The hydrogen-based reduction and electric smelting technology is a green and low-carbon process for treating low-grade ore and complex symbiotic iron ore.In this study,the hydrogen-based reduction of boron-bearing iro...The hydrogen-based reduction and electric smelting technology is a green and low-carbon process for treating low-grade ore and complex symbiotic iron ore.In this study,the hydrogen-based reduction of boron-bearing iron concentrate and the low-temperature separation compared with the high-temperature melting separation of slag and iron from a boron-bearing iron concentrate were studied.The metallization rate of the boron-bearing iron concentrate reached 99.63%after hydrogen-based reduction at 1050℃,and the metallic iron was interwoven with olivine(Mg_(2)SiO_(4))in the reduced ore.In addition,the high-temperature melting separation of iron and slag could be accomplished at 1550℃for 60 min,where boron was mainly distributed in the form of a glass phase in the slag with a mass fraction of B_(2)O_(3)of 22.69%,and 0.35%of boron(mass fraction)was melted into liquid iron.By contrast,iron and slag were efficiently separated at a lower temperature(1300℃)for 10 min and enhanced by super-gravity.Almost all the boron content was enriched into a suanite phase in the slag with a considerably high mass fraction of B_(2)O_(3)(35.61%)and a high recovery ratio(99.37%),and the mass fraction of boron decreased to 0.15%in iron.Compared with high-temperature melting separation,low-temperature separation combined with hydrogen-based reduction greatly improved the enrichment of boron in slag and prevented the melting of boron into iron.展开更多
The steel industry’s transition to hydrogen-based ironmaking necessitates a deeper understanding of magnetite ore reduction,a crucial yet underexplored pathway for decarbonization.This study systematically investigat...The steel industry’s transition to hydrogen-based ironmaking necessitates a deeper understanding of magnetite ore reduction,a crucial yet underexplored pathway for decarbonization.This study systematically investigates the combined effects of particle size and gangue composition on hydrogen-based reduction behavior of four industrial magnetite ore concentrates with varying CaO and MgO con-tents.Thermogravimetric analysis at 973 K,interrupted reduction experiments,and post-reduction characterization steps are used to eval-uate reduction extent and phase transformations across different particle size fractions and bulk ores.The finer fractions generally exhibit faster and more complete reduction.However,this trend is overridden by gangue effects in certain ores.Magnetite ores with MgO as gangue tend to form magnesio-wustite solid solution(Mg,Fe)O during reduction,resulting in dense microstructures that impede hydrogen diffusion and limit reduction progress.In contrast,magnetite ores with CaO as gangue facilitate the formation of intermediate calcium fer-rites,which promote porous morphology and enhanced reducibility.Notably,even the finer particles of ore containing MgO show a lower reduction degree than the coarser particles of the ore containing CaO as gangue.This highlights the dominant role of gangue composition in governing reduction kinetics,intermediate phase formation and final product morphology.These findings contribute to the growing knowledge necessary to enable fossil-free ironmaking by emphasizing the importance of considering both granulometric characteristics and heterogeneity when evaluating magnetite ores for hydrogen-based reduction.展开更多
Iron tailings are a common solid waste resource,posing serious environmental and spatial challenges.This study proposed a novel hydrogen-based reduction roasting(HRR)technology for the processing of iron tailings usin...Iron tailings are a common solid waste resource,posing serious environmental and spatial challenges.This study proposed a novel hydrogen-based reduction roasting(HRR)technology for the processing of iron tailings using a combined beneficiation and metallurgy approach.Pilot-cale experiment results indicated that under the gas composition of CO:H_(2)=1:3,and optimal roasting conditions at a reduction temperature of 520℃,the majority of weakly magnetic hematite transforms into strongly magnetic magnetite during the reduction process.Combining roasting products with a magnetic separation-grinding-magnetic selection process yields a final iron concentrate with a grade of 56.68%iron and a recovery rate of 86.54%.Theoretical calculations suggested the annual production value can reach 29.7 million USD and a reduction of 20.79 tons of CO_(2) emissions per year.This highlights that the use of HRR in conjunction with traditional beneficiation processes can effectively achieve comprehensive utilization of iron tailings,thereby reducing environmental impact.展开更多
The novel process of hydrogen-based shaft furnaces(HSFs)has attracted considerable attention because of their significant reduction of CO_(2)emissions.In this study,the interaction of H_(2)and CO with Fe_(tet1)-and Fe...The novel process of hydrogen-based shaft furnaces(HSFs)has attracted considerable attention because of their significant reduction of CO_(2)emissions.In this study,the interaction of H_(2)and CO with Fe_(tet1)-and Fe_(oct2)-terminated Fe_(3)O_(4)(111)surfaces under HSF conditions,including their adsorption and reduction behaviors,was investigated using the density functional theory method.The results indicated that the H_(2)molecule adsorbed onto the Fe_(tet1)-terminated surface with an adsorption energy(AE)of-1.36 eV,whereas the CO molecule preferentially adsorbed on the Fe_(oct2)-terminated surface with an AE of-1.56 eV.Both H_(2)and CO can readily undergo reduction on the Fe_(tet1)-terminated surface(corresponding to energy barriers of 0.83 eV and 2.23 eV,respectively),but kinetically the reaction of H2is more favorable than that of CO.With regard to the thermodynamics at 400-1400 K,the H_(2)was easy to be adsorbed,while the CO would like to react on the Fe_(tet1)-terminated surface.These thermodynamically tendencies were reversed on the Fe_(oct2)-terminated surface.The thermodynamic disadvantage of the reaction of H_(2)on the Fe_(tet1)-terminated surface was offset by an increase in the temperature.Furthermore,the adsorption of H2 and CO on the Fe_(tet1)-terminated surface was competitive,whereas the adsorption of them on the Fe_(oct2)-terminated surface was synergistic.Therefore,iron ores with a higher proportion of Fe_(tet1)-terminated surface can be applied for the HSF process.In conjunction with the increases in the reduction temperature and the ratio of H_(2)in the reducing gas would promote efficient HSF smelting.These observations provide effective guidance for optimizing the practical operation parameters and advancing the development of the HSF process.展开更多
