In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations we...In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.展开更多
The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile con...The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile content of biochar ranged from 16.19%to 45.35%,and the alkali metal content,ash content,and specific surface area were significantly reduced.The optimal route for biochar pro-duction is hydrothermal carbonization-pyrolysis(P-HC),resulting in biochar with a higher calorific value,C=C structure,and increased graphitization degree.The apparent activation energy(E)of the sample ranges from 199.1 to 324.8 kJ/mol,with P-HC having an E of 277.8 kJ/mol,lower than that of raw biomass,primary biochar,and anthracite.This makes P-HC more suitable for blast furnace injection fuel.Additionally,the paper proposes a path for P-HC injection in blast furnaces and calculates potential environmental benefits.P-HC of-fers the highest potential for carbon emission reduction,capable of reducing emissions by 96.04 kg/t when replacing 40wt%coal injec-tion.展开更多
Study of physisorbed and chemisorbed carbon dioxide (CO<sub>2</sub>) species was carried out on the NaX zeolite modified by cationic exchanges with bivalent cations (Ca<sup>2+</sup> and Ba<s...Study of physisorbed and chemisorbed carbon dioxide (CO<sub>2</sub>) species was carried out on the NaX zeolite modified by cationic exchanges with bivalent cations (Ca<sup>2+</sup> and Ba<sup>2+</sup>) by temperature-programmed desorption of CO<sub>2</sub> (CO<sub>2</sub>-TPD). Others results were obtained by infrared to complete the study. The results of this research showed, in the physisorption region (213 - 473 K), that the cationic exchanges on NaX zeolite with bivalent cations increase slightly the interactions of CO<sub>2</sub> molecule with adsorbents and/or cationic site. Indeed, the desorption energies of physisorbed CO<sub>2</sub> obtained on the reference zeolite NaX (13.5 kJ·mol<sup>-1</sup>) are lower than that of exchanged zeolites E-CaX and E-BaX (15.77 and 15.17 kJ·mol<sup>-1</sup> respectively). In the chemisorbed CO<sub>2</sub> region (573 - 873 K), the desorption energies related to desorbed species (bidentate carbonates: CO<sub>3</sub>2-</sup>) on the exchanged zeolites E-CaX and E-BaX are about 81 kJ·mol<sup>-1</sup>, higher than the desorbed species (bicarbonates: HCO<sub>3</sub>2-</sup>) on the reference R-NaX (62 kJ·mol<sup>-1</sup>). In addition, the exchanged E-BaX zeolite develops the secondary adsorption sites corresponding to bicarbonates species with desorption energies of 35 kJ·mol<sup>-1</sup> lower to desorption energies of bicarbonates noted on the reference zeolite NaX.展开更多
Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption...Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption have limited the development of HTC technology. In conventional batch reactors, the temperature and pressure are typically coupled at saturated states. In this study, a decoupled temperature and pressure hydrothermal(DTPH) reaction system was developed to decrease the temperature of the HTC reaction of lignocellulosic biomass(rice straw and poplar leaves). The properties of hydrochars were analyzed by scanning electron microscopy(SEM), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), Raman spectroscopy, X-ray diffraction(XRD), thermogravimetric analyzer(TGA), etc. to propose the reaction mechanism. The results showed that the HTC reaction of lignocellulosic biomass could be realized at a low temperature of 200℃ in the DTPH process, breaking the temperature limit(230℃) in the conventional process. The DTPH method could break the barrier of the crystalline structure of cellulose in the lignocellulosic biomass with high cellulose content, realizing the carbonization of cellulose and hemicellulose with the dehydration, unsaturated bond formation, and aromatization. The produced hydrochar had an appearance of carbon microspheres, with high calorific values, abundant oxygen-containing functional groups, a certain degree of graphitization, and good thermal stability. Cellulose acts not only as a barrier to protect itself and hemicellulose from decomposition, but also as a key precursor for the formation of carbon microspheres. This study shows a promising method for synthesizing carbon materials from lignocellulosic biomass with a carbon-negative effect.展开更多
Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-pu...Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-purpose propylene production route in recent years.Nitrogen-doped carbon(NC)nanopolyhedra supported cobalt catalysts were synthesized in one-step of ZIF-67 pyrolysis and investigated further in PDH.XPS,TEM and N_(2) adsorption-desorption were used to study the influence of carbonization temperature on as-prepared NC supported cobalt catalysts.The temperature is found to affect the cobalt phase and nitrogen species of the catalysts.And the positive correlation was established between Co0 proportion and space time yield of propylene,indicating that the modulation of carbonization temperature could be important for catalytic performance.展开更多
Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethyle...Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethylene terephthalate(PET)is attractive due to its excellent stability and degradation-resistant.Therefore,merging China’s carbon peak and carbon neutrality goals would be beneficial.In this review,we summarize the current state-of-the-art of carbon emission decrease from a multi-scale perspective technologically.We suggest that the carbon peak for waste PET can be achieved by employing the closed-loop supply chain,including recycling,biomass utilization,carbon capture and utilization.Waste PET can be a valuable and renewable resource in the whole life cycle.Undoubtedly,all kinds of PET plastics can be ultimately converted into CO_(2),which can also be feedstock for various kinds of chemical products,including ethyl alcohol,formic acid,soda ash,PU,starch and so on.As a result,the closed-loop supply chain can help the PET plastics industry drastically reduce its carbon footprint.展开更多
Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discus...Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discussed based on a systematic three-dimensional low-carbon analysis from the aspects of resource utilization(Y),energy utilization(Q),and energy cleanliness which is evaluated by a process general emission factor(PGEF)on all the related processes,including the current blast furnace(BF)-basic oxygen furnace(BOF)integrated process and the specific sub-processes,as well as the electric arc furnace(EAF)process,typical direct reduction(DR)process,and smelting reduction(SR)process.The study indicates that the three-dimensional aspects,particularly the energy structure,should be comprehensively considered to quantitatively evaluate the decarbonization road map based on novel technologies or processes.Promoting scrap utilization(improvement of Y)and the substitution of carbon-based energy(improvement of PGEF)in particular is critical.In terms of process scale,promoting the development of the scrap-based EAF or DR-EAF process is highly encouraged because of their lower PGEF.The three-dimensional method is expected to extend to other processes or industries,such as the cement production and thermal electricity generation industries.展开更多
Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed ...Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.展开更多
The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)shielding.However,for macroscopic CNT assemblies,such as CNT film,achieving high ...The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)shielding.However,for macroscopic CNT assemblies,such as CNT film,achieving high electrical and mechanical properties remains challenging,which heavily depends on the tube-tube interac-tions of CNTs.Herein,we develop a novel strategy based on metal-organic decomposition(MOD)to fabricate a flexible silver-carbon nanotube(Ag-CNT)film.The Ag particles are introduced in situ into the CNT film through annealing of MOD,leading to enhanced tube-tube interactions.As a result,the electrical conductivity of Ag-CNT film is up to 6.82×10^(5) S m^(-1),and the EMI shielding effectiveness of Ag-CNT film with a thickness of~7.8μm exceeds 66 dB in the ultra-broad frequency range(3-40 GHz).The tensile strength and Young’s modulus of Ag-CNT film increase from 30.09±3.14 to 76.06±6.20 MPa(~253%)and from 1.12±0.33 to 8.90±0.97 GPa(~795%),respectively.Moreover,the Ag-CNT film exhibits excellent near-field shield-ing performance,which can effectively block wireless transmission.This innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.展开更多
NiMZn/C@melamine sponge-derived carbon(MSDC)composites(M=Co,Fe,and Mn)were prepared by a vacuum pump-ing solution method followed by carbonization.A large number of carbon nanotubes(CNTs)homogeneously attached to the ...NiMZn/C@melamine sponge-derived carbon(MSDC)composites(M=Co,Fe,and Mn)were prepared by a vacuum pump-ing solution method followed by carbonization.A large number of carbon nanotubes(CNTs)homogeneously attached to the surfaces of the three-dimensional cross-linked of the sponge-derived carbon in the NiCoZn/C@MSDC composite,and CNTs were detected in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.Ni_(3)ZnC_(0.7),Ni_(3)Fe,and MnO in-situ formed in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.The CNTs in the NiCoZn/C@MSDC composite efficiently modulated its complex permittivity.Thus,the composite exhibited the best performance among the composites,with the minimum reflection loss(RL_(min))of-33.1 dB at 18 GHz and thickness of 1.4 mm.The bandwidth for RL of≤-10 dB was up to 5.04 GHz at the thickness of 1.7 mm and loading of 25wt%.The op-timized impedance matching,enhanced interfacial and dipole polarization,remarkable conduction loss,and multiple reflections and scat-tering of the incident microwaves improved the microwave absorption performance.The effects of Co,Ni,and Fe on the phase and mor-phology provided an alternative way for developing highly efficient and broadband microwave absorbers.展开更多
Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research ob...Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.展开更多
Global warming has greatly threatened the human living environment and carbon capture and storage(CCS)technology is recognized as a promising way to reduce carbon emissions.Mineral storage is considered a reliable opt...Global warming has greatly threatened the human living environment and carbon capture and storage(CCS)technology is recognized as a promising way to reduce carbon emissions.Mineral storage is considered a reliable option for long-term carbon storage.Basalt rich in alkaline earth elements facilitates rapid and permanent CO_(2) fixation as carbonates.However,the complex CO_(2)-fluid-basalt interaction poses challenges for assessing carbon storage potential.Under different reaction conditions,the carbonation products and carbonation rates vary.Carbon mineralization reactions also induce petrophysical and mechanical responses,which have potential risks for the long-term injectivity and the carbon storage safety in basalt reservoirs.In this paper,recent advances in carbon mineralization storage in basalt based on laboratory research are comprehensively reviewed.The assessment methods for carbon storage potential are introduced and the carbon trapping mechanisms are investigated with the identification of the controlling factors.Changes in pore structure,permeability and mechanical properties in both static reactions and reactive percolation experiments are also discussed.This study could provide insight into challenges as well as perspectives for future research.展开更多
