Sodium-ion batteries are receiving more and more attention due to their low cost and abundant sodium storage capacity,and are considered to be a promising alternative to lithium-ion batteries.A large number of studies...Sodium-ion batteries are receiving more and more attention due to their low cost and abundant sodium storage capacity,and are considered to be a promising alternative to lithium-ion batteries.A large number of studies have shown that constructing heterostructures are considered an effective strategy to solve the hysteresis problem of electronic and ion dynamics in sodiumion battery anode materials.Herein,a nickel-cobalt bimetallic coordination polymer(NiCoCP)was synthesized using a coprecipitation method,and a CoSe_(2)@NiSe_(2) cross-stacked structure was obtained through high-temperature carbonization and selenization processes.CoSe_(2)@NiSe_(2) has a unique heterostructure and carbon film,which synergistically increases a large number of adsorption sites and alleviates the diffusion energy barrier,thereby improving the rapid diffusion kinetics of Na^(+)ions.It has superior rate performance and long-lasting cycle life.For sodium-ion batteries(SIBs),the specific capacity of CoSe_(2)@NiSe_(2) is around 460 mA h g^(-1) after 400 cycles at 1.0 A g^(-1).For potassium-ion batteries(PIBs),CoSe_(2)@NiSe_(2) also exhibits excellent cycling stability,maintaining a specific capacity of 160 mA h g^(-1) after 700 cycles at 1.0 A g^(-1).This study provides a new way to prepare metal selenide heterostructure as the promising anode material for SIBs.展开更多
A flexible electrode of nickel diselenide/carbon fiber cloth(NiSe/CFC) is fabricated at room temperature by a simple and efficient electrodeposition method. Owing to NiSecharacter of nanostructure and high conductivit...A flexible electrode of nickel diselenide/carbon fiber cloth(NiSe/CFC) is fabricated at room temperature by a simple and efficient electrodeposition method. Owing to NiSecharacter of nanostructure and high conductivity, the as-synthesized electrodes possess perfect pseudocapacitive property with high specific capacitance and excellent rate capability. In three-electrode system, the electrode specific capacitance of the NiSe/CFC electrode varies from 1058 F gto 996.3 F gat 2 A gto 10 A grespectively, which shows great rate capability. Moreover, the NiSeelectrode is assembled with an active carbon(AC) electrode to form an asymmetric supercapacitor with an extended potential window of 1.6 V. The asymmetric supercapacitor possesses an excellent energy density 32.7 Wh kgwith a power density 800 W kgat the current density of 1 A g. The nanosheet array on carbon fiber cloth with high flexibility, specific capacitance and rate capacitance render the NiSeto be regarded as the promising material for the high performance superconductor.展开更多
Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2)...Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2)consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2)catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2)exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2)for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.展开更多
Metal selenides,such as NiSe2,have exhibited great potentials as multifunctional materials for energy storage and conversation.However,the utilization of pure NiSe2 as electrode materials is limited by its poor cyclin...Metal selenides,such as NiSe2,have exhibited great potentials as multifunctional materials for energy storage and conversation.However,the utilization of pure NiSe2 as electrode materials is limited by its poor cycling stability,low electrical conductivity,and insufficient electrochemically active sites.To remedy these defects,herein,a novel NiSe2/Ti3C2Tx hybrid with strong interfacial interaction and electrical properties is fabricated,by wrapping NiSe2 octahedral crystal with ultrathin Ti3C2Tx MXene nanosheet.The NiSe2/Ti3C2Tx hybrid exhibits excellent electrochemical performance,with a high specific capacitance of 531.2 Fg-1 at1 A g-1 for supercapacitor,low overpotential of 200 mV at 10 mA g-1,and small Tafel slope of 37.7 mV dec-1 for hydrogen evolution reaction(HER).Furthermore,greater cycling stabilities for NiSe2/Ti3C2Tx hybrid in both supercapacitor and HER have also been achieved.These significant improvements compared with unmodified NiSe2 should be owing to thestrong interfacial interaction between NiSe2 octahedral crystal and Ti3C2Tx MXene,which provides enhanced conductivity,fast charge transfer as well as abundant active sites,and highlight the promising potentials in combinations of MXene with metal selenides for multifunctional applications such as energy storage and conversion.展开更多
