AuPt nano particles are bi-functional catalysts for Oxygen Reduction Reaction (ORR) and Oxygen Evolution Reaction (OER) that were taken place on air electrodes in lithium air batteries. Magnetic field has been app...AuPt nano particles are bi-functional catalysts for Oxygen Reduction Reaction (ORR) and Oxygen Evolution Reaction (OER) that were taken place on air electrodes in lithium air batteries. Magnetic field has been applied during electrodeposition for the preparation of AuPt particles. With the increase of the magnetic flux density under constant current density, the grain size decreases from - 1μm to 200nm and the activity of the AuPt catalyst increases. The magnetic field oriented vertical to the electric field has a promotion effect on increasing the catalytic ability of AuPt/carbon electrode. By pulse plating, the grain size decreases to about 100nm. By adjusting parameters of the electric field and the magnetic field, controllable in-situ preparation of AuPt catalyst with various morphology and catalytic activity could be achieved.展开更多
Co0.85Se magnetic nanoparticles supported on carbon nanotubes were prepared by a one‐step hydrothermal method.The saturation magnetization and coercivity of the MWCNTs/Co0.85Se nanocomposites increased due to a decre...Co0.85Se magnetic nanoparticles supported on carbon nanotubes were prepared by a one‐step hydrothermal method.The saturation magnetization and coercivity of the MWCNTs/Co0.85Se nanocomposites increased due to a decrease in the Co0.85Se nanoparticle size in the MWCNTs/Co0.85Se nanocomposites and an increase in the distance between the Co0.85Se nanoparticles,which increased the specific surface area,thereby benefiting the electrocatalytic performance of the catalyst.Moreover,the MWCNTs/Co0.85Se nanocomposites exhibited an excellent hydrogen evolution reaction performance owing to the presence of MWCNTs,which enhanced the mass transport during the electrocatalytic reactions.Furthermore,in an acid solution,the 30 wt%MWCNTs/Co0.85Se composite catalyst exhibited a current density of 10 mA cm^‒2 at a small overpotential of 266 mV vs.RHE,a small Tafel slope of 60.5 mV dec^‐1,and good stability for HER.展开更多
Doping is an effective way to improve the activity of photocatalysts.The effect of doping on the magnetic properties of some photocatalysts that are easily recycled was studied using the local spin density approximati...Doping is an effective way to improve the activity of photocatalysts.The effect of doping on the magnetic properties of some photocatalysts that are easily recycled was studied using the local spin density approximation(LSDA)+U method on typical divalent metal oxide semiconductors CuO,NiO,Ni‐doped CuO,and Cu‐doped NiO.It is found that the influence of Ni doping on the spatial structure of CuO and that of Cu doping on the spatial structure of NiO are negligible because of the similar radii of Ni2+and Cu2+.The valence band and conduction band for Ni‐doped CuO are clearly spin‐split,corresponding to a net effective magnetic moment ofμeff=1.66μB.This may improve the photocatalytic efficiency and raise the recycle rate of photocatalysts.In the Cu‐doped NiO system,the presence of Cu3d states near to the Fermi level increases the width of the valence band and narrows the band gap with respect to that in pure NiO.Beyond the Cu3d states,within the band gap,appear two energy levels around the Fermi level,which may effectively separate the electron‐hole pair and also lead to enhanced absorption of visible light and infrared light.It can be concluded that the observed changes in the band structure may be helpful for improving the activity of photocatalysts and the doped systems have net magnetic moments,meaning that they are easily recycled and can be reused.展开更多
A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was de...A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was developed. The DPB was firstly self‐assembled on the Fe3O4NPs, and the re‐sulting Fe3O4NPs/DPB composite was then absorbed on the designed MBCPE. The MBCPE was used to attract the magnetic nanoparticles to the electrode surface. Owing to its high conductivity and large effective surface area, the novel electrode had a very large current response for the electrocat‐alytic oxidation of hydrazine. The modified electrode was characterized by voltammetry, scanning electron microscopy, electrochemical impedance spectroscopy, infrared spectroscopy, and UV‐visible spectroscopy. Voltammetric methods were used to study the electrochemical behaviour of hydrazine on MBCPE/Fe3O4NPs/DPB in phosphate buffer solution (pH = 7.0). The MBCPE/Fe3O4NPs/DPB, acting as an electrochemical