Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing...Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.展开更多
The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous me...The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.展开更多
Photocatalytic water oxidation is a crucial counter-electrode reaction in the process of photoelectrochemical energy conversion.Despite its importance,challenges remain in effectively and sustainably converting water ...Photocatalytic water oxidation is a crucial counter-electrode reaction in the process of photoelectrochemical energy conversion.Despite its importance,challenges remain in effectively and sustainably converting water to oxygen,particularly with readily available and inexpensive electrolyte solutions such as seawater.While metal oxide materials have demonstrated their advantages in promoting efficiency by reducing overpotential and improving light utilization,stability remains limited by corrosion in multicomponent seawater.In this paper,we reviewed the relationship between four basic concepts including photoelectrochemistry,metal oxide,water oxidation and seawater to better understand the challenges and opportunities in photoelectrochemical(PEC)seawater oxidation.To overcome these challenges,the advances in material design,interfacial modification,local environment control and reactor design have been further reviewed to benefit the industrial PEC seawater oxidation.Noticeably,we demonstrate engineered layered metal oxide electrodes and cell structures that enable powerful and stable seawater oxidation.We also outline and advise on the future direction in this area.展开更多
Traditional selection of combustion catalysis is time-consuming and labor-intensive.Theoretical calculation is expected to resolve this problem.The adsorption energy of HMX and O atoms on 13 metal oxides was calculate...Traditional selection of combustion catalysis is time-consuming and labor-intensive.Theoretical calculation is expected to resolve this problem.The adsorption energy of HMX and O atoms on 13 metal oxides was calculated using DMol3,since HMX and O are key substances in decomposition process.And the relationship between the adsorption energy of HMX,O on metal oxides(TiO_(2),Al_(2)O_(3),PbO,CuO,Fe_(2)O_(3),Co_(3)O_(4),Bi_(2)O_(3),NiO)and experimental T30 values(time required for the decomposition depth of HMX to reach 30%)was depicted as volcano plot.Thus,the T30 values of other metal oxides was predicted based on their adsorption energy on volcano plot and validated by previous experimental data.Further,the adsorption energy of HMX on ZrO_(2)and MnO_(2)was predicted based on the linear relationship between surface energy and adsorption energy,and T30 values were estimated based on volcano plot.The apparent activation energy data of HMX/MgO,HMX/SnO_(2),HMX/ZrO_(2),and HMX/MnO_(2)obtained from DSC experiments are basically consistent with our predicted T30 values,indicating that it is feasible to predict the catalytic activity based on the adsorption calculation,and it is expected that these simple structural properties can predict adsorption energy to reduce the large quantities of computation and experiment cost.展开更多
Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The dire...Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.展开更多
Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from t...Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.展开更多
Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TM...Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TMOs)are regarded as potential substitutes for PGMs because of their stability in oxidizing environments and excellent catalytic performance.In this study,comprehensive investigation into the influence of elastic strains on the adsorption energies of carbon(C),hydrogen(H)and oxygen(O)on TMOs was conducted.Based on density functional theory(DFT)calculations,these effects in both tetragonal structures(PtO_(2),PdO_(2))and hexagonal structures(ZnO,CdO),along with their respective transition metals were systematically explored.It was identified that the optimal adsorption sites on metal oxides pinpointed the top of oxygen or the top of metal atom,while face-centered cubic(FCC)and hexagonal close-packed(HCP)holes were preferred for the transition metals.Furthermore,under the influence of elastic strains,the results demonstrated significant disparities in the adsorption energies of H and O between oxides and transition metals.Despite these differences,the effect of elastic strains on the adsorption energies of C,H and O on TMOs mirrored those on transition metals:adsorption energies increased under compressive strains,indicating weaker adsorption,and decreased under tension strains,indicating stronger adsorption.This behavior was rationalized based on the d-band model for adsorption atop a metallic atom or the p-band model for adsorption atop an oxygen atom.Consequently,elastic strains present a promising avenue for tailoring the catalytic properties of TMOs.展开更多
Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocol...Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocols,high-temperature heating process,incompatible solvents,etc.),it is still challenging to achieve efficient and reliable all-metal-oxide-based devices.Here,we developed efficient inverted PSCs(IPSCs)based on solution-processed nickel oxide(NiO_(x))and tin oxide(SnO_(2))nanoparticles,working as hole and electron transport materials respectively,enabling a fast and balanced charge transfer for photogenerated charge carriers.Through further understanding and optimizing the perovskite/metal oxide interfaces,we have realized an outstanding power conversion efficiency(PCE)of 23.5%(the bandgap of the perovskite is 1.62 eV),which is the highest efficiency among IPSCs based on all-metal-oxide charge transport materials.Thanks to these stable metal oxides and improved interface properties,ambient stability(retaining 95%of initial PCE after 1 month),thermal stability(retaining 80%of initial PCE after 2 weeks)and light stability(retaining 90%of initial PCE after 1000 hours aging)of resultant devices are enhanced significantly.In addition,owing to the low-temperature fabrication procedures of the entire device,we have obtained a PCE of over 21%for flexible IPSCs with enhanced operational stability.展开更多
Metal oxide-based electrocatalysts are promising alternatives to platinum group metals for water splitting due to their low cost,abundant raw materials,and impressive stability.This review covers recent progress in va...Metal oxide-based electrocatalysts are promising alternatives to platinum group metals for water splitting due to their low cost,abundant raw materials,and impressive stability.This review covers recent progress in various metal oxides tailored for hydrogen and oxygen evolution reactions,discussing their crystal structure,composition,and surface modification influence on performance.Strategies like surface engineering,doping,and nanostructuring are evaluated for enhancing catalytic activity and stability.The key considerations for commercialization are highlighted,emphasizing ongoing research,innovation,and future scope to drive widespread adoption of water-splitting technology for a cleaner and sustainable future.展开更多
Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structur...Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.展开更多
Most of volatile organic compounds (VOCs) are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalys...Most of volatile organic compounds (VOCs) are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalysts. Many catalysts including transition metal oxides, mixed metal oxides, and sup‐ported noble metals have been developed. Among these catalysts, the porous ones attract much attention. In this review, we focus on recent advances in the synthesis of ordered mesoporous and macroporous transition metal oxides, perovskites, and supported noble metal catalysts and their catalytic oxidation of VOCs. The porous catalysts outperformed their bulk counterparts. This excel‐lent catalytic performance was due to their high surface areas, high concentration of adsorbed oxy‐gen species, low temperature reducibility, strong interaction between noble metal and support and highly dispersed noble metal nanoparticles and unique porous structures. Catalytic oxidation of carbon monoxide over typical catalysts was also discussed. We made conclusive remarks and pro‐posed future work for the removal of VOCs.展开更多
As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants....As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.展开更多
Room-temperature gas sensors have aroused great attention in current gas sensor technology because of deemed demand of cheap,low power consumption and portable sensors for rapidly growing Internet of things applicatio...Room-temperature gas sensors have aroused great attention in current gas sensor technology because of deemed demand of cheap,low power consumption and portable sensors for rapidly growing Internet of things applications.As an important approach,light illumination has been exploited for room-temperature operation with improving gas sensor's attributes including sensitivity,speed and selectivity.This review provides an overview of the utilization of photoactivated nanomaterials in gas sensing field.First,recent advances in gas sensing of some exciting different nanostructures and hybrids of metal oxide semiconductors under light illumination are highlighted.Later,excellent gas sensing performance of emerging two-dimensional materialsbased sensors under light illumination is discussed in details with proposed gas sensing mechanism.Originated impressive features from the interaction of photons with sensing materials are elucidated in the context of modulating sensing characteristics.Finally,the review concludes with key and constructive insights into current and future perspectives in the light-activated nanomaterials for optoelectronic gas sensor applications.展开更多
