Exploiting efficient urea oxidation reaction(UOR)and hydrogen evolution reaction(HER)catalysts are significant for energy-saving H2 production through urea-assisted water electrolysis,but it is still challenging.Herei...Exploiting efficient urea oxidation reaction(UOR)and hydrogen evolution reaction(HER)catalysts are significant for energy-saving H2 production through urea-assisted water electrolysis,but it is still challenging.Herein,carbon-encapsulated CoNi coupled with CoNiMoO(CoNi@CN-CoNiMoO)is prepared by solvothermal method and calcination to enhance the activity/stability of urea-assisted water electrolysis at large current density.It exhibits good activity for UOR(E10/1,000=1.29/1.40 V)and HER(E-10/-1000=-45/-245 mV)in 1.0 M KOH+0.5 M urea solution.For the UOR||HER system,CoNi@CN-CoNiMoO only needs 1.58 V at 500 mA cm-2 and shows good stability.Density functional theory calculation suggests that the strong electronic interaction at the interface between NiCo alloy and N-doping-carbon layers can optimize the adsorption/desorption energy of UOR/HER intermediates and accelerate the water dissociation,which can expedite urea decomposition and Volmer step,thus increasing the UOR and HER activity,respectively.This work provides a new solution to design UOR/HER catalysts for H2 production through urea-assisted water electrolysis.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
Developing the high activity,low cost and robust large-current-density-based electrocatalysts is of great significance for the industrial electrolytic water splitting.However,the current range of most reported materia...Developing the high activity,low cost and robust large-current-density-based electrocatalysts is of great significance for the industrial electrolytic water splitting.However,the current range of most reported materials is small,which makes it difficult for them to play their roles in practical applications.Here,a self-supported amorphous FexNi1-xMo O4/IF treated with ammonium fluoride (AF_(0.1)-FNMO/IF) is synthesized by one-step hydrothermal method.With the help of NH4F,AF_(0.1)-FNMO/IF exhibits a vertically cross-linked nanosheet with spherical structure.Electrochemical measurement shows that AF_(0.1)-FNMO/IF affords a large current density ordeal and only need low overpotentials of 289 and 345 m V to reach a current response of 500 m A/cm ^(2)for oxygen evolution reaction and hydrogen evolution reaction,respectively,together with long-time stability (both at 500,1000 and 2000 m A/cm ^(2)) in 1.0 mol/L KOH solution.Using it as bifunctional catalyst for overall water splitting,the current densities of 100,500,1000 and1500 m A/cm ^(2)are achieved at a cell voltage of 1.71,1.88,1.94 and 1.97 V with excellent durability,which is much better than that of most published electrodes.The work provides valuable insight for designing higher activity nickel iron-based molybdate catalysts with large current density.展开更多
Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeW...Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeWO_(4)-WO_(3) heterostructure catalyst growing on nickel foam (FeWO_(4)-WO_(3)/NF) by a combination of hydrothermal and calcination method. It shows good catalytic activity with ultralow potentials for OER (ζ_(10) = 1.43 V, ζ_(1.000) = 1.56 V) and HzOR (ζ_(10) = −0.034 V, ζ_(1.000) = 0.164 V). Moreover, there is little performance degradation after being tested for _(10)0 h at 1,000 (OER) and _(10)0 (HzOR) mA·cm−2, indicating good stability. The superior performance could be attributed to the wolframite structure and heterostructure: The former provides a high electrical conductivity to ensure the electronic transfer capability, and the later induces interfacial electron redistribution to enhance the intrinsic activity and stability. The work offers a brand-new way to prepare good performance catalysts for OER and HzOR, especially at large current density.展开更多
Highly efficient and stable bifunctional electrocatalysts that can be used for large-current-density electrolysis of alkaline seawater are highly desirable for carbon-neutral economies,but their facile and controllabl...Highly efficient and stable bifunctional electrocatalysts that can be used for large-current-density electrolysis of alkaline seawater are highly desirable for carbon-neutral economies,but their facile and controllable synthesis remains a challenge.Here,self-assembled ultralow Ru,Ni-doped Fe_(2)O_(3) with a lily shaped morphology was synthesized on iron foam(RuNi-Fe_(2)O_(3)/IF)via a facile one-step hydrothermal process,in which the intact lily shaped RuNi-Fe_(2)O_(3)/IF was obtained by adjusting the ratio of Ru/Ni.Benefitting from the Ru/Ni