A systematic and green low-temperature sulfation roasting−water leaching strategy was put forward to achieve a very high fluorine removal rate of 97.82%for spent carbon cathode(SCC),which was believed as a hazardous s...A systematic and green low-temperature sulfation roasting−water leaching strategy was put forward to achieve a very high fluorine removal rate of 97.82%for spent carbon cathode(SCC),which was believed as a hazardous solid waste.And the carbon could be recycled with a purity of 90.29 wt.%in the flaky microstructure.Thermodynamic analysis and the results of SEM,XRD and EDS indicate that most of the fluoride could convert into water-soluble sulfate at low temperature.And the highest fluorine removal rate could be obtained when<0.15 mm SCC particles were mixed with sulfuric acid at a liquid-to-solid ratio of 1:1,and then roasted at 300℃ for 0.5 h.The sulfate was removed to purify the carbon via water-leaching process.Avrami exponents and corresponding activation energy for the roasting and leaching process demonstrated that both processes are controlled by diffusion.展开更多
To recover metal from copper slags,a new process involving two steps of oxidative desulfurization followed by smelting reduction was proposed in which one hazardous waste(waste cathode carbon)was used to treat another...To recover metal from copper slags,a new process involving two steps of oxidative desulfurization followed by smelting reduction was proposed in which one hazardous waste(waste cathode carbon)was used to treat another(copper slags).The waste cathode carbon is used not only as a reducing agent but also as a fluxing agent to decrease slag melting point.Upon holding for 60 min in air atmosphere first and then smelting with 14.4 wt%waste cathode carbon and 25 wt%CaO for 180 min in high purity Ar atmosphere at 1450℃,the recovery rates of Cu and Fe reach 95.89%and 94.64%,respectively,and meanwhile greater than 90%of the fluoride from waste cathode carbon is transferred into the final slag as CaF_(2) and Ca_(2)Si_(2)F_(2)O_(7),which makes the content of soluble F in the slag meet the national emission standard.Besides,the sulphur content in the obtained Fe-Cu alloy is low to 0.03 wt%.展开更多
A laboratory-scale intermediate-temperature H2S fuel cell with a configuration of H2S, (metal sulfide-based composite anode)/Li2SO4+Al2O3/(NiO-based composite cathode), air was developed and studied for production of ...A laboratory-scale intermediate-temperature H2S fuel cell with a configuration of H2S, (metal sulfide-based composite anode)/Li2SO4+Al2O3/(NiO-based composite cathode), air was developed and studied for production of power and for desulfurization of a fuel gas process stream. The cell was run at typical temperature (600—650℃) and ambient pressure, but its electrochemical performance may be limited by electrolyte membrane thickness. The membrane and its performance in cell have been characterized using scanning electron microscope (SEM) and electrochemical impedance spectrum (EIS) techniques. Composite anodes based on metal sulfides, Ag powder and electrolyte behaved well and stably in H2S stream, and composite cathodes based mainly on nickel oxide, Ag powder and electrolyte had superior per-formance to Pt catalyst. The maximum power density of up to 70mW?cm-2 and current density of as high as 250mA?cm-2 were obtained at 650℃. However, the long-term cell stability remains to be investigated.展开更多
Carbon-sulfur composites as the cathode of rechargeable Li-S batteries have shown outstanding electrochemical performance for high power devices. Here, we report the promising electrochemical charge-discharge properti...Carbon-sulfur composites as the cathode of rechargeable Li-S batteries have shown outstanding electrochemical performance for high power devices. Here, we report the promising electrochemical charge-discharge properties of a carbon-sulfur composite, in which sulfur is impregnated in porous hollow carbon spheres （PHCSs） via a melt-diffusion method. Instrumental analysis shows that the PHCSs, which were prepared by a facile template strategy, are characterized by high specific surface area （1520 m2.g 1）, large pore volume （2.61 cm^3·g^-1）, broad pore size distribution from micropores to mesopores, and high electronic conductivity （2.22 S·cm-1）. The carbon-sulfur composite with a sulfur content of 50.2 wt.% displays an initial discharge capacity of 1450 mA.h·g^-1 （which is 86.6% of the theoretical specific capacity） and a reversible discharge capacity of 1357 mA.h·g^-1 after 50 cycles at 0.05 C charge-discharge rate. At a higher rate of 0.5 C, the capacity stabilized at around 800 mA-h·g^-1 after 30 cycles. The results illustrate that the porous carbon-sulfur composites with hierarchically porous structure have potential application as the cathode of Li-S batteries because of their effective improvement of the electronic conductivity, the repression of the volume expansion, and the reduction of the shuttling loss.展开更多
Due to its high energy density,lithium-sulfur(Li-S)battery is considered as the most promising candidate for the energy storage systems,but its practical application is hindered by the dissolution of lithium polysulfi...Due to its high energy density,lithium-sulfur(Li-S)battery is considered as the most promising candidate for the energy storage systems,but its practical application is hindered by the dissolution of lithium polysulfides in the electrolyte.In this work,N-bromophthalimide(C8H4NO2Br,NBP),an aromatic molecule with carbophilic,sulfiphilic,lithiophilic,and solvophilic nature,is introduced into active graphene(AG)to fabricate the sulfur composite cathode.The carbophilic NBP is anchored readily on the AG surface viaπ−πstacking interaction.During discharging,the dissolved lithium polysulfide anion(LiS−n)is grafted into the sulfiphilic NBP spontaneously via SN2 substitution reaction to form C8H4NO2SnLi,which brings the dissolved LiS−n back to the AG surface in the composite cathode.Moreover,the lithiophilic and solvophilic nature of NBP improve the wettability of the porous composite cathode,and the electrolyte molecule is easily penetrated into the micro-mesopores of AG to facilitate the diffusion of the electrolyte.Thus,NBP,as a multi-functional compound in Li-S battery,can immobilize LiS−n and enhance the diffusion of the electrolyte.The above features of NBP endow the sulfur composite cathode with improved electrochemical performance in the cycling stability.展开更多
基金the Natural Science Foundation of Hunan Province,China(No.2020JJ1007).
