The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction tempera...The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction temperature(>250℃)is the prerequisite to ensure high conversion of esters.Here,we report a highly dispersed MoO_(x)-Ru/C bimetallic catalyst for the efficient hydrogenolysis of esters to alkanes under 150°C.The optimal catalyst exhibits>99%conversion of methyl stearate and 99%selectivity to diesel-range alkanes,reaching a high rate of up to 2.0 mmol gcat^(–1)h^(–1),5 times higher than that of Ru/C catalyst(MoO_(x)/C is inert).Integrated experimental and theoretical investigations attribute the high performance to the abundant MoO_(x)-Ru interfacial sites on the catalyst surface,which offers high activity for the C–O cleavage of esters.Furthermore,the dispersed MoO_(x)species significantly weaken the hydrocracking activity of the metallic Ru for C–C bonds,thus yielding alkane products without carbon loss.This study provides a facile and novel strategy for the design of high-performance heterogeneous catalysts for the hydrodeoxygenation of biomass-derived esters to alkane products.展开更多
The high activity and stability of intermetallic PtCo nanocatalysts toward oxygen reduction reaction make them a top candidate as low-Pt cathode catalysts in proton exchange membrane fuel cells(PEMFCs).However,forming...The high activity and stability of intermetallic PtCo nanocatalysts toward oxygen reduction reaction make them a top candidate as low-Pt cathode catalysts in proton exchange membrane fuel cells(PEMFCs).However,forming intermetallic structures typically requires high-temperature annealing,posing a challenge for achieving well-size control and highly ordered structures.Here we report the design and synthesis of bimetallic co re@shell structured precursors for affording high-performance intermetallic PtCo catalysts.The fabrication of the core@shell precursor involves using a molecular ligand containing both sulfur and oxygen donors to selectively bind with Pt colloidal nanoparticles as the core and chelate Co ions as the shell.During high-temperature annealing,the ligand transforms into carbon coatings around alloy nanoparticles,preventing particle sintering;meanwhile,Co ions in the shell can easily diffuse into the Pt core,which helps to increase the thermodynamic driving force for forming intermetallic structures.These benefits enable us to obtain the catalyst with finely dispersed nanoparticles(~3.5 nm)and a high ordering degree of 72%.With 0.1 mgPt/cm^(2)cathode loading,the catalyst delivers superior performance and durability in PEMFCs,showing an initial mass activity of 0.56 A/mgPt,an initial power density of 1.05 W/cm^(2)at 0.67 V(H_(2)-air),and a voltage loss of 26 mV at 0.8 A/cm^(2)after the accelerated durability test.展开更多
Immiscible bimetal systems,of which tungsten–copper(W–Cu)is a typical representative,have crucial applications in fields requiring both mechanical and physical properties.Nevertheless,it is a major challenge to dete...Immiscible bimetal systems,of which tungsten–copper(W–Cu)is a typical representative,have crucial applications in fields requiring both mechanical and physical properties.Nevertheless,it is a major challenge to determine how to give full play to the advantages of the two phases of the bimetal and achieve outstanding comprehensive properties.In this study,an ultrafine-grained W–Cu bimetal with spatially connected Cu and specific Wislands was fabricated through a designed powder-mixing process and subsequent rapid low-temperature sintering.The prepared bimetal concurrently has a high yield strength,large plastic strain,and high electrical conductivity.The stress distribution and strain response of individual phases in different types of W–Cu bimetals under loading were quantified by means of a simulation.The high yield strength of the reported bimetal results from the microstructure refinement and high contiguity of the grains in the W islands,which enhance the contribution of W to the total plastic deformation of the bimetal.The high electrical conductivity is attributed to the increased mean free path of the Cu and the reduced proportion of phase boundaries due to the specific phase combination of W islands and Cu.This work provides new insight into modulating phase configuration in immiscible metallic composites to achieve high-level multi-objective properties.展开更多
