We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni ...We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni Fe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped Ni Fe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 m V at the current density of 10 m A cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped Ni Fe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.展开更多
The binding energy spectra and electron momentum distributions for the complete valence orbitals of ethanethiol were measured for the first time by binary （e, 2e） electron momentum spectroscopy employing non-coplana...The binding energy spectra and electron momentum distributions for the complete valence orbitals of ethanethiol were measured for the first time by binary （e, 2e） electron momentum spectroscopy employing non-coplanar symmetric kinematics at an impact energy of 1200 eV plus binding energy. The experimental results are generally consistent with the theoretical calculations using density functional theory and Hartree-Fock methods with various basis sets. A possible satellite line at 17.8 eV in binding energy spectrum was observed and studied by electron momentum spectroscopy.展开更多
The bioavailability of five divalent cationic heavy metals （Pb, Cd, Cu, Zn and Ni） in 10 superficial sediment samples from Baihua Lake was assessed based on the molar ratio of simultaneously extracted metals （SEMs...The bioavailability of five divalent cationic heavy metals （Pb, Cd, Cu, Zn and Ni） in 10 superficial sediment samples from Baihua Lake was assessed based on the molar ratio of simultaneously extracted metals （SEMs） to acid volatile sulfide （AVS）. Atomic absorption spectrometry （AAS） and X-ray powder diffraction （XRD） were used to determine the heavy metal concentrations and examine the mineralogy of the crystalline phases, respectively. The AVS loadings in sediments from Baihua Lake ranged from 64.30 to 350.08 ~rnol/g （dry weight）. The corresponding SEM levels for the sampling sites varied from 1.770 to 14.660 vrnol/g. The molar ratio of SEMs to AVS ranged from 0.014 to 0.084 with a mean value of 0.034. The XRD analysis also confirmed the presence of some metal sulfides in sediments from Baihua Lake. The SEMs/AVS ratios for all sampling sites were significantly lower than 1.0, indicating that AVS in the sediments was sufficient to bind the five heavy metals; thus, these heavy metals are currently not significantly bioavailable to benthic organisms. Comparing the SEMs results to published guideline values for metal toxicity to benthic organisms in sediments, however, suggests that Zn and Ni pose a risk at some sampling locations in Baihua Lake.展开更多
Shuttle effect is one of the most serious disadvantages in lithium-sulfur battery which results in poor cycle performance and hinders the commercialization of Li-S battery.To reduce the dissolution of polysulfides int...Shuttle effect is one of the most serious disadvantages in lithium-sulfur battery which results in poor cycle performance and hinders the commercialization of Li-S battery.To reduce the dissolution of polysulfides into the electrolyte and prolong the cycling stability,nanoparticle-stacked metal nitride derived from layered double hydroxides(LDHs)as an interlayer was inserted between sulfur cathode and separator to confine polysulfides by physical and chemical interactions.Meanwhile,the surface of metal nitride will form an oxide passivation layer.The passivation layer possesses hydrophilic metal-O group and provides a polar surface for strong binding with polysulfide.What’s more,the nanoparticlesstacked structure could immerge and retain electrolyte well,which could enhance the ability of promoting the electron exchange rate.The sulfur electrode with nanoparticle-stacked metal nitride interlayer has an excellent cycle performance owing to the interactions between metal nitride and polysulfides.The battery delivered an initial capacity of 764.6 m Ahg^(-1) and still possesses a capacity of 477.5 mAhg^(-1) with the retention of 62.4% after 800 cycles.展开更多
The microscopic process of oxidative etching of two-dimensional molybdenum disulfide(2D MoS_2) at an atomic scale is investigated using a correlative transmission electron microscope(TEM)-etching study.MoS_2 flakes on...The microscopic process of oxidative etching of two-dimensional molybdenum disulfide(2D MoS_2) at an atomic scale is investigated using a correlative transmission electron microscope(TEM)-etching study.MoS_2 flakes on graphene TEM grids are precisely tracked and characterized by TEM before and after the oxidative etching. This allows us to determine the structural change with an atomic resolution on the edges of the domains, of well-oriented triangular pits and along the grain boundaries. We observe that the etching mostly starts from the open edges, grain boundaries and pre-existing atomic defects.A zigzag Mo edge is assigned as the dominant termination of the triangular pits, and profound terraces and grooves are observed on the etched edges. Based on the statistical TEM analysis, we reveal possible routes for the kinetics of the oxidative etching in 2D MoS_2, which should also be applicable for other 2D transition metal dichalcogenide materials like MoSe_2 and WS_2.展开更多
Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin di...Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin disulfide(SnS_(2))nanoparticles are embedded between interlayers of twodimensional porous carbon nanosheets(PCNs),forming a multi-functional nanocomposite(PCN-SnS_(2))as a cathode carrier for Li-S batteries.The graphitized carbon nanosheets improve the overall conductivity of the electrode,and the abundant pores not only facilitate ion transfer and electrolyte permeation,but also buffer the volume change during the charge and discharge process to ensure the integrity of the electrode material.More importantly,the physical confinement of PCN,as well as the strong chemical adsorption and catalytic reaction of small SnS_(2)nanoparticles,synergistically reduce the shuttle effect of polysulfides.The interaction between a porous layered structure and physical-chemical confinement gives the PCN-SnS_(2)-S electrode high electrochemical performance.Even at a high rate of 2 C,a discharge capacity of 650 mA h g^(-1)is maintained after 150 cycles,underscoring the positive results of SnS_(2)-based materials for Li-S batteries.The galvanostatic intermittent titration technique results further confirm that the PCN-SnS_(2)-S electrode has a high Li+transmission rate,which reduces the activation barrier and improves the electrochemical reaction kinetics.This work provides strong evidence that reducing the size of SnS_(2)nanostructures is beneficial for capturing and reacting with polysulfides to alleviate their shuttle effect in Li-S batteries.展开更多
文摘We report a facile way to prepare sulfur(S) doped Ni4/5 Fe1/5-layered double hydroxide(LDH) electrocatalysts for oxygen evolution reaction(OER). The influence of S doping amount on the OER activity of the resulted Ni Fe-LDHs was studied and the optimal surface S content was ca. 0.43 at%. The developed S-doped Ni Fe-LDH exhibits excellent OER catalyst activity in 1.0 M KOH with overpotential of only 257 m V at the current density of 10 m A cm^-2. Moreover, the catalyst could maintain high activity after 30 h stability test. The high activity of the S-doped Ni Fe-LDH catalysts may originate from the synergistic effect between S and the Fe sites. This work provides a simple but efficient way to improve the OER performance of transition metal oxides/(oxy)hydroxides.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.10734040） and the Foundation for Major Research Program of Education Department of Anhui Province （No.ZD2007002-1）.
文摘The binding energy spectra and electron momentum distributions for the complete valence orbitals of ethanethiol were measured for the first time by binary （e, 2e） electron momentum spectroscopy employing non-coplanar symmetric kinematics at an impact energy of 1200 eV plus binding energy. The experimental results are generally consistent with the theoretical calculations using density functional theory and Hartree-Fock methods with various basis sets. A possible satellite line at 17.8 eV in binding energy spectrum was observed and studied by electron momentum spectroscopy.
基金Supported by the National Natural Science Foundation of China(No.20967003)the Project of the Government of Guiyang City(No.[2010]5-2)
文摘The bioavailability of five divalent cationic heavy metals （Pb, Cd, Cu, Zn and Ni） in 10 superficial sediment samples from Baihua Lake was assessed based on the molar ratio of simultaneously extracted metals （SEMs） to acid volatile sulfide （AVS）. Atomic absorption spectrometry （AAS） and X-ray powder diffraction （XRD） were used to determine the heavy metal concentrations and examine the mineralogy of the crystalline phases, respectively. The AVS loadings in sediments from Baihua Lake ranged from 64.30 to 350.08 ~rnol/g （dry weight）. The corresponding SEM levels for the sampling sites varied from 1.770 to 14.660 vrnol/g. The molar ratio of SEMs to AVS ranged from 0.014 to 0.084 with a mean value of 0.034. The XRD analysis also confirmed the presence of some metal sulfides in sediments from Baihua Lake. The SEMs/AVS ratios for all sampling sites were significantly lower than 1.0, indicating that AVS in the sediments was sufficient to bind the five heavy metals; thus, these heavy metals are currently not significantly bioavailable to benthic organisms. Comparing the SEMs results to published guideline values for metal toxicity to benthic organisms in sediments, however, suggests that Zn and Ni pose a risk at some sampling locations in Baihua Lake.
