Over the last two decades,extensive study has been done on two-dimensional Molybdenum Sulphide(MoS_(2))due to its outstanding features in energy storage applications.Although MoS_(2)has a lot of active sulphur edges,t...Over the last two decades,extensive study has been done on two-dimensional Molybdenum Sulphide(MoS_(2))due to its outstanding features in energy storage applications.Although MoS_(2)has a lot of active sulphur edges,the presence of inactive surfaces leads to limit conductivity and efficiency.Hence,in this article,we aimed to promote the additional active sites by doping various weight percentages(2%,4%,6%,8%and 10%)of Nickel(Ni)into the MoS_(2)matrix by simple hydrothermal technique,and their doping effects were investigated with the help of Physio-chemical analyses.X-ray diffraction(XRD)pattern,Raman,and chemical composition(XPS)analyses were used to confirm the Ni incorporation in MoS_(2)nanosheets.Microscopic investigations demonstrated that Ni-doped MoS_(2)nanosheets were vertically aligned with enhanced interlayer spacing.Cyclic voltammetry,Galvanostatic charge-discharge,and electrochemical impedance spectroscopy investigations were used to characterize the electrochemical characteristics.The 6%Ni-doped MoS_(2)electrode material showed better CSPof 528.7 F/g@1 A/g and excellent electrochemical stability(85%of capacitance retention after 10,000 cycles at 5 A/g)compared to other electrode materials.Furthermore,the solid-state asymmetric supercapacitor was assembled using Nidoped MoS_(2)and graphite as anode and cathode materials and analysed the electrochemical properties in the two-electrode system.To determine the impact of the Ni-atom on the MoS_(2)surface,firstprinciples computations were performed.Further,it was examined for electronic band structure,the projected density of states(PDOS)and Bader charge transfer analyses.展开更多
Magnetic properties of diluted magnetic semiconductors (DMSs), Ni-doped ZnO materials, prepared by sol-gel method were investigated by measuring magnetization as functions of magnetic field. The Ni content affects the...Magnetic properties of diluted magnetic semiconductors (DMSs), Ni-doped ZnO materials, prepared by sol-gel method were investigated by measuring magnetization as functions of magnetic field. The Ni content affects the magnetic properties at low sintered temperature but it has few effects on the magnetic properties at high sintered temperature. The sintered temperature has great effects on the magnetic properties of Ni/ZnO at high original mole ratio of Ni/Zn while it has slight effects on the magnetic properties of Ni/ZnO at low original mole ratio of Ni/Zn whatever low or high sintered temperature.展开更多
The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst.Herein,the urchin-like Ni-doped W_(18)O_(49)/NF with enriched active sites was prepared by solvothermal ...The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst.Herein,the urchin-like Ni-doped W_(18)O_(49)/NF with enriched active sites was prepared by solvothermal method followed by a low-temperature pyrolysis treatment was reported.Results demonstrate that the incorporation of Ni-doping triggers the lattice distortion of W_(18)O_(49) for the increasement of oxygen defects.Further,high-valent W^(6+)are partially reduced to low-valent W^(4+),wherein the electrons originate from the oxidation process of Ni^(2+)to Ni^(3+).The Ni^(3+)ions show an enhanced orbital overlap with the OER reaction intermediates.The generated W^(4+)ions contribute to release oxygen vacancies,eventually reorganizing Ni-doped W_(18)O_(49)/NF to unique electrochemical active species with a special amorphous-crystalline interface(AM/NiWO_x/NiOOH/NF).Simultaneously,the reconstruction results in an optimized valence band and conduction band.Eventually,the resultant AM/NiWO_x/NiOOH/NF with abundant active sites and improved oxidation/reduction capability exhibits more superior catalytic performance compared with the Ni-doped W_(18)O_(49)/NF counterpart.This study gives more insights in the electrochemical evolution of the tungsten-based oxide and provides effective strategies for optimizing the catalytic activity of materials with inherent hydrogen evolution reaction limitations.展开更多
