In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study invest...In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N_(2)/CO_(2) isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.展开更多
This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0...This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.展开更多
It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the effica...Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.展开更多
Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NO_(x))emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature c...Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NO_(x))emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature catalysts has become a current research focus.In this study,Nb was used to dope and modify the Mn_(7)-Cu_(3)/BCN catalyst to construct the Mn_(7)-Cu_(3)-Nb_(x)/BCN system.The doping amount was optimized through selective catalytic reduction(SCR)activity tests.The reaction mechanism was explored by combining in situ DRIFTS and density functional theory(DFT)simulations.Experimental findings revealed that the catalyst doped with 0.05%Nb achieved the optimal performance,sustaining a NO conversion efficiency of≥94%within the temperature window of 150−275℃while demonstrating improved resistance to alkali metal K poisoning.Mechanistic analyses showed that at low temperatures,the catalyst facilitated the SCR reaction via both the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)pathways,with the synergistic interaction between multiple active sites driving the efficient conversion of NH3 and NO.DFT calculations further confirmed that both pathways had the characteristics of low reaction energy barriers and significant exothermicity,ensuring the high activity and feasibility of the low-temperature reaction.The findings provided foundational theoretical support for the design of Nb-doped Mn-Cu-supported catalysts and the exploration of the underlying working mechanisms.展开更多
The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-...The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-step method to model the paleo-geothermal gradient using low-temperature thermochronology.(1)It uses the Monte Carlo approach to generate thermal histories in a vertical section randomly and calculates the entire thermal history within the goodnessof-fit thresholds based on different paleo-geothermal gradients.(2)It selects the optimum paleogeothermal gradient by comparing the entire thermal history within different goodness-of-fit thresholds.We validated the method with apatite(U-Th)/He and fission track data collected from two drill cores in the Haiyuan-Liupanshan region.The result revealed that the best-fit paleo-geothermal gradient was~42℃/km during the Early Cretaceous–Miocene and has decreased rapidly to 20℃/km since~10 Ma.The crust thickening in the study area may explain the rapid reduction in the paleogeothermal gradient since~10 Ma.Our results are consistent with earlier studies in the region,suggesting that our simple and more intuitive approach provides an alternative method for paleogeothermal gradient modeling.展开更多
Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temp...Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.展开更多
Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O cosolvent ...Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO_(3) nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO_(3) nanorods,thereby inhibiting the corrosion from H_(2)O molecules in the electrolyte and suppressing the dissolution of MoO_(3).In addition,EG molecule disturbs the hydrogen-bond network between H_(2)O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO_(3) nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO_(3) nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g^(-1)in a three-electrode system.After assembling with CuHCF cathode,under-40℃,the full battery displays negligible capacity decay for over 2500 cycles at 1 A g^(-1).These results indicate that the cosolvent strategy has the promising potential in enhancing the performance of aqueous proton batteries.展开更多
The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solv...The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO_(3)^(-),as the functional additive,compresses the electric field around Li^(+)through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.展开更多
Solid oxide cells(SOCs)are attractive electrochemical energy conversion/storage technologies for electricity/green hydrogen production because of the high efficiencies,all-solid structure,and superb reversibility.Neve...Solid oxide cells(SOCs)are attractive electrochemical energy conversion/storage technologies for electricity/green hydrogen production because of the high efficiencies,all-solid structure,and superb reversibility.Nevertheless,the widespread applications of SOCs are remarkably restricted by the inferior stability and high material costs induced by the high operational temperatures(600-800℃).Tremendous research efforts have been devoted to suppressing the operating temperatures of SOCs to decrease the overall costs and enhance the long-term durability.However,fuel