Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and ...Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and high performance electrochemical oxidation system for wastewater treatment,granular active carbon(GAC) was decorated by doping Ce,Sn,Sb to synthesize Sn-Sb-Ce/GAC using sol-gel method as particle electrode filled into a three-dimensional(3D) electrochemical reactor.Scanning electron microscopy(SEM),energy-dispersive spectroscopy(EDS) and X-ray diffraction(XRD) experiments revealed that the Sn-Sb-Ce/GAC particle electrode crystal particles were compact and uniform,and the surface structure was improved.The ten cyclic experiments indicated that the Sn-Sb-Ce/GAC particle electrode had high stability and low dissolution of the loaded active substance.The degradation mechanism of MIT was studied under the optimal working conditions of 3D electrode system with GAC of 5 g/L,current density of 20 mA/cm^(2),initial pH 5,electrolyte concentration of Na_(2)SO_(4)0.02 mol/L and reaction time of 120 min.The indirect electrochemical degradation of MIT was dominated by active substance pathway that active chlorine rather than free radicals(·OH) played the main role.Comparing with conventional two-dimensional(2D) electrode system,the 3D electrochemical system has larger active electrode area,higher treatment efficiency and lower energy consumption than the former.The 3D electrochemical system could remove 96.5% of MIT from the actual high-salt reverse osmosis concentrate wastewater in 30 min.It has a certain removal effect on UV_(254)in wastewater,but has a better removal effect on fluorescent substances.This study proposed a new strategy to develop transition metal and rare earth metal particle electrodes using carbon-based materials for high efficient electrocatalytic oxidation in the electrochemical treatment system.展开更多
Unmanaged wood waste,particularly in countries like Nepal,presents serious environmental concerns due to open burning and improper disposal,leading to carbon emissions,air pollution and land degradation.This study int...Unmanaged wood waste,particularly in countries like Nepal,presents serious environmental concerns due to open burning and improper disposal,leading to carbon emissions,air pollution and land degradation.This study introduces an environmentally sustainable strategy to upcycle Toona ciliata wood scrap—an abundant and underutilized lignocellulosic biomass—into high performance carbon electrodes for green energy storage applications.Activated carbon(TCWAC)was synthesized via single-step pyrolytic carbonization followed by phosphoric acid activation,yielding a material with high specific surface area,hierarchical porosity,and excellent electrical conductivity.Electrochemical measurements using a three-electrode configuration in 6 M KOH revealed optimized potential windows of -1.0 to -0.2 V(TCWAC),-1.2 to 0 V(TCWAC-Mn),and -1.15 to -0.4 V(TCWAC-Fe).TCWAC exhibited a specific capacitance of 156.3 Fg^(-1)at 1 Ag^(-1),with an energy density of 3.5 Whkg^(-1),and 80.2% capacity retention after 1000 charge-discharge cycles.Composites with MnO_(2)and Fe_(2)O_(3)were also evaluated.TWAC-Mn delivered 489.4 Fg^(-1),25.1 Whkg^(-1),and 99.1% retention,whereas,TWAC-Fe achieved 321.3 Fg^(-1),6.3 Whkg^(-1),and 90.3% retention.The superior performance of MnO_(2)is attributed to its multiple oxidation states,facilitating reversible faradaic redox and enhanced pseudocapacitance.This work offers the first direct,systematic comparison of MnO_(2)and Fe_(2)O_(3)composites on a common biomass-carbon matrix under identical synthesis and testing conditions.The finding provides mechanistic insight into charge storage behaviour and demonstrate a scalable route for converting biomass waste into sustainable electrode materials,contributing to cleaner energy solutions and improved biomass valorization.展开更多
Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evo...Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evolution, and damage mechanics to simulate the growth of central cracks in cathode particles（Li Mn_2 O_4） by an extended finite element method by considering the influence of multiple factors. The simulation shows that particles are likely to crack at a high discharge rate, when the particle radius is large, or when the initial central crack is longer. It also shows that the maximum principal tensile stress decreases and cracking becomes more difficult when the influence of crack surface diffusion is considered. The fracturing process occurs according to the following stages： no crack growth, stable crack growth, and unstable crack growth. Changing the charge/discharge strategy before unstable crack growth sets in is beneficial to prevent further capacity fading during electrochemical cycling.展开更多
