The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this stu...The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this study,molecular dynamics(MD)simulations are employed to examine mineral-like model surfaces with varying degrees of hydrophobicity,modulated by surface charges,to elucidate the adsorption behavior of nanobubbles at the interface.Our findings not only contribute to the fundamental understanding of nanobubbles but also have potential applications in the mining industry.We observed that as the surface charge increases,the contact angle of the nanobubbles increases accordingly with shape transformation from a pancake-like gas film to a cap-like shape,and ultimately forming a stable nanobubble upon an ordered water monolayer.When the solid–water interactions are weak with a small partial charge,the hydrophobic gas(N_(2))molecules accumulate near the solid surfaces.However,we have found,for the first time,that gas molecules assemble a nanobubble on the water monolayer adjacent to the solid surfaces with large partial charges.Such phenomena are attributed to the formation of a hydrophobic water monolayer with a hydrogen bond network structure near the surface.展开更多
Herein,a ternary supramolecular assembly(BPP-BQ?CB[8]-SCD)is successfully constructed by a bromophenylpyridine-tethered-bromoisoquinoline(BPP-BQ),cucurbit[8]uril(CB[8])and sulfonatedβ-cyclodextrin(SCD)via successive ...Herein,a ternary supramolecular assembly(BPP-BQ?CB[8]-SCD)is successfully constructed by a bromophenylpyridine-tethered-bromoisoquinoline(BPP-BQ),cucurbit[8]uril(CB[8])and sulfonatedβ-cyclodextrin(SCD)via successive assembling way,exhibiting progressively enhanced green roomtemperature phosphorescence(RTP).The self-aggregates of BPP-BQ?CB[8]-SCD accommodate an energy acceptor rhodamine B(Rh B)to form a light-harvesting system(BPP-BQ?CB[8]-SCD@Rh B)with further enhanced yellow long-lifetime luminescence with large Stokes shift based on triplet-singlet F?rster resonance energy transfer(TS-FRET).Crucially,the introduction of a photoactive diarylethene achieves the long-lived photoluminescence of BPP-BQ?CB[8]-SCD@Rh B to be switched with the efficiency of up to98%through logically ordered lowering/enhancing RTP performance of the energy donor and intercepting/restoring TS-FRET pathway,when stimulated by host-vip competition and light illumination in sequence.Moreover,BPP-BQ?CB[8]-SCD@Rh B is evenly doped into polyvinyl alcohol or polyacrylamide to obtain high-performance luminescent films with long afterglow.The abovementioned logically ordered stimulus-switched long-lived emission enables the light-harvesting system in both solution and solid state to be applied in high-security-level information encryption and transformation,and anticounterfeiting.展开更多
Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,...Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.展开更多
Mimicking the electric microenvironment of natural tissue is a promising strategy for developing biomedical implants. However, current research has not taken biomimetic electrical functional units into consideration w...Mimicking the electric microenvironment of natural tissue is a promising strategy for developing biomedical implants. However, current research has not taken biomimetic electrical functional units into consideration when designing biomedical implants. In this research, ordered structures with Schottky heterojunction functional unit (OSSH) were constructed on titanium implant surfaces for bone regeneration regulation. The Schottky heterojunction functional unit is composed of periodically distributed titanium microdomain and titanium oxide microdomain with different carrier densities and surface potentials. The OSSH regulates the M2-type polarization of macrophages to a regenerative immune response by activating the PI3K-AKT-mTOR signal pathway and further promotes osteogenic differentiation of rat bone marrow mesenchymal stem cells. This work provides fundamental insights into the biological effects driven by the Schottky heterojunction functional units that can electrically modulate osteogenesis.展开更多
Weak interactions prevent the magnetic particles from achieving excellent electromagnetic wave absorp-tion(EMA)at a low filler loading(FL).The construction of one-dimensional magnetic metal fibers(1D-MMFs)contributes ...Weak interactions prevent the magnetic particles from achieving excellent electromagnetic wave absorp-tion(EMA)at a low filler loading(FL).The construction of one-dimensional magnetic metal fibers(1D-MMFs)contributes to the formation of an electromagnetic(EM)coupling network,enhancing EM properties at a low FL.However,precisely controlling the length of 1D-MMFs to regulate permittivity at low FL poses a challenge.Herein,a novel magnetic field-assisted growth strategy was used to fabricate Co-based fibers with adjustable permittivity and aspect ratios.With a variety of FL changes,centimeter-level Co long fibers(Co-lf)consistently exhibited higher permittivity than Co particles and Co short fibers due to the enhancement of the effective EM coupling.The Co-lf exhibits excellent EMA performance(-54.85 dB,5.8 GHz)at 10 wt.%FL.Meanwhile,heterogeneous interfaces were introduced to increase the interfacial polarization through a fine phosphorylation design,resulting in elevated EMA performances(-51.50 dB,6.6 GHz)at 10 wt.%FL for Co_(2)P/Co long fibers.This study improves the orderliness of the particle arrangement by regulating the length of 1D-MMFs,which affects the behavior of electrons inside the fibers,providing a new perspective for improving the EMA properties of magnetic materials at a low FL.展开更多
