High-entropy alloy(HEA)nanoparticles(NPs)have attracted great attention in electrocatalysis due to their tailorable complex compositions and unique properties.Herein,we introduce Fe,Co,Ni,Cr and Mn into the metal-poly...High-entropy alloy(HEA)nanoparticles(NPs)have attracted great attention in electrocatalysis due to their tailorable complex compositions and unique properties.Herein,we introduce Fe,Co,Ni,Cr and Mn into the metal-polyphenol coordination system to prepare HEA NPs enclosed in N-doped carbon(FeCoNiCrMn)with great potential for catalyzing oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).The unique high-entropy structural characteristics in FeCoNiCrMn facilitate effective interplay between metal species,leading to improved ORR(E_(1/2)=0.89 V)and OER(η=330 mV,j=10 mA·cm^(−2))activity.Additionally,FeCoNiCrMn exhibits excellent open-circuit voltage(1.523 V),power density(110 mW·cm^(−2))and long-term durability,outperforming Pt/C+IrO_(2) electrodes as a cathode catalyst in Zn-air batteries(ZABs).Such polyphenol-assisted alloying method broadens and simplifies the development of HEA electrocatalysts for high-performance ZABs.展开更多
Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and...Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and environmental processes due to their strong oxidative power[1].Generating ROS in a controlled manner under mild conditions is essential for achieving selective oxidation reactions.Light-driven methods are especially appealing for this purpose,as they offer precise control over where and when ROS are produced.展开更多
The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically appl...The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically applied.The traditional lattice oxygen oxidation mechanism(LOM)offers an advantageous route by circumventing the formation of M-OOH^(*)in the adsorption evolution mechanism(AEM),thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order.Fortunately,the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen,which could be activated by rational band structure design for direct O-O coupling,where the M–O bond maintains its initial bond order.Here,non-bonding oxygen was introduced into NiFe_(2)O_(4)via annealing in an oxygen-deficient atmosphere.Then,in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons,thereby facilitating the transformation of the redox center from metal to oxygen.LOM based on non-bonding oxygen(LOMNB)was successfully activated within NiFe_(2)O_(4),exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^(-2)and excellent durability of stable operation for over 150 h.Additionally,catalysts featuring varying band structures were synthesized for comparative analysis,and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2p holes are critical prerequisites for triggering and sustaining the LOMNB pathway in transition metal spinel oxides.These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.展开更多
This article comments on the research by Zhang et al on the role of advanced heart failure and transplant teams in extracorporeal membrane oxygenation(ECMO)management.The study by Zhang et al indicates that direct adv...This article comments on the research by Zhang et al on the role of advanced heart failure and transplant teams in extracorporeal membrane oxygenation(ECMO)management.The study by Zhang et al indicates that direct advanced heart failure and transplant involvement improves survival in ECMO patients,especially those on veno-arterial ECMO.However,the optimal approach varies due to multiple factors.This article discusses the clinical implications,research design limitations,and future directions to enhance ECMO care.展开更多
Oxygen evolution reaction(OER)is often regarded as a crucial bottleneck in the field of renewable energy storage and conversion.To further accelerate the sluggish kinetics of OER,a cation and anion modulation strategy...Oxygen evolution reaction(OER)is often regarded as a crucial bottleneck in the field of renewable energy storage and conversion.To further accelerate the sluggish kinetics of OER,a cation and anion modulation strategy is reported here,which has been proven to be effective in preparing highly active electrocatalyst.For example,the cobalt,sulfur,and phosphorus modulated nickel hydroxide(denoted as NiCoPSOH)only needs an overpotential of 232 mV to reach a current density of 20 mA cm^(–2),demonstrating excellent OER performances.The cation and anion modulation facilitates the generation of high-valent Ni species,which would activate the lattice oxygen and switch the OER reaction pathway from conventional adsorbate evolution mechanism to lattice oxygen mechanism(LOM),as evidenced by the results of electrochemical measurements,Raman spectroscopy and differential electrochemical mass spectrometry.The LOM pathway of NiCoPSOH is further verified by the theoretical calculations,including the upshift of O 2p band center,the weakened Ni–O bond and the lowest energy barrier of rate-limiting step.Thus,the anion and cation modulated catalyst NiCoPSOH could effectively accelerate the sluggish OER kinetics.Our work provides a new insight into the cation and anion modulation,and broadens the possibility for the rational design of highly active electrocatalysts.展开更多
Singlet oxygen(^(1)O_(2)),as an electrophilic oxidant,is essential for the selective water decontamination of pollutants from water.Herein,we showcase a high-performing electrocatalytic filtration system composed of c...Singlet oxygen(^(1)O_(2)),as an electrophilic oxidant,is essential for the selective water decontamination of pollutants from water.Herein,we showcase a high-performing electrocatalytic filtration system composed of carbon nanotubes functionalized with CoFe alloy nanoparticles(CoFeCNT)to selectively facilitate the electrochemical activation of O_(2)to^(1)O_(2).Benefiting from the prominently featured bimetal active sites of CoFeCNT,nearly complete production of^(1)O_(2)is achieved by the electrocatalytic activation of O_(2).Additionally,the proposed system exhibits a consistent pollutant removal efficiency>90%in a flow-through reactor over 48 h of continuous operation without a noticeable decline in performance,highlighting the dependable stability of the system for practical applications.The flow-through configuration demonstrates a striking 8-fold enhancement in tetracycline oxidation compared to a conventional batch reactor.This work provides a molecular level understanding of the oxygen reduction reaction,showing promising potential for the selective removal of emerging organic contaminants from water.展开更多
