Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a sim...Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge,due to the difficulty of achieving an optimal match between polymers and fillers.In this study,we incorporate a porous carbon-based zinc oxide composite(C@ZnO)into high-permeability polymers of intrinsic microporosity(PIMs)to fabricate MMMs.The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility,mitigating the formation of non-selective voids in the resulting MMMs.Concurrently,C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs.As a result,the CO_(2) permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer,while the CO_(2)/N_(2) and CO_(2)/CH_(4) selectivity reached 21.5 and 14.4,respectively,substantially surpassing the 2008 Robeson upper bound.Additionally,molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO_(2) affinity of C@ZnO.In summary,we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.展开更多
Tibetan Plateau,as one of the most carbon intensive regions in China,is crucial in the carbon cycle,and accurately estimating its vegetation carbon density(C_(VEG))is essential for assessing regional and national carb...Tibetan Plateau,as one of the most carbon intensive regions in China,is crucial in the carbon cycle,and accurately estimating its vegetation carbon density(C_(VEG))is essential for assessing regional and national carbon balance.However,the spatial distribution of regional C_(VEG) is not available remains highly uncertain due to lack of systematic research,especially for different organs.Here,we investigated the spatial distribution patterns and driving factors of C_(VEG) among different plant organs(leaf,branch,trunk and root)by systematically field grid-sampling 2040 field-plots of plant communities over the Tibetan Plateau from 2019 to 2020.The results showed that the carbon content of plant organs ranged from 255.53 to 515.58 g kg^(-1),with the highest in branches and the lowest in roots.Among the different plant functional groups,the highest C_(VEG) was found in evergreen coniferous forests,and the lowest in desert grasslands,with an average C_(VEG) of 1603.98 g m^(-2).C_(VEG) increased spatially from northwest to southeast over the Tibetan Plateau,with MAP being the dominant factor.Furthermore,the total vegetation carbon stock on the Tibetan Plateau was estimated to be 1965.62 Tg for all vegetation types.Based on the comprehensive field survey dataset,the Random Forest model effectively predicted and mapped the spatial distribution of C_(VEG)(including aboveground,belowground,and the total biomass carbon density)over the Tibetan Plateau with notable accuracy(validation R2 values were 71%,56%,and 64%for C_(AGB),C_(BGB),and C_(VEG),respectively)at a spatial resolution of 1 km×1 km.Our findings can help improve the accuracy of regional carbon stock estimations and provide parameters for carbon cycle model optimization and remote sensing calibration in the future.展开更多
The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportio...The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst design.Herein,a Ni2+-loaded porous poly(ionic liquids)(PIL)precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing temperature.The catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO_(2)into CO.Operando Ni K-edge X-ray absorption near-edge structure(XANES)spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and NPs.The charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active sites.In the electroreduction of CO_(2),the coexistence of Ni SAs and NPs strengthened the CO_(2)activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO_(2)→*COOH step,and therefore promoted the catalysis efficiency.展开更多
With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its ...With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.展开更多
Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogena...Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.展开更多
Chloroform and other volatile organic pollutants have garnered widespread attention from the public and researchers,because of their potential harm to the respiratory system,nervous system,skin,and eyes.However,resear...Chloroform and other volatile organic pollutants have garnered widespread attention from the public and researchers,because of their potential harm to the respiratory system,nervous system,skin,and eyes.However,research on chloroform vapor sensing is still in its early stages,primarily due to the lack of specific recognition motif.Here we report a mesoporous photonic crystal sensor incorporating carbon dots-based nanoreceptor(HMSS@CDs-PCs)for enhanced chloroform sensing.The colloidal PC packed with hollow mesoporous silica spheres provides an interconnected ordered macro-meso-hierarchical porous structure,ideal for rapid gas sensing utilizing the photonic bandgap shift as the readout signal.The as-synthesized CDs with pyridinic-N-oxide functional groups adsorbed in the hollow mesoporous silica spheres are found to not only serve as the chloroform adsorption sites,but also a molecular glue that prevents crack formation in the colloidal PC.The sensitivity of HMSS@CDs-PCs sensor is 0.79 nm ppm^(-1)and an impressively low limit of detection is 3.22 ppm,which are the best reported values in fast-response chloroform vapor sensor without multi-signal assistance.The positive response time is 7.5 s and the negative response time 9 s.Furthermore,relatively stable sensing can be maintained within a relative humidity of 20%-85%RH and temperature of 25-55℃.This study demonstrates that HMSS@CDs-PCs sensors have practical application potential in indoor and outdoor chloroform vapor detection.展开更多
