To ensure the safe transportation of radioactive materials,numerous countries have established specific standards.For the transfer of fissile materials,it is imperative that the material within the packaging remains i...To ensure the safe transportation of radioactive materials,numerous countries have established specific standards.For the transfer of fissile materials,it is imperative that the material within the packaging remains in a subcritical state during routine,normal,and accidental transport conditions.In the event of an accident,the rods within the storage tank may become rearranged,introducing uncertainty that must be accounted for to ensure that criticality analysis results are conservative.Historically,this uncertainty was addressed overly conservatively due to limited research on non-uniform arrangement scenarios,which proved unsuitable for criticality safety analysis of spent fuel packages.This paper introduced three distinct methods to non-uniformly rearrange fuel rods—Uniform Arrangement by Blocks,Layer-by-Layer Determination,and Birdcage Deformation—and meticulously evaluates the influences of rod rearrangement on the effective multiplication factor of neutrons,k eff,utilizing the Monte Carlo method.Ultimately,this study presents a holistic method capable of encompassing the entire spectrum of potential effects stemming from the rearrangement of fuel rods during rods mispositioning accident.By augmenting the safety margin,this approach proves to be adeptly suited for the criticality safety analysis of nuclear fuel transport containers.展开更多
This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0...This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.展开更多
Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy a...Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy and renewable electricity.As a key component,efficient oxygen electrocatalyst for promoting sluggish reaction kinetics of oxygen reduction and evolution reaction(ORR and OER)under harsh operation conditions severely limited progress of these devices.Among various candidates,Ptgroup(Pt,Ir,and Ru)-based electrocatalysts are still the most active ORR/OER catalysts.However,the scarcity,high cost,and questionable stability restrict the widespread applications and the commercialization of PEMWE/PEMFC.Progresses in synthesizing atomically dispersed single/multiple-atom catalysts(SACs/MACs)offer new opportunities to Pt-group ORR/OER catalysts owing to nearly 100% metal utilization and high catalytic activities.Extensive efforts have been continuously devoted to optimizing the local structure of Pt-group OER/ORR catalysts at atom-level for further enhancing stability and activity.In this review,universal synthesis methods to prepare Ptgroup SACs are discussed first,highlighting crucial factors which affect the structure and catalytic performance.Afterward,advanced characterization techniques for directly confirming atomic dispersed metal atoms were introduced,including aberration-corrected high-angle-annular-dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy.Importantly,considerations for rational catalyst design and typical Pt-group SACs/MACs are summarized regarding the regulation strategy of atomically dispersed metal sites and various supports,and effects of metal-support interaction on the catalytic performance.Finally,key challenges and proposed perspectives for future development of atomically dispersed Pt-group oxygen electrocatalysts for fuel cell and electrolyzer are briefly discussed.展开更多
The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in a...The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in alcohol systems,we propose a rational catalyst design strategy focusing on morphological and compositional optimization.Sodium borohydride-derived PtCuMo alloy aerogels(AA)exhibit abundant grain boundary defects,while solvothermally prepared nanowire arrays(NA)maintain excellent single-crystalline characteristics.Density functional theory calculations demonstrate that engineered grain boundaries can effectively broaden the adsorption energy window for key reaction intermediates,enabling superior adaptability to diverse catalytic pathways.By precisely controlling Cu content,we identified Pt_(3)Cu_(3)Mo_(0.5)AA as the optimal catalyst configuration,demonstrating 150% enhancement in methanol oxidation reaction activity compared to Pt_(3)Cu_(6)Mo_(0.5)NA(1.5 vs.0.6 A·mg_(Pt)^(-1))and 17% improvement in ethanol oxidation reaction performance versus Pt_(3)Cu_(1)Mo_(0.5)NA(0.82 vs.0.70 A·mg_(Pt)^(-1)).Practical application testing using gas diffusion electrodes(anode loading:0.85 mg_(Pt)·cm^(-2))achieved a mass-specific power density of 14.14 W·g_(Pt)^(-1)in 1:1 methanol/ethanol blends,representing a 3.5-fold improvement over commercial Pt/C benchmarks.This work establishes a fundamental framework for developing highperformance,broad-spectrum electrocatalysts in advanced fuel cell systems.展开更多
Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy convers...Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.展开更多
Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety...Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety.The objective of this study is to design a subcritical reactor using a pressurized water reactor(PWR)conventional fuel following two safety points.In the first approach,deeply placed SCR cores with an infinite multiplication factor(k_(∞))of less than unity were identified using the DRAGON lattice code.In the second approach,subcritical reactor cores with an effective multiplication factor(k_(eff))of less than unity were determined by coupling the cell calculations of the DRAGON lattice code and core calculations of the DONJON code.For the deeply subcritical reactor design,it was found that the reactor would remain inherently subcritical while using fuel rods with ^(235)U enrichment of up to 0.9%,regardless of the pitch of the fuel rods.In the second approach,the optimal pitches(1.3 to 2.3 cm)were determined for different fuel enrichment values from 1 to 5%.Subsequently,the k_(eff) was obtained for a fuel rod arrangement of 8×8 to 80×80,and the states in which the reactor would be subcritical were determined for different fuel enrichments at the corresponding optimal pitch.To validate the models used in the DRAGON and DONJON codes,the k_(eff) of the Isfahan Light Water Subcritical Reactor(LWSCR)was experimentally measured and compared with the results of the calculations.Finally,the effects of fuel and moderator temperature changes were investigated to ensure that the designed assemblies remained in the subcritical state at all operational temperatures.展开更多
Although intermediate temperature solid oxide fuel cells(IT-SOFCs)show great potential to address energy conversion challenges,the sluggish oxygen reduction reaction(ORR)kinetics of cathode materials has severely hind...Although intermediate temperature solid oxide fuel cells(IT-SOFCs)show great potential to address energy conversion challenges,the sluggish oxygen reduction reaction(ORR)kinetics of cathode materials has severely hindered extended applications.Herein,we have demonstrated that Bi^(3+)doping on the A-site synergistically regulates the phase transition and electron spin state in La_(0.3)Bi_(0.3)Ca_(0.4)FeO_(3-δ)(LBCF3)for improved performance.An orthorhombic to cubic phase transition occurred with Bi^(3+)doping increases oxygen vacancy concentration and thus increases oxygen ion migration capacity.Simultaneously,the change of Fe from low to medium electron spin state strengths O_(2)adsorption and improves catalytic performances.Consequently,a peak power density improvement up to 48%(from 1.21 to 1.79 W·cm^(-2))at 800℃ is realized in the anodesupported single cell using LBCF3 as cathode,which remains stable for over 270 h at 750℃.展开更多
