While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the ...While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the rare-earth elements were rarely concerned.Herein,we demonstrate the material synthesis and MIT properties of RENiO_(3) containing valence variable rare-earth compositions,such as Ce,Pr,Sm,Eu and Tb.The metastable perovskite structure of SmNiO_(3) and EuNiO_(3) with a rare-earth valence states variable towards+2 can be effectively synthesized under high oxygen pressures as it is necessary to reduce their formation free energies.This is in contrast to Ce and Tb,in which situations the variable rare-earth valence state towards+4 reduces their ionic radius and prohibits their occupation or co-occupation of the rare-earth site within the perovskite structured RENiO_(3).Nevertheless,PrNiO_(3) with MIT properties can be effectively synthesized at lower oxygen pressures,owing to the higher stability to form a fully occupied 6s orbit associated Pr3+compared to the half-filled one related to Pr4+.The present work provides guidance for regulating the MIT properties of RENiO_(3).展开更多
The chemical and electrochemical stability of lanthanide nickelates La2 NiO4+δ(LNO),Pr2 NiO4+δ(PNO)and their mixed compounds La(2-x)PrxNiO4+δ(LPNOs)with x=0.5,1 or 1.5 is reported.The aim is to promote these materi...The chemical and electrochemical stability of lanthanide nickelates La2 NiO4+δ(LNO),Pr2 NiO4+δ(PNO)and their mixed compounds La(2-x)PrxNiO4+δ(LPNOs)with x=0.5,1 or 1.5 is reported.The aim is to promote these materials as efficient electrodes for solid oxide fuel cell(SOFC)and/or solid oxide electrolysis cell(SOEC).La2 NiO4+δand La1.5Pr0.5NiO4+δcompounds are chemically very stable as powders over one month in the temperature range 600-800℃,while the other materials rich in praseodymium progressively decompose into various perovskite-deriving components with additional Pr6 O11.Despite their uneven properties,all these materials are quite efficient and sustainable as electrodes on top of gadolinium doped ceria(GDCBL)//yttrium doped zirconia(8 YSZ)electrolyte,for one month at 700℃without polarization.Under polarization(300 mA·cm-2),the electrochemical performances of LNO,PNO and La1.5Pr0.5NiO4+δ(LP5 NO)quickly degrade in SOFC mode,i.e.for the oxygen reduction reaction,while they show durability in SOEC mode,i.e.for the oxide oxidation reaction.展开更多
The rare-earth nickelates(RENiO_(3)) exhibit an exceptional complex electronic phase diagram and multiple electronic phase transitions that enrich promising applications in correlated electronic devices beyond convent...The rare-earth nickelates(RENiO_(3)) exhibit an exceptional complex electronic phase diagram and multiple electronic phase transitions that enrich promising applications in correlated electronic devices beyond conventional semiconductors.Nevertheless,the practical applications of RENiO_(3) are challenged by their intrinsic thermodynamic metastability in material synthesis and high material cost.Therefore,developing an economical strategy to achieve the batch synthesis of RENiO_(3) is of vital importance.In this work,we enlarged the synthesis amount of RENiO_(3) up to 20 g per batch using chloride(KCI) assisted molten salt reaction.By optimizing the reaction conditions,the powder of RENiO_(3) with the cubic shape and average size of ~2μm was effectively synthesized,while their phase purity exceeded 95%.In addition,the cost to synthesize RENiO_(3) was further reduced by using rare-earth extraction intermediate products as the raw materials,instead of using the pure rare-earth precursors.It also achieved wide adjustments in the metal-to-insulator-transition temperature from160 to 420 K without significantly reducing the transition sharpness.By enlarging the synthesis amount and the reducing the cost,it paves the way to the device application of RENiO_(3).展开更多
Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited...Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited on the direct current(DC)electrical transports.Up to date,the MIT from the perspective of alternation current(AC)transport and its potential electronic applications remains yet unclear.Herein,we demonstrate the frequency(f_(AC))dependence in the impedance(Z=Z’+iZ″)of typical MIT materials,such as thin film rare-earth nickelates(Re NiO_(3)),across the critical MIT temperature(T_(MIT)).Apart from the abrupt change in the impedance modulus(|Z|)across the critical temperature(T_(MIT))similar to the DC transport,the MIT also triggers non-continuous variation in the impedance phase(θ),and this enables the f_(AC)-regulations in the Z’-T tendencies(Z’=|Z|cosθ).At the critical f_(AC) range(e.g.,104-106 Hz),the con-versing variations in|Z|-T and cosθ-T across T_(MIT) result in non-monotonic delta-shape Z’-T tendency in Sm_(x) Nd_(1-x) NiO_(3),the full width half maximum of which is effectively narrowed compared to the situation with the absence of MIT.Further imparting lower or higher f_(AC) elevate the domination in|Z|-T and cosθ-T,respectively,but also enables abrupt Z’-T tendencies across T_(MIT) showing negative temperature coefficient of resistance(NTCR)or positive temperature coefficient of resistance(PTCR).By introducing f_(AC) as a new freedom,the MIT behavior can be more comprehensively regulated electronically,and this extends the vision in exploring the new electronic applications based on the correlated MIT materials from the AC perspective.展开更多