Hard carbon (HC) has been considered as promising anode material for sodium-ion batteries (SIBs).The optimization of hard carbon’s microstructure and solid electrolyte interface (SEI) property are demonstrated effect...Hard carbon (HC) has been considered as promising anode material for sodium-ion batteries (SIBs).The optimization of hard carbon’s microstructure and solid electrolyte interface (SEI) property are demonstrated effective in enhancing the Na+storage capability,however,a one-step regulation strategy to achieve simultaneous multi-scale structures optimization is highly desirable.Herein,we have systematically investigated the effects of boron doping on hard carbon’s microstructure and interface chemistry.A variety of structure characterizations show that appropriate amount of boron doping can increase the size of closed pores via rearrangement of carbon layers with improved graphitization degree,which provides more Na+storage sites.In-situ Fourier transform infrared spectroscopy/electrochemical impedance spectroscopy (FTIR/EIS) and X-ray photoelectron spectroscopy (XPS) analysis demonstrate the presence of more BC3and less B–C–O structures that result in enhanced ion diffusion kinetics and the formation of inorganic rich and robust SEI,which leads to facilitated charge transfer and excellent rate performance.As a result,the hard carbon anode with optimized boron doping content exhibits enhanced rate and cycling performance.In general,this work unravels the critical role of boron doping in optimizing the pore structure,interface chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced Na+storage performance.展开更多
Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,...Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.展开更多
The Cu^(+)/Cu^(0)sites of copper-based catalysts are crucial for enhancing the production of multicarbon(C_(2+))products from electrochemical CO_(2)reduction reaction(eCO_(2)RR).However,the unstable Cu^(+)and insuffic...The Cu^(+)/Cu^(0)sites of copper-based catalysts are crucial for enhancing the production of multicarbon(C_(2+))products from electrochemical CO_(2)reduction reaction(eCO_(2)RR).However,the unstable Cu^(+)and insufficient Cu^(+)/Cu^(0)active sites lead to their limited selectivity and stability for C_(2+)production.Herein,we embedded copper oxide(CuO_(x))particles into porous nitrogen-doped carbon nanofibers(CuO_(x)@PCNF)by pyrolysis of the electrospun fiber film containing ZIF-8 and Cu_(2)O particles.The porous nitrogendoped carbon nanofibers protected and dispersed Cu^(+)species,and its micro porous structure enhanced the interaction between CuO_(x)and reactants during eCO_(2)RR.The obtained CuO_(x)@PCNF created more effective and stable Cu^(+)/Cu^(0)active sites.It showed a high Faradaic efficiency of 62.5%for C_(2+)products in Hcell,which was 2 times higher than that of bare CuO_(x)(~31.1%).Furthermore,it achieved a maximum Faradaic efficiency of 80.7%for C_(2+)products in flow cell.In situ characterization and density functional theory(DFT)calculation confirmed that the N-doped carbon layer protected Cu^(+)from electrochemical reduction and lowered the energy barrier for the dimerization of^(*)CO.Stable and exposed Cu^(+)/Cu^(0)active sites enhanced the enrichment of^(*)CO and promoted the C-C coupling reaction on the catalyst surface,which facilitated the formation of C_(2+)products.展开更多
Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,...Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,acetamide,and urea through an efficient catalytical process that involves C–C and C–N coupling.However,the origin of the coupling activity remained unclear,which substantially hinders the rational design of Cu-based catalysts for the N-integrated CO_(2)reduction reaction(CO_(2)RR).To address this challenge,this work performed advanced density functional theory calculations incorporating explicit solvation based on a Cu_(2)-based N-doped carbon(Cu_(2)N_(6)C_(10))catalyst for CO_(2)RR.These calculations are aimed to gain insight into the reaction mechanisms for the synthesis of ethylene,acetamide,and urea via coupling in the interfacial reaction micro-environment.Due to the sluggishness of CO_(2),the formation of a solvation electric layer by anions(F^(-),Cl^(-),Br^(-),and I^(-))and cations(Na+,Mg^(2+),K+,and Ca^(2+))leads to electron transfer towards the Cu surface.This process significantly accelerates the reduction of CO_(2).These results reveal that*CO intermediates play a pivotal role in N-integrated CO_(2)RR.Remarkably,the Cu_(2)-based N-doped carbon catalyst examined in this study has demonstrated the most potential for C–N coupling to date.Our findings