CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet...CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR.展开更多
Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic fram...Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.展开更多
Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen e...Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.展开更多
Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential fo...Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential for catalyst design.Herein,we prepared two Cu-Ag bimetallic catalysts with Ag nanoparticles attached to the top or the bottom of Cu nanowires.When tested in a flow cell,the Cu-Ag catalyst with Ag nanoparticles on the bottom achieved a faradaic efficiency of 54%for ethylene production,much higher than the catalyst with Ag nanoparticles on the top.The catalysts were further studied in the H-cell and zero-gap MEA cell.It was found that placing the two metals in the intensified reaction zone is crucial to triggering the tandem reaction of bimetallic catalysts.Our work elucidates the structure-activity relationship of bimetallic catalysts for CO_(2) reduction and demonstrates the importance of considering both catalyst structures and cell characteristics to achieve high activity and selectivity.展开更多
The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ab...The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of challenge.Here,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 h.Interestingly,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such catalysts.The results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.展开更多
In this paper,the effect of the Si content on microstructure evolution,mechanical properties,and fracture behavior of the Al-xSi/AZ91D bimetallic composites prepared by compound casting was investigated systematically...In this paper,the effect of the Si content on microstructure evolution,mechanical properties,and fracture behavior of the Al-xSi/AZ91D bimetallic composites prepared by compound casting was investigated systematically.The obtained results showed that all the Al-xSi/AZ91D bimetallic composites had a metallurgical reaction layer(MRL),whose thickness increased with increasing Si content for the hypoeutectic Al-Si/AZ91D composites,while the hypereutectic Al-Si/AZ91D composites were opposite.The MRL included eutectic layer(E layer),intermetallic compound layer(IMC layer)and transition region layer(T layer).In the IMC layer,the hypereutectic Al-Si/AZ91D composites contained some Si solid solution and flocculent Mg_(2)Si+Al-Mg IMCs phases not presented in the hypoeutectic Al-Si/AZ91D composites.Besides,increasing Si content,the thickness proportion of the T layer increased,forming an inconsistent preferred orientation of the MRL.The shear strengths of the Al-xSi/AZ91D bimetallic composites enhanced with increasing Si content,and the Al-15Si/AZ91D composite obtained a maximum shear strength of 58.6 MPa,which was 73.4% higher than the Al-6Si/AZ91D composite.The fractures of the Al-xSi/AZ91D bimetallic composites transformed from the T layer into the E layer with the increase of the Si content.The improvement of the shear strength of the Al-xSi/AZ91D bimetallic composites was attributed to the synergistic action of the Mg_(2)Si particle reinforcement,the reduction of oxidizing inclusions and the ratio of Al-Mg IMCs as well as the orientation change of the MRL.展开更多
A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of th...A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.展开更多
Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile...Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.展开更多
Lithium-sulfur(Li-S)batteries are considered highly promising as next-generation energy storage systems due to high theoretical capacity(2600 Wh kg^(-1))and energy density(1675 mA h g^(-1))as well as the abundant natu...Lithium-sulfur(Li-S)batteries are considered highly promising as next-generation energy storage systems due to high theoretical capacity(2600 Wh kg^(-1))and energy density(1675 mA h g^(-1))as well as the abundant natural reserves,low cost of elemental sulfur,and environmentally friendly properties.However,several challenges impede its commercialization including low conductivity of sulfur itself,the severe“shuttle effect”caused by lithium polysulfides(LiPSs)during charge–discharge processes,volume expansion effects and sluggish reaction kinetics.As a solution,polar metal particles and their compounds have been introduced as the main hosts for sulfur cathode due to their robust catalytic activity and adsorption capability,effectively suppressing the“shuttle effect”of Li PSs.Bimetallic alloys and their compounds with multi-functional properties exhibit remarkable electrochemical performance more readily when compared to single-metal materials.Well-designed bimetallic materials demonstrate larger specific surface areas and richer active sites,enabling simultaneous high adsorption capability and strong catalytic properties.The synergistic effect of the“adsorption-catalysis”sites accelerates the adsorptiondiffusion-conversion process of Li PSs,ultimately achieving a long-lasting Li-S battery.Herein,the latest progress and performance of bimetallic materials in cathodes,separators,and interlayers of Li-S batteries are systematically reviewed.Firstly,the principles and challenges of Li-S batteries are briefly analyzed.Then,various mechanisms for suppressing“shuttle effects”of Li PSs are emphasized at the microscale.Subsequently,the performance parameters of various bimetallic materials are comprehensively summarized,and some improvement strategies are proposed based on these findings.Finally,the future prospects of bimetallic materials are discussed,with the hope of providing profound insights for the rational design and manufacturing of high-performance bimetallic materials for LSBs.展开更多