chemical substitution,the as-synthesized RuNi-Fe_(2)O_(3)/IF can act as free-standing dual-function electrodes that are applied to electrocatalysis for the hydrogen evolution(HER)and oxygen evolution reactions(OER)in 1.0 mol L^(-1) KOH,requiring an overpotential of 75.0 mV to drive 100 mA cm^(-2) for HER and 329.0 mV for OER.Moreover,the overall water splitting catalyzed by RuNi-Fe_(2)O_(3)/IF only demands ultralow cell voltages of 1.66 and 1.73 V to drive 100 mA cm^(-2) in 1.0 mol L^(-1) KOH and 1.0 mol L^(-1) KOH seawater electrolytes,respectively.The electrodes show remarkable long-term durability,maintaining current densities exceeding 100 mA cm^(-2) for more than 100 h and thus outperforming the two-electrode system composed of noble catalysts.This work provides an efficient,economical method to synthesize self-standing bifunctional electrodes for large-current-density alkaline seawater electrolysis,which is of significant importance for ecological protection and energy exploitation.展开更多
Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic C...Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)electrocatalysts.The composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled precisely.Our results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)properties.Specifically,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without decay.The results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting.展开更多
Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based...Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.展开更多
Li-CO_(2)batteries(LCBs)suffer from high overpotentials caused by sluggish CO_(2)reaction kinetics.This work designs a Te-doped Fe_(3)O_(4)(Te-Fe_(3)O_(4))flower-like microsphere catalyst to lower the overpotential an...Li-CO_(2)batteries(LCBs)suffer from high overpotentials caused by sluggish CO_(2)reaction kinetics.This work designs a Te-doped Fe_(3)O_(4)(Te-Fe_(3)O_(4))flower-like microsphere catalyst to lower the overpotential and improve the reversibility of LCBs.Experimental results reveal that Te doping modifies the electronic structure of Fe_(3)O_(4)and reduces the overpotential.The stable Te-O bond between Te and C_(2)O^(2-)_(4)could effectively inhibit the dispro-portionation reaction of the latter,enabling the Te-Fe_(3)O_(4)cathodes to exhibit a remarkable capacity(9485 mAh g^(-1))and a long cycling life(155 cycles)with an overpotential of 1.21 V and an energy efficiency of about 80%at a high current density(2000 mA g^(-1)).Through the interaction between Te and Li_(2)C_(2)O_(4)to inhibit the dispro-portionation reaction,this work successfully achieves long-term cycling of LCBs with low overpotential at high current density.展开更多
Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni...Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni/MoO_(2) nano-needle with three-phase heterojunction(Ni/MoO_(2)@CN)for accelerating the WS under industrial alkaline condition.Density functional theory calculations reveal that the electrons are redistributed at the three-phase heterojunction interface,which optimizes the adsorption energy of H-and O-containing intermediates to obtain the best ΔG_(H*) for hydrogen evolution reaction(HER)and decrease the ΔG value of ratedetermining step for oxygen evolution reaction(OER),thus enhancing the HER/OER catalytic activity.Electrochemical results confirm that Ni/MoO_(2)@CN exhibits good activity for HER(ƞ_(-10)=33 mV,ƞ_(-1000)=267 mV)and OER(ƞ_(10)=250 mV,ƞ_(1000)=420 mV).It shows a low potential of 1.86 V at 1000 mA cm^(−2) for WS in 6.0 M KOH solution at 60℃ and can steadily operate for 330 h.This good HER/OER performance can be attributed to the three-phase heterojunction with high intrinsic activity and the self-supporting nano-needle with more active sites,faster mass diffusion,and bubbles release.This work provides a unique idea for designing high efficiency catalytic materials for WS.展开更多
Earth-abundant electrocatalysts for large-current-density water splitting under alkaline condition are desirable.Oxygen evolution reaction,which is a bottleneck of the overall water splitting,faces the problems of com...Earth-abundant electrocatalysts for large-current-density water splitting under alkaline condition are desirable.Oxygen evolution reaction,which is a bottleneck of the overall water splitting,faces the problems of complicated reconstruction and deficiency in rational design of active sites.Herein,we report a series of transition metal chalcogenides for alkaline OER.Among them,FeCoNi(S)displayed a low overpotential of 293 m V to deliver a current density of 500 m A cm^(-2),which is in the top level of non-precious metal based OER electrocatalysts.A combination of(ex)in situ characterizations and DFT calculation shows that Ni(Fe,Co)trimetallic oxyhydroxides were the active sites for highly-efficient OER.Furthermore,for FeCoNi(S),when used as a bifunctional catalyst for water splitting,it only required a cell voltage of 1.84 V to deliver~500 m A cm^(-2) with extraordinary long-term stability over 2000 h.This work provides the comprehension of high-efficiency,robust catalysts for OER and overall water splitting at large current densities in alkaline media.展开更多