The development of highly efficient non-precious metal-nitrogen-carbon(M-N-C)electrocatalysts is a key scientific issue for improving the performance of metal-air batteries and fuel cells.Due to the symmetric charge d...The development of highly efficient non-precious metal-nitrogen-carbon(M-N-C)electrocatalysts is a key scientific issue for improving the performance of metal-air batteries and fuel cells.Due to the symmetric charge distribution of the traditional M-N_(4)active site,the adsorption energy of the key oxygen intermediates in the process of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is difficult to reach the optimal value,which seriously limits the catalytic efficiency.The core of solving this problem lies in the accurate modulation of the coordination environment of the M-N_(4)site,which can realize the breakthrough improvement of the catalytic performance by synergistically optimizing the geometric configuration and electronic structure.In this paper,we systematically analyze the ORR/OER reaction mechanism and then comprehensively review the four main strategies to optimize the coordination environment of M-N-C:metal site regulation,coordination number engineering,non-metal atom doping,and carbon support regulation.Through an in-depth analysis of the structure-activity relationship between the coordination configuration and catalytic performance,the core challenges faced by current research are pointed out,and future research directions are envisioned.This work aims to provide theoretical references for the directional construction of highly efficient M-N-C catalysts with optimized coordination environments.展开更多
The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed tw...The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed two co-corresponding authors(Hongxiang Zhang and Honggen Peng).But the corresponding author of Honggen Peng was omitted in the final published manuscript.So,we apply to designate Honggen Peng(penghonggen@ncu.edu.cn)as the second co-corresponding author and the corresponding unit is“a,b">.展开更多
Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaus...Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaust temperatures below 200℃,particularly under conditions of frequent idling.Herein,we report an effective strategy utilizing non-thermal plasma(NTP)to activate Olatt in Ce_(1–x)Co_(x)O_(2–δ)catalysts,achieving dramatic enhancement of the soot combustion rate at low temperatures.At 200℃ and 4.3 W(discharge power,P_(dis)),NTP-Ce_(0.8)Co_(0.2)O_(2–δ)achieved 96.9%soot conversion(X_(C)),99.0%CO_(2) selectivity(S(CO_(2)))and a maximum energy conversion efficiency(Emax)of 14.7 g kWh^(–1).Compared with previously reported results,NTP-Ce_(0.8)Co_(0.2)O_(2–δ)exhibits the highest S(CO_(2))and Emax values.Remarkably,even without heating,X_(C),Emax,and S(CO_(2))reached 92.1%,6.1 g kWh–1,and 97.5%,respectively,at 6.3 W(P_(dis)).The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO_(2) crystal lattice and forms an asymmetric Ce–O–Co structure,making oxygen“easy come,easy go”,thereby enabling the rapid combustion of soot over NTP-Ce_(0.8)Co_(0.2)O_(2–δ).This study highlights the great potential of NTP for activating Olatt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.展开更多
Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong...Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong acid in PEMWE systems pose a major challenge to the stability of electrocatalysts,and the development of efficient and corrosion-resistant catalysts is urgently needed.Currently,iridium(Ir)-based catalysts have gained great attention due to their promising activity and stability,while the extremely low reserves of Ir in the earth seriously hinder the commercialization of PEMWE.Therefore,a systematic understanding of the latest advances in Ir-based catalysts is necessary to guide their rational design to meet the industrial requirements.In this review,the general reaction mechanisms and advanced characterization techniques for mechanism recognition are first introduced.Afterwards,the systematic design strategies and performances of Ir-based catalysts,including metallic Ir,Ir oxides,and Ir-based perovskites,are summarized in detail.Finally,the conclusions,challenges,and prospects for Ir-based electrocatalysts are presented.展开更多
Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunc...Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunctional electrocatalysts and limited understanding of the structure-activity relationships.Pyrrole-type single-atom catalysts(SACs)with unique electronic structures have emerged as promising electrocatalysts.In this work,we combine density functional theory(DFT)calculations and experimental studies to systematically explore the structure-activity relationships and potential of pyrrole-type transition metal-N_(3)(TM-po-N_(3))as bifunctional catalysts.DFT calculations reveal that differences in the dependence of ORR and OER activities on the free energy of adsorption of reaction intermediates significantly affect the TM-po-N_(3)bifunctional activity and identify magnetic Cu-po-N_(3)as the best candidate.The bifunctional activity of Cu-po-N_(3)originates from interactions between spin-polarized out-of-plane Cu_3d and O_2s+2p orbitals.Theoretical predictions are validated experimentally,showing that the synthesized Cu-SAC/NC exhibits excellent bifunctional performance with a small potential gap of 0.666 V.Additionally,the assembled R-ZABs display a high-power density of 170 mW cm^(-2)and long-term stability,with the charge-discharge voltage gap increasing by only 0.01 V over 240 h.This work provides new insights into the design of efficient bifunctional catalysts.展开更多
Extracorporeal membrane oxygenation(ECMO) has been developed for nearly 70 years,and it is the main technology to treat cardiopulmonary failure and continue to maintain life.As the core component of the ECMO system,th...Extracorporeal membrane oxygenation(ECMO) has been developed for nearly 70 years,and it is the main technology to treat cardiopulmonary failure and continue to maintain life.As the core component of the ECMO system,the gas exchange membrane possesses low gas permeability and plasma leakage at present.In addition,the membrane material exists low blood compatibility,causing the formation of thrombosis.Therefore,the membrane material with high gas permeability and blood compatibility are urgently needed.This paper summarizes the membrane development process,preparation method,and modification method.It provides a new idea for the preparation and coating modification as artificial lung membrane.展开更多