electrodes as key components in SOCs suffer from insufficient(electro)catalytic activity and inferior impurity tolerance/redox resistance at reduced temperatures.Nanostructures and relevant nanomaterials exhibit great potential to boost the performance of fuel electrodes for low-temperature(LT)-SOCs due to the unique surface/interface properties,enlarged active sites,and strong interaction.Herein,an in-time review about advances in the design and fabrication of nanostructured fuel electrodes for LT-SOCs is presented by emphasizing the crucial role of nanostructure construction in boosting the performance of fuel electrodes and the relevant/distinct material design strategies.The main achievements,remaining challenges,and research trends about the development of nanostructured fuel electrodes in LT-SOCs are also presented,aiming to offer important insights for the future development of energy storage/conversion technologies.展开更多
Electrochemical reaction is emerging as a powerful approach for glucose detection and biomass conversion.However,it has been rarely explored for glucose detection and biomass conversion into valueadded chemicals.Previ...Electrochemical reaction is emerging as a powerful approach for glucose detection and biomass conversion.However,it has been rarely explored for glucose detection and biomass conversion into valueadded chemicals.Previously reported glucose oxidase reduction(GOR)catalysts exhibit issues such as low activity,limited detection range,poor sensitivity,and overreliance on noble metals.Here,we employ an impregnation method to load transition metal nickel onto carbon nanotubes(CNT)and fabricated Ni/CNT30 catalyst via a discharge process.Ni/CNT30 catalyst exhibits a remarkably high catalytic activity of up to 3336.7μA·cm^(-2)·mmol^(-1)·L,a detection limit of 2.43μmol·L^(-1),outstanding stability,and excellent resistance to impurities and interference,surpassing other noble metal-based and oxide-based materials.Hence,this material provides a new approach for the preparation of glucose sensors to achieve precise mobile measurement of glucose concentration and biofuel cells in future.展开更多
Developing a high-efficiency catalyst with both superior low-temperature activity and good N_(2)selectivity is still challenging for the NH_(3)selective catalytic reduction(SCR)of NO_(x)from mobile sources.Herein,we d...Developing a high-efficiency catalyst with both superior low-temperature activity and good N_(2)selectivity is still challenging for the NH_(3)selective catalytic reduction(SCR)of NO_(x)from mobile sources.Herein,we demonstrate the improved low-temperature activity and N_(2)selectivity by regulating the redox and acidic properties of MnCe oxides supported on etched ZSM-5 supports.The etched ZSM-5 enables the highly dispersed state of MnCeOx species and strong interaction between Mn and Ce species,which promotes the reduction of CeO2,facilitates electron transfer from Mn to Ce,and generates more Mn^(4+)and Ce^(3+)species.The strong redox capacity contributes to forming the reactive nitrate species and-NH_(2)species from oxidative dehydrogenation of NH_(3).Moreover,the adsorbed NH_(3)and-NH_(2)species are the reactive intermediates that promote the formation of N_(2).This work demonstrates an effective strategy to enhance the low-temperature activity and N_(2)selectivity of SCR catalysts,contributing to the NO_(x)control for the low-temperature exhaust gas during the cold-start of diesel vehicles.展开更多
The development of efficient low-load platinum catalysts for CO oxidation is critical for large-scale industrial applications and environmental protection.In this study,a strategy of N_(2)treatment triggered the self-...The development of efficient low-load platinum catalysts for CO oxidation is critical for large-scale industrial applications and environmental protection.In this study,a strategy of N_(2)treatment triggered the self-reforming into fully exposed Pt cluster catalysts was proposed.By adjusting the coordination environment of Pt species on the defect support through N_(2)treatment,the CO catalytic activity was significantly enhanced,achieving complete CO oxidation at 130℃with a Pt loading of only 0.1 wt.%.The turnover frequency of N_(2)-treated Pt_(FEC)/Ti-D at 160℃was 18.3 times that of untreated Pt_(SA)/Ti-D.Comprehensive characterization results indicated that the N_(2)treatment of the Pt single-atom defect catalyst facilitated the reconfiguration and evolution of the defect structure,leading to the aggregation of Pt single atoms into fully exposed Pt clusters.Notably,these fully exposed Pt clusters exhibited a reduced coordination of Pt–O in the first coordination shell compared to single atoms,which resulted in the formation of Pt–Pt metal coordination.This unique coordination structure enhanced the adsorption and activation of CO and O_(2)on the catalyst,thereby resulting in exceptionally low-temperature CO oxidation activity.This work demonstrates a promising strategy for the design,synthesis,and industrial application of efficient low-platinum load catalysts.展开更多
Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as...Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.展开更多