The basic theory and principle of the artificial Controlled Source Radio Magneto Telluric(CSRMT) method is studied and a novel CSRMT transmitter in kH z frequency band is designed. The specific circuit and measured re...The basic theory and principle of the artificial Controlled Source Radio Magneto Telluric(CSRMT) method is studied and a novel CSRMT transmitter in kH z frequency band is designed. The specific circuit and measured results of some key modules in transmitter are presented, and some outdoor experimental tests have been carried out, which shows that the completed prototype of transmitter can generate a continuous sine current with frequency up to 35.33 k Hz, peak-to-peak amplitude up to 40 A, and realize a reliable transmitting mode with multi-frequency and high-current. The transmitter has a wide operating band, large magnetic moment and high waveform fidelity, and can meet the requirements of shallow geological exploration with high-resolution.展开更多
This study examined lightning activity and its relationship to precipitation and convective available potential energy （CAPE） in South China during 2001-12, based on data from the Guangdong Lightning Location System...This study examined lightning activity and its relationship to precipitation and convective available potential energy （CAPE） in South China during 2001-12, based on data from the Guangdong Lightning Location System, the Tropical Rainfall Measuring Mission satellite, and the ERA-Interim dataset. Two areas of high lightning density are identified： one over the Pearl River Delta, and the other to the north of Leizhou Peninsula. Large peak-current cloud-to-ground （LPCCG） lightning （〉75 kA） shows weaker land-offshore contrasts than total CG lightning, in which negative cloud-to-ground （NCG） lightning occurs more prominently than positive cloud-to-ground （PCG） lightning on land, While the frequency of total CG lightning shows a main peak in June and a second peak in August, the LPCCG lightning over land shows only a single peak in June. The ratio of positive LPCCG to total lightning is significantly greater during February-April than during other times of the year. Diurnally, CG lightning over land shows only one peak in the afternoon, whereas CG lightning offshore shows morning and afternoon peaks. The rain yield per flash is on the order of 107-108 kg per flash across the analysis region, and its spatial distribution is opposite to that of lightning density. Our data show that lightning activity over land is more sensitive than that over offshore waters to CAPE. The relationships between lightning activity and both precipitation and CAPE are associated with convection activity in the analysis region.展开更多
Cobalt-based phosphides show excellent hydrogen evolution reaction(HER)performance,however,improving the intrinsic activity and stability of it in alkaline electrolyte still remains a challenge.Herein,CoRuOH/Co_(2)P/C...Cobalt-based phosphides show excellent hydrogen evolution reaction(HER)performance,however,improving the intrinsic activity and stability of it in alkaline electrolyte still remains a challenge.Herein,CoRuOH/Co_(2)P/CF with heterojunction structure was developed by means of molten salt and rapid hydrolysis(30 s).The OH-from rapid surface hydrolysis of Co_(2)P as a hydrogen adsorption site can facilitate the formation of thin CoRuOH layer as a water dissociation site,which may bring out better synergistic effect for alkaline HER.Moreover,the covering of CoRuOH can improve the stability of Co_(2)P for HER.When drives at 100 mA/cm^(2),it only requires overpotential of 81 mV in 1.0 mol/L KOH(25℃).Even at higher current density(1000 mA/cm^(2)),CoRuOH/Co_(2)P/CF can also operate stability for at least 100 h.When coupling with NiFe-LDH/IF in a two-electrode system,the voltage of NiFe-LDH/IF(+)||CoRuOH/Co_(2)P/CF(-)at 1000 mA/cm^(2)is merely 1.77 V with 100 h,demonstrating great potential for water splitting.The implementation of this work provides a new strategy and reference for the further improvement of transition metal phosphides as HER electrocatalysts.展开更多
