^(99)Mo是重要的医用放射性核素,溶剂萃取法是反应堆辐照^(235)U靶生产裂变^(99)Mo的分离方法之一。为探讨离子液体Cyphos IL 101用于裂变^(99)Mo分离的可能性,本研究评价了离子液体Cyphos IL 101在硝酸体系中对Mo(Ⅵ)的萃取行为,重点...^(99)Mo是重要的医用放射性核素,溶剂萃取法是反应堆辐照^(235)U靶生产裂变^(99)Mo的分离方法之一。为探讨离子液体Cyphos IL 101用于裂变^(99)Mo分离的可能性,本研究评价了离子液体Cyphos IL 101在硝酸体系中对Mo(Ⅵ)的萃取行为,重点考察了稀释剂、水相初始pH、萃取时间、温度、离子液体浓度等对萃取Mo(Ⅵ)的影响。结果表明,选用甲苯作为稀释剂时,Cyphos IL 101对Mo(Ⅵ)的萃取效果最好,在pH=3条件下,萃取率高达98.87%;萃取为自发进行的过程,且可在5 min达到平衡;选用1 mol/L Na_(2)CO_(3)作为反萃剂,一次反萃可将负载有机相中96.56%的Mo反萃到水相中。构建的离子液体Cyphos IL 101萃取体系对Mo与主要杂质Sr、Cs、Te等有很好的分离效果,体现了其对Mo(Ⅵ)的高选择性萃取能力。以上结果可为将离子液体Cyphos IL 101引入裂变^(99)Mo的分离工艺流程提供参考。展开更多
Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages ...Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages of amorphous materials to optimize the interfacial structure for efficient Na^(+)storage.Herein,the dense homologous amorphous/crystalline heterointerfaces are in situ achieved in N-doped carbon nanobundles via self-polymerization and precise nitriding(Mo–N/Mo_(2)N@C).The amorphous Mo–N rich in unsaturated vacancy defects provides abundant active sites with isotropic ion-transport channels,and can effectively alleviate structural stress from crystalline Mo_(2)N.Meanwhile,the conductive Mo_(2)N can facilitate effective electron transfer,augmented further by the carbon encapsulation.Theoretical calculations reveal that the dense heterointerfaces can optimize the electronic structure and shift the d-p orbital centers of Mo and N upward,thereby enhancing the adsorption and mobility of Na^(+),and ultimately improving the charge transport and storage efficiency of the electrode.The Mo–N/Mo_(2)N@C as an anode delivers a 46.9%increase in reversible capacity over Mo_(2)N@C,reaching 461.1 m Ah.g^(–1)at 0.1 A.g^(–1),along with improved rate capability and cycling stability,underlining its practical utility.These results suggest that the homologous interfacial coupling can boost the storage properties of nitrides,providing a valuable reference for improving the properties of electrodes with low theoretical capacities.展开更多
Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5...Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5)P_(4)catalysts on nickel foam with efficient hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performance in alkaline media.Density Functional Theory(DFT)calculations and experimental studies have shown that Mo doping deadeneds the interaction between H and O atomic orbitals of transition state water molecules,effectively weakening the activation energy of H_(2)O dissociation.Therefore,Mo doping is favorable for enhancing HER activity with overpotential at 10 mA cm^(-2)of 93 mV and Tafel slope of 40.1 mV dec^(-1)in 1 M KOH.Besides,it exhibits high alkaline OER activity with an ultra-low overpotential of 200 mV at 10 mA cm^(-2).Moreover,this catalyst only needs 1.537 V in a dual-electrode configuration of the electrolytic cell,which is much lower than the commercial Pt/C-RuO_(2)couple(1.614 V).In addition,we have developed and constructed a solar thermoelectric generator(TEG)that is capable of floating on water.This TEG has a continuous power output and an exceptionally long lifespan,providing a stable power supply to the synthesized catalyst electrolyzer.It can produce a maximum power output of over 90 mW,meeting the requirement of converting solar radiation heat into usable electricity.As a result,the system achieves productivity of 0.11 mL min^(-1)H_(2).This solar thermal energy conversion technology shows the possibility of large-scale industrial production of H_(2)and provides a new idea for exploring heat source utilization.展开更多
文摘^(99)Mo是重要的医用放射性核素,溶剂萃取法是反应堆辐照^(235)U靶生产裂变^(99)Mo的分离方法之一。为探讨离子液体Cyphos IL 101用于裂变^(99)Mo分离的可能性,本研究评价了离子液体Cyphos IL 101在硝酸体系中对Mo(Ⅵ)的萃取行为,重点考察了稀释剂、水相初始pH、萃取时间、温度、离子液体浓度等对萃取Mo(Ⅵ)的影响。结果表明,选用甲苯作为稀释剂时,Cyphos IL 101对Mo(Ⅵ)的萃取效果最好,在pH=3条件下,萃取率高达98.87%;萃取为自发进行的过程,且可在5 min达到平衡;选用1 mol/L Na_(2)CO_(3)作为反萃剂,一次反萃可将负载有机相中96.56%的Mo反萃到水相中。构建的离子液体Cyphos IL 101萃取体系对Mo与主要杂质Sr、Cs、Te等有很好的分离效果,体现了其对Mo(Ⅵ)的高选择性萃取能力。以上结果可为将离子液体Cyphos IL 101引入裂变^(99)Mo的分离工艺流程提供参考。