Solar interfacial evaporation(SIE),is currently one of the most potential water supply technologies in the remote,insular,and disaster-stricken areas.However,the existence of volatile organic compounds(VOCs)in water d...Solar interfacial evaporation(SIE),is currently one of the most potential water supply technologies in the remote,insular,and disaster-stricken areas.However,the existence of volatile organic compounds(VOCs)in water deteriorates the distillate quality,threatening human health.Herein,we constructed a carbonbased bimetallic(C/FeCo)photothermal membrane by electrospinning technique.Results illustrated that the membrane can catalytically degrade VOCs during SIE with persulfate(PDS)mediation.PDS,as well as phenol,was mainly reacted on the interface of the photothermal membrane instead of in the bulk solution.The interception efficiency of phenol achieved nearly 100%using the C/FeCo membrane during SIE.Hydroxyl radical(•OH),sulfate radical(SO_(4)•−),superoxide radical(O_(2)•−),and singlet oxygen(^(1)O_(2))were identified as the main active substances to degrade VOCs.We also conducted SIE experiments using actual river water to evaluate the practical performance of the C/FeCo membrane.This work holds the promise of VOCs interception during SIE and enlarges the application of solar distillation in water/wastewater treatment.展开更多
Although bimetallic phosphide cocatalysts have attracted considerable interest in photocatalysis research owing to their advantageous thermodynamic characteristics,superstable and efficient cocatalysts have rarely bee...Although bimetallic phosphide cocatalysts have attracted considerable interest in photocatalysis research owing to their advantageous thermodynamic characteristics,superstable and efficient cocatalysts have rarely been produced through the modulation of their structure and composition.In this study,a series of bimetallic nickel-iron phosphide(Ni_(x)Fe_(2-x)P,where 0<x<2)cocatalysts with controllable structures and overpotentials were designed by adjusting the atomic ratio of Ni/Fe onto nonmetallic elemental red phosphorus(RP)for the photocatalytic selective oxidation of benzyl alcohol(BA)coupled with hydrogen production.The catalysts exhibited an outstanding photocatalytic activity for benzaldehyde and a high H_(2)yield.The RP regulated by bimetallic phosphide cocatalysts(Ni_(x)Fe_(2-x)P)demonstrated higher photocatalytic oxidation-reduction activity than that regulated by monometallic phosphide cocatalysts(Ni_(2)P and Fe2P).In particular,the RP regulated by Ni_(1.25)Fe_(0.75)P exhibited the best photocatalytic performance.In addition,experimental and theoretical calculations further illustrated that Ni_(1.25)Fe_(0.75)P,with the optimized electronic structure,possessed good electrical conductivity and provided strong adsorption and abundant active sites,thereby accelerating electron migration and lowering the reaction energy barrier of RP.This finding offers valuable insights into the rational design of highly effective cocatalysts aimed at optimizing the photocatalytic activity of composite photocatalysts.展开更多
Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-program...Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-programmed reduction （TPR）. Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/（C4 olefin＋C4 paraffin） ratio, and C5 olefin/（C5 olefin＋C5 paraffin） decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.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
The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Tran...The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Transition metal catalysts offer a cost-effective alternative to precious metals for catalyzing HMF oxidation, with transition bimetallic catalysts emerging as particularly promising candidates. In this review, we delve into the intricate reaction pathways and electrochemical mechanisms underlying HMF oxidation, emphasizing the pivotal role of transition bimetallic catalysts in enhancing catalytic efficiency. Subsequently, various types of transition bimetallic catalysts are explored, detailing their synthesis methods and structural modulation strategies. By elucidating the mechanisms behind catalyst modification and performance enhancement, this review sets the stage for upcoming advancements in the field, ultimately advancing the electrochemical HMF conversion and facilitating the transition towards sustainable chemical production.展开更多
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
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
