In this paper,we present a novel first-order digitalΣΔconverter tailored for digital-to-analog applications,focusing on achieving both high yield and reduced silicon estate.Our approach incorporates a substantial le...In this paper,we present a novel first-order digitalΣΔconverter tailored for digital-to-analog applications,focusing on achieving both high yield and reduced silicon estate.Our approach incorporates a substantial level of dithering noise into the input signal,strategically aimed at mitigating the spurious frequencies commonly encountered in such converters.Validation of our design is performed through simulations using a high-level simulator specialized in mixed-signal circuit analysis.The results underscore the enhanced performance of our circuit,especially in reducing spurious frequencies,highlighting its efficiency and effectiveness.The final circuit exhibits an effective number of bits of 13.展开更多
Long-term responses of floating structures pose a great concern in their design phase. Existing approaches for addressing long-term extreme responses are extremely cumbersome for adoption. This work aims to develop an...Long-term responses of floating structures pose a great concern in their design phase. Existing approaches for addressing long-term extreme responses are extremely cumbersome for adoption. This work aims to develop an approach for the long-term extreme-response analysis of floating structures. A modified gradient-based retrieval algorithm in conjunction with the inverse first-order reliability method(IFORM) is proposed to enable the use of convolution models in long-term extreme analysis of structures with an analytical formula of response amplitude operator(RAO). The proposed algorithm ensures convergence stability and iteration accuracy and exhibits a higher computational efficiency than the traditional backtracking method. However, when the RAO of general offshore structures cannot be analytically expressed, the convolutional integration method fails to function properly. A numerical discretization approach is further proposed for offshore structures in the case when the analytical expression of the RAO is not feasible. Through iterative discretization of environmental contours(ECs) and RAOs, a detailed procedure is proposed to calculate the long-term response extremes of offshore structures. The validity and accuracy of the proposed approach are tested using a floating offshore wind turbine as a numerical example. The long-term extreme heave responses of various return periods are calculated via the IFORM in conjunction with a numerical discretization approach. The environmental data corresponding to N-year structural responses are located inside the ECs, which indicates that the selection of design points directly along the ECs yields conservative design results.展开更多
This paper introduces a novel approach for parameter sensitivity evaluation and efficient slope reliability analysis based on quantile-based first-order second-moment method(QFOSM).The core principles of the QFOSM are...This paper introduces a novel approach for parameter sensitivity evaluation and efficient slope reliability analysis based on quantile-based first-order second-moment method(QFOSM).The core principles of the QFOSM are elucidated geometrically from the perspective of expanding ellipsoids.Based on this geometric interpretation,the QFOSM is further extended to estimate sensitivity indices and assess the significance of various uncertain parameters involved in the slope system.The proposed method has the advantage of computational simplicity,akin to the conventional first-order second-moment method(FOSM),while providing estimation accuracy close to that of the first-order reliability method(FORM).Its performance is demonstrated with a numerical example and three slope examples.The results show that the proposed method can efficiently estimate the slope reliability and simultaneously evaluate the sensitivity of the uncertain parameters.The proposed method does not involve complex optimization or iteration required by the FORM.It can provide a valuable complement to the existing approximate reliability analysis methods,offering rapid sensitivity evaluation and slope reliability analysis.展开更多
Investigating natural-inspired applications is a perennially appealing subject for scientists. The current increase in the speed of natural-origin structure growth may be linked to their superior mechanical properties...Investigating natural-inspired applications is a perennially appealing subject for scientists. The current increase in the speed of natural-origin structure growth may be linked to their superior mechanical properties and environmental resilience. Biological composite structures with helicoidal schemes and designs have remarkable capacities to absorb impact energy and withstand damage. However, there is a dearth of extensive study on the influence of fiber redirection and reorientation inside the matrix of a helicoid structure on its mechanical performance and reactivity. The present study aimed to explore the static and transient responses of a bio-inspired helicoid laminated composite(B-iHLC) shell under the influence of an explosive load using an isomorphic method. The structural integrity of the shell is maintained by a viscoelastic basis known as the Pasternak foundation, which encompasses two coefficients of stiffness and one coefficient of damping. The equilibrium equations governing shell dynamics are obtained by using Hamilton's principle and including the modified first-order shear theory,therefore obviating the need to employ a shear correction factor. The paper's model and approach are validated by doing numerical comparisons with respected publications. The findings of this study may be used in the construction of military and civilian infrastructure in situations when the structure is subjected to severe stresses that might potentially result in catastrophic collapse. The findings of this paper serve as the foundation for several other issues, including geometric optimization and the dynamic response of similar mechanical structures.展开更多
