Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using model...Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_(2-x)Ni_xO_(4)(0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic(FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni^(3+)increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_(1.6)Ni_(0.4)O_(4) shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe_(2)O_(4) and unactivated ZnFe_(1.6)Ni_(0.4)O_(4), and even superior to the benchmark IrO_(2) under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe_(2)O_(4). We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.展开更多
Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of ...Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of the electronic structure of NiS_(x),which accelerates the dissociation of H2O and the adsorption of OH−in the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)processes,respectively.In addition,the magnetically active Mo-NiS_(x)/NF can further enhance the HER and OER activity under an applied magnetic field due to the magnetoresistance effect and the ferromagnetic(FM)exchange-field penetration effect.As a result,Mo-NiS_(x)/NF requires low overpotentials of 307 mV at 50mA cm^(−2)(for OER)and 136 mV at 10mA cm^(−2)(for HER)under a magnetic field of 10000 G.Furthermore,the electrolytic cell constructed by the bifunctional Mo-NiS_(x)/NFs as both the cathode and the anode shows a low cell voltage of 1.594 V at 10 mA cm^(−2)with optimal stability over 60 h under the magnetic field.Simultaneous enhancement of the HER and OER processes by an external magnetic field through rational design of electrocatalysts might be promising for overall water splitting applications.展开更多
NiOx/Ni81Fe19 and Co/AlOx/Co magnetic multilayers were fabricated by reactive RF/DC magnetron sputtering on clean glass substrates and oxidized Si (100) substrates, respectively. The exchange biasing field (H-ex) betw...NiOx/Ni81Fe19 and Co/AlOx/Co magnetic multilayers were fabricated by reactive RF/DC magnetron sputtering on clean glass substrates and oxidized Si (100) substrates, respectively. The exchange biasing field (H-ex) between NiO4 and Ni81Fe19 as a function of NiOx oxidation states was studied by X-ray photoelectron spectroscopy (XPS). The oxidation states and the oxide thickness of Al layers in magnetic multilayer films consisting of Co/AlOx/Co were also analyzed. It is found that the H-sr of NiOx/Ni81Fe19 films only depends on Ni2+ but not on Ni3+ or Ni. The bottom Co can be completely covered by depositing an A I layer thicker than 2.0 nm. The oxide layer was Al2O3, and its thickness was 1.15 mn.展开更多
Ta/NTiO/NiFe/Ta multilayers were prepared by radio frequency reactive and dc magnetron sputtering. The exchange coupling field between NiO and NiFe reached 9.6 x 10(3) A/m. The compositions and chemical states at the ...Ta/NTiO/NiFe/Ta multilayers were prepared by radio frequency reactive and dc magnetron sputtering. The exchange coupling field between NiO and NiFe reached 9.6 x 10(3) A/m. The compositions and chemical states at the interface region of NiO/NiFe were studied using the X-ray photoelectron spectroscopy (XPS) and peak decomposition technique, The results show that there are two thermodynamically favorable reactions at NiO/NiFe interface: NiO+Fe = Ni + FeO and 3NiO+2Fe =3 Ni+Fe2O3. The thickness of the chemical reaction area estimated by angle-resolved XPS was about 1-1.5 nm. These interface reaction products appear magnetic defects, and the exchange coupling field H-ex and the coereivity H-c of NiO/NiFe are affected by these defects.展开更多
In this work, we experimentally investigated the thermal stability of the interlayer exchange coupling field(Hex) and strength(-Jiec) in synthetic antiferromagnetic(SAF) structure of [Pt(0.6)/Co(0.6)]2/Ru(tRu)/[Co(0.6...In this work, we experimentally investigated the thermal stability of the interlayer exchange coupling field(Hex) and strength(-Jiec) in synthetic antiferromagnetic(SAF) structure of [Pt(0.6)/Co(0.6)]2/Ru(tRu)/[Co(0.6)/Pt(0.6)]4multilayers with perpendicular anisotropy. Depending on the thickness of the spacing ruthenium(Ru) layer, the observed interlayer exchange coupling can be either ferromagnetic or antiferromagnetic. The Hexwere studied by measuring the magnetization hysteresis loops in the temperature range from 100 K to 700 K as well as the theoretical calculation of the-Jiec. It is found that the interlayer coupling in the multilayers is very sensitive to the thickness of Ru and temperature. The Hexexhibits either a linear or a non-linear dependence on the temperature for different thickness of Ru. Furthermore, our SAF multilayers show a high thermal stability even up to 600 K(Hex= 3.19 kOe,-Jiec= 1.97 erg/cm~2 for tRu=0.6 nm, the unit 1 Oe = 79.5775 A·m-1), which was higher than the previous studies.展开更多