The study of the oxygen evolution reaction(OER)mechanism is vital for advancing our understanding of this pivotal energy conversion process.This review synthesizes recent advancements in OER mechanism,emphasizing the ...The study of the oxygen evolution reaction(OER)mechanism is vital for advancing our understanding of this pivotal energy conversion process.This review synthesizes recent advancements in OER mechanism,emphasizing the intricate relationship between catalytic mechanisms and catalyst design.This review discusses the connotation and cutting-edge progress of traditional mechanisms such as adsorbate evolution mechanism(AEM)and lattice oxygen mechanism(LOM)as well as emerging pathways including oxide path mechanism(OPM),oxo-oxo coupling mechanism(OCM),and intramolecular oxygen coupling mechanism(IMOC)etc.Innovative research progress on the coexistence and transformation of multiple mechanisms is highlighted,and the intrinsic factors that influence these dynamic processes are summarized.Advanced characterization techniques and theoretical modeling are underscored as indispensable tools for revealing these complex interactions.This review provides guiding principles for mechanism-based catalyst design.Finally,in view of the multidimensional challenges currently faced by OER mechanisms,prospects for future research are given to bridge the gap between mechanism innovation and experimental verification and application.This comprehensive review provides valuable perspectives for advancing clean energy technologies and achieving sustainable development.展开更多
Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were...Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.展开更多
The dearth of efficacious and economic bifunctional oxygen electrocatalysts has constituted a significant impediment to the actual implementation of high-performance metal-air batteries.Here,we construct an efficaciou...The dearth of efficacious and economic bifunctional oxygen electrocatalysts has constituted a significant impediment to the actual implementation of high-performance metal-air batteries.Here,we construct an efficacious bifunctional oxygen electrocatalyst ZnFeNiCoCr high-entropy alloy(HEA)nanoparticles for oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)using a facile sol-gel strategy.The synthesized ZnFeNiCoCr HEA exhibits excellent bifunctional properties due to the synergistic effect between the metal elements.The overpotential of 305 mV at 10 mA·cm^(-2)for OER and a half-wave potential of 0.864 V for ORR,which is excellent to that of commercial RuO_(2)and Pt/C.Consequently,ZnFeNiCoCr HEA is utilized as a cathode catalyst for zinc-air batteries.The specific capacity of a zinc-air battery based on this HEA is 743 mAh·g^(-1)and the battery undergoes a continuous charge/discharge cycle for over 400 h.The ZnFeNiCoCr HEA catalyst holds significant application potential in diverse electrochemical energy storage and conversion devices.展开更多
Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional th...Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.展开更多
The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(...The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(3))by hydroxyl radical(OH)to form ROS poses significant challenges.The micelle balllike bimetallic La-Nb oxides(LNOx)have been developed as a bifunctional electrocatalyst for both the EOP and 3e^(-)ORR reactions.The LNO20 demonstrated a 9.8%of Faradaic efficiency(FE)in O_(3)production and a transfer number of 2.8 electrons in the 3e^(-)ORR.Theoretical calculations support the notion that the five-membered ring mechanism in LNO20 facilitates O_(3)production.Additionally,the incorporation of La provides active sites that enhance the activation of hydrogen peroxide(^(*)H_(2)O_(2))and the generation of OH.This innovative approach synergistically integrates EOP and 3e^(-)ORR,enhancing the activation of O_(3)to produce ROS,demonstrating exceptional efficacy in the degradation of organic pollutants and antimicrobial activity.The study paves the way for designing advanced electrocatalysts for EOP and 3e^(-)ORR and offers insights into utilizing electrochemical method to support other antibacterial strategies.展开更多
Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains...Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains a great challenge to avoid the inhomogeneous distribution and aggregation of metal single-atomic active centers in the construction of bifunctional electrocatalysts with atomically dispersed multimetallic sites because of the common calcination method.Herein,we report a novel catalyst with phthalocyanine-assembled Fe-Co-Ni single-atomic triple sites dispersed on sulfur-doped graphene using a simple ultrasonic procedure without calcination,and X-ray absorption fine structure(XAFS),aberration-corrected scanning transmission electron microscopy(AC-STEM),and other detailed characterizations are performed to demonstrate the successful synthesis.The novel catalyst shows extraordinary bifunctional ORR/OER activities with a fairly low potential difference(ΔE=0.621 V)between the OER overpotential(Ej10=315 mV at 10 m A cm^(-2))and the ORR half-wave potential(Ehalf-wave=0.924 V).Moreover,the above catalyst shows excellent ZAB performance,with an outstanding specific capacity(786 mAh g^(-1)),noteworthy maximum power density(139 mW cm^(-2)),and extraordinary rechargeability(discharged and charged at 5 mA cm^(-2) for more than 1000 h).Theoretical calculations reveal the vital importance of the preferable synergetic coupling effect between adjacent active sites in the Fe-Co-Ni trimetallic single-atomic sites during the ORR/OER processes.This study provides a new avenue for the investigation of bifunctional electrocatalysts with atomically dispersed trimetallic sites,which is intended for enhancing the ORR/OER performance in ZABs.展开更多
