The reduction of global carbon emissions and the achievement of carbon neutrality have become the focus of addressing climate change and global warming.Electrochemical CO_(2) reduction(CO_(2)RR),as a technology that c...The reduction of global carbon emissions and the achievement of carbon neutrality have become the focus of addressing climate change and global warming.Electrochemical CO_(2) reduction(CO_(2)RR),as a technology that can efficiently convert CO_(2) into value-added products,is receiving widespread attention.This article reviews the current research status of Cu/metal oxide heterostructures in the field of electrochemical reduction of CO_(2).The review first introduces the importance of electrochemical reduction of CO_(2) and the application potential of Cu/metal oxide heterostructures in this field.Subsequently,a comprehensive discussion is presented on the exploration of various Cu/metal oxide heterostructures and their corresponding structure-performance relationship,with particular emphasis on the catalysts'activity,selectivity,stability and the nature of active sites.Lastly,the review provides an overview of the current research challenges and future development trends in this field.展开更多
Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,a...Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,and 8 wt.%)on the wettability and interfacial reaction between the alloy and shell were investigated by a sessile-drop experiment.The results show that increasing the Al_(2)O_(3) doping contents(0−8 wt.%)reduces the porosity(21.74%−10.08%)and roughness(3.22−1.34μm)of the shell surface.The increase in Cr_(2)O_(3) dopant content(2−8 wt.%)further exacerbates the interfacial reaction,leading to an increase in the thickness of the reaction layer(2.6−3.1μm)and a decrease in the wetting angle(93.9°−91.0°).The addition of Al_(2)O_(3) and TiO_(2) dopants leads to the formation of Al_(2)TiO_(5) composite oxides in the reaction products,which effectively inhibits the interfacial reaction.The increase in TiO_(2) dopant contents(0−8 wt.%)further promotes the formation of Al_(2)TiO_(5),which decreases the thickness of the interfacial reaction layer(3.9−1.2μm)and increases the wetting angle(95.0°−103.8°).The introduced dopants enhance the packing density of the shell surface,while simultaneously suppress the diffusion of active metal elements from the alloy matrix to the interface.展开更多
Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances ar...Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.展开更多
Two-dimensional(2D)metal oxides(2DMOs),such as MoO_(2),have made impressive strides in recent years,and their applicability in a number of fields such as electronic devices,optoelectronic devices and lasers has been d...Two-dimensional(2D)metal oxides(2DMOs),such as MoO_(2),have made impressive strides in recent years,and their applicability in a number of fields such as electronic devices,optoelectronic devices and lasers has been demonstrated.However,2DMOs present challenges in their synthesis using conventional methods due to their non-van der Waals nature.We report that KCl acts as a flux to prepare large-area 2DMOs with sub-millimeter scale.We systematically investigate the effects of temperature,homogeneous time and cooling rate on the products in the flux method,demonstrating that in this reaction a saturated homogenous solution is obtained upon the melting of the salt and precursor.Afterward,the cooling rate was adjusted to regulate the thickness of the target crystals,leading to the precipitation of 2D non-layered material from the supersaturated solution;by applying this method,the highly crystalline non-layered 2D MoO_(2)flakes with so far the largest lateral size of up to sub-millimeter scale(~464μm)were yielded.Electrical studies have revealed that the 2D MoO_(2)features metallic properties,with an excellent sheet resistance as low as 99Ω·square^(-1 )at room temperature,and exhibits a property of charge density wave in the measurement of resistivity as a function of temperature.展开更多
Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as lumi...Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as luminescent materials,magnetic materials,catalytic materials,electronic devices,they have an important strategic position.In the field of electrocatalysis,rare earth metal elements have great potential for development due to their unique 4f electron layer structure,spin orbit coupling,high reactivity,controllable coordination number,and rich optical properties.However,there is currently a lack of systematic reviews on the modification strategies of rare earth metal elements and the latest developments in electrocatalysis.Therefore,in order to stimulate the enthusiasm of researchers,this review focuses on the application progress of rare earth metal element modified metal oxides in multiple fields such as wastewater treatment,hydrogen peroxide synthesis,hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and machine learning assisted research.In depth analysis of its electrocatalytic mechanism in various application scenarios and key factors affecting electrocatalytic performance.This review is of great significance for further developing high-performance and multifunctional electrocatalysts,and is expected to provide strong support for the development of energy,environment,and chemical industries.展开更多