This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It...This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It includes the description of the main types of metal oxide catalysts, of their various preparation procedures and of the main reactions catalysed by them (acid-base type, selective and total oxidations, bi-functional catalysis, photocatalysis, biomass treatments, environmental catalysis and some of the numerous industrial applications). Challenges and prospectives are also discussed.展开更多
g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photo...g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photoabsorption.Rationally designing g-C_(3)N_(4)-based heterojunction is promising for improving photocatalytic activity.Besides,g-C_(3)N_(4) exhibits great potentials in electrochemical energy storage.In view of the excellent performance of typical transition metal oxides(TMOs)in photocatalysis and energy storage,this review summarized the advances of TMOs/g-C_(3)N_(4) heterojunctions in the above two areas.Firstly,we introduce several typical TMOs based on their crystal structures and band structures.Then,we summarize different kinds of TMOs/g-C_(3)N_(4) heterojunctions,including type Ⅰ/Ⅱ heterojunction,Z-scheme,p-n junction and Schottky junction,with diverse photocatalytic applications(pollutant degradation,water splitting,CO_(2) reduction and N_(2) fixation)and supercapacitive energy storage.Finally,some promising strategies for improving the performance of TMOs/g-C_(3)N_(4) were proposed.Particularly,the exploration of photocatalysis-assisted supercapacitors was discussed.展开更多
Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)a...Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)as precursors,are extensively used as catalysts for VOCs oxidation due to their uniformity advantage.This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years.Particularly,it addresses the VOCs abatement performance over MMO,noble metal/MMO,core-shell structured MMO,and integral MMO film catalysts originating from LDHs.Moreover,it highlights the water vapor effect and oxidation mechanism.This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.展开更多
With the rapid development of the Internet of Things,there is a great demand for portable gas sensors.Metal oxide semiconductors(MOS)are one of the most traditional and well-studied gas sensing materials and have been...With the rapid development of the Internet of Things,there is a great demand for portable gas sensors.Metal oxide semiconductors(MOS)are one of the most traditional and well-studied gas sensing materials and have been widely used to prepare various commercial gas sensors.However,it is limited by high operating temperature.The current research works are directed towards fabricating high-performance flexible room-temperature(FRT)gas sensors,which are effective in simplifying the structure of MOS-based sensors,reducing power consumption,and expanding the application of portable devices.This article presents the recent research progress of MOS-based FRT gas sensors in terms of sensing mechanism,performance,flexibility characteristics,and applications.This review comprehensively summarizes and discusses five types of MOS-based FRT gas sensors,including pristine MOS,noble metal nanoparticles modified MOS,organic polymers modified MOS,carbon-based materials(carbon nanotubes and graphene derivatives)modified MOS,and two-dimensional transition metal dichalcogenides materials modified MOS.The effect of light-illuminated to improve gas sensing performance is further discussed.Furthermore,the applications and future perspectives of FRT gas sensors are also discussed.展开更多
Metal oxide (TiO2 or Co304) doped activated carbon nanofibers (ACNFs) were prepared by electrospinning. These nanofibers were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and B...Metal oxide (TiO2 or Co304) doped activated carbon nanofibers (ACNFs) were prepared by electrospinning. These nanofibers were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and Brunner- Emmett-Teller method (BET). The results show that the average diameters of ACNFs were within the range of 200-500 nm, and the lengths were several tens of micrometers. The specific surface areas were 1146.7 m2/g for TiO2-doped ACNFs and 1238.5 m2/g for Co304-doped ACNFs, respectively. The electrospun nanofibers were used for adsorption of low concentration sulfur dioxide (SO2). The results showed that the adsorption rates of these ACNFs increased with an increase in SO2concentration. When the SO2 concentration was 1.0 μg/mL, the adsorption rates of TiO2-doped ACNFs and Co3Oa-doped ACNFs were 66.2% and 67.1%, respectively. The adsorption rate also increased as the adsorption time increased. When the adsorption time was 40 min, the adsorption rates were 67.6% and 69.0% for TiO2-doped ACNFs and Co304-doped ACNFs, respectively. The adsorption rate decreased as the adsorption temperature increased below 60℃, while it increased as the adsorption temperature increased to more than 60℃.展开更多
