In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrol...In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrolyte composed of ionic liquids(ILs),NaCl,and H_(2)SO_(4),integrating extraction and electrochemical oxidation to effectively remove different aromatic sulfur compounds with sulfur removals of 100%.Additionally,H_(2)is co-produced at the cathode,supporting refinery processes and reducing H_(2)storage and transportation costs,thereby improving economic viability.Detailed mechanism analysis shows that IL selectively extracts and concentrates sulfur compounds,while NaCl and H2SO4 facilitate ClO^(-)generation,serving as the in-situ oxidant.The EC-EODS system operates without external catalysts,relying on graphite electrodes that generate superoxide radicals from ClO^(-).Moreover,a strategy for the separation of desulfurization products as well as the electrolyte is proposed as well.The EC-EODS system offers a sustainable,high-efficiency strategy for desulfurization,with economic benefits through sulfur oxidation and H_(2)co-generation.展开更多
The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towa...The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towards methanol electro-oxidation was evaluated by cyclic voltammetry in 1 mol/L KOH solution.XRD and TEM analyses revealed that nano-decomposition of quasicrystal grains occurred in the initial stage of dealloying,and the fully dealloyed sample was composed of FCC-Pd phase.Scanning electron microscopy observation indicated that a maze-like nanoporous pattern was formed in the dealloyed sample,consisting of percolated pores of 5.20 nm in diameter in a skeleton of randomly-orientated Pd nano-ligaments with a uniform thickness of^5 nm.A retention of^12 at.%Al in the Pd nano-ligments was determined by energy dispersive X-ray spectroscopy(EDS).The nanoporous Pd demonstrated obvious electro-catalytic activity towards methanol electro-oxidation in alkaline environment.展开更多
Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope（SEM）, X-ray diffraction（XRD） and cyclic voltammetry...Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope（SEM）, X-ray diffraction（XRD） and cyclic voltammetry（CV） measurements. The electro-catalytic activity for degradation of sulfisoxazole（SIZ） was investigated by using prepared graphene or graphite anode. The results showed that the degradation of SIZ was much more rapid on the graphene than that on the graphite electrode. Moreover, the graphene electrode exhibited good stability and recyclability. The analysis on the intermediate products and the measurement of active species during the SIZ degradation demonstrated that indirect oxidation is the dominant mechanism, involving the electro-catalytic generation of OH and O_2^- as the main active oxygen species. This study implies that graphene is a promising potential electrode material for long-term application to electro-catalytic degradation of organic pollutants.展开更多
The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nan...The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nanopowder modified electrode was prepared using the drop coating method,which displayed excellent electrocatalytic activity towards the oxidation of dopamine and uric acid compared with the bare glassy carbon electrode in phosphate buffer solution at pH=7.0.Linear responses for dopamine and uric acid were obtained in the ranges of3.3μmol/L to 249.1μmol/L and 6.7μmol/L to 386.3μmol/L with detection limits of 1.5μmol/L and 2.7μmol/L(S/N=3),respectively.The response time was less than 2 s in case of dopamine and 3 s in case of uric acid,respectively.The results demonstrated that the graphene nanopowder had potential for detecting dopamine and uric acid.展开更多
Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is i...Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is in a range of 200-500 nm with many porous.The B-α-Ni(OH)2nanoflowers were developed as electrocatalysts for urea electro-oxidation in alkaline media with more than 10 times enhancement in current density compared to bulk nickel hydroxide powders.Results demonstrated that the obtained B-α-Ni(OH)2electrode exhibited high activity and good stability.The positive correlation between the scan rates and the anodic currents implied a single diffusion-controlled kinetic process.The enhanced electro-catalytic oxidation of urea using B-α-Ni(OH)2 nanoflowers has promising applications in urea-rich wastewater remediation,hydrogen production,and fuel cells.展开更多
Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatmen...Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatment of such wastewater. Moreover, since such wastewater is also not suitable for the growth of microorganisms, the way of wastewater treatment by microorganisms is also greatly limited. For this kind of industrial waste water, apart from the degradation of organic matters, the separation of inorganic salts and waste water is also required to meet the sewage discharge standard. Based on this, the article focuses on the coal chemical high salt wastewater electro-catalytic oxidation pilot study.展开更多