The sticking behavior of pellets affects the continuity of production in hydrogen-based shaft furnace.The coupling influences of V_(2)O_(5) and reduction temperature on reduction sticking behavior and mechanism evolut...The sticking behavior of pellets affects the continuity of production in hydrogen-based shaft furnace.The coupling influences of V_(2)O_(5) and reduction temperature on reduction sticking behavior and mechanism evolution of pellets under hydrogen atmosphere are investigated.The increase in V_(2)O_(5) addition aggravated the reduction sticking behavior,which is attributed to the combined functions of the development of unique interwoven structure in the metallic iron interconnections at the reduction sticking interface and the deterioration of reduction swelling behavior of pellets.In addition,the strength of metallic iron interconnections enhanced and reduction sticking behavior aggravated with the increase in reduction temperature.Importantly,compared to other reduction temperatures,the reduction sticking behavior of pellets was most significantly aggravated with the increase in V_(2)O_(5) addition at 1000℃.And the values of sticking index increased from 10.22%to 15.36% as the V_(2)O_(5) addition increased from 0 to 1.00 wt.%at 1000℃.展开更多
Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model versi...Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model version 6 with a machine-learning-integrated four-mode version of the Modal Aerosol Module, we quantify global BC aging responses to emission reductions for 2011–2018 and for 2050 and 2100 under carbon neutrality. During 2011–18, global trends in BC aging degree(mass ratio of coatings to BC, R_(BC)) exhibited marked regional disparities, with a significant increase in China(5.4% yr^(-1)), which contrasts with minimal changes in the USA, Europe, and India. The divergence is attributed to opposing trends in secondary organic aerosol(SOA) and sulfate coatings, driven by regional changes in the emission ratios of corresponding coating precursors to BC(volatile organic compounds-VOCs/BC and SO_(2)/BC). Projections under carbon neutrality reveal that R_(BC) will increase globally by 47%(118%) in 2050(2100), with strong convergent increases expected across major source regions. The R_(BC) increase, primarily driven by enhanced SOA coatings due to sharper BC reductions relative to VOCs, will enhance the global BC mass absorption cross-section(MAC) by 11%(17%) in 2050(2100).Consequently, although the global BC burden will decline sharply by 60%(76%), the enhanced MAC partially offsets the magnitude of the decline in the BC direct radiative effect, resulting in the moderation of global BC DRE decreases to 88%(92%) of the BC burden reductions in 2050(2100). This study highlights the globally enhanced BC aging and light absorption capacity under carbon neutrality, thereby partly offsetting the impact of BC direct emission reductions on future changes in BC radiative effects globally.展开更多
In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride ...In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride molten salt as the reaction medium at 923 K.The study assessed the effects of lithium thermochemical reduction and electrolytic reduction of ZnO.The volatilization behavior of metal oxides in molten salts,the equivalent of a reducing agent,reduction time,amount of molten salt,stirring time,and the method of reduction feed were investigated for their impacts on the reduction yield and product composition.X-ray powder diffraction(XRD)analysis of the products showed that lithium reduction of ZnO not only produced metallic Zn but also formed a LiZn alloy.Electrolytic reduction can be used to obtain the metallic Zn product by controlling the potential below-2.2 V(vs Ag/Ag^(+)).Moreover,sintered oxides and higher electrode potentials could enhance the efficiency of electrolysis.Under the optimal reaction conditions determined experimentally,the lithium reduction experiment achieved a yield of 77.2%after a 12-h test,and the electrolytic reduction reached a yield of 85.4%after a 6-h test.展开更多
A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affordi...A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affording aldehydes in isolated yields of up to 88%with broad functional group tolerance,including cyano,halogen,alkenyl,ketone,and ester groups.Moreover,the method enables gram-scale aldehyde synthesis and shows high efficiency in reducing in situ generated acyl chlorides,thereby enhancing its synthetic practicality.展开更多
This paper presents an efficient model reduction technique for linear time-varying systems based on shifted Legendre polynomials.The approach constructs approximate low-rank decomposition factors of finite-time Gramia...This paper presents an efficient model reduction technique for linear time-varying systems based on shifted Legendre polynomials.The approach constructs approximate low-rank decomposition factors of finite-time Gramians directly from the expansion coefficients of impulse responses.Leveraging these factors,we develop two model reduction algorithms that integrate the low-rank square root method with dominant subspace projection.Our method is computationally efficient and flexible,requiring only a few matrix-vector operations and a singular value decomposition of a low-dimensional matrix,thereby avoiding the need to solve differential Lyapunov equations.Numerical experiments confirm the effectiveness of the proposed approach.展开更多
This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the correspo...This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the corresponding ester[Fe_(2)(CO)_(6)(μ‑tedt)](2),where tedt=SCH_(2)CH(CH_(2)OOC(5‑C_(3)HNSCH_(3)))S.Further reactions of complex 2 with tri(ptolyl)phosphine(tp)or tris(4‑fluorophenyl)phosphine(fp)gave the phosphine‑substituted derivatives[Fe_(2)(CO)_(5)(tp)(μ‑tedt)](3)and[Fe_(2)(CO)_(5)(fp)(μ‑tedt)](4).The structures of the newly prepared complexes were elucidated by elemental analysis,NMR,IR,and X‑ray photoelectron spectroscopy.Moreover,single‑crystal X‑ray diffraction analysis confirmed their molecular structures,showing that they contain a di‑iron core ligated by a bridged dithiolate bearing a thiazole moiety and terminal carbonyls.The electrochemical and electrocatalytic proton reduction were probed by cyclic voltammetry,revealing that three complexes can catalyze the reduction of protons to H_(2) under the electrochemical conditions.For comparison,complex 4 possessed the best efficiency with a turnover frequency of 23.5 s^(-1)at 10 mmol·L^(-1)HOAc concentration.In addition,the fungicidal activity of these complexes was also investigated in this study.CCDC:2477511,2;2477512,3;2477513,4.展开更多
Experts and officials shared their insights on poverty reduction cooperation and sustainable development during the 2025 International Seminar on Global Poverty Reduction Partnerships.