The magnetic and structural properties of 2% Ni-doped ZnO powers prepared by sol-gel method were studied. X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM) of the sample do not show ...The magnetic and structural properties of 2% Ni-doped ZnO powers prepared by sol-gel method were studied. X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM) of the sample do not show existence of any signal of second phase. The X-photoelectron spectroscopy (XPS) of the sample shows the chemical valence of Ni is +2 and the real Ni concentration is 2.19% determined by X-ray fluorescence spectra (XRFS). The magnetic property performed with superconducting quantum interference device (SQUID) shows that the sample exhibits ferromagnetism above room temperature and the Curie temperature (TC) is about 600 K.展开更多
Ni-doped ZnO nanopowder (Zn0.98Ni0.2O) was synthesized by improved coprecipitation method. The average particle size of the powder was estimated to be 50 nm. The powder was then processed by thermal treatment. Sampl...Ni-doped ZnO nanopowder (Zn0.98Ni0.2O) was synthesized by improved coprecipitation method. The average particle size of the powder was estimated to be 50 nm. The powder was then processed by thermal treatment. Samples were annealed at 1 073, 1 273, and 1 473 K, respectively. The solubility of NiO in ZnO and the lattice parameters of ZnO both increased with the temperature. The magnetic property of the doped samples was examined, and hysteresis loops were got. The results showed all the samples were ferromagnetic, while powder processed at 1 273 K for 4 h got a highest saturation magnetization (Ms) of 0.0457 emu/g. Also, magnetic properties were related to the grain size of the powder.展开更多
The selective cleavage of C-O and C-C is facing a challenge in the field of catalysis.In the present work,we studied the influence of doped Ni on the structure and electronic properties,as well as the selective C-O/C-...The selective cleavage of C-O and C-C is facing a challenge in the field of catalysis.In the present work,we studied the influence of doped Ni on the structure and electronic properties,as well as the selective C-O/C-C bond cleavages in the hydrodeoxygenation of palmitic acid over Ni-Mo_(2)C catalyst.The catalytic activity on Ni doped Mo_(2)C with TOF of 6.9×10^(3)h^(-1)is much superior to intrinsic Mo_(2)C catalyst,which is also higher than most noble metal catalysts.Structurally,the doped Ni raises the active particle dispersion and the coordination numbers of Mo species(Mo-C and Mo-O),improves the graphitization degree to promote the electron transfer,and increases the amount of Lewis and Br?nsted acid,which are responsible for the excellent hydrodeoxygenation performance.The Ni promotes simultaneously C-O and C-C bonds cleavage to produce pentadecane and hexadecane owing to the increase of electron-rich Mo sites after Ni doping.These findings contribute to the understanding of the nature of Ni-doped Mo_(2)C on the roles as catalytic active sites for C-O and C-C bonds cleavage.展开更多
Element doping has been proved to be a useful method to correct for the mass bias fractionation when analyzing iron isotope compositions.We present a systematic re-assessment on how the doped nickel may affect the iro...Element doping has been proved to be a useful method to correct for the mass bias fractionation when analyzing iron isotope compositions.We present a systematic re-assessment on how the doped nickel may affect the iron isotope analysis in this study by carrying out several experiments.We find three important factors that can affect the analytical results,including the Ni:Fe ratio in the analyte solutions,the match of the Ni:Fe ratio between the unknown sample and standard solutions,and the match of the Fe concentration between the sample and standard solutions.Thus,caution is required when adding Ni to the analyte Fe solutions before analysis.Using our method,theδ56Fe and δ57Fe values of the USGS standards W-2 a,BHVO-2,BCR-2,AGV-2 and GSP-2 are consistent with the recommended literature values,and the long-term(one year) external reproducibility is better than 0.03 and 0.05‰(2 SD) for δ56Fe and δ57Fe,respectively.Therefore,the analytical method established in our laboratory is a method of choice for high quantity Fe isotope data in geological materials.展开更多