An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.Thi...An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.This method is applied to the primary fragments of antisymmetrized molecular dynamics(AMD)simulations for ^(46)Fe+^(46)Fe,^(40)Ca+^(40)Ca and ^(48)Ca+^(48)Ca at 35 MeV/nucleon,in order to make direct comparison to the results from the K(N,Z)method of Ono et al.In our improved method,the extracted values of a_(sym)/T increase as the size of isotopes increases whereas,in the K(N,Z)method,the results show rather constant behavior.This increase in our result is attributed to the surface contribution of the symmetry energy in finite nuclei.In order to evaluate the surface contribution,the relation a_(sym)/T=[a_(sym)^((V))(1-k_(S/V) A^(-1/3))]/T is applied and k_(S/V)=1.20~1.25 was extracted.This value is smaller than those extracted from the mass table,reflecting the weakened surface contribution at higher temperature regime.Δμ/T,the difference of the neutron-proton chemical potentials relative to the temperature,is also extracted in this method at the same time.The average values of the extractedΔμ/T,Δμ/T show a linear dependence on the proton-neutron a_(sym)metry parameter of the system,δ_(sys),andΔμ/T=(15.1±0.2)δ_(sys)-(0.5±0.1)is obtained.展开更多
Using Euler’s first-order explicit(EE)method and the peridynamic differential operator(PDDO)to discretize the time and internal crystal-size derivatives,respectively,the Euler’s first-order explicit method–peridyna...Using Euler’s first-order explicit(EE)method and the peridynamic differential operator(PDDO)to discretize the time and internal crystal-size derivatives,respectively,the Euler’s first-order explicit method–peridynamic differential operator(EE–PDDO)was obtained for solving the one-dimensional population balance equation in crystallization.Four different conditions during crystallization were studied:size-independent growth,sizedependent growth in a batch process,nucleation and size-independent growth,and nucleation and size-dependent growth in a continuous process.The high accuracy of the EE–PDDO method was confirmed by comparing it with the numerical results obtained using the second-order upwind and HR-van methods.The method is characterized by non-oscillation and high accuracy,especially in the discontinuous and sharp crystal size distribution.The stability of the EE–PDDO method,choice of weight function in the PDDO method,and optimal time step are also discussed.展开更多
Methane generation in landfills and its inadequate management represent the major avoidable source of anthropogenic methane today. This paper models methane production and the potential resources expected (electrical ...Methane generation in landfills and its inadequate management represent the major avoidable source of anthropogenic methane today. This paper models methane production and the potential resources expected (electrical energy production and potential carbon credits from avoided CH4 emissions) from its proper management in a municipal solid waste landfill located in Ouagadougou, Burkina Faso. The modeling was carried out using two first-order decay (FOD) models (LandGEM V3.02 and SWANA) using parameters evaluated on the basis of the characteristics of the waste admitted to the landfill and weather data for the site. At the same time, production data have been collected since 2016 in order to compare them with the model results. The results obtained from these models were compared to experimental one. For the simulation of methane production, the SWANA model showed better consistency with experimental data, with a coefficient of determination (R²) of 0.59 compared with the LandGEM model, which obtained a coefficient of 0.006. Thus, despite the low correlation values linked to the poor consistency of experimental data, the SWANA model models methane production much better than the LandGEM model. Thus, despite the low correlation values linked to the poor consistency of the experimental data, the SWANA model models methane production much better than the LandGEM V3.02 model. It was noted that the poor consistency of the experimental data justifies these low coefficients, and that they can be improved in the future thanks to ongoing in situ measurements. According to the SWANA model prediction, in 27 years of operation a biogas plant with 33% electrical efficiency using biogas from the Polesgo landfill would avoid 1,340 GgCO2e. Also, the evaluation of revenues due to electricity and carbon credit gave a total revenue derived from methane production of US$27.38 million at a cost of US$10.5/tonne CO2e.展开更多
α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organi...α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organic compounds with diverse structures.Herein,the advances in the research areas ofα-trifluoromethyl ketone synthesis and their defluorination reactions are reviewed.Discussion on the mechanisms of the typical reactions has also been provided,in hope of affording some guides to the chemistry ofα-trifluoromethyl ketones in the synthetic methods toward themselves and their derivatives.展开更多
Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nano...Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.展开更多
Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange...Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.展开更多
