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
Experts and officials shared their insights on poverty reduction cooperation and sustainable development during the 2025 International Seminar on Global Poverty Reduction Partnerships.
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
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
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
Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-...Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-doped carbon(Fe/SNC)via in situ incorporation of 2-aminothiazole molecules into zeolitic imidazolate framework-8(ZIF-8)through coordination between metal ions and organic ligands.Sulfur and nitrogen doping in carbon supports effectively modulates the electronic structure of the catalyst,increases the Brunauer-Emmett-Teller surface area,and exposes more Fe-N_(x)active centers.Fe-loaded,S and N co-doped carbon with Fe/S molar ratio of 1:10(Fe/SNC-10)exhibits a half-wave potential of 0.902 V vs.RHE.After 5000 cycles of cyclic voltammetry,its half-wave potential decreases by only 20 mV vs.RHE,indicating excellent stability.Due to sulfur s lower electronegativity,the electronic structure of the Fe-N_(x)active center is modulated.Additionally,the larger atomic radius of sulfur introduces defects into the carbon support.As a result,Fe/SNC-10 demonstrates superior ORR activity and stability in alkaline solution compared with Fe-loaded N-doped carbon(Fe/NC).Furthermore,the zinc-air battery assembled with the Fe/SNC-10 catalyst shows enhanced performance relative to those assembled with Fe/NC and Pt/C catalysts.This work offers a novel design strategy for advanced energy storage and conversion applications.展开更多
The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a serie...The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a series of RuCo/C catalysts were synthesized by NaBH4 reduction method under the premise that the total metal mass percentage was 20%.X-ray diffraction(XRD)patterns and scanning electron microscopy(SEM)confirmed the formation of single-phase nanoparticles with an average size of 33 nm.Cyclic voltammograms(CV)and linear sweep voltammograms(LSV)tests indicated that RuCo(2:1)/C catalyst had the optimal ORR properties.Additionally,the RuCo(2:1)/C catalyst remarkably sustained 98.1% of its activity even after 3000 cycles,surpassing the performance of Pt/C(84.8%).Analysis of the elemental state of the catalyst surface after cycling using X-ray photoelectron spectroscopy(XPS)revealed that the Ru^(0) percentage of RuCo(2:1)/C decreased by 2.2%(from 66.3% to 64.1%),while the Pt^(0) percentage of Pt/C decreased by 7.1%(from 53.3% to 46.2%).It is suggested that the synergy between Ru and Co holds the potential to pave the way for future low-cost and highly stable ORR catalysts,offering significant promise in the context of PEMFCs.展开更多
Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution insurface and ground water,disrupting the balance of the global nitrogen cycle.Electrochemical nitrate...Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution insurface and ground water,disrupting the balance of the global nitrogen cycle.Electrochemical nitrate reduction(eNO_(3)RR)emerges as an attractive strategy to simultaneously enable nitrate removal and decentralized ammo-nia fabrication,restoring the globally perturbed nitrogen cycle.However,complex deoxygenation-hydrogenationprocesses and sluggish proton-electron transfer kinetics significantly hinder practical application of eNO_(3)RR.In this study,we developed carbon-coated Cu-Ni bimetallic catalysts derived from metal-organic frameworks(MOFs)to facilitate eNO_(3)RR.The unique structural features of catalyst promote enhanced synergy between Cuand Ni,effectively addressing critical challenges in nitrate reduction.Comprehensive structural and electrochem-ical analysis demonstrate that electrochemical nitrate-to-nitrite conversion mainly takes place on active Cu sites,the introduction of Ni could efficiently accelerate the generation of aquatic active hydrogen,promoting the hy-drogenation of oxynitrides during eNO_(3)RR.In addition,Ni introduction could push up the d-band center of thecatalyst,thus enhancing the adsorption and activation of nitrate and the corresponding intermediates.Detailedreaction pathways for nitrate-to-ammonia conversion are illuminated by rotating disk electrode(RDE),in-situFourier-transform infrared spectroscopy,in-situ Raman spectrum and electrochemical impedance spectroscopy(EIS).Benefiting from the synergistic effect of Cu and Ni,optimum catalyst exhibited excellent nitrate reductionperformance.This work provides a new idea for elucidating the underlying eNO_(3)RR reaction mechanisms andcontributes a promising strategy for designing efficient bimetallic electrocatalysts.展开更多
Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural ga...Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural gases.We used the GC-Py-GC-IRMS method to study TSR and obtained a novel finding related to intramolecular carbon isotope fractionation in natural propane.The results show that theΔC-T(δ^(13)C_(central)-13 C_(terminal))andδ^(13)C_(central)values significantly increased to 44.7‰and 11.9‰,respectively,with increasing TSR alteration.In contrast,the 13 C_(terminal)values of propane remained largely unaltered by the TSR reaction.This difference in position-specific isotope fractionation can be attributed to the central carbon’s reactivity being higher than that of terminal carbon during TSR.In sum,the results indicate that theδ^(13)C_(terminal)values of propane can serve as robust indicators for source rock identification of natural gas altered by post-generation reactions such as TSR and anaerobic microbial oxidation.展开更多
The hydrogen reduction kinetics of tungsten trioxide(WO_(3))was investigated via non-isothermal thermogravimetric analysis.Under the local gas-solid reduction conditions,the particle morphology of tungsten powders was...The hydrogen reduction kinetics of tungsten trioxide(WO_(3))was investigated via non-isothermal thermogravimetric analysis.Under the local gas-solid reduction conditions,the particle morphology of tungsten powders was found to be consistent with that of raw material WO_(3).The removal of oxygen from tungsten oxide during hydrogen reduction led to the formation of porous structures between the reduced particles,which were obviously different from the polyhedral single-crystal configuration of tungsten powders obtained via chemical vapor deposition.Moreover,the two-stage hydrogen reduction mechanisms of WO_(3) under the local gas-solid reduction conditions can be described using the composite autocatalytic function.The activation energies of the first and second stages of the hydrogen reduction of WO_(3) were determined to be 121 and 135 kJ/mol,respectively.展开更多
Seawater zinc-air batteries are promising energy storage devices due to their high energy density and utilization of seawater electrolytes.However,their efficiency is hindered by the sluggish oxygen reduction reaction...Seawater zinc-air batteries are promising energy storage devices due to their high energy density and utilization of seawater electrolytes.However,their efficiency is hindered by the sluggish oxygen reduction reaction(ORR)and chlorideinduced degradation over conventional catalysts.In this study,we proposed a universal synthetic strategy to construct heteroatom axially coordinated Fe–N_(4) single-atom seawater catalyst materials(Cl–Fe–N_(4) and S–Fe–N_(4)).X-ray absorption spectroscopy confirmed their five-coordinated square pyramidal structure.Systematic evaluation of catalytic activities revealed that compared with S–Fe–N_(4),Cl–Fe–N_(4) exhibits smaller electrochemical active surface area and specific surface area,yet demonstrates higher limiting current density(5.8 mA cm^(−2)).The assembled zinc-air batteries using Cl–Fe–N_(4) showed superior power density(187.7 mW cm^(−2) at 245.1 mA cm^(−2)),indicating that Cl axial coordination more effectively enhances the intrinsic ORR activity.Moreover,Cl–Fe–N_(4) demonstrates stronger Cl−poisoning resistance in seawater environments.Chronoamperometry tests and zinc-air battery cycling performance evaluations confirmed its enhanced stability.Density functional theory calculations revealed that the introduction of heteroatoms in the axial direction regulates the electron center of Fe single atom,leading to more active reaction intermediates and increased electron density of Fe single sites,thereby enhancing the reduction in adsorbed intermediates and hence the overall ORR catalytic activity.展开更多
Iron and steel industry is one of the main sources of air pollution emissions in China.The sintering process is an important link in the blast furnace ironmaking process,but it is also accompanied by a large number of...Iron and steel industry is one of the main sources of air pollution emissions in China.The sintering process is an important link in the blast furnace ironmaking process,but it is also accompanied by a large number of pollutants.Under the background of ultra-low emissions,iron and steel enterprises urgently need to upgrade their existing processes to address the existing process in practical application problems.In this study,a steel group in Gansu Province was taken as an example.By comparing and analyzing the pollutant emission characteristics before and after the ultra-low emission retrofit,the collaborative control effect of the combined process on SO_(2),NO_(x),particulate matter,and dioxins after the new retrofit was systematically evaluated.The results show that after the retrofit,the concentrations of particulate matter,SO_(2) and NO_(x) have dropped to near-zero levels,and the dioxin removal efficiency has reached 98.87%,with all indicators being better than the national ultra-low emission standards.The study confirms that the optimal combination of multi-pollutant collaborative treatment technologies is the key to achieving efficient emission reduction,among which selective catalytic reduction technology has a particularly significant synergistic removal effect on NO_(x) and dioxins.This study provides an important technical reference and practical basis for the ultra-low emission retrofit of the steel industry,and has important guiding significance for promoting the green retrofit of the industry.Its ultra-low emission retrofit is of great significance for achieving green and low-carbon development.展开更多
Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchan...Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchange strategy for the in-situ growth of BiVO_(4) on an InVO_(4) substrate to generate a Z-scheme heterojunction of InVO_(4)/BiVO_(4) .This in-situ partial transformation approach endows the InVO_(4)/BiVO_(4) heterojunction with a tightly connected interface,resulting in a significant improvement in charge separation efficiency between InVO_(4) and BiVO_(4).Moreover,the construction of the heterojunction reduces the formation energy barrier of the ^(*)COOH intermediate during the photoreduction of CO_(2) and increases the desorption energy barrier of the ^(*)CO intermediate,facilitating the deep reduction of ^(*)CO.Consequently,the InVO_(4)/BiVO_(4) heterojunction is capable of photocatalytic CO_(2) reduction to CH_(3)OH with high efficiency and selectivity.Under conditions where water serves as the electron source and a light intensity of 100 m W/cm^(2),the yield of CH_(3)OH reaches 130.5 μmol g^(-1)h^(-1) with a selectivity of 92 %,outperforming photocatalysts reported under similar conditions.展开更多
Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient ...Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.展开更多
Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that...Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.展开更多
Background:Childhood leukemia,a malignant proliferative disorder of the hematopoietic system and the most common childhood cancer,poses a significant threat to the lives and health of affected children.For parents,a l...Background:Childhood leukemia,a malignant proliferative disorder of the hematopoietic system and the most common childhood cancer,poses a significant threat to the lives and health of affected children.For parents,a leukemia diagnosis in their child is a profoundly traumatic event.As primary caregivers,they endure immense psychological distress and caregiving stress throughout the prolonged and demanding treatment process,which can adversely affect their own well-being and caregiving capacity.However,the psychological mechanisms,such as the role of mindfulness,linking caregiver stress to parental coping strategies remain underexplored,and evidence-based interventions to support these parents are needed.Methods:In Study 1,we administered a cross-sectional survey to 242 parents of children with leukemia who were hospitalized at the Affiliated Hospital of Qingdao University between January and August 2024.Participants completed measures assessing caregiver burden,mindful attention awareness,and parental coping style.In Study 2,we further evaluated the effects of a Mindfulness-Based Stress Reduction(MBSR)intervention.Results:The results of Study 1 revealed:(1)The caregiving stress significantly and negatively predicted coping style(β=−1.18,95%CI[−2.18,−0.18],p<0.01).(2)Caregiving stress also significantly and negatively predicted mindfulness(β=−1.90,95%CI[−2.43,−1.38],p<0.01).(3)Conversely,mindfulness significantly and positively predicted coping style(β=0.85,95%CI[0.62,1.07],p<0.01).These findings suggest that mindfulness mediates the relationship between caregiver burden and coping style.In Study 2,the experimental group showed a significant decrease in caregiver stress post-intervention(t=2.24,p<0.05),a significant increase in mindfulness(t=−4.61,p<0.001),and a significant improvement in coping style(t=−2.36,p<0.01).No significant changes were observed in the control group.Conclusion:MBSR can effectively enhance mindfulness and promote adaptive coping strategies,while reducing caregiver burden among parents of children with leukemia.展开更多
Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespr...Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.展开更多