The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics app...The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics applications,e.g.ocean electric field sensor,bio-sensor,and neuron synapse logical devices.Nevertheless,these applications are obstructed by the present ineffectiveness in the thin film growth of the metastable RENiO_(3)with flexibly adjustable rare-earth compositions and electronic structures.Herein,we demonstrate a metal-organic decompositions(MOD)approach that can effectively grow metastable RENiO_(3)covering a large variety of the rare-earth composition without introducing any vacuum process.Unlike the previous chemical growths for RENiO_(3)relying on strict interfacial coherency that limit the film thickness,the MOD growth using reactive isooctanoate percussors is tolerant to lattice defects and therefore achieves comparable film thickness to vacuum depositions.Further indicated by positron annihilation spectroscopy,the RENiO_(3)grown by MOD exhibit large amount of lattice defects that improves their hydrogen incorporation amount and electron transfers,as demonstrated by the resonant nuclear reaction analysis and near edge X-ray absorption fine structure analysis.This effectively enlarges the magnitude in the resistance regulations in particular for RENiO_(3)with lighter RE,shedding a light on the extrinsic regulation of the hydrogen induced quantum transitions for correlated oxides semiconductors kinetically via defect engineering.展开更多
The effect of Cr addition on nickel aluminium bronze(NAB)alloy microstructure,mechanical properties,and erosion-corrosion behaviour has been studied.The results show that Cr addition does not change the composition of...The effect of Cr addition on nickel aluminium bronze(NAB)alloy microstructure,mechanical properties,and erosion-corrosion behaviour has been studied.The results show that Cr addition does not change the composition of the precipitated phases,more Cr entered theκphase and a small amount of Cr solubilized in the matrix,which increase the hardness of theκand matrix and decrease the potential difference between theκand matrix.NAB alloy with Cr shows high erosion-corrosion resistance at high flow rate conditions,due to its lower phase potential difference and higher surface hardness.At the flow rate of 3 m·s^(-1),the corrosion rate is 0.076 mm·year^(-1),which is~20%lower than that of the unadded Cr sample.Moreover,the corrosion product film contains Cr_(2)O_(3)and Cr^(3+),which improves the densification of the film and raises alloy’s corrosion resistance with Cr addition.The combination of mechanical and corrosion resistant properties may qualify this alloy as a potential candidate material for sustainable and safe equipment.展开更多
Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficul...Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficult recovery of the catalysts in a powdery form.Herein,a three-dimensional(3D)framework of Fe-incorporated Ni_(3)S_(2)nanosheets in-situ grown on Ni foam(Fe-Ni_(3)S_(2)@NF)was fabricated by a facile two-step hydrothermal process and applied to trigger peroxymonosulfate(PMS)oxidation of organic compounds inwater.A homogeneous growth environment enabled the uniform and scalable growth of Fe-Ni_(3)S_(2)nanosheets on the Ni foam.Fe-Ni_(3)S_(2)@NF possessed outstanding activity and durability in activating PMS,as it effectively facilitated electron transfer from organic pollutants to PMS.Fe-Ni_(3)S_(2)@NF initially supplied electrons to PMS,causing the catalyst to undergo oxidation,and subsequently accepted electrons from organic compounds,returning to its initial state.The introduction of Fe into the Ni_(3)S_(2)lattice enhanced electrical conductivity,promoting mediated electron transfer between PMS and organic compounds.The 3D conductive Ni foam provided an ideal platform for the nucleation and growth of Fe-Ni_(3)S_(2),accelerating pollutant abatement due to its porous structure and high conductivity.Furthermore,its monolithic nature simplified the catalyst recycling process.A continuous flow packed-bed reactor by encapsulating Fe-Ni_(3)S_(2)@NF catalyst achieved complete pollutant abatement with continuous operation for 240 h,highlighting its immense potential for practical environmental remediation.This study presents a facile synthesis method for creating a novel type of monolithic catalyst with high activity and durability for decontamination through Fenton-like processes.展开更多
A pyrimidine derivative,6-phenyl-2-thiouracil(PT),was synthesized for developing a corrosion inhibitor(CI)applied in the protection of the nickel−aluminum bronze(NAB)in seawater.The anti-corrosion effect of PT was eva...A pyrimidine derivative,6-phenyl-2-thiouracil(PT),was synthesized for developing a corrosion inhibitor(CI)applied in the protection of the nickel−aluminum bronze(NAB)in seawater.The anti-corrosion effect of PT was evaluated by the mass loss experiment,electrochemical tests and surface analysis.The results show that PT exhibits excellent inhibition performance and the maximum inhibition efficiency of PT reaches 99.6%.The interaction mechanism was investigated through X-ray photoelectron spectroscopy(XPS)and molecule dynamics simulation based on the density functional theory(DFT).The S-Cu,Al-N and Cu-N bonds are formed by the chemical interactions,leading to the adsorption of PT on the NAB surface.The diffusion of corrosive species is hindered considerably by the protective PT film with composition of(PT-Cu)_(ads)and(PT-Al)_(ads)on the PT/NAB interface.The degree of suppression is increased with the addition of more PT molecules.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is impera...The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is imperative to develop NO_(2)and CO_(2)sensors for ambient conditions,that can be used in indoor air quality monitoring,breath analysis,food spoilage detection,etc.In the present study,two thin film nanocomposite(nickel oxide-graphene and nickel oxide-silver nanowires)gas sensors are fabricated using direct ink writing.The nano-composites are investigated for their structural,optical,and electrical properties.Later the nano-composite is deposited on the interdigitated electrode(IDE)pattern to form NO_(2)and CO_(2)sensors.The deposited films are then exposed to NO_(2)and CO_(2)gases separately and their response and recovery times are determined using a custom-built gas sensing setup.Nickel oxide-graphene provides a good response time and recovery time of 10 and 9 s,respectively for NO_(2),due to the higher electron affinity of graphene towards NO_(2).Nickel oxide-silver nanowire nano-composite is suited for CO_(2)gas because silver is an excellent electrocatalyst for CO_(2)by giving response and recovery times of 11 s each.This is the first report showcasing NiO nano-composites for NO_(2)and CO_(2)sensing at room temperature.展开更多
Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In t...Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In this study,a flake-like nickel cobaltate/re-duced graphene oxide/melamine-derived carbon foam(FNC/RGO/MDCF)was successfully fabricated through a combination of solvo-thermal treatment and high-temperature pyrolysis.Results indicated that RGO was evenly distributed in the MDCF skeleton,providing ef-fective support for the load growth of FNC on its surface.Sample S3,the FNC/RGO/MDCF composite prepared by solvothermal method for 16 h,exhibited a minimum reflection loss(RL_(min))of-66.44 dB at a thickness of 2.29 mm.When the thickness was reduced to 1.50 mm,the optimal effective absorption bandwidth was 3.84 GHz.Analysis of the absorption mechanism of FNC/RGO/MDCF revealed that its excellent absorption performance was primarily attributed to the combined effects of conduction loss,multiple reflection,scattering,in-terface polarization,and dipole polarization.展开更多
La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation pr...La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.展开更多
An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The r...An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The reductive hydroarylation of acrylates with aryl halides was successfully achieved without requiring exogenous photoredox catalysts.This reaction is highlighted by the simple and mild conditions,good functional group tolerance,thus providing a complementary approach for alkenes reductive Heck reaction.展开更多
Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of...Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of polyfluoroarenes with alkyl halides under mild conditions is reported.Polyfluoroarenes(3~6 F)can reacted smoothly with a diverse range of alkyl halides,such as primary,secondary,and tertiary alkyl iodides.The efficient formation of C(sp2)—C(sp3)can be achieved through the combination of Ni catalysis and(Bpin)2/K2CO3 as terminal reductant.展开更多
High-performance pure nickel N6/steel 45#composite plate(N6/45#)was prepared using explosive welding technique.The microstructure of the interface and nearby regions was characterized and analyzed by optical microscop...High-performance pure nickel N6/steel 45#composite plate(N6/45#)was prepared using explosive welding technique.The microstructure of the interface and nearby regions was characterized and analyzed by optical microscope,scanning electron microscope,electron backscatter diffraction,and mechanical property testing,and the microstructural features and mechanical properties of the explosive welding interface were explored.The results show that along the direction of explosive welding,the pure nickel N6/steel 45#composite plate interface gradually evolves from a flat bond to a typical wavy bond.The grains at the crests and troughs exhibit high heterogeneity,and the closer to the interface,the finer the grains.Recrystallization and low-stress deformation bands are formed at the bonding interface.Nanoindentation tests reveal that plastic deformation occurs in the interfacial bonding zone,and the nanohardness values in the crest regions are higher than that in the trough regions.The tensile strength of the N6/45#interface is 599.8 MPa,with an average shear strength of 326.3 MPa.No separation phenomenon is observed between N6 and 45#after the bending test.展开更多
With the development of the new energy industry and the depletion of nickel sulfide ore resources,laterite nickel ore has become the main source of primary nickel,and nickel for power batteries has become a new growth...With the development of the new energy industry and the depletion of nickel sulfide ore resources,laterite nickel ore has become the main source of primary nickel,and nickel for power batteries has become a new growth point in consumption.This paper systematically summarizes the processes,parameters,products,recovery rates,environmental indicators,costs,advantages,disadvantages and the latest research progress of mainstream nickel extraction processes from laterite nickel ore.It also provides a comparative analysis of the environmental impact and economic efficiency of different nickel extraction processes.It is found that the current nickel extraction processes from laterite nickel ore globally for commercial production mainly include the RKEF process for producing ferronickel and the HPAL process for producing intermediate products.The former accounts for about 80%of laterite nickel ore production.Compared to each other,the investment cost per ton of nickel metal production capacity for the RKEF is about 43000$,with an operational cost of about 16000$per ton of nickel metal and a total nickel recovery rate of 77%–90%.Its products are mainly used in stainless steels.For the HPAL process,the investment cost per ton of nickel metal production capacity is about 56000$,with an operational cost of about 15000$per ton of nickel metal and a total nickel recovery rate of 83%–90%.Its products are mainly used in power batteries.The significant differences between the two lies in energy consumption and carbon emissions,with the RKEF being 2.18 and 2.37 times that of the HPAL,respectively.Although the use of clean energy can greatly reduce the operational cost and environmental impact of RKEF,if RKEF is converted to producing high Ni matte,its economic and environmental performance still cannot match that of the HPAL and oxygen-enriched side-blown processes.Therefore,it can be inferred that with the increasing demand for nickel in power batteries,HPAL and oxygen-enriched side blowing processes will play a greater role in laterite nickel extraction.展开更多