Decomposition of hexachlorobenzene(HCB)was investigated over several metal oxides(i.e.,MgO,CaO,BaO,La2O3,CeO2,MnO2, Fe2O3,and Co3O4)supported on Al2O3,which was achieved in closed system at a temperature of 300°C...Decomposition of hexachlorobenzene(HCB)was investigated over several metal oxides(i.e.,MgO,CaO,BaO,La2O3,CeO2,MnO2, Fe2O3,and Co3O4)supported on Al2O3,which was achieved in closed system at a temperature of 300°C.Catalysts were prepared by incipient wetness impregnation with different metal oxides loading and impregnating solvents.The decomposition effciency of different catalysts for this reaction depends on the nature of the metal oxide used,and Al2O3 supported La2O3 was found to be the most active one.Pe...展开更多
Difference of montmorillonite (Mt), illite (It) and kaolinite (Kt) in lead sorption characteristics and the effects of amorphous Fe and Al oxide coatings on the characteristics were experimentally studied with logisti...Difference of montmorillonite (Mt), illite (It) and kaolinite (Kt) in lead sorption characteristics and the effects of amorphous Fe and Al oxide coatings on the characteristics were experimentally studied with logistic model. The sorption curves had sigmoid feature due to use of acetate-type buffer solution. With the model the sorption process could be divided into four stages and the sorption characteristics at the stages were discussed. The results showed that, after Mt, It and Kt were coated by amorphous Fe oxide, their maximum sorption capacity (MSC) and percentage of high-SSC concentration scope (HCS) of Pb2+ increased markedly, but the specific sorption capacity (SSC) decreased. With regard to effects of amorphous Al oxide coating, except for It+AI, the SSC of other samples showed a downtrend, despite that their MSC remained unchanged. Eventually, the gray correlation degrees to Pb2+ sorption for different physicochemical characteristics of the clay minerals were indicated to be higher for hydronium, zero point of surface charge and hydroxy, but lower for specific surface area, density of surface charge and amount of surface charges.展开更多
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Ministry of Science and ICT(MSIT)(RS-2023-00251283,and 2022M3D1A2083618)by the Ministry of Education(2020R1A6A1A03040516).
文摘Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.
基金funded by the National Natural Science Foundation of China,China (Nos.52272303 and 52073212)the General Program of Municipal Natural Science Foundation of Tianjin,China (Nos.17JCYBJC22700 and 17JCYBJC17000)the State Scholarship Fund of China Scholarship Council,China (Nos.201709345012 and 201706255009)。
文摘The global energy-related CO_(2) emissions have rapidly increased as the world economy heavily relied on fossil fuels.This paper explores the pressing challenge of CO_(2) emissions and highlights the role of porous metal oxide materials in the electrocatalytic reduction of CO_(2)(CO_(2)RR).The focus is on the development of robust and selective catalysts,particularly metal and metal-oxide-based materials.Porous metal oxides offer high surface area,enhancing the accessibility to active sites and improving reaction kinetics.The tunability of these materials allows for tailored catalytic behavior,targeting optimized reaction mechanisms for CO_(2)RR.The work also discusses the various synthesis strategies and identifies key structural and compositional features,addressing challenges like high overpotential,poor selectivity,and low stability.Based on these insights,we suggest avenues for future research on porous metal oxide materials for electrochemical CO_(2) reduction.
基金supported by the National Key Research and Development Program of China (2022YFB3803600)the National Natural Science Foundation of China (22302067)+2 种基金the Innovation Program of Shanghai Municipal Education Commission (2021-0107-00-02-E00106)the Science and Technology Commission of Shanghai Municipality (22230780200,20DZ2250400)Fundamental Research Funds for the Central Universities (222201717003)。
文摘Photocatalytic water oxidation is a crucial counter-electrode reaction in the process of photoelectrochemical energy conversion.Despite its importance,challenges remain in effectively and sustainably converting water to oxygen,particularly with readily available and inexpensive electrolyte solutions such as seawater.While metal oxide materials have demonstrated their advantages in promoting efficiency by reducing overpotential and improving light utilization,stability remains limited by corrosion in multicomponent seawater.In this paper,we reviewed the relationship between four basic concepts including photoelectrochemistry,metal oxide,water oxidation and seawater to better understand the challenges and opportunities in photoelectrochemical(PEC)seawater oxidation.To overcome these challenges,the advances in material design,interfacial modification,local environment control and reactor design have been further reviewed to benefit the industrial PEC seawater oxidation.Noticeably,we demonstrate engineered layered metal oxide electrodes and cell structures that enable powerful and stable seawater oxidation.We also outline and advise on the future direction in this area.