The metal vapor synthesis (MVS) methed was used to prepare activatedcarbon supported nickel electrode. The electrocatalytic activity of the electrode forhydrogen evolution reaction(HGR) in alkaline solution was studie...The metal vapor synthesis (MVS) methed was used to prepare activatedcarbon supported nickel electrode. The electrocatalytic activity of the electrode forhydrogen evolution reaction(HGR) in alkaline solution was studied. Cathodicpolarization curves showed the electrocatalytic activity of Ni/C electrode prepared byMVS method was higher than that of the one prepared by conventional method.展开更多
In this paper,the functional polymeric active materials were prepared by the grafting copolymerization and their structure and properties were studied.The results show that the structure and properties of these ac- ti...In this paper,the functional polymeric active materials were prepared by the grafting copolymerization and their structure and properties were studied.The results show that the structure and properties of these ac- tive materials have the relative large effects on the properties of gadolinium ion selective electrodes.展开更多
The activated nitrogen-enriched novel carbons (NENCs) were prepared by direct carbonization using polyaniline coating activated mesocarbon microbead composites as the precursor. Herein the influences of the carbonizat...The activated nitrogen-enriched novel carbons (NENCs) were prepared by direct carbonization using polyaniline coating activated mesocarbon microbead composites as the precursor. Herein the influences of the carbonization temperature on the structure and morphology of the NENCs samples were investigated by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N2 adsorption/desorption isotherm at 77 K. The electrochemical properties of the supercapacitors were characterized by cyclic voltammetry, galvanostatic charge/discharge, electrochemical impedance spectroscopy (EIS), cycle life, leakage current and self-discharge measurements in 6 mol/L KOH solution. The results demonstrate that the NENC samples carbonized at 600 °C show the highest specific capacitance of 385 F/g at the current density of 1 A/g and the lowest ESR value (only 0.93?). Furthermore, the capacity retention ratio of the NENCs-600 supercapacitor is 92.8 % over 2500 cycles.展开更多
Polyvinyl alcohol （PVA）-sodium polyacrylate （PAAS）-KOH-H2O alkaline polymer electrolyte film with high ionic conductivity was prepared by a solution-casting method. Polymer Ni（OH）2/activated carbon （AC） hybrid...Polyvinyl alcohol （PVA）-sodium polyacrylate （PAAS）-KOH-H2O alkaline polymer electrolyte film with high ionic conductivity was prepared by a solution-casting method. Polymer Ni（OH）2/activated carbon （AC） hybrid supercapacitors with different electrode active material mass ratios （positive to negative） were fabricated using this alkaline polymer electrolyte, nickel hydroxide positive electrodes, and AC negative electrodes. Galvanostatic charge/ discharge and electrochemical impedance spectroscopy （EIS） methods were used to study the electrochemical performance of the capacitors, such as charge/discharge specific capacitance, rate charge/discharge ability, and charge/discharge cyclic stability. Experimental results showed that with the decreasing of active material mass ratio m（Ni（OH）2）/m（AC）, the charge/discharge specific capacitance increases, but the rate charge/discharge ability and the charge/discharge cyclic stability decrease.展开更多
Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase p...Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase purity and crystalline size of the synthesized materials were ascertained by using powder X-ray diffraction.The shape and morphology of synthesized materials were characterized by field-emission scanning electron microscopy（FE-SEM） and high resolution transmission electron microscopy（HR-TEM）.The electrocatalytic activity of α-Mo2 C for I-/I3^-redox couple was investigated by the cyclic voltammetry.The synthesized α-Mo2 C was subsequently applied as counter electrode in dye-sensitized solar cells to replace the expensive platinum.展开更多
Sodium-ion capacitors(NICs)trigger considerable attention due to their higher specific energy than electrical double-layer capacitors(EDLCs)at comparable specific power.However,the presodiation process of the anodic h...Sodium-ion capacitors(NICs)trigger considerable attention due to their higher specific energy than electrical double-layer capacitors(EDLCs)at comparable specific power.However,the presodiation process of the anodic host is extremely crucial for the construction of high-performance NICs.Herein,a positive EDL electrode containing activated carbon(AC)mixed with sodium cyanide(NaCN)as a sacrificial material was electrochemically oxidized to presodiate a Sn_(4)P_(3) anodic host buffered by hard carbon(HC).The oxidation of CN-occurred ca.2.9 V vs.Na/Na+and finished by a short region of linearly increasing