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
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
Rational design and controllable synthesis of practical electrodes with high sta bility and activity at high current density for a hydrogen evolution reaction(HER)are critical for renewable and sustainable energy conv...Rational design and controllable synthesis of practical electrodes with high sta bility and activity at high current density for a hydrogen evolution reaction(HER)are critical for renewable and sustainable energy conversion.However,high-performance TiO_(2)-based electrocatalysts for HER are quite limited,and the cat alytic active centers still remain elusive.Herein,a simple strategy is demonstrated for the synthesis of TiO_(2)-carbon composite(TiO_(2)/C)with high HER performance and stability.The remarkable HER performance of TiO_(2)/C can be ascribed to the doping of carbon atoms,which leads to stronger hybridization of Ti 3d and O 2p orbitals,thus substantially improving the electrocatalytic efficiency.This study elucidates that the hydrogen evolution activity of oxide electrocatalysts can be largely improved by regulating their electronic structures by doping carbon atoms and also provides an effective strategy for designing heterostructured electro catalysts with high catalytic activity and stability at high current density for HER.展开更多
The hydrogen-iron(HyFe)flow cell has great potential for long-duration energy storage by capitalizing on the advantages of both electrolyzers and flow batteries.However,its operation at high current density(high power...The hydrogen-iron(HyFe)flow cell has great potential for long-duration energy storage by capitalizing on the advantages of both electrolyzers and flow batteries.However,its operation at high current density(high power)and over continuous cycling testing has yet to be demonstrated.In this paper,we discuss our design and demonstration of a water management strategy that supports high current and long cycling performance of a HyFe flow cell.Water molecules associated with the movement of protons from the iron electrode to the hydrogen electrode are sufficient to hydrate the membrane and electrode at a low current density of 100 mA cm^(-2)during the charge process.At higher charge current density,more aggressive measures must be taken to counter back-diffusion driven by the acid concentration gradient between the iron and hydrogen electrodes.Our water management approach is based on water vapor feeding in the hydrogen electrode,and water evaporation in the iron electrode,thus enabling the high current density operation of 300 mA cm^(-2).展开更多
A static model of the forced cooling of inductors used for induction heating is proposed in order to achieve better coil design to prolong its lifetime and prevent failures.The main aim is to define for the most commo...A static model of the forced cooling of inductors used for induction heating is proposed in order to achieve better coil design to prolong its lifetime and prevent failures.The main aim is to define for the most common copper tubes and inductor geometries an equivalent convection heat transmission coefficient depending upon temperature and pressure of the cooling fluid,in order to model the very complex physics of forced cooling with a strongly simplified method.The model,called 'Line Region Model',considers only the coil's copper tube and its internal surface(interface copper-water)as boundary where the heat exchange conditions are imposed.展开更多
The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-...The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.展开更多
Retaining satisfactory electrocatalytic performance under high current density plays a crucial role in industrial water splitting but is still limited to the enormous energy loss because of insufficient exposure of ac...Retaining satisfactory electrocatalytic performance under high current density plays a crucial role in industrial water splitting but is still limited to the enormous energy loss because of insufficient exposure of active sites caused by the blocked mass/charge transportation at this condition.Herein,we present a freestanding lamellar nanoporous Ni-Co-Mn alloy electrode(Lnp-NCM)designed by a refined variant of the“dealloying-coarsening-dealloying”protocol for highly efficient bifunctional electrocatalyst,where large porous channels distribute on the surface and small porous channels at the interlayer.With its 3D lamellar architecture regulating,the electrocatalytic properties of the electrodes with different distances between lamellas are compared,and faster energy conversion kinetics is achieved with efficient bubble transport channels and abundant electroactive sites.Note that the optimized sample(Lnp-NCM4)is expected to be a potential bifunctional electrocatalyst with low overpotentials of 258 and 439 mV at high current densities of 1000 and 900 mA·cm^(-2)for hydrogen and oxygen evolution reactions(HER and OER),respectively.During overall water splitting in a two-electrode cell with Lnp-NCM4 as cathode and anode,it only needs an ultralow cell voltage of 1.75 V to produce 100 mA·cm^(-2)with remarkable long-term stability over 50 h.This study on lamellar nanoporous electrode design approaches industrial water splitting requirements and paves a way for developing other catalytic systems.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current ...Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.展开更多
Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, no...Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, notably, issues related to low electrical conductivity, poor catalytic activity, and stability, especially at high current density. Herein, we report the design of Ce-and Ladoped Co Ni Fe-layered double hydroxide(Ce La Co Ni Fe-LDH) nanosheets through a facile and scalable in situ self-assembly strategy that displays enhanced OER activity. Experimental and theoretical investigations provide insights into the impact of Ceand La-doping by comparing Ce Co Ni Fe-LDH, La Co Ni Fe-LDH, and pristine Co Ni Fe-LDH, all synthesized using the same methodology. These results reveal that doping Ce^(3+)and La^(3+)into Co Ni Fe-LDH substantially improves its electronic structure,resulting in enhanced conductivity, more oxygen vacancies(Vo), electron interaction, and active site formation. Consequently,significantly reduced overpotentials of 175, 314, and 424 m V at 10, 100, and 500 m A cm^(-2), respectively, and a highly stable current density of 120 h in 1 M KOH were achieved. Notably, these performance metrics surpass those of unmodified LDHs and are competitive with many lanthanide-doped transition metal-based LDH electrocatalysts, as well as noble metal catalysts like ruthenium catalysts. This work represents a pioneering effort in doping Ce^(3+)and La^(3+)ions into a functional Co Ni Fe-based electrocatalyst, offering inspiring OER performance and scalability potential.展开更多
The application of Li-O_(2)batteries(LOBs)with ultra-high theoretical energy density is limited due to the slow redox kinetics and serious side reactions,especially in high-rate cycles.Herein,CeO_(2)is constructed on ...The application of Li-O_(2)batteries(LOBs)with ultra-high theoretical energy density is limited due to the slow redox kinetics and serious side reactions,especially in high-rate cycles.Herein,CeO_(2)is constructed on the surface of Mn_(2)O_(3)through an interface engineering strategy,and Mn_(2)O_(3)@CeO_(2)heterojunction with good activity and stability at high current density is prepared.The interfacial properties of catalyst and formation mechanism of Li_(2)O_(2)are deeply studied by density functional theory(DFT)and experiments,revealing the charge-discharge reaction mechanism of LOBs.The results show that the strong electron coupling between Mn_(2)O_(3)and CeO_(2)can promote the formation of oxygen vacancies.Heterojunction combined with oxygen vacancy can improve the affinity for O_(2)and LiO_(2)reaction intermediates,inducing the formation of thin-film Li_(2)O_(2)with low potential and easy decomposition,thus improving the cycle stability at high current density.Consequently,it achieved a high specific capacity of 12545 at 1000 mA g^(-1)and good cyclability of 120 cycles at 4000 mA g^(-1).This work thus sheds light on designing efficient and stable catalysts for LOBs under high current density.展开更多
Electromigration in Cu has been extensively investigated as the root cause of typical breakdown failure in Cu interconnects. In this study Cu nanowires connected to Au electrodes are fabricated and observed using in s...Electromigration in Cu has been extensively investigated as the root cause of typical breakdown failure in Cu interconnects. In this study Cu nanowires connected to Au electrodes are fabricated and observed using in situ transmission electron microscopy to investigate the electro- and thermo-migration processes that are induced by direct current sweeps. We observe the dynamic evolution of different mass transport mechanisms. A current density on the order of 106 A/cm^2 and a temperature of approximately 400 ℃ are sufficient to induce electro- and thermo-migration, respectively. Observations of the migration processes activated by increasing temperatures indicate that the migration direction of Cu atoms is dependent on the net force from the electric field and electron wind. This work is expected to support future design efforts to improve the robustness of Cu interconnects.展开更多
Graphene has demonstrated its potential in several practical applications owing to its remarkable electronic and physical properties. In this study, we successfully fabricated a suspended graphene device with a width ...Graphene has demonstrated its potential in several practical applications owing to its remarkable electronic and physical properties. In this study, we successfully fabricated a suspended graphene device with a width down to 20 nm. The morphological evolution of graphene under various electric field effects was systematically examined using an in-situ transmission electron microscope （TEM）. The hourglass-shaped graphene sample instantly broke apart at 7.5 mA, indicating an impressive breakdown current density. The current-carrying capacity was calculated to be -1.6 × 10^9 A.cm-2, which is several orders higher than that of copper. The current-carrying capacity depended on the resistivity of graphene. In addition, atomic volume changes occurred in the multilayer graphene samples due to surface diffusion and Ostwald ripening （OR）, indicating that the breakdown mechanism is well approximated by the electric field. This study not only provides a theory to explain the breakdown behavior but also presents the effects on materials contacted with a graphene layer used as the transmission path.展开更多
