The physical fundamentals and influences upon electrode materials' open-circuit voltage (OCV) and the spatial distribution of electrochemical potential in the full cell are briefly reviewed. We hope to illustrate t...The physical fundamentals and influences upon electrode materials' open-circuit voltage (OCV) and the spatial distribution of electrochemical potential in the full cell are briefly reviewed. We hope to illustrate that a better understanding of these scientific problems can help to develop and design high voltage cathodes and interfaces with low Ohmic drop. OCV is one of the main indices to evaluate the performance of lithium ion batteries (LIBs), and the enhancement of OCV shows promise as a way to increase the energy density. Besides, the severe potential drop at the interfaces indicates high resistance there, which is one of the key factors limiting power density.展开更多
The dependences of electrochemical potential at the interface between carbon nanotubes and electrolyte upon temperature and electrolyte concentration are studied. Carbon nanotubes were synthesized by hot filament chem...The dependences of electrochemical potential at the interface between carbon nanotubes and electrolyte upon temperature and electrolyte concentration are studied. Carbon nanotubes were synthesized by hot filament chemical vapor deposition with Si as the substrate. Four substances were tested: NaCl solution, KCl solution, water and alcohol. It is found that for NaCl and KCl solutions, at the interface, there is a large electrochemical potential which increases with temperature and is larger for an electrolyte of higher concentration. There is a significant field effect of carbon nanotubes with electrolyte as the gate, and the effect depends on the ionizability of the electrolyte. Such physicochemical property invests carbon nanotube a potential application in nanoelectronics.展开更多
Ir catalyst possesses a good electrocatalytic activity and selectivity for the oxidation of NH3 and/or NH4OH at Ir anode in the potential fixed electrochemical sensor with the neutral solution. Owing to the same elect...Ir catalyst possesses a good electrocatalytic activity and selectivity for the oxidation of NH3 and/or NH4OH at Ir anode in the potential fixed electrochemical sensor with the neutral solution. Owing to the same electrochemical behavior of NH3 and NH4OH in a NaClO4 solution, NH4OH can be used instead of NH3 for the experimental convenience. It was found that the potential of the oxidation peak of NH4OH at the Ir/GC electrode in NaClO4 solutions is at about 0.85 V, and the current density of the oxidation peak of NH4OH is linearly proportional to the concentration of NHaOH. The electrocatalytic oxidation of NH4OH is diffusion-controlled. Especially, Ir has no electrocatalytic activity for the CO oxidation, illustrating that CO does not interfere in the measurement of NH4OH and the potential fixed electrochemical NH3 sensor with the neutral solution, and the anodic Ir catalyst possesses a good selectivity. Therefore, Ir may have practical application in the potential fixed electrochemical NH3 sensor with the neutral solution.展开更多
This paper reports the intrinsic-structure DC characteristics computed from the analytical electrochemical current theory of the bipolar field-effect transistor (BiFET) with two identical MOS gates on nanometer-thic...This paper reports the intrinsic-structure DC characteristics computed from the analytical electrochemical current theory of the bipolar field-effect transistor (BiFET) with two identical MOS gates on nanometer-thick pure-base of silicon with no generation-recombination-trapping. Numerical solutions are rapidly obtained for the three potential variables,electrostatic and electron and hole electrochemical potentials,to give the electron and hole surface and volume channel currents,using our cross-link two-route or zig-zag one-route recursive iteration algorithms. Boundary conditions on the three potentials dominantly affect the intrinsic-structure DC characteristics,illustrated by examples covering 20-decades of current (10-22 to 10-2 A/Square at 400cm^2/(V · s) mobility for 1.5nm gate-oxide, and 30nm-thick pure-base). Aside from the domination of carrier space-charge-limited drift current in the strong surface channels,observed in the theory is also the classical drift current saturation due to physical pinch-off of an impure-base volume channel depicted by the 1952 Shockley junction-gate field-effect transistor theory,and its extension to complete cut-off of the pure-base volume channel,due to vanishing carrier screening by the few electron and hole carriers in the pure-base,with Debye length (25mm) much larger than device dimension (25nm).展开更多
This paper describes the foundation underlying the device physics and theory of the semiconductor field effect transistor which is applicable to any devices with two carrier species in an electric field. The importanc...This paper describes the foundation underlying the device physics and theory of the semiconductor field effect transistor which is applicable to any devices with two carrier species in an electric field. The importance of the boundary conditions on the device current-voltage characteristics is discussed. An illustration is given of the transfer DCIV characteristics computed for two boundary conditions,one on electrical potential,giving much higher drift-limited parabolic current through the intrinsic transistor, and the other on the electrochemical potentials, giving much lower injection-over-thebarrier diffusion-limited current with ideal 60mV per decade exponential subthreshold roll-off, simulating electron and hole contacts. The two-MOS-gates on thin pure-body silicon field-effect transistor is used as examples展开更多