A series of Au/Co_(x)Fe_(3-x)O_(4) catalysts was synthesized using the sol-deposition method by depositing 2–5 nm Au particles on Fe-doped Co_(3)O_(4).Co_(2)FeO_(4),with a Co/Fe molar ratio of 2:1,exhibited higher sp...A series of Au/Co_(x)Fe_(3-x)O_(4) catalysts was synthesized using the sol-deposition method by depositing 2–5 nm Au particles on Fe-doped Co_(3)O_(4).Co_(2)FeO_(4),with a Co/Fe molar ratio of 2:1,exhibited higher specific surface area,Co^(3+)/Co^(2+)ratio,and oxygen vacancy content compared to Co_(3)O_(4).As a result,it displayed better performance in CO oxidation,achieving a total conversion temperature(T100)of 96℃.Au greatly improved the catalytic efficiency of all Co_(x)Fe_(3-x)O_(4) samples,with the 0.2%Au/Co_(2)FeO_(4) catalyst achieving a further decrease in T100 to 73℃.Stability tests conducted at room temperature on the 1%Au/Co_(x)Fe_(3-x)O_(4) catalysts demonstrated a slowed deactivation rate after Fe-doping.The reaction pathway for CO oxidation catalyzed by Au/Co_(2)FeO_(4) followed the Mars-van Krevelen mechanism.展开更多
Enhancing the electrocatalytic activity of the electrode materials,specifically oxygen reduction reaction(ORR),at lower operating temperatures(<600℃)is the prime rank to realize the commercialization of solid oxid...Enhancing the electrocatalytic activity of the electrode materials,specifically oxygen reduction reaction(ORR),at lower operating temperatures(<600℃)is the prime rank to realize the commercialization of solid oxide fuel cells(SOFCs)research.Herein,a new hexagonal structure-based cathode material was developed with the co-doping of Gd_(2)O_(3)and Cr_(2)O_(3)of parent SrFe_(12)O_(19)oxide,respectively.At 550-475℃,Sr_(0.90)Gd_(0.10)Fe_(11.90)Cr_(0.10)O_(19)(SFO-10)cathode sample leading to the large peak power density(PPD)of 395 mW/cm^(2),has appropriate surface oxygen defects(O_(β))up to 17%,as verified by X-ray photoelectron microscopy(XPS).Theoretical calculations reveal that the co-doping of Gd and Cr oxides creates lattice disorder at the hexagonal lattice,which decreases the energy barrier for ion transport and enhances the electrocatalytic characteristics of ORR.Consequently,the SFO-10 cathode shows a favorable ORR activity with the least lower polarization resistance(ASR)at 550℃with gadolinium-doped ceria(GDC)electrolyte.This work provides a self-assembled single-phase hexagonal cathode to accelerate the lowtemperature hindrance of SOFC technology.展开更多
α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 ...α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 particles. Kinetic studies on the bismuth oxidation at low-temperatures were carried out by TGA method. The results show that bismuth beads should be reunited and oxidized to become irregular Bi2O3 powders. The bismuth oxidation follows shrinking core model, and its controlling mechanism varies at different reaction time. Within 0-10 min, the kinetics is controlled by chemical reaction, after that it is controlled by O2 diffusion in the solid α-Bi2O3 layer. The apparent activation energy is determined as 55.19 kJ/mol in liquid-phase oxidation.展开更多
Co3O4 catalysts prepared with different precipitants（NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3）were investigated for the oxidation of formaldehyde（HCHO）.Among these,KHCO3-precipitated Co3O4（KHCO3-Co） was the most...Co3O4 catalysts prepared with different precipitants（NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3）were investigated for the oxidation of formaldehyde（HCHO）.Among these,KHCO3-precipitated Co3O4（KHCO3-Co） was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~＋ and CO3^（2-）,thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3＋/Co^2＋molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~＋ and CO3^（2-） on the Co3O4 surface and the favorable Co^3＋/Co^2＋ ratio.展开更多
Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The...Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.展开更多
Three different chromizing coatings were produced on Ni substrate using a conventional pack-cementation method with Al2O3,Al2O3＋CeO2 and CeO2 acting as filler,respectively,at a greatly decreased temperature（700 ℃）...Three different chromizing coatings were produced on Ni substrate using a conventional pack-cementation method with Al2O3,Al2O3＋CeO2 and CeO2 acting as filler,respectively,at a greatly decreased temperature（700 ℃）.Effects of different fillers on the isothermal and cyclic oxidation resistance of chromizing coating in air at 850 ℃ were comparably investigated.Microstructure results show that the addition of CeO2 into the filler significantly retards the grain growth of the chromizing coating.Oxidation results indicate that the chromizing coating using CeO2 as filler exhibits somewhat increased oxidation resistance than the normal chromizmg coating,while the chromizing coating using Al2O3＋CeO2 as filler exhibits much better oxidation resistance.The effects of different fillers on the oxidation behaviors were discussed in detail.展开更多
基金supported by the National Natural Science Foundation of China(No.52374247)the Joint Funds of the National Natural Science Foundation of China(No.U24B2042).