The rational construction of electrocatalysts with desired features is significant but challenging for superior water splitting at high current density. Herein, amorphous Co Ni S nanosheets are synthesized on nickel f...The rational construction of electrocatalysts with desired features is significant but challenging for superior water splitting at high current density. Herein, amorphous Co Ni S nanosheets are synthesized on nickel foam(NF) through a facile structure evolution strategy and present advanced performance at high current densities in water splitting. The high catalytic activity can be attributed to the sufficient active sites exposed by the flexible amorphous configuration. Moreover, the hydrophilicity and aerophobicity of a-CoNiS/NF promote surface wettability of the self-supporting electrode and avoid the aggregation of bubbles, which expedites the diffusion of electrolyte and facilitates the mass transfer. As a result, the optimized electrode demonstrates low overpotentials of 289 and 434 m V at 500 m A/cm^(2) under alkaline conditions for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), respectively. Impressively, an electrolytic water splitting cell assembled by bifunctional a-Co Ni S/NF operates with a low cell voltage of 1.46 V@10 mA/cm^(2) and reaches 1.79 V at 500 mA/cm^(2). The strategy sheds light on a competitive platform for the reasonable design of non-precious-metal electrocatalysts under high current density.展开更多
Alkaline water electrolysis poses significant potential for large-sc ale indus trial hydrogen generation,but is impeded by the absence of an efficient electrocatalyst capable of operating at high current densities whi...Alkaline water electrolysis poses significant potential for large-sc ale indus trial hydrogen generation,but is impeded by the absence of an efficient electrocatalyst capable of operating at high current densities while maintaining with minimal overpotential.Herein,we construct a mechanically stable and highly active RuSe_(2)/MXene heterojunction electrocatalyst.A typical SC-Ti_(3)C_(2)T_(x)MXene substrate was successfully prepared by supercritical CO_(2)(SC-CO_(2))etching,combined by subsequent DMSO intercalation treatment.Further,the RuSe_(2)nanoparticles were uniformly deposited on the surface of SC-Ti_(3)C_(2)T_(x).Theoretical calculations and experimental results demonstrate that fluorine-rich MXene exhibits stable binding with the active 1T phase RuSe_(2).The as-prepared representative RuSe_(2)@SC-Ti_(3)C_(2)T_(x)-3 heterostructure showed exceptional alkaline hydrogen evolution performance,demonstrating an overpotential of 15 mV at 10 mA cm^(-2)and a Tafel slope of 21.84 mV dec^(-1),which presents excellent HER performance and stability at high-current-density conditions.Moreover,the overpotential under the current density of 500 mA cm^(-2)is merely 182 mV,and the HER efficiency remains unaffected even after 5000 cycles and 120 h of continuous testing.展开更多
We report on the room-temperature cascade laser （QCL） at λ -4.7μm. cw operation of a surface grating Both grating design and material distributed feedback （DFB） quantum optimization are used to decrease the thre...We report on the room-temperature cascade laser （QCL） at λ -4.7μm. cw operation of a surface grating Both grating design and material distributed feedback （DFB） quantum optimization are used to decrease the threshold current density and to increase the output power. For a high-reflectivity-coated 13-μm-wide and 4- mm-long laser, high wall-plug efficiency of 6% is obtained at 20℃ from a single facet producing over I W of ew output power. The threshold current density of DFB QCL is as low as 1.13kA/cm^2 at 10℃ and 1.34kA/cm2 at 30℃ in cw mode. Stable single-mode emission with a side-mode suppression ratio of about 30 dB is observed in tile working temperature range of 20-50℃.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
Powder in tube process（PIT） was adopted for the fabrication of single filament Bi-2223 tapes, and a heat treatment process including the first heat treatment（HT1）, intermediate rolling（IR）, and second heat treat...Powder in tube process（PIT） was adopted for the fabrication of single filament Bi-2223 tapes, and a heat treatment process including the first heat treatment（HT1）, intermediate rolling（IR）, and second heat treatment（HT2） was performed. The phase evolution mechanism and microstructure changes during these heat treatment processes were systematically discussed. The influences of HT1 parameters on the phase evolution process of Bi-2223 tapes were discussed. With the optimized HT1 process, a proper Bi-2223 content of about 90% was achieved. HT2 process was also optimized by adding a post annealing process. An obvious increase of current capacity was obtained due to the enhancement of intergrain connections. Single filament Bi-2223 tapes with the critical current of Ic-90 A were fabricated with the optimized sintering process.展开更多
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.