The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot elec...The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot electrons and phonons)transfers on the interface between two metals.We have designed and synthesized Au@Cu bimetallic nanoparticles with Au as core and Cu as shell.By using transient absorption spectroscopy,we find that there are two plasmon induced heat funneling processes from Au core to Cu shell.One is the electron temperature equilibrium(electron heat transfer)with equilibration time of~560 fs.The other is the lattice temperature equilibrium(lattice heat transfer)with equilibration time of~13 ps.This plasmon induced heat funneling may be universal in similar bimetallic nanostructures,so our finding could contribute to further understanding the catalytic mechanism of bimetallic plasmonic photothermal catalysis.展开更多
Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the mo...Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the most promising solutions for providing hydrogen fuel.Nickel iron bimetallic electrocatalysts have abundant sources,low cost,clean and pollution-free properties,and strong catalytic performance,This article mainly reviews the development and research of bimetallic nickel iron oxides and nickel iron alloys in recent years,and explores their synthesis methods,properties,and stability in depth.展开更多
To solve low efficiency,environmental pollution,and toxicity for synthesizing zeolitic imidazolate frameworks(ZIFs)in organic solvents,a KOH-assisted aqueous strategy is proposed to synthesize bimetallic ZIFs polyhedr...To solve low efficiency,environmental pollution,and toxicity for synthesizing zeolitic imidazolate frameworks(ZIFs)in organic solvents,a KOH-assisted aqueous strategy is proposed to synthesize bimetallic ZIFs polyhedrons,which are used as precursors to prepare bimetallic selenide and N-doped carbon(NC)composites.Among them,Fe–Co–Se/NC retains the three-dimensional(3D)polyhedrons with mesoporous structure,and Fe–Co–Se nanoparticles are uniform in size and evenly distributed.When assessed as anode material for lithium-ion batteries,Fe–Co–Se/NC achieves an excellent initial specific capacity of 1165.9 m Ah·g^(-1)at 1.0 A·g^(-1),and the reversible capacity of Fe–Co–Se/NC anode is 1247.4 m Ah·g^(-1)after 550 cycles.It is attributed to that the uniform composite of bimetallic selenides and N-doped carbon can effectively tune redox active sites,the stable 3D structure of Fe–Co–Se/NCs guarantees the structural stability and wettability of the electrolyte,and the uniform distribution of Fe–Co–S nanoparticles in size esuppresses the volume expansion and accelerates the electrochemical reaction kinetics.展开更多
The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.He...The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.Herein,we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride(CN).In this Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst,the noble-metal active sites are maximized,and the single-atomic Co_(1)N_4sites are tuned to Co_(1)N_3sites by photogenerated electrons arising from the introduced single-atomic Pt_(1)N_4sites.Mechanism studies and density functional theory(DFT)calculations reveal that the 3d orbitals of Co_(1)N_3single sites are filled with unpaired d-electrons,which lead to the improved visible-light response,carrier separation and charge migration for CN photocatalysts.Thereafter,the protons adsorption and activation are promoted.Taking this advantage of long-range electron synergy in bimetallic single atomic sites,the photocatalytic hydrogen evolution activity over Pt_(1)-Co_(1)/CN achieves 915.8 mmol g^(-1)Pt h^(-1),which is 19.8 times higher than Co_(1)/CN and 3.5 times higher to Pt_(1)/CN.While this electron-synergistic effect is not so efficient for Pt nanoclusters.These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts.展开更多
Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structur...Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.展开更多
Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity...Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity of products pose significant challenges.As an emerging material,bimetallic catalysts have been widely reported for their unique advantages,such as tunable electronic structures,suitable adsorption/desorption of CO_(2) and intermediates,and optimizable d-band centers of active sites through bimetallic synergy.These catalysts provide a remarkable platform for converting CO_(2) into high value-added chemicals.This review comprehensively summarizes recent research advances in bimetallic catalysts for CO_(2)RR.Firstly,the challenges associated with CO_(2)RR,including activity and selectivity are analyzed,followed by a discussion on the unique advantages of bimetallic catalysts.Next,their synthesis strategies are categorized into dual-atom site catalysts(DACs),bimetallic nanoparticles and nanoclusters,binary metal semiconductors,and layered double hydroxides(LDHs).Additionally,advanced characterization techniques of bimetallic catalysts and their applications in CO_(2)RR are thoroughly introduced.Finally,the prospects and challenges for the application of bimetallic materials are highlighted.This review aims to provide inspiration for CO_(2)RR into high-value chemicals and shed light on the research of bimetallic materials.展开更多
The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt...The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt phthalocyanine(PPcFeCo)with excellent thermal stability and three-dimensional graphene(3D-G).The bimetallic synergistic effect of PPcFeCo,verified by DFT(Density functional theory)calculation,andπ-πinteractions enhances the catalytic activity and durability of the PPcFeCo/3D-G.Regarding electrochemical performance,the PPcFeCo/3D-G with a high electron transfer number(3.98,@0.768 V vs.RHE)has excellent half-wave potential(E_(1/2)=0.890 V vs.RHE)and exhibits outstanding reversibility(ΔE=0.700 V,ΔE=Ej=10-E_(1/2)).The liquid ZAB(LZAB)employed PPcFeCo/3D-G displays a high power density(222 m W cm^(-2)),a specific capacity(792 m A h g-1),and excellent durability(120 h).This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.展开更多
Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anod...Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anode of the Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies(Ov-BMO-Cu)are in-situ generated by phase separation and hydrogen etching using nanoporous Cu-Mn alloy as selfsacrificial templates.On this basis,we have elucidated the relationship between the phase evolution,oxygen vacancies and sodium-ion storage mechanisms,further demonstrating the evolution of oxygen vacancies and the inhibition effect of manganese oxides as an“anchor”on grain aggregation of copper oxides.The kinetic analyses confirm that the expanded lattice space and increased oxygen vacancies of cycled Ov-BMO-Cu synergistically guarantee effective sodium-ion diffusion and storage mechanisms.Therefore,the Ov-BMO-Cu electrode exhibits higher reversible capacities of 4.04 mA h cm^(-2)at 0.2 mA cm^(-2)after 100 cycles and 2.20 m A h cm^(-2)at 1.0 mA cm^(-2)after 500 cycles.Besides,the presodiated Ov-BMO-Cu anode delivers a considerable reversible capacity of 0.79 m A h cm^(-2)at 1.0 mA cm^(-2)after 60 cycles in full cells with Na_(3)V_(2)(PO_(4))_(3)cathode,confirming its outstanding practicality.Thus,this work is expected to provide enlightenment for designing high-capacity bimetallic oxide anodes.展开更多
Efficient and stable oxygen evolution electrocatalysts are indispensable for industrial applications of water splitting and hydrogen production.Herein,a simple and practical method was applied to fabricate(Mo,Fe)P2O7@...Efficient and stable oxygen evolution electrocatalysts are indispensable for industrial applications of water splitting and hydrogen production.Herein,a simple and practical method was applied to fabricate(Mo,Fe)P2O7@NF electrocatalyst by directly growing Mo/Fe bimetallic pyrophosphate derived from Prussian blue analogues on three-dimensional porous current collector.In alkaline media,the developed material possesses good hydrophilic features and exhibits best-in-class oxygen evolution reaction(OER)performances.Surprisingly,the(Mo,Fe)P_(2)O_(7)@NF only requires overpotentials of 250 and 290 mV to deliver 100 and 600 mA cm^(-2)in 1 mol L^(-1)KOH,respectively.Furthermore,the(Mo,Fe)P_(2)O_(7)@NF shows outstanding performances in alkaline salty water and 1 mol L^(-1)high purity KOH.A worthwhile pathway is provided to combine bimetallic pyrophosphate with commercial Ni foam to form robust electrocatalysts for stable electrocatalytic OER,which has a positive impact on both hydrogen energy application and environmental restoration.展开更多
Platinum-based nanocomposites have been considered as one of the most promising catalysts for methanol oxidation reactions(MORs), which yet still suffer from low electrochemical activity and electron-transfer properti...Platinum-based nanocomposites have been considered as one of the most promising catalysts for methanol oxidation reactions(MORs), which yet still suffer from low electrochemical activity and electron-transfer properties. Apart from van-der-Waals heterostructures,herein, we report a novel nanocomposite with the structure of Pt–Ru bimetallic nanoparticles covalently-bonded onto multi-walled carbon nanotubes (MWCNTs)(Pt–Ru@MWCNT), which have been successfully fabricated via a facile and green synthesis method. It is demonstrated that the Pt–Ru@MWCNT nanocomposite possesses much enhanced electrocatalytic activity with the electrochemical active surface area(ECSA) of 110.4 m^(2)·g^(-1)for Pt towards MOR, which is 2.67 and 4.0 times higher than those of 20wt%commercial Pt@C and Pt-based nanocomposite prepared by other method, due to the improved electron-transfer properties originated from M–O–C covalent bonds. This work provides us a new strategy for the structural design of highly-efficient electrocatalysts in boosting MOR performance.展开更多
Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(...Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(ORR) kinetics on the cathode remains by far the most critical bottleneck hindering the practical application of MFC. An ideal cathode catalyst should possess excellent ORR activity, stability, and costeffectiveness, experiments have demonstrated that bimetallic catalysts are one of the most promising ORR catalysts currently. Based on this, this review mainly analyzes the reaction mechanism(ORR mechanisms, synergistic effects), advantages(combined with characterization technologies), and typical synthesis methods of bimetallic catalysts, focusing on the application effects of early Pt-M(M = Fe, Co, and Ni) alloys to bifunctional catalysts in MFC, pointing out that the main existing challenges remain economic analysis, long-term durability and large-scale application, and looking forward to this. At last, the research trend of bimetallic catalysts suitable for MFC is evaluated, and it is considered that the development and research of metal-organic framework(MOF)-based bimetallic catalysts are still worth focusing on in the future, intending to provide a reference for MFC to achieve energy-efficient wastewater treatment.展开更多
基金financially supported by the National Natural Science Foundation of China(52072409)the Major Scientific and Technological Innovation Project of Shandong Province(2020CXGC010403)+1 种基金the Taishan Scholar Project(No.ts201712020)the Natural Science Foundation of Shandong Province(ZR2021QE062)
文摘CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21978119,22202088)Key Research and Development Plan of Hainan Province(ZDYF2022SHFZ285)Jiangsu Funding Program for Excellent Postdoctoral Talent(2022ZB636)。
文摘Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.
