Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz...Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.展开更多
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca...Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.展开更多
Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics t...Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.展开更多
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ...The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.展开更多
Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)...Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.展开更多
We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in...We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.展开更多
Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlatio...Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.展开更多
Decarbonization and decontamination of the iron and steel industry(ISI),which contributes up to 15%to anthropogenic CO_(2) emissions(or carbon emissions)and significant proportions of air and water pollutant emissions...Decarbonization and decontamination of the iron and steel industry(ISI),which contributes up to 15%to anthropogenic CO_(2) emissions(or carbon emissions)and significant proportions of air and water pollutant emissions in China,are challenged by the huge demand for steel.Carbon and pollutants often share common emission sources,indicating that emission reduction could be achieved synergistically.Here,we explored the inherent potential of measures to adjust feedstock composition and technological structure and to control the size of the ISI to achieve carbon emission reduction(CER)and pollution emission reduction(PER).We investigated five typical pollutants in this study,namely,petroleum hydrocarbon pollutants and chemical oxygen demand in wastewater,particulate matter,SO_(2),and NO_(x) in off gases,and examined synergies between CER and PER by employing cross elasticity for the period between 2022 and 2035.The results suggest that a reduction of 8.7%-11.7%in carbon emissions and 20%-31%in pollution emissions(except for particulate matter emissions)could be achieved by 2025 under a high steel scrap ratio(SSR)scenario.Here,the SSR and electric arc furnace(EAF)ratio serve critical roles in enhancing synergies between CER and PER(which vary with the type of pollutant).However,subject to a limited volume of steel scrap,a focused increase in the EAF ratio with neglection of the available supply of steel scrap to EAF facilities would lead to an increase carbon and pollution emissions.Although CER can be achieved through SSR and EAF ratio optimization,only when the crude steel production growth rate remains below 2.2%can these optimization measures maintain the emissions in 2030 at a similar level to that in 2021.Therefore,the synergistic effects between PER and CER should be considered when formulating a development route for the ISI in the future.展开更多
Successfully utilized non-axisymmetric endwalls to enhance turbine efficiencies(aerodynamic and turbine inlet temperatures)by controlling the characteristics of the secondary flow in a blade passage.This is accomplish...Successfully utilized non-axisymmetric endwalls to enhance turbine efficiencies(aerodynamic and turbine inlet temperatures)by controlling the characteristics of the secondary flow in a blade passage.This is accomplished by steady-state numerical hydrodynamics and deep knowledge of the field of flow.Because of the interaction between mainstream and purge flow contributing supplementary losses in the stage,non-axisymmetric endwalls are highly susceptible to the inception of purge flow exit compared to the flat and any advantage rapidly vanishes.The conclusions reveal that the supreme endwall pattern could yield a lowering of the gross pressure loss at the design stage and is related to the size of the top-loss location being productively lowered.This has led to diminished global thermal exchange lowered in the passage of the vane alone.The reverse flow adjacent to the suction side corner of the endwall is migrated farther from the vane surface,as the deviated pressure spread on the endwall accelerates the flow and progresses the reverse flow core still downstream.The depleted association between the tornado-like vortex and the corner vortex adjacent to the suction side corner of the endwall is the dominant mechanism of control in the contoured end wall.In this publication,we show that the non-axisymmetric endwall contouring by selective numerical shape change method at most prominent locations is advantageous in lowering the thermal load in turbines to augment the net heat flux reduction as well as the aerodynamic performance using multi-objective optimization.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
The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to C...The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.展开更多
N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher ...N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.展开更多