reveal that through the process of a condensation reaction between*CO and NH_(2)OH for urea synthesis,*NO_(3)-is reduced to*NH_(3),and*CO_(2)to*CCO at dual Cu atom sites.This dual-site reduction facilitates the synthesis of acetamide through a nucleophilic reaction between NH_(3)and the ketene intermediate.Furthermore,we found that the I-and Mg^(2+)ions,influenced by pH,were highly effective for acetamide and ammonia synthesis,except when F-and Ca^(2+)were present.Furthermore,the mechanisms of C–N bond formation were investigated via ab-initio molecular dynamics simulations,and we found that adjusting the micro-environment can change the dominant side reaction,shifting from hydrogen production in acidic conditions to water reduction in alkaline ones.This study introduces a novel approach using ion-H_(2)O cages to significantly enhance the efficiency of C–N coupling reactions.展开更多
TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bul...TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.展开更多
Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbo...Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbon neutrality system that balances energy production and carbon reduction becomes crucial for the transformation of such basins.Under the framework of a green and intelligent energy system primarily based on“four news”,new energy,new electricity,new energy storage,and new intelligence,integrating a“super energy system”composed of a huge amount of underground resources of coal,oil,gas and heat highly overlapping with abundant wind and solar energy resources above ground,and a regional intelligent energy consumption system with coordinated development and utilization of fossil energy and new energy,with a carbon neutrality system centered around carbon cycling is essential.This paper aims to select the traditional oil and gas basins as“super energy basins”with the conditions to build world-class energy production and demonstration bases for carbon neutrality.The Ordos Basin has unique regional advantages,including abundant fossil fuel and new energy resources,as well as matching CO_(2)sources and sinks,position it as a carbon neutrality“super energy basin”which explores the path of transformation of traditional oil and gas basins.Under the integrated development concept and mode of“coal+oil+gas+new energy+carbon capture,utilization and storage(CCUS)/carbon capture and storage(CCS)”,the carbon neutrality in super energy basin is basically achieved,which enhance energy supply and contribute to the carbon peak and carbon neutrality goals,establish a modern energy industry and promote regional green and sustainable development.The pioneering construction of the world-class carbon neutrality“super energy system”demonstration basin in China represented by the Ordos Basin will reshape the new concept and new mode of exploration and development of super energy basins,which is of great significance to the global energy revolution under carbon neutrality.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
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
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
In the Mediterranean region,despite bamboo being an alien species that can seriously alter plant and ani-mal biocoenosis,the area occupied by bamboo plantations continues to increase,especially for the purpose to sequ...In the Mediterranean region,despite bamboo being an alien species that can seriously alter plant and ani-mal biocoenosis,the area occupied by bamboo plantations continues to increase,especially for the purpose to seques-ter carbon(C).However,the C dynamics in the soil-plant system when bamboo is grown outside its native area are poorly understood.Here we investigated the C mitigation potential of the fast-growing Moso bamboo(Phyllostachys edulis)introduced in Italy for climate-change mitigation.We analyzed aboveground(AGB)and belowground(as root/shoot ratio)biomass,litter and soil organic C(SOC)at O-15-and 15-30-cm depths in a 4-year-old bamboo plantation in comparison with the former annual cropland on which the bamboo was established.To have an idea of the maximum C stored at an ecosystem level,a natural forest adjacent the two sites was also considered.In the plantation,C accumulation as AGB was stimulated,with 14.8±3.1 Mg C ha^(-1) stored in 3 years;because thinning was done to remove culms from the first year,the mean sequestration rate was 4.9 Mg C ha^(-1) a^(-1).The sequestration rates were high but comparable to other fast-growing tree species in Italy(e.g.,Pinus nigra).SOC was significantly higher in the bamboo plantation than in the cropland only at the 0-15 cm depth,but SOC stock did not differ.Possibly 4 years were not enough time for a clear increase in SOC,or the high nutrient uptake by bamboos might have depleted the soil nutrients,thus inhibiting the soil organic matter formation by bacteria.In comparison,the natural forest had significantly higher C levels in all the pools.For C dynamics at an ecosystem level,the bamboo plantation on the former annual cropland led to substantial C removal from the atmosphere(about 12 Mg C ha^(-1) a^(-1)).However,despite the promising C sequestration rates by bamboo,its introduction should be carefully considered due to potential ecological problems caused by this species in overexploited environments such as the Mediterranean area.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