The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment,so treating diesel engine exhaust is critical.At present,the most effective method for eliminating so...The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment,so treating diesel engine exhaust is critical.At present,the most effective method for eliminating soot particles is post-treatment technology.Preparation of economically viable and highly active soot combustion catalysts is a pivotal element of post-treatment technology.In this study,different single-metal oxide catalysts with fibrous structures and alkali metal-modified hollow nanotubular Mn-based oxide catalysts were synthesized using centrifugal spinning method.Activity evaluation results showed that the manganese oxide catalyst has the best catalytic activity among the prepared single-metal oxide catalysts.Further research on alkali metal modification showed that doping alkali metals is beneficial for improving the oxidation state of manganese and generating a large number of reactive oxygen species.Combined with the structural effect brought by the hollow nanotube structure,the alkali metal-modified Mn-based oxide catalysts exhibit superior catalytic performance.Among them,the Cs-modified Mn-based oxide catalyst exhibits the best catalytic performance because of its rich active oxygen species,excellent NO oxidation ability,abundant Mn^(4+)ions(M^(n4)+/Mn^(n+)=64.78%),and good redox ability.The T_(10),T_(50),T_(90),and CO_(2)selectivity of the Cs-modified Mn-based oxide catalyst were 267°C,324°C,360°C,and 97.8%,respectively.展开更多
Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and re...Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.展开更多
Nitric oxide(NO)modulates several cancer-related physiological processes and has advanced the development of green methods for cancer treatment and integrated platforms for combination or synergistic therapies.Althoug...Nitric oxide(NO)modulates several cancer-related physiological processes and has advanced the development of green methods for cancer treatment and integrated platforms for combination or synergistic therapies.Although a nanoengineering strategy has been proposed to overcome deficiencies of NO gas or small NO donor molecules,such as short half-life,lipophilicity,non-selectivity,and poor stability,it remains challenging to prepare NO nanomedicines with simple composition,multiple functions and enhanced therapeutic efficacy.Herein,we build a liquid metal nanodroplet(LMND)-based NO nanogenerator(LMND@HSG)that is stabilized by a bioreducible guanylated hyperbranched poly(amido amine)(HSG)ligand.Mechanically,the tumor microenvironment specifically triggers a cascade process of glutathione elimination,reactive oxygen species(ROS)generation,and NO release.According to actual demand,the ROS and NO concentrations could be readily controlled by tuning the LMND and HSG feed amounts.Along with the intrinsic anticancer property of LMND(ROS-mediated apoptosis and anti-angiogenesis),LMND@HSG administration could further enhance tumor growth suppression compared with LMND and HSG alone.Fromthis study,leveraging LMND for NO gas therapy provides more possibilities for the prospect of LMND-based anticancer nanomedicines.展开更多
The labels of VU1 and VU2 in Fig.1(b)of the paper[Chin.Phys.B 34046801(2025)]were not correctly placed.The correct figure is provided.This modification does not affect the result presented in the paper.
The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most s...The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].展开更多
Nanodroplets of Gallium-Based Liquid Metal(LM)have applications in stretchable electronics,electrochemical sensors,energy storage,hyperthermia,and rapid polymerization.The gallium oxide layer around LMNDs prevents agg...Nanodroplets of Gallium-Based Liquid Metal(LM)have applications in stretchable electronics,electrochemical sensors,energy storage,hyperthermia,and rapid polymerization.The gallium oxide layer around LMNDs prevents aggregation.However,LM nanodroplets(LMNDs)are neither mechanically nor chemically stable.The ultrathin oxide layer ruptures under slight pressure,hindering their use in stretchable electronics.The shell also dissolves in slightly acidic/alkaline solutions,making them unstable for energy storage and electrochemical sensing.We demonstrate the synthesis of a dry LM powder with an LM core and a reduced graphene oxide shell.Graphene oxide provides excellent mechanical and chemical stability and permits electrical conductivity.Its porous structure does not block ion exchange between the LM droplets and the environment,allowing LMNDs to be used in energy storage and electrochemical sensing.The resulting EGaIn powders benefit from higher surface and long-term stability,addressing LMND limitations.We report using GO@EGaIn nanocomposite as an anode for alkali-ion batteries in a novel Ag-EGaIn cell with impressive energy storage capacity.The combination of liquid deformability of LMNDs,higher surface area in the nano form,and the stability of GO@EGaIn dry powder expands the applications of liquid metals in electronics and energy storage.展开更多
Kagome materials are known for hosting exotic quantum states,including quantum spin liquids,charge density waves,and unconventional superconductivity.The search for kagome monolayers is driven by their ability to exhi...Kagome materials are known for hosting exotic quantum states,including quantum spin liquids,charge density waves,and unconventional superconductivity.The search for kagome monolayers is driven by their ability to exhibit neat and well-defined kagome bands near the Fermi level,which are more easily realized in the absence of interlayer interactions.However,this absence also destabilizes the monolayer forms of many bulk kagome materials,posing significant challenges to their discovery.In this work,we propose a strategy to address this challenge by utilizing oxygen vacancies in transition metal oxides within a“1+3”design framework.Through high-throughput computational screening of 349 candidate materials,we identified 12 thermodynamically stable kagome monolayers with diverse electronic and magnetic properties.These materials were classified into three categories based on their lattice geometry,symmetry,band gaps,and magnetic configurations.Detailed analysis of three representative monolayers revealed kagome band features near their Fermi levels,with orbital contributions varying between oxygen 2p and transition metal d states.This study demonstrates the feasibility of the“1+3”strategy,offering a promising approach to uncovering low-dimensional kagome materials and advancing the exploration of their quantum phenomena.展开更多
