The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rati...The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rational design of heterostructure electrocatalysts with abundant active sites and strong interfacial electronic interactions is a promising but still challenging strategy for preventing shuttling of polysulfides in lithium-sulfur batteries.Herein,ultrathin nonlayered NiO/Ni_(3)S_(2)heterostructure nanosheets are developed through topochemical transformation of layered Ni(OH)_(2)templates to improve the utilization of sulfur and facilitate stable cycling of batteries.As a multifunction catalyst,NiO/Ni_(3)S_(2)not only enhances the adsorption of polysulfides and shorten the transport path of Li ions and electrons but also promotes the Li_(2)S formation and transformation,which are verified by both in-situ Raman spectroscopy and electrochemical investigations.Thus,the cell with NiO/Ni_(3)S_(2)as electrocatalyst delivers an area capacity of 4.8 mAh cm^(-2)under the high sulfur loading(6 mg cm^(-2))and low electrolyte/sulfur ratio(4.3 pL mg^(-1)).The strategy can be extended to 2D Ni foil,demonstrating its prospects in the construction of electrodes with high gravimetric/volumetric energy densities.The designed electrocatalyst of ultrathin nonlayered heterostructure will shed light on achieving high energy density lithium-sulfur batteries.展开更多
In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for impr...In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for improving the water oxidation activity of electrocatalysts has emerged as an effective strategy.Herein,we report the facile development of a Ni_(3)S_(2)-CeO_(2)hybrid nanostructure via an electrodeposition method.Benefiting from the strong interfacial interaction between Ni_(3)S_(2)and CeO_(2),the electron transfer is notably improved and the water oxidation activity of Ni_(3)S_(2)nanosheets is significantly enhanced.In 1.0 M KOH,the Ni_(3)S_(2)-CeO_(2)electrocatalyst achieves a current density of 20 mA cm-2 at a low overpotential of 264 mV,which is 92 mV lower than that of Ni_(3)S_(2).Moreover,Ni_(3)S_(2)-CeO_(2)exhibits superior electrochemical stability.Density functional theory calculations demonstrate that the enhanced OER electrocatalytic performance of Ni_(3)S_(2)-CeO_(2)can be ascribed to an increase in the binding strength of the reaction intermediates at the Ni_(3)S_(2)-CeO_(2)interface.展开更多
Carbon black and Cr_(2)AlC were used as raw materials to obtain a large number of Cr_(3)C_(2)nanosheets by means of the molten salt heat treatment at 1100℃for 1.5 hours.Results showed that carbon black can promote th...Carbon black and Cr_(2)AlC were used as raw materials to obtain a large number of Cr_(3)C_(2)nanosheets by means of the molten salt heat treatment at 1100℃for 1.5 hours.Results showed that carbon black can promote the decomposition of a large number of Cr_(2)AlC to form Cr_(3)C_(2)and Cr_(7)C_(3)nanoparticles at 1100℃in the absence of molten salt.Under a molten salt environment,carbon black can promote the complete decomposition of Cr_(2)AlC to form Cr_(3)C_(2)and Cr_(7)C_(3)nanosheets.The thickness of chromium carbide nanosheets is approximately 10-20 nm,and the length is approximately 100-200 nm.The addition of excess carbon black can promote the complete decomposition of Cr_(2)AlC into a material with Cr_(3)C_(2)as the main phase.展开更多
Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nano...Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nanosheet array on Ni foam(Co-Ni_(3)S_(2)/NF)as a high-efficiency OER electrocatalyst for seawater.In alkaline conditions,Co-Ni_(3)S_(2)/NF requires an overpotential of only 368 mV to drive 100 mA·cm^(–2),superior to Ni_(3)S_(2)/NF(385 mV).Besides,it exhibits at least 50-h continuous electrolysis.展开更多
Doping can change the band structure of semiconductors,thereby affecting their electrical,optical,and magnetic properties.In this study,we describe the synthesis of two-dimensional(2D)Se-doped Cr_(2)S_(3)(Se-Cr_(2)S_(...Doping can change the band structure of semiconductors,thereby affecting their electrical,optical,and magnetic properties.In this study,we describe the synthesis of two-dimensional(2D)Se-doped Cr_(2)S_(3)(Se-Cr_(2)S_(3))nanosheets using the chemical vapor deposition method.In these semiconductor nanosheets,the Se doping concentration can be controlled by tuning the Se/S mass ratio in the precursor.At the doping concentrations of 10.05%and 2.05%,the room temperature conductivity and mobility were