Understanding the spatial variation,temporal changes,and their underlying driving forces of carbon sequestration in various forests is of great importance for understanding the carbon cycle and carbon management optio...Understanding the spatial variation,temporal changes,and their underlying driving forces of carbon sequestration in various forests is of great importance for understanding the carbon cycle and carbon management options.How carbon density and sequestration in various Cunninghamia lanceolata forests,extensively cultivated for timber production in subtropical China,vary with biodiversity,forest structure,environment,and cultural factors remain poorly explored,presenting a critical knowledge gap for realizing carbon sequestration supply potential through management.Based on a large-scale database of 449 permanent forest inventory plots,we quantified the spatial-temporal heterogeneity of aboveground carbon densities and carbon accumulation rates in Cunninghamia lanceolate forests in Hunan Province,China,and attributed the contributions of stand structure,environmental,and management factors to the heterogeneity using quantile age-sequence analysis,partial least squares path modeling(PLS-PM),and hot-spot analysis.The results showed lower values of carbon density and sequestration on average,in comparison with other forests in the same climate zone(i.e.,subtropics),with pronounced spatial and temporal variability.Specifically,quantile regression analysis using carbon accumulation rates along an age sequence showed large differences in carbon sequestration rates among underperformed and outperformed forests(0.50 and 1.80 Mg·ha^(-1)·yr^(-1)).PLS-PM demonstrated that maximum DBH and stand density were the main crucial drivers of aboveground carbon density from young to mature forests.Furthermore,species diversity and geotopographic factors were the significant factors causing the large discrepancy in aboveground carbon density change between low-and high-carbon-bearing forests.Hotspot analysis revealed the importance of culture attributes in shaping the geospatial patterns of carbon sequestration.Our work highlighted that retaining largesized DBH trees and increasing shade-tolerant tree species were important to enhance carbon sequestration in C.lanceolate forests.展开更多
Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate ...CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.展开更多
The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving c...The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.展开更多
MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivi...MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivity,good hydrophilicity,and tunable terminations.Among various types of MXenes,Ti_(3)C_(2)T_(x) is the most widely studied for use in capacitive energy storage applications,especially in supercapacitors(SCs).However,the stacking and oxidation of MXene sheets inevitably lead to a significant loss of electrochemically active sites.To overcome such challenges,carbon materials are frequently incorporated into MXenes to enhance their electrochemical properties.This review introduces the common strategies used for synthesizing Ti_(3)C_(2)T_(x),followed by a comprehensive overview of recent developments in Ti_(3)C_(2)T_(x)/carbon composites as electrode materials for SCs.Ti_(3)C_(2)T_(x)/carbon composites are categorized based on the dimensions of carbons,including 0D carbon dots,1D carbon nanotubes and fibers,2D graphene,and 3D carbon materials(activated carbon,polymer-derived carbon,etc.).Finally,this review also provides a perspective on developing novel MXenes/carbon composites as electrodes for application in SCs.展开更多
Vertically oriented carbon structures constructed from low-dimen-sional carbon materials are ideal frameworks for high-performance thermal inter-face materials(TIMs).However,improving the interfacial heat-transfer eff...Vertically oriented carbon structures constructed from low-dimen-sional carbon materials are ideal frameworks for high-performance thermal inter-face materials(TIMs).However,improving the interfacial heat-transfer efficiency of vertically oriented carbon structures is a challenging task.Herein,an orthotropic three-dimensional(3D)hybrid carbon network(VSCG)is fabricated by depositing vertically aligned carbon nanotubes(VACNTs)on the surface of a horizontally oriented graphene film(HOGF).The interfacial interaction between the VACNTs and HOGF is then optimized through an annealing strategy.After regulating the orientation structure of the VACNTs and filling the VSCG with polydimethylsi-loxane(PDMS),VSCG/PDMS composites with excellent 3D thermal conductive properties are obtained.The highest in-plane and through-plane thermal conduc-tivities of the composites are 113.61 and 24.37 W m^(-1)K^(-1),respectively.The high contact area of HOGF and good compressibility of VACNTs imbue the VSCG/PDMS composite with low thermal resistance.In addition,the interfacial heat-transfer efficiency of VSCG/PDMS composite in the TIM performance was improved by 71.3%compared to that of a state-of-the-art thermal pad.This new structural design can potentially realize high-performance TIMs that meet the need for high thermal conductivity and low contact thermal resistance in interfacial heat-transfer processes.展开更多
Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing...Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.展开更多