This paper introduces a novel hybrid FEM-BEM method for calculating 3D eddy cur-rent field. In the eddy current region, the eddy current density J is solved by the finite element method (FEM) which is discretized by b...This paper introduces a novel hybrid FEM-BEM method for calculating 3D eddy cur-rent field. In the eddy current region, the eddy current density J is solved by the finite element method (FEM) which is discretized by brick finite element mesh, while in the eddy current free re-gion, the magnetic field intensity H is solved by the boundary element method (BEM) which is dis-cretized by rectangular boundary element mesh. Under the boundary conditions, an algebraic equation group is obtained that only includes J by eliminating H. This method has many advan-tages over traditional ones, such as fewer variables, more convenient coupling between the FEM and the BEM and wider application to multiply-connected regions. The calculated values of two models are in good agreement with experimental results. This shows the validity of our method.展开更多
A 1500 mA,10 MHz self-adaptive on-time （SOT） controlled buck DC-DC converter is presented. Both a low-cost ripple compensation scheme （RCS） and a self-adaptive on-time generator （SAOTG） are proposed to solve the...A 1500 mA,10 MHz self-adaptive on-time （SOT） controlled buck DC-DC converter is presented. Both a low-cost ripple compensation scheme （RCS） and a self-adaptive on-time generator （SAOTG） are proposed to solve the system stability and frequency variation problem. Meanwhile a self-adaptive power transistor sizing （SAPTS） technique is used to optimize the efficiency especially with a heavy load. The circuit is implemented in a 2P4M 0.35μm CMOS process. A small external inductor of 0.47 μH and a capacitor of 4.7 μF are used to lower the cost of the converter and keep the output ripple to less than 10 mV. The measurement results show that the overshoot of the load transient response is 8 mV @ 200 mA step and the dynamic voltage scaling （DVS） performance is a rise of 16/zs/V and a fall of 20 μs/V. With a SAPTS technique and PFM control, the efficiency is maintained at more than 81% for a load range of 20 to 1500 mA and the peak efficiency reaches 88.43%.展开更多
The overheating problems of terminal connectors severely threaten the operation of ultra-high voltage projects and cause enormous losses of economy,so a higher currentcarrying reliability of the connectors has an impo...The overheating problems of terminal connectors severely threaten the operation of ultra-high voltage projects and cause enormous losses of economy,so a higher currentcarrying reliability of the connectors has an important engineering significance with the development of transmission capacity.In this paper,a bivariate mathematical model of contact resistance as functions of temperature and tightening torque was deduced based on the large current temperature rise tests.To perform such analysis,four typical terminal connectors,namely:overlapping terminal of aluminum plates,overlapping terminal of copper plates,overlapping terminal of plates with clad layer and overlapping terminal of copper rod with aluminum clamp,were chosen for the experiments.The changing rules of DC resistance with different tightening torques and different currents were studied.Then the empirical formula of contact resistance was deduced.Finally,temperature calculations of different terminal connectors were realized to verify the effectiveness of the bivariate mathematical model.展开更多
基金the National Natural Science Foundation of China(22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University。
文摘Exploiting efficient urea oxidation reaction(UOR)and hydrogen evolution reaction(HER)catalysts are significant for energy-saving H2 production through urea-assisted water electrolysis,but it is still challenging.Herein,carbon-encapsulated CoNi coupled with CoNiMoO(CoNi@CN-CoNiMoO)is prepared by solvothermal method and calcination to enhance the activity/stability of urea-assisted water electrolysis at large current density.It exhibits good activity for UOR(E10/1,000=1.29/1.40 V)and HER(E-10/-1000=-45/-245 mV)in 1.0 M KOH+0.5 M urea solution.For the UOR||HER system,CoNi@CN-CoNiMoO only needs 1.58 V at 500 mA cm-2 and shows good stability.Density functional theory calculation suggests that the strong electronic interaction at the interface between NiCo alloy and N-doping-carbon layers can optimize the adsorption/desorption energy of UOR/HER intermediates and accelerate the water dissociation,which can expedite urea decomposition and Volmer step,thus increasing the UOR and HER activity,respectively.This work provides a new solution to design UOR/HER catalysts for H2 production through urea-assisted water electrolysis.