基金supported by the Inner Mongolia R&D Program Plan(2021ZD0042,2021EEDSCXSFQZD006)the National Natural Science Foundation of China(21902123)the Natural Science Basic Research Program of Shaanxi(2023-JC-ZD-22)。
文摘Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.
基金the funding support from the National Key Research and Development Program of China(2019YFE0123400)the Tianjin Distinguished Young Scholars Fund(20JCJQJC00260)+4 种基金the Major Science and Technology Project of Anhui Province(202203f07020007)the Anhui Conch Group Co.,Ltdthe“111”Project(B16027)the funding support from the Natural Science Foundation of China(22209081)the fellowship of China Postdoctoral Science Foundation(2021M690082)。
文摘Developing bimetallic catalysts is an effective strategy for enhancing the activity and selectivity of electrochemical CO_(2) reduction reactions,where understanding the structure-activity relationship is essential for catalyst design.Herein,we prepared two Cu-Ag bimetallic catalysts with Ag nanoparticles attached to the top or the bottom of Cu nanowires.When tested in a flow cell,the Cu-Ag catalyst with Ag nanoparticles on the bottom achieved a faradaic efficiency of 54%for ethylene production,much higher than the catalyst with Ag nanoparticles on the top.The catalysts were further studied in the H-cell and zero-gap MEA cell.It was found that placing the two metals in the intensified reaction zone is crucial to triggering the tandem reaction of bimetallic catalysts.Our work elucidates the structure-activity relationship of bimetallic catalysts for CO_(2) reduction and demonstrates the importance of considering both catalyst structures and cell characteristics to achieve high activity and selectivity.
基金financially supported by the National Natural Science Foundation of China with grant number of 22172082 and 21978137。
文摘The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of challenge.Here,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 h.Interestingly,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such catalysts.The results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.
基金the supports provided by the National Natural Science Foundation of China(Nos.52075198 and 52271102)the China Postdoctoral Science Foundation(No.2021M691112)+1 种基金the State Key Lab of Advanced Metals and Materials(No.2021-ZD07)the Analytical and Testing Center,HUST。
文摘In this paper,the effect of the Si content on microstructure evolution,mechanical properties,and fracture behavior of the Al-xSi/AZ91D bimetallic composites prepared by compound casting was investigated systematically.The obtained results showed that all the Al-xSi/AZ91D bimetallic composites had a metallurgical reaction layer(MRL),whose thickness increased with increasing Si content for the hypoeutectic Al-Si/AZ91D composites,while the hypereutectic Al-Si/AZ91D composites were opposite.The MRL included eutectic layer(E layer),intermetallic compound layer(IMC layer)and transition region layer(T layer).In the IMC layer,the hypereutectic Al-Si/AZ91D composites contained some Si solid solution and flocculent Mg_(2)Si+Al-Mg IMCs phases not presented in the hypoeutectic Al-Si/AZ91D composites.Besides,increasing Si content,the thickness proportion of the T layer increased,forming an inconsistent preferred orientation of the MRL.The shear strengths of the Al-xSi/AZ91D bimetallic composites enhanced with increasing Si content,and the Al-15Si/AZ91D composite obtained a maximum shear strength of 58.6 MPa,which was 73.4% higher than the Al-6Si/AZ91D composite.The fractures of the Al-xSi/AZ91D bimetallic composites transformed from the T layer into the E layer with the increase of the Si content.The improvement of the shear strength of the Al-xSi/AZ91D bimetallic composites was attributed to the synergistic action of the Mg_(2)Si particle reinforcement,the reduction of oxidizing inclusions and the ratio of Al-Mg IMCs as well as the orientation change of the MRL.