The technical bottleneck of carbon materials as counter electrodes(CEs)lies in their limited electrical conduc-tivity,extended ion diffusion paths,poor dispersion,and high contact resistance.Problem-oriented in-situ s...The technical bottleneck of carbon materials as counter electrodes(CEs)lies in their limited electrical conduc-tivity,extended ion diffusion paths,poor dispersion,and high contact resistance.Problem-oriented in-situ self-grown N-doped CNTs-coated Ni nanoparticles based on N-doped carbonaceous structures derived from pitaya peel(PC)are adopted to construct Ni-N-C hybrid 3D ionized network sites(Ni@NCNTs/PC-4)as CEs.Structural characterization,micromorphological and chemical composition analyses revealed the 3D network structure of Ni@NCNTs/PC-4 with abundant active sites.They effectively shorten the diffusion distance of I 3−ions with a smaller charge transfer resistance(5.21Ω)than that of PC(12.53Ω).DSSCs based on Ni@NCNTs/PC-4 display good optoelectronic properties,in which the short-circuit current density(Jsc)is 13.27 mA/cm^(2),higher than those of Pt(11.66 mA/cm^(2))and PC(6.99 mA/cm^(2)).The PCE value(5.13%)of DSSCs based on Ni@NCNTs/PC-4 is also higher than that of DSSCs based on PC(2.47%).Overall,this work provides a preliminary research and new ideas for further in-depth study of biomass-derived 3D structured-carbons that contribute to key electrodes in DSSCs.展开更多
Regulating the selectivity of CO2 photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the se...Regulating the selectivity of CO2 photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the selectivity of CO2 photoreduction. Prototypical ZnCo2O4 atomic layers with/without Ni-doping were first synthesized. Density functional theory calculations reveal that introducing Ni atoms creates several new energy levels and increases the density-of-states at the conduction band minimum. Synchrotron radiation photoemission spectroscopy demonstrates that the band structures are suitable for CO2 photoreduction, while the surface photovoltage spectra demonstrate that Ni doping increases the carrier separation efficiency. In situ diffuse reflectance Fourier transform infrared spectra disclose that the CO2^- radical is the main intermediate, while temperature-programed desorption curves reveal that the ZnCo2O4 atomic layers with/without Ni doping favor the respective CO and CH4 desorption. The Ni-doped ZnCo2O4 atomic layers exhibit a 3.5-time higher CO selectivity than the ZnCo2O4 atomic layers. This work establishes a clear correlation between elemental doping and selectivity regulation for CO2 photoreduction, opening new possibilities for tailoring solar-driven photocatalytic behaviors.展开更多
Ni-doped BiFeO_(3) powders with the composition BiFe_(1-x)Ni_(x)O_(3)(x=0.05,0.1 and 0.15)were prepared by a self-propagating high-temperature synthesis(SHS),using metal nitrates as oxidizers and glycine as fuel.The X...Ni-doped BiFeO_(3) powders with the composition BiFe_(1-x)Ni_(x)O_(3)(x=0.05,0.1 and 0.15)were prepared by a self-propagating high-temperature synthesis(SHS),using metal nitrates as oxidizers and glycine as fuel.The X-ray diffraction(XRD)patterns depict that Ni-doped BiFeO_(3) ceramics crystallize in a rhombhohedral phase.The scanning electron micrographs of Ni-doped BiFeO_(3) ceramics show a dense morphology with interconnected structure.It is found that,the room-temperature magnetization measurements in Ni-incorporated BiFeO_(3) ceramics give rise to nonzero magnetization.The magnetization of Ni-doped BiFeO_(3) ceramics is significantly enhanced when Ni doping concentration reaches to x=0.1 at 5 K.The variations of dielectric constant with temperature in BiFe_(0.95)Ni_(0.05)O_(3),BiFe_(0.9)Ni_(0.1)O_(3) and BiFe_(0.85)Ni_(0.15)O_(3) samples exhibit clear dielectric anomalies approximately around 450℃,425℃and 410℃respectively,which correspond to antiferromagnetic to paramagnetic phase transition of the parent compound BiFeO_(3).展开更多
Nickel-CeO_(2)-based materials are commonly used for the thermal catalytic hydrogenation of CO_(2).However,high Ni loadings and low CO selectivity restrict their use in the reverse water–gas shift(RWGS)reaction.Herei...Nickel-CeO_(2)-based materials are commonly used for the thermal catalytic hydrogenation of CO_(2).However,high Ni loadings and low CO selectivity restrict their use in the reverse water–gas shift(RWGS)reaction.Herein,we demonstrate a highly active,robust,and low-Ni-doped(1.1 wt.%)CeO_(2) catalyst(1.0-Ni-CeO_(2)).The Ni-based-mass-specific CO formation rate reaches up to 1,542 mmol·gNi^(−1)·h^(−1) with 100%CO selectivity at 300°C for 100 h,among the best values reported in the literature.Density functional theory(DFT)and diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that the enhanced catalytic activity is attributed to the abundant Ce–H species,while the high selectivity results from low CO affinity.More importantly,a new reaction mechanism is proposed,which involves the reduction of bicarbonate to generate formate intermediate and CO by the H−released from Ce–H species.The new findings in this work will benefit the design of economic,efficient,and robust catalysts for low-temperature RWGS reactions.展开更多