文摘In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N_(2)/CO_(2) isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.
基金financially supported by the National Natural Science Foundation of China(No.22309067)the Open Project Program of the State Key Laboratory of Materials-Oriented Chemical Engineering,China(No.KL21-05)the Marine Equipment and Technology Institute,Jiangsu University of Science and Technology,China(No.XTCX202404)。
文摘This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
基金supported by the National Key R&D Program of China (2021YFA1502802)the National Natural Science Foundation of China (U21B2092, 22202213, 22402210, 22502215, 22502214, 22572200, and 22579171)+3 种基金the International Partnership Program of Chinese Academy of Sciences (172GJHZ2022028MI)the Shenyang Bureau of Science and Technology (24-213-3-25)the Natural Science Foundation of Liaoning Province (2025BS0153)Zhongke Technology Achievement Transfer and Transformation Center of Henan Province 2025119
文摘Single-atom catalysts(SACs)have demonstrated excellent performance in heterogeneous catalytic reactions owing to their maximized atomic efficiency,distinctive geometric,and electronic configurations.However,the efficacy of SACs remains limited for certain reactions requiring simultaneous activation of multiple reactants over metallic active sites.Herein,we report an atomically dispersed Pt1Ru1 dual-atom pair site anchored on nanodiamond@graphene(ND@G)for CO oxidation.The Pt1Ru1 dual-atom catalyst shows an exceptional turnover frequency(TOF)of 17.6.10^(-2)s^(-1)at significantly lower temperature(30℃),achieving a tenfold increase in TOF compared to singleatom Pt1/ND@G catalyst(1.5.10^(-2)s^(-1))and surpassing to previously reported Pt-based catalysts under similar conditions.Moreover,the catalyst demonstrates excellent stability,maintaining its activity for 40 h at 80℃without significant deactivation.The superior catalytic performance of Pt-Ru dual-atom catalysts is attributed to the synergistic effect between Pt and Ru atoms with enhanced metallicity for improving simultaneous adsorption and activation of CO and O_(2),and the tuning of conventional competitive reactant adsorption into a non-competitive pathway over dual-atom pair sites.The present work manifests the advantages of dual-atom pair sites in heterogeneous catalysis and paves the way for precise design of catalysts at the atomic scale.
基金Supported by National Key Research and Development Program of China(2020YFD1100302)。
文摘Under the context of global energy transition and carbon neutrality,controlling nitrogen oxide(NO_(x))emissions from biomass combustion is of great significance,and the development of high-efficiency low-temperature catalysts has become a current research focus.In this study,Nb was used to dope and modify the Mn_(7)-Cu_(3)/BCN catalyst to construct the Mn_(7)-Cu_(3)-Nb_(x)/BCN system.The doping amount was optimized through selective catalytic reduction(SCR)activity tests.The reaction mechanism was explored by combining in situ DRIFTS and density functional theory(DFT)simulations.Experimental findings revealed that the catalyst doped with 0.05%Nb achieved the optimal performance,sustaining a NO conversion efficiency of≥94%within the temperature window of 150−275℃while demonstrating improved resistance to alkali metal K poisoning.Mechanistic analyses showed that at low temperatures,the catalyst facilitated the SCR reaction via both the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)pathways,with the synergistic interaction between multiple active sites driving the efficient conversion of NH3 and NO.DFT calculations further confirmed that both pathways had the characteristics of low reaction energy barriers and significant exothermicity,ensuring the high activity and feasibility of the low-temperature reaction.The findings provided foundational theoretical support for the design of Nb-doped Mn-Cu-supported catalysts and the exploration of the underlying working mechanisms.
基金supported by the National Natural Science Foundation of China(Nos.42072229,42030301,41102131,41972049,41972302 and 41977231)the Guangdong Basic and Applied Basic Research Foundation(No.2025A1515010724)+3 种基金the Guangdong Natural Science Foundation(No.2021A1515011658)the Science and Technology Program of Guangzhou(No.202002030184)the Special Fund for Basic Scientific Research of Central Colleges,Chang'an University(No.300102260502)the Deep Earth Probe and Mineral Resources Exploration-National Science and Technology Major Project(No.2024ZD1001003)。
文摘The paleo-geothermal gradient is a crucial parameter for converting the thermal history to the exhumation history.However,the precise estimation of this parameter has been a challenge.This paper presents a simple two-step method to model the paleo-geothermal gradient using low-temperature thermochronology.(1)It uses the Monte Carlo approach to generate thermal histories in a vertical section randomly and calculates the entire thermal history within the goodnessof-fit thresholds based on different paleo-geothermal gradients.(2)It selects the optimum paleogeothermal gradient by comparing the entire thermal history within different goodness-of-fit thresholds.We validated the method with apatite(U-Th)/He and fission track data collected from two drill cores in the Haiyuan-Liupanshan region.The result revealed that the best-fit paleo-geothermal gradient was~42℃/km during the Early Cretaceous–Miocene and has decreased rapidly to 20℃/km since~10 Ma.The crust thickening in the study area may explain the rapid reduction in the paleogeothermal gradient since~10 Ma.Our results are consistent with earlier studies in the region,suggesting that our simple and more intuitive approach provides an alternative method for paleogeothermal gradient modeling.