The vibrational resolved spectra of MO_(2)^(-)/MO_(2)(M=Ti,Zr,and Hf)are reported by using photoelectron imaging and theoretical calculations.The results indicate that all the ground states of anionic and neutral MO_(...The vibrational resolved spectra of MO_(2)^(-)/MO_(2)(M=Ti,Zr,and Hf)are reported by using photoelectron imaging and theoretical calculations.The results indicate that all the ground states of anionic and neutral MO_(2)(M=Ti,Zr,and Hf)compounds are formed in bent insertion structures.The observed ground-state adiabatic detachment energy(ADE)is measured to be 1.597±0.003,1.651±0.003,and 2.119±0.003 eV for TiO_(2)^(-),ZrO_(2)^(-),and HfO_(2)^(-),respectively.The vibrational frequencies of the anionic and neutral MO_(2)are also determined from the experimental spectra.The results of theoretical calculations show that the electronic configurations of MO_(2)^(-)are^(2)A_(1)with C_(2v)point group.Bond order analysis indicates that the two M-O bonds are all multiple characters.展开更多
Metal oxide catalysts are widely employed in propane dehydrogenation(PDH)for propylene synthesis,requiring sequential reduction-reaction-regeneration cycles.However,the eff ect of water present in the inlet gas or rea...Metal oxide catalysts are widely employed in propane dehydrogenation(PDH)for propylene synthesis,requiring sequential reduction-reaction-regeneration cycles.However,the eff ect of water present in the inlet gas or reactor on the catalytic per-formance of various metal oxides remains insuffi ciently understood.This study examines the infl uence of water on supported metal oxide catalysts,specifi cally CoO x/Al_(2)O_(3),VO x/Al_(2)O_(3),and an industrial analog CrO x/Al_(2)O_(3) catalyst.By combining titration experiments,in situ Fourier transform infrared spectroscopy,kinetic analysis,and isotopic techniques,we demon-strate that even trace amounts of water can markedly suppress PDH performance via dissociative adsorption on the oxide surface.Methanol pretreatment eff ectively scavenges adsorbed water,recovering Lewis acid-base sites and consequently restoring PDH activity.This work underscores the profound inhibitory role of trace water in PDH over metal oxide catalysts and illustrates the potential of methanol pretreatment as an effective strategy to mitigate this limitation.展开更多
With the advantages of mature preparation technology,structural adjustability and suitability for large-scale application,Zn powder anode is considered to be an ideal electrode for realizing low-cost,high-energy-densi...With the advantages of mature preparation technology,structural adjustability and suitability for large-scale application,Zn powder anode is considered to be an ideal electrode for realizing low-cost,high-energy-density aqueous Zn metal batteries.However,the high specific surface of Zn powders leads to severe side reactions such as hydrogen evolution and corrosion,thus limiting their widespread use Here,this work develops a novel CuO@Zn powder anode with a synergy effect of surface wrapping and compositing.Zn powders are uniformly wrapped by small CuO particles due to the strong adsorption between Zn and CuO.The wrapped CuO particles build a good conductive framework to inhibit the structural collapse of the Zn powder caused by corrosion and non-uniform deposition.Meanwhile,CuO can also be used as a seed to guide the uniform deposition of Zn ions through its strong binding energy with Zn.As a result,the Cu O@Zn anode can maintain a long cyclic life of 900 h at current density of 1 mA·cm^(-2)and capacity of 1 mAh·cm^(-2),as well as contribute to an excellent capacity retention of 92% after 800cycles for CuO@Zn||NH_(4)V_(4)O_(10)full cell.Even at high current density of 5 A·g^(-1),the full cell exhibits a specific capacity of more than 200 mAh·g^(-1)after 800 cycles,with a good capacity retention of 89%.This work provides a new idea for developing high-performance Zn powder-based anodes.展开更多
Cryogenic magnetic cooling based on the principle of the magnetocaloric effects(MCEs)of magnetic solids has been recognized as an alternative cooling technology due to its significant economic and social benefits.Desi...Cryogenic magnetic cooling based on the principle of the magnetocaloric effects(MCEs)of magnetic solids has been recognized as an alternative cooling technology due to its significant economic and social benefits.Designing novel magnetic materials with good magnetocaloric performance is a prerequisite for practical applications.In this study,three gadolinium-transition metal-based high entropy oxides(HEOs)of Gd(Fe_(1/4)Ni_(1/4)Al_(1/4)Cr_(1/4))O_(3),Gd(Fe_(1/5)Ni_(1/5)Al_(1/5)Cr_(1/5)Co_(1/5))O_(3),and Gd(Fe_(1/6)Ni_(1/6)Al_(1/6)Cr_(1/6)Co_(1/6)Mn_(1/6))O_(3)were designed and systematically characterized regarding their structural and cryogenic magnetic properties.These HEOs were confirmed to crystallize into a single-phase perovskite-type orthorhombic structure with a homogeneous microstructure,reveal a second-order magnetic transition at low temperatures,and exhibit significant cryogenic MCEs.The magnetocaloric performances of the present HEOs,identified by magnetic entropy changes,relative cooling power,and temperature-averaged entropy changes,were com-parable with recently reported candidate materials.The present study indicates potential applications for cryogenic magnetic cooling of the present HEOs and provides meaningful clues for designing and exploring HEOs with good cryogenic magnetocaloric performances.展开更多