Efficient heterogeneous catalysts play a very important role in the value‐updated green hydrogen production from urea‐containing wastewater.Herein,NiSe_(2)/MoSe_(2)heterostructured catalyst with optimized interfacia...Efficient heterogeneous catalysts play a very important role in the value‐updated green hydrogen production from urea‐containing wastewater.Herein,NiSe_(2)/MoSe_(2)heterostructured catalyst with optimized interfacial electron redistribution and urea adsorption energies via a strong built‐in electric field was demonstrated effective for the urea‐assisted water splitting reactions.Efficient catalytic performance was found on NiSe_(2)/MoSe_(2)hybrid microsphere owing to the combined merits such as the unique structure features,the strong synergetic coupling effects,the increased active sites,and the high amount of intrinsic Ni^(3+)species.Excellent urea oxidation activity was found to drive 10 mA cm^(‒2)at the potential of 1.33 V when loaded on the glassy carbon electrode,and a cell voltage of 1.47 V was required in the NiSe_(2)/MoSe_(2)||Pt/C urea‐water electrolyzer to drive 10 mA cm^(‒2),about 220 mV less than that of water electrolysis,indicating a less energy consumption technique during the electrolysis.The spectroscopic and theoretical analysis revealed the effective synergy of the Ni-Se bond and Mo-Se bond that would be promising for efficient catalyst system construction.展开更多
Nickel diselenide(NiSe_(2)) is a promising low-cost catalyst for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER),due to its suitable d-electron configuration and high electrical conductivity.S...Nickel diselenide(NiSe_(2)) is a promising low-cost catalyst for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER),due to its suitable d-electron configuration and high electrical conductivity.Several representative elements,e.g.,Co,Fe and P,have been utilized as cation or anion to promote the electrocatalytic activity of NiSe_(2) by modulating the interaction with Se element,whilst the catalyst stability is less concerned.In this work,the catalytic Ni nanoparticles were in-situ encapsulated in carbon nanotubes grown on three-dimensional conducting carbon framework.Subsequent phosphorization and selenization yield dispersed P-doped NiSe_(2) nanoparticles protected by carbon shell with highly exposed yet stable active sides,resulting in significantly promoted HER and OER activities as well as accelerated kinetics.In detail,the P-NiSe_(2)@N-CNTs/NC hybrid catalyst deliver low overpotentials of 95 and 306 mV at10 mA cm^(-2) for HER and OER in alkaline media,respectively.DFT calculations reveal that P doping reduces the electron density surrounding Ni atoms while accumulates the charges to Se, respectively,which in turn reduces the energy barriers for both water dissociation and intermediates adsorption for both HER and OER.As a concept of proof,a cell assembled by P-NiSe_(2)@N-CNTs/NC hybrid catalystbased anode and cathode performs a low applied voltage of 1.609 V to reach 10 mA cm^(-2),and outstanding long-term stability.展开更多
Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in seconda...Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.展开更多
Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to N...Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to NiSe2 nano-octahe-dra to fabricate the NiSe2-(100)/Ni(OH)2-(110)heterojunction.The heterojunction composite and Ni(OH)2(performing high electrochemical activity)is ideal high-rate battery-type supercapacitor electrode.The NiSe2/Ni(OH)2 electrode exhibits a high specific capacity of 909 C g^-1 at 1 A g^-1 and 597 C g^-1 at 20 A g^-1.The assembled asymmetric supercapacitor composed of the NiSe2/Ni(OH)2 cathode and p-phenylenediamine-functional reduced graphene oxide anode achieves an ultrahigh specific capacity of 303 C g^-1 at 1 A g^-1 and a superior energy density of 76.1 Wh kg^-1 at 906 W kg^-1,as well as an outstanding cycling stability of 82%retention for 8000 cycles at 10 A g^-1.To the best of our knowledge,this is the first example of NiSe2/Ni(OH)2 heterojunction exhibiting such remarkable supercapacitor performance.This work not only provides a promising candidate for next-generation energy storage device but also offers a possible universal strategy to fabricate metal selenides/metal hydroxides heterojunctions.展开更多
