A novel C/Pb composite has been successfully prepared by electmless plating to reduce the hydrogenevolution and achieve the high reversibility of the anode of lead-carbon battery (LCB). The depositedlead on the surf...A novel C/Pb composite has been successfully prepared by electmless plating to reduce the hydrogenevolution and achieve the high reversibility of the anode of lead-carbon battery (LCB). The depositedlead on the surface of C/Pb composite was found to be uniform and adherent to carbon surface. Becauselead has been stuck on the surface of C/Pb composite, the embedded structure suppresses the hydrogenevolution of lead-carbon anode and strengthens the connection between carbon additive and sponge lead.Compared with the blank anode, the lead-carbon anode with C/Pb composite displays excellent charge-discharge reversibility, which is attributed to the good connection between carbon additives and leadthat has been stuck on the surface of C/Pb composite during the preparation process. The addition of CIPb composite maintains a solid anode structure with high specific surface area and power volume, andthereby, it plays a significant role in the highly reversible lead-carbon anode.展开更多
Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs...Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.展开更多
Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,t...Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core structure.This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of duration.This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction.Consequently,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be promoted.This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.展开更多
In order to understand the effect of powders ground from reactive sandstone replacing cement on reducing or suppressing alkali-silica reaction(ASR), and to identify the mechanism of suppressing ASR by this powders, ...In order to understand the effect of powders ground from reactive sandstone replacing cement on reducing or suppressing alkali-silica reaction(ASR), and to identify the mechanism of suppressing ASR by this powders, mortar and paste containing reactive sandstone powders of four replacement levels ranging from 10wt% to 40wt% and four specific surfaces areas ranging from 210 m^2/kg to 860 m^2/kg were studied. The experimental results showed that incorporation of 40wt% reactive sandstone powders could suppress ASR effectively except for mortar containing reactive sandstone powders with specific surface area of 610 m^2/kg, which disagreed with the most results reported that the higher reactive powder specific surface area, the smaller ASR expansion. By means of fl ame photometry, Fourier transform infrared spectroscopy(FT-IR) and thermo gravimetric analysis(TG), the mechanism of reactive sandstone powders on reducing or suppressing ASR was soluble alkalis type of reactive sandstone powders and the competition of liberating and bonding alkali of cement paste containing reactive sandstone powders,when the ability of alkali bonding was greater than the ability of alkali liberation, ASR caused by reactive sandstone was supressed effectively.展开更多
A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel...A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel carbon-sulfur nano-composite were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) and X-ray diffraction (XRD). The electrochemical performances of nano-composite were characterized by charge-discharge characteristic, cyclic voltammetry and electrochemical impendence spectroscopy (EIS). The experimental results indicate that the electrochemical capability of nano- composite material was superior to that of traditional S-containing composite material. The cathode made by carbon-sulfur nano-composite material shows a good cycle ability and a high specific charge-discharge capacity. The HSAAC shows a vital role in adsorbing sublimed sulfur and the polysulfides within the cathode and is an excellent electric conductor for a sulfur cathode and prevents the shuttle behavior of the lithium-sulfur battery.展开更多
Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating su...Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) in certain conditions. Equivalent circuits were used to fit the spectra at different discharge states. The variations of impedance spectra, charge-transfer resistance and double layer capacitance were discussed. The changes of EIS with potential were analyzed based on a plausible electrical equivalent circuit model, and some parameters were measured and analyzed about electrochemical performance and state of charge and discharge of the electrode. The good accuracy in fitting values of the model to the experimental data indicates that the mathematical model gives out a satisfying description upon the mechanism of high rate of capacity fade in lithium-sulfur battery.展开更多