Herein,we describe a nickel-catalyzed reductive decarboxylative difluoromethylation reaction of alkenes using inexpensive and easy-to-handle difluoroacetic anhydride(DFAA)/pyridine N-oxide reagent system.A variety of ...Herein,we describe a nickel-catalyzed reductive decarboxylative difluoromethylation reaction of alkenes using inexpensive and easy-to-handle difluoroacetic anhydride(DFAA)/pyridine N-oxide reagent system.A variety of C(sp^(3))-CF_(2)H containing compounds were prepared through a hydrodifluoromethylation process.Besides,various gem–difluoroalkenes bearing CF_(2)H group were synthesized via defluorinative reductive cross-coupling process from trifluoromethyl-substituted alkenes using this new reaction system.Difluoroacetic anhydride has been then extended to other common alkyl anhydrides,and the corresponding hydroalkylation and defluoroalkylation processes have been successfully achieved.This method features broad substrate scope,good functional group tolerance as well as high efficiency.展开更多
Some novel manganese and nickel complexes were synthesized by reacting manganese(Ⅱ) dichloride and nickel(Ⅱ) dichloride with pyridyl-imine ligands differing in the nature of the substituents at the imino nitrogen at...Some novel manganese and nickel complexes were synthesized by reacting manganese(Ⅱ) dichloride and nickel(Ⅱ) dichloride with pyridyl-imine ligands differing in the nature of the substituents at the imino nitrogen atom. All the complexes were characterized by analytical and infrared data: for some of them single crystals were obtained, and their molecular structure was determined by X-ray diffraction. The complexes were used in association with methylaluminoxane(MAO) for the polymerization of 1,3-butadiene obtaining active and selective catalysts giving predominantly 1,2 polybutadiene in case of manganese catalysts and exclusively cis-1,4 polybutadiene in case of nickel catalysts.展开更多
Researchers have shown significant interest in modulating the peroxidase-like activity of nanozymes.Among these,bimetallic nanozymes have shown superior peroxidase-like activity over monometallic counterparts,offering...Researchers have shown significant interest in modulating the peroxidase-like activity of nanozymes.Among these,bimetallic nanozymes have shown superior peroxidase-like activity over monometallic counterparts,offering enhanced performance and cost-efficiency in nanozyme designs.Herein,bimetallic nanozymes comprising nickel(Ni)and osmium(Os)incorporated into hyaluronate(HA)have been developed,resulting in HA-Nin/Os nanoclusters.Subsequently,comprehensive characterizations have been conducted.Further investigation has revealed that HA-Nin/Os efficiently catalyzed 3,3,5,5-tetramethylbenzidine(TMB)oxidation with hydrogen peroxide(H_(2)O_(2)),confirming its peroxidase-like behavior and role as a nanozyme.Impressively,HA-Ni_(2)/Os(Ni/Os=2:1)displays heightened substrate affinity,accelerated reaction rates,enhanced hydroxyl radical production in acidic conditions,and exhibits activity unit of 1224 U/mg,representing more than two-fold increase compared to non-Ni-supported Os nanozyme.Theoretical calculations indicate that Ni support enhances the peroxidase-like process of Os nanozyme by improving H_(2)O_(2) adsorption and TMB oxidation.Crucially,the support of Ni does not significantly alter the other enzyme-like activities of Os nanozymes,thereby enabling Ni to selectively enhance their peroxidase-like activity.In terms of application,the peroxidase-like ability of HA-Ni_(2)/Os,facilitated by HA's carboxyl groups enabling crosslinking,proves effective in a squamous carcinoma antigen immunoassay.Moreover,HA-Ni_(2)/Os exhibit reliable stability,promising as a peroxidase substitute.This work underscores the advantages of incorporating Ni into Os,specifically enhancing peroxidase-like activity,highlighting the potential of Os bimetallic nanozymes for peroxidase-based applications.展开更多
Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NH...Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.展开更多
基金Project supported by the National Key Research and Development Program of China(2021YFA0718900)the National Natural Science Foundation of China(62074014,52073090)。
文摘While the metal to insulator transition(MIT)of d-band correlated perovskite nickelates(RENiO_(3))are widely adjustable via their rare-earth composition,the roles of potential valence variabilities associated with the rare-earth elements were rarely concerned.Herein,we demonstrate the material synthesis and MIT properties of RENiO_(3) containing valence variable rare-earth compositions,such as Ce,Pr,Sm,Eu and Tb.The metastable perovskite structure of SmNiO_(3) and EuNiO_(3) with a rare-earth valence states variable towards+2 can be effectively synthesized under high oxygen pressures as it is necessary to reduce their formation free energies.This is in contrast to Ce and Tb,in which situations the variable rare-earth valence state towards+4 reduces their ionic radius and prohibits their occupation or co-occupation of the rare-earth site within the perovskite structured RENiO_(3).Nevertheless,PrNiO_(3) with MIT properties can be effectively synthesized at lower oxygen pressures,owing to the higher stability to form a fully occupied 6s orbit associated Pr3+compared to the half-filled one related to Pr4+.The present work provides guidance for regulating the MIT properties of RENiO_(3).