The changes and gastric digestive properties of gel were investigated for oxidiz ed myofibrillar protein(MP)(0–1 mmol/L H_(2)O_(2))treated by 30%substitution of NaCl with KCl,MgCl_(2),and KCl/MgCl_(2).Mild oxidation ...The changes and gastric digestive properties of gel were investigated for oxidiz ed myofibrillar protein(MP)(0–1 mmol/L H_(2)O_(2))treated by 30%substitution of NaCl with KCl,MgCl_(2),and KCl/MgCl_(2).Mild oxidation level(0.3 mmol/L H_(2)O_(2))facilitated the protein unfolding,and MgCl_(2)obviously intervened the protein selfassembly by forming the salt bridge and more disulfide bonds.At the same oxidation concentration,the sodium-reduced MP substituted with KCl formed dense network structure with better gel strength(increased by 6%–18%)and water retention in comparision to the gel without sodium reduction.The KCl-substituted gel chewing work was also relatively higher among the low-sodium samples at the first chewing cycle.Reversely,the relatively soft structure and lower gel viscosity in simulated oral chewing were found in MgCl_(2)-substituted gel.These changes decreased the contact limit between pepsin and protein for better gastric disintegration or pepsin diffusivity,and increased the proportion of small molecular weight peptides(25.83%,<5 kDa).Therefore,partial substitution of NaCl with other salt replacers could influence the physicochemical properties of low-sodium MP suspension or gel under different oxidation degree and the subsequent gastric digestion characteristics.展开更多
Owing to their global search capabilities and gradient-free operation,metaheuristic algorithms are widely applied to a wide range of optimization problems.However,their computational demands become prohibitive when ta...Owing to their global search capabilities and gradient-free operation,metaheuristic algorithms are widely applied to a wide range of optimization problems.However,their computational demands become prohibitive when tackling high-dimensional optimization challenges.To effectively address these challenges,this study introduces cooperative metaheuristics integrating dynamic dimension reduction(DR).Building upon particle swarm optimization(PSO)and differential evolution(DE),the proposed cooperative methods C-PSO and C-DE are developed.In the proposed methods,the modified principal components analysis(PCA)is utilized to reduce the dimension of design variables,thereby decreasing computational costs.The dynamic DR strategy implements periodic execution of modified PCA after a fixed number of iterations,resulting in the important dimensions being dynamically identified.Compared with the static one,the dynamic DR strategy can achieve precise identification of important dimensions,thereby enabling accelerated convergence toward optimal solutions.Furthermore,the influence of cumulative contribution rate thresholds on optimization problems with different dimensions is investigated.Metaheuristic algorithms(PSO,DE)and cooperative metaheuristics(C-PSO,C-DE)are examined by 15 benchmark functions and two engineering design problems(speed reducer and composite pressure vessel).Comparative results demonstrate that the cooperative methods achieve significantly superior performance compared to standard methods in both solution accuracy and computational efficiency.Compared to standard metaheuristic algorithms,cooperative metaheuristics achieve a reduction in computational cost of at least 40%.The cooperative metaheuristics can be effectively used to tackle both high-dimensional unconstrained and constrained optimization problems.展开更多
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 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.
基金financial support of the National Natural Science Foundation of China(No.52472271)the National Key Research and Development Program of China(No.2023YFE0115800)。
文摘Heteroatom-doped carbon is considered a promising alternative to commercial Pt/C as an efficient catalyst for the oxygen reduction reaction(ORR).This study presents the synthesis of iron-loaded,sulfur and nitrogen co-doped carbon(Fe/SNC)via in situ incorporation of 2-aminothiazole molecules into zeolitic imidazolate framework-8(ZIF-8)through coordination between metal ions and organic ligands.Sulfur and nitrogen doping in carbon supports effectively modulates the electronic structure of the catalyst,increases the Brunauer-Emmett-Teller surface area,and exposes more Fe-N_(x)active centers.Fe-loaded,S and N co-doped carbon with Fe/S molar ratio of 1:10(Fe/SNC-10)exhibits a half-wave potential of 0.902 V vs.RHE.After 5000 cycles of cyclic voltammetry,its half-wave potential decreases by only 20 mV vs.RHE,indicating excellent stability.Due to sulfur s lower electronegativity,the electronic structure of the Fe-N_(x)active center is modulated.Additionally,the larger atomic radius of sulfur introduces defects into the carbon support.As a result,Fe/SNC-10 demonstrates superior ORR activity and stability in alkaline solution compared with Fe-loaded N-doped carbon(Fe/NC).Furthermore,the zinc-air battery assembled with the Fe/SNC-10 catalyst shows enhanced performance relative to those assembled with Fe/NC and Pt/C catalysts.This work offers a novel design strategy for advanced energy storage and conversion applications.