Modern aircraft tend to use fuel thermal management systems to cool onboard heat sources.However,the design of heat transfer architectures for fuel thermal management systems relies on the experience of the engineers ...Modern aircraft tend to use fuel thermal management systems to cool onboard heat sources.However,the design of heat transfer architectures for fuel thermal management systems relies on the experience of the engineers and lacks theoretical guidance.This paper proposes a concise graph representation method based on graph theory for fuel thermal management systems,which can represent all possible connections between subsystems.A generalized optimization algorithm is proposed for fuel thermal management system architecture to minimize the heat sink.This algorithm can autonomously arrange subsystems with heat production differences and efficiently utilize the architecture of the fuel heat sink.At the same time,two evaluation indices are proposed from the perspective of subsystems.These indices intuitively and clearly show that the reason for the high efficiency of heat sink utilization is the balanced and moderate cooling of each subsystem and verify the rationality of the architecture optimization method.A set of simulations are also conducted,which demonstrate that the fuel tank temperature has no effect on the performance of the architecture.This paper provides a reference for the architectural design of aircraft fuel thermal management systems.The metrics used in this paper can also be utilized to evaluate the existing architecture.展开更多
Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it ...Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it is necessary for the quality of hydrogen to adhere to the standards set by ISO 14687:2019,which sets maximum limits for 14 impurities in hydrogen,aiming to prevent any degradation of fuel cell performance.Ammonia(NH_(3))is a prominent pollutant in fuel cells,and accurate measurements of its concentration are crucial for hydrogen fuel cell quantity.In this study,a novel detection platform was developed for determining NH_(3)in real hydrogen samples.The online analysis platform integrates a self-developed online dilution module with a Fourier transform infrared spectrometer(ODM-FTIR).The ODM-FTIR can be operated fully automatically with remote operation.Under the optimum conditions,this method achieved a wide linear range between(50∼1000)nmol/mol.The limit of detection(LOD)was as low as 2 nmol/mol with a relative standard deviation(RSD,n=7)of 3.6%at a content of 50 nmol/mol.To ensure that the quality of the hydrogen products meets the requirement of proton exchange membrane fuel cell vehicles(PEMFCV),the developed ODM-FTIR system was applied to monitor the NH_(3)content in Chengdu Hydrogen Energy Co.,Ltd.for 21 days during Chengdu 2021 FISU World University Games.The proposed method retains several unique advantages,including a low detection limit,excellent repeatability,high accuracy,high speed,good stability,and calibration flexibility.It is an effective analytical method for accurately quantifying NH_(3)in hydrogen,especially suitable for online analysis.It also provides a new idea for the analysis of other impurity components in hydrogen.展开更多
This paper provides a comprehensive review of various experimental methods used to study carbon corrosion in automotive polymer exchange membrane fuel cells.Quantifying the extent of carbon corrosion is essential for ...This paper provides a comprehensive review of various experimental methods used to study carbon corrosion in automotive polymer exchange membrane fuel cells.Quantifying the extent of carbon corrosion is essential for advancing the technology and implementing effective mitigation strategies.While studying degradation events directly within a real-world fuel cell vehicle offers the most reliable insights,the high costs and time demands make it necessary to develop specialised experimental techniques that provide high-resolution data more efficiently and cost-effectively.This review explores the various experimental approaches utilised in automotive application induced carbon corrosion studies globally,including load profiles,test setups,break-in procedures,and cell recovery protocols.In this paper,emphasis is placed on the standardised procedures proposed by leading institutions worldwide,accompanied by critical discussions on these protocols.Furthermore,the paper highlights modified or innovative procedures developed by smaller institutions,universities,and individual researchers,thereby offering a comprehensive overview essential for carbon corrosion analysis.The review also discusses the fundamental principles,benefits,and limitations of various procedures,offering guidance on selecting the most appropriate approach for a given study.Lastly,it addresses the limitations within the current body of literature and outlines potential future prospects.展开更多
Developing low-cost and high-performance nanofiber-based polyelectrolyte membranes for fuel cell applications is a promising solution to energy depletion.Due to the high specific surface area and one-dimensional longr...Developing low-cost and high-performance nanofiber-based polyelectrolyte membranes for fuel cell applications is a promising solution to energy depletion.Due to the high specific surface area and one-dimensional longrange continuous structure of the nanofiber,ion-charged groups can be induced to form long-range continuous ion transfer channels in the nanofiber composite membrane,significantly increasing the ion conductivity of the membrane.This review stands apart from previous endeavors by offering a comprehensive overview of the strategies employed over the past decade in utilizing both electrospun and natural nanofibers as key components of proton exchange membranes and anion exchange membranes for fuel cells.Electrospun nanofibers are categorized based on their material properties into two primary groups:(1)ionomer nanofibers,inherently endowed with the ability to conduct H+(such as perfluorosulfonic acid or sulfonated poly(ether ether ketone))or OH-(e.g.,FAA-3),and(2)nonionic polymer nanofibers,comprising inert polymers like polyvinylidene difluoride,polytetrafluoroethylene,and polyacrylonitrile.Notably,the latter often necessitates surface modifications to impart ion transport channels,given their inherent proton inertness.Furthermore,this review delves into the recent progress made with three natural nanofibers derived from biodegradable cellulose—cellulose nanocrystals,cellulose nanofibers,and bacterial nanofibers—as crucial elements in polyelectrolyte membranes.The effect of the physical structure of such nanofibers on polyelectrolyte membrane properties is also briefly discussed.Lastly,the review emphasizes the challenges and outlines potential solutions for future research in the field of nanofiber-based polyelectrolyte membranes,aiming to propel the development of high-performance polymer electrolyte fuel cells.展开更多