基金the financial support from the Key Project of Shaanxi Provincial Natural Science Foundation-Key Project of Laboratory(2025SYS-SYSZD-117)the Natural Science Basic Research Program of Shaanxi(2025JCYBQN-125)+8 种基金Young Talent Fund of Xi'an Association for Science and Technology(0959202513002)the Key Industrial Chain Technology Research Program of Xi'an(24ZDCYJSGG0048)the Key Research and Development Program of Xianyang(L2023-ZDYF-SF-077)Postdoctoral Fellowship Program of CPSF(GZC20241442)Shaanxi Postdoctoral Science Foundation(2024BSHSDZZ070)Research Funds for the Interdisciplinary Projects,CHU(300104240913)the Fundamental Research Funds for the Central Universities,CHU(300102385739,300102384201,300102384103)the Scientific Innovation Practice Project of Postgraduate of Chang'an University(300103725063)the financial support from the Australian Research Council。
文摘Lithium-ion batteries(LIBs),while dominant in energy storage due to high energy density and cycling stability,suffer from severe capacity decay,rate capability degradation,and lithium dendrite formation under low-temperature(LT)operation.Therefore,a more comprehensive and systematic understanding of LIB behavior at LT is urgently required.This review article comprehensively reviews recent advancements in electrolyte engineering strategies aimed at improving the low-temperature operational capabilities of LIBs.The study methodically examines critical performance-limiting mechanisms through fundamental analysis of four primary challenges:insufficient ionic conductivity under cryogenic conditions,kinetically hindered charge transfer processes,Li+transport limitations across the solidelectrolyte interphase(SEI),and uncontrolled lithium dendrite growth.The work elaborates on innovative optimization approaches encompassing lithium salt molecular design with tailored dissociation characteristics,solvent matrix optimization through dielectric constant and viscosity regulation,interfacial engineering additives for constructing low-impedance SEI layers,and gel-polymer composite electrolyte systems.Notably,particular emphasis is placed on emerging machine learning-guided electrolyte formulation strategies that enable high-throughput virtual screening of constituent combinations and prediction of structure-property relationships.These artificial intelligence-assisted rational design frameworks demonstrate significant potential for accelerating the development of next-generation LT electrolytes by establishing quantitative composition-performance correlations through advanced data-driven methodologies.
基金supported by the National Natural Science Foundation of China(22409071)Natural Foundation of Shandong Province(ZR2024QB120)+2 种基金Youth Innovation Group Plan of Shandong Province(2024KJG046)Higher-Level Talent Initial Scientific Research and Discipline Construction Fund(511/1009530)Joint Funds of the National Natural Science Foundation of China(No.U22A20140)。
文摘Protons emerge as superior charge carriers due to the lowest mass-to-charge ratio,ultra-high natural abundance,and the smallest ionic radius.Herein,2.0 M H_(2) SO_(4) dissolved in EG(ethylene glycol)/H_(2)O cosolvent is investigated as an aqueous proton battery electrolyte,which not only enhances the cycling performance of MoO_(3) nanorod anode but also improves its low-temperature electrochemical performance.Specifically,the EG tightly adsorbs onto the surface of MoO_(3) nanorods,thereby inhibiting the corrosion from H_(2)O molecules in the electrolyte and suppressing the dissolution of MoO_(3).In addition,EG molecule disturbs the hydrogen-bond network between H_(2)O molecules,which greatly decreases the freezing point of the electrolyte,endowing the MoO_(3) nanorods with excellent low-temperature electrochemical performance.Therefore,the MoO_(3) nanorods exhibit a capacity retention of 96.9%after 2000 cycles at a current density of 10 A g^(-1)in a three-electrode system.After assembling with CuHCF cathode,under-40℃,the full battery displays negligible capacity decay for over 2500 cycles at 1 A g^(-1).These results indicate that the cosolvent strategy has the promising potential in enhancing the performance of aqueous proton batteries.
