An experimental investigation of the saturation ion current densities (Jions) in hydrogen inductively coupled plasma (ICP) produced by a large-power (2-32 kW) radio frequency (RF) generator is reported, then s...An experimental investigation of the saturation ion current densities (Jions) in hydrogen inductively coupled plasma (ICP) produced by a large-power (2-32 kW) radio frequency (RF) generator is reported, then some reasonable explanations are given out. With the increase of RF power, the experimental results show three stages: in the first stage (2-14 kW), the electron temperature will rise with the increase of RF power in the ICP, thus, the Jions increases continually as the electron temperature rises in the ICP. In the second stage (14 20 kW), as some H- ions lead to the mutual neutralization (MN), the slope of Jio^s variation firstly decreases then increases. In the third stage (20-32 kW), both the electronic detachment (ED) and the associative detachment (AD) in the ICP result in the destruction of H- ions, therefore, the increased amplitude of the Jions in the third stage is weaker than the one in the first stage. In addition, with the equivalent transformer model, we successfully Explain that the Jions at different radial locations in ICP has the same rule. Finally, it is found that the Jions has nothing to do with the outer/inner puffing gas pressure ratio, which is attributed to the high-speed movement of hydrogen molecules.展开更多
The article theoretically studied the charge-exchange effects on space charge limitedelectron and ion current densities of non-relativistic one-dimensional slab ion diode, and comparedwith those of without charge exch...The article theoretically studied the charge-exchange effects on space charge limitedelectron and ion current densities of non-relativistic one-dimensional slab ion diode, and comparedwith those of without charge exchange.展开更多
Hydrogen evolution reaction is a critical reaction in water splitting for hydrogen production.However,developing effective and stable non‐noble‐metal electrocatalysts which work well at high current densities demand...Hydrogen evolution reaction is a critical reaction in water splitting for hydrogen production.However,developing effective and stable non‐noble‐metal electrocatalysts which work well at high current densities demanded by industry still remain great challenge.Herein,taking advantage of the highly tunable metal‐organic framework(MOF)templates,nitrogen doped binary transition metal phosphides electrocatalysts(N‐CoP_(x)/Ni_(2)P)with three‐dimensional(3D)conductive network structure were successfully synthesized.The 3D open porous channels could expose more catalytically active sites;nitrogen doping and the synergistic effect between CoP and Ni_(2)P can increase the electron density of Co atoms at active sites,further optimizing the Gibbs free energy of hydrogen(ΔGH*)and water(ΔG_(H_(2)O*)).As a result,the obtained N‐CoP_(x)/Ni_(2)P catalyst exhibits extraordinary electrocatalytic activity in a wide pH range.Especially,it requires an extremely low overpotential of 152 mV to deliver a high current density of 650 mA cm^(–2) in alkaline media.This work may shed some light on the rational design of cheap electrocatalysts and electrode materials that work well at high current densities.展开更多
Alkaline water electrolysis provides a promising route for"green hydrogen"generation,where anodic oxygen evolution reaction(OER)plays a crucial role in coupling with cathodic hydrogen evolution reaction.To d...Alkaline water electrolysis provides a promising route for"green hydrogen"generation,where anodic oxygen evolution reaction(OER)plays a crucial role in coupling with cathodic hydrogen evolution reaction.To date,the development of highly active and durable OER catalysts based on earth-abundant elements has drawn wide attention;nevertheless,their performance under high current densities(HCDs≥1000 mA cm^(-2))has been less emphasized.This situation has seriously impeded large-scale electrolysis industrialization.In this review,in order to provide a guideline for designing high-performance OER electrocatalysts,the effects of HCD on catalytic performance involving electron transfer,mass transfer,and physical/chemical stability are summarized.Furthermore,the design principles were pointed out for obtaining efficient and robust OER electrocatalysts in light of recent progress of OER electrocatalysts working above 1000 mA cm^(-2).These include the aspects of developing self-supported catalytic electrodes,enhancing intrinsic activity,enhancing the catalyst-support interaction,engineering surface wettability,and introducing protective layer.Finally,summaries and outlooks in achieving OER at industrially relevant HCDs are proposed.展开更多
Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-laye...Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.展开更多
The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali electrolysis.Currently,the endeavor to fabricate electrodes capable of yielding high current ...The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali electrolysis.Currently,the endeavor to fabricate electrodes capable of yielding high current density at minimal overpotential remains a central challenge in advancing the realm of chlorine evolution reactions.Here,we grow TiO_(2)and RuO_(2)on MXene@carbon cloth(CC)through the favorable affinity and induced deposition effect between the surface functional groups of MXene and the metal.A self-supported electrode(RuTiO_(2)/MXene@CC)with strong binding at the electrocatalyst-support interface and weak adhesion at electrocatalyst-bubble interface is constructed.The RuTiO_(2)/MXene@CC can reduce the electron density of RuO_(2)by regulating the electron redistribution at the heterogeneous interface,thus enhancing the adsorption of Cl−.RuTiO_(2)/MXene@CC could achieve a high current density of 1000 mA·cm^(−2)at a small overpotential of 220 mV,superior to commercial dimensionally stable anodes(DSA).This study provides a new strategy for constructing efficient CER catalysts at high current density.展开更多