The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode...The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.展开更多
The current study presents for the first time the preparation of a NiAl(68%(mass)Ni)intermetallic compound through the induction heating technique as a cathode for alkaline water electrolysis.The high-purity target wa...The current study presents for the first time the preparation of a NiAl(68%(mass)Ni)intermetallic compound through the induction heating technique as a cathode for alkaline water electrolysis.The high-purity target was confirmed by X-ray diffraction and scanning electron microscopy combined with energy dispersive X-ray analysis.The chemical activation of Al from the NiAl electrode was achieved in a 25%NaOH solution at 353 K for 72 h.The performance and stability tests in a 1 mol·L^(-1)KOH solution at 298 K demonstrated that the enhancement of the hydrogen evolution reactionwas 13 times higher in the activated NiAl electrode than in the non-activated NiAl electrode.In addition,the electrochemical tests showed that the activated NiAl electrode exhibited the best hydrogen evolution reaction performance.Based on the findings,it is believed that the induction heating technique is a promising route for preparing a highly active and cost-effective NiAl electrode for green hydrogen production.展开更多
The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging prob...The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging problems. In this paper, Electrocatalytically active palladium nanoparticles(Pd NPs) on MWNTs with the high-performance and excellent solubility polymer, poly(dimethylbenzimidazolium) iodide(P(DMBI)-I-)as modifier and glue was first discussed. The results of transmission electron microscopy(TEM) demonstrate a better dispersion of MWNTs with the assist of P(DMBI)-I-. The Raman spectra indicate a strong π-π interaction between MWNTs and P(DMBI)-I-. Taking advantages of the coordination effect of imidazole groups and the electrostatic attraction to Pd NPs, the prepared Pd/MWNTs-P(DMBI)-I-(Pd/MPDI-) hybrid is of well electrocatalytic activity to the ethanol fuel cells by electrochemical measurements. So it is believed that P(DMBI)-Ican be further applied in the dispersion of different carbon-based materials and metal nanoparticles for fabricating more novel composites for catalyst and electrode material.展开更多
Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxi...Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxidation of hydrazine and that involved in the rate-determining step were four and one,respectively.The interfering effect of some cations,anions and organic compounds were examined.Peak current for this process varied linearly with the square root of the scan rate.The kinetic parameters,such as the electron transfer coefficient(α) and catalytic rate constant(k) ,were determined using cyclic voltammetry,linear sweep voltammetry and chronoamperometry.The electro-catalytic response was optimized with regards to the pH,scan rate,hydrazine concentration and other variables.展开更多
基金financial support from the National Key R&D Program of China(No.2022YFA1504404,2022YFA1504403)National Science Foundation for Distinguished Young Scholars(No.22425808)+2 种基金National Natural Science Foundation of China(No.22178154)China Postdoctoral Science Foundation(No.2024M753617)Natural Science Foundation of Jiangsu Province(No.BK20230068).
文摘In this study,we present an extraction-coupled electro-catalytic oxidative desulfurization(EC-EODS)system that achieves efficient sulfur removal from fuel oils without external oxidants.The system utilizes an electrolyte composed of ionic liquids(ILs),NaCl,and H_(2)SO_(4),integrating extraction and electrochemical oxidation to effectively remove different aromatic sulfur compounds with sulfur removals of 100%.Additionally,H_(2)is co-produced at the cathode,supporting refinery processes and reducing H_(2)storage and transportation costs,thereby improving economic viability.Detailed mechanism analysis shows that IL selectively extracts and concentrates sulfur compounds,while NaCl and H2SO4 facilitate ClO^(-)generation,serving as the in-situ oxidant.The EC-EODS system operates without external catalysts,relying on graphite electrodes that generate superoxide radicals from ClO^(-).Moreover,a strategy for the separation of desulfurization products as well as the electrolyte is proposed as well.The EC-EODS system offers a sustainable,high-efficiency strategy for desulfurization,with economic benefits through sulfur oxidation and H_(2)co-generation.