基金support from the Heilongjiang Touyan Innovation Team Program(HITTY-20190033)National Natural Science Foundation of China(22278096)Innovation Special Project on Science and Technology for Carbon Peaking and Carbon Neutrality in Jiangsu Province(WSSJH20230015)。
文摘The reliable operation of lithium-ion batteries(LIBs)in low temperatures has long been hindered by severe side reactions on graphite anodes.To develop a commercially viable low-temperature electrolyte,we design a solvent-resistant Nitrate-coordinated electrolyte.The practical Ah-level graphite LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) pouch cell with the newly developed electrolyte demonstrates a significant breakthrough in cycling stability,exhibiting negligible capacity fade after 250 cycles at-30℃ and 0.1 C.NO_(3)^(-),as the functional additive,compresses the electric field around Li^(+)through electrostatic interactions,mimicking the Debye-screening effect and inducing the coordinative exclusion of free ethyl acetate molecules at low temperatures.The transformation from contact ion pairs(CIPs)formed by Pto solventseparated ion pairs is significantly restrained,which mitigates the continuous reactions between the electrolyte and inevitable lithium deposition at low temperature.Additionally,this customized inert CIPs form a solid electrolyte interphase on graphite that exhibits remarkable ionic conductivity and rigidity,preventing excessive Li dendrite growth.This finding offers new insights into the relationship of microstructure-performance for low-temperature electrolytes,demonstrating that relying solely on inert CIPs can also inhibit the decomposition of the interfacial electrolyte,and inspires a unique design concept for high-performance,commercially viable LIBs that operate reliably in sub-zero environments.
基金supported by the National Key R&D Program of China(No.2022YFB4002502)the National Natural Science Foundation of China(No.22279057)。
文摘Solid oxide cells(SOCs)are attractive electrochemical energy conversion/storage technologies for electricity/green hydrogen production because of the high efficiencies,all-solid structure,and superb reversibility.Nevertheless,the widespread applications of SOCs are remarkably restricted by the inferior stability and high material costs induced by the high operational temperatures(600-800℃).Tremendous research efforts have been devoted to suppressing the operating temperatures of SOCs to decrease the overall costs and enhance the long-term durability.However,fuel electrodes as key components in SOCs suffer from insufficient(electro)catalytic activity and inferior impurity tolerance/redox resistance at reduced temperatures.Nanostructures and relevant nanomaterials exhibit great potential to boost the performance of fuel electrodes for low-temperature(LT)-SOCs due to the unique surface/interface properties,enlarged active sites,and strong interaction.Herein,an in-time review about advances in the design and fabrication of nanostructured fuel electrodes for LT-SOCs is presented by emphasizing the crucial role of nanostructure construction in boosting the performance of fuel electrodes and the relevant/distinct material design strategies.The main achievements,remaining challenges,and research trends about the development of nanostructured fuel electrodes in LT-SOCs are also presented,aiming to offer important insights for the future development of energy storage/conversion technologies.
基金supported by the National Natural Science Foundation of China(22408225 and 22478241)the Postdoctoral Fellowship Program of CPSF(GZC20240999).
文摘Electrochemical reaction is emerging as a powerful approach for glucose detection and biomass conversion.However,it has been rarely explored for glucose detection and biomass conversion into valueadded chemicals.Previously reported glucose oxidase reduction(GOR)catalysts exhibit issues such as low activity,limited detection range,poor sensitivity,and overreliance on noble metals.Here,we employ an impregnation method to load transition metal nickel onto carbon nanotubes(CNT)and fabricated Ni/CNT30 catalyst via a discharge process.Ni/CNT30 catalyst exhibits a remarkably high catalytic activity of up to 3336.7μA·cm^(-2)·mmol^(-1)·L,a detection limit of 2.43μmol·L^(-1),outstanding stability,and excellent resistance to impurities and interference,surpassing other noble metal-based and oxide-based materials.Hence,this material provides a new approach for the preparation of glucose sensors to achieve precise mobile measurement of glucose concentration and biofuel cells in future.
基金the National Natural Science Foundation of China(Nos.22125604,22106100,21976117,22276119)Shanghai Rising-Star Program(No.22QA1403700).