Four-electron oxygen evolving reaction is limited by proton adsorption and desorption,making its reaction kinetics sluggish,which poses a major challenge for catalyst design.Here,we present an unsaturated coordination...Four-electron oxygen evolving reaction is limited by proton adsorption and desorption,making its reaction kinetics sluggish,which poses a major challenge for catalyst design.Here,we present an unsaturated coordination interface by constructing a fast electron transfer channel between Cu_(2)V_(2)O_(7)(CVO)and BiVO4(BVO).X-ray absorption spectroscopy(XAS)and theoretical calculations results confirm that CVO and BVO between interfaces are bonded by the way of unsaturated coordination oxygen(Ouc).The Ouc optimizes the O-O coupled energy barrier at the V active site and promotes the disconnection of O-H bond,which increases the photocurrent intensity of CVO by 6 times.In addition,due to the high electronegativity of the Ouc,the bonding energies of Bi-O and Cu-O at the interface are enhanced,resulting in the long-term stability of the photoanode during the water splitting.Finally,by integrating the working electrode with a polysilicon solar cell,we assembled a device that demonstrated exceptional catalytic performance,achieving a hydrogen production rate of 100.6μmol·cm^(-2),and maintaining a hydrogen-to-oxygen volume ratio of 2:1 after continuous operation for 4 h.This discovery aids in a deeper understanding of photoanode design and offers further insights for industrial applications.展开更多
The top-bottom combined blowing converter mainly adopts the blowing method of top-blowing oxygen and bottom-blowing nitrogen.In the production process,there are some disadvantages,such as a significant temperature dif...The top-bottom combined blowing converter mainly adopts the blowing method of top-blowing oxygen and bottom-blowing nitrogen.In the production process,there are some disadvantages,such as a significant temperature difference between the top and bottom of the molten pool,inadequate gas permeability of bottom blowing,and low decarburization efficiency.Therefore,we propose a novel bottom-blowing gas doped oxygen process to enhance the smelting conditions in the converter.The 500 kg medium frequency induction furnace with top and bottom-blowing function was used to explore the influence of the proportion of bottom-blowing gas doped oxygen on the smelting effect in different smelting cycles.Subsequently,industrial experimental verification was carried out on a 60 t converter.The results of intermediate frequency furnace experiments demonstrate that the bottom-blowing gas doped oxygen process exhibits a superior heating rate and decarburization efficiency during the initial and final stages of blowing compared to pure N2 used for bottom-blowing.Simultaneously,the dephosphorization efficiency exhibited an initial increase followed by a subsequent decrease as the bottom-blowing oxygen content increased.The industrial test of 60 t converter validates the findings above.Moreover,when the oxygen content in bottom-blowing gas is 5%,the average blowing time reduces by 54 s,and the minimum endpoint carbon-oxygen equilibrium reaches 0.00219 under this condition.The results demonstrate that the appropriate amount of oxygen doped in bottom-blowing gas can effectively enhance the metallurgical conditions of the converter and improve production efficiency.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(No.22120230104).
文摘High-entropy alloy(HEA)nanoparticles(NPs)have attracted great attention in electrocatalysis due to their tailorable complex compositions and unique properties.Herein,we introduce Fe,Co,Ni,Cr and Mn into the metal-polyphenol coordination system to prepare HEA NPs enclosed in N-doped carbon(FeCoNiCrMn)with great potential for catalyzing oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).The unique high-entropy structural characteristics in FeCoNiCrMn facilitate effective interplay between metal species,leading to improved ORR(E_(1/2)=0.89 V)and OER(η=330 mV,j=10 mA·cm^(−2))activity.Additionally,FeCoNiCrMn exhibits excellent open-circuit voltage(1.523 V),power density(110 mW·cm^(−2))and long-term durability,outperforming Pt/C+IrO_(2) electrodes as a cathode catalyst in Zn-air batteries(ZABs).Such polyphenol-assisted alloying method broadens and simplifies the development of HEA electrocatalysts for high-performance ZABs.
文摘Reactive oxygen species(ROS),including singlet oxygen(^(1)O_(2)),hydroxyl radicals(·OH),and superoxide anions(O_(2)^(·-)),are highly reactive molecules that play central roles in many chemical,biological,and environmental processes due to their strong oxidative power[1].Generating ROS in a controlled manner under mild conditions is essential for achieving selective oxidation reactions.Light-driven methods are especially appealing for this purpose,as they offer precise control over where and when ROS are produced.
文摘The oxygen evolution reaction(OER)serves as a fundamental half–reaction in the electrolysis of water for hydrogen production,which is restricted by the sluggish OER reaction kinetics and unable to be practically applied.The traditional lattice oxygen oxidation mechanism(LOM)offers an advantageous route by circumventing the formation of M-OOH^(*)in the adsorption evolution mechanism(AEM),thus enhancing the reaction kinetics of the OER but resulting in possible structural destabilization due to the decreased M–O bond order.Fortunately,the asymmetry of tetrahedral and octahedral sites in transition metal spinel oxides permits the existence of non-bonding oxygen,which could be activated by rational band structure design for direct O-O coupling,where the M–O bond maintains its initial bond order.Here,non-bonding oxygen was introduced into NiFe_(2)O_(4)via annealing in an oxygen-deficient atmosphere.Then,in-situ grown sulfate species on octahedral nickel sites significantly improved the reactivity of the non-bonding oxygen electrons,thereby facilitating the transformation of the redox center from metal to oxygen.LOM based on non-bonding oxygen(LOMNB)was successfully activated within NiFe_(2)O_(4),exhibiting a low overpotential of 206 mV to achieve a current density of 10 mA cm^(-2)and excellent durability of stable operation for over 150 h.Additionally,catalysts featuring varying band structures were synthesized for comparative analysis,and it was found that the reversible redox processes of non-bonding oxygen and the accumulation of non-bonding oxygen species containing 2p holes are critical prerequisites for triggering and sustaining the LOMNB pathway in transition metal spinel oxides.These findings may provide valuable insights for the future development of spinel-oxide-based LOM catalysts.