基金Funded by the 111 Project(No.B17034)Open Project of Hubei Key Laboratory of Power System Design and Test for Electrical Vehicle(No.ZDSYS202212)+1 种基金Innovative Research Team Development Program of Ministry of Education of China(No.IRT_17R83)the Science and Technology Project of China Southern Power Grid Co.,Ltd.(No.GDKJXM20222546)。
文摘The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a series of RuCo/C catalysts were synthesized by NaBH4 reduction method under the premise that the total metal mass percentage was 20%.X-ray diffraction(XRD)patterns and scanning electron microscopy(SEM)confirmed the formation of single-phase nanoparticles with an average size of 33 nm.Cyclic voltammograms(CV)and linear sweep voltammograms(LSV)tests indicated that RuCo(2:1)/C catalyst had the optimal ORR properties.Additionally,the RuCo(2:1)/C catalyst remarkably sustained 98.1% of its activity even after 3000 cycles,surpassing the performance of Pt/C(84.8%).Analysis of the elemental state of the catalyst surface after cycling using X-ray photoelectron spectroscopy(XPS)revealed that the Ru^(0) percentage of RuCo(2:1)/C decreased by 2.2%(from 66.3% to 64.1%),while the Pt^(0) percentage of Pt/C decreased by 7.1%(from 53.3% to 46.2%).It is suggested that the synergy between Ru and Co holds the potential to pave the way for future low-cost and highly stable ORR catalysts,offering significant promise in the context of PEMFCs.
基金supported by the Natural Science Foundation of China(No.52101279)the Key Scientific Research Foundation of Education department of Hunan Province(No.24A0003)the Scientific Research Project of Education Department of Hunan Province(No.21B000)and the Fundamental Research Funds for the Central Universities of Central South University.
文摘Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution insurface and ground water,disrupting the balance of the global nitrogen cycle.Electrochemical nitrate reduction(eNO_(3)RR)emerges as an attractive strategy to simultaneously enable nitrate removal and decentralized ammo-nia fabrication,restoring the globally perturbed nitrogen cycle.However,complex deoxygenation-hydrogenationprocesses and sluggish proton-electron transfer kinetics significantly hinder practical application of eNO_(3)RR.In this study,we developed carbon-coated Cu-Ni bimetallic catalysts derived from metal-organic frameworks(MOFs)to facilitate eNO_(3)RR.The unique structural features of catalyst promote enhanced synergy between Cuand Ni,effectively addressing critical challenges in nitrate reduction.Comprehensive structural and electrochem-ical analysis demonstrate that electrochemical nitrate-to-nitrite conversion mainly takes place on active Cu sites,the introduction of Ni could efficiently accelerate the generation of aquatic active hydrogen,promoting the hy-drogenation of oxynitrides during eNO_(3)RR.In addition,Ni introduction could push up the d-band center of thecatalyst,thus enhancing the adsorption and activation of nitrate and the corresponding intermediates.Detailedreaction pathways for nitrate-to-ammonia conversion are illuminated by rotating disk electrode(RDE),in-situFourier-transform infrared spectroscopy,in-situ Raman spectrum and electrochemical impedance spectroscopy(EIS).Benefiting from the synergistic effect of Cu and Ni,optimum catalyst exhibited excellent nitrate reductionperformance.This work provides a new idea for elucidating the underlying eNO_(3)RR reaction mechanisms andcontributes a promising strategy for designing efficient bimetallic electrocatalysts.
基金supported by the Helium Enrichment and Detection in Natural Gas Reservoirs Related to Oil and Gas Fields project(Grant No.2025ZD1010500)the Deep Earth Probe and Mineral Resources Exploration―National Science and Technology Major Project.-。
文摘Thermochemical sulfate reduction(TSR)is an important organic-inorganic reaction that occurs within sedimentary basins and alters the original chemical compositions and isotopic structures of hydrocarbons in natural gases.We used the GC-Py-GC-IRMS method to study TSR and obtained a novel finding related to intramolecular carbon isotope fractionation in natural propane.The results show that theΔC-T(δ^(13)C_(central)-13 C_(terminal))andδ^(13)C_(central)values significantly increased to 44.7‰and 11.9‰,respectively,with increasing TSR alteration.In contrast,the 13 C_(terminal)values of propane remained largely unaltered by the TSR reaction.This difference in position-specific isotope fractionation can be attributed to the central carbon’s reactivity being higher than that of terminal carbon during TSR.In sum,the results indicate that theδ^(13)C_(terminal)values of propane can serve as robust indicators for source rock identification of natural gas altered by post-generation reactions such as TSR and anaerobic microbial oxidation.