Hexavalent chromium(Cr(Ⅵ)) is an extremely toxic pollutant in aqueous environment.Chemical reduction is the most employed method in decontamination of Cr(Ⅵ).However,the chemical reduction was usually conducted in ac...Hexavalent chromium(Cr(Ⅵ)) is an extremely toxic pollutant in aqueous environment.Chemical reduction is the most employed method in decontamination of Cr(Ⅵ).However,the chemical reduction was usually conducted in acidic media,resulting in considerable waste of acid reagents and the following neutralizing agents.In this study,kinetics and mechanisms of Cr(Ⅵ) reduction by sulfite in alkaline conditions(pH:7-10) were investigated.It reveals that Cr(Ⅵ) reduction follows pseudo-zero-order kinetics,where the rate constants increased markedly with an in situ irradiation of Far-UVC(UV_(222)).Decreasing pH levels slightly favored the reduction.Iodide ion displayed a notable accelerating effect,which not only save the energy input but also minimize the reductant usage.Chloride,sulfate,and carbonate ions exhibit little effect on the reduction,whereas nitrate and nitrite ions,dissolved oxygen as well as Cu(Ⅱ) suppressed the reduction significantly,implying that hydrated electrons produced by UV222 played the most important role in the reaction.Compared to the UV254/sulfite/iodide process,UV222/sulfite/iodide demonstrates clear advantages in the reduction kinetics and the sulfite utilization efficiency,underscoring its potential for effective Cr(Ⅵ) remediation in various environmental settings.展开更多
Objective: To investigate the therapeutic advantages of closed reduction and Kirschner wire fixation versus open reduction and plate fixation in patients with hand surgery fractures. Methods: The sample was collected ...Objective: To investigate the therapeutic advantages of closed reduction and Kirschner wire fixation versus open reduction and plate fixation in patients with hand surgery fractures. Methods: The sample was collected from May 2021 to May 2025, consisting of 80 patients with hand surgery fractures. These patients were randomly divided into two groups using the red and blue ball method: the plate fixation group (40 cases, treated with open reduction and plate fixation) and the Kirschner wire fixation group (40 cases, treated with closed reduction and Kirschner wire fixation). The therapeutic effects between the two groups were randomly compared. Results: The Kirschner wire fixation group outperformed the plate fixation group in all indicators except for hand function scores (p < 0.05). There was no statistically significant difference in hand function scores between the two groups (p > 0.05). Conclusion: Compared with open reduction and plate fixation, closed reduction and Kirschner wire fixation for patients with hand surgery fractures achieves a more pronounced therapeutic effect, with advantages such as less trauma, shorter operation time, less bleeding, and a lower incidence of complications. It is suitable for hand surgery fractures with good stability. Open reduction and plate internal fixation have greater advantages in complex fractures and cases requiring high stability, and are worthy of promotion and application.展开更多
The energy transition inspired by carbon neutrality targets and the increasing threat of extreme events raise multi-objective development requirements for power systems.This paper proposes a multi-objective resource a...The energy transition inspired by carbon neutrality targets and the increasing threat of extreme events raise multi-objective development requirements for power systems.This paper proposes a multi-objective resource allocation model to determine the type,number and location of flexible resources to increase the values of resilience,carbon reduction and renewable energy consumption.To evaluate the values of resilience,a restoration model for transmission systems is established that considers the coordination of fossil-fuel generators,energy storage systems(ESSs)and renewable energy generators in building restoration paths.The collaborative power-carbon-tradable green certificate(TGC)market model is then applied to evaluate the resource values in terms of carbon reduction and renewable energy consumption.Finally,the model is formulated as a mixed-integer linear programming(MILP)with a nonconvex feasible domain,and the normalized normal constraint(NNC)method is applied to obtain approximate Pareto frontiers for decision makers.Case studies validate the effectiveness of the proposed model in improving multi-factor values and analyze the impact of resource regulation capacity on values of restoration and carbon reduction.展开更多
Electrochemical nitrate reduction reaction(NO_(3)RR)is a sustainable strategy to treat wastewater and produce ammonia.However,it is still a challenge to prepare electrocatalysts with high activity and selectivity.Here...Electrochemical nitrate reduction reaction(NO_(3)RR)is a sustainable strategy to treat wastewater and produce ammonia.However,it is still a challenge to prepare electrocatalysts with high activity and selectivity.Herein,the CuO_(x) nanowires supported Ru nanoclusters(Ru-CuO_(x))were fabricated via a three-step procedure for efficient nitrate conversion and highly selective ammonia generation.The prepared RuCuO_(x) shows a high ammonia yield rate of 2286.5μg h^(-1) cm^(-2) at-0.7 V vs.RHE and Faradaic efficiency(FE)of 80.1%at-0.4 V vs.RHE.Additionally,the nitrate conversion rate exceeds 90%at the potential range from-0.2 to-0.7 V vs.RHE,and the ammonia selectivity can reach 97.7%at-0.7 V vs.RHE in100 mg L^(-1) NaNO_(3) solution.The systematic characterizations clarify that the introduction of Ru not only regulates the electronic structure of CuO_(x) and accelerates the reconstruction of CuO_(x) to Cu but also promotes H2O dissociation to generate active hydrogen.Moreover.in-situ Raman spectroscopy reveals that the formed Ru-Cu is considered the actual active species during the NO_(3)RR.Density functional theory(DFT)calculations further prove that the obtained Ru-Cu facilitates the adsorption of nitrate and lowers the Gibbs free energy of the rate-determining step,thus improving the NO_(3)RR performance.展开更多
In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry bet...In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed.Herein,two novel imide-linked 1D COFs with phthalocyanine building blocks,namely NiPc-CZDM-COF and NiPc-CZDL-COF,were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II)(NiPc(COOH)_(8))with 9H-carbazole-3,6-diamine(CZDM)and 4,4′-(9H-carbazole-3,6-diyl)dianiline(CZDL),respectively.Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Due to their high ratio of exposed active centers on the edge sites of porous ribbons,both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0%and 7.5% according to the electrochemical measurement,resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%.In particular,NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH_(3) partial current density of−246 mA/cm^(2),ammonia yield rate of 19.5 mg cm^(−2) h^(−1),and turnover frequency of 5.8 s^(−1) at−1.2 V in an H-type cell associated with its higher conductivity.This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.展开更多