Bimetallic nanocrystals have attracted considerable attention because of their complicated systems,which are far superior to those of their individual constituents.A TiO_(2)-confined PtMnP bimetallic catalyst(PtMnP@Ti...Bimetallic nanocrystals have attracted considerable attention because of their complicated systems,which are far superior to those of their individual constituents.A TiO_(2)-confined PtMnP bimetallic catalyst(PtMnP@TiO_(2)) was prepared using an ultrasonic-assisted coincident strategy,which demonstrated exceptional catalytic activity in the universal hydrogen evolution reaction (HER).Owing to the bimetallic synergistic effect and TiO_(2) confinement,PtMnP@TiO_(x)showed ultrasmall metal nanoparticles (NPs),a higher active Pt^(0) content,adequate activation at the porous surface,and abundant acid sites.Simulations were performed to visualize the strain properties of Mn and Pt during the bending process and demonstrate the high activity of Pt.The Pt-Mn bimetallic catalysts were enriched with Pt NPs,convoyed by electron transfer from Mn to Pt.Briefly,PtMnP@TiO_(2) showed robust evolution reaction activities (an overpotential of 220 mV at a current density of 10 mA cm^(-2) and a Tafel slope of 186 mV dec^(-1))and the ability to contrast stated catalysts without ultrasonication-plasma.This protocol revealed that the geometrical and electronic effects of Pt and P surrounding the Mn species in PtMnP@TiO_(2) were crucial for increasing the catalytic activity (99%) and durability (over 20 cycles),which were far superior to those of other reported catalysts.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
In the present study,microstructural evolution,mechanical and creep properties of Al/SiC/Cu composite stripsfabricated via accumulative roll bonding(ARB)process were studied.The obtained results showed the formation o...In the present study,microstructural evolution,mechanical and creep properties of Al/SiC/Cu composite stripsfabricated via accumulative roll bonding(ARB)process were studied.The obtained results showed the formation of anatomic diffusion layer with thickness of about 17μm at the interface during the ARB under three creep loadingconditions namely 30 MPa at 225℃,35 MPa at 225℃,and 35 MPa at 275℃.An generated intermetallic compoundresulted in a 40%increase of interface thickness near Al.The stress level decreased by 13%at constant temperature withno signi fi cant effect on the interface thickness,and the creep failure time declined by 44%.It was observed that atconstant temperatures,the second slope of the creep curve reached to 39%with increasing stress level,then,it dropped to2%with a little temperature rising.After creep test under 35 MPa at 275℃,the sample displays the presence of 60%Aland 40%Cu,containing brittle Al_(2)Cu intermetallic compound at the interface.Applied temperature and stress had effecton the creep properties,specially increasing the slope of creep curves with higher stresses.展开更多
Recently,there has been considerable interest in high-efficiency ultraviolet(UV)photodetectors for their potential practical uses.In this study,a high-quality UV photodetector was fabricated using a combination of Ag ...Recently,there has been considerable interest in high-efficiency ultraviolet(UV)photodetectors for their potential practical uses.In this study,a high-quality UV photodetector was fabricated using a combination of Ag and Au NPs with GaN film.The GaN film was deposited using sputtering technique,whereas Ag and Au films were grown using thermal evaporation technique.Ag-Au bimetallic nanoparticles were formed by treating them at the various annealing temperature to improve the interaction between light and the photoactive layers of the photodetectors.The optimal annealing temperature to achieve the best performance of a photodetector is 650℃.This led to a photoresponsivity of 98.5 A/W and the ON/OFF ratio of 705 at low bias voltage of 1 V.This work establishes the foundation for the advancement of high-performance UV photodetectors.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
The construction of CoeMn mixed-metal oxide catalysts derived from bimetallic metaleorganic frameworks(MOFs)has great significance for catalytic destruction of toluene.Hence,a series of Co_(a)Mn_(b)O_(x)-MOFs with dif...The construction of CoeMn mixed-metal oxide catalysts derived from bimetallic metaleorganic frameworks(MOFs)has great significance for catalytic destruction of toluene.Hence,a series of Co_(a)Mn_(b)O_(x)-MOFs with different physicochemical properties were successfully synthesized via pyrolysis of CoeMn bimetallic MOFs.Attributing to the higher specific surface area,more active sites(Co^(3+)and Mn^(3+)),stronger reducibility,and abundant defect sites,the as-prepared Co_(1)Mn_(1)O_(x)-MOFs displayed an optimal catalytic performance,especially the excellent water vapor resistance.The result of the in situ diffuse reflectance infrared Fourier transform spectroscopy demonstrated that toluene can be degraded at relatively low temperatures(<100℃).Benzyl alcohol,benzaldehyde,benzoic acid,and maleic anhydride were the main intermediate products in toluene degradation process.This work reveals the value of bimetallic MOFs derived Co-Mn oxides for toluene oxidation and presents a novel avenue for designing mixed-metal oxide catalysts with potential applications in volatile organic compounds(VOCs)catalytic oxidation.展开更多
