An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) det...An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO-12v (GO applied to a negative potential of-1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode (GC/ERGO-0.8v) were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.展开更多
In this work, a two-step electrodeposition method was employed to prepare BiPO4 nanorod/reduced graphene oxide/FTO composite electrodes(BiPO4/r GO/FTO). The BiPO4/r GO/FTO composite electrode showed the higher photoel...In this work, a two-step electrodeposition method was employed to prepare BiPO4 nanorod/reduced graphene oxide/FTO composite electrodes(BiPO4/r GO/FTO). The BiPO4/r GO/FTO composite electrode showed the higher photoelectrocatalytic(PEC) activity for the removal of methyl orange than pure BiPO4, which was 2.8 times higher than that of BiPO4/FTO electrode. The effects of working voltage and BiPO4 deposition time on the degradation efficiency of methyl orange were investigated. The optimum BiPO4 deposition time was 45 min and the optimum working voltage was 1.2 V. The trapping experiments showed that hydroxyl radicals(·OH) and superoxide radicals(·O2-) were the major reactive species in PEC degradation process. The BiPO4/r GO/FTO composite electrode showed the high stability and its methyl orange removal efficiency remained unchanged after four testing cycles. The reasons for the enhanced PEC efficiency of the BiPO4/r GO/FTO composite electrode was ascribed to the broad visible-light absorption range, the rapid transmission of photogenerated charges, and the mixed BiPO4 phase by the introduction of r GO in the composite electrode films.展开更多
In this work,we initially synthesized Sb2S3 with uniform flower-like structures via a facile hydrothermal method through the modification of the Sb source and pH value.Afterward,Sb2S3 with a nanosheet structure was su...In this work,we initially synthesized Sb2S3 with uniform flower-like structures via a facile hydrothermal method through the modification of the Sb source and pH value.Afterward,Sb2S3 with a nanosheet structure was successfully synthesized on reduced graphene oxide(Sb2S3@RGO).The flower-like Sb2S3 and the Sb2S3@RGO nanosheets were tested as the counter electrode(CE)of dye-sensitized solar cells,and the latter exhibited a higher electrocatalytic property than the former owing to the introduction of graphene.The results from electrochemical tests indicated that the as-prepared Sb2S3@RGO nanosheets possess higher catalytic activity,charge-transfer ability,and electrochemical stability than Sb2S3,RGO,and Pt CEs.More notably,the power conversion efficiency of Sb2S3@RGO reached 8.17%,which was higher than that of the standard Pt CE(7.75%).展开更多
The development of highly efficient and costeffective oxygen evolution reaction(OER)electrocatalysts for renewable energy systems is vitally essential.Modulation of the electronic structure through heteroatom doping i...The development of highly efficient and costeffective oxygen evolution reaction(OER)electrocatalysts for renewable energy systems is vitally essential.Modulation of the electronic structure through heteroatom doping is considered as one of the most potential strategies to boost OER performances.Herein,a rational design of Mn-doped NiFe layered double hydroxide/reduced graphene oxide(Mn-NiFe LDH/rGO)is demonstrated by a facile hydrothermal approach,which exhibits outstanding OER activity and durability.Experimental results and density functional theory(DFT)calculations manifest that the introduction of Mn can reprogram the electronic structure of surface active sites and alter the intermediate adsorption energy,consequently reducing the potential limiting activation energy for OER.Specifically,the optimal Mn-NiFe LDH/rGO composite shows an enhanced OER performance with an ultralow overpotential of 240 mV@10 mA cm^(-2),Tafel slope of 40.0 mV dec^(-1) and excellent stability.Such superior OER activity is comparable to those of the recently reported state-of-the-art OER catalysts.This work presents an advanced strategy for designing electrocatalysts with high activity and low cost for energy conversion applications.展开更多
Although organic electrode materials have merits of abundant resources,diverse structures and environmental friendliness,their performance for electrochemical energy storage is far insufficient.In this work,a thiourea...Although organic electrode materials have merits of abundant resources,diverse structures and environmental friendliness,their performance for electrochemical energy storage is far insufficient.In this work,a thiourea-based polyimide/reduced graphene oxide(PNTCSA/RGO)composite was synthesized via a condensation polymerization method.As a cathode material in lithium-ion batteries,excellent performance is demonstrated with high reversible capacity(144.2 mA h g^−1),high discharge voltage(∼2.5 V),and long cycling life(over 2000 cycles at 500 mA g^−1),which are comparable to those of other well documented in organic electrodes.Encouraging electrochemical performance is also demonstrated for sodium ion batteries(a cycling life of 800 cycles at 500 mA g^−1),while poor performance is delivered in potassium ion batteries.Theoretical studies reveal that the active sites are carbonyl groups for all alkali ions but one inserted alkali metal ion is shared by two carbonyl groups from the two neighbor units.More importantly,K ions have stronger interaction with S atoms than Li/Na ions,which may lead to poor structure reversibility and account for the poor cycling performance.Our findings provide a fundamental understanding of polyimide based polymer electrodes and help to design and develop high performance organic electrode materials for alkali metal ion batteries.展开更多
