The practical application of lithium–sulfur(Li–S)batteries is limited by the easy dissolution of polysulfides in the electrolyte,resulting in the lithium polysulfide(LPS)shuttle effect.Several two-dimensional(2D)mat...The practical application of lithium–sulfur(Li–S)batteries is limited by the easy dissolution of polysulfides in the electrolyte,resulting in the lithium polysulfide(LPS)shuttle effect.Several two-dimensional(2D)materials with abundant active binding sites and high surface-to-volume ratios have been developed to prepare functional separators that suppress the diffusion of polysulfides.However,the influence of modified layer thickness on Li+transport has not been considered.Herein,we synthesized individual and multilayered 2D Ti3C2Tx MXene nanosheets and used them to fabricate a series of Ti3C2Tx-PP modified separators.The separators had mass loadings ranging from 0.16 to 0.016 mg cm-2,which is the lowest value reported for 2D materials to the best of our knowledge.The corresponding reductions in thickness ranged from 1.2μm to 100 nm.LPS shuttling was effectively suppressed,even at the lowest mass loading of 0.016 mg cm-2.Suppression was due to the strong interaction between LPS intermediates and Ti atoms and hydroxyl functional groups on the separator surface.The lithium-ion diffusion coefficient increased with the reduction of Ti3C2Tx layers on the separator.Superior cycling stability and rate performance were attained when the separator with a Ti3C2Tx-PP mass loading of 0.016 mg cm-2 was incorporated into a Li–S battery.Carbon nanotubes(CNTs)were introduced into the separators to further improve the electrical and Li+ionic conductivity in the cross-plane direction of the 2D Ti3C2Txlayers.With the ultralightweight Ti3C2Tx/CNTs modified PP separator,the cell maintained a capacity of 640 m Ah g-1after 200cycles at 1C with a capacity decay of only 0.079%per cycle.展开更多
High performance supercapacitors coupled with mechanical flexibility are needed to drive flexible and wearable electronics that have anesthetic appeal and multi-functionality. Two dimensional（2D） materials have attr...High performance supercapacitors coupled with mechanical flexibility are needed to drive flexible and wearable electronics that have anesthetic appeal and multi-functionality. Two dimensional（2D） materials have attracted attention owing to their unique physicochemical and electrochemical properties, in addition to their ability to form hetero-structures with other nanomaterials further improving mechanical and electrochemical properties. After a brief introduction of supercapacitors and 2D materials, recent progress on flexible supercapacitors using 2D materials is reviewed. Here we provide insights into the structure–property relationships of flexible electrodes, in particular free-standing films. We also present our perspectives on the development of flexible supercapacitors.展开更多
The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we desi...The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.展开更多
基金financially supported by the National Natural Science Foundation of China(21706292)support from the Hunan Provincial Science and Technology Plan Project,China(No.2017TP1001).
文摘The practical application of lithium–sulfur(Li–S)batteries is limited by the easy dissolution of polysulfides in the electrolyte,resulting in the lithium polysulfide(LPS)shuttle effect.Several two-dimensional(2D)materials with abundant active binding sites and high surface-to-volume ratios have been developed to prepare functional separators that suppress the diffusion of polysulfides.However,the influence of modified layer thickness on Li+transport has not been considered.Herein,we synthesized individual and multilayered 2D Ti3C2Tx MXene nanosheets and used them to fabricate a series of Ti3C2Tx-PP modified separators.The separators had mass loadings ranging from 0.16 to 0.016 mg cm-2,which is the lowest value reported for 2D materials to the best of our knowledge.The corresponding reductions in thickness ranged from 1.2μm to 100 nm.LPS shuttling was effectively suppressed,even at the lowest mass loading of 0.016 mg cm-2.Suppression was due to the strong interaction between LPS intermediates and Ti atoms and hydroxyl functional groups on the separator surface.The lithium-ion diffusion coefficient increased with the reduction of Ti3C2Tx layers on the separator.Superior cycling stability and rate performance were attained when the separator with a Ti3C2Tx-PP mass loading of 0.016 mg cm-2 was incorporated into a Li–S battery.Carbon nanotubes(CNTs)were introduced into the separators to further improve the electrical and Li+ionic conductivity in the cross-plane direction of the 2D Ti3C2Txlayers.With the ultralightweight Ti3C2Tx/CNTs modified PP separator,the cell maintained a capacity of 640 m Ah g-1after 200cycles at 1C with a capacity decay of only 0.079%per cycle.
基金Funding from the Australian Research Council Centre of Excellence Scheme(CE 140100012)the funding from National Natural Science Foundation of China(51502206)+1 种基金the CSC scholarship from the Ministry of Education of PR Chinathe support of the CSC scholarship from the Ministry of Education of PR China
文摘High performance supercapacitors coupled with mechanical flexibility are needed to drive flexible and wearable electronics that have anesthetic appeal and multi-functionality. Two dimensional（2D） materials have attracted attention owing to their unique physicochemical and electrochemical properties, in addition to their ability to form hetero-structures with other nanomaterials further improving mechanical and electrochemical properties. After a brief introduction of supercapacitors and 2D materials, recent progress on flexible supercapacitors using 2D materials is reviewed. Here we provide insights into the structure–property relationships of flexible electrodes, in particular free-standing films. We also present our perspectives on the development of flexible supercapacitors.
文摘The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.
基金Supported by the National Natural Science Foundation of China(No.U1504218,No.51572007)the Ph.D Initial Scientific Research Fund of Anyang Institute of Technology(No.BSJ2016006)~~