Objective Burning solid cooking fuel contributes to household air pollution and is associated with frailty.However,how solid cooking fuel use contributes to the development of frailty has not been well illustrated.Met...Objective Burning solid cooking fuel contributes to household air pollution and is associated with frailty.However,how solid cooking fuel use contributes to the development of frailty has not been well illustrated.Methods This study recruited 8,947 participants aged≥45 years from the China Health and Retirement Longitudinal Study,2011–2018.Group-based trajectory modeling was employed to identify frailty trajectories.Multinomial logistic regression was used to assess the association between solid cooking fuel use and frailty trajectories.Population-attributable fractions were used to estimate the frailty burden from solid fuel use.Results We identified three frailty trajectories:low-stable(n=5,789),moderate-increasing(n=2,603),and fast-increasing(n=555).Solid fuel use was associated with higher odds of being in the moderate-increasing(OR:1.24,95%CI:1.08–1.42)and fast-increasing(OR:1.48,95%CI:1.14–1.92)trajectories.These associations were strengthened by longer solid fuel use(P for trend<0.001).Switching to clean fuel significantly reduced the risk of being in these trajectories compared with persistent solid fuel users.Without solid fuel,8%of moderate-and 19%of fast-increasing trajectories demonstrated frailty development like the low-stable group.Conclusion Solid cooking fuel use is associated with frailty trajectories in middle-aged and older Chinese populations.展开更多
Minimizing the thermal expansion coefficient(TEC)mismatch between the cathode and electrolyte in solid oxide fuel cells is crucial for achieving stable,durable operation and high performance.Recently,materials with ne...Minimizing the thermal expansion coefficient(TEC)mismatch between the cathode and electrolyte in solid oxide fuel cells is crucial for achieving stable,durable operation and high performance.Recently,materials with negative thermal expansion(NTE)have at-tracted significant attention as effective additives for tailoring the thermomechanical properties of electrodes and enhancing cell durability.In this work,for the first time,single-phase NTE perovskite Sm_(0.85)Zn_(0.15)MnO_(3−δ)(SZM15)was successfully synthesized via the sol-gel method,eliminating the unwanted ZnO phase typically observed in materials obtained through the conventional solid-state reaction route.The sol-gel approach proved highly advantageous,offering low cost,robustness,excellent chemical homogeneity,precise compositional control,and high phase purity.After optimization of synthesis parameters,a negative TEC of approximately−6.5×10^(−6)K^(−1)was achieved in the 400-850℃range.SZM15 was then incorporated as an additive(10wt%-50wt%)into a SmBa0.5Sr0.5CoCuO_(5+δ)(SBSCCO)cathode to tune the thermomechanical properties with a La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(0.2)O_(3−δ)(LSGM)electrolyte,achieving a minimal TEC mismatch of only 1%.Notably,the SBSCCO+10wt%SZM15 composite cathode exhibited the lowest polarization resistance of 0.019Ω·cm^(2)at 900℃,showing approximately 70%lower than that of the pristine cathode.Excellent long-term stability after 100 h of operation was achieved.In addition,a high peak power density of 680 mW·cm^(−2)was achieved in a Ni-YSZ(yttria-stabilized zirconia)|YSZ|Ce_(0.9)Gd_(0.1)O_(2−δ)(GDC10)|SBSCCO+10wt%SZM15 anode-supported fuel cell at 850℃,highlighting the effectiveness of incorporating NTE materials as a promising strategy for regulating the thermomechanical properties and improving the long-term stability of intermediate temperature solid oxide fuel cells(IT-SOFCs).展开更多
3D printing technology enhances the combustion characteristics of hybrid rocket fuels by enabling complex geometries. However, improvements in regression rates and energy properties of monotonous 3D printed fuels have...3D printing technology enhances the combustion characteristics of hybrid rocket fuels by enabling complex geometries. However, improvements in regression rates and energy properties of monotonous 3D printed fuels have been limited. This study explores the impact of poly(vinylidene fluoride) and polydopamine-coated aluminum particles on the thermal and combustion properties of 3D printed hybrid rocket fuels. Physical self-assembly and anti-solvent methods were employed for constructing composite μAl particles. Characterization using SEM, XRD, XPS, FTIR, and μCT revealed a core-shell structure and homogeneous elemental distribution. Thermal analysis showed that PVDF coatings significantly increased the heat of combustion for aluminum particles, with maximum enhancement observed in μAl@PDA@PVDF(denoted as μAl@PF) at 6.20 k J/g. Subsequently, 3D printed fuels with varying pure and composite μAl particle contents were prepared using 3D printing. Combustion tests indicated higher regression rates for Al@PF/Resin composites compared to pure resin, positively correlating with particle content. The fluorocarbon-alumina reaction during the combustion stage intensified Al particle combustion, reducing residue size. A comprehensive model based on experiments provides insights into the combustion process of PDA and PVDF-coated droplets. This study advances the design of 3D-printed hybrid rocket fuels, offering strategies to improve regression rates and energy release, crucial for enhancing solid fuel performance for hybrid propulsion.展开更多
Hydrogen fuel cells are expected to play a central role in the next-generation energy paradigm.However,owing to practical limitations,hydrogen is supplied in the form of refined hydrocarbons or alcohols in industrial ...Hydrogen fuel cells are expected to play a central role in the next-generation energy paradigm.However,owing to practical limitations,hydrogen is supplied in the form of refined hydrocarbons or alcohols in industrial applications.Among them,methanol is widely used as a hydrogen source,and CO is inevitably generated during its oxidation process.Even a small amount of CO(∼20 ppm)strongly binds to Pt used as a catalyst,and deactivates it.In addition to CO,surface adsorption of organic cations by binder or ionomer use in alkaline fuel cells is also one of the poisoning issues to be overcome.Herein,we propose FePt bimetallic catalysts that can resist unavoidable CO and organic cation poisoning.Our synthetic strategy,including annealing and acid treatment,allows the catalysts to possess different alloying degrees and surface structures,which in turn induce different levels of resistance to CO and organic-cation poisonings.The correlation between the surface and bulk structures of the catalysts and poisoning resistance was elucidated through X-ray photoemission spectroscopy and electrochemical analysis.The results revealed that an FePt catalyst having an ordered atomic arrangement displayed a better poisoning resistance than that having a disordered arrangement.展开更多
The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels...The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels and background variability,particularly owing to the influence of terrestrial biospheric fluxes.This necessitates the development of a regional inversion methodology based on atmospheric CO_(2)observations to verify bottom-up estimations independently.This study presents a promising approach for estimating China's FFCO_(2)emissions by incorporating the model residual errors(MREs)of the column-averaged dry-air mole fractions of CO_(2)(XCO_(2))from FFCO_(2)emissions(MREff)retained in the analysis of natural flux optimization.China's FFCO_(2)emissions during the COVID-19 lockdown in 2020 are estimated using the GEOS-Chem adjoint model.The relationship between the MREff and FFCO_(2)is determined using the model based on a regional FFCO_(2)anomaly suggested by posterior NOx emissions from air-quality data assimilation.The MREff is typically one-tenth in magnitude,but some positively skewed outliers exceed 1 ppm because the prior emissions lack lockdown impacts,thereby exerting considerable observation forcing given the satellite retrieval uncertainties.We initialize the FFCO_(2)with posterior NOx emissions and optimize the colinear emission ratio.Synthetic data experiments demonstrate that this approach reduces the FFCO_(2)bias to less than 10%.The real-data experiments estimate 19%lower FFCO_(2)with GOSAT XCO_(2)and 26%lower with OCO-2 XCO_(2)than the bottom-up estimations.This study proves the feasibility of our regional FFCO_(2)inversion,highlighting the importance of addressing the outlier behaviors observed in satellite XCO_(2)retrievals.展开更多
Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon ele...Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon electrocatalyst(M-N-C)is considered an effective alternative to precious metal catalysts.However,its relatively poor performance in acidic environments has always been a problem plaguing its practical application in PEMFCs.This study presents a sequential deposition methodology for constructing a composite catalytic system of Fe-N-C and ionic liquid(IL),which exhibits improved performance at both half-cell and membrane electrode assembly scales.The presence of IL significantly inhibits H_(2)O_(2)production,preferentially promoting the 4e–O_(2)reduction reaction,resulting in improved electrocatalytic activity and stability.Additionally,the enhanced PEMFC performance of IL containing electrodes is a direct result of the improved ionic and reactant accessibility of the pore confined Fe-N-C catalysts where the IL minimizes local resistive transport losses.This study establishes a strategic foundation for the practical utilization of non-precious metal catalysts in PEMFCs and other energy converting technologies.展开更多
Photoinduced[2+2]cycloaddition of biomass-derived cycloolefin is a promising approach to synthesize high-energy bio-fuels,however,the conversion efficiency and selectivity are still low.Herein,we provide an acid-promo...Photoinduced[2+2]cycloaddition of biomass-derived cycloolefin is a promising approach to synthesize high-energy bio-fuels,however,the conversion efficiency and selectivity are still low.Herein,we provide an acid-promoted photocycloaddition approach to synthesize a new kind of spiral fuel from biomass-derived cyclohexanone (CHOE) and camphene (CPE).BrΦnsted acids show higher catalytic activity than Lewis acids,and acetic acid (HOAc) possesses the best catalytic performance,with CHOE conversion up to 99.1%.Meanwhile,the HOAc-catalytic effect has been confirmed for[2+2]photocycloaddition of other biomass-derived ketenes and olefins.The catalytic mechanism and dynamics have been investigated,and show that HOAc can bond with C=O groups of CHOE to form H–CHOE complex,which leads to higher light adsorption and longer triplet lifetime.Meanwhile,H–CHOE complex reduces the energy gap between CHOE LUMO and CPE HOMO,shortens the distance of ring-forming atoms,and then decreases the energy barrier (from 103.3 kcal mol^(-1)to 95.8 kcal mol^(-1)) of rate-limiting step.After hydrodeoxygenation,the targeted bio-spiral fuel shows high density of 0.992 g cm^(-3),high neat heat of combustion of 41.89 MJ L^(-1),low kinetic viscosity of 5.69 mm^(2)s^(-1)at 20℃,which is very promising to serve as high-performance aerospace fuel.展开更多
Atomically dispersed metal site(ADMS)materials have emerged as a promising class of materials for electrocatalysis reactions in the field of energy conversion.Characterized by individual metal atoms dispersed on suita...Atomically dispersed metal site(ADMS)materials have emerged as a promising class of materials for electrocatalysis reactions in the field of energy conversion.Characterized by individual metal atoms dispersed on suitable supports,ADMS materials provide unique catalytic sites with highly tunable electronic structures.This review summarizes recent advancements in the field,with a focus on the critical roles of support materials,coordination environments,and the mechanisms underlying catalytic activity at the atomic level.First,commonly used density functional theory(DFT)simulations are reviewed,emphasizing their pivotal role in elucidating reaction mechanisms and predicting the behavior of ADMS in electrochemical reactions for hydrogen energy utilization.Then,advancements in ADMS for half-cell electrochemical reactions,including oxygen evolution reaction,hydrogen evolution reaction,and oxygen reduction reaction,as well as their applications in fuel cells and water splitting,are summarized.Finally,the challenges and future prospects of ADMS are discussed.This review underscores the transformative potential of ADMS in electrocatalysis,paving the way for innovative and sustainable energy conversion technologies.展开更多
The commercialization of solid oxide fuel cells depends on the cathode,which possesses both high catalytic activity and a thermal-expansion coefficient(TEC)that aligns with the electrolyte.Although the cobalt-based ca...The commercialization of solid oxide fuel cells depends on the cathode,which possesses both high catalytic activity and a thermal-expansion coefficient(TEC)that aligns with the electrolyte.Although the cobalt-based cathode La_(0.6)Sr_(0.4)CoO_(3)(LSC)offers excellent catalytic performance,its TEC is significantly larger than that of the electrolyte.In this study,we mechanically mix Sm_(0.2)Ce_(0.8)O_(2−δ)(SDC)with LSC to create a composite cathode.By incorporating 50wt%SDC,the TEC decreases significantly from 18.29×10^(−6) to 13.90×10^(−6) K^(−1).Under thermal-shock conditions ranging from room temperature to 800℃,the growth rate of polarization resistance is only 0.658%per cycle,i.e.,merely 49%that of pure LSC.The button cell comprising the LSC-SDC composite cathode operates stably for over 900 h without Sr segregation,with a voltage growth rate of 1.11%/kh.A commercial flat-tube cell(active area:70 cm^(2))compris-ing the LSC-SDC composite cathode delivers 54.8 W at 750℃.The distribution of relaxation-time shows that the non-electrode portion is the main rate-limiting step.This study demonstrates that the LSC-SDC mixture strategy effectively improves the compatibility with the electrolyte while maintaining a high output,thus rendering it a promising commercial cathode material.展开更多
文摘To ensure the safe transportation of radioactive materials,numerous countries have established specific standards.For the transfer of fissile materials,it is imperative that the material within the packaging remains in a subcritical state during routine,normal,and accidental transport conditions.In the event of an accident,the rods within the storage tank may become rearranged,introducing uncertainty that must be accounted for to ensure that criticality analysis results are conservative.Historically,this uncertainty was addressed overly conservatively due to limited research on non-uniform arrangement scenarios,which proved unsuitable for criticality safety analysis of spent fuel packages.This paper introduced three distinct methods to non-uniformly rearrange fuel rods—Uniform Arrangement by Blocks,Layer-by-Layer Determination,and Birdcage Deformation—and meticulously evaluates the influences of rod rearrangement on the effective multiplication factor of neutrons,k eff,utilizing the Monte Carlo method.Ultimately,this study presents a holistic method capable of encompassing the entire spectrum of potential effects stemming from the rearrangement of fuel rods during rods mispositioning accident.By augmenting the safety margin,this approach proves to be adeptly suited for the criticality safety analysis of nuclear fuel transport containers.
