This paper describes the conductivity modifications induced by heavy ion implantation in pyrolysis products obtained by thermal treatment of polyacrylonitrile (PAN) thin films at temperatures of 435℃ (PAN435) and...This paper describes the conductivity modifications induced by heavy ion implantation in pyrolysis products obtained by thermal treatment of polyacrylonitrile (PAN) thin films at temperatures of 435℃ (PAN435) and 750℃ (PAN750) under vacuum. Ionic species having different chemical reactivities such as Kr, As, Cl. and F ions were utilized to allow interpretation of the conductivity' data either in terms of implantation induced molecular rearrangements or in terms of specific chemical doping effects. The temperature dependence of conductivity in the range between 25-3000C followed nearly a simple activation conduction relationship from which the temperature coefficients of resistivity (ct) were determined. In this temperature range, PAN750 provided the smallest α value compared with ion implanted PAN750 or with products obtained at the lower pyrolysis temperature. However. the corresponding lowest rate of conductivity change with temperatures (0.49%/℃) obtained in this study far exceeds the specification value required for thin film resistor applications (〈 0.1%/℃).展开更多
Surface tailoring of Pt-based nanocatalysts is an effective pathway to promote their electrocatalytic performance and multifunctionality.Here,we report two kinds of one-dimensional(1D)ultrafine PtCu nanowires(smooth s...Surface tailoring of Pt-based nanocatalysts is an effective pathway to promote their electrocatalytic performance and multifunctionality.Here,we report two kinds of one-dimensional(1D)ultrafine PtCu nanowires(smooth surface&rugged surface)synthesized via a wet chemical method and their distinct catalytic performances in electro-oxidation of alcohols.The alloyed PtCu nanowires having rough surfaces with atomic steps exhibit superior catalytic activity toward multiple electrochemical reactions compared with the smooth counterpart.Density functional theory simulations show the excellent reactivity of rugged PtCu na-nowires and attribute it to the surface synergetic Pt-Cu site which accounts for the promotion of water dissociation and the dehydrogenation of the carboxyl intermediate.The current study provides an insight into reasonable design of alloy nanocatalysts in energy-related electrocatalytic systems.展开更多
Introducing redox species into the electrolytes of traditional electric double layer capacitors(EDLCs)is an efficient strategy to enhance their energy density owing to Faradic reactions.However,few studies have elucid...Introducing redox species into the electrolytes of traditional electric double layer capacitors(EDLCs)is an efficient strategy to enhance their energy density owing to Faradic reactions.However,few studies have elucidated the effect of the molecular structures of organic redox species on the performance of relative supercapacitors,which is important in the development of redox additives for super-capacitors.In this context,we synthesized several viologens and used them as new organic redox additives for super-capacitors with organic electrolytes.The detailed experimental analysis and theoretical calculation results show that the electrochemical performance of viologens relies heavily on their side chains and conjugated cores.Specifically,the side chains of the viologens affect their electronic structures and are consistent with behaviours between the molecules and the electrode pores due to the size effect,thus influencing their specific capacities.In addition,a larger conjugated aromatic core endows viologens with a smaller band gap and a higher degree of electron delocalization,resulting in better rate performance and cycling stability.Consequently,aπ-conjugated viologen derivative is selected as a favourable additive and enables an EDLC-type supercapacitor to exhibit a high energy density(34.0 W h kg^−1 at 856 W kg^−1)and good cycling performance.展开更多
文摘This paper describes the conductivity modifications induced by heavy ion implantation in pyrolysis products obtained by thermal treatment of polyacrylonitrile (PAN) thin films at temperatures of 435℃ (PAN435) and 750℃ (PAN750) under vacuum. Ionic species having different chemical reactivities such as Kr, As, Cl. and F ions were utilized to allow interpretation of the conductivity' data either in terms of implantation induced molecular rearrangements or in terms of specific chemical doping effects. The temperature dependence of conductivity in the range between 25-3000C followed nearly a simple activation conduction relationship from which the temperature coefficients of resistivity (ct) were determined. In this temperature range, PAN750 provided the smallest α value compared with ion implanted PAN750 or with products obtained at the lower pyrolysis temperature. However. the corresponding lowest rate of conductivity change with temperatures (0.49%/℃) obtained in this study far exceeds the specification value required for thin film resistor applications (〈 0.1%/℃).
基金financial support from the National Natural Science Foundation of China(21571001,21631001U1532141)+2 种基金the Ministry of Education,and the Education Department of AnhuiSouthern University of Science and Technology(SUSTech),China(2020B121201002)the computational resource support from the Center for Computational Science and Engineering at SUSTech。
文摘Surface tailoring of Pt-based nanocatalysts is an effective pathway to promote their electrocatalytic performance and multifunctionality.Here,we report two kinds of one-dimensional(1D)ultrafine PtCu nanowires(smooth surface&rugged surface)synthesized via a wet chemical method and their distinct catalytic performances in electro-oxidation of alcohols.The alloyed PtCu nanowires having rough surfaces with atomic steps exhibit superior catalytic activity toward multiple electrochemical reactions compared with the smooth counterpart.Density functional theory simulations show the excellent reactivity of rugged PtCu na-nowires and attribute it to the surface synergetic Pt-Cu site which accounts for the promotion of water dissociation and the dehydrogenation of the carboxyl intermediate.The current study provides an insight into reasonable design of alloy nanocatalysts in energy-related electrocatalytic systems.
基金funding support from the Ministry of Science and Technology of China(2012CB933403)Beijing Natural Science Foundation(2182086)the National Natural Science Foundation of China(51425302 and 51302045)。
文摘Introducing redox species into the electrolytes of traditional electric double layer capacitors(EDLCs)is an efficient strategy to enhance their energy density owing to Faradic reactions.However,few studies have elucidated the effect of the molecular structures of organic redox species on the performance of relative supercapacitors,which is important in the development of redox additives for super-capacitors.In this context,we synthesized several viologens and used them as new organic redox additives for super-capacitors with organic electrolytes.The detailed experimental analysis and theoretical calculation results show that the electrochemical performance of viologens relies heavily on their side chains and conjugated cores.Specifically,the side chains of the viologens affect their electronic structures and are consistent with behaviours between the molecules and the electrode pores due to the size effect,thus influencing their specific capacities.In addition,a larger conjugated aromatic core endows viologens with a smaller band gap and a higher degree of electron delocalization,resulting in better rate performance and cycling stability.Consequently,aπ-conjugated viologen derivative is selected as a favourable additive and enables an EDLC-type supercapacitor to exhibit a high energy density(34.0 W h kg^−1 at 856 W kg^−1)and good cycling performance.