The commercialization of lithium-sulfur(Li-S) batteries is obstructed by the sluggish sulfur electrochemical reaction,severe polysulfide shuttling effect,and damaging dendritic lithium growth.Herein,a threedimensional...The commercialization of lithium-sulfur(Li-S) batteries is obstructed by the sluggish sulfur electrochemical reaction,severe polysulfide shuttling effect,and damaging dendritic lithium growth.Herein,a threedimensional(3D) conductive carbon nanofibers skeleton-based bifunctional electrode host material is fabricated,which consists of a two-dimensional(2D) ultra-thin NiSe_(2)-CoSe_(2)heterostructured nanosheet built on one-dimensional(1D) carbon nanofibers(NiSe_(2)-CoSe_(2)@CNF).When serving as cathodic host,the heterostructured NiSe_(2)-CoSe_(2)@CNF offers a synergistic function of polysulfide confinement and catalysis conversion.The S/NiSe_(2)-CoSe_(2)@CNF cathode shows outstanding cycling stability of 0.03% capacity decay rate per cycle over 500 cycles at 1 C.As anodic host,the NiSe_(2)-CoSe_(2)@CNF with high-flux Li+diffusion property and good lithiophilic capability realizes dendrite-free Li plating/stripping behavior.Benefiting from these synergistically merits,the Li-S full cell with S/NiSe_(2)-CoSe_(2)@CNFILi/NiSe_(2)-CoSe_(2)@CNF electrodes exhibits excellent electrochemical performance including a high specific capacity of1021 mA h g^(-1)over 100 cycles at 0.2 C and reversible areal capacity of 3.05 mA h cm^(-2)under a high sulfur loading of 4.33 mg cm^(-2)at 0.1 C.The pouch cell also delivers ultra-stable Li/S electrochemistry.This study demonstrates a rational and universal electrode construction strategy for developing practical and high-energy Li-S batteries.展开更多
Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and u...Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.展开更多
A heterostructured electrocatalyst of small NiSe_(2) nanoparticles confined NiMoN nanorods(NiSe_(2)-NPs/NiMoN-NRs)is prepared to accelerate both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in...A heterostructured electrocatalyst of small NiSe_(2) nanoparticles confined NiMoN nanorods(NiSe_(2)-NPs/NiMoN-NRs)is prepared to accelerate both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in a same alkaline medium.The synergistic effects caused by the combination of merits derived from NiSe_(2) and NiMoN phases trigger an optimum electronic structure with high density of state at near Fermi level and enhance adsorption free energy,thereby resulting in excellent catalytic activities and strengthened working stability.The catalyst requires a low overpotential of 58 mV for HER and 241 mV for OER to reach 10 mA cm^(−2) in 1.0 M KOH electrolyte.A twoelectrode electrolyzer based on the developed catalyst shows outstanding cell voltage of 1.51 and 1.46 V to reach 10 mA cm^(−2) in 1.0 M and 30 wt%KOH solution at 25℃ for overall water splitting,respectively.In addition,the solardriven water splitting process delivers a high solar-to-H_(2) conversion efficiency of∼18.4%,impressively unveiling that the developed bifunctional catalyst is highly potential for overall water splitting to produce green hydrogen fuel.展开更多
Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkal...Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkaline nickel-zinc batteries.Herein,we innovatively design P-NiMoO_(4)/NiSe_(2)heterostructures with rich oxygen vacancy via a selective component segregation.The P substitution in NiMoO_(4)activate Ni atoms,leading to the spin-state transition of Ni-3d orbitals from high-spin to low-spin,which promote the uniform and rapid nucleation of NiSe_(2)on the surface of NiMoO_(4)during subsequent selenization process.After selenization,the in situ formed P-NiMoO_(4)/NiSe_(2)heterostructures exhibits continuous increased unoccupied states of Ni 3d-orbitals and higher Ni valence state.The synergistic effect of P doping and selenization modulate the d-band center(ɛd)level of Ni 3d,thereby promoting d-p orbital hybridization between Ni 3d and O 2p of OH−as well as OH−adsorption ability.Consequently,the P-NiMoO_(4)/NiSe_(2)exhibits a top-level specific capacity of 390.7 mA h g^(−1)at 1 A g^(−1),2.8-fold higher than that of pristine NiMoO_(4),accompanied by remarkable rate capability and structural stability.Moreover,the assembled pouch-type battery and flexible devices demonstrate the practical application potential.This work provides fundamental insights into orbital-level engineering of battery materials for enhanced redox kinetics and cycling stability.展开更多
