High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress aro...High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress arouses the deformation of large integrated die-castings.Herein,the development of non-heat treatment Al alloys is becoming the hot topic.In addition,HPDC contains externally solidified crystals(ESCs),which are detrimental to the mechanical properties of castings.To achieve high strength and toughness of non-heat treatment die-casting Al-Si alloy,we used AlSi9Mn alloy as matrix with the introduction of Zr,Ti,Nb,and Ce.Their influences on ESCs and mechanical properties were systematically investigated through three-dimensional reconstruction and thermodynamic simulation.Our results reveal that the addition of Ti increased ESCs'size and porosity,while the introduction of Nb refined ESCs and decreased porosity.Meanwhile,large-sized Al_3(Zr,Ti)phases formed and degraded the mechanical properties.Subsequent introduction of Ce resulted in the poisoning effect and reduced mechanical properties.展开更多
To improve the comprehensive mechanical properties of Al-Si-Cu alloy,it was treated by a high-pressure torsion process,and the effect of the deformation degree on the microstructure and properties of the Al-Si-Cu allo...To improve the comprehensive mechanical properties of Al-Si-Cu alloy,it was treated by a high-pressure torsion process,and the effect of the deformation degree on the microstructure and properties of the Al-Si-Cu alloy was studied.The results show that the reinforcements(β-Si andθ-CuAl_(2)phases)of the Al-Si-Cu alloy are dispersed in theα-Al matrix phase with finer phase size after the treatment.The processed samples exhibit grain sizes in the submicron or even nanometer range,which effectively improves the mechanical properties of the material.The hardness and strength of the deformed alloy are both significantly raised to 268 HV and 390.04 MPa by 10 turns HPT process,and the fracture morphology shows that the material gradually transits from brittle to plastic before and after deformation.The elements interdiffusion at the interface between the phases has also been effectively enhanced.In addition,it is found that the severe plastic deformation at room temperature induces a ternary eutectic reaction,resulting in the formation of ternary Al+Si+CuAl_(2)eutectic.展开更多
Repairs of corroded high-pressure pipelines are essential for fluids transportation under high pressure.One of the methods used in their repairs is the use of layered composites.The composite used must have the necess...Repairs of corroded high-pressure pipelines are essential for fluids transportation under high pressure.One of the methods used in their repairs is the use of layered composites.The composite used must have the necessary strength.Therefore,the experiments and analytical solutions presented in this paper are performed according to the relevant standards and codes,including ASME PCC-2,ASME B31.8S,ASME B31.4,ISO 24817 and ASME B31.G.In addition,the experimental tests are replicated numerically using the finite element method.Setting the strain gauges at different distances from the defect location,can reduce the nonlinear effects,deformation,and fluctuations due to the high pressure.The direct relationship between the depth of an axial defect and the stress concentration is observed at the inner side edges of the defect.Composite reparation reduces the non-linearities related to the sharp variation of the geometry and a more reliable numerical simulation could be performed.展开更多
To thoroughly study the extinguishing effect of a high-pressure water mist fire extinguishing system when a transformer fire occurs,a 3D experimental model of a transformer is established in this work by employing Fir...To thoroughly study the extinguishing effect of a high-pressure water mist fire extinguishing system when a transformer fire occurs,a 3D experimental model of a transformer is established in this work by employing Fire Dynamics Simulator(FDS)software.More specifically,by setting different parameters,the process of the highpressure water mist fire extinguishing system with the presence of both diverse ambient temperatures and water mist sprinkler laying conditions is simulated.In addition,the fire extinguishing effect of the employed high-pressure water mist system with the implementation of different strategies is systematically analyzed.The extracted results show that a fire source farther away fromthe centerline leads to a lower local temperature distribution.In addition,as the ambient temperature increases,the temperature above the fire source decreases,while the temperature and the concentrationof theupperflue gas layer bothdecrease.Interestingly,after thehigh-pressurewatermist sprinkler begins to operate,both the temperature distribution above the fire source and the concentration of the flue gas decrease,which indicates that the high-pressure water mist system plays the role of cooling and dust removal.By comparing various sprinkler laying methods,it is found that the lower sprinkler height has a better effect on the temperature above the fire source,the temperature of the upper flue gas layer,and the concentration of the flue gas.Moreover,when the sprinkler is spread over thewhole transformer,the cooling effect on both the temperature above the fire source and the temperature of the upper flue gas layer is good,whereas the change in the concentration of the flue gas above the fire source is not obvious compared to the case where the sprinkler is not fully spread.展开更多