基金supported by the National Key Research&Development Program of China(No.2022YFC2904905)the National Natural Science Foundation of China(No.52274400)+1 种基金the Project of Zhongyuan Critical Metals Laboratory,China(No.GJJSGFZD202302)the Science and Technology Project of Henan Province,China(No.232102230044)。
文摘The hydrogen reduction kinetics of tungsten trioxide(WO_(3))was investigated via non-isothermal thermogravimetric analysis.Under the local gas-solid reduction conditions,the particle morphology of tungsten powders was found to be consistent with that of raw material WO_(3).The removal of oxygen from tungsten oxide during hydrogen reduction led to the formation of porous structures between the reduced particles,which were obviously different from the polyhedral single-crystal configuration of tungsten powders obtained via chemical vapor deposition.Moreover,the two-stage hydrogen reduction mechanisms of WO_(3) under the local gas-solid reduction conditions can be described using the composite autocatalytic function.The activation energies of the first and second stages of the hydrogen reduction of WO_(3) were determined to be 121 and 135 kJ/mol,respectively.
基金funded by the Innovative Research Group Project of the National Natural Science Foundation of China(52121004)the Research Development Fund(No.RDF-21-02-060)by Xi’an Jiaotong-Liverpool University+1 种基金support received from the Suzhou Industrial Park High Quality Innovation Platform of Functional Molecular Materials and Devices(YZCXPT2023105)the XJTLU Advanced Materials Research Center(AMRC).
文摘Seawater zinc-air batteries are promising energy storage devices due to their high energy density and utilization of seawater electrolytes.However,their efficiency is hindered by the sluggish oxygen reduction reaction(ORR)and chlorideinduced degradation over conventional catalysts.In this study,we proposed a universal synthetic strategy to construct heteroatom axially coordinated Fe–N_(4) single-atom seawater catalyst materials(Cl–Fe–N_(4) and S–Fe–N_(4)).X-ray absorption spectroscopy confirmed their five-coordinated square pyramidal structure.Systematic evaluation of catalytic activities revealed that compared with S–Fe–N_(4),Cl–Fe–N_(4) exhibits smaller electrochemical active surface area and specific surface area,yet demonstrates higher limiting current density(5.8 mA cm^(−2)).The assembled zinc-air batteries using Cl–Fe–N_(4) showed superior power density(187.7 mW cm^(−2) at 245.1 mA cm^(−2)),indicating that Cl axial coordination more effectively enhances the intrinsic ORR activity.Moreover,Cl–Fe–N_(4) demonstrates stronger Cl−poisoning resistance in seawater environments.Chronoamperometry tests and zinc-air battery cycling performance evaluations confirmed its enhanced stability.Density functional theory calculations revealed that the introduction of heteroatoms in the axial direction regulates the electron center of Fe single atom,leading to more active reaction intermediates and increased electron density of Fe single sites,thereby enhancing the reduction in adsorbed intermediates and hence the overall ORR catalytic activity.
基金supported by the Key Research and Development Program of Gansu Province(22YF7FA070)the National Natural Science Foundation of China(22406076,22466026)the Basic Research Project of Yunnan Province(202301BE070001-017,202401CF070139,202401AS070085)。
文摘Iron and steel industry is one of the main sources of air pollution emissions in China.The sintering process is an important link in the blast furnace ironmaking process,but it is also accompanied by a large number of pollutants.Under the background of ultra-low emissions,iron and steel enterprises urgently need to upgrade their existing processes to address the existing process in practical application problems.In this study,a steel group in Gansu Province was taken as an example.By comparing and analyzing the pollutant emission characteristics before and after the ultra-low emission retrofit,the collaborative control effect of the combined process on SO_(2),NO_(x),particulate matter,and dioxins after the new retrofit was systematically evaluated.The results show that after the retrofit,the concentrations of particulate matter,SO_(2) and NO_(x) have dropped to near-zero levels,and the dioxin removal efficiency has reached 98.87%,with all indicators being better than the national ultra-low emission standards.The study confirms that the optimal combination of multi-pollutant collaborative treatment technologies is the key to achieving efficient emission reduction,among which selective catalytic reduction technology has a particularly significant synergistic removal effect on NO_(x) and dioxins.This study provides an important technical reference and practical basis for the ultra-low emission retrofit of the steel industry,and has important guiding significance for promoting the green retrofit of the industry.Its ultra-low emission retrofit is of great significance for achieving green and low-carbon development.