Deliberate modulation of the electronic structure via interface engineering is one of promising perspectives to build advanced catalysts for urea oxidation reaction(UOR)at high current densities.However,it still remai...Deliberate modulation of the electronic structure via interface engineering is one of promising perspectives to build advanced catalysts for urea oxidation reaction(UOR)at high current densities.However,it still remains some challenges originating from the intrinsically sluggish UOR dynamics and the high energy barrier for urea adsorption.In response,we report the coupled NiSe_(2)nanowrinkles with Ni_(5)P_(4)nanorods heterogeneous structure onto Ni foam(denoted as NiSe_(2)@Ni_(5)P_(4)/NF)through successive phosphorization and selenization strategy,in which the produced closely contacted interface could provide high-flux electron transfer pathways.Theoretical findings decipher that the fast charge transfer takes place at the interfacial region from Ni_(5)P_(4)to NiSe_(2),which is conducive to optimizing adsorption energy of urea molecules.As expected,the well-designed NiSe_(2)@Ni_(5)P_(4)/NF only requires the low potential of 1.402 V at the current density of 500 mA·cm^(-2).More importantly,a small Tafel slope of 27.6 mV·dec^(-1),a high turnover frequency(TOF)value of 1.037 s^(-1)as well as the prolonged stability of 950 h at the current density of 100 mA·cm^(-2)are also achieved.This study enriches the understanding on the electronic structure modulation via interface engineering and offers bright prospect to design advanced UOR catalysts.展开更多
Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange memb...Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.展开更多
Developing highly efficient nickel or iron based hydroxide electrocatalysts is primary essential but challenging for oxygen evolution reaction(OER)at ultra-high current densities.Herein,we developed a facile method to...Developing highly efficient nickel or iron based hydroxide electrocatalysts is primary essential but challenging for oxygen evolution reaction(OER)at ultra-high current densities.Herein,we developed a facile method to prepare nitrogen and iron doped nickel(Ⅱ)hydroxide nanosheets on self-supported conductive nickel foam(denoted as Fe,N-Ni(OH)_(2)/NF)through ammonia hydrothermal and impregnation methods.Owing to the optimization of the electronic structure by nitrogen doping and the strong synergistic effect between Fe and Ni(OH)_(2),the three-dimensional(3 D)Fe,N-Ni(OH)_(2)/NF nanosheets delivered superior electrocatalytic OER performances in basic solution with low potentials of 1.57 V and1.59 V under 500 mA/cm^(2)and 1000 mA/cm^(2)respectively and robust operation for 10 h with ignored activity decay,comparing well with the potentials of previously reported NiFe based electrocatalysts as well as the benchmark commercial Ir/C/NF.In-situ Raman spectroscopy revealed that the main active species were NiOOH during the OER process.The present results are expected to provide new insights into the study of OER process towards ultra-high current densities.展开更多
The Nd:TiO_(2 )PEO coatings were formed in a phosphate-based electrolyte with the addition of Nd_(2)O_(3 )under the current density of 150,200,250 and 300 m A/cm^(2).SEM results showed that the micropores decreased on...The Nd:TiO_(2 )PEO coatings were formed in a phosphate-based electrolyte with the addition of Nd_(2)O_(3 )under the current density of 150,200,250 and 300 m A/cm^(2).SEM results showed that the micropores decreased on quantity and increased on scale with the increasing current density.AFM results revealed that the roughness of the coatings increased with the increasing current density.Phase and composition analysis showed that the Nd:TiO_(2) coatings were mainly composed of anatase and rutile phase.And the anatase phase content has reached the maximum value at the current density of 250 m A/cm^(2).XPS results indicated that Ti2p spin-orbit components of the Nd:TiO_(2) coatings are shifted towards higher binding energy,compared with the pure TiO_(2) coating,suggesting that some of the Nd^(3+)ions are combined with TiO_(2) lattice and led to dislocation.Photocatalytic test showed that the photocatalytic activity of Nd:TiO_(2) coatings varied in the same pattern with the anatase content variation in Nd:TiO_(2) coatings.The photocatalytic experiment results show that the photocatalytic activity of Nd:TiO_(2) coatings can be greatly enhanced with moderate amount of Nd^(3+).However,excessive amount of Nd^(3+)does not have an effective impact on the photoctalytic activity improvement.展开更多
Many magnetohydrodynamic stability analyses require generation of a set of equilibria with a fixed safety factor q-profile while varying other plasma parameters.A neural network(NN)-based approach is investigated that...Many magnetohydrodynamic stability analyses require generation of a set of equilibria with a fixed safety factor q-profile while varying other plasma parameters.A neural network(NN)-based approach is investigated that facilitates such a process.Both multilayer perceptron(MLP)-based NN and convolutional neural network(CNN)models are trained to map the q-profile to the plasma current density J-profile,and vice versa,while satisfying the Grad–Shafranov radial force balance constraint.When the initial target models are trained,using a database of semianalytically constructed numerical equilibria,an initial CNN with one convolutional layer is found to perform better than an initial MLP model.In particular,a trained initial CNN model can also predict the q-or J-profile for experimental tokamak equilibria.The performance of both initial target models is further improved by fine-tuning the training database,i.e.by adding realistic experimental equilibria with Gaussian noise.The fine-tuned target models,referred to as fine-tuned MLP and fine-tuned CNN,well reproduce the target q-or J-profile across multiple tokamak devices.As an important application,these NN-based equilibrium profile convertors can be utilized to provide a good initial guess for iterative equilibrium solvers,where the desired input quantity is the safety factor instead of the plasma current density.展开更多