基金supported by Key Science and Technology Innovation Team of Shaanxi Province(No.2022TD-33)National Natural Science Foundation of China(Grant Nos.21373161,21504067)。
文摘Traditional selection of combustion catalysis is time-consuming and labor-intensive.Theoretical calculation is expected to resolve this problem.The adsorption energy of HMX and O atoms on 13 metal oxides was calculated using DMol3,since HMX and O are key substances in decomposition process.And the relationship between the adsorption energy of HMX,O on metal oxides(TiO_(2),Al_(2)O_(3),PbO,CuO,Fe_(2)O_(3),Co_(3)O_(4),Bi_(2)O_(3),NiO)and experimental T30 values(time required for the decomposition depth of HMX to reach 30%)was depicted as volcano plot.Thus,the T30 values of other metal oxides was predicted based on their adsorption energy on volcano plot and validated by previous experimental data.Further,the adsorption energy of HMX on ZrO_(2)and MnO_(2)was predicted based on the linear relationship between surface energy and adsorption energy,and T30 values were estimated based on volcano plot.The apparent activation energy data of HMX/MgO,HMX/SnO_(2),HMX/ZrO_(2),and HMX/MnO_(2)obtained from DSC experiments are basically consistent with our predicted T30 values,indicating that it is feasible to predict the catalytic activity based on the adsorption calculation,and it is expected that these simple structural properties can predict adsorption energy to reduce the large quantities of computation and experiment cost.
基金Financial support from the National Key Research and Development Program of China(2022YFB3805602)the National Natural Science Foundation of China(22138001,22288102)the Fundamental Research Funds for the Central Universities。
文摘Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so on.The direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol carbonate.Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.
基金supported by the Shanghai Agricultural Science and Technology Program (2022-02-08-00-12-F01176)he National Natural Science Foundation of China (52006135)
文摘Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.
基金Science and Technology Commission of Shanghai Municipality(21ZR1472900,22ZR1471600)。
文摘Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TMOs)are regarded as potential substitutes for PGMs because of their stability in oxidizing environments and excellent catalytic performance.In this study,comprehensive investigation into the influence of elastic strains on the adsorption energies of carbon(C),hydrogen(H)and oxygen(O)on TMOs was conducted.Based on density functional theory(DFT)calculations,these effects in both tetragonal structures(PtO_(2),PdO_(2))and hexagonal structures(ZnO,CdO),along with their respective transition metals were systematically explored.It was identified that the optimal adsorption sites on metal oxides pinpointed the top of oxygen or the top of metal atom,while face-centered cubic(FCC)and hexagonal close-packed(HCP)holes were preferred for the transition metals.Furthermore,under the influence of elastic strains,the results demonstrated significant disparities in the adsorption energies of H and O between oxides and transition metals.Despite these differences,the effect of elastic strains on the adsorption energies of C,H and O on TMOs mirrored those on transition metals:adsorption energies increased under compressive strains,indicating weaker adsorption,and decreased under tension strains,indicating stronger adsorption.This behavior was rationalized based on the d-band model for adsorption atop a metallic atom or the p-band model for adsorption atop an oxygen atom.Consequently,elastic strains present a promising avenue for tailoring the catalytic properties of TMOs.