基金financially supported the National Key R&D Program of China (No.2022YFA1502902)the National Natural Science Foundation of China (NSFC,Nos.22475152 and U21A20286)the 111 Project of China (No.D17003)。
文摘Converting CO_(2) into methanol(CH_(3)OH),a high-value-added liquid-phase product,through efficient and highly selective photocatalysis remains a significant challenge.Herein,we present a straightforward cation exchange strategy for the in-situ growth of BiVO_(4) on an InVO_(4) substrate to generate a Z-scheme heterojunction of InVO_(4)/BiVO_(4) .This in-situ partial transformation approach endows the InVO_(4)/BiVO_(4) heterojunction with a tightly connected interface,resulting in a significant improvement in charge separation efficiency between InVO_(4) and BiVO_(4).Moreover,the construction of the heterojunction reduces the formation energy barrier of the ^(*)COOH intermediate during the photoreduction of CO_(2) and increases the desorption energy barrier of the ^(*)CO intermediate,facilitating the deep reduction of ^(*)CO.Consequently,the InVO_(4)/BiVO_(4) heterojunction is capable of photocatalytic CO_(2) reduction to CH_(3)OH with high efficiency and selectivity.Under conditions where water serves as the electron source and a light intensity of 100 m W/cm^(2),the yield of CH_(3)OH reaches 130.5 μmol g^(-1)h^(-1) with a selectivity of 92 %,outperforming photocatalysts reported under similar conditions.
基金the financial support from the Shandong Province colleges and universities youth innovation technology plan innovation team project(2022KJ285)the Natural Science Foundation of Shandong Province(ZR2022QE076)+1 种基金the National Natural Science Foundation of China(52202092)the Science and Technology Support Plan for Youth Innovation of Colleges and Universities of Shandong Province of China(2023KJ104).
文摘Exploring high-performance electrocatalysts for the nitrate reduction reaction(NO_(3)RR)is crucial for environmental nitrate removal and ammonia synthesis.Single-atom collaboration with cluster can provide sufficient active sites for catalysts to promote NO_(3)RR,yet the unclear synergistic effect between the two hinders their rational design.Herein,a series of Ir_(3)clusters and metal single atoms co-embedded in graphitic carbon nitride(g-CN)catalysts(Ir_(3)M1)were constructed,and the synergistic effects of Ir_(3)clusters and M1 single atoms on the NO_(3)RR catalytic mechanism and activity were systematically explored using density functional theory(DFT)calculations combined with machine learning.Comprehensive evaluations of structural stability and catalytic activity demonstrate that the synergy between single atoms and clusters effectively balances the adsorption energies of key intermediates,yielding exceptional catalytic performance(the limiting potential of Ir_(3)Ti_(1)can reach−0.22 V).Machine learning models further clarify the synergistic mechanism,where the geometric configurations of clusters serve as critical features for modulating the catalytic activity of single-atom sites,whereas the electronic structures of single atoms directly govern the reactivity of cluster sites.This DFT-machine learning approach provides theoretical guidelines for catalyst design and a predictive framework for efficient NO_(3)RR electrocatalysts.
基金Funded by the National Natural Science Foundation of China Guangdong(No.22279096)。
文摘Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.
基金approved by the Ethics Review Committee of Northwest Normal University(Approval No.:[2023028]).All participants signed the informed consent in this study.
文摘Background:Childhood leukemia,a malignant proliferative disorder of the hematopoietic system and the most common childhood cancer,poses a significant threat to the lives and health of affected children.For parents,a leukemia diagnosis in their child is a profoundly traumatic event.As primary caregivers,they endure immense psychological distress and caregiving stress throughout the prolonged and demanding treatment process,which can adversely affect their own well-being and caregiving capacity.However,the psychological mechanisms,such as the role of mindfulness,linking caregiver stress to parental coping strategies remain underexplored,and evidence-based interventions to support these parents are needed.Methods:In Study 1,we administered a cross-sectional survey to 242 parents of children with leukemia who were hospitalized at the Affiliated Hospital of Qingdao University between January and August 2024.Participants completed measures assessing caregiver burden,mindful attention awareness,and parental coping style.In Study 2,we further evaluated the effects of a Mindfulness-Based Stress Reduction(MBSR)intervention.Results:The results of Study 1 revealed:(1)The caregiving stress significantly and negatively predicted coping style(β=−1.18,95%CI[−2.18,−0.18],p<0.01).(2)Caregiving stress also significantly and negatively predicted mindfulness(β=−1.90,95%CI[−2.43,−1.38],p<0.01).(3)Conversely,mindfulness significantly and positively predicted coping style(β=0.85,95%CI[0.62,1.07],p<0.01).These findings suggest that mindfulness mediates the relationship between caregiver burden and coping style.In Study 2,the experimental group showed a significant decrease in caregiver stress post-intervention(t=2.24,p<0.05),a significant increase in mindfulness(t=−4.61,p<0.001),and a significant improvement in coping style(t=−2.36,p<0.01).No significant changes were observed in the control group.Conclusion:MBSR can effectively enhance mindfulness and promote adaptive coping strategies,while reducing caregiver burden among parents of children with leukemia.