基金PEREN project(reference:ANR-2011-PREG-016–05)the ECOREVE project(reference:ANR-18-CE05-0036-01)the Agence Nationale de la Recherche(A.N.R.,France)for supporting these scientific works and for the financial support。
文摘The chemical and electrochemical stability of lanthanide nickelates La2 NiO4+δ(LNO),Pr2 NiO4+δ(PNO)and their mixed compounds La(2-x)PrxNiO4+δ(LPNOs)with x=0.5,1 or 1.5 is reported.The aim is to promote these materials as efficient electrodes for solid oxide fuel cell(SOFC)and/or solid oxide electrolysis cell(SOEC).La2 NiO4+δand La1.5Pr0.5NiO4+δcompounds are chemically very stable as powders over one month in the temperature range 600-800℃,while the other materials rich in praseodymium progressively decompose into various perovskite-deriving components with additional Pr6 O11.Despite their uneven properties,all these materials are quite efficient and sustainable as electrodes on top of gadolinium doped ceria(GDCBL)//yttrium doped zirconia(8 YSZ)electrolyte,for one month at 700℃without polarization.Under polarization(300 mA·cm-2),the electrochemical performances of LNO,PNO and La1.5Pr0.5NiO4+δ(LP5 NO)quickly degrade in SOFC mode,i.e.for the oxygen reduction reaction,while they show durability in SOEC mode,i.e.for the oxide oxidation reaction.
基金financially supported by the National Key Research and Development Program of China (No. 2021YFA0718900)the National Natural Science Foundation of China (Nos.52073090 and 62074014)+1 种基金the Fundamental Research Funds for the Central Universities (No.FRF-TP-19-023A3Z)Beijing New-star Plan of Science and Technology (No. Z191100001119071)。
文摘The rare-earth nickelates(RENiO_(3)) exhibit an exceptional complex electronic phase diagram and multiple electronic phase transitions that enrich promising applications in correlated electronic devices beyond conventional semiconductors.Nevertheless,the practical applications of RENiO_(3) are challenged by their intrinsic thermodynamic metastability in material synthesis and high material cost.Therefore,developing an economical strategy to achieve the batch synthesis of RENiO_(3) is of vital importance.In this work,we enlarged the synthesis amount of RENiO_(3) up to 20 g per batch using chloride(KCI) assisted molten salt reaction.By optimizing the reaction conditions,the powder of RENiO_(3) with the cubic shape and average size of ~2μm was effectively synthesized,while their phase purity exceeded 95%.In addition,the cost to synthesize RENiO_(3) was further reduced by using rare-earth extraction intermediate products as the raw materials,instead of using the pure rare-earth precursors.It also achieved wide adjustments in the metal-to-insulator-transition temperature from160 to 420 K without significantly reducing the transition sharpness.By enlarging the synthesis amount and the reducing the cost,it paves the way to the device application of RENiO_(3).
基金financially supported by the National Key Re-search and Development Program of China(No.2021YFA0718900)the National Natural Science Foundation of China(Nos.62074014 and 52073090)the Beijing New-star Plan of Science and Tech-nology(No.Z191100001119071).
文摘Although the metal to insulator transition(MIT)observed in d-band correlated metal oxides enables promising applications(e.g.,correlated logical devices and Mottronic devices),its present recognition is mainly limited on the direct current(DC)electrical transports.Up to date,the MIT from the perspective of alternation current(AC)transport and its potential electronic applications remains yet unclear.Herein,we demonstrate the frequency(f_(AC))dependence in the impedance(Z=Z’+iZ″)of typical MIT materials,such as thin film rare-earth nickelates(Re NiO_(3)),across the critical MIT temperature(T_(MIT)).Apart from the abrupt change in the impedance modulus(|Z|)across the critical temperature(T_(MIT))similar to the DC transport,the MIT also triggers non-continuous variation in the impedance phase(θ),and this enables the f_(AC)-regulations in the Z’-T tendencies(Z’=|Z|cosθ).At the critical f_(AC) range(e.g.,104-106 Hz),the con-versing variations in|Z|-T and cosθ-T across T_(MIT) result in non-monotonic delta-shape Z’-T tendency in Sm_(x) Nd_(1-x) NiO_(3),the full width half maximum of which is effectively narrowed compared to the situation with the absence of MIT.Further imparting lower or higher f_(AC) elevate the domination in|Z|-T and cosθ-T,respectively,but also enables abrupt Z’-T tendencies across T_(MIT) showing negative temperature coefficient of resistance(NTCR)or positive temperature coefficient of resistance(PTCR).By introducing f_(AC) as a new freedom,the MIT behavior can be more comprehensively regulated electronically,and this extends the vision in exploring the new electronic applications based on the correlated MIT materials from the AC perspective.
基金financially supported by the National Key Research and Development Program of China(No.2021YFA0718900)National Natural Science Foundation of China(Nos.62074014,52073090,and 52103284)。
文摘The multiple quantum transitions within d-band correlation oxides such as rare-earth nickelates(RENiO_(3))triggered by critical temperatures and/or hydrogenation opened up a new paradigm for correlated electronics applications,e.g.ocean electric field sensor,bio-sensor,and neuron synapse logical devices.Nevertheless,these applications are obstructed by the present ineffectiveness in the thin film growth of the metastable RENiO_(3)with flexibly adjustable rare-earth compositions and electronic structures.Herein,we demonstrate a metal-organic decompositions(MOD)approach that can effectively grow metastable RENiO_(3)covering a large variety of the rare-earth composition without introducing any vacuum process.Unlike the previous chemical growths for RENiO_(3)relying on strict interfacial coherency that limit the film thickness,the MOD growth using reactive isooctanoate percussors is tolerant to lattice defects and therefore achieves comparable film thickness to vacuum depositions.Further indicated by positron annihilation spectroscopy,the RENiO_(3)grown by MOD exhibit large amount of lattice defects that improves their hydrogen incorporation amount and electron transfers,as demonstrated by the resonant nuclear reaction analysis and near edge X-ray absorption fine structure analysis.This effectively enlarges the magnitude in the resistance regulations in particular for RENiO_(3)with lighter RE,shedding a light on the extrinsic regulation of the hydrogen induced quantum transitions for correlated oxides semiconductors kinetically via defect engineering.