Two-dimensional(2D)catalytic ozonation membranes are promising for the treatment of micropollutants in wastewater due to simultaneous ozone-catalyzed degradation and membrane filtration processes.However,it remains ch...Two-dimensional(2D)catalytic ozonation membranes are promising for the treatment of micropollutants in wastewater due to simultaneous ozone-catalyzed degradation and membrane filtration processes.However,it remains challenging for 2D catalytic ozonation membranes to efficiently degrade micropollutants due to low mass-transfer efficiency and poor catalytic activity.Herein,Fe/Mn bimetallic metal-organic framework(MOF)intercalated lamellar MnO_(2) membranes with fast and robust ozone-catalyzed mass-transfer channels were developed on the surface of the hollow fiber ceramic membrane(HFCM)to obtain 2D Fe/Mn-MOF@MnO_(2)-HFCM for efficiently degrading micropollutants in wastewater.The intercalation of Fe/Mn-MOF expanded the interlayer spacing of the MnO_(2) membrane,thereby providing abundant transport channels for rapid passage of water.More notably,the Fe/Mn-MOF provided enriched reactive sites as well as high electron transfer efficiency based on the redox cycling between Mn^(3+)/Mn^(4+) and Fe^(2+)/Fe^(3+),ensuring the effective catalytic oxidative degradation of micropollutants including tetracycline hydrochloride(TCH),methylene blue,and methyl blue.Moreover,the carboxyl groups on the MOF formed covalent bonds(-COO-)with the hydroxyl groups in MnO_(2) between layers,which increased the interaction between MnO_(2) nanosheets to form stable interlayer channels.Specifically,the optimal composite membrane achieved a high removal rate of TCH micropollutant(93.4%),high water treatment capacity(282 L·m^(-2)·h^(-1)·MPa^(-1)),and excellent longterm stability(1200 min).This study provides a simple and easily scalable strategy to construct fast,efficient,and stable 2D catalytic mass-transfer channels for the efficient treatment of micropollutants in wastewater.展开更多
To modify the thermodynamics and kinetic performance of magnesium hydride(MgH_(2))for solid-state hydrogen storage,Ni_(3)V_(2)O_(8)-rGO(rGO represents reduced graphene oxide)and Ni_(3)V_(2)O_(8)nanocomposites were pre...To modify the thermodynamics and kinetic performance of magnesium hydride(MgH_(2))for solid-state hydrogen storage,Ni_(3)V_(2)O_(8)-rGO(rGO represents reduced graphene oxide)and Ni_(3)V_(2)O_(8)nanocomposites were prepared by hydrothermal and subsequent heat treatment.The beginning hydrogen desorption temperature of 7 wt.%Ni_(3)V_(2)O_(8)-rGO modified MgH_(2)was reduced to 208℃,while the additive-free MgH_(2)and 7 wt.%Ni_(3)V_(2)O_(8)doped MgH_(2)appeared to discharge hydrogen at 340 and 226℃,respectively.A charging capacity of about 4.7 wt.%H_(2)for MgH_(2)+7 wt.%Ni_(3)V_(2)O_(8)-rGO was achieved at 125℃ in 10 min,while the dehydrogenated MgH_(2)took 60 min to absorb only 4.6 wt.%H_(2)at 215℃.The microstructure analysis confirmed that the in-situ generated Mg_(2)Ni/Mg_(2)N_(i)H_(4) and metallic V contributed significantly to the enhanced performance of MgH_(2).In addition,the presence of rGO in the MgH_(2)+7 wt.%Ni_(3)V_(2)O_(8)-rGO composite reduced particle aggregation tendency of Mg/MgH_(2),leading to improving the cyclic stability of MgH_(2)during 20 cycles.展开更多
文摘The efficient hydrogenolysis of esters to alkanes is the key protocol for producing advanced biofuels from renewable plant oils or fats.Due to the low reactivity of the carbonyl group in esters,a high reaction temperature(>250℃)is the prerequisite to ensure high conversion of esters.Here,we report a highly dispersed MoO_(x)-Ru/C bimetallic catalyst for the efficient hydrogenolysis of esters to alkanes under 150°C.The optimal catalyst exhibits>99%conversion of methyl stearate and 99%selectivity to diesel-range alkanes,reaching a high rate of up to 2.0 mmol gcat^(–1)h^(–1),5 times higher than that of Ru/C catalyst(MoO_(x)/C is inert).Integrated experimental and theoretical investigations attribute the high performance to the abundant MoO_(x)-Ru interfacial sites on the catalyst surface,which offers high activity for the C–O cleavage of esters.Furthermore,the dispersed MoO_(x)species significantly weaken the hydrocracking activity of the metallic Ru for C–C bonds,thus yielding alkane products without carbon loss.This study provides a facile and novel strategy for the design of high-performance heterogeneous catalysts for the hydrodeoxygenation of biomass-derived esters to alkane products.