Developing suitable electrode materials for electrochemical energy storage devices by biomorph assisted design has become a fascinating topic due to the fantastic properties derived from bio-architectures.Herein,zephy...Developing suitable electrode materials for electrochemical energy storage devices by biomorph assisted design has become a fascinating topic due to the fantastic properties derived from bio-architectures.Herein,zephyranthes-like Co_(2)NiSe_(4)arrays grown on butterfly wings derived three-dimensional(3D)carbon framework(Z-Co_(2)NiSe_(4)/BWC)is fabricated via hydrothermal assembly and further conversion method.Benefiting from its unique structure and multi-components,the obtained Z-Co_(2)NiSe_(4)/BWC electrode for supercapacitor delivers an excellent specific capacitance of 2,280 F·g^(-1)at 1 A·g^(-1).Impressively,the constructed asymmetric supercapacitor using Co_(2)NiSe_(4)/BWC as positive electrode and activated butterfly wings carbon as negative electrode acquires a high energy density of 42.9 Wh·kg^(-1)at a power density of 800 W·kg^(-1)with robust stability of 94.6%capacitance retention at 10 A·g^(-1)after 5,000 cycles.Moreover,the Z-Co_(2)NiSe_(4)/BWC as anode for sodium-ion batteries exhibits a high specific capacity of 568 mAh·g^(-1)at 0.1 A·g^(-1)and high cycling stability(maintaining 80.1%of the second cycle after 100 cycles).The outstanding electrochemical performances are ascribed to that the synergistic effect of bimetallic selenides and N-doped carbon improves electrochemical activities and conductivity.One-dimensional(1D)nanoneedles grown on 3D porous framework increase the exposure of redox-active sites,endow adequate transmission channels of electrons/ions,and guarantee stability of the electrode during charge/discharge processes.This study will shed light on the avenue towards extending such nanohybrids to excellent energy storage applications.展开更多
Two-dimensional(2D)ternary chalcogenides have attracted great attentions because of their novel chemical and physical properties arising from the synergistic effect and stoichiometric variation with the additional thi...Two-dimensional(2D)ternary chalcogenides have attracted great attentions because of their novel chemical and physical properties arising from the synergistic effect and stoichiometric variation with the additional third element compared with their binary counterparts.Here,high-quality 2D tantalum nickel selenide(Ta_(2)NiSe_(5))nanosheets are successfully fabricated by a liquid-phase exfoliation(LPE)method.The ultrafast excited carrier relaxation time and nonlinear optical absorption response are investigated and reveal that the prepared 2D Ta_(2)NiSe_(5)nanosheets have excellent broadband saturable absorption properties,which are further illustrated by three passively Q-switched(PQS)allsolid-state lasers operating at 1.0,2.0 and 2.8μm with the Ta_(2)NiSe_(5)nanosheet-based saturable absorber(SA).Furthermore,mode-locked laser operation with the pulse width as short as 356 fs is also realized at 1.0μm.This work not only demonstrates the excellent nonlinear optical proprieties and optical modulation performance of Ta_(2)NiSe_(5),but also paves the way for exploring the photonic and optoelectronic proprieties of ternary chalcogenide materials.展开更多
基金supported by the National Natural Science Foundation of China(52472194,52101243)the Natural Science Foundation of Guangdong Province,China(2023A1515012619,2025A1515012571,2025A1515010345)the Science and Technology Planning Project of Guangzhou(202201010565).
文摘Sodium-ion batteries are receiving more and more attention due to their low cost and abundant sodium storage capacity,and are considered to be a promising alternative to lithium-ion batteries.A large number of studies have shown that constructing heterostructures are considered an effective strategy to solve the hysteresis problem of electronic and ion dynamics in sodiumion battery anode materials.Herein,a nickel-cobalt bimetallic coordination polymer(NiCoCP)was synthesized using a coprecipitation method,and a CoSe_(2)@NiSe_(2) cross-stacked structure was obtained through high-temperature carbonization and selenization processes.CoSe_(2)@NiSe_(2) has a unique heterostructure and carbon film,which synergistically increases a large number of adsorption sites and alleviates the diffusion energy barrier,thereby improving the rapid diffusion kinetics of Na^(+)ions.It has superior rate performance and long-lasting cycle life.For sodium-ion batteries(SIBs),the specific capacity of CoSe_(2)@NiSe_(2) is around 460 mA h g^(-1) after 400 cycles at 1.0 A g^(-1).For potassium-ion batteries(PIBs),CoSe_(2)@NiSe_(2) also exhibits excellent cycling stability,maintaining a specific capacity of 160 mA h g^(-1) after 700 cycles at 1.0 A g^(-1).This study provides a new way to prepare metal selenide heterostructure as the promising anode material for SIBs.