基金supported by Beijing Nova Program(No.20230484371)the National Key Research and Development Program of China(No.2021YFB3700700).
文摘The effect of Cr addition on nickel aluminium bronze(NAB)alloy microstructure,mechanical properties,and erosion-corrosion behaviour has been studied.The results show that Cr addition does not change the composition of the precipitated phases,more Cr entered theκphase and a small amount of Cr solubilized in the matrix,which increase the hardness of theκand matrix and decrease the potential difference between theκand matrix.NAB alloy with Cr shows high erosion-corrosion resistance at high flow rate conditions,due to its lower phase potential difference and higher surface hardness.At the flow rate of 3 m·s^(-1),the corrosion rate is 0.076 mm·year^(-1),which is~20%lower than that of the unadded Cr sample.Moreover,the corrosion product film contains Cr_(2)O_(3)and Cr^(3+),which improves the densification of the film and raises alloy’s corrosion resistance with Cr addition.The combination of mechanical and corrosion resistant properties may qualify this alloy as a potential candidate material for sustainable and safe equipment.
基金supported by the National Natural Science Foundation of China(No.21876039)Y.Yao acknowledges the scholarship support from the China Scholarship Council(No.202106695010)Partial support from the Australian Research Council for DP230102406 is also acknowledged.
文摘Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficult recovery of the catalysts in a powdery form.Herein,a three-dimensional(3D)framework of Fe-incorporated Ni_(3)S_(2)nanosheets in-situ grown on Ni foam(Fe-Ni_(3)S_(2)@NF)was fabricated by a facile two-step hydrothermal process and applied to trigger peroxymonosulfate(PMS)oxidation of organic compounds inwater.A homogeneous growth environment enabled the uniform and scalable growth of Fe-Ni_(3)S_(2)nanosheets on the Ni foam.Fe-Ni_(3)S_(2)@NF possessed outstanding activity and durability in activating PMS,as it effectively facilitated electron transfer from organic pollutants to PMS.Fe-Ni_(3)S_(2)@NF initially supplied electrons to PMS,causing the catalyst to undergo oxidation,and subsequently accepted electrons from organic compounds,returning to its initial state.The introduction of Fe into the Ni_(3)S_(2)lattice enhanced electrical conductivity,promoting mediated electron transfer between PMS and organic compounds.The 3D conductive Ni foam provided an ideal platform for the nucleation and growth of Fe-Ni_(3)S_(2),accelerating pollutant abatement due to its porous structure and high conductivity.Furthermore,its monolithic nature simplified the catalyst recycling process.A continuous flow packed-bed reactor by encapsulating Fe-Ni_(3)S_(2)@NF catalyst achieved complete pollutant abatement with continuous operation for 240 h,highlighting its immense potential for practical environmental remediation.This study presents a facile synthesis method for creating a novel type of monolithic catalyst with high activity and durability for decontamination through Fenton-like processes.
基金supported by the National Natural Science Foundation of China(No.52171069).
文摘A pyrimidine derivative,6-phenyl-2-thiouracil(PT),was synthesized for developing a corrosion inhibitor(CI)applied in the protection of the nickel−aluminum bronze(NAB)in seawater.The anti-corrosion effect of PT was evaluated by the mass loss experiment,electrochemical tests and surface analysis.The results show that PT exhibits excellent inhibition performance and the maximum inhibition efficiency of PT reaches 99.6%.The interaction mechanism was investigated through X-ray photoelectron spectroscopy(XPS)and molecule dynamics simulation based on the density functional theory(DFT).The S-Cu,Al-N and Cu-N bonds are formed by the chemical interactions,leading to the adsorption of PT on the NAB surface.The diffusion of corrosive species is hindered considerably by the protective PT film with composition of(PT-Cu)_(ads)and(PT-Al)_(ads)on the PT/NAB interface.The degree of suppression is increased with the addition of more PT molecules.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
文摘The rapid industrial growth and increasing population have led to significant pollution and deterioration of the natural atmospheric environment.Major atmospheric pollutants include NO_(2)and CO_(2).Hence,it is imperative to develop NO_(2)and CO_(2)sensors for ambient conditions,that can be used in indoor air quality monitoring,breath analysis,food spoilage detection,etc.In the present study,two thin film nanocomposite(nickel oxide-graphene and nickel oxide-silver nanowires)gas sensors are fabricated using direct ink writing.The nano-composites are investigated for their structural,optical,and electrical properties.Later the nano-composite is deposited on the interdigitated electrode(IDE)pattern to form NO_(2)and CO_(2)sensors.The deposited films are then exposed to NO_(2)and CO_(2)gases separately and their response and recovery times are determined using a custom-built gas sensing setup.Nickel oxide-graphene provides a good response time and recovery time of 10 and 9 s,respectively for NO_(2),due to the higher electron affinity of graphene towards NO_(2).Nickel oxide-silver nanowire nano-composite is suited for CO_(2)gas because silver is an excellent electrocatalyst for CO_(2)by giving response and recovery times of 11 s each.This is the first report showcasing NiO nano-composites for NO_(2)and CO_(2)sensing at room temperature.