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
Global forests are increasingly crucial for achiev-ing net-zero carbon emissions,with a quarter of the miti-gation efforts under the Paris Climate Agreement directed towards forests.In China,forests currently contribu...Global forests are increasingly crucial for achiev-ing net-zero carbon emissions,with a quarter of the miti-gation efforts under the Paris Climate Agreement directed towards forests.In China,forests currently contribute to 13%of the global land’s carbon sink,but their stability and per-sistence remain uncertain.We examined and identified that published studies suffered from oversimplifications of eco-system succession and tree demographic dynamics,as well as poor constraints on land quality.Consequently,substan-tial estimations might have been suffered from underrepre-sented or ignored crucial factors,including tree demographic dynamics,and disturbances and habitat shifts caused by global climate change.We argue that these essential factors should be considered to enhance the reliability and accuracy of assessments of the potential for forest carbon sinks.展开更多
基金financial support from the National Natural Science Foundation of China(Nos.22108258 and 52003251)Program for Science&Technology Innovation Talents in Universities of Henan Province(24HASTIT004)+1 种基金Outstanding Youth Fund of Henan Scientific Committee(222300420085)Science and Technology Joint Project of Henan Province(222301420041)。
文摘Mixed matrix membranes(MMMs)have demonstrated significant promise in energy-intensive gas separations by amalgamating the unique properties of fillers with the facile processability of polymers.However,achieving a simultaneous enhancement of permeability and selectivity remains a formidable challenge,due to the difficulty of achieving an optimal match between polymers and fillers.In this study,we incorporate a porous carbon-based zinc oxide composite(C@ZnO)into high-permeability polymers of intrinsic microporosity(PIMs)to fabricate MMMs.The dipole–dipole interaction between C@ZnO and PIMs ensures their exceptional compatibility,mitigating the formation of non-selective voids in the resulting MMMs.Concurrently,C@ZnO with abundant interconnected pores can provide additional low-resistance pathways for gas transport in MMMs.As a result,the CO_(2) permeability of the optimized C@ZnO/PIM-1 MMMs is elevated to 13,215 barrer,while the CO_(2)/N_(2) and CO_(2)/CH_(4) selectivity reached 21.5 and 14.4,respectively,substantially surpassing the 2008 Robeson upper bound.Additionally,molecular simulation results further corroborate that the augmented membrane gas selectivity is attributed to the superior CO_(2) affinity of C@ZnO.In summary,we believe that this work not only expands the application of MMMs for gas separation but also heralds a paradigm shift in the application of porous carbon materials.
基金supported by CAS Project for Young Scientists in Basic Research(YSBR-037)the National Natural Science Foundation of China(42141004,32430067)by the Second Tibetan Plateau Scientific Expedition and Research Program(STEP,2019QZKK060602).
文摘Tibetan Plateau,as one of the most carbon intensive regions in China,is crucial in the carbon cycle,and accurately estimating its vegetation carbon density(C_(VEG))is essential for assessing regional and national carbon balance.However,the spatial distribution of regional C_(VEG) is not available remains highly uncertain due to lack of systematic research,especially for different organs.Here,we investigated the spatial distribution patterns and driving factors of C_(VEG) among different plant organs(leaf,branch,trunk and root)by systematically field grid-sampling 2040 field-plots of plant communities over the Tibetan Plateau from 2019 to 2020.The results showed that the carbon content of plant organs ranged from 255.53 to 515.58 g kg^(-1),with the highest in branches and the lowest in roots.Among the different plant functional groups,the highest C_(VEG) was found in evergreen coniferous forests,and the lowest in desert grasslands,with an average C_(VEG) of 1603.98 g m^(-2).C_(VEG) increased spatially from northwest to southeast over the Tibetan Plateau,with MAP being the dominant factor.Furthermore,the total vegetation carbon stock on the Tibetan Plateau was estimated to be 1965.62 Tg for all vegetation types.Based on the comprehensive field survey dataset,the Random Forest model effectively predicted and mapped the spatial distribution of C_(VEG)(including aboveground,belowground,and the total biomass carbon density)over the Tibetan Plateau with notable accuracy(validation R2 values were 71%,56%,and 64%for C_(AGB),C_(BGB),and C_(VEG),respectively)at a spatial resolution of 1 km×1 km.Our findings can help improve the accuracy of regional carbon stock estimations and provide parameters for carbon cycle model optimization and remote sensing calibration in the future.