Tamanu oil, derived from the nuts of Calophyllum inophyllum, has gained increasing attention for its potential in acne management due to its purported anti-inflammatory and wound-healing properties. This analysis eval...Tamanu oil, derived from the nuts of Calophyllum inophyllum, has gained increasing attention for its potential in acne management due to its purported anti-inflammatory and wound-healing properties. This analysis evaluates the efficacy of tamanu oil in acne treatment with a specific focus on its impact on inflammation and scar reduction. The novelty of this research lies in its comprehensive analysis of tamanu oil’s dual mechanism of action: reducing acne-related inflammation and promoting the healing of acne scars. Clinical trials and laboratory analyses were conducted to assess the oil’s effectiveness in diminishing erythema, swelling, and post-acne scarring compared to conventional treatments. Preliminary findings demonstrate that tamanu oil significantly reduces inflammation and accelerates wound healing, potentially offering a promising adjunct or alternative to standard acne therapies. Future research should aim to optimize formulation and application protocols, long-term effects, and comparative therapeutic efficacy with other anti-inflammatory agents. Tamanu oil offers a novel and effective approach to acne management, with potential advantages that go beyond inflammation reduction to include enhanced scar reduction, making it a subject that warrants further investigation.展开更多
The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as titanomagnetite.However,the defluidization of reduc...The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as titanomagnetite.However,the defluidization of reduced iron particles with a high metallization degree at a high temperature will seriously affect the operation of fluidized bed reduction.Coupling the pre-oxidation enhancing reduction and the particle surface modification of titanomagnetite,the behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized bed reduction of titanomagnetite are systematically studied in this paper.Pre-oxidation treatment of titanomagnetite can significantly lower the critical stable reduction fluidization gas velocity to 0.17 m/s,which is reduced by 56%compared to that of titanomagnetite reduction without pre-oxidation,while achieving a metallization degree of>90%,Corresponding to the different reduction fluidization behaviors,three pre-oxidation operation regions have been divided,taking oxidation degrees of 26%and 86%as the boundaries.Focusing on the particle surface morphology evolution in the pre-oxidation-reduction process,the relationship between the surface morphology of pre-oxidized ore and the reduced iron with fluidization properties is built.The improving method of pre-oxidation on the reduction fluidization provides a novel approach to prevent defluidization by particle surface modification,especially for the fluidized bed reduction of poly-metallic iron ore.展开更多
Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electroche...Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.展开更多
To improve the cruise flight performance of aircraft, two new configurations of plasma actuators(grid-type and super-dense array) were investigated to reduce the turbulent skin friction drag of a low-speed airfoil. Th...To improve the cruise flight performance of aircraft, two new configurations of plasma actuators(grid-type and super-dense array) were investigated to reduce the turbulent skin friction drag of a low-speed airfoil. The induced jet characteristics of the two actuators in quiescent air were diagnosed with high-speed particle image velocimetry(PIV), and their drag reduction efficiencies were examined under different operating conditions in a wind tunnel. The results showed that the grid-type plasma actuator was capable of producing a wall-normal jet array(peak magnitude: 1.07 m/s) similar to that generated in a micro-blowing technique, while the superdense array plasma actuator created a wavy wall-parallel jet(magnitude: 0.94 m/s) due to the discrete spanwise electrostatic forces. Under a comparable electrical power consumption level,the super-dense array plasma actuator array significantly outperformed the grid-type configuration,reducing the total airfoil friction drag by approximately 22% at a free-stream velocity of 20 m/s.The magnitude of drag reduction was proportional to the dimensionless jet velocity ratio(r), and a threshold r = 0.014 existed under which little impact on airfoil drag could be discerned.展开更多
The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing mul...The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and pathways.Herein,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))production.The results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against aggregation.Furthermore,co-activation of the inert N_(2)reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond elongation.Our high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N_(2)–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.20×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions.展开更多
Nanoparticles(NPs)have gained significant attention as a functional material due to their ability to effectively enhance pressure reduction in injection processes in ultra-low permeability reservoirs.NPs are typically...Nanoparticles(NPs)have gained significant attention as a functional material due to their ability to effectively enhance pressure reduction in injection processes in ultra-low permeability reservoirs.NPs are typically studied in controlled laboratory conditions,and their behavior in real-world,complex environments such as ultra-low permeability reservoirs,is not well understood due to the limited scope of their applications.This study investigates the efficacy and underlying mechanisms of NPs in decreasing injection pressure under various injection conditions(25—85℃,10—25 MPa).The results reveal that under optimal injection conditions,NPs effectively reduce injection pressure by a maximum of 22.77%in core experiment.The pressure reduction rate is found to be positively correlated with oil saturation and permeability,and negatively correlated with temperature and salinity.Furthermore,particle image velocimetry(PIV)experiments(25℃,atmospheric pressure)indicate that the pressure reduction is achieved by NPs through the reduction of wall shear resistance and wettability change.This work has important implications for the design of water injection strategies in ultra-low permeability reservoirs.展开更多