The demand for ^(238)Pu (nuclear battery heat source) drives the separation of its precursor,^(237)Np,from spent nuclear fuel (SNF).However,the co-existence of multi-valence states (Ⅳ/Ⅴ/Ⅵ) of Np and similar redox b...The demand for ^(238)Pu (nuclear battery heat source) drives the separation of its precursor,^(237)Np,from spent nuclear fuel (SNF).However,the co-existence of multi-valence states (Ⅳ/Ⅴ/Ⅵ) of Np and similar redox behavior with Pu(Ⅳ) hinder the effective separation of Np.N-Butyraldehyde (n-C_(3)H_(7)CHO) selectively reduces Np(Ⅵ) to Np(Ⅴ) without reducing Pu(Ⅳ).Herein,we examined the reduction mechanisms of Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO using relativistic density functional theory.Based on the results of the potential energy profiles,the reductions of both Np(Ⅵ) and Pu(Ⅳ) by n-C_(3)H_(7)CHO are thermodynamically feasible,whereas only the former is kinetically achievable.It uncovers that n-C_(3)H_(7)CHO can only reduce Np(Ⅵ) to Np(Ⅴ) owing to kinetically controlled selective reduction.The analyses of spin density and bond distance indicate that the reduction nature for the first Np(Ⅵ)/Pu(Ⅳ) belongs to hydrogen atom transfer,whereas that for the second one involves outer-sphere electron transfer.Localized molecular orbitals (LMOs) analysis discloses the bonding evolution during the reduction process of Np(Ⅵ)/Pu(Ⅳ).This study elucidates the reason behind the kinetically controlled selective reduction of Np(Ⅵ)/Pu(Ⅳ) by nC3H7CHO at the molecular level and offers in-depth perspectives on the isolation of specific metal ions from the view of kinetic control.展开更多
Controllable synthesis of ultrathin metallene nanosheets and rational design of their spatial arrangement in favor of electrochemical catalysis are critical for their renewable energy applications.Here,a biomimetic de...Controllable synthesis of ultrathin metallene nanosheets and rational design of their spatial arrangement in favor of electrochemical catalysis are critical for their renewable energy applications.Here,a biomimetic design of“Trunk-Branch-Leaf”strategy is proposed to prepare the ultrathin edge-riched Zn-ene“leaves”with a thickness of~2.5 nm,adjacent Zn-ene cross-linked with each other,which are supported by copper nanoneedle“branches”on copper mesh“trunks,”named as Zn-ene/Cu-CM.The resulting superstructure enables the formation of an interconnected network and multiple channels,which can be used as an electrocatalytic CO_(2) reduction reaction(CO_(2)RR)electrode to allow a fast charge and mass transfer as well as a large electrolyte reservoir.By virtue of the distinctive structure,the obtained Zn-ene/Cu-CM electrode exhibits excellent selectivity and activity toward CO production with a maximum Faradaic efficiency of 91.3%and incredible partial current density up to 40 mA cm^(−2),outperforming most of the state-of-the-art Zn-based electrodes for CO_(2) reduction.The phenolphthalein color probe combined with in situ attenuated total reflection-infrared spectroscopy uncovered the formation of the localized pseudo-alkaline microenvironment at the interface of the Zn-ene/Cu-CM electrode.Theoretical calculations confirmed that the localized pH as the origin is responsible for the adsorption of CO_(2) at the interface and the generation of *COOH and *CO intermediates.This study offers valuable insights into developing efficient electrodes through synergistic regulation of reaction microenvironments and active sites,thereby facilitating the electrolysis of practical CO_(2) conversion.展开更多
Phosphorus tends to migrate into metallic iron during the direct reduction of high-phosphorus oolitic iron ore,leading to undesirable phosphorus enrichment in metallic iron.However,the underlying reduction and migrati...Phosphorus tends to migrate into metallic iron during the direct reduction of high-phosphorus oolitic iron ore,leading to undesirable phosphorus enrichment in metallic iron.However,the underlying reduction and migration mechanisms remain poorly understood.Phosphorus behavior during coal-based reduction was systematically investigated through theoretical modeling and experimental approaches.Thermodynamic analysis revealed that the carbon reduction of solid Ca_(3)(PO_(4))_(2)to gaseous P_(2)requires temperatures exceeding 1400℃.Notably,this threshold significantly decreases to 1130.5℃in the presence of SiO_(2)and Al_(2)O_(3).Further investigations demonstrated that Ca_(3)(PO_(4))_(2)co-reduces with Fe_(x)O_(γ)in the presence of SiO_(2)-Al_(2)O_(3)-Fe_(x)O_(γ),forming Fe_(3)P(instead of gaseous P_(2))at a markedly lower temperature of 778.7℃.Mechanistic studies indicate that the inherent thermal stability of Ca_(3)(PO_(4))_(2)inhibits the generation of reactive[P_(2)O_(5)].However,SiO_(2)-Al_(2)O_(3)coexistence destabilizes Ca_(3)(PO_(4))_(2)while exponentially enhancing[P_(2)O_(5)]activity.This synergistic effect dramatically promotes the phosphorus mineral reduction.Characterization confirmed that Ca_(3)(PO_(4))_(2)migrated into the slag phase(4FeO·Al_(2)O_(3)·3SiO_(2)·CaO·P_(2)O_(5)).Subsequently,the reactive P_(2)O_(5)in slag is reduced with metallic iron to form Fe_(3)P,which further dissolves into theα-Fe matrix through solid-state diffusion,ultimately generating Fe-P solid solutions.展开更多
Promoting the synergistic governance of pollution control(PC)and carbon reduction(CR)in the agricultural sector was an important way for the Chinese government to implement the“dual carbon”initiative and respond to ...Promoting the synergistic governance of pollution control(PC)and carbon reduction(CR)in the agricultural sector was an important way for the Chinese government to implement the“dual carbon”initiative and respond to climate change.Based on the data of China’s crop production from 31 provincial-level regions from 1997 to 2022,this paper constructs a framework consisting of spatiotemporal evolution,synergy effect measurement,differences in contributions across regions,and influencing factors analysis to reveal the relationship between agricultural PC and CR.The results showed that the annual growth rates of pollutant emissions and carbon emissions were 1.85%and 0.79%,respectively.However,the annual decline rates of their emission intensities were 3.14%and 4.32%,respectively.This indicated that China’s actions to reduce pollution and carbon emissions in agriculture have achieved good results,that the effect of PC was weaker than that of CR and had an obvious“policy node effect.”Simultaneously,the synergy between PC and CR evolved from“basic coordination”to“basic imbalance.”The contribution of inter-regional differences was relatively large,while intra-regional differences were smaller,highlighting the importance of reducing regional disparities in promoting the synergistic governance of PC and CR.The basic conditions,industrial structure,input intensity,and development potential of agricultural development were key factors in widening the coupling coordination gap between PC and CR,and the influence of these significant factors exhibited clear spatiotemporal heterogeneity.These findings have provided important evidence for understanding China’s agricultural environmental governance strategies and could offer experiential insights for developing countries in advancing the coordinated governance of agricultural PC and CR.展开更多
文摘The hydrogen-based reduction and electric smelting technology is a green and low-carbon process for treating low-grade ore and complex symbiotic iron ore.In this study,the hydrogen-based reduction of boron-bearing iron concentrate and the low-temperature separation compared with the high-temperature melting separation of slag and iron from a boron-bearing iron concentrate were studied.The metallization rate of the boron-bearing iron concentrate reached 99.63%after hydrogen-based reduction at 1050℃,and the metallic iron was interwoven with olivine(Mg_(2)SiO_(4))in the reduced ore.In addition,the high-temperature melting separation of iron and slag could be accomplished at 1550℃for 60 min,where boron was mainly distributed in the form of a glass phase in the slag with a mass fraction of B_(2)O_(3)of 22.69%,and 0.35%of boron(mass fraction)was melted into liquid iron.By contrast,iron and slag were efficiently separated at a lower temperature(1300℃)for 10 min and enhanced by super-gravity.Almost all the boron content was enriched into a suanite phase in the slag with a considerably high mass fraction of B_(2)O_(3)(35.61%)and a high recovery ratio(99.37%),and the mass fraction of boron decreased to 0.15%in iron.Compared with high-temperature melting separation,low-temperature separation combined with hydrogen-based reduction greatly improved the enrichment of boron in slag and prevented the melting of boron into iron.