基金the funding support from the National Natural Science Foundation of China(Grants 22325903,22221003,and 22071225)the National Key Research and Development Program of China(Grant 2018YFA0702001)+1 种基金the Plan for Anhui Major Provincial Science&Technology Project(Grants 202203a0520013 and 2021d05050006)the USTC Research Funds of the Double First-Class Initiative(Grant YD2060002032).
文摘The high activity and stability of intermetallic PtCo nanocatalysts toward oxygen reduction reaction make them a top candidate as low-Pt cathode catalysts in proton exchange membrane fuel cells(PEMFCs).However,forming intermetallic structures typically requires high-temperature annealing,posing a challenge for achieving well-size control and highly ordered structures.Here we report the design and synthesis of bimetallic co re@shell structured precursors for affording high-performance intermetallic PtCo catalysts.The fabrication of the core@shell precursor involves using a molecular ligand containing both sulfur and oxygen donors to selectively bind with Pt colloidal nanoparticles as the core and chelate Co ions as the shell.During high-temperature annealing,the ligand transforms into carbon coatings around alloy nanoparticles,preventing particle sintering;meanwhile,Co ions in the shell can easily diffuse into the Pt core,which helps to increase the thermodynamic driving force for forming intermetallic structures.These benefits enable us to obtain the catalyst with finely dispersed nanoparticles(~3.5 nm)and a high ordering degree of 72%.With 0.1 mgPt/cm^(2)cathode loading,the catalyst delivers superior performance and durability in PEMFCs,showing an initial mass activity of 0.56 A/mgPt,an initial power density of 1.05 W/cm^(2)at 0.67 V(H_(2)-air),and a voltage loss of 26 mV at 0.8 A/cm^(2)after the accelerated durability test.
基金supported by the National Natural Science Foundation of China(92163107,52171061,and 52371128)the National Key Research and Development Program of China(2022YFB3708800 and 2021YFB3501502).
文摘Immiscible bimetal systems,of which tungsten–copper(W–Cu)is a typical representative,have crucial applications in fields requiring both mechanical and physical properties.Nevertheless,it is a major challenge to determine how to give full play to the advantages of the two phases of the bimetal and achieve outstanding comprehensive properties.In this study,an ultrafine-grained W–Cu bimetal with spatially connected Cu and specific Wislands was fabricated through a designed powder-mixing process and subsequent rapid low-temperature sintering.The prepared bimetal concurrently has a high yield strength,large plastic strain,and high electrical conductivity.The stress distribution and strain response of individual phases in different types of W–Cu bimetals under loading were quantified by means of a simulation.The high yield strength of the reported bimetal results from the microstructure refinement and high contiguity of the grains in the W islands,which enhance the contribution of W to the total plastic deformation of the bimetal.The high electrical conductivity is attributed to the increased mean free path of the Cu and the reduced proportion of phase boundaries due to the specific phase combination of W islands and Cu.This work provides new insight into modulating phase configuration in immiscible metallic composites to achieve high-level multi-objective properties.
基金the National Natural Science Foundation of China(No.52070052)the National Natural Science Foundation of China(No.52300082)+3 种基金National Key Research and Development Program of China(No.2022YFB3805903)the State Key Laboratory of Urban Water Resource and Environment in HIT of China(No.2022TS14)the China Postdoctoral Science Foundation(No.2023M730881)Postdoctoral Fellowship Program of CPSF(No.GZB20230964)。
文摘Solar interfacial evaporation(SIE),is currently one of the most potential water supply technologies in the remote,insular,and disaster-stricken areas.However,the existence of volatile organic compounds(VOCs)in water deteriorates the distillate quality,threatening human health.Herein,we constructed a carbonbased bimetallic(C/FeCo)photothermal membrane by electrospinning technique.Results illustrated that the membrane can catalytically degrade VOCs during SIE with persulfate(PDS)mediation.PDS,as well as phenol,was mainly reacted on the interface of the photothermal membrane instead of in the bulk solution.The interception efficiency of phenol achieved nearly 100%using the C/FeCo membrane during SIE.Hydroxyl radical(•OH),sulfate radical(SO_(4)•−),superoxide radical(O_(2)•−),and singlet oxygen(^(1)O_(2))were identified as the main active substances to degrade VOCs.We also conducted SIE experiments using actual river water to evaluate the practical performance of the C/FeCo membrane.This work holds the promise of VOCs interception during SIE and enlarges the application of solar distillation in water/wastewater treatment.