基金supported by the National Natural Science Foundation of China(No.21501015)the Hunan Provincial Natural Science Foundation,China(No.2022JJ30604)Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation,China(No.2022CL01)。
文摘A composite solid electrolyte comprising a Cu-Al bimetallic metal-organic framework(CAB),lithium salt(LiTFSI)and polyethylene oxide(PEO)was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes.Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.%CAB(PL-CAB-10%)exhibits high ionic conductivity(8.42×10~(-4)S/cm at 60℃),high Li+transference number(0.46),wide electrochemical window(4.91 V),good thermal stability,and outstanding mechanical properties.Furthermore,PL-CAB-10%exhibits excellent cycle stability in both Li-Li symmetric battery and Li/PL-CAB-10%/LiFePO4 asymmetric battery setups.These enhanced performances are primarily attributable to the introduction of the versatile CAB.The abundant metal sites in CAB can react with TFSI~-and PEO through Lewis acid-base interactions,promoting LiTFSI dissociation and improving ionic conductivity.Additionally,regular pores in CAB provide uniformly distributed sites for cation plating during cycling.
基金supported by the National Natural Science Committee of China-Liaoning Provincial People's Government Joint Fund(U1908204)National Natural Science Foundation of China(21876006,21976009,and 21961160743)+2 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal Institutions(IDHT20190503)Natural Science Foundation of Beijing Municipal Commission of Education(KM201710005004)Development Program for the Youth Outstanding-Notch Talent of Beijing Municipal Commission of Education(CIT&TCD201904019)。
文摘Developing the alternative supported noble metal catalysts with low cost,high catalytic efficiency,and good resistance toward carbon dioxide and water vapor is critically demanded for the oxidative removal of volatile organic compounds(VOCs).In this work,we prepared the mesoporous chromia-supported bimetallic Co and Ni single-atom(Co_(1)Ni_(1)/meso-Cr_(2)O_(3))and bimetallic Co and Ni nanoparticle(Co_(NP)Ni_(NP)/mesoCr_(2)O_(3))catalysts adopting the one-pot polyvinyl pyrrolidone(PVP)-and polyvinyl alcohol(PVA)-protecting approaches,respectively.The results indicate that the Co_(1)Ni_(1)/meso-Cr_(2)O_(3)catalyst exhibited the best catalytic activity for n-hexane(C_(6)H_(14))combustion(T_(50%)and T_(90%)were 239 and 263℃ at a space velocity of 40,000 mL g^(-1)h^(-1);apparent activation energy and specific reaction rate at 260℃ were 54.7 kJ mol^(-1)and 4.3×10^(-7)mol g^(-1)_(cat)s^(-1),respectively),which was associated with its higher(Cr^(5+)+Cr^(6+))amount,large n-hexane adsorption capacity,and good lattice oxygen mobility that could enhance the deep oxidation of n-hexane,in which Ni_(1) was beneficial for the enhancements in surface lattice oxygen mobility and low-temperature reducibility,while Co_(1) preferred to generate higher contents of the high-valence states of chromium and surface oxygen species as well as adsorption and activation of n-hexane.n-Hexane combustion takes place via the Mars van Krevelen(MvK)mechanism,and its reaction pathways are as follows:n-hexane→olefins or 3-hexyl hydroperoxide→3-hexanone,2-hexanone or 2,5-dimethyltetrahydrofuran→2-methyloxirane or 2-ethyl-oxetane→acrylic acid→CO_x→CO_(2)and H_(2)O.
基金supported by the National Natural Science Foundation of China (52203066,51973157,61904123)the Tianjin Natural Science Foundation (18JCQNJC02900)+3 种基金National innovation and entrepreneurship training program for college students (202310058007)Tianjin Municipal college students’innovation and entrepreneurship training program (202310058088)the Science&Technology Development Fund of Tianjin Education Commission for Higher Education (Grant No.2018KJ196)State Key Laboratory of Membrane and Membrane Separation,Tiangong University。
文摘Lithium-sulfur(Li-S)batteries are considered highly promising as next-generation energy storage systems due to high theoretical capacity(2600 Wh kg^(-1))and energy density(1675 mA h g^(-1))as well as the abundant natural reserves,low cost of elemental sulfur,and environmentally friendly properties.However,several challenges impede its commercialization including low conductivity of sulfur itself,the severe“shuttle effect”caused by lithium polysulfides(LiPSs)during charge–discharge processes,volume expansion effects and sluggish reaction kinetics.As a solution,polar metal particles and their compounds have been introduced as the main hosts for sulfur cathode due to their robust catalytic activity and adsorption capability,effectively suppressing the“shuttle effect”of Li PSs.Bimetallic alloys and their compounds with multi-functional properties exhibit remarkable electrochemical performance more readily when compared to single-metal materials.Well-designed bimetallic materials demonstrate larger specific surface areas and richer active sites,enabling simultaneous high adsorption capability and strong catalytic properties.The synergistic effect of the“adsorption-catalysis”sites accelerates the adsorptiondiffusion-conversion process of Li PSs,ultimately achieving a long-lasting Li-S battery.Herein,the latest progress and performance of bimetallic materials in cathodes,separators,and interlayers of Li-S batteries are systematically reviewed.Firstly,the principles and challenges of Li-S batteries are briefly analyzed.Then,various mechanisms for suppressing“shuttle effects”of Li PSs are emphasized at the microscale.Subsequently,the performance parameters of various bimetallic materials are comprehensively summarized,and some improvement strategies are proposed based on these findings.Finally,the future prospects of bimetallic materials are discussed,with the hope of providing profound insights for the rational design and manufacturing of high-performance bimetallic materials for LSBs.