基金National Natural Science Foundation of China(grants 22072065,22178162,and 22222806)Distinguished Youth Foundation of Jiangsu Province(grant BK20220053)Six talent peaks project in Jiangsu Province(grant JNHB-035)。
文摘The synergy of single atoms(SAs)and nanoparticles(NPs)has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction(CO_(2)RR);however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst design.Herein,a Ni2+-loaded porous poly(ionic liquids)(PIL)precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing temperature.The catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO_(2)into CO.Operando Ni K-edge X-ray absorption near-edge structure(XANES)spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and NPs.The charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active sites.In the electroreduction of CO_(2),the coexistence of Ni SAs and NPs strengthened the CO_(2)activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO_(2)→*COOH step,and therefore promoted the catalysis efficiency.
基金supported by the National Research Foundation(NRF)of Korea grant funded by the Korean government(MSIT)(No.NRF-2021 M3 H4A1A02045962).
文摘With the increasing prevalence of lithium-ion batteries(LIBs)applications,the demand for high-capacity next-generation materials has also increased.SiO_(x)is currently considered a promising anode material due to its exceptionally high capacity for LIBs.However,the significant volumetric changes of SiO_(x)during cycling and its initial Coulombic efficiency(ICE)complicate its use,whether alone or in combination with graphite materials.In this study,a three-dimensional conductive binder network with high electronic conductivity and robust elasticity for graphite/SiO_(x)blended anodes was proposed by chemically anchoring carbon nanotubes and carboxymethyl cellulose binders using tannic acid as a chemical cross-linker.In addition,a dehydrogenation-based prelithiation strategy employing lithium hydride was utilized to enhance the ICE of SiO_(x).The combination of these two strategies increased the CE of SiO_(x)from 74%to87%and effectively mitigated its volume expansion in the graphite/SiO_(x)blended electrode,resulting in an efficient electron-conductive binder network.This led to a remarkable capacity retention of 94%after30 cycles,even under challenging conditions,with a high capacity of 550 mA h g^(-1)and a current density of 4 mA cm^(-2).Furthermore,to validate the feasibility of utilizing prelithiated SiO_(x)anode materials and the conductive binder network in LIBs,a full cell incorporating these materials and a single-crystalline Ni-rich cathode was used.This cell demonstrated a~27.3%increase in discharge capacity of the first cycle(~185.7 mA h g^(-1))and exhibited a cycling stability of 300 cycles.Thus,this study reports a simple,feasible,and insightful method for designing high-performance LIB electrodes.
基金National Natural Science Foundation of China (Nos. 22371244 and 21573192)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX22_3463)。
文摘Transition metal-carbonate interfaces often act as active sites in heterogeneous catalytic reactions.The interface between transition metal and metal carbonate exhibits a dynamic equilibrium during the CO_(2)hydrogenation reaction,involving surface carbonate hydrogenation and CO_(2)chemisorption.Nonetheless,there have been few reports on engineering the activity of the interface between transition metal and alkaline earth metal carbonate for catalytic CO_(2)conversion.This work demonstrated that the incorporation of CaH_(2)in Ni/CaCO_(3)enhances the CO_(2)methanation activity of the catalysts.The CO_(2)conversion for Ni/CaH_(2)-CaCO_(3)reached 68.5%at 400°C,which was much higher than that of the Ni/CaCO_(3)(31.6%) and Ni/CaH_(2)-CaO (42.4%) catalysts.Furthermore,the Ni/CaH_(2)-CaCO_(3)catalysts remained stable during the stability test for 24 h at 400°C and 8 bar.Our research revealed that CaH_(2)played a crucial role in promoting the activity of the Ni-carbonate interface for CO_(2)methanation.CaH_(2)could modify the electronic structure of Ni and tune the structural properties of CaCO_(3)to generate medium basic sites (OH groups),which are favorable for the activation of H2and CO_(2).In-situ Fourier transform infrared spectroscopy (FTIR) analysis combined with density functional theory calculations demonstrated that CO_(2)activation occurs at the hydroxyl group (OH) on the CaH_(2)-modified Ni-carbonate surface,leading to the formation of CO_(3)H*species.Furthermore,our study has confirmed that CO_(2)methanation over the Ni/CaH_(2)-CaCO_(3)catalysts proceeds via the formate pathway.