文摘Although bimetallic phosphide cocatalysts have attracted considerable interest in photocatalysis research owing to their advantageous thermodynamic characteristics,superstable and efficient cocatalysts have rarely been produced through the modulation of their structure and composition.In this study,a series of bimetallic nickel-iron phosphide(Ni_(x)Fe_(2-x)P,where 0<x<2)cocatalysts with controllable structures and overpotentials were designed by adjusting the atomic ratio of Ni/Fe onto nonmetallic elemental red phosphorus(RP)for the photocatalytic selective oxidation of benzyl alcohol(BA)coupled with hydrogen production.The catalysts exhibited an outstanding photocatalytic activity for benzaldehyde and a high H_(2)yield.The RP regulated by bimetallic phosphide cocatalysts(Ni_(x)Fe_(2-x)P)demonstrated higher photocatalytic oxidation-reduction activity than that regulated by monometallic phosphide cocatalysts(Ni_(2)P and Fe2P).In particular,the RP regulated by Ni_(1.25)Fe_(0.75)P exhibited the best photocatalytic performance.In addition,experimental and theoretical calculations further illustrated that Ni_(1.25)Fe_(0.75)P,with the optimized electronic structure,possessed good electrical conductivity and provided strong adsorption and abundant active sites,thereby accelerating electron migration and lowering the reaction energy barrier of RP.This finding offers valuable insights into the rational design of highly effective cocatalysts aimed at optimizing the photocatalytic activity of composite photocatalysts.
文摘Silica, alumina, and activated carbon supported iron-cobalt catalysts were prepared by incipient wetness impregnation. These catalysts have been characterized by BET, X-ray diffraction （XRD）, and temperature-programmed reduction （TPR）. Activity and selectivity of iron-cobalt supported on different carriers for CO hydrogenation were studied under the conditions of 1.5 MPa, 493 K, 630 h^-1, and H2/CO ratio of 1.6. The results indicate that the activity, C4 olefin/（C4 olefin＋C4 paraffin） ratio, and C5 olefin/（C5 olefin＋C5 paraffin） decrease in the order of Fe-Co/SiO2, Fe-Co/AC1, Fe-Co/Al2O3 and Fe- Co/AC2. The activity of Fe-Co/SiO2 reached a maximum. The results of TPR show that the Fe-Co/SiO2 catalyst is to some extent different. XRD patterns show that the Fe-Co/SiO2 catalyst differs significantly from the others; it has two diffraction peaks. The active spinel phase is correlated with the supports.
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Hubei Provincial Natural Science Foundation of China (2023AFB0049)Scientific Research Fund Project of Wuhan Institute of Technology (K202232 and K2023028)Graduate Education Innovation Fund of Wuhan Institute of Technology (CX2023091)。
文摘The electrochemical oxidation of 5-hydroxymethylfurfural(HMF) represents a significant avenue for sustainable chemical synthesis, owing to its potential to generate high-value derivatives from biomass feedstocks. Transition metal catalysts offer a cost-effective alternative to precious metals for catalyzing HMF oxidation, with transition bimetallic catalysts emerging as particularly promising candidates. In this review, we delve into the intricate reaction pathways and electrochemical mechanisms underlying HMF oxidation, emphasizing the pivotal role of transition bimetallic catalysts in enhancing catalytic efficiency. Subsequently, various types of transition bimetallic catalysts are explored, detailing their synthesis methods and structural modulation strategies. By elucidating the mechanisms behind catalyst modification and performance enhancement, this review sets the stage for upcoming advancements in the field, ultimately advancing the electrochemical HMF conversion and facilitating the transition towards sustainable chemical production.