The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetal...The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.展开更多
The industrial sector is the primary source of carbon emissions in China.In pursuit of meeting its carbon reduction targets,China aims to promote resource consumption sustainability,reduce energy consumption,and achie...The industrial sector is the primary source of carbon emissions in China.In pursuit of meeting its carbon reduction targets,China aims to promote resource consumption sustainability,reduce energy consumption,and achieve carbon neutrality within its processing industries.An effective strategy to promote energy savings and carbon reduction throughout the life cycle of materials is by applying life cycle engineering technology.This strategy aims to attain an optimal solution for material performance,resource consumption,and environmental impact.In this study,five types of technologies were considered:raw material replacement,process reengineering,fuel replacement,energy recycling and reutilization,and material recycling and reutilization.The meaning,methodology,and development status of life cycle engineering technology abroad and domestically are discussed in detail.A multidimensional analysis of ecological design was conducted from the perspectives of resource and energy consumption,carbon emissions,product performance,and recycling of secondary resources in a manufacturing process.This coupled with an integrated method to analyze carbon emissions in the entire life cycle of a material process industry was applied to the nonferrous industry,as an example.The results provide effective ideas and solutions for achieving low or zero carbon emission production in the Chinese industry as recycled aluminum and primary aluminum based on advanced technologies had reduced resource consumption and emissions as compared to primary aluminum production.展开更多
基金supported by the National Natural Science Foundation of China(22234005,21974070)the Natural Science Foundation of Jiangsu Province(BK20222015)。
文摘Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.
基金supported by the National Natural Science Foundation of China (22178149)Jiangsu Distinguished Professor Program+4 种基金Natural Science Foundation of Jiangsu Province for Outstanding Youth Scientists (BK20211599)Key R and D Project of Zhenjiang City (CQ2022001)Scientific Research Startup Foundation of Jiangsu University (Nos. 202096 and 22JDG020)Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment of Fuzhou University (SKLPEE-KF202310)the Opening Project of Structural Optimization and Application of Functional Molecules Key Laboratory of Sichuan Province (2023GNFZ-01)。
文摘Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.
基金supported by National Natural Science Foundation of China(12372049)Science and Technology Program of China National Accreditation Service for Confor-mity Assessment(2022CNAS15)+1 种基金Sichuan Science and Technology Program(2023JDRC0062)Independent Project of State Key Laboratory of Rail Transit Vehicle System(2023TPL-T06).
文摘Reducing the aerodynamic drag and noise levels of high-speed pantographs is important for promoting environmentally friendly,energy efficient and rapid advances in train technology.Using computational fluid dynamics theory and the K-FWH acoustic equation,a numerical simulation is conducted to investigate the aerodynamic characteristics of high-speed pantographs.A component optimization method is proposed as a possible solution to the problemof aerodynamic drag and noise in high-speed pantographs.The results of the study indicate that the panhead,base and insulator are the main contributors to aerodynamic drag and noise in high-speed pantographs.Therefore,a gradual optimization process is implemented to improve the most significant components that cause aerodynamic drag and noise.By optimizing the cross-sectional shape of the strips and insulators,the drag and noise caused by airflow separation and vortex shedding can be reduced.The aerodynamic drag of insulator with circular cross section and strips with rectangular cross section is the largest.Ellipsifying insulators and optimizing the chamfer angle and height of the windward surface of the strips can improve the aerodynamic performance of the pantograph.In addition,the streamlined fairing attached to the base can eliminate the complex flow and shield the radiated noise.In contrast to the original pantograph design,the improved pantograph shows a 21.1%reduction in aerodynamic drag and a 1.65 dBA reduction in aerodynamic noise.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(NRF,2021R1C1C1013953,2022K1A4A7A04094394,2022K1A4A7A04095890)。
文摘The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.