基金supported by the National Key Research and Development Program of China(No.2022YFB3205500)National Natural Science Foundation of China(Nos.U23A20360 and 62303192)QL wishes to thank Water Research Australia(WRA 1144/21)for funding support.
文摘Chloroform and other volatile organic pollutants have garnered widespread attention from the public and researchers,because of their potential harm to the respiratory system,nervous system,skin,and eyes.However,research on chloroform vapor sensing is still in its early stages,primarily due to the lack of specific recognition motif.Here we report a mesoporous photonic crystal sensor incorporating carbon dots-based nanoreceptor(HMSS@CDs-PCs)for enhanced chloroform sensing.The colloidal PC packed with hollow mesoporous silica spheres provides an interconnected ordered macro-meso-hierarchical porous structure,ideal for rapid gas sensing utilizing the photonic bandgap shift as the readout signal.The as-synthesized CDs with pyridinic-N-oxide functional groups adsorbed in the hollow mesoporous silica spheres are found to not only serve as the chloroform adsorption sites,but also a molecular glue that prevents crack formation in the colloidal PC.The sensitivity of HMSS@CDs-PCs sensor is 0.79 nm ppm^(-1)and an impressively low limit of detection is 3.22 ppm,which are the best reported values in fast-response chloroform vapor sensor without multi-signal assistance.The positive response time is 7.5 s and the negative response time 9 s.Furthermore,relatively stable sensing can be maintained within a relative humidity of 20%-85%RH and temperature of 25-55℃.This study demonstrates that HMSS@CDs-PCs sensors have practical application potential in indoor and outdoor chloroform vapor detection.
基金National Key Research and Development Program of China (2022YFE0206300)National Natural Science Foundation of China (U21A2081,22075074, 22209047)+3 种基金Guangdong Basic and Applied Basic Research Foundation (2024A1515011620)Hunan Provincial Natural Science Foundation of China (2024JJ5068)Foundation of Yuelushan Center for Industrial Innovation (2023YCII0119)Student Innovation Training Program (S202410532594,S202410532357)。
文摘Hard carbon (HC) has been considered as promising anode material for sodium-ion batteries (SIBs).The optimization of hard carbon’s microstructure and solid electrolyte interface (SEI) property are demonstrated effective in enhancing the Na+storage capability,however,a one-step regulation strategy to achieve simultaneous multi-scale structures optimization is highly desirable.Herein,we have systematically investigated the effects of boron doping on hard carbon’s microstructure and interface chemistry.A variety of structure characterizations show that appropriate amount of boron doping can increase the size of closed pores via rearrangement of carbon layers with improved graphitization degree,which provides more Na+storage sites.In-situ Fourier transform infrared spectroscopy/electrochemical impedance spectroscopy (FTIR/EIS) and X-ray photoelectron spectroscopy (XPS) analysis demonstrate the presence of more BC3and less B–C–O structures that result in enhanced ion diffusion kinetics and the formation of inorganic rich and robust SEI,which leads to facilitated charge transfer and excellent rate performance.As a result,the hard carbon anode with optimized boron doping content exhibits enhanced rate and cycling performance.In general,this work unravels the critical role of boron doping in optimizing the pore structure,interface chemistry and diffusion kinetics of hard carbon,which enables rational design of sodium-ion battery anode with enhanced Na+storage performance.
基金China Postdoctoral Science Foundation (2023M733451)Dalian Innovation Team in Key Areas(2020RT06)Engineering Research Center for Key Aromatic Compounds and LiaoNing Key Laboratory,Liaoning Provincial Natural Science Foundation (Doctoral Research Start-up Fund 2024-BSBA-37)。
文摘Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.
基金supported by the National Natural Science Foundation of China(22222601 and 22076019)the Fundamental Research Funds for the Central Universities(DUT23LAB611).