基金support of the Key Science Research Project in Colleges and Universities of Anhui Province,China(No.2022AH050813)the Medical Special Cultivation Project of Anhui University of Science and Technology,China(No.YZ2023H2A002).
文摘Carbon-based foams with a three-dimensional structure can serve as a lightweight template for the rational design and control-lable preparation of metal oxide/carbon-based composite microwave absorption materials.In this study,a flake-like nickel cobaltate/re-duced graphene oxide/melamine-derived carbon foam(FNC/RGO/MDCF)was successfully fabricated through a combination of solvo-thermal treatment and high-temperature pyrolysis.Results indicated that RGO was evenly distributed in the MDCF skeleton,providing ef-fective support for the load growth of FNC on its surface.Sample S3,the FNC/RGO/MDCF composite prepared by solvothermal method for 16 h,exhibited a minimum reflection loss(RL_(min))of-66.44 dB at a thickness of 2.29 mm.When the thickness was reduced to 1.50 mm,the optimal effective absorption bandwidth was 3.84 GHz.Analysis of the absorption mechanism of FNC/RGO/MDCF revealed that its excellent absorption performance was primarily attributed to the combined effects of conduction loss,multiple reflection,scattering,in-terface polarization,and dipole polarization.
基金the financial support by the National Nat-ural Science Foundation of China(Nos.52201282,52071281,52371239)the China Postdoctoral Science Foundation(No.2023M742945)+4 种基金Hebei Provincial Postdoctoral Science Foundation(No.B2023003023)the Science Research Project of Hebei Education Department(No.BJK2022033)the Natural Science Foundation of Hebei Province(No.C2022203003)the Inner Mongolia Science and Technology Major Project(No.2020ZD0012)the Baotou Science and Technology Planning Project(No.XM2022BT09).
文摘La-Mg-Ni-based hydrogen storage alloys with superlattice structures are the new generation anode material for nickel metal hydride(Ni-MH)batteries owing to the advantages of high capacity and exceptional activation properties.However,the cycling stability is not currently satisfactory enough which plagues its application.Herein,a strategy of partially substituting La with the Y element is proposed to boost the capacity durability of La-Mg-Ni-based alloys.Furthermore,phase structure regulation is implemented simultaneously to obtain the A5 B19-type alloy with good crystal stability specifically.It is found that Y promotes the phase formation of the Pr5 Co19-type phase after annealing at 985℃.The alloy containing Y contributes to the superior rate capability resulting from the promoted hydrogen diffusion rate.Notably,Y substitution enables strengthening the anti-pulverization ability of the alloy in terms of increasing the volume match between[A_(2)B_(4)]and[AB5]subunits,and effectively enhances the anti-corrosion ability of the alloy due to high electronegativity,realizing improved long-term cycling stability of the alloy from 74.2%to 78.5%after cycling 300 times.The work is expected to shed light on the composition and structure design of the La-Mg-Ni-based hydrogen storage alloy for Ni-MH batteries.
文摘An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The reductive hydroarylation of acrylates with aryl halides was successfully achieved without requiring exogenous photoredox catalysts.This reaction is highlighted by the simple and mild conditions,good functional group tolerance,thus providing a complementary approach for alkenes reductive Heck reaction.
文摘Polyfluoroarenes represent an essential group of compounds in the fields of medical and material chemistry.It is still a challenge to synthesize alkylated polyfluoroarenes.Herein,a Ni-catalyzed reductive alkylation of polyfluoroarenes with alkyl halides under mild conditions is reported.Polyfluoroarenes(3~6 F)can reacted smoothly with a diverse range of alkyl halides,such as primary,secondary,and tertiary alkyl iodides.The efficient formation of C(sp2)—C(sp3)can be achieved through the combination of Ni catalysis and(Bpin)2/K2CO3 as terminal reductant.
基金Natural Science Foundation of Shanxi Province(202203021221149)Key Research and Development Program of Shanxi Province(202302010101006,202202150401016)+1 种基金Scientific Research Start-up Fund for the Introduction of Talents in Shanxi Institute of Electronic Science and Technology(2023RKJ021)Key R&D Program of Linfen City(2334)。
文摘High-performance pure nickel N6/steel 45#composite plate(N6/45#)was prepared using explosive welding technique.The microstructure of the interface and nearby regions was characterized and analyzed by optical microscope,scanning electron microscope,electron backscatter diffraction,and mechanical property testing,and the microstructural features and mechanical properties of the explosive welding interface were explored.The results show that along the direction of explosive welding,the pure nickel N6/steel 45#composite plate interface gradually evolves from a flat bond to a typical wavy bond.The grains at the crests and troughs exhibit high heterogeneity,and the closer to the interface,the finer the grains.Recrystallization and low-stress deformation bands are formed at the bonding interface.Nanoindentation tests reveal that plastic deformation occurs in the interfacial bonding zone,and the nanohardness values in the crest regions are higher than that in the trough regions.The tensile strength of the N6/45#interface is 599.8 MPa,with an average shear strength of 326.3 MPa.No separation phenomenon is observed between N6 and 45#after the bending test.
基金This research was jointly supported by the China Geological Survey Project(DD20211404)the Natural Science Foundation of Inner Mongolia Autonomous Region(2019LH05028).
