ABO_(3)-type perovskite oxides(e.g.,LaCoO_(3))with flexible and adjustable A-and B-sites are ideal model catalysts to unravel the relationship between the electronic structure and electrocatalytic activity(e.g.,oxygen...ABO_(3)-type perovskite oxides(e.g.,LaCoO_(3))with flexible and adjustable A-and B-sites are ideal model catalysts to unravel the relationship between the electronic structure and electrocatalytic activity(e.g.,oxygen reduction/evolution reactions,ORR/OER).It has been well understood in our recent work that the secondary metal dopant at B-site(e.g.,Mn in LaMn_(x)Co_(1-x)O_(3))can regulate the electronic structure and improve the ORR/OER activity.In this work,the Mn-Ni pairs are employed as the dual dopant in LaMn_(x)Ni_(y)Co_(z)O_(3)(x+y+z=1)catalysts toward bifunctional ORR and OER.The structure-property relationships between the triple metal B-site(Mn,Ni and Co)and the electrochemical performance are particularly investigated.Compared to the individual Mn doping(e.g.,LaMnCoO3(Mn:Co=1:3)catalyst),the dual Mn-Ni doping significantly improves the ORR mass activity@0.8 V by 1.54 times;meanwhile,the OER overpotential@10 mA cm^(-2) is reduced from 420 to 370 mV,and the OER current density at 1.55 V is increased by 2.43 times.Reasonably,the potential gap between EDRR@-1 mA cm^(-2) and EDER@10 mA cm^(-2) is achieved as only 0.76 V by using the optimal LaMn_(x)Ni_(y)Co_(z)O_(3)(x:y:z=1:2:3)catalyst.It is revealed that the dual Mn-Ni dopant efficiently optimizes electron structures of the LaMnNiCoO_(3)(1:2:3)catalyst,which not only decreases the e_(g) orbital electron number,but also modulates the O 2 p-band closer to the Femi level,accounting for the enhanced bifunctional activity.展开更多
Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-prot...Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-proton transfers more complex when determining kinetics and mass transfer information.Understanding how HER competes with other electrochemical reduction reactions is crucial for both fundamental studies and system performance improvements.In this study,we employed the oxygen reduction reaction(ORR)as a model reaction to investigate HER competition on a polycrystalline-Au surface,using a rotating ring and disk electrode.It’s proved that water molecules serve as the proton source for ORR in alkaline,neutral,and even acidic electrolytes,and a 4-electron process can be achieved when the overpotential is sufficiently high.The competition from H⁺reduction becomes noticeable at the H⁺concentration higher than 2 mmol L^(–1)and intensi-fies as the H^(+)concentration increases.Based on the electrochemical results,we obtained an equivalent circuit diagram for the ORR system with competition from the H+reduction reaction,showing that these reactions occur in parallel and compete with each other.Electrochemical impedance spectroscopy measurements further confirm this argument.Additionally,we discover that the contribution of H+mass transfer to the total H^(+)reduction current is significant and comparable to the kinetic current.We believe this work will deepen our understanding of HER and its competition in electrochemical reduction systems.展开更多
Artificial carbon fixation is a promising pathway for achieving the carbon cycle and environment remediation.However,the sluggish kinetics of oxygen evolution reaction(OER)and poor selectivity of CO_(2) reduction seri...Artificial carbon fixation is a promising pathway for achieving the carbon cycle and environment remediation.However,the sluggish kinetics of oxygen evolution reaction(OER)and poor selectivity of CO_(2) reduction seriously limited the overall conversion efficiencies of solar energy to chemical fuels.Herein,we demonstrated a facile and feasible strategy to rationally regulate the coordination environment and electronic structure of surface-active sites on both photoanode and cathode.More specifically,the defect engineering has been employed to reduce the coordination number of ultrathin FeNi catalysts decorated on BiVO4 photoanodes,resulting in one of the highest OER activities of 6.51 mA cm^(−2)(1.23 VRHE,AM 1.5G).Additionally,single-atom cobalt(II)phthalocyanine anchoring on the N-rich carbon substrates to increase Co–N coordination number remarkably promotes CO_(2) adsorption and activation for high selective CO production.Their integration achieved a record activity of 109.4μmol cm^(−2) h−1 for CO production with a faradaic efficiency of>90%,and an outstanding solar conversion efficiency of 5.41%has been achieved by further integrating a photovoltaic utilizing the sunlight(>500 nm).展开更多
The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challen...The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challenging.Herein,N-doped carbon(N-C)anchored atomically dispersed Ni-N_(3)site with proximity defects(Ni-N_(3)D)induced by Te atoms doping is reported.Benefitting from the inductive effect of proximity defect,the Ni-N_(3)D/Te-N-C catalyst performs excellent ORR and HER performance in alkaline and acid condition.Both in situ characterization and theoretical calculation reveal that the existence of proximity defect effect is conducive to lower rate-determining-step energy barrier of ORR and HER,thus accelerating the multielectron reaction kinetics.This work paves a novel strategy for constructing highactivity bifunctional SACs by defect engineering for development of sustainable energy.展开更多
A novel photocatalytic cocatalyst, MoC quantum dots integrated into N-doped carbon microflowers (MoC–NC), was synthesized, establishing a key Mo–N interfacial bond. The Mo–N bond's regulation was achieved by ad...A novel photocatalytic cocatalyst, MoC quantum dots integrated into N-doped carbon microflowers (MoC–NC), was synthesized, establishing a key Mo–N interfacial bond. The Mo–N bond's regulation was achieved by adjusting the pH of Mo-polydopamine precursor solutions. A composite photocatalyst, MoC–NC/CdS (MNS), was formed by in situ growth of nano-CdS on MoC–NC. The pH during synthesis, crucial for Mo–N bond formation, significantly influenced Cr(Ⅵ) reduction and H_(2) evolution performance. The optimal MNS, created at pH 9.0, demonstrated 99.2% reduction efficiency for Cr(Ⅵ) in 20 min and H_(2) evolution rate of 11.4 mmol g^(-1) h^(-1) over 3 h, outperforming Pt/CdS. Mechanistic studies and density functional theory revealed MoC–NC's role in enhancing light absorption, reaction kinetics, and electron transport, attributing to its ultra-small quantum dots and abundant Mo–N bonds.展开更多
Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)th...Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)that featured with interconnected three-dimensional(3D)ordered porous hierarchies(3DOM FeCo/NC)are prepared,and its electrocatalytic activity is studied.Due to the open structure of 3D ordered macro-pores that greatly improves the mass transfer capacity of the catalytic process and enhances the utilization of active sites inside the catalyst,as well as the uniform distribution of Fe and Co bimetallic sites on the porous skeleton,3DOM FeCo/NC exhibits superior bi-functional catalytic activities for both hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR).The overpotential of HER is lower than that of commercial Pt/C when performed at high current density(>235 mA cm^(-2))in1.0 M KOH,and the half-wave potential(0.896 V)of ORR in 0.1 M KOH is also superior to that of 20% commercial Pt/C and most other similar catalysts.The effective utilization and synergistic effect of CoFe_(2)O_(4)and CoFe hetero-metallic sites remarkably enhance the electrocatalytic activity.Furthermore,3DOM FeCo/NC is assembled as an air electrode in Zn-air battery,and exhibits satisfactory maximum power density,open-circuit voltage,and charge/discharge stability over benchmark Pt/C+IrO_(2).This work contributes new insights into the design of transition-metal-based multifunctional catalysts,and has great potential for energy conversion and storage.展开更多
Owing to their multi-elemental compositions and unique high-entropy mixing states,high-entropy alloy(HEA)nanoparticles(NPs)displaying tunable activities and enhanced stabilities thus have become a rapidly growing area...Owing to their multi-elemental compositions and unique high-entropy mixing states,high-entropy alloy(HEA)nanoparticles(NPs)displaying tunable activities and enhanced stabilities thus have become a rapidly growing area of research in recent years.However,the integration of multiple elements into HEA NPs at the nanoscale remains a formidable challenge,especially when it comes to the precise control of particle size,elemental composition and content.Herein,a simple and universal high-energy laser assisted reduction approach is presented,which achieves the preparation of HEA NPs with a wide range of multi-component,controllable particle sizes and constitution on different substrates within seconds.Laser on carbon nanofibers induced momentary high-temperature annealing(>2000 K and ramping/cooling rates>10^(5)K s^(-1))to successfully decorate HEA NPs up to twenty elements with excellent compatibility for large-scale synthesis(20.0×20.0 cm^(2)of carbon cloth).The IrPdPtRhRu exhibit robust electrocatalytic hydrogen evolution reaction(HER)activities and low overpotentials of 16,28,and 12 mV at a current density of 10 mA cm^(-2)in alkaline(1.0 M KOH),alkaline simulated seawater(1.0 M KOH+0.5 M NaCl),and acidic(0.5 M H_(2)SO_(4))electrolytes,respectively,and excellent stability(7 days and>2000 cycles)at the alkaline HER.展开更多
Mg-3Gd(wt.%)samples with different initial grain sizes were prepared to evaluate the grain size effect on microstructural evolution during cold rolling and subsequent annealing hardening response.The deformation behav...Mg-3Gd(wt.%)samples with different initial grain sizes were prepared to evaluate the grain size effect on microstructural evolution during cold rolling and subsequent annealing hardening response.The deformation behavior and mechanical response of the as-rolled and annealed samples were systematically investigated by a combination of electron microscopy and microhardness characterization.The results show that the twinning activities were highly suppressed in the fine-grained samples during rolling.Upon increasing the rolling reduction to 40%,ultra-fine grain structures with a volume fraction of∼28%were formed due to the activation of multiple slip systems.Conversely,twinning dominated the early stages of deformation in the coarse-grained samples.After a 10%rolling reduction,numerous twins with a volume fraction of∼23%were formed.Further increasing the rolling reduction to 40%,high-density dislocations were activated and twin structures with a volume fraction of∼36%were formed.The annealing hardening response of deformed samples was effectively enhanced compared to that of the non-deformed samples,which was attributed to the enhanced Gd segregation along grain boundaries,twin boundaries and dislocation cores.Moreover,the grain size and rolling reduction were found to affect the microstructure evolution during annealing,resulting in a notable difference in the annealing hardening response of Mg-3Gd alloy between samples of different grain sizes deformed to different strains.These findings highlight the crucial importance of microstructural and processing parameters in the design of high-strength,cost-effective Mg alloys.展开更多
Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associate...Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associated with important reduction reactions,such as oxygen reduction reaction(ORR),which leads to the production of hydrogen peroxide(H_(2)O_(2)).These transitions are instrumental in the emergence and evolution of life.In this study,transition metals were loaded onto nitrogen-doped carbon(NDC)prepared under the primitive Earth's atmospheric conditions.These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination.The chemical pathways initiated by the pristine and metal-loaded NDC were investigated.This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.展开更多