基金supported by the National Naural Science Foudation of China(No.21873013 and No.22273006).
文摘The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot electrons and phonons)transfers on the interface between two metals.We have designed and synthesized Au@Cu bimetallic nanoparticles with Au as core and Cu as shell.By using transient absorption spectroscopy,we find that there are two plasmon induced heat funneling processes from Au core to Cu shell.One is the electron temperature equilibrium(electron heat transfer)with equilibration time of~560 fs.The other is the lattice temperature equilibrium(lattice heat transfer)with equilibration time of~13 ps.This plasmon induced heat funneling may be universal in similar bimetallic nanostructures,so our finding could contribute to further understanding the catalytic mechanism of bimetallic plasmonic photothermal catalysis.
文摘Hydrogen energy has become one of the recognized clean energy sources worldwide due to its advantages such as low cost,renewable energy,and green environmental protec-tion.Electrolytic water is currently one of the most promising solutions for providing hydrogen fuel.Nickel iron bimetallic electrocatalysts have abundant sources,low cost,clean and pollution-free properties,and strong catalytic performance,This article mainly reviews the development and research of bimetallic nickel iron oxides and nickel iron alloys in recent years,and explores their synthesis methods,properties,and stability in depth.
基金financially supported by the National Natural Science Foundation of China(No.52102100)the Natural Science Foundation of Jiangsu Province(No.BK20181469)the Guangdong Basic and Applied Basic Research Foundation,China(No.2020A1515110035)。
文摘To solve low efficiency,environmental pollution,and toxicity for synthesizing zeolitic imidazolate frameworks(ZIFs)in organic solvents,a KOH-assisted aqueous strategy is proposed to synthesize bimetallic ZIFs polyhedrons,which are used as precursors to prepare bimetallic selenide and N-doped carbon(NC)composites.Among them,Fe–Co–Se/NC retains the three-dimensional(3D)polyhedrons with mesoporous structure,and Fe–Co–Se nanoparticles are uniform in size and evenly distributed.When assessed as anode material for lithium-ion batteries,Fe–Co–Se/NC achieves an excellent initial specific capacity of 1165.9 m Ah·g^(-1)at 1.0 A·g^(-1),and the reversible capacity of Fe–Co–Se/NC anode is 1247.4 m Ah·g^(-1)after 550 cycles.It is attributed to that the uniform composite of bimetallic selenides and N-doped carbon can effectively tune redox active sites,the stable 3D structure of Fe–Co–Se/NCs guarantees the structural stability and wettability of the electrolyte,and the uniform distribution of Fe–Co–S nanoparticles in size esuppresses the volume expansion and accelerates the electrochemical reaction kinetics.
基金the support of the National Natural Science Foundation of China (22002118,22208262,52271228,52202298,52201279,51834009,51801151)the Natural Science Foundation of Shaanxi Province (2021JQ-468,2020JZ-47)+2 种基金the Natural Science Foundation of Shaanxi Provincial Department of Education (21JP086)the Postdoctoral Research Foundation of China (2020 M683528,2020TQ0245,2018M633643XB)the Hundred Talent Program of Shaanxi Province。
文摘The development of novel single-atom catalysts with optimal electron configuration and economical noble-metal cocatalyst for efficient photocatalytic hydrogen production is of great importance,but still challenging.Herein,we fabricate Pt and Co single-atom sites successively on polymeric carbon nitride(CN).In this Pt_(1)-Co_(1)/CN bimetallic single-atom catalyst,the noble-metal active sites are maximized,and the single-atomic Co_(1)N_4sites are tuned to Co_(1)N_3sites by photogenerated electrons arising from the introduced single-atomic Pt_(1)N_4sites.Mechanism studies and density functional theory(DFT)calculations reveal that the 3d orbitals of Co_(1)N_3single sites are filled with unpaired d-electrons,which lead to the improved visible-light response,carrier separation and charge migration for CN photocatalysts.Thereafter,the protons adsorption and activation are promoted.Taking this advantage of long-range electron synergy in bimetallic single atomic sites,the photocatalytic hydrogen evolution activity over Pt_(1)-Co_(1)/CN achieves 915.8 mmol g^(-1)Pt h^(-1),which is 19.8 times higher than Co_(1)/CN and 3.5 times higher to Pt_(1)/CN.While this electron-synergistic effect is not so efficient for Pt nanoclusters.These results demonstrate the synergistic effect at electron-level and provide electron-level guidance for the design of efficient photocatalysts.
