Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective int...Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.展开更多
This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applicati...This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.展开更多
China’s low-carbon development path will make significant contributions to achieving global sustainable development goals.Due to the diverse natural and economic conditions across different regions in China,there exi...China’s low-carbon development path will make significant contributions to achieving global sustainable development goals.Due to the diverse natural and economic conditions across different regions in China,there exists an imbalance in the distribution of car-bon emissions.Therefore,regional cooperation serves as an effective means to attain low-carbon development.This study examined the pattern of carbon emissions and proposed a potential joint emission reduction strategy by utilizing the industrial carbon emission intens-ity(ICEI)as a crucial factor.We utilized social network analysis and Local Indicators of Spatial Association(LISA)space-time trans-ition matrix to investigate the spatiotemporal connections and discrepancies of ICEI in the cities of the Pearl River Basin(PRB),China from 2010 to 2020.The primary drivers of the ICEI were determined through geographical detectors and multi-scale geographically weighted regression.The results were as follows:1)the overall ICEI in the Pearl River Basin is showing a downward trend,and there is a significant spatial imbalance.2)There are numerous network connections between cities regarding the ICEI,but the network structure is relatively fragile and unstable.3)Economically developed cities such as Guangzhou,Foshan,and Dongguan are in the center of the network while playing an intermediary role.4)Energy consumption,industrialization,per capita GDP,urbanization,science and techno-logy,and productivity are found to be the most influential variables in the spatial differentiation of ICEI,and their combination in-creased the explanatory power of the geographic variation of ICEI.Finally,through the analysis of differences and connections in urban carbon emissions under different economic levels and ICEI,the study suggests joint carbon reduction strategies,which are centered on carbon transfer,financial support,and technological assistance among cities.展开更多
Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selectiv...Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selective extraction of lithium from spent Li-CoO_(2)(LCO)cathodes to overcome the incomplete recovery and loss of lithium during the recycling process.The LCO layered structure was destroyed and lithium was completely converted into water-soluble Li2CO_(3)under a suitable temperature to control the reduced state of the cobalt oxide.The Co metal agglomerates generated during medium-temperature carbon reduction roasting were broken by wet grinding and ultrasonic crushing to release the entrained lithium.The results showed that 99.10%of the whole lithium could be recovered as Li2CO_(3)with a purity of 99.55%.This work provided a new perspective on the preferentially selective extraction of lithium from spent lithium batteries.展开更多
Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and s...Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and stability,organic integration from electrode design to device assembly is required.To address these challenges,a free-standing reduced graphene oxide(rGO)/carbon film with a unique sandwich structure has been designed via the assistance of vacuum-assistant filtration for lithium-ion capacitors(LICs).The graphene acts as not only a binder to construct a three-dimensional conductive network but also an active material to provide additional capacitive lithium storage sites,thus enabling fast ion/electron transport and improving the capacity.The designed rGO/hard carbon(rGO/HC)and rGO/activated carbon(rGO/AC)free-standing films exhibit enhanced specific capacities(513.7 mA h g^(-1)for rGO/HC and 102.8 mA h g^(-1)for rGO/AC)and excellent stability.Moreover,the integrated flexible quasi-solid-state rGO/AC//rGO/HC LIC devices possess a maximum energy density of 138.3 Wh kg^(-1),a high power density of 11 kW kg^(-1),and improved cycling performance(84.4%capacitance maintained after 10,000 cycles),superior to the AC//HC LIC(43.5%retention).Such a strategy enlightens the development of portable flexible LICs.展开更多
This study investigated the effect of magnesium application on peanut growth and yield under two nitrogen(N)application rates in acidic soil in southern China.The chlorophyll content,net photosynthetic rate and dry ma...This study investigated the effect of magnesium application on peanut growth and yield under two nitrogen(N)application rates in acidic soil in southern China.The chlorophyll content,net photosynthetic rate and dry matter accumulation of the N-sensitive cultivar decreased under reduced N treatments,whereas no effect was observed on the relevant indicators in the N-insensitive variety GH1026.Mg application increased the net photosynthetic rate by increasing the expression of genes involved in chlorophyll synthesis and Rubisco activity in the leaves during the pegging stage under 50%N treatment,while no effect on the net photosynthetic rate was observed under the 100%N treatment.The rate of dry matter accumulation at the early growth stage,total dry matter accumulation and pod yield at harvest increased after Mg application under 50%N treatment by increasing the transportation of assimilates from stems and leaves to pods in both peanut varieties,whereas no effect was found under 100%N treatment.Moreover,Mg application increased the NUE under 50%N treatment.No improvement of NUE in either peanut variety was found under 100%N treatment,while Mg application under the 50%N treatment can obtain a higher economic benefit than the 100%N treatment.In acidic soil,application of 307.5 kg ha^(-1)of Mg sulfate fertilizer under 50%reduced nitrogen application is a suitable fertilizer management measure for improving carbon assimilation,NUE and achieve high peanut yields in southern China.展开更多
Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials.However,the controllable construction of high-density and specific topologi...Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials.However,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging task.Herein,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations.To experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-πinteractions.The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive network.The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the catalyst.This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.展开更多
In this paper,we study reduced rings in which every element is a sum of three tripotents that commute,and determine the integral domains over which every n£n matrix is a sum of three tripotents.It is proved that ...In this paper,we study reduced rings in which every element is a sum of three tripotents that commute,and determine the integral domains over which every n£n matrix is a sum of three tripotents.It is proved that for an integral domain R,every matrix in M_(n)(R)is a sum of three tripotents if and only if R■Zp with p=2,3,5 or 7.展开更多
Three-dimensional(3D)porous absorbents have attracted significant attention in the oily wastewater treatment technology due to their high porosity and elasticity.Given their amphiphilic surface,they have a propensity ...Three-dimensional(3D)porous absorbents have attracted significant attention in the oily wastewater treatment technology due to their high porosity and elasticity.Given their amphiphilic surface,they have a propensity to simultaneously absorb water and oil,which restricts their range of applications.In this study,a reduced graphene oxide and titanium dioxide nanocomposite(rGO/TiO_(2))was used to fabricate an ultra-hydrophobic melamine sponge(MS)through interfacial modification using a solution immersion technique.To further modify it,poly-dimethylsiloxane(PDMS)was grafted onto its surface to establish stronger covalent bonds with the composite.The water contact angle of the sponge(rGO/TiO_(2)/PDMS/MS)was 164.2°,which satisfies the condition for ultrahydrophobicity.The evidence of its water repellency was demonstrated by the Cassie-Baxter theory and the lotus leaf effect.As a result of the increased density of rGO/TiO_(2)/PDMS/MS,it recorded an initial capacity that was 2 g/g lower than the raw MS for crude oil absorption.The raw MS retained 53% of its initial absorption capacity after 20 cycles of absorption,while rGO/TiO_(2)/PDMS/MS retained 97%,suggesting good recyclability.Excellent oil and organic solvent recovery(90%-96%)was demonstrated by rGO/TiO_(2)/PDMS/MS in oil-water combinations.In a continuous separation system,it achieved a remarkable separation efficiency of 2.4×10^(6)L/(m^(3)·h),and in turbulent emulsion separation,it achieved a demulsification efficiency of 90%-91%.This study provides a practical substitute for massive oil spill cleaning.展开更多
In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constrain...In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constraint of an actuator,uncertainties in aerodynamic parameters and measurements,and control system complexity.Owing to the fairly high rotation speed,the dynamic model of this missile is strongly nonlinear,uncertain and coupled in pitch,yaw and roll channels.A theoretical equivalent resultant force and uncertainty compensation method are comprehensively used to realize decoupling of pitch and yaw.In response to the strong nonlinear and time-varying characteristics of the dynamic system,the quasi-linear model whose parameters are obtained by interpolation of points selected as the segmentation points in the trajectory envelope,is used for calculation in each step.To cope with the system uncertainty caused by model approximation,parameter uncertainty and ballistic interference,an extended state estimator is used to compensate the output feedback according to the test ballistic angle.In order to improve the tracking efficiency and ensure the tracking error convergence with only translational motion information,the virtual guide point,whose derivative is deduced according to the Lyapunov principle,is calculated in real time according to the projection relationship between the real-time position and the reference trajectory,and a virtual line-of-sight angle and the backstepping method are used for the design of the guidance and control system.In order to avoid the influence of control input saturation on the guidance and control performance due to the actuator limitation and improve the robustness of the system,an anti-saturation compensator is designed according to the two-step method.The feasibility and effectiveness of the path-following controller is verified through closed-loop flight simulations with measurement,control,and condition uncertainties.The results indicate that the designed controller can converge to the reference path and evidently decrease the distance between the impact point and target under different uncertainties.展开更多