Against the background of“carbon peak and carbon neutrality,”it is of great practical significance to develop non-blast furnace ironmaking technology for the sustainable development of steel industry.Carbon-bearing ...Against the background of“carbon peak and carbon neutrality,”it is of great practical significance to develop non-blast furnace ironmaking technology for the sustainable development of steel industry.Carbon-bearing iron ore pellet is an innovative burden of direct reduction ironmaking due to its excellent self-reducing property,and the thermal strength of pellet is a crucial metallurgical property that affects its wide application.The carbon-bearing iron ore pellet without binders(CIPWB)was prepared using iron concentrate and anthracite,and the effects of reducing agent addition amount,size of pellet,reduction temperature and time on the thermal compressive strength of CIPWB during the reduction process were studied.Simultaneously,the mechanism of the thermal strength evolution of CIPWB was revealed.The results showed that during the low-temperature reduction process(300-500℃),the thermal compressive strength of CIPWB linearly increases with increasing the size of pellet,while it gradually decreases with increasing the anthracite ratio.When the CIPWB with 8%anthracite is reduced at 300℃for 60 min,the thermal strength of pellet is enhanced from 13.24 to 31.88 N as the size of pellet increases from 8.04 to 12.78 mm.Meanwhile,as the temperature is 500℃,with increasing the anthracite ratio from 2%to 8%,the thermal compressive strength of pellet under reduction for 60 min remarkably decreases from 41.47 to 8.94 N.Furthermore,in the high-temperature reduction process(600-1150℃),the thermal compressive strength of CIPWB firstly increases and then reduces with increasing the temperature,while it as well as the temperature corresponding to the maximum strength decreases with increasing the anthracite ratio.With adding 18%anthracite,the thermal compressive strength of pellet reaches the maximum value at 800℃,namely 35.00 N,and obtains the minimum value at 1050℃,namely 8.60 N.The thermal compressive strength of CIPWB significantly depends on the temperature,reducing agent dosage,and pellet size.展开更多
The Cu/1010 steel bimetal laminated composites(BLCs)were rolled to different thicknesses to investigate the effect of rolling direction and reduction on the microstructure evolution and mechanical properties.The diffe...The Cu/1010 steel bimetal laminated composites(BLCs)were rolled to different thicknesses to investigate the effect of rolling direction and reduction on the microstructure evolution and mechanical properties.The difference of mechanical properties between the Cu and 1010 steel causes different thickness reductions,percentage spread,and cladding ratios.The formation of strong texture induces larger strength of the rolled samples,and as the volume fraction of 1010 steel is larger in Route-A,its strength is consistently greater than that in Route-B.The obstruction of interface to crystal and dislocation slip results in the formation of interface distortion,inducing dislocation density gradient when the rolling reduction is low in Route-A.The slip planes of the Cu and 1010 steel are more prone to suffer the normal strain,while the shear strain of other crystal planes is obviously larger than the normal strain under rolling load near the interface.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
Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhou...Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhouse effect and energy shortage.Herein,Cr-doped zinc sulfide(ZnS)with accompanying sulphur vacancies(Vs)photocatalytic materials is developed by a facile hydrothermal method.The Cr dopants centralize photoinduced holes and Vs trap electrons,forming a synergistic effect for accelerating charge separation and transfer.The reaction energy barrier for both H2 evolution and CO_(2) reduction has been optimized.Therefore,in the absence of a cocatalyst,the optimal catalyst(Zn_(0.94) Cr_(0.06) S)achieves an out-standing H_(2) evolution activity of 20.3 mmol g^(-1) h^(-1),which is approximately 2.9 times higher than 6.9 mmol g^(-1) h^(-1) for pristine ZnS.In addition,in the gas-solid reaction system without co-catalysts or sacrificial agents,the Zn_(0.94) Cr_(0.06) S exhibits a considerable CO evolution rate of 19.56μmol g^(-1) h^(-1),about 10.1 times higher than ZnS(1.94μmol g^(-1) h^(-1)).Both the performances for H_(2) evolution and CO_(2) reduction of Zn_(0.94) Cr_(0.06) S outperform most of the previously reported photocatalysts.Particularly,the Zn_(0.94) Cr_(0.06) S possesses superior stability,the photoactivity of which exhibits no noticeable deactiva-tion after six cycles’reactions.This work may shed light on the rational design and fabrication of highly efficient materials via combining individual element doping and defect engineering.展开更多
After the heavy reduction(HR)process was carried out at the solidification end of the continuous casting slab,the austenite grains were refined by recrystallization,which improved the thermoplasticity of the slab.Howe...After the heavy reduction(HR)process was carried out at the solidification end of the continuous casting slab,the austenite grains were refined by recrystallization,which improved the thermoplasticity of the slab.However,the reduction in deformation during the HR process initiated stress concentration at the slab surface,and the crack risk increased.To effectively evaluate the risk of slab surface cracks under these complex conditions,the effect of the HR on the austenite recrystallization and thermoplasticity of a microalloyed slab surface was investigated by 15-pass reduction thermal simulation according to the wide and thick slab continuous casting process.The softening fraction was introduced as a global internal variable to quantitatively analyze various recrystallized re-refined grains.After the critical strain reaches the critical strain of dynamic recrystallization,a variety of recrystallization modes alternately occur.Among them,the contribution rate of dynamic crystallization to the later refinement reaches more than 50%.The contribution rates of static recrystallization and metadynamic recrystallization to grain refinement are almost the same.The thermoplasticity of the slab surface first increases and then decreases with increasing reduction pass.It was verified by transmission electron microscopy that the main reason for the decrease in thermoplasticity is that the dislocation multiplication rate increases,resulting in a sharp increase in stress and a decrease in thermoplasticity.展开更多