基金financial support from the National Natural Science Foundation of China(No.22272038)the Science and Technology Planning Project of Guangzhou City(No.2023A03J0026)。
文摘Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO_(2)reduction(PCO_(2)R)systems.Herein,monoclinic Cu_(2)(OH)_(2)CO_(3)is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO_(2)R in the absence of any sacrificial agent and cocatalysts.Based on a Cu_(2)(OH)_(2)^(13)CO_(3)photocatalyst and 13CO_(2)two-sided^(13)C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO_(2)transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu_(2)(OH)_(2)CO_(3)are definitely revealed.The PCO_(2)R activity of Cu_(2)(OH)_(2)CO_(3)is comparable to some of state-of-the-art novel photocatalysts.Significantly,the PCO_(2)R properties can be further greatly enhanced by simply combining Cu_(2)(OH)_(2)CO_(3)with typical TiO_(2)to construct composites photocatalyst.The highest CO_(2)and CH_(4)production rates by 7.5 wt%Cu_(2)(OH)_(2)CO_(3)-TiO_(2)reach 16.4μmol g^(-1)h^(-1)and 116.0μmol g^(-1)h^(-1),respectively,which are even higher than that of some of PCO_(2)R systems containing sacrificial agents or precious metals modified photocatalysts.This work provides a better understanding for the PCO_(2)R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.
基金the Natural Science Foundation of China(11922415,12274471)Guangdong Basic and Applied Basic Research Foundation(2022A1515011168,2019A1515011718,2019A1515011337)the Key Research and Development Program of Guangdong Province,China(2019B110209003).
文摘We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.
基金support from the National Science Foundation of China(22078190)the National Key R&D Plan of China(2020YFB1505802).
文摘Joint time–frequency analysis is an emerging method for interpreting the underlying physics in fuel cells,batteries,and supercapacitors.To increase the reliability of time–frequency analysis,a theoretical correlation between frequency-domain stationary analysis and time-domain transient analysis is urgently required.The present work formularizes a thorough model reduction of fractional impedance spectra for electrochemical energy devices involving not only the model reduction from fractional-order models to integer-order models and from high-to low-order RC circuits but also insight into the evolution of the characteristic time constants during the whole reduction process.The following work has been carried out:(i)the model-reduction theory is addressed for typical Warburg elements and RC circuits based on the continued fraction expansion theory and the response error minimization technique,respectively;(ii)the order effect on the model reduction of typical Warburg elements is quantitatively evaluated by time–frequency analysis;(iii)the results of time–frequency analysis are confirmed to be useful to determine the reduction order in terms of the kinetic information needed to be captured;and(iv)the results of time–frequency analysis are validated for the model reduction of fractional impedance spectra for lithium-ion batteries,supercapacitors,and solid oxide fuel cells.In turn,the numerical validation has demonstrated the powerful function of the joint time–frequency analysis.The thorough model reduction of fractional impedance spectra addressed in the present work not only clarifies the relationship between time-domain transient analysis and frequency-domain stationary analysis but also enhances the reliability of the joint time–frequency analysis for electrochemical energy devices.
基金supported by the National Key Research and Development Program of China(2019YFC1904800)the National Natural Science Foundation of China(72274105).
文摘Decarbonization and decontamination of the iron and steel industry(ISI),which contributes up to 15%to anthropogenic CO_(2) emissions(or carbon emissions)and significant proportions of air and water pollutant emissions in China,are challenged by the huge demand for steel.Carbon and pollutants often share common emission sources,indicating that emission reduction could be achieved synergistically.Here,we explored the inherent potential of measures to adjust feedstock composition and technological structure and to control the size of the ISI to achieve carbon emission reduction(CER)and pollution emission reduction(PER).We investigated five typical pollutants in this study,namely,petroleum hydrocarbon pollutants and chemical oxygen demand in wastewater,particulate matter,SO_(2),and NO_(x) in off gases,and examined synergies between CER and PER by employing cross elasticity for the period between 2022 and 2035.The results suggest that a reduction of 8.7%-11.7%in carbon emissions and 20%-31%in pollution emissions(except for particulate matter emissions)could be achieved by 2025 under a high steel scrap ratio(SSR)scenario.Here,the SSR and electric arc furnace(EAF)ratio serve critical roles in enhancing synergies between CER and PER(which vary with the type of pollutant).However,subject to a limited volume of steel scrap,a focused increase in the EAF ratio with neglection of the available supply of steel scrap to EAF facilities would lead to an increase carbon and pollution emissions.Although CER can be achieved through SSR and EAF ratio optimization,only when the crude steel production growth rate remains below 2.2%can these optimization measures maintain the emissions in 2030 at a similar level to that in 2021.Therefore,the synergistic effects between PER and CER should be considered when formulating a development route for the ISI in the future.