基金financially supported by the National Natural Science Foundation of China(No.22309067)the Open Project Program of the State Key Laboratory of Materials-Oriented Chemical Engineering,China(No.KL21-05)the Marine Equipment and Technology Institute,Jiangsu University of Science and Technology,China(No.XTCX202404)。
文摘This study focused on improving the cathode performance of Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.15)O_(3-δ)(BSCN)-based perovskite materials through molybdenum(Mo)doping.Pure BSCN and Mo-modified-BSCN—Ea_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.1)Mo_(0.05)O_(3-δ)(B S CNM_(0.05)),Ba_(0.6)Sr_(0.4)Co_(0.85)Nb_(0.05)Mo_(0.1)O_(3-δ)(BSCNM_(0.1)),and Ba_(0.6)Sr_(0.4)Co_(0.85)Mo_(0.15)O_(3-δ)(BSCM)—with Mo doping contents of 5mol%,10mol%,and15mol%,respectively,were successfully prepared using the sol-gel method.The effects of Mo doping on the crystal structure,conductivity,thermal expansion coefficient,oxygen reduction reaction(ORR)activity,and electrochemical performance were systematically evaluated using X-ray diffraction analysis,thermally induced characterization,electrochemical impedance spectroscopy,and single-cell performance tests.The results revealed that Mo doping could improve the conductivity of the materials,suppress their thermal expansion effects,and significantly improve the electrochemical performance.Surface chemical state analysis using X-ray photoelectron spectroscopy revealed that 5mol%Mo doping could facilitate a high adsorbed oxygen concentration leading to enhanced ORR activity in the materials.Density functional theory calculations confirmed that Mo doping promoted the ORR activity in the materials.At an operating temperature of 600℃,the BSCNM_(0.05)cathode material exhibited significantly enhanced electrochemical impedance characteristics,with a reduced area specific resistance of 0.048Ω·cm~2,which was lower than that of the undoped BSCN matrix material by 32.39%.At the same operating temperature,an anode-supported single cell using a BSCNM_(0.05)cathode achieved a peak power density of 1477 mW·cm^(-2),which was 30.71%,56.30%,and 171.50%higher than those of BSCN,BSCNM_(0.1),and B SCM,respectively.The improved ORR activity and electrochemical performance of BSCNM_(0.05)indicate that it can be used as a cathode material in low-temperature solid oxide fuel cells.
基金supported by the National Key Research and Development Program of China(No.2021YFB4000603)the National Natural Science Foundation of China(Nos.52273277 and U24A2062)+2 种基金Jilin Province Science and Technology Development Plan Funding Project(No.SKL202302039)Youth Innovation Promotion Association CAS(No.2021223)funding from National Natural Science Foundation of China Outstanding Youth Science Foundation of China(Overseas).
文摘Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy and renewable electricity.As a key component,efficient oxygen electrocatalyst for promoting sluggish reaction kinetics of oxygen reduction and evolution reaction(ORR and OER)under harsh operation conditions severely limited progress of these devices.Among various candidates,Ptgroup(Pt,Ir,and Ru)-based electrocatalysts are still the most active ORR/OER catalysts.However,the scarcity,high cost,and questionable stability restrict the widespread applications and the commercialization of PEMWE/PEMFC.Progresses in synthesizing atomically dispersed single/multiple-atom catalysts(SACs/MACs)offer new opportunities to Pt-group ORR/OER catalysts owing to nearly 100% metal utilization and high catalytic activities.Extensive efforts have been continuously devoted to optimizing the local structure of Pt-group OER/ORR catalysts at atom-level for further enhancing stability and activity.In this review,universal synthesis methods to prepare Ptgroup SACs are discussed first,highlighting crucial factors which affect the structure and catalytic performance.Afterward,advanced characterization techniques for directly confirming atomic dispersed metal atoms were introduced,including aberration-corrected high-angle-annular-dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy.Importantly,considerations for rational catalyst design and typical Pt-group SACs/MACs are summarized regarding the regulation strategy of atomically dispersed metal sites and various supports,and effects of metal-support interaction on the catalytic performance.Finally,key challenges and proposed perspectives for future development of atomically dispersed Pt-group oxygen electrocatalysts for fuel cell and electrolyzer are briefly discussed.
基金financially supported by the National Natural Science Foundation of China(No.52073214)Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008).
文摘The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in alcohol systems,we propose a rational catalyst design strategy focusing on morphological and compositional optimization.Sodium borohydride-derived PtCuMo alloy aerogels(AA)exhibit abundant grain boundary defects,while solvothermally prepared nanowire arrays(NA)maintain excellent single-crystalline characteristics.Density functional theory calculations demonstrate that engineered grain boundaries can effectively broaden the adsorption energy window for key reaction intermediates,enabling superior adaptability to diverse catalytic pathways.By precisely controlling Cu content,we identified Pt_(3)Cu_(3)Mo_(0.5)AA as the optimal catalyst configuration,demonstrating 150% enhancement in methanol oxidation reaction activity compared to Pt_(3)Cu_(6)Mo_(0.5)NA(1.5 vs.0.6 A·mg_(Pt)^(-1))and 17% improvement in ethanol oxidation reaction performance versus Pt_(3)Cu_(1)Mo_(0.5)NA(0.82 vs.0.70 A·mg_(Pt)^(-1)).Practical application testing using gas diffusion electrodes(anode loading:0.85 mg_(Pt)·cm^(-2))achieved a mass-specific power density of 14.14 W·g_(Pt)^(-1)in 1:1 methanol/ethanol blends,representing a 3.5-fold improvement over commercial Pt/C benchmarks.This work establishes a fundamental framework for developing highperformance,broad-spectrum electrocatalysts in advanced fuel cell systems.
基金financially supported by the National Key R&D Program of China(No.2024YFF0506300)National Natural Science Foundation of China(No.52336009)+5 种基金Key Research and Development Program of Shaanxi(No.2024CY2-GJHX-66)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010429)Natural Science Basic Research Plan in Shaanxi Province of China(No.2024JC-YBQN-0475)Xidian University Specially Funded Project for Interdisciplinary Exploration(No.TZJH2024063)the Fundamental Research Funds for the Central Universities(No.QTZX23061)the Innovation Center of Nuclear Power Technology(No.HDLCXZX-2022-ZH-013).
文摘Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.
文摘Subcritical reactors(SCRs)or subcritical assemblies(SCAs)are the main infrastructure for designing power reactors.These reactors are widely used for training and research because of their high level of inherent safety.The objective of this study is to design a subcritical reactor using a pressurized water reactor(PWR)conventional fuel following two safety points.In the first approach,deeply placed SCR cores with an infinite multiplication factor(k_(∞))of less than unity were identified using the DRAGON lattice code.In the second approach,subcritical reactor cores with an effective multiplication factor(k_(eff))of less than unity were determined by coupling the cell calculations of the DRAGON lattice code and core calculations of the DONJON code.For the deeply subcritical reactor design,it was found that the reactor would remain inherently subcritical while using fuel rods with ^(235)U enrichment of up to 0.9%,regardless of the pitch of the fuel rods.In the second approach,the optimal pitches(1.3 to 2.3 cm)were determined for different fuel enrichment values from 1 to 5%.Subsequently,the k_(eff) was obtained for a fuel rod arrangement of 8×8 to 80×80,and the states in which the reactor would be subcritical were determined for different fuel enrichments at the corresponding optimal pitch.To validate the models used in the DRAGON and DONJON codes,the k_(eff) of the Isfahan Light Water Subcritical Reactor(LWSCR)was experimentally measured and compared with the results of the calculations.Finally,the effects of fuel and moderator temperature changes were investigated to ensure that the designed assemblies remained in the subcritical state at all operational temperatures.
基金supported by the Xinjiang Autonomous Region Key Research Project(No.2022D01D31)the Start-up Grant of Xinjiang University,the Basic Research Fund for Autonomous Region Universities(No.XJEDU2024P015)the Natural Science Foundation of Xinjiang Uygur Autonomous Region(No.2022D01C668).