The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-bas...The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-based catalyst PrO_(x)-NC,and optimized the calcination temperature and proportion.The PrO_(x)-NC-900 catalyst has high durability and activity and exhibits superior ORR performance in alkaline electrolytes with an onset potential(E_(0))of 0.96 V and a half-wave potential(E_(1/2))of 0.85 V.The research results indicate that the ORR performance of rare earth oxide composite carbon catalysts can be improved by adjusting oxygen vacancies(Ov).In addition,high specific surface area,N rich defect carbon.increased oxygen vacancies,and the synergistic effect of oxygen vacancies and N-doped carbon interfacial layer play a significant part in the enhancement of ORR.The performance of the zinc air battery assembled with PrO_(x)-NC-900 is significantly improved,and rare earth oxides and carbon frameworks originating from metal organic frameworks(MOFs)contribute to the oxygen electrocatalyst and electron transfer rate of the zinc air battery.This catalyst provides promising information for the development of rare earth metal oxide nanostructures as potential candidate materials for ORR in alkaline media.展开更多
An analysis has been developed to study the unsteady free convection flow of an incompressible visco-elastic fluid on a continuously moving vertical porous plate in the presence of a first-order chemical reaction. The...An analysis has been developed to study the unsteady free convection flow of an incompressible visco-elastic fluid on a continuously moving vertical porous plate in the presence of a first-order chemical reaction. The governing equations are solved numerically using an implicit finite difference technique. The obtained numerical solutions are compared with the analytical solutions. The velocity profiles are presented. A parametric analysis is performed to illustrate the influences of the visco-elastic parameter, the dimensionless chemical reaction parameter, and the plate moving velocity on the steady state velocity profiles, the time dependent friction coefficient, the Nusselt number, and the Sherwood number.展开更多
Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this s...Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.展开更多
Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capac...Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to thei...Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.展开更多
Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal int...Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.展开更多
Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal s...Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.展开更多
An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The r...An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The reductive hydroarylation of acrylates with aryl halides was successfully achieved without requiring exogenous photoredox catalysts.This reaction is highlighted by the simple and mild conditions,good functional group tolerance,thus providing a complementary approach for alkenes reductive Heck reaction.展开更多
Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-c...Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-coupling reactions are among the most straightforward and effective methods for synthesizing chiral carbonyl compounds, including esters, amides, and ketones. The advances in asymmetric carbonylative cross-coupling reactions using various O-, N-, C-, and S-containing nucleophiles or electrophiles over the past decade are summarized.展开更多
文摘In this paper,we present a novel first-order digitalΣΔconverter tailored for digital-to-analog applications,focusing on achieving both high yield and reduced silicon estate.Our approach incorporates a substantial level of dithering noise into the input signal,strategically aimed at mitigating the spurious frequencies commonly encountered in such converters.Validation of our design is performed through simulations using a high-level simulator specialized in mixed-signal circuit analysis.The results underscore the enhanced performance of our circuit,especially in reducing spurious frequencies,highlighting its efficiency and effectiveness.The final circuit exhibits an effective number of bits of 13.
基金Supported by the National Natural Science Foundation of China (Grant Nos.52088102 and 51879287)National Key Research and Development Program of China (Grant No.2022YFB2602301)。
文摘Long-term responses of floating structures pose a great concern in their design phase. Existing approaches for addressing long-term extreme responses are extremely cumbersome for adoption. This work aims to develop an approach for the long-term extreme-response analysis of floating structures. A modified gradient-based retrieval algorithm in conjunction with the inverse first-order reliability method(IFORM) is proposed to enable the use of convolution models in long-term extreme analysis of structures with an analytical formula of response amplitude operator(RAO). The proposed algorithm ensures convergence stability and iteration accuracy and exhibits a higher computational efficiency than the traditional backtracking method. However, when the RAO of general offshore structures cannot be analytically expressed, the convolutional integration method fails to function properly. A numerical discretization approach is further proposed for offshore structures in the case when the analytical expression of the RAO is not feasible. Through iterative discretization of environmental contours(ECs) and RAOs, a detailed procedure is proposed to calculate the long-term response extremes of offshore structures. The validity and accuracy of the proposed approach are tested using a floating offshore wind turbine as a numerical example. The long-term extreme heave responses of various return periods are calculated via the IFORM in conjunction with a numerical discretization approach. The environmental data corresponding to N-year structural responses are located inside the ECs, which indicates that the selection of design points directly along the ECs yields conservative design results.