The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past...The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.展开更多
In this work,we reported a series of monolithic 3D-printed Ni-Mo alloy electrodes for highly efficient water splitting at high current density(1500 mA cm^(-2))with excellent stability,which provides a solution to scal...In this work,we reported a series of monolithic 3D-printed Ni-Mo alloy electrodes for highly efficient water splitting at high current density(1500 mA cm^(-2))with excellent stability,which provides a solution to scale up Ni-Mo catalysts for HER to industry use.All possible Ni-Mo metal/alloy phases were achieved by tuning the atomic composition and heat treatment procedure,and they were investigated through both experiment and simulation,and the optimal NiMo phase shows the best performance.Density functional theory(DFT)calculations elucidate that the NiMo phase has the lowest H2O dissociation energy,which further explains the exceptional performance of NiMo.In addition,the microporosity was modulated via controlled thermal treatment,indicating that the 1100℃sintered sample has the best catalytic performance,which is attributed to the high electrochemically active surface area(ECSA).Finally,the four different macrostructures were achieved by 3D printing,and they further improved the catalytic performance.The gyroid structure exhibits the best catalytic performance of driving 500 mA cm^(-2)at a low overpotential of 228 mV and 1500 mA cm^(-2)at 325 mV,as it maximizes the efficient bubble removal from the electrode surface,which offers the great potential for high current density water splitting.展开更多
Plasma electrolytic oxidation (PEO) ceramic coatings were fabricated in a silicate-based electrolyte with the addition of potassium fluorozirconate (K2ZrF6) on 6063 aluminum alloy, and the effects of current density o...Plasma electrolytic oxidation (PEO) ceramic coatings were fabricated in a silicate-based electrolyte with the addition of potassium fluorozirconate (K2ZrF6) on 6063 aluminum alloy, and the effects of current density on microstructure and properties of the PEO coatings were studied. It was found that pore density of the coatings decreased with increasing the current density. The tribological and hardness tests suggested that the ceramic coating produced under the current density of 15 A/dm2showed the best mechanical property, which matched well with the phase analysis. Electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization curves proved that the coating obtained under 15 A/dm2 displayed the best anti-corrosion property, which was directly connected with morphologies of coatings.展开更多
Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique...Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique. The effects of current density on the chemical composition, electrocatalytic activity, and stability of the composite anode material were investigated by energy dispersive X-ray spectroscopy(EDXS), anode polarization curves, quasi-stationary polarization(Tafel) curves, electrochemical impedance spectroscopy(EIS), scanning electron microscopy(SEM), and X-ray diffraction(XRD). Results reveal that the composite electrode obtained at 1 A/dm2 possesses the lowest overpotential(0.610 V at 500 A/m2) for oxygen evolution, the best electrocatalytic activity, the longest service life(360 h at 40 °C in 150 g/L H2SO4 solution under 2 A/cm2), and the lowest cell voltage(2.75 V at 500 A/m2). Furthermore, with increasing current density, the coating exhibits grain growth and the decrease of content of Mn O2. Only a slight effect on crystalline structure is observed.展开更多
AlAs/GaAs/In0.1Ga0.9As/GaAs/AlAs double-barrier resonant tunneling diodes (DBRTDs) grown on a semi-insulated GaAs substrate with molecular beam epitaxy is demonstrated. By sandwiching the In0.1 Ga0.9 As layer betwee...AlAs/GaAs/In0.1Ga0.9As/GaAs/AlAs double-barrier resonant tunneling diodes (DBRTDs) grown on a semi-insulated GaAs substrate with molecular beam epitaxy is demonstrated. By sandwiching the In0.1 Ga0.9 As layer between GaAs layers, potential wells beside the two sides of barrier are deepened, resulting in an increase of the peak-to-valley current ratio (PVCR) and a peak current density. A special shape of collector is designed in order to reduce contact resistance and non-uniformity of the current;as a result the total chrrent density in the device is increased. The use of thin barriers is also helpful for the improvement of the PVCR and the peak current density in DBRTDs. The devices exhibit a maximum PVCR of 13.98 and a peak current density of 89kA/cm^2 at room temperature.展开更多
Developing highly effective and stable non-noble metalbased bifunctional catalyst working at high current density is an urgent issue for water electrolysis(WE).Herein,we prepare the N-doped graphene-decorated NiCo all...Developing highly effective and stable non-noble metalbased bifunctional catalyst working at high current density is an urgent issue for water electrolysis(WE).Herein,we prepare the N-doped graphene-decorated NiCo alloy coupled with mesoporous NiCoMoO nano-sheet grown on 3D nickel foam(NiCo@C-NiCoMoO/NF)for water splitting.NiCo@C-NiCoMoO/NF exhibits outstanding activity with low overpotentials for hydrogen and oxygen evolution reaction(HER:39/266 mV;OER:260/390 mV)at±10 and±1000 mA cm^(−2).More importantly,in 6.0 M KOH solution at 60℃ for WE,it only requires 1.90 V to reach 1000 mA cm−2 and shows excellent stability for 43 h,exhibiting the potential for actual application.The good performance can be assigned to N-doped graphene-decorated NiCo alloy and mesoporous NiCoMoO nano-sheet,which not only increase the intrinsic activity and expose abundant catalytic activity sites,but also enhance its chemical and mechanical stability.This work thus could provide a promising material for industrial hydrogen production.展开更多