sensor, exhibited very high electrocatalytic activity for the oxidation of hydrazine. The presence of DPB was found to reduce the oxidation potential of hydrazine and increase the catalytic current. The dependence of the electrocatalytic current on the hydrazine concentration exhibited two linear ranges, 0.1–0.4 μmol/L and 0.7–12.0 μmol/L, with a detection limit of 18.0 nmol/L. Additionally, the simultaneous determination of hydrazine and phe‐nol was investigated using the MBCPE/Fe3O4NPs/DPB electrode. Voltammetric experiments showed a linear range of 100–470 μmol/L and a detection limit of 24.3 μmol/L for phenol, and the proposed electrode was applied to the determination of hydrazine and phenol in water samples.展开更多
Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture ...Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture of reaction mechanism,yet the reactants for water splitting reactions are unfortunately not fully understood.Here we utilize magnetic field to understand proton transport in HER,and hydroxide ion transport in OER,to discuss the possible implications on understanding the reactants for HER and OER.Magnetic field is a known tool for changing the movement of charged species like ions,e.g.the magnetic‐field‐improved Cu^(2+)transportation near the electrode in Cu electrodeposition.However,applying a magnetic field does not affect the HER or OER rate across various pH,which challenges the traditional opinion that charged species(i.e.proton and hydroxide ion)act as the reactant.This anomalous response of HER and OER to magnetic field,and the fact that the transport of proton and hydroxide ion follow Grotthuss mechanism,collectively indicate water may act as the universal reactant for HER and OER across various pH.With the aid of magnetic field,this work serves as an understanding of water might be the reactant in HER and OER,and possibly in other electrocatalysis reactions involving protonation and deprotonation step.A model that simply focuses on the charged species but overlooking the complexity of the whole electrolyte phase where water is the dominant species,may not reasonably reflect the electrochemistry of HER and OER in aqueous electrolyte.展开更多
To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can p...To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can promote anion movement and the generation of active species,resulting more organic compounds to be oxidized and degraded.Oxidation parameters such as treatment time,current density and initial pH of the wastewater were systematically discussed and optimized.The mineralization of organic compounds is improved by over 15% under a magnetic density of 22 mT while the current density is 50 A/m2,pH is 1.8 and the reaction time is 1.5 h.The results indicate that the magnetic field assisted electrocatalytic oxidation has considerable potential in electroplating wastewater treatment.展开更多
We first received and examined X-ray spectroscopy of uranium catalyst. We studied magnetic and relativistic effects in uranium catalysts, and the movement of charged particles under the effect of a uniform electric fi...We first received and examined X-ray spectroscopy of uranium catalyst. We studied magnetic and relativistic effects in uranium catalysts, and the movement of charged particles under the effect of a uniform electric field and uniform magnetic field. We proposed the mechanism of the motion of charged particles under the influence of a uniform electric field and a uniform magnetic field.展开更多
In order to f urther improve the photosensitizing activity of hypocrellin B(HB), the complex o f 5,8 di Br HB with Al 3+ was designed and synthesized in high yield. Th e complex of aluminium ion with 5,8 di Br HB is a...In order to f urther improve the photosensitizing activity of hypocrellin B(HB), the complex o f 5,8 di Br HB with Al 3+ was designed and synthesized in high yield. Th e complex of aluminium ion with 5,8 di Br HB is a new water soluble perylene quinonoid derivative with enhanced absorption over HB in the phototherapeutic wi ndow (600-900 nm). Electron paramagnetic resonance (EPR) measurement and 9,10 diphenyl anthracene bleaching methods were used to investigate the photosensiti zing activity of [Al 2(5,8 di Br HB)Cl 4] n in the prese nce of oxygen. Singlet oxygen, superoxide anion radical, hydroxyl radical can be generated by [Al 2(5,8 di Br HB)Cl 4] n photosensit ization. The results showed that the production of hydroxyl radical ( · OH) by [Al 2(5,8 di Br HB)Cl 4] n photosensitization comes from the Fenton Haber Weiss reaction and the decom position of DMPO 1O 2 adduct. Formation of H 2O 2 as one of main intermedi ates in the photogeneration of hydroxyl radical was detected by using the cataly zed oxidation of the DPD reagent by the POD enzyme method. Moreover, the experim ents of EPR spin trap and catalase enzyme excluded the effect of organoperoxide on DPD oxidization. These results further support the proposed mechanism of · OH formation.展开更多