基金supported by the National Natural Science Foundation of China(Grant Nos.52109144,52025094 and 52222905).
文摘This paper introduces a novel approach for parameter sensitivity evaluation and efficient slope reliability analysis based on quantile-based first-order second-moment method(QFOSM).The core principles of the QFOSM are elucidated geometrically from the perspective of expanding ellipsoids.Based on this geometric interpretation,the QFOSM is further extended to estimate sensitivity indices and assess the significance of various uncertain parameters involved in the slope system.The proposed method has the advantage of computational simplicity,akin to the conventional first-order second-moment method(FOSM),while providing estimation accuracy close to that of the first-order reliability method(FORM).Its performance is demonstrated with a numerical example and three slope examples.The results show that the proposed method can efficiently estimate the slope reliability and simultaneously evaluate the sensitivity of the uncertain parameters.The proposed method does not involve complex optimization or iteration required by the FORM.It can provide a valuable complement to the existing approximate reliability analysis methods,offering rapid sensitivity evaluation and slope reliability analysis.
文摘Investigating natural-inspired applications is a perennially appealing subject for scientists. The current increase in the speed of natural-origin structure growth may be linked to their superior mechanical properties and environmental resilience. Biological composite structures with helicoidal schemes and designs have remarkable capacities to absorb impact energy and withstand damage. However, there is a dearth of extensive study on the influence of fiber redirection and reorientation inside the matrix of a helicoid structure on its mechanical performance and reactivity. The present study aimed to explore the static and transient responses of a bio-inspired helicoid laminated composite(B-iHLC) shell under the influence of an explosive load using an isomorphic method. The structural integrity of the shell is maintained by a viscoelastic basis known as the Pasternak foundation, which encompasses two coefficients of stiffness and one coefficient of damping. The equilibrium equations governing shell dynamics are obtained by using Hamilton's principle and including the modified first-order shear theory,therefore obviating the need to employ a shear correction factor. The paper's model and approach are validated by doing numerical comparisons with respected publications. The findings of this study may be used in the construction of military and civilian infrastructure in situations when the structure is subjected to severe stresses that might potentially result in catastrophic collapse. The findings of this paper serve as the foundation for several other issues, including geometric optimization and the dynamic response of similar mechanical structures.
文摘An improved method is proposed for the extraction of the symmetry energy coefficient relative to the temperature,a_(sym)/T,in the heavy-ion reactions near the Fermi energy region,based on the modified Fisher Model.This method is applied to the primary fragments of antisymmetrized molecular dynamics(AMD)simulations for ^(46)Fe+^(46)Fe,^(40)Ca+^(40)Ca and ^(48)Ca+^(48)Ca at 35 MeV/nucleon,in order to make direct comparison to the results from the K(N,Z)method of Ono et al.In our improved method,the extracted values of a_(sym)/T increase as the size of isotopes increases whereas,in the K(N,Z)method,the results show rather constant behavior.This increase in our result is attributed to the surface contribution of the symmetry energy in finite nuclei.In order to evaluate the surface contribution,the relation a_(sym)/T=[a_(sym)^((V))(1-k_(S/V) A^(-1/3))]/T is applied and k_(S/V)=1.20~1.25 was extracted.This value is smaller than those extracted from the mass table,reflecting the weakened surface contribution at higher temperature regime.Δμ/T,the difference of the neutron-proton chemical potentials relative to the temperature,is also extracted in this method at the same time.The average values of the extractedΔμ/T,Δμ/T show a linear dependence on the proton-neutron a_(sym)metry parameter of the system,δ_(sys),andΔμ/T=(15.1±0.2)δ_(sys)-(0.5±0.1)is obtained.
文摘Using Euler’s first-order explicit(EE)method and the peridynamic differential operator(PDDO)to discretize the time and internal crystal-size derivatives,respectively,the Euler’s first-order explicit method–peridynamic differential operator(EE–PDDO)was obtained for solving the one-dimensional population balance equation in crystallization.Four different conditions during crystallization were studied:size-independent growth,sizedependent growth in a batch process,nucleation and size-independent growth,and nucleation and size-dependent growth in a continuous process.The high accuracy of the EE–PDDO method was confirmed by comparing it with the numerical results obtained using the second-order upwind and HR-van methods.The method is characterized by non-oscillation and high accuracy,especially in the discontinuous and sharp crystal size distribution.The stability of the EE–PDDO method,choice of weight function in the PDDO method,and optimal time step are also discussed.