基金Foundation item:Project(51671045)supported by the National Natural Science Foundation of ChinaProject(DUT18GF112)supported by the Fundamental Research Funds for the Central Universities,ChinaProject(TZ2016004)supported by the Science Challenge Project,China
文摘The formation of nanoporous Pd was studied by electro-chemical dealloying a rapidly-quenched Al70Pd17Fe13 quasicrystal alloy in dilute NaCl aqueous solution,and the electro-catalytic activity of the nanoporous Pd towards methanol electro-oxidation was evaluated by cyclic voltammetry in 1 mol/L KOH solution.XRD and TEM analyses revealed that nano-decomposition of quasicrystal grains occurred in the initial stage of dealloying,and the fully dealloyed sample was composed of FCC-Pd phase.Scanning electron microscopy observation indicated that a maze-like nanoporous pattern was formed in the dealloyed sample,consisting of percolated pores of 5.20 nm in diameter in a skeleton of randomly-orientated Pd nano-ligaments with a uniform thickness of^5 nm.A retention of^12 at.%Al in the Pd nano-ligments was determined by energy dispersive X-ray spectroscopy(EDS).The nanoporous Pd demonstrated obvious electro-catalytic activity towards methanol electro-oxidation in alkaline environment.
基金supported by the National Natural Science Foundation of China (Nos. 21377067, 21407092, 21177072)the Master's Degree Thesis Excellent Training Fund of Three Gorges University (No. 2014PY074)
文摘Graphite and graphene electrodes were prepared by using pure graphite as precursor. The electrode materials were characterized by a scanning electron microscope（SEM）, X-ray diffraction（XRD） and cyclic voltammetry（CV） measurements. The electro-catalytic activity for degradation of sulfisoxazole（SIZ） was investigated by using prepared graphene or graphite anode. The results showed that the degradation of SIZ was much more rapid on the graphene than that on the graphite electrode. Moreover, the graphene electrode exhibited good stability and recyclability. The analysis on the intermediate products and the measurement of active species during the SIZ degradation demonstrated that indirect oxidation is the dominant mechanism, involving the electro-catalytic generation of OH and O_2^- as the main active oxygen species. This study implies that graphene is a promising potential electrode material for long-term application to electro-catalytic degradation of organic pollutants.
基金supported by the National Natural Science Foundation(11179033)Beijing Natural Science Foundation(2102012)
文摘The graphene nanopowder for electro-catalytic oxidation of dopamine and uric acid in the presence of ascorbic acid has been investigated by cyclic voltammetry,linear polarization and chronoamperometry.The graphene nanopowder modified electrode was prepared using the drop coating method,which displayed excellent electrocatalytic activity towards the oxidation of dopamine and uric acid compared with the bare glassy carbon electrode in phosphate buffer solution at pH=7.0.Linear responses for dopamine and uric acid were obtained in the ranges of3.3μmol/L to 249.1μmol/L and 6.7μmol/L to 386.3μmol/L with detection limits of 1.5μmol/L and 2.7μmol/L(S/N=3),respectively.The response time was less than 2 s in case of dopamine and 3 s in case of uric acid,respectively.The results demonstrated that the graphene nanopowder had potential for detecting dopamine and uric acid.
基金Supported by the National Natural Science Foundation of China(21403053,U1404503)
文摘Boron-dopedα-Ni(OH)2nanoflowers(B-α-Ni(OH)2)were synthesized by a liquidphase method using P123(EO20PO70EO20)as a template and NaBH4 as alkali and boron sources.The average size of these B-α-Ni(OH)2nanoflowers is in a range of 200-500 nm with many porous.The B-α-Ni(OH)2nanoflowers were developed as electrocatalysts for urea electro-oxidation in alkaline media with more than 10 times enhancement in current density compared to bulk nickel hydroxide powders.Results demonstrated that the obtained B-α-Ni(OH)2electrode exhibited high activity and good stability.The positive correlation between the scan rates and the anodic currents implied a single diffusion-controlled kinetic process.The enhanced electro-catalytic oxidation of urea using B-α-Ni(OH)2 nanoflowers has promising applications in urea-rich wastewater remediation,hydrogen production,and fuel cells.