文摘The steel industry’s transition to hydrogen-based ironmaking necessitates a deeper understanding of magnetite ore reduction,a crucial yet underexplored pathway for decarbonization.This study systematically investigates the combined effects of particle size and gangue composition on hydrogen-based reduction behavior of four industrial magnetite ore concentrates with varying CaO and MgO con-tents.Thermogravimetric analysis at 973 K,interrupted reduction experiments,and post-reduction characterization steps are used to eval-uate reduction extent and phase transformations across different particle size fractions and bulk ores.The finer fractions generally exhibit faster and more complete reduction.However,this trend is overridden by gangue effects in certain ores.Magnetite ores with MgO as gangue tend to form magnesio-wustite solid solution(Mg,Fe)O during reduction,resulting in dense microstructures that impede hydrogen diffusion and limit reduction progress.In contrast,magnetite ores with CaO as gangue facilitate the formation of intermediate calcium fer-rites,which promote porous morphology and enhanced reducibility.Notably,even the finer particles of ore containing MgO show a lower reduction degree than the coarser particles of the ore containing CaO as gangue.This highlights the dominant role of gangue composition in governing reduction kinetics,intermediate phase formation and final product morphology.These findings contribute to the growing knowledge necessary to enable fossil-free ironmaking by emphasizing the importance of considering both granulometric characteristics and heterogeneity when evaluating magnetite ores for hydrogen-based reduction.
基金National Natural Science Foundation of China(52104249)Liaoning Joint Fund General Support Program Project(2023-MSBA-126)the Fundamental Research Funds for the Central Universities(N2401019).
文摘Iron tailings are a common solid waste resource,posing serious environmental and spatial challenges.This study proposed a novel hydrogen-based reduction roasting(HRR)technology for the processing of iron tailings using a combined beneficiation and metallurgy approach.Pilot-cale experiment results indicated that under the gas composition of CO:H_(2)=1:3,and optimal roasting conditions at a reduction temperature of 520℃,the majority of weakly magnetic hematite transforms into strongly magnetic magnetite during the reduction process.Combining roasting products with a magnetic separation-grinding-magnetic selection process yields a final iron concentrate with a grade of 56.68%iron and a recovery rate of 86.54%.Theoretical calculations suggested the annual production value can reach 29.7 million USD and a reduction of 20.79 tons of CO_(2) emissions per year.This highlights that the use of HRR in conjunction with traditional beneficiation processes can effectively achieve comprehensive utilization of iron tailings,thereby reducing environmental impact.
基金financially supported by the Key Program of National Natural Science Foundation of China(No.U23A20608)the Liaoning Province Science and Technology Plan Joint Program(Key Research and Development Program Project),China(No.2023JH2/101800058)+3 种基金the Science&Technology Plan Project of Hebei Province,China(No.23314601L)the Project of Hydrogen-Based Shaft Furnace Reduction-Electric Furnace Melting And Separation Technology Research and Application for High-Titanium Magnetite Iron Ore(No.HG2023239)the General Program of National Natural Science Foundation of China(No.52274253)the Special Project for Major Scientific and Technological Achievements Transformation in Hebei Province,China(No.23284101Z)。
文摘The novel process of hydrogen-based shaft furnaces(HSFs)has attracted considerable attention because of their significant reduction of CO_(2)emissions.In this study,the interaction of H_(2)and CO with Fe_(tet1)-and Fe_(oct2)-terminated Fe_(3)O_(4)(111)surfaces under HSF conditions,including their adsorption and reduction behaviors,was investigated using the density functional theory method.The results indicated that the H_(2)molecule adsorbed onto the Fe_(tet1)-terminated surface with an adsorption energy(AE)of-1.36 eV,whereas the CO molecule preferentially adsorbed on the Fe_(oct2)-terminated surface with an AE of-1.56 eV.Both H_(2)and CO can readily undergo reduction on the Fe_(tet1)-terminated surface(corresponding to energy barriers of 0.83 eV and 2.23 eV,respectively),but kinetically the reaction of H2is more favorable than that of CO.With regard to the thermodynamics at 400-1400 K,the H_(2)was easy to be adsorbed,while the CO would like to react on the Fe_(tet1)-terminated surface.These thermodynamically tendencies were reversed on the Fe_(oct2)-terminated surface.The thermodynamic disadvantage of the reaction of H_(2)on the Fe_(tet1)-terminated surface was offset by an increase in the temperature.Furthermore,the adsorption of H2 and CO on the Fe_(tet1)-terminated surface was competitive,whereas the adsorption of them on the Fe_(oct2)-terminated surface was synergistic.Therefore,iron ores with a higher proportion of Fe_(tet1)-terminated surface can be applied for the HSF process.In conjunction with the increases in the reduction temperature and the ratio of H_(2)in the reducing gas would promote efficient HSF smelting.These observations provide effective guidance for optimizing the practical operation parameters and advancing the development of the HSF process.
基金supported by the authors are especially grateful to the National Natural Science Foundation of China(Grant No.51904063)the Key Program of National Natural Science Foundation of China(No.U23A20608)+6 种基金Fundamental Research Funds for the Central Universities(N2025023,N2225046)Postdoctoral Followship Program of CPSF(GZC20230392)Science&Technology Plan Project of Liaoning Province(2022JH24/10200027)Science&Technology Plan Project of Hebei Province(23314601L)Science and Technology Program of Liaoning of China(2023JH2/101700304)China Postdoctoral Science Foundation(2023M740551)Liaoning Province Science and Technology Plan Joint Program(Key Research and Development Program Project)(2023JH2/101800058).
文摘The sticking behavior of pellets affects the continuity of production in hydrogen-based shaft furnace.The coupling influences of V_(2)O_(5) and reduction temperature on reduction sticking behavior and mechanism evolution of pellets under hydrogen atmosphere are investigated.The increase in V_(2)O_(5) addition aggravated the reduction sticking behavior,which is attributed to the combined functions of the development of unique interwoven structure in the metallic iron interconnections at the reduction sticking interface and the deterioration of reduction swelling behavior of pellets.In addition,the strength of metallic iron interconnections enhanced and reduction sticking behavior aggravated with the increase in reduction temperature.Importantly,compared to other reduction temperatures,the reduction sticking behavior of pellets was most significantly aggravated with the increase in V_(2)O_(5) addition at 1000℃.And the values of sticking index increased from 10.22%to 15.36% as the V_(2)O_(5) addition increased from 0 to 1.00 wt.%at 1000℃.