The chemical compositions of the sludge after treatment are tested by fully chemical analysis techniques. Its crystalline phase structure changes of the sludge calcined at different temperature are characterized by XR...The chemical compositions of the sludge after treatment are tested by fully chemical analysis techniques. Its crystalline phase structure changes of the sludge calcined at different temperature are characterized by XRD method. Nitrogen gas isothermal adsorption method (77 K) is applied to measure the influences of ammonium bicarbonate on specific surface area and pore structure of activated alumina synthesized from waste aluminum sludge. The result shows that the amount of Al2O3 in the sludge accounts for more than 94%, and Na2Owt% in a 0.1-0.2% range. By calcining raw sludge at 600℃, monophase γ-Al2O3 is obtained. And this can satisfy the performance requirements of activated alumina adsorbent. The specific surface area of the specimen with NH4HCO3 added has expanded from 179 to 249 m^2/g and the pore volume from 0.25 to 1.11 cm^3/g as well as the average pore diameter from 5.6 to 17.8 nm. All these show that NH4HCO3 is an effective pore-expansion agent to remarkably improve the structure and performance of activated alumina synthesized from waste aluminum sludge.展开更多
Rigorous assessment of heterogeneous electrocatalysts for electrochemical water splitting has been a critical issue mainly due to insufficient standard protocols to measure and report experimental data.In this perspec...Rigorous assessment of heterogeneous electrocatalysts for electrochemical water splitting has been a critical issue mainly due to insufficient standard protocols to measure and report experimental data.In this perspective,we highlight some common pitfalls when measuring and reporting electrocatalytic data,which should be avoided to ensure the accuracy and reproducibility and to advance the water splitting field.We advocate to prevent the introduction of artefacts from the counter and reference electrodes,as well as the impurities in the electrolyte when conducting electrocatalyst activity measurements.In addition,we encourage the use of the electrochemically active surface area(ECSA)-normalized current densities to represent the intrinsic activity of the reported catalysts for a better comparison with previously known materials.Suitable ECSA measurement methods should be employed based on the nature of catalysts.Recommendations made in this perspective will hopefully assist in identifying advanced catalysts for water splitting research.展开更多
In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, us...In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO2 activation and Potassium hydroxide(KOH) activation. CO2 adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO2 concentration range of10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N2 and CO2 adsorption at 77 and 273 K, respectively.Central composite design was used to evaluate the combined effects of temperature and concentration of CO2 on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm3/g and surface area of 1400 m2/g had the highest CO2 adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO2 and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO2 activated carbons remained remarkably stable after50 cycles with low temperature(160°C) regeneration.展开更多
基金the financial support provided by the National Natural Science Foundation of China (No.21573093)the National Key Research and Development Program (No.2017YFB0307501)Guangdong Innovative and Entrepreneurial Research Team Program (No.2013C092)
文摘A novel C/Pb composite has been successfully prepared by electmless plating to reduce the hydrogenevolution and achieve the high reversibility of the anode of lead-carbon battery (LCB). The depositedlead on the surface of C/Pb composite was found to be uniform and adherent to carbon surface. Becauselead has been stuck on the surface of C/Pb composite, the embedded structure suppresses the hydrogenevolution of lead-carbon anode and strengthens the connection between carbon additive and sponge lead.Compared with the blank anode, the lead-carbon anode with C/Pb composite displays excellent charge-discharge reversibility, which is attributed to the good connection between carbon additives and leadthat has been stuck on the surface of C/Pb composite during the preparation process. The addition of CIPb composite maintains a solid anode structure with high specific surface area and power volume, andthereby, it plays a significant role in the highly reversible lead-carbon anode.
基金supported by the National Natural Science Foundation of China(Nos.51872157,52072208)Shenzhen Technical Plan Project(JCYJ20170817161753629)+1 种基金Fundamental Research Project of Shenzhen(No.JCYJ20190808153609561)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01N111).