基金supports from the National Natural Science Foundation of China(Grant Nos.12305372 and 22376217)the National Key Research&Development Program of China(Grant Nos.2022YFA1603802 and 2022YFB3504100)+1 种基金the projects of the key laboratory of advanced energy materials chemistry,ministry of education(Nankai University)key laboratory of Jiangxi Province for persistent pollutants prevention control and resource reuse(2023SSY02061)are gratefully acknowledged.
文摘Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.
基金supported by the National Natural Science Foundation of China(32172257)the Ministry of Science and Technology of the People’s Republic of China(DL2022163005L)+2 种基金the Science and Technology Program of Qingyuan(2022KJJH018)the Postdoctoral Innovative Talent Support Program(BX20230130)the 111 Project(B17018).
文摘The changes and gastric digestive properties of gel were investigated for oxidiz ed myofibrillar protein(MP)(0–1 mmol/L H_(2)O_(2))treated by 30%substitution of NaCl with KCl,MgCl_(2),and KCl/MgCl_(2).Mild oxidation level(0.3 mmol/L H_(2)O_(2))facilitated the protein unfolding,and MgCl_(2)obviously intervened the protein selfassembly by forming the salt bridge and more disulfide bonds.At the same oxidation concentration,the sodium-reduced MP substituted with KCl formed dense network structure with better gel strength(increased by 6%–18%)and water retention in comparision to the gel without sodium reduction.The KCl-substituted gel chewing work was also relatively higher among the low-sodium samples at the first chewing cycle.Reversely,the relatively soft structure and lower gel viscosity in simulated oral chewing were found in MgCl_(2)-substituted gel.These changes decreased the contact limit between pepsin and protein for better gastric disintegration or pepsin diffusivity,and increased the proportion of small molecular weight peptides(25.83%,<5 kDa).Therefore,partial substitution of NaCl with other salt replacers could influence the physicochemical properties of low-sodium MP suspension or gel under different oxidation degree and the subsequent gastric digestion characteristics.
基金funded by National Natural Science Foundation of China(Nos.12402142,11832013 and 11572134)Natural Science Foundation of Hubei Province(No.2024AFB235)+1 种基金Hubei Provincial Department of Education Science and Technology Research Project(No.Q20221714)the Opening Foundation of Hubei Key Laboratory of Digital Textile Equipment(Nos.DTL2023019 and DTL2022012).
文摘Owing to their global search capabilities and gradient-free operation,metaheuristic algorithms are widely applied to a wide range of optimization problems.However,their computational demands become prohibitive when tackling high-dimensional optimization challenges.To effectively address these challenges,this study introduces cooperative metaheuristics integrating dynamic dimension reduction(DR).Building upon particle swarm optimization(PSO)and differential evolution(DE),the proposed cooperative methods C-PSO and C-DE are developed.In the proposed methods,the modified principal components analysis(PCA)is utilized to reduce the dimension of design variables,thereby decreasing computational costs.The dynamic DR strategy implements periodic execution of modified PCA after a fixed number of iterations,resulting in the important dimensions being dynamically identified.Compared with the static one,the dynamic DR strategy can achieve precise identification of important dimensions,thereby enabling accelerated convergence toward optimal solutions.Furthermore,the influence of cumulative contribution rate thresholds on optimization problems with different dimensions is investigated.Metaheuristic algorithms(PSO,DE)and cooperative metaheuristics(C-PSO,C-DE)are examined by 15 benchmark functions and two engineering design problems(speed reducer and composite pressure vessel).Comparative results demonstrate that the cooperative methods achieve significantly superior performance compared to standard methods in both solution accuracy and computational efficiency.Compared to standard metaheuristic algorithms,cooperative metaheuristics achieve a reduction in computational cost of at least 40%.The cooperative metaheuristics can be effectively used to tackle both high-dimensional unconstrained and constrained optimization problems.
