Enrichment of As and Au at the overgrowth rims of arsenian pyrite is a distinctive feature of Carlin-type gold ores.Revealing distribution of such key elements in high resolution is of fundamental importance yet often...Enrichment of As and Au at the overgrowth rims of arsenian pyrite is a distinctive feature of Carlin-type gold ores.Revealing distribution of such key elements in high resolution is of fundamental importance yet often proves challenging.In this study,repeated non-oxidative acid etching of ore samples from Shuiyindong gold deposit was applied to enable elemental depth profiling of goldbearing arsenian pyrite grains.ICP-OES and AAS were used to determine the dissolved Fe,As,and Au concentrations in each of the etching solutions,and XPS was carried out to exam the etched mineral surfaces.In contrast to conventional ion beam etching that may cause substantial sample damage,our acid etching method does not seem to significantly alter the composition and chemical state of the samples.The etched depths directly converted from the measured elemental concentrations can reproducibly reach a very high resolution of~1 nm,and can be conveniently controlled through varying the etching time.While the Fe and As depth profiles consistently reflect the surface oxidation property of arsenian pyrite,the Au profile displaying an obvious upward trend reveals the ore fluid evolution at the late stage of mineralization.Based on our experimental results,we demonstrate that our wet chemistry method is capable of effective depth profiling of gold ore and perhaps other geological samples,with advantages surpassing many instrumental techniques including negligible sample damage,nanoscale resolution as well as isotropic etching.展开更多
Crystalline and nanostructured cobalt (CoFe2O4), nickel (NiFe2O4), zinc (ZnFe2O4) and manganese (MnFe2O4) spinel ferrites are synthesized with high yields, crystallinity and purity through an easy, quick, repr...Crystalline and nanostructured cobalt (CoFe2O4), nickel (NiFe2O4), zinc (ZnFe2O4) and manganese (MnFe2O4) spinel ferrites are synthesized with high yields, crystallinity and purity through an easy, quick, reproducible and low-temperature hydrothermal assisted route starting from an aqueous suspension of copredpitated metal oxalates. The use of water as a reaction medium is a further advantage of the chosen protocol. Additionally, the zinc spinel is also prepared through an alternative route combining copredpitation of oxalates from an aqueous solution with thermal decomposition under reflux conditions. The nanocrystalline powders are obtained as a pure crystalline phase already at the extremely low tem- perature of 75 ℃ and no further thermal treatment is needed. The structure and microstructure of the prepared materials is investigated by means of X-ray powder diffraction (XRPD), while X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma-atomic emission spectroscopy (ICP-AES) analyses are used to gain information about the surface and bulk composition of the samples, respectively, confirming the expected stoichiometry. To investigate the effect of the synthesis protocol on the morphology of the obtained ferrites, transmission electron microscopy (TEM) observations are performed on selected samples. The magnetic properties of the cobalt and manganese spinels are also investigated using a superconducting quantum device magnetometer (SQUID) revealing hard and soft ferrimagnetic behavior, respectively.展开更多
Rechargeable aqueous Zn-ion batteries(AZIBs)are one of the most promising energy storage devices for large-scale energy storage owing to their high specific capacity,eco-friendliness,low cost and high safety.Neverthel...Rechargeable aqueous Zn-ion batteries(AZIBs)are one of the most promising energy storage devices for large-scale energy storage owing to their high specific capacity,eco-friendliness,low cost and high safety.Nevertheless,zinc metal anodes suffer from severe dendrite growth and side reactions,resulting in the inferior electrochemical performance of AZIBs.To address these problems,surface modification of zinc metal anodes is a facile and effective method to regulate the interaction between the zinc anode and an electrolyte.In this review,the current challenges and strategies for zinc metal anodes are presented.Furthermore,recent advances in surface modification strategies to improve their electrochemical performance are concluded and discussed.Finally,challenges and prospects for future development of zinc metal anodes are proposed.We hope this review will be useful for designing and fabricating highperformance AZIBs and boosting their practical applications.展开更多