基金UK Engineering and Physical Sciences Research Council(EPSRC)New Investigator Award(2018,EP/R043272/1)Newton Advanced Fellowship(192097)for financial support+3 种基金the Royal Society,the Engineering and Physical Sciences Research Council(EPSRC,EP/R023980/1,EP/V027131/1)the European Research Council(ERC)under the European Union's Horizon 2020 research and innovation program(HYPERION,Grant Agreement Number 756962)the Royal Society and Tata Group(UF150033)EPSRC SPECIFIC IKC(EP/N020863/1)
文摘Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocols,high-temperature heating process,incompatible solvents,etc.),it is still challenging to achieve efficient and reliable all-metal-oxide-based devices.Here,we developed efficient inverted PSCs(IPSCs)based on solution-processed nickel oxide(NiO_(x))and tin oxide(SnO_(2))nanoparticles,working as hole and electron transport materials respectively,enabling a fast and balanced charge transfer for photogenerated charge carriers.Through further understanding and optimizing the perovskite/metal oxide interfaces,we have realized an outstanding power conversion efficiency(PCE)of 23.5%(the bandgap of the perovskite is 1.62 eV),which is the highest efficiency among IPSCs based on all-metal-oxide charge transport materials.Thanks to these stable metal oxides and improved interface properties,ambient stability(retaining 95%of initial PCE after 1 month),thermal stability(retaining 80%of initial PCE after 2 weeks)and light stability(retaining 90%of initial PCE after 1000 hours aging)of resultant devices are enhanced significantly.In addition,owing to the low-temperature fabrication procedures of the entire device,we have obtained a PCE of over 21%for flexible IPSCs with enhanced operational stability.
文摘Metal oxide-based electrocatalysts are promising alternatives to platinum group metals for water splitting due to their low cost,abundant raw materials,and impressive stability.This review covers recent progress in various metal oxides tailored for hydrogen and oxygen evolution reactions,discussing their crystal structure,composition,and surface modification influence on performance.Strategies like surface engineering,doping,and nanostructuring are evaluated for enhancing catalytic activity and stability.The key considerations for commercialization are highlighted,emphasizing ongoing research,innovation,and future scope to drive widespread adoption of water-splitting technology for a cleaner and sustainable future.
基金supported by National Key R&D Program of China(2021YFA1502803)the National Natural Science Foundation of China(NSFC)(21972066,91745202)+3 种基金NSFC-Royal Society Joint Program(21661130149)L.P.thanks the Royal Society and Newton Fund for a Royal Society-Newton Advanced Fellowshipsupported by the Research Funds for the Frontiers Science Centre for Critical Earth Material Cycling,Nanjing Universitya Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.
基金supported by the National High Technology Research and Development Program (863 Program,2015AA034603)the National Natural Science Foundation of China (21377008,201077007,20973017)+1 种基金Foundation on the Creative Research Team Construction Promotion Project of Beijing Municipal InstitutionsScientific Research Base Construction-Science and Technology Creation Platform National Materials Research Base Construction~~
文摘Most of volatile organic compounds (VOCs) are harmful to the atmosphere and human health. Cata‐lytic combustion is an effective way to eliminate VOCs. The key issue is the availability of high per‐formance catalysts. Many catalysts including transition metal oxides, mixed metal oxides, and sup‐ported noble metals have been developed. Among these catalysts, the porous ones attract much attention. In this review, we focus on recent advances in the synthesis of ordered mesoporous and macroporous transition metal oxides, perovskites, and supported noble metal catalysts and their catalytic oxidation of VOCs. The porous catalysts outperformed their bulk counterparts. This excel‐lent catalytic performance was due to their high surface areas, high concentration of adsorbed oxy‐gen species, low temperature reducibility, strong interaction between noble metal and support and highly dispersed noble metal nanoparticles and unique porous structures. Catalytic oxidation of carbon monoxide over typical catalysts was also discussed. We made conclusive remarks and pro‐posed future work for the removal of VOCs.
基金This work was financially supported by the Science and Technology project of Jiangsu province(BN2015021,XZ-SZ201819).
文摘As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.