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financially supported by National Natural Science Foundation of China (No. 52174283)Shandong Provincial Natural Science Foundation (No. ZR2020MB044)+1 种基金Innovation Fund Project for Graduate Students of China University of Petroleum (East China) (No. 22CX04026A)the Fundameantal Research Funds for the Central Universities。
文摘Developing the high activity,low cost and robust large-current-density-based electrocatalysts is of great significance for the industrial electrolytic water splitting.However,the current range of most reported materials is small,which makes it difficult for them to play their roles in practical applications.Here,a self-supported amorphous FexNi1-xMo O4/IF treated with ammonium fluoride (AF_(0.1)-FNMO/IF) is synthesized by one-step hydrothermal method.With the help of NH4F,AF_(0.1)-FNMO/IF exhibits a vertically cross-linked nanosheet with spherical structure.Electrochemical measurement shows that AF_(0.1)-FNMO/IF affords a large current density ordeal and only need low overpotentials of 289 and 345 m V to reach a current response of 500 m A/cm ^(2)for oxygen evolution reaction and hydrogen evolution reaction,respectively,together with long-time stability (both at 500,1000 and 2000 m A/cm ^(2)) in 1.0 mol/L KOH solution.Using it as bifunctional catalyst for overall water splitting,the current densities of 100,500,1000 and1500 m A/cm ^(2)are achieved at a cell voltage of 1.71,1.88,1.94 and 1.97 V with excellent durability,which is much better than that of most published electrodes.The work provides valuable insight for designing higher activity nickel iron-based molybdate catalysts with large current density.
基金This work is supported by the National Natural Science Foundation of China(No.21872040)the Hundred Talents Program of Guangxi Universities,the Excellent Scholars and Innovation Team of Guangxi Universities,Guangxi Major Projects of Science and Technology(No.GXMPSTAA17202032),Guangxi Ba-Gui Scholars Program.
文摘Developing high performance anode catalysts for oxygen evolution reaction (OER) and hydrazine oxidation reaction (HzOR) at large current density is an efficient pathway to produce hydrogen. Herein, we synthesize a FeWO_(4)-WO_(3) heterostructure catalyst growing on nickel foam (FeWO_(4)-WO_(3)/NF) by a combination of hydrothermal and calcination method. It shows good catalytic activity with ultralow potentials for OER (ζ_(10) = 1.43 V, ζ_(1.000) = 1.56 V) and HzOR (ζ_(10) = −0.034 V, ζ_(1.000) = 0.164 V). Moreover, there is little performance degradation after being tested for _(10)0 h at 1,000 (OER) and _(10)0 (HzOR) mA·cm−2, indicating good stability. The superior performance could be attributed to the wolframite structure and heterostructure: The former provides a high electrical conductivity to ensure the electronic transfer capability, and the later induces interfacial electron redistribution to enhance the intrinsic activity and stability. The work offers a brand-new way to prepare good performance catalysts for OER and HzOR, especially at large current density.