Because the grinding temperature is high when grinding using conventional disordered grinding wheels,the grinding quality improvement is limited when using single abrasive ordered grinding wheels,and the wheel prepara...Because the grinding temperature is high when grinding using conventional disordered grinding wheels,the grinding quality improvement is limited when using single abrasive ordered grinding wheels,and the wheel preparation process is complex and costly when using microstructured grinding wheels,abrasive groups ordered grinding wheels are widely investigated.However,there is a paucity of systematic analyses and comprehensive reviews focused on abrasive groups ordered grinding wheels.Therefore,this paper defines abrasive groups ordered grinding wheels and classifies them,based on their unique characteristics,into groups such as abrasive blocks ordered grinding wheel,fine grain structured grinding wheel,abrasive clusters ordered grinding wheel,and abrasive fibers ordered grinding wheel.We provide an overview of the latest advances in wheel structures,preparation methods,and abrasive selection for various types of abrasive groups ordered grinding wheels.Furthermore,we conduct a comparative analysis of the existing types,significant advantages,and challenges associated with the four types of abrasive groups ordered grinding wheels.Looking ahead,given the potential of abrasive groups ordered grinding wheels in reducing grinding force and temperature,we recommend further exploration of their application in combination with special processing techniques.This could pave the way for the development of machining processes that are more environmentally friendly,energy-efficient,and precise.展开更多
Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)th...Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)that featured with interconnected three-dimensional(3D)ordered porous hierarchies(3DOM FeCo/NC)are prepared,and its electrocatalytic activity is studied.Due to the open structure of 3D ordered macro-pores that greatly improves the mass transfer capacity of the catalytic process and enhances the utilization of active sites inside the catalyst,as well as the uniform distribution of Fe and Co bimetallic sites on the porous skeleton,3DOM FeCo/NC exhibits superior bi-functional catalytic activities for both hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR).The overpotential of HER is lower than that of commercial Pt/C when performed at high current density(>235 mA cm^(-2))in1.0 M KOH,and the half-wave potential(0.896 V)of ORR in 0.1 M KOH is also superior to that of 20% commercial Pt/C and most other similar catalysts.The effective utilization and synergistic effect of CoFe_(2)O_(4)and CoFe hetero-metallic sites remarkably enhance the electrocatalytic activity.Furthermore,3DOM FeCo/NC is assembled as an air electrode in Zn-air battery,and exhibits satisfactory maximum power density,open-circuit voltage,and charge/discharge stability over benchmark Pt/C+IrO_(2).This work contributes new insights into the design of transition-metal-based multifunctional catalysts,and has great potential for energy conversion and storage.展开更多
Music recommendation systems are essential due to the vast amount of music available on streaming platforms,which can overwhelm users trying to find new tracks that match their preferences.These systems analyze users...Music recommendation systems are essential due to the vast amount of music available on streaming platforms,which can overwhelm users trying to find new tracks that match their preferences.These systems analyze users’emotional responses,listening habits,and personal preferences to provide personalized suggestions.A significant challenge they face is the“cold start”problem,where new users have no past interactions to guide recommendations.To improve user experience,these systems aimto effectively recommendmusic even to such users by considering their listening behavior and music popularity.This paper introduces a novel music recommendation system that combines order clustering and a convolutional neural network,utilizing user comments and rankings as input.Initially,the system organizes users into clusters based on semantic similarity,followed by the utilization of their rating similarities as input for the convolutional neural network.This network then predicts ratings for unreviewed music by users.Additionally,the system analyses user music listening behaviour and music popularity.Music popularity can help to address cold start users as well.Finally,the proposed method recommends unreviewed music based on predicted high rankings and popularity,taking into account each user’s music listening habits.The proposed method combines predicted high rankings and popularity by first selecting popular unreviewedmusic that themodel predicts to have the highest ratings for each user.Among these,the most popular tracks are prioritized,defined by metrics such as frequency of listening across users.The number of recommended tracks is aligned with each user’s typical listening rate.The experimental findings demonstrate that the new method outperformed other classification techniques and prior recommendation systems,yielding a mean absolute error(MAE)rate and rootmean square error(RMSE)rate of approximately 0.0017,a hit rate of 82.45%,an average normalized discounted cumulative gain(nDCG)of 82.3%,and a prediction accuracy of new ratings at 99.388%.展开更多