基金the financial support of the Department of Science and Engineering Research Board (SERB) (Sanction Order No. CRG/2019/000112)。
文摘Room-temperature gas sensors have aroused great attention in current gas sensor technology because of deemed demand of cheap,low power consumption and portable sensors for rapidly growing Internet of things applications.As an important approach,light illumination has been exploited for room-temperature operation with improving gas sensor's attributes including sensitivity,speed and selectivity.This review provides an overview of the utilization of photoactivated nanomaterials in gas sensing field.First,recent advances in gas sensing of some exciting different nanostructures and hybrids of metal oxide semiconductors under light illumination are highlighted.Later,excellent gas sensing performance of emerging two-dimensional materialsbased sensors under light illumination is discussed in details with proposed gas sensing mechanism.Originated impressive features from the interaction of photons with sensing materials are elucidated in the context of modulating sensing characteristics.Finally,the review concludes with key and constructive insights into current and future perspectives in the light-activated nanomaterials for optoelectronic gas sensor applications.
文摘This short review paper aims at assembling the present state of the art of the multiuses of metal oxides in heterogeneous catalysis, concerning liquid and gaseous phases of the reactant mixtures on solid catalysts. It includes the description of the main types of metal oxide catalysts, of their various preparation procedures and of the main reactions catalysed by them (acid-base type, selective and total oxidations, bi-functional catalysis, photocatalysis, biomass treatments, environmental catalysis and some of the numerous industrial applications). Challenges and prospectives are also discussed.
基金financially supported by the National Natural Science Foundation (No.52072347, 51972288, 51672258 and 51572246)the Fundamental Research Funds for the Central Universities (No. 2652019144 and 2652018287)+1 种基金the financial supports from the Science and Technology Program of Guangdong Province (2019A050510012)Shenzhen Science, Technology and Innovation Commission (SGDX2019081623240364).
文摘g-C_(3)N_(4) emerges as a star 2D photocatalyst due to its unique layered structure,suitable band structure and low cost.However,its photocatalytic application is limited by the fast charge recombination and low photoabsorption.Rationally designing g-C_(3)N_(4)-based heterojunction is promising for improving photocatalytic activity.Besides,g-C_(3)N_(4) exhibits great potentials in electrochemical energy storage.In view of the excellent performance of typical transition metal oxides(TMOs)in photocatalysis and energy storage,this review summarized the advances of TMOs/g-C_(3)N_(4) heterojunctions in the above two areas.Firstly,we introduce several typical TMOs based on their crystal structures and band structures.Then,we summarize different kinds of TMOs/g-C_(3)N_(4) heterojunctions,including type Ⅰ/Ⅱ heterojunction,Z-scheme,p-n junction and Schottky junction,with diverse photocatalytic applications(pollutant degradation,water splitting,CO_(2) reduction and N_(2) fixation)and supercapacitive energy storage.Finally,some promising strategies for improving the performance of TMOs/g-C_(3)N_(4) were proposed.Particularly,the exploration of photocatalysis-assisted supercapacitors was discussed.
基金supported by the National Key R&D Program of China(2017YFC0211503,2016YFC0207100)the Strategic Priority Research Program(A)of the Chinese Academy of Sciences(XDA23030300)+2 种基金the National Natural Science Foundation of China(21401200,51672273)the Open Research Fund of State Key Laboratory of Multi-phase Complex Systems(MPCS-2017-D-06)the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment,CAS(CERAE201805)~~
文摘Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds(VOCs)purification.Mixed metal oxides(MMOs),after topological transformation using layered double hydroxides(LDHs)as precursors,are extensively used as catalysts for VOCs oxidation due to their uniformity advantage.This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years.Particularly,it addresses the VOCs abatement performance over MMO,noble metal/MMO,core-shell structured MMO,and integral MMO film catalysts originating from LDHs.Moreover,it highlights the water vapor effect and oxidation mechanism.This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.
基金This work is supported by This work was supported by the National Key R&D Program of China(Nos.2020YFB2008604 and 2021YFB3202500)the National Natural Science Foundation of China(Nos.61874034 and 51861135105)+1 种基金the International Science and Technology Cooperation Program of Shanghai Science and Technology Innovation Action Plan(No.21520713300)Fudan University-CIOMP Joint Fund(E02632Y7H0).