Tin disulfide(SnS_(2)),due to large interlayer spacing and high theoretical capacity,is regarded as a prospective anode material for lithium-ion batteries.Nevertheless,the poor electron conductivity of SnS_(2) and hug...Tin disulfide(SnS_(2)),due to large interlayer spacing and high theoretical capacity,is regarded as a prospective anode material for lithium-ion batteries.Nevertheless,the poor electron conductivity of SnS_(2) and huge volumetric change during the lithiation/delithiation process lead to a rapid capacity decay of the battery,hindering its commercialization.To address these issues,herein,SnS_(2) is in-situ grown on the surface of carbon nanotubes(CNT)and then encapsulated with a layer of porous amorphous carbon(CNT/SnS_(2)@C)by simple solvothermal and further carbonization treatment.The synergistic effect of CNT and porous carbon layer not only enhances the electrical co nductivity of SnS_(2) but also limits the huge volumetric change to avoid the pulverization and detachment of SnS_(2).Density functional theo ry calculations show that CNT/SnS_(2)@C has high Li^(+)adsorption and lithium storage capacity achieving high reaction kinetics.Consequently,cells with the CNT/SnS_(2)@C anode exhibit a high lithium storage capacity of 837mAh/g after 100 cycles at 0.1 A/g and retaining a capacity of 529.8 mAh/g under 1.0 A/g after 1000 cycles.This study provides a fundamental understanding of the electrochemical processes and beneficial guidance to design high-performance SnS_(2)-based anodes for LIBs.展开更多
基金financially supported by the National Natural Science Foundation of China(Approval No.42172168).
文摘In order to obtain liquefied products with higher yields of aromatic molecules to produce mesophase pitch,a good understanding of the relevant reaction mechanisms is required.Reactive molecular dynamics simulations were used to study the thermal reactions of pyrene,1-methylpyrene,7,8,9,10-tetrahydrobenzopyrene,and mixtures of pyrene with 1-octene,cyclohexene,or styrene.The reactant conversion rates,reaction rates,and product distributions were calculated and compared,and the mechanisms were analyzed and discussed.The results demonstrated that methyl and naphthenic structures in aromatics might improve the conversion rates of reactants in hydrogen transfer processes,but their steric hindrances prohibited the generation of high polymers.The naphthenic structures could generate more free radicals and presented a more obvious inhibition effect on the condensation of polymers compared with the methyl side chains.It was discovered that when different olefins were mixed with pyrene,1-octene primarily underwent pyrolysis reactions,whereas cyclohexene mainly underwent hydrogen transfer reactions with pyrene and styrene,mostly producing superconjugated biradicals through condensation reactions with pyrene.In the mixture systems,the olefins scattered aromatic molecules,hindering the formation of pyrene trimers and higher polymers.According to the reactive molecular dynamics simulations,styrene may enhance the yield of dimer and enable the controlled polycondensation of pyrene.
基金the National Key R&D Program of China(No.2022YFE0208100)the National Natural Science Foundation of China(No.5274316)+1 种基金the Key Research and Development Plan of Anhui Province,China(No.202210700037)the Major Science and Technology Project of Xinjiang Uygur Autonomous Region,China(No.2022A01003).
文摘The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection fuel.The results showed that after upgrading,the volatile content of biochar ranged from 16.19%to 45.35%,and the alkali metal content,ash content,and specific surface area were significantly reduced.The optimal route for biochar pro-duction is hydrothermal carbonization-pyrolysis(P-HC),resulting in biochar with a higher calorific value,C=C structure,and increased graphitization degree.The apparent activation energy(E)of the sample ranges from 199.1 to 324.8 kJ/mol,with P-HC having an E of 277.8 kJ/mol,lower than that of raw biomass,primary biochar,and anthracite.This makes P-HC more suitable for blast furnace injection fuel.Additionally,the paper proposes a path for P-HC injection in blast furnaces and calculates potential environmental benefits.P-HC of-fers the highest potential for carbon emission reduction,capable of reducing emissions by 96.04 kg/t when replacing 40wt%coal injec-tion.
文摘Study of physisorbed and chemisorbed carbon dioxide (CO<sub>2</sub>) species was carried out on the NaX zeolite modified by cationic exchanges with bivalent cations (Ca<sup>2+</sup> and Ba<sup>2+</sup>) by temperature-programmed desorption of CO<sub>2</sub> (CO<sub>2</sub>-TPD). Others results were obtained by infrared to complete the study. The results of this research showed, in the physisorption region (213 - 473 K), that the cationic exchanges on NaX zeolite with bivalent cations increase slightly the interactions of CO<sub>2</sub> molecule with adsorbents and/or cationic site. Indeed, the desorption energies of physisorbed CO<sub>2</sub> obtained on the reference zeolite NaX (13.5 kJ·mol<sup>-1</sup>) are lower than that of exchanged zeolites E-CaX and E-BaX (15.77 and 15.17 kJ·mol<sup>-1</sup> respectively). In the chemisorbed CO<sub>2</sub> region (573 - 873 K), the desorption energies related to desorbed species (bidentate carbonates: CO<sub>3</sub>2-</sup>) on the exchanged zeolites E-CaX and E-BaX are about 81 kJ·mol<sup>-1</sup>, higher than the desorbed species (bicarbonates: HCO<sub>3</sub>2-</sup>) on the reference R-NaX (62 kJ·mol<sup>-1</sup>). In addition, the exchanged E-BaX zeolite develops the secondary adsorption sites corresponding to bicarbonates species with desorption energies of 35 kJ·mol<sup>-1</sup> lower to desorption energies of bicarbonates noted on the reference zeolite NaX.