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supported bythe Natural Scientific Foundation of China(Grants 21878001,22078002,21776001,21875001,21978002,21808002,22008001,and U1710114).
文摘Rational design and controllable synthesis of practical electrodes with high sta bility and activity at high current density for a hydrogen evolution reaction(HER)are critical for renewable and sustainable energy conversion.However,high-performance TiO_(2)-based electrocatalysts for HER are quite limited,and the cat alytic active centers still remain elusive.Herein,a simple strategy is demonstrated for the synthesis of TiO_(2)-carbon composite(TiO_(2)/C)with high HER performance and stability.The remarkable HER performance of TiO_(2)/C can be ascribed to the doping of carbon atoms,which leads to stronger hybridization of Ti 3d and O 2p orbitals,thus substantially improving the electrocatalytic efficiency.This study elucidates that the hydrogen evolution activity of oxide electrocatalysts can be largely improved by regulating their electronic structures by doping carbon atoms and also provides an effective strategy for designing heterostructured electro catalysts with high catalytic activity and stability at high current density for HER.
基金support primarily from the U.S.Department of Energy Advanced Research Projects Agency-Energy 2015 OPEN program under Contract No.67995support by Energy Storage Materials Initiative(ESMI),which is a Laboratory Directed Research and Development Project at Pacific Northwest National Laboratory(PNNL).PNNL is a multiprogram national laboratory operated for the U.S.Department of Energy(DOE)by Battelle Memorial Institute under Contract no.DE-AC05-76RL01830.
文摘The hydrogen-iron(HyFe)flow cell has great potential for long-duration energy storage by capitalizing on the advantages of both electrolyzers and flow batteries.However,its operation at high current density(high power)and over continuous cycling testing has yet to be demonstrated.In this paper,we discuss our design and demonstration of a water management strategy that supports high current and long cycling performance of a HyFe flow cell.Water molecules associated with the movement of protons from the iron electrode to the hydrogen electrode are sufficient to hydrate the membrane and electrode at a low current density of 100 mA cm^(-2)during the charge process.At higher charge current density,more aggressive measures must be taken to counter back-diffusion driven by the acid concentration gradient between the iron and hydrogen electrodes.Our water management approach is based on water vapor feeding in the hydrogen electrode,and water evaporation in the iron electrode,thus enabling the high current density operation of 300 mA cm^(-2).
文摘A static model of the forced cooling of inductors used for induction heating is proposed in order to achieve better coil design to prolong its lifetime and prevent failures.The main aim is to define for the most common copper tubes and inductor geometries an equivalent convection heat transmission coefficient depending upon temperature and pressure of the cooling fluid,in order to model the very complex physics of forced cooling with a strongly simplified method.The model,called 'Line Region Model',considers only the coil's copper tube and its internal surface(interface copper-water)as boundary where the heat exchange conditions are imposed.
基金sponsored by the National Natural Science Foundation of China(Nos.5210125 and 52375422)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069,B2020208083 and E202320801).