In this work, analysis of electromigration-induced void morphological evolution in solder interconnects is performed based on mass diffusion theory. The analysis is conducted for three typical experimentally observed ...In this work, analysis of electromigration-induced void morphological evolution in solder interconnects is performed based on mass diffusion theory. The analysis is conducted for three typical experimentally observed void shapes: circular, ellipse, and cardioid. Void morphological evolution is governed by the competition between the electric field and surface capillary force. In the developed model, both the electric field and capillary force on the void's surface are solved analytically. Based on the mass conversation principle, the normal velocity on the void surface during diffusion is obtained. The void morphological evolution behavior is investigated, and a physical model is developed to predict void collapse to a crack or to split into sub-voids under electric current. It is noted that when the electric current is being applied from the horizontal direction, a circular void may either move stably along the electric current direction or collapse to a finger shape, depending on the relative magnitude of the electric current and surface capillary force. However, the elliptical-shaped void will elongate along the electric current direction and finally collapse to the finger shape. On the other hand, the cardioid-shaped void could bifurcate into two sub-voids when the electric current reaches a critical value. The theoretical predictions agree well with the experimental observations.展开更多
Oxide coatings were prepared on magnesium alloys in electrolyte solution of Na2SiO3 at different current densities(3,4 and 5 A/cm 2 )with micro-arc oxidation process.X-ray diffractometry(XRD)results show that the oxid...Oxide coatings were prepared on magnesium alloys in electrolyte solution of Na2SiO3 at different current densities(3,4 and 5 A/cm 2 )with micro-arc oxidation process.X-ray diffractometry(XRD)results show that the oxide coatings formed on magnesium alloys are mainly composed of MgO and MgAl2O4 phases;in addition,the content of MgO increases with increasing the current density.The morphology and surface roughness of the coatings were characterized by confocal laser scanning microscopy (CLSM).The results show that the surface roughness(Ra)decreases with increasing the current density.Moreover,the electrochemical corrosion results prove that the MgO coating produced in the electrolyte Na2SiO3 at current density of 5 A/cm 2 shows the best corrosion resistance.展开更多
The nanocrystalline Fe-Ni-Cr coatings were electrodeposited by using the pulse current technique.The SEM results showed that the coatings had a mixed morphology of small nodules and fine cauliflower structures at low ...The nanocrystalline Fe-Ni-Cr coatings were electrodeposited by using the pulse current technique.The SEM results showed that the coatings had a mixed morphology of small nodules and fine cauliflower structures at low current densities.Also,the Cr content was increased at expense of Fe and Ni contents at high current densities.XRD patterns confirmed that the pulse current density had a positive effect on the grain refinement.The results of vibrating sample magnetometer(VSM)measurements demonstrated that by increasing the current density,the saturation magnetization was decreased and the coercivity was increased due to the enhancement of Cr content and the reduction of the grain size.The friction coefficient and wear rate values were decreased by increasing the pulse current density.Also,both the adhesive and abrasive wear mechanisms were observed on the worn surfaces.The abrasive grooves and the amount of wear debris were decreased by increasing the pulse current density.展开更多
基金supported by the National Magnetic Confinement Fusion Science Program of China(Nos.2011GB108011 and 2010GB103001)the Major International(Regional)Project Cooperation and Exchanges of China(No.11320101005)the Startup Fund from Fuzhou University(No.510071)
文摘An experimental investigation of the saturation ion current densities (Jions) in hydrogen inductively coupled plasma (ICP) produced by a large-power (2-32 kW) radio frequency (RF) generator is reported, then some reasonable explanations are given out. With the increase of RF power, the experimental results show three stages: in the first stage (2-14 kW), the electron temperature will rise with the increase of RF power in the ICP, thus, the Jions increases continually as the electron temperature rises in the ICP. In the second stage (14 20 kW), as some H- ions lead to the mutual neutralization (MN), the slope of Jio^s variation firstly decreases then increases. In the third stage (20-32 kW), both the electronic detachment (ED) and the associative detachment (AD) in the ICP result in the destruction of H- ions, therefore, the increased amplitude of the Jions in the third stage is weaker than the one in the first stage. In addition, with the equivalent transformer model, we successfully Explain that the Jions at different radial locations in ICP has the same rule. Finally, it is found that the Jions has nothing to do with the outer/inner puffing gas pressure ratio, which is attributed to the high-speed movement of hydrogen molecules.
