This paper deals with a novel dual shield TIG welding method named gas pool coupled activating TIG( GPCA-TIG)welding. The welding method divides the shielding gas into two layers. Inert gas such as Ar is adopted as th...This paper deals with a novel dual shield TIG welding method named gas pool coupled activating TIG( GPCA-TIG)welding. The welding method divides the shielding gas into two layers. Inert gas such as Ar is adopted as the inner layer gas to protect the tungsten electrode and the molten pool metal. Pure O_2,N_2 or mixture of them are used as the outer layer gas to increase the weld penetration and improve the low temperature toughness of weld metal. Through analyzing the interaction between outer gas and arc and the distributions and existing forms of oxygen and nitrogen elements,the transfer behaviors of nitrogen and oxygen from arc to pool were investigated. The results show that,the interaction between the outer gas and arc plasma makes the arc slightly constrict. The incoming oxygen enriches on the molten pool surface and exists in the form of iron oxide,chromium oxide,manganese oxide and silicon oxygen compounds. The incoming nitrogen evenly distributes in the molten pool and exists in the form of nitrogen atom.展开更多
Oxygen reduction reaction(ORR)plays an important role in the next-generation energy storage technologies,whereas it involves the sluggish and complicated proton-coupled electron transfer(PCET)steps that greatly limit ...Oxygen reduction reaction(ORR)plays an important role in the next-generation energy storage technologies,whereas it involves the sluggish and complicated proton-coupled electron transfer(PCET)steps that greatly limit the ORR kinetics.Therefore,it is urgent to construct an efficient catalyst that could simultaneously achieve the rapid oxygen-containing intermediates conversion and fast PCET process but remain challenging.Herein,the adjacent Fe_(3)C nanoparticles coupling with single Fe sites on the bubble-wrap-like porous N-doped carbon(Fe_(3)C@FeSA-NC)were deliberately constructed.Theoretical investigations reveal that the adjacent Fe_(3)C nanoparticles speed up the water dissociation and serve as proton-feeding centers for boosting the ORR kinetics of single Fe sites.Benefiting from the synergistic effect of the Fe_(3)C and single Fe sites,the Fe_(3)C@FeSA-NC affords an excellent half-wave potential of 0.88 V,and enables the assembled Zn-air batteries with the high peak power density of 164.5 mW·cm^(-2)and long-term stability of over 200 h at high current densities at 50 mA·cm^(-2).This work clarifies the mechanism for improving ORR kinetics of single atomic sites by engineering the adjacent proton-feeding centers,shedding light on the rational design of cost-effective electrocatalysts for energy conversion and storage technologies.展开更多
Due to 4f electron characteristics and alternation valence, cerium involved in an oxidation-reduction reaction in plant, closely relating to photosynthesis. Our studies proved that cerium could promote photosynthesis ...Due to 4f electron characteristics and alternation valence, cerium involved in an oxidation-reduction reaction in plant, closely relating to photosynthesis. Our studies proved that cerium could promote photosynthesis and greatly improve spinach growth. However, the mechanism of promoting energy transfer and conversion by cerium remains unclear. Here we reported that the effects of Ce^3＋ on energy transfer and oxygen evolution in photosystem Ⅱ （PS Ⅱ ） isolated from spinach, which was related to 4f electron characteristics and alternation valence in Ce molecule. The methods of absorption spectrum, fluorescence spectrum were used in the research. Results showed that Ce^3＋ treatment at low concentration could suitably change PS Ⅱ mieroenvironment, increase the absorbance of visible light, improve the energy transfer among amino acids within PS Ⅱ protein-pigment complex, and accelerate energy transport from tyrosine residue to chlorophyll a. In summary, the photochemical activity of PS Ⅱ （fluorescence quantum yield） and its oxygen evolving rate were enhanced by Ce^3＋.展开更多