文摘Methane generation in landfills and its inadequate management represent the major avoidable source of anthropogenic methane today. This paper models methane production and the potential resources expected (electrical energy production and potential carbon credits from avoided CH4 emissions) from its proper management in a municipal solid waste landfill located in Ouagadougou, Burkina Faso. The modeling was carried out using two first-order decay (FOD) models (LandGEM V3.02 and SWANA) using parameters evaluated on the basis of the characteristics of the waste admitted to the landfill and weather data for the site. At the same time, production data have been collected since 2016 in order to compare them with the model results. The results obtained from these models were compared to experimental one. For the simulation of methane production, the SWANA model showed better consistency with experimental data, with a coefficient of determination (R²) of 0.59 compared with the LandGEM model, which obtained a coefficient of 0.006. Thus, despite the low correlation values linked to the poor consistency of experimental data, the SWANA model models methane production much better than the LandGEM model. Thus, despite the low correlation values linked to the poor consistency of the experimental data, the SWANA model models methane production much better than the LandGEM V3.02 model. It was noted that the poor consistency of the experimental data justifies these low coefficients, and that they can be improved in the future thanks to ongoing in situ measurements. According to the SWANA model prediction, in 27 years of operation a biogas plant with 33% electrical efficiency using biogas from the Polesgo landfill would avoid 1,340 GgCO2e. Also, the evaluation of revenues due to electricity and carbon credit gave a total revenue derived from methane production of US$27.38 million at a cost of US$10.5/tonne CO2e.
文摘α-Trifluoromethyl ketones are a class of useful compounds with versatile applications.Their synthetic application via the transformation of the C—F bonds is of particular interest by allowing the synthesis of organic compounds with diverse structures.Herein,the advances in the research areas ofα-trifluoromethyl ketone synthesis and their defluorination reactions are reviewed.Discussion on the mechanisms of the typical reactions has also been provided,in hope of affording some guides to the chemistry ofα-trifluoromethyl ketones in the synthetic methods toward themselves and their derivatives.
文摘Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.
基金supported by the National Natural Science Foundation of China(Nos.22272105 and 22002110)Natural Science Foundation of Shanghai(No.23ZR1423900)。
文摘Nitrogen-doping of carbon support(N-C)for platinum(Pt)nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction(ORR)in proton exchange membrane fuel cells.For fundamental understanding,clearly identifying the metalsupport effect on enhancement mechanisms of ORR electrocatalysis is definitely needed.In this work,the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations,electrochemical measurements and theoretical DFT-calculations/AIMD-simulations.The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H_(2)-O_(2)fuel cell.Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles,which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.
基金Project supported by the National Natural Science Foundation of China(22062019)the Natural Science Foundation of Inner Mongolia of China(2022QN02002)Science and Technology Program of Inner Mongolia Autonomous Region,China(2020PT0003)。
文摘The development of an e fficacious and easily prepared no nprecious metal electrocatalyst is crucial for the oxygen reduction reaction(ORR).This work used a dual template method to prepare the amorphous rare earth-based catalyst PrO_(x)-NC,and optimized the calcination temperature and proportion.The PrO_(x)-NC-900 catalyst has high durability and activity and exhibits superior ORR performance in alkaline electrolytes with an onset potential(E_(0))of 0.96 V and a half-wave potential(E_(1/2))of 0.85 V.The research results indicate that the ORR performance of rare earth oxide composite carbon catalysts can be improved by adjusting oxygen vacancies(Ov).In addition,high specific surface area,N rich defect carbon.increased oxygen vacancies,and the synergistic effect of oxygen vacancies and N-doped carbon interfacial layer play a significant part in the enhancement of ORR.The performance of the zinc air battery assembled with PrO_(x)-NC-900 is significantly improved,and rare earth oxides and carbon frameworks originating from metal organic frameworks(MOFs)contribute to the oxygen electrocatalyst and electron transfer rate of the zinc air battery.This catalyst provides promising information for the development of rare earth metal oxide nanostructures as potential candidate materials for ORR in alkaline media.