We report the discovery of TiO_(2)-Ⅱ in the unmelted rock of the shocked Suizhou L6 chondrite.Natural TiO_(2)-Ⅱ was previously found in ultrahigh-pressure metamorphic and mantle-derived rocks,terrestrial impact stru...We report the discovery of TiO_(2)-Ⅱ in the unmelted rock of the shocked Suizhou L6 chondrite.Natural TiO_(2)-Ⅱ was previously found in ultrahigh-pressure metamorphic and mantle-derived rocks,terrestrial impact structures,and tektite.Our microscopic,Raman spectroscopic,electron microprobe and transmission electron microscopic investigations have revealed:(1) All observed TiO_(2)-Ⅱ grains are related with ilmenite and pyrophanite;(2) TiO_(2)-Ⅱ occurs as needle-and leaf-shaped inclusions in llmenite and patch-,tape-shaped body in pyrophanite;(3)The composition of TiO_(2)-Ⅱ is identical with that of its precursor rutile;(4) The Raman spectrum of TiO_(2)-Ⅱ is in good agreement with that of natural and synthesized α-PbO_(2)-type TiO_(2);(5) TiO_(2)-Ⅱ occurs mainly in the form of well-ordered nano-domains and small mis-orientation among the domains can be observed.(6) All electron diffraction reflections from TiO_(2)-Ⅱ can be indexed to α-PbO_(2)structure in space group Pbcn with lattice parameters of a=4.481 ?,b=5.578 A and c=4.921 A;(7) The exsolution inclusions of rutile from host ilmenite are mostly connected with an alternation process along the lamellar twinning plane of ilmenite induced by shockinduced high pressure and high temperature;(8) The P-T regime of 20-25 GPa and 1000 ℃ estimated for the Suizhou unmelted rock is suitable for phase transition of rutile into TiO_(2)-Ⅱ phase.展开更多
The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for ...The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.展开更多
Monoclinicα-MoP_(2),with the OsGe2-type structure(space group C2/m,Z=4)and lattice parameters a=8.7248(11)Å,b=3.2322(4)Å,c=7.4724(9)Å,andβ=119.263°,was synthesized under a pressure of 4~GPa at a ...Monoclinicα-MoP_(2),with the OsGe2-type structure(space group C2/m,Z=4)and lattice parameters a=8.7248(11)Å,b=3.2322(4)Å,c=7.4724(9)Å,andβ=119.263°,was synthesized under a pressure of 4~GPa at a temperature between 1100℃and 1200℃.The structure ofα-MoP_(2) and its relationship to other transition metal diphosphides are discussed.Surprisingly,the ambient pressure phase orthorhombicβ-MoP_(2)(space group Cmc21)is denser in structure thanα-MoP_(2).Room-temperature high-pressure x-ray diffraction studies exclude the possibility of phase transition fromβ-MoP_(2) to α-MoP_(2),suggesting thatα-MoP_(2) is a stable phase at ambient conditions;this is also supported by the total energy and phonon calculations.展开更多
The high-pressure diagram of V–N compounds is enriched by proposed seven new stable high-pressure phases.The P-1-VN_4with the armchair N-rich structure may be quenched to ambient conditions.The formed N–N covalent b...The high-pressure diagram of V–N compounds is enriched by proposed seven new stable high-pressure phases.The P-1-VN_4with the armchair N-rich structure may be quenched to ambient conditions.The formed N–N covalent bond plays an important role for the structural stability of N-chain.The charge transfer results in a V–N ionic bond interaction,which further improves the stability of N-chain structure.The P-1-VN_4,P4mnc-VN_8,and Immm-VN_(10)with the outstanding detonation properties have potential application in explosive field.展开更多
The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving t...The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.展开更多
Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate th...Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate the reaction pathways and inhibit competing reactions(e.g.hydrogenolysis) for efficient and selective NH_(3) production in an aqueous solution environment.Here,we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO_(2)^(-)on the electrode surface,which ensures the ultimate selectivity for NH_(3).With these properties,Pd@N_(0.14)C with the highest N content achieved excellent catalytic performance for the reduction of NO_(2)^(-)to NH_(3) with the 100% Faraday efficiency at-0.5 and-0.6 V vs,reversible hydrogen electrode(RHE) for NH_(3) production,which was significantly better than Pd/C and Pd@N_(x)C samples with lower N content.This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH_(3) electrosynthesis.展开更多
Previous studies have revealed that ammonia nitrogen has several adverse effects on clam Ruditapes philippinarum.However,knowledge is lacking regarding the related proteins involved in the toxicological responses,whic...Previous studies have revealed that ammonia nitrogen has several adverse effects on clam Ruditapes philippinarum.However,knowledge is lacking regarding the related proteins involved in the toxicological responses,which is vital to elucidate the underlying mechanism of ammonia nitrogen.In this study,clams R.philippinarum were exposed to ammonia nitrogen for 21 d at two environmentally relevant concentrations.The tandem mass tags approach(TMT)was applied to assay the differentially expressed proteins(DEPs)in clam gill tissues on the 3 rd and 21 st day.Finally,a total of 7263 proteins were identified.Bioinformatics analyses revealed that clam protein profiles changed in dose-and time dependent manner after ammonia nitrogen exposure.We inferred that the clams may face heavy challenges after ammonia exposure,such as unbalanced gender ratio,lysosomal disease,energy lack,neurological disorders,altered glutamine metabolism,increased lipid synthesis,and impaired immunity.Variation profiles of enzyme activities of glutaminase and glutamine synthase provided direct evidence to verify the related inference from proteome data.Most of the inferred toxic effects merit further study.This study identified important proteins related to ammonia nitrogen toxicity in the clam and indicated the severe stress of marine ammonia pollution on the healthy development of mollusc aquaculture.展开更多