文摘Highly efficient and stable bifunctional electrocatalysts that can be used for large-current-density electrolysis of alkaline seawater are highly desirable for carbon-neutral economies,but their facile and controllable synthesis remains a challenge.Here,self-assembled ultralow Ru,Ni-doped Fe_(2)O_(3) with a lily shaped morphology was synthesized on iron foam(RuNi-Fe_(2)O_(3)/IF)via a facile one-step hydrothermal process,in which the intact lily shaped RuNi-Fe_(2)O_(3)/IF was obtained by adjusting the ratio of Ru/Ni.Benefitting from the Ru/Ni chemical substitution,the as-synthesized RuNi-Fe_(2)O_(3)/IF can act as free-standing dual-function electrodes that are applied to electrocatalysis for the hydrogen evolution(HER)and oxygen evolution reactions(OER)in 1.0 mol L^(-1) KOH,requiring an overpotential of 75.0 mV to drive 100 mA cm^(-2) for HER and 329.0 mV for OER.Moreover,the overall water splitting catalyzed by RuNi-Fe_(2)O_(3)/IF only demands ultralow cell voltages of 1.66 and 1.73 V to drive 100 mA cm^(-2) in 1.0 mol L^(-1) KOH and 1.0 mol L^(-1) KOH seawater electrolytes,respectively.The electrodes show remarkable long-term durability,maintaining current densities exceeding 100 mA cm^(-2) for more than 100 h and thus outperforming the two-electrode system composed of noble catalysts.This work provides an efficient,economical method to synthesize self-standing bifunctional electrodes for large-current-density alkaline seawater electrolysis,which is of significant importance for ecological protection and energy exploitation.
基金financially supported by the National Natural Science Foundation of China(Nos.52002294 and 52202111)the Key Research and Development Program of Hubei Province(No.2021BAA208)+3 种基金the Knowledge Innovation Program of Wuhan-Shuguang Project(No.2022010801020364)City University of Hong Kong Donation Research Grant(No.DON-RMG 9229021)City University of Hong Kong Donation Grant(No.9220061)City University of Hong Kong Strategic Research Grant(SRG)(No.7005505)。
文摘Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)electrocatalysts.The composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled precisely.Our results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)properties.Specifically,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without decay.The results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting.
基金supported by the National Natural Science Foundation of China(22162025,22068037)the Youth Innovation Team of Shaanxi Universities+2 种基金the Open and Innovation Fund of Hubei Three Gorges Laboratory(SK232001)the Regional Innovation Capability Leading Program of Shaanxi(2022QFY07-03,2022QFY07-06)the Shaanxi Province Training Program of Innovation and Entrepreneurship for Undergraduates(S202210719108)。
文摘Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.
基金supported by the National Natural Science Foundation of China(22162004)the Natural Science Foundation of Guangxi Province(2022JJD120011)the Innovation Project of Guangxi Graduate Education(YCBZ2023012,YCSW2023115,YCBZ2023048).
文摘Li-CO_(2)batteries(LCBs)suffer from high overpotentials caused by sluggish CO_(2)reaction kinetics.This work designs a Te-doped Fe_(3)O_(4)(Te-Fe_(3)O_(4))flower-like microsphere catalyst to lower the overpotential and improve the reversibility of LCBs.Experimental results reveal that Te doping modifies the electronic structure of Fe_(3)O_(4)and reduces the overpotential.The stable Te-O bond between Te and C_(2)O^(2-)_(4)could effectively inhibit the dispro-portionation reaction of the latter,enabling the Te-Fe_(3)O_(4)cathodes to exhibit a remarkable capacity(9485 mAh g^(-1))and a long cycling life(155 cycles)with an overpotential of 1.21 V and an energy efficiency of about 80%at a high current density(2000 mA g^(-1)).Through the interaction between Te and Li_(2)C_(2)O_(4)to inhibit the dispro-portionation reaction,this work successfully achieves long-term cycling of LCBs with low overpotential at high current density.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Hundred Talents Program of Guangxi Universities,the Excellent Scholars and Innovation Team of Guangxi Universities+1 种基金the Innovation Project of Guangxi Graduate Education(YCBZ2021011)the High-performance Computing Platform of Guangxi University.