文摘Although intermediate temperature solid oxide fuel cells(IT-SOFCs)show great potential to address energy conversion challenges,the sluggish oxygen reduction reaction(ORR)kinetics of cathode materials has severely hindered extended applications.Herein,we have demonstrated that Bi^(3+)doping on the A-site synergistically regulates the phase transition and electron spin state in La_(0.3)Bi_(0.3)Ca_(0.4)FeO_(3-δ)(LBCF3)for improved performance.An orthorhombic to cubic phase transition occurred with Bi^(3+)doping increases oxygen vacancy concentration and thus increases oxygen ion migration capacity.Simultaneously,the change of Fe from low to medium electron spin state strengths O_(2)adsorption and improves catalytic performances.Consequently,a peak power density improvement up to 48%(from 1.21 to 1.79 W·cm^(-2))at 800℃ is realized in the anodesupported single cell using LBCF3 as cathode,which remains stable for over 270 h at 750℃.
文摘Modern aircraft tend to use fuel thermal management systems to cool onboard heat sources.However,the design of heat transfer architectures for fuel thermal management systems relies on the experience of the engineers and lacks theoretical guidance.This paper proposes a concise graph representation method based on graph theory for fuel thermal management systems,which can represent all possible connections between subsystems.A generalized optimization algorithm is proposed for fuel thermal management system architecture to minimize the heat sink.This algorithm can autonomously arrange subsystems with heat production differences and efficiently utilize the architecture of the fuel heat sink.At the same time,two evaluation indices are proposed from the perspective of subsystems.These indices intuitively and clearly show that the reason for the high efficiency of heat sink utilization is the balanced and moderate cooling of each subsystem and verify the rationality of the architecture optimization method.A set of simulations are also conducted,which demonstrate that the fuel tank temperature has no effect on the performance of the architecture.This paper provides a reference for the architectural design of aircraft fuel thermal management systems.The metrics used in this paper can also be utilized to evaluate the existing architecture.
基金financial support by Sichuan Science and Technology,China(No.2023YFG0070).
文摘Fuel cell electric vehicles hold great promise for a diverse range of applications in reducing greenhouse gas emissions.In power fuel cell systems,hydrogen fuel serves as an energy vector.To ensure its suitability,it is necessary for the quality of hydrogen to adhere to the standards set by ISO 14687:2019,which sets maximum limits for 14 impurities in hydrogen,aiming to prevent any degradation of fuel cell performance.Ammonia(NH_(3))is a prominent pollutant in fuel cells,and accurate measurements of its concentration are crucial for hydrogen fuel cell quantity.In this study,a novel detection platform was developed for determining NH_(3)in real hydrogen samples.The online analysis platform integrates a self-developed online dilution module with a Fourier transform infrared spectrometer(ODM-FTIR).The ODM-FTIR can be operated fully automatically with remote operation.Under the optimum conditions,this method achieved a wide linear range between(50∼1000)nmol/mol.The limit of detection(LOD)was as low as 2 nmol/mol with a relative standard deviation(RSD,n=7)of 3.6%at a content of 50 nmol/mol.To ensure that the quality of the hydrogen products meets the requirement of proton exchange membrane fuel cell vehicles(PEMFCV),the developed ODM-FTIR system was applied to monitor the NH_(3)content in Chengdu Hydrogen Energy Co.,Ltd.for 21 days during Chengdu 2021 FISU World University Games.The proposed method retains several unique advantages,including a low detection limit,excellent repeatability,high accuracy,high speed,good stability,and calibration flexibility.It is an effective analytical method for accurately quantifying NH_(3)in hydrogen,especially suitable for online analysis.It also provides a new idea for the analysis of other impurity components in hydrogen.
文摘This paper provides a comprehensive review of various experimental methods used to study carbon corrosion in automotive polymer exchange membrane fuel cells.Quantifying the extent of carbon corrosion is essential for advancing the technology and implementing effective mitigation strategies.While studying degradation events directly within a real-world fuel cell vehicle offers the most reliable insights,the high costs and time demands make it necessary to develop specialised experimental techniques that provide high-resolution data more efficiently and cost-effectively.This review explores the various experimental approaches utilised in automotive application induced carbon corrosion studies globally,including load profiles,test setups,break-in procedures,and cell recovery protocols.In this paper,emphasis is placed on the standardised procedures proposed by leading institutions worldwide,accompanied by critical discussions on these protocols.Furthermore,the paper highlights modified or innovative procedures developed by smaller institutions,universities,and individual researchers,thereby offering a comprehensive overview essential for carbon corrosion analysis.The review also discusses the fundamental principles,benefits,and limitations of various procedures,offering guidance on selecting the most appropriate approach for a given study.Lastly,it addresses the limitations within the current body of literature and outlines potential future prospects.
基金National Natural Science Foundation of China,Grant/Award Numbers:52173091,62101391。
文摘Developing low-cost and high-performance nanofiber-based polyelectrolyte membranes for fuel cell applications is a promising solution to energy depletion.Due to the high specific surface area and one-dimensional longrange continuous structure of the nanofiber,ion-charged groups can be induced to form long-range continuous ion transfer channels in the nanofiber composite membrane,significantly increasing the ion conductivity of the membrane.This review stands apart from previous endeavors by offering a comprehensive overview of the strategies employed over the past decade in utilizing both electrospun and natural nanofibers as key components of proton exchange membranes and anion exchange membranes for fuel cells.Electrospun nanofibers are categorized based on their material properties into two primary groups:(1)ionomer nanofibers,inherently endowed with the ability to conduct H+(such as perfluorosulfonic acid or sulfonated poly(ether ether ketone))or OH-(e.g.,FAA-3),and(2)nonionic polymer nanofibers,comprising inert polymers like polyvinylidene difluoride,polytetrafluoroethylene,and polyacrylonitrile.Notably,the latter often necessitates surface modifications to impart ion transport channels,given their inherent proton inertness.Furthermore,this review delves into the recent progress made with three natural nanofibers derived from biodegradable cellulose—cellulose nanocrystals,cellulose nanofibers,and bacterial nanofibers—as crucial elements in polyelectrolyte membranes.The effect of the physical structure of such nanofibers on polyelectrolyte membrane properties is also briefly discussed.Lastly,the review emphasizes the challenges and outlines potential solutions for future research in the field of nanofiber-based polyelectrolyte membranes,aiming to propel the development of high-performance polymer electrolyte fuel cells.