基金the financial joint support by the National Natural Science Foundation of China(nos.91422301,51472094,61474047)
文摘A flexible electrode of nickel diselenide/carbon fiber cloth(NiSe/CFC) is fabricated at room temperature by a simple and efficient electrodeposition method. Owing to NiSecharacter of nanostructure and high conductivity, the as-synthesized electrodes possess perfect pseudocapacitive property with high specific capacitance and excellent rate capability. In three-electrode system, the electrode specific capacitance of the NiSe/CFC electrode varies from 1058 F gto 996.3 F gat 2 A gto 10 A grespectively, which shows great rate capability. Moreover, the NiSeelectrode is assembled with an active carbon(AC) electrode to form an asymmetric supercapacitor with an extended potential window of 1.6 V. The asymmetric supercapacitor possesses an excellent energy density 32.7 Wh kgwith a power density 800 W kgat the current density of 1 A g. The nanosheet array on carbon fiber cloth with high flexibility, specific capacitance and rate capacitance render the NiSeto be regarded as the promising material for the high performance superconductor.
基金The work is supported by the National Natural Science Foundation of China(21972124)the Priority Academic Program Development of Jiangsu Higher Education Institution.the support of the Six Talent Peaks Project of Jiangsu Province(XCL-070-2018)。
文摘Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2)consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2)catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2)exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2)for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.
基金supported by Grants from the Danish National Research FoundationAUFFNOVA project from Aarhus Universitets Forsknings fund,EU H2020RISE 2016-MNR4SCell project+4 种基金National Natural Science Foundation of China(Nos.21528501,51272296,and 51571195)the Chongqing Graduate Student Research Innovation Project(No.CYB15046)support from the Key Program of the Chinese Academy of Sciences(KJZD-EW-M05-3)the financial support of China Scholarship Council(CSC)the support of Fundamental Research Funds for the Central Universities,China(YJ201893)
文摘Metal selenides,such as NiSe2,have exhibited great potentials as multifunctional materials for energy storage and conversation.However,the utilization of pure NiSe2 as electrode materials is limited by its poor cycling stability,low electrical conductivity,and insufficient electrochemically active sites.To remedy these defects,herein,a novel NiSe2/Ti3C2Tx hybrid with strong interfacial interaction and electrical properties is fabricated,by wrapping NiSe2 octahedral crystal with ultrathin Ti3C2Tx MXene nanosheet.The NiSe2/Ti3C2Tx hybrid exhibits excellent electrochemical performance,with a high specific capacitance of 531.2 Fg-1 at1 A g-1 for supercapacitor,low overpotential of 200 mV at 10 mA g-1,and small Tafel slope of 37.7 mV dec-1 for hydrogen evolution reaction(HER).Furthermore,greater cycling stabilities for NiSe2/Ti3C2Tx hybrid in both supercapacitor and HER have also been achieved.These significant improvements compared with unmodified NiSe2 should be owing to thestrong interfacial interaction between NiSe2 octahedral crystal and Ti3C2Tx MXene,which provides enhanced conductivity,fast charge transfer as well as abundant active sites,and highlight the promising potentials in combinations of MXene with metal selenides for multifunctional applications such as energy storage and conversion.
文摘Efficient heterogeneous catalysts play a very important role in the value‐updated green hydrogen production from urea‐containing wastewater.Herein,NiSe_(2)/MoSe_(2)heterostructured catalyst with optimized interfacial electron redistribution and urea adsorption energies via a strong built‐in electric field was demonstrated effective for the urea‐assisted water splitting reactions.Efficient catalytic performance was found on NiSe_(2)/MoSe_(2)hybrid microsphere owing to the combined merits such as the unique structure features,the strong synergetic coupling effects,the increased active sites,and the high amount of intrinsic Ni^(3+)species.Excellent urea oxidation activity was found to drive 10 mA cm^(‒2)at the potential of 1.33 V when loaded on the glassy carbon electrode,and a cell voltage of 1.47 V was required in the NiSe_(2)/MoSe_(2)||Pt/C urea‐water electrolyzer to drive 10 mA cm^(‒2),about 220 mV less than that of water electrolysis,indicating a less energy consumption technique during the electrolysis.The spectroscopic and theoretical analysis revealed the effective synergy of the Ni-Se bond and Mo-Se bond that would be promising for efficient catalyst system construction.