We introduce the concepts of unitary, almost unitary and strongly almost unitary subset of an ordered semigroup. For the notions of almost unitary and strongly almost unitary subset of an ordered semigroup, we use the...We introduce the concepts of unitary, almost unitary and strongly almost unitary subset of an ordered semigroup. For the notions of almost unitary and strongly almost unitary subset of an ordered semigroup, we use the notion of translational hull of an ordered semigroup. If (S,⋅,≤) is an ordered semigroup having an element e such that e ≤ e<sup>2</sup> and U is a nonempty subset of S such that u ≤ eu, u ≤ ue for all u ∈ U, we show that U is almost unitary in S if and only if U is unitary in . Also if (S,⋅,≤) is an ordered semigroup, e ∉ S, U is a nonempty subset of S, S<sup>e</sup>:= S ∪ {e} and U<sup>e</sup>:= U ∪ {e}, we give conditions that an (“extension” of S) ordered semigroup and the subset U<sup>e</sup> of S<sup>e</sup> must satisfy in order for U to be almost unitary or strongly almost unitary in S (in case U is strongly almost unitary in S, then the given conditions are equivalent).展开更多
The development of cation-disordered rocksalt(DRX)cathodes has garnered worldwide attention due to their high capacity,broad chemical space and excellent structural flexibility.However,their low intrinsic Li-ion condu...The development of cation-disordered rocksalt(DRX)cathodes has garnered worldwide attention due to their high capacity,broad chemical space and excellent structural flexibility.However,their low intrinsic Li-ion conductivity necessitates extensive particle pulverization,typically achieved through ball-milling process,which impedes large-scale production.In this work,we present a proton-exchange assisted strategy to activate the Li-ion transport in Mn-based DRX cathodes.Short-range spinel-like ordering is observed to form within the DRX matrix after the post treatment,which significantly enhances the intrinsic Li ion mobility.Notably,more than 280 mAh g^(-1)discharge capacity can be delivered at a slow rate from micrometer-sized particles with an overall disordered cation arrangement,which retains more than150 m Ah g^(-1)when cycled at a very high rate of 2000 mA g^(-1).Furthermore,we also demonstrate that the electrochemical performance of the post-treated cathodes can be further optimized by fine-tuning the reaction parameters.展开更多
To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the c...Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.展开更多
Based on experiments and first-principles calculations,the microstructures and mechanical properties of as-cast and solution treated Mg-10Gd-4Y-xZn-0.6Zr(x=0,1,2,wt.%)alloys are investigated.The transformation process...Based on experiments and first-principles calculations,the microstructures and mechanical properties of as-cast and solution treated Mg-10Gd-4Y-xZn-0.6Zr(x=0,1,2,wt.%)alloys are investigated.The transformation process of long-period stacking ordered(LPSO)structure during solidification and heat treatment and its effect on the mechanical properties of experimental alloys are discussed.Results reveal that the stacking faults and 18R LPSO phases appear in the as-cast Mg-10Gd-4Y-1Zn-0.6Zr and Mg-10Gd-4Y-2Zn-0.6Zr alloys,respectively.After solution treatment,the stacking faults and 18R LPSO phase transform into 14H LPSO phase.The Enthalpies of formation and reaction energy of 14H and 18R LPSO are calculated based on first-principles.Results show that the alloying ability of 18R is stronger than that of 14H.The reaction energies show that the 14H LPSO phase is more stable than the 18R LPSO.The elastic properties of the 14H and 18R LPSO phases are also evaluated by first-principles calculations,and the results are in good agreement with the experimental results.The precipitation of LPSO phase improves the tensile strength,yield strength and elongation of the alloy.After solution treatment,the Mg-10Gd-4Y-2Zn-0.6Zr alloy has the best mechanical properties,and its ultimate tensile strength and yield strength are 278.7 MPa and 196.4 MPa,respectively.The elongation of Mg-10Gd-4Y-2Zn-0.6Zr reaches 15.1,which is higher than that of Mg-10Gd-4Y0.6Zr alloy.The improving mechanism of elastic modulus by the LPSO phases and the influence on the alloy mechanical properties are also analyzed.展开更多
The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction...The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.展开更多
Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells.However,the main challenge is...Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells.However,the main challenge is to develop high performance,low cost and chemically stable electrocatalysts to decline the energy barriers and enhance the sluggish kinetics of hydrogen evolution reaction(HER).Herein,a three-dimensional hierarchically ordered macroporous Ru-CoP@NC electrocatalyst(3DOM Ru-CoP@NC)derived from ordered macro-microporous metal-organic frameworks has been prepared using the precursor@template and double-solvent methods.The prepared 3DOM Ru-CoP@NC catalyst exhibits an overpotential of 15 mV(j=10 mA·cm^(-2))and a reaction Tafel slope of 38 mV·dec^(-1)in alkaline electrolyte,which are superior to commercial Pt@C catalyst.Additionally,the overpotential and reaction Tafel slope of this catalyst in acidic media are 45 mV and 50 mV·dec^(-1),respectively.The outstanding HER activities of 3DOM Ru-CoP@NC catalysts are ascribed to the 3D highly interconnectedreticular nanospaces that can increase effective reaction active sites.The N dope d carbon framework improves the electronic properties and conductivity.Moreover,the strong interaction of Ru and CoP nanoparticles also boosts the HER process.These results indicate that 3DOM Ru-CoP@NC catalysts with high catalytic activities have a broad application prospect in the future.展开更多
The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,th...The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.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
Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we...Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we prepared mesoporous carbon nanofibers(mCNFs)functionalized with ordered PtFe alloys(O-PtFe-mCNFs)by a composite micelle interface-induced co-assembly method using poly(ethylene oxide)-block-polystyrene(PEO-b-PS)as a template.When employed as electrocatalysts,O-PtFe-mCNFs exhibited superior electrocatalytic performance for the NO_(3RR)compared to the mCNFs functionalized with disordered PtFe alloys(D-PtFe-mCNFs).Notably,the NH_(3)production performance was particularly outstanding,with a maximum NH_(3)yield of up to 959.6μmol/(h·cm~2).Furthermore,the Faraday efficiency(FE)was even 88.0%at-0.4 V vs.reversible hydrogen electrode(RHE).This finding provides compelling evidence of the potential of ordered PtFe alloy catalysts for the electrocatalytic NO_(3)RR.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.12022508,12074394,and 22125604)Shanghai Supercomputer Center of ChinaShanghai Snowlake Technology Co.Ltd.
文摘The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this study,molecular dynamics(MD)simulations are employed to examine mineral-like model surfaces with varying degrees of hydrophobicity,modulated by surface charges,to elucidate the adsorption behavior of nanobubbles at the interface.Our findings not only contribute to the fundamental understanding of nanobubbles but also have potential applications in the mining industry.We observed that as the surface charge increases,the contact angle of the nanobubbles increases accordingly with shape transformation from a pancake-like gas film to a cap-like shape,and ultimately forming a stable nanobubble upon an ordered water monolayer.When the solid–water interactions are weak with a small partial charge,the hydrophobic gas(N_(2))molecules accumulate near the solid surfaces.However,we have found,for the first time,that gas molecules assemble a nanobubble on the water monolayer adjacent to the solid surfaces with large partial charges.Such phenomena are attributed to the formation of a hydrophobic water monolayer with a hydrogen bond network structure near the surface.
基金the National Natural Science Foundation of China(Nos.21801063,22305070 and U20041101)the Top-Notch Talents Program of Henan Agricultural University(Nos.30501049 and 30501032)for financial support。
文摘Herein,a ternary supramolecular assembly(BPP-BQ?CB[8]-SCD)is successfully constructed by a bromophenylpyridine-tethered-bromoisoquinoline(BPP-BQ),cucurbit[8]uril(CB[8])and sulfonatedβ-cyclodextrin(SCD)via successive assembling way,exhibiting progressively enhanced green roomtemperature phosphorescence(RTP).The self-aggregates of BPP-BQ?CB[8]-SCD accommodate an energy acceptor rhodamine B(Rh B)to form a light-harvesting system(BPP-BQ?CB[8]-SCD@Rh B)with further enhanced yellow long-lifetime luminescence with large Stokes shift based on triplet-singlet F?rster resonance energy transfer(TS-FRET).Crucially,the introduction of a photoactive diarylethene achieves the long-lived photoluminescence of BPP-BQ?CB[8]-SCD@Rh B to be switched with the efficiency of up to98%through logically ordered lowering/enhancing RTP performance of the energy donor and intercepting/restoring TS-FRET pathway,when stimulated by host-vip competition and light illumination in sequence.Moreover,BPP-BQ?CB[8]-SCD@Rh B is evenly doped into polyvinyl alcohol or polyacrylamide to obtain high-performance luminescent films with long afterglow.The abovementioned logically ordered stimulus-switched long-lived emission enables the light-harvesting system in both solution and solid state to be applied in high-security-level information encryption and transformation,and anticounterfeiting.