Li-rich cathode materials have been considered as promising candidates for high-energy lithium ion batteries (LIBs). In this study, we report a new series of Li-rich materials (Li[Li1/B-2x/BMn2/3-x/3Nix]O2 (0.09 ...Li-rich cathode materials have been considered as promising candidates for high-energy lithium ion batteries (LIBs). In this study, we report a new series of Li-rich materials (Li[Li1/B-2x/BMn2/3-x/3Nix]O2 (0.09 ≤x≤ 0.2)) doped with small amounts of Ni as cathode materials in LIBs, which exhibited unusual phenomenon of capacity increase up to tens of cycles due to the continuous activation of the Li2MnO3 phase. Both experimental and computational results indicate that unlike commonly studied Ni-doped Li-rich cathode materials, smaller amounts of Ni doping can promote the stepwise Li2MnO3 activation to obtain increased specific capacity and better cycling capability. In contrast, excessive Ni will over-activate the Li2MnO3 and result in a large capacity loss in the first cycle. The Lil.25Mn0.625Ni0.12sO2 material with an optimized content of Ni delivered a superior high capacity of -280 mAh.g-1 and good cycling stability at room temperature.展开更多
Metal sulfides have been regarded as promising anodes for potassium-ion batteries(PIBs)due to their high theoretical capacities,while the performance is limited by their intrinsic poor conductivity and large volume fl...Metal sulfides have been regarded as promising anodes for potassium-ion batteries(PIBs)due to their high theoretical capacities,while the performance is limited by their intrinsic poor conductivity and large volume fluctuation during the insertion/extraction of large potassium ion.Herein,the battery performance of iron sulfide anode is significantly enhanced through yolk-shell(Y-S)structure design and nickel doping,aiming to realize good structure stability and superior electron/ion transportation.For potassium storage,as-prepared Y-S Ni-FeS_(2)@C shows excellent cyclic performance and sustains high capacities of 328 mA h g^(-1)after 100 cycles at 0.2 A g^(-1)and 226 mA h g^(-1)after 1000 cycles at 1 A g^(-1).Especially,it displays a superior rate capacity of 200 mA h g^(-1)at 20 A g^(-1),higher than that of Y-S FeS_(2)@C and most as-reported metal sulfide anodes for PIBs.The experimental analysis and theoretical calculation illuminate the effect of Ni-doping on decreasing the particle size of iron sulfide and enhancing the ion/electron transport ability,thus accounting for the exceptional rate capability of Y-S Ni-FeS_(2)@C composite.展开更多
Developing robust and efficient non-noble electrocatalysts for the hydrogen evolution reaction(HER)is paramount for sustainably producing hydrogen fuel from electrochemical water splitting.Engineering morphology and c...Developing robust and efficient non-noble electrocatalysts for the hydrogen evolution reaction(HER)is paramount for sustainably producing hydrogen fuel from electrochemical water splitting.Engineering morphology and chemical composition are significant for fabricating electrocatalysts with superior activity and durability.Herein,novel Ni-doped CoSe_(2)composites are prepared by a facile one-step hydrothermal method.The optimized 1T-phase Co_(0.75)Ni_(0.25)Se_(2)shows excellent HER performance,exhibiting overpotential of as low as 172 mV at 10 mA·cm^(–2) and a small Tafel slope of 32.4 mV·dec^(–1) in 0.5 mol·L^(-1) H_(2)SO_(4)solution,approaching that of com-mercial Pt/C electrocatalyst(30.7 mV·dec^(–1)).Furthermore,the electrocatalyst possesses superior long-term stability under acidic condition.Physicochemical measurements indicate that the homogeneous nanoparticles morphology,the unique electronic structure,and the 1T-phase are responsible for its superior HER performance.This work comes up with a promising strategy in synthesizing other earth-abundant and low-cost catalysts for industrial applications.展开更多