基金supported by the National Natural Science Foundation of China (51901055)the Natural Science Foundation of Heilongjiang Province (LH2019E025)+3 种基金the Fundamental Research Funds of the Central University, the Shenzhen Science and Technology Innovation Committee (JCYJ20200109113212238)the China Postdoctoral Science Foundation (Grant nos. 2019M651260, 2020T130139)the Heilongjiang Postdoctoral Fund (LBH-Z19009)the Heilongjiang Touyan Innovation Team Program。
文摘Nickel diselenide(NiSe_(2)) is a promising low-cost catalyst for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER),due to its suitable d-electron configuration and high electrical conductivity.Several representative elements,e.g.,Co,Fe and P,have been utilized as cation or anion to promote the electrocatalytic activity of NiSe_(2) by modulating the interaction with Se element,whilst the catalyst stability is less concerned.In this work,the catalytic Ni nanoparticles were in-situ encapsulated in carbon nanotubes grown on three-dimensional conducting carbon framework.Subsequent phosphorization and selenization yield dispersed P-doped NiSe_(2) nanoparticles protected by carbon shell with highly exposed yet stable active sides,resulting in significantly promoted HER and OER activities as well as accelerated kinetics.In detail,the P-NiSe_(2)@N-CNTs/NC hybrid catalyst deliver low overpotentials of 95 and 306 mV at10 mA cm^(-2) for HER and OER in alkaline media,respectively.DFT calculations reveal that P doping reduces the electron density surrounding Ni atoms while accumulates the charges to Se, respectively,which in turn reduces the energy barriers for both water dissociation and intermediates adsorption for both HER and OER.As a concept of proof,a cell assembled by P-NiSe_(2)@N-CNTs/NC hybrid catalystbased anode and cathode performs a low applied voltage of 1.609 V to reach 10 mA cm^(-2),and outstanding long-term stability.
基金financially supported by the Shenzhen Science and Technology Program(JCYJ20220530141012028),ChinaThe National Natural Science Foundation of China(22005178),China+2 种基金The Key Research and Development Program of Shandong Province(2021ZLGX01),ChianThe fellowship of China Postdoctoral Science Foundation(2022M722333),Chianthe Jiangsu Funding Program for Excellent Postdoctoral Talent,Chian。
文摘Hollow nanostructures with external shells and inner voids have been proved to greatly shorten the transport distance of ions/electrons and buffer volume change,especially for the large-sized potassium-ions in secondary batteries.In this work,hollow carbon(HC) nanospheres embedded with S,P co-doped NiSe_(2)nanoparticles are fabricated by "drop and dry" and "dissolving and precipitation" processes to form Ni(OH)2nanocrystals followed by annealing with S and P dopants to form nanoparticles.The resultant S,P-NiSe_(2)/HC composite exhibits excellent cyclic performance with 131.6 mA h g^(-1)at1000 mA g^(-1)after 3000 cycles for K^(+)storage and a capacity of 417.1 mA h g^(-1)at 1000 mA g^(-1)after1000 cycles for Li^(+)storage.K-ion full cells are assembled and deliver superior cycling stability with a ca pacity of 72.5 mA h g^(-1)at 200 mA g^(-1)after 500 cycles.The hollow carbon shell with excellent electrical conductivity effectively promotes the transporta tion and tolerates large volume variation for both K^(+)and Li^(+).Density functional theory calculations confirm that the S and P co-doping NiSe_(2) enables stronger adsorption of K^(+)ions and higher electrical conductivity that contributes to the improved electrochemical performance.
基金the NSFC(Grant Nos.21875285 and 21805155)Taishan Scholars Program(ts201511019)+1 种基金Key Research and Development Projects of Shandong Province(2019JZZY010331)the Fundamental Research Funds for the Central Universities(19CX05001A).
文摘Constructing heterojunction is a promising way to improve the charge transfer efficiency and can thus promote the electrochemical properties.Herein,a facile and effective epitaxial-like growth strategy is applied to NiSe2 nano-octahe-dra to fabricate the NiSe2-(100)/Ni(OH)2-(110)heterojunction.The heterojunction composite and Ni(OH)2(performing high electrochemical activity)is ideal high-rate battery-type supercapacitor electrode.The NiSe2/Ni(OH)2 electrode exhibits a high specific capacity of 909 C g^-1 at 1 A g^-1 and 597 C g^-1 at 20 A g^-1.The assembled asymmetric supercapacitor composed of the NiSe2/Ni(OH)2 cathode and p-phenylenediamine-functional reduced graphene oxide anode achieves an ultrahigh specific capacity of 303 C g^-1 at 1 A g^-1 and a superior energy density of 76.1 Wh kg^-1 at 906 W kg^-1,as well as an outstanding cycling stability of 82%retention for 8000 cycles at 10 A g^-1.To the best of our knowledge,this is the first example of NiSe2/Ni(OH)2 heterojunction exhibiting such remarkable supercapacitor performance.This work not only provides a promising candidate for next-generation energy storage device but also offers a possible universal strategy to fabricate metal selenides/metal hydroxides heterojunctions.
