As a low-cost visible-light-driven metal-free catalyst, graphitic carbon nitride(g-CN) has attracted increasing attention due to its wide applications for solar energy conversion, environmental purification,and organi...As a low-cost visible-light-driven metal-free catalyst, graphitic carbon nitride(g-CN) has attracted increasing attention due to its wide applications for solar energy conversion, environmental purification,and organic photosynthesis. In particular, the catalytic performance of g-CNcan be easily modulated by modifying morphology, doping, and copolymerization. Simultaneous optimization, however, has little been achieved. Herein, a facile one-pot strategy is developed to synthesize porous B-doped g-CNnanosheets by using HBOand urea as the precursor during thermal polymerization. The resultant B-doped g-CNnanosheets retain the original framework of bulk g-CN, while induce prominently enhanced visible light harvesting and narrowing band gap by 0.32 eV compared to pure g-CN. Moreover, the adsorption capacity and photodegradation kinetics of methylene blue(MB) under visible light irradiation over B-doped g-CNnanosheets can be improved by 20.5 and 17 times, respectively. The synthesized porous B-doped g-CNnanosheets also exhibit higher activities than pure g-CNas bifunctional electrocatalyst for both oxygen evolution reaction(OER) and oxygen reduction reaction(ORR). The enhanced catalyst performance of porous B-doped g-CNnanosheets stems from the strong synergistic effect originating from the larger exposed active sites generated by the exfoliation of g-CNinto nanosheets and the porous structure, as well as the better conductivity owing to B-doping. This work provides a simple, effective, and robust method for the synthesis of g-CN-based nanomaterial with superior properties to meet the needs of various applications.展开更多
Ni-rich layered oxides are considered promising cathodes for advanced lithium-ion batteries(LIBs)in the future,owing to their high capacity and low cost.However,the issues on structural and interfacial stability of Ni...Ni-rich layered oxides are considered promising cathodes for advanced lithium-ion batteries(LIBs)in the future,owing to their high capacity and low cost.However,the issues on structural and interfacial stability of Ni-rich cathodes still pose substantial obstacles in the practical application of advanced LIBs.Here,we employ a one-step method to synthesize a B-doped and La_(4)NiLiO_(8)-coated LiNi_(0.82)5Co_(0.115)Mn_(0.06)O_(2)(BL-1)cathode with reliable structure and interface,for the first time.The La_(4)NiLiO_(8)coating layer can prevent cathodes from electrolyte assault and facilitate Li+diffusion kinetics.Moreover,B-doping can effectively restrain the pernicious H_(2)-H_(3) phase transition and adjust the orientation of primary particles to a radial alignment,which is obstructive to the arise of microcracks induced by the change of anisotropic volume.Specifically,when tested in pouch cells,the BL-1 cathode exhibits outstanding capacity retention of 93.49%after 500 cycles at 1 C.This dual-modification strategy dramatically enhances the stability of the structure and interface for Ni-rich cathode materials,consequently accelerating the commercialization process of high-energy–density LIBs.展开更多
Neutron-sensitive microchannel plates(nMCPs)have applications in neutron detection,including energy spectrum measurements,neutron-induced cross sections,and neutron imaging.10B-doped MCPs(B-MCPs)have attracted signifi...Neutron-sensitive microchannel plates(nMCPs)have applications in neutron detection,including energy spectrum measurements,neutron-induced cross sections,and neutron imaging.10B-doped MCPs(B-MCPs)have attracted significant attention owing to their potential for exhibiting a high neutron detection efficiency over a large neutron energy range.Good spatial and temporal resolutions are useful for neutron energy-resolved imaging.However,their practical applications still face many technical challenges.In this study,a B-MCP with 10 mol%10B was tested for its response to wide-energy neutrons from eV to MeV at the Back-n white neutron source at the China Spallation Neutron Source.The