文摘Over the last two decades,extensive study has been done on two-dimensional Molybdenum Sulphide(MoS_(2))due to its outstanding features in energy storage applications.Although MoS_(2)has a lot of active sulphur edges,the presence of inactive surfaces leads to limit conductivity and efficiency.Hence,in this article,we aimed to promote the additional active sites by doping various weight percentages(2%,4%,6%,8%and 10%)of Nickel(Ni)into the MoS_(2)matrix by simple hydrothermal technique,and their doping effects were investigated with the help of Physio-chemical analyses.X-ray diffraction(XRD)pattern,Raman,and chemical composition(XPS)analyses were used to confirm the Ni incorporation in MoS_(2)nanosheets.Microscopic investigations demonstrated that Ni-doped MoS_(2)nanosheets were vertically aligned with enhanced interlayer spacing.Cyclic voltammetry,Galvanostatic charge-discharge,and electrochemical impedance spectroscopy investigations were used to characterize the electrochemical characteristics.The 6%Ni-doped MoS_(2)electrode material showed better CSPof 528.7 F/g@1 A/g and excellent electrochemical stability(85%of capacitance retention after 10,000 cycles at 5 A/g)compared to other electrode materials.Furthermore,the solid-state asymmetric supercapacitor was assembled using Nidoped MoS_(2)and graphite as anode and cathode materials and analysed the electrochemical properties in the two-electrode system.To determine the impact of the Ni-atom on the MoS_(2)surface,firstprinciples computations were performed.Further,it was examined for electronic band structure,the projected density of states(PDOS)and Bader charge transfer analyses.
基金This work was financially supported by Korea Research Foundation of the Korea Government(MOEHRD)(KRF-2005-210-C00024).
文摘Magnetic properties of diluted magnetic semiconductors (DMSs), Ni-doped ZnO materials, prepared by sol-gel method were investigated by measuring magnetization as functions of magnetic field. The Ni content affects the magnetic properties at low sintered temperature but it has few effects on the magnetic properties at high sintered temperature. The sintered temperature has great effects on the magnetic properties of Ni/ZnO at high original mole ratio of Ni/Zn while it has slight effects on the magnetic properties of Ni/ZnO at low original mole ratio of Ni/Zn whatever low or high sintered temperature.
基金supported by the National Natural Science Foundation of China (52073166)the China Scholarship Council (CSC) for the Research Training Program of Guojuan Hai to study at University of Wollongong(201908610223)+5 种基金the Xi’an Key Laboratory of Green Manufacture of Ceramic Materials Foundation (2019220214SYS017CG039)the Key Program for International S&T Cooperation Projects of Shaanxi Province(2020KW-038, 2020GHJD-04)the Science and Technology Program of Xi’an,China (2020KJRC0009)the Scientific Research Program Funded by Shaanxi Provincial Education Department(No. 20JY001)Science and Technology Resource Sharing Platform of Shaanxi Province (2020PT-022)Science and Technology Plan of Weiyang District,Xi’an (202009)。
文摘The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst.Herein,the urchin-like Ni-doped W_(18)O_(49)/NF with enriched active sites was prepared by solvothermal method followed by a low-temperature pyrolysis treatment was reported.Results demonstrate that the incorporation of Ni-doping triggers the lattice distortion of W_(18)O_(49) for the increasement of oxygen defects.Further,high-valent W^(6+)are partially reduced to low-valent W^(4+),wherein the electrons originate from the oxidation process of Ni^(2+)to Ni^(3+).The Ni^(3+)ions show an enhanced orbital overlap with the OER reaction intermediates.The generated W^(4+)ions contribute to release oxygen vacancies,eventually reorganizing Ni-doped W_(18)O_(49)/NF to unique electrochemical active species with a special amorphous-crystalline interface(AM/NiWO_x/NiOOH/NF).Simultaneously,the reconstruction results in an optimized valence band and conduction band.Eventually,the resultant AM/NiWO_x/NiOOH/NF with abundant active sites and improved oxidation/reduction capability exhibits more superior catalytic performance compared with the Ni-doped W_(18)O_(49)/NF counterpart.This study gives more insights in the electrochemical evolution of the tungsten-based oxide and provides effective strategies for optimizing the catalytic activity of materials with inherent hydrogen evolution reaction limitations.