Nanomagnetic CoPt truncated octahedral nanoparticles (TONPs) were successfully synthesised through a facile one-pot strategy. These single crystal CoPt TONPs with an average size of about 8 nm exhibit excellent elec...Nanomagnetic CoPt truncated octahedral nanoparticles (TONPs) were successfully synthesised through a facile one-pot strategy. These single crystal CoPt TONPs with an average size of about 8 nm exhibit excellent electrocatalytic performance of both activity and stability for methanol oxidation reaction (MOR). The mass and specific activities of CoPt TONPs is 8 and 6 times higher than that of standard commercial Pt/C, respectively. After accelerated durability test (ADT), the loss of electrochemical surface area (ECSA) for CoPt TONPs is only 18.5%, which is significantly less than that of commercial Pt/C (68.2%), indicating that CoPt TONPs possess much better stability than commercial Pt/C in the prolonged operation. The Curie temperature of CoPt TONPs down to 8 nm is as high as 350 K with weak ferromagntism at room temperature (RT), which is greatly valuable for recycling in the eletrocatalytic applications.展开更多
Three different nanorod-like gallium oxides with mono/poly-crystalline nature(α, β, and α/β-Ga2O3) were prepared by regulating the amount of polyethylene glycol(PEG) 6000 in the range of 0.2–0.8 g proportionally ...Three different nanorod-like gallium oxides with mono/poly-crystalline nature(α, β, and α/β-Ga2O3) were prepared by regulating the amount of polyethylene glycol(PEG) 6000 in the range of 0.2–0.8 g proportionally via a hydrothermal method combined with further calcination. The bandgap of the products, given by UV-Vis diffuse reflectance spectra(UV-Vis DRS), was in the order of α-Ga2O3 > α/β-Ga2O3 > β-Ga2O3. To further investigate the photocatalysis performance of the catalysts, the decomposition of rhodamine B(Rh B) by Ga2O3 under UV light illumination(λ < 387 nm) was presented and complete degradation could be achieved within 30 min, a result that showed the highest efficiency. The photocatalytic oxidation mechanism is further discussed and prominently related to the active species: hydroxyl radical(·OH) and superoxide radical(O·-2), which were confirmed by electron paramagnetic resonance(EPR).展开更多
基金This work was supported by the National Natural Science Foundation of China (No.51304056), the China Postdoctoral Science Foundation (No.2013M531049), the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry, and the Fundamental Research Funds for the Central Universities (No.HIT.NSRIF.2011021).
文摘AuPt nano particles are bi-functional catalysts for Oxygen Reduction Reaction (ORR) and Oxygen Evolution Reaction (OER) that were taken place on air electrodes in lithium air batteries. Magnetic field has been applied during electrodeposition for the preparation of AuPt particles. With the increase of the magnetic flux density under constant current density, the grain size decreases from - 1μm to 200nm and the activity of the AuPt catalyst increases. The magnetic field oriented vertical to the electric field has a promotion effect on increasing the catalytic ability of AuPt/carbon electrode. By pulse plating, the grain size decreases to about 100nm. By adjusting parameters of the electric field and the magnetic field, controllable in-situ preparation of AuPt catalyst with various morphology and catalytic activity could be achieved.
文摘Co0.85Se magnetic nanoparticles supported on carbon nanotubes were prepared by a one‐step hydrothermal method.The saturation magnetization and coercivity of the MWCNTs/Co0.85Se nanocomposites increased due to a decrease in the Co0.85Se nanoparticle size in the MWCNTs/Co0.85Se nanocomposites and an increase in the distance between the Co0.85Se nanoparticles,which increased the specific surface area,thereby benefiting the electrocatalytic performance of the catalyst.Moreover,the MWCNTs/Co0.85Se nanocomposites exhibited an excellent hydrogen evolution reaction performance owing to the presence of MWCNTs,which enhanced the mass transport during the electrocatalytic reactions.Furthermore,in an acid solution,the 30 wt%MWCNTs/Co0.85Se composite catalyst exhibited a current density of 10 mA cm^‒2 at a small overpotential of 266 mV vs.RHE,a small Tafel slope of 60.5 mV dec^‐1,and good stability for HER.