neutron detection efficiency was calibrated at 1 eV,which is approximately 300 times that of an ordinary MCP and indicates the success of 10 B doping.The factors that caused the reduction in the detection efficiency were simulated and discussed.The neutron energy spectrum obtained using B-MCP was compared with that obtained by other measurement methods,and showed very good consistency for neutron energies below tens of keV.The response is more complicated at higher neutron energy,at which point the elastic and nonelastic reactions of all nuclides of B-MCP gradually become dominant.This is beneficial for the detection of neutrons,as it compensates for the detection efficiency of B-MCP for high-energy neutrons.展开更多
This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% im...This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% impurity concentration. Our comprehensive analysis encompasses structural properties, electronic band structures, and charge density distributions. The optimized lattice constant and band gap energy of 3C-SiC were found to be 4.373 Å and 1.36 eV respectively, which is in agreement with previous research (Bui, 2012;Muchiri et al., 2018). Our results show that B doping narrows the band gap, enhances electrical conductivity, and influences charge transfer interactions. The charge density analysis reveals substantial interactions between B dopants and surrounding carbon atoms. This work not only enhances our understanding of the material’s electronic properties, but also highlights the importance of charge density analysis for characterizing charge transfer mechanisms and their implications in the 3C-SiC semiconductors.展开更多
Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped ...Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped graphene(BG)-supported bimetallic oxides of Co and Ni were obtained and served as OER electrocatalysts.Surprisingly,the annealed Co-Ni-Ox/BG with a Co/Ni ratio of 1:1 exhibits high performance toward oxygen evolution in alkaline electrolyte.The overpotential is only 310 mV at the current density of 10 mA cm-2,superior to many mono-metallic oxides reported before,and even comparable to the commercial RuO2.The regulation of charge distribution in bimetallic oxides and the strong synergistic coupling effects together contribute to the superior electrocatalytic performance of the Co-Ni-Ox/BG toward OER.This study also offers several effective ways to design high-performance OER electrocatalysts for water splitting.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
文摘As a low-cost visible-light-driven metal-free catalyst, graphitic carbon nitride(g-CN) has attracted increasing attention due to its wide applications for solar energy conversion, environmental purification,and organic photosynthesis. In particular, the catalytic performance of g-CNcan be easily modulated by modifying morphology, doping, and copolymerization. Simultaneous optimization, however, has little been achieved. Herein, a facile one-pot strategy is developed to synthesize porous B-doped g-CNnanosheets by using HBOand urea as the precursor during thermal polymerization. The resultant B-doped g-CNnanosheets retain the original framework of bulk g-CN, while induce prominently enhanced visible light harvesting and narrowing band gap by 0.32 eV compared to pure g-CN. Moreover, the adsorption capacity and photodegradation kinetics of methylene blue(MB) under visible light irradiation over B-doped g-CNnanosheets can be improved by 20.5 and 17 times, respectively. The synthesized porous B-doped g-CNnanosheets also exhibit higher activities than pure g-CNas bifunctional electrocatalyst for both oxygen evolution reaction(OER) and oxygen reduction reaction(ORR). The enhanced catalyst performance of porous B-doped g-CNnanosheets stems from the strong synergistic effect originating from the larger exposed active sites generated by the exfoliation of g-CNinto nanosheets and the porous structure, as well as the better conductivity owing to B-doping. This work provides a simple, effective, and robust method for the synthesis of g-CN-based nanomaterial with superior properties to meet the needs of various applications.