基金supported by National Natural Science Foundation of China(52376104,52201158)Joint Funds of the National Natural Science Foundation of China(U20A20302)+3 种基金Innovative group projects in Hebei Province(E2021202006)the project of Science and Technology in the Universities of Hebei Province(JZX2023006)Natural Science Foundation of Hebei Province(C202202003)Hebei University of Technology Cross-disciplinary(XKJC-2024001)。
文摘Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.
基金supported by the National Natural Science Foundation of China(Nos.52072127,52201297,U21A2055,and U22A20160)the China Postdoctoral Science Foundation(No.2022M711200)the Royal Society(No.IEC/NSFC/191344)(UK).
文摘Mimicking the electric microenvironment of natural tissue is a promising strategy for developing biomedical implants. However, current research has not taken biomimetic electrical functional units into consideration when designing biomedical implants. In this research, ordered structures with Schottky heterojunction functional unit (OSSH) were constructed on titanium implant surfaces for bone regeneration regulation. The Schottky heterojunction functional unit is composed of periodically distributed titanium microdomain and titanium oxide microdomain with different carrier densities and surface potentials. The OSSH regulates the M2-type polarization of macrophages to a regenerative immune response by activating the PI3K-AKT-mTOR signal pathway and further promotes osteogenic differentiation of rat bone marrow mesenchymal stem cells. This work provides fundamental insights into the biological effects driven by the Schottky heterojunction functional units that can electrically modulate osteogenesis.
基金supported by the National Key Research and Development Program of China(No.2024YFE0100600)the National Natural Science Foundation of China(No.52373303)+1 种基金the Shanghai Municipal Science and Technology Major Project(No.2021SHZDZX0100)the Fundamental Research Funds for the Central Universities and the Interdisciplinary Joint Research and Development Project of Tongji University(No.2022-4-ZD-01).
文摘Weak interactions prevent the magnetic particles from achieving excellent electromagnetic wave absorp-tion(EMA)at a low filler loading(FL).The construction of one-dimensional magnetic metal fibers(1D-MMFs)contributes to the formation of an electromagnetic(EM)coupling network,enhancing EM properties at a low FL.However,precisely controlling the length of 1D-MMFs to regulate permittivity at low FL poses a challenge.Herein,a novel magnetic field-assisted growth strategy was used to fabricate Co-based fibers with adjustable permittivity and aspect ratios.With a variety of FL changes,centimeter-level Co long fibers(Co-lf)consistently exhibited higher permittivity than Co particles and Co short fibers due to the enhancement of the effective EM coupling.The Co-lf exhibits excellent EMA performance(-54.85 dB,5.8 GHz)at 10 wt.%FL.Meanwhile,heterogeneous interfaces were introduced to increase the interfacial polarization through a fine phosphorylation design,resulting in elevated EMA performances(-51.50 dB,6.6 GHz)at 10 wt.%FL for Co_(2)P/Co long fibers.This study improves the orderliness of the particle arrangement by regulating the length of 1D-MMFs,which affects the behavior of electrons inside the fibers,providing a new perspective for improving the EMA properties of magnetic materials at a low FL.
基金Supported by National Natural Science Foundation of China(Grant No.52175401)Hunan Provincial Postgraduate Scientific Research Innovation Project(Grant No.QL20230244)+1 种基金Enterprise Innovation and Development Joint Program of National Natural Science Foundation of China(Grant No.U20B2032)Hunan Provincial Science and Technology Innovation Program(Grant No.2022RC1050).
文摘Because the grinding temperature is high when grinding using conventional disordered grinding wheels,the grinding quality improvement is limited when using single abrasive ordered grinding wheels,and the wheel preparation process is complex and costly when using microstructured grinding wheels,abrasive groups ordered grinding wheels are widely investigated.However,there is a paucity of systematic analyses and comprehensive reviews focused on abrasive groups ordered grinding wheels.Therefore,this paper defines abrasive groups ordered grinding wheels and classifies them,based on their unique characteristics,into groups such as abrasive blocks ordered grinding wheel,fine grain structured grinding wheel,abrasive clusters ordered grinding wheel,and abrasive fibers ordered grinding wheel.We provide an overview of the latest advances in wheel structures,preparation methods,and abrasive selection for various types of abrasive groups ordered grinding wheels.Furthermore,we conduct a comparative analysis of the existing types,significant advantages,and challenges associated with the four types of abrasive groups ordered grinding wheels.Looking ahead,given the potential of abrasive groups ordered grinding wheels in reducing grinding force and temperature,we recommend further exploration of their application in combination with special processing techniques.This could pave the way for the development of machining processes that are more environmentally friendly,energy-efficient,and precise.
