SnS,a well-known van der Waals chalcogenide,is susceptible to oxidation in high-temperature or highhumidity environments,significantly impacting its functional performance and device stability.Conversely,oxidation can...SnS,a well-known van der Waals chalcogenide,is susceptible to oxidation in high-temperature or highhumidity environments,significantly impacting its functional performance and device stability.Conversely,oxidation can be used as an effective strategy for surface engineering,allowing for structure modulation or design,property tuning and application exploration.However,there is currently a gap in understanding the relationship between the oxidation behavior of SnS,the structure of its oxidized surface,and the dependence on oxidation temperature.In this study,we systematically investigated the evolution of SnS surfaces under thermal oxidation using electron microscopy.The microstructure evolution(e.g.,surface structures,phases,defects,and interface)of SnS during high-temperature oxidation has been fully characterized and studied based on cross-sectional samples.Various surface heterostructures were constructed,including SnO_(2)/SnS,SnO_(2)/SnS_(2)/SnS,and SnO_(2)/Sn_(2)S_(3)/SnS,offering significant potential for the surface functionalization of SnS-based systems.Accordingly,oxidation mechanisms at different stages were elucidated based on the detailed and clear picture of microstructures.This research not only deepens our understanding of the fundamental science of SnS oxidation but also provides valuable insights for preventing and developing surface oxidation engineering in SnS and other van der Waals chalcogenides/materials.展开更多
Tin sulfide(SnS)is a promising non-toxic thermoelectric(TE)material to replace SnSe(Se is toxic),due to its similar structure and low thermal conductivity(k)comparable to SnSe.However,the poor electrical conductivity(...Tin sulfide(SnS)is a promising non-toxic thermoelectric(TE)material to replace SnSe(Se is toxic),due to its similar structure and low thermal conductivity(k)comparable to SnSe.However,the poor electrical conductivity(s)of SnS results in lower TE performance.In this work,high pressure was utilized to regulate the electronic structure,thereby mediating the conflict of electron and phonon transport to optimize the TE performance.In situ measurements of thermoelectric properties for SnS under high pressure and high temperature revealed that although the Seebeck coefficient(S)and k slightly decrease with increasing pressure,the s dramatically increases with increasing pressure,finally increasing the dimensionless figure of merit(ZT).The s increases from 2135 S·m^(-1)to 83549 S·m^(-1)as the pressure increases from 1 GPa to 5 GPa at 325 K,representing an increase of an order of magnitude.The high s of SnS leads to an increase in the PF to 1436μW·m^(-1)·K^(-2)at 5 GPa and 652 K.The maximum ZT value of 0.77 at 5 GPa and 652 K was obtained,which is 4 times the maximum ZT under ambient pressure and is comparable to that of doped SnS.The increase in s is due to the fact that pressure modulates the band structure of SnS by narrowing the band gap from 1.013 eV to 0.712 eV.This study presents a valuable guide for searching new high TE performance materials using high pressure.展开更多
Lithium-sulfur batteries(LSBs)offer high energy density and low cost but face challenges such as low sulfur utilization,lithium polysulfides(LiPSs)shuttling,and limited reaction kinetics.To address these issues,we rat...Lithium-sulfur batteries(LSBs)offer high energy density and low cost but face challenges such as low sulfur utilization,lithium polysulfides(LiPSs)shuttling,and limited reaction kinetics.To address these issues,we rationally design a Ti_(3)C_(2)T_(x)/SnS Mott-Schottky heterostructure with a built-in electric field.This three-dimensional(3D)porous architecture can enhance sulfur loading,facilitate electrolyte penetration,and expose more adsorption and catalytic sites.More importantly,the built-in electric field facilitates charge transfer and directs LiPSs migration from SnS to Ti_(3)C_(2)T_(x).The oriented migration of LiPSs enables rapid catalytic conversion at the Ti_(3)C_(2)T_(x)/SnS heterogeneous interface,enhancing electrocatalytic activity and sulfur reduction reaction kinetics.The Ti_(3)C_(2)T_(x)/SnS/S cathode achieves a high initial capacity(1367.1 mAh g^(-1)),excellent rate performance(602.7 mAh g^(-1)at 3 C),and stable long cycling performance with an average capacity decay rate of only 0.029%per cycle at 2 C.Additionally,a high-sulfur-loaded 3 Dprinted cathode with loading of 12.7 mg cm^(-2)manufactured using 3D printing exhibits an areal capacity of 15.0 mAh cm^(-2),retaining 8.9 mAh cm^(-2)after 70 cycles.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.11904039,52125103,52071041,U21A2054 and 12104071)。
文摘SnS,a well-known van der Waals chalcogenide,is susceptible to oxidation in high-temperature or highhumidity environments,significantly impacting its functional performance and device stability.Conversely,oxidation can be used as an effective strategy for surface engineering,allowing for structure modulation or design,property tuning and application exploration.However,there is currently a gap in understanding the relationship between the oxidation behavior of SnS,the structure of its oxidized surface,and the dependence on oxidation temperature.In this study,we systematically investigated the evolution of SnS surfaces under thermal oxidation using electron microscopy.The microstructure evolution(e.g.,surface structures,phases,defects,and interface)of SnS during high-temperature oxidation has been fully characterized and studied based on cross-sectional samples.Various surface heterostructures were constructed,including SnO_(2)/SnS,SnO_(2)/SnS_(2)/SnS,and SnO_(2)/Sn_(2)S_(3)/SnS,offering significant potential for the surface functionalization of SnS-based systems.Accordingly,oxidation mechanisms at different stages were elucidated based on the detailed and clear picture of microstructures.This research not only deepens our understanding of the fundamental science of SnS oxidation but also provides valuable insights for preventing and developing surface oxidation engineering in SnS and other van der Waals chalcogenides/materials.