The degradation process of organosol coated tinplate in beverage was investigated by electrochemical noise (EN) technique combined with morphology characterization.EN data were analyzed using phase space reconstructio...The degradation process of organosol coated tinplate in beverage was investigated by electrochemical noise (EN) technique combined with morphology characterization.EN data were analyzed using phase space reconstruction theory.With the correlation dimensions obtained from the phase space reconstruction,the chaotic behavior of EN was quantitatively evaluated.The results show that both electrochemical potential noise (EPN) and electrochemical current noise (ECN) have chaotic properties.The correlation dimensions of EPN increase with corrosion extent,while those of ECN seem nearly unchanged.The increased correlation dimensions of EPN during the degradation process are associated with the increased susceptibility to local corrosion.展开更多
Mixed ions and electron conductors(MIECs)are an important family of electrocatalysts for electrochemical devices,such as reversible solid oxide cells,rechargeable metal-air batteries,and oxygen transport membranes.Con...Mixed ions and electron conductors(MIECs)are an important family of electrocatalysts for electrochemical devices,such as reversible solid oxide cells,rechargeable metal-air batteries,and oxygen transport membranes.Concurrent ionic and electronic transports in these materials play a key role in electrocatalytic activity.An in-depth fundamental understanding of the transport phenomena is critically needed to develop better MIECs.In this brief review,we introduced generic ionic and electronic transport theory based on irreversible thermodynamics and applied it to practical oxide-based materials with oxygen vacancies and electrons/holes as the predominant defects.Two oxide systems,namely CeO_(2)-based and La CrO_(3)-based materials,are selected as case studies to illustrate the utility of the transport theory in predicting oxygen partial pressure distribution across MIECs,electrochemical electronic/ionic leakage currents,and the effects of external load current on the leakage currents.展开更多
Room temperature ionic liquids (ILs) composed of cations and anions, as well as deep eutectic solvents (DESs) composed of hydrogen bond donors (HBDs) and hydrogen bond acceptors (HBAs), are regarded as green s...Room temperature ionic liquids (ILs) composed of cations and anions, as well as deep eutectic solvents (DESs) composed of hydrogen bond donors (HBDs) and hydrogen bond acceptors (HBAs), are regarded as green solvents due to their low volatility. They have been used widely for electrochemically driven reactions because they exhibit high conductivity and excellent elec- trochemical stability. However, no systematic investigations on the electrochemical potential windows (EPWs), which could be used to characterize the electrochemical stability, have been reported. In this regard, the EPWs of 33 ILs and 23 DESs have been studied utilizing cyclic voltammetry (CV) method and the effects of structural factors (cations and anions of ILs, and HBDs and HBAs of DESs) and external factors (electrode, water content) on the EPWs have been comprehensively investi- gated. The electrochemical stability of selected 1Ls comprising five traditional cations, namely imidazolium, pyridinium, pyr- rolidinium, piperidinium and ammonium and 13 kinds of versatile anions was studied. The results show that for ILs, both cati- on and anion play an important role on the reductive and oxidative potential limit. For a same IL at different working electrode, for example, glassy carbon (GC), gold (Au) and platinum (Pt) electrode, the largest potential window is almost observed on the GC working electrode. The investigations on the EPWs of choline chloride (ChCl), choline bromide (ChBr), choline iodide (ChI), and methyl urea based DESs show that the DES composed of ChCl and methyl urea has the largest potential window. This work may aid the selection of ILs or DESs for use as a direct electrolyte or a solvent in electrochemical applications.展开更多
With the development of surface and interface science and technology,methods for the online modulation of interfacial performance by external stimuli are in high demand.Switching between ultra-low and high friction st...With the development of surface and interface science and technology,methods for the online modulation of interfacial performance by external stimuli are in high demand.Switching between ultra-low and high friction states is a particular goal owing to its applicability to the development of precision machines and nano/micro-electromechanical systems.In this study,reversible switching between superlubricity and high friction is realized by controlling the electric potential of a gold surface in aqueous salt solution sliding against a SiO_(2) microsphere.Applying positive potential results creates an ice-like water layer with high hydrogen bonding and adhesion at the interface,leading to nonlinear high friction.However,applying negative potential results in free water on the gold surface and negligible adhesion at the interface,causing linear ultra-low friction(friction coefficient of about 0.004,superlubricity state).A quantitative description of how the external load and interfacial adhesion affected friction force was developed,which agrees well with the experimental results.Thus,this work quantitatively reveals the mechanism of potential-controlled switching between superlubricity and high-friction states.Controlling the interfacial behavior via the electric potential could inspire novel design strategies for nano/micro-electromechanical and nano/micro-fluidic systems.展开更多