文摘The article theoretically studied the charge-exchange effects on space charge limitedelectron and ion current densities of non-relativistic one-dimensional slab ion diode, and comparedwith those of without charge exchange.
文摘Hydrogen evolution reaction is a critical reaction in water splitting for hydrogen production.However,developing effective and stable non‐noble‐metal electrocatalysts which work well at high current densities demanded by industry still remain great challenge.Herein,taking advantage of the highly tunable metal‐organic framework(MOF)templates,nitrogen doped binary transition metal phosphides electrocatalysts(N‐CoP_(x)/Ni_(2)P)with three‐dimensional(3D)conductive network structure were successfully synthesized.The 3D open porous channels could expose more catalytically active sites;nitrogen doping and the synergistic effect between CoP and Ni_(2)P can increase the electron density of Co atoms at active sites,further optimizing the Gibbs free energy of hydrogen(ΔGH*)and water(ΔG_(H_(2)O*)).As a result,the obtained N‐CoP_(x)/Ni_(2)P catalyst exhibits extraordinary electrocatalytic activity in a wide pH range.Especially,it requires an extremely low overpotential of 152 mV to deliver a high current density of 650 mA cm^(–2) in alkaline media.This work may shed some light on the rational design of cheap electrocatalysts and electrode materials that work well at high current densities.
基金supported by the National Natural Science Foundation of China(Grant nos.91963129 and 51776094)the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(Grant no.2018B030322001)the Basic Research Project of Science and Technology Plan of Shenzhen(Grant no.JCYJ20180504165655180).
文摘Alkaline water electrolysis provides a promising route for"green hydrogen"generation,where anodic oxygen evolution reaction(OER)plays a crucial role in coupling with cathodic hydrogen evolution reaction.To date,the development of highly active and durable OER catalysts based on earth-abundant elements has drawn wide attention;nevertheless,their performance under high current densities(HCDs≥1000 mA cm^(-2))has been less emphasized.This situation has seriously impeded large-scale electrolysis industrialization.In this review,in order to provide a guideline for designing high-performance OER electrocatalysts,the effects of HCD on catalytic performance involving electron transfer,mass transfer,and physical/chemical stability are summarized.Furthermore,the design principles were pointed out for obtaining efficient and robust OER electrocatalysts in light of recent progress of OER electrocatalysts working above 1000 mA cm^(-2).These include the aspects of developing self-supported catalytic electrodes,enhancing intrinsic activity,enhancing the catalyst-support interaction,engineering surface wettability,and introducing protective layer.Finally,summaries and outlooks in achieving OER at industrially relevant HCDs are proposed.
基金supported by the National Key Research and Development Program of China(No.2021YFA1500900)the National Natural Science Foundation of China(Nos.52071174,21832003,21972061)+1 种基金the Natural Science Foundation of Jiangsu Province,Major Project(No.BK20212005)the Foundation of Science and Technology of Suzhou(No.SYC2022102).
文摘Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis technology.Herein,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 h.The outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D architecture.Specifically,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both electrodes.This study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.
基金the National Natural Science Foundation of China(Nos.21971132,52072197,and 52272222)Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)+5 种基金Major Scientific and Technological Innovation Project(No.2019JZZY020405)Major Basic Research Program of Natural Science Foundation of Shandong Province(No.ZR2020ZD09)Taishan Scholar Young Talent Program(No.tsqn201909114)the 111 Project of China(No.D20017)Shandong Province Double-Hundred Talent Plan(No.WST2020003)State Key Laboratory of Heavy Oil Processing(No.SKLHOP202202006).
文摘The chlorine evolution reaction(CER)is a crucial step in the production of chlorine gas and active chlorine by chlor-alkali electrolysis.Currently,the endeavor to fabricate electrodes capable of yielding high current density at minimal overpotential remains a central challenge in advancing the realm of chlorine evolution reactions.Here,we grow TiO_(2)and RuO_(2)on MXene@carbon cloth(CC)through the favorable affinity and induced deposition effect between the surface functional groups of MXene and the metal.A self-supported electrode(RuTiO_(2)/MXene@CC)with strong binding at the electrocatalyst-support interface and weak adhesion at electrocatalyst-bubble interface is constructed.The RuTiO_(2)/MXene@CC can reduce the electron density of RuO_(2)by regulating the electron redistribution at the heterogeneous interface,thus enhancing the adsorption of Cl−.RuTiO_(2)/MXene@CC could achieve a high current density of 1000 mA·cm^(−2)at a small overpotential of 220 mV,superior to commercial dimensionally stable anodes(DSA).This study provides a new strategy for constructing efficient CER catalysts at high current density.
基金The authors extend their appreciation to the Deanship of Scientific Research at Imam Mohammad Ibn Saud Islamic University(IMSIU)for funding and supporting this work through Research Partnership Program(No.RP-21-09-75).