As the most significant green ecological resource in densely populated and economically developed areas,urban landscaping plays a pivotal role in carbon sink value and multiple ecosystem service functions.It is a cruc...As the most significant green ecological resource in densely populated and economically developed areas,urban landscaping plays a pivotal role in carbon sink value and multiple ecosystem service functions.It is a crucial element in the advancement of green and low-carbon initiatives in China’s major cities and the realization of a carbon-neutral vision.By analyzing the relationship between carbon emission reduction and urban landscaping,the paper sorts out and summarizes the basic principles of urban landscaping design,proposes the role of landscape design in urban landscaping,and plans countermeasures for carbon reduction in urban landscaping,with a view to optimizing the construction and management of urban landscaping.展开更多
Many important problems in science and engineering require solving the so-called parametric partial differential equations(PDEs),i.e.,PDEs with different physical parameters,boundary conditions,shapes of computational...Many important problems in science and engineering require solving the so-called parametric partial differential equations(PDEs),i.e.,PDEs with different physical parameters,boundary conditions,shapes of computational domains,etc.Typical reduced order modeling techniques accelerate the solution of the parametric PDEs by projecting them onto a linear trial manifold constructed in the ofline stage.These methods often need a predefined mesh as well as a series of precomputed solution snapshots,and may struggle to balance between the efficiency and accuracy due to the limitation of the linear ansatz.Utilizing the nonlinear representation of neural networks(NNs),we propose the Meta-Auto-Decoder(MAD)to construct a nonlinear trial manifold,whose best possible performance is measured theoretically by the decoder width.Based on the meta-learning concept,the trial manifold can be learned in a mesh-free and unsupervised way during the pre-training stage.Fast adaptation to new(possibly heterogeneous)PDE parameters is enabled by searching on this trial manifold,and optionally fine-tuning the trial manifold at the same time.Extensive numerical experiments show that the MAD method exhibits a faster convergence speed without losing the accuracy than other deep learning-based methods.展开更多
Photocatalysis has emerged as a promising alternative for converting and utilizing CO_(2).Polymeric carbon nitride(PCN),typically synthesized through the one-step thermal polycondensation of nitrogen-rich precursors,h...Photocatalysis has emerged as a promising alternative for converting and utilizing CO_(2).Polymeric carbon nitride(PCN),typically synthesized through the one-step thermal polycondensation of nitrogen-rich precursors,has shown considerable promise due to its adjustable band structure and inherent safety.Over the past five years,significant literature in this field has identified five primary methods for modifying PCN:morphology modulation,element doping,defect induction,co-catalyst loading,and heterojunction construction.A detailed discussion on how each modification method influences light absorption,charge separation,and surface reaction efficiencies in photocatalysis is provided.Based on these findings,several future directions for the development of PCN-based materials are proposed,such as designing tailored PCN structures for specific photocatalytic reactions and using theoretical calculations to verify and correct results from current characterization methods.Despite the challenges associated with the large-scale synthesis of PCN materials with controllable structures and satisfactory performance,this work offers valuable insights for advancing photocatalytic PCN-based systems for large-scale solar fuel production.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
Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore ...Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.展开更多
Excessive consumption of refined grains harms human health and ecosystem viability.Whole grains,as a healthy and sustainable alternative to refined grains,can benefit individual health by providing dietary fiber,B vit...Excessive consumption of refined grains harms human health and ecosystem viability.Whole grains,as a healthy and sustainable alternative to refined grains,can benefit individual health by providing dietary fiber,B vitamins,and bioactive substances.Additionally,they aid in improving the environment due to their higher extraction rate and lower carbon emission during the processing stage.However,few studies have attempted to evaluate the economic and social benefits of increasing the amount of whole grain in grain intake.This paper estimates the potential savings in healthcare costs and reduced food carbon footprints(CFs)that could result from a shift toward whole grain consumption following the Chinese Dietary Guidelines(CDG).We investigate hypothetical scenarios where a certain proportion(5–100%)of Chinese adults could increase their whole grain intakes as proposed by CDG to meet the average shortfall of 30.2 g.In that case,the healthcare costs for associated diseases(e.g.,type2 diabetes mellitus(T2DM),cardiovascular disease(CVD),and colorectal cancer(CRC))are expected to reduce by a substantial amount,from USD 2.82 to 56.37 billion;the carbon emission levels are also projected to decrease by0.24–5.72 million tons.This study provides compelling evidence that advocating for the transition towards greater consumption of whole grain products could benefit individual health,the environment,and society,by reducing both healthcare costs and carbon emissions.展开更多
Electrochemical CO_(2)reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily ac...Electrochemical CO_(2)reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2)electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2)and a Faradaic efficiency of 93.0%at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2)reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.展开更多