文摘Constructing heterojunction is an effective strategy to develop high-performance non-preciousmetal-based catalysts for electrochemical water splitting(WS).Herein,we design and prepare an N-doped-carbon-encapsulated Ni/MoO_(2) nano-needle with three-phase heterojunction(Ni/MoO_(2)@CN)for accelerating the WS under industrial alkaline condition.Density functional theory calculations reveal that the electrons are redistributed at the three-phase heterojunction interface,which optimizes the adsorption energy of H-and O-containing intermediates to obtain the best ΔG_(H*) for hydrogen evolution reaction(HER)and decrease the ΔG value of ratedetermining step for oxygen evolution reaction(OER),thus enhancing the HER/OER catalytic activity.Electrochemical results confirm that Ni/MoO_(2)@CN exhibits good activity for HER(ƞ_(-10)=33 mV,ƞ_(-1000)=267 mV)and OER(ƞ_(10)=250 mV,ƞ_(1000)=420 mV).It shows a low potential of 1.86 V at 1000 mA cm^(−2) for WS in 6.0 M KOH solution at 60℃ and can steadily operate for 330 h.This good HER/OER performance can be attributed to the three-phase heterojunction with high intrinsic activity and the self-supporting nano-needle with more active sites,faster mass diffusion,and bubbles release.This work provides a unique idea for designing high efficiency catalytic materials for WS.
基金the financial support from the Hunan Provincial Science and Technology Plan Project(No.2020JJ4710)the Hunan Key Laboratory of Two-Dimensional Materials(No.2018TP1010)+1 种基金the postdoctoral research funding plan in Central South University(No.140050022)the support from National Natural Science Foundation of China(No.12004439)。
文摘Earth-abundant electrocatalysts for large-current-density water splitting under alkaline condition are desirable.Oxygen evolution reaction,which is a bottleneck of the overall water splitting,faces the problems of complicated reconstruction and deficiency in rational design of active sites.Herein,we report a series of transition metal chalcogenides for alkaline OER.Among them,FeCoNi(S)displayed a low overpotential of 293 m V to deliver a current density of 500 m A cm^(-2),which is in the top level of non-precious metal based OER electrocatalysts.A combination of(ex)in situ characterizations and DFT calculation shows that Ni(Fe,Co)trimetallic oxyhydroxides were the active sites for highly-efficient OER.Furthermore,for FeCoNi(S),when used as a bifunctional catalyst for water splitting,it only required a cell voltage of 1.84 V to deliver~500 m A cm^(-2) with extraordinary long-term stability over 2000 h.This work provides the comprehension of high-efficiency,robust catalysts for OER and overall water splitting at large current densities in alkaline media.
文摘The basic theory and principle of the artificial Controlled Source Radio Magneto Telluric(CSRMT) method is studied and a novel CSRMT transmitter in kH z frequency band is designed. The specific circuit and measured results of some key modules in transmitter are presented, and some outdoor experimental tests have been carried out, which shows that the completed prototype of transmitter can generate a continuous sine current with frequency up to 35.33 k Hz, peak-to-peak amplitude up to 40 A, and realize a reliable transmitting mode with multi-frequency and high-current. The transmitter has a wide operating band, large magnetic moment and high waveform fidelity, and can meet the requirements of shallow geological exploration with high-resolution.
基金supported by Basic Research Fund of Chinese Academy of Meteorological Sciences(Grant No.2013Z006 and 2014R017)National Key Basic Research Program of China(2014CB441402 and 2014CB441406)Technology Foundation for Selected Overseas Chinese Scholar,Ministry of Personnel of China
文摘This study examined lightning activity and its relationship to precipitation and convective available potential energy （CAPE） in South China during 2001-12, based on data from the Guangdong Lightning Location System, the Tropical Rainfall Measuring Mission satellite, and the ERA-Interim dataset. Two areas of high lightning density are identified： one over the Pearl River Delta, and the other to the north of Leizhou Peninsula. Large peak-current cloud-to-ground （LPCCG） lightning （〉75 kA） shows weaker land-offshore contrasts than total CG lightning, in which negative cloud-to-ground （NCG） lightning occurs more prominently than positive cloud-to-ground （PCG） lightning on land, While the frequency of total CG lightning shows a main peak in June and a second peak in August, the LPCCG lightning over land shows only a single peak in June. The ratio of positive LPCCG to total lightning is significantly greater during February-April than during other times of the year. Diurnally, CG lightning over land shows only one peak in the afternoon, whereas CG lightning offshore shows morning and afternoon peaks. The rain yield per flash is on the order of 107-108 kg per flash across the analysis region, and its spatial distribution is opposite to that of lightning density. Our data show that lightning activity over land is more sensitive than that over offshore waters to CAPE. The relationships between lightning activity and both precipitation and CAPE are associated with convection activity in the analysis region.