For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based ...For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based species(N—C)/NOx is optimized using the Non-dominated Sorting Genetic Algorithm II(NSGA-II)with 200 generations.The optimized mechanism(named as 937b)is validated against combustion characteristics of ammonia/methane(which is used to examine the accuracy of N—C interactions)and ammonia/diesel blends.The ignition delay times(IDTs),the laminar flame speeds and most of key intermediate species during the combustion of ammonia/methane blends can be accurately simulated by 937b under a wide range of conditions.As for ammonia/diesel blends with various diesel energy fractions,reasonable predictions on the IDTs under pressures from 1.0 MPa to5.0 MPa as well as the laminar flame speeds are also achieved by 937b.In particular,with regard to the IDT simulations of ammonia/diesel blends,937b makes progress in both aspects of overall accuracy and computational efficiency,compared to a detailed ammonia/diesel mechanism.Further kinetic analysis reveals that the reaction pathway of ammonia during the combustion of ammonia/diesel blend mainly differs in the tendencies of oxygen additions to NH_2 and NH with different equivalence ratios.展开更多
For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions...For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.展开更多
This study aimed to investigate the effects of ammonia addition on ethylene counter-flow diffusion flames with different diluents on the fuel or oxidizer side,using kinetic analyses.A special emphasis was put on asses...This study aimed to investigate the effects of ammonia addition on ethylene counter-flow diffusion flames with different diluents on the fuel or oxidizer side,using kinetic analyses.A special emphasis was put on assessing the coupled chemical effects of NH_(3) and CO_(2) on C2H4 combustion chemistry.The chemical effects could be evaluated by comparing fictitious inert NH_(3) or CO_(2) with normal active NH_(3) or CO_(2).The results revealed that the addition of NH_(3) decreased the mole fractions and production rates of key soot precursors,such as acetylene,propynyl,and benzene.When CO_(2) was used as the dilution gas,the coupled chemical effects of NH_(3) and CO_(2) were affected by the chemical effects of CO_(2) to varying degrees.With the oxidizer-side CO_(2) addition,the coupled chemical effects of NH_(3) and CO_(2) reduced the mole fractions of H,O,OH radicals,acetylene,propynyl,and benzene,while the effects differed from the fuel-side CO_(2) addition.The coupled chemical effects of NH_(3) and CO_(2) also promoted the formation of aldehyde contaminants,such as acetaldehyde,to some extent,particularly with CO_(2) addition on the oxidizer side.展开更多
The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia syn...The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.展开更多
Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and i...Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and is regarded as a future technology for production of CO_(2)-free pure hydrogen.Herein,a heterostructural Pt-Ir dual-layer electrode is developed and shown to achieve successful long-term operation in an ammonia electrolyzer with an anion exchange membrane(AEM).This electrolyzer consisted of eight membra ne electrode assemblies(MEAs)with a total geometric area of 200 cm~2 on the anode side,which resulted in a hydrogen production rate of 25 L h~(-1).We observed the degradation in MEA performance attributed to changes in the anode catalyst layer during hydrogen production via ammonia electrolysis.Furthermore,we demonstrated the relationship between the ammonia oxidation reaction(AOR)and the oxygen evolution reaction(OER).展开更多
Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the...Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.展开更多
Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading t...Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.展开更多
Ammonia serves both as a widely used fertilizer and environmentally friendly energy source due to its high energy density,rich hydrogen content,and emissions-free combustion.Additionally,it offers convenient transport...Ammonia serves both as a widely used fertilizer and environmentally friendly energy source due to its high energy density,rich hydrogen content,and emissions-free combustion.Additionally,it offers convenient transportation and storage as a hydrogen carrier.The dominant method used for large-scale ammonia production is the Haber-Bosch process,which requires high temperatures and pressures and is energy-intensive.However,non-thermal plasma offers an eco-friendly alternative for ammonia synthesis,gaining significant attention.It enables ammonia production at lower temperatures and pressures using plasma technology.This review provides insights into the catalyst and reactor developments,which are pivotal for promoting ammonia efficiency and addressing existing challenges.At first,the reaction kinetics and mechanisms are introduced to gain a comprehensive understanding of the reaction pathways involved in plasma-assisted ammonia synthesis.Thereafter,the enhancement of ammonia synthesis efficiency is discussed by developing and optimizing plasma reactors and effective catalysts.The effect of other feeding sources,such as water and methane,instead of hydrogen is also presented.Finally,the challenges and possible solutions are outlined to facilitate energy-saving and enhance ammonia efficiency in the future.展开更多
Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagat...Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagation speed of ammonia pose significant challenges to its application in engines. Non-equilibrium plasma has been identified as a promising method, but current research on plasma-enhanced ammonia combustion is limited and primarily focuses on ignition characteristics revealed by kinetic models. In this study, low-temperature and low-pressure chemistry in plasma-assisted ammonia oxidative pyrolysis is investigated by integrated studies of steady-state GC measurements and mathematical simulation. The detailed kinetic mechanism of NH_(3) decomposition in plasma-driven Ar/NH_(3) and Ar/NH_(3)/O_(2) mixtures has been developed. The numerical model has good agreements with the experimental measurements in NH_(3)/O_(2) consumption and N_(2)/H_(2) generation, which demonstrates the rationality of modelling. Based on the modelling results, species density profiles, path flux and sensitivity analysis for the key plasmaproduced species such as NH_(2), NH, H_(2), OH, H, O, O(^(1)D), O_(2)(a^(1)△_(g)), O_(2)(b^(1)∑_(g)^(+)), Ar^(*), H^(-), Ar^(+), NH_(3)^(+), O_(2)^(-) in the discharge and afterglow are analyzed in detail to illustrate the effectiveness of the active species on NH_(3) excitation and decomposition at low temperature and relatively higher E/N values. The results revealed that NH_(2), NH, H as well as H_(2) are primarily generated through the electron collision reactions e + NH_(3)→ e + NH_(2)+ H, e + NH_(3)→ e + NH + H_(2) and the excited-argon collision reaction Ar^(*) + NH_(3)+ H → Ar + NH_(2)+ 2H, which will then react with highly reactive oxidative species such as O_(2)^(*), O^(*), O, OH, and O_(2) to produce stable products of NOx and H_(2)O. NH_(3)→ NH is found a specific pathway for NH_(3) consumption with plasma assistance, which further highlights the enhanced kinetic effects.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52175284 and 52474396)the National Key Research and Development Program of China(No.2022YFB3404201)。
文摘High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress arouses the deformation of large integrated die-castings.Herein,the development of non-heat treatment Al alloys is becoming the hot topic.In addition,HPDC contains externally solidified crystals(ESCs),which are detrimental to the mechanical properties of castings.To achieve high strength and toughness of non-heat treatment die-casting Al-Si alloy,we used AlSi9Mn alloy as matrix with the introduction of Zr,Ti,Nb,and Ce.Their influences on ESCs and mechanical properties were systematically investigated through three-dimensional reconstruction and thermodynamic simulation.Our results reveal that the addition of Ti increased ESCs'size and porosity,while the introduction of Nb refined ESCs and decreased porosity.Meanwhile,large-sized Al_3(Zr,Ti)phases formed and degraded the mechanical properties.Subsequent introduction of Ce resulted in the poisoning effect and reduced mechanical properties.
基金Funded by the National Natural Science Foundation of China(No.51905215)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCX23_1233)+1 种基金Major Scientific and Technological Innovation Project of Shandong Province of China(No.2019JZZY020111)the National College Students Innovation and Entrepreneurship Training Program of China(No.CX2022415)。
文摘To improve the comprehensive mechanical properties of Al-Si-Cu alloy,it was treated by a high-pressure torsion process,and the effect of the deformation degree on the microstructure and properties of the Al-Si-Cu alloy was studied.The results show that the reinforcements(β-Si andθ-CuAl_(2)phases)of the Al-Si-Cu alloy are dispersed in theα-Al matrix phase with finer phase size after the treatment.The processed samples exhibit grain sizes in the submicron or even nanometer range,which effectively improves the mechanical properties of the material.The hardness and strength of the deformed alloy are both significantly raised to 268 HV and 390.04 MPa by 10 turns HPT process,and the fracture morphology shows that the material gradually transits from brittle to plastic before and after deformation.The elements interdiffusion at the interface between the phases has also been effectively enhanced.In addition,it is found that the severe plastic deformation at room temperature induces a ternary eutectic reaction,resulting in the formation of ternary Al+Si+CuAl_(2)eutectic.
文摘Repairs of corroded high-pressure pipelines are essential for fluids transportation under high pressure.One of the methods used in their repairs is the use of layered composites.The composite used must have the necessary strength.Therefore,the experiments and analytical solutions presented in this paper are performed according to the relevant standards and codes,including ASME PCC-2,ASME B31.8S,ASME B31.4,ISO 24817 and ASME B31.G.In addition,the experimental tests are replicated numerically using the finite element method.Setting the strain gauges at different distances from the defect location,can reduce the nonlinear effects,deformation,and fluctuations due to the high pressure.The direct relationship between the depth of an axial defect and the stress concentration is observed at the inner side edges of the defect.Composite reparation reduces the non-linearities related to the sharp variation of the geometry and a more reliable numerical simulation could be performed.
基金supported by Science and Technology Projects Funded by State Grid Corporation of China (5200202024105A0000).
