Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response me...Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response mechanisms of different nitrogen dopants at high frequencies are still unclear.In this study,melamine foam carbons with different configurations of surfacedoped N were formed by gradient carbonization,and the effects of the configurations on the high-frequency response behavior of the supercapacitors were analyzed.Using a combination of experiments and first-principle calculations,we found that pyrrolic N,characterized by a higher adsorption energy,increases the charge storage capacity of the electrode at high frequencies.On the other hand,graphitic N,with a lower adsorption energy,increases the speed of ion response.We propose the use of adsorption energy as a practical descriptor for electrode/electrolyte design in high-frequency applications,offering a more universal approach for improving the performance of N-doped carbon materials in supercapacitors.展开更多
近年来,人们对利用低温炭化工艺制备煤基无定形炭材料作为锂离子电池(LIBs)和钠离子电池(SIBs)的负极材料产生了兴趣。然而,煤衍生炭材料的炭化机制仍然不太清楚。因此,本文选取烟煤为原料,探究了煤炭到无定形炭材料的化学、微晶和孔隙...近年来,人们对利用低温炭化工艺制备煤基无定形炭材料作为锂离子电池(LIBs)和钠离子电池(SIBs)的负极材料产生了兴趣。然而,煤衍生炭材料的炭化机制仍然不太清楚。因此,本文选取烟煤为原料,探究了煤炭到无定形炭材料的化学、微晶和孔隙结构演变过程。随着温度的升高(低于1000℃),材料结构发生局部变化,碳层的迁移和小分子物质的释放导致了层间距(3.69-3.82A)和缺陷密度(1.26-1.90)逐渐增大,并且产生了丰富的纳米微孔结构。当温度升至1000~1600℃时,层间距和缺陷密度开始逐渐减小。在LIBs中,经1000℃炭化制备的样品表现出最佳的电化学性能。在0.1 C倍率测试下可逆容量达到384 mAh g^(-1),在5 C倍率下仍能保持170 mAh g^(-1),表现出优异的倍率性能。在SIBs中,经1200℃炭化制备的样品在0.1 C倍率测试下具有270.1 mAh g^(-1)的可逆容量和高达86.8%的首次库伦效率。本研究为煤基炭材料的精细化制备提供了理论支撑。展开更多
有序碳和无序碳都普遍被用作硅(Si)的复合材料。但是具有不同结晶度和孔结构的碳对硅基负极电化学性能的影响仍存在争议。本工作在严格控制碳含量和表面官能团的基础上,选择沥青(Pitch)和酚醛树脂(PR)作为有序碳和无序碳的前驱体,制备...有序碳和无序碳都普遍被用作硅(Si)的复合材料。但是具有不同结晶度和孔结构的碳对硅基负极电化学性能的影响仍存在争议。本工作在严格控制碳含量和表面官能团的基础上,选择沥青(Pitch)和酚醛树脂(PR)作为有序碳和无序碳的前驱体,制备了硅碳复合材料(Si@C)并系统地研究了其电化学行为。有序的晶体结构有利于复合物中的电子传输,中孔和大孔有利于锂离子的扩散。具有有序结构和小孔容的碳质涂层为Si的膨胀提供了很好的缓冲,电极在50次循环后仍保持结构完整性。然而,无序和多孔的结构降低了结构的稳定性并产生了很大的极化,这使得循环过程中体积不断膨胀,导致电化学性能较差。Si@C-Pitch在5 A g^(−1)下的容量是Si@C-PR的8倍,在0.5 A g^(−1)下100次循环后的容量保持率是Si@C-PR的1.9倍。该研究可为Si@C负极中炭材料的选择提供了理论指导。展开更多
锂硫电池作为高能量密度的二次电池存在硫的低导电性和多硫化物的穿梭效应等问题。通过制备高还原度的氧化石墨烯隔膜,并将其应用于锂硫电池。利用石墨烯片层形成的空间位阻和小介孔结构,可阻挡多硫化物的迁移以及其高导电性可减弱电池...锂硫电池作为高能量密度的二次电池存在硫的低导电性和多硫化物的穿梭效应等问题。通过制备高还原度的氧化石墨烯隔膜,并将其应用于锂硫电池。利用石墨烯片层形成的空间位阻和小介孔结构,可阻挡多硫化物的迁移以及其高导电性可减弱电池极化。在0.2 C下,采用高还原氧化石墨烯隔膜的锂硫电池初始比容量达到了1143.2 m Ah/g,经过100次循环后容量保持率为74.25%。此外,在2 C下仍有626.1 m Ah/g的比容量。表明高还原氧化石墨烯隔膜可以有效提升锂硫电池的电化学性能,体现出卓越的长循环稳定性和杰出的倍率性能。展开更多
Biomarkers in higher plants played an important role to estimate exposure effects of pollutants in soil ecosystem and have received increasing attention in recent years. The qualitative and quantitative modifications ...Biomarkers in higher plants played an important role to estimate exposure effects of pollutants in soil ecosystem and have received increasing attention in recent years. The qualitative and quantitative modifications arising in amplified fragment length polymorphism (AFLP) profiles as a measure of DNA effects were compared with a number of parameters, namely, the root length, total soluble protein content in root tips, chlorophylls content and shoot size to select the most sensitive biomarker responding to copper stress in the range of 0--600 mg/kg. The changes occurring in AFLP profiles of root tips following Cu treatment included loss of normal bands and appearance of new bands and variation in band intensity in comparison to that of the normal seedlings, A reduction in root length was observed at the 200 mg/kg of copper, which was accompanied with a decrease in total soluble protein content. According to their sensitivity to the copper toxicity, the above indicator rank in the following order: AFLP profiles 〉 total soluble protein content 〉 root length 〉 chlorophylls content 〉 shoot. We concluded that the AFLP offered a useful alternative hiomarker assay for the detection of genotoxic effects of environmental pollutants.展开更多
文摘Nitrogen doping has been widely used to improve the performance of carbon electrodes in supercapacitors,particularly in terms of their high-frequency response.However,the charge storage and electrolyte ion response mechanisms of different nitrogen dopants at high frequencies are still unclear.In this study,melamine foam carbons with different configurations of surfacedoped N were formed by gradient carbonization,and the effects of the configurations on the high-frequency response behavior of the supercapacitors were analyzed.Using a combination of experiments and first-principle calculations,we found that pyrrolic N,characterized by a higher adsorption energy,increases the charge storage capacity of the electrode at high frequencies.On the other hand,graphitic N,with a lower adsorption energy,increases the speed of ion response.We propose the use of adsorption energy as a practical descriptor for electrode/electrolyte design in high-frequency applications,offering a more universal approach for improving the performance of N-doped carbon materials in supercapacitors.