A versatile wet chemistry method is developed for filling of subnanometer sized metal particles in carbon nanotubes with a diameter smaller than 1.5 nm. As an example, we showed that a confined bi-component Pd-V catal...A versatile wet chemistry method is developed for filling of subnanometer sized metal particles in carbon nanotubes with a diameter smaller than 1.5 nm. As an example, we showed that a confined bi-component Pd-V catalyst exhibit a higher benzene hydroxylation activity compared with that within multi-walled carbon nanotubes.展开更多
Electrochemical CO_(2) reduction reaction(CO_(2)RR),powered by renewable energy,emerges as a promising approach against environmental issues and energy crisis by converting CO_(2) into val‐ue‐added chemicals.Single ...Electrochemical CO_(2) reduction reaction(CO_(2)RR),powered by renewable energy,emerges as a promising approach against environmental issues and energy crisis by converting CO_(2) into val‐ue‐added chemicals.Single atom catalysts(SACs)with isolated metal atoms dispersed on supports exhibit outstanding performance for CO_(2) electroreduction,because of their strong single at‐om‐support interactions,maximum metal utilization and excellent catalytic activity.However,SACs suffer from agglomeration of particles,low metal loading,and difficulty in large‐scale production.In addition,molecular catalysts as another single atom‐based catalyst,consisting of ligands molecules connected to metal ions,exhibited similar metal‐nitrogen(M‐N)active centers as that in met‐al‐nitrogen‐carbon(M‐N‐C)SACs,which were highly active to CO_(2) reduction due to their well‐defined active sites and tunability over the steric and electronic properties of the active sites.Nonetheless,molecular catalysts are challenged by generally moderate activity,selectivity and sta‐bility,poor conductivity and aggregation.Many works have been devoted to overcoming these is‐sues of SACs and molecular catalysts for efficient CO_(2)RR,but only limited reviews for systematic summary of their fabrication,application,and characterizations,which were highlighted in this review.Firstly,we summarize recent advanced strategies in preparing SACs for CO_(2)RR,including wet‐chemistry approaches(defect engineering,spatial confinement,and coordination design),other synthetic methods and large‐scale production of SACs.Besides,electrochemical applications of SACs and molecular catalysts on CO_(2)RR are discussed,which involved the faradaic efficiency and partial current density of the desired product as well as the catalyst stability.In addition,ex‐situ and in‐situ/operando characterization techniques are briefly assessed,benefiting probing the active sites and understanding the CO_(2)RR catalytic mechanisms.Finally,future directions for the devel‐opment of single atom‐based catalysts(SACs,molecular catalysts)are pointed out.展开更多
The Sr2 CeO4:Ln3+(Ln=Eu,Dy)fine phosphor particles were prepared by a facile wet chemical approach,in which the consecutive hydrothermal-combustion reaction was performed.The doping of Ln3+into Sr2 CeO4 has little inf...The Sr2 CeO4:Ln3+(Ln=Eu,Dy)fine phosphor particles were prepared by a facile wet chemical approach,in which the consecutive hydrothermal-combustion reaction was performed.The doping of Ln3+into Sr2 CeO4 has little influence on the structure of host,and the as-prepared samples display wellcrystallized spherical or elliptical shape with an average particle size at about 100-200 nm.For Eu3+ions-doped Sr2 CeO4,with the increase of Eu3+-doping concentration,the blue light emission band with the maximum at 468 nm originating from a Ce4+→O2-charge transfer of the host decreases obviously and the characteristic red light emission of Eu3+(5 D0→7 F2 transition at 618 nm)is enhanced gradually.Simultaneously,the fluorescent lifetime of the broadband emission of Sr2 CeO4 decreases with the doping of Eu3+,indicating an efficient energy transfer from the host to the doping Eu3+ions.The ene rgy transfer efficiency from the host to Eu3+was investigated in detail,and the emitting color of Sr2 CeO4:Eu3+can be easily tuned from blue to red by varying the doping concentration of Eu3+ions.Moreover,the luminescence of Dy3+-doped Sr2 CeO4 was also studied.Similar energy transfer pheno menon can be observed,and the incorporation of Dy3+into Sr2 CeO4 host leads to the characteristic emission of 4 F9/2→6 H15/2(488 nm,blue light)and 4 F9/2→6 H13/2(574 nm,yellow light)of Dy3+.The Sr2 CeO4:Ln3+fine particles with tunable luminescence are quite beneficial for its potential applications in the optoelectronic fields.展开更多
基金Financial supports from the B-type Strategic Priority Program of the Chinese Academy of Sciences(Grant No.XDB41000000)the National Natural Science Foundation of China(41872046,41902041 and 41173074)the Natural Science Research Project of Education Department of Guizhou Province(No.KY[2018]004)are sincerely acknowledged.