文摘Deliberate modulation of the electronic structure via interface engineering is one of promising perspectives to build advanced catalysts for urea oxidation reaction(UOR)at high current densities.However,it still remains some challenges originating from the intrinsically sluggish UOR dynamics and the high energy barrier for urea adsorption.In response,we report the coupled NiSe_(2)nanowrinkles with Ni_(5)P_(4)nanorods heterogeneous structure onto Ni foam(denoted as NiSe_(2)@Ni_(5)P_(4)/NF)through successive phosphorization and selenization strategy,in which the produced closely contacted interface could provide high-flux electron transfer pathways.Theoretical findings decipher that the fast charge transfer takes place at the interfacial region from Ni_(5)P_(4)to NiSe_(2),which is conducive to optimizing adsorption energy of urea molecules.As expected,the well-designed NiSe_(2)@Ni_(5)P_(4)/NF only requires the low potential of 1.402 V at the current density of 500 mA·cm^(-2).More importantly,a small Tafel slope of 27.6 mV·dec^(-1),a high turnover frequency(TOF)value of 1.037 s^(-1)as well as the prolonged stability of 950 h at the current density of 100 mA·cm^(-2)are also achieved.This study enriches the understanding on the electronic structure modulation via interface engineering and offers bright prospect to design advanced UOR catalysts.
基金This work was supported by the National Key R&D Program of China(2016YFB0600901)the National Natural Science Foundation of China(21573222,91545202)+4 种基金Dalian National Laboratory for Clean Energy(DNL180404,DNL201924)Dalian Institute of Chemical Physics(DMTO201702)Dalian Outstanding Young Scientist Foundation(2017RJ03)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020200)the CAS Youth Innovation Promotion(Y201938).
文摘Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years.However,the research and development of electrolyzer device for CO2RR is scarce.Here we use anion exchange membrane to develop zerogap electrolyzers for CO2RR.The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes are investigated.The Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the Cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.
文摘Developing highly efficient nickel or iron based hydroxide electrocatalysts is primary essential but challenging for oxygen evolution reaction(OER)at ultra-high current densities.Herein,we developed a facile method to prepare nitrogen and iron doped nickel(Ⅱ)hydroxide nanosheets on self-supported conductive nickel foam(denoted as Fe,N-Ni(OH)_(2)/NF)through ammonia hydrothermal and impregnation methods.Owing to the optimization of the electronic structure by nitrogen doping and the strong synergistic effect between Fe and Ni(OH)_(2),the three-dimensional(3 D)Fe,N-Ni(OH)_(2)/NF nanosheets delivered superior electrocatalytic OER performances in basic solution with low potentials of 1.57 V and1.59 V under 500 mA/cm^(2)and 1000 mA/cm^(2)respectively and robust operation for 10 h with ignored activity decay,comparing well with the potentials of previously reported NiFe based electrocatalysts as well as the benchmark commercial Ir/C/NF.In-situ Raman spectroscopy revealed that the main active species were NiOOH during the OER process.The present results are expected to provide new insights into the study of OER process towards ultra-high current densities.
基金Supported by the Open Project Foundation of Industrial Perception and Intelligent Manufacturing Equipment Engineering Research Center of Jiangsu Province (No. ZK220504)the Open Project Foundation of High-tech Key Laboratory of Agricultural Equipment and Intelligence of Jiangsu Province (No. MAET202104)+1 种基金the Open Project Foundation of Jiangsu Wind Power Engineering Technology Center (No. ZK220302)the Qing Lan Project of Jiangsu Province,China。
文摘The Nd:TiO_(2 )PEO coatings were formed in a phosphate-based electrolyte with the addition of Nd_(2)O_(3 )under the current density of 150,200,250 and 300 m A/cm^(2).SEM results showed that the micropores decreased on quantity and increased on scale with the increasing current density.AFM results revealed that the roughness of the coatings increased with the increasing current density.Phase and composition analysis showed that the Nd:TiO_(2) coatings were mainly composed of anatase and rutile phase.And the anatase phase content has reached the maximum value at the current density of 250 m A/cm^(2).XPS results indicated that Ti2p spin-orbit components of the Nd:TiO_(2) coatings are shifted towards higher binding energy,compared with the pure TiO_(2) coating,suggesting that some of the Nd^(3+)ions are combined with TiO_(2) lattice and led to dislocation.Photocatalytic test showed that the photocatalytic activity of Nd:TiO_(2) coatings varied in the same pattern with the anatase content variation in Nd:TiO_(2) coatings.The photocatalytic experiment results show that the photocatalytic activity of Nd:TiO_(2) coatings can be greatly enhanced with moderate amount of Nd^(3+).However,excessive amount of Nd^(3+)does not have an effective impact on the photoctalytic activity improvement.