基金financially supported by the National Natural Science Foundation of China(22172082,21978137,and 21878162)the Natural Science Foundation of Tianjin(20JCZDJC00770)+1 种基金the NCC Fund(NCC2020FH05)the Fundamental Research Funds for the Central Universities。
文摘Electrochemical CO_(2)reduction to formate is a potential approach to achieving global carbon neutrality.Here,Cu1Bi1bimetallic catalyst was prepared by a co-precipitation method.It has a ginger like composite structure(CuO/CuBi_(2)O_(4))and exhibited a high formate faradaic efficiency of 98.07%at–0.98 V and a large current density of–56.12 mA.cm^(-2)at–1.28 V,which is twice as high as Bi2O3catalyst.Especially,high selectivity(FE^(–)_(HCOO)>85%)is maintained over a wide potential window of 500 mV.In-situ Raman measurements and structure characterization revealed that the reduced Cu1Bi1bimetallic catalyst possesses abundant Cu-Bi interfaces and residual Bi-O structures.The abundant Cu-Bi interface structures on the catalyst surface can provide abundant active sites for CO_(2)RR,while the Bi-O structures may stabilize the CO_(2)^(*–)intermediate.The synergistic effect of abundant Cu-Bi interfaces and Bi-O species promotes the efficient synthesis of formate by following the OCHO^(*)pathway.
基金the financial support provided by National Natural Science Foundation of China (22008163)Postgraduate Research & Practice Innovation Program of Jiangsu Province+2 种基金Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment (SKLPEE-KF202309)Natural Science Research Project of Higher Education Institutions in Jiangsu Province (20KJB150042, 21KJB150038)Natural Science Foundation of Jiangsu Province (BK20231342, BK20210867)。
文摘Carbon dioxide reduction reaction(CO_(2)RR) represents an efficient approach to achieving carbon neutrality and simultaneously generating clean energy.However,the strong stability of CO_(2) molecules and the diversity of products pose significant challenges.As an emerging material,bimetallic catalysts have been widely reported for their unique advantages,such as tunable electronic structures,suitable adsorption/desorption of CO_(2) and intermediates,and optimizable d-band centers of active sites through bimetallic synergy.These catalysts provide a remarkable platform for converting CO_(2) into high value-added chemicals.This review comprehensively summarizes recent research advances in bimetallic catalysts for CO_(2)RR.Firstly,the challenges associated with CO_(2)RR,including activity and selectivity are analyzed,followed by a discussion on the unique advantages of bimetallic catalysts.Next,their synthesis strategies are categorized into dual-atom site catalysts(DACs),bimetallic nanoparticles and nanoclusters,binary metal semiconductors,and layered double hydroxides(LDHs).Additionally,advanced characterization techniques of bimetallic catalysts and their applications in CO_(2)RR are thoroughly introduced.Finally,the prospects and challenges for the application of bimetallic materials are highlighted.This review aims to provide inspiration for CO_(2)RR into high-value chemicals and shed light on the research of bimetallic materials.
基金financially supported by the National Natural Science Foundation of China(22172093 and 21776167)。
文摘The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt phthalocyanine(PPcFeCo)with excellent thermal stability and three-dimensional graphene(3D-G).The bimetallic synergistic effect of PPcFeCo,verified by DFT(Density functional theory)calculation,andπ-πinteractions enhances the catalytic activity and durability of the PPcFeCo/3D-G.Regarding electrochemical performance,the PPcFeCo/3D-G with a high electron transfer number(3.98,@0.768 V vs.RHE)has excellent half-wave potential(E_(1/2)=0.890 V vs.RHE)and exhibits outstanding reversibility(ΔE=0.700 V,ΔE=Ej=10-E_(1/2)).The liquid ZAB(LZAB)employed PPcFeCo/3D-G displays a high power density(222 m W cm^(-2)),a specific capacity(792 m A h g-1),and excellent durability(120 h).This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.