基金Supported by National Natural Science Foundation of China,No.82200353Jiangsu Province Double Innovation Doctoral Program,No.JSSCBS20221948+3 种基金Suzhou Gusu Health Talent Program,No.(2022)043Suzhou Gusu Health Talent Plan Talent Research Project,No.GSWS2022014Jiangsu Province College Students’Innovation and Entrepreneurship Training Program Project,No.202410285087Zand“Boxi”Talent Casting Plan of the First Affiliated Hospital of Soochow University。
文摘This article comments on the research by Zhang et al on the role of advanced heart failure and transplant teams in extracorporeal membrane oxygenation(ECMO)management.The study by Zhang et al indicates that direct advanced heart failure and transplant involvement improves survival in ECMO patients,especially those on veno-arterial ECMO.However,the optimal approach varies due to multiple factors.This article discusses the clinical implications,research design limitations,and future directions to enhance ECMO care.
文摘Oxygen evolution reaction(OER)is often regarded as a crucial bottleneck in the field of renewable energy storage and conversion.To further accelerate the sluggish kinetics of OER,a cation and anion modulation strategy is reported here,which has been proven to be effective in preparing highly active electrocatalyst.For example,the cobalt,sulfur,and phosphorus modulated nickel hydroxide(denoted as NiCoPSOH)only needs an overpotential of 232 mV to reach a current density of 20 mA cm^(–2),demonstrating excellent OER performances.The cation and anion modulation facilitates the generation of high-valent Ni species,which would activate the lattice oxygen and switch the OER reaction pathway from conventional adsorbate evolution mechanism to lattice oxygen mechanism(LOM),as evidenced by the results of electrochemical measurements,Raman spectroscopy and differential electrochemical mass spectrometry.The LOM pathway of NiCoPSOH is further verified by the theoretical calculations,including the upshift of O 2p band center,the weakened Ni–O bond and the lowest energy barrier of rate-limiting step.Thus,the anion and cation modulated catalyst NiCoPSOH could effectively accelerate the sluggish OER kinetics.Our work provides a new insight into the cation and anion modulation,and broadens the possibility for the rational design of highly active electrocatalysts.
基金supported by the Natural Science Foundation of Shanghai(No.23ZR1401300)the National Natural Science Foundation of China(No.52170068).
文摘Singlet oxygen(^(1)O_(2)),as an electrophilic oxidant,is essential for the selective water decontamination of pollutants from water.Herein,we showcase a high-performing electrocatalytic filtration system composed of carbon nanotubes functionalized with CoFe alloy nanoparticles(CoFeCNT)to selectively facilitate the electrochemical activation of O_(2)to^(1)O_(2).Benefiting from the prominently featured bimetal active sites of CoFeCNT,nearly complete production of^(1)O_(2)is achieved by the electrocatalytic activation of O_(2).Additionally,the proposed system exhibits a consistent pollutant removal efficiency>90%in a flow-through reactor over 48 h of continuous operation without a noticeable decline in performance,highlighting the dependable stability of the system for practical applications.The flow-through configuration demonstrates a striking 8-fold enhancement in tetracycline oxidation compared to a conventional batch reactor.This work provides a molecular level understanding of the oxygen reduction reaction,showing promising potential for the selective removal of emerging organic contaminants from water.
基金supported by the Natural Science Foundation of Hebei Province(no.E2024501010)the National Natural Science Foundation of China(no.52374301)+1 种基金the Shijiazhuang Basic Research Project(no.241790667A)the Performance Subsidy Fund for Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province(no.22567627H)。
文摘The development of highly efficient non-precious metal-nitrogen-carbon(M-N-C)electrocatalysts is a key scientific issue for improving the performance of metal-air batteries and fuel cells.Due to the symmetric charge distribution of the traditional M-N_(4)active site,the adsorption energy of the key oxygen intermediates in the process of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is difficult to reach the optimal value,which seriously limits the catalytic efficiency.The core of solving this problem lies in the accurate modulation of the coordination environment of the M-N_(4)site,which can realize the breakthrough improvement of the catalytic performance by synergistically optimizing the geometric configuration and electronic structure.In this paper,we systematically analyze the ORR/OER reaction mechanism and then comprehensively review the four main strategies to optimize the coordination environment of M-N-C:metal site regulation,coordination number engineering,non-metal atom doping,and carbon support regulation.Through an in-depth analysis of the structure-activity relationship between the coordination configuration and catalytic performance,the core challenges faced by current research are pointed out,and future research directions are envisioned.This work aims to provide theoretical references for the directional construction of highly efficient M-N-C catalysts with optimized coordination environments.