文摘With the development of the new energy industry and the depletion of nickel sulfide ore resources,laterite nickel ore has become the main source of primary nickel,and nickel for power batteries has become a new growth point in consumption.This paper systematically summarizes the processes,parameters,products,recovery rates,environmental indicators,costs,advantages,disadvantages and the latest research progress of mainstream nickel extraction processes from laterite nickel ore.It also provides a comparative analysis of the environmental impact and economic efficiency of different nickel extraction processes.It is found that the current nickel extraction processes from laterite nickel ore globally for commercial production mainly include the RKEF process for producing ferronickel and the HPAL process for producing intermediate products.The former accounts for about 80%of laterite nickel ore production.Compared to each other,the investment cost per ton of nickel metal production capacity for the RKEF is about 43000$,with an operational cost of about 16000$per ton of nickel metal and a total nickel recovery rate of 77%–90%.Its products are mainly used in stainless steels.For the HPAL process,the investment cost per ton of nickel metal production capacity is about 56000$,with an operational cost of about 15000$per ton of nickel metal and a total nickel recovery rate of 83%–90%.Its products are mainly used in power batteries.The significant differences between the two lies in energy consumption and carbon emissions,with the RKEF being 2.18 and 2.37 times that of the HPAL,respectively.Although the use of clean energy can greatly reduce the operational cost and environmental impact of RKEF,if RKEF is converted to producing high Ni matte,its economic and environmental performance still cannot match that of the HPAL and oxygen-enriched side-blown processes.Therefore,it can be inferred that with the increasing demand for nickel in power batteries,HPAL and oxygen-enriched side blowing processes will play a greater role in laterite nickel extraction.
基金financial support from the National Natural Science Foundation of China(NSFC,No.21877067)Tsinghua-Peking Centre for Life Science。
文摘Herein,we describe a nickel-catalyzed reductive decarboxylative difluoromethylation reaction of alkenes using inexpensive and easy-to-handle difluoroacetic anhydride(DFAA)/pyridine N-oxide reagent system.A variety of C(sp^(3))-CF_(2)H containing compounds were prepared through a hydrodifluoromethylation process.Besides,various gem–difluoroalkenes bearing CF_(2)H group were synthesized via defluorinative reductive cross-coupling process from trifluoromethyl-substituted alkenes using this new reaction system.Difluoroacetic anhydride has been then extended to other common alkyl anhydrides,and the corresponding hydroalkylation and defluoroalkylation processes have been successfully achieved.This method features broad substrate scope,good functional group tolerance as well as high efficiency.
文摘Some novel manganese and nickel complexes were synthesized by reacting manganese(Ⅱ) dichloride and nickel(Ⅱ) dichloride with pyridyl-imine ligands differing in the nature of the substituents at the imino nitrogen atom. All the complexes were characterized by analytical and infrared data: for some of them single crystals were obtained, and their molecular structure was determined by X-ray diffraction. The complexes were used in association with methylaluminoxane(MAO) for the polymerization of 1,3-butadiene obtaining active and selective catalysts giving predominantly 1,2 polybutadiene in case of manganese catalysts and exclusively cis-1,4 polybutadiene in case of nickel catalysts.
基金financial support from the Natural Science Foundation of Fujian Province(No.2022J01271)the Joint Funds for the Innovation of Science and Technology,Fujian Province(No.2023Y9226)+1 种基金the Introduced High-Level Talent Team Project of Quanzhou City(No.2023CT008)the Doctoral Research Foundation Project of the Second Affiliated Hospital of Fujian Medical University(No.BS202201)。
文摘Researchers have shown significant interest in modulating the peroxidase-like activity of nanozymes.Among these,bimetallic nanozymes have shown superior peroxidase-like activity over monometallic counterparts,offering enhanced performance and cost-efficiency in nanozyme designs.Herein,bimetallic nanozymes comprising nickel(Ni)and osmium(Os)incorporated into hyaluronate(HA)have been developed,resulting in HA-Nin/Os nanoclusters.Subsequently,comprehensive characterizations have been conducted.Further investigation has revealed that HA-Nin/Os efficiently catalyzed 3,3,5,5-tetramethylbenzidine(TMB)oxidation with hydrogen peroxide(H_(2)O_(2)),confirming its peroxidase-like behavior and role as a nanozyme.Impressively,HA-Ni_(2)/Os(Ni/Os=2:1)displays heightened substrate affinity,accelerated reaction rates,enhanced hydroxyl radical production in acidic conditions,and exhibits activity unit of 1224 U/mg,representing more than two-fold increase compared to non-Ni-supported Os nanozyme.Theoretical calculations indicate that Ni support enhances the peroxidase-like process of Os nanozyme by improving H_(2)O_(2) adsorption and TMB oxidation.Crucially,the support of Ni does not significantly alter the other enzyme-like activities of Os nanozymes,thereby enabling Ni to selectively enhance their peroxidase-like activity.In terms of application,the peroxidase-like ability of HA-Ni_(2)/Os,facilitated by HA's carboxyl groups enabling crosslinking,proves effective in a squamous carcinoma antigen immunoassay.Moreover,HA-Ni_(2)/Os exhibit reliable stability,promising as a peroxidase substitute.This work underscores the advantages of incorporating Ni into Os,specifically enhancing peroxidase-like activity,highlighting the potential of Os bimetallic nanozymes for peroxidase-based applications.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22278092,22078116 and 22222805)Guangdong Provincial Key Research and Development Program(No.2020B1111380002)+2 种基金Science and Technology Research Project of Guangzhou(Nos.2023A03J0034,2023A04J0077 and 202102020467)State Key Laboratory of Pulp and Paper Engineering(No.202313)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464).
文摘Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.