文摘The stability and electrocatalytic efficiency of transition metal oxides for water splitting is determined by geometric and electronic structure,especially under high current densities.Herein,a newly designed lamella-heterostructured nanoporous CoFe/CoFe_(2)O_(4) and CeO_(2−x),in situ grown on nickel foam(NF),holds great promise as a high-efficient bifunctional electrocatalyst(named R-CoFe/Ce/NF)for water splitting.Experimental characterization verifies surface reconstruction from CoFe alloy/oxide to highly active CoFeOOH during in situ electrochemical polarization.By virtues of three-dimensional nanoporous architecture and abundant electroactive CoFeOOH/CeO_(2−x) heterostructure interfaces,the R-CoFe/Ce/NF electrode achieves low overpotentials for oxygen evolution(η_(10)=227 mV;η_(500)=450 mV)and hydrogen evolution(η_(10)=35 mV;η_(408)=560 mV)reactions with high normalized electrochemical active surface areas,respectively.Additionally,the alkaline full water splitting electrolyzer of R-CoFe/Ce/NF||R-CoFe/Ce/NF achieves a current density of 50 mA·cm^(−2) only at 1.75 V;the decline of activity is satisfactory after 100-h durability test at 300 mA·cm^(−2).Density functional theory also demonstrates that the electron can transfer from CeO_(2−x) by virtue of O atom to CoFeOOH at CoFeOOH/CeO_(2−x) heterointerfaces and enhancing the adsorption of reactant,thus optimizing electronic structure and Gibbs free energies for the improvement of the activity for water splitting.
基金supported by the National Natural Science Foundation of China(No.52101251)the Science Research Project of Hebei Education Department(No.BJK2023058)the Natural Science Foundation of Hebei Province(Nos.E2020208069 and B2020208083).
文摘Retaining satisfactory electrocatalytic performance under high current density plays a crucial role in industrial water splitting but is still limited to the enormous energy loss because of insufficient exposure of active sites caused by the blocked mass/charge transportation at this condition.Herein,we present a freestanding lamellar nanoporous Ni-Co-Mn alloy electrode(Lnp-NCM)designed by a refined variant of the“dealloying-coarsening-dealloying”protocol for highly efficient bifunctional electrocatalyst,where large porous channels distribute on the surface and small porous channels at the interlayer.With its 3D lamellar architecture regulating,the electrocatalytic properties of the electrodes with different distances between lamellas are compared,and faster energy conversion kinetics is achieved with efficient bubble transport channels and abundant electroactive sites.Note that the optimized sample(Lnp-NCM4)is expected to be a potential bifunctional electrocatalyst with low overpotentials of 258 and 439 mV at high current densities of 1000 and 900 mA·cm^(-2)for hydrogen and oxygen evolution reactions(HER and OER),respectively.During overall water splitting in a two-electrode cell with Lnp-NCM4 as cathode and anode,it only needs an ultralow cell voltage of 1.75 V to produce 100 mA·cm^(-2)with remarkable long-term stability over 50 h.This study on lamellar nanoporous electrode design approaches industrial water splitting requirements and paves a way for developing other catalytic systems.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
基金the National Key Research and Development Program of China(grant no.2021YFA1501002)National Natural Science Foundation of China(grant nos.22025208,22075300,and 21902162)+1 种基金DNL Cooperation Fund,CAS(grant no.DNL202008)Chinese Academy of Sciences,and Australian Research Council(grant no.DE220100746).
文摘Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.
基金supported by the National Natural Science Foundation of China (22122113)the National Key R&D Program of China (2022YFB3506200)。
文摘Polymetallic layered double hydroxides are promising cost-effective catalysts for the oxygen evolution reaction(OER) due to their versatile anionic and cationic tunability. Nevertheless, several challenges persist, notably, issues related to low electrical conductivity, poor catalytic activity, and stability, especially at high current density. Herein, we report the design of Ce-and Ladoped Co Ni Fe-layered double hydroxide(Ce La Co Ni Fe-LDH) nanosheets through a facile and scalable in situ self-assembly strategy that displays enhanced OER activity. Experimental and theoretical investigations provide insights into the impact of Ceand La-doping by comparing Ce Co Ni Fe-LDH, La Co Ni Fe-LDH, and pristine Co Ni Fe-LDH, all synthesized using the same methodology. These results reveal that doping Ce^(3+)and La^(3+)into Co Ni Fe-LDH substantially improves its electronic structure,resulting in enhanced conductivity, more oxygen vacancies(Vo), electron interaction, and active site formation. Consequently,significantly reduced overpotentials of 175, 314, and 424 m V at 10, 100, and 500 m A cm^(-2), respectively, and a highly stable current density of 120 h in 1 M KOH were achieved. Notably, these performance metrics surpass those of unmodified LDHs and are competitive with many lanthanide-doped transition metal-based LDH electrocatalysts, as well as noble metal catalysts like ruthenium catalysts. This work represents a pioneering effort in doping Ce^(3+)and La^(3+)ions into a functional Co Ni Fe-based electrocatalyst, offering inspiring OER performance and scalability potential.