increased by nearly 4 and 2 orders of magnitude,respectively.In addition,the response time of an ultrathin Se-Cr_(2)S_(3)photodetector was 200 times shorter than that of an undoped Cr_(2)S_(3)nanosheet photodetector.4.07%-Se-Cr_(2)S_(3)nanosheets show ferrimagnetic behavior with a Curie temperature of~200 K,which is 80 K higher than that of undoped Cr_(2)S_(3)nanosheets.A density functional theory calculation indicated that the Se doping can induce the formation of intercalated Cr vacancies in SeCr_(2)S_(3)and enhance its metallic characteristics.Our results demonstrated that Se-Cr_(2)S_(3)has significant potential in future electronic,optoelectronic,and spintronic devices.展开更多
Rational structure design and regulation are of paramount importance for obtaining electrode materials with desirable electrochemical performance.Here,a novel binder-free electrode with the hollow Co_(9)S_(8) core@mul...Rational structure design and regulation are of paramount importance for obtaining electrode materials with desirable electrochemical performance.Here,a novel binder-free electrode with the hollow Co_(9)S_(8) core@multi-shell structure(CS-x@MXene@Bi_(2)O_(3))derived from metal-organic frameworks(MOFs)precursor is well designed by the electrospinning,sulfuration,carbonization,and hydrothermal processes.In this architecture,the concentration of Co_(9)S_(8)(CS-x)is optimized for an ideal flexible substrate,which alleviates the dimensional variation for long cycle life.The unique cores and the MXene flakes engineered by Bi_(2)O_(3) multiple shells can be responsible for the superior characteristics,including a fast electronic pathway,large specific surface area,enhanced electrical conductivity,and improved electrochemical performance.As expected,the obtained CS-2@MXene@Bi_(2)O_(3) binder-free electrode exhibits a high discharge capacitance of 646.1 F g^(–1)(1 A g^(–1)).Two binder-free electrodes can be assembled into a solid-state supercapacitor with desirable energy and power density,and long-term cyclic stability is demonstrated through 5000 cycles.Given these advantages,the CS-2@MXene@Bi_(2)O_(3) is selected as the electrode in a foldable supercapacitor.More importantly,the specific capacitance is reserved after various deformations.Therefore,it is expected that binder-free electrode materials with the unique core@shell structure design could be applied in wearable and portable energy conversion devices.展开更多
The separation efficiency of electrons and holes and the enhancement of the surface reductive reaction in the metal sulfide semiconductor photocatalysts are important factors in boosting photocatalytic H_(2)evolution ...The separation efficiency of electrons and holes and the enhancement of the surface reductive reaction in the metal sulfide semiconductor photocatalysts are important factors in boosting photocatalytic H_(2)evolution from water.The control of both interface morphology and the charge-carrier utilization of metal sulfide-based photocatalysts can effectively improve the separation efficiency of electrons and holes and increase the surface reaction active sites,which are considered to be effective methods to improve the photocatalytic activity of semiconductors.Here,the Ti_(3)C_(2)(Mxene)modified all-sulfide 2D/2D Sscheme heterojunction Ti_(3)C_(2)/Zn In_(2)S_(4)(ZIS)/CdS composite material was firstly synthesized by a two-step solvothermal method.The formation of all-sulfide S-scheme heterojunction improves the efficiency of electron-hole separation.The intimate 2D/2D van der Waals structure provides a strong interaction force and a large contact area to enhance charge transfer.The addition of 2D Ti_(3)C_(2)forms the accumulation layer,reducing the recombination of electrons and holes.Under the synergistic promotion,the highest hydrogen production of the prepared Ti_(3)C_(2)/ZIS/CdS composite photocatalyst could reach 8.93 mmol/h/g.This work not only enriches the photocatalytic systems through integrating the ohmic junction and the 2D/2D all-sulfide S-scheme heterojunction,but also provides a satisfactory design strategy for engineering interfacial morphology and charge-carrier utilization.展开更多
基金supported by the National Natural Science Foundation of China(Grant nos.62090013,61974043,and 91833303)the National Key R&D Program of China(Grant no.2019YFB2203403)+1 种基金the Projects of Science and Technology Commission of Shanghai Municipality(Grant nos.21JC1402100 and 19511120100)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning.