文摘To thoroughly study the extinguishing effect of a high-pressure water mist fire extinguishing system when a transformer fire occurs,a 3D experimental model of a transformer is established in this work by employing Fire Dynamics Simulator(FDS)software.More specifically,by setting different parameters,the process of the highpressure water mist fire extinguishing system with the presence of both diverse ambient temperatures and water mist sprinkler laying conditions is simulated.In addition,the fire extinguishing effect of the employed high-pressure water mist system with the implementation of different strategies is systematically analyzed.The extracted results show that a fire source farther away fromthe centerline leads to a lower local temperature distribution.In addition,as the ambient temperature increases,the temperature above the fire source decreases,while the temperature and the concentrationof theupperflue gas layer bothdecrease.Interestingly,after thehigh-pressurewatermist sprinkler begins to operate,both the temperature distribution above the fire source and the concentration of the flue gas decrease,which indicates that the high-pressure water mist system plays the role of cooling and dust removal.By comparing various sprinkler laying methods,it is found that the lower sprinkler height has a better effect on the temperature above the fire source,the temperature of the upper flue gas layer,and the concentration of the flue gas.Moreover,when the sprinkler is spread over thewhole transformer,the cooling effect on both the temperature above the fire source and the temperature of the upper flue gas layer is good,whereas the change in the concentration of the flue gas above the fire source is not obvious compared to the case where the sprinkler is not fully spread.
文摘We report the discovery of TiO_(2)-Ⅱ in the unmelted rock of the shocked Suizhou L6 chondrite.Natural TiO_(2)-Ⅱ was previously found in ultrahigh-pressure metamorphic and mantle-derived rocks,terrestrial impact structures,and tektite.Our microscopic,Raman spectroscopic,electron microprobe and transmission electron microscopic investigations have revealed:(1) All observed TiO_(2)-Ⅱ grains are related with ilmenite and pyrophanite;(2) TiO_(2)-Ⅱ occurs as needle-and leaf-shaped inclusions in llmenite and patch-,tape-shaped body in pyrophanite;(3)The composition of TiO_(2)-Ⅱ is identical with that of its precursor rutile;(4) The Raman spectrum of TiO_(2)-Ⅱ is in good agreement with that of natural and synthesized α-PbO_(2)-type TiO_(2);(5) TiO_(2)-Ⅱ occurs mainly in the form of well-ordered nano-domains and small mis-orientation among the domains can be observed.(6) All electron diffraction reflections from TiO_(2)-Ⅱ can be indexed to α-PbO_(2)structure in space group Pbcn with lattice parameters of a=4.481 ?,b=5.578 A and c=4.921 A;(7) The exsolution inclusions of rutile from host ilmenite are mostly connected with an alternation process along the lamellar twinning plane of ilmenite induced by shockinduced high pressure and high temperature;(8) The P-T regime of 20-25 GPa and 1000 ℃ estimated for the Suizhou unmelted rock is suitable for phase transition of rutile into TiO_(2)-Ⅱ phase.
基金supported by the National Natural Science Foundation of China(22108238,21878259)the Zhejiang Provincial Natural Science Foundation of China(LR18B060001)+5 种基金Anhui Provincial Natural Science Founda-tion(1908085QB68)the Natural Science Foundation of the Anhui Higher Education Institutions of China(KJ2020A0275)Major Science and Technology Project of Anhui Province(201903a05020055)Foundation of Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology(ZJKL-ACEMT-1802)China Postdoctoral Science Foundation(2019M662060,2020T130580)Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology(BM2012110).
文摘The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.92065201,11874264,and 11974154)the Starting Grant of ShanghaiTech University and Analytical Instrumentation Center,SPST,ShanghaiTech University (Grant No.SPST-AIC10112914)support from the Natural Science Foundation of Shandong Province,China (Grant No.ZR2022MA004)。
文摘Monoclinicα-MoP_(2),with the OsGe2-type structure(space group C2/m,Z=4)and lattice parameters a=8.7248(11)Å,b=3.2322(4)Å,c=7.4724(9)Å,andβ=119.263°,was synthesized under a pressure of 4~GPa at a temperature between 1100℃and 1200℃.The structure ofα-MoP_(2) and its relationship to other transition metal diphosphides are discussed.Surprisingly,the ambient pressure phase orthorhombicβ-MoP_(2)(space group Cmc21)is denser in structure thanα-MoP_(2).Room-temperature high-pressure x-ray diffraction studies exclude the possibility of phase transition fromβ-MoP_(2) to α-MoP_(2),suggesting thatα-MoP_(2) is a stable phase at ambient conditions;this is also supported by the total energy and phonon calculations.
文摘The high-pressure diagram of V–N compounds is enriched by proposed seven new stable high-pressure phases.The P-1-VN_4with the armchair N-rich structure may be quenched to ambient conditions.The formed N–N covalent bond plays an important role for the structural stability of N-chain.The charge transfer results in a V–N ionic bond interaction,which further improves the stability of N-chain structure.The P-1-VN_4,P4mnc-VN_8,and Immm-VN_(10)with the outstanding detonation properties have potential application in explosive field.
基金supported by the National Key R&D Program of China(Nos.2022YFA1503104 and 2022YFA1503102)the Natural Science Foundation of Shandong Province(No.2022HWYQ-009)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20230243)Taishan Scholars Project(No.tspd20230601)Qilu Young Scholars Program of Shandong University.