Photocatalytic water oxidation is a crucial step in water splitting,but is generally restricted by the slow kinetics.Therefore,it is necessary to develop high-performance water oxidation photocatalysts.Herein,the Fe-d...Photocatalytic water oxidation is a crucial step in water splitting,but is generally restricted by the slow kinetics.Therefore,it is necessary to develop high-performance water oxidation photocatalysts.Herein,the Fe-doped Bi2WO6 nanosheets with oxygen vacancies(OVs)were synthesized for enhanced photocatalytic water oxidation efficiency,showing a synergistic effect between Fe dopants and OVs.When a molar fraction of 2%Fe was doped into the Bi2WO6 nanosheets,the visible-light-driven photocatalytic oxygen evolution rate was increased up to 131.3μmol·h^(-1)·g_(cat)^(-1)under ambient conditions,which was more than 3 times that of pure Bi2WO6 nanosheets.The proper doping concentration of Fe could promote the formation of OVs and at the same time modulate the band structure of catalysts,especially the position of the valence band maximum(VBM),leading to effective visible-light absorption and enhanced oxidizing ability of photogenerated holes.With ameliorated localized electron distribution,fast charge transfer channel emerged between the OVs and adjacent metal atoms,which accelerated the charge carrier transfer and promoted the separation of photoexcited electrons and holes.This work provides feasible approaches for designing efficient two-dimensional semiconductor water oxidation photocatalysts that could utilize visible-light,which will make more use of solar energy.展开更多
Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.E...Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.Engineering the doping of 2D TMDs,especially hole doping is highly desirable towards their device function.Herein,controllable oxygen-induced p-type doping in a range of hexagonal(MoTe2,WSe2,MoSe2 and PtSe2)and pentagonal(PdSe2)2D TMDs are demonstrated.Scanning tunneling microscopy,electrical transport and X-ray photoelectron spectroscopy are used to probe the origin of oxygen-derived hole doping.Three mechanisms are postulated that contribute to the hole doping in 2D TMDs,namely charge transfer from absorbed oxygen molecules,surface oxides,and chalcogen atom substitution.This work provides insights into the doping effects of oxygen,enabling the engineering of 2D TMDs properties for nanoelectronic applications.展开更多
基金supported by National Natural Science Foundation of China(Grant No.51265029)
文摘This paper deals with a novel dual shield TIG welding method named gas pool coupled activating TIG( GPCA-TIG)welding. The welding method divides the shielding gas into two layers. Inert gas such as Ar is adopted as the inner layer gas to protect the tungsten electrode and the molten pool metal. Pure O_2,N_2 or mixture of them are used as the outer layer gas to increase the weld penetration and improve the low temperature toughness of weld metal. Through analyzing the interaction between outer gas and arc and the distributions and existing forms of oxygen and nitrogen elements,the transfer behaviors of nitrogen and oxygen from arc to pool were investigated. The results show that,the interaction between the outer gas and arc plasma makes the arc slightly constrict. The incoming oxygen enriches on the molten pool surface and exists in the form of iron oxide,chromium oxide,manganese oxide and silicon oxygen compounds. The incoming nitrogen evenly distributes in the molten pool and exists in the form of nitrogen atom.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52261145700 and 22279124)the Natural Science Foundation of Shandong Province(No.ZR2020ZD10)the Fundamental Research Funds for the Central Universities(No.202262010).
文摘Oxygen reduction reaction(ORR)plays an important role in the next-generation energy storage technologies,whereas it involves the sluggish and complicated proton-coupled electron transfer(PCET)steps that greatly limit the ORR kinetics.Therefore,it is urgent to construct an efficient catalyst that could simultaneously achieve the rapid oxygen-containing intermediates conversion and fast PCET process but remain challenging.Herein,the adjacent Fe_(3)C nanoparticles coupling with single Fe sites on the bubble-wrap-like porous N-doped carbon(Fe_(3)C@FeSA-NC)were deliberately constructed.Theoretical investigations reveal that the adjacent Fe_(3)C nanoparticles speed up the water dissociation and serve as proton-feeding centers for boosting the ORR kinetics of single Fe sites.Benefiting from the synergistic effect of the Fe_(3)C and single Fe sites,the Fe_(3)C@FeSA-NC affords an excellent half-wave potential of 0.88 V,and enables the assembled Zn-air batteries with the high peak power density of 164.5 mW·cm^(-2)and long-term stability of over 200 h at high current densities at 50 mA·cm^(-2).This work clarifies the mechanism for improving ORR kinetics of single atomic sites by engineering the adjacent proton-feeding centers,shedding light on the rational design of cost-effective electrocatalysts for energy conversion and storage technologies.