基金financial support from the National Natural Science Foundation of China (52102236)supported by the Foundation (KF202021) of the Key Laboratory of Pulp and Paper Science&Technology of Ministry of Education of Chinathe Overseas Faculty Supporting Project in Hebei Province (C20210335)。
文摘The commercialization of lithium-sulfur(Li-S) batteries is obstructed by the sluggish sulfur electrochemical reaction,severe polysulfide shuttling effect,and damaging dendritic lithium growth.Herein,a threedimensional(3D) conductive carbon nanofibers skeleton-based bifunctional electrode host material is fabricated,which consists of a two-dimensional(2D) ultra-thin NiSe_(2)-CoSe_(2)heterostructured nanosheet built on one-dimensional(1D) carbon nanofibers(NiSe_(2)-CoSe_(2)@CNF).When serving as cathodic host,the heterostructured NiSe_(2)-CoSe_(2)@CNF offers a synergistic function of polysulfide confinement and catalysis conversion.The S/NiSe_(2)-CoSe_(2)@CNF cathode shows outstanding cycling stability of 0.03% capacity decay rate per cycle over 500 cycles at 1 C.As anodic host,the NiSe_(2)-CoSe_(2)@CNF with high-flux Li+diffusion property and good lithiophilic capability realizes dendrite-free Li plating/stripping behavior.Benefiting from these synergistically merits,the Li-S full cell with S/NiSe_(2)-CoSe_(2)@CNFILi/NiSe_(2)-CoSe_(2)@CNF electrodes exhibits excellent electrochemical performance including a high specific capacity of1021 mA h g^(-1)over 100 cycles at 0.2 C and reversible areal capacity of 3.05 mA h cm^(-2)under a high sulfur loading of 4.33 mg cm^(-2)at 0.1 C.The pouch cell also delivers ultra-stable Li/S electrochemistry.This study demonstrates a rational and universal electrode construction strategy for developing practical and high-energy Li-S batteries.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2021QB055,ZR2023MB017,ZR2022JQ10)the National Natural Science Foundation of China(21901146,220781792,22274083)。
文摘Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.
基金supported by the Regional Leading Research Center Program(2019R1A5A8080326)BRL Program(2020R1A4A1018259)through the National Research Foundation funded by the Ministry of Science and ICT of the Republic of Korea.
文摘A heterostructured electrocatalyst of small NiSe_(2) nanoparticles confined NiMoN nanorods(NiSe_(2)-NPs/NiMoN-NRs)is prepared to accelerate both the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in a same alkaline medium.The synergistic effects caused by the combination of merits derived from NiSe_(2) and NiMoN phases trigger an optimum electronic structure with high density of state at near Fermi level and enhance adsorption free energy,thereby resulting in excellent catalytic activities and strengthened working stability.The catalyst requires a low overpotential of 58 mV for HER and 241 mV for OER to reach 10 mA cm^(−2) in 1.0 M KOH electrolyte.A twoelectrode electrolyzer based on the developed catalyst shows outstanding cell voltage of 1.51 and 1.46 V to reach 10 mA cm^(−2) in 1.0 M and 30 wt%KOH solution at 25℃ for overall water splitting,respectively.In addition,the solardriven water splitting process delivers a high solar-to-H_(2) conversion efficiency of∼18.4%,impressively unveiling that the developed bifunctional catalyst is highly potential for overall water splitting to produce green hydrogen fuel.
基金supported by the National Natural Science Foundation of China(Grant no.22209083).The authors appreciate Shiyanjia Lab(www.shiyanjia.com)for providing invaluable assistance with the science analysis.