Clean steel encompasses a multitude of concepts that are based on fulfilling customer requirements and can be produced in many ways depending on the existing equipment and detailed customer demands.A common feature of...Clean steel encompasses a multitude of concepts that are based on fulfilling customer requirements and can be produced in many ways depending on the existing equipment and detailed customer demands.A common feature of all clean steel production is tight process control along with continuous monitoring.To meet an increasing demand for cold-rolled(CR)steel sheets of improved mechanical properties,and to cope with the change of the annealing process from a batch-type to a continuous process,it is necessary to establish a technique for making ultralow carbon(ULC)steel with a C-concentration lower than 20 ppm for the steelmaking process associated with a major challenge to guarantee the competitiveness with observance of environmental requirements.Steel ladle lining plays an important role on the energy consumption during the production and the refractory lining design contributes to minimize thermal bath loss,carbon pick up and shell temperature.A new generation of unfired zero carbon refractories was developed with two specific approaches:(1)replacement of firing bricks reducing CO_(2) footprint and(2)replacement of carbon containing with performance increasing.Bricks can be used in working and safety linings with a unique microstructure with better heat scattering and similar thermomechanical properties.This work presents customers’performance compared to traditional products highlighting energy savings.展开更多
In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream proces...In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.展开更多
Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membr...Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.展开更多
基金provided by Guizhou Provincial Science and Technology Projects for Platform and Talent Team Plan(GCC[2023]007)Fok Ying Tung Education Foundation(171095)National Natural Science Foundation of China(11964006).
文摘Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.
基金CONCYTEC and PROCIENCIA agencies from Peru in the framework of the call for Basic Research Projects2019-01[contract number401-2019-FONDECYT].
文摘This study investigates the influence of electropolymerization conditions on the deposition of polypyrrole(PPy)onto cotton-derived carbon fiber(CF)modified with reduced graphene oxide(rGO)for supercapacitors applications using an experimental/theorical approach.The surface modification of CF by rGO and/or by PPy electrodeposited at 10,25 and 50 mV s^(-1) was thoroughly examined physicochemical and electrochemically.Composite electrodes comprising CF-rGo-PPy,synthesized via electropolymerization at 25 mV s^(-1),demonstrated a remarkable increase in capacitance,showcasing~742 F g^(-1) compared to 153 F g^(-1) for CF.SEM,N_(2)-surface area,XPS,and TD-DFT approach revealed that the higher capacitance observed in CF-rGo-PPy electrodes underscores the influence of morphology and charged nitrogen species on the electrochemical performance of these modified electrodes.Notably,this electrode material achieves a specific capacitance retention of~96%of their initial capacitance after 10000 cycles at 0.5 A g^(-1) measured in a two-electrodes cell configuration.This work also discusses the influence of the scan rate used for pyrrole electropolymerization on the pseudocapacitance contribution of PPy and its possible effect on the porosity of the material.These results highlight the importance of appropriate electropolymerization conditions that allow obtaining the synergistic effect between CF,rGO and PPy.
基金Under the auspices of the Philosophy and Social Science Planning Project of Guizhou,China(No.21GZZD59)。
文摘China’s low-carbon development path will make significant contributions to achieving global sustainable development goals.Due to the diverse natural and economic conditions across different regions in China,there exists an imbalance in the distribution of car-bon emissions.Therefore,regional cooperation serves as an effective means to attain low-carbon development.This study examined the pattern of carbon emissions and proposed a potential joint emission reduction strategy by utilizing the industrial carbon emission intens-ity(ICEI)as a crucial factor.We utilized social network analysis and Local Indicators of Spatial Association(LISA)space-time trans-ition matrix to investigate the spatiotemporal connections and discrepancies of ICEI in the cities of the Pearl River Basin(PRB),China from 2010 to 2020.The primary drivers of the ICEI were determined through geographical detectors and multi-scale geographically weighted regression.The results were as follows:1)the overall ICEI in the Pearl River Basin is showing a downward trend,and there is a significant spatial imbalance.2)There are numerous network connections between cities regarding the ICEI,but the network structure is relatively fragile and unstable.3)Economically developed cities such as Guangzhou,Foshan,and Dongguan are in the center of the network while playing an intermediary role.4)Energy consumption,industrialization,per capita GDP,urbanization,science and techno-logy,and productivity are found to be the most influential variables in the spatial differentiation of ICEI,and their combination in-creased the explanatory power of the geographic variation of ICEI.Finally,through the analysis of differences and connections in urban carbon emissions under different economic levels and ICEI,the study suggests joint carbon reduction strategies,which are centered on carbon transfer,financial support,and technological assistance among cities.