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ...N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.展开更多
Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore ...Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.展开更多
The oxygen reduction/evolution reactions(ORR/OER) are a key electrode process in the development of electrochemical energy conversion and storage devices,such as metal-air batteries and reversible fuel cells.The searc...The oxygen reduction/evolution reactions(ORR/OER) are a key electrode process in the development of electrochemical energy conversion and storage devices,such as metal-air batteries and reversible fuel cells.The search for low-cost high-performance nanocarbon-based metal-free and non-precious metal bifunctional electrocatalysts for ORR/OER alternatives to the widely-used noble metal-based catalysts is a research focus.This review aims to outline the opportunities and available options for these nanocarbon-based bifunctional electrocatalysts.Through discussion of some current scientific issues,we summarize the development and breakthroughs of these electrocatalysts.Then we provide our perspectives on these issues and suggestions for some areas in the further work.We hope that this review can improve the interest in nanocarbon-based metal-free and non-precious metal bifunctional electrocatalysts for ORR/OER.展开更多
The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish red...The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish redox kinetics and the polysulfide shuttling effect.Metal–organic framework(MOF)electrocatalysts have emerged as good platforms for catalyzing SRR and SER,but their catalytic performance is challenged by poor electrical conductivity and limited chemical stability.Functionalized MOFs and their hybrids may be beneficial for stabilizing and improving the desired catalytic properties to achieve high-performance LSBs.This review provides a detailed overview of engineering principles for improving the activity,selectivity,and stability of MOFrelated electrocatalysts via composition modulation and nanostructure design as well as hybrid assembly.It presents and discusses the various advances achieved by using in situ characterization techniques,simulations,and theoretical calculations to reveal the dynamic evolution of MOF-related electrocatalysts,enabling an in-depth understanding of the catalysis mechanism at the molecular/atomic level.Lastly,prospects and possible research directions for MOF-related sulfur electrocatalysts are proposed.展开更多
The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the micro...The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was investigated.Furthermore,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric method.The findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and interconnect.This provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron coke.Accelerating the heating rate in non-isothermal gasification can enhance the reactivity of iron coke.The metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon atoms.The kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore structure.Moreover,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.展开更多
Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significan...Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase evolution.Herein,accordion-shaped Co/Co_(3)O_(4)@N-doped carbon nanosheets(Co/Co_(3)O_(4)@NC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation process.The results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial polarization.Moreover,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic diffraction.Specifically,the synthesized Co/Co_(3)O_(4)@NC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon matrix.This design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.21433003,21805064 and 21773049)National Key Research and Development Program of China(Program No.2016YFB0101207)。
文摘ABO_(3)-type perovskite oxides(e.g.,LaCoO_(3))with flexible and adjustable A-and B-sites are ideal model catalysts to unravel the relationship between the electronic structure and electrocatalytic activity(e.g.,oxygen reduction/evolution reactions,ORR/OER).It has been well understood in our recent work that the secondary metal dopant at B-site(e.g.,Mn in LaMn_(x)Co_(1-x)O_(3))can regulate the electronic structure and improve the ORR/OER activity.In this work,the Mn-Ni pairs are employed as the dual dopant in LaMn_(x)Ni_(y)Co_(z)O_(3)(x+y+z=1)catalysts toward bifunctional ORR and OER.The structure-property relationships between the triple metal B-site(Mn,Ni and Co)and the electrochemical performance are particularly investigated.Compared to the individual Mn doping(e.g.,LaMnCoO3(Mn:Co=1:3)catalyst),the dual Mn-Ni doping significantly improves the ORR mass activity@0.8 V by 1.54 times;meanwhile,the OER overpotential@10 mA cm^(-2) is reduced from 420 to 370 mV,and the OER current density at 1.55 V is increased by 2.43 times.Reasonably,the potential gap between EDRR@-1 mA cm^(-2) and EDER@10 mA cm^(-2) is achieved as only 0.76 V by using the optimal LaMn_(x)Ni_(y)Co_(z)O_(3)(x:y:z=1:2:3)catalyst.It is revealed that the dual Mn-Ni dopant efficiently optimizes electron structures of the LaMnNiCoO_(3)(1:2:3)catalyst,which not only decreases the e_(g) orbital electron number,but also modulates the O 2 p-band closer to the Femi level,accounting for the enhanced bifunctional activity.