基金Project supported by the Special Fund for Major State Basic Research Project (G2000068305), the Hi-Tech Research Project (2004AA31G050), and the National Natural Science Foundation of China (60390072)
文摘The magnetic and structural properties of 2% Ni-doped ZnO powers prepared by sol-gel method were studied. X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM) of the sample do not show existence of any signal of second phase. The X-photoelectron spectroscopy (XPS) of the sample shows the chemical valence of Ni is +2 and the real Ni concentration is 2.19% determined by X-ray fluorescence spectra (XRFS). The magnetic property performed with superconducting quantum interference device (SQUID) shows that the sample exhibits ferromagnetism above room temperature and the Curie temperature (TC) is about 600 K.
文摘Ni-doped ZnO nanopowder (Zn0.98Ni0.2O) was synthesized by improved coprecipitation method. The average particle size of the powder was estimated to be 50 nm. The powder was then processed by thermal treatment. Samples were annealed at 1 073, 1 273, and 1 473 K, respectively. The solubility of NiO in ZnO and the lattice parameters of ZnO both increased with the temperature. The magnetic property of the doped samples was examined, and hysteresis loops were got. The results showed all the samples were ferromagnetic, while powder processed at 1 273 K for 4 h got a highest saturation magnetization (Ms) of 0.0457 emu/g. Also, magnetic properties were related to the grain size of the powder.
基金financially supported by the National Natural Science Foundation of China(21972099)the Application Foundation Program of Sichuan Province(2021YJ0305)+1 种基金the 111 project(B17030).Shanghai Synchrotron Radiation Facility(SSRF)for XAS experiments and the support by the project from NPL of CAEP(2019BB08)。
文摘The selective cleavage of C-O and C-C is facing a challenge in the field of catalysis.In the present work,we studied the influence of doped Ni on the structure and electronic properties,as well as the selective C-O/C-C bond cleavages in the hydrodeoxygenation of palmitic acid over Ni-Mo_(2)C catalyst.The catalytic activity on Ni doped Mo_(2)C with TOF of 6.9×10^(3)h^(-1)is much superior to intrinsic Mo_(2)C catalyst,which is also higher than most noble metal catalysts.Structurally,the doped Ni raises the active particle dispersion and the coordination numbers of Mo species(Mo-C and Mo-O),improves the graphitization degree to promote the electron transfer,and increases the amount of Lewis and Br?nsted acid,which are responsible for the excellent hydrodeoxygenation performance.The Ni promotes simultaneously C-O and C-C bonds cleavage to produce pentadecane and hexadecane owing to the increase of electron-rich Mo sites after Ni doping.These findings contribute to the understanding of the nature of Ni-doped Mo_(2)C on the roles as catalytic active sites for C-O and C-C bonds cleavage.
基金This work was supported by National Nature Science Foundation of China(Grant Numbers 41776067 and 41630968).
文摘Element doping has been proved to be a useful method to correct for the mass bias fractionation when analyzing iron isotope compositions.We present a systematic re-assessment on how the doped nickel may affect the iron isotope analysis in this study by carrying out several experiments.We find three important factors that can affect the analytical results,including the Ni:Fe ratio in the analyte solutions,the match of the Ni:Fe ratio between the unknown sample and standard solutions,and the match of the Fe concentration between the sample and standard solutions.Thus,caution is required when adding Ni to the analyte Fe solutions before analysis.Using our method,theδ56Fe and δ57Fe values of the USGS standards W-2 a,BHVO-2,BCR-2,AGV-2 and GSP-2 are consistent with the recommended literature values,and the long-term(one year) external reproducibility is better than 0.03 and 0.05‰(2 SD) for δ56Fe and δ57Fe,respectively.Therefore,the analytical method established in our laboratory is a method of choice for high quantity Fe isotope data in geological materials.
基金supported by the National Natural Science Foundation of China(31960293).