Seed-mediated growth is the most general way to controllably synthesize bimetal nano-heterostructures. Despite successful instances through trial and error were reported, the way for second metal depositing on the see...Seed-mediated growth is the most general way to controllably synthesize bimetal nano-heterostructures. Despite successful instances through trial and error were reported, the way for second metal depositing on the seed. namely whether the symmetry of resulted nano-heterostructure follows the original crystal symmetry of seed metal, remains an unpredictable issue to date. In this work, we propose that the ther- modynamic factor, i.e., the difference of equilibrium electrochemical potentials (corresponding to their Fermi levels) of two metals in the growth solution, plays a key role for the symmetry breaking of bimetal nano-heterostructures during the seed-mediated growth. As a proof-of-principle experiment, by revers- ing the relative position of Fermi levels of the Pd nanocube seeds and the second metal Au with changing the concentration of reductant (L-ascorbic acid) in the growth solution, the structure of as-prepared prod- ucts successfully evolved from centrosymmetric Pd@Au core-shell trisoctabedra to asymmetric Pd-Au hetero-dimers. The idea was further demonstrated by the growth of Ag on the Pd seeds. The present work intends to reveal the origin of symmetry breaking in the seed-mediated growth of nano-heterostructures from the viewpoint of thermodynamics, and these new insights will in turn help to achieve rational con- struction of bimetal nano-heterostructures with soecific functions.展开更多
Corrosion evolution during immersion tests (up to 43 days) of NiCu steel in deaerated 0.1 mol/L bicarbonate solutions was investigated by electrochemical measurements, scanning electron microscopy (SEM) and X-ray ...Corrosion evolution during immersion tests (up to 43 days) of NiCu steel in deaerated 0.1 mol/L bicarbonate solutions was investigated by electrochemical measurements, scanning electron microscopy (SEM) and X-ray diffraction (XRD). Results show that NiCu steel transformed from the anodic dissolution in the early stage of immersion to a metastable passive state in the final stage as the open-circuit potential value shifted positively, which was aroused by the precipitation of corrosion products. This process was mainly promoted by the trace amount of oxygen. Simultaneously, dominant cathodic reaction transformed from the hydrogen evolution in early stage to reduction processes of corrosion products in later stages. Possible corrosion processes were discussed with the assistance of a corresponding Pourbaix diagram.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.51325206 and 51372228)National Basic Research Program of China(Grant No.2012CB932900)Shanghai Pujiang Program,China(Grant No.14PJ1403900)
文摘The physical fundamentals and influences upon electrode materials' open-circuit voltage (OCV) and the spatial distribution of electrochemical potential in the full cell are briefly reviewed. We hope to illustrate that a better understanding of these scientific problems can help to develop and design high voltage cathodes and interfaces with low Ohmic drop. OCV is one of the main indices to evaluate the performance of lithium ion batteries (LIBs), and the enhancement of OCV shows promise as a way to increase the energy density. Besides, the severe potential drop at the interfaces indicates high resistance there, which is one of the key factors limiting power density.
文摘The dependences of electrochemical potential at the interface between carbon nanotubes and electrolyte upon temperature and electrolyte concentration are studied. Carbon nanotubes were synthesized by hot filament chemical vapor deposition with Si as the substrate. Four substances were tested: NaCl solution, KCl solution, water and alcohol. It is found that for NaCl and KCl solutions, at the interface, there is a large electrochemical potential which increases with temperature and is larger for an electrolyte of higher concentration. There is a significant field effect of carbon nanotubes with electrolyte as the gate, and the effect depends on the ionizability of the electrolyte. Such physicochemical property invests carbon nanotube a potential application in nanoelectronics.
基金Supported by RAE Engineering Center, RAE Systems Inc. Fund, China
文摘Ir catalyst possesses a good electrocatalytic activity and selectivity for the oxidation of NH3 and/or NH4OH at Ir anode in the potential fixed electrochemical sensor with the neutral solution. Owing to the same electrochemical behavior of NH3 and NH4OH in a NaClO4 solution, NH4OH can be used instead of NH3 for the experimental convenience. It was found that the potential of the oxidation peak of NH4OH at the Ir/GC electrode in NaClO4 solutions is at about 0.85 V, and the current density of the oxidation peak of NH4OH is linearly proportional to the concentration of NHaOH. The electrocatalytic oxidation of NH4OH is diffusion-controlled. Especially, Ir has no electrocatalytic activity for the CO oxidation, illustrating that CO does not interfere in the measurement of NH4OH and the potential fixed electrochemical NH3 sensor with the neutral solution, and the anodic Ir catalyst possesses a good selectivity. Therefore, Ir may have practical application in the potential fixed electrochemical NH3 sensor with the neutral solution.