文摘Hydrogen evolution reaction(HER)is unavoidable in many electrochemical synthesis systems,such as CO_(2)reduction,N2reduction,and H_(2)O_(2)synthesis.It makes those electrochemical reactions with multiple electron-proton transfers more complex when determining kinetics and mass transfer information.Understanding how HER competes with other electrochemical reduction reactions is crucial for both fundamental studies and system performance improvements.In this study,we employed the oxygen reduction reaction(ORR)as a model reaction to investigate HER competition on a polycrystalline-Au surface,using a rotating ring and disk electrode.It’s proved that water molecules serve as the proton source for ORR in alkaline,neutral,and even acidic electrolytes,and a 4-electron process can be achieved when the overpotential is sufficiently high.The competition from H⁺reduction becomes noticeable at the H⁺concentration higher than 2 mmol L^(–1)and intensi-fies as the H^(+)concentration increases.Based on the electrochemical results,we obtained an equivalent circuit diagram for the ORR system with competition from the H+reduction reaction,showing that these reactions occur in parallel and compete with each other.Electrochemical impedance spectroscopy measurements further confirm this argument.Additionally,we discover that the contribution of H+mass transfer to the total H^(+)reduction current is significant and comparable to the kinetic current.We believe this work will deepen our understanding of HER and its competition in electrochemical reduction systems.
基金supported by the National Natural Science Foundation of China(21832005,22072168,22002175)Major Program of the Lanzhou Institute of Chemical Physics,CAS(No.ZYFZFX-3)+1 种基金Major Science and Technology Projects in Gansu Province(22ZD6GA003)West Light Foundation of The Chinese Academy of Sciences(xbzg-zdsys-202209).
文摘Artificial carbon fixation is a promising pathway for achieving the carbon cycle and environment remediation.However,the sluggish kinetics of oxygen evolution reaction(OER)and poor selectivity of CO_(2) reduction seriously limited the overall conversion efficiencies of solar energy to chemical fuels.Herein,we demonstrated a facile and feasible strategy to rationally regulate the coordination environment and electronic structure of surface-active sites on both photoanode and cathode.More specifically,the defect engineering has been employed to reduce the coordination number of ultrathin FeNi catalysts decorated on BiVO4 photoanodes,resulting in one of the highest OER activities of 6.51 mA cm^(−2)(1.23 VRHE,AM 1.5G).Additionally,single-atom cobalt(II)phthalocyanine anchoring on the N-rich carbon substrates to increase Co–N coordination number remarkably promotes CO_(2) adsorption and activation for high selective CO production.Their integration achieved a record activity of 109.4μmol cm^(−2) h−1 for CO production with a faradaic efficiency of>90%,and an outstanding solar conversion efficiency of 5.41%has been achieved by further integrating a photovoltaic utilizing the sunlight(>500 nm).
基金financially supported by the National Natural Science Foundation of China(22478432,22108306,22178388)Taishan Scholars Program of Shandong Province(tsqn201909065)+2 种基金Shandong Provincial Natural Science Foundation(ZR2024JQ004)Innovation Fund Project for Graduate Student of China University of Petroleum(East China)the Fundamental Research Funds for the Central Universities(No.25CX04020A)。
文摘The development of single atom catalysts(SACs)with asymmetric active sites by defect regulation provides an encourage potential for oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER),but highly challenging.Herein,N-doped carbon(N-C)anchored atomically dispersed Ni-N_(3)site with proximity defects(Ni-N_(3)D)induced by Te atoms doping is reported.Benefitting from the inductive effect of proximity defect,the Ni-N_(3)D/Te-N-C catalyst performs excellent ORR and HER performance in alkaline and acid condition.Both in situ characterization and theoretical calculation reveal that the existence of proximity defect effect is conducive to lower rate-determining-step energy barrier of ORR and HER,thus accelerating the multielectron reaction kinetics.This work paves a novel strategy for constructing highactivity bifunctional SACs by defect engineering for development of sustainable energy.
基金supported by the National Natural Science Foundation of China(Nos.22078118 and 42277219)the Natural Science Foundation of Guangdong Province,China(No.2023A1515010740).
文摘A novel photocatalytic cocatalyst, MoC quantum dots integrated into N-doped carbon microflowers (MoC–NC), was synthesized, establishing a key Mo–N interfacial bond. The Mo–N bond's regulation was achieved by adjusting the pH of Mo-polydopamine precursor solutions. A composite photocatalyst, MoC–NC/CdS (MNS), was formed by in situ growth of nano-CdS on MoC–NC. The pH during synthesis, crucial for Mo–N bond formation, significantly influenced Cr(Ⅵ) reduction and H_(2) evolution performance. The optimal MNS, created at pH 9.0, demonstrated 99.2% reduction efficiency for Cr(Ⅵ) in 20 min and H_(2) evolution rate of 11.4 mmol g^(-1) h^(-1) over 3 h, outperforming Pt/CdS. Mechanistic studies and density functional theory revealed MoC–NC's role in enhancing light absorption, reaction kinetics, and electron transport, attributing to its ultra-small quantum dots and abundant Mo–N bonds.