基金supported by the National Natural Science Foundation of China (42505149,41925023,U2342223,42105069,and 91744208)the China Postdoctoral Science Foundation (2025M770303)+1 种基金the Fundamental Research Funds for the Central Universities (14380230)the Jiangsu Funding Program for Excellent Postdoctoral Talent,and Jiangsu Collaborative Innovation Center of Climate Change。
文摘Countries around the world have been making efforts to reduce pollutant emissions. However, the response of global black carbon(BC) aging to emission changes remains unclear. Using the Community Atmosphere Model version 6 with a machine-learning-integrated four-mode version of the Modal Aerosol Module, we quantify global BC aging responses to emission reductions for 2011–2018 and for 2050 and 2100 under carbon neutrality. During 2011–18, global trends in BC aging degree(mass ratio of coatings to BC, R_(BC)) exhibited marked regional disparities, with a significant increase in China(5.4% yr^(-1)), which contrasts with minimal changes in the USA, Europe, and India. The divergence is attributed to opposing trends in secondary organic aerosol(SOA) and sulfate coatings, driven by regional changes in the emission ratios of corresponding coating precursors to BC(volatile organic compounds-VOCs/BC and SO_(2)/BC). Projections under carbon neutrality reveal that R_(BC) will increase globally by 47%(118%) in 2050(2100), with strong convergent increases expected across major source regions. The R_(BC) increase, primarily driven by enhanced SOA coatings due to sharper BC reductions relative to VOCs, will enhance the global BC mass absorption cross-section(MAC) by 11%(17%) in 2050(2100).Consequently, although the global BC burden will decline sharply by 60%(76%), the enhanced MAC partially offsets the magnitude of the decline in the BC direct radiative effect, resulting in the moderation of global BC DRE decreases to 88%(92%) of the BC burden reductions in 2050(2100). This study highlights the globally enhanced BC aging and light absorption capacity under carbon neutrality, thereby partly offsetting the impact of BC direct emission reductions on future changes in BC radiative effects globally.
文摘In order to explore the reduction pathways of zinc oxide in LiCl molten salt and the optimal process,experiments were conducted in an alumina crucible using metallic lithium as the reducing agent and lithium chloride molten salt as the reaction medium at 923 K.The study assessed the effects of lithium thermochemical reduction and electrolytic reduction of ZnO.The volatilization behavior of metal oxides in molten salts,the equivalent of a reducing agent,reduction time,amount of molten salt,stirring time,and the method of reduction feed were investigated for their impacts on the reduction yield and product composition.X-ray powder diffraction(XRD)analysis of the products showed that lithium reduction of ZnO not only produced metallic Zn but also formed a LiZn alloy.Electrolytic reduction can be used to obtain the metallic Zn product by controlling the potential below-2.2 V(vs Ag/Ag^(+)).Moreover,sintered oxides and higher electrode potentials could enhance the efficiency of electrolysis.Under the optimal reaction conditions determined experimentally,the lithium reduction experiment achieved a yield of 77.2%after a 12-h test,and the electrolytic reduction reached a yield of 85.4%after a 6-h test.
文摘A method for the rapid reduction of acyl chlorides to aldehydes was developed using pinacolborane(HBpin)as the reducing agent.The method exhibits excellent generality for both aromatic and aliphatic substrates,affording aldehydes in isolated yields of up to 88%with broad functional group tolerance,including cyano,halogen,alkenyl,ketone,and ester groups.Moreover,the method enables gram-scale aldehyde synthesis and shows high efficiency in reducing in situ generated acyl chlorides,thereby enhancing its synthetic practicality.
文摘This paper presents an efficient model reduction technique for linear time-varying systems based on shifted Legendre polynomials.The approach constructs approximate low-rank decomposition factors of finite-time Gramians directly from the expansion coefficients of impulse responses.Leveraging these factors,we develop two model reduction algorithms that integrate the low-rank square root method with dominant subspace projection.Our method is computationally efficient and flexible,requiring only a few matrix-vector operations and a singular value decomposition of a low-dimensional matrix,thereby avoiding the need to solve differential Lyapunov equations.Numerical experiments confirm the effectiveness of the proposed approach.
文摘This paper reports the preparation of three di‑iron complexes containing a thiazole moiety.Esterification of complex[Fe_(2)(CO)_(6)(μ‑SCH_(2)CH(CH_(2)OH)S)](1)with 4‑methylthiazole‑5‑carboxylic acid gave the corresponding ester[Fe_(2)(CO)_(6)(μ‑tedt)](2),where tedt=SCH_(2)CH(CH_(2)OOC(5‑C_(3)HNSCH_(3)))S.Further reactions of complex 2 with tri(ptolyl)phosphine(tp)or tris(4‑fluorophenyl)phosphine(fp)gave the phosphine‑substituted derivatives[Fe_(2)(CO)_(5)(tp)(μ‑tedt)](3)and[Fe_(2)(CO)_(5)(fp)(μ‑tedt)](4).The structures of the newly prepared complexes were elucidated by elemental analysis,NMR,IR,and X‑ray photoelectron spectroscopy.Moreover,single‑crystal X‑ray diffraction analysis confirmed their molecular structures,showing that they contain a di‑iron core ligated by a bridged dithiolate bearing a thiazole moiety and terminal carbonyls.The electrochemical and electrocatalytic proton reduction were probed by cyclic voltammetry,revealing that three complexes can catalyze the reduction of protons to H_(2) under the electrochemical conditions.For comparison,complex 4 possessed the best efficiency with a turnover frequency of 23.5 s^(-1)at 10 mmol·L^(-1)HOAc concentration.In addition,the fungicidal activity of these complexes was also investigated in this study.CCDC:2477511,2;2477512,3;2477513,4.
文摘Experts and officials shared their insights on poverty reduction cooperation and sustainable development during the 2025 International Seminar on Global Poverty Reduction Partnerships.
基金supported by the National Key R&D Program of China(No.2023YFE0112100)the Science and Technology Planning Project of Fujian Province(No.2023Y4015)the Marine and Fishery Devel-opment Special Fund of Xiamen(No.23YYST064QCB36).
文摘Hexavalent chromium(Cr(Ⅵ)) is an extremely toxic pollutant in aqueous environment.Chemical reduction is the most employed method in decontamination of Cr(Ⅵ).However,the chemical reduction was usually conducted in acidic media,resulting in considerable waste of acid reagents and the following neutralizing agents.In this study,kinetics and mechanisms of Cr(Ⅵ) reduction by sulfite in alkaline conditions(pH:7-10) were investigated.It reveals that Cr(Ⅵ) reduction follows pseudo-zero-order kinetics,where the rate constants increased markedly with an in situ irradiation of Far-UVC(UV_(222)).Decreasing pH levels slightly favored the reduction.Iodide ion displayed a notable accelerating effect,which not only save the energy input but also minimize the reductant usage.Chloride,sulfate,and carbonate ions exhibit little effect on the reduction,whereas nitrate and nitrite ions,dissolved oxygen as well as Cu(Ⅱ) suppressed the reduction significantly,implying that hydrated electrons produced by UV222 played the most important role in the reaction.Compared to the UV254/sulfite/iodide process,UV222/sulfite/iodide demonstrates clear advantages in the reduction kinetics and the sulfite utilization efficiency,underscoring its potential for effective Cr(Ⅵ) remediation in various environmental settings.