potential with a total capacity close to the theoretical value of 547 mAh g^(-1).The operando electrochemical mass spectrometry(EMS)analysis of the atmosphere in the cell together with the internal pressure measurements realized during the galvanostatic oxidation of a YP80F-NaCN electrode demonstrate that the process occurs without any gas evolution.A precursor cell of an NIC was constructed in a pouch with YP80FNaCN and HC/Sn_(4)P_(3) electrodes.After the oxidative sodium transfer from NaCN to HC/Sn_(4)P_(3),the realized YP80F//Nax(HC/Sn_(4)P_(3))NIC demonstrated a discharge capacitance retention higher than 80%for 8900 cycles in the voltage range from 2.0 to 3.8 V.The infrared analysis of the anode obtained by the herein described transfer process detected polycyanogen,which stabilizes the electrode structure during cycling,and thereof is at the origin of the enhanced life span of the NIC.展开更多
Click chemistry is a rapid,reliable,and powerful function and a highly selective organic reaction that facilitates the efficient synthesis of various molecules by joining small units.This approach has found widespread...Click chemistry is a rapid,reliable,and powerful function and a highly selective organic reaction that facilitates the efficient synthesis of various molecules by joining small units.This approach has found widespread applications in fields such as drug development,chemical synthesis,and molecular biology.In recent years,the reaction of alkali-catalyzed polymerization of thiol and sulfur has been employed to prepare various sulfur-containing polymers,which are applied as electrochemical active electrode materials in the pursuit of good performance.In this study,it is surprising to find that the reaction mechanism exhibits characteristics of both the alkali-catalyzed sulfhydryl Micheal addition reaction and thiol-epoxy click chemistry;for the first time,thiol-sulfur click chemistry is defined in detail,providing a comprehensive description of its underlying scientific principles.The introduction of this new reaction pathway holds significant potential for advancing research and the development of sulfur-containing polymers.Based on this novel click chemistry,a new sulfur-containing polymer,polydivinylthioether hexasulfide,has been designed and successfully applied as a cathode material in lithium-organosulfide batteries.This material demonstrates excellent electrochemical performance,achieving an initial capacity that reaches 790.5 mAh g−1(82.6%of theoretical capacity),and in a long-term cycle test,the capacity decay rate is only 0.063%after 1,000 cycles.展开更多
基金the financial supports from Major Science and Technology project of China Power Engineering Consulting Group Co., Ltd. "Research on Green and digital Intelligent Technology of Sewage Treatment Plant" (No. CEEC2023-ZDYF-09)Technology Innovation Ability Improvement Project of Shandong Province, China (No. 2022TSGC1247)。
文摘Advanced oxidation processes are promising for degradation of the highly chemical stability and refractory methylisothiazolinone(MIT) bactericides in relevant industrial wastewater.In order to assemble a low cost and high performance electrochemical oxidation system for wastewater treatment,granular active carbon(GAC) was decorated by doping Ce,Sn,Sb to synthesize Sn-Sb-Ce/GAC using sol-gel method as particle electrode filled into a three-dimensional(3D) electrochemical reactor.Scanning electron microscopy(SEM),energy-dispersive spectroscopy(EDS) and X-ray diffraction(XRD) experiments revealed that the Sn-Sb-Ce/GAC particle electrode crystal particles were compact and uniform,and the surface structure was improved.The ten cyclic experiments indicated that the Sn-Sb-Ce/GAC particle electrode had high stability and low dissolution of the loaded active substance.The degradation mechanism of MIT was studied under the optimal working conditions of 3D electrode system with GAC of 5 g/L,current density of 20 mA/cm^(2),initial pH 5,electrolyte concentration of Na_(2)SO_(4)0.02 mol/L and reaction time of 120 min.The indirect electrochemical degradation of MIT was dominated by active substance pathway that active chlorine rather than free radicals(·OH) played the main role.Comparing with conventional two-dimensional(2D) electrode system,the 3D electrochemical system has larger active electrode area,higher treatment efficiency and lower energy consumption than the former.The 3D electrochemical system could remove 96.5% of MIT from the actual high-salt reverse osmosis concentrate wastewater in 30 min.It has a certain removal effect on UV_(254)in wastewater,but has a better removal effect on fluorescent substances.This study proposed a new strategy to develop transition metal and rare earth metal particle electrodes using carbon-based materials for high efficient electrocatalytic oxidation in the electrochemical treatment system.