基金the Science and Technology Key Project of Anhui Province,China(No.2022e03020004).
文摘Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selective extraction of lithium from spent Li-CoO_(2)(LCO)cathodes to overcome the incomplete recovery and loss of lithium during the recycling process.The LCO layered structure was destroyed and lithium was completely converted into water-soluble Li2CO_(3)under a suitable temperature to control the reduced state of the cobalt oxide.The Co metal agglomerates generated during medium-temperature carbon reduction roasting were broken by wet grinding and ultrasonic crushing to release the entrained lithium.The results showed that 99.10%of the whole lithium could be recovered as Li2CO_(3)with a purity of 99.55%.This work provided a new perspective on the preferentially selective extraction of lithium from spent lithium batteries.
基金financially supported by the National Natural Science Foundation of China(52077207 and 51907193)the Key Research Program of Frontier Sciences,CAS(ZDBS-LY-JSC047)the Youth Innovation Promotion Association CAS(2020145)。
文摘Practical applications of diverse flexible wearable electronics require electrochemical energy storage(EES)devices with multiple configurations.Moreover,to fabricate flexible EES devices with high energy density and stability,organic integration from electrode design to device assembly is required.To address these challenges,a free-standing reduced graphene oxide(rGO)/carbon film with a unique sandwich structure has been designed via the assistance of vacuum-assistant filtration for lithium-ion capacitors(LICs).The graphene acts as not only a binder to construct a three-dimensional conductive network but also an active material to provide additional capacitive lithium storage sites,thus enabling fast ion/electron transport and improving the capacity.The designed rGO/hard carbon(rGO/HC)and rGO/activated carbon(rGO/AC)free-standing films exhibit enhanced specific capacities(513.7 mA h g^(-1)for rGO/HC and 102.8 mA h g^(-1)for rGO/AC)and excellent stability.Moreover,the integrated flexible quasi-solid-state rGO/AC//rGO/HC LIC devices possess a maximum energy density of 138.3 Wh kg^(-1),a high power density of 11 kW kg^(-1),and improved cycling performance(84.4%capacitance maintained after 10,000 cycles),superior to the AC//HC LIC(43.5%retention).Such a strategy enlightens the development of portable flexible LICs.
基金supported by the Guangdong Technical System of Peanut and Soybean Industry(2023KJ136-05)China Agriculture Research System(CARS-15)。
文摘This study investigated the effect of magnesium application on peanut growth and yield under two nitrogen(N)application rates in acidic soil in southern China.The chlorophyll content,net photosynthetic rate and dry matter accumulation of the N-sensitive cultivar decreased under reduced N treatments,whereas no effect was observed on the relevant indicators in the N-insensitive variety GH1026.Mg application increased the net photosynthetic rate by increasing the expression of genes involved in chlorophyll synthesis and Rubisco activity in the leaves during the pegging stage under 50%N treatment,while no effect on the net photosynthetic rate was observed under the 100%N treatment.The rate of dry matter accumulation at the early growth stage,total dry matter accumulation and pod yield at harvest increased after Mg application under 50%N treatment by increasing the transportation of assimilates from stems and leaves to pods in both peanut varieties,whereas no effect was found under 100%N treatment.Moreover,Mg application increased the NUE under 50%N treatment.No improvement of NUE in either peanut variety was found under 100%N treatment,while Mg application under the 50%N treatment can obtain a higher economic benefit than the 100%N treatment.In acidic soil,application of 307.5 kg ha^(-1)of Mg sulfate fertilizer under 50%reduced nitrogen application is a suitable fertilizer management measure for improving carbon assimilation,NUE and achieve high peanut yields in southern China.
基金partly supported by the National Natural Science Foundation of China(22078052)the National Key R&D Program of China(2022YFB4101602)the Fundamental Research Funds for the Central Universities(DUT22LAB612)。
文摘Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials.However,the controllable construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging task.Herein,the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations.To experimentally verify this,the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P),subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO)viaπ-πinteractions.The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-orderedπelectron delocalization system as conductive network.The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%,superior to the Pt reference(7.97%).Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates,thus enhancing the electrocatalytic activity of the catalyst.This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.