文摘Nickel-rich LiNi_(1-x-y)Co_(x)Mn_(y)O_(2)(NCM,1-x-y≥0.6)is known as a promising cathode material for lithium-ion batteries since its superiority of high voltage and large capacity.However,polycrystalline Ni-rich NCMs suffer from poor cycle stability,limiting its further application.Herein,single crystal and polycrystalline LiNi_(0.84)Co_(0.07)Mn_(0.09)O_(2)cathode materials are compared to figure out the relation of the morphology and the electrochemical storage performance.According to the Li^(+)diffusion coefficient,the lower capacity of single crystal samples is mainly ascribed to the limited Li+diffusion in the large bulk.In situ XRD illustrates that the polycrystalline and single crystal NCMs show a virtually identical manner and magnitude in lattice contraction and expansion during cycling.Also,the electrochemically active surface area(ECSA)measurement is employed in lithium-ion battery study for the first time,and these two cathodes show huge discrepancy in the ECSA after the initial cycle.These results suggest that the single crystal sample exhibits reduced cracking,surface side reaction,and Ni/Li mixing but suffers the lower Li^(+)diffusion kinetics.This work offers a view of how the morphology of Ni-rich NCM effects the electrochemical performance,which is instructive for developing a promising strategy to achieve good rate performance and excellent cycling stability.
基金the financial support of the Training Program of the Major Research Plan of the National Natural Science Foundation of China(92061124)the National Natural Science Foundation of China(21975292,21978331,22068008,and 52101186)+3 种基金the Guangdong Basic and Applied Basic Research Foundation(2021A1515010167 and 2022A1515011196)the Guangzhou Key R&D Program/Plan Unveiled Flagship Project(20220602JBGS02)the Guangzhou Basic and Applied Basic Research Project(202201011449)the Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202220 and FC202216)。
文摘Colloidal synthesis of metal nanoclusters will inevitably lead to the blockage of catalytically active sites by organic ligands.Here,taking[Au_(25)(PET)_(18)]-(PET=2-phenylethanethiol)nanocluster as a model catalyst,this work reports a feasible procedure to achieve the controllably partial removal of thiolate ligands from unsupported[Au_(25)(PET)_(18)]-nanoclusters with the preservation of the core structure.This procedure shortens the processing duration by rapid heating and cooling on the basis of traditional annealing treatment,avoiding the reconfiguration or agglomeration of Au_(25)nanoclusters,where the degree of dethiolation can be regulated by the control of duration.This work finds that a moderate degree of dethiolation can expose the Au active sites while maintaining the suppression of the competing hydrogen evolution reaction.Consequently,the activity and selectivity towards CO formation in electrochemical CO_(2)reduction reaction of Au_(25)nanoclusters can be promoted.This work provides a new approach for the removal of thiolate ligands from atomically precise gold nanoclusters.
基金Funded partly by the the National 973 Program of China(No.2013CB035901)the National Natural Science Foundation of China(No.51379163)
文摘In order to understand the effect of powders ground from reactive sandstone replacing cement on reducing or suppressing alkali-silica reaction(ASR), and to identify the mechanism of suppressing ASR by this powders, mortar and paste containing reactive sandstone powders of four replacement levels ranging from 10wt% to 40wt% and four specific surfaces areas ranging from 210 m^2/kg to 860 m^2/kg were studied. The experimental results showed that incorporation of 40wt% reactive sandstone powders could suppress ASR effectively except for mortar containing reactive sandstone powders with specific surface area of 610 m^2/kg, which disagreed with the most results reported that the higher reactive powder specific surface area, the smaller ASR expansion. By means of fl ame photometry, Fourier transform infrared spectroscopy(FT-IR) and thermo gravimetric analysis(TG), the mechanism of reactive sandstone powders on reducing or suppressing ASR was soluble alkalis type of reactive sandstone powders and the competition of liberating and bonding alkali of cement paste containing reactive sandstone powders,when the ability of alkali bonding was greater than the ability of alkali liberation, ASR caused by reactive sandstone was supressed effectively.