文摘Unmanaged wood waste,particularly in countries like Nepal,presents serious environmental concerns due to open burning and improper disposal,leading to carbon emissions,air pollution and land degradation.This study introduces an environmentally sustainable strategy to upcycle Toona ciliata wood scrap—an abundant and underutilized lignocellulosic biomass—into high performance carbon electrodes for green energy storage applications.Activated carbon(TCWAC)was synthesized via single-step pyrolytic carbonization followed by phosphoric acid activation,yielding a material with high specific surface area,hierarchical porosity,and excellent electrical conductivity.Electrochemical measurements using a three-electrode configuration in 6 M KOH revealed optimized potential windows of -1.0 to -0.2 V(TCWAC),-1.2 to 0 V(TCWAC-Mn),and -1.15 to -0.4 V(TCWAC-Fe).TCWAC exhibited a specific capacitance of 156.3 Fg^(-1)at 1 Ag^(-1),with an energy density of 3.5 Whkg^(-1),and 80.2% capacity retention after 1000 charge-discharge cycles.Composites with MnO_(2)and Fe_(2)O_(3)were also evaluated.TWAC-Mn delivered 489.4 Fg^(-1),25.1 Whkg^(-1),and 99.1% retention,whereas,TWAC-Fe achieved 321.3 Fg^(-1),6.3 Whkg^(-1),and 90.3% retention.The superior performance of MnO_(2)is attributed to its multiple oxidation states,facilitating reversible faradaic redox and enhanced pseudocapacitance.This work offers the first direct,systematic comparison of MnO_(2)and Fe_(2)O_(3)composites on a common biomass-carbon matrix under identical synthesis and testing conditions.The finding provides mechanistic insight into charge storage behaviour and demonstrate a scalable route for converting biomass waste into sustainable electrode materials,contributing to cleaner energy solutions and improved biomass valorization.
基金support of the National Natural Science Foundation of China (11472165 and 11332005)
文摘Mechanical degradation, especially fractures in active particles in an electrode, is a major reason why the capacity of lithiumion batteries fades. This paper proposes a model that couples Li-ion diffusion, stress evolution, and damage mechanics to simulate the growth of central cracks in cathode particles（Li Mn_2 O_4） by an extended finite element method by considering the influence of multiple factors. The simulation shows that particles are likely to crack at a high discharge rate, when the particle radius is large, or when the initial central crack is longer. It also shows that the maximum principal tensile stress decreases and cracking becomes more difficult when the influence of crack surface diffusion is considered. The fracturing process occurs according to the following stages： no crack growth, stable crack growth, and unstable crack growth. Changing the charge/discharge strategy before unstable crack growth sets in is beneficial to prevent further capacity fading during electrochemical cycling.
文摘The metal vapor synthesis (MVS) methed was used to prepare activatedcarbon supported nickel electrode. The electrocatalytic activity of the electrode forhydrogen evolution reaction(HGR) in alkaline solution was studied. Cathodicpolarization curves showed the electrocatalytic activity of Ni/C electrode prepared byMVS method was higher than that of the one prepared by conventional method.
文摘In this paper,the functional polymeric active materials were prepared by the grafting copolymerization and their structure and properties were studied.The results show that the structure and properties of these ac- tive materials have the relative large effects on the properties of gadolinium ion selective electrodes.
基金Projects(51072173,51272221)supported by the National Natural Science Foundation of ChinaProject(20094301110005)supported by Specialized Research Fund for the Doctoral Program of Higher Education,ChinaProject(2013FJ4062)supported by Science and Technology Plan Foundation of Hunan Province,China
文摘The activated nitrogen-enriched novel carbons (NENCs) were prepared by direct carbonization using polyaniline coating activated mesocarbon microbead composites as the precursor. Herein the influences of the carbonization temperature on the structure and morphology of the NENCs samples were investigated by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N2 adsorption/desorption isotherm at 77 K. The electrochemical properties of the supercapacitors were characterized by cyclic voltammetry, galvanostatic charge/discharge, electrochemical impedance spectroscopy (EIS), cycle life, leakage current and self-discharge measurements in 6 mol/L KOH solution. The results demonstrate that the NENC samples carbonized at 600 °C show the highest specific capacitance of 385 F/g at the current density of 1 A/g and the lowest ESR value (only 0.93?). Furthermore, the capacity retention ratio of the NENCs-600 supercapacitor is 92.8 % over 2500 cycles.
基金Supported by Leading Academic Discipline Project of Shanghai Municipal Education Commission (J50102)
文摘Polyvinyl alcohol （PVA）-sodium polyacrylate （PAAS）-KOH-H2O alkaline polymer electrolyte film with high ionic conductivity was prepared by a solution-casting method. Polymer Ni（OH）2/activated carbon （AC） hybrid supercapacitors with different electrode active material mass ratios （positive to negative） were fabricated using this alkaline polymer electrolyte, nickel hydroxide positive electrodes, and AC negative electrodes. Galvanostatic charge/ discharge and electrochemical impedance spectroscopy （EIS） methods were used to study the electrochemical performance of the capacitors, such as charge/discharge specific capacitance, rate charge/discharge ability, and charge/discharge cyclic stability. Experimental results showed that with the decreasing of active material mass ratio m（Ni（OH）2）/m（AC）, the charge/discharge specific capacitance increases, but the rate charge/discharge ability and the charge/discharge cyclic stability decrease.