基金Supported by Key Laboratory of Financial Mathematics of Fujian Province University(Putian University)(JR202203)the NSF of Anhui Province(2008085MA06).
文摘In this paper,we study reduced rings in which every element is a sum of three tripotents that commute,and determine the integral domains over which every n£n matrix is a sum of three tripotents.It is proved that for an integral domain R,every matrix in M_(n)(R)is a sum of three tripotents if and only if R■Zp with p=2,3,5 or 7.
基金supported by the Universiti Brunei Darussalam Research Funding(Grant No.UBD/OAVCRI/CRGWG(022)/171001).
文摘Three-dimensional(3D)porous absorbents have attracted significant attention in the oily wastewater treatment technology due to their high porosity and elasticity.Given their amphiphilic surface,they have a propensity to simultaneously absorb water and oil,which restricts their range of applications.In this study,a reduced graphene oxide and titanium dioxide nanocomposite(rGO/TiO_(2))was used to fabricate an ultra-hydrophobic melamine sponge(MS)through interfacial modification using a solution immersion technique.To further modify it,poly-dimethylsiloxane(PDMS)was grafted onto its surface to establish stronger covalent bonds with the composite.The water contact angle of the sponge(rGO/TiO_(2)/PDMS/MS)was 164.2°,which satisfies the condition for ultrahydrophobicity.The evidence of its water repellency was demonstrated by the Cassie-Baxter theory and the lotus leaf effect.As a result of the increased density of rGO/TiO_(2)/PDMS/MS,it recorded an initial capacity that was 2 g/g lower than the raw MS for crude oil absorption.The raw MS retained 53% of its initial absorption capacity after 20 cycles of absorption,while rGO/TiO_(2)/PDMS/MS retained 97%,suggesting good recyclability.Excellent oil and organic solvent recovery(90%-96%)was demonstrated by rGO/TiO_(2)/PDMS/MS in oil-water combinations.In a continuous separation system,it achieved a remarkable separation efficiency of 2.4×10^(6)L/(m^(3)·h),and in turbulent emulsion separation,it achieved a demulsification efficiency of 90%-91%.This study provides a practical substitute for massive oil spill cleaning.
文摘In this paper,an integrated guidance and control method based on an adaptive path-following controller is proposed to control a spin-stabilized projectile with only translational motion information under the constraint of an actuator,uncertainties in aerodynamic parameters and measurements,and control system complexity.Owing to the fairly high rotation speed,the dynamic model of this missile is strongly nonlinear,uncertain and coupled in pitch,yaw and roll channels.A theoretical equivalent resultant force and uncertainty compensation method are comprehensively used to realize decoupling of pitch and yaw.In response to the strong nonlinear and time-varying characteristics of the dynamic system,the quasi-linear model whose parameters are obtained by interpolation of points selected as the segmentation points in the trajectory envelope,is used for calculation in each step.To cope with the system uncertainty caused by model approximation,parameter uncertainty and ballistic interference,an extended state estimator is used to compensate the output feedback according to the test ballistic angle.In order to improve the tracking efficiency and ensure the tracking error convergence with only translational motion information,the virtual guide point,whose derivative is deduced according to the Lyapunov principle,is calculated in real time according to the projection relationship between the real-time position and the reference trajectory,and a virtual line-of-sight angle and the backstepping method are used for the design of the guidance and control system.In order to avoid the influence of control input saturation on the guidance and control performance due to the actuator limitation and improve the robustness of the system,an anti-saturation compensator is designed according to the two-step method.The feasibility and effectiveness of the path-following controller is verified through closed-loop flight simulations with measurement,control,and condition uncertainties.The results indicate that the designed controller can converge to the reference path and evidently decrease the distance between the impact point and target under different uncertainties.
文摘As the most significant green ecological resource in densely populated and economically developed areas,urban landscaping plays a pivotal role in carbon sink value and multiple ecosystem service functions.It is a crucial element in the advancement of green and low-carbon initiatives in China’s major cities and the realization of a carbon-neutral vision.By analyzing the relationship between carbon emission reduction and urban landscaping,the paper sorts out and summarizes the basic principles of urban landscaping design,proposes the role of landscape design in urban landscaping,and plans countermeasures for carbon reduction in urban landscaping,with a view to optimizing the construction and management of urban landscaping.