基金financially supported by the National Natural Science Foundation of China(51902149,51674131,22305108)the Fundamental Research Funds for Public Universities in Liaoning(LJ232410140033)the Scientific Research Funding of the Education Department of Liaoning Province(JYTZD2023070,LJKFZ20220180,LJKMZ20220453)。
文摘Optimizing active sites and enhancing mass transfer capability are of paramount importance for the improvement of electrocatalyst activity.On this basis,CoFe_(2)O_(4)/CoFe nanoparticles(NPs)loaded N-doped carbon(NC)that featured with interconnected three-dimensional(3D)ordered porous hierarchies(3DOM FeCo/NC)are prepared,and its electrocatalytic activity is studied.Due to the open structure of 3D ordered macro-pores that greatly improves the mass transfer capacity of the catalytic process and enhances the utilization of active sites inside the catalyst,as well as the uniform distribution of Fe and Co bimetallic sites on the porous skeleton,3DOM FeCo/NC exhibits superior bi-functional catalytic activities for both hydrogen evolution reaction(HER)and oxygen reduction reaction(ORR).The overpotential of HER is lower than that of commercial Pt/C when performed at high current density(>235 mA cm^(-2))in1.0 M KOH,and the half-wave potential(0.896 V)of ORR in 0.1 M KOH is also superior to that of 20% commercial Pt/C and most other similar catalysts.The effective utilization and synergistic effect of CoFe_(2)O_(4)and CoFe hetero-metallic sites remarkably enhance the electrocatalytic activity.Furthermore,3DOM FeCo/NC is assembled as an air electrode in Zn-air battery,and exhibits satisfactory maximum power density,open-circuit voltage,and charge/discharge stability over benchmark Pt/C+IrO_(2).This work contributes new insights into the design of transition-metal-based multifunctional catalysts,and has great potential for energy conversion and storage.
基金supported by the National Natural Science Foundation of China(Grant No.52072274 and 52104309)the Knowledge Innovation Project of Wuhan,China(2023020201010131).
文摘Owing to their multi-elemental compositions and unique high-entropy mixing states,high-entropy alloy(HEA)nanoparticles(NPs)displaying tunable activities and enhanced stabilities thus have become a rapidly growing area of research in recent years.However,the integration of multiple elements into HEA NPs at the nanoscale remains a formidable challenge,especially when it comes to the precise control of particle size,elemental composition and content.Herein,a simple and universal high-energy laser assisted reduction approach is presented,which achieves the preparation of HEA NPs with a wide range of multi-component,controllable particle sizes and constitution on different substrates within seconds.Laser on carbon nanofibers induced momentary high-temperature annealing(>2000 K and ramping/cooling rates>10^(5)K s^(-1))to successfully decorate HEA NPs up to twenty elements with excellent compatibility for large-scale synthesis(20.0×20.0 cm^(2)of carbon cloth).The IrPdPtRhRu exhibit robust electrocatalytic hydrogen evolution reaction(HER)activities and low overpotentials of 16,28,and 12 mV at a current density of 10 mA cm^(-2)in alkaline(1.0 M KOH),alkaline simulated seawater(1.0 M KOH+0.5 M NaCl),and acidic(0.5 M H_(2)SO_(4))electrolytes,respectively,and excellent stability(7 days and>2000 cycles)at the alkaline HER.
基金financial support from the National Key Research and Development Program of China(No.2021YFB3702101)National Natural Science Foundation of China(No.52130107,52071038)+5 种基金Fundamental Research Funds for the Central Universities(No.2023CDJXY-018)the“111”Project(No.B16007)by the Ministry of Education and the State Administration of Foreign Experts Affairs of Chinasupport to the Norwegian Micro-and Nano-Fabrication Facility,NorFab(No.295864)the Norwegian Laboratory for Mineral and Materials Characterization,MiMaC(No.269842/F50)the RCN INRPART project IntMat(No.309724)the Center for Research based Innovation SFI PhysMet(No.309584).
文摘Mg-3Gd(wt.%)samples with different initial grain sizes were prepared to evaluate the grain size effect on microstructural evolution during cold rolling and subsequent annealing hardening response.The deformation behavior and mechanical response of the as-rolled and annealed samples were systematically investigated by a combination of electron microscopy and microhardness characterization.The results show that the twinning activities were highly suppressed in the fine-grained samples during rolling.Upon increasing the rolling reduction to 40%,ultra-fine grain structures with a volume fraction of∼28%were formed due to the activation of multiple slip systems.Conversely,twinning dominated the early stages of deformation in the coarse-grained samples.After a 10%rolling reduction,numerous twins with a volume fraction of∼23%were formed.Further increasing the rolling reduction to 40%,high-density dislocations were activated and twin structures with a volume fraction of∼36%were formed.The annealing hardening response of deformed samples was effectively enhanced compared to that of the non-deformed samples,which was attributed to the enhanced Gd segregation along grain boundaries,twin boundaries and dislocation cores.Moreover,the grain size and rolling reduction were found to affect the microstructure evolution during annealing,resulting in a notable difference in the annealing hardening response of Mg-3Gd alloy between samples of different grain sizes deformed to different strains.These findings highlight the crucial importance of microstructural and processing parameters in the design of high-strength,cost-effective Mg alloys.
基金supported by the National Key Technologies R&D Program of China(Nos.2022YFE0114800 and 2021YFA1502100)National Natural Science Foundation of China(Nos.22075047,22032002,U1905214,21961142019)the 111 Project(Nos.D16008)。
文摘Solar-induced water oxidation reaction(WOR)for oxygen evolution is a critical step in the transformation of Earth's atmosphere from a reducing to an oxidation one during its primordial stages.WOR is also associated with important reduction reactions,such as oxygen reduction reaction(ORR),which leads to the production of hydrogen peroxide(H_(2)O_(2)).These transitions are instrumental in the emergence and evolution of life.In this study,transition metals were loaded onto nitrogen-doped carbon(NDC)prepared under the primitive Earth's atmospheric conditions.These metal-loaded NDC samples were found to catalyze both WOR and ORR under light illumination.The chemical pathways initiated by the pristine and metal-loaded NDC were investigated.This study provides valuable insights into potential mechanisms relevant to the early evolution of our planet.