基金support from the Program for the Development of Science and Technology of Jilin Province(Grant No.SKL202402004)the Jilin Province Major Science and Technology Program(Grant No.20240211002GX)the Open Research Fund of the Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education(Jilin Normal University,202405).
文摘Tin sulfide(SnS)is a promising non-toxic thermoelectric(TE)material to replace SnSe(Se is toxic),due to its similar structure and low thermal conductivity(k)comparable to SnSe.However,the poor electrical conductivity(s)of SnS results in lower TE performance.In this work,high pressure was utilized to regulate the electronic structure,thereby mediating the conflict of electron and phonon transport to optimize the TE performance.In situ measurements of thermoelectric properties for SnS under high pressure and high temperature revealed that although the Seebeck coefficient(S)and k slightly decrease with increasing pressure,the s dramatically increases with increasing pressure,finally increasing the dimensionless figure of merit(ZT).The s increases from 2135 S·m^(-1)to 83549 S·m^(-1)as the pressure increases from 1 GPa to 5 GPa at 325 K,representing an increase of an order of magnitude.The high s of SnS leads to an increase in the PF to 1436μW·m^(-1)·K^(-2)at 5 GPa and 652 K.The maximum ZT value of 0.77 at 5 GPa and 652 K was obtained,which is 4 times the maximum ZT under ambient pressure and is comparable to that of doped SnS.The increase in s is due to the fact that pressure modulates the band structure of SnS by narrowing the band gap from 1.013 eV to 0.712 eV.This study presents a valuable guide for searching new high TE performance materials using high pressure.
基金the financial support from the National Natural Science Foundation of China(52203340)the Guangdong Basic and Applied Basic Research Foundation(2025A1515012287)+1 种基金the Natural Science Foundation of Hubei Province(Joint Fund,2025AFD334)the Hubei Key Laboratory of Energy Storage and Power Battery(Hubei University of Automotive Technology,ZDK22024B06)。
文摘Lithium-sulfur batteries(LSBs)offer high energy density and low cost but face challenges such as low sulfur utilization,lithium polysulfides(LiPSs)shuttling,and limited reaction kinetics.To address these issues,we rationally design a Ti_(3)C_(2)T_(x)/SnS Mott-Schottky heterostructure with a built-in electric field.This three-dimensional(3D)porous architecture can enhance sulfur loading,facilitate electrolyte penetration,and expose more adsorption and catalytic sites.More importantly,the built-in electric field facilitates charge transfer and directs LiPSs migration from SnS to Ti_(3)C_(2)T_(x).The oriented migration of LiPSs enables rapid catalytic conversion at the Ti_(3)C_(2)T_(x)/SnS heterogeneous interface,enhancing electrocatalytic activity and sulfur reduction reaction kinetics.The Ti_(3)C_(2)T_(x)/SnS/S cathode achieves a high initial capacity(1367.1 mAh g^(-1)),excellent rate performance(602.7 mAh g^(-1)at 3 C),and stable long cycling performance with an average capacity decay rate of only 0.029%per cycle at 2 C.Additionally,a high-sulfur-loaded 3 Dprinted cathode with loading of 12.7 mg cm^(-2)manufactured using 3D printing exhibits an areal capacity of 15.0 mAh cm^(-2),retaining 8.9 mAh cm^(-2)after 70 cycles.