High volumetric specific capacitance is essential for flexible supercapacitors.In this paper,a flexible composite electrode with ultrahigh volumetric specific capacitance and good rate performance is designed and prep...High volumetric specific capacitance is essential for flexible supercapacitors.In this paper,a flexible composite electrode with ultrahigh volumetric specific capacitance and good rate performance is designed and prepared.The film electrode is composed of non-porous compact polyaniline as the matrix and a small amount of reduced graphene oxide sheets as the conductive filler.The film is prepared by a newly developed solution casting method,where the casting solution is obtained by self-assembly of polyaniline and graphene oxide in a blended solution.A systematical investigation on the effect of reduced graphene oxide sheets reveals that they serve as both the conductive filler and the diffusion barrier.With the optimized reduced graphene oxide content,a large volumetric specific capacitance of 1354 F cm^−3 at 2.4 A cm^−3 is achieved,and good rate performance is also obtained because of the good ionic conductivity of polyaniline.This work provides a high performance electrode for flexible supercapacitors,and the solution casting method is also valuable in fabricating other organic electrode materials.展开更多
基金supported by the National Natural Science Foundation of China(21007033)the Fundamental Research Funds of Shandong University(2015JC017)~~
文摘An electrochemically reduced graphene oxide sample, ERGO_0.8v, was prepared by electrochemical reduction of graphene oxide (GO) at -0.8 V, which shows unique electrocatalytic activity toward tetracycline (TTC) detection compared to the ERGO-12v (GO applied to a negative potential of-1.2 V), GO, chemically reduced GO (CRGO)-modified glassy carbon electrode (GC) and bare GC electrodes. The redox peaks of TTC on an ERGO-0.8v-modifled glass carbon electrode (GC/ERGO-0.8v) were within 0-0.5 V in a pH 3.0 buffer solution with the oxidation peak current correlating well with TTC concentration over a wide range from 0.1 to 160 mg/L Physical characterizations with Fourier transform infrared (FT-IR), Raman, and X-ray photoelectron spectroscopies (XPS) demonstrated that the oxygen-containing functional groups on GO diminished after the electrochemical reduction at -0.8 V, yet still existed in large amounts, and the defect density changed as new sp2 domains were formed. These changes demonstrated that this adjustment in the number of oxygen-containing groups might be the main factor affecting the electrocatalytic behavior of ERGO. Additionally, the defect density and sp2 domains also exert a profound influence on this behavior. A possible mechanism for the TTC redox reaction at the GC/ERGO-0.8v electrode is also presented. This work suggests that the electrochemical reduction is an effective method to establish new catalytic activities of GO by setting appropriate parameters.
基金partly supported by the National Natural Science Foundations of China(21577132,21978276)the Fundamental Research Funds for the Central Universities(2652018326,2652018298,2652018297)the Beijing Municipal Education Commission Key Science and Technology Project Fund(KZ201910853043)~~
文摘In this work, a two-step electrodeposition method was employed to prepare BiPO4 nanorod/reduced graphene oxide/FTO composite electrodes(BiPO4/r GO/FTO). The BiPO4/r GO/FTO composite electrode showed the higher photoelectrocatalytic(PEC) activity for the removal of methyl orange than pure BiPO4, which was 2.8 times higher than that of BiPO4/FTO electrode. The effects of working voltage and BiPO4 deposition time on the degradation efficiency of methyl orange were investigated. The optimum BiPO4 deposition time was 45 min and the optimum working voltage was 1.2 V. The trapping experiments showed that hydroxyl radicals(·OH) and superoxide radicals(·O2-) were the major reactive species in PEC degradation process. The BiPO4/r GO/FTO composite electrode showed the high stability and its methyl orange removal efficiency remained unchanged after four testing cycles. The reasons for the enhanced PEC efficiency of the BiPO4/r GO/FTO composite electrode was ascribed to the broad visible-light absorption range, the rapid transmission of photogenerated charges, and the mixed BiPO4 phase by the introduction of r GO in the composite electrode films.