文摘The nitrite(NO_(2)^(−))to ammonia(NH3)electroreduction reaction(NO_(2)^(−)RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH_(3) selectivity is to facilitate adsorption and activation of NO_(2)^(−),which is generally undesirable in unitary species.In this work,an efficient NO_(2)^(−)RR catalyst is constructed by cooperating Pd with In2O3,in which NO_(2)^(−)could adsorb on interfacial dual-site through“Pd–N–O–In”linkage,leading to strengthened NO_(2)^(−)adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In_(2)O_(3)composite exhibits moderate H^(*)adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH_(3)yield rate of 622.76 mmol h^(−1)g^(−1)cat with a Faradaic efficiency(FE)of 95.72%,good selectivity of 91.96%,and cycling stability towards the NO_(2)^(−)RR,surpassing unitary In_(2)O_(3)and Pd/C electrocatalysts.Besides,computed results indicate that NH_(3)production on Pd/In_(2)O_(3)follows the deoxidation to hydrogenation pathway.This work highlights the significance of H^(*)and NO_(2)^(−)adsorption modulation and N=O activation in NO_(2)^(−)RR electrochemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.
文摘Electrochemical nitrite reduction reaction(NO_(2)^(-)RR) is a potential sustainable route for regulating the nitrogen cycle and ambient ammonia(NH_(3)) synthesis.However,it remains a challenge to precisely regulate the reaction pathways and inhibit competing reactions(e.g.hydrogenolysis) for efficient and selective NH_(3) production in an aqueous solution environment.Here,we utilize the Schottky barrier-induced surface electric field to construct high-density electron-deficient Pd nanoparticles by modulating the N content in the carbon carrier to promote the enrichment and immobilization of NO_(2)^(-)on the electrode surface,which ensures the ultimate selectivity for NH_(3).With these properties,Pd@N_(0.14)C with the highest N content achieved excellent catalytic performance for the reduction of NO_(2)^(-)to NH_(3) with the 100% Faraday efficiency at-0.5 and-0.6 V vs,reversible hydrogen electrode(RHE) for NH_(3) production,which was significantly better than Pd/C and Pd@N_(x)C samples with lower N content.This study opens new avenues for rational construction of efficient electrocatalysts for nitrite removal and NH_(3) electrosynthesis.
基金Supported by the Natural Science Foundation of Shandong Province(No.ZR 2023 MD 059)the National Natural Science Foundation of China(No.41876135)。
文摘Previous studies have revealed that ammonia nitrogen has several adverse effects on clam Ruditapes philippinarum.However,knowledge is lacking regarding the related proteins involved in the toxicological responses,which is vital to elucidate the underlying mechanism of ammonia nitrogen.In this study,clams R.philippinarum were exposed to ammonia nitrogen for 21 d at two environmentally relevant concentrations.The tandem mass tags approach(TMT)was applied to assay the differentially expressed proteins(DEPs)in clam gill tissues on the 3 rd and 21 st day.Finally,a total of 7263 proteins were identified.Bioinformatics analyses revealed that clam protein profiles changed in dose-and time dependent manner after ammonia nitrogen exposure.We inferred that the clams may face heavy challenges after ammonia exposure,such as unbalanced gender ratio,lysosomal disease,energy lack,neurological disorders,altered glutamine metabolism,increased lipid synthesis,and impaired immunity.Variation profiles of enzyme activities of glutaminase and glutamine synthase provided direct evidence to verify the related inference from proteome data.Most of the inferred toxic effects merit further study.This study identified important proteins related to ammonia nitrogen toxicity in the clam and indicated the severe stress of marine ammonia pollution on the healthy development of mollusc aquaculture.
基金the National Natural Science Foundation of China(project code:52202470)Jilin Province Natural Science Foundation(project codes:20220101205JC,20220101212JC)+2 种基金Jilin Province Specific Project of Industrial Technology Research&Development(project code:2020C025-2)2021 Interdisciplinary Integration and Innovation Project of Jilin University(project code:XJRCYB07)Free Exploration Project of Changsha Automotive Innovation Research Institute of Jilin University(project code:CAIRIZT20220202)。
文摘For the deep understanding on combustion of ammonia/diesel,this study develops a reduced mechanism of ammonia/diesel with 227 species and 937 reactions.The sub-mechanism on ammonia/interactions of N-based and C-based species(N—C)/NOx is optimized using the Non-dominated Sorting Genetic Algorithm II(NSGA-II)with 200 generations.The optimized mechanism(named as 937b)is validated against combustion characteristics of ammonia/methane(which is used to examine the accuracy of N—C interactions)and ammonia/diesel blends.The ignition delay times(IDTs),the laminar flame speeds and most of key intermediate species during the combustion of ammonia/methane blends can be accurately simulated by 937b under a wide range of conditions.As for ammonia/diesel blends with various diesel energy fractions,reasonable predictions on the IDTs under pressures from 1.0 MPa to5.0 MPa as well as the laminar flame speeds are also achieved by 937b.In particular,with regard to the IDT simulations of ammonia/diesel blends,937b makes progress in both aspects of overall accuracy and computational efficiency,compared to a detailed ammonia/diesel mechanism.Further kinetic analysis reveals that the reaction pathway of ammonia during the combustion of ammonia/diesel blend mainly differs in the tendencies of oxygen additions to NH_2 and NH with different equivalence ratios.