基金supported by the National Natural Science Foundation of China(21701043,51402100,50702020,21573066 and 81171461)the Provincial Natural Science Foundation of Hunan(2016JJ1006,2016TP1009 and 11JJ4013)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province
文摘Shuttle effect is one of the most serious disadvantages in lithium-sulfur battery which results in poor cycle performance and hinders the commercialization of Li-S battery.To reduce the dissolution of polysulfides into the electrolyte and prolong the cycling stability,nanoparticle-stacked metal nitride derived from layered double hydroxides(LDHs)as an interlayer was inserted between sulfur cathode and separator to confine polysulfides by physical and chemical interactions.Meanwhile,the surface of metal nitride will form an oxide passivation layer.The passivation layer possesses hydrophilic metal-O group and provides a polar surface for strong binding with polysulfide.What’s more,the nanoparticlesstacked structure could immerge and retain electrolyte well,which could enhance the ability of promoting the electron exchange rate.The sulfur electrode with nanoparticle-stacked metal nitride interlayer has an excellent cycle performance owing to the interactions between metal nitride and polysulfides.The battery delivered an initial capacity of 764.6 m Ahg^(-1) and still possesses a capacity of 477.5 mAhg^(-1) with the retention of 62.4% after 800 cycles.
基金supported by the National Basic Research Program of China(2014CB932500,2015CB921004)the National Natural Science Foundation of China(51472215,51222202,61571197 and 61172011)the 111 project(B16042)
文摘The microscopic process of oxidative etching of two-dimensional molybdenum disulfide(2D MoS_2) at an atomic scale is investigated using a correlative transmission electron microscope(TEM)-etching study.MoS_2 flakes on graphene TEM grids are precisely tracked and characterized by TEM before and after the oxidative etching. This allows us to determine the structural change with an atomic resolution on the edges of the domains, of well-oriented triangular pits and along the grain boundaries. We observe that the etching mostly starts from the open edges, grain boundaries and pre-existing atomic defects.A zigzag Mo edge is assigned as the dominant termination of the triangular pits, and profound terraces and grooves are observed on the etched edges. Based on the statistical TEM analysis, we reveal possible routes for the kinetics of the oxidative etching in 2D MoS_2, which should also be applicable for other 2D transition metal dichalcogenide materials like MoSe_2 and WS_2.
基金the National Key R&D Program of China(2016YFA0202602)the National Natural Science Foundation of China(U1663225)+3 种基金the Fundamental Research Funds for the Central Universities(2020-YB-009)the Academy of Scientific Research and Technology(6611,ASRT,Egypt)the 111 National project(B20002)from the Ministry of Science and Technology and the Ministry of Education,ChinaSinopec Ministry of Science and Technology Basic Prospective Research Project(217027-5 and 218025-9)。
文摘Lithium-sulfur(Li-S)batteries have attracted significant attention for their high specific capacity,non-toxic and harmless advantages.However,the shuttle effect limits their development.In this work,small-sized tin disulfide(SnS_(2))nanoparticles are embedded between interlayers of twodimensional porous carbon nanosheets(PCNs),forming a multi-functional nanocomposite(PCN-SnS_(2))as a cathode carrier for Li-S batteries.The graphitized carbon nanosheets improve the overall conductivity of the electrode,and the abundant pores not only facilitate ion transfer and electrolyte permeation,but also buffer the volume change during the charge and discharge process to ensure the integrity of the electrode material.More importantly,the physical confinement of PCN,as well as the strong chemical adsorption and catalytic reaction of small SnS_(2)nanoparticles,synergistically reduce the shuttle effect of polysulfides.The interaction between a porous layered structure and physical-chemical confinement gives the PCN-SnS_(2)-S electrode high electrochemical performance.Even at a high rate of 2 C,a discharge capacity of 650 mA h g^(-1)is maintained after 150 cycles,underscoring the positive results of SnS_(2)-based materials for Li-S batteries.The galvanostatic intermittent titration technique results further confirm that the PCN-SnS_(2)-S electrode has a high Li+transmission rate,which reduces the activation barrier and improves the electrochemical reaction kinetics.This work provides strong evidence that reducing the size of SnS_(2)nanostructures is beneficial for capturing and reacting with polysulfides to alleviate their shuttle effect in Li-S batteries.