Against the backdrop of increasingly prominent global energy shortages and environmental issues,the development of efficient energy conversion and storage technologies has become crucial.Zero-dimensional(0D)metal oxid...Against the backdrop of increasingly prominent global energy shortages and environmental issues,the development of efficient energy conversion and storage technologies has become crucial.Zero-dimensional(0D)metal oxide composites exhibit significant application value in the field of energy chemistry due to their unique properties,such as quantum size effect and high specific surface area.From a broad perspective,this paper reviews the main synthesis methods of these composites,including sol-gel method,hydrothermal/solvothermal method,precipitation method,and template method,while analyzing the characteristics of each method.It further discusses their applications in photocatalytic hydrogen production,fuel cells,lithium-ion batteries,and supercapacitors.Additionally,the current challenges,such as material dispersibility and interface bonding,are pointed out,and future development directions are prospected,aiming to provide references for related research.展开更多
Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient cat...Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.展开更多
Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,...Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,and XRD raw data were kept and can be offered.The correct Fig.2 has been provided in this Correction.展开更多
Electrochemical CO_(2) reduction reaction(CO_(2)RR),driven by renewable energy,offers a promising solution to mitigate increasing CO_(2) emissions and establish a carbon-neutral cycle.Copper is a highly selective and ...Electrochemical CO_(2) reduction reaction(CO_(2)RR),driven by renewable energy,offers a promising solution to mitigate increasing CO_(2) emissions and establish a carbon-neutral cycle.Copper is a highly selective and active catalyst for CO_(2)RR but suffers from structural reconstruction challenges.Hybrid organic/inorganic materials address these issues by offering customizable compositions and interfaces.Recently,Buonsanti’s team developed hybrid Cu@AlOx nanocrystals with tunable alumina shells via a colloidal atomic layer deposition approach,achieving stable and selective methane production during CO_(2)RR.Mechanistic studies reveal that the alumina shell stabilizes oxidized copper species through Cu^(2+)-O-Al motifs coordinated with AlO_(4) Lewis acid sites,reducing copper dissolution and structural reconstruction.This study provides key insights into the mechanism underlying stabilization,highlighting the critical role of Lewis acidity in preserving the structural integrity of the catalyst.This highlight review aims to inspire the development of other high-performance and stable catalysts through colloidal atomic layer deposition strategies.展开更多
基金supported by the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCX23_0120)the National Natural Science Foundation of China(Nos.22275088 and 52101260)+3 种基金the Project of Shuangchuang Scholar of Jiangsu Province(No.JSSCBS20210212)the Fundamental Research Funds for the Central Universities(No.30921011203)the Start-Up Grant(No.AE89991/340)from Nanjing University of Science and Technology,the Foundation of Jiangsu Educational Committee(No.22KJB310008)the Senior Talent Program of Jiangsu University(No.20JDG073).
文摘The reduction of global carbon emissions and the achievement of carbon neutrality have become the focus of addressing climate change and global warming.Electrochemical CO_(2) reduction(CO_(2)RR),as a technology that can efficiently convert CO_(2) into value-added products,is receiving widespread attention.This article reviews the current research status of Cu/metal oxide heterostructures in the field of electrochemical reduction of CO_(2).The review first introduces the importance of electrochemical reduction of CO_(2) and the application potential of Cu/metal oxide heterostructures in this field.Subsequently,a comprehensive discussion is presented on the exploration of various Cu/metal oxide heterostructures and their corresponding structure-performance relationship,with particular emphasis on the catalysts'activity,selectivity,stability and the nature of active sites.Lastly,the review provides an overview of the current research challenges and future development trends in this field.
基金supported by the National Natural Science Foundation of China (No. 52374292)China Baowu Low Carbon Metallurgy Innovation Foundation, China (No. BWLCF202309)the Natural Science Foundation of Changsha City, China (No. KQ2208271)。
文摘Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,and 8 wt.%)on the wettability and interfacial reaction between the alloy and shell were investigated by a sessile-drop experiment.The results show that increasing the Al_(2)O_(3) doping contents(0−8 wt.%)reduces the porosity(21.74%−10.08%)and roughness(3.22−1.34μm)of the shell surface.The increase in Cr_(2)O_(3) dopant content(2−8 wt.%)further exacerbates the interfacial reaction,leading to an increase in the thickness of the reaction layer(2.6−3.1μm)and a decrease in the wetting angle(93.9°−91.0°).The addition of Al_(2)O_(3) and TiO_(2) dopants leads to the formation of Al_(2)TiO_(5) composite oxides in the reaction products,which effectively inhibits the interfacial reaction.The increase in TiO_(2) dopant contents(0−8 wt.%)further promotes the formation of Al_(2)TiO_(5),which decreases the thickness of the interfacial reaction layer(3.9−1.2μm)and increases the wetting angle(95.0°−103.8°).The introduced dopants enhance the packing density of the shell surface,while simultaneously suppress the diffusion of active metal elements from the alloy matrix to the interface.
基金funding support from General Research Fund[Project No.14300525]from the Research Grants Council(RGC)of Hong Kong SAR,Chinafunding support from Natural Science Foundation of China(NSFC)Young Scientists Fund(Project No.22305203)+2 种基金NSFC Projects Nos.22309123,22422303,22303011,22033002,92261112 and U21A20328support from the Hong Kong Branch of National Precious Metals Material Engineering Research Center(NPMM)at City University of Hong Kongsupport from Young Collaborative Research Grant[Project No.C1003-23Y]support from RGC of Hong Kong SAR,China.