文摘With the rapid development of the Internet of Things,there is a great demand for portable gas sensors.Metal oxide semiconductors(MOS)are one of the most traditional and well-studied gas sensing materials and have been widely used to prepare various commercial gas sensors.However,it is limited by high operating temperature.The current research works are directed towards fabricating high-performance flexible room-temperature(FRT)gas sensors,which are effective in simplifying the structure of MOS-based sensors,reducing power consumption,and expanding the application of portable devices.This article presents the recent research progress of MOS-based FRT gas sensors in terms of sensing mechanism,performance,flexibility characteristics,and applications.This review comprehensively summarizes and discusses five types of MOS-based FRT gas sensors,including pristine MOS,noble metal nanoparticles modified MOS,organic polymers modified MOS,carbon-based materials(carbon nanotubes and graphene derivatives)modified MOS,and two-dimensional transition metal dichalcogenides materials modified MOS.The effect of light-illuminated to improve gas sensing performance is further discussed.Furthermore,the applications and future perspectives of FRT gas sensors are also discussed.
基金the National Natural Science Foundation of China(Nos.50802010,50972021,21076028,and 61078061)the Program for Liaoning Excellent Talents in Universities(No.LJQ2011047)
文摘Metal oxide (TiO2 or Co304) doped activated carbon nanofibers (ACNFs) were prepared by electrospinning. These nanofibers were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and Brunner- Emmett-Teller method (BET). The results show that the average diameters of ACNFs were within the range of 200-500 nm, and the lengths were several tens of micrometers. The specific surface areas were 1146.7 m2/g for TiO2-doped ACNFs and 1238.5 m2/g for Co304-doped ACNFs, respectively. The electrospun nanofibers were used for adsorption of low concentration sulfur dioxide (SO2). The results showed that the adsorption rates of these ACNFs increased with an increase in SO2concentration. When the SO2 concentration was 1.0 μg/mL, the adsorption rates of TiO2-doped ACNFs and Co3Oa-doped ACNFs were 66.2% and 67.1%, respectively. The adsorption rate also increased as the adsorption time increased. When the adsorption time was 40 min, the adsorption rates were 67.6% and 69.0% for TiO2-doped ACNFs and Co304-doped ACNFs, respectively. The adsorption rate decreased as the adsorption temperature increased below 60℃, while it increased as the adsorption temperature increased to more than 60℃.
基金supported by the Knowledge Innova-tion Program of the Chinese Academy of Sciences(No.KZCX2-YW-420)the National Natural Science Foun-dation of China(No.20621703).
文摘Decomposition of hexachlorobenzene(HCB)was investigated over several metal oxides(i.e.,MgO,CaO,BaO,La2O3,CeO2,MnO2, Fe2O3,and Co3O4)supported on Al2O3,which was achieved in closed system at a temperature of 300°C.Catalysts were prepared by incipient wetness impregnation with different metal oxides loading and impregnating solvents.The decomposition effciency of different catalysts for this reaction depends on the nature of the metal oxide used,and Al2O3 supported La2O3 was found to be the most active one.Pe...
文摘Difference of montmorillonite (Mt), illite (It) and kaolinite (Kt) in lead sorption characteristics and the effects of amorphous Fe and Al oxide coatings on the characteristics were experimentally studied with logistic model. The sorption curves had sigmoid feature due to use of acetate-type buffer solution. With the model the sorption process could be divided into four stages and the sorption characteristics at the stages were discussed. The results showed that, after Mt, It and Kt were coated by amorphous Fe oxide, their maximum sorption capacity (MSC) and percentage of high-SSC concentration scope (HCS) of Pb2+ increased markedly, but the specific sorption capacity (SSC) decreased. With regard to effects of amorphous Al oxide coating, except for It+AI, the SSC of other samples showed a downtrend, despite that their MSC remained unchanged. Eventually, the gray correlation degrees to Pb2+ sorption for different physicochemical characteristics of the clay minerals were indicated to be higher for hydronium, zero point of surface charge and hydroxy, but lower for specific surface area, density of surface charge and amount of surface charges.