基金supported by the National Key R&D Program of China under Grant No.2021ZD0110400.
文摘Many important problems in science and engineering require solving the so-called parametric partial differential equations(PDEs),i.e.,PDEs with different physical parameters,boundary conditions,shapes of computational domains,etc.Typical reduced order modeling techniques accelerate the solution of the parametric PDEs by projecting them onto a linear trial manifold constructed in the ofline stage.These methods often need a predefined mesh as well as a series of precomputed solution snapshots,and may struggle to balance between the efficiency and accuracy due to the limitation of the linear ansatz.Utilizing the nonlinear representation of neural networks(NNs),we propose the Meta-Auto-Decoder(MAD)to construct a nonlinear trial manifold,whose best possible performance is measured theoretically by the decoder width.Based on the meta-learning concept,the trial manifold can be learned in a mesh-free and unsupervised way during the pre-training stage.Fast adaptation to new(possibly heterogeneous)PDE parameters is enabled by searching on this trial manifold,and optionally fine-tuning the trial manifold at the same time.Extensive numerical experiments show that the MAD method exhibits a faster convergence speed without losing the accuracy than other deep learning-based methods.
基金the National Natural Science Foundation of China(22209207)the National Key Research and Development Program of China(2022YFB4002400).
文摘Photocatalysis has emerged as a promising alternative for converting and utilizing CO_(2).Polymeric carbon nitride(PCN),typically synthesized through the one-step thermal polycondensation of nitrogen-rich precursors,has shown considerable promise due to its adjustable band structure and inherent safety.Over the past five years,significant literature in this field has identified five primary methods for modifying PCN:morphology modulation,element doping,defect induction,co-catalyst loading,and heterojunction construction.A detailed discussion on how each modification method influences light absorption,charge separation,and surface reaction efficiencies in photocatalysis is provided.Based on these findings,several future directions for the development of PCN-based materials are proposed,such as designing tailored PCN structures for specific photocatalytic reactions and using theoretical calculations to verify and correct results from current characterization methods.Despite the challenges associated with the large-scale synthesis of PCN materials with controllable structures and satisfactory performance,this work offers valuable insights for advancing photocatalytic PCN-based systems for large-scale solar fuel production.
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.
基金the financial support from the Postdoctoral Science Foundation of China(2022M720131)Spring Sunshine Collaborative Research Project of the Ministry of Education(202201660)+3 种基金Youth Project of Gansu Natural Science Foundation(22JR5RA542)General Project of Gansu Philosophy and Social Science Foundation(2022YB014)National Natural Science Foundation of China(72034003,72243006,and 71874074)Fundamental Research Funds for the Central Universities(2023lzdxjbkyzx008,lzujbky-2021-sp72)。
文摘Since the carbon neutrality target was proposed,many countries have been facing severe challenges to carbon emission reduction sustainably.This study is conducted using a tripartite evolutionary game model to explore the impact of the central environmental protection inspection(CEPI)on driving carbon emission reduction,and to study what factors influence the strategic choices of each party and how they interact with each other.The research results suggest that local governments and manufacturing enterprises would choose strategies that are beneficial to carbon reduction when CEPI increases.When the initial willingness of all parties increases 20%,50%—80%,the time spent for the whole system to achieve stability decreases from 100%,60%—30%.The evolutionary result of“thorough inspection,regulation implementation,low-carbon management”is the best strategy for the tripartite evolutionary game.Moreover,the smaller the cost and the larger the benefit,the greater the likelihood of the three-party game stability strategy appears.This study has important guiding significance for other developing countries to promote carbon emission reduction by environmental policy.
基金the National Natural Science Foundation of China(72203214 and 72061147002)China Scholarship Council(CSC)(201913043)。
文摘Excessive consumption of refined grains harms human health and ecosystem viability.Whole grains,as a healthy and sustainable alternative to refined grains,can benefit individual health by providing dietary fiber,B vitamins,and bioactive substances.Additionally,they aid in improving the environment due to their higher extraction rate and lower carbon emission during the processing stage.However,few studies have attempted to evaluate the economic and social benefits of increasing the amount of whole grain in grain intake.This paper estimates the potential savings in healthcare costs and reduced food carbon footprints(CFs)that could result from a shift toward whole grain consumption following the Chinese Dietary Guidelines(CDG).We investigate hypothetical scenarios where a certain proportion(5–100%)of Chinese adults could increase their whole grain intakes as proposed by CDG to meet the average shortfall of 30.2 g.In that case,the healthcare costs for associated diseases(e.g.,type2 diabetes mellitus(T2DM),cardiovascular disease(CVD),and colorectal cancer(CRC))are expected to reduce by a substantial amount,from USD 2.82 to 56.37 billion;the carbon emission levels are also projected to decrease by0.24–5.72 million tons.This study provides compelling evidence that advocating for the transition towards greater consumption of whole grain products could benefit individual health,the environment,and society,by reducing both healthcare costs and carbon emissions.