文摘Successfully utilized non-axisymmetric endwalls to enhance turbine efficiencies(aerodynamic and turbine inlet temperatures)by controlling the characteristics of the secondary flow in a blade passage.This is accomplished by steady-state numerical hydrodynamics and deep knowledge of the field of flow.Because of the interaction between mainstream and purge flow contributing supplementary losses in the stage,non-axisymmetric endwalls are highly susceptible to the inception of purge flow exit compared to the flat and any advantage rapidly vanishes.The conclusions reveal that the supreme endwall pattern could yield a lowering of the gross pressure loss at the design stage and is related to the size of the top-loss location being productively lowered.This has led to diminished global thermal exchange lowered in the passage of the vane alone.The reverse flow adjacent to the suction side corner of the endwall is migrated farther from the vane surface,as the deviated pressure spread on the endwall accelerates the flow and progresses the reverse flow core still downstream.The depleted association between the tornado-like vortex and the corner vortex adjacent to the suction side corner of the endwall is the dominant mechanism of control in the contoured end wall.In this publication,we show that the non-axisymmetric endwall contouring by selective numerical shape change method at most prominent locations is advantageous in lowering the thermal load in turbines to augment the net heat flux reduction as well as the aerodynamic performance using multi-objective optimization.
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Natural Science Foundation of Shandong Province,Grant/Award Number:ZR2022MB106national training program of innovation and entrepreneurship for undergraduates,Grant/Award Number:202210424099National Natural Science Foundation of China,Grant/Award Numbers:21601067,21701057,21905147。
文摘The photocatalytic conversion of CO_(2)into solar‐powered fuels is viewed as a forward‐looking strategy to address energy scarcity and global warming.This work demonstrated the selective photoreduction of CO_(2)to CO using ultrathin Bi_(12)O_(17)Cl_(2)nanosheets decorated with hydrothermally synthesized bismuth clusters and oxygen vacancies(OVs).The characterizations revealed that the coexistences of OVs and Bi clusters generated in situ contributed to the high efficiency of CO_(2)–CO conversion(64.3μmol g^(−1)h^(−1))and perfect selectivity.The OVs on the facet(001)of the ultrathin Bi_(12)O_(17)Cl_(2)nanosheets serve as sites for CO_(2)adsorption and activation sites,capturing photoexcited electrons and prolonging light absorption due to defect states.In addition,the Bi‐cluster generated in situ offers the ability to trap holes and the surface plasmonic resonance effect.This study offers great potential for the construction of semiconductor hybrids as multiphotocatalysts,capable of being used for the elimination and conversion of CO_(2)in terms of energy and environment.
基金We acknowledge the National Natural Science Foundation of China(No.22275134)for fi nancial support.
文摘N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively studied.However,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon materials.Consequently,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not clear.In this study,we discover a two-step oxida-tion process of N-doped carbon during the ORR.The fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional groups.This oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)ORR.Subsequently,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant species.We also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.
文摘Tamanu oil, derived from the nuts of Calophyllum inophyllum, has gained increasing attention for its potential in acne management due to its purported anti-inflammatory and wound-healing properties. This analysis evaluates the efficacy of tamanu oil in acne treatment with a specific focus on its impact on inflammation and scar reduction. The novelty of this research lies in its comprehensive analysis of tamanu oil’s dual mechanism of action: reducing acne-related inflammation and promoting the healing of acne scars. Clinical trials and laboratory analyses were conducted to assess the oil’s effectiveness in diminishing erythema, swelling, and post-acne scarring compared to conventional treatments. Preliminary findings demonstrate that tamanu oil significantly reduces inflammation and accelerates wound healing, potentially offering a promising adjunct or alternative to standard acne therapies. Future research should aim to optimize formulation and application protocols, long-term effects, and comparative therapeutic efficacy with other anti-inflammatory agents. Tamanu oil offers a novel and effective approach to acne management, with potential advantages that go beyond inflammation reduction to include enhanced scar reduction, making it a subject that warrants further investigation.
基金grateful for financial support from the National Natural Science Foundation of China(Nos.22378405 and 51974287)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA29040100)the National Key Research and Development Program of China(No.2023YFC2908002).