The exchange bias field of NiFe/FeMn films with Ta/ Cu buffer was proved tobe lower than that of the films with Ta buffer. The crystallographic texture, surface roughness andelements distribution were examined in thes...The exchange bias field of NiFe/FeMn films with Ta/ Cu buffer was proved tobe lower than that of the films with Ta buffer. The crystallographic texture, surface roughness andelements distribution were examined in these two sets of samples, and there is no apparentdifference for the texture and roughness. However, the segregation of Cu atoms above NiFe surface inthe multilayer of Ta/Cu/NiFe has been observed by using the angle-resolved X-ray photoelectronspectroscopy (XPS). The decrease of the exchange bias field for NiFe/FeMn films with Ta/ Cu bufferlayers is mainly caused by the Cu atoms segregation at the interface between NiFe and FeMn.展开更多
The NiFe/FeMn bilayers with different buffer layers (Ta or Ta/Cu) were prepared by magnetron sputtering. Results show that the exchange coupling field of NiFe/FeMn fllms with Ta buffer is higher than that of the films...The NiFe/FeMn bilayers with different buffer layers (Ta or Ta/Cu) were prepared by magnetron sputtering. Results show that the exchange coupling field of NiFe/FeMn fllms with Ta buffer is higher than that of the films with Ta/ Cu buffer. We analysed the reasons by investigating the crystallographic texture, surface roughness and surface segregation of both fllms, respectively. We found that the decrease of the exchange coupling fields of NiFe/FeMn fllms with Ta/ Cu buffer layers was mainly caused by the Cu surface segregation on NiFe surface.展开更多
基金supported by the National Key R&D Program of China (2020YFA0710000)the National Natural Science Foundation of China (22278307, 22008170, 21978200, 22161142002, and 22121004)+2 种基金the Applied Basic Research Program of Qinghai Province (2023-ZJ-701)the Haihe Laboratory of Sustainable Chemical Transformationsthe Tianjin Research Innovation Project for Postgraduate Students (2022BKYZ035)。
文摘Sluggish reaction kinetics of oxygen evolution reaction(OER), resulting from multistep proton-coupled electron transfer and spin constriction, limits overall efficiency for most reported catalysts. Herein, using modeled ZnFe_(2-x)Ni_xO_(4)(0 ≤ x ≤ 0.4) spinel oxides, we aim to develop better OER electrocatalyst through combining the construction of ferromagnetic(FM) ordering channels and generation of highly active reconstructed species. The number of symmetry-breaking Fe–O–Ni structure links to the formation of FM ordering electron transfer channels. Meanwhile, as the number of Ni^(3+)increases, more ligand holes are formed, beneficial for redirecting surface reconstruction. The electro-activated ZnFe_(1.6)Ni_(0.4)O_(4) shows the highest specific activity, which is 13 and 2.5 times higher than that of ZnFe_(2)O_(4) and unactivated ZnFe_(1.6)Ni_(0.4)O_(4), and even superior to the benchmark IrO_(2) under the overpotential of 350 mV. Applying external magnetic field can make electron spin more aligned, and the activity can be further improved to 39 times of ZnFe_(2)O_(4). We propose that intriguing FM exchange-field interaction at FM/paramagnetic interfaces can penetrate FM ordering channels into reconstructed oxyhydroxide layers, thereby activating oxyhydroxide layers as spin-filter to accelerate spin-selective electron transfer. This work provides a new guideline to develop highly efficient spintronic catalysts for water oxidation and other spin-forbidden reactions.
基金National Natural Science Foundation of China,Grant/Award Numbers:21871065,22071038Heilongjiang Touyan Team,Grant/Award Number:HITTY‐20190033Interdisciplinary Research Foundation of HIT,Grant/Award Number:IR2021205。
文摘Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of the electronic structure of NiS_(x),which accelerates the dissociation of H2O and the adsorption of OH−in the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)processes,respectively.In addition,the magnetically active Mo-NiS_(x)/NF can further enhance the HER and OER activity under an applied magnetic field due to the magnetoresistance effect and the ferromagnetic(FM)exchange-field penetration effect.As a result,Mo-NiS_(x)/NF requires low overpotentials of 307 mV at 50mA cm^(−2)(for OER)and 136 mV at 10mA cm^(−2)(for HER)under a magnetic field of 10000 G.Furthermore,the electrolytic cell constructed by the bifunctional Mo-NiS_(x)/NFs as both the cathode and the anode shows a low cell voltage of 1.594 V at 10 mA cm^(−2)with optimal stability over 60 h under the magnetic field.Simultaneous enhancement of the HER and OER processes by an external magnetic field through rational design of electrocatalysts might be promising for overall water splitting applications.