文摘This paper reports the intrinsic-structure DC characteristics computed from the analytical electrochemical current theory of the bipolar field-effect transistor (BiFET) with two identical MOS gates on nanometer-thick pure-base of silicon with no generation-recombination-trapping. Numerical solutions are rapidly obtained for the three potential variables,electrostatic and electron and hole electrochemical potentials,to give the electron and hole surface and volume channel currents,using our cross-link two-route or zig-zag one-route recursive iteration algorithms. Boundary conditions on the three potentials dominantly affect the intrinsic-structure DC characteristics,illustrated by examples covering 20-decades of current (10-22 to 10-2 A/Square at 400cm^2/(V · s) mobility for 1.5nm gate-oxide, and 30nm-thick pure-base). Aside from the domination of carrier space-charge-limited drift current in the strong surface channels,observed in the theory is also the classical drift current saturation due to physical pinch-off of an impure-base volume channel depicted by the 1952 Shockley junction-gate field-effect transistor theory,and its extension to complete cut-off of the pure-base volume channel,due to vanishing carrier screening by the few electron and hole carriers in the pure-base,with Debye length (25mm) much larger than device dimension (25nm).
文摘This paper describes the foundation underlying the device physics and theory of the semiconductor field effect transistor which is applicable to any devices with two carrier species in an electric field. The importance of the boundary conditions on the device current-voltage characteristics is discussed. An illustration is given of the transfer DCIV characteristics computed for two boundary conditions,one on electrical potential,giving much higher drift-limited parabolic current through the intrinsic transistor, and the other on the electrochemical potentials, giving much lower injection-over-thebarrier diffusion-limited current with ideal 60mV per decade exponential subthreshold roll-off, simulating electron and hole contacts. The two-MOS-gates on thin pure-body silicon field-effect transistor is used as examples
基金Supported by Major State Basic Research Program of China ("973" Program,No. 2011CB610505)Specialized Research Fund for the Doctoral Program of Higher Education (No. 20120032110029)
文摘The degradation process of organosol coated tinplate in beverage was investigated by electrochemical noise (EN) technique combined with morphology characterization.EN data were analyzed using phase space reconstruction theory.With the correlation dimensions obtained from the phase space reconstruction,the chaotic behavior of EN was quantitatively evaluated.The results show that both electrochemical potential noise (EPN) and electrochemical current noise (ECN) have chaotic properties.The correlation dimensions of EPN increase with corrosion extent,while those of ECN seem nearly unchanged.The increased correlation dimensions of EPN during the degradation process are associated with the increased susceptibility to local corrosion.
基金based on the work supported by the U.S.Department of Energy’s Office of Energy Efficiency and Renewable Energy through the Fuel Cell Technologies Office under award number DE-EE-0008842the National Science Foundation,United States for funding this study under award number 1801284。
文摘Mixed ions and electron conductors(MIECs)are an important family of electrocatalysts for electrochemical devices,such as reversible solid oxide cells,rechargeable metal-air batteries,and oxygen transport membranes.Concurrent ionic and electronic transports in these materials play a key role in electrocatalytic activity.An in-depth fundamental understanding of the transport phenomena is critically needed to develop better MIECs.In this brief review,we introduced generic ionic and electronic transport theory based on irreversible thermodynamics and applied it to practical oxide-based materials with oxygen vacancies and electrons/holes as the predominant defects.Two oxide systems,namely CeO_(2)-based and La CrO_(3)-based materials,are selected as case studies to illustrate the utility of the transport theory in predicting oxygen partial pressure distribution across MIECs,electrochemical electronic/ionic leakage currents,and the effects of external load current on the leakage currents.