基金The financial support from the Key-Area Research and Development Program of Guangdong Province (2020B1111380001)the Beijing Municipal Natural Science Foundation (2222012)+1 种基金the National Natural Science Foundation of China (Grant No.52070116)the Tsinghua University-Shanxi Clean Energy Research Institute Innovation Project Seed Fund。
文摘Hydrothermal carbonization(HTC) of lignocellulosic biomass is a promising technology for the production of carbon materials with negative carbon emissions. However, the high reaction temperature and energy consumption have limited the development of HTC technology. In conventional batch reactors, the temperature and pressure are typically coupled at saturated states. In this study, a decoupled temperature and pressure hydrothermal(DTPH) reaction system was developed to decrease the temperature of the HTC reaction of lignocellulosic biomass(rice straw and poplar leaves). The properties of hydrochars were analyzed by scanning electron microscopy(SEM), Fourier transform infrared(FTIR) spectroscopy, X-ray photoelectron spectroscopy(XPS), Raman spectroscopy, X-ray diffraction(XRD), thermogravimetric analyzer(TGA), etc. to propose the reaction mechanism. The results showed that the HTC reaction of lignocellulosic biomass could be realized at a low temperature of 200℃ in the DTPH process, breaking the temperature limit(230℃) in the conventional process. The DTPH method could break the barrier of the crystalline structure of cellulose in the lignocellulosic biomass with high cellulose content, realizing the carbonization of cellulose and hemicellulose with the dehydration, unsaturated bond formation, and aromatization. The produced hydrochar had an appearance of carbon microspheres, with high calorific values, abundant oxygen-containing functional groups, a certain degree of graphitization, and good thermal stability. Cellulose acts not only as a barrier to protect itself and hemicellulose from decomposition, but also as a key precursor for the formation of carbon microspheres. This study shows a promising method for synthesizing carbon materials from lignocellulosic biomass with a carbon-negative effect.
基金This work is supported by the National Natural Science Foundation of China(Grant Nos.21802167,21961132026,92034302,21878331,91645108)the National Key Research and Development Program Nanotechnology Specific Project(No.2020YFA0210903).
文摘Propylene is a significant basic material for petrochemicals such as polypropylene,propylene oxide,etc.With abundant propane supply from shale gas,propane dehydrogenation(PDH)becomes extensively attractive as an on-purpose propylene production route in recent years.Nitrogen-doped carbon(NC)nanopolyhedra supported cobalt catalysts were synthesized in one-step of ZIF-67 pyrolysis and investigated further in PDH.XPS,TEM and N_(2) adsorption-desorption were used to study the influence of carbonization temperature on as-prepared NC supported cobalt catalysts.The temperature is found to affect the cobalt phase and nitrogen species of the catalysts.And the positive correlation was established between Co0 proportion and space time yield of propylene,indicating that the modulation of carbonization temperature could be important for catalytic performance.
基金The authors acknowledge the financial support provided by the Key R&D Program of Shaanxi Province(No.2022SF-168)Xi’an Programs for Science and Technology Plan(Nos.2020KJRC0090 and 21XJZZ0045)+5 种基金Xi’an Beilin District Programs for Science and Technology Plan(No.GX2247)the Outstanding Chinese and Foreign Youth Exchange Program of China Association for Science and Technology(CAST)in 2019the Opening Project of Shanxi Key Laboratory of Advanced Manufacturing Technology(No.XJZZ202001)the Scientific Research Project of Shaanxi Education Department(No.20JS108)Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(No.KFKT2021-01)Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology,Shaanxi University of Science and Technology(No.KFKT2021-01).
文摘Greenhouse gas emissions from waste plastics have caused global warming all over the world,which has been a central threat to the ecological environment for humans,flora and fauna.Among waste plastics,waste polyethylene terephthalate(PET)is attractive due to its excellent stability and degradation-resistant.Therefore,merging China’s carbon peak and carbon neutrality goals would be beneficial.In this review,we summarize the current state-of-the-art of carbon emission decrease from a multi-scale perspective technologically.We suggest that the carbon peak for waste PET can be achieved by employing the closed-loop supply chain,including recycling,biomass utilization,carbon capture and utilization.Waste PET can be a valuable and renewable resource in the whole life cycle.Undoubtedly,all kinds of PET plastics can be ultimately converted into CO_(2),which can also be feedstock for various kinds of chemical products,including ethyl alcohol,formic acid,soda ash,PU,starch and so on.As a result,the closed-loop supply chain can help the PET plastics industry drastically reduce its carbon footprint.