基金supported by the National Natural Science Foundation of China(22162004)the Natural Science Foundation of Guangxi Province(2022JJD120011)+1 种基金the Innovation Project of Guangxi Graduate Education(YCBZ2023012)the High-performance Computing Platform of Guangxi University.
文摘The application of Li-O_(2)batteries(LOBs)with ultra-high theoretical energy density is limited due to the slow redox kinetics and serious side reactions,especially in high-rate cycles.Herein,CeO_(2)is constructed on the surface of Mn_(2)O_(3)through an interface engineering strategy,and Mn_(2)O_(3)@CeO_(2)heterojunction with good activity and stability at high current density is prepared.The interfacial properties of catalyst and formation mechanism of Li_(2)O_(2)are deeply studied by density functional theory(DFT)and experiments,revealing the charge-discharge reaction mechanism of LOBs.The results show that the strong electron coupling between Mn_(2)O_(3)and CeO_(2)can promote the formation of oxygen vacancies.Heterojunction combined with oxygen vacancy can improve the affinity for O_(2)and LiO_(2)reaction intermediates,inducing the formation of thin-film Li_(2)O_(2)with low potential and easy decomposition,thus improving the cycle stability at high current density.Consequently,it achieved a high specific capacity of 12545 at 1000 mA g^(-1)and good cyclability of 120 cycles at 4000 mA g^(-1).This work thus sheds light on designing efficient and stable catalysts for LOBs under high current density.
文摘Electromigration in Cu has been extensively investigated as the root cause of typical breakdown failure in Cu interconnects. In this study Cu nanowires connected to Au electrodes are fabricated and observed using in situ transmission electron microscopy to investigate the electro- and thermo-migration processes that are induced by direct current sweeps. We observe the dynamic evolution of different mass transport mechanisms. A current density on the order of 106 A/cm^2 and a temperature of approximately 400 ℃ are sufficient to induce electro- and thermo-migration, respectively. Observations of the migration processes activated by increasing temperatures indicate that the migration direction of Cu atoms is dependent on the net force from the electric field and electron wind. This work is expected to support future design efforts to improve the robustness of Cu interconnects.
文摘Graphene has demonstrated its potential in several practical applications owing to its remarkable electronic and physical properties. In this study, we successfully fabricated a suspended graphene device with a width down to 20 nm. The morphological evolution of graphene under various electric field effects was systematically examined using an in-situ transmission electron microscope （TEM）. The hourglass-shaped graphene sample instantly broke apart at 7.5 mA, indicating an impressive breakdown current density. The current-carrying capacity was calculated to be -1.6 × 10^9 A.cm-2, which is several orders higher than that of copper. The current-carrying capacity depended on the resistivity of graphene. In addition, atomic volume changes occurred in the multilayer graphene samples due to surface diffusion and Ostwald ripening （OR）, indicating that the breakdown mechanism is well approximated by the electric field. This study not only provides a theory to explain the breakdown behavior but also presents the effects on materials contacted with a graphene layer used as the transmission path.
基金supported by the National Natural Science Foundation of China (Nos. 51871119, 22101132, and 22075141)Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province (No. BK20220039)+4 种基金Jiangsu Provincial Founds for Natural Science Foundation (No. BK20210311)China Postdoctoral Science Foundation (Nos. 2018M640481 and 2019T120426)the Natural Science Foundation of Jiangsu Province (No. BK20210311)Jiangsu Postdoctoral Research Fund (No. 2019K003)the Postgraduate Research & Practice Innovation Program of NUAA (No. xcxjh20210607)。
文摘The rational construction of electrocatalysts with desired features is significant but challenging for superior water splitting at high current density. Herein, amorphous Co Ni S nanosheets are synthesized on nickel foam(NF) through a facile structure evolution strategy and present advanced performance at high current densities in water splitting. The high catalytic activity can be attributed to the sufficient active sites exposed by the flexible amorphous configuration. Moreover, the hydrophilicity and aerophobicity of a-CoNiS/NF promote surface wettability of the self-supporting electrode and avoid the aggregation of bubbles, which expedites the diffusion of electrolyte and facilitates the mass transfer. As a result, the optimized electrode demonstrates low overpotentials of 289 and 434 m V at 500 m A/cm^(2) under alkaline conditions for hydrogen evolution reaction(HER) and oxygen evolution reaction(OER), respectively. Impressively, an electrolytic water splitting cell assembled by bifunctional a-Co Ni S/NF operates with a low cell voltage of 1.46 V@10 mA/cm^(2) and reaches 1.79 V at 500 mA/cm^(2). The strategy sheds light on a competitive platform for the reasonable design of non-precious-metal electrocatalysts under high current density.