文摘Objective: To investigate the therapeutic advantages of closed reduction and Kirschner wire fixation versus open reduction and plate fixation in patients with hand surgery fractures. Methods: The sample was collected from May 2021 to May 2025, consisting of 80 patients with hand surgery fractures. These patients were randomly divided into two groups using the red and blue ball method: the plate fixation group (40 cases, treated with open reduction and plate fixation) and the Kirschner wire fixation group (40 cases, treated with closed reduction and Kirschner wire fixation). The therapeutic effects between the two groups were randomly compared. Results: The Kirschner wire fixation group outperformed the plate fixation group in all indicators except for hand function scores (p < 0.05). There was no statistically significant difference in hand function scores between the two groups (p > 0.05). Conclusion: Compared with open reduction and plate fixation, closed reduction and Kirschner wire fixation for patients with hand surgery fractures achieves a more pronounced therapeutic effect, with advantages such as less trauma, shorter operation time, less bleeding, and a lower incidence of complications. It is suitable for hand surgery fractures with good stability. Open reduction and plate internal fixation have greater advantages in complex fractures and cases requiring high stability, and are worthy of promotion and application.
基金supported by the Science and Technology Project of the State Grid Corporation of China“Research on Comprehensive Value Evaluation Method of Flexible Adjusting Resources under Carbon-electricity-certificate Market Coupling Environment”(No.5108-202455038A-1-1-ZN).
文摘The energy transition inspired by carbon neutrality targets and the increasing threat of extreme events raise multi-objective development requirements for power systems.This paper proposes a multi-objective resource allocation model to determine the type,number and location of flexible resources to increase the values of resilience,carbon reduction and renewable energy consumption.To evaluate the values of resilience,a restoration model for transmission systems is established that considers the coordination of fossil-fuel generators,energy storage systems(ESSs)and renewable energy generators in building restoration paths.The collaborative power-carbon-tradable green certificate(TGC)market model is then applied to evaluate the resource values in terms of carbon reduction and renewable energy consumption.Finally,the model is formulated as a mixed-integer linear programming(MILP)with a nonconvex feasible domain,and the normalized normal constraint(NNC)method is applied to obtain approximate Pareto frontiers for decision makers.Case studies validate the effectiveness of the proposed model in improving multi-factor values and analyze the impact of resource regulation capacity on values of restoration and carbon reduction.
基金the Natural Science Foundation of China(Grant No.NSFC-22072062,22202098)the Science and Technology Project of China Northern Rare Earth(BFXT-2023-D-0048 and BFXT-2022-D-0078)。
文摘Electrochemical nitrate reduction reaction(NO_(3)RR)is a sustainable strategy to treat wastewater and produce ammonia.However,it is still a challenge to prepare electrocatalysts with high activity and selectivity.Herein,the CuO_(x) nanowires supported Ru nanoclusters(Ru-CuO_(x))were fabricated via a three-step procedure for efficient nitrate conversion and highly selective ammonia generation.The prepared RuCuO_(x) shows a high ammonia yield rate of 2286.5μg h^(-1) cm^(-2) at-0.7 V vs.RHE and Faradaic efficiency(FE)of 80.1%at-0.4 V vs.RHE.Additionally,the nitrate conversion rate exceeds 90%at the potential range from-0.2 to-0.7 V vs.RHE,and the ammonia selectivity can reach 97.7%at-0.7 V vs.RHE in100 mg L^(-1) NaNO_(3) solution.The systematic characterizations clarify that the introduction of Ru not only regulates the electronic structure of CuO_(x) and accelerates the reconstruction of CuO_(x) to Cu but also promotes H2O dissociation to generate active hydrogen.Moreover.in-situ Raman spectroscopy reveals that the formed Ru-Cu is considered the actual active species during the NO_(3)RR.Density functional theory(DFT)calculations further prove that the obtained Ru-Cu facilitates the adsorption of nitrate and lowers the Gibbs free energy of the rate-determining step,thus improving the NO_(3)RR performance.
基金supported by the Natural Science Foundation(NSF)of China(Nos.22205015,22175020,and 22235001)the National Postdoctoral Program for Innovative Talents(No.BX20220032)+2 种基金the China Postdoctoral Science Foundation Funded Project(No.2022BG013)the Fundamental Research Funds for the Central Universities(Nos.00007709,00007770,and FRFBR-23-02B)University of Science and Technology Beijing is gratefully acknowledged.
文摘In comparison with their 2D and 3D counterparts,1D covalent organic frameworks(COFs)have rarely been investigated due to the synthetic challenge arising from the strict necessary matching in the molecular symmetry between corresponding building blocks and linking units in addition to the unmanageable packing of 1D organic chains once formed.Herein,two novel imide-linked 1D COFs with phthalocyanine building blocks,namely NiPc-CZDM-COF and NiPc-CZDL-COF,were fabricated from the hydrothermal synthesis reaction of 2,3,9,10,16,17,23,24-octacarboxyphthalocyaninato nickel(II)(NiPc(COOH)_(8))with 9H-carbazole-3,6-diamine(CZDM)and 4,4′-(9H-carbazole-3,6-diyl)dianiline(CZDL),respectively.Two COFs have high crystallinity on the basis of powder X-ray diffraction analysis and high-resolution transmission electron microscopy.Due to their high ratio of exposed active centers on the edge sites of porous ribbons,both NiPc-CZDM-COF and NiPc-CZDL-COF electrodes display high utilization efficiency of NiPc electroactive sites of 8.0%and 7.5% according to the electrochemical measurement,resulting in their excellent capacity toward electrocatalytic nitrate reduction with the nitrate-to-NH3 Faradaic efficiency of nearly 100%.In particular,NiPc-CZDM-COF electrode exhibits superior electrocatalytic performance with high NH_(3) partial current density of−246 mA/cm^(2),ammonia yield rate of 19.5 mg cm^(−2) h^(−1),and turnover frequency of 5.8 s^(−1) at−1.2 V in an H-type cell associated with its higher conductivity.This work reveals the good potential of 1D porous crystalline materials in electrocatalysis.
基金supported by the National Natural Science Foundation of China(Nos.22376197,U2441225,22076188).