文摘The technical bottleneck of carbon materials as counter electrodes(CEs)lies in their limited electrical conduc-tivity,extended ion diffusion paths,poor dispersion,and high contact resistance.Problem-oriented in-situ self-grown N-doped CNTs-coated Ni nanoparticles based on N-doped carbonaceous structures derived from pitaya peel(PC)are adopted to construct Ni-N-C hybrid 3D ionized network sites(Ni@NCNTs/PC-4)as CEs.Structural characterization,micromorphological and chemical composition analyses revealed the 3D network structure of Ni@NCNTs/PC-4 with abundant active sites.They effectively shorten the diffusion distance of I 3−ions with a smaller charge transfer resistance(5.21Ω)than that of PC(12.53Ω).DSSCs based on Ni@NCNTs/PC-4 display good optoelectronic properties,in which the short-circuit current density(Jsc)is 13.27 mA/cm^(2),higher than those of Pt(11.66 mA/cm^(2))and PC(6.99 mA/cm^(2)).The PCE value(5.13%)of DSSCs based on Ni@NCNTs/PC-4 is also higher than that of DSSCs based on PC(2.47%).Overall,this work provides a preliminary research and new ideas for further in-depth study of biomass-derived 3D structured-carbons that contribute to key electrodes in DSSCs.
文摘Regulating the selectivity of CO2 photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the selectivity of CO2 photoreduction. Prototypical ZnCo2O4 atomic layers with/without Ni-doping were first synthesized. Density functional theory calculations reveal that introducing Ni atoms creates several new energy levels and increases the density-of-states at the conduction band minimum. Synchrotron radiation photoemission spectroscopy demonstrates that the band structures are suitable for CO2 photoreduction, while the surface photovoltage spectra demonstrate that Ni doping increases the carrier separation efficiency. In situ diffuse reflectance Fourier transform infrared spectra disclose that the CO2^- radical is the main intermediate, while temperature-programed desorption curves reveal that the ZnCo2O4 atomic layers with/without Ni doping favor the respective CO and CH4 desorption. The Ni-doped ZnCo2O4 atomic layers exhibit a 3.5-time higher CO selectivity than the ZnCo2O4 atomic layers. This work establishes a clear correlation between elemental doping and selectivity regulation for CO2 photoreduction, opening new possibilities for tailoring solar-driven photocatalytic behaviors.
基金This study was supported by UGC-SAP,DRS Phase II of Indiathe author Y.A.Chaudhari is very much thankful for the funding agency.
文摘Ni-doped BiFeO_(3) powders with the composition BiFe_(1-x)Ni_(x)O_(3)(x=0.05,0.1 and 0.15)were prepared by a self-propagating high-temperature synthesis(SHS),using metal nitrates as oxidizers and glycine as fuel.The X-ray diffraction(XRD)patterns depict that Ni-doped BiFeO_(3) ceramics crystallize in a rhombhohedral phase.The scanning electron micrographs of Ni-doped BiFeO_(3) ceramics show a dense morphology with interconnected structure.It is found that,the room-temperature magnetization measurements in Ni-incorporated BiFeO_(3) ceramics give rise to nonzero magnetization.The magnetization of Ni-doped BiFeO_(3) ceramics is significantly enhanced when Ni doping concentration reaches to x=0.1 at 5 K.The variations of dielectric constant with temperature in BiFe_(0.95)Ni_(0.05)O_(3),BiFe_(0.9)Ni_(0.1)O_(3) and BiFe_(0.85)Ni_(0.15)O_(3) samples exhibit clear dielectric anomalies approximately around 450℃,425℃and 410℃respectively,which correspond to antiferromagnetic to paramagnetic phase transition of the parent compound BiFeO_(3).
基金the Science and Technology Project of Shenzhen(No.JCYJ20190806155814624)the National Natural Science Foundation of China(No.22002120)the Fundamental Research Funds for the Central Universities(No.3102017jc01001).
文摘Nickel-CeO_(2)-based materials are commonly used for the thermal catalytic hydrogenation of CO_(2).However,high Ni loadings and low CO selectivity restrict their use in the reverse water–gas shift(RWGS)reaction.Herein,we demonstrate a highly active,robust,and low-Ni-doped(1.1 wt.%)CeO_(2) catalyst(1.0-Ni-CeO_(2)).The Ni-based-mass-specific CO formation rate reaches up to 1,542 mmol·gNi^(−1)·h^(−1) with 100%CO selectivity at 300°C for 100 h,among the best values reported in the literature.Density functional theory(DFT)and diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)results reveal that the enhanced catalytic activity is attributed to the abundant Ce–H species,while the high selectivity results from low CO affinity.More importantly,a new reaction mechanism is proposed,which involves the reduction of bicarbonate to generate formate intermediate and CO by the H−released from Ce–H species.The new findings in this work will benefit the design of economic,efficient,and robust catalysts for low-temperature RWGS reactions.