基金financially supported by the National Natural Science Foundation of China(No.51762021)the Natural Science Foundation of Jiangxi province(Nos.20224ACB204008,20242BAB25223,and 20242BAB25248)the Special Funding Program for Graduate Student Innovation of Jiangxi Province(No.YC2024-S594)。
文摘Optimizing the interfacial environments of electrodes has emerged as an effective strategy to improve their electrochemical properties.Amorphous/crystalline interfacial coupling can effectively utilize the advantages of amorphous materials to optimize the interfacial structure for efficient Na^(+)storage.Herein,the dense homologous amorphous/crystalline heterointerfaces are in situ achieved in N-doped carbon nanobundles via self-polymerization and precise nitriding(Mo–N/Mo_(2)N@C).The amorphous Mo–N rich in unsaturated vacancy defects provides abundant active sites with isotropic ion-transport channels,and can effectively alleviate structural stress from crystalline Mo_(2)N.Meanwhile,the conductive Mo_(2)N can facilitate effective electron transfer,augmented further by the carbon encapsulation.Theoretical calculations reveal that the dense heterointerfaces can optimize the electronic structure and shift the d-p orbital centers of Mo and N upward,thereby enhancing the adsorption and mobility of Na^(+),and ultimately improving the charge transport and storage efficiency of the electrode.The Mo–N/Mo_(2)N@C as an anode delivers a 46.9%increase in reversible capacity over Mo_(2)N@C,reaching 461.1 m Ah.g^(–1)at 0.1 A.g^(–1),along with improved rate capability and cycling stability,underlining its practical utility.These results suggest that the homologous interfacial coupling can boost the storage properties of nitrides,providing a valuable reference for improving the properties of electrodes with low theoretical capacities.
基金supported by the Hainan Provincial Natural Science Foundation of China(Nos.522MS038 and 522QN282)the National Natural Science Foundation of China(Nos.52172086 and 52301268)the Start-up Research Foundation of Hainan University(No.KYQD(ZR)-22019).
文摘Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future.In this work,we prepared porous nanosheet Mo doping Ni_(5)P_(4)catalysts on nickel foam with efficient hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performance in alkaline media.Density Functional Theory(DFT)calculations and experimental studies have shown that Mo doping deadeneds the interaction between H and O atomic orbitals of transition state water molecules,effectively weakening the activation energy of H_(2)O dissociation.Therefore,Mo doping is favorable for enhancing HER activity with overpotential at 10 mA cm^(-2)of 93 mV and Tafel slope of 40.1 mV dec^(-1)in 1 M KOH.Besides,it exhibits high alkaline OER activity with an ultra-low overpotential of 200 mV at 10 mA cm^(-2).Moreover,this catalyst only needs 1.537 V in a dual-electrode configuration of the electrolytic cell,which is much lower than the commercial Pt/C-RuO_(2)couple(1.614 V).In addition,we have developed and constructed a solar thermoelectric generator(TEG)that is capable of floating on water.This TEG has a continuous power output and an exceptionally long lifespan,providing a stable power supply to the synthesized catalyst electrolyzer.It can produce a maximum power output of over 90 mW,meeting the requirement of converting solar radiation heat into usable electricity.As a result,the system achieves productivity of 0.11 mL min^(-1)H_(2).This solar thermal energy conversion technology shows the possibility of large-scale industrial production of H_(2)and provides a new idea for exploring heat source utilization.