文摘Industrial wastewater from modern industrial production often contains excessive organic hazardous substances or excessive salts, acids and bases, etc. Traditional methods cannot play an effective role in the treatment of such wastewater. Moreover, since such wastewater is also not suitable for the growth of microorganisms, the way of wastewater treatment by microorganisms is also greatly limited. For this kind of industrial waste water, apart from the degradation of organic matters, the separation of inorganic salts and waste water is also required to meet the sewage discharge standard. Based on this, the article focuses on the coal chemical high salt wastewater electro-catalytic oxidation pilot study.
基金Project(50925417)supported by the National Natureal Science Foundation for Distinguished Young Scholar of ChinaProject(51074191)supported by the National Natural Science Foundation of China
文摘The electrochemical degradation of reed pulp black liquor containing lignin pretreated by acidification method was investigated using a three-dimensional electrode reactor. Using activated carbon as particle electrode, the effects of p H value, reaction temperature, electrolysis time and current on residual concentration of total organic carbon(TOC) were discussed in detail. The optimal conditions were obtained: pH 2.5, influent flow rate of 200 mL/min, 25 °C, 300 mA and 2h of electrolysis time, and the removal efficiency of TOC maintains at 35.57 %. The results of the electrochemical method indicate that ·OH radicals are produced in activated carbon anode in the electrolysis process and then adsorbed on the activated carbon surface. Microcell consists of ·OH radicals and the absorbed lignin. With the microcell reaction, the lignin is degraded, while the anodic polarized curve illustrates that the lignin is obviously oxidized in the anode. The contributions of direct and indirect electrolyses to the TOC removal ratio are about 50%, respectively.
文摘The current study presents for the first time the preparation of a NiAl(68%(mass)Ni)intermetallic compound through the induction heating technique as a cathode for alkaline water electrolysis.The high-purity target was confirmed by X-ray diffraction and scanning electron microscopy combined with energy dispersive X-ray analysis.The chemical activation of Al from the NiAl electrode was achieved in a 25%NaOH solution at 353 K for 72 h.The performance and stability tests in a 1 mol·L^(-1)KOH solution at 298 K demonstrated that the enhancement of the hydrogen evolution reactionwas 13 times higher in the activated NiAl electrode than in the non-activated NiAl electrode.In addition,the electrochemical tests showed that the activated NiAl electrode exhibited the best hydrogen evolution reaction performance.Based on the findings,it is believed that the induction heating technique is a promising route for preparing a highly active and cost-effective NiAl electrode for green hydrogen production.
文摘The multi walled carbon nanotubes(MWNTs) have always been as the catalyst supporting materials,but for high-performance composite catalysts, the dispersion and functionalization of MWNTs are important challenging problems. In this paper, Electrocatalytically active palladium nanoparticles(Pd NPs) on MWNTs with the high-performance and excellent solubility polymer, poly(dimethylbenzimidazolium) iodide(P(DMBI)-I-)as modifier and glue was first discussed. The results of transmission electron microscopy(TEM) demonstrate a better dispersion of MWNTs with the assist of P(DMBI)-I-. The Raman spectra indicate a strong π-π interaction between MWNTs and P(DMBI)-I-. Taking advantages of the coordination effect of imidazole groups and the electrostatic attraction to Pd NPs, the prepared Pd/MWNTs-P(DMBI)-I-(Pd/MPDI-) hybrid is of well electrocatalytic activity to the ethanol fuel cells by electrochemical measurements. So it is believed that P(DMBI)-Ican be further applied in the dispersion of different carbon-based materials and metal nanoparticles for fabricating more novel composites for catalyst and electrode material.
文摘Electro-catalytic oxidation and detection of hydrazine on a glassy carbon electrode,at pH 6.0,was studied by using alizarin red S as a homogeneous mediator.The overall number of electrons involved in the catalytic oxidation of hydrazine and that involved in the rate-determining step were four and one,respectively.The interfering effect of some cations,anions and organic compounds were examined.Peak current for this process varied linearly with the square root of the scan rate.The kinetic parameters,such as the electron transfer coefficient(α) and catalytic rate constant(k) ,were determined using cyclic voltammetry,linear sweep voltammetry and chronoamperometry.The electro-catalytic response was optimized with regards to the pH,scan rate,hydrazine concentration and other variables.