文摘An analysis has been developed to study the unsteady free convection flow of an incompressible visco-elastic fluid on a continuously moving vertical porous plate in the presence of a first-order chemical reaction. The governing equations are solved numerically using an implicit finite difference technique. The obtained numerical solutions are compared with the analytical solutions. The velocity profiles are presented. A parametric analysis is performed to illustrate the influences of the visco-elastic parameter, the dimensionless chemical reaction parameter, and the plate moving velocity on the steady state velocity profiles, the time dependent friction coefficient, the Nusselt number, and the Sherwood number.
基金financially supported by the National Natural Science Foundation of China(No.5217042069)the Young Elite Scientist Sponsorship Program by China Association for Science and Technology(CAST)(No.YESS20200103)the Fundamental Research Funds for the Central Universities(No.265QZ2022004)。
文摘Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(No.12304077)the Natural Science Foundation of Science and Technology Department of Sichuan Province(No.23NSFSC6224)+3 种基金Sichuan Science and Technology Program(No.2024NSFSC0989)the Key Laboratory of Computational Physics of Sichuan Province(No.YBUJSWL-YB-2022-03)the Material Corrosion and Protection Key Laboratory of Sichuan Province(No.2023CL14 and No.2023CL01)the National Innovation Practice Project(No.202411079005S).
文摘Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide(LLO),leading to voltage and capacity fading.Herein,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room temperature.Density functional theory(DFT)calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry(DEMS)indicates that the Cr_(x)B complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li^(+)migration,The voltage and capacity fading of the modified cathode(LLO-C_(r)B)are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface(CEI)composed of balanced organic/inorganic composition.Therefore,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g^(-1)(with a retention rate of 95.1%).This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金financial support by the National Natural Science Foundation of China(No.52102241)Doctor of Suzhou University Scientific Research Foundation(Nos.2022BSK019,2020BS015)+2 种基金the Primary Research and Development Program of Anhui Province(No.201904a05020087)the Natural Science Research Project in Universities of Anhui Province in China(Nos.2022AH051386,KJ2021A1114)the Foundation(No.GZKF202211)of State Key Laboratory of Biobased Material and Green Papermaking Qilu University of Technology。
文摘Available online Alkaline water electrolysis(AWE)is a prominent technique for obtaining a sustainable hydrogen source and effectively managing the energy infrastructure.Noble metal-based electrocatalysts,owing to their exceptional hydrogen binding energy,exhibit remarkable catalytic activity and long-term stability in the hydrogen evolution reaction(HER).However,the restricted accessibility and exorbitant cost of noble-metal materials pose obstacles to their extensive adoption in industrial contexts.This review investigates strategies aimed at reducing the dependence on noble-metal electrocatalysts and developing a cost-effective alkaline HER catalyst,while considering the principles of sustainable development.The initial discussion covers the fundamental principle of HER,followed by an overview of prevalent techniques for synthesizing catalysts based on noble metals,along with a thorough examination of recent advancements.The subsequent discussion focuses on the strategies employed to improve noble metalbased catalysts,including enhancing the intrinsic activity at active sites and increasing the quantity of active sites.Ultimately,this investigation concludes by examining the present state and future direction of research in the field of electrocatalysis for the HER.
基金financially supported by the National Natural Science Foundation of China(22309137,22279095)Open subject project State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2023001).
文摘Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.
文摘Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.
文摘An efficient visible-light induced nickel-catalyzed reductive Heck reaction of alkenes by using mild organic reductant Hantzsch ester(HEH)instead of traditional metal reductants or hydride reagents was developed.The reductive hydroarylation of acrylates with aryl halides was successfully achieved without requiring exogenous photoredox catalysts.This reaction is highlighted by the simple and mild conditions,good functional group tolerance,thus providing a complementary approach for alkenes reductive Heck reaction.
文摘Chiral carbonyl compounds frequently occur in natural products and pharmaceuticals. Additionally, they serve as important intermediates in organic synthesis. Transition metal-catalyzed asymmetric carbonylative cross-coupling reactions are among the most straightforward and effective methods for synthesizing chiral carbonyl compounds, including esters, amides, and ketones. The advances in asymmetric carbonylative cross-coupling reactions using various O-, N-, C-, and S-containing nucleophiles or electrophiles over the past decade are summarized.