文摘Electrocatalytic nitric oxide(NO)reduction reaction(NORR)is a promising and sustainable process that can simultaneously realize green ammonia(NH3)synthesis and hazardous NO removal.However,current NORR performances are far from practical needs due to the lack of efficient electrocatalysts.Engineering the lattice of metal-based nanomaterials via phase control has emerged as an effective strategy to modulate their intrinsic electrocatalytic properties.Herein,we realize boron(B)-insertion-induced phase regulation of rhodium(Rh)nanocrystals to obtain amorphous Rh_(4)B nanoparticles(NPs)and hexagonal close-packed(hcp)RhB NPs through a facile wet-chemical method.A high Faradaic efficiency(92.1±1.2%)and NH_(3) yield rate(629.5±11.0μmol h^(−1) cm^(−2))are achieved over hcp RhB NPs,far superior to those of most reported NORR nanocatalysts.In situ spectro-electrochemical analysis and density functional theory simulations reveal that the excellent electrocatalytic performances of hcp RhB NPs are attributed to the upshift of d-band center,enhanced NO adsorption/activation profile,and greatly reduced energy barrier of the rate-determining step.A demonstrative Zn-NO battery is assembled using hcp RhB NPs as the cathode and delivers a peak power density of 4.33 mW cm−2,realizing simultaneous NO removal,NH3 synthesis,and electricity output.
基金supported by the National Key Research and Development Program of China(Nos.2023YFB3608703 and 2023YFB3608700)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(Nos.2021ZZ122 and 2020ZZ110)Fujian provincial projects(Nos.2021HZ0114 and 2021J01583).
文摘Two-dimensional(2D)metal oxides(2DMOs),such as MoO_(2),have made impressive strides in recent years,and their applicability in a number of fields such as electronic devices,optoelectronic devices and lasers has been demonstrated.However,2DMOs present challenges in their synthesis using conventional methods due to their non-van der Waals nature.We report that KCl acts as a flux to prepare large-area 2DMOs with sub-millimeter scale.We systematically investigate the effects of temperature,homogeneous time and cooling rate on the products in the flux method,demonstrating that in this reaction a saturated homogenous solution is obtained upon the melting of the salt and precursor.Afterward,the cooling rate was adjusted to regulate the thickness of the target crystals,leading to the precipitation of 2D non-layered material from the supersaturated solution;by applying this method,the highly crystalline non-layered 2D MoO_(2)flakes with so far the largest lateral size of up to sub-millimeter scale(~464μm)were yielded.Electrical studies have revealed that the 2D MoO_(2)features metallic properties,with an excellent sheet resistance as low as 99Ω·square^(-1 )at room temperature,and exhibits a property of charge density wave in the measurement of resistivity as a function of temperature.
基金supported by the National Key Research and Development Program of China(No.2023YFC3708005)The Fundamental Research Funds for the Central Universities,Nankai University(No.63241208)supported by the National Natural Science Foundation of China(Nos.21872102 and 22172080)。
文摘Rare earth metal elements include lanthanide elements as well as scandium and yttrium,totaling seventeen metal elements.Due to the wide application prospects of rare earth metal elements in various fields such as luminescent materials,magnetic materials,catalytic materials,electronic devices,they have an important strategic position.In the field of electrocatalysis,rare earth metal elements have great potential for development due to their unique 4f electron layer structure,spin orbit coupling,high reactivity,controllable coordination number,and rich optical properties.However,there is currently a lack of systematic reviews on the modification strategies of rare earth metal elements and the latest developments in electrocatalysis.Therefore,in order to stimulate the enthusiasm of researchers,this review focuses on the application progress of rare earth metal element modified metal oxides in multiple fields such as wastewater treatment,hydrogen peroxide synthesis,hydrogen evolution reaction(HER),carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and machine learning assisted research.In depth analysis of its electrocatalytic mechanism in various application scenarios and key factors affecting electrocatalytic performance.This review is of great significance for further developing high-performance and multifunctional electrocatalysts,and is expected to provide strong support for the development of energy,environment,and chemical industries.
基金supported by National Key R&D Program of China(2022YFB3506200,2022YFB3504100)National Natural Science Foundation of China(22072095,22372107,22202058)+3 种基金Excellent Youth Science Foundation of Liaoning Province(2022-YQ-20)Shenyang Science and Technology Planning Project(22-322-3-28)Liaoning Xingliao talented youth Top talent program(XLYC2203007)University Joint Education Project for China-Central and Eastern European Countries(2021097).
文摘The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment,so treating diesel engine exhaust is critical.At present,the most effective method for eliminating soot particles is post-treatment technology.Preparation of economically viable and highly active soot combustion catalysts is a pivotal element of post-treatment technology.In this study,different single-metal oxide catalysts with fibrous structures and alkali metal-modified hollow nanotubular Mn-based oxide catalysts were synthesized using centrifugal spinning method.Activity evaluation results showed that the manganese oxide catalyst has the best catalytic activity among the prepared single-metal oxide catalysts.Further research on alkali metal modification showed that doping alkali metals is beneficial for improving the oxidation state of manganese and generating a large number of reactive oxygen species.Combined with the structural effect brought by the hollow nanotube structure,the alkali metal-modified Mn-based oxide catalysts exhibit superior catalytic performance.Among them,the Cs-modified Mn-based oxide catalyst exhibits the best catalytic performance because of its rich active oxygen species,excellent NO oxidation ability,abundant Mn^(4+)ions(M^(n4)+/Mn^(n+)=64.78%),and good redox ability.The T_(10),T_(50),T_(90),and CO_(2)selectivity of the Cs-modified Mn-based oxide catalyst were 267°C,324°C,360°C,and 97.8%,respectively.
