Carbonate electrolytes are one of the most desirable electrolytes for high-energy lithium-sulfur batteries(LSBs)because of their successful implementation in commercial Li-ion batteries.The low-polysulfide-solubility ...Carbonate electrolytes are one of the most desirable electrolytes for high-energy lithium-sulfur batteries(LSBs)because of their successful implementation in commercial Li-ion batteries.The low-polysulfide-solubility feature of some carbonate solvents also makes them very promising for overcoming the shuttle effects of LSBs.However,regular sulfur electrodes experience undesired electrochemical mechanisms in carbonate electrolytes due to side reactions.In this study,we report a catalytic redox mechanism of sulfur in propylene carbonate(PC)electrolyte based on a compari-son study.The catalytic mechanism is characterized by the interactions between polysulfides and dual N/O functional groups on the host carbon,which largely prevents side reactions between polysulfides and the carbonate electrolyte.Such a mechanism coupled with the low-polysulfide-solubility feature leads to stable cycling of LSBs in PC electrolyte.Favorable dual N/O functional groups are identified via a density functional theory study.This work provides an alternative route for enabling LSBs in carbonate electrolytes.展开更多
Despite the high amount of scientific work dedicated to the gold nanoparticles in catalysis, most of the research has been performed utilising supported nanoparticles obtained by traditional impreg‐nation of gold sal...Despite the high amount of scientific work dedicated to the gold nanoparticles in catalysis, most of the research has been performed utilising supported nanoparticles obtained by traditional impreg‐nation of gold salts onto a support, co‐precipitation or deposition‐precipitation methods which do not benefit from the recent advances in nanotechnologies. Only more recently, gold catalyst scien‐tists have been exploiting the potential of preforming the metal nanoparticles in a colloidal suspen‐sion before immobilisation with great results in terms of catalytic activity and the morphology con‐trol of mono‐and bimetallic catalysts. On the other hand, the last decade has seen the emergence of more advanced control in gold metal nanoparticle synthesis, resulting in a variety of anisotropic gold nanoparticles with easily accessible new morphologies that offer control over the coordination of surface atoms and the optical properties of the nanoparticles （tunable plasmon band） with im‐mense relevance for catalysis. Such morphologies include nanorods, nanostars, nanoflowers, den‐dritic nanostructures or polyhedral nanoparticles to mention a few. In addition to highlighting newly developed methods and properties of anisotropic gold nanoparticles, in this review we ex‐amine the emerging literature that clearly indicates the often superior catalytic performance and amazing potential of these nanoparticles to transform the field of heterogeneous catalysis by gold by offering potentially higher catalytic performance, control over exposed active sites, robustness and tunability for thermal‐, electro‐and photocatalysis.展开更多
文摘Carbonate electrolytes are one of the most desirable electrolytes for high-energy lithium-sulfur batteries(LSBs)because of their successful implementation in commercial Li-ion batteries.The low-polysulfide-solubility feature of some carbonate solvents also makes them very promising for overcoming the shuttle effects of LSBs.However,regular sulfur electrodes experience undesired electrochemical mechanisms in carbonate electrolytes due to side reactions.In this study,we report a catalytic redox mechanism of sulfur in propylene carbonate(PC)electrolyte based on a compari-son study.The catalytic mechanism is characterized by the interactions between polysulfides and dual N/O functional groups on the host carbon,which largely prevents side reactions between polysulfides and the carbonate electrolyte.Such a mechanism coupled with the low-polysulfide-solubility feature leads to stable cycling of LSBs in PC electrolyte.Favorable dual N/O functional groups are identified via a density functional theory study.This work provides an alternative route for enabling LSBs in carbonate electrolytes.
基金supported by the Science and Engineering Research Council through Grant(152-70-00017)Use of Computing Resources at the A*STAR Computational Resource Centre and National Supercomputer Centre,Singapore
基金supported by the Project from Institute of Chemical and Engineering Sciences (ICES), Singapore (ICES/15-1G4B01)~~
文摘Despite the high amount of scientific work dedicated to the gold nanoparticles in catalysis, most of the research has been performed utilising supported nanoparticles obtained by traditional impreg‐nation of gold salts onto a support, co‐precipitation or deposition‐precipitation methods which do not benefit from the recent advances in nanotechnologies. Only more recently, gold catalyst scien‐tists have been exploiting the potential of preforming the metal nanoparticles in a colloidal suspen‐sion before immobilisation with great results in terms of catalytic activity and the morphology con‐trol of mono‐and bimetallic catalysts. On the other hand, the last decade has seen the emergence of more advanced control in gold metal nanoparticle synthesis, resulting in a variety of anisotropic gold nanoparticles with easily accessible new morphologies that offer control over the coordination of surface atoms and the optical properties of the nanoparticles （tunable plasmon band） with im‐mense relevance for catalysis. Such morphologies include nanorods, nanostars, nanoflowers, den‐dritic nanostructures or polyhedral nanoparticles to mention a few. In addition to highlighting newly developed methods and properties of anisotropic gold nanoparticles, in this review we ex‐amine the emerging literature that clearly indicates the often superior catalytic performance and amazing potential of these nanoparticles to transform the field of heterogeneous catalysis by gold by offering potentially higher catalytic performance, control over exposed active sites, robustness and tunability for thermal‐, electro‐and photocatalysis.