基金the National Natural Science Foundation of China under Grant No. 19890310.]
文摘NiOx/Ni81Fe19 and Co/AlOx/Co magnetic multilayers were fabricated by reactive RF/DC magnetron sputtering on clean glass substrates and oxidized Si (100) substrates, respectively. The exchange biasing field (H-ex) between NiO4 and Ni81Fe19 as a function of NiOx oxidation states was studied by X-ray photoelectron spectroscopy (XPS). The oxidation states and the oxide thickness of Al layers in magnetic multilayer films consisting of Co/AlOx/Co were also analyzed. It is found that the H-sr of NiOx/Ni81Fe19 films only depends on Ni2+ but not on Ni3+ or Ni. The bottom Co can be completely covered by depositing an A I layer thicker than 2.0 nm. The oxide layer was Al2O3, and its thickness was 1.15 mn.
基金This work was financially supported by the National Natural Science Foundation of China (No. 19890310).
文摘Ta/NTiO/NiFe/Ta multilayers were prepared by radio frequency reactive and dc magnetron sputtering. The exchange coupling field between NiO and NiFe reached 9.6 x 10(3) A/m. The compositions and chemical states at the interface region of NiO/NiFe were studied using the X-ray photoelectron spectroscopy (XPS) and peak decomposition technique, The results show that there are two thermodynamically favorable reactions at NiO/NiFe interface: NiO+Fe = Ni + FeO and 3NiO+2Fe =3 Ni+Fe2O3. The thickness of the chemical reaction area estimated by angle-resolved XPS was about 1-1.5 nm. These interface reaction products appear magnetic defects, and the exchange coupling field H-ex and the coereivity H-c of NiO/NiFe are affected by these defects.
基金Project supported by the National Natural Science Foundation of China(Grant No.11704191)the Jiangsu Specially-Appointed Professor,the Natural Science Foundation of Jiangsu Province of China(Grant No.BK20171026)the Six-Talent Peaks Project in Jiangsu Province,China(Grant No.XYDXX-038)
文摘In this work, we experimentally investigated the thermal stability of the interlayer exchange coupling field(Hex) and strength(-Jiec) in synthetic antiferromagnetic(SAF) structure of [Pt(0.6)/Co(0.6)]2/Ru(tRu)/[Co(0.6)/Pt(0.6)]4multilayers with perpendicular anisotropy. Depending on the thickness of the spacing ruthenium(Ru) layer, the observed interlayer exchange coupling can be either ferromagnetic or antiferromagnetic. The Hexwere studied by measuring the magnetization hysteresis loops in the temperature range from 100 K to 700 K as well as the theoretical calculation of the-Jiec. It is found that the interlayer coupling in the multilayers is very sensitive to the thickness of Ru and temperature. The Hexexhibits either a linear or a non-linear dependence on the temperature for different thickness of Ru. Furthermore, our SAF multilayers show a high thermal stability even up to 600 K(Hex= 3.19 kOe,-Jiec= 1.97 erg/cm~2 for tRu=0.6 nm, the unit 1 Oe = 79.5775 A·m-1), which was higher than the previous studies.
文摘The exchange bias field of NiFe/FeMn films with Ta/ Cu buffer was proved tobe lower than that of the films with Ta buffer. The crystallographic texture, surface roughness andelements distribution were examined in these two sets of samples, and there is no apparentdifference for the texture and roughness. However, the segregation of Cu atoms above NiFe surface inthe multilayer of Ta/Cu/NiFe has been observed by using the angle-resolved X-ray photoelectronspectroscopy (XPS). The decrease of the exchange bias field for NiFe/FeMn films with Ta/ Cu bufferlayers is mainly caused by the Cu atoms segregation at the interface between NiFe and FeMn.
基金This work was supported by the National Natural Science Foundation of China (Grant No. 19890310).
文摘The NiFe/FeMn bilayers with different buffer layers (Ta or Ta/Cu) were prepared by magnetron sputtering. Results show that the exchange coupling field of NiFe/FeMn fllms with Ta buffer is higher than that of the films with Ta/ Cu buffer. We analysed the reasons by investigating the crystallographic texture, surface roughness and surface segregation of both fllms, respectively. We found that the decrease of the exchange coupling fields of NiFe/FeMn fllms with Ta/ Cu buffer layers was mainly caused by the Cu surface segregation on NiFe surface.