文摘The practical application of Lithium-Sulfur batteries largely depends on highly efficient utilization and conversion of sulfur under the realistic condition of high-sulfur content and low electrolyte/sulfur ratio.Rational design of heterostructure electrocatalysts with abundant active sites and strong interfacial electronic interactions is a promising but still challenging strategy for preventing shuttling of polysulfides in lithium-sulfur batteries.Herein,ultrathin nonlayered NiO/Ni_(3)S_(2)heterostructure nanosheets are developed through topochemical transformation of layered Ni(OH)_(2)templates to improve the utilization of sulfur and facilitate stable cycling of batteries.As a multifunction catalyst,NiO/Ni_(3)S_(2)not only enhances the adsorption of polysulfides and shorten the transport path of Li ions and electrons but also promotes the Li_(2)S formation and transformation,which are verified by both in-situ Raman spectroscopy and electrochemical investigations.Thus,the cell with NiO/Ni_(3)S_(2)as electrocatalyst delivers an area capacity of 4.8 mAh cm^(-2)under the high sulfur loading(6 mg cm^(-2))and low electrolyte/sulfur ratio(4.3 pL mg^(-1)).The strategy can be extended to 2D Ni foil,demonstrating its prospects in the construction of electrodes with high gravimetric/volumetric energy densities.The designed electrocatalyst of ultrathin nonlayered heterostructure will shed light on achieving high energy density lithium-sulfur batteries.
文摘In the pursuit of stable,high performance Ni-based oxygen evolution reaction(OER)electrocatalysts,modifying the local chemical compositions or fabricating hybrid nanostructures to generate abundant interfaces for improving the water oxidation activity of electrocatalysts has emerged as an effective strategy.Herein,we report the facile development of a Ni_(3)S_(2)-CeO_(2)hybrid nanostructure via an electrodeposition method.Benefiting from the strong interfacial interaction between Ni_(3)S_(2)and CeO_(2),the electron transfer is notably improved and the water oxidation activity of Ni_(3)S_(2)nanosheets is significantly enhanced.In 1.0 M KOH,the Ni_(3)S_(2)-CeO_(2)electrocatalyst achieves a current density of 20 mA cm-2 at a low overpotential of 264 mV,which is 92 mV lower than that of Ni_(3)S_(2).Moreover,Ni_(3)S_(2)-CeO_(2)exhibits superior electrochemical stability.Density functional theory calculations demonstrate that the enhanced OER electrocatalytic performance of Ni_(3)S_(2)-CeO_(2)can be ascribed to an increase in the binding strength of the reaction intermediates at the Ni_(3)S_(2)-CeO_(2)interface.
基金the National Natural Science Foundation of China(No.51864028)Key Scientific and Technological Projects in Henan Province(No.212102210465)+2 种基金Key Scientific Research Project Plan of Colleges and Universities in Henan Province(No.22A430041,22B430035)National Innovation and Entrepreneurship Training Program for College Students(No.202110465013)National Natural Science Foundation of China(No.U2030207)。
文摘Carbon black and Cr_(2)AlC were used as raw materials to obtain a large number of Cr_(3)C_(2)nanosheets by means of the molten salt heat treatment at 1100℃for 1.5 hours.Results showed that carbon black can promote the decomposition of a large number of Cr_(2)AlC to form Cr_(3)C_(2)and Cr_(7)C_(3)nanoparticles at 1100℃in the absence of molten salt.Under a molten salt environment,carbon black can promote the complete decomposition of Cr_(2)AlC to form Cr_(3)C_(2)and Cr_(7)C_(3)nanosheets.The thickness of chromium carbide nanosheets is approximately 10-20 nm,and the length is approximately 100-200 nm.The addition of excess carbon black can promote the complete decomposition of Cr_(2)AlC into a material with Cr_(3)C_(2)as the main phase.
基金This research was funded by Deputy for Research&Innovation,Ministry of Education through Initiative of Institutional Funding at University of Ha’il–Saudi Arabia through project number IFP-22098.
文摘Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nanosheet array on Ni foam(Co-Ni_(3)S_(2)/NF)as a high-efficiency OER electrocatalyst for seawater.In alkaline conditions,Co-Ni_(3)S_(2)/NF requires an overpotential of only 368 mV to drive 100 mA·cm^(–2),superior to Ni_(3)S_(2)/NF(385 mV).Besides,it exhibits at least 50-h continuous electrolysis.