文摘The authors regret<During the submission process,Hongxiang Zhang and Honggen Peng served as the first and the second corresponding author,respectively.The original manuscript submitted for this paper also listed two co-corresponding authors(Hongxiang Zhang and Honggen Peng).But the corresponding author of Honggen Peng was omitted in the final published manuscript.So,we apply to designate Honggen Peng(penghonggen@ncu.edu.cn)as the second co-corresponding author and the corresponding unit is“a,b">.
文摘Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaust temperatures below 200℃,particularly under conditions of frequent idling.Herein,we report an effective strategy utilizing non-thermal plasma(NTP)to activate Olatt in Ce_(1–x)Co_(x)O_(2–δ)catalysts,achieving dramatic enhancement of the soot combustion rate at low temperatures.At 200℃ and 4.3 W(discharge power,P_(dis)),NTP-Ce_(0.8)Co_(0.2)O_(2–δ)achieved 96.9%soot conversion(X_(C)),99.0%CO_(2) selectivity(S(CO_(2)))and a maximum energy conversion efficiency(Emax)of 14.7 g kWh^(–1).Compared with previously reported results,NTP-Ce_(0.8)Co_(0.2)O_(2–δ)exhibits the highest S(CO_(2))and Emax values.Remarkably,even without heating,X_(C),Emax,and S(CO_(2))reached 92.1%,6.1 g kWh–1,and 97.5%,respectively,at 6.3 W(P_(dis)).The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO_(2) crystal lattice and forms an asymmetric Ce–O–Co structure,making oxygen“easy come,easy go”,thereby enabling the rapid combustion of soot over NTP-Ce_(0.8)Co_(0.2)O_(2–δ).This study highlights the great potential of NTP for activating Olatt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.
基金supported by the National Natural Science Foundation of China(22202053,22109035,52362031,and 52274297)the start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084,23068,and 23169)+4 种基金the Hainan Province Science and Technology Special Fund(ZDYF2024SHFZ074)the Collaborative Innovation Center of Marine Science and Technology,Hainan University(XTCX2022HYC04)the specific research fund of The Innovation Platform for Academicians of Hainan Province(YSPTZX202315)the Research Fund Program of Guangdong Provincial Key Laboratory of Fuel Cell Technology(FC202307)the Open Fund Project of Key Laboratory of Electrochemical Energy Storage and Energy Conversion in Hainan Province of China(KFKT2023002)。
文摘Hydrogen production from water electrolysis,in particular from proton exchange membrane water electrolyzers(PEMWE),is a key approach to realizing a carbon-free energy cycle.However,the high anodic potential and strong acid in PEMWE systems pose a major challenge to the stability of electrocatalysts,and the development of efficient and corrosion-resistant catalysts is urgently needed.Currently,iridium(Ir)-based catalysts have gained great attention due to their promising activity and stability,while the extremely low reserves of Ir in the earth seriously hinder the commercialization of PEMWE.Therefore,a systematic understanding of the latest advances in Ir-based catalysts is necessary to guide their rational design to meet the industrial requirements.In this review,the general reaction mechanisms and advanced characterization techniques for mechanism recognition are first introduced.Afterwards,the systematic design strategies and performances of Ir-based catalysts,including metallic Ir,Ir oxides,and Ir-based perovskites,are summarized in detail.Finally,the conclusions,challenges,and prospects for Ir-based electrocatalysts are presented.
基金supported by the Hainan Province Science and Technology Special Fund(ZDYF2020037)the National Natural Science Foundation of China(22109035,52164028,52274297,22462006)+3 种基金the Postdoctoral Science Foundation of Hainan Province(RZ2100007123)the Basic and Applied Basic Research Foundation of Guangdong Province(2019A1515110558)the Start-up Research Foundation of Hainan University(KYQD(ZR)-20008,20083,20084,21125)Hainan University(XTCX2022HYC05)。
文摘Efficient catalysis of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is essential for the rechargeable zinc-air batteries(R-ZABs).However,challenges remain due to the scarcity of effective bifunctional electrocatalysts and limited understanding of the structure-activity relationships.Pyrrole-type single-atom catalysts(SACs)with unique electronic structures have emerged as promising electrocatalysts.In this work,we combine density functional theory(DFT)calculations and experimental studies to systematically explore the structure-activity relationships and potential of pyrrole-type transition metal-N_(3)(TM-po-N_(3))as bifunctional catalysts.DFT calculations reveal that differences in the dependence of ORR and OER activities on the free energy of adsorption of reaction intermediates significantly affect the TM-po-N_(3)bifunctional activity and identify magnetic Cu-po-N_(3)as the best candidate.The bifunctional activity of Cu-po-N_(3)originates from interactions between spin-polarized out-of-plane Cu_3d and O_2s+2p orbitals.Theoretical predictions are validated experimentally,showing that the synthesized Cu-SAC/NC exhibits excellent bifunctional performance with a small potential gap of 0.666 V.Additionally,the assembled R-ZABs display a high-power density of 170 mW cm^(-2)and long-term stability,with the charge-discharge voltage gap increasing by only 0.01 V over 240 h.This work provides new insights into the design of efficient bifunctional catalysts.
基金the support of this work by State Key Laboratory of Tribology in Advanced Equipment,Tsinghua University(61012205321)。
文摘Extracorporeal membrane oxygenation(ECMO) has been developed for nearly 70 years,and it is the main technology to treat cardiopulmonary failure and continue to maintain life.As the core component of the ECMO system,the gas exchange membrane possesses low gas permeability and plasma leakage at present.In addition,the membrane material exists low blood compatibility,causing the formation of thrombosis.Therefore,the membrane material with high gas permeability and blood compatibility are urgently needed.This paper summarizes the membrane development process,preparation method,and modification method.It provides a new idea for the preparation and coating modification as artificial lung membrane.