基金supported by the National Natural Science Foundation of China (21173267, 21473252)
文摘Room temperature ionic liquids (ILs) composed of cations and anions, as well as deep eutectic solvents (DESs) composed of hydrogen bond donors (HBDs) and hydrogen bond acceptors (HBAs), are regarded as green solvents due to their low volatility. They have been used widely for electrochemically driven reactions because they exhibit high conductivity and excellent elec- trochemical stability. However, no systematic investigations on the electrochemical potential windows (EPWs), which could be used to characterize the electrochemical stability, have been reported. In this regard, the EPWs of 33 ILs and 23 DESs have been studied utilizing cyclic voltammetry (CV) method and the effects of structural factors (cations and anions of ILs, and HBDs and HBAs of DESs) and external factors (electrode, water content) on the EPWs have been comprehensively investi- gated. The electrochemical stability of selected 1Ls comprising five traditional cations, namely imidazolium, pyridinium, pyr- rolidinium, piperidinium and ammonium and 13 kinds of versatile anions was studied. The results show that for ILs, both cati- on and anion play an important role on the reductive and oxidative potential limit. For a same IL at different working electrode, for example, glassy carbon (GC), gold (Au) and platinum (Pt) electrode, the largest potential window is almost observed on the GC working electrode. The investigations on the EPWs of choline chloride (ChCl), choline bromide (ChBr), choline iodide (ChI), and methyl urea based DESs show that the DES composed of ChCl and methyl urea has the largest potential window. This work may aid the selection of ILs or DESs for use as a direct electrolyte or a solvent in electrochemical applications.
基金the National Natural Science Foundation of China(Nos.51901112 and 51425502)China Postdoctoral Science Foundation(No.2018M630145)the Major Scientific Research and Development Project in Jiangxi(No.20173ABC28008).
文摘With the development of surface and interface science and technology,methods for the online modulation of interfacial performance by external stimuli are in high demand.Switching between ultra-low and high friction states is a particular goal owing to its applicability to the development of precision machines and nano/micro-electromechanical systems.In this study,reversible switching between superlubricity and high friction is realized by controlling the electric potential of a gold surface in aqueous salt solution sliding against a SiO_(2) microsphere.Applying positive potential results creates an ice-like water layer with high hydrogen bonding and adhesion at the interface,leading to nonlinear high friction.However,applying negative potential results in free water on the gold surface and negligible adhesion at the interface,causing linear ultra-low friction(friction coefficient of about 0.004,superlubricity state).A quantitative description of how the external load and interfacial adhesion affected friction force was developed,which agrees well with the experimental results.Thus,this work quantitatively reveals the mechanism of potential-controlled switching between superlubricity and high-friction states.Controlling the interfacial behavior via the electric potential could inspire novel design strategies for nano/micro-electromechanical and nano/micro-fluidic systems.
基金supported by the National Basic Research Program of China(2015CB93230)the National Key Research and Development Program of China(2017YFA0206801)+1 种基金the National Natural Science Foundation of China(21333008,21671163,21721001,and 21773190)the Fundamental Research Funds for the Central Universities(20720160026)
文摘Seed-mediated growth is the most general way to controllably synthesize bimetal nano-heterostructures. Despite successful instances through trial and error were reported, the way for second metal depositing on the seed. namely whether the symmetry of resulted nano-heterostructure follows the original crystal symmetry of seed metal, remains an unpredictable issue to date. In this work, we propose that the ther- modynamic factor, i.e., the difference of equilibrium electrochemical potentials (corresponding to their Fermi levels) of two metals in the growth solution, plays a key role for the symmetry breaking of bimetal nano-heterostructures during the seed-mediated growth. As a proof-of-principle experiment, by revers- ing the relative position of Fermi levels of the Pd nanocube seeds and the second metal Au with changing the concentration of reductant (L-ascorbic acid) in the growth solution, the structure of as-prepared prod- ucts successfully evolved from centrosymmetric Pd@Au core-shell trisoctabedra to asymmetric Pd-Au hetero-dimers. The idea was further demonstrated by the growth of Ag on the Pd seeds. The present work intends to reveal the origin of symmetry breaking in the seed-mediated growth of nano-heterostructures from the viewpoint of thermodynamics, and these new insights will in turn help to achieve rational con- struction of bimetal nano-heterostructures with soecific functions.
基金supported by the National Natural Science Foundation of China (No. 51471175)
文摘Corrosion evolution during immersion tests (up to 43 days) of NiCu steel in deaerated 0.1 mol/L bicarbonate solutions was investigated by electrochemical measurements, scanning electron microscopy (SEM) and X-ray diffraction (XRD). Results show that NiCu steel transformed from the anodic dissolution in the early stage of immersion to a metastable passive state in the final stage as the open-circuit potential value shifted positively, which was aroused by the precipitation of corrosion products. This process was mainly promoted by the trace amount of oxygen. Simultaneously, dominant cathodic reaction transformed from the hydrogen evolution in early stage to reduction processes of corrosion products in later stages. Possible corrosion processes were discussed with the assistance of a corresponding Pourbaix diagram.