基金Financial support from Ministerio de Ciencia e Innovación through projects PID2022-140143OB-I00(MCIN/AEI/10.13039/501100011033)and SO-CEX2019-000925-S(MCIN/AEI/10.13039/5011000110)supported by Marie Sk?odowska-Curie Actions Individual Fellowship grant funding to AMB,grant 101031365-SolTIMEthe support from the MSCA-COFUND I2:ICIQ Impulsion(GA 801474)。
文摘For carbon-free electrochemical fuel formation,the electrochemical cell must be powered by renewable energy.Obtaining solar-powered H_(2) fuel from water typically requires multiple photovoltaic cells and/or junctions to drive the water splitting reaction.Because of the lower thermodynamic requirements to oxidize ammonia compared to water,solar cells with smaller open circuit voltages can provide the required potential for ammonia splitting.In this work,a single perovskite solar cell with an open-circuit potential of 1.08 V is coupled to a 2-electrode electrochemical cell employing hybrid electroanodes functionalized with Ru-based molecular catalysts.The device is active for more than 30 min,producing N_(2) and H_(2) in a 1:2.9 ratio with 89%faradaic efficiency with no external applied bias.This work illustrates that hydrogen production from ammonia can be driven by conventional semiconductors.
基金National Natural Science Foundation of China(52076110,52106160)Jiangsu Provincial Natural Science Foundation of China(BK20200490,BK20220955)Fundamental Research Funds for the Central Universities(30923010208 and 30920031103).
文摘This study aimed to investigate the effects of ammonia addition on ethylene counter-flow diffusion flames with different diluents on the fuel or oxidizer side,using kinetic analyses.A special emphasis was put on assessing the coupled chemical effects of NH_(3) and CO_(2) on C2H4 combustion chemistry.The chemical effects could be evaluated by comparing fictitious inert NH_(3) or CO_(2) with normal active NH_(3) or CO_(2).The results revealed that the addition of NH_(3) decreased the mole fractions and production rates of key soot precursors,such as acetylene,propynyl,and benzene.When CO_(2) was used as the dilution gas,the coupled chemical effects of NH_(3) and CO_(2) were affected by the chemical effects of CO_(2) to varying degrees.With the oxidizer-side CO_(2) addition,the coupled chemical effects of NH_(3) and CO_(2) reduced the mole fractions of H,O,OH radicals,acetylene,propynyl,and benzene,while the effects differed from the fuel-side CO_(2) addition.The coupled chemical effects of NH_(3) and CO_(2) also promoted the formation of aldehyde contaminants,such as acetaldehyde,to some extent,particularly with CO_(2) addition on the oxidizer side.
基金the Science and Engineering Research Board(SERB),Government of India for funding this work(Sanction No.EEQ/2021/001116)。
文摘The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia synthesis.While the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia production.These hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the process.Researchers have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical reaction.Through mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the barriers.This review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst surface.It delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen reduction.By unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.
基金supported by the research program funded by the TKG Huchemssupported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)granted financial resources from the Ministry of Trade,Industry&Energy,Republic of Korea(20213030040590)supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(2021R1A5A1028138)。
文摘Ammonia allows storage and transport of hydrogen over long distances and is an attractive potential hydrogen carrier.Electrochemical decomposition has recently been used for the conversion of ammonia to hydrogen and is regarded as a future technology for production of CO_(2)-free pure hydrogen.Herein,a heterostructural Pt-Ir dual-layer electrode is developed and shown to achieve successful long-term operation in an ammonia electrolyzer with an anion exchange membrane(AEM).This electrolyzer consisted of eight membra ne electrode assemblies(MEAs)with a total geometric area of 200 cm~2 on the anode side,which resulted in a hydrogen production rate of 25 L h~(-1).We observed the degradation in MEA performance attributed to changes in the anode catalyst layer during hydrogen production via ammonia electrolysis.Furthermore,we demonstrated the relationship between the ammonia oxidation reaction(AOR)and the oxygen evolution reaction(OER).
基金supported by the National Natural Science Foundation of China[Nos.U21A20332,52103226,52202275,52203314,and 12204253]the Distinguished Young Scholars Fund of Jiangsu Province[No.BK20220061]the Fellowship of China Postdoctoral Science Foundation[No.2021M702382]。
文摘Ammonia(NH_(3))is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH_(3)synthesis is highly dependent on the conventional Haber–Bosch process that operates under harsh conditions,which consumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH_(3)under normal temperature and pressure conditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N_(2)and high N≡N cracking energy render the achievements of high NH_(3) yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NO_(x)^(-))are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NO_(x)^(-)−are ideal raw materials for NH_(3) production.Therefore,electrocatalytic NO_(x)^(-)−reduction to NH_(3)(eNO_(x)RR)is a prospective strategy to simultaneously realise environmental protection and NH_(3) synthesis.This review offers a comprehensive understanding of the thriving eNO_(x)RR under ambient conditions.At first,the popular theory and mechanism of eNO_(x)RR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NO_(x)−reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NO_(x)^(-1) reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH_(3) in the future.