基金supported by the National Natural Science Foundation of China(Grant Nos.51872086,62174051,51991340,and 51991343)the Natural Science Foundation of Hunan Province(Grant No.2020JJ1001)+2 种基金the Hunan Province“Huxiang Talents”Project(Grant No.2021RC3038)the Double First-Class Initiative of Hunan University(Grant No.531109100004)the Shenzhen Basic Research Project(Grant No.JCYJ20210324142012035)。
文摘Doping can change the band structure of semiconductors,thereby affecting their electrical,optical,and magnetic properties.In this study,we describe the synthesis of two-dimensional(2D)Se-doped Cr_(2)S_(3)(Se-Cr_(2)S_(3))nanosheets using the chemical vapor deposition method.In these semiconductor nanosheets,the Se doping concentration can be controlled by tuning the Se/S mass ratio in the precursor.At the doping concentrations of 10.05%and 2.05%,the room temperature conductivity and mobility were increased by nearly 4 and 2 orders of magnitude,respectively.In addition,the response time of an ultrathin Se-Cr_(2)S_(3)photodetector was 200 times shorter than that of an undoped Cr_(2)S_(3)nanosheet photodetector.4.07%-Se-Cr_(2)S_(3)nanosheets show ferrimagnetic behavior with a Curie temperature of~200 K,which is 80 K higher than that of undoped Cr_(2)S_(3)nanosheets.A density functional theory calculation indicated that the Se doping can induce the formation of intercalated Cr vacancies in SeCr_(2)S_(3)and enhance its metallic characteristics.Our results demonstrated that Se-Cr_(2)S_(3)has significant potential in future electronic,optoelectronic,and spintronic devices.
基金supported by the Outstanding Youth Fund of Heilongjiang Province (JQ 2020B002)Guangxi Science and Technology Base and Talent Special Project (AD21075001)the Reform and Development Fund Project of Local University supported by the Central Government。
基金support from the National Natural Science Foundation of China(no.52072307)。
文摘Rational structure design and regulation are of paramount importance for obtaining electrode materials with desirable electrochemical performance.Here,a novel binder-free electrode with the hollow Co_(9)S_(8) core@multi-shell structure(CS-x@MXene@Bi_(2)O_(3))derived from metal-organic frameworks(MOFs)precursor is well designed by the electrospinning,sulfuration,carbonization,and hydrothermal processes.In this architecture,the concentration of Co_(9)S_(8)(CS-x)is optimized for an ideal flexible substrate,which alleviates the dimensional variation for long cycle life.The unique cores and the MXene flakes engineered by Bi_(2)O_(3) multiple shells can be responsible for the superior characteristics,including a fast electronic pathway,large specific surface area,enhanced electrical conductivity,and improved electrochemical performance.As expected,the obtained CS-2@MXene@Bi_(2)O_(3) binder-free electrode exhibits a high discharge capacitance of 646.1 F g^(–1)(1 A g^(–1)).Two binder-free electrodes can be assembled into a solid-state supercapacitor with desirable energy and power density,and long-term cyclic stability is demonstrated through 5000 cycles.Given these advantages,the CS-2@MXene@Bi_(2)O_(3) is selected as the electrode in a foldable supercapacitor.More importantly,the specific capacitance is reserved after various deformations.Therefore,it is expected that binder-free electrode materials with the unique core@shell structure design could be applied in wearable and portable energy conversion devices.
基金financially supported by the National Natural Science Foundation of China(Nos.21975084 and 51672089)the Ding Ying Talent Project of South China Agricultural University for their support。
文摘The separation efficiency of electrons and holes and the enhancement of the surface reductive reaction in the metal sulfide semiconductor photocatalysts are important factors in boosting photocatalytic H_(2)evolution from water.The control of both interface morphology and the charge-carrier utilization of metal sulfide-based photocatalysts can effectively improve the separation efficiency of electrons and holes and increase the surface reaction active sites,which are considered to be effective methods to improve the photocatalytic activity of semiconductors.Here,the Ti_(3)C_(2)(Mxene)modified all-sulfide 2D/2D Sscheme heterojunction Ti_(3)C_(2)/Zn In_(2)S_(4)(ZIS)/CdS composite material was firstly synthesized by a two-step solvothermal method.The formation of all-sulfide S-scheme heterojunction improves the efficiency of electron-hole separation.The intimate 2D/2D van der Waals structure provides a strong interaction force and a large contact area to enhance charge transfer.The addition of 2D Ti_(3)C_(2)forms the accumulation layer,reducing the recombination of electrons and holes.Under the synergistic promotion,the highest hydrogen production of the prepared Ti_(3)C_(2)/ZIS/CdS composite photocatalyst could reach 8.93 mmol/h/g.This work not only enriches the photocatalytic systems through integrating the ohmic junction and the 2D/2D all-sulfide S-scheme heterojunction,but also provides a satisfactory design strategy for engineering interfacial morphology and charge-carrier utilization.