基金financially supported by the China Postdoctoral Science Foundation(Nos.2021TQ0300 and 2021M702946)Henan Science and Technology Department(Nos.242102231034 and 242301420040)+1 种基金the joint project from Henan Province,the China-National Natural Science Foundation(No.U2004208)the Central Plains Science and Technology Innovation Leading Talent Project(No.234200510008)
文摘Alkaline water electrolysis poses significant potential for large-sc ale indus trial hydrogen generation,but is impeded by the absence of an efficient electrocatalyst capable of operating at high current densities while maintaining with minimal overpotential.Herein,we construct a mechanically stable and highly active RuSe_(2)/MXene heterojunction electrocatalyst.A typical SC-Ti_(3)C_(2)T_(x)MXene substrate was successfully prepared by supercritical CO_(2)(SC-CO_(2))etching,combined by subsequent DMSO intercalation treatment.Further,the RuSe_(2)nanoparticles were uniformly deposited on the surface of SC-Ti_(3)C_(2)T_(x).Theoretical calculations and experimental results demonstrate that fluorine-rich MXene exhibits stable binding with the active 1T phase RuSe_(2).The as-prepared representative RuSe_(2)@SC-Ti_(3)C_(2)T_(x)-3 heterostructure showed exceptional alkaline hydrogen evolution performance,demonstrating an overpotential of 15 mV at 10 mA cm^(-2)and a Tafel slope of 21.84 mV dec^(-1),which presents excellent HER performance and stability at high-current-density conditions.Moreover,the overpotential under the current density of 500 mA cm^(-2)is merely 182 mV,and the HER efficiency remains unaffected even after 5000 cycles and 120 h of continuous testing.
基金Supported by the National Basic Research Program of China under Grant Nos 2013CB632801 and 2013CB632803the National Natural Science Foundation of China under Grant Nos 61435014,61306058 and 61274094the Beijing Natural Science Foundation under Grant No 4144086
文摘We report on the room-temperature cascade laser （QCL） at λ -4.7μm. cw operation of a surface grating Both grating design and material distributed feedback （DFB） quantum optimization are used to decrease the threshold current density and to increase the output power. For a high-reflectivity-coated 13-μm-wide and 4- mm-long laser, high wall-plug efficiency of 6% is obtained at 20℃ from a single facet producing over I W of ew output power. The threshold current density of DFB QCL is as low as 1.13kA/cm^2 at 10℃ and 1.34kA/cm2 at 30℃ in cw mode. Stable single-mode emission with a side-mode suppression ratio of about 30 dB is observed in tile working temperature range of 20-50℃.
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Funded by the National Natural Science Foundation of China(No.51472206)the National ITER Program of China(2015GB115001)the Program for Innovative Research Team in Shaanxi Province(No.2013KCT-07)
文摘Powder in tube process（PIT） was adopted for the fabrication of single filament Bi-2223 tapes, and a heat treatment process including the first heat treatment（HT1）, intermediate rolling（IR）, and second heat treatment（HT2） was performed. The phase evolution mechanism and microstructure changes during these heat treatment processes were systematically discussed. The influences of HT1 parameters on the phase evolution process of Bi-2223 tapes were discussed. With the optimized HT1 process, a proper Bi-2223 content of about 90% was achieved. HT2 process was also optimized by adding a post annealing process. An obvious increase of current capacity was obtained due to the enhancement of intergrain connections. Single filament Bi-2223 tapes with the critical current of Ic-90 A were fabricated with the optimized sintering process.