基金supported by the National Natural Science Foundation of China(21377044,11304234,21573085)the Key Project of Natural Science Foundation of Hubei Province(2015CFA037)~~
文摘Doping is an effective way to improve the activity of photocatalysts.The effect of doping on the magnetic properties of some photocatalysts that are easily recycled was studied using the local spin density approximation(LSDA)+U method on typical divalent metal oxide semiconductors CuO,NiO,Ni‐doped CuO,and Cu‐doped NiO.It is found that the influence of Ni doping on the spatial structure of CuO and that of Cu doping on the spatial structure of NiO are negligible because of the similar radii of Ni2+and Cu2+.The valence band and conduction band for Ni‐doped CuO are clearly spin‐split,corresponding to a net effective magnetic moment ofμeff=1.66μB.This may improve the photocatalytic efficiency and raise the recycle rate of photocatalysts.In the Cu‐doped NiO system,the presence of Cu3d states near to the Fermi level increases the width of the valence band and narrows the band gap with respect to that in pure NiO.Beyond the Cu3d states,within the band gap,appear two energy levels around the Fermi level,which may effectively separate the electron‐hole pair and also lead to enhanced absorption of visible light and infrared light.It can be concluded that the observed changes in the band structure may be helpful for improving the activity of photocatalysts and the doped systems have net magnetic moments,meaning that they are easily recycled and can be reused.
文摘A magnetic bar carbon paste electrode (MBCPE) modified with Fe3O4 magnetic nanoparticles (Fe3O4NPs) and 2‐(3,4‐dihydroxyphenyl) benzothiazole (DPB) for the electrochemical determina‐tion of hydrazine was developed. The DPB was firstly self‐assembled on the Fe3O4NPs, and the re‐sulting Fe3O4NPs/DPB composite was then absorbed on the designed MBCPE. The MBCPE was used to attract the magnetic nanoparticles to the electrode surface. Owing to its high conductivity and large effective surface area, the novel electrode had a very large current response for the electrocat‐alytic oxidation of hydrazine. The modified electrode was characterized by voltammetry, scanning electron microscopy, electrochemical impedance spectroscopy, infrared spectroscopy, and UV‐visible spectroscopy. Voltammetric methods were used to study the electrochemical behaviour of hydrazine on MBCPE/Fe3O4NPs/DPB in phosphate buffer solution (pH = 7.0). The MBCPE/Fe3O4NPs/DPB, acting as an electrochemical sensor, exhibited very high electrocatalytic activity for the oxidation of hydrazine. The presence of DPB was found to reduce the oxidation potential of hydrazine and increase the catalytic current. The dependence of the electrocatalytic current on the hydrazine concentration exhibited two linear ranges, 0.1–0.4 μmol/L and 0.7–12.0 μmol/L, with a detection limit of 18.0 nmol/L. Additionally, the simultaneous determination of hydrazine and phe‐nol was investigated using the MBCPE/Fe3O4NPs/DPB electrode. Voltammetric experiments showed a linear range of 100–470 μmol/L and a detection limit of 24.3 μmol/L for phenol, and the proposed electrode was applied to the determination of hydrazine and phenol in water samples.
基金supported by the Singapore MOE Tier 2 MOE2018-T2-2-027the Singapore National Research Foundation under its Campus for Research Excellence and Technological Enterprise (CREATE) Programme
文摘Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture of reaction mechanism,yet the reactants for water splitting reactions are unfortunately not fully understood.Here we utilize magnetic field to understand proton transport in HER,and hydroxide ion transport in OER,to discuss the possible implications on understanding the reactants for HER and OER.Magnetic field is a known tool for changing the movement of charged species like ions,e.g.the magnetic‐field‐improved Cu^(2+)transportation near the electrode in Cu electrodeposition.However,applying a magnetic field does not affect the HER or OER rate across various pH,which challenges the traditional opinion that charged species(i.e.proton and hydroxide ion)act as the reactant.This anomalous response of HER and OER to magnetic field,and the fact that the transport of proton and hydroxide ion follow Grotthuss mechanism,collectively indicate water may act as the universal reactant for HER and OER across various pH.With the aid of magnetic field,this work serves as an understanding of water might be the reactant in HER and OER,and possibly in other electrocatalysis reactions involving protonation and deprotonation step.A model that simply focuses on the charged species but overlooking the complexity of the whole electrolyte phase where water is the dominant species,may not reasonably reflect the electrochemistry of HER and OER in aqueous electrolyte.
