,along with a declined In 4d-band center(Inɛ4d)to inhibit its backward reaction.A stable STH efficiency of 2.23%under AM 1.5 G irradiation at 65°C has been obtained over the activated d^(10)electronic configuration with a lowered activation energy for H_(2)evolution,verified by femtosecond transient absorption spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations of dynamics.These findings devote to activating d^(10)electronic configuration for resolving the reaction energy barrier and dynamical bottleneck of forward HOS,which expands the exploration of high-efficiency catalytic materials.
基金support provided by the National Natural Science Foundation of China(Grant Nos.51972048,U23A20605)support provided by the Performance subsidy fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(Grant No.22567627H)the additional data in the revised manuscriptsupported by the National Key Research and Development Program of China(No.2022YFB3706300).
文摘High-entropy materials(HEMs),which are newly manufactured compounds that contain five or more metal cations,can be a platform with desired properties,including improved electrocatalytic performance owing to the inherent complexity.Here,a strain engineering methodology is proposed to design transition-metal-based HEM by Li manipulation(LiTM)with tunable lattice strain,thus tailoring the electronic structure and boosting electrocatalytic performance.As confirmed by the experiments and calculation results,tensile strain in the LiTM after Li manipulation can optimize the d-band center and increase the electrical conductivity.Accordingly,the asprepared LiTM-25 demonstrates optimized oxygen evolution reaction and hydrogen evolution reaction activity in alkaline saline water,requiring ultralow overpotentials of 265 and 42 mV at 10 mA cm−2,respectively.More strikingly,LiTM-25 retains 94.6%activity after 80 h of a durability test when assembled as an anion-exchange membrane water electrolyzer.Finally,in order to show the general efficacy of strain engineering,we incorporate Li into electrocatalysts with higher entropies as well.
基金supported by the National Basic Research Program of China(973 program)under Grant No.2014CB347800 and No.2012CB315803the National High-Tech R&D Program of China(863 program)under Grant No.2013AA013303+1 种基金the Natural Science Foundation of China under Grant No.61170291,No.61133006,and No.61161140454ZTE IndustryAcademia-Research Cooperation Funds
文摘Many ＂rich - connected＂ topologies with multiple parallel paths between smwers have been proposed for data center networks recently to provide high bisection bandwidth, but it re mains challenging to fully utilize the high network capacity by appropriate multi- path routing algorithms. As flow-level path splitting may lead to trafl＇ic imbalance between paths due to flow- size difference, packet-level path splitting attracts more attention lately, which spreads packets from flows into multiple available paths and significantly improves link utilizations. However, it may cause packet reordering, confusing the TCP congestion control algorithm and lowering the throughput of flows. In this paper, we design a novel packetlevel multi-path routing scheme called SOPA, which leverag- es OpenFlow to perform packet-level path splitting in a round- robin fashion, and hence significantly mitigates the packet reordering problem and improves the network throughput. Moreover, SOPA leverages the topological feature of data center networks to encode a very small number of switches along the path into the packet header, resulting in very light overhead. Compared with random packet spraying （RPS）, Hedera and equal-cost multi-path routing （ECMP）, our simulations demonstrate that SOPA achieves 29.87%, 50.41% and 77.74% higher network throughput respectively under permutation workload, and reduces average data transfer completion time by 53.65%, 343.31% and 348.25% respectively under production workload.
文摘Using the method of Picus and Beer invariants, general expressions are obtained for the total intensity I and the degree of circular polarization Рcirc.of the luminescence of GaAs-type semiconductors with the participation of shallow acceptor levels in a longitudinal magnetic field H. Special cases are analyzed depending on the value and direction of the magnetic field strength, as well as on the constants of the g-factor of the acceptor g1,g2and the conduction band electron ge. In the case of a strong magnetic field H// [100], [111], [110], a numerical calculation of the angular dependence of the quantities I and Рcirc.was performed for some critical values of g2/g1, at which Рcirc.exhibits a sharp anisotropy in the range from −100% to +100%, and the intensity of the crystal radiation along the magnetic field tends to a minimum value.