基金financially supported by the National Natural Science Foundation of China(51902149,51674131,22305108)the Fundamental Research Funds for Public Universities in Liaoning(LJ232410140033)the Scientific Research Funding of the Education Department of Liaoning Province(JYTZD2023070,LJKFZ20220180,LJKMZ20220453)。
文摘Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)that featured with interconnected three-dimensional(3D)ordered porous hierarchies(3DOM FeCo/NC)are prepared,and its electrocatalytic activity is studied.Due to the open structure of 3D ordered macro-pores that greatly improves the mass transfer capacity of the catalytic process and enhances the utilization of active sites inside the catalyst,as well as the uniform distribution of Fe and Co bimetallic sites on the porous skeleton,3DOM FeCo/NC exhibits superior bi-functional catalytic activities for both hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR).The overpotential of HER is lower than that of commercial Pt/C when performed at high current density(>235 mA cm^(-2))in1.0 M KOH,and the half-wave potential(0.896 V)of ORR in 0.1 M KOH is also superior to that of 20% commercial Pt/C and most other similar catalysts.The effective utilization and synergistic effect of CoFe_(2)O_(4)and CoFe hetero-metallic sites remarkably enhance the electrocatalytic activity.Furthermore,3DOM FeCo/NC is assembled as an air electrode in Zn-air battery,and exhibits satisfactory maximum power density,open-circuit voltage,and charge/discharge stability over benchmark Pt/C+IrO_(2).This work contributes new insights into the design of transition-metal-based multifunctional catalysts,and has great potential for energy conversion and storage.
基金funded by the National Nature Sciences Foundation of China with Grant No.42250410321。
文摘Music recommendation systems are essential due to the vast amount of music available on streaming platforms,which can overwhelm users trying to find new tracks that match their preferences.These systems analyze users’emotional responses,listening habits,and personal preferences to provide personalized suggestions.A significant challenge they face is the“cold start”problem,where new users have no past interactions to guide recommendations.To improve user experience,these systems aimto effectively recommendmusic even to such users by considering their listening behavior and music popularity.This paper introduces a novel music recommendation system that combines order clustering and a convolutional neural network,utilizing user comments and rankings as input.Initially,the system organizes users into clusters based on semantic similarity,followed by the utilization of their rating similarities as input for the convolutional neural network.This network then predicts ratings for unreviewed music by users.Additionally,the system analyses user music listening behaviour and music popularity.Music popularity can help to address cold start users as well.Finally,the proposed method recommends unreviewed music based on predicted high rankings and popularity,taking into account each user’s music listening habits.The proposed method combines predicted high rankings and popularity by first selecting popular unreviewedmusic that themodel predicts to have the highest ratings for each user.Among these,the most popular tracks are prioritized,defined by metrics such as frequency of listening across users.The number of recommended tracks is aligned with each user’s typical listening rate.The experimental findings demonstrate that the new method outperformed other classification techniques and prior recommendation systems,yielding a mean absolute error(MAE)rate and rootmean square error(RMSE)rate of approximately 0.0017,a hit rate of 82.45%,an average normalized discounted cumulative gain(nDCG)of 82.3%,and a prediction accuracy of new ratings at 99.388%.
文摘We introduce the concepts of unitary, almost unitary and strongly almost unitary subset of an ordered semigroup. For the notions of almost unitary and strongly almost unitary subset of an ordered semigroup, we use the notion of translational hull of an ordered semigroup. If (S,⋅,≤) is an ordered semigroup having an element e such that e ≤ e<sup>2</sup> and U is a nonempty subset of S such that u ≤ eu, u ≤ ue for all u ∈ U, we show that U is almost unitary in S if and only if U is unitary in . Also if (S,⋅,≤) is an ordered semigroup, e ∉ S, U is a nonempty subset of S, S<sup>e</sup>:= S ∪ {e} and U<sup>e</sup>:= U ∪ {e}, we give conditions that an (“extension” of S) ordered semigroup and the subset U<sup>e</sup> of S<sup>e</sup> must satisfy in order for U to be almost unitary or strongly almost unitary in S (in case U is strongly almost unitary in S, then the given conditions are equivalent).