基金supported by the State Key Laboratory of Advanced Metallurgy,China(Project Code:41603006).
文摘Decarbonization is a critical issue for peaking CO_(2) emissions of energy-intensive industries,such as the iron and steel industry.The decarbonization options of China’s ironmaking and steelmaking sector were discussed based on a systematic three-dimensional low-carbon analysis from the aspects of resource utilization(Y),energy utilization(Q),and energy cleanliness which is evaluated by a process general emission factor(PGEF)on all the related processes,including the current blast furnace(BF)-basic oxygen furnace(BOF)integrated process and the specific sub-processes,as well as the electric arc furnace(EAF)process,typical direct reduction(DR)process,and smelting reduction(SR)process.The study indicates that the three-dimensional aspects,particularly the energy structure,should be comprehensively considered to quantitatively evaluate the decarbonization road map based on novel technologies or processes.Promoting scrap utilization(improvement of Y)and the substitution of carbon-based energy(improvement of PGEF)in particular is critical.In terms of process scale,promoting the development of the scrap-based EAF or DR-EAF process is highly encouraged because of their lower PGEF.The three-dimensional method is expected to extend to other processes or industries,such as the cement production and thermal electricity generation industries.
基金the National Natural Science Foundation of China(Nos.52102036 and52301192)the Sichuan Science and Technology Program,China(No.2021JDRC0099)+3 种基金Taishan Scholars and Young Experts Program of Shandong Province,China(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution,China(Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province,China(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams)“Sanqin Scholars”Innovation Teams Project of Shaanxi Province,China(Clean Energy Materials and High-Performance Devices Innovation Team of Shaanxi Dongling Smelting Co.,Ltd.)。
文摘Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.
基金The authors gratefully acknowledge financial support from the National Natural Science Foundation of China(52103090)the Natural Science Foundation of Guangdong Province(2022A1515011780)Autonomous deployment project of China National Key Laboratory of Materials for Integrated Circuits(NKLJC-Z2023-B03).
文摘The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)shielding.However,for macroscopic CNT assemblies,such as CNT film,achieving high electrical and mechanical properties remains challenging,which heavily depends on the tube-tube interac-tions of CNTs.Herein,we develop a novel strategy based on metal-organic decomposition(MOD)to fabricate a flexible silver-carbon nanotube(Ag-CNT)film.The Ag particles are introduced in situ into the CNT film through annealing of MOD,leading to enhanced tube-tube interactions.As a result,the electrical conductivity of Ag-CNT film is up to 6.82×10^(5) S m^(-1),and the EMI shielding effectiveness of Ag-CNT film with a thickness of~7.8μm exceeds 66 dB in the ultra-broad frequency range(3-40 GHz).The tensile strength and Young’s modulus of Ag-CNT film increase from 30.09±3.14 to 76.06±6.20 MPa(~253%)and from 1.12±0.33 to 8.90±0.97 GPa(~795%),respectively.Moreover,the Ag-CNT film exhibits excellent near-field shield-ing performance,which can effectively block wireless transmission.This innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.
基金supported by research pro-grams of National Natural Science Foundation of China(Nos.52101274 and 52377026)Natural Science Foundation of Shandong Province,China(Nos.ZR2020QE011 and ZR2022ME089)+4 种基金Taishan Scholars and Young Experts Pro-gram of Shandong Province,China(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution,China(Research and Innovation Team of Structural-Functional Polymer Composites)Special Fin-ancial of Shandong Province,China(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams),Youth Top Talent Foundation of Yantai University(No.2219008)Graduate Innovation Foundation of Yantai University(No.GIFYTU2240)College Student Innovation and Entrepreneurship Training Program Project(No.202311066088).
文摘NiMZn/C@melamine sponge-derived carbon(MSDC)composites(M=Co,Fe,and Mn)were prepared by a vacuum pump-ing solution method followed by carbonization.A large number of carbon nanotubes(CNTs)homogeneously attached to the surfaces of the three-dimensional cross-linked of the sponge-derived carbon in the NiCoZn/C@MSDC composite,and CNTs were detected in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.Ni_(3)ZnC_(0.7),Ni_(3)Fe,and MnO in-situ formed in the NiFeZn/C@MSDC and NiMnZn/C@MSDC composites.The CNTs in the NiCoZn/C@MSDC composite efficiently modulated its complex permittivity.Thus,the composite exhibited the best performance among the composites,with the minimum reflection loss(RL_(min))of-33.1 dB at 18 GHz and thickness of 1.4 mm.The bandwidth for RL of≤-10 dB was up to 5.04 GHz at the thickness of 1.7 mm and loading of 25wt%.The op-timized impedance matching,enhanced interfacial and dipole polarization,remarkable conduction loss,and multiple reflections and scat-tering of the incident microwaves improved the microwave absorption performance.The effects of Co,Ni,and Fe on the phase and mor-phology provided an alternative way for developing highly efficient and broadband microwave absorbers.