文摘The study of the oxygen evolution reaction(OER)mechanism is vital for advancing our understanding of this pivotal energy conversion process.This review synthesizes recent advancements in OER mechanism,emphasizing the intricate relationship between catalytic mechanisms and catalyst design.This review discusses the connotation and cutting-edge progress of traditional mechanisms such as adsorbate evolution mechanism(AEM)and lattice oxygen mechanism(LOM)as well as emerging pathways including oxide path mechanism(OPM),oxo-oxo coupling mechanism(OCM),and intramolecular oxygen coupling mechanism(IMOC)etc.Innovative research progress on the coexistence and transformation of multiple mechanisms is highlighted,and the intrinsic factors that influence these dynamic processes are summarized.Advanced characterization techniques and theoretical modeling are underscored as indispensable tools for revealing these complex interactions.This review provides guiding principles for mechanism-based catalyst design.Finally,in view of the multidimensional challenges currently faced by OER mechanisms,prospects for future research are given to bridge the gap between mechanism innovation and experimental verification and application.This comprehensive review provides valuable perspectives for advancing clean energy technologies and achieving sustainable development.
基金supported by the National Natural Science Foundation of China(No.U21A20293).
文摘Harnessing the redox potential of biochar to activate airborne O_(2)for contaminant removal is challenging.In this study,ferrihydrite(Fh)modified the boron(B),nitrogen(N)co-doped biochars(BCs)composites(Fh/B(n)NC)were developed for enhancing the degradation of a model pollutant,tetracycline(TC),merely by airborne O_(2).Fh/B(3)NC showed excellent O_(2)activation activity for efficient TC degradation with a apparent TC degradation rate of 5.54,6.88,and 22.15 times that of B(3)NC,Fh,and raw BCs,respectively,where 1O_(2)and H_(2)O_(2)were identified as the dominant ROS for TC degradation.The B incorporation into the carbon lattice of Fh/B(3)NC promoted the generation of electron donors,sp2 C and the reductive B species,hence boosting Fe(III)reduction and 1O_(2)generation.O_(2)adsorption was enhanced due to the positively charged adsorption sites(C-B+and N-C+).And 1O_(2)was generated via Fe(II)catalyzed low-efficient successive one-electron transfer(O_(2)→O_(2)·−→1O_(2),H_(2)O_(2)),as well as biochar catalyzed high-efficient two-electron transfer(O_(2)→H_(2)O_(2)→1O_(2))that does not involve.O_(2)−as the intermediate.Moreover,Fh/B,N co-doped biochar showed a wide pH range,remarkable anti-interference capabilities,and effective detoxification.These findings shed new light on the development of environmentally benign BCs materials capable of degradading organic pollutants.
基金supported by the National Natural Science Foundation of China(Nos.U22A20143 and 22201262).
文摘The dearth of efficacious and economic bifunctional oxygen electrocatalysts has constituted a significant impediment to the actual implementation of high-performance metal-air batteries.Here,we construct an efficacious bifunctional oxygen electrocatalyst ZnFeNiCoCr high-entropy alloy(HEA)nanoparticles for oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)using a facile sol-gel strategy.The synthesized ZnFeNiCoCr HEA exhibits excellent bifunctional properties due to the synergistic effect between the metal elements.The overpotential of 305 mV at 10 mA·cm^(-2)for OER and a half-wave potential of 0.864 V for ORR,which is excellent to that of commercial RuO_(2)and Pt/C.Consequently,ZnFeNiCoCr HEA is utilized as a cathode catalyst for zinc-air batteries.The specific capacity of a zinc-air battery based on this HEA is 743 mAh·g^(-1)and the battery undergoes a continuous charge/discharge cycle for over 400 h.The ZnFeNiCoCr HEA catalyst holds significant application potential in diverse electrochemical energy storage and conversion devices.
基金supported by the National Natural Science Foundation of China(Nos.22102167 and U21A20317)。
文摘Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.