基金financially supported by the National Natural Science Foundation of China(Nos.52174283 and 52274308)。
文摘Cobalt-based phosphides show excellent hydrogen evolution reaction(HER)performance,however,improving the intrinsic activity and stability of it in alkaline electrolyte still remains a challenge.Herein,CoRuOH/Co_(2)P/CF with heterojunction structure was developed by means of molten salt and rapid hydrolysis(30 s).The OH-from rapid surface hydrolysis of Co_(2)P as a hydrogen adsorption site can facilitate the formation of thin CoRuOH layer as a water dissociation site,which may bring out better synergistic effect for alkaline HER.Moreover,the covering of CoRuOH can improve the stability of Co_(2)P for HER.When drives at 100 mA/cm^(2),it only requires overpotential of 81 mV in 1.0 mol/L KOH(25℃).Even at higher current density(1000 mA/cm^(2)),CoRuOH/Co_(2)P/CF can also operate stability for at least 100 h.When coupling with NiFe-LDH/IF in a two-electrode system,the voltage of NiFe-LDH/IF(+)||CoRuOH/Co_(2)P/CF(-)at 1000 mA/cm^(2)is merely 1.77 V with 100 h,demonstrating great potential for water splitting.The implementation of this work provides a new strategy and reference for the further improvement of transition metal phosphides as HER electrocatalysts.
文摘This paper introduces a novel hybrid FEM-BEM method for calculating 3D eddy cur-rent field. In the eddy current region, the eddy current density J is solved by the finite element method (FEM) which is discretized by brick finite element mesh, while in the eddy current free re-gion, the magnetic field intensity H is solved by the boundary element method (BEM) which is dis-cretized by rectangular boundary element mesh. Under the boundary conditions, an algebraic equation group is obtained that only includes J by eliminating H. This method has many advan-tages over traditional ones, such as fewer variables, more convenient coupling between the FEM and the BEM and wider application to multiply-connected regions. The calculated values of two models are in good agreement with experimental results. This shows the validity of our method.
文摘A 1500 mA,10 MHz self-adaptive on-time （SOT） controlled buck DC-DC converter is presented. Both a low-cost ripple compensation scheme （RCS） and a self-adaptive on-time generator （SAOTG） are proposed to solve the system stability and frequency variation problem. Meanwhile a self-adaptive power transistor sizing （SAPTS） technique is used to optimize the efficiency especially with a heavy load. The circuit is implemented in a 2P4M 0.35μm CMOS process. A small external inductor of 0.47 μH and a capacitor of 4.7 μF are used to lower the cost of the converter and keep the output ripple to less than 10 mV. The measurement results show that the overshoot of the load transient response is 8 mV @ 200 mA step and the dynamic voltage scaling （DVS） performance is a rise of 16/zs/V and a fall of 20 μs/V. With a SAPTS technique and PFM control, the efficiency is maintained at more than 81% for a load range of 20 to 1500 mA and the peak efficiency reaches 88.43%.
基金This work was supported by the National Natural Science Foundation of China(51678548)the Science and Technology Project of the State Grid Corporation of China(GC71-16-003).
文摘The overheating problems of terminal connectors severely threaten the operation of ultra-high voltage projects and cause enormous losses of economy,so a higher currentcarrying reliability of the connectors has an important engineering significance with the development of transmission capacity.In this paper,a bivariate mathematical model of contact resistance as functions of temperature and tightening torque was deduced based on the large current temperature rise tests.To perform such analysis,four typical terminal connectors,namely:overlapping terminal of aluminum plates,overlapping terminal of copper plates,overlapping terminal of plates with clad layer and overlapping terminal of copper rod with aluminum clamp,were chosen for the experiments.The changing rules of DC resistance with different tightening torques and different currents were studied.Then the empirical formula of contact resistance was deduced.Finally,temperature calculations of different terminal connectors were realized to verify the effectiveness of the bivariate mathematical model.