文摘The demand for ^(238)Pu (nuclear battery heat source) drives the separation of its precursor,^(237)Np,from spent nuclear fuel (SNF).However,the co-existence of multi-valence states (Ⅳ/Ⅴ/Ⅵ) of Np and similar redox behavior with Pu(Ⅳ) hinder the effective separation of Np.N-Butyraldehyde (n-C_(3)H_(7)CHO) selectively reduces Np(Ⅵ) to Np(Ⅴ) without reducing Pu(Ⅳ).Herein,we examined the reduction mechanisms of Np(Ⅵ) and Pu(Ⅳ) by n-C3H7CHO using relativistic density functional theory.Based on the results of the potential energy profiles,the reductions of both Np(Ⅵ) and Pu(Ⅳ) by n-C_(3)H_(7)CHO are thermodynamically feasible,whereas only the former is kinetically achievable.It uncovers that n-C_(3)H_(7)CHO can only reduce Np(Ⅵ) to Np(Ⅴ) owing to kinetically controlled selective reduction.The analyses of spin density and bond distance indicate that the reduction nature for the first Np(Ⅵ)/Pu(Ⅳ) belongs to hydrogen atom transfer,whereas that for the second one involves outer-sphere electron transfer.Localized molecular orbitals (LMOs) analysis discloses the bonding evolution during the reduction process of Np(Ⅵ)/Pu(Ⅳ).This study elucidates the reason behind the kinetically controlled selective reduction of Np(Ⅵ)/Pu(Ⅳ) by nC3H7CHO at the molecular level and offers in-depth perspectives on the isolation of specific metal ions from the view of kinetic control.
基金supports of the National Natural Science Foundation of China(NSFC)(52021004,52394202)key project of the Joint Fund for Innovation and Development of Chongqing Natural Science Foundation(CSTB2022NSCQ-LZX0013)+1 种基金the National Natural Science Foundation of China(NSFC)(52301232,and 52476056)the Natural Science Foundation of Chongqing Province(2024NSCQ-MSX1109).
文摘Controllable synthesis of ultrathin metallene nanosheets and rational design of their spatial arrangement in favor of electrochemical catalysis are critical for their renewable energy applications.Here,a biomimetic design of“Trunk-Branch-Leaf”strategy is proposed to prepare the ultrathin edge-riched Zn-ene“leaves”with a thickness of~2.5 nm,adjacent Zn-ene cross-linked with each other,which are supported by copper nanoneedle“branches”on copper mesh“trunks,”named as Zn-ene/Cu-CM.The resulting superstructure enables the formation of an interconnected network and multiple channels,which can be used as an electrocatalytic CO_(2) reduction reaction(CO_(2)RR)electrode to allow a fast charge and mass transfer as well as a large electrolyte reservoir.By virtue of the distinctive structure,the obtained Zn-ene/Cu-CM electrode exhibits excellent selectivity and activity toward CO production with a maximum Faradaic efficiency of 91.3%and incredible partial current density up to 40 mA cm^(−2),outperforming most of the state-of-the-art Zn-based electrodes for CO_(2) reduction.The phenolphthalein color probe combined with in situ attenuated total reflection-infrared spectroscopy uncovered the formation of the localized pseudo-alkaline microenvironment at the interface of the Zn-ene/Cu-CM electrode.Theoretical calculations confirmed that the localized pH as the origin is responsible for the adsorption of CO_(2) at the interface and the generation of *COOH and *CO intermediates.This study offers valuable insights into developing efficient electrodes through synergistic regulation of reaction microenvironments and active sites,thereby facilitating the electrolysis of practical CO_(2) conversion.
基金supported by the National Key Research and Development Program of China(Nos.2023YFC3903900 and 2023YFC3903904)the National Natural Science Foundation Youth Foundation of China(No.52404356)the China Baowu Low Carbon Metallurgy Innovation Foundation(No.BWLCF202216)。
文摘Phosphorus tends to migrate into metallic iron during the direct reduction of high-phosphorus oolitic iron ore,leading to undesirable phosphorus enrichment in metallic iron.However,the underlying reduction and migration mechanisms remain poorly understood.Phosphorus behavior during coal-based reduction was systematically investigated through theoretical modeling and experimental approaches.Thermodynamic analysis revealed that the carbon reduction of solid Ca_(3)(PO_(4))_(2)to gaseous P_(2)requires temperatures exceeding 1400℃.Notably,this threshold significantly decreases to 1130.5℃in the presence of SiO_(2)and Al_(2)O_(3).Further investigations demonstrated that Ca_(3)(PO_(4))_(2)co-reduces with Fe_(x)O_(γ)in the presence of SiO_(2)-Al_(2)O_(3)-Fe_(x)O_(γ),forming Fe_(3)P(instead of gaseous P_(2))at a markedly lower temperature of 778.7℃.Mechanistic studies indicate that the inherent thermal stability of Ca_(3)(PO_(4))_(2)inhibits the generation of reactive[P_(2)O_(5)].However,SiO_(2)-Al_(2)O_(3)coexistence destabilizes Ca_(3)(PO_(4))_(2)while exponentially enhancing[P_(2)O_(5)]activity.This synergistic effect dramatically promotes the phosphorus mineral reduction.Characterization confirmed that Ca_(3)(PO_(4))_(2)migrated into the slag phase(4FeO·Al_(2)O_(3)·3SiO_(2)·CaO·P_(2)O_(5)).Subsequently,the reactive P_(2)O_(5)in slag is reduced with metallic iron to form Fe_(3)P,which further dissolves into theα-Fe matrix through solid-state diffusion,ultimately generating Fe-P solid solutions.
基金National Social Science Fund of China,No.22BGL182。
文摘Promoting the synergistic governance of pollution control(PC)and carbon reduction(CR)in the agricultural sector was an important way for the Chinese government to implement the“dual carbon”initiative and respond to climate change.Based on the data of China’s crop production from 31 provincial-level regions from 1997 to 2022,this paper constructs a framework consisting of spatiotemporal evolution,synergy effect measurement,differences in contributions across regions,and influencing factors analysis to reveal the relationship between agricultural PC and CR.The results showed that the annual growth rates of pollutant emissions and carbon emissions were 1.85%and 0.79%,respectively.However,the annual decline rates of their emission intensities were 3.14%and 4.32%,respectively.This indicated that China’s actions to reduce pollution and carbon emissions in agriculture have achieved good results,that the effect of PC was weaker than that of CR and had an obvious“policy node effect.”Simultaneously,the synergy between PC and CR evolved from“basic coordination”to“basic imbalance.”The contribution of inter-regional differences was relatively large,while intra-regional differences were smaller,highlighting the importance of reducing regional disparities in promoting the synergistic governance of PC and CR.The basic conditions,industrial structure,input intensity,and development potential of agricultural development were key factors in widening the coupling coordination gap between PC and CR,and the influence of these significant factors exhibited clear spatiotemporal heterogeneity.These findings have provided important evidence for understanding China’s agricultural environmental governance strategies and could offer experiential insights for developing countries in advancing the coordinated governance of agricultural PC and CR.