基金supported by National Natural Science Foundation of China (Nos. 12205033, 12105317, 11905022 and 11975062)Dalian Youth Science and Technology Project (No. 2022RQ039)+1 种基金the Fundamental Research Funds for the Central Universities (No. 3132023192)the Young Scientists Fund of the Natural Science Foundation of Sichuan Province (No. 2023NSFSC1291)
文摘Many magnetohydrodynamic stability analyses require generation of a set of equilibria with a fixed safety factor q-profile while varying other plasma parameters.A neural network(NN)-based approach is investigated that facilitates such a process.Both multilayer perceptron(MLP)-based NN and convolutional neural network(CNN)models are trained to map the q-profile to the plasma current density J-profile,and vice versa,while satisfying the Grad–Shafranov radial force balance constraint.When the initial target models are trained,using a database of semianalytically constructed numerical equilibria,an initial CNN with one convolutional layer is found to perform better than an initial MLP model.In particular,a trained initial CNN model can also predict the q-or J-profile for experimental tokamak equilibria.The performance of both initial target models is further improved by fine-tuning the training database,i.e.by adding realistic experimental equilibria with Gaussian noise.The fine-tuned target models,referred to as fine-tuned MLP and fine-tuned CNN,well reproduce the target q-or J-profile across multiple tokamak devices.As an important application,these NN-based equilibrium profile convertors can be utilized to provide a good initial guess for iterative equilibrium solvers,where the desired input quantity is the safety factor instead of the plasma current density.
文摘The electrolysis of water powered by renewable energy sources offers a promising method of"green hydrogen"production,which is considered to be at the heart of future carbon-neutral energy systems.In the past decades,researchers have reported a number of hydrogen evolution reaction(HER)electrocatalysts with activity comparable to that of commercial Pt/C,but most of them are tested within a small current density range,typically no more than 500 mA cm^(-2).To realize the industrial application of hydrogen production from water electrolysis,it is essential to develop high-efficiency HER electrocatalysts at high current density(HCD≥500 mA cm^(-2)).Nevertheless,it remains challenging and significant to rational design HCD electrocatalysts for HER.In this paper,the design strategy of HCD electrocatalysts is discussed,and some HCD electrocatalysts for HER are reviewed in seven categories(alloy,metal oxide,metal hydroxide,metal sulfide/selenide,metal nitride,metal phosphide and other derived electrocatalysts).At the end of this article,we also pro-pose some viewpoints and prospects for the future development and research directions of HCD electrocatalysts for HER.
文摘In this work,we reported a series of monolithic 3D-printed Ni-Mo alloy electrodes for highly efficient water splitting at high current density(1500 mA cm^(-2))with excellent stability,which provides a solution to scale up Ni-Mo catalysts for HER to industry use.All possible Ni-Mo metal/alloy phases were achieved by tuning the atomic composition and heat treatment procedure,and they were investigated through both experiment and simulation,and the optimal NiMo phase shows the best performance.Density functional theory(DFT)calculations elucidate that the NiMo phase has the lowest H2O dissociation energy,which further explains the exceptional performance of NiMo.In addition,the microporosity was modulated via controlled thermal treatment,indicating that the 1100℃sintered sample has the best catalytic performance,which is attributed to the high electrochemically active surface area(ECSA).Finally,the four different macrostructures were achieved by 3D printing,and they further improved the catalytic performance.The gyroid structure exhibits the best catalytic performance of driving 500 mA cm^(-2)at a low overpotential of 228 mV and 1500 mA cm^(-2)at 325 mV,as it maximizes the efficient bubble removal from the electrode surface,which offers the great potential for high current density water splitting.
基金Project(51371039)supported by the National Natural Science Foundation of China
文摘Plasma electrolytic oxidation (PEO) ceramic coatings were fabricated in a silicate-based electrolyte with the addition of potassium fluorozirconate (K2ZrF6) on 6063 aluminum alloy, and the effects of current density on microstructure and properties of the PEO coatings were studied. It was found that pore density of the coatings decreased with increasing the current density. The tribological and hardness tests suggested that the ceramic coating produced under the current density of 15 A/dm2showed the best mechanical property, which matched well with the phase analysis. Electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization curves proved that the coating obtained under 15 A/dm2 displayed the best anti-corrosion property, which was directly connected with morphologies of coatings.
基金Projects(51004056,51004057)supported by the National Natural Science Foundation of ChinaProject(KKZ6201152009)supported by the Opening Foundation of Key Laboratory of Inorganic Coating Materials,Chinese Academy of Sciences+2 种基金Project(2010ZC052)supported by the Applied Basic Research Foundation of Yunnan Province,ChinaProject(20125314110011)supported by the Specialized Research Fund for the Doctoral Program of Higher Education,ChinaProject(2010247)supported by Analysis&Testing Foundation of Kunming University of Science and Technology,China
文摘Al/conductive coating/α-Pb O2-Ce O2-Ti O2/β-PbO 2-MnO 2-WC-Zr O2 composite electrode material was prepared on Al/conductive coating/α-PbO 2-Ce O2-Ti O2 substrate by electrochemical oxidation co-deposition technique. The effects of current density on the chemical composition, electrocatalytic activity, and stability of the composite anode material were investigated by energy dispersive X-ray spectroscopy(EDXS), anode polarization curves, quasi-stationary polarization(Tafel) curves, electrochemical impedance spectroscopy(EIS), scanning electron microscopy(SEM), and X-ray diffraction(XRD). Results reveal that the composite electrode obtained at 1 A/dm2 possesses the lowest overpotential(0.610 V at 500 A/m2) for oxygen evolution, the best electrocatalytic activity, the longest service life(360 h at 40 °C in 150 g/L H2SO4 solution under 2 A/cm2), and the lowest cell voltage(2.75 V at 500 A/m2). Furthermore, with increasing current density, the coating exhibits grain growth and the decrease of content of Mn O2. Only a slight effect on crystalline structure is observed.