文摘Developing a high-efficiency catalyst with both superior low-temperature activity and good N_(2)selectivity is still challenging for the NH_(3)selective catalytic reduction(SCR)of NO_(x)from mobile sources.Herein,we demonstrate the improved low-temperature activity and N_(2)selectivity by regulating the redox and acidic properties of MnCe oxides supported on etched ZSM-5 supports.The etched ZSM-5 enables the highly dispersed state of MnCeOx species and strong interaction between Mn and Ce species,which promotes the reduction of CeO2,facilitates electron transfer from Mn to Ce,and generates more Mn^(4+)and Ce^(3+)species.The strong redox capacity contributes to forming the reactive nitrate species and-NH_(2)species from oxidative dehydrogenation of NH_(3).Moreover,the adsorbed NH_(3)and-NH_(2)species are the reactive intermediates that promote the formation of N_(2).This work demonstrates an effective strategy to enhance the low-temperature activity and N_(2)selectivity of SCR catalysts,contributing to the NO_(x)control for the low-temperature exhaust gas during the cold-start of diesel vehicles.
基金supported by the National Natural Science Foundation of China(52170118,52322004,52230002)the China Postdoctoral Science Foundation(2024M763296).
文摘The development of efficient low-load platinum catalysts for CO oxidation is critical for large-scale industrial applications and environmental protection.In this study,a strategy of N_(2)treatment triggered the self-reforming into fully exposed Pt cluster catalysts was proposed.By adjusting the coordination environment of Pt species on the defect support through N_(2)treatment,the CO catalytic activity was significantly enhanced,achieving complete CO oxidation at 130℃with a Pt loading of only 0.1 wt.%.The turnover frequency of N_(2)-treated Pt_(FEC)/Ti-D at 160℃was 18.3 times that of untreated Pt_(SA)/Ti-D.Comprehensive characterization results indicated that the N_(2)treatment of the Pt single-atom defect catalyst facilitated the reconfiguration and evolution of the defect structure,leading to the aggregation of Pt single atoms into fully exposed Pt clusters.Notably,these fully exposed Pt clusters exhibited a reduced coordination of Pt–O in the first coordination shell compared to single atoms,which resulted in the formation of Pt–Pt metal coordination.This unique coordination structure enhanced the adsorption and activation of CO and O_(2)on the catalyst,thereby resulting in exceptionally low-temperature CO oxidation activity.This work demonstrates a promising strategy for the design,synthesis,and industrial application of efficient low-platinum load catalysts.
基金supported by the National Natural Science Foundation of China(No.52401284)the Natural Science Foundation of Jiangsu Province(No.BK20240957)+1 种基金the Key Research and Development Program of Nantong(No.GZ2024005)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_3677)。
文摘Over recent decades,fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence.Especially,ammonia has gained increasing attention as an attractive alternative to hydrogen,offering comparable energy density while maintaining carbon-free characteristics,along with superior storage and transport properties that give direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.Central to this technology is the anodic ammonia oxidation reaction(AOR),where platinum(Pt)remains the most efficient catalyst after years of intensive research.This review offers a comprehensive overview of Ptbased AOR electrocatalysts with potential for application in low-temperature DAFCs.Following an introductory section highlighting key historical developments and catalytic breakthroughs,a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented.Subsequently,it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites,highlighting material innovations and performance enhancements.Afterward,key challenges and future research directions for advancing AOR electrocatalysts are identified,with the aim of providing valuable guidance for developing practical,highperformance,and low-temperature DAFC systems.
基金supported by the Fundamental Research Program of Shanxi Province of China(202203021211103,202303021212172,202403021211196).
文摘A series of Au/Co_(x)Fe_(3-x)O_(4) catalysts was synthesized using the sol-deposition method by depositing 2–5 nm Au particles on Fe-doped Co_(3)O_(4).Co_(2)FeO_(4),with a Co/Fe molar ratio of 2:1,exhibited higher specific surface area,Co^(3+)/Co^(2+)ratio,and oxygen vacancy content compared to Co_(3)O_(4).As a result,it displayed better performance in CO oxidation,achieving a total conversion temperature(T100)of 96℃.Au greatly improved the catalytic efficiency of all Co_(x)Fe_(3-x)O_(4) samples,with the 0.2%Au/Co_(2)FeO_(4) catalyst achieving a further decrease in T100 to 73℃.Stability tests conducted at room temperature on the 1%Au/Co_(x)Fe_(3-x)O_(4) catalysts demonstrated a slowed deactivation rate after Fe-doping.The reaction pathway for CO oxidation catalyzed by Au/Co_(2)FeO_(4) followed the Mars-van Krevelen mechanism.