文摘A systematic and green low-temperature sulfation roasting−water leaching strategy was put forward to achieve a very high fluorine removal rate of 97.82%for spent carbon cathode(SCC),which was believed as a hazardous solid waste.And the carbon could be recycled with a purity of 90.29 wt.%in the flaky microstructure.Thermodynamic analysis and the results of SEM,XRD and EDS indicate that most of the fluoride could convert into water-soluble sulfate at low temperature.And the highest fluorine removal rate could be obtained when<0.15 mm SCC particles were mixed with sulfuric acid at a liquid-to-solid ratio of 1:1,and then roasted at 300℃ for 0.5 h.The sulfate was removed to purify the carbon via water-leaching process.Avrami exponents and corresponding activation energy for the roasting and leaching process demonstrated that both processes are controlled by diffusion.
基金Project(U1602272)supported by the National Natural Science Foundation of China。
文摘To recover metal from copper slags,a new process involving two steps of oxidative desulfurization followed by smelting reduction was proposed in which one hazardous waste(waste cathode carbon)was used to treat another(copper slags).The waste cathode carbon is used not only as a reducing agent but also as a fluxing agent to decrease slag melting point.Upon holding for 60 min in air atmosphere first and then smelting with 14.4 wt%waste cathode carbon and 25 wt%CaO for 180 min in high purity Ar atmosphere at 1450℃,the recovery rates of Cu and Fe reach 95.89%and 94.64%,respectively,and meanwhile greater than 90%of the fluoride from waste cathode carbon is transferred into the final slag as CaF_(2) and Ca_(2)Si_(2)F_(2)O_(7),which makes the content of soluble F in the slag meet the national emission standard.Besides,the sulphur content in the obtained Fe-Cu alloy is low to 0.03 wt%.
基金Supported by the Natural Science Foundation of Guangdong Province (No. 05006552).
文摘A laboratory-scale intermediate-temperature H2S fuel cell with a configuration of H2S, (metal sulfide-based composite anode)/Li2SO4+Al2O3/(NiO-based composite cathode), air was developed and studied for production of power and for desulfurization of a fuel gas process stream. The cell was run at typical temperature (600—650℃) and ambient pressure, but its electrochemical performance may be limited by electrolyte membrane thickness. The membrane and its performance in cell have been characterized using scanning electron microscope (SEM) and electrochemical impedance spectrum (EIS) techniques. Composite anodes based on metal sulfides, Ag powder and electrolyte behaved well and stably in H2S stream, and composite cathodes based mainly on nickel oxide, Ag powder and electrolyte had superior per-formance to Pt catalyst. The maximum power density of up to 70mW?cm-2 and current density of as high as 250mA?cm-2 were obtained at 650℃. However, the long-term cell stability remains to be investigated.
文摘Carbon-sulfur composites as the cathode of rechargeable Li-S batteries have shown outstanding electrochemical performance for high power devices. Here, we report the promising electrochemical charge-discharge properties of a carbon-sulfur composite, in which sulfur is impregnated in porous hollow carbon spheres （PHCSs） via a melt-diffusion method. Instrumental analysis shows that the PHCSs, which were prepared by a facile template strategy, are characterized by high specific surface area （1520 m2.g 1）, large pore volume （2.61 cm^3·g^-1）, broad pore size distribution from micropores to mesopores, and high electronic conductivity （2.22 S·cm-1）. The carbon-sulfur composite with a sulfur content of 50.2 wt.% displays an initial discharge capacity of 1450 mA.h·g^-1 （which is 86.6% of the theoretical specific capacity） and a reversible discharge capacity of 1357 mA.h·g^-1 after 50 cycles at 0.05 C charge-discharge rate. At a higher rate of 0.5 C, the capacity stabilized at around 800 mA-h·g^-1 after 30 cycles. The results illustrate that the porous carbon-sulfur composites with hierarchically porous structure have potential application as the cathode of Li-S batteries because of their effective improvement of the electronic conductivity, the repression of the volume expansion, and the reduction of the shuttling loss.
基金financially supported by the National Natural Science Foundation of China (21573112, 21935006, 21421001 and 21373118)
文摘Due to its high energy density,lithium-sulfur(Li-S)battery is considered as the most promising candidate for the energy storage systems,but its practical application is hindered by the dissolution of lithium polysulfides in the electrolyte.In this work,N-bromophthalimide(C8H4NO2Br,NBP),an aromatic molecule with carbophilic,sulfiphilic,lithiophilic,and solvophilic nature,is introduced into active graphene(AG)to fabricate the sulfur composite cathode.The carbophilic NBP is anchored readily on the AG surface viaπ−πstacking interaction.During discharging,the dissolved lithium polysulfide anion(LiS−n)is grafted into the sulfiphilic NBP spontaneously via SN2 substitution reaction to form C8H4NO2SnLi,which brings the dissolved LiS−n back to the AG surface in the composite cathode.Moreover,the lithiophilic and solvophilic nature of NBP improve the wettability of the porous composite cathode,and the electrolyte molecule is easily penetrated into the micro-mesopores of AG to facilitate the diffusion of the electrolyte.Thus,NBP,as a multi-functional compound in Li-S battery,can immobilize LiS−n and enhance the diffusion of the electrolyte.The above features of NBP endow the sulfur composite cathode with improved electrochemical performance in the cycling stability.