基金Under the auspices of National Natural Science Foundation of China(No.42171230)。
文摘Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.
基金funding support from the National Key R&D Program of China(Grant No.2022YFE0115800)the Creative Groups of Natural Science Foundation of Hubei Province(Grant No.2021CFA030)Shanxi Provincial Key Research and Development Project(Grant No.202102090301009).
文摘Global warming has greatly threatened the human living environment and carbon capture and storage(CCS)technology is recognized as a promising way to reduce carbon emissions.Mineral storage is considered a reliable option for long-term carbon storage.Basalt rich in alkaline earth elements facilitates rapid and permanent CO_(2) fixation as carbonates.However,the complex CO_(2)-fluid-basalt interaction poses challenges for assessing carbon storage potential.Under different reaction conditions,the carbonation products and carbonation rates vary.Carbon mineralization reactions also induce petrophysical and mechanical responses,which have potential risks for the long-term injectivity and the carbon storage safety in basalt reservoirs.In this paper,recent advances in carbon mineralization storage in basalt based on laboratory research are comprehensively reviewed.The assessment methods for carbon storage potential are introduced and the carbon trapping mechanisms are investigated with the identification of the controlling factors.Changes in pore structure,permeability and mechanical properties in both static reactions and reactive percolation experiments are also discussed.This study could provide insight into challenges as well as perspectives for future research.
基金the National Natural Science Foundation of China(Nos.U20A2089 and 41971152)the Research Foundation of the Department of Natural Resources of Hunan Province(No.20230138ST)to SLthe open research fund of Technology Innovation Center for Ecological Conservation and Restoration in Dongting Lake Basin,Ministry of Natural Resources(No.2023005)to YZ。
文摘Understanding the spatial variation,temporal changes,and their underlying driving forces of carbon sequestration in various forests is of great importance for understanding the carbon cycle and carbon management options.How carbon density and sequestration in various Cunninghamia lanceolata forests,extensively cultivated for timber production in subtropical China,vary with biodiversity,forest structure,environment,and cultural factors remain poorly explored,presenting a critical knowledge gap for realizing carbon sequestration supply potential through management.Based on a large-scale database of 449 permanent forest inventory plots,we quantified the spatial-temporal heterogeneity of aboveground carbon densities and carbon accumulation rates in Cunninghamia lanceolate forests in Hunan Province,China,and attributed the contributions of stand structure,environmental,and management factors to the heterogeneity using quantile age-sequence analysis,partial least squares path modeling(PLS-PM),and hot-spot analysis.The results showed lower values of carbon density and sequestration on average,in comparison with other forests in the same climate zone(i.e.,subtropics),with pronounced spatial and temporal variability.Specifically,quantile regression analysis using carbon accumulation rates along an age sequence showed large differences in carbon sequestration rates among underperformed and outperformed forests(0.50 and 1.80 Mg·ha^(-1)·yr^(-1)).PLS-PM demonstrated that maximum DBH and stand density were the main crucial drivers of aboveground carbon density from young to mature forests.Furthermore,species diversity and geotopographic factors were the significant factors causing the large discrepancy in aboveground carbon density change between low-and high-carbon-bearing forests.Hotspot analysis revealed the importance of culture attributes in shaping the geospatial patterns of carbon sequestration.Our work highlighted that retaining largesized DBH trees and increasing shade-tolerant tree species were important to enhance carbon sequestration in C.lanceolate forests.
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金supported by the General Project of Top-Design of Multi-Scale Nature-Social ModelsData Support and Decision Support System for NSFC Carbon Neutrality Major Project(42341202)the Basic Scientific Research Fund of the Chinese Academy of Meteorological Sciences(2021Z014)。
文摘CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.
基金financial support from the King Abdullah University of Science and Technology(KAUST).
文摘The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.
基金supported by the Basic Scientific Research Funds for Colleges and Universities affiliated to Hebei Province(JST2022005)Thanks are given to the financial support from the National Natural Science Foundation of China(22005099).