基金Project(2008ZX07101-006-09) supported by the Major Science and Technology Program for Water Pollution Control and Treatment of China
文摘To degrade the organic compounds in the electroplating wastewater,magnetic field was tentatively introduced into electrocatalytic oxidation on Ti-PbO2 anode.The magnetic field assisted electrocatalytic oxidation can promote anion movement and the generation of active species,resulting more organic compounds to be oxidized and degraded.Oxidation parameters such as treatment time,current density and initial pH of the wastewater were systematically discussed and optimized.The mineralization of organic compounds is improved by over 15% under a magnetic density of 22 mT while the current density is 50 A/m2,pH is 1.8 and the reaction time is 1.5 h.The results indicate that the magnetic field assisted electrocatalytic oxidation has considerable potential in electroplating wastewater treatment.
文摘We first received and examined X-ray spectroscopy of uranium catalyst. We studied magnetic and relativistic effects in uranium catalysts, and the movement of charged particles under the effect of a uniform electric field and uniform magnetic field. We proposed the mechanism of the motion of charged particles under the influence of a uniform electric field and a uniform magnetic field.
文摘In order to f urther improve the photosensitizing activity of hypocrellin B(HB), the complex o f 5,8 di Br HB with Al 3+ was designed and synthesized in high yield. Th e complex of aluminium ion with 5,8 di Br HB is a new water soluble perylene quinonoid derivative with enhanced absorption over HB in the phototherapeutic wi ndow (600-900 nm). Electron paramagnetic resonance (EPR) measurement and 9,10 diphenyl anthracene bleaching methods were used to investigate the photosensiti zing activity of [Al 2(5,8 di Br HB)Cl 4] n in the prese nce of oxygen. Singlet oxygen, superoxide anion radical, hydroxyl radical can be generated by [Al 2(5,8 di Br HB)Cl 4] n photosensit ization. The results showed that the production of hydroxyl radical ( · OH) by [Al 2(5,8 di Br HB)Cl 4] n photosensitization comes from the Fenton Haber Weiss reaction and the decom position of DMPO 1O 2 adduct. Formation of H 2O 2 as one of main intermedi ates in the photogeneration of hydroxyl radical was detected by using the cataly zed oxidation of the DPD reagent by the POD enzyme method. Moreover, the experim ents of EPR spin trap and catalase enzyme excluded the effect of organoperoxide on DPD oxidization. These results further support the proposed mechanism of · OH formation.
基金supported by the National Basic Research Program of China(2015CB921401)the National Instrument Program of China(2012YQ120048)+2 种基金the National Natural Science Foundation of China(51625101,51431009,51471183,51331002,51371015,11274371 and 11674023)the Instrument Development Program of Chinese Academy of Sciences(YZ201345)the Fundamental Research Funds for the Central Universities(FRF-BR-15-009B)
文摘Nanomagnetic CoPt truncated octahedral nanoparticles (TONPs) were successfully synthesised through a facile one-pot strategy. These single crystal CoPt TONPs with an average size of about 8 nm exhibit excellent electrocatalytic performance of both activity and stability for methanol oxidation reaction (MOR). The mass and specific activities of CoPt TONPs is 8 and 6 times higher than that of standard commercial Pt/C, respectively. After accelerated durability test (ADT), the loss of electrochemical surface area (ECSA) for CoPt TONPs is only 18.5%, which is significantly less than that of commercial Pt/C (68.2%), indicating that CoPt TONPs possess much better stability than commercial Pt/C in the prolonged operation. The Curie temperature of CoPt TONPs down to 8 nm is as high as 350 K with weak ferromagntism at room temperature (RT), which is greatly valuable for recycling in the eletrocatalytic applications.
基金funded by the National Natural Science Foundation of China(21377067,21177072,and 21207079)the Natural Science Foundation for the Innovation Group of Hubei Province,China(2009CDA020)
文摘Three different nanorod-like gallium oxides with mono/poly-crystalline nature(α, β, and α/β-Ga2O3) were prepared by regulating the amount of polyethylene glycol(PEG) 6000 in the range of 0.2–0.8 g proportionally via a hydrothermal method combined with further calcination. The bandgap of the products, given by UV-Vis diffuse reflectance spectra(UV-Vis DRS), was in the order of α-Ga2O3 > α/β-Ga2O3 > β-Ga2O3. To further investigate the photocatalysis performance of the catalysts, the decomposition of rhodamine B(Rh B) by Ga2O3 under UV light illumination(λ < 387 nm) was presented and complete degradation could be achieved within 30 min, a result that showed the highest efficiency. The photocatalytic oxidation mechanism is further discussed and prominently related to the active species: hydroxyl radical(·OH) and superoxide radical(O·-2), which were confirmed by electron paramagnetic resonance(EPR).