文摘AlAs/GaAs/In0.1Ga0.9As/GaAs/AlAs double-barrier resonant tunneling diodes (DBRTDs) grown on a semi-insulated GaAs substrate with molecular beam epitaxy is demonstrated. By sandwiching the In0.1 Ga0.9 As layer between GaAs layers, potential wells beside the two sides of barrier are deepened, resulting in an increase of the peak-to-valley current ratio (PVCR) and a peak current density. A special shape of collector is designed in order to reduce contact resistance and non-uniformity of the current;as a result the total chrrent density in the device is increased. The use of thin barriers is also helpful for the improvement of the PVCR and the peak current density in DBRTDs. The devices exhibit a maximum PVCR of 13.98 and a peak current density of 89kA/cm^2 at room temperature.
基金supported by the National Natural Science Foundation of China(21872040)the Hundred Talents Program of Guangxi Universitiesthe Excellent Scholars and Innovation Team of Guangxi Universities。
文摘Developing highly effective and stable non-noble metalbased bifunctional catalyst working at high current density is an urgent issue for water electrolysis(WE).Herein,we prepare the N-doped graphene-decorated NiCo alloy coupled with mesoporous NiCoMoO nano-sheet grown on 3D nickel foam(NiCo@C-NiCoMoO/NF)for water splitting.NiCo@C-NiCoMoO/NF exhibits outstanding activity with low overpotentials for hydrogen and oxygen evolution reaction(HER:39/266 mV;OER:260/390 mV)at±10 and±1000 mA cm^(−2).More importantly,in 6.0 M KOH solution at 60℃ for WE,it only requires 1.90 V to reach 1000 mA cm−2 and shows excellent stability for 43 h,exhibiting the potential for actual application.The good performance can be assigned to N-doped graphene-decorated NiCo alloy and mesoporous NiCoMoO nano-sheet,which not only increase the intrinsic activity and expose abundant catalytic activity sites,but also enhance its chemical and mechanical stability.This work thus could provide a promising material for industrial hydrogen production.
基金supported by the National Natural Science Foundation of China (Grant 11572249)the Aerospace Technology Foundation (Grant N2014KC0068)the Aeronautical Science Foundation of China (Grant N2014KC0073)
文摘In this work, analysis of electromigration-induced void morphological evolution in solder interconnects is performed based on mass diffusion theory. The analysis is conducted for three typical experimentally observed void shapes: circular, ellipse, and cardioid. Void morphological evolution is governed by the competition between the electric field and surface capillary force. In the developed model, both the electric field and capillary force on the void's surface are solved analytically. Based on the mass conversation principle, the normal velocity on the void surface during diffusion is obtained. The void morphological evolution behavior is investigated, and a physical model is developed to predict void collapse to a crack or to split into sub-voids under electric current. It is noted that when the electric current is being applied from the horizontal direction, a circular void may either move stably along the electric current direction or collapse to a finger shape, depending on the relative magnitude of the electric current and surface capillary force. However, the elliptical-shaped void will elongate along the electric current direction and finally collapse to the finger shape. On the other hand, the cardioid-shaped void could bifurcate into two sub-voids when the electric current reaches a critical value. The theoretical predictions agree well with the experimental observations.
基金Project(20080505)supported by Science and Technology Department of Jilin Province,China
文摘Oxide coatings were prepared on magnesium alloys in electrolyte solution of Na2SiO3 at different current densities(3,4 and 5 A/cm 2 )with micro-arc oxidation process.X-ray diffractometry(XRD)results show that the oxide coatings formed on magnesium alloys are mainly composed of MgO and MgAl2O4 phases;in addition,the content of MgO increases with increasing the current density.The morphology and surface roughness of the coatings were characterized by confocal laser scanning microscopy (CLSM).The results show that the surface roughness(Ra)decreases with increasing the current density.Moreover,the electrochemical corrosion results prove that the MgO coating produced in the electrolyte Na2SiO3 at current density of 5 A/cm 2 shows the best corrosion resistance.
文摘The nanocrystalline Fe-Ni-Cr coatings were electrodeposited by using the pulse current technique.The SEM results showed that the coatings had a mixed morphology of small nodules and fine cauliflower structures at low current densities.Also,the Cr content was increased at expense of Fe and Ni contents at high current densities.XRD patterns confirmed that the pulse current density had a positive effect on the grain refinement.The results of vibrating sample magnetometer(VSM)measurements demonstrated that by increasing the current density,the saturation magnetization was decreased and the coercivity was increased due to the enhancement of Cr content and the reduction of the grain size.The friction coefficient and wear rate values were decreased by increasing the pulse current density.Also,both the adhesive and abrasive wear mechanisms were observed on the worn surfaces.The abrasive grooves and the amount of wear debris were decreased by increasing the pulse current density.