文摘Enrichment of As and Au at the overgrowth rims of arsenian pyrite is a distinctive feature of Carlin-type gold ores.Revealing distribution of such key elements in high resolution is of fundamental importance yet often proves challenging.In this study,repeated non-oxidative acid etching of ore samples from Shuiyindong gold deposit was applied to enable elemental depth profiling of goldbearing arsenian pyrite grains.ICP-OES and AAS were used to determine the dissolved Fe,As,and Au concentrations in each of the etching solutions,and XPS was carried out to exam the etched mineral surfaces.In contrast to conventional ion beam etching that may cause substantial sample damage,our acid etching method does not seem to significantly alter the composition and chemical state of the samples.The etched depths directly converted from the measured elemental concentrations can reproducibly reach a very high resolution of~1 nm,and can be conveniently controlled through varying the etching time.While the Fe and As depth profiles consistently reflect the surface oxidation property of arsenian pyrite,the Au profile displaying an obvious upward trend reveals the ore fluid evolution at the late stage of mineralization.Based on our experimental results,we demonstrate that our wet chemistry method is capable of effective depth profiling of gold ore and perhaps other geological samples,with advantages surpassing many instrumental techniques including negligible sample damage,nanoscale resolution as well as isotropic etching.
文摘Crystalline and nanostructured cobalt (CoFe2O4), nickel (NiFe2O4), zinc (ZnFe2O4) and manganese (MnFe2O4) spinel ferrites are synthesized with high yields, crystallinity and purity through an easy, quick, reproducible and low-temperature hydrothermal assisted route starting from an aqueous suspension of copredpitated metal oxalates. The use of water as a reaction medium is a further advantage of the chosen protocol. Additionally, the zinc spinel is also prepared through an alternative route combining copredpitation of oxalates from an aqueous solution with thermal decomposition under reflux conditions. The nanocrystalline powders are obtained as a pure crystalline phase already at the extremely low tem- perature of 75 ℃ and no further thermal treatment is needed. The structure and microstructure of the prepared materials is investigated by means of X-ray powder diffraction (XRPD), while X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma-atomic emission spectroscopy (ICP-AES) analyses are used to gain information about the surface and bulk composition of the samples, respectively, confirming the expected stoichiometry. To investigate the effect of the synthesis protocol on the morphology of the obtained ferrites, transmission electron microscopy (TEM) observations are performed on selected samples. The magnetic properties of the cobalt and manganese spinels are also investigated using a superconducting quantum device magnetometer (SQUID) revealing hard and soft ferrimagnetic behavior, respectively.
基金supported by the National Key Research and Development Program of China(2020YFB1713500)the Chinese 02 Special Fund(2017ZX02408003)+2 种基金the Open Fund of National Joint Engineering Research Center for abrasion control and molding of metal materials(HKDNM201807)the Student Research Training Plan of Henan University of Science and Technology(2020026)the National Undergraduate Innovation and Entrepreneurship Training Program(202010464031,202110464005)。
文摘Rechargeable aqueous Zn-ion batteries(AZIBs)are one of the most promising energy storage devices for large-scale energy storage owing to their high specific capacity,eco-friendliness,low cost and high safety.Nevertheless,zinc metal anodes suffer from severe dendrite growth and side reactions,resulting in the inferior electrochemical performance of AZIBs.To address these problems,surface modification of zinc metal anodes is a facile and effective method to regulate the interaction between the zinc anode and an electrolyte.In this review,the current challenges and strategies for zinc metal anodes are presented.Furthermore,recent advances in surface modification strategies to improve their electrochemical performance are concluded and discussed.Finally,challenges and prospects for future development of zinc metal anodes are proposed.We hope this review will be useful for designing and fabricating highperformance AZIBs and boosting their practical applications.