文摘The direct reduction process is an important development direction of low-carbon ironmaking and efficient comprehensive utilization of poly-metallic iron ore,such as titanomagnetite.However,the defluidization of reduced iron particles with a high metallization degree at a high temperature will seriously affect the operation of fluidized bed reduction.Coupling the pre-oxidation enhancing reduction and the particle surface modification of titanomagnetite,the behavior and mechanism of pre-oxidation improvement on fluidization in the fluidized bed reduction of titanomagnetite are systematically studied in this paper.Pre-oxidation treatment of titanomagnetite can significantly lower the critical stable reduction fluidization gas velocity to 0.17 m/s,which is reduced by 56%compared to that of titanomagnetite reduction without pre-oxidation,while achieving a metallization degree of>90%,Corresponding to the different reduction fluidization behaviors,three pre-oxidation operation regions have been divided,taking oxidation degrees of 26%and 86%as the boundaries.Focusing on the particle surface morphology evolution in the pre-oxidation-reduction process,the relationship between the surface morphology of pre-oxidized ore and the reduced iron with fluidization properties is built.The improving method of pre-oxidation on the reduction fluidization provides a novel approach to prevent defluidization by particle surface modification,especially for the fluidized bed reduction of poly-metallic iron ore.
基金financially supported by the Natural Science Foundation of Shandong Province (ZR2020QB132,ZR2020MB025)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL202108SIC)the Taishan Scholar Program of Shandong Province (ts201712046)。
文摘Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.
基金supported by National Natural Science Foundation of China (Nos.12002384, U2341277,and 52025064)Foundation Strengthening Program (No.2021JJ-0786)。
文摘To improve the cruise flight performance of aircraft, two new configurations of plasma actuators(grid-type and super-dense array) were investigated to reduce the turbulent skin friction drag of a low-speed airfoil. The induced jet characteristics of the two actuators in quiescent air were diagnosed with high-speed particle image velocimetry(PIV), and their drag reduction efficiencies were examined under different operating conditions in a wind tunnel. The results showed that the grid-type plasma actuator was capable of producing a wall-normal jet array(peak magnitude: 1.07 m/s) similar to that generated in a micro-blowing technique, while the superdense array plasma actuator created a wavy wall-parallel jet(magnitude: 0.94 m/s) due to the discrete spanwise electrostatic forces. Under a comparable electrical power consumption level,the super-dense array plasma actuator array significantly outperformed the grid-type configuration,reducing the total airfoil friction drag by approximately 22% at a free-stream velocity of 20 m/s.The magnitude of drag reduction was proportional to the dimensionless jet velocity ratio(r), and a threshold r = 0.014 existed under which little impact on airfoil drag could be discerned.
基金financially supported in China by the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province (No. JC2018004)
文摘The co-catalysis between single atom catalyst(SAC)and its support has recently emerged as a promising strategy to synergistically boost the catalytic activity of some complex electrochemical reactions,encompassing multiple intermediates and pathways.Herein,we utilized defective BC_(3)monolayer-supported SACs as a prototype to investigate the cooperative effects of SACs and their support on the catalytic performance of the nitrogen reduction reaction(NRR)for ammonia(NH_(3))production.The results showed that these SACs can be firmly stabilized on these defective BC_(3)supports with high stability against aggregation.Furthermore,co-activation of the inert N_(2)reactant was observed in certain embedded SACs and their neighboring B atoms on certain BC3 sheets due to the noticeable charge transfer and significant N–N bond elongation.Our high-throughput screening revealed that the Mo/DV_(CC)and W/DV_(CC)exhibit superior NRR catalytic performance,characterized by a low limiting potential of−0.33 and−0.43 V,respectively,which can be further increased under acid conditions based on the constant potential method.Moreover,varying NRR catalytic activities can be attributed to the differences in the valence state of active sites.Remarkably,further microkinetic modeling analysis displayed that the turnover frequency of N_(2)–to–NH_(3)conversion on Mo/DV_(CC)is as large as 1.20×10^(−3)s^(−1)site^(−1) at 700 K and 100 bar,thus guaranteeing its ultra-fast reaction rate.Our results not only suggest promising advanced electrocatalysts for NRR but also offer an effective avenue to regulate the electrocatalytic performance via the co-catalytic metal–support interactions.