基金supported by the National Natural Science Foundation of China(82222064,81973147)the National Key Research and Development Program(2022YFC2010100)the Shandong University Distinguished Young Scholars。
文摘Objective Burning solid cooking fuel contributes to household air pollution and is associated with frailty.However,how solid cooking fuel use contributes to the development of frailty has not been well illustrated.Methods This study recruited 8,947 participants aged≥45 years from the China Health and Retirement Longitudinal Study,2011–2018.Group-based trajectory modeling was employed to identify frailty trajectories.Multinomial logistic regression was used to assess the association between solid cooking fuel use and frailty trajectories.Population-attributable fractions were used to estimate the frailty burden from solid fuel use.Results We identified three frailty trajectories:low-stable(n=5,789),moderate-increasing(n=2,603),and fast-increasing(n=555).Solid fuel use was associated with higher odds of being in the moderate-increasing(OR:1.24,95%CI:1.08–1.42)and fast-increasing(OR:1.48,95%CI:1.14–1.92)trajectories.These associations were strengthened by longer solid fuel use(P for trend<0.001).Switching to clean fuel significantly reduced the risk of being in these trajectories compared with persistent solid fuel users.Without solid fuel,8%of moderate-and 19%of fast-increasing trajectories demonstrated frailty development like the low-stable group.Conclusion Solid cooking fuel use is associated with frailty trajectories in middle-aged and older Chinese populations.
基金supported by the research project within the program“Excellence Initiative-Research University”for the AGH University of Krakow(IDUB AGH,Action 21)Kun Zheng acknowledges financial support from AGH University of Krakow(No.16.16.210.476).
文摘Minimizing the thermal expansion coefficient(TEC)mismatch between the cathode and electrolyte in solid oxide fuel cells is crucial for achieving stable,durable operation and high performance.Recently,materials with negative thermal expansion(NTE)have at-tracted significant attention as effective additives for tailoring the thermomechanical properties of electrodes and enhancing cell durability.In this work,for the first time,single-phase NTE perovskite Sm_(0.85)Zn_(0.15)MnO_(3−δ)(SZM15)was successfully synthesized via the sol-gel method,eliminating the unwanted ZnO phase typically observed in materials obtained through the conventional solid-state reaction route.The sol-gel approach proved highly advantageous,offering low cost,robustness,excellent chemical homogeneity,precise compositional control,and high phase purity.After optimization of synthesis parameters,a negative TEC of approximately−6.5×10^(−6)K^(−1)was achieved in the 400-850℃range.SZM15 was then incorporated as an additive(10wt%-50wt%)into a SmBa0.5Sr0.5CoCuO_(5+δ)(SBSCCO)cathode to tune the thermomechanical properties with a La_(0.8)Sr_(0.2)Ga_(0.8)Mg_(0.2)O_(3−δ)(LSGM)electrolyte,achieving a minimal TEC mismatch of only 1%.Notably,the SBSCCO+10wt%SZM15 composite cathode exhibited the lowest polarization resistance of 0.019Ω·cm^(2)at 900℃,showing approximately 70%lower than that of the pristine cathode.Excellent long-term stability after 100 h of operation was achieved.In addition,a high peak power density of 680 mW·cm^(−2)was achieved in a Ni-YSZ(yttria-stabilized zirconia)|YSZ|Ce_(0.9)Gd_(0.1)O_(2−δ)(GDC10)|SBSCCO+10wt%SZM15 anode-supported fuel cell at 850℃,highlighting the effectiveness of incorporating NTE materials as a promising strategy for regulating the thermomechanical properties and improving the long-term stability of intermediate temperature solid oxide fuel cells(IT-SOFCs).
基金funded by the National Natural Science Foundation of China(Grant No.06101213)the National Natural Science Foundation of China(Grant No.22105160).
文摘3D printing technology enhances the combustion characteristics of hybrid rocket fuels by enabling complex geometries. However, improvements in regression rates and energy properties of monotonous 3D printed fuels have been limited. This study explores the impact of poly(vinylidene fluoride) and polydopamine-coated aluminum particles on the thermal and combustion properties of 3D printed hybrid rocket fuels. Physical self-assembly and anti-solvent methods were employed for constructing composite μAl particles. Characterization using SEM, XRD, XPS, FTIR, and μCT revealed a core-shell structure and homogeneous elemental distribution. Thermal analysis showed that PVDF coatings significantly increased the heat of combustion for aluminum particles, with maximum enhancement observed in μAl@PDA@PVDF(denoted as μAl@PF) at 6.20 k J/g. Subsequently, 3D printed fuels with varying pure and composite μAl particle contents were prepared using 3D printing. Combustion tests indicated higher regression rates for Al@PF/Resin composites compared to pure resin, positively correlating with particle content. The fluorocarbon-alumina reaction during the combustion stage intensified Al particle combustion, reducing residue size. A comprehensive model based on experiments provides insights into the combustion process of PDA and PVDF-coated droplets. This study advances the design of 3D-printed hybrid rocket fuels, offering strategies to improve regression rates and energy release, crucial for enhancing solid fuel performance for hybrid propulsion.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(Nos.2022M3J1A1063917 and 2021M3H4A3A02086681).
文摘Hydrogen fuel cells are expected to play a central role in the next-generation energy paradigm.However,owing to practical limitations,hydrogen is supplied in the form of refined hydrocarbons or alcohols in industrial applications.Among them,methanol is widely used as a hydrogen source,and CO is inevitably generated during its oxidation process.Even a small amount of CO(∼20 ppm)strongly binds to Pt used as a catalyst,and deactivates it.In addition to CO,surface adsorption of organic cations by binder or ionomer use in alkaline fuel cells is also one of the poisoning issues to be overcome.Herein,we propose FePt bimetallic catalysts that can resist unavoidable CO and organic cation poisoning.Our synthetic strategy,including annealing and acid treatment,allows the catalysts to possess different alloying degrees and surface structures,which in turn induce different levels of resistance to CO and organic-cation poisonings.The correlation between the surface and bulk structures of the catalysts and poisoning resistance was elucidated through X-ray photoemission spectroscopy and electrochemical analysis.The results revealed that an FePt catalyst having an ordered atomic arrangement displayed a better poisoning resistance than that having a disordered arrangement.
基金jointly supported by the National Key Research and Development Plan(Grant No.2023YFB3907405)the National Natural Science Foundation of China(Grant No.42175132)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-037)。
文摘The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels and background variability,particularly owing to the influence of terrestrial biospheric fluxes.This necessitates the development of a regional inversion methodology based on atmospheric CO_(2)observations to verify bottom-up estimations independently.This study presents a promising approach for estimating China's FFCO_(2)emissions by incorporating the model residual errors(MREs)of the column-averaged dry-air mole fractions of CO_(2)(XCO_(2))from FFCO_(2)emissions(MREff)retained in the analysis of natural flux optimization.China's FFCO_(2)emissions during the COVID-19 lockdown in 2020 are estimated using the GEOS-Chem adjoint model.The relationship between the MREff and FFCO_(2)is determined using the model based on a regional FFCO_(2)anomaly suggested by posterior NOx emissions from air-quality data assimilation.The MREff is typically one-tenth in magnitude,but some positively skewed outliers exceed 1 ppm because the prior emissions lack lockdown impacts,thereby exerting considerable observation forcing given the satellite retrieval uncertainties.We initialize the FFCO_(2)with posterior NOx emissions and optimize the colinear emission ratio.Synthetic data experiments demonstrate that this approach reduces the FFCO_(2)bias to less than 10%.The real-data experiments estimate 19%lower FFCO_(2)with GOSAT XCO_(2)and 26%lower with OCO-2 XCO_(2)than the bottom-up estimations.This study proves the feasibility of our regional FFCO_(2)inversion,highlighting the importance of addressing the outlier behaviors observed in satellite XCO_(2)retrievals.