基金support of the National Natural Science Foundation of China(52074080,52004001,and 51574002).
文摘Against the background of“carbon peak and carbon neutrality,”it is of great practical significance to develop non-blast furnace ironmaking technology for the sustainable development of steel industry.Carbon-bearing iron ore pellet is an innovative burden of direct reduction ironmaking due to its excellent self-reducing property,and the thermal strength of pellet is a crucial metallurgical property that affects its wide application.The carbon-bearing iron ore pellet without binders(CIPWB)was prepared using iron concentrate and anthracite,and the effects of reducing agent addition amount,size of pellet,reduction temperature and time on the thermal compressive strength of CIPWB during the reduction process were studied.Simultaneously,the mechanism of the thermal strength evolution of CIPWB was revealed.The results showed that during the low-temperature reduction process(300-500℃),the thermal compressive strength of CIPWB linearly increases with increasing the size of pellet,while it gradually decreases with increasing the anthracite ratio.When the CIPWB with 8%anthracite is reduced at 300℃for 60 min,the thermal strength of pellet is enhanced from 13.24 to 31.88 N as the size of pellet increases from 8.04 to 12.78 mm.Meanwhile,as the temperature is 500℃,with increasing the anthracite ratio from 2%to 8%,the thermal compressive strength of pellet under reduction for 60 min remarkably decreases from 41.47 to 8.94 N.Furthermore,in the high-temperature reduction process(600-1150℃),the thermal compressive strength of CIPWB firstly increases and then reduces with increasing the temperature,while it as well as the temperature corresponding to the maximum strength decreases with increasing the anthracite ratio.With adding 18%anthracite,the thermal compressive strength of pellet reaches the maximum value at 800℃,namely 35.00 N,and obtains the minimum value at 1050℃,namely 8.60 N.The thermal compressive strength of CIPWB significantly depends on the temperature,reducing agent dosage,and pellet size.
基金the National Key Research and Development Program of China(No.2018YFE0306103)the National Natural Science Foundation of China(No.52071050)+1 种基金the Science and Technology Innovation Project of Ningbo,China(No.2021Z032)the Program of China Scholarships Council(No.202106060148).
文摘The Cu/1010 steel bimetal laminated composites(BLCs)were rolled to different thicknesses to investigate the effect of rolling direction and reduction on the microstructure evolution and mechanical properties.The difference of mechanical properties between the Cu and 1010 steel causes different thickness reductions,percentage spread,and cladding ratios.The formation of strong texture induces larger strength of the rolled samples,and as the volume fraction of 1010 steel is larger in Route-A,its strength is consistently greater than that in Route-B.The obstruction of interface to crystal and dislocation slip results in the formation of interface distortion,inducing dislocation density gradient when the rolling reduction is low in Route-A.The slip planes of the Cu and 1010 steel are more prone to suffer the normal strain,while the shear strain of other crystal planes is obviously larger than the normal strain under rolling load near the interface.
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 National Natural Sci-ence Foundation of China(No.52002158)the Natural Science Foundation of Jiangxi Province(Nos.20204BCJL23039,20192ACBL21027)The authors would like to thank Prince Sultan University for computational support and Wenjuan Li from Shiyan-jia Lab(www.shiyanjia.com)for the XPS analysis.
文摘Driven by endless solar energy,photocatalytic H2 evolution from water splitting and CO_(2) conversion to hydrocarbon fuels over semiconductor photocatalysts are of great potential to simultaneously settle the greenhouse effect and energy shortage.Herein,Cr-doped zinc sulfide(ZnS)with accompanying sulphur vacancies(Vs)photocatalytic materials is developed by a facile hydrothermal method.The Cr dopants centralize photoinduced holes and Vs trap electrons,forming a synergistic effect for accelerating charge separation and transfer.The reaction energy barrier for both H2 evolution and CO_(2) reduction has been optimized.Therefore,in the absence of a cocatalyst,the optimal catalyst(Zn_(0.94) Cr_(0.06) S)achieves an out-standing H_(2) evolution activity of 20.3 mmol g^(-1) h^(-1),which is approximately 2.9 times higher than 6.9 mmol g^(-1) h^(-1) for pristine ZnS.In addition,in the gas-solid reaction system without co-catalysts or sacrificial agents,the Zn_(0.94) Cr_(0.06) S exhibits a considerable CO evolution rate of 19.56μmol g^(-1) h^(-1),about 10.1 times higher than ZnS(1.94μmol g^(-1) h^(-1)).Both the performances for H_(2) evolution and CO_(2) reduction of Zn_(0.94) Cr_(0.06) S outperform most of the previously reported photocatalysts.Particularly,the Zn_(0.94) Cr_(0.06) S possesses superior stability,the photoactivity of which exhibits no noticeable deactiva-tion after six cycles’reactions.This work may shed light on the rational design and fabrication of highly efficient materials via combining individual element doping and defect engineering.
基金supported by the National Natural Science Foundation of China(51974078)the Applied Basic Research Program of Liaoning Province(2022JH2/101300002,2022JH25/10200003)the Applied Basic Research Program of Liaoning Province,and the State Key Laboratory of Metal Material for Marine Equipment and Application Project(SKLMEA-K202204).