基金Project supported by the Scientific and Technological Innovation Team of Nanjing(NINGJIAOGAOSHI 2021 No.16)。
文摘Enhancing the electrocatalytic activity of the electrode materials,specifically oxygen reduction reaction(ORR),at lower operating temperatures(<600℃)is the prime rank to realize the commercialization of solid oxide fuel cells(SOFCs)research.Herein,a new hexagonal structure-based cathode material was developed with the co-doping of Gd_(2)O_(3)and Cr_(2)O_(3)of parent SrFe_(12)O_(19)oxide,respectively.At 550-475℃,Sr_(0.90)Gd_(0.10)Fe_(11.90)Cr_(0.10)O_(19)(SFO-10)cathode sample leading to the large peak power density(PPD)of 395 mW/cm^(2),has appropriate surface oxygen defects(O_(β))up to 17%,as verified by X-ray photoelectron microscopy(XPS).Theoretical calculations reveal that the co-doping of Gd and Cr oxides creates lattice disorder at the hexagonal lattice,which decreases the energy barrier for ion transport and enhances the electrocatalytic characteristics of ORR.Consequently,the SFO-10 cathode shows a favorable ORR activity with the least lower polarization resistance(ASR)at 550℃with gadolinium-doped ceria(GDC)electrolyte.This work provides a self-assembled single-phase hexagonal cathode to accelerate the lowtemperature hindrance of SOFC technology.
基金Project (2006BAB02B05-04- 01/02) supported by the National Key Technologies R&D Program of China
文摘α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 particles. Kinetic studies on the bismuth oxidation at low-temperatures were carried out by TGA method. The results show that bismuth beads should be reunited and oxidized to become irregular Bi2O3 powders. The bismuth oxidation follows shrinking core model, and its controlling mechanism varies at different reaction time. Within 0-10 min, the kinetics is controlled by chemical reaction, after that it is controlled by O2 diffusion in the solid α-Bi2O3 layer. The apparent activation energy is determined as 55.19 kJ/mol in liquid-phase oxidation.
基金supported by the National Natural Science Foundation of China(21577088)~~
文摘Co3O4 catalysts prepared with different precipitants（NH3·H2O,KOH,NH4HCO3,K2CO3 and KHCO3）were investigated for the oxidation of formaldehyde（HCHO）.Among these,KHCO3-precipitated Co3O4（KHCO3-Co） was the most active low-temperature catalyst,and was able to completely oxidize HCHO at the 100-ppm level to CO2 at 90℃.In situ diffuse reflectance infrared spectroscopy demonstrated that hydroxyl groups on the catalyst surface were regenerated by K~＋ and CO3^（2-）,thus promoting the oxidation of HCHO.Moreover,H2-temperature programmed reduction and X-ray photoelectron spectroscopy showed that employing KHCO3 as the precipitant increased the Co^3＋/Co^2＋molar ratio on the surface of the Co3O4 catalyst,thus further promoting oxidation.Structural characterization revealed that catalysts precipitated with carbonate or bicarbonate reagents exhibited greater specific surface areas and pore volumes.Overall,these data suggest that the high activity observed during the Co3O4 catalyzed oxidation of HCHO can be primarily attributed to the presence of K~＋ and CO3^（2-） on the Co3O4 surface and the favorable Co^3＋/Co^2＋ ratio.
文摘Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.
基金Project (11551419) supported by Scientific Research Fund of Heilongjiang Provincial Education DepartmentProject (12511469) supported by Heilongjiang Provincial Science and Technology Department
文摘Three different chromizing coatings were produced on Ni substrate using a conventional pack-cementation method with Al2O3,Al2O3＋CeO2 and CeO2 acting as filler,respectively,at a greatly decreased temperature（700 ℃）.Effects of different fillers on the isothermal and cyclic oxidation resistance of chromizing coating in air at 850 ℃ were comparably investigated.Microstructure results show that the addition of CeO2 into the filler significantly retards the grain growth of the chromizing coating.Oxidation results indicate that the chromizing coating using CeO2 as filler exhibits somewhat increased oxidation resistance than the normal chromizmg coating,while the chromizing coating using Al2O3＋CeO2 as filler exhibits much better oxidation resistance.The effects of different fillers on the oxidation behaviors were discussed in detail.