基金Project supported by the National Natural Science Foundation of China (20671067, 30470150)
文摘Due to 4f electron characteristics and alternation valence, cerium involved in an oxidation-reduction reaction in plant, closely relating to photosynthesis. Our studies proved that cerium could promote photosynthesis and greatly improve spinach growth. However, the mechanism of promoting energy transfer and conversion by cerium remains unclear. Here we reported that the effects of Ce^3＋ on energy transfer and oxygen evolution in photosystem Ⅱ （PS Ⅱ ） isolated from spinach, which was related to 4f electron characteristics and alternation valence in Ce molecule. The methods of absorption spectrum, fluorescence spectrum were used in the research. Results showed that Ce^3＋ treatment at low concentration could suitably change PS Ⅱ mieroenvironment, increase the absorbance of visible light, improve the energy transfer among amino acids within PS Ⅱ protein-pigment complex, and accelerate energy transport from tyrosine residue to chlorophyll a. In summary, the photochemical activity of PS Ⅱ （fluorescence quantum yield） and its oxygen evolving rate were enhanced by Ce^3＋.
基金This work was financially supported by the National Key R&D Program of China(No.2017YFA0207301)the National Natural Science Foundation of China(Nos.21622107,11621063,U1532265,and 21890750)+1 种基金the Youth Innovation Promotion Association CAS(No.2016392),the Key Research Program of Frontier Sciences(No.QYZDY-SSW-SLH011)the Major Program of Development Foundation of Hefei Center for Physical Science and Technology(No.2017FXZY003).
文摘Photocatalytic water oxidation is a crucial step in water splitting,but is generally restricted by the slow kinetics.Therefore,it is necessary to develop high-performance water oxidation photocatalysts.Herein,the Fe-doped Bi2WO6 nanosheets with oxygen vacancies(OVs)were synthesized for enhanced photocatalytic water oxidation efficiency,showing a synergistic effect between Fe dopants and OVs.When a molar fraction of 2%Fe was doped into the Bi2WO6 nanosheets,the visible-light-driven photocatalytic oxygen evolution rate was increased up to 131.3μmol·h^(-1)·g_(cat)^(-1)under ambient conditions,which was more than 3 times that of pure Bi2WO6 nanosheets.The proper doping concentration of Fe could promote the formation of OVs and at the same time modulate the band structure of catalysts,especially the position of the valence band maximum(VBM),leading to effective visible-light absorption and enhanced oxidizing ability of photogenerated holes.With ameliorated localized electron distribution,fast charge transfer channel emerged between the OVs and adjacent metal atoms,which accelerated the charge carrier transfer and promoted the separation of photoexcited electrons and holes.This work provides feasible approaches for designing efficient two-dimensional semiconductor water oxidation photocatalysts that could utilize visible-light,which will make more use of solar energy.
基金This work was financially supported by the National Natural Science Foundation of China(No.51472164)Shenzhen Peacock Plan(No.KQTD2016053112042971)+3 种基金the Educational Commission of Guangdong Province(Nos.2015KGJHZ006 and 2016KCXTD006)the Science and Technology Planning Project of Guangdong Province(No.2016B050501005)A.T.S.W.acknowledges funding support from MOE Tier 2 grant R 144-000-382-112,A*STAR Pharos Program(No.1527300025)facility support from the NUS Centre for Advanced 2D Materials(CA2DM).
文摘Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.Engineering the doping of 2D TMDs,especially hole doping is highly desirable towards their device function.Herein,controllable oxygen-induced p-type doping in a range of hexagonal(MoTe2,WSe2,MoSe2 and PtSe2)and pentagonal(PdSe2)2D TMDs are demonstrated.Scanning tunneling microscopy,electrical transport and X-ray photoelectron spectroscopy are used to probe the origin of oxygen-derived hole doping.Three mechanisms are postulated that contribute to the hole doping in 2D TMDs,namely charge transfer from absorbed oxygen molecules,surface oxides,and chalcogen atom substitution.This work provides insights into the doping effects of oxygen,enabling the engineering of 2D TMDs properties for nanoelectronic applications.