文摘After the heavy reduction(HR)process was carried out at the solidification end of the continuous casting slab,the austenite grains were refined by recrystallization,which improved the thermoplasticity of the slab.However,the reduction in deformation during the HR process initiated stress concentration at the slab surface,and the crack risk increased.To effectively evaluate the risk of slab surface cracks under these complex conditions,the effect of the HR on the austenite recrystallization and thermoplasticity of a microalloyed slab surface was investigated by 15-pass reduction thermal simulation according to the wide and thick slab continuous casting process.The softening fraction was introduced as a global internal variable to quantitatively analyze various recrystallized re-refined grains.After the critical strain reaches the critical strain of dynamic recrystallization,a variety of recrystallization modes alternately occur.Among them,the contribution rate of dynamic crystallization to the later refinement reaches more than 50%.The contribution rates of static recrystallization and metadynamic recrystallization to grain refinement are almost the same.The thermoplasticity of the slab surface first increases and then decreases with increasing reduction pass.It was verified by transmission electron microscopy that the main reason for the decrease in thermoplasticity is that the dislocation multiplication rate increases,resulting in a sharp increase in stress and a decrease in thermoplasticity.
基金We acknowledge the National Natural Science Foundation of China(No.22275134)for fi nancial support.
文摘N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.
基金the financial support from the Postdoctoral Science Foundation of China(2022M720131)Spring Sunshine Collaborative Research Project of the Ministry of Education(202201660)+3 种基金Youth Project of Gansu Natural Science Foundation(22JR5RA542)General Project of Gansu Philosophy and Social Science Foundation(2022YB014)National Natural Science Foundation of China(72034003,72243006,and 71874074)Fundamental Research Funds for the Central Universities(2023lzdxjbkyzx008,lzujbky-2021-sp72)。
文摘Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.
基金the financial support provided by the National Natural Science Foundation of China(Grant Nos.51932005 and 21773269)the Joint Research Fund LiaoningShenyang National Laboratory for Materials Science(Grant No.20180510047)Liao Ning Revitalization Talents Program(XLYC1807175)。
文摘The oxygen reduction/evolution reactions(ORR/OER) are a key electrode process in the development of electrochemical energy conversion and storage devices,such as metal-air batteries and reversible fuel cells.The search for low-cost high-performance nanocarbon-based metal-free and non-precious metal bifunctional electrocatalysts for ORR/OER alternatives to the widely-used noble metal-based catalysts is a research focus.This review aims to outline the opportunities and available options for these nanocarbon-based bifunctional electrocatalysts.Through discussion of some current scientific issues,we summarize the development and breakthroughs of these electrocatalysts.Then we provide our perspectives on these issues and suggestions for some areas in the further work.We hope that this review can improve the interest in nanocarbon-based metal-free and non-precious metal bifunctional electrocatalysts for ORR/OER.
基金supported by the National Key R&D Program of China(2021YFB3800300)Beijing Outstanding Young Scientists Program(BJJWZYJH01201910007023)Yuanguang Scholars Program,Hebei University of Technology(282022554).
文摘The electrocatalytic sulfur reduction reaction(SRR)and sulfur evolution reaction(SER),two fundamental multistep conversion processes in lithium–sulfur batteries(LSBs),are root-cause solutions to overcome sluggish redox kinetics and the polysulfide shuttling effect.Metal–organic framework(MOF)electrocatalysts have emerged as good platforms for catalyzing SRR and SER,but their catalytic performance is challenged by poor electrical conductivity and limited chemical stability.Functionalized MOFs and their hybrids may be beneficial for stabilizing and improving the desired catalytic properties to achieve high-performance LSBs.This review provides a detailed overview of engineering principles for improving the activity,selectivity,and stability of MOFrelated electrocatalysts via composition modulation and nanostructure design as well as hybrid assembly.It presents and discusses the various advances achieved by using in situ characterization techniques,simulations,and theoretical calculations to reveal the dynamic evolution of MOF-related electrocatalysts,enabling an in-depth understanding of the catalysis mechanism at the molecular/atomic level.Lastly,prospects and possible research directions for MOF-related sulfur electrocatalysts are proposed.
基金financially supported by the National Science Foundation of China(Nos.51974212 and 52274316)the China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202116)+1 种基金the Science and Technology Major Project of Wuhan(No.2023020302020572)the Foundation of Key Laboratory for Ferrous Metallurgy and Resources Utilization of Ministry of Education(No.FMRUlab23-04)。
文摘The utilization of iron coke provides a green pathway for low-carbon ironmaking.To uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was investigated.Furthermore,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric method.The findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and interconnect.This provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron coke.Accelerating the heating rate in non-isothermal gasification can enhance the reactivity of iron coke.The metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon atoms.The kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore structure.Moreover,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.
基金financially supported by the National Natural Science Foundation of China(52373271)Science,Technology and Innovation Commission of Shenzhen Municipality under Grant(KCXFZ20201221173004012)+1 种基金National Key Research and Development Program of Shaanxi Province(No.2023-YBNY-271)Open Testing Foundation of the Analytical&Testing Center of Northwestern Polytechnical University(2023T019).
文摘Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase evolution.Herein,accordion-shaped Co/Co_(3)O_(4)@N-doped carbon nanosheets(Co/Co_(3)O_(4)@NC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation process.The results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial polarization.Moreover,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic diffraction.Specifically,the synthesized Co/Co_(3)O_(4)@NC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon matrix.This design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.