基金the Science and Technique Key Foundation of Guangdong Province(No.2003A1100101,2003C105006)
文摘A novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) under certain conditions. The physical and chemical per- formances of the novel carbon-sulfur nano-composite were characterized by scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) and X-ray diffraction (XRD). The electrochemical performances of nano-composite were characterized by charge-discharge characteristic, cyclic voltammetry and electrochemical impendence spectroscopy (EIS). The experimental results indicate that the electrochemical capability of nano- composite material was superior to that of traditional S-containing composite material. The cathode made by carbon-sulfur nano-composite material shows a good cycle ability and a high specific charge-discharge capacity. The HSAAC shows a vital role in adsorbing sublimed sulfur and the polysulfides within the cathode and is an excellent electric conductor for a sulfur cathode and prevents the shuttle behavior of the lithium-sulfur battery.
文摘Carbon-sulfur nano-composite cathodes for lithium rechargeable batteries were investigated by electrochemical impedance spectroscopy (EIS). The novel carbon-sulfur nano-composite material was synthesized by heating sublimed sulfur and high surface area activated carbon (HSAAC) in certain conditions. Equivalent circuits were used to fit the spectra at different discharge states. The variations of impedance spectra, charge-transfer resistance and double layer capacitance were discussed. The changes of EIS with potential were analyzed based on a plausible electrical equivalent circuit model, and some parameters were measured and analyzed about electrochemical performance and state of charge and discharge of the electrode. The good accuracy in fitting values of the model to the experimental data indicates that the mathematical model gives out a satisfying description upon the mechanism of high rate of capacity fade in lithium-sulfur battery.
文摘The chemical compositions of the sludge after treatment are tested by fully chemical analysis techniques. Its crystalline phase structure changes of the sludge calcined at different temperature are characterized by XRD method. Nitrogen gas isothermal adsorption method (77 K) is applied to measure the influences of ammonium bicarbonate on specific surface area and pore structure of activated alumina synthesized from waste aluminum sludge. The result shows that the amount of Al2O3 in the sludge accounts for more than 94%, and Na2Owt% in a 0.1-0.2% range. By calcining raw sludge at 600℃, monophase γ-Al2O3 is obtained. And this can satisfy the performance requirements of activated alumina adsorbent. The specific surface area of the specimen with NH4HCO3 added has expanded from 179 to 249 m^2/g and the pore volume from 0.25 to 1.11 cm^3/g as well as the average pore diameter from 5.6 to 17.8 nm. All these show that NH4HCO3 is an effective pore-expansion agent to remarkably improve the structure and performance of activated alumina synthesized from waste aluminum sludge.
基金the Fund of the Australian Renewable Energy Agency(ARENA)and the Fund of the Australian Research Council(No.FT170100224)。
文摘Rigorous assessment of heterogeneous electrocatalysts for electrochemical water splitting has been a critical issue mainly due to insufficient standard protocols to measure and report experimental data.In this perspective,we highlight some common pitfalls when measuring and reporting electrocatalytic data,which should be avoided to ensure the accuracy and reproducibility and to advance the water splitting field.We advocate to prevent the introduction of artefacts from the counter and reference electrodes,as well as the impurities in the electrolyte when conducting electrocatalyst activity measurements.In addition,we encourage the use of the electrochemically active surface area(ECSA)-normalized current densities to represent the intrinsic activity of the reported catalysts for a better comparison with previously known materials.Suitable ECSA measurement methods should be employed based on the nature of catalysts.Recommendations made in this perspective will hopefully assist in identifying advanced catalysts for water splitting research.
基金Funding for this research is provided by Natural Sciences and Engineering Research Council (NSERC) of Canada
文摘In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO2 activation and Potassium hydroxide(KOH) activation. CO2 adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO2 concentration range of10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N2 and CO2 adsorption at 77 and 273 K, respectively.Central composite design was used to evaluate the combined effects of temperature and concentration of CO2 on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm3/g and surface area of 1400 m2/g had the highest CO2 adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO2 and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO2 activated carbons remained remarkably stable after50 cycles with low temperature(160°C) regeneration.