文摘MXenes are a family of two-dimensional(2D)layered transition metal carbides/nitrides that show promising potential for energy storage applications due to their high-specific surface areas,excellent electron conductivity,good hydrophilicity,and tunable terminations.Among various types of MXenes,Ti_(3)C_(2)T_(x) is the most widely studied for use in capacitive energy storage applications,especially in supercapacitors(SCs).However,the stacking and oxidation of MXene sheets inevitably lead to a significant loss of electrochemically active sites.To overcome such challenges,carbon materials are frequently incorporated into MXenes to enhance their electrochemical properties.This review introduces the common strategies used for synthesizing Ti_(3)C_(2)T_(x),followed by a comprehensive overview of recent developments in Ti_(3)C_(2)T_(x)/carbon composites as electrode materials for SCs.Ti_(3)C_(2)T_(x)/carbon composites are categorized based on the dimensions of carbons,including 0D carbon dots,1D carbon nanotubes and fibers,2D graphene,and 3D carbon materials(activated carbon,polymer-derived carbon,etc.).Finally,this review also provides a perspective on developing novel MXenes/carbon composites as electrodes for application in SCs.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52130303,52327802,52303101,52173078,51973158)the China Postdoctoral Science Foundation(2023M732579)+2 种基金Young Elite Scientists Sponsorship Program by CAST(No.2022QNRC001)National Key R&D Program of China(No.2022YFB3805702)Joint Funds of Ministry of Education(8091B032218).
文摘Vertically oriented carbon structures constructed from low-dimen-sional carbon materials are ideal frameworks for high-performance thermal inter-face materials(TIMs).However,improving the interfacial heat-transfer efficiency of vertically oriented carbon structures is a challenging task.Herein,an orthotropic three-dimensional(3D)hybrid carbon network(VSCG)is fabricated by depositing vertically aligned carbon nanotubes(VACNTs)on the surface of a horizontally oriented graphene film(HOGF).The interfacial interaction between the VACNTs and HOGF is then optimized through an annealing strategy.After regulating the orientation structure of the VACNTs and filling the VSCG with polydimethylsi-loxane(PDMS),VSCG/PDMS composites with excellent 3D thermal conductive properties are obtained.The highest in-plane and through-plane thermal conduc-tivities of the composites are 113.61 and 24.37 W m^(-1)K^(-1),respectively.The high contact area of HOGF and good compressibility of VACNTs imbue the VSCG/PDMS composite with low thermal resistance.In addition,the interfacial heat-transfer efficiency of VSCG/PDMS composite in the TIM performance was improved by 71.3%compared to that of a state-of-the-art thermal pad.This new structural design can potentially realize high-performance TIMs that meet the need for high thermal conductivity and low contact thermal resistance in interfacial heat-transfer processes.
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Ministry of Science and ICT(MSIT)(RS-2023-00251283,and 2022M3D1A2083618)by the Ministry of Education(2020R1A6A1A03040516).
文摘Advancements in sensor technology have significantly enhanced atmospheric monitoring.Notably,metal oxide and carbon(MO_(x)/C)hybrids have gained attention for their exceptional sensitivity and room-temperature sensing performance.However,previous methods of synthesizing MO_(x)/C composites suffer from problems,including inhomogeneity,aggregation,and challenges in micropatterning.Herein,we introduce a refined method that employs a metal–organic framework(MOF)as a precursor combined with direct laser writing.The inherent structure of MOFs ensures a uniform distribution of metal ions and organic linkers,yielding homogeneous MO_(x)/C structures.The laser processing facilitates precise micropatterning(<2μm,comparable to typical photolithography)of the MO_(x)/C crystals.The optimized MOF-derived MO_(x)/C sensor rapidly detected ethanol gas even at room temperature(105 and 18 s for response and recovery,respectively),with a broad range of sensing performance from 170 to 3,400 ppm and a high response value of up to 3,500%.Additionally,this sensor exhibited enhanced stability and thermal resilience compared to previous MOF-based counterparts.This research opens up promising avenues for practical applications in MOF-derived sensing devices.
基金the financial support from the Australian Research CouncilCentre for Materials Science,Queensland University of Technology。
文摘Tin disulfide(SnS_(2)),due to large interlayer spacing and high theoretical capacity,is regarded as a prospective anode material for lithium-ion batteries.Nevertheless,the poor electron conductivity of SnS_(2) and huge volumetric change during the lithiation/delithiation process lead to a rapid capacity decay of the battery,hindering its commercialization.To address these issues,herein,SnS_(2) is in-situ grown on the surface of carbon nanotubes(CNT)and then encapsulated with a layer of porous amorphous carbon(CNT/SnS_(2)@C)by simple solvothermal and further carbonization treatment.The synergistic effect of CNT and porous carbon layer not only enhances the electrical co nductivity of SnS_(2) but also limits the huge volumetric change to avoid the pulverization and detachment of SnS_(2).Density functional theo ry calculations show that CNT/SnS_(2)@C has high Li^(+)adsorption and lithium storage capacity achieving high reaction kinetics.Consequently,cells with the CNT/SnS_(2)@C anode exhibit a high lithium storage capacity of 837mAh/g after 100 cycles at 0.1 A/g and retaining a capacity of 529.8 mAh/g under 1.0 A/g after 1000 cycles.This study provides a fundamental understanding of the electrochemical processes and beneficial guidance to design high-performance SnS_(2)-based anodes for LIBs.