文摘Li-rich cathode materials have been considered as promising candidates for high-energy lithium ion batteries (LIBs). In this study, we report a new series of Li-rich materials (Li[Li1/B-2x/BMn2/3-x/3Nix]O2 (0.09 ≤x≤ 0.2)) doped with small amounts of Ni as cathode materials in LIBs, which exhibited unusual phenomenon of capacity increase up to tens of cycles due to the continuous activation of the Li2MnO3 phase. Both experimental and computational results indicate that unlike commonly studied Ni-doped Li-rich cathode materials, smaller amounts of Ni doping can promote the stepwise Li2MnO3 activation to obtain increased specific capacity and better cycling capability. In contrast, excessive Ni will over-activate the Li2MnO3 and result in a large capacity loss in the first cycle. The Lil.25Mn0.625Ni0.12sO2 material with an optimized content of Ni delivered a superior high capacity of -280 mAh.g-1 and good cycling stability at room temperature.
基金supported by the Science and Technology Planning Project of Fujian Province(2021J01151)CAS Key Laboratory of Design and Assembly of Functional Nanostructures(2013DP173231)+1 种基金the Award Program for Fujian Minjiang Scholar Professorship(2021)the Start-up Funding from FJNU。
文摘Metal sulfides have been regarded as promising anodes for potassium-ion batteries(PIBs)due to their high theoretical capacities,while the performance is limited by their intrinsic poor conductivity and large volume fluctuation during the insertion/extraction of large potassium ion.Herein,the battery performance of iron sulfide anode is significantly enhanced through yolk-shell(Y-S)structure design and nickel doping,aiming to realize good structure stability and superior electron/ion transportation.For potassium storage,as-prepared Y-S Ni-FeS_(2)@C shows excellent cyclic performance and sustains high capacities of 328 mA h g^(-1)after 100 cycles at 0.2 A g^(-1)and 226 mA h g^(-1)after 1000 cycles at 1 A g^(-1).Especially,it displays a superior rate capacity of 200 mA h g^(-1)at 20 A g^(-1),higher than that of Y-S FeS_(2)@C and most as-reported metal sulfide anodes for PIBs.The experimental analysis and theoretical calculation illuminate the effect of Ni-doping on decreasing the particle size of iron sulfide and enhancing the ion/electron transport ability,thus accounting for the exceptional rate capability of Y-S Ni-FeS_(2)@C composite.
基金financially supported by the National Natural Science Foundation of China (Nos. 52002254 and 51773049)the National Program for Support of Top-notch Young Professionals, China Aerospace Science and Technology Corporation-Harbin Institute of Technology Joint Center for Technology Innovation Fund (No. HIT15-1A01)+4 种基金Shanghai Academy of Spaceflight Technology Fund (No. SAST2017-126)the Scientific and Technological Cooperation and Development Fund (No. 2017KJHZ002)Sichuan Science and Technology Program (No. 2020YJ0262)Chunhui Plan of Ministry of Education of China, Fundamental Research Funds for the Central Universities, China (No. YJ201893)State Key Laboratory of Advanced Metals and Materials, China (No. 2019-Z03)。
文摘Developing robust and efficient non-noble electrocatalysts for the hydrogen evolution reaction(HER)is paramount for sustainably producing hydrogen fuel from electrochemical water splitting.Engineering morphology and chemical composition are significant for fabricating electrocatalysts with superior activity and durability.Herein,novel Ni-doped CoSe_(2)composites are prepared by a facile one-step hydrothermal method.The optimized 1T-phase Co_(0.75)Ni_(0.25)Se_(2)shows excellent HER performance,exhibiting overpotential of as low as 172 mV at 10 mA·cm^(–2) and a small Tafel slope of 32.4 mV·dec^(–1) in 0.5 mol·L^(-1) H_(2)SO_(4)solution,approaching that of com-mercial Pt/C electrocatalyst(30.7 mV·dec^(–1)).Furthermore,the electrocatalyst possesses superior long-term stability under acidic condition.Physicochemical measurements indicate that the homogeneous nanoparticles morphology,the unique electronic structure,and the 1T-phase are responsible for its superior HER performance.This work comes up with a promising strategy in synthesizing other earth-abundant and low-cost catalysts for industrial applications.