文摘Electrochemical CO_(2)reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy conversion.The development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2)electroreduction remains challenging yet indispensable.In this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx sites.Benefiting from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be ensured.As a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2)and a Faradaic efficiency of 93.0%at-1.0 V vs.RHE,outperforming those of its PEI-free analog.Apart from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term stability.The findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2)reduction.Furthermore,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.
文摘Clean steel encompasses a multitude of concepts that are based on fulfilling customer requirements and can be produced in many ways depending on the existing equipment and detailed customer demands.A common feature of all clean steel production is tight process control along with continuous monitoring.To meet an increasing demand for cold-rolled(CR)steel sheets of improved mechanical properties,and to cope with the change of the annealing process from a batch-type to a continuous process,it is necessary to establish a technique for making ultralow carbon(ULC)steel with a C-concentration lower than 20 ppm for the steelmaking process associated with a major challenge to guarantee the competitiveness with observance of environmental requirements.Steel ladle lining plays an important role on the energy consumption during the production and the refractory lining design contributes to minimize thermal bath loss,carbon pick up and shell temperature.A new generation of unfired zero carbon refractories was developed with two specific approaches:(1)replacement of firing bricks reducing CO_(2) footprint and(2)replacement of carbon containing with performance increasing.Bricks can be used in working and safety linings with a unique microstructure with better heat scattering and similar thermomechanical properties.This work presents customers’performance compared to traditional products highlighting energy savings.
基金support from the National Natural Science Foundation of China(21978128,91934302)partial support from the State Key Laboratory of Materials-oriented Chemical Engineering(ZK202006)also acknowledged.Additionallysupported by the“Cultivation Program for The Excellent Doctoral Dissertation of Nanjing Tech University(3800124701)”.
文摘In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream processes.This study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen Plus.Following this,process optimization and energy integration were implemented to provide optimized operation conditions.Lastly,a life cycle assessment was carried out to assess the carbon footprint of the coupled process.Results reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous products.By optimizing systemic energy through heat integration,an energy efficiency of 86.30%was achieved.Additionally,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.
基金finically supported by the National Natural Science Foundation of China(22075055)the Guangxi Science and Technology Project(AB16380030)。
文摘Transition metal-nitrogen-carbon(M-N-C)as a promising substitute for the conventional noble metalbased catalyst still suffers from low activity and durability for oxygen reduction reaction(ORR)in proton exchange membrane fuel cells(PEMFCs).To tackle the issue,herein,a new type of sulfur-doped ironnitrogen-hard carbon(S-Fe-N-HC)nanosheets with high activity and durability in acid media were developed by using a newly synthesized precursor of amide-based polymer with Fe ions based on copolymerizing two monomers of 2,5-thiophene dicarboxylic acid(TDA)as S source and 1,8-diaminonaphthalene(DAN)as N source via an amination reaction.The as-synthesized S-Fe-N-HC features highly dispersed atomic Fe Nxmoieties embedded into rich thiophene-S doped hard carbon nanosheets filled with highly twisted graphite-like microcrystals,which is distinguished from the majority of M-N-C with soft or graphitic carbon structures.These unique characteristics endow S-Fe-N-HC with high ORR activity and outstanding durability in 0.5 M H_(2)SO_(4).Its initial half-wave potential is 0.80 V and the corresponding loss is only 21 m V after 30,000 cycles.Meanwhile,its practical PEMFC performance is a maximum power output of 628.0 mW cm^(-2)and a slight power density loss is 83.0 m W cm^(-2)after 200-cycle practical operation.Additionally,theoretical calculation shows that the activity of Fe Nxmoieties on ORR can be further enhanced by sulfur doping at meta-site near FeN_(4)C.These results evidently demonstrate that the dual effect of hard carbon substrate and S doping derived from the precursor platform of amid-polymers can effectively enhance the activity and durability of Fe-N-C catalysts,providing a new guidance for developing advanced M-N-C catalysts for ORR.