文摘近年来,人们对利用低温炭化工艺制备煤基无定形炭材料作为锂离子电池(LIBs)和钠离子电池(SIBs)的负极材料产生了兴趣。然而,煤衍生炭材料的炭化机制仍然不太清楚。因此,本文选取烟煤为原料,探究了煤炭到无定形炭材料的化学、微晶和孔隙结构演变过程。随着温度的升高(低于1000℃),材料结构发生局部变化,碳层的迁移和小分子物质的释放导致了层间距(3.69-3.82A)和缺陷密度(1.26-1.90)逐渐增大,并且产生了丰富的纳米微孔结构。当温度升至1000~1600℃时,层间距和缺陷密度开始逐渐减小。在LIBs中,经1000℃炭化制备的样品表现出最佳的电化学性能。在0.1 C倍率测试下可逆容量达到384 mAh g^(-1),在5 C倍率下仍能保持170 mAh g^(-1),表现出优异的倍率性能。在SIBs中,经1200℃炭化制备的样品在0.1 C倍率测试下具有270.1 mAh g^(-1)的可逆容量和高达86.8%的首次库伦效率。本研究为煤基炭材料的精细化制备提供了理论支撑。
文摘有序碳和无序碳都普遍被用作硅(Si)的复合材料。但是具有不同结晶度和孔结构的碳对硅基负极电化学性能的影响仍存在争议。本工作在严格控制碳含量和表面官能团的基础上,选择沥青(Pitch)和酚醛树脂(PR)作为有序碳和无序碳的前驱体,制备了硅碳复合材料(Si@C)并系统地研究了其电化学行为。有序的晶体结构有利于复合物中的电子传输,中孔和大孔有利于锂离子的扩散。具有有序结构和小孔容的碳质涂层为Si的膨胀提供了很好的缓冲,电极在50次循环后仍保持结构完整性。然而,无序和多孔的结构降低了结构的稳定性并产生了很大的极化,这使得循环过程中体积不断膨胀,导致电化学性能较差。Si@C-Pitch在5 A g^(−1)下的容量是Si@C-PR的8倍,在0.5 A g^(−1)下100次循环后的容量保持率是Si@C-PR的1.9倍。该研究可为Si@C负极中炭材料的选择提供了理论指导。
文摘锂硫电池作为高能量密度的二次电池存在硫的低导电性和多硫化物的穿梭效应等问题。通过制备高还原度的氧化石墨烯隔膜,并将其应用于锂硫电池。利用石墨烯片层形成的空间位阻和小介孔结构,可阻挡多硫化物的迁移以及其高导电性可减弱电池极化。在0.2 C下,采用高还原氧化石墨烯隔膜的锂硫电池初始比容量达到了1143.2 m Ah/g,经过100次循环后容量保持率为74.25%。此外,在2 C下仍有626.1 m Ah/g的比容量。表明高还原氧化石墨烯隔膜可以有效提升锂硫电池的电化学性能,体现出卓越的长循环稳定性和杰出的倍率性能。
基金The National Basic Research Program (973) of China (No. 2004CB418506) the National Natural Science Foundation of China(No. 20377043 20337010)
文摘Biomarkers in higher plants played an important role to estimate exposure effects of pollutants in soil ecosystem and have received increasing attention in recent years. The qualitative and quantitative modifications arising in amplified fragment length polymorphism (AFLP) profiles as a measure of DNA effects were compared with a number of parameters, namely, the root length, total soluble protein content in root tips, chlorophylls content and shoot size to select the most sensitive biomarker responding to copper stress in the range of 0--600 mg/kg. The changes occurring in AFLP profiles of root tips following Cu treatment included loss of normal bands and appearance of new bands and variation in band intensity in comparison to that of the normal seedlings, A reduction in root length was observed at the 200 mg/kg of copper, which was accompanied with a decrease in total soluble protein content. According to their sensitivity to the copper toxicity, the above indicator rank in the following order: AFLP profiles 〉 total soluble protein content 〉 root length 〉 chlorophylls content 〉 shoot. We concluded that the AFLP offered a useful alternative hiomarker assay for the detection of genotoxic effects of environmental pollutants.