文摘The Cu^(+)/Cu^(0)sites of copper-based catalysts are crucial for enhancing the production of multicarbon(C_(2+))products from electrochemical CO_(2)reduction reaction(eCO_(2)RR).However,the unstable Cu^(+)and insufficient Cu^(+)/Cu^(0)active sites lead to their limited selectivity and stability for C_(2+)production.Herein,we embedded copper oxide(CuO_(x))particles into porous nitrogen-doped carbon nanofibers(CuO_(x)@PCNF)by pyrolysis of the electrospun fiber film containing ZIF-8 and Cu_(2)O particles.The porous nitrogendoped carbon nanofibers protected and dispersed Cu^(+)species,and its micro porous structure enhanced the interaction between CuO_(x)and reactants during eCO_(2)RR.The obtained CuO_(x)@PCNF created more effective and stable Cu^(+)/Cu^(0)active sites.It showed a high Faradaic efficiency of 62.5%for C_(2+)products in Hcell,which was 2 times higher than that of bare CuO_(x)(~31.1%).Furthermore,it achieved a maximum Faradaic efficiency of 80.7%for C_(2+)products in flow cell.In situ characterization and density functional theory(DFT)calculation confirmed that the N-doped carbon layer protected Cu^(+)from electrochemical reduction and lowered the energy barrier for the dimerization of^(*)CO.Stable and exposed Cu^(+)/Cu^(0)active sites enhanced the enrichment of^(*)CO and promoted the C-C coupling reaction on the catalyst surface,which facilitated the formation of C_(2+)products.
基金National Natural Science Foundation of China(U22B20149,22308376)Outstanding Young Scholars Foundation of China University of Petroleum(Beijing)(2462023BJRC015)Foundation of United Institute for Carbon Neutrality(CNIF20230209)。
文摘Dual atomic catalysts(DAC),particularly copper(Cu_(2))-based nitrogen(N)doped graphene,show great potential to effectively convert CO_(2)and nitrate(NO_(3)-)into important industrial chemicals such as ethylene,glycol,acetamide,and urea through an efficient catalytical process that involves C–C and C–N coupling.However,the origin of the coupling activity remained unclear,which substantially hinders the rational design of Cu-based catalysts for the N-integrated CO_(2)reduction reaction(CO_(2)RR).To address this challenge,this work performed advanced density functional theory calculations incorporating explicit solvation based on a Cu_(2)-based N-doped carbon(Cu_(2)N_(6)C_(10))catalyst for CO_(2)RR.These calculations are aimed to gain insight into the reaction mechanisms for the synthesis of ethylene,acetamide,and urea via coupling in the interfacial reaction micro-environment.Due to the sluggishness of CO_(2),the formation of a solvation electric layer by anions(F^(-),Cl^(-),Br^(-),and I^(-))and cations(Na+,Mg^(2+),K+,and Ca^(2+))leads to electron transfer towards the Cu surface.This process significantly accelerates the reduction of CO_(2).These results reveal that*CO intermediates play a pivotal role in N-integrated CO_(2)RR.Remarkably,the Cu_(2)-based N-doped carbon catalyst examined in this study has demonstrated the most potential for C–N coupling to date.Our findings reveal that through the process of a condensation reaction between*CO and NH_(2)OH for urea synthesis,*NO_(3)-is reduced to*NH_(3),and*CO_(2)to*CCO at dual Cu atom sites.This dual-site reduction facilitates the synthesis of acetamide through a nucleophilic reaction between NH_(3)and the ketene intermediate.Furthermore,we found that the I-and Mg^(2+)ions,influenced by pH,were highly effective for acetamide and ammonia synthesis,except when F-and Ca^(2+)were present.Furthermore,the mechanisms of C–N bond formation were investigated via ab-initio molecular dynamics simulations,and we found that adjusting the micro-environment can change the dominant side reaction,shifting from hydrogen production in acidic conditions to water reduction in alkaline ones.This study introduces a novel approach using ion-H_(2)O cages to significantly enhance the efficiency of C–N coupling reactions.
基金support from the Natural Science Foundation of Shanghai(23ZR1423800),Shuguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(18SG35)Open Research Fund of Shanghai Key Laboratory of Green Chemistry and Chemical Processes(East China Normal University)Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University.
文摘TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.