基金financially supported by the National Natural Science Foundation of China(51774051,52072323,52122211)the Science and Technology Planning Project of Hunan Province(2019RS2034)+1 种基金the Hunan High-tech Industry Science and Technology Innovation Leading Plan(2020GK2072)the Changsha City Fund for Distinguished and Innovative Young Scholars(KQ1707014)。
文摘Ni-rich layered oxides are considered promising cathodes for advanced lithium-ion batteries(LIBs)in the future,owing to their high capacity and low cost.However,the issues on structural and interfacial stability of Ni-rich cathodes still pose substantial obstacles in the practical application of advanced LIBs.Here,we employ a one-step method to synthesize a B-doped and La_(4)NiLiO_(8)-coated LiNi_(0.82)5Co_(0.115)Mn_(0.06)O_(2)(BL-1)cathode with reliable structure and interface,for the first time.The La_(4)NiLiO_(8)coating layer can prevent cathodes from electrolyte assault and facilitate Li+diffusion kinetics.Moreover,B-doping can effectively restrain the pernicious H_(2)-H_(3) phase transition and adjust the orientation of primary particles to a radial alignment,which is obstructive to the arise of microcracks induced by the change of anisotropic volume.Specifically,when tested in pouch cells,the BL-1 cathode exhibits outstanding capacity retention of 93.49%after 500 cycles at 1 C.This dual-modification strategy dramatically enhances the stability of the structure and interface for Ni-rich cathode materials,consequently accelerating the commercialization process of high-energy–density LIBs.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515030074)the National Natural Science Foundation of China(No.12035017)。
文摘Neutron-sensitive microchannel plates(nMCPs)have applications in neutron detection,including energy spectrum measurements,neutron-induced cross sections,and neutron imaging.10B-doped MCPs(B-MCPs)have attracted significant attention owing to their potential for exhibiting a high neutron detection efficiency over a large neutron energy range.Good spatial and temporal resolutions are useful for neutron energy-resolved imaging.However,their practical applications still face many technical challenges.In this study,a B-MCP with 10 mol%10B was tested for its response to wide-energy neutrons from eV to MeV at the Back-n white neutron source at the China Spallation Neutron Source.The neutron detection efficiency was calibrated at 1 eV,which is approximately 300 times that of an ordinary MCP and indicates the success of 10 B doping.The factors that caused the reduction in the detection efficiency were simulated and discussed.The neutron energy spectrum obtained using B-MCP was compared with that obtained by other measurement methods,and showed very good consistency for neutron energies below tens of keV.The response is more complicated at higher neutron energy,at which point the elastic and nonelastic reactions of all nuclides of B-MCP gradually become dominant.This is beneficial for the detection of neutrons,as it compensates for the detection efficiency of B-MCP for high-energy neutrons.
文摘This study delves into the charge transfer mechanism of boron (B)-doped 3C-SiC through first-principles investigations. We explore the effects of B doping on the electronic properties of 3C-SiC, focusing on a 12.5% impurity concentration. Our comprehensive analysis encompasses structural properties, electronic band structures, and charge density distributions. The optimized lattice constant and band gap energy of 3C-SiC were found to be 4.373 Å and 1.36 eV respectively, which is in agreement with previous research (Bui, 2012;Muchiri et al., 2018). Our results show that B doping narrows the band gap, enhances electrical conductivity, and influences charge transfer interactions. The charge density analysis reveals substantial interactions between B dopants and surrounding carbon atoms. This work not only enhances our understanding of the material’s electronic properties, but also highlights the importance of charge density analysis for characterizing charge transfer mechanisms and their implications in the 3C-SiC semiconductors.
基金the financial supports from the National Natural Science Foundation of China(21902062 and 21705056)the Natural Science Foundation of Shandong Province(ZR2019YQ10 and ZR2018PB009)+1 种基金the Young Taishan Scholars Program(tsqn201812080)the Open Funds of the State Key Laboratory of Electroanalytical Chemistry(SKLEAC201901)。
文摘Developing electrocatalysts with high performance and low cost for the oxygen evolution reaction(OER)is of great importance for fabricating renewable energy storage and conversion devices.Here,a series of boron-doped graphene(BG)-supported bimetallic oxides of Co and Ni were obtained and served as OER electrocatalysts.Surprisingly,the annealed Co-Ni-Ox/BG with a Co/Ni ratio of 1:1 exhibits high performance toward oxygen evolution in alkaline electrolyte.The overpotential is only 310 mV at the current density of 10 mA cm-2,superior to many mono-metallic oxides reported before,and even comparable to the commercial RuO2.The regulation of charge distribution in bimetallic oxides and the strong synergistic coupling effects together contribute to the superior electrocatalytic performance of the Co-Ni-Ox/BG toward OER.This study also offers several effective ways to design high-performance OER electrocatalysts for water splitting.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