基金supported by the National Natural Science Foundation of China (Grant No 21173215, 21033009 and 11079005)
文摘A versatile wet chemistry method is developed for filling of subnanometer sized metal particles in carbon nanotubes with a diameter smaller than 1.5 nm. As an example, we showed that a confined bi-component Pd-V catalyst exhibit a higher benzene hydroxylation activity compared with that within multi-walled carbon nanotubes.
基金supported by the Australian Research Council(FT170100224)。
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR),powered by renewable energy,emerges as a promising approach against environmental issues and energy crisis by converting CO_(2) into val‐ue‐added chemicals.Single atom catalysts(SACs)with isolated metal atoms dispersed on supports exhibit outstanding performance for CO_(2) electroreduction,because of their strong single at‐om‐support interactions,maximum metal utilization and excellent catalytic activity.However,SACs suffer from agglomeration of particles,low metal loading,and difficulty in large‐scale production.In addition,molecular catalysts as another single atom‐based catalyst,consisting of ligands molecules connected to metal ions,exhibited similar metal‐nitrogen(M‐N)active centers as that in met‐al‐nitrogen‐carbon(M‐N‐C)SACs,which were highly active to CO_(2) reduction due to their well‐defined active sites and tunability over the steric and electronic properties of the active sites.Nonetheless,molecular catalysts are challenged by generally moderate activity,selectivity and sta‐bility,poor conductivity and aggregation.Many works have been devoted to overcoming these is‐sues of SACs and molecular catalysts for efficient CO_(2)RR,but only limited reviews for systematic summary of their fabrication,application,and characterizations,which were highlighted in this review.Firstly,we summarize recent advanced strategies in preparing SACs for CO_(2)RR,including wet‐chemistry approaches(defect engineering,spatial confinement,and coordination design),other synthetic methods and large‐scale production of SACs.Besides,electrochemical applications of SACs and molecular catalysts on CO_(2)RR are discussed,which involved the faradaic efficiency and partial current density of the desired product as well as the catalyst stability.In addition,ex‐situ and in‐situ/operando characterization techniques are briefly assessed,benefiting probing the active sites and understanding the CO_(2)RR catalytic mechanisms.Finally,future directions for the devel‐opment of single atom‐based catalysts(SACs,molecular catalysts)are pointed out.
基金Project supported by National Natural Science Foundation of China(51972097)This work was financially supported by the Science Foundation of Hebei Normal University,China(L2019K11).This work was also financially supported by the project WINLEDS—POCI-01-0145-FEDER-030351 and developed within the scope of the project CICECO-Aveiro Institute of Materials,FCT Ref.UID/CTM/50011/2019,financed by national funds through the FCT/MCTES.
文摘The Sr2 CeO4:Ln3+(Ln=Eu,Dy)fine phosphor particles were prepared by a facile wet chemical approach,in which the consecutive hydrothermal-combustion reaction was performed.The doping of Ln3+into Sr2 CeO4 has little influence on the structure of host,and the as-prepared samples display wellcrystallized spherical or elliptical shape with an average particle size at about 100-200 nm.For Eu3+ions-doped Sr2 CeO4,with the increase of Eu3+-doping concentration,the blue light emission band with the maximum at 468 nm originating from a Ce4+→O2-charge transfer of the host decreases obviously and the characteristic red light emission of Eu3+(5 D0→7 F2 transition at 618 nm)is enhanced gradually.Simultaneously,the fluorescent lifetime of the broadband emission of Sr2 CeO4 decreases with the doping of Eu3+,indicating an efficient energy transfer from the host to the doping Eu3+ions.The ene rgy transfer efficiency from the host to Eu3+was investigated in detail,and the emitting color of Sr2 CeO4:Eu3+can be easily tuned from blue to red by varying the doping concentration of Eu3+ions.Moreover,the luminescence of Dy3+-doped Sr2 CeO4 was also studied.Similar energy transfer pheno menon can be observed,and the incorporation of Dy3+into Sr2 CeO4 host leads to the characteristic emission of 4 F9/2→6 H15/2(488 nm,blue light)and 4 F9/2→6 H13/2(574 nm,yellow light)of Dy3+.The Sr2 CeO4:Ln3+fine particles with tunable luminescence are quite beneficial for its potential applications in the optoelectronic fields.