基金Supported by the National Natural Science Foundation of China(42072187)PetroChina Science and Technology Special Project(2021ZZ01-05)。
文摘Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbon neutrality system that balances energy production and carbon reduction becomes crucial for the transformation of such basins.Under the framework of a green and intelligent energy system primarily based on“four news”,new energy,new electricity,new energy storage,and new intelligence,integrating a“super energy system”composed of a huge amount of underground resources of coal,oil,gas and heat highly overlapping with abundant wind and solar energy resources above ground,and a regional intelligent energy consumption system with coordinated development and utilization of fossil energy and new energy,with a carbon neutrality system centered around carbon cycling is essential.This paper aims to select the traditional oil and gas basins as“super energy basins”with the conditions to build world-class energy production and demonstration bases for carbon neutrality.The Ordos Basin has unique regional advantages,including abundant fossil fuel and new energy resources,as well as matching CO_(2)sources and sinks,position it as a carbon neutrality“super energy basin”which explores the path of transformation of traditional oil and gas basins.Under the integrated development concept and mode of“coal+oil+gas+new energy+carbon capture,utilization and storage(CCUS)/carbon capture and storage(CCS)”,the carbon neutrality in super energy basin is basically achieved,which enhance energy supply and contribute to the carbon peak and carbon neutrality goals,establish a modern energy industry and promote regional green and sustainable development.The pioneering construction of the world-class carbon neutrality“super energy system”demonstration basin in China represented by the Ordos Basin will reshape the new concept and new mode of exploration and development of super energy basins,which is of great significance to the global energy revolution under carbon neutrality.
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supported by the “Project funded by the European Union-Next Generation EU”
文摘In the Mediterranean region,despite bamboo being an alien species that can seriously alter plant and ani-mal biocoenosis,the area occupied by bamboo plantations continues to increase,especially for the purpose to seques-ter carbon(C).However,the C dynamics in the soil-plant system when bamboo is grown outside its native area are poorly understood.Here we investigated the C mitigation potential of the fast-growing Moso bamboo(Phyllostachys edulis)introduced in Italy for climate-change mitigation.We analyzed aboveground(AGB)and belowground(as root/shoot ratio)biomass,litter and soil organic C(SOC)at O-15-and 15-30-cm depths in a 4-year-old bamboo plantation in comparison with the former annual cropland on which the bamboo was established.To have an idea of the maximum C stored at an ecosystem level,a natural forest adjacent the two sites was also considered.In the plantation,C accumulation as AGB was stimulated,with 14.8±3.1 Mg C ha^(-1) stored in 3 years;because thinning was done to remove culms from the first year,the mean sequestration rate was 4.9 Mg C ha^(-1) a^(-1).The sequestration rates were high but comparable to other fast-growing tree species in Italy(e.g.,Pinus nigra).SOC was significantly higher in the bamboo plantation than in the cropland only at the 0-15 cm depth,but SOC stock did not differ.Possibly 4 years were not enough time for a clear increase in SOC,or the high nutrient uptake by bamboos might have depleted the soil nutrients,thus inhibiting the soil organic matter formation by bacteria.In comparison,the natural forest had significantly higher C levels in all the pools.For C dynamics at an ecosystem level,the bamboo plantation on the former annual cropland led to substantial C removal from the atmosphere(about 12 Mg C ha^(-1) a^(-1)).However,despite the promising C sequestration rates by bamboo,its introduction should be carefully considered due to potential ecological problems caused by this species in overexploited environments such as the Mediterranean area.
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 China National Science Foundation(No.32371663,32361143869,32001166,and 42130506)the National Key Research and Development Program of China(No.2021YFD2200405)the Special Technology Innovation Fund of Carbon Peak and Carbon Neutrality in Jiangsu Province(No.BK20231515).
文摘Global forests are increasingly crucial for achiev-ing net-zero carbon emissions,with a quarter of the miti-gation efforts under the Paris Climate Agreement directed towards forests.In China,forests currently contribute to 13%of the global land’s carbon sink,but their stability and per-sistence remain uncertain.We examined and identified that published studies suffered from oversimplifications of eco-system succession and tree demographic dynamics,as well as poor constraints on land quality.Consequently,substan-tial estimations might have been suffered from underrepre-sented or ignored crucial factors,including tree demographic dynamics,and disturbances and habitat shifts caused by global climate change.We argue that these essential factors should be considered to enhance the reliability and accuracy of assessments of the potential for forest carbon sinks.