基金the financial support from the Beijing Municipal Natural Science Foundation (No. 1242015)National Undergraduate Innovation and Entrepreneurship Training Program of China (No. 202310015019)Discipline Construction of Material Science and Engineering(Nos. 21090122014 and 21090123007)。
文摘Ammonia is one of the most important chemical raw materials in both manufacture and life of human.Traditionally Haber-Bosch method for ammonia synthesis involves high temperature and high pressure conditions,leading to significant energy consumption and environmental pollution.Non-thermal plasma(NTP) is a promising alternative approach to ammonia synthesis at low temperature and atmospheric pressure.In this study,the synergistic effect of nanosecond pulsed dielectric barrier discharge(np-DBD) and Ni-MOF-74 catalyst was investigated in ammonia synthesis by utilizing nitrogen and hydrogen as feedstock.The results demonstrated that the plasma catalytic-synthesis process parameters play a crucial role in the synthesis process of ammonia.The highest ammonia synthesis rate of 5145.16 μmol·g^(-1)·h^(-1)with an energy efficiency of 1.27 g·kWh^(-1)was observed in the presence of the Ni-MOF-74 catalyst,which was3.7 times higher than that without Ni-MOF-74 catalyst.The synergistic effect of Ni-MOF-74catalyst and nanosecond pulsed plasma was explored by in-situ plasma discharge diagnostics.
基金the financial support provided by the Canada Research Chair program and the Natural Science and Engineering Research Council of Canada (NSERC)
文摘Ammonia serves both as a widely used fertilizer and environmentally friendly energy source due to its high energy density,rich hydrogen content,and emissions-free combustion.Additionally,it offers convenient transportation and storage as a hydrogen carrier.The dominant method used for large-scale ammonia production is the Haber-Bosch process,which requires high temperatures and pressures and is energy-intensive.However,non-thermal plasma offers an eco-friendly alternative for ammonia synthesis,gaining significant attention.It enables ammonia production at lower temperatures and pressures using plasma technology.This review provides insights into the catalyst and reactor developments,which are pivotal for promoting ammonia efficiency and addressing existing challenges.At first,the reaction kinetics and mechanisms are introduced to gain a comprehensive understanding of the reaction pathways involved in plasma-assisted ammonia synthesis.Thereafter,the enhancement of ammonia synthesis efficiency is discussed by developing and optimizing plasma reactors and effective catalysts.The effect of other feeding sources,such as water and methane,instead of hydrogen is also presented.Finally,the challenges and possible solutions are outlined to facilitate energy-saving and enhance ammonia efficiency in the future.
基金the grant support from the National Natural Science Foundation of China (No. 21975018, 22278032)。
文摘Ammonia is gaining increasing attention as a green alternative fuel for achieving large-scale carbon emission reduction. Despite its potential technical prospects, the harsh ignition conditions and slow flame propagation speed of ammonia pose significant challenges to its application in engines. Non-equilibrium plasma has been identified as a promising method, but current research on plasma-enhanced ammonia combustion is limited and primarily focuses on ignition characteristics revealed by kinetic models. In this study, low-temperature and low-pressure chemistry in plasma-assisted ammonia oxidative pyrolysis is investigated by integrated studies of steady-state GC measurements and mathematical simulation. The detailed kinetic mechanism of NH_(3) decomposition in plasma-driven Ar/NH_(3) and Ar/NH_(3)/O_(2) mixtures has been developed. The numerical model has good agreements with the experimental measurements in NH_(3)/O_(2) consumption and N_(2)/H_(2) generation, which demonstrates the rationality of modelling. Based on the modelling results, species density profiles, path flux and sensitivity analysis for the key plasmaproduced species such as NH_(2), NH, H_(2), OH, H, O, O(^(1)D), O_(2)(a^(1)△_(g)), O_(2)(b^(1)∑_(g)^(+)), Ar^(*), H^(-), Ar^(+), NH_(3)^(+), O_(2)^(-) in the discharge and afterglow are analyzed in detail to illustrate the effectiveness of the active species on NH_(3) excitation and decomposition at low temperature and relatively higher E/N values. The results revealed that NH_(2), NH, H as well as H_(2) are primarily generated through the electron collision reactions e + NH_(3)→ e + NH_(2)+ H, e + NH_(3)→ e + NH + H_(2) and the excited-argon collision reaction Ar^(*) + NH_(3)+ H → Ar + NH_(2)+ 2H, which will then react with highly reactive oxidative species such as O_(2)^(*), O^(*), O, OH, and O_(2) to produce stable products of NOx and H_(2)O. NH_(3)→ NH is found a specific pathway for NH_(3) consumption with plasma assistance, which further highlights the enhanced kinetic effects.