文摘Developing high-performance Ni cathodes and understanding the relationship between electron states of Ni 3d orbital and energy storage mechanism from an atomic-orbital perspective are crucial yet challenging for alkaline nickel-zinc batteries.Herein,we innovatively design P-NiMoO_(4)/NiSe_(2)heterostructures with rich oxygen vacancy via a selective component segregation.The P substitution in NiMoO_(4)activate Ni atoms,leading to the spin-state transition of Ni-3d orbitals from high-spin to low-spin,which promote the uniform and rapid nucleation of NiSe_(2)on the surface of NiMoO_(4)during subsequent selenization process.After selenization,the in situ formed P-NiMoO_(4)/NiSe_(2)heterostructures exhibits continuous increased unoccupied states of Ni 3d-orbitals and higher Ni valence state.The synergistic effect of P doping and selenization modulate the d-band center(ɛd)level of Ni 3d,thereby promoting d-p orbital hybridization between Ni 3d and O 2p of OH−as well as OH−adsorption ability.Consequently,the P-NiMoO_(4)/NiSe_(2)exhibits a top-level specific capacity of 390.7 mA h g^(−1)at 1 A g^(−1),2.8-fold higher than that of pristine NiMoO_(4),accompanied by remarkable rate capability and structural stability.Moreover,the assembled pouch-type battery and flexible devices demonstrate the practical application potential.This work provides fundamental insights into orbital-level engineering of battery materials for enhanced redox kinetics and cycling stability.
基金The work was financially supported by the Natural Science Foundation of Jiangsu Province(No.BK20181469)the Science and Technology Planning Social Development Project of Zhenjiang City(No.SSH20190140049).
文摘Developing suitable electrode materials for electrochemical energy storage devices by biomorph assisted design has become a fascinating topic due to the fantastic properties derived from bio-architectures.Herein,zephyranthes-like Co_(2)NiSe_(4)arrays grown on butterfly wings derived three-dimensional(3D)carbon framework(Z-Co_(2)NiSe_(4)/BWC)is fabricated via hydrothermal assembly and further conversion method.Benefiting from its unique structure and multi-components,the obtained Z-Co_(2)NiSe_(4)/BWC electrode for supercapacitor delivers an excellent specific capacitance of 2,280 F·g^(-1)at 1 A·g^(-1).Impressively,the constructed asymmetric supercapacitor using Co_(2)NiSe_(4)/BWC as positive electrode and activated butterfly wings carbon as negative electrode acquires a high energy density of 42.9 Wh·kg^(-1)at a power density of 800 W·kg^(-1)with robust stability of 94.6%capacitance retention at 10 A·g^(-1)after 5,000 cycles.Moreover,the Z-Co_(2)NiSe_(4)/BWC as anode for sodium-ion batteries exhibits a high specific capacity of 568 mAh·g^(-1)at 0.1 A·g^(-1)and high cycling stability(maintaining 80.1%of the second cycle after 100 cycles).The outstanding electrochemical performances are ascribed to that the synergistic effect of bimetallic selenides and N-doped carbon improves electrochemical activities and conductivity.One-dimensional(1D)nanoneedles grown on 3D porous framework increase the exposure of redox-active sites,endow adequate transmission channels of electrons/ions,and guarantee stability of the electrode during charge/discharge processes.This study will shed light on the avenue towards extending such nanohybrids to excellent energy storage applications.
基金financially supported by the National Natural Science Foundation of China (61975095, 61675116, and 61575110)the Young Scholars Program of Shandong University (2017WLJH48)+3 种基金the Youth Cross Innovation Group of Shandong University (2020QNQT)the Key Research and Development Program of Shandong Province (2019JZZY020206)Shenzhen Science and Technology Research and Development Funds (JCYJ20180305163932273)the Program of State Key Laboratory of Quantum Optics and Quantum Optics Devices (KF201908)
文摘Two-dimensional(2D)ternary chalcogenides have attracted great attentions because of their novel chemical and physical properties arising from the synergistic effect and stoichiometric variation with the additional third element compared with their binary counterparts.Here,high-quality 2D tantalum nickel selenide(Ta_(2)NiSe_(5))nanosheets are successfully fabricated by a liquid-phase exfoliation(LPE)method.The ultrafast excited carrier relaxation time and nonlinear optical absorption response are investigated and reveal that the prepared 2D Ta_(2)NiSe_(5)nanosheets have excellent broadband saturable absorption properties,which are further illustrated by three passively Q-switched(PQS)allsolid-state lasers operating at 1.0,2.0 and 2.8μm with the Ta_(2)NiSe_(5)nanosheet-based saturable absorber(SA).Furthermore,mode-locked laser operation with the pulse width as short as 356 fs is also realized at 1.0μm.This work not only demonstrates the excellent nonlinear optical proprieties and optical modulation performance of Ta_(2)NiSe_(5),but also paves the way for exploring the photonic and optoelectronic proprieties of ternary chalcogenide materials.