基金supported by the Natural Science Foundation of China(5207123251871165)。
文摘Understanding the crystal phase evolution of bimetallic oxide anodes is the main concern to profoundly reveal the conversion reaction kinetics and sodium-ion storage mechanisms.Herein,an integrated selfsupporting anode of the Cu-decorated Cu-Mn bimetallic oxides with oxygen vacancies(Ov-BMO-Cu)are in-situ generated by phase separation and hydrogen etching using nanoporous Cu-Mn alloy as selfsacrificial templates.On this basis,we have elucidated the relationship between the phase evolution,oxygen vacancies and sodium-ion storage mechanisms,further demonstrating the evolution of oxygen vacancies and the inhibition effect of manganese oxides as an“anchor”on grain aggregation of copper oxides.The kinetic analyses confirm that the expanded lattice space and increased oxygen vacancies of cycled Ov-BMO-Cu synergistically guarantee effective sodium-ion diffusion and storage mechanisms.Therefore,the Ov-BMO-Cu electrode exhibits higher reversible capacities of 4.04 mA h cm^(-2)at 0.2 mA cm^(-2)after 100 cycles and 2.20 m A h cm^(-2)at 1.0 mA cm^(-2)after 500 cycles.Besides,the presodiated Ov-BMO-Cu anode delivers a considerable reversible capacity of 0.79 m A h cm^(-2)at 1.0 mA cm^(-2)after 60 cycles in full cells with Na_(3)V_(2)(PO_(4))_(3)cathode,confirming its outstanding practicality.Thus,this work is expected to provide enlightenment for designing high-capacity bimetallic oxide anodes.
基金This work was supported by National Natural Science Foundation of China(No.51873198)the Engineering and Physical Sciences Research Council(EPSRC,EP/V027433/1)the Royal Society(RGSyR1y211080)。
文摘Efficient and stable oxygen evolution electrocatalysts are indispensable for industrial applications of water splitting and hydrogen production.Herein,a simple and practical method was applied to fabricate(Mo,Fe)P2O7@NF electrocatalyst by directly growing Mo/Fe bimetallic pyrophosphate derived from Prussian blue analogues on three-dimensional porous current collector.In alkaline media,the developed material possesses good hydrophilic features and exhibits best-in-class oxygen evolution reaction(OER)performances.Surprisingly,the(Mo,Fe)P_(2)O_(7)@NF only requires overpotentials of 250 and 290 mV to deliver 100 and 600 mA cm^(-2)in 1 mol L^(-1)KOH,respectively.Furthermore,the(Mo,Fe)P_(2)O_(7)@NF shows outstanding performances in alkaline salty water and 1 mol L^(-1)high purity KOH.A worthwhile pathway is provided to combine bimetallic pyrophosphate with commercial Ni foam to form robust electrocatalysts for stable electrocatalytic OER,which has a positive impact on both hydrogen energy application and environmental restoration.
基金the support from Shanghai QingZhen Test Technology Co.,Ltd.,China (No.880772)Dalian Jin Dian Biotechnology Co.,Ltd.,China (No.880988)+5 种基金Anhui Chromatographic Instrument Co.,Ltd.,China (No.880511)the Key Project of Anhui Provincial Department of Education,China (No.2023AH051634)the Innovative Research Team of Undergraduates,China (Nos.S202110879087 and S202210879085)the Research Funds of Anhui Science and Technology University,China (No.FZ220179)the Foundation of Anhui Science and Technology University,China (No.HCWD202001)the Science and Technology Planning Project of Bengbu City,China (No.2022gx10)。
文摘Platinum-based nanocomposites have been considered as one of the most promising catalysts for methanol oxidation reactions(MORs), which yet still suffer from low electrochemical activity and electron-transfer properties. Apart from van-der-Waals heterostructures,herein, we report a novel nanocomposite with the structure of Pt–Ru bimetallic nanoparticles covalently-bonded onto multi-walled carbon nanotubes (MWCNTs)(Pt–Ru@MWCNT), which have been successfully fabricated via a facile and green synthesis method. It is demonstrated that the Pt–Ru@MWCNT nanocomposite possesses much enhanced electrocatalytic activity with the electrochemical active surface area(ECSA) of 110.4 m^(2)·g^(-1)for Pt towards MOR, which is 2.67 and 4.0 times higher than those of 20wt%commercial Pt@C and Pt-based nanocomposite prepared by other method, due to the improved electron-transfer properties originated from M–O–C covalent bonds. This work provides us a new strategy for the structural design of highly-efficient electrocatalysts in boosting MOR performance.
基金supported by the National Key R&D Program of China (2019YFC1804102)the National Natural Science Foundation of China (32171615)。
文摘Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(ORR) kinetics on the cathode remains by far the most critical bottleneck hindering the practical application of MFC. An ideal cathode catalyst should possess excellent ORR activity, stability, and costeffectiveness, experiments have demonstrated that bimetallic catalysts are one of the most promising ORR catalysts currently. Based on this, this review mainly analyzes the reaction mechanism(ORR mechanisms, synergistic effects), advantages(combined with characterization technologies), and typical synthesis methods of bimetallic catalysts, focusing on the application effects of early Pt-M(M = Fe, Co, and Ni) alloys to bifunctional catalysts in MFC, pointing out that the main existing challenges remain economic analysis, long-term durability and large-scale application, and looking forward to this. At last, the research trend of bimetallic catalysts suitable for MFC is evaluated, and it is considered that the development and research of metal-organic framework(MOF)-based bimetallic catalysts are still worth focusing on in the future, intending to provide a reference for MFC to achieve energy-efficient wastewater treatment.