基金supported by National Natural Science Fundation of China(Nos.52170086,22308194,U22A20423)Natural Science Foundation of Shandong Province(No.ZR2021ME013)+1 种基金Taishan Scholars Program of Shandong Province(No.tsqn202211012)Shandong Provincial Excellent Youth(No.ZR2022YQ47)。
文摘Although the powder Fenton-like catalysts have exhibited high catalytic performances towards pollutant degradation,they cannot be directly used for Fenton-like industrialization considering the problems of loss and recovery.Therefore,the membrane fixation of catalyst is an important step to realize the actual application of Fenton-like catalysts.In this work,an efficient catalyst was developed with Co-N_(x)configuration facilely reconstructed on the surface of Co_(3)O_(4)(Co-N_(x)/Co_(3)O_(4)),which exhibited superior catalytic activity.We further fixed the highly efficient Co-N_(x)/Co_(3)O_(4)onto three kinds of organic membranes and one kind of inorganic ceramic membrane installing with the residual PMS treatment device to investigate its catalytic stability and sustainability.Results indicated that the inorganic ceramic membrane(CM)can achieve high water flux of 710 L m-2h-1,and the similar water flux can be achieved by Co-N_(x)/Co_(3)O_(4)/CM even without the pressure extraction.We also employed the Co-N_(x)/Co_(3)O_(4)/CM system to the wastewater secondary effluent,and the pollutant in complicated secondary effluent could be highly removed by the Co-N_(x)/Co_(3)O_(4)/CM system.This paper provides a new point of view for the application of metal-based catalysts with M-N_(x)coordination in catalytic reaction device.
基金the National Natural Science Foundation of China(22075114,32371434,82301630)the Natural Science Foundation of Jiangsu Province(BK20211034)the financial support from Jiangsu Provincial Medical Key Laboratory(Key Laboratory of Nuclear Medicine).
文摘Nitric oxide(NO)modulates several cancer-related physiological processes and has advanced the development of green methods for cancer treatment and integrated platforms for combination or synergistic therapies.Although a nanoengineering strategy has been proposed to overcome deficiencies of NO gas or small NO donor molecules,such as short half-life,lipophilicity,non-selectivity,and poor stability,it remains challenging to prepare NO nanomedicines with simple composition,multiple functions and enhanced therapeutic efficacy.Herein,we build a liquid metal nanodroplet(LMND)-based NO nanogenerator(LMND@HSG)that is stabilized by a bioreducible guanylated hyperbranched poly(amido amine)(HSG)ligand.Mechanically,the tumor microenvironment specifically triggers a cascade process of glutathione elimination,reactive oxygen species(ROS)generation,and NO release.According to actual demand,the ROS and NO concentrations could be readily controlled by tuning the LMND and HSG feed amounts.Along with the intrinsic anticancer property of LMND(ROS-mediated apoptosis and anti-angiogenesis),LMND@HSG administration could further enhance tumor growth suppression compared with LMND and HSG alone.Fromthis study,leveraging LMND for NO gas therapy provides more possibilities for the prospect of LMND-based anticancer nanomedicines.
文摘The labels of VU1 and VU2 in Fig.1(b)of the paper[Chin.Phys.B 34046801(2025)]were not correctly placed.The correct figure is provided.This modification does not affect the result presented in the paper.
基金financial support from the National Key R&D Program of China(2021YFB3500700)the National Natural Science Foundation of China(22473042,22003016,and 92145302).
文摘The use of metal oxides has been extensively documented in the literature and applied in a variety of contexts,including but not limited to energy storage,chemical sensors,and biomedical applications.One of the most significant applications of metal oxides is heterogeneous catalysis,which represents a pivotal technology in industrial production on a global scale.Catalysts serve as the primary enabling agents for chemical reactions,and among the plethora of catalysts,metal oxides including magnesium oxide(MgO),ceria(CeO_(2))and titania(TiO_(2)),have been identified to be particularly effective in catalyzing a variety of reactions[1].Theoretical calculations based on density functional theory(DFT)and a multitude of other quantum chemistry methods have proven invaluable in elucidating the mechanisms of metal-oxide-catalyzed reactions,thereby facilitating the design of high-performance catalysts[2].
基金supported by the European Research Council,ERC project Liquid3D,grant number 101045072Access to the TAIL-UC facility,funded under the QREN-Mais Centro project ICT_2009_02_012_1890,is gratefully acknowledged+1 种基金the Foundation for Science and Technology(FCT)for support provided through the Concurso Estímulo ao Emprego Científico Individual,6th edition(reference 2023.08684.CEECIND)Support came as well from the projects Future Packaging,“Embalagem do Futuro”,Supported by the Portuguese Recovery and Resilience Plan(PRR)and the Next Generation EU European Funds,Green Agenda for Industrial Sector project 59.