基金the financial support from the National Key R&D Program of China(2022YFA1504200)the Zhejiang Provincial Natural Science Foundation(No.LR22B060003)+2 种基金the National Natural Science Foundation of China(22322810,22078293,22141001,and 22008211)the Fundamental Research Funds for the Provincial Universities of Zhejiang(RF-C2023004)the Midea Group-Zhejiang University of Technology Joint Development Funding(KYY-HX-20240263)。
文摘The anodic electrochemical ozone production(EOP)and the cathodic three-electron oxygen reduction reaction(3e^(-)ORR)are effective processes for generating active oxygen species(ROS).However,the activation of ozone(O_(3))by hydroxyl radical(OH)to form ROS poses significant challenges.The micelle balllike bimetallic La-Nb oxides(LNOx)have been developed as a bifunctional electrocatalyst for both the EOP and 3e^(-)ORR reactions.The LNO20 demonstrated a 9.8%of Faradaic efficiency(FE)in O_(3)production and a transfer number of 2.8 electrons in the 3e^(-)ORR.Theoretical calculations support the notion that the five-membered ring mechanism in LNO20 facilitates O_(3)production.Additionally,the incorporation of La provides active sites that enhance the activation of hydrogen peroxide(^(*)H_(2)O_(2))and the generation of OH.This innovative approach synergistically integrates EOP and 3e^(-)ORR,enhancing the activation of O_(3)to produce ROS,demonstrating exceptional efficacy in the degradation of organic pollutants and antimicrobial activity.The study paves the way for designing advanced electrocatalysts for EOP and 3e^(-)ORR and offers insights into utilizing electrochemical method to support other antibacterial strategies.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22305071,52472200,52271176,and52072114)the 111 Project(Grant No.D17007)+3 种基金Henan Center for Outstanding Overseas Scientists(Grant No.GZS2022017)the China Postdoctoral Science Foundation(Grant No.2022M721049)the Henan Province Key Research and Development Project(Grant No.231111520500)the Natural Science Foundation of Henan Province(Grant No.252300421556)。
文摘Development of high-efficiency bifunctional oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)electrocatalysts is vital for the widespread application of zinc-air batteries(ZABs).However,it still remains a great challenge to avoid the inhomogeneous distribution and aggregation of metal single-atomic active centers in the construction of bifunctional electrocatalysts with atomically dispersed multimetallic sites because of the common calcination method.Herein,we report a novel catalyst with phthalocyanine-assembled Fe-Co-Ni single-atomic triple sites dispersed on sulfur-doped graphene using a simple ultrasonic procedure without calcination,and X-ray absorption fine structure(XAFS),aberration-corrected scanning transmission electron microscopy(AC-STEM),and other detailed characterizations are performed to demonstrate the successful synthesis.The novel catalyst shows extraordinary bifunctional ORR/OER activities with a fairly low potential difference(ΔE=0.621 V)between the OER overpotential(Ej10=315 mV at 10 m A cm^(-2))and the ORR half-wave potential(Ehalf-wave=0.924 V).Moreover,the above catalyst shows excellent ZAB performance,with an outstanding specific capacity(786 mAh g^(-1)),noteworthy maximum power density(139 mW cm^(-2)),and extraordinary rechargeability(discharged and charged at 5 mA cm^(-2) for more than 1000 h).Theoretical calculations reveal the vital importance of the preferable synergetic coupling effect between adjacent active sites in the Fe-Co-Ni trimetallic single-atomic sites during the ORR/OER processes.This study provides a new avenue for the investigation of bifunctional electrocatalysts with atomically dispersed trimetallic sites,which is intended for enhancing the ORR/OER performance in ZABs.
基金supported by the Natural Science Foundation of China(Nos.22278094 and 22379033)Guangdong Graduate Education Innovation Program(No.2023JGXM_102)+2 种基金the Basic and Applied Basic Research Program of Guangzhou(No.SL2024A03J00499)the University Innovation Team Scientific Research Project of Guangzhou(No.202235246)Hainan Province Graduate Innovation Research Project(No.Qhyb2023-143).
文摘Four-electron oxygen evolving reaction is limited by proton adsorption and desorption,making its reaction kinetics sluggish,which poses a major challenge for catalyst design.Here,we present an unsaturated coordination interface by constructing a fast electron transfer channel between Cu_(2)V_(2)O_(7)(CVO)and BiVO4(BVO).X-ray absorption spectroscopy(XAS)and theoretical calculations results confirm that CVO and BVO between interfaces are bonded by the way of unsaturated coordination oxygen(Ouc).The Ouc optimizes the O-O coupled energy barrier at the V active site and promotes the disconnection of O-H bond,which increases the photocurrent intensity of CVO by 6 times.In addition,due to the high electronegativity of the Ouc,the bonding energies of Bi-O and Cu-O at the interface are enhanced,resulting in the long-term stability of the photoanode during the water splitting.Finally,by integrating the working electrode with a polysilicon solar cell,we assembled a device that demonstrated exceptional catalytic performance,achieving a hydrogen production rate of 100.6μmol·cm^(-2),and maintaining a hydrogen-to-oxygen volume ratio of 2:1 after continuous operation for 4 h.This discovery aids in a deeper understanding of photoanode design and offers further insights for industrial applications.
基金supported by the National Natural Science Foundation of China(No.U21A20317)the National Key Research and Development Program of China(No.2017YFB0304201).
文摘The top-bottom combined blowing converter mainly adopts the blowing method of top-blowing oxygen and bottom-blowing nitrogen.In the production process,there are some disadvantages,such as a significant temperature difference between the top and bottom of the molten pool,inadequate gas permeability of bottom blowing,and low decarburization efficiency.Therefore,we propose a novel bottom-blowing gas doped oxygen process to enhance the smelting conditions in the converter.The 500 kg medium frequency induction furnace with top and bottom-blowing function was used to explore the influence of the proportion of bottom-blowing gas doped oxygen on the smelting effect in different smelting cycles.Subsequently,industrial experimental verification was carried out on a 60 t converter.The results of intermediate frequency furnace experiments demonstrate that the bottom-blowing gas doped oxygen process exhibits a superior heating rate and decarburization efficiency during the initial and final stages of blowing compared to pure N2 used for bottom-blowing.Simultaneously,the dephosphorization efficiency exhibited an initial increase followed by a subsequent decrease as the bottom-blowing oxygen content increased.The industrial test of 60 t converter validates the findings above.Moreover,when the oxygen content in bottom-blowing gas is 5%,the average blowing time reduces by 54 s,and the minimum endpoint carbon-oxygen equilibrium reaches 0.00219 under this condition.The results demonstrate that the appropriate amount of oxygen doped in bottom-blowing gas can effectively enhance the metallurgical conditions of the converter and improve production efficiency.