基金supported by the National Natural Science Foundation of China(Nos.52074249,U1663206,52204069)Fundamental Research Funds for the Central Universities。
文摘Nanoparticles(NPs)have gained significant attention as a functional material due to their ability to effectively enhance pressure reduction in injection processes in ultra-low permeability reservoirs.NPs are typically studied in controlled laboratory conditions,and their behavior in real-world,complex environments such as ultra-low permeability reservoirs,is not well understood due to the limited scope of their applications.This study investigates the efficacy and underlying mechanisms of NPs in decreasing injection pressure under various injection conditions(25—85℃,10—25 MPa).The results reveal that under optimal injection conditions,NPs effectively reduce injection pressure by a maximum of 22.77%in core experiment.The pressure reduction rate is found to be positively correlated with oil saturation and permeability,and negatively correlated with temperature and salinity.Furthermore,particle image velocimetry(PIV)experiments(25℃,atmospheric pressure)indicate that the pressure reduction is achieved by NPs through the reduction of wall shear resistance and wettability change.This work has important implications for the design of water injection strategies in ultra-low permeability reservoirs.
基金Natural Science Foundation of Jiangsu Province (BK20210735)National Natural Science Foundation of China (52201269, 52302296)+4 种基金Collaborative Innovation Center of Suzhou Nano Science and Technologythe 111 Projectthe Suzhou Key Laboratory of Functional Nano and Soft MaterialsJiangsu Key Laboratory for Carbon-Based Functional Materials & Devicesthe funding from the Gusu leading talent plan for scientific and technological innovation and entrepreneurship (ZXL2022487)。
文摘The development of electrocatalysts for the oxygen reduction reaction(ORR) that bears high selectivity,exceptional activity,and long-term stability is crucial for advancing various green energy technologies.Intermetallics composed of platinum and transition metals are considered to be promising candidates for this purpose.However,they typically face challenges such as unfavorable intrinsic activity and a propensity for particle aggregation,diminishing their ORR performance.Against this backdrop,we present our findings on a N-doped carbon confined Pt_(3)Co intermetallic doped with p-block metal tin(Pt_(3)Co_(x)Sn_(1-x)/NC).The introduction of Sn induces lattice strain due to its larger atomic size,which leads to the distortion of the Pt_(3)Co lattice structure,while the coupling of carbon polyhedra inhibits the particle aggregation.The optimized Pt_(3)Co_(0.8)Sn_(0.2)/NC catalyst demonstrates an impressive half-wave potential of 0.86 V versus RHE,surpassing both Pt_(3)Co/NC and Pt_(3)Sn/NC catalysts.Moreover,the Pt_(3)Co_(0.8)Sn_(0.2)/NC exhibits a mass-specific activity as high as 1.4 A mg_(Pt)^(-1),ranking it in the top level among the intermetallicsbased ORR electrocatalysts.When further employed as a cathode material in a self-assembled zinc-air battery,it shows stable operation for over 80 h.These results underscore the significant impact of lattice strain engineering through the strategic doping of p-block metal in the carbon-confined Pt_(3)Co intermetallic,thereby enhancing the catalytic efficiency for the ORR.
基金supported by the National Key Research and Development Programs(2021YFB3704201 and 2021YFB3700902).
文摘The industrial sector is the primary source of carbon emissions in China.In pursuit of meeting its carbon reduction targets,China aims to promote resource consumption sustainability,reduce energy consumption,and achieve carbon neutrality within its processing industries.An effective strategy to promote energy savings and carbon reduction throughout the life cycle of materials is by applying life cycle engineering technology.This strategy aims to attain an optimal solution for material performance,resource consumption,and environmental impact.In this study,five types of technologies were considered:raw material replacement,process reengineering,fuel replacement,energy recycling and reutilization,and material recycling and reutilization.The meaning,methodology,and development status of life cycle engineering technology abroad and domestically are discussed in detail.A multidimensional analysis of ecological design was conducted from the perspectives of resource and energy consumption,carbon emissions,product performance,and recycling of secondary resources in a manufacturing process.This coupled with an integrated method to analyze carbon emissions in the entire life cycle of a material process industry was applied to the nonferrous industry,as an example.The results provide effective ideas and solutions for achieving low or zero carbon emission production in the Chinese industry as recycled aluminum and primary aluminum based on advanced technologies had reduced resource consumption and emissions as compared to primary aluminum production.