文摘Nanodroplets of Gallium-Based Liquid Metal(LM)have applications in stretchable electronics,electrochemical sensors,energy storage,hyperthermia,and rapid polymerization.The gallium oxide layer around LMNDs prevents aggregation.However,LM nanodroplets(LMNDs)are neither mechanically nor chemically stable.The ultrathin oxide layer ruptures under slight pressure,hindering their use in stretchable electronics.The shell also dissolves in slightly acidic/alkaline solutions,making them unstable for energy storage and electrochemical sensing.We demonstrate the synthesis of a dry LM powder with an LM core and a reduced graphene oxide shell.Graphene oxide provides excellent mechanical and chemical stability and permits electrical conductivity.Its porous structure does not block ion exchange between the LM droplets and the environment,allowing LMNDs to be used in energy storage and electrochemical sensing.The resulting EGaIn powders benefit from higher surface and long-term stability,addressing LMND limitations.We report using GO@EGaIn nanocomposite as an anode for alkali-ion batteries in a novel Ag-EGaIn cell with impressive energy storage capacity.The combination of liquid deformability of LMNDs,higher surface area in the nano form,and the stability of GO@EGaIn dry powder expands the applications of liquid metals in electronics and energy storage.
基金financial support from the National Key Research&Development Program of China(Grant No.2023YFA1406500)the National Natural Science Foundation of China(Grant Nos.12104504,52461160327 and 92477205)the Fundamental Research Funds for the Central Universities,and the Research Funds of Renmin University of China[Grant Nos.22XNKJ30(W.J.)and 24XNKJ17(C.W.)]。
文摘Kagome materials are known for hosting exotic quantum states,including quantum spin liquids,charge density waves,and unconventional superconductivity.The search for kagome monolayers is driven by their ability to exhibit neat and well-defined kagome bands near the Fermi level,which are more easily realized in the absence of interlayer interactions.However,this absence also destabilizes the monolayer forms of many bulk kagome materials,posing significant challenges to their discovery.In this work,we propose a strategy to address this challenge by utilizing oxygen vacancies in transition metal oxides within a“1+3”design framework.Through high-throughput computational screening of 349 candidate materials,we identified 12 thermodynamically stable kagome monolayers with diverse electronic and magnetic properties.These materials were classified into three categories based on their lattice geometry,symmetry,band gaps,and magnetic configurations.Detailed analysis of three representative monolayers revealed kagome band features near their Fermi levels,with orbital contributions varying between oxygen 2p and transition metal d states.This study demonstrates the feasibility of the“1+3”strategy,offering a promising approach to uncovering low-dimensional kagome materials and advancing the exploration of their quantum phenomena.
基金supported by the National Natural Science Foundation of China(No.22273065)Shandong Energy institute(SEI U202312)"Strategic Priority Research Program"of the Chinese Academy of Sciences(No.XDA02020000).
文摘The vibrational resolved spectra of MO_(2)^(-)/MO_(2)(M=Ti,Zr,and Hf)are reported by using photoelectron imaging and theoretical calculations.The results indicate that all the ground states of anionic and neutral MO_(2)(M=Ti,Zr,and Hf)compounds are formed in bent insertion structures.The observed ground-state adiabatic detachment energy(ADE)is measured to be 1.597±0.003,1.651±0.003,and 2.119±0.003 eV for TiO_(2)^(-),ZrO_(2)^(-),and HfO_(2)^(-),respectively.The vibrational frequencies of the anionic and neutral MO_(2)are also determined from the experimental spectra.The results of theoretical calculations show that the electronic configurations of MO_(2)^(-)are^(2)A_(1)with C_(2v)point group.Bond order analysis indicates that the two M-O bonds are all multiple characters.
基金supported by the National Key R&D Program of China(No.2023YFA1507800)the National Science Foundation of China(Nos.22121004,22122808,22478279,and 22108201)+1 种基金the Haihe Laboratory of Sustainable Chemical Trans-formations,the Program of Introducing Talents of Discipline to Uni-versities(No.BP0618007)the XPLORER PRIZE.
文摘Metal oxide catalysts are widely employed in propane dehydrogenation(PDH)for propylene synthesis,requiring sequential reduction-reaction-regeneration cycles.However,the eff ect of water present in the inlet gas or reactor on the catalytic per-formance of various metal oxides remains insuffi ciently understood.This study examines the infl uence of water on supported metal oxide catalysts,specifi cally CoO x/Al_(2)O_(3),VO x/Al_(2)O_(3),and an industrial analog CrO x/Al_(2)O_(3) catalyst.By combining titration experiments,in situ Fourier transform infrared spectroscopy,kinetic analysis,and isotopic techniques,we demon-strate that even trace amounts of water can markedly suppress PDH performance via dissociative adsorption on the oxide surface.Methanol pretreatment eff ectively scavenges adsorbed water,recovering Lewis acid-base sites and consequently restoring PDH activity.This work underscores the profound inhibitory role of trace water in PDH over metal oxide catalysts and illustrates the potential of methanol pretreatment as an effective strategy to mitigate this limitation.