基金the financial support from the Department of Atomic Energy–Board of Research in Nuclear Sciences(DAE-BRNS)(Grant No.2013/37P/1/BRNS),Mumbai,India
文摘Nanowire-shaped α-Mo O3 was synthesized on a large scale by hydrothermal route.Nanocrystalline α-Mo2 C phase was obtained by the carburization of α-Mo O3 nanowires with urea as a carbon source precursor.The phase purity and crystalline size of the synthesized materials were ascertained by using powder X-ray diffraction.The shape and morphology of synthesized materials were characterized by field-emission scanning electron microscopy（FE-SEM） and high resolution transmission electron microscopy（HR-TEM）.The electrocatalytic activity of α-Mo2 C for I-/I3^-redox couple was investigated by the cyclic voltammetry.The synthesized α-Mo2 C was subsequently applied as counter electrode in dye-sensitized solar cells to replace the expensive platinum.
基金the Foundation for Polish Science(FNP)for funding the HYCAP project(research grant TEAM TECH/POIR.04.04.00-00-3D6F/16-00)carried out within the TEAM TECH program co-financed by the European Union under the European Regional Development Fund。
文摘Sodium-ion capacitors(NICs)trigger considerable attention due to their higher specific energy than electrical double-layer capacitors(EDLCs)at comparable specific power.However,the presodiation process of the anodic host is extremely crucial for the construction of high-performance NICs.Herein,a positive EDL electrode containing activated carbon(AC)mixed with sodium cyanide(NaCN)as a sacrificial material was electrochemically oxidized to presodiate a Sn_(4)P_(3) anodic host buffered by hard carbon(HC).The oxidation of CN-occurred ca.2.9 V vs.Na/Na+and finished by a short region of linearly increasing potential with a total capacity close to the theoretical value of 547 mAh g^(-1).The operando electrochemical mass spectrometry(EMS)analysis of the atmosphere in the cell together with the internal pressure measurements realized during the galvanostatic oxidation of a YP80F-NaCN electrode demonstrate that the process occurs without any gas evolution.A precursor cell of an NIC was constructed in a pouch with YP80FNaCN and HC/Sn_(4)P_(3) electrodes.After the oxidative sodium transfer from NaCN to HC/Sn_(4)P_(3),the realized YP80F//Nax(HC/Sn_(4)P_(3))NIC demonstrated a discharge capacitance retention higher than 80%for 8900 cycles in the voltage range from 2.0 to 3.8 V.The infrared analysis of the anode obtained by the herein described transfer process detected polycyanogen,which stabilizes the electrode structure during cycling,and thereof is at the origin of the enhanced life span of the NIC.
基金supported by the National Natural Science Foundation of China(52463013 and 52073133)the Major Science and Technology Project of Gansu Province(22ZD6GA008)the Incubation Program of Excelent Doctoral Dissertation-Lanzhou Univer-sity of Technology.
文摘Click chemistry is a rapid,reliable,and powerful function and a highly selective organic reaction that facilitates the efficient synthesis of various molecules by joining small units.This approach has found widespread applications in fields such as drug development,chemical synthesis,and molecular biology.In recent years,the reaction of alkali-catalyzed polymerization of thiol and sulfur has been employed to prepare various sulfur-containing polymers,which are applied as electrochemical active electrode materials in the pursuit of good performance.In this study,it is surprising to find that the reaction mechanism exhibits characteristics of both the alkali-catalyzed sulfhydryl Micheal addition reaction and thiol-epoxy click chemistry;for the first time,thiol-sulfur click chemistry is defined in detail,providing a comprehensive description of its underlying scientific principles.The introduction of this new reaction pathway holds significant potential for advancing research and the development of sulfur-containing polymers.Based on this novel click chemistry,a new sulfur-containing polymer,polydivinylthioether hexasulfide,has been designed and successfully applied as a cathode material in lithium-organosulfide batteries.This material demonstrates excellent electrochemical performance,achieving an initial capacity that reaches 790.5 mAh g−1(82.6%of theoretical capacity),and in a long-term cycle test,the capacity decay rate is only 0.063%after 1,000 cycles.