基金国家自然科学基金(22202124,22208376)山西省科技创新团队专项资金(202304051001023)+3 种基金山西省重点研发计划(202302060301009)山西省国家留学基金委(2023-008,2023-009)山东省自然科学基金(ZR2023LFG005)青岛新能源山东实验室开放项目(QNESL OP 202303).
文摘Developing efficient and stable non-precious metal catalysts is essential for replacing platinum-based catalysts in polymer electrolyte membrane fuel cells(PEMFCs).The transition metal and nitrogen co-doped carbon electrocatalyst(M-N-C)is considered an effective alternative to precious metal catalysts.However,its relatively poor performance in acidic environments has always been a problem plaguing its practical application in PEMFCs.This study presents a sequential deposition methodology for constructing a composite catalytic system of Fe-N-C and ionic liquid(IL),which exhibits improved performance at both half-cell and membrane electrode assembly scales.The presence of IL significantly inhibits H_(2)O_(2)production,preferentially promoting the 4e–O_(2)reduction reaction,resulting in improved electrocatalytic activity and stability.Additionally,the enhanced PEMFC performance of IL containing electrodes is a direct result of the improved ionic and reactant accessibility of the pore confined Fe-N-C catalysts where the IL minimizes local resistive transport losses.This study establishes a strategic foundation for the practical utilization of non-precious metal catalysts in PEMFCs and other energy converting technologies.
基金the support from National Key R&D Program of China (2021YFC2103704)the National Natural Science Foundation of China (22222808)+4 种基金the Natural Science Foundation of Shandong Province (ZR2023QB152)the Youth Innovation Team Plan of Shandong Province (2022KJ270)the China National Postdoctoral Program for Innovative Talents (BX20240251)the Aeronautical Science Foundation of China (2023Z073048003)the Haihe Laboratory of Sustainable Chemical Transformations。
文摘Photoinduced[2+2]cycloaddition of biomass-derived cycloolefin is a promising approach to synthesize high-energy bio-fuels,however,the conversion efficiency and selectivity are still low.Herein,we provide an acid-promoted photocycloaddition approach to synthesize a new kind of spiral fuel from biomass-derived cyclohexanone (CHOE) and camphene (CPE).BrΦnsted acids show higher catalytic activity than Lewis acids,and acetic acid (HOAc) possesses the best catalytic performance,with CHOE conversion up to 99.1%.Meanwhile,the HOAc-catalytic effect has been confirmed for[2+2]photocycloaddition of other biomass-derived ketenes and olefins.The catalytic mechanism and dynamics have been investigated,and show that HOAc can bond with C=O groups of CHOE to form H–CHOE complex,which leads to higher light adsorption and longer triplet lifetime.Meanwhile,H–CHOE complex reduces the energy gap between CHOE LUMO and CPE HOMO,shortens the distance of ring-forming atoms,and then decreases the energy barrier (from 103.3 kcal mol^(-1)to 95.8 kcal mol^(-1)) of rate-limiting step.After hydrodeoxygenation,the targeted bio-spiral fuel shows high density of 0.992 g cm^(-3),high neat heat of combustion of 41.89 MJ L^(-1),low kinetic viscosity of 5.69 mm^(2)s^(-1)at 20℃,which is very promising to serve as high-performance aerospace fuel.
基金supported by the National Natural Science Foundation of China(22005072,21965006)Guizhou Provincial Key Technology R&D Program(Qian Ke He support(2023)General 122)+3 种基金Guiyang Guian Science and Technology Personnel Training Project([2024]2-13)Youth Science and Technology Talent Development Project from Guizhou Provincial Department of Education(KY[2022]163)Guizhou Provincial Science and Technology Foundation(KYJZ[2024]029)the ETS Marcelle-Gauvreau Engineering Research Chair program.
文摘Atomically dispersed metal site(ADMS)materials have emerged as a promising class of materials for electrocatalysis reactions in the field of energy conversion.Characterized by individual metal atoms dispersed on suitable supports,ADMS materials provide unique catalytic sites with highly tunable electronic structures.This review summarizes recent advancements in the field,with a focus on the critical roles of support materials,coordination environments,and the mechanisms underlying catalytic activity at the atomic level.First,commonly used density functional theory(DFT)simulations are reviewed,emphasizing their pivotal role in elucidating reaction mechanisms and predicting the behavior of ADMS in electrochemical reactions for hydrogen energy utilization.Then,advancements in ADMS for half-cell electrochemical reactions,including oxygen evolution reaction,hydrogen evolution reaction,and oxygen reduction reaction,as well as their applications in fuel cells and water splitting,are summarized.Finally,the challenges and future prospects of ADMS are discussed.This review underscores the transformative potential of ADMS in electrocatalysis,paving the way for innovative and sustainable energy conversion technologies.
基金the financial support from the National Natural Science Foundation of China(No.22209191)Ningbo Key R&D Project(No.2023Z155).
文摘The commercialization of solid oxide fuel cells depends on the cathode,which possesses both high catalytic activity and a thermal-expansion coefficient(TEC)that aligns with the electrolyte.Although the cobalt-based cathode La_(0.6)Sr_(0.4)CoO_(3)(LSC)offers excellent catalytic performance,its TEC is significantly larger than that of the electrolyte.In this study,we mechanically mix Sm_(0.2)Ce_(0.8)O_(2−δ)(SDC)with LSC to create a composite cathode.By incorporating 50wt%SDC,the TEC decreases significantly from 18.29×10^(−6) to 13.90×10^(−6) K^(−1).Under thermal-shock conditions ranging from room temperature to 800℃,the growth rate of polarization resistance is only 0.658%per cycle,i.e.,merely 49%that of pure LSC.The button cell comprising the LSC-SDC composite cathode operates stably for over 900 h without Sr segregation,with a voltage growth rate of 1.11%/kh.A commercial flat-tube cell(active area:70 cm^(2))compris-ing the LSC-SDC composite cathode delivers 54.8 W at 750℃.The distribution of relaxation-time shows that the non-electrode portion is the main rate-limiting step.This study demonstrates that the LSC-SDC mixture strategy effectively improves the compatibility with the electrolyte while maintaining a high output,thus rendering it a promising commercial cathode material.