基金funding support from the National Natural Science Foundation of Chinathe Institute of WeiqiaoUCAS Science and Technologythe Fundamental Research Funds for the Central Universities。
文摘The development of cation-disordered rocksalt(DRX)cathodes has garnered worldwide attention due to their high capacity,broad chemical space and excellent structural flexibility.However,their low intrinsic Li-ion conductivity necessitates extensive particle pulverization,typically achieved through ball-milling process,which impedes large-scale production.In this work,we present a proton-exchange assisted strategy to activate the Li-ion transport in Mn-based DRX cathodes.Short-range spinel-like ordering is observed to form within the DRX matrix after the post treatment,which significantly enhances the intrinsic Li ion mobility.Notably,more than 280 mAh g^(-1)discharge capacity can be delivered at a slow rate from micrometer-sized particles with an overall disordered cation arrangement,which retains more than150 m Ah g^(-1)when cycled at a very high rate of 2000 mA g^(-1).Furthermore,we also demonstrate that the electrochemical performance of the post-treated cathodes can be further optimized by fine-tuning the reaction parameters.
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金Ministry of Trade,Industry and Energy,Grant/Award Number:20010095Korea Evaluation Institute of Industrial Technology,Grant/Award Number:20012341。
文摘Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.
基金supported by the National Key Research and Development Program of China[grant No.2018YFB2001800]National Natural Science Foundation of China[grant No.51871184]Dalian High-level Talents Innovation Support Program[grant No.2021RD06]。
文摘Based on experiments and first-principles calculations,the microstructures and mechanical properties of as-cast and solution treated Mg-10Gd-4Y-xZn-0.6Zr(x=0,1,2,wt.%)alloys are investigated.The transformation process of long-period stacking ordered(LPSO)structure during solidification and heat treatment and its effect on the mechanical properties of experimental alloys are discussed.Results reveal that the stacking faults and 18R LPSO phases appear in the as-cast Mg-10Gd-4Y-1Zn-0.6Zr and Mg-10Gd-4Y-2Zn-0.6Zr alloys,respectively.After solution treatment,the stacking faults and 18R LPSO phase transform into 14H LPSO phase.The Enthalpies of formation and reaction energy of 14H and 18R LPSO are calculated based on first-principles.Results show that the alloying ability of 18R is stronger than that of 14H.The reaction energies show that the 14H LPSO phase is more stable than the 18R LPSO.The elastic properties of the 14H and 18R LPSO phases are also evaluated by first-principles calculations,and the results are in good agreement with the experimental results.The precipitation of LPSO phase improves the tensile strength,yield strength and elongation of the alloy.After solution treatment,the Mg-10Gd-4Y-2Zn-0.6Zr alloy has the best mechanical properties,and its ultimate tensile strength and yield strength are 278.7 MPa and 196.4 MPa,respectively.The elongation of Mg-10Gd-4Y-2Zn-0.6Zr reaches 15.1,which is higher than that of Mg-10Gd-4Y0.6Zr alloy.The improving mechanism of elastic modulus by the LPSO phases and the influence on the alloy mechanical properties are also analyzed.
基金supported by the National Key Research and Development Program of China(2021YFB4001301)the Science and Technology Commission of Shanghai Municipality(21DZ1208600)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2021ZD105)。
文摘The long-range periodically ordered atomic structures in intermetallic nanoparticles(INPs)can significantly enhance both the electrocatalytic activity and electrochemical stability toward the oxygen reduction reaction(ORR)compared to the disordered atomic structures in ordinary solid-solution alloy NPs.Accordingly,through a facile and scalable synthetic method,a series of carbon-supported ultrafine Pt_3Co_(x)Mn_(1-x)ternary INPs are prepared in this work,which possess the"skin-like"ultrathin Pt shells,the ordered L1_(2) atomic structure,and the high-even dispersion on supports(L1_(2)-Pt_3Co_(x)Mn_(1-x)/~SPt INPs/C).Electrochemical results present that the composition-optimized L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C exhibits the highest electrocata lytic activity among the series,which are also much better than those of the pristine ultrafine Pt/C.Besides,it also has a greatly enhanced electrochemical stability.In addition,the effects of annealing temperature and time are further investigated.More importantly,such superior ORR electrocatalytic performance of L1_(2)-Pt_3Co_(0.7)Mn_(0.3)/~SPt INPs/C are also well demonstrated in practical fuel cells.Physicochemical characterization analyses further reveal the major origins of the greatly enhanced ORR electrocata lytic performance:the Pt-Co-Mn alloy-induced geometric and ligand effects as well as the extremely high L1_(2) atomic-ordering degree.This work not only successfully develops a highly active and stable ordered ternary intermetallic ORR electrocatalyst,but also elucidates the corresponding"structure-function"relationship,which can be further applied in designing other intermetallic(electro)catalysts.