基金funded by the Tianjin science and technology support key projects(18YFZCSF00500)the National Science Fund for Distinguished Young Scholars(21425729)the National Natural Science Foundation of China
文摘In this work,we initially synthesized Sb2S3 with uniform flower-like structures via a facile hydrothermal method through the modification of the Sb source and pH value.Afterward,Sb2S3 with a nanosheet structure was successfully synthesized on reduced graphene oxide(Sb2S3@RGO).The flower-like Sb2S3 and the Sb2S3@RGO nanosheets were tested as the counter electrode(CE)of dye-sensitized solar cells,and the latter exhibited a higher electrocatalytic property than the former owing to the introduction of graphene.The results from electrochemical tests indicated that the as-prepared Sb2S3@RGO nanosheets possess higher catalytic activity,charge-transfer ability,and electrochemical stability than Sb2S3,RGO,and Pt CEs.More notably,the power conversion efficiency of Sb2S3@RGO reached 8.17%,which was higher than that of the standard Pt CE(7.75%).
基金the National Natural Science Foundation of China(51902003 and 21771003)Anhui Province Natural Science Foundation(2008085QB53)the Natural Science Research Project of Anhui Province Education Department(KJ2019A0581)。
文摘The development of highly efficient and costeffective oxygen evolution reaction(OER)electrocatalysts for renewable energy systems is vitally essential.Modulation of the electronic structure through heteroatom doping is considered as one of the most potential strategies to boost OER performances.Herein,a rational design of Mn-doped NiFe layered double hydroxide/reduced graphene oxide(Mn-NiFe LDH/rGO)is demonstrated by a facile hydrothermal approach,which exhibits outstanding OER activity and durability.Experimental results and density functional theory(DFT)calculations manifest that the introduction of Mn can reprogram the electronic structure of surface active sites and alter the intermediate adsorption energy,consequently reducing the potential limiting activation energy for OER.Specifically,the optimal Mn-NiFe LDH/rGO composite shows an enhanced OER performance with an ultralow overpotential of 240 mV@10 mA cm^(-2),Tafel slope of 40.0 mV dec^(-1) and excellent stability.Such superior OER activity is comparable to those of the recently reported state-of-the-art OER catalysts.This work presents an advanced strategy for designing electrocatalysts with high activity and low cost for energy conversion applications.
基金This work was financially supported by the National Natural Science Foundation of China(51672188 and 21703036).
文摘Although organic electrode materials have merits of abundant resources,diverse structures and environmental friendliness,their performance for electrochemical energy storage is far insufficient.In this work,a thiourea-based polyimide/reduced graphene oxide(PNTCSA/RGO)composite was synthesized via a condensation polymerization method.As a cathode material in lithium-ion batteries,excellent performance is demonstrated with high reversible capacity(144.2 mA h g^−1),high discharge voltage(∼2.5 V),and long cycling life(over 2000 cycles at 500 mA g^−1),which are comparable to those of other well documented in organic electrodes.Encouraging electrochemical performance is also demonstrated for sodium ion batteries(a cycling life of 800 cycles at 500 mA g^−1),while poor performance is delivered in potassium ion batteries.Theoretical studies reveal that the active sites are carbonyl groups for all alkali ions but one inserted alkali metal ion is shared by two carbonyl groups from the two neighbor units.More importantly,K ions have stronger interaction with S atoms than Li/Na ions,which may lead to poor structure reversibility and account for the poor cycling performance.Our findings provide a fundamental understanding of polyimide based polymer electrodes and help to design and develop high performance organic electrode materials for alkali metal ion batteries.
基金financially supported by the National Natural Science Foundation of China (21774104 and 21975210)the Natural Science Foundation of Fujian Province (2018J06015)
文摘High volumetric specific capacitance is essential for flexible supercapacitors.In this paper,a flexible composite electrode with ultrahigh volumetric specific capacitance and good rate performance is designed and prepared.The film electrode is composed of non-porous compact polyaniline as the matrix and a small amount of reduced graphene oxide sheets as the conductive filler.The film is prepared by a newly developed solution casting method,where the casting solution is obtained by self-assembly of polyaniline and graphene oxide in a blended solution.A systematical investigation on the effect of reduced graphene oxide sheets reveals that they serve as both the conductive filler and the diffusion barrier.With the optimized reduced graphene oxide content,a large volumetric specific capacitance of 1354 F cm^−3 at 2.4 A cm^−3 is achieved,and good rate performance is also obtained because of the good ionic conductivity of polyaniline.This work provides a high performance electrode for flexible supercapacitors,and the solution casting method is also valuable in fabricating other organic electrode materials.