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 Research Foundation of Republic Korea (NRF-2022R1A2C1004392)。
文摘Bimetallic nanocrystals have attracted considerable attention because of their complicated systems,which are far superior to those of their individual constituents.A TiO_(2)-confined PtMnP bimetallic catalyst(PtMnP@TiO_(2)) was prepared using an ultrasonic-assisted coincident strategy,which demonstrated exceptional catalytic activity in the universal hydrogen evolution reaction (HER).Owing to the bimetallic synergistic effect and TiO_(2) confinement,PtMnP@TiO_(x)showed ultrasmall metal nanoparticles (NPs),a higher active Pt^(0) content,adequate activation at the porous surface,and abundant acid sites.Simulations were performed to visualize the strain properties of Mn and Pt during the bending process and demonstrate the high activity of Pt.The Pt-Mn bimetallic catalysts were enriched with Pt NPs,convoyed by electron transfer from Mn to Pt.Briefly,PtMnP@TiO_(2) showed robust evolution reaction activities (an overpotential of 220 mV at a current density of 10 mA cm^(-2) and a Tafel slope of 186 mV dec^(-1))and the ability to contrast stated catalysts without ultrasonication-plasma.This protocol revealed that the geometrical and electronic effects of Pt and P surrounding the Mn species in PtMnP@TiO_(2) were crucial for increasing the catalytic activity (99%) and durability (over 20 cycles),which were far superior to those of other reported catalysts.
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In the present study,microstructural evolution,mechanical and creep properties of Al/SiC/Cu composite stripsfabricated via accumulative roll bonding(ARB)process were studied.The obtained results showed the formation of anatomic diffusion layer with thickness of about 17μm at the interface during the ARB under three creep loadingconditions namely 30 MPa at 225℃,35 MPa at 225℃,and 35 MPa at 275℃.An generated intermetallic compoundresulted in a 40%increase of interface thickness near Al.The stress level decreased by 13%at constant temperature withno signi fi cant effect on the interface thickness,and the creep failure time declined by 44%.It was observed that atconstant temperatures,the second slope of the creep curve reached to 39%with increasing stress level,then,it dropped to2%with a little temperature rising.After creep test under 35 MPa at 275℃,the sample displays the presence of 60%Aland 40%Cu,containing brittle Al_(2)Cu intermetallic compound at the interface.Applied temperature and stress had effecton the creep properties,specially increasing the slope of creep curves with higher stresses.
基金supported by the Physics development program grant funded by Vietnam Academy of Science and Technology (VAST) (KHCBVL.06/24-25)support by the Korea Evaluation Institute of Industrial Technology (KEIT)grant funded by the Korean government (MOTIE) (No.RS-2022-00143570).
文摘Recently,there has been considerable interest in high-efficiency ultraviolet(UV)photodetectors for their potential practical uses.In this study,a high-quality UV photodetector was fabricated using a combination of Ag and Au NPs with GaN film.The GaN film was deposited using sputtering technique,whereas Ag and Au films were grown using thermal evaporation technique.Ag-Au bimetallic nanoparticles were formed by treating them at the various annealing temperature to improve the interaction between light and the photoactive layers of the photodetectors.The optimal annealing temperature to achieve the best performance of a photodetector is 650℃.This led to a photoresponsivity of 98.5 A/W and the ON/OFF ratio of 705 at low bias voltage of 1 V.This work establishes the foundation for the advancement of high-performance UV photodetectors.
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financial support of the National Natural Science Foundation of China(22408252,22078215)Natural Science Foundation for Youths of Shanxi Province(202103021223347)+1 种基金Taiyuan Institute of Technology Talent Introduction Research funding Project(2022KJ010)Shanxi Province Science and Technology Major Special Plan“Reveal The List and Take Charge”Project(202201090301014).
文摘The construction of CoeMn mixed-metal oxide catalysts derived from bimetallic metaleorganic frameworks(MOFs)has great significance for catalytic destruction of toluene.Hence,a series of Co_(a)Mn_(b)O_(x)-MOFs with different physicochemical properties were successfully synthesized via pyrolysis of CoeMn bimetallic MOFs.Attributing to the higher specific surface area,more active sites(Co^(3+)and Mn^(3+)),stronger reducibility,and abundant defect sites,the as-prepared Co_(1)Mn_(1)O_(x)-MOFs displayed an optimal catalytic performance,especially the excellent water vapor resistance.The result of the in situ diffuse reflectance infrared Fourier transform spectroscopy demonstrated that toluene can be degraded at relatively low temperatures(<100℃).Benzyl alcohol,benzaldehyde,benzoic acid,and maleic anhydride were the main intermediate products in toluene degradation process.This work reveals the value of bimetallic MOFs derived Co-Mn oxides for toluene oxidation and presents a novel avenue for designing mixed-metal oxide catalysts with potential applications in volatile organic compounds(VOCs)catalytic oxidation.
基金supported by the National Key Research and Development Program(2021YFB3801303)the National Natural Science Foundation of China(22408161,21921006)+1 种基金the Key Research and Development Program of Jiangsu Provincial Department of Science and Technology(BE2022033-3)the State Key Laboratory of Materials-Oriented Chemical Engineering(SKL-MCE-22A03).
文摘Two-dimensional(2D)catalytic ozonation membranes are promising for the treatment of micropollutants in wastewater due to simultaneous ozone-catalyzed degradation and membrane filtration processes.However,it remains challenging for 2D catalytic ozonation membranes to efficiently degrade micropollutants due to low mass-transfer efficiency and poor catalytic activity.Herein,Fe/Mn bimetallic metal-organic framework(MOF)intercalated lamellar MnO_(2) membranes with fast and robust ozone-catalyzed mass-transfer channels were developed on the surface of the hollow fiber ceramic membrane(HFCM)to obtain 2D Fe/Mn-MOF@MnO_(2)-HFCM for efficiently degrading micropollutants in wastewater.The intercalation of Fe/Mn-MOF expanded the interlayer spacing of the MnO_(2) membrane,thereby providing abundant transport channels for rapid passage of water.More notably,the Fe/Mn-MOF provided enriched reactive sites as well as high electron transfer efficiency based on the redox cycling between Mn^(3+)/Mn^(4+) and Fe^(2+)/Fe^(3+),ensuring the effective catalytic oxidative degradation of micropollutants including tetracycline hydrochloride(TCH),methylene blue,and methyl blue.Moreover,the carboxyl groups on the MOF formed covalent bonds(-COO-)with the hydroxyl groups in MnO_(2) between layers,which increased the interaction between MnO_(2) nanosheets to form stable interlayer channels.Specifically,the optimal composite membrane achieved a high removal rate of TCH micropollutant(93.4%),high water treatment capacity(282 L·m^(-2)·h^(-1)·MPa^(-1)),and excellent longterm stability(1200 min).This study provides a simple and easily scalable strategy to construct fast,efficient,and stable 2D catalytic mass-transfer channels for the efficient treatment of micropollutants in wastewater.
基金the financial support from the National Natural Science Foundation of China(No.51801078).
文摘To modify the thermodynamics and kinetic performance of magnesium hydride(MgH_(2))for solid-state hydrogen storage,Ni_(3)V_(2)O_(8)-rGO(rGO represents reduced graphene oxide)and Ni_(3)V_(2)O_(8)nanocomposites were prepared by hydrothermal and subsequent heat treatment.The beginning hydrogen desorption temperature of 7 wt.%Ni_(3)V_(2)O_(8)-rGO modified MgH_(2)was reduced to 208℃,while the additive-free MgH_(2)and 7 wt.%Ni_(3)V_(2)O_(8)doped MgH_(2)appeared to discharge hydrogen at 340 and 226℃,respectively.A charging capacity of about 4.7 wt.%H_(2)for MgH_(2)+7 wt.%Ni_(3)V_(2)O_(8)-rGO was achieved at 125℃ in 10 min,while the dehydrogenated MgH_(2)took 60 min to absorb only 4.6 wt.%H_(2)at 215℃.The microstructure analysis confirmed that the in-situ generated Mg_(2)Ni/Mg_(2)N_(i)H_(4) and metallic V contributed significantly to the enhanced performance of MgH_(2).In addition,the presence of rGO in the MgH_(2)+7 wt.%Ni_(3)V_(2)O_(8)-rGO composite reduced particle aggregation tendency of Mg/MgH_(2),leading to improving the cyclic stability of MgH_(2)during 20 cycles.