基金financially supported by the National Natural Science Foundation of China(Nos.U20A20237,52371218,51863005,52271205,51871065,51971068and52101245)the Scientific Research and Technology Development Program of Guangxi(Nos.AA19182014,AD 17195073,AA17202030-1,AB21220027 and 2021AB17045)+6 种基金the National Natural Science Foundation of Guangxi Province(Nos.2021GXNSFBA075057,2018GXNSFDA281051,2014GXNSFAA118401 and 2013GXNSFBA019244)the Scientific Research and Technology Development Program of Guilin(Nos.20210102-4 and 20210216-1)Guangxi Bagui Scholar FoundationGuilin Lijiang Scholar FoundationGuangxi Collaborative Innovation Centre of Structure and Property for New Energy and MaterialsGuangxi Advanced Functional Materials FoundationApplication Talents Small Highlands and Chinesisch-Deutsche Kooperationsgruppe(No.GZ1528)。
文摘Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells.However,the main challenge is to develop high performance,low cost and chemically stable electrocatalysts to decline the energy barriers and enhance the sluggish kinetics of hydrogen evolution reaction(HER).Herein,a three-dimensional hierarchically ordered macroporous Ru-CoP@NC electrocatalyst(3DOM Ru-CoP@NC)derived from ordered macro-microporous metal-organic frameworks has been prepared using the precursor@template and double-solvent methods.The prepared 3DOM Ru-CoP@NC catalyst exhibits an overpotential of 15 mV(j=10 mA·cm^(-2))and a reaction Tafel slope of 38 mV·dec^(-1)in alkaline electrolyte,which are superior to commercial Pt@C catalyst.Additionally,the overpotential and reaction Tafel slope of this catalyst in acidic media are 45 mV and 50 mV·dec^(-1),respectively.The outstanding HER activities of 3DOM Ru-CoP@NC catalysts are ascribed to the 3D highly interconnectedreticular nanospaces that can increase effective reaction active sites.The N dope d carbon framework improves the electronic properties and conductivity.Moreover,the strong interaction of Ru and CoP nanoparticles also boosts the HER process.These results indicate that 3DOM Ru-CoP@NC catalysts with high catalytic activities have a broad application prospect in the future.
基金gratefully acknowledge the financial support of the National Natural Science Foundation of China(22108145 and 21978143)the Shandong Province Natural Science Foundation(ZR2020QB189)+1 种基金State Key Laboratory of Heavy Oil Processing(SKLHOP202203008)the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering(STHGYX2201).
文摘The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method.During the preparation of the Fe-NC catalyst,the complexation of N elements in urea could anchor Fe,and the formation of C3N4during urea pyrolysis could also prevent migration and aggregation of Fe species,which jointly improve the dispersion and stability of Fe.The FeN4sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation,while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process,which together promote catalytic degradation of m-cresol by PMS activation.Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO_(4)^(-)·and·OH,and partially based on·OH as the active components,and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed.This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.
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National Natural Science Foundation of China(Nos.52225204,52173233 and 52202085)Innovation Program of Shanghai Municipal Education Commission,China(No.2021-01-07-00-03-E00109)+3 种基金Natural Science Foundation of Shanghai,China(No.23ZR1479200)“Shuguang Program”Supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission,China(No.20SG33)Fundamental Research Funds for the Central Universities,China(No.2232024Y-01)DHU Distinguished Young Professor Program,China(Nos.LZA2022001 and LZB2023002)。
文摘Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we prepared mesoporous carbon nanofibers(mCNFs)functionalized with ordered PtFe alloys(O-PtFe-mCNFs)by a composite micelle interface-induced co-assembly method using poly(ethylene oxide)-block-polystyrene(PEO-b-PS)as a template.When employed as electrocatalysts,O-PtFe-mCNFs exhibited superior electrocatalytic performance for the NO_(3RR)compared to the mCNFs functionalized with disordered PtFe alloys(D-PtFe-mCNFs).Notably,the NH_(3)production performance was particularly outstanding,with a maximum NH_(3)yield of up to 959.6μmol/(h·cm~2).Furthermore,the Faraday efficiency(FE)was even 88.0%at-0.4 V vs.reversible hydrogen electrode(RHE).This finding provides compelling evidence of the potential of ordered PtFe alloy catalysts for the electrocatalytic NO_(3)RR.