基金financially supported by the National Natural Science Foundation of China(No.52072411)the Central South University Innovation-Driven Research Programme(No.2023CXQD038)。
文摘With the advantages of mature preparation technology,structural adjustability and suitability for large-scale application,Zn powder anode is considered to be an ideal electrode for realizing low-cost,high-energy-density aqueous Zn metal batteries.However,the high specific surface of Zn powders leads to severe side reactions such as hydrogen evolution and corrosion,thus limiting their widespread use Here,this work develops a novel CuO@Zn powder anode with a synergy effect of surface wrapping and compositing.Zn powders are uniformly wrapped by small CuO particles due to the strong adsorption between Zn and CuO.The wrapped CuO particles build a good conductive framework to inhibit the structural collapse of the Zn powder caused by corrosion and non-uniform deposition.Meanwhile,CuO can also be used as a seed to guide the uniform deposition of Zn ions through its strong binding energy with Zn.As a result,the Cu O@Zn anode can maintain a long cyclic life of 900 h at current density of 1 mA·cm^(-2)and capacity of 1 mAh·cm^(-2),as well as contribute to an excellent capacity retention of 92% after 800cycles for CuO@Zn||NH_(4)V_(4)O_(10)full cell.Even at high current density of 5 A·g^(-1),the full cell exhibits a specific capacity of more than 200 mAh·g^(-1)after 800 cycles,with a good capacity retention of 89%.This work provides a new idea for developing high-performance Zn powder-based anodes.
基金supported by the National Natural Science Foundation of China(No.52171174).The authors acknowledge Dr.Chao Zhang from the Instrumentation Service Center for Physical Sciences at Westlake University for magnetization measurements.
文摘Cryogenic magnetic cooling based on the principle of the magnetocaloric effects(MCEs)of magnetic solids has been recognized as an alternative cooling technology due to its significant economic and social benefits.Designing novel magnetic materials with good magnetocaloric performance is a prerequisite for practical applications.In this study,three gadolinium-transition metal-based high entropy oxides(HEOs)of Gd(Fe_(1/4)Ni_(1/4)Al_(1/4)Cr_(1/4))O_(3),Gd(Fe_(1/5)Ni_(1/5)Al_(1/5)Cr_(1/5)Co_(1/5))O_(3),and Gd(Fe_(1/6)Ni_(1/6)Al_(1/6)Cr_(1/6)Co_(1/6)Mn_(1/6))O_(3)were designed and systematically characterized regarding their structural and cryogenic magnetic properties.These HEOs were confirmed to crystallize into a single-phase perovskite-type orthorhombic structure with a homogeneous microstructure,reveal a second-order magnetic transition at low temperatures,and exhibit significant cryogenic MCEs.The magnetocaloric performances of the present HEOs,identified by magnetic entropy changes,relative cooling power,and temperature-averaged entropy changes,were com-parable with recently reported candidate materials.The present study indicates potential applications for cryogenic magnetic cooling of the present HEOs and provides meaningful clues for designing and exploring HEOs with good cryogenic magnetocaloric performances.
文摘Against the backdrop of increasingly prominent global energy shortages and environmental issues,the development of efficient energy conversion and storage technologies has become crucial.Zero-dimensional(0D)metal oxide composites exhibit significant application value in the field of energy chemistry due to their unique properties,such as quantum size effect and high specific surface area.From a broad perspective,this paper reviews the main synthesis methods of these composites,including sol-gel method,hydrothermal/solvothermal method,precipitation method,and template method,while analyzing the characteristics of each method.It further discusses their applications in photocatalytic hydrogen production,fuel cells,lithium-ion batteries,and supercapacitors.Additionally,the current challenges,such as material dispersibility and interface bonding,are pointed out,and future development directions are prospected,aiming to provide references for related research.
基金National Natural Science Foundation of China,Grant/Award Number:22179029Fundamental Research Funds for the Central Universities,Grant/Award Number:buctrc202324+2 种基金Young Elite Scientists Sponsorship Program by BAST,Grant/Award Number:BYESS2023093Ministero dell'Istruzione,dell'Universitàe della Ricerca,Grant/Award Number:2022FNL89YKempestiftelserna。
文摘Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.
文摘Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,and XRD raw data were kept and can be offered.The correct Fig.2 has been provided in this Correction.
基金supported by the National Natural Science Foundation of China(No.22101289)Hundred Talents Programs in Chinese Academy of Science,and the Ningbo S&T Innovation 2025 Major Special Program(No.2022Z205).
文摘Electrochemical CO_(2) reduction reaction(CO_(2)RR),driven by renewable energy,offers a promising solution to mitigate increasing CO_(2) emissions and establish a carbon-neutral cycle.Copper is a highly selective and active catalyst for CO_(2)RR but suffers from structural reconstruction challenges.Hybrid organic/inorganic materials address these issues by offering customizable compositions and interfaces.Recently,Buonsanti’s team developed hybrid Cu@AlOx nanocrystals with tunable alumina shells via a colloidal atomic layer deposition approach,achieving stable and selective methane production during CO_(2)RR.Mechanistic studies reveal that the alumina shell stabilizes oxidized copper species through Cu^(2+)-O-Al motifs coordinated with AlO_(4) Lewis acid sites,reducing copper dissolution and structural reconstruction.This study provides key insights into the mechanism underlying stabilization,highlighting the critical role of Lewis acidity in preserving the structural integrity of the catalyst.This highlight review aims to inspire the development of other high-performance and stable catalysts through